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写真a

エイナガ ヒサヒロ
永長 久寛
EINAGA HISAHIRO
所属
総合理工学研究院 物質科学部門 教授
グリーンテクノロジー研究教育センター (併任)
シンクロトロン光利用研究センター (併任)
工学部 融合基礎工学科(併任)
総合理工学府 総合理工学専攻(併任)
職名
教授
連絡先
メールアドレス
電話番号
0925837525
プロフィール
触媒は物質変換をつかさどるキーマテリアルであり、特に、環境・エネルギー分野において緊急かつ社会的な課題が山積している現状から、触媒化学の果たす役割はますます重要である。複合酸化物触媒、金属ナノ粒子、ゼオライト、クラスターをベースとした触媒材料の設計・開発を行うとともに、これらの機能無機材料の物性・触媒特性の制御を試み、様々な環境・エネルギープロセスへの応用展開を図っている。
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学位

  • 博士(工学)

研究テーマ・研究キーワード

  • 研究テーマ: 金属ナノ粒子をベースとした触媒材料の精密設計

    研究キーワード: ナノ粒子、触媒、無機合成化学

    研究期間: 2004年4月

  • 研究テーマ: オゾンを酸化剤とした触媒酸化技術の開発

    研究キーワード: オゾン、触媒、酸化反応

    研究期間: 2002年4月

  • 研究テーマ: 光触媒材料の開発と環境浄化プロセスへの応用

    研究キーワード: 光触媒、環境負荷物質、浄化技術

    研究期間: 1995年4月

受賞

  • Catalysis Today Top Cited Article Award

    2006年1月   Elsevier  

  • Innovation and Creativity Prize Paper Award 2004

    2004年10月   Industry Applications Society IEEE  

  • James Melcher Paper Award

    2002年10月   Industry Applications Society IEEE  

論文

  • Catalytic performances of perovskite oxides for CO oxidation under microwave irradiation 査読 国際誌

    Hisahiro Einaga, Yusaku Nasu, Manabu Oda, H. Saito

    CHEMICAL ENGINEERING JOURNAL   283   97 - 104   2016年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.cej.2015.07.051

  • Codeposition of Colloidal Platinum Particles and Iron Chloride Precursor on TiO2 for Efficient Catalytic Oxidation of CO to CO2 査読 国際誌

    Hisahiro Einaga, Ryo Shiranita, H. Saito, Hata, Satoshi

    CHEMISTRY LETTERS   44 ( 12 )   1786 - 1788   2015年12月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1246/cl.150903

  • Catalytic Properties of Supported Metal Oxides for Oxidation Using Ozone 査読 国際誌

    Hisahiro Einaga, Nanako Maeda, Yusuke Nagai

    Catalysis Science & Technology   5   3147 - 3158   2015年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1039/C5CY00315F

  • Catalytic properties of copper-manganese mixed oxides supported on SiO2 for benzene oxidation with ozone 査読 国際誌

    Hisahiro Einaga, Nanako Maeda, Shintaro Yamamoto, 寺岡 靖剛

    CATALYSIS TODAY   245   22 - 27   2015年5月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.cattod.2014.09.018

  • Kinetic analysis of TiO2-catalyzed heterogeneous photocatalytic oxidation of ethylene using computational fluid dynamics

    Hisahiro Einaga, Junya Tokura, Yasutake Teraoka, Kazuhide Ito

    CHEMICAL ENGINEERING JOURNAL   263   2015年3月

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    記述言語:英語  

    DOI: 10.1016/j.cej.2014.11.017

  • Catalytic Properties of Copper Manganese Mixed Oxides Prepared by Coprecipitation Using Tetraammonium Hydroxide 査読 国際誌

    Hisahiro Einaga, Akihiro Kiya, Satoru Yoshioka, 寺岡 靖剛

    Catalysis Science & Technology   4   3713 - 3722   2015年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1039/C4CY00660G

  • CO oxidation over TiO2-supported Pt-Fe Catalysts Prepared by Coimpregnation Methods 査読 国際誌

    Hisahiro Einaga, Narihiro Urahama, 藤 章裕, 寺岡 靖剛

    Catalysis Letters   1653 - 1660   2014年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1007/s10562-014-1316-3

  • Preparation of platinum nanoparticles on TiO2 from DNA-protected particles 査読 国際誌

    永長 久寛, 川原田純基, 木村加奈, 寺岡 靖剛

    Colloids and Surfaces A: Physicochemical and Engineering Aspects   455   179 - 184   2014年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.colsurfa.2014.04.056

  • Catalytic Oxidation of Benzene by Ozone over Manganese Oxides Supported on USY zeolite 査読 国際誌

    永長 久寛, 寺岡 靖剛, 尾形 敦

    Journal of catalysis   305   227 - 237   2013年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.jcat.2013.05.016

  • Effect of Catalyst Composition and Preparation Conditions on Catalytic Properties of Unsupported Manganese Oxides for Benzene Oxidation with Ozone

    永長 久寛, 前田菜那子, 寺岡 靖剛

    Applied Catalysis B: Environmental   142-143   406 - 413   2013年5月

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    記述言語:英語  

    DOI: 10.1016/j.apcatb.2013.05.041

  • Photocatalytic Oxidation Processes for Toluene Oxidation over TiO2 Catalysts 査読 国際誌

    永長 久寛, 望月啓介, Yasutake Teraoka

    Catalysts   3   219 - 231   2013年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.3390/catal3010219

  • Preparation of highly dispersed platinum catalysts on various oxides by using polymer-protected nanoparticles 査読 国際誌

    K. Kimura, H. Einaga and Y. Teraoaka

    Catalysis Today   164 ( 1 )   2011年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Benzene Oxidation with Ozone over Manganese Oxide Supported on Zeolite Catalysts 査読 国際誌

    H. Einaga, Y. Teraoka and A. Ogata

    Catalysis Today   164 ( 1 )   2011年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Catalytic Properties of Platinum Supported on Titanium Dioxide by Liquid-phase Adsorption of Colloidal Nanoparticles 査読 国際誌

    K. Kimura, H. Einaga, Y. Teraoaka,

    Catalysis Letters   139   2010年10月

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    掲載種別:研究論文(学術雑誌)  

  • Complete Oxidation of Benzene over Perovskite-type Oxide Catalysts 査読 国際誌

    H. Einaga, S. Hyodo, and Y. Teraoka

    Topics in Catal.   53   2010年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Catalytic Oxidation of Benzene in Gas Phase over Alumina-supported Silver Catalysts 国際誌

    H. Einaga, A. Ogata

    Environ. Sci Technol   44   2010年4月

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    掲載種別:研究論文(学術雑誌)  

  • Catalytic Oxidation of Benzene with Ozone over SiO2-supported Manganese Oxides 査読 国際誌

    H. Einaga and A. Ogata

    J. Hazard. Mater.   2009年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Relationship between the Structure of Manganese Oxides on Alumina and Catalytic Activities for Benzene Oxidation with Ozone 査読 国際誌

    H. Einaga, M. Harada and A. Ogata

    Catal. Lett.   2009年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • In-Situ XAFS Studies of Au Particle Formation by Photoreduction in Polymer Solutions 査読 国際誌

    Masafumi Harada, Hisahiro Einaga

    Langmuir   2007年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Catalytic oxidation of benzene with ozone over Mn ion-exchanged zeolites 査読 国際誌

    H. Einaga, S. Futamura

    Catal. Commun.   2007年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Preparation of Pt/Rh Bimetallic Colloidal Particles in Polymer Solutions Using Borohydride-Reduction 査読 国際誌

    Masafumi Harada, Hisahiro Einaga

    J. Colloid.Interf. Sci.   2007年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Effect of Water Vapor on Catalytic Oxidation of Benzene with Ozone on Alumina-supported Manganese Oxides 査読 国際誌

    H. Einaga, S. Futamura,

    J. Catal.   2006年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Structural Changes in Alumina-supported Manganese Oxides during Ozone Decomposition

    H. Einaga, M. Harada, S. Futamura

    Chem. Phys. Lett.   2005年5月

  • Photochemical Preparation of PVP-stabilized Platinum Colloids and Their Deposition on Titanium Dioxide 査読 国際誌

    H. Einaga, M. Harada

    Langmuir   2005年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Oxidation Behavior of of Cyclohexane on Alumina-supported Manganese Oxides with Ozone 査読 国際誌

    H. Einaga, S. Futamura

    Appl. Catal. B: Environ.   2005年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Improvement of Catalyst Durability by Deposition of Rh on TiO2 in Photooxidation of Aromatic Compounds 査読 国際誌

    H. Einaga, T. Ibusuki, S. Futamura

    Environ. Sci. Technol.   2004年1月

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    記述言語:日本語   掲載種別:研究論文(学術雑誌)  

  • Catalytic Oxidation of Benzene with Ozone over Alumina-supported Manganese Oxides 査読 国際誌

    H. Einaga, S. Futamura

    J. Catal.   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Photocatalytic Oxidation of Benzene in Air 査読 国際誌

    H. Einaga, T. Ibusuki, S. Futamura

    J. Solar Energy Eng.   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Generation of Active Sites for CO Photooxidation on TiO2 by Platinum Deposition 査読 国際誌

    H. Einaga, M. Harada, S. Futamura, T. Ibusuki

    J. Phys. Chem. B   2003年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Heterogeneous Photocatalytic Oxidation of Benzene, Toluene, Cyclohexene and Cyclohexane in Humidified Air, Comparison of Decomposition Behavior on Photoirradiated TiO2 Catalyst 査読 国際誌

    H Einaga, S. Futamura, T. Ibusuki

    Appl. Catal., B: Environ.   2002年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Complete Oxidation of Benzene in Gas Phase by Platinized Titania Photocatalysts 査読 国際誌

    H. Einaga, S. Futamura, T. Ibusuki

    Environ. Sci. & Technol.   2001年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Performance Evaluation of a Hybrid System Comprising Silent Discharge Plasma and Manganese Oxide Catalysts for Benzene Decomposition 査読 国際誌

    H. Einaga, T. Ibusuki, S. Futamura

    IEEE Trans. Ind. Applicat.   2001年1月

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    掲載種別:研究論文(学術雑誌)  

  • Photocatalytic Decomposition of Benzene over TiO2 in a Humidified Airstream 査読 国際誌

    H. Einaga, S. Futamura, T. Ibusuki

    Phys. Chem. Chem. Phys   1999年12月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • The Stabilization of Active Oxygen Species by Pt Supported on TiO2 査読 国際誌

    H.Einaga, A. Ogata, S. Futamura, T. Ibusuki

    Chem. Phys. Lett.   1900年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Structural analysis of manganese oxides supported on SiO2 for benzene oxidation with ozone 査読 国際誌

    永長 久寛, 山本晋太郎, 前田菜那子, 寺岡 靖剛

    Catalysis Today   242 ( Part B )   287 - 293   1900年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.cattod.2014.05.018

  • Effect of manganese oxides supported on zeolite Y on catalytic oxidation of benzene by ozone

    Zheng, XR; Einaga, H

    CATALYSIS TODAY   446   2025年2月   ISSN:0920-5861 eISSN:1873-4308

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    出版者・発行元:Catalysis Today  

    Manganese oxide catalysts with different structures and loading levels were supported on zeolite Y catalysts using a dry impregnation method for the oxidation of low concentrations of benzene with ozone. X-ray diffraction (XRD) and X-ray absorption fine structure (XAFS) studies revealed that manganese oxide was highly dispersed on the zeolite in a low oxidation state for those prepared with the acetate precursor, and highly oxidized and aggregated manganese oxide for those prepared with the nitrate precursor. In the reaction at 70 ℃, the benzene oxidation rate, CO2 selectivity, and ozone/benzene decomposition ratio were independent of the manganese loading, manganese precursor, and zeolite Y porosity. These catalytic properties were found to be less dependent on the manganese oxide structure. A slight increase in the reaction temperature enhanced both the catalytic activity and the catalyst performance, while the presence of water vapor had no significant impact. The XAFS analysis of the spent catalysts indicated that during the benzene decomposition reaction, the structure of the manganese oxide loaded on the catalyst was altered, and its oxidation state was uniformly reduced.

    DOI: 10.1016/j.cattod.2024.115104

    Web of Science

    Scopus

  • Structural Changes in Manganese Oxides on Zeolite Y in Benzene Oxidation with Ozone and Post-Heat Treatment

    Zheng, XR; Einaga, H

    CATALYSIS LETTERS   155 ( 1 )   2025年1月   ISSN:1011-372X eISSN:1572-879X

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    出版者・発行元:Catalysis Letters  

    MnOX supported on a zeolite Y catalyst (MnOX/Y) is widely utilized for the removal of volatile organic compounds (VOCs), providing an understanding of catalyst structural changes and the factors influencing these changes. This study introduces a heat treatment method to recover the catalyst. The efficacy of the treated catalysts in enhancing the oxidation of benzene by ozone was improved. Investigation of the behavior of catalysts prepared from acetate and nitrate precursors revealed a common trend: MnOX in the catalysts was readily reduced to MnO by intermediate products, acids, aldehydes, and phenols formed during the benzene ozonation process, as evidenced by X-ray absorption fine structure temperature-programmed reduction and in situ Fourier-transform infrared spectroscopy analyses. Heat treatment at 200 °C was found to be insufficient for the restoration of the MnOX structure, which was attributed to the persistence of acids and hydrocarbons within the catalyst. 500 °C was determined to be more appropriate for the regeneration of the used catalysts, indicating the critical role of the heat treatment conditions in maintaining the effectiveness of the MnOX/Y catalysts in VOC removal applications. Graphical Abstract: (Figure presented.)

    DOI: 10.1007/s10562-024-04836-2

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  • Microwave-enhanced catalytic conversion of fatty acid ester to olefins by Na-ZSM-5

    Ota, S; Fukushima, J; Kimijima, K; Kimura, M; Igura, N; Tezuka, N; Sato, T; Einaga, H; Tsubaki, S

    CHEMICAL ENGINEERING JOURNAL   497   2024年10月   ISSN:1385-8947 eISSN:1873-3212

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    出版者・発行元:Chemical Engineering Journal  

    The bio-based production of essential chemicals is important for the sustainability of the chemical industry. Here, we demonstrate efficient olefin production from methyl oleate using Na substituted ZSM-5 (Na-ZSM-5) and microwave irradiation. Na-ZSM-5 exhibits superior microwave heating properties compared to H-ZSM-5 and other zeolites. It was more effective in converting methyl oleate to olefins such as ethylene and propylene than H-ZSM-5 or Y zeolites. Microwave irradiation promoted the conversion efficiency of methyl oleate by Na-ZSM-5, achieving an olefin yield over four times higher than that obtained with conventional heating (CH) using an electric furnace. Meanwhile, the aromatization to benzene, toluene and xylene (BTX) was suppressed using Na-ZSM-5, which was attributed to the removal of strong acid sites. In addition, in situ microwave XRD revealed that microwaves promoted temperature-dependent structural changes in Na-ZSM-5 at lower temperatures than CH, suggesting that microwaves form localized high temperatures in the zeolite. These localized high temperatures effectively enhance olefin production via microwave irradiation.

    DOI: 10.1016/j.cej.2024.154737

    Web of Science

    Scopus

  • Boosting Benzene’s Ozone Catalytic Oxidation at Mild Temperatures over Highly Dispersed Ag-Doped Mn<inf>3</inf>O<inf>4</inf>

    Guo H., Cen L., Deng K., Mo W., Hajime H., Hu D., Zhang P., Shangguan W., Huang H., Einaga H.

    Catalysts   14 ( 9 )   2024年9月   eISSN:2073-4344

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    出版者・発行元:Catalysts  

    Transition metal oxides show high activity while still facing the challenges of low mineralization and poor durability in the ozone catalytic oxidation (OCO) of volatile organic compounds (VOCs). Improving the oxygen mobility and low-temperature reducibility of transition metal oxides was found to be an effective way to address the above challenges. Here, highly dispersed Ag was added to Mn3O4 via the co-precipitation oxalate route, and the obtained Ag/Mn3O4 exhibited higher mineralization and stability in benzene catalytic ozonation at room temperature. Compared to Mn3O4, the concentration of CO2 formed from benzene oxidation over Ag/Mn3O4 was significantly increased, from 585.4 ppm to 810.9 ppm, while CO generation was greatly suppressed to only one tenth of its original value (194 ppm vs. 19 ppm). In addition, Ag/Mn3O4 exhibited higher catalytic stability than Mn3O4. The introduction of Ag obviously improved the oxygen mobility and low-temperature reducibility of Mn3O4. Moreover, the highly dispersed Ag also promoted the activity of surface oxygen species and the chemisorption of benzene on Mn3O4. The above physicochemical properties contributed to the excellent catalytic performance and durability of Ag/Mn3O4. This research could shed light on the improvement in VOC mineralization via ozone catalytic oxidation.

    DOI: 10.3390/catal14090554

    Web of Science

    Scopus

  • Comparative Evaluation of Microwave Heating Performance across Structurally Diverse Tungsten Oxides

    Ni, ZT; Hojo, H; Einaga, H

    JOURNAL OF PHYSICAL CHEMISTRY C   128 ( 33 )   13807 - 13815   2024年8月   ISSN:1932-7447 eISSN:1932-7455

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    出版者・発行元:Journal of Physical Chemistry C  

    Microwave heating is an effective method for efficiently heating a target material, allowing the chemical reaction processes to proceed quickly. In catalytic reactions under microwave irradiation, it is essential to understand the relationship between the structure and physical properties of the material to be used as a catalyst and microwave heating. In this study, we focused on tungsten oxides, which absorb microwaves and convert them into heat, and we compared the microwave heating properties of tungsten oxides with different structures. The heating properties of tungsten oxides under microwave irradiation are highly dependent on their morphologies. WO3 nanoflakes with a monoclinic phase structure have a more rapidly heated surface than tungsten oxides with other morphologies. The heating characteristics of each tungsten oxide were consistent with the dielectric loss factor obtained by the perturbation method. Finite element analysis was used to gain a better understanding of the thermal distribution of materials during microwave irradiation.

