出版者・発行元：Advanced Functional Materials  

Micro/nanoscale lasers that span the entire visible spectrum, especially those in red, green, and blue colors, are not only essential for a variety of optical devices but also have important applications in visible color communication, multi-color fluorescence sensing, and wavelength division multiplexing. Despite the great efforts made to achieve multi-color lasing using a variety of approaches, on-chip white light emission and even red, green, and blue multi-color lasers still suffer from considerable challenges in micro-nano structures. Here, CdSxSe1−x, CdS, and ZnS micro-tripod structures are successfully prepared using chemical vapor deposition approaches. The micro-photoluminescence (µ-PL) spectra and PL-mapping of these micro-tripods reveal various emissions at 630, 508, and 460 nm, respectively. Additionally, white-light emissions based on these composition-tunable tripods are realized through an end-coupling structure system. Moreover, room-temperature modes tunable lasers are observed clearly from three legs of these micro-tripods, with a low threshold of ≈48.39 µJ cm−2 and a high quality factor of 1227.3. The realization of micro-tripods-based lasers may provide an innovative way for highly integrated photonic circuits and communications.

DOI： 10.1002/adfm.202403135

Scopus

出版者・発行元：Materials Today Energy  

Ammonia, with its wide-ranging applications in global industries, plays an indispensable role in the growth and sustainability of modern society. Electrochemical nitrate reduction (eNO3RR) presents an environmentally friendly pathway for ammonia production, sidestepping the energy consumption and greenhouse gas emissions associated with the conventional Haber–Bosch process. However, developing efficient and selective catalysts for eNO3RR is challenging due to its intricate multiproton-coupled electron transfer process and the competing hydrogen evolution reaction. This review dives deep into the recent advancements in eNO3RR, shedding light on the mechanism through in situ spectroscopic studies and innovative strategies for catalyst design. We first lay out the possible reaction pathways and products in eNO3RR and then introduce a variety of in situ electrochemical characterizations that provide real-time insights into the reaction mechanism. We also explore strategies for rational electrocatalyst design to optimize the performance. Representative examples of advanced materials with high activity, selectivity, and stability are highlighted to underscore the progress made in this field. Finally, we outline emerging opportunities and future directions, such as developing multifunctional nanostructured catalysts through integrated computational and combinatorial approaches. This review aims to provide valuable insights and guidance for developing nitrate electroreduction and the efficient production of green ammonia in industry.

DOI： 10.1016/j.mtener.2024.101610

Scopus

出版者・発行元：Chem Catalysis  

Competing hydrogen evolution reaction (HER) and sluggish multi-electron/proton-involved steps are the major obstacles to improving the efficiency and selectivity of electrochemical nitrate reduction to ammonia (eNO3RR). Herein, we modified Co3O4 nanoparticles with doped rare-earth La atoms and carboxylic (COO−)-based organic ligands. The COO− groups efficiently reduce the water activity around the active sites by forming hydrogen bonds, thus controlling proton accessibility and regulating the adsorption selectivity between nitrate ions and protons. Simultaneously, introducing oxygen vacancies through La doping establishes active sites with a strong affinity for nitrate ions and an electron-rich local environment conducive to eNO3RR. The electrocatalyst exhibits superior activity and selectivity with an ammonia Faradaic efficiency of up to 99.41% and a yield rate of 5.62 mg h−1 mgcat−1 at −0.3 V vs. reversible hydrogen electrode (RHE). Notably, the catalyst maintains over 90% Faradaic efficiency for NH3 production across a broad potential range of 400 mV, surpassing most recently reported eNO3RR electrocatalysts.

DOI： 10.1016/j.checat.2024.101024

Scopus

出版者・発行元：ACS Nano  

Precise synthesis of all-inorganic lead halide perovskite nanowire heterostructures and superlattices with designable modulation of chemical compositions is essential for tailoring their optoelectronic properties. Nevertheless, controllable synthesis of perovskite nanostructure heterostructures remains challenging and underexplored to date. Here, we report a rational strategy for wafer-scale synthesis of one-dimensional periodic CsPbCl3/CsPbI3 superlattices. We show that the highly parallel array of halide perovskite nanowires can be prepared roughly as horizontally guided growth on an M-plane sapphire. A periodic patterning of the sapphire substrate enables position-selective ion exchange to obtain highly periodic CsPbCl3/CsPbI3 nanowire superlattices. This patterning is further confirmed by micro-photoluminescence investigations, which show that two separate band-edge emission peaks appear at the interface of a CsPbCl3/CsPbI3 heterojunction. Additionally, compared with the pure CsPbCl3 nanowires, photodetectors fabricated using these periodic heterostructure nanowires exhibit superior photoelectric performance, namely, high ION/IOFF ratio (104), higher responsivity (49 A/W), and higher detectivity (1.51 × 1013 Jones). Moreover, a spatially resolved visible image sensor based on periodic nanowire superlattices is demonstrated with good imaging capability, suggesting promising application prospects in future photoelectronic imaging systems. All these results based on the periodic CsPbCl3/CsPbI3 nanowire superlattices provides an attractive material platform for integrated perovskite devices and circuits.

DOI： 10.1021/acsnano.4c05205

Scopus

出版者・発行元：ACS Applied Materials and Interfaces  

Recently emerged lead halide perovskite CsPbX3 (X = Cl, Br, and I) nanocrystals (PNCs) have attracted tremendous attention due to their excellent optical properties. However, the poor water stability, unsatisfactory luminescence efficiency, disappointing lead leakage, and toxicity have restricted their practical applications in photoelectronics and biomedical fields. Herein, a controllable encapsulated strategy is investigated to realize CsPbX3 PNCs/PVP @PMMA composites with superior luminescence properties and excellent biocompatibility. Additionally, the synthesized CsPbBr3 and CsPbBr0.6I2.4 PNCs/PVP@PMMA structures exhibit green and red emissions with a maximal photoluminescence quantum yield (PLQY) of about 70.24% and 98.26%, respectively. These CsPbX3 PNCs/PVP@PMMA structures show high emission efficiency, excellent stability after water storage for 18 months, and low cytotoxicity at the PNC concentration at 500 μg mL-1. Moreover, white light-emitting diode (WLED) devices based on mixtures of CsPbBr3 and CsPbBr0.6I2.4 PNCs/PVP@PMMA perovskite structures are investigated, which exhibit excellent warm-white light emissions at room temperature. A flexible manipulation method is used to fabricate the white light emitters based on these perovskite composites, providing a fantastic platform for fabricating solid-state white light sources and full-color displays.

DOI： 10.1021/acsami.4c06854

Scopus

出版者・発行元：ACS Nano  

Two-dimensional (2D) tellurium (Te) is emerging as a promising p-type candidate for constructing complementary metal-oxide-semiconductor (CMOS) architectures. However, its small bandgap leads to a high leakage current and a low on/off current ratio. Although alloying Te with selenium (Se) can tune its bandgap, thermally evaporated SexTe1-x thin films often suffer from grain boundaries and high-density defects. Herein, we introduce a precursor-confined chemical vapor deposition (CVD) method for synthesizing single-crystalline SexTe1-x alloy nanosheets. These nanosheets, with tunable compositions, are ideal for high-performance field-effect transistors (FETs) and 2D inverters. The preformation of Se-Te frameworks in our developed CVD method plays a critical role in the growth of SexTe1-x nanosheets with high crystallinity. Optimizing the Se composition resulted in a Se0.30Te0.70 nanosheet-based p-type FET with a large on/off current ratio of 4 × 105 and a room-temperature hole mobility of 120 cm2·V-1·s-1, being eight times higher than thermally evaporated SexTe1-x with similar composition and thickness. Moreover, we successfully fabricated an inverter based on p-type Se0.30Te0.70 and n-type MoS2 nanosheets, demonstrating a typical voltage transfer curve with a gain of 30 at an operation voltage of Vdd = 3 V.

DOI： 10.1021/acsnano.4c05323

Scopus

出版者・発行元：Advanced Optical Materials  

Van der Waals (vdW) heterostructures have gained significant attention in photodetectors due to their seamless integration with materials possessing diverse functionalities. In this study, the fabrication of a Te nanomesh/black-Si vdW heterostructure is presented, and investigated its photoresponse properties. The heterostructure exhibits a pronounced rectification behavior, characterized by a rectification ratio of 2.2 × 104. Notably, the heterostructure device demonstrates commendable photoresponse properties, including a high responsivity of 350 mA W−1, an extensive linear dynamic range of 45.5 dB, a high specific detectivity of 9.6 × 1011 Jones, and a wide spectral response ranging from 400 to 1550 nm. Furthermore, the heterostructure exhibits rapid response, with a rise time and a decay time of 70 and 140 µs, respectively. These exceptional photoresponse properties can be attributed to the robust internal built-in electrical field at the hetero-interface and the augmented light absorption in black-Si. The outstanding photoresponse properties of the heterostructure make it a promising candidate for multiwavelength single-pixel imaging, enabling the collection of mask patterns under varying wavelengths of light radiation. This work provides a novel approach for fabricating mixed-dimensional vdW heterostructures, offering promising prospects for advancements in optoelectronics.