    DOI: 10.1021/acs.jpcc.4c02936

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  • Fundamental insights and recent advances in catalytic oxidation processes using ozone for the control of volatile organic compounds

    Einaga H., Zheng X.

    Environmental Science and Pollution Research   31 ( 31 )   43540 - 43560   2024年7月   ISSN:09441344

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    記述言語:英語   出版者・発行元:Environmental Science and Pollution Research  

    The development of technologies for highly efficient treatment of emissions containing low concentrations of volatile organic compounds (VOCs) remains an important challenge. Catalytic oxidation with ozone (catalytic ozonation) is useful for the oxidative decomposition of VOCs, particularly aromatic compounds, under ambient temperature conditions. Only inexpensive transition metal oxides are required as catalysts, and Mn-based catalysts are widely used for catalytic ozonation. This review describes the oxidation reaction mechanisms, reaction pathways of aromatic hydrocarbons, and dependence of the catalytic ozonation activity on the reaction conditions. The reasons why Mn oxides are effective in catalytic ozonation are also explained. The structure of the catalytic active sites and the types of supporting materials contributing to the reaction are also discussed in detail, with the aim of establishing a VOC control technology. In addition, recent progress in catalytic oxidation processes using ozone as an oxidant has been outlined, focusing on catalyst materials and reaction conditions.

    DOI: 10.1007/s11356-024-34004-3

    Scopus

    PubMed

  • Microwave-assisted CO oxidation over LaNiO<sub>3</sub> and Ce-promoted LaNiO<sub>3</sub>

    Hamashima, T; Sugiyama, T; Hojo, H; Einaga, H

    JOURNAL OF THE TAIWAN INSTITUTE OF CHEMICAL ENGINEERS   158   2024年5月   ISSN:1876-1070 eISSN:1876-1089

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    出版者・発行元:Journal of the Taiwan Institute of Chemical Engineers  

    Microwave-assisted catalytic reactions have been investigated for energy-efficient chemical processes. However, catalysts with comparatively high heating properties, activities, and economics have been developed with limited success. In this study, we investigated the catalytic properties of Ce addition to LaNiO3 catalyst, which has high CO oxidation activity and high microwave heating properties. Ce-added catalysts exhibited high heating properties under microwave heating. Increasing the Ce content in the catalyst enhanced the dielectric loss factor, the ability to absorb microwaves and convert them to heat, and improved the microwave heating properties of the catalyst. The catalytic activity toward CO oxidation over Ce-added catalysts decreased in the order of La0.8Ce0.2NiO3 > La0.9Ce0.1NiO3 > LaNiO3 at all oxygen partial pressures when compared to the same microwave power. To clarify the role of Ce addition, temperature programmed reduction (TPR) by H2, CO, and XAFS measurements were performed. TPR results suggested that Ce promotes oxygen mobility and then affects both CO oxidation and microwave heating properties.

    DOI: 10.1016/j.jtice.2023.105041

    Web of Science

    Scopus

  • Promoted catalytic oxidation of benzene over Mn-Ni solid solutions: Effect of metal oxygen bond parameters

    Guo, H; Huang, HB; Zhu, Q; Shangguan, WF; Einaga, H; Zhang, YX

    APPLIED CATALYSIS A-GENERAL   671   2024年2月   ISSN:0926-860X eISSN:1873-3875

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    出版者・発行元:Applied Catalysis A: General  

    In this work, Mn-Ni solid solutions were obtained by doping Ni into MnOx via solution combustion synthesis and the resulting catalysts were then applied to benzene oxidation. Various characterizations revealed that Ni doping changed the metal oxygen bond parameters, such as coordination numbers (CNs) and bond length. Both Mn-O and Ni-O bonds in Mn-Ni solid solutions exerted reduced CNs, while the bond length of Mn-O bonds was extended, making the oxygen species more chemically reactive., which further improved physicochemical properties (such as reducibility, oxygen mobility, surface active oxygen species etc.) and catalytic performance. Remarkably, the solid solutions with a Mn/Ni molar ratio of 4:1 (named Mn4Ni1) showed Mn-O and Ni-O bonds with lower CNs and longer bond lengths, which enhanced the activity and mobility of oxygen species, reducibility and chemisorption capacity of benzene. Therefore, Mn4Ni1 demonstrated optimal benzene oxidation activity and showed the lowest T90 (192 °C). The potential reaction mechanism was proposed according to the analysis results of C6H6-TPSR and in-situ FTIR. Furthermore, promoted oxidation of benzene and phenolate species on Mn4Ni1 could inhibit accumulation of intermediates and avoid catalyst poisoning and deactivation. This strategy shed light to the design of catalysts in environmental catalysis and thermal catalysis.

    DOI: 10.1016/j.apcata.2024.119575

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  • Lattice-Plane-Dependent Distribution of Ce<SUP>3+</SUP> at Pt and CeO<sub>2</sub> Interfaces for Pt/CeO<sub>2</sub> Catalysts

    Hojo, H; Nakashima, M; Yoshizaki, S; Einaga, H

    ACS NANO   18 ( 6 )   4775 - 4782   2024年1月   ISSN:1936-0851 eISSN:1936-086X

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    記述言語:英語   出版者・発行元:ACS Nano  

    The interaction between a metal and a support, which is known as the metal-support interaction, often plays a determining role in the catalytic properties of supported metal catalysts. Herein, we have developed model Pt/CeO2 catalysts, which enabled us to investigate the interface atomic and electronic structures between Pt and the {001}, {011}, and {111} planes of CeO2 using scanning transmission electron microscopy and electron energy-loss spectroscopy. We found that the number of Ce3+ ions around the Pt nanoparticles followed the order {001} > {011} > {111}, which was the opposite order of the generally accepted stability of low index surfaces of CeO2. Systematic first-principles calculations revealed that the presence of Pt nanoparticles facilitated the formation of oxygen vacancies and that the appearance of the Ptδ+ state was preferred when Pt nanoparticles were in contact with CeO2 {001} planes due to direct charge transfer from Pt to CeO2. These results provide important insights into the nature of the metal-support interaction for a comprehensive understanding of the properties of supported metal catalysts.

    DOI: 10.1021/acsnano.3c09092

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  • WO<sub>3</sub>-based Materials for Photocatalytic and Photoelectrocatalytic Selective Oxidation Reactions

    Wang, ZR; Einaga, H

    CHEMCATCHEM   15 ( 21 )   2023年11月   ISSN:1867-3880 eISSN:1867-3899

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    出版者・発行元:ChemCatChem  

    Selective oxidation reactions are crucial in producing various chemicals in the industry. However, most catalytic processes for these reactions use harsh reaction conditions. Recently, heterogeneous photo(electro)catalysis has been considered promising for selective oxidation reactions under mild conditions. Semiconductor materials are frequently used as heterogeneous photocatalysts because they can produce active species that contribute to the oxidation of organic compounds under light irradiation. Among various semiconductor photocatalysts, tungsten oxide (WO3) is one of the most promising candidates due to its advantages, including high stability, wide light adsorption range, proper band structures, and unique catalytic mechanism. This paper reviews the WO3-based materials for photocatalytic (PC) and photoelectrocatalytic (PEC) selective oxidations. We summarize the strategies for designing WO3 structures, which include morphology control, crystal facet optimization, and defect engineering. Then, the finely designed WO3 structures for PC and PEC oxidation of several typical organic compounds have been discussed based on catalytic mechanism and performance. Finally, we propose the prospects and challenges of WO3 photocatalysts and photoanodes in selective oxidation reactions.

    DOI: 10.1002/cctc.202300723

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  • Enhanced Benzene Oxidation of Sintered Pd/γ-Al<sub>2</sub>O<sub>3</sub> Catalysts by SO<sub>2</sub> Treatment

    Shigenobu, S; Sugiyama, T; Hojo, H; Einaga, H

    CATALYSIS LETTERS   153 ( 11 )   3423 - 3432   2023年11月   ISSN:1011-372X eISSN:1572-879X

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    出版者・発行元:Catalysis Letters  

    The effect of sulfurization by SO2 on the activity of Pd/γ-Al2O3 for benzene oxidation was investigated. The activity decreased by heat treatment at 800 °C due to Pd particle coarsening. SO2 treatment at 600 °C suppressed the formation of byproduct compounds on the catalyst and improved the activity of the sintered Pd/γ-Al2O3 catalyst. Graphical Abstract: [Figure not available: see fulltext.]

    DOI: 10.1007/s10562-022-04233-7

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  • Catalytic degradation of benzene over non-thermal plasma coupled Co-Ni binary metal oxide nanosheet catalysts

    Jiang, Z; Fang, DX; Liang, YT; He, YY; Einaga, H; Shangguan, WF

    JOURNAL OF ENVIRONMENTAL SCIENCES   132   1 - 11   2023年10月   ISSN:1001-0742 eISSN:1878-7320

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    記述言語:英語   出版者・発行元:Journal of Environmental Sciences (China)  

    Non-thermal plasma (NTP) has been demonstrated as one of the promising technologies that can degrade volatile organic compounds (VOCs) under ambient condition. However, one of the key challenges of VOCs degradation in NTP is its relatively low mineralization rate, which needs to be addressed by introducing catalysts. Therefore, the design and optimization of catalysts have become the focus of NTP coupling catalysis research. In this work, a series of two-dimensional nanosheet Co-Ni metal oxides were synthesized by microwave method and investigated for the catalytic oxidation of benzene in an NTP-catalysis coupling system. Among them, Co2Ni1Ox achieves 60% carbon dioxide (CO2) selectivity (SCO2) when the benzene removal efficiency (REbenzene) reaches more than 99%, which is a significant enhancement compared with the CO2 selectivity obtained without any catalysts (38%) under the same input power. More intriguingly, this SCO2 is also significantly higher than that of single metal oxides, NiO or Co3O4, which is only around 40%. Such improved performance of this binary metal oxide catalyst is uniquely attributed to the synergistic effects of Co and Ni in Co2Ni1Ox catalyst. The introduction of Co2Ni1Ox was found to promote the generation of acrolein significantly, one of the key intermediates found in NTP alone system reported previously, suggest the benzene ring open reaction is promoted. Compared with monometallic oxides NiO and Co3O4, Co2Ni1Ox also shows higher active oxygen proportion, better oxygen mobility, and stronger low-temperature redox capability. The above factors result in the improved catalytic performance of Co2Ni1Ox in the NTP coupling removal of benzene.

    DOI: 10.1016/j.jes.2022.09.030

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  • Recent trends in phenol synthesis by photocatalytic oxidation of benzene

    Wang Z., Hisahiro E.

    Dalton Transactions   52 ( 28 )   9525 - 9540   2023年6月   ISSN:14779226

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    記述言語:英語   出版者・発行元:Dalton Transactions  

    Phenol is an important intermediate for manufacturing chemical products in industry. In recent decades, phenol synthesis by one-pot oxidation of benzene has aroused tremendous interest in phenol synthesis due to the enormous energy consumption of the three-step cumene method in the industry. Photocatalysis is promising for the selective conversion of benzene to phenol because it can proceed under mild reaction conditions. However, overoxidation of phenol by photocatalysts with high oxidation ability decreases the yield and selectivity, which is the major limiting factor. Thus, increasing the phenol formation efficiency plays a crucial role in photocatalytic systems for benzene oxidation. In this context, selective photocatalytic benzene oxidation over several types of photocatalytic systems has been developed rapidly in the past few years. In this perspective, current homogeneous and heterogeneous photocatalytic systems for this reaction have been reviewed systematically first. Then, an overview of some strategies from the last decade for increasing phenol selectivity has been provided. In the end, a summary and outlook on the challenges and future directions in the research field are included in this perspective, which would be of great interest for further improving the selectivity of the photocatalytic benzene oxidation reaction.

    DOI: 10.1039/d3dt01360j

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  • Insights into the effect of cobalt substitution into copper-manganese oxides on enhanced benzene oxidation activity

    Ding, SY; Zhu, C; Hojo, H; Einaga, H

    APPLIED CATALYSIS B-ENVIRONMENTAL   323   2023年4月   ISSN:0926-3373 eISSN:1873-3883

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    出版者・発行元:Applied Catalysis B: Environmental  

    Co-substituted Cu-Mn spinel oxides were synthesized, characterized, and catalytic performance for benzene oxidation was evaluated. Spinel phases, and the substitution of Mn sites by Co were confirmed for the ternary oxides. Co0.2Cu0.8MnOy showed the highest activities with the lowest apparent activation energy among the ternary oxides. The improved catalytic properties due to Co substitution are attributed to more activated lattice oxygen, stronger adsorption of benzene, and a larger specific surface area. Density functional theory simulations also revealed that the Co substitution enhanced the reactivity of the lattice oxygen. Adsorbed and activated benzene reacted with lattice oxygen to form abundant oxygen defects, which promoted O2 adsorption and dissociation, contributing to enhanced catalytic activity. The effect of water vapor on the catalytic benzene oxidation was also clarified.

    DOI: 10.1016/j.apcatb.2022.122099

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  • Reduction Mechanism for CeO<sub>2</sub> Revealed by Direct Observation of the Oxygen Vacancy Distribution in Shape‐Controlled CeO<sub>2</sub>

    北條 元, 廣田 利輝, 伊藤 蒼, 永長 久寛

    ADVANCED MATERIALS INTERFACES   10 ( 6 )   2201954   2023年2月   ISSN:21967350 eISSN:21967350

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    記述言語:英語   出版者・発行元:Wiley  

    CeO2 and CeO2-based materials are widely used as catalysts and catalyst supports for a variety of chemical reactions. The ability to form oxygen vacancies plays an important role in the catalytic activities in these materials. Therefore, revealing the reduction mechanism for CeO2 is crucial to understanding the catalytic activities. In this study, shape-controlled CeO2 nanoparticles are fabricated and the distribution of surface oxygen vacancies on the (100) and (111) surfaces is systematically studied using scanning transmission electron microscopy and electron energy-loss spectroscopy and the response to H2 reduction treatment. It is successfully demonstrated that both catalytic activities and the ability to form oxygen vacancies are strongly dependent on the type of lattice planes. Moreover, the present results provide important insights into the reduction mechanism for CeO2, in which bulk oxygen instead of the widely believed surface capping oxygen makes no small contribution to the initial reduction step.

    DOI: 10.1002/admi.202201954

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  • Catalytic properties of LaNiO3 and Mn-modified LaNiO3 catalysts for oxidation of CO and benzene

    Hojo, H; Inohara, Y; Ichitsubo, R; Einaga, H

    CATALYSIS TODAY   410   127 - 134   2023年2月   ISSN:0920-5861 eISSN:1873-4308

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    出版者・発行元:Catalysis Today  

    ABO3-type perovskite oxides containing transition metals at the B site are effective catalysts for oxidation reactions. In this study, LaNiO3 was prepared by the hydrolysis-precipitation method, and LaNiO3 was modified with Mn by the impregnation method. LaNiO3 showed higher CO oxidation activity than LaCoO3, LaMnO3, and LaFeO3. The high activity of LaNiO3 was attributed to the reactivity of the lattice oxygen in LaNiO3, as confirmed by temperature-programmed reduction by H2 (H2-TPR) and CO-TPR studies. The Mn-modified LaNiO3 exhibited higher activity for benzene oxidation than LaNiO3. The CO oxidation properties of the Mn-modified LaNiO3 catalysts correlated with their H2-reduction properties, whereas benzene oxidation properties were improved by the increasing amount of Mn on the catalyst surface.

    DOI: 10.1016/j.cattod.2022.07.002

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  • Enhanced Photocatalytic Benzene Oxidation to Phenol over Monoclinic WO<sub>3</sub> Nanorods under Visible Light

    Wang, ZR; Zhu, C; Ni, ZT; Hojo, H; Einaga, H

    ACS CATALYSIS   12 ( 24 )   14976 - 14989   2022年12月   ISSN:2155-5435

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    出版者・発行元:ACS Catalysis  

    The photocatalytic oxidation of benzene to phenol driven by visible light (λ > 420 nm) at room temperature and under ambient pressure is a promising process. In particular, the application of heterogeneous catalysts to benzene photooxidation, where the catalyst and product are easily separated, facilitates the construction of practical processes. Here, we report that a Pt-loaded 1D monoclinic WO3nanorod (Pt/m-WNR) exhibited higher activities than other Pt/WO3catalysts with different crystal structures and morphologies in water under ambient conditions and visible light. Pt/m-WNR showed high stability in repeated reactions. Furthermore, other typical photocatalysts (TiO2, Bi2WO6, Bi2MoO6, BiOBr, and C3N4) showed negligible phenol formation using Pt as a cocatalyst. Both experimental results and density functional theory calculations show that the specific performance of Pt/m-WNR is due to the efficient reduction of O2to produce hydroxyl radicals via H2O2as an intermediate. Notably, m-WNR shows much higher phenol formation than h-WNR, although h-WNR has a higher surface area. The higher activity of m-WNR may be due to its lower work function to provide electrons for O2reduction. A lower work function will favorably form a higher Schottky barrier with Pt nanoparticles to suppress the recombination of photogenerated charge carriers. The effect of the Schottky barrier is further confirmed by different activities using various metal particles as cocatalysts.