DOI： 10.1002/adom.202400056

Scopus

出版者・発行元：Matter  

van der Waals (vdWs) dielectrics are widely used in nanoelectronics to preserve the intrinsic properties of two-dimensional (2D) semiconductors. However, achieving aligned growth of 2D semiconductors and their direct utilization on original vdWs epitaxial dielectrics to avoid disorders poses significant challenges. Here, a hydromechanical strategy for aligned epitaxy of 2D materials on naturally occurring vdWs mica dielectrics is developed. By combining density functional theory with Lagrange's group theorem, a quantitative criterion for 2D material epitaxy on 6-fold symmetric vdWs dielectrics is established. Moreover, the as-grown ultrathin Bi2O2Se-channeled field-effect transistor, with a hybrid dielectric layer, achieves a superior current on/off ratio (1.4 × 107) and high carrier mobility (22.4 cm2 V−1 S−1) by directly integrating as-grown 2D materials/vdWs dielectrics. This work provides a powerful methodological platform for aligned 2D material synthesis, alignment direction prediction, and intrinsic property investigation, laying the foundation for advanced electronics on as-grown 2D materials/vdWs dielectrics.

DOI： 10.1016/j.matt.2024.04.013

Scopus

出版者・発行元：Materials Today Electronics  

Perovskites have emerged as a promising new generation of photovoltaic conversion materials, gradually surpassing traditional silicon-based materials in solar cell research. This development is primarily due to their superior power-conversion efficiency (PCE), simple fabrication process, and cost-effective production. However, the low stability of perovskite ionic crystals poses a significant challenge to their stability, hindering the progress of perovskite materials and devices. Although two-dimensional (2D) perovskites offer improved stability, adding organic amine ions results in a quantum confinement effect that reduces the optoelectronic performance of devices. To counter this issue, the strategic design of suitable spacer cations offers a potential solution. Aromatic amine ions possess greater polarity and structural adjustability compared to aliphatic amine ions, making them advantageous in mitigating the quantum confinement effect. This review focuses on phenylethylammonium (PEA) as a representative aromatic spacer cation. It categorizes the evolution of these cations into four trajectories: alkyl chain modification, substitution of hydrogen atoms on the aromatic ring with specific substituents, replacement of benzene rings with aromatic heterocycles, and utilization of multiple aromatic rings instead of a monoaromatic ring. The structure, properties, and corresponding device performance of aromatic spacer cations utilized in reported 2D perovskites are discussed, followed by the presentation of a series of factors for selecting and designing aromatic amine ions for future development.

DOI： 10.1016/j.mtelec.2024.100100

Scopus

出版者・発行元：Advanced Functional Materials  

Zinc (Zn) has arisen as a significant suppressor of vacancy formation in halide perovskites, establishing its pivotal role in defect engineering for these materials. Herein, the Zn-catalyzed vapor-liquid-solid (VLS) route is reported to render black-phase CsPbI3 nanowires (NWs) operationally stable at room temperature. Based on first-principle calculations, the doped Zn2+ can not only lead to the partial crystal lattice distortion but also reduce the formation energy (absolute value) from the black phase to the yellow phase, improving the stability of the desired black-phase CsPbI3 NWs. A series of contrast tests further confirm the stabilization effect of the Zn-doped strategy. Besides, the polarization-sensitive characteristics of black-phase CsPbI3 NWs are revealed. This work highlights the importance of phase stabilization engineering for CsPbI3 NWs and their potential applications in anisotropic optoelectronics.

DOI： 10.1002/adfm.202314309

Scopus

出版者・発行元：Advanced Materials  

Multiple cation-composited perovskites are demonstrated as a promising approach to improving the performance and stability of perovskite solar cells (PSCs). However, recipes developed for fabricating high-performance perovskites in laboratories are always not transferable in large-scale production, as perovskite crystallization is highly sensitive to processing conditions. Here, using an in situ optical method, the ambient temperature effect on the crystallization process in multiple cation-composited perovskites is investigated. It is found that the typical solvent-coordinated intermediate phase in methylammonium lead iodide (MAPbI3) is absent in formamidinium lead iodide (FAPbI3), and nucleation is almost completed in FAPbI3 right after spin-coating. Interestingly, it is found that there is noticeable nuclei aggregation in Formamidinium (FA)-based perovskites even during the spin-coating process, which is usually only observed during the annealing in MAPbI3. Such aggregation is further promoted at a higher ambient temperature or in higher FA content. Instead of the general belief of stress release-induced crack formation, it is proposed that the origin of the cracks in FA-based perovskites is due to the aggregation-induced solute depletion effect. This work reveals the limiting factors for achieving high-quality FA-based perovskite films and helps to unlock the existing narrow processing window for future large-scale production.