    DOI: 10.1021/acscatal.2c03832

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  • Catalytic Oxidation of CO to CO2 over CeO2-Supported Pd-Cu Catalysts under Dilute O2 Conditions

    Shigenobu, S; Hojo, H; Einaga, H

    INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH   61 ( 43 )   15856 - 15865   2022年10月   ISSN:0888-5885

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    出版者・発行元:Industrial and Engineering Chemistry Research  

    Catalytic CO oxidation processes under dilute oxygen conditions are key industrial and environmental processes. CeO2-supported Pd and Pd-Cu catalysts (Pd/CeO2and Pd-Cu/CeO2) were prepared by impregnation, and the effect of Cu addition on the catalytic properties of CO oxidation was investigated under CO/O2stoichiometric conditions. The activity of Pd/CeO2was superior to that of Pd/TiO2and Pd/Al2O3at low temperatures. The Cu addition to Pd/CeO2with a Cu/Pd molar ratio of approximately 1-5 enhanced the CO oxidation activity. Small PdO particles were distributed over the CeO2surfaces, and Cu addition decreased the size of the Pd particles on the CeO2and increased the fraction of highly reactive Pd sites. As the Cu/Pd mole fraction in the Pd-Cu/CeO2catalyst increased to 10, the PdO on CeO2agglomerated significantly, and the CO oxidation activity decreased.

    DOI: 10.1021/acs.iecr.2c02199

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  • Direct identification of the charge state in a single platinum nanoparticle on titanium oxide

    Aso, R; Hojo, H; Takahashi, Y; Akashi, T; Midoh, Y; Ichihashi, F; Nakajima, H; Tamaoka, T; Yubuta, K; Nakanishi, H; Einaga, H; Tanigaki, T; Shinada, H; Murakami, Y

    SCIENCE   378 ( 6616 )   202 - 206   2022年10月   ISSN:0036-8075 eISSN:1095-9203

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    記述言語:英語   出版者・発行元:Science  

    A goal in the characterization of supported metal catalysts is to achieve particle-by-particle analysis of the charge state strongly correlated with the catalytic activity. Here, we demonstrate the direct identification of the charge state of individual platinum nanoparticles (NPs) supported on titanium dioxide using ultrahigh sensitivity and precision electron holography. Sophisticated phase-shift analysis for the part of the NPs protruding into the vacuum visualized slight potential changes around individual platinum NPs. The analysis revealed the number (only one to six electrons) and sense (positive or negative) of the charge per platinum NP. The underlying mechanism of platinum charging is explained by the work function differences between platinum and titanium dioxide (depending on the orientation relationship and lattice distortion) and by first-principles calculations in terms of the charge transfer processes.

    DOI: 10.1126/science.abq5868

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  • Microwave-assisted removal of benzene with high efficiency on cobalt modified copper-manganese spinel oxides

    Ding, SY; Hojo, H; Einaga, H

    JOURNAL OF ENVIRONMENTAL CHEMICAL ENGINEERING   10 ( 5 )   2022年10月   ISSN:2213-2929 eISSN:2213-3437

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    出版者・発行元:Journal of Environmental Chemical Engineering  

    Microwave-assisted process has been demonstrated to have immense potential for promoting chemical reactions and reducing energy consumption. In this study, catalytic oxidation of benzene was carried out over Co-Cu-Mn mixed oxides (CoxMn1-xCuOy) under microwave irradiation. The spinel-type mixed oxides were mainly formed for the Co-Cu-Mn mixed oxides with different Co/Mn ratios. The substitution of Mn sites by Co was confirmed by Fourier and Wavelet transformed extended x-ray absorption fine structure spectra. As the Co/Mn ratio increased, the heating characteristics of the catalysts under microwave irradiation monotonically improved. The benzene oxidation activity increased on the Co/Mn ratio of 2/3 due to the enhanced specific surface area, benzene adsorption properties, and lattice-oxygen reactivity. Microwave inducing significantly lowered the reaction temperature required for benzene oxidation. Co0.4Mn0.6CuOy completely oxidized benzene at a relatively low microwave power compared to pristine Cu-Mn oxides. The Co-Cu-Mn oxides showed high activity and stability for benzene oxidation even under humid conditions. Combining pre-adsorption and thermal oxidation processes on Co0.4Mn0.6CuOy improved the low concentration of benzene oxidation efficiency by rapid microwave heating. The compound of Co0.4Mn0.6CuOy and Co0.8Mn0.2CuOy mixed at 3:1 showed even higher activity than Co0.4Mn0.6CuOy.

    DOI: 10.1016/j.jece.2022.108212

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  • Insights into the Hydrogenolysis Mechanism of Diphenyl Ether over Cl-Modified Pt/?-Al2O3 Catalysts by Experimental and Theoretical Studies

    Zhu, C; Hojo, H; Einaga, H

    ACS SUSTAINABLE CHEMISTRY & ENGINEERING   10 ( 27 )   8897 - 8907   2022年6月   ISSN:2168-0485

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    出版者・発行元:ACS Sustainable Chemistry and Engineering  

    Catalytic hydrogenolysis is an efficient method for converting lignin-derived aryl ethers into monoaromatic products by cleaving the C-O bond and maintaining the phenyl rings. However, it is difficult to obtain aromatics with high selectivity because ring hydrogenation proceeds in parallel. Herein, we showed that a Cl-modified Pt/γ-Al2O3 catalyst exhibited higher selectivity for aromatics (91.6%) compared to unmodified Pt/γ-Al2O3 (3.9%) in C-O bond cleavage of diphenyl ether (DPE, 4-O-5 linkage in lignin). Characterization of the catalysts and density functional theory (DFT) calculations indicated that the Cl species preferred to localize at the terrace sites of Pt nanoparticles (NPs). Due to the decrease in the number of active sites, the Cl-modified Pt/γ-Al2O3 catalyst exhibited low activity for 2-propanol dehydrogenation, and thus the catalytic activity for the hydrogenation of aromatic products was suppressed. On the other hand, DPE adsorbed at the low coordination site, which caused the phenyl rings to move away from the metal surface; this configuration was unfavorable for the hydrogenation reaction. According to DFT calculations, the high selectivity for benzene was mainly attributed to the lower energy barrier for C-O bond cleavage of phenol at the low-coordination sites.

    DOI: 10.1021/acssuschemeng.2c02038

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  • Improved and Reduced Performance of Cu- and Ni-Substituted Co<sub>3</sub>O<sub>4</sub> Catalysts with Varying Co<sub>oh</sub>/Co<sub>Td</sub> and Co<SUP>3+</SUP>/Co<SUP>2+</SUP> Ratios for the Complete Catalytic Oxidation of VOCs

    Ma, Y; Wang, L; Ma, JZ; Liu, FD; Einaga, H; He, H

    ENVIRONMENTAL SCIENCE & TECHNOLOGY   56 ( 13 )   9751 - 9761   2022年6月   ISSN:0013-936X eISSN:1520-5851

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    記述言語:英語   出版者・発行元:Environmental Science and Technology  

    The Co3O4spinel is one of the most promising transition metal oxide (TMO) catalysts for volatile organic compound (VOC) treatment. Substituting effects have usually been utilized to improve the catalytic performance of the Co3O4spinel. In this study, Cu- and Ni-substituted Co3O4catalysts derived from mixed metal-organic frameworks (MMOFs) retained similar spinel structures but exhibited improved and reduced performance for o-xylene oxidation, respectively. Physicochemical characterization and DFT calculations revealed that Cu and Ni substitution into the Co3O4spinel varied the valence (Co3+/Co2+) and geometry (CoOh/CoTd) distributions of Co cations through different partial electron transfer and substitution sites. The higher Co3+/Co2+and CoOh/CoTdratios of the CuCo2O4catalyst contributed to the superior reducibility and oxygen mobility, which facilitated the oxidation of intermediates at lower temperatures in the catalytic oxidation of o-xylene. Meanwhile, the NiCo2O4catalyst with lower Co3+/Co2+and CoOh/CoTdratios could not completely oxidize intermediates under the same conditions due to inferior redox properties. Therefore, the CuCo2O4catalyst showed superior catalytic activity and stability to the NiCo2O4catalyst for the catalytic oxidation of o-xylene. This work provides insights into the synthesis of substituted Co3O4catalysts from MMOFs and mechanism of substituting effects, which might guide the design of efficient TMO catalysts for VOC treatment.

    DOI: 10.1021/acs.est.2c02450

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  • Rational Design of Cu-Doped ZnS Nanospheres for Photocatalytic Evolution of H<sub>2</sub> with Visible Light

    Liu, X; Zhang, Y; Matsushima, S; Sugiyama, T; Hojo, H; Einaga, H

    ACS APPLIED ENERGY MATERIALS   5 ( 2 )   1849 - 1857   2022年2月   ISSN:2574-0962

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    出版者・発行元:ACS Applied Energy Materials  

    Photocatalytic reactions to produce hydrogen from water under visible-light irradiation are an important key process for solar energy utilization. Because Cu-doped ZnS undergoes redox reactions upon irradiation with visible light, these materials have been applied to hydrogen production. In this study, Cu-doped ZnS catalysts were prepared by a solvothermal method, and their structures were investigated using scanning electron microscopy, high-resolution transmission electron microscopy, X-ray diffraction, and ultraviolet-visible spectroscopic studies. Cu-doped ZnS consists of nanospherical particles with a diameter of 50 nm. Cu2+ doping in ZnS causes structural distortion of the ZnS. The local structures were analyzed by X-ray absorption fine structure studies. As the amount of Cu added to ZnS increased, the degree of distortion of the ZnS structure also increased, and this degree of distortion reached a maximum when the Cu/Zn ratio was 0.07 (7% Cu doping). Cu-doped ZnS exhibited high activity in the hydrogen production reaction from water using Na2S and Na2SO3 as sacrificial agents under visible-light irradiation (λ > 420 nm), and the highest activity was observed at 7% Cu doping.

    DOI: 10.1021/acsaem.1c03323

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  • Enhanced catalytic performance of spinel-type Cu-Mn oxides for benzene oxidation under microwave irradiation

    Ding, SY; Zhu, C; Hojo, H; Einaga, H

    JOURNAL OF HAZARDOUS MATERIALS   424 ( Pt C )   127523   2022年2月   ISSN:0304-3894 eISSN:1873-3336

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    記述言語:英語   出版者・発行元:Journal of Hazardous Materials  

    Microwave-assisted heterogeneous catalytic oxidation of benzene was investigated over Cu-Mn spinel oxides. The spinel oxides were synthesized by a coprecipitation method from metal nitrate hydrolysis in a solution using tetramethylammonium hydroxide (TMAH) as a precipitation reagent. The catalysts were characterized by X-ray diffraction, X-ray photoelectron spectroscopy, X-ray absorption fine structure, scanning electron microscopy, transmission electron microscope and H2-temperature-programmed reduction studies. Microwave absorption by the Cu-Mn spinel oxide is mainly driven by dielectric losses (dielectric heating). Cu-Mn spinel oxide with a Cu/Mn ratio of 1 exhibited superior activity to single oxides under microwave heating, demonstrating lower apparent activation energy than that obtained under conventional heating. Microwave irradiation lowered the reaction temperature required for benzene oxidation compared with conventional heating. Transient tests were used to investigate the reactivity of oxygen species in the catalytic reaction, and the high reactivity of Cu-Mn spinel oxides was related to the high reactivity of lattice oxygen on the catalyst surface. The reactivity of the oxygen species was enhanced under microwave heating, leading to an enhanced benzene oxidation reaction. The combination of adsorption and catalytic oxidation processes using Cu-Mn spinel oxides and zeolites efficiently decomposed benzene at low concentrations.

    DOI: 10.1016/j.jhazmat.2021.127523

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  • Automatic electron hologram acquisition of catalyst nanoparticles using particle detection with image processing and machine learning

    Ichihashi, F; Koyama, A; Akashi, T; Miyauchi, S; Morooka, K; Hojo, H; Einaga, H; Takahashi, Y; Tanigaki, T; Shinada, H; Murakami, Y

    APPLIED PHYSICS LETTERS   120 ( 6 )   2022年2月   ISSN:0003-6951 eISSN:1077-3118

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    出版者・発行元:Applied Physics Letters  

    To enable better statistical analysis of catalyst nanoparticles by high-resolution electron holography, we improved the particle detection accuracy of our previously developed automated hologram acquisition system by using an image classifier trained with machine learning. The detection accuracy of 83% was achieved with the small training data of just 232 images showing nanoparticles by utilizing transfer learning based on VGG16 to train the image classifier. Although the construction of training data generally requires much effort, the time needed to select the training data candidates was significantly shortened by utilizing a pattern matching technique. Experimental results showed that the high-resolution hologram acquisition efficiency was improved by factors of about 100 and 6 compared to a scan method and a pattern-matching-only method, respectively.

    DOI: 10.1063/5.0074231

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  • O-13 マイクロ波によるリグノセルロースの触媒的急速熱分解の促進

    椿 俊太郎, 濱田 由紀, 小原 則子, 福島 潤, 西岡 将輝, 杉山 武晴, 永長 久寛, 田 旺帝, 和田 雄二, 安田 誠

    バイオマス科学会議発表論文集   17 ( 0 )   29 - 30   2022年1月   ISSN:24238333 eISSN:24238341

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    記述言語:日本語   出版者・発行元:一般社団法人 日本エネルギー学会  

    <p>Microwave irradiation accelerated hydrogen production by catalytic pyrolysis of crystalline cellulose and bamboo via Ni-SiO<sub>2</sub>-Al<sub>2</sub>O<sub>3</sub>. The Debye-Waller factor measured by microwave in situ XAFS suggested that the reaction was accelerated due to the localized high temperature of Ni nanoparticles formed by microwave irradiation. We demonstrated that synergy of the microwave-enhanced pyrolysis of biomass and localized high temperature of Ni nanoparticles accelerate the catalytic pyrolysis of lignocellulose to produce hydrogen.</p>

    DOI: 10.20550/jiebiomassronbun.17.0_29

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  • Atomic and Electronic Structure of Pt/TiO<sub>2</sub> Catalysts and Their Relationship to Catalytic Activity

    Hojo, H; Gondo, M; Yoshizaki, S; Einaga, H

    NANO LETTERS   22 ( 1 )   145 - 150   2022年1月   ISSN:1530-6984 eISSN:1530-6992

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    記述言語:英語   出版者・発行元:Nano Letters  

    Understanding the nature of the interaction between a metal and support, which is known as the metal–support interaction, in supported metal catalysts is crucial to design catalysts with desired properties. Here, we have developed model Pt/TiO2 catalysts based on the deposition of colloidal Pt nanoparticles and studied their atomic and electronic structures before and after a postdeposition treatment that induces catalytic activity using aberration-corrected scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations. Direct contact between Pt nanoparticles and TiO2 is realized after the postdeposition treatment, which is accompanied by the formation of a Ti3+ state on the TiO2 surface close to the Pt nanoparticles and a Ptδ+ state on the Pt nanoparticles. The origin of these two states and their effect on the catalytic properties are discussed. These findings pave the way for a comprehensive understanding of metal–support interactions in supported metal catalysts.

    DOI: 10.1021/acs.nanolett.1c03485

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  • One-step oxidation of benzene to phenol with H<sub>3</sub>PW<sub>12</sub>O<sub>40</sub> under photoirradiation: Effect of operating conditions

    Wang, ZR; Hojo, H; Einaga, H

    CHEMICAL ENGINEERING JOURNAL   427   2022年1月   ISSN:1385-8947 eISSN:1873-3212

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    出版者・発行元:Chemical Engineering Journal  

    The synthesis of phenol by one-pot oxidation of benzene with dioxygen (O2) is a significant conceptual and practical challenge because benzene has low reactivity to O2 at room temperature and ambient pressure. Furthermore, phenol is more reactive than benzene and is easily overoxidized, so complete oxidation is more likely to proceed in the benzene oxidation reaction, which generally results in lower phenol yield and selectivity. Herein, we report that a heteropolyacid H3PW12O40 functions as a photocatalyst for benzene oxidation reaction in an aqueous acetonitrile solution using O2 in high phenol yield (23–41%) and selectivity (80–90%). The addition of acetonitrile to the reaction solution significantly inhibited the complexation between phenol and H3PW12O40, preventing phenol overoxidation. Furthermore, no decomposition of H3PW12O40 during the reaction was evidenced by UV–VIS spectra. This photocatalyst can be used repeatedly with only a slight decrease in the rate of phenol formation. For the mechanistic study, the initial rates, which depended on the reaction conditions, were investigated in detail. The benzene oxidation under anaerobic conditions was also conducted as a control experiment. A color change of reaction solution from colorless to blue has confirmed the reduction of H3PW12O40 during the catalytic process and the formation of reduced H3PW12O40 detected in the UV–VIS spectra. A kinetic isotope effect (KIE), kH/kD = 1.15, is found for the oxidation of benzene/benzene‑d6, indicating electron transfer is the principal C−H bond activation process in the mechanism. We identified hydrogen peroxide as an intermediate and found that phenol was generated in both the photocatalytic reduction and reoxidation process in our system.

    DOI: 10.1016/j.cej.2021.131369

    Web of Science

    Scopus

  • Photocatalytic oxidation process for treatment of gas phase benzene using Ti3+ self-doped TiO2 microsphere with sea urchin-like structure 査読 国際誌

    X. Liu, Y. Zhang, S. Matsushima, H. Hojo, H. Einaga

    Chemical Engineering Journal   402   126220   2020年11月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Promoting effect of 2000 ppm H2S on the dry reforming reaction of CH4 over pure CeO2, and in-situ observation of the behavior of sulfur during the reaction 査読 国際誌

    K. Taira, T. Sugiyama, H. Einaga, K. Nakao, K. Suzuki

    Journal of Catalysis   389   611 - 622   2020年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Efficient visible light photocatalysis enabled by the interaction between dual cooperative defect sites 査読

    Rongjie Qi, Pengfei Yu, Jiachen Zhang, Weiqi Guo, Yaoyu He, Hajime Hojo, Hisahiro Einaga, Qun Zhang, Xiaosong Liu, Zhi Jiang, Wenfeng Shangguan

    Applied Catalysis B: Environmental   274   2020年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Modifying photocatalyst with defects offers effective pathway to tailor light absorption properties, but may result in more sluggish kinetics. Therefore, enhanced light absorption often could not guarantee increased activity. Here, we report a dual defect strategy to extend light absorption with minimal loss in charge dynamics. Fine-tuned amount of dual defect, i.e., nitrogen defects and single-site copper, is simultaneously generated in polymer carbon nitride(PCN) through in-situ vapor diffusion method. Surface nitrogen defect extends the light absorption to long-wavelength via sub-band absorption. The interaction between nitrogen and single-site copper at certain concentration retains the charge dynamics by making the photogenerated electrons more delocalized through the newly-formed copper-nitrogen bonds. As a result, champion modified PCN exhibits robust hydrogen production activity, roughly 4.5-fold greater than the pristine counterpart in both visible and full light ranges. More intriguingly, this synergism provides PCN with efficient visible light activity even in faint tailing optical absorption region(>450 nm).

    DOI: 10.1016/j.apcatb.2020.119099

  • Effective low-temperature catalytic abatement of benzene over porous Mn-Ni composite oxides synthesized via the oxalate route 査読

    Hao Guo, Yizhuo Li, Zhi Jiang, Zhixiang Zhang, Mingxia Chen, Hisahiro Einaga, Wenfeng Shangguan

    Journal of Chemical Technology and Biotechnology   95 ( 4 )   1008 - 1015   2020年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    BACKGROUND: Benzene (C6H6) is a typical kind of volatile organic compound (VOC) which can exert great harm to both human health and the environment, and, thus, which needs to be eliminated before its emission. In this work, porous manganese–nickel (Mn-Ni) composite oxide catalysts were synthesized through the oxalate route and applied to thermal catalytic oxidation of C6H6. By means of activity tests and relative physico-chemical characterizations, the factors affecting the activity of those Mn-Ni composite oxides were explored. RESULTS: Nitrogen (N2)-adsorption/desorption and X-ray photoelectron spectroscopy (XPS) measurements indicated that the Brunauer–Elmett–Teller (BET) surface area and the content of surface-adsorbed oxygen species were increased due to the addition of Ni into Mn oxide (MnOx). Meanwhile, the oxygen mobility and reducibility also were improved in the Mn-Ni composite oxides. Accordingly, compared with MnOx, the Mn-Ni catalysts showed higher activity for thermal catalytic oxidation of C6H6. Moreover, porous Mn-Ni composite oxides with a Mn:Ni molar ratio of 4:1 (Mn4Ni1) displayed the best catalytic activity. Further investigation indicated that the excellent catalytic performance of Mn4Ni1 composite oxides could be ascribed mainly to the larger BET surface area and the richer content of surface-adsorbed oxygen species, as well as stronger oxygen mobility and better reducibility compared with other Mn-Ni catalysts. CONCLUSIONS: The Mn4Ni1 composite oxides showed a lowest T90 value of 172 °C (C6H6 concentration 200 ppm, WHSV 60 000 mL g−1 h−1) among all of the obtained Mn-Ni composite oxides. Moreover, it also exhibited favourable catalytic stability at 210 °C in the presence or absence of moisture.

    DOI: 10.1002/jctb.6280

  • Catalyst design of Pt/TiO2 microsphere for benzene oxidation under microwave irradiation 査読

    Xin Liu, Siyu Ding, Saki Shigenobu, Hajime Hojo, Hisahiro Einaga

    Catalysis Today   2020年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Pt/TiO2 microspheres with sea-urchin like structures were prepared by sequential processes including the preparation of TiO2 by a hydrothermal method and the preheating of the TiO2, the deposition of Pt nanoparticles on the TiO2 surface, followed by post heating in O2/N2 and H2. The TiO2 and Pt/TiO2 catalysts were characterized by XRD, Raman, SEM, TEM and N2 adsorption studies. The average diameter of TiO2 microspheres was about 250 nm. The TiO2 microspheres were composed of TiO2 nanoparticles with the size of 20−30 nm. Pt particles with the size of 3 nm were highly dispersed on the TiO2 microsphere by liquid phase adsorption of colloidal Pt particles. The heating of TiO2 at 300 °C before and after the Pt deposition did not change the size of TiO2 microsphere and reduced the surface area from 238 to 137 m2 g−1. The Pt/TiO2 microsphere exhibited higher catalytic activity for benzene oxidation than Pt/TiO2 P25 under normal outer heating, whereas pristine TiO2 exhibited almost no activity. Activated carbon was used as a catalyst with a mixture of Pt/TiO2 microspheres when performing the catalytic reaction under microwave heating. The mixture of Pt/TiO2 and activated carbon showed higher benzene oxidation activity under microwave irradiation than under normal external heating. The mixture was applied to benzene adsorption-catalytic oxidation combined processes.

    DOI: 10.1016/j.cattod.2020.05.021

  • The distinctive effects of glucose-derived carbon on the performance of ni-based catalysts in methane dry reforming 査読

    U. P.M. Ashik, Shusaku Asano, Shinji Kudo, Doan Pham Minh, Srinivas Appari, Einaga Hisahiro, Jun Ichiro Hayashi

    Catalysts   10 ( 1 )   2020年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    This study aimed to investigate the effect of carbon derived from glucose (C) on the physicochemical characteristics and catalytic activity of Ni, supported over SiO2, ZSM-5, and TiO2 in methane dry reforming. Among the Ni catalysts without C, Ni/SiO2 exhibited the highest CH4-CO2 conversion and stability at all experimented temperatures. On the other hand, the C-incorporated catalysts prepared by glucose impregnation, followed by pyrolysis, showed dissimilar performances. C improved the stability of Ni/SiO2 in the reforming at 650C and 750C and increased the CH4 and CO2 conversion to the level close to the thermodynamic equilibrium at 850C. However, this element did not substantially affect the activity of Ni/ZSM-5 and exerted a retarding effect on Ni/TiO2. Characterizations with H2-TPD, XRD, EXAFS, and STEM-EDS revealed that the different influences of C by the supports were attributed to the extent of metal dispersion and metal-support interaction.

    DOI: 10.3390/catal10010021

  • Effect of catalyst composition and reactor configuration on benzene oxidation with a nonthermal plasma-catalyst combined reactor 査読

    Shoma Hamada, Hajime Hojo, Hisahiro Einaga

    Catalysis Today   144 - 152   2019年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Plasma-catalysis system comprising surface discharge reactor (SDR)and catalysts were constructed and tested for benzene decomposition. In benzene oxidation with SDR, benzene conversion and the amount of COx formed monotonically increased with input energy, but the benzene decomposition behavior was not related with ozone formation. The loading of metal oxides, Al2O3, TiO2 and CeO2 in SDR greatly promoted benzene oxidation and CO2 formation. The highest activity was obtained with manganese oxides dispersed on ultrastable zeolite Y (Mn/USY). In the range of low input power, the amount of ozone formed increased with the input power, and ozone can be efficiently consumed in benzene oxidation by loading the Mn/USY catalyst in the latter part of SDR. In the higher power range where the amount of ozone decreased with increasing the power, the loading of Mn/USY catalyst inside the reactor was more effective because not only ozone but also short-lived species formed in SDR were utilized for benzene oxidation. The addition of water vapor to reaction gas did not affect benzene conversion and COx formation with SDR-Mn/USY catalyst system. The preadsorbed benzene on the Mn/USY catalyst can be oxidized to CO2 with high selectivity compared with homogeneous oxidation of benzene in SDR.

    DOI: 10.1016/j.cattod.2018.07.055

  • Simultaneous catalytic elimination of formaldehyde and ozone over one-dimensional rod-like manganese dioxide at ambient temperature 査読

    Yi Zhang, Jin Shi, Wenjian Fang, Mingxia Chen, Zhixiang Zhang, Zhi Jiang, Wenfeng Shangguan, Hisahiro Einaga

    Journal of Chemical Technology and Biotechnology   94 ( 7 )   2305 - 2317   2019年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Background: Formaldehyde (HCHO) and ozone (O3) are seriously hazardous materials to human health, especially in the indoor environment, and need to be inhibited. Manganese dioxide (MnO2) catalysts have been extensively studied in the field of environmental pollution owing to their various morphologies and crystal structures. In this study, one-dimensional rod-like MnO2 catalysts were prepared by a hydrothermal method. The crystal form and other factors affecting the activity were explored through an activity test and various characterization methods. The decomposition process of HCHO and O3 on the most active catalyst was analyzed by in situ diffuse reflection infrared Fourier transform spectroscopy (DRIFTS). Results: α-MnO2 displayed the best catalytic performance and achieved 90% HCHO conversion, 100% carbon dioxide (CO2) yield and 100% O3 decomposition under different experimental conditions. The characterization results illustrated that the crystal phase of α-MnO2 has a suitable tunnel structure for HCHO adsorption, also leading to greater mobility of adsorbed oxygen species, abundant oxygen vacancies and active surface oxygen species, which could be the reason for the superior catalytic performance of α-MnO2. Formate and dioxymethylene (DOM) species were identified as the dominant intermediates by in situ DRIFTS. The surface hydroxyl (OH) group was confirmed to play an essential role in the complete oxidation of carbonaceous intermediates into harmless CO2 and water (H2O). Conclusion: α-MnO2 exhibited the best catalytic performance among the as-prepared samples and can efficiently eliminate HCHO and O3 in the environment.

    DOI: 10.1002/jctb.6023

  • The Effect of SO 2 and H 2 O on the Interaction Between Pt and TiO 2 (P-25) During Catalytic CO Oxidation 査読

    Kenji Taira, Hisahiro Einaga

    Catalysis Letters   149 ( 4 )   965 - 973   2019年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    The deactivation of noble metal catalysts by SO
    2
    and H
    2
    O is a common issue in the post combustion treatment of flue gases from sintering processes in the steel industry. In an effort to develop SO
    2
    -tolerant CO-oxidation catalysts, herein, we investigated the effect of SO
    2
    and H
    2
    O on the catalytic activity of Pt/TiO
    2
    (P-25) catalysts for CO oxidation using X-ray photoelectron spectroscopy (XPS), transmission electron microscopy (TEM), and diffuse-reflectance infrared Fourier-transform (DRIFT) spectroscopy. Pt/TiO
    2
    (P-25) catalysts, in the absence of SO
    2
    and presence of H
    2
    O, enhanced the activity and stability of CO oxidation, while being largely suppressed and irreversibly deactivated in the presences of SO
    2
    . The XPS and TEM results suggested that variations in the Pt particle size and oxidation state were not major causes of the deactivation. Instead, according to DRIFT spectra, the interaction between CO and H
    2
    O at the metal-support interface was weakened after the formation of TiOSO
    4
    on the TiO
    2
    surface in the presence of SO
    2
    . This resulted in a loss of the previously observed enhancement of CO oxidation under humid conditions. These results indicate that in the presence of SO
    2
    , the formation of TiOSO
    4
    is the major cause of irreversible deactivation. Therefore, removal of the TiOSO
    4
    layer from the TiO
    2
    surface is a crucial step for catalyst regeneration. Graphical Abstract: [Figure not available: see fulltext.].

    DOI: 10.1007/s10562-019-02672-3

  • Removal of benzene by non-thermal plasma catalysis over manganese oxides through a facile synthesis method 査読

    Hao Guo, Xin Liu, Hajime Hojo, Xin Yao, Hisahiro Einaga, Wenfeng Shangguan

    Environmental Science and Pollution Research   26 ( 8 )   8237 - 8247   2019年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Three manganese oxide catalysts (MnO
    x
    ) were synthesized via a simple method, and then they were introduced into the non-thermal plasma (NTP) system for benzene removal. The XRD and EXAFS results showed the MnO
    x
    were mainly in the Mn
    3
    O
    4
    phase, and from the analysis of N
    2
    adsorption/desorption isotherms, we knew the MnO
    x
    calcined at 250 °C (Mn250) had the largest surface area of 274.5 m
    2
     g
    −1
    . Besides, Mn250 also exerted higher benzene adsorption capacity (0.430 mmol g
    −1
    ) according to C
    6
    H
    6
    -TPD. O
    2
    -TPD indicated that Mn250 showed better oxygen mobility than Mn300. Moreover, by analyzing XPS results, it revealed that Mn250 exhibited rich abundant of surface adsorbed oxygen species (O
    ads
    ) and moderate ratio of Mn
    4+
    /Mn
    3+
    , and the reducibility temperature was also the lowest among all the MnO
    x
    catalysts drawn by H
    2
    -TPR profiles. As a result, Mn250 combined with NTP could remove 96.9% of benzene at a low input power of 3 W (benzene concentration 200 ppm, and GHSV 60,000 mL g
    cat.

    −1
     h
    −1
    ), performing the best catalytic activity among the three catalysts and plasma only. Furthermore, the “NTP + Mn250” system also produced the highest CO
    2
    concentration and lowest CO concentration in downstream, and the residual O
    3
    after catalytic reaction was also the lowest, that is to say, the synergistic effect between NTP and Mn250 was more effective than other catalysts in benzene removal. [Figure not available: see fulltext.].

    DOI: 10.1007/s11356-019-04264-5

  • Catalytic Removal of Benzene at Mild Temperature over Manganese Oxide Catalysts 査読

    Hao Guo, Zhixiang Zhang, Hajime Hojo, Mingxia Chen, Hisahiro Einaga, Wenfeng Shangguan

    Catalysis Surveys from Asia   2019年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Series of MnO
    x
    catalysts were synthesized through oxalate route and calcined at facile temperatures. Characterizations through XRD, N
    2
    -adsorption/desorption, HRTEM, C
    6
    H
    6
    -TPD, O
    2
    -TPD, XPS, and H
    2
    -TPR revealed that MnO
    x
    calcined at 250 °C (N250) with a main crystal phase of Mn
    2
    O
    3
    showed micro-mesopores and largest specific surface area, and therefore had a high adsorption capacity of C
    6
    H
    6
    . N250 also presented better oxygen mobility, rich surface adsorbed oxygen species (O
    ads
    ), and proper ratio of surface Mn
    4+
    /Mn
    3+
    . The starting temperature of H
    2
    -TPR of N250 was the lowest among the obtained MnO
    x
    samples. As a result, N250 exhibited the lowest T
    90
    value of 191 °C in C
    6
    H
    6
    thermal catalytic oxidation (WHSV 60,000 mL g
    cat
    .
    −1
     h
    −1
    , initial C
    6
    H
    6
    concentration 190 ppm) among all the catalysts, and this T
    90
    value is lower than those reported in many research. At last, a potential reaction pathway was proposed according to the results of in-situ FTIR measurement.

    DOI: 10.1007/s10563-019-09268-2

  • Ozone-assisted catalysis of CO In situ Fourier transform IR evidence of the cooperative effect of a bimetallic Ag-Pd catalyst 査読

    Akihiro Tou, Hyun Ha Kim, Hisahiro Einaga, Yoshiyuki Teramoto, Atsushi Ogata

    Chemical Engineering Journal   355   380 - 389   2019年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    The room-temperature oxidation of CO using ozone-assisted catalysis (OAC) over monometallic or bimetallic catalysts supported on γ-Al2O3 is presented. Within the tested particle size range, ozone decomposition was insensitive to the size of the Ag particles (6.6–11.9 nm) at weight hourly space velocities of up to 360 L·g−1·h−1. Among the tested monometallic catalysts (Ag Pd, Fe, Mn, and Cu), Ag showed the highest activity for CO oxidation. Bimetallic catalysts (Ag-M or Pd-M where M = Cu, La, Ru, and Fe) were also considered by adding a second metal or perovskite oxide (LaFeO3) to Ag. A cooperative effect was observed with the bimetallic Ag-Pd catalyst for the OAC of CO oxidation at room temperature, whereas the other bimetallic catalysts showed slightly lower performance compared to the monometallic catalyst. A high ozone utilization efficiency of 0.94 was achieved with the bimetallic Ag-Pd/γ-Al2O3 catalyst. High-angle annular dark-field scanning tunneling electron microscopy (HAADF) and energy dispersive X-ray (EDX) spectroscopy measurements confirmed the proximity of the two components, which is essential for their interaction. The in situ FTIR measurements revealed that the cooperative effect in the bimetallic Ag-Pd catalyst involved modification of CO adsorption and the suppression of product accumulation. Two typical IR absorption bands of linear- (2090 cm−1) and bridge-CO (1918 cm−1) on Pd disappeared in the presence of Ag nanoparticles. Thus, the presence of Ag in contact with Pd inhibited the accumulation of carbonates, which led to enhanced catalytic performance. Adsorption site-dependent CO oxidation on Pd was also confirmed by the in situ Fourier transform IR measurement.