DOI： 10.1002/adma.202307635

Scopus

出版者・発行元：Nano Letters  

Time-resolved or time-correlation measurements using cathodoluminescence (CL) reveal the electronic and optical properties of semiconductors, such as their carrier lifetimes, at the nanoscale. However, halide perovskites, which are promising optoelectronic materials, exhibit significantly different decay dynamics in their CL and photoluminescence (PL). We conducted time-correlation CL measurements of CsPbBr3 using Hanbury Brown-Twiss interferometry and compared them with time-resolved PL. The measured CL decay time was on the order of subnanoseconds and was faster than PL decay at an excited carrier density of 2.1 × 1018 cm-3. Our experiment and analytical model revealed the CL dynamics induced by individual electron incidences, which are characterized by highly localized carrier generation followed by a rapid decrease in carrier density due to diffusion. This carrier diffusion can play a dominant role in the CL decay time for undoped semiconductors, in general, when the diffusion dynamics are faster than the carrier recombination.

DOI： 10.1021/acs.nanolett.4c00483

Scopus

出版者・発行元：Journal of Materials Chemistry A  

Searching for a stable and efficient electrocatalyst for the hydrogen evolution reaction is still challenging, especially under a wider pH operation condition. In this study, a multicomponent Ni17W3/MoO3−x/WO3−x catalyst was designed and synthesized, in which the unique hierarchical structure of entangled nanorods confined in a polyhedral framework ensures the maximum utilization of active sites. Significantly, electrochemical performance can be regulated by adjusting the oxygen vacancy concentration of the metal support. Combined with various characterization techniques, we discovered that abundant oxygen vacancies in the MoO3−x/WO3−x support not only significantly enhanced the hydrogen insertion/extraction kinetics in the metal oxide but also increased the hydration capacity, resulting in an efficient hydrogen adsorption/transfer/desorption kinetics on the Ni17W3/MoO3−x/WO3−x surface and interface. As a result, the fabricated electrocatalyst exhibits an ultralow overpotential of 16, 42, and 14 mV at 10 mA cm−2 in alkaline, neutral, and acid electrolytes, respectively. Our work proves the important role of metal oxide supports in the hydrogen spillover process.

DOI： 10.1039/d4ta00729h

Scopus

出版者・発行元：ChemCatChem  

Developing highly efficient and stable electrocatalysts with large current densities for hydrogen and oxygen evolution is still challenging. Herein, Ni and Fe co-doped cobalt carbonate hydroxide catalysts were designed in situ on the three-dimensional porous NiFe foam through a facile one-step hydrothermal strategy. Inductively coupled plasma atomic emission spectrum, transmission electron microscopy-element mapping, X-ray photoelectron spectroscopy, and DFT calculations demonstrate that the three-dimensional NiFe foam substrate not only serves as the porous substrate, which enhances the exposed number of active sites, but also enhances the intrinsic activities of single active sites via introducing Ni and Fe dopants in the cobalt carbonate hydroxide catalyst during the hydrothermal process. The obtained hybrid electrocatalyst can be employed as a highly efficient and stable bifunctional electrocatalyst for the oxygen and hydrogen evolution reactions, with overpotentials of 340 mV and 371 mV at 1000 mA cm−2, respectively. In addition, tests in an alkaline electrolyzer revealed that the current density could reach 1000 mA cm−2 at a voltage of 2 V and maintain stable operation for 100 h.

DOI： 10.1002/cctc.202301324

Scopus

出版者・発行元：Advanced Materials  

The demand for economical and efficient data processing has led to a surge of interest in neuromorphic computing based on emerging two-dimensional (2D) materials in recent years. As a rising van der Waals (vdW) p-type Weyl semiconductor with many intriguing properties, tellurium (Te) has been widely used in advanced electronics/optoelectronics. However, its application in floating gate (FG) memory devices for information processing has never been explored. Herein, an electronic/optoelectronic FG memory device enabled by Te-based 2D vdW heterostructure for multimodal reservoir computing (RC) is reported. When subjected to intense electrical/optical stimuli, the device exhibits impressive nonvolatile electronic memory behaviors including ≈108 extinction ratio, ≈100 ns switching speed, >4000 cycles, >4000-s retention stability, and nonvolatile multibit optoelectronic programmable characteristics. When the input stimuli weaken, the nonvolatile memory degrades into volatile memory. Leveraging these rich nonlinear dynamics, a multimodal RC system with high recognition accuracy of 90.77% for event-type multimodal handwritten digit-recognition is demonstrated.

DOI： 10.1002/adma.202308502

Scopus

出版者・発行元：ACS Nano  

Enzyme-mimicking confined catalysis has attracted great interest in heterogeneous catalytic systems that can regulate the geometric or electronic structure of the active site and improve its performance. Herein, a liquid-assisted chemical vapor deposition (LCVD) strategy is proposed to simultaneously confine the single-atom Ru sites onto sidewalls and Janus Ni/NiO nanoparticles (NPs) at the apical nanocavities to thoroughly energize the N-doped carbon nanotube arrays (denoted as Ni/NiO@Ru-NC). The bifunctional Ni/NiO@Ru-NC electrocatalyst exhibits overpotentials of 88 and 261 mV for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) at 100 mA cm-2 in alkaline solution, respectively, all ranking the top tier among the carbon-supported metal-based electrocatalysts. Moreover, once integrated into an anion-exchange membrane water electrolysis (AEMWE) system, Ni/NiO@Ru-NC can act as an efficient and robust bifunctional electrocatalyst to operate stably for 50 h under 500 mA cm-2. Theoretical calculations and experimental exploration demonstrate that the confinement of Ru single atoms and Janus Ni/NiO NPs can regulate the electron distribution with strong orbital couplings to activate the NC nanotube from sidewall to top, thus boosting overall water splitting.