    DOI: 10.1016/j.cej.2018.08.159

  • Contribution of catalytic performance of CeO2 in nonthermal plasma chemical reaction 査読

    Yusuke Egawa, Shoma Hamada, Hisahiro Einaga

    Evergreen   5 ( 3 )   34 - 37   2018年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Benzene is a harmful material that must be to be removed from flue gases. In this study, the performance of a surface discharge plasma-catalysis combined reactor for benzene decomposition was studied. Benzene conversion and CO2 selectivity increased upon loading a CeO2 catalyst onto the plasma reactor. The conversion and selectivity depended on the surface area of the CeO2. FTIR studies revealed that byproduct organic compounds are formed on the CeO2, confirming that benzene oxidation occurs on the CeO2 catalysts.

    DOI: 10.5109/1957498

  • Ag-loaded cerium-zirconium solid solution oxide nano-fibrous webs and their catalytic activity for soot and CO oxidation 査読

    Chanmin Lee, Yukwon Jeon, Taehyen Kim, Akihiro Tou, Joo Il Park, Hisahiro Einaga, Yong Gun Shul

    Fuel   212   395 - 404   2018年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    The catalytic combustion of soot and CO is one of the key technologies required to meet rigorous emission standards. Recently, solid solution materials have been employed in heterogeneous catalysts because of their remarkable intrinsic activities and good stabilities. However, the low number of contact points between soot particles and the catalyst remains a challenge to enhancing catalytic performance. Thus, we herein report the preparation of Ce-ZrO2 solid solution nano-fibrous web catalysts with a hierarchical structure using an electrospinning method, where Ag particles were loaded onto the surface of the Ce-ZrO2 webs. X-ray diffraction, scanning transmission electron microscopy, and energy dispersive spectroscopic studies allowed us to investigate the morphological and crystal structures of the prepared Ce-ZrO2 and Ag/Ce-ZrO2 web catalysts. Moreover, the relationship between the Ce/Zr ratio and activated oxygen is discussed based on X-ray photoelectron spectroscopy results. Following the catalytic oxidation of soot and CO using our novel materials, we found that the Ce0.67Zr0.33O2 web exhibited higher catalytic activities than the Ce0.5Zr0.5O2 and Ce0.33Zr0.67O2 webs, respectively. In addition, Ag/Ce0.67Zr0.33O2 exhibited enhanced catalytic activity compared with the pristine Ce0.67Zr0.33O2 for the oxidation of both soot (e.g., 500 °C vs. 544 °C at 50% conversion) and CO (e.g., 282 °C vs. 408 °C at 50% conversion). It therefore appeared that our proposed Ce-ZrO2 solid solution nano-fibrous web catalysts bearing Ag particles exhibited superior redox properties and enhanced surface areas, and as such, are promising candidates for use in the oxidation of both soot and CO.

    DOI: 10.1016/j.fuel.2017.10.007

  • Distribution ratio of Pt on anatase and rutile TiO2 particles, determined by x-ray diffraction and transmission electron microscopy analysis of Pt/TiO2(P25) 査読

    Kenji Taira, Hisahiro Einaga

    Evergreen   5 ( 4 )   13 - 17   2018年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    The TiO2(P25)-supported Pt catalyst has drawn significant interest from researchers due to its high activity. Analysis of the origin of this high catalytic activity must address the heterogeneity of the catalyst, since TiO2(P25) comprises both anatase and rutile phases. Thus, in this study, we demonstrate a simple method for determining the ratio of Pt particles on anatase and rutile by X-ray diffraction and transmission electron microscopy, without employing special equipment. Such a cost-effective method for determining the Pt distribution will accelerate research into the use of TiO2(P25) as a catalyst support.

    DOI: 10.5109/2174853

  • Sulfur dioxide-tolerant strontium chromate for the catalytic oxidation of diesel particulate matter 査読

    Rohini Khobragade, Hisahiro Einaga, Suman Jain, Govindachetty Saravanan, Nitin Labhsetwar

    Catalysis Science and Technology   8 ( 6 )   1712 - 1721   2018年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    A sulfur dioxide (SO2)-tolerant, stable mixed oxide as an alternative to platinum (Pt) group metal (PGM) catalysts has been explored for the catalytic oxidation of particulate matter (PM) due to its low-cost, desirable physiochemical properties, thermal stability, tailoring options, etc. Herein, a mixed oxide of Sr and Cr was prepared via a solution combustion method by mixing stoichiometric amounts of Sr- and Cr-precursors with citric acid and urea as fuels followed by calcination at 800 °C in air. A pure mixed oxide phase of Sr and Cr (SrCrO4) (P21/n [14]) (a = 0.7090 nm, b = 0.7394 nm, and c = 0.6755 nm) has been successfully prepared, and the SrCrO4 particles are larger in size with semi-oval shapes due to their agglomeration at elevated temperatures. The SrCrO4 catalyst shows significantly improved intrinsic catalytic performance for PM oxidation in the tested temperature range as compared to the reference catalysts, Pt/Al2O3 and Pt-dispersed SrCrO4 (Pt/SrCrO4) (loading weight: 5 wt%) are used as internal reference catalysts. The onset temperature (i.e., intrinsic catalytic activity at 10% conversion, T10) is observed at 426 °C, which is significantly lower than that of the reference Pt/Al2O3 (T10 = 537 °C) and comparable with that of the Pt/SrCrO4 catalyst (T10 = 414 °C). The SrCrO4 catalyst shows a stable, multi-cycle PM oxidation performance for the tested five cycles, and both its crystalline structure and morphology remain unchanged even after its multiple cycles of use. The structure of the SrCrO4 catalyst is stable even after moisture and SO2 treatments, and the catalytic PM oxidation activity of SrCrO4 is not compromised even after these harsh treatments. Importantly, the SrCrO4 catalyst is also stable after PM oxidation conducted using real world PM from a heavy-duty vehicle. These results demonstrate that the mixed oxide phase of SrCrO4 shows promise for PM oxidation.

    DOI: 10.1039/c7cy02553j

  • Simultaneously catalytic decomposition of formaldehyde and ozone over manganese cerium oxides at room temperature Promotional effect of relative humidity on the MnCeOx solid solution 査読

    Yi Zhang, Minxia Chen, Zhixiang Zhang, Zhi Jiang, Wenfeng Shangguan, Hisahiro Einaga

    Catalysis Today   2018年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Manganese cerium oxides were synthesized by Pechini method and were used for investigating the performance of solid solution and the influence of water vapor presence on catalytic decomposition of formaldehyde and ozone at room temperature. Compared with the pristine manganese oxides and cerium dioxide, MnCeOx catalyst exhibited the best performance on HCHO oxidation and excellent ozone decomposition under dry air conditions although the CO2 yield is much lower than that of the solo cerium oxide. The as-prepared catalysts were characterized by XRD, XPS, N2 adsorption-desorption, H2-TPR and O2-TPD techniques. These characterization results revealed that the MnCeOx catalyst formed a solid solution of manganese and cerium, and exhibited relatively abundance oxygen vacancies and the most surface lattice oxygen species, enhancing remarkable adsorption and redox properties. MnCeOx catalyst has ∼100% HCHO conversion into CO2 in the catalytic activity test while the relative humidity is higher than 50% in this work, which could be suitable for indoor air purification. In situ DRIFTS results demonstrated that this excellent performance of HCHO complete oxidation is attributed to the continuously replenished surface hydroxyl groups generated from the interaction of water vapor and ozone on the surface of MnCeOx catalyst. This composite oxide is a promising catalyst for removing formaldehyde and ozone in the indoor environment.

    DOI: 10.1016/j.cattod.2018.04.027

  • Phosphate-Modified TiO2/ZrO2 Nanofibrous Web Composite Membrane for Enhanced Performance and Durability of High-Temperature Proton Exchange Membrane Fuel Cells 査読

    Chanmin Lee, Jeongho Park, Yukwon Jeon, Joo Il Park, Hisahiro Einaga, Yen B. Truong, Illias L. Kyratzis, Isao Mochida, Jonghyun Choi, Yong Gun Shul

    Energy & Fuels   31 ( 7 )   7645 - 7652   2017年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    An Aquivion/titanium zirconium oxide nanofibrous web composite membrane was prepared and tested as a proton exchange membrane in a hydrogen/air fuel cell. The incorporation of a small dose (9 wt % membrane) of a uniformly distributed electrospun titanium zirconium oxide (TiO2/ZrO2; Ti/Zr = 1:1 atomic ratio) nanofibrous web significantly improved hydromechanical stability of the composite membranes, which exhibited approximately 2 times higher water retention and 30 times lower dimensional change than a pristine Aquivion membrane under in-water membrane hydration conditions. Phosphate functionalities were successfully added onto the nanofiber surface, as confirmed by X-ray photoelectron spectroscopy (XPS) analysis. The added phosphate functionality resulted in higher proton conductivity of the prepared composite membrane compared to the non-modified TiO2/ZrO2 nanofibrous web composite membrane [e.g., 0.027 S cm-1 versus 0.021 S cm-1 at 120°C and 40% relative humidity (RH)]. A single cell test also showed the effect of an added TiO2/ZrO2 nanofibrous web. A single cell with an Aquivion/TiO2/ZrO2 nanofibrous web composite membrane outperformed a single cell with a pristine Aquivion membrane in fully humidified conditions (100% RH at 75 and 90°C). The Aquivion/phosphate-modified TiO2/ZrO2 nanofibrous web composite membrane showed the best single cell performance at all four testing conditions, including the fully humidified medium-temperature conditions (e.g., Pmax = 1.18 W cm-2 at 75°C and 100% RH, and Pmax = 0.97 W cm-2 at 90°C and 100% RH) and partially humidified high-temperature conditions (Pmax = 0.45 W cm-2 at 120°C and 40% RH, and Pmax = 0.21 W cm-2 at 140°C and 20% RH). The composite membrane also displayed excellent durability evidenced by the accelerated lifetime (ALT) test results. Overall, the phosphate-modified TiO2/ZrO2 nanofibrous web composite membrane enhanced the electrical properties and durability of the fuel cell, especially at high temperatures (>120°C).

    DOI: 10.1021/acs.energyfuels.7b00941

  • Silver and manganese oxide catalysts supported on mesoporous ZrO2 nanofiber mats for catalytic removal of benzene and diesel soot 査読

    Chanmin Lee, Yong Gun Shul, Hisahiro Einaga

    Catalysis Today   281   460 - 466   2017年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Mesoporous zirconia (ZrO2) nanofibers were synthesized by an electrospinning method and calcination at 600 °C. Ag and Mn oxides were separately or simultaneously deposited on the ZrO2 nanofibers by impregnation methods. The structure of the ZrO2 supported nanofiber materials were examined by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), energy dispersive spectroscopy (EDS) and X-ray photoelectron spectroscopy (XPS). Ag and Mn oxides were homogeneously deposited on the surface of ZrO2 nanofibers. Metallic Ag species and Mn2O3 were formed on the ZrO2 nanofibers when they were separately deposited, whereas the codeposition of Ag and Mn changed the oxidation state of Mn oxides on the catalyst surface. The supported catalysts were evaluated for their soot and benzene oxidation performance. The co-deposition of Ag and Mn lowered the light-off temperature for benzene oxidation. The soot oxidation performance was comparable for the Ag/ZrO2, Mn/ZrO2 and Ag-Mn/ZrO2 catalysts under tight contact mode, whereas Ag/ZrO2 exhibited the highest activity and the activity decreased with decreasing the Ag content under loose contact mode.

    DOI: 10.1016/j.cattod.2016.05.050

  • Autothermal reforming of heavy-hydrocarbon fuels by morphology controlled perovskite catalysts using carbon templates 査読

    Yukwon Jeon, Chanmin Lee, Junki Rhee, Gicheon Lee, Jae ha Myung, Myunggeun Park, Joo Il Park, Hisahiro Einaga, Yong Gun Shul

    Fuel   187   446 - 456   2017年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    A novel synthesis of morphology-controlled perovskite networked with LaCr0.8Ru0.2O3 nanoparticles was introduced using activated carbons as sacrificial templates. These catalysts were used for the hydrogen production by heavy-hydrocarbon autothermal reforming. To investigate the effect of the carbon templates, morphology-controlled perovskites using activated carbons and a non-templated catalyst were prepared to determine how carbon templates influence the chemical structure of the perovskite. The carbon templates produced a crystalline structure with the well incorporation of Ru under mild calcination conditions. The morphology of the hollow fibers provided a higher specific surface area than that of the porous grain catalyst with a similar average particle size (∼80 nm). It was found that the hollow fibers showed a unique pore structure with large macropores from 1 to 100 μm, which might offer a higher surface area and enhanced mass transfer of the reactants. This provided a higher activation energy for H2 production than the porous grain and non-templated catalysts during the autothermal reforming of heavy hydrocarbons. As a result, the fibrous feature and well-defined chemical structure were crucial factors when cracking the hydrocarbon chain. The hollow fiber catalyst showed high reforming efficiency for H2 production (>65 mol%) from heavy-hydrocarbon fuels during long-term experiments, featuring substantial durability with low carbon deposition and no structural changes.

    DOI: 10.1016/j.fuel.2016.09.065

  • Nano-sized nickel catalyst for deep hydrogenation of lignin monomers and first-principles insight into the catalyst preparation 査読

    Shi Chao Qi, Lu Zhang, Hisahiro Einaga, Shinji Kudo, Koyo Norinaga, Hayashi Jun-Ichiro

    Journal of Materials Chemistry A   5 ( 8 )   3948 - 3965   2017年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    This paper reports, for the first time, complete arene hydrogenation of phenolic compounds as lignin monomers over a non-noble metal catalyst supported by a general material. A type of nano-sized Ni catalyst was prepared in ethanol and in situ supported by ZSM-5 zeolite through general borohydride reduction of Ni2+ to Ni0, but with application of a simple ligand, pyridine. This catalyst showed an activity so high as to completely or near completely hydrogenate the aromatic rings of phenol and its twelve derivatives as potential lignin monomers at 180 °C. The activity was clearly higher than that of another type of conventional Ni catalyst prepared in the absence of pyridine. Analyses of the catalysts by TEM/EDS, XPS, XAFS and others demonstrated that pyridine had crucial roles in selective formation of nano-sized Ni and maintenance of its activity by appropriate interaction with the support. This paper also shows our theoretical approach to the mechanism of the borohydride reduction. First-principles calculations based on density functional theory (DFT) revealed the reaction pathway from Ni2+ to Ni0 and the role of pyridine, which was validated by some experimental facts. The DFT calculations also explain the variety of reactivities of the lignin monomers, which are strongly influenced by their molecular electrostatic and steric nature.

    DOI: 10.1039/c6ta08538e

  • Catalytic Properties of CeO2-Supported LaMnO3 for NO Oxidation 査読

    Hisahiro Einaga, Wataru Yoshida, Chanmin Lee, Keisuke Kusaba

    Catalysis Letters   146 ( 12 )   2495 - 2503   2016年12月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Abstract: CeO2-supported LaMnO3 perovskite oxides were prepared to study their catalytic properties in the oxidation of NO to NO2. To prepare the catalyst and investigate the interaction between LaMnO3 and CeO2, two deposition methods were used. Extended X-ray absorption fine structure studies confirmed that perovskite oxide phases were formed on the CeO2 support. Moreover, X-ray photoelectron spectroscopy and temperature-programmed reduction with H2 studies revealed that the reduction temperatures for perovskite oxides and CeO2 support decreased by the deposition followed by calcination at 650 °C, and that the interaction between the LaMnO3 and CeO2 support can be controlled by changing the preparation method. The LaMnO3/CeO2 catalyst in which LaMnO3 was highly dispersed on CeO2 exhibited higher NO oxidation activity than either LaMnO3 or CeO2. The thermal stability of the LaMnO3/CeO2 catalyst was compared with that of alumina-supported LaMnO3 catalysts over 850–1050 °C. Graphical Abstract: [Figure not available: see fulltext.]

    DOI: 10.1007/s10562-016-1878-3

  • SOx tolerant Pt/TiO2 catalysts for CO oxidation and the effect of TiO2 supports on catalytic activity 査読

    Kenji Taira, Kenji Nakao, Kimihito Suzuki, Hisahiro Einaga

    Environmental Science & Technology   50 ( 17 )   9773 - 9780   2016年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    We developed a new technique for mitigating catalyst deactivation caused by SO2 in exhaust gases. A series of 0.1 wt %-Pt/TiO2 catalysts with different surface, crystal, and pore structures were prepared and tested for CO oxidation activity in the presence of SO2 and H2O. The order of the CO oxidation activity under the influence of SO2 was much different from that in the absence of SO2. Catalysts with a high ratio of larger pores exhibited higher catalytic activity under the influence of SO2 and H2O in the temperature range of 250-300 °C, whereas other parameters, such as BET surface area and crystal structure of the TiO2 support, had minor effects on the CO oxidation activity. The oxidation state of Pt differed significantly depending on the kind of TiO2 support. Some catalysts were less active without H2 reduction pretreatment due to the presence of oxidized Pt species.

    DOI: 10.1021/acs.est.6b01652

  • Three-dimensional arrangements of perovskite-type oxide nano-fiber webs for effective soot oxidation 査読

    Chanmin Lee, Yukwon Jeon, Satoshi Hata, Joo Il Park, Ryutaro Akiyoshi, Hikaru Saito, Yasutake Teraoka, Yong Gun Shul, Hisahiro Einaga

    Applied Catalysis B: Environmental   191   157 - 164   2016年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Perovskite-type oxides have been widely applied in heterogeneous catalytic reactions, such as soot oxidation. However, a poor contact point between the catalyst and solid reactant (soot) often limits the catalytic performance. Here, we report La1 - xSrxCo0.2Fe0.8O3 - δ perovskite oxide catalysts with a unique three-dimensional (3D) fiber web structure that increases the high-contact area by trapping soot in the unique pore structure for effective catalytic activity. This feature was carefully analyzed using scanning transmission electron microscopy (STEM) tomography to investigate the location of the soot on the web. The structure of the web, with a thickness of approximately 55 μm, indicated that the soot particles were caught by the 3D pores between the fibers. The relationship between the Sr amount and activate oxygen was also characterized by means of XPS. The results show that the Sr amount of 0.4 produced the highest amount of active oxygen species (O-) that are essential for soot oxidation reaction. The developed catalyst exhibited a good catalytic performance due to the optimized perovskite chemical structure and the greatly increased number of the contact points owing to the 3D inter-fiber spaces. Hence, our proposed approach is reasonable for application to real soot combustion processes and can also be easily extended to numerous other catalytic processes to enhance the catalytic activity.

    DOI: 10.1016/j.apcatb.2016.03.001

  • Three-dimensional Arrangements of Perovskite-type Oxide Nano-fiber Webs for Effective Soot Oxidation 査読 国際誌

    Chanmin Lee, Yukwon Jeon, Hata, Satoshi, JOO-IL PARK, Ryutaro Akiyoshi, H. Saito, Yasutake Teraoka, Yong-Gun Shul, Hisahiro Einaga

    Applied Catalysis B: Environmental   2016年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Silver and Manganese Oxide Catalysts Supported on Mesoporous ZrO2 Nanofiber Mats for Catalytic Removal of Benzene and Diesel Soot 招待 査読 国際誌

    Chanmin Lee, Yong-Gun Shul, Hisahiro Einaga

    Catalysis Today   2016年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Effect of aging on the CO oxidation properties of copper manganese oxides prepared by hydrolysis-coprecipitation using tetramethyl ammonium hydroxide 招待 査読 国際誌

    Hisahiro Einaga, Akihiro Kiya

    REACTION KINETICS MECHANISMS AND CATALYSIS   117 ( 2 )   521 - 536   2016年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1007/s11144-016-0974-0

  • Structural Analysis of Mesoporous ZrO2 and TiO2 Nanofiber Mats Prepared by Electrospinning Methods 査読

    Chanmin Lee, Y.-G. Shul, 永長 久寛

    九州大学大学院総合理工学報告   37   1 - 5   2016年2月

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    記述言語:日本語   掲載種別:研究論文(学術雑誌)  

    リポジトリ公開URL: https://hdl.handle.net/2324/1560666

  • Factors Affecting the Catalytic Performance of La-K-Mn-O Perovskite Oxides for Diesel Soot Oxidation 招待 査読 国際誌

    Hironobu Shimokawa, Hajime Kusaba, Hisahiro Einaga, Yasutake Teraoka

    BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN   88 ( 10 )   1486 - 1493   2015年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1246/bcsj.20150186

  • Ag supported on electrospun macro-structure CeO2 fibrous mats for diesel soot oxidation 査読

    Chanmin Lee, Joo Il Park, Yong Gun Shul, Hisahiro Einaga, Yasutake Teraoka

    Applied Catalysis B: Environmental   174-175   185 - 192   2015年9月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Ceria oxide (CeO2) nanofibers with diameters of 241-253nm were produced via the electrospinning method. They were then applied as new support materials for silver nanoparticles and their effectiveness as diesel soot oxidation catalysts was examined. The crystal structure of the Ag was confirmed by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron microscopy (HR-TEM), and energy dispersive spectroscopy (EDS). The diesel soot oxidation experiment was performed using a mixture of carbon black and the fabricated catalyst. In the tight contact and loose contact modes, the highest temperatures of both the CeO2-fiber-supported Ag catalysts (Ag/CeO2) calcined at 500°C and the CeO2 fibers calcined at 500°C were shifted to a lower temperature range, compared with JRC-CEO-3 (a commercial catalyst). In addition, the activation energy also showed similar behavior. Thus, the fibrous CeO2 and Ag/CeO2 have been shown to be effective and promising catalysts for soot oxidation.

    DOI: 10.1016/j.apcatb.2015.03.008

  • Preparation of Supported LaMnO3 Catalysts by Selective Deposition on Alumina and Their Catalytic Activity for Propane Oxidation 招待 査読 国際誌

    Teruaki Asada, Hisahiro Einaga, Hajime Kusaba, Yasutake Teraoka

    BULLETIN OF THE CHEMICAL SOCIETY OF JAPAN   88 ( 8 )   1036 - 1046   2015年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1246/bcsj.20150111

  • In-situ reforming of the volatiles from fast pyrolysis of ligno-cellulosic biomass over zeolite catalysts for aromatic compound production 招待 査読 国際誌

    Kazuhiro Uemura, Srinivas Appari, Shinji Kudo, Jun-ichiro Hayashi, Hisahiro Einaga, Koyo Norinaga

    FUEL PROCESSING TECHNOLOGY   136   73 - 78   2015年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.fuproc.2014.10.002

  • Preparation and Characterization of Pd Loaded Sr-deficient K2NiF4-type (La, Sr)2MnO4 Catalysts for NO-CO reaction 査読 国際誌

    Tomoki Uchiyama, Reiko Karita, Maiko Nishibori, Hisahiro Einaga, Yasutake Teraoka

    Catalysis Today   251   7 - 13   2015年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1016/j.cattod.2014.09.033

  • Ag Supported on Electrospun Macro-structure CeO2 Fibrous Mats for Diesel Soot Oxidation 査読 国際誌

    Chanmin Lee, Joo-Il Park, Yong-Gun Shul, Hisahiro Einaga, Yasutake Teraoka

    Applied Catalysis B: Environmental   185 - 192   2015年7月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Comparison of catalytic properties of supported metal oxides for benzene oxidation using ozone 査読

    Hisahiro Einaga, Nanako Maeda, Yusuke Nagai

    Catalysis Science and Technology   5 ( 6 )   3147 - 3158   2015年6月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Catalytic oxidation of gaseous benzene using ozone over SiO2-supported metal oxides (oxides of Mn, Fe, Co, Ni, and Cu) was performed at 343 K. The supported metal oxides were prepared from metal nitrates via impregnation followed by calcination at 873 K. X-ray diffraction studies revealed that aggregated metal oxides were formed on the supports. The quantities of the exposed metal oxides on SiO2 were determined using temperature-programmed desorption of formic acid species adsorbed on the catalysts. The turnover frequencies (TOFs) for ozone decomposition and catalytic oxidation of benzene with ozone were also compared for the supported metal oxides. The TOFs for ozone decomposition with the supported metal oxides decreased in the order: Cu > Co ~ Ni > Fe > Mn. Conversely, the SiO2-supported Mn oxide (Mn/SiO2) catalyst exhibited the highest activity for catalytic oxidation of benzene with ozone and the highest efficiency for ozone utilization. FTIR studies revealed that benzene ring cleavage continuously proceeded on the Mn/SiO2 catalyst, and oxygen-containing species, which were readily oxidized to CO2 and CO in the presence of ozone, accumulated on the catalyst surface. The Fe-, Co-, Ni-, and Cu-oxides suffered from catalyst deactivation due to the build-up of by-product compounds, which was attributed to their low activity for oxidation of these substances. These results suggest that the most important steps in benzene oxidation with ozone on metal oxides are the formation and oxidation of by-product compounds. The higher activity of the Mn oxide catalyst for benzene oxidation is ascribed to the facile oxidation of these by-product compounds.

    DOI: 10.1039/c5cy00315f

  • Formation of tetravalent Fe ions in LaFeO3 perovskite through mechanochemical modification by ball milling 査読

    Tomoki Uchiyama, Maiko Nishibori, Hisahiro Einaga, Yasutake Teraoka

    Journal of the American Ceramic Society   98 ( 4 )   1047 - 1051   2015年4月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Mechanochemical modification of previously synthesized LaFeO3 perovskite-type oxide by a high-energy ball milling was investigated to introduce Fe4+ ions or transform some Fe3+ into Fe4+ in LaFeO3. X-ray absorption fine structure studies revealed that the formation of Fe4+ ions into LaFeO3 perovskite has been achieved at first time by ball milling at room temperature without any additives or replacement of La3+ ions by some divalent cations. The structural model of Fe4+ containing LaFeO3 could be described as with a modified perovskite having equal amounts of La and Fe vacancies, which is supported by a good correlation between the results of Fe K-edge XANES spectra and O2-TPD. The synthesis of Fe4+-containing LaFeO3 perovskite by ball milling was able to produce the O2 adsorption capacity of nonsubstituted perovskite-type oxide.

    DOI: 10.1111/jace.13513

  • Effect of co-deposition of LaFeO3 on the catalytic properties of Pd on Al2O3 support for CO–O2 and NO–CO reactions 査読

    Akihiro Tou, Hisahiro Einaga, Yasutake Teraoka

    Reaction Kinetics, Mechanisms and Catalysis   114 ( 2 )   409 - 420   2015年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Pd/LaFeO3/Al2O3 catalysts were prepared by co-deposition of Pd and LaFeO3 perovskite oxides in the intrapores of Al2O3 by the incipient wetness method. Pd and LaFeO3 perovskite oxides were highly dispersed on Al2O3 in the inside pore. H2-TPR studies revealed that the oxidation state, dispersion and redox properties of Pd were affected by the presence of LaFeO3 with close proximity. The Pd and LaFeO3 co-deposited Al2O3 catalysts exhibited much higher activity for CO oxidation and NO–CO reaction than Pd/Al2O3 catalysts.

    DOI: 10.1007/s11144-014-0823-y

  • Efficient hydrogen production from formic acid using TiO2-supported AgPd@Pd nanocatalysts 査読 国際誌

    服部 真史, Hisahiro Einaga, 大尾 岳史, Masaharu Tsuji

    JOURNAL OF MATERIALS CHEMISTRY A   3 ( 8 )   4453 - 4461   2015年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    DOI: 10.1039/c4ta06988a

  • Ce-based catalysts for simultaneous removal of both diesel soot and NOx 査読

    Shu Jie Wang, Gu Chu Zou, Yao Xu, Ming Xia Chen, Wen Feng Shangguan, Hisahiro Einaga, Yasutake Teraoka

    Journal of Molecular Catalysis   29 ( 1 )   60 - 67   2015年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Ce-based oxides were prepared by citric acid complex method and characterized by nitrogen physisorption, XRD, BET, H2-TPR and XPS; their catalytic performances in simultaneous removal of diesel soot and NOx were investigated on a thermogravimetric apparatus and a tubular reactor. Co0.1/CeLa0.05 prevailed over all the detected materials in catalytic performance for simultaneous removal of soot and NOx. T50 of this catalyst (temperature for 50% soot combustion)was 301℃, and the yield of N2 was 41.4%. A majority of cobalt oxides were dispersed on the surface of Ce-La solid solution. The mutual transformation between Co3+ and Co2+enhanced the redox ability and oxygen storage capacity of pure ceria oxide, achieving lower temperature of combustion. Cerium-cobalt complex oxide doped with lanthanum presented a tremendous increase of surface area, leading to higher yield of N2. The formation of trace amount of LaCoO3 promoted oxygen vacancies creation, thus affecting positively to the soot combustion activity.

  • Catalytic properties of copper-manganese mixed oxides prepared by coprecipitation using tetramethylammonium hydroxide 査読

    Hisahiro Einaga, Akihiro Kiya, Satoru Yoshioka, Yasutake Teraoka

    Catalysis Science and Technology   4 ( 10 )   3713 - 3722   2014年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Copper-manganese (Cu-Mn) mixed oxide catalysts were prepared by a coprecipitation technique from metal nitrates in aqueous solution using tetramethylammonium hydroxide (TMAH) as a pH regulator. The structures and properties of the mixed oxide catalysts were investigated by X-ray diffraction, extended X-ray absorption fine structure, X-ray photoelectron spectroscopy and H2-TPR studies. Spinel-type mixed oxides were mainly formed in the Cu-Mn mixed oxides in which Cu and Mn species occupied both tetrahedrally and octahedrally coordinated sites. The occupancy of Cu and Mn in these sites depended on the Cu/Mn ratio. The average oxidation state of Cu was evaluated to be 2+ and was almost independent of the Cu/Mn ratio; reduced Cu species were also formed on the surface sites. By incorporation of Cu into Mn oxides, the average oxidation state of Mn increased both in the bulk sites and on the surface sites. The concentration of Mn on the surface sites was higher than that in the bulk sites. The Cu-Mn mixed catalysts exhibited higher activity than corresponding single-metal oxides at the reaction temperature range of 343-403 K. Formation of Cu-Mn spinel-type oxides gave rise to the increase in the catalyst surface area and the rate for CO oxidation normalized by surface area, and the Cu-Mn mixed oxides with the Cu/Mn molar ratio of 1 exhibited the highest activity for CO oxidation. CO-TPR studies revealed that in the temperature range of 343-403 K, the lattice oxygen at the first layer of the mixed oxides reacted with CO to form CO2. This journal is

    DOI: 10.1039/c4cy00660g

  • Preparation of alumina-supported Pd and LaMnO3 catalysts with the site-selective deposition and their catalytic activity for NO-CO reaction

    Tou, A, Hisahiro Einaga, Yasutake Teraoka

    CATALYSIS TODAY   201   2013年3月

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    記述言語:英語  

    DOI: 10.1016/j.cattod.2012.04.033

  • Comparison of catalytic performance of Ag- and K-based catalysts for diesel soot combustion

    Hironobu Shimokawa, Yasuyuki Kurihara, Hajime Kusaba, Hisahiro Einaga, Yasutake Teraoka

    CATALYSIS TODAY   185 ( 1 )   2012年5月

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    記述言語:英語  

    DOI: 10.1016/j.cattod.2011.10.030

  • Roles of Bi, M and VO4 tetrahedron in photocatalytic properties of novel Bi0.5M0.5VO4 (M = La, Eu, Sm and Y) solid solutions for overall water splitting

    H. Liu, J. Yuan, Z. Jiang, W. Shangguan, Hisahiro Einaga, Yasutake Teraoka

    Journal of Solid State Chemistry   186   2012年5月

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    記述言語:英語  

  • Roles of Bi, M and VO 4 tetrahedron in photocatalytic properties of novel Bi 0.5M 0.5VO 4 (M=La, Eu, Sm and Y) solid solutions for overall water splitting 査読

    Hui Liu, Jian Yuan, Zhi Jiang, Wenfeng Shangguan, Hisahiro Einaga, Yasutake Teraoka

    Journal of Solid State Chemistry   186   70 - 75   2012年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

    Novel Bi 0.5M 0.5VO 4 (BMV; M=La, Eu, Sm and Y) solid solutions were prepared and studied in this paper. All the samples were proved to produce H 2 and O 2 simultaneously from pure water under the irradiation of UV light. MO bond lengths were proved to increase with M cations by refining cell parameters and atomic positions. Besides, band gaps, energy gaps and photocatalytic activities of BMV also changed with M cations. Both of MO and VO bond lengths were suggested to account for this phenomenon. Inactive A 0.5Y 0.5VO 4 (A=La, Ce) for water splitting proved incorporation of Bi rather than distortion of VO 4 tetrahedron was a critical factor for improving efficiency of overall water splitting by facilitating the generation of electron and hole with lighter effective masses. Replacement of Bi by M cations not only gave indirect effect on band structure but also raised position of conduction band minimum to meet requirement of H 2 production.