DOI： 10.1021/acsnano.3c11705

Scopus

出版者・発行元：Advanced Functional Materials  

Dion–Jacobson-type 2D halide perovskites (DJPs) present an ideal alternative to their 3D counterparts due to their superior stability and exceptional optoelectronic properties. Despite the numerous DJPs proposed in recent years, the impact of different spacer cations on DJPs remains unclear. This understanding is crucial for researchers to select suitable materials and is an urgent requirement for the development of higher-performance DJPs-based devices. In this study, the influence of the chain-like spacer cations with varying branch chains and chain lengths is thoroughly examined using both theoretical and experimental methods. The findings reveal that spacer cations with high polarity components along the main chain direction enhance the stability and photoelectric properties of DJPs. Additionally, it is found that the chain length of the spacer cation plays a critical role. Chain lengths that are too long or too short can detrimentally affect the photoelectric performance and stability of DJPs. These insights will guide researchers in selecting suitable spacer cations and in innovating new types of DJPs.

DOI： 10.1002/adfm.202409987

Scopus

出版者・発行元：Advanced Functional Materials  

Quasi-2D perovskite thin films hold great promise for creating highly efficient and stable optoelectronic devices. Regulating the intermediate phase during crystallization is crucial for determining film quality, directly impacting device performance. In this study, the bifunctional molecule L-carnitine is introduced into the quasi-2D precursor solution to modulate the intermediate phase during crystallization. The results demonstrate that the strong coordination between L-carnitine and PbI2 effectively impedes the combination of PbI2 and dimethyl sulfoxide (DMSO), preventing the formation of the PbI2·DMSO intermediate phase. This elimination of the intermediate phase mitigates the potential hazards associated with DMSO escape during subsequent annealing, significantly enhancing film quality. Furthermore, the bifunctional groups in L-carnitine interact with the perovskite, effectively passivating film defects and enhancing thermal and illumination stability. As a result, the L-carnitine-modified quasi-2D perovskite photodetector exhibits outstanding performance, with a responsivity of 2724 mA W−1 and a detectivity of 9.10 × 1010 Jones. This research proposes a novel strategy to regulate intermediate phases during crystallization and passivate defects synergistically, enabling the production of high-quality perovskite films and high-performance perovskite optoelectronic devices.

DOI： 10.1002/adfm.202412965

Scopus

出版者・発行元：Advanced Materials  

As a true 1D system, group-VIA tellurium (Te) is composed of van der Waals bonded molecular chains within a triangular crystal lattice. This unique crystal structure endows Te with many intriguing properties, including electronic, optoelectronic, thermoelectric, piezoelectric, chirality, and topological properties. In addition, the bandgap of Te exhibits thickness dependence, ranging from 0.31 eV in bulk to 1.04 eV in the monolayer limit. These diverse properties make Te suitable for a wide range of applications, addressing both established and emerging challenges. This review begins with an elaboration of the crystal structures and fundamental properties of Te, followed by a detailed discussion of its various synthesis methods, which primarily include solution phase, and chemical and physical vapor deposition technologies. These methods form the foundation for designing Te-centered devices. Then the device applications enabled by Te nanostructures are introduced, with an emphasis on electronics, optoelectronics, sensors, and large-scale circuits. Additionally, performance optimization strategies are discussed for Te-based field-effect transistors. Finally, insights into future research directions and the challenges that lie ahead in this field are shared.

DOI： 10.1002/adma.202408969

Scopus

出版者・発行元：Small  

As demand for higher integration density and smaller devices grows, silicon-based complementary metal-oxide-semiconductor (CMOS) devices will soon reach their ultimate limits. 2D transition metal dichalcogenides (TMDs) semiconductors, known for excellent electrical performance and stable atomic structure, are seen as promising materials for future integrated circuits. However, controlled and reliable doping of 2D TMDs, a key step for creating homogeneous CMOS logic components, remains a challenge. In this study, a continuous electrical polarity modulation of monolayer WS2 from intrinsic n-type to ambipolar, then to p-type, and ultimately to a quasi-metallic state is achieved simply by introducing controllable amounts of vanadium (V) atoms into the WS2 lattice as p-type dopants during chemical vapor deposition (CVD). The achievement of purely p-type field-effect transistors (FETs) is particularly noteworthy based on the 4.7 at% V-doped monolayer WS2, demonstrating a remarkable on/off current ratio of 105. Expanding on this triumph, the first initial prototype of ultrathin homogeneous CMOS inverters based on monolayer WS2 is being constructed. These outcomes validate the feasibility of constructing homogeneous CMOS devices through the atomic doping process of 2D materials, marking a significant milestone for the future development of integrated circuits.