    DOI: 10.1016/j.jssc.2011.11.035

  • Preliminary study on catalytic combustion-type sensor for the detection of diesel particulate matter

    Cheol-Beom Lim, 永長 久寛, Yoshihiko Sadaoka, 寺岡 靖剛

    SENSORS AND ACTUATORS B-CHEMICAL   160 ( 1 )   2011年12月

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    記述言語:英語  

    DOI: 10.1016/j.snb.2011.08.009

  • Novel photocatalyst of V-based solid solutions for overall water splitting 査読 国際誌

    H. Liu, J. Yuan, Z. Jiang, W. Shangguan, H. Einaga and Y. Teraoka

    Journal of Materials Chemistry   21 ( 41 )   2011年10月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Catalytic performance of supported precious metal catalysts for the combustion of diesel particulate matter

    Cheol-Beom Lim, 草場 一, 永長 久寛, 寺岡 靖剛

    CATALYSIS TODAY   175 ( 1 )   2011年10月

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    記述言語:英語  

    DOI: 10.1016/j.cattod.2011.03.062

  • Complete oxidation of egg albumin on photoirradiated TiO2: Factors controlling the catalytic performance in solid-solid heterogeneous systems 査読 国際誌

    Kawanami, H. Einaga, and Y. Teraoka

    Research on Chemical Intermediates   37 ( 6 )   2011年6月

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    掲載種別:研究論文(学術雑誌)  

  • 担持金属酸化物触媒によるベンゼンのオゾン酸化反応

    前田菜那子, 永長久寛, 寺岡靖剛

    触媒   53(2), pp.65-67 (2011). ( 2 )   2011年3月

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    記述言語:日本語   掲載種別:研究論文(その他学術会議資料等)  

  • Relationship between Cation Arrangement and Photocatalytic Activity for Sr-Al-Nb-O Double Perovskite 査読 国際誌

    H. Iwakura, H. Einaga, and Y. Teraoka,

    Inorganic Chemistry   2010年12月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Performance of an ozone decomposition catalyst in hybrid plasma reactors for volatile organic compound removal 査読 国際誌

    A. Ogata, K. Saito, H.-H. Kima, M. Sugasawaa, H. Aritani, H. Einaga

    Plasma Chem. Plasma Process   30   2010年2月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Small-Angle X-ray Scattering Study of Metal Nanoparticles Prepared by Photoreduction in Aqueous Solutions of Sodium Dodecyl Sulfate 国際誌

    M. Harada, K. Saijo, N. Sakamoto, H. Einaga

    Colloid. Surf. A: Physicochem. Engineer. Aspects   345   2009年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Preparation of Alumina-supported LaFeO3 Catalysts and their Catalytic Activity for Propane Combustion 査読 国際誌

    T. Asada, T. Kayama, H. Kusaba, H. Einaga, Y. Teraoka

    Catal. Today   2008年12月

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    掲載種別:研究論文(学術雑誌)  

  • Effect of Surface Area of La-K-Mn-O Perovskites Catalysts on Diesel Particulate Oxidation 査読 国際誌

    H. Shimokawa, H. Kusaba, H. Einaga, Y. Teraoka

    Catal. Today   2008年12月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • In situ Diffuse Reflectance FTIR Measurements of TiO2 and Pt/TiO2 in Photooxidation of Benzene and Ethylene 査読 国際誌

    Hisahiro Einaga, Yasutake Teraoka

    Res. Chem. Intermed.   2008年1月

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    掲載種別:研究論文(学術雑誌)  

  • オゾン-触媒複合系におけるVOC 分解に有効な活性酸素種の検討 査読

    齋藤圭市, 尾形 敦, 金賢 夏, 二タ村 森, 有谷博文, 永長久寛

    静電気学会誌   2008年1月

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    記述言語:日本語   掲載種別:研究論文(学術雑誌)  

  • Formation Mechanism of Pt Particles by Photo-reduction of Pt Ions in Polymer Solutions 査読 国際誌

    M. Harada, H. Einaga

    Langmuir   2006年3月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Zeolite-Combined Plasma Reactor for Decomposition of Toluene 査読 国際誌

    S.-M. Oh, H.-H. Kim, H. Einaga, A. Ogata, S. Futamura and D.-W. Park

    Thin Solid Films   2006年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Effect of Silver Deposition on TiO2 for Photocatalytic Oxidation of Benzene in Gas Phase 査読 国際誌

    H. Einaga

    React. Kin. Catal. Lett.   2006年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Efficient decomposition of perfluorocarboxylic acids in water by photochemical approaches 査読 国際誌

    H. Hori, E. Hayakawa, A. Yamamoto, N. Yamashita, S. Taniyasu, H. Einaga, S. Kutsuna, H. Kitagawa, R. Arakawa

    Organohalogen Compounds   2005年8月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Effect of zeolite in surface discharge plasma on the decomposition of toluene 査読 国際誌

    S.-M. Oh, H.-H. Kim, A. Ogata, H. Einaga, S. Futamura, Dong-Wha Park

    Catal. Lett.   2005年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Photochemical Deposition of Platinum on TiO2 by using Poly(vinyl Alcohol) as an Electron Donor and a Protecting Polymer 査読 国際誌

    M. Harada, H. Einaga

    Catal. Commun.   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Decomposition of Environmentally Persistent Perfluorooctanoic Acid in Water by Photochemical Approaches 査読 国際誌

    H. Hori, E. Hayakawa, H. Einaga, S. Kutsuna, K. Koike, T. Ibusuki, H. Kitagawa, R. Arakawa

    Environ. Sci. Technol.   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Synergistic Effect of Silent Discharge Plasma and Catalysts on Benzene Decomposition 査読 国際誌

    S. Futamura, H. Einaga, H. Kabashima and Lee Yong Hwan

    Catal. Today   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Comparative Study on the Catalytic Activities of Alumina-supported Metal Oxides for Oxidation of Benzene and Cyclohexane with Ozone 査読 国際誌

    H. Einaga, S. Futamura

    React. Kin. Catal. Lett.   2004年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Decomposition of Environmentally Persistent Trifluoroacetic Acid to Fluoride Ions by a Homogeneous Photocatalyst in Water 査読 国際誌

    H. Hori, Y. Takano, K. Koike, K. Takeuchi, H. Einaga

    Environ. Sci. Technol.   2003年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Photochemical Decomposition of Pentafluoropropionic Acid to Fluoride Ions with A Water-soluble Heteropolyacid Photocatalyst 査読 国際誌

    H. Hori, Y. Takano, K. Koike, S. Kutsuna, H. Einaga, T. Ibusuki

    Appl. Catal., B: Environmental   2003年1月

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Effective Combination of Nonthermal Plasma and Catalysts for Decomposition of Benzene in Air 査読 国際誌

    A. Ogata, H. Einaga, H. Kabashima, S. Futamura, S. Kushiyama, H.-H. Kim

    Appl. Catal., B: Environmental   2003年1月

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    掲載種別:研究論文(学術雑誌)  

  • 空気気流中のベンゼン分解反応における無声放電リアクタと酸化チタンの複合効果 査読

    永長久寛、椛島 一、二タ村森

    静電気学会誌   2002年1月

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    記述言語:日本語   掲載種別:研究論文(学術雑誌)  

  • Pt/TiO2光触媒による空気中ベンゼンの完全酸化反応 査読

    永長 久寛、二タ村 森、指宿 堯嗣

    石油学会誌   1999年1月

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    記述言語:日本語   掲載種別:研究論文(学術雑誌)  

  • Improvement of Catalyst Durability in Benzene Photooxidation by Rhodium Deposition on TiO2 査読 国際誌

    H. Einaga, S. Futamura, T. Ibusuki

    Chem. Lett.   1900年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

  • Decomposition of Nonafluoropentanoic Acid by Heteropolyacid Photocatalyst H3PW12O40 in Aqueous Solution 査読 国際誌

    H. Hori, E. Hayakawa, K. Koike, H. Einaga, T. Ibusuki

    J. Mol. Catal. A: Chem.   1900年

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    記述言語:英語   掲載種別:研究論文(学術雑誌)  

▼全件表示

書籍等出版物

  • 空気浄化テクノロジーの新展開 —VOC削減対策に向けて—

    永長 久寛,金 賢夏,尾形 敦,二タ村 森(担当:共著)

    シーエムシー出版  2006年7月 

     詳細を見る

    担当ページ:第6章 低温プラズマ技術   記述言語:日本語   著書種別:学術書

講演・口頭発表等

  • オゾンを酸化剤としたMn系酸化物触媒によるベンゼンの分解反応

    前田菜那子、永長久寛、寺岡靖剛

    第106回触媒討論会  2011年5月 

     詳細を見る

    開催年月日: 2010年9月

    会議種別:口頭発表(一般)  

    国名:日本国  

  • バイメタリックナノ粒子の調製とその担持方法に関する検討

    木村加奈、永長久寛、寺岡靖剛

    第106回触媒討論会  2010年9月 

     詳細を見る

    開催年月日: 2010年9月

    会議種別:口頭発表(一般)  

    開催地:甲府   国名:日本国  

  • Mn系複合金属酸化物によるベンゼンのオゾン酸化反応

    前田菜那子、永長久寛、寺岡靖剛

    第47回化学関連支部合同九州大会  2010年7月 

     詳細を見る

    開催年月日: 2010年7月

    開催地:北九州   国名:日本国  

  • Catalytic oxidation of benzene with ozone over manganese oxide catalysts supported on zeolite Y

    永長久寛、寺岡靖剛、尾形敦

    The Sixth Tokyo Conference on Advanced Catalytic Science and Technology & The Fifth Asia Pacific Congress on Catalysis  2010年7月 

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    開催年月日: 2010年7月

    会議種別:口頭発表(一般)  

    開催地:Sapporo   国名:日本国  

  • Catalytic oxidation processes for air pollution control 国際会議

    Hisahiro Einaga, Yasutake Teraoka

    The 5th International Symposium of Novel Carbon Resource Sciences  2010年4月 

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    開催年月日: 2010年4月

    会議種別:口頭発表(一般)  

    開催地:Perth   国名:オーストラリア連邦  

  • オゾンを酸化剤とした揮発性有機化合物の触媒酸化分解技術

    永長久寛、寺岡靖剛、尾形敦

    日本化学会第90春季年会  2010年3月 

     詳細を見る

    開催年月日: 2010年3月

    会議種別:口頭発表(一般)  

    開催地:大阪   国名:日本国  

  • オゾンを酸化剤とした触媒反応~低濃度VOC処理技術の開発~ 招待

    永長 久寛

    触媒学会西日本地区講演会  2008年11月 

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    開催年月日: 2008年11月

    会議種別:口頭発表(一般)  

    開催地:長崎   国名:日本国  

  • Catalytic Oxidation of Benzene with Ozone over Supported Manganese Oxides 国際会議

    Hisahiro Einaga, Yasutake Teraoka, and Atsushi Ogata

    14th International Congress on Catalysis(ICC)  2008年7月 

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    開催年月日: 2008年7月

    会議種別:口頭発表(一般)  

    開催地:ソウル   国名:大韓民国  

  • 担持酸化マンガン触媒によるベンゼンのオゾン酸化反応―活性を支配する因子の検討と高活性化の試み―

    永長久寛、尾形敦、原田雅史

    第99回触媒討論会  2007年3月 

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    会議種別:口頭発表(一般)  

    開催地:神戸市   国名:日本国  

  • 担持酸化マンガン触媒によるベンゼンのオゾン酸化反応

    永長 久寛、二タ村 森

    日本オゾン協会第15回年次研究講演会  2005年9月 

     詳細を見る

    会議種別:口頭発表(一般)  

    開催地:大津   国名:日本国  

  • オゾンを酸化剤としたVOCsの触媒分解反応 -水蒸気の添加効果-

    永長 久寛、二タ村 森

    第96触媒討論会  2005年9月 

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    会議種別:口頭発表(一般)  

    開催地:熊本   国名:日本国  

  • オゾンを酸化剤とした VOCの触媒分解反応

    永長 久寛、二タ村 森

    第38回酸化反応討論会  2005年11月 

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    会議種別:口頭発表(一般)  

    開催地:札幌   国名:日本国  

  • Preparation of Platinum Nanoparticles on TiO2 for Improvement of Photocatalytic Activities 国際会議

    H. Einaga, M. Harada

    第16回日本MRS学術シンポジウム  2005年12月 

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    会議種別:口頭発表(一般)  

    開催地:東京   国名:日本国  

  • Benzene oxidation with ozone over supported manganese oxide catalysts: effect of catalyst support, reaction temperature and water vapor 国際会議

    H. Einaga, S. Futamura

    TOCAT5 (5th Tokyo Conference on Advanced Catalytic Science and Technology)  2006年7月 

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    会議種別:口頭発表(一般)  

    開催地:東京   国名:日本国  

  • Preparation of PVP-stabilized platinum nanoparticles and their deposition on TiO2 photocatalyst 国際会議

    H. Einaga, M. Harada

    TOCAT5 (5th Tokyo Conference on Advanced Catalytic Science and Technology)  2006年7月 

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    会議種別:口頭発表(一般)  

    開催地:東京   国名:日本国  

  • Sr-Al-Nb系ペロブスカイト型酸化物の金属イオン規則配列構造制御と光触媒特性

    岩倉大典、草場 一、永長久寛、寺岡靖剛

    第106回触媒討論会  2010年9月 

     詳細を見る

    開催年月日: 2011年9月

    会議種別:口頭発表(一般)  

    開催地:甲府   国名:日本国  

  • メカノケミカル法を用いたRh含有La-Mn系ペロブスカイト触媒の調製とキャラクタリゼーション

    大野諒平、草場 一、永長久寛、寺岡靖剛

    第106回触媒討論会  2010年9月 

     詳細を見る

    開催年月日: 2010年9月

    開催地:甲府   国名:日本国  

  • アルミナ細孔内へのPdとLaMnO3の共担持触媒の調製とその特性

    藤 章裕、草場 一、永長久寛、寺岡靖剛

    第106回触媒討論会  2010年9月 

     詳細を見る

    開催年月日: 2010年9月

    会議種別:口頭発表(一般)  

    開催地:甲府   国名:日本国  

  • アルミナ細孔内外に担持した Pd - LaMnO3 触媒の NO - CO 反応活性

    藤章裕、草場一、永長久寛、寺岡靖剛

    第47回化学関連支部合同九州大会  2010年7月 

     詳細を見る

    開催年月日: 2010年7月

    開催地:北九州   国名:日本国  

  • CeO2およびAg/CeO2触媒によるPM燃焼反応

    末永康朗、草場一、永長久寛、寺岡靖剛

    第47回化学関連支部合同九州大会  2010年7月 

     詳細を見る

    開催年月日: 2010年7月

    開催地:北九州   国名:日本国  

  • CeO2/Ag系金呈色顔料の発色条件の検討

    中山裕葵、永長久寛、寺岡靖剛

    第27回希土類討論会  2010年5月 

     詳細を見る

    開催年月日: 2010年5月

    会議種別:口頭発表(一般)  

    国名:日本国  

  • 酸化チタン光触媒による生体分子の酸化分解反応

    川浪明土、永長久寛、寺岡靖剛

    2010年3月 

     詳細を見る

    開催年月日: 2010年3月

    会議種別:口頭発表(一般)  

    開催地:大阪   国名:日本国  

  • トルエン光触媒酸化反応における中間生成物の追跡

    望月啓介、草場 一、永長久寛、寺岡靖剛

    日本化学会第89春季年会  2009年3月 

     詳細を見る

    開催年月日: 2009年3月

    会議種別:口頭発表(一般)  

    開催地:千葉   国名:日本国  

  • 白金ナノ粒子担持触媒の調製と触媒特性

    木村加奈、永長久寛、寺岡靖剛

    第103回触媒討論会  2009年3月 

     詳細を見る

    開催年月日: 2009年3月

    会議種別:口頭発表(一般)  

    開催地:埼玉   国名:日本国  

  • 酸化チタン光触媒上でのトルエン分解過程の追跡

    望月啓介、草場 一、永長久寛、寺岡靖剛

    2008年日本化学会西日本大会  2008年11月 

     詳細を見る

    開催年月日: 2008年11月

    会議種別:口頭発表(一般)  

    開催地:長崎   国名:日本国  

  • La-Mn-O系複合酸化物触媒によるベンゼン酸化分解反応

    兵頭伸哉、草場 一、永長久寛、寺岡靖剛

    第102回触媒討論会  2008年9月 

     詳細を見る

    開催年月日: 2008年9月

    会議種別:口頭発表(一般)  

    開催地:名古屋   国名:日本国  

  • TiO2および貴金属担持TiO2のトルエン分解特性

    望月啓介、草場 一、永長久寛、寺岡靖剛

    第15回九州夏期セラミックス研究会  2008年8月 

     詳細を見る

    開催年月日: 2008年8月

    開催地:福岡   国名:日本国  

  • ペロブスカイト型複合金属酸化物の合成とベンゼン酸化分解特性

    兵頭伸哉、草場 一、永長久寛、寺岡靖剛

    第15回九州夏期セラミックス研究会  2008年8月 

     詳細を見る

    開催年月日: 2008年8月

    会議種別:口頭発表(一般)  

    開催地:福岡   国名:日本国  

  • 酸化チタンおよび貴金属担持酸化チタンによるトルエンの光酸化反応

    望月啓介、草場 一、永長久寛、寺岡靖剛

    第45回化学関連支部合同九州大会  2008年7月 

     詳細を見る

    開催年月日: 2008年7月

    会議種別:口頭発表(一般)  

    開催地:北九州   国名:日本国  

  • ペロブスカイト型複合金属酸化物触媒によるベンゼンの完全酸化反応

    兵頭伸哉、草場 一、永長久寛、寺岡靖剛

    第45回化学関連支部合同九州大会  2008年7月 

     詳細を見る

    開催年月日: 2008年7月

    会議種別:口頭発表(一般)  

    開催地:北九州   国名:日本国  

  • VOC排出規制と対策技術 招待

    永長 久寛

    第3回工業化学定例会  2006年5月 

     詳細を見る

    会議種別:口頭発表(一般)  

    開催地:東京   国名:日本国  

  • Catalytic Oxidation with Ozone for Control of Volatile Organic Compounds in Flue Gases 国際会議

    H. Einaga, S. Futamura

    The 16th Regional Conference of Clean Air and Environment in Asia Pacific Area  2005年8月 

     詳細を見る

    会議種別:口頭発表(一般)  

    開催地:東京   国名:日本国  

  • Catalytic ozonation of volatile organic compounds over supported manganese oxides 国際会議

    Hisahiro Einaga, Shigeru Futamura

    Pacifichem2005  2005年12月 

     詳細を見る

    会議種別:口頭発表(一般)  

    開催地:ホノルル、ハワイ   国名:アメリカ合衆国  

  • XAFS measurements of the structural changes in manganese oxide catalysts 国際会議

    Hisahiro Einaga, Masafumi Harada, and Shigeru Futamura

    Pacifichem2005  2005年12月 

     詳細を見る

    会議種別:口頭発表(一般)  

    開催地:ホノルル、ハワイ   国名:アメリカ合衆国  

▼全件表示

MISC

  • オゾンを利用したMn触媒によるVOC分解技術

    永長 久寛

    触媒   2008年6月

     詳細を見る

    記述言語:日本語   掲載種別:記事・総説・解説・論説等(学術雑誌)  

  • オゾンを酸化剤としたVOC分解技術—温和な条件下で作動する触媒酸化技術の利用

    永長 久寛

    クリーンテクノロジー   2006年9月

     詳細を見る

    記述言語:日本語   掲載種別:記事・総説・解説・論説等(学術雑誌)  

  • 低温プラズマを用いた有害大気汚染物質分解技術の開発

    尾形 敦,金 賢夏,永長 久寛

    応用物理   2008年9月

     詳細を見る

    記述言語:日本語  

  • 触媒を利用した低温プラズマ法によるVOC分解技術の研究・開発動向

    金 賢夏、永長 久寛,尾形 敦

    環境管理   2004年1月

     詳細を見る

    記述言語:日本語   掲載種別:記事・総説・解説・論説等(学術雑誌)  

産業財産権

特許権   出願件数: 1件   登録件数: 2件
実用新案権   出願件数: 0件   登録件数: 0件
意匠権   出願件数: 0件   登録件数: 0件
商標権   出願件数: 0件   登録件数: 0件

所属学協会

  • 石油学会

  • 日本オゾン協会

  • 光化学協会

  • 触媒学会

  • 米国化学会

  • 日本化学会

  • 日本電磁波エネルギー応用学会

▼全件表示

委員歴

  • 触媒学会   幹事   国内

    2011年3月 - 2012年2月   

  • 触媒学会   討論会委員   国内

    2008年3月 - 2010年2月   

  • 石油学会九州・沖縄支部   幹事   国内

    2007年3月 - 現在   

  • 触媒学会   代議員   国内

    2006年3月 - 現在   

  • 触媒学会   幹事   国内

    2005年3月 - 2006年2月   

学術貢献活動

  • 座長(Chairmanship)

    石油学会  ( 山口 ) 2011年11月

     詳細を見る

    種別:大会・シンポジウム等 

  • 座長(Chairmanship)

    触媒討論会第106回討論会  ( 甲府 ) 2010年9月

     詳細を見る

    種別:大会・シンポジウム等 

  • 座長(Chairmanship)

    触媒学会第104回討論会  ( 宮崎 ) 2009年9月 - 2011年9月

     詳細を見る

    種別:大会・シンポジウム等 

  • 座長(Chairmanship)

    触媒学会第102回討論会  ( 名古屋大学 ) 2008年9月

     詳細を見る

    種別:大会・シンポジウム等 

  • 司会(Moderator)

    第一回九州大学炭素資源国際教育研究センター講演会  ( 九州大学筑紫キャンパス ) 2008年5月 - 2009年5月

     詳細を見る

    種別:大会・シンポジウム等 

  • 座長(Chairmanship)

    第100回触媒討論会  ( 北海道札幌市 ) 2007年9月 - 現在

     詳細を見る

    種別:大会・シンポジウム等 

  • 座長(Chairmanship)

    第99回触媒討論会  ( 神戸市 ) 2007年3月 - 現在

     詳細を見る

    種別:大会・シンポジウム等 

  • 幹事

    触媒学会つくば地区講演会  ( 茨城県つくば市 ) 2005年12月 - 現在

     詳細を見る

    種別:大会・シンポジウム等 

    参加者数:100

▼全件表示

共同研究・競争的資金等の研究課題

  • マイクロ波援用高度炭化水素循環技術の開発

    2022年 - 2024年

    エネルギー研究教育機構 モジュール予算

      詳細を見る

    担当区分:研究代表者  資金種別:学内資金・基金等

  • 低濃度汚染物質の吸着・濃縮と急速昇温分解を可能にするマイクロ波援用触媒プロセス

    研究課題/領域番号:21H03635  2021年 - 2023年

    日本学術振興会  科学研究費助成事業  基盤研究(B)

    永長 久寛, 宮脇 仁

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

    工場、事業所から排出される低濃度のVOCの処理の高効率化は環境保全の観点から喫緊の課題である。本研究では、炭素系材料とペロブスカイト型酸化物触媒の高いマイクロ波加熱特性を生かし、低濃度のVOCの吸脱着と濃縮、酸化分解過程を速やかに進行させる高効率VOC分解プロセスを開発し、その有効性について実証する。VOC吸脱着特性とマイクロ波加熱特性に寄与する炭素系材料の物性、マイクロ波加熱下でのVOC分解活性を支配するペロブスカイト型酸化物の物性を制御し、シングルモード、マルチモードマイクロ波リアクタでの機能を精査する。小規模のVOC発生源に対応できるVOC分解プロセスの構築に必要な基盤技術を確立する。

    CiNii Research

  • 結晶面・格子歪みの精密制御による高反応性格子酸素の設計

    研究課題/領域番号:20H02824  2020年4月 - 2023年3月

    科学研究費助成事業  基盤研究(B)

    北條 元, 永長 久寛

      詳細を見る

    資金種別:科研費

    金属酸化物はそれ自身、またはそれに貴金属等を担持したものが様々な触媒材料として用いられている。これらの酸化物における触媒活性は、その格子酸素の反応性に大きく左右される。そのため、格子酸素の反応性を制御するための指針を得ることは、学術的な観点からだけでなく応用的な観点からも重要な課題である。本研究では、酸化セリウム(CeO2)を基盤材料として、高い反応性の格子酸素を実現するための材料設計指針を確立することを目的とする。

    CiNii Research

  • オゾン-マイクロ波援用触媒反応を基盤とした難処理排ガス浄化技術の開発

    2020年 - 2022年

    科学技術振興機構 研究成果最適展開支援プログラム(A-STEP)

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • 金属酸化物の酸化特性を利用しためっき廃液処理と肥料製造プロセスの開発

    研究課題/領域番号:20K21866  2020年 - 2021年

    日本学術振興会  科学研究費助成事業  挑戦的研究(萌芽)

    永長 久寛

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

    リン化合物は化学工業から農業用肥料まで幅広く使用される汎用製品であるが、枯渇性の資源である一方、環境中に排出されると海水の汚染につながるため、排水処理方法の高度化が求められている.本研究では、産業界から排出されるリン資源の回収と再利用、肥料化を目的として、めっき廃液中のホスフィン酸イオンを効率よく亜リン酸イオンに転換する触媒酸化還元サイクルを構築する.

    CiNii Research

  • 産業環境保全のための次世代型空気質制御技術の開発

    2020年

    2020年度JKA補助事業

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • 吸着-触媒材料-低温プラズマ複合化によるVOC処理技術の確立

    2019年 - 2021年

    科学技術振興機構

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • 表面金属種の配列を制御した二元系金属担持触媒の開発

    研究課題/領域番号:16K06856  2016年 - 2018年

    日本学術振興会  科学研究費助成事業  基盤研究(C)

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

  • 鉄鋼スラグを触媒とした環境浄化プロセスの開発

    2014年 - 2015年

    研究成果最適展開支援プログラム(A-STEP)

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • オゾン酸化触媒の選択酸化特性に基づくポリエステルの新規再利用プロセスの開発

    研究課題/領域番号:25550071  2013年 - 2015年

    科学研究費助成事業  挑戦的萌芽研究

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

  • オゾン酸化触媒の選択酸化特性に基づくポリエステルの新規再利用プロセスの開発

    2013年

    科学研究費助成事業  挑戦的萌芽研究

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

  • 中小規模発生源対策用VOC分解処理システムの開発

    2011年 - 2012年

    科学技術振興機構 A-STEP

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • オゾンを酸化剤とした低温作動型VOC酸化触媒反応の研究

    2010年4月 - 2013年3月

      詳細を見る

    担当区分:研究代表者 

    本研究は,オゾンを酸化剤とした低温酸化触媒プロセスについて,室温もしくはそれ以下の低温条件下で高い活性を示す触媒材料の開発と反応機構の解明を目的とする.ゼオライトに担持したMn酸化物を触媒とし, ゼオライトの細孔構造と疎水性を緻密に制御すること,Mnの担持方法を高度化することにより,触媒の物性と活性の相関性について明らかにするとともに水蒸気共存下で揮発性有機化合物(VOC)を効率良くCO2まで酸化分解・無害化する触媒材料を探索する.また,速度論および分光法を駆使し,水蒸気添加によるVOC酸化分解活性向上の発現メカニズムを解明する.

  • 原位置浄化型省エネルギーVOC触媒分解プロセスの開発

    2010年 - 2011年

    鉄鋼業環境保全技術開発基金 2010年度研究助成

      詳細を見る

    担当区分:研究代表者  資金種別:学内資金・基金等

  • オゾンを酸化剤とした低温作動型VOC酸化触媒反応の開発

    研究課題/領域番号:22560765  2010年

    日本学術振興会  科学研究費助成事業  基盤研究(C)

      詳細を見る

    担当区分:研究代表者  資金種別:科研費

  • 革新的ゼロエミッション石炭ガス化発電プロジェクト

    2009年4月 - 2014年3月

    新エネルギー・産業技術総合開発機構 

      詳細を見る

    担当区分:研究分担者 

    本事業では、石炭ガス化システムから回収したCO2を酸化剤の一部として用いることにより、石炭ガス化システムの効率を大幅に向上することのできるCO2回収型次世代IGCCシステムの実用基盤技術開発を行う。具体的には、本システムに関し、CO2による石炭ガス化性能向上効果の解明と実証、乾式ガス精製技術の最適化、実用規模プラントのFSなどを実施する。また、本技術について、アジアなど環太平洋地域の多様な石炭に対する適応性を検討する。

  • 原位置浄化型省エネルギーVOC触媒分解プロセスの開発

    2009年 - 2010年

    鉄鋼業環境保全技術開発基金 2009年度研究助成

      詳細を見る

    担当区分:研究代表者  資金種別:学内資金・基金等

  • エアロゾル感染防止のための低温酸化触媒技術の開発

    2009年

    科学技術振興機構シーズ発掘試験

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • 度環境技術開発等推進費「外場援用システム触媒による持続発展可能なVOC排出制御技術に関する研究」

    2008年8月 - 2011年3月

    環境省 

      詳細を見る

    担当区分:研究分担者 

    シリカ系あるいはペロブスカイト系の材料を中心とした低環境負荷型触媒の探索・創製と、触媒機能を補強あるいは増幅させる外場援用手段をマッチングさせることによる有害大気汚染物質の排出抑制技術の構築を目指す。同時に、共通基盤技術であるVOCセンサの開発を行う。

  • 外場援用システム触媒による持続発展可能なVOC排出抑制技術に関する研究

    2008年 - 2010年

    環境技術開発等推進費

      詳細を見る

    担当区分:研究分担者  資金種別:受託研究

  • 貴金属合金ナノ粒子合成法の開発

    2008年

    科学技術振興機構シーズ発掘試験

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

  • ダイレクトメタノール形燃料電池電極用の高活性酸化触媒の研究開発

    2004年 - 2005年

      詳細を見る

    担当区分:研究分担者  資金種別:受託研究

  • 錯体光触媒による環境残留性パーフルオロ酸化合物の無害化処理

    2003年 - 2004年

    日本学術振興会  科学研究費助成事業  基盤研究(B)

      詳細を見る

    担当区分:研究分担者  資金種別:科研費

  • マイクロバブルによる極限反応場を利用した排水中有害化学物質の分解に関する研究

    2002年 - 2003年

    日本学術振興会  科学研究費助成事業  基盤研究(B)

      詳細を見る

    担当区分:研究分担者  資金種別:科研費

  • 太陽エネルギー利用環境浄化システムの開発

    2000年 - 2002年

      詳細を見る

    担当区分:研究代表者  資金種別:受託研究

▼全件表示

教育活動概要

  • 触媒化学は無機化学、反応工学、物理化学、分析化学、有機反応化学などの学術分野、エネルギー・環境工学などの技術分野と密接に関わっており、触媒化学の研究を通してこれらの知識や技術を指導する。現在、環境・エネルギー分野においては、有害化学物質の汚染、石油代替エネルギーの開発など、多くの問題、課題が山積している。これらの解決には個々の学術分野の進展とともに、分野横断的・学際的な領域に研究を展開し、新しい分野を開拓していくことが必要である。無機材料化学をベースとした基礎・応用研究を通して環境・エネルギー問題に積極的に取り組む研究者・技術者を育成する。

担当授業科目

  • 環境触媒化学 d

    2023年12月 - 2024年2月   冬学期

  • 触媒化学Ⅱ

    2023年10月 - 2024年3月   後期

  • 触媒化学Ⅰ

    2023年10月 - 2023年12月   秋学期

  • 無機化学第一(S2-16)

    2023年4月 - 2023年9月   前期

  • シンクロトロン光概論

    2023年4月 - 2023年9月   前期

  • 材料機能設計基盤特論 Ⅰ e

    2023年4月 - 2023年6月   春学期

  • 無機化学第一(S2-16)

    2022年4月 - 2022年9月   前期

  • 無機化学第一【基礎物質科学】

    2022年4月 - 2022年9月   前期

  • シンクロトロン光概論

    2022年4月 - 2022年9月   前期

  • シンクロトロン光概論

    2022年4月 - 2022年9月   前期

  • 無機化学第一【元素科学】

    2022年4月 - 2022年9月   前期

  • 環境触媒化学 d

    2021年12月 - 2022年2月   冬学期

  • 無機材料科学Ⅰ

    2021年12月 - 2022年2月   冬学期

  • 先端表面反応化学 i

    2021年6月 - 2021年8月   夏学期

  • シンクロトロン光概論

    2021年4月 - 2021年9月   前期

  • 材料機能設計基盤特論 Ⅰ e

    2021年4月 - 2021年6月   春学期

  • 固体材料設計学

    2020年10月 - 2021年3月   後期

  • 無機材料科学Ⅰ

    2020年10月 - 2021年3月   後期

  • Basic Physical Chemistry II

    2020年4月 - 2020年9月   前期

  • 固体材料設計学

    2019年10月 - 2020年3月   後期

  • 無機材料科学Ⅰ

    2019年10月 - 2020年3月   後期

  • 固体材料設計学

    2018年10月 - 2019年3月   後期

  • 無機材料科学Ⅰ

    2018年10月 - 2019年3月   後期

  • Basic Physical Chemistry II

    2018年10月 - 2019年3月   後期

  • 固体材料設計学

    2017年10月 - 2018年3月   後期

  • 無機材料科学Ⅰ

    2017年10月 - 2018年3月   後期

  • Basic Physical Chemistry I & II

    2017年10月 - 2018年3月   後期

  • Physical Chemistry I&II

    2016年10月 - 2017年3月   後期

  • 無機材料科学Ⅰ

    2016年10月 - 2017年3月   後期

  • 基礎化学熱力学

    2016年10月 - 2017年3月   後期

  • 固体材料設計学

    2016年10月 - 2017年3月   後期

  • 炭素資源学

    2015年10月 - 2016年3月   後期

  • 無機材料科学Ⅰ

    2015年10月 - 2016年3月   後期

  • 固体材料設計学

    2015年10月 - 2016年3月   後期

  • Physical Chemistry I&II

    2015年10月 - 2016年3月   後期

  • Basic Physical Cehmistry I & II

    2014年10月 - 2015年3月   後期

  • 無機材料科学Ⅰ

    2014年10月 - 2015年3月   後期

  • 基礎熱力学

    2014年4月 - 2014年9月   前期

  • 課題協学

    2014年4月 - 2014年9月   前期

  • エネルギー物質工学演習

    2013年10月 - 2014年3月   後期

  • 基礎熱力学

    2013年4月 - 2013年9月   前期

  • エネルギー材料科学

    2013年4月 - 2013年9月   前期

  • 化学反応論Ⅱ

    2013年4月 - 2013年9月   前期

  • 無機材料科学Ⅰ

    2012年10月 - 2013年3月   後期

  • エネルギー物質工学実験Ⅱ

    2012年10月 - 2013年3月   後期

  • 化学反応論Ⅱ

    2012年4月 - 2012年9月   前期

  • エネルギー物質工学実験Ⅰ

    2012年4月 - 2012年9月   前期

  • 基礎熱力学

    2012年4月 - 2012年9月   前期

  • エネルギー材料科学

    2012年4月 - 2012年9月   前期

  • 固体材料設計学

    2011年10月 - 2012年3月   後期

  • 基礎物質科学

    2011年10月 - 2012年3月   後期

  • 基礎熱力学

    2011年4月 - 2011年9月   前期

  • エネルギー物質工学演習

    2011年4月 - 2011年9月   前期

  • 化学結合論

    2007年10月 - 2008年3月   後期

  • エネルギー材料科学

    2006年10月 - 2007年3月   後期

  • 固体材料設計学

    2006年10月 - 2007年3月   後期

▼全件表示

その他教育活動及び特記事項

  • 2016年  クラス担任  学部

社会貢献活動

  • 化学への招待 福岡県下の青少年(主に高校生)を対象として、夏休みに九州大学大学院で先端科学技術に関連した化学実験を行ない、研究室見学会を開催することで、青少年の化学に対する興味を育てると同時に、理科・化学教育に携わる大学の若手先生方との交流を企画した。

    日本化学会九州支部  九州大学筑紫キャンパス  2009年7月

     詳細を見る

    対象:社会人・一般, 学術団体, 企業, 市民団体, 行政機関

    種別:講演会

学内運営に関わる各種委員・役職等

  • 2022年4月 - 2024年3月   センター グリーンテクノロジー研究教育センター 副センター長

  • 2022年4月 - 2024年3月   研究所 シンクロトロン光利用研究センター 副センター長

  • 2018年4月 - 2020年3月   全学 シンクロトロン光利用研究センター 副センター長

  • 2017年4月 - 2018年3月   部門 物質科学副部門長

  • 2017年4月 - 2018年3月   専攻 物質理工学専攻長

  • 2016年4月 - 2018年3月   センター シンクロトロン光利用研究センター 副センター長

  • 2012年4月 - 2013年3月   学府 総合理工学府 副学務委員

  • 2011年4月 - 2013年3月   学科 エネルギー科学科教務委員

▼全件表示