DOI： 10.1002/smll.202402217

Scopus

出版者・発行元：Small  

The strategic integration of low-dimensional InAs-based materials and emerging van der Waals systems is advancing in various scientific fields, including electronics, optics, and magnetics. With their unique properties, these InAs-based van der Waals materials and devices promise further miniaturization of semiconductor devices in line with Moore's Law. However, progress in this area lags behind other 2D materials like graphene and boron nitride. Challenges include synthesizing pure crystalline phase InAs nanostructures and single-atomic-layer 2D InAs films, both vital for advanced van der Waals heterostructures. Also, diverse surface state effects on InAs-based van der Waals devices complicate their performance evaluation. This review discusses the experimental advances in the van der Waals epitaxy of InAs-based materials and the working principles of InAs-based van der Waals devices. Theoretical achievements in understanding and guiding the design of InAs-based van der Waals systems are highlighted. Focusing on advancing novel selective area growth and remote epitaxy, exploring multi-functional applications, and incorporating deep learning into first-principles calculations are proposed. These initiatives aim to overcome existing bottlenecks and accelerate transformative advancements in integrating InAs and van der Waals heterostructures.

DOI： 10.1002/smll.202403129

Scopus

出版者・発行元：Small  

Aqueous zinc metal batteries are regarded as a promising energy storage solution for a green and sustainable society in the future. However, the practical application of metallic zinc anode is plagued by the thermodynamic instability issue of water molecules in conventional electrolytes, which leads to severe dendrite growth and side reactions. In this work, an ultra-thin and high areal capacity metallic zinc anode is achieved by utilizing crystalline water with a stable stoichiometric ratio. Unlike conventional electrolytes, the designed electrolyte can effectively suppress the reactivity of water molecules and diminish the detrimental corrosion on the metallic zinc anode, while preserving the inherent advantages of water molecules, including great kinetic performance in electrolytes and H+ capacity contribution in cathodes. Based on the comprehensive performance of the designed electrolyte, the 10 µm Zn||10 µm Zn symmetric cell stably ran for 1000 h at the current density of 1 mA cm−2, and the areal capacity of 1 mAh cm−2, whose depth-of-discharge is over 17.1%. The electrochemical performance of the 10 µm Zn||9.3 mg cm−2 polyaniline (PANI) full-cell demonstrates the feasibility of the designed electrolyte. This work provides a crucial understanding of balancing activity of water molecules in aqueous zinc metal batteries.

DOI： 10.1002/smll.202404865

Scopus

出版者・発行元：Nano Energy  

Recent advances in the use of organic-inorganic hybrid perovskites have been investigated in a variety of applications, such as solar cells, photodetectors, light-emitting devices, and lasers, because of their outstanding semiconductor properties. Furthermore, the perovskite structure can host extrinsic elements, making it a promising candidate for battery applications. Previous studies have shown that organic-inorganic hybrid perovskites can be suitable anode materials for both lithium- and sodium-ion batteries. However, multivalent rechargeable batteries with perovskite materials have not yet been realized. Herein, we studied the electrochemical performance of three-dimensional (CH3NH3PbI3 (MAPbI3) and long-chain alkylammonium (C4H9NH3)2(CH3NH3)3Pb4I13 ((iBA)2(MA)3Pb4I13) thin films as electrode materials for rechargeable Al-ion batteries. Our results showed that (iBA)2(MA)3Pb4I13 presented a specific capacity of 257 mAh g–1 at a current density of 0.1 A g−1 and delivered 108 mAh g–1 after 250 cycles at a current density of 0.3 A g−1 with a retention of as high as 91 %, demonstrating a crucial role of isobutyl amine (C4H9NH3) due to the unique hydrogen-bonding interaction of isobutyl amine that hinders the shuttle effect of polyiodide. The results open a new direction for the use of organic–inorganic hybrid perovskites for new secondary aluminum ion batteries.

DOI： 10.1016/j.nanoen.2023.108273

Scopus

出版者・発行元：Materials Today  

Electrochemical nitrate reduction reaction (NO3RR) is a promising alternative technique for NH3 generation toward the energy-consuming Haber-Bosch process. Nevertheless, it remains hindered by the competitive hydrogen evolution reaction (HER). Herein, the piezoelectric effect of electron-rich BaTiO3 with oxygen vacancies is introduced to promote NO3RR performance. Combining with metal particles (Ru, Pd and Pt), the catalyst achieves a maximal Faradaic efficiency of 95.3% and NH3 yield rate of 6.87 mg h−1 mgcat.−1. Upon piezoelectricity, the interface between metal nanoparticles and BaTiO3 is effectively modulated from Schottky contact to ohmic contact, which leads to unobstructed electron transfer. Abundant hydrogen radicals (·H) can be then produced from the collision between plentiful electrons and polar water molecules adsorbed on the polar surface. Such ·H can significantly facilitate the hydrogenation of reaction intermediates in NO3RR. Meanwhile, this process suppresses the Volmer-Heyrovsky step, therefore inhibiting the HER within a wide range of external potential. This work suggests a new strategy for promoting the performance of multi-electron-involved catalytic reactions.

DOI： 10.1016/j.mattod.2023.03.011

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adfm.202302866

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/d2tc05289j

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/smtd.202201567

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adma.202211598

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1007/s12274-021-3907-9

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adpr.202200166

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1021/acs.nanolett.2c03612

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.jmst.2022.05.063

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/lpor.202200486

出版者・発行元：Advanced Functional Materials  

The visual system, one of the most crucial units of the human perception system, combines the functions of multi-wavelength signal detection and data processing. Herein, the large-scale artificial synaptic device arrays based on the organic molecule-nanowire heterojunctions with tunable photoconductivity are proposed and demonstrated. The organic thin films of p-type 2,7-dioctyl[1]benzothieno[3,2-b][1] benzothiophene (C8-BTBT) or n-type phenyl-C61-butyric acid methyl ester (PC61BM) are used to wrap the InGaAs nanowire parallel arrays to configure two different type-I heterojunctions, respectively. Due to the difference in carrier injection, persistent negative photoconductivity (NPC) or positive photoconductivity (PPC) are achieved in these heterojunctions. The irradiation with different wavelengths (solar-blind to visible ranges) can stimulate the heterojunction devices, effectively mimicking the synaptic behaviors with two different photoconductivities. The long-term and multi-state light memory are also realized through synergistic photoelectric modulation. Notably, the arrays with different photoconductivities are adopted to build the hardware kernel for the visual system. Due to the tunable photoconductivity and response to multiple wavelengths, the recognition rate of neural networks can reach 100% with lower complexity and power consumption. Evidently, these photosynaptic devices are illustrated with retina-like behaviors and capabilities for large-area integration, which reveals their promising potential for artificial visual systems.

DOI： 10.1002/adfm.202209091

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.apcatb.2022.121995

出版者・発行元：Nano Energy  

Development of highly active and durable electrocatalysts for acidic oxygen evolution reaction (OER) remains an unresolved grand challenge. Here, we reported the amorphous IrOx/CeO2 nanowires as highly active and acid-stable OER catalysts through a facile electro-spinning/calcination approach. The amorphous catalysts delivered a high mass activity of 167 A gIr−1 at 1.51 V, a low overpotential of 220 mV at 10 mA cm−2, and a stable performance for 300 h of continuous operation in acid. As revealed by complementary experimental and theoretical calculation results, the intimate nanoscale feature of IrOx/CeO2 creates abundant binary interfaces, at which CeO2 as an electron buffer regulates the adsorption of oxygen intermediates, lowers the activation barrier of OER, and suppresses the over-oxidation and dissolution of Ir, thereby significantly enhancing the OER activity and stability. This work provides a new strategy for designing highly active and acid-resistant OER catalysts.

DOI： 10.1016/j.nanoen.2022.107960

Scopus

出版者・発行元：Light: Science and Applications  

With luminescent concentrators, the high quantum yield luminescence emitted by embedded chromophores, featuring a broad absorption spectrum, can be well-tuned to match the peak response of integrated photodetectors. This integration can substantially enhance the device photoresponse all the way from deep UV to near-IR. [Figure not available: see fulltext.]

DOI： 10.1038/s41377-022-00819-3

Scopus

出版者・発行元：Advanced Electronic Materials  

Controllable self-catalyzed growth of semiconductor nanowires (NWs) is of great importance, particularly to avoid impurities coming from foreign catalysts to deteriorate the NW properties. Although this catalyst-free NW growth has many obvious advantages, there are very limited works focused on all-inorganic CsPbBr3 perovskite NWs, which is one of the recent champion materials for electronics and optoelectronics. Here, a direct self-catalyzed synthesis of freestanding CsPbBr3 NWs via vapor–liquid–solid growth mechanism by chemical vapor deposition is developed. Notably, mainipulation of the substrate surface roughness is the key enabling parameter for the self-catalyzed NW growth here. It is revealed that the surface energy of substrates, modulated by its surface roughness, is found to effectively mediate the self-catalytic growth of CsPbBr3 NWs. When configured into photodetectors, the intrinsic p-type CsPbBr3 NWs exhibit good optoelectronic performance with a photoresponivity of ≈2000 A W−1, a detectivity of ≈2.57 × 1012 Jones, and a fast response down to 362 µs. All these results evidently indicate the technological potential of this self-catalyzed synthesizing route for other high-quality all-inorganic perovskite NWs.

DOI： 10.1002/aelm.202200727

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1088/1674-4926/43/11/112201

出版者・発行元：Advanced Energy and Sustainability Research  

Two-dimensional (2D) heterostructures, typically integrating two or more different components with well-defined interfaces, have shown great prospects in energy storage and conversion applications owing to their unique structural merits and synergistic interface effects. This review provides a comprehensive overview of the rational construction of 2D heterostructures pertaining to electrocatalytic water-splitting applications. The unique emphasis is given to the state-of-the-art progress on synthesized strategies of various well-organized 2D heterostructures. Moreover, the review offers insights into 2D heterostructures in electrocatalytic water splitting from the viewpoint of the structure–activity relationship using progressive examples. Finally, this review concludes with the potential challenges and prospects in the field, which may provide a guideline for developing more efficient 2D heterostructures to incentivize commercial implementation in this exciting research field.

DOI： 10.1002/aesr.202200059

Scopus

出版者・発行元：Advanced Optical Materials  

All-inorganic halide perovskites (AIHPs) are promising photovoltaic materials that have been extensively studied in the last decade. In addition, lead-free AIHPs are preferred because of their non-toxic and environmentally friendly nature. However, the quality of AIHPs fabricated by conventional solution processing methods is usually unsatisfactory, which leads to poor photoelectric performance. Herein, a facile polydimethylsiloxane-assisted slow evaporation method that can be readily used to synthesize high-quality AIHP microcrystals (MCs) (CsPbBr3, Cs2AgBiBr6, and L-Cs3Sb2I9) is demonstrated. The photodetection properties of the synthesized AIHP MCs and their spin-coated thin-film counterparts are thoroughly studied and compared. Owing to their superior crystallinity, AIHP MCs show better photoelectric performance than spin-coated films. The responsivity of the CsPbBr3 microcrystal photodetectors is ≈590 000 mA W−1. This work proposes a universal solution-processing method for the successful fabrication of high-quality all-inorganic lead-based (CsPbBr3), lead-free (L-Cs3Sb2I9), and double (Cs2AgBiBr6) perovskites, which can overcome the bottleneck in the development of halide perovskites and promote their applications.

DOI： 10.1002/adom.202201127

Scopus

出版者・発行元：Nano Energy  

Rational design of bifunctional two-dimensional (2D) heterostructures with excellent activity and durability remains a great challenge for electrocatalytic water splitting. Herein, we propose a topochemical domain engineering to realize 2D mosaic heterostructures with ultrafine phosphide nanodomains highly dispersed on the surface of Ru doped CoMoO4 nanosheets (denoted as Ru-CMOP), which are vertically interconnected on the conductive skeleton assembling a 3D array structure. The as-prepared Ru-CMOP electrocatalyst exhibits excellent activity and long-term stability with the overpotentials of 114 and 286 mV at 100 mA cm−2 for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in 1.0 M KOH solution, respectively, outperforming most reported metal phosphide-based bifunctional heterostructures. Moreover, an assembled electrolyzer using the Ru-CMOP as anode and cathode simultaneously delivers cell voltages of 1.697 V and 1.828 V to achieve 100 mA cm−2 and 500 mA cm−2, respectively, with outstanding durability at 250 mA cm−2 for 120 h. Density functional theory calculations and experimental results indicate that the strongly coupled heterointerfaces with built-in electric field can facilitate electron transfer while multi-porous nanosheet arrays contribute to active sites exposure and mass/gas transport, thereby synergistically accelerating the reaction kinetics. Additionally, combining with a commercial silicon photovoltaic solar cell, the electrolyzer can be efficiently and robustly established, demonstrating the great potential for practical photovoltaic-electrolysis applications.

DOI： 10.1016/j.nanoen.2022.107566

Scopus

出版者・発行元：ACS Nano  

The continuous downscaling of semiconducting channels in transistors has driven the development of modern electronics. However, with the component transistors becoming smaller and denser on a single chip, the continued downscaling progress has touched the physical limits. In this Perspective, we suggest that the emerging one-dimensional (1D) material system involving inorganic atomic chains (ACs) that are packed by van der Waals (vdW) interactions may tackle this issue. Stemming from their 1D crystal structures and naturally terminated surfaces, 1D ACs could potentially shrink transistors to atomic-scale diameters. Also, we argue that 1D ACs with few-atom widths allow us to revisit 1D materials and uncover physical properties distinct from conventional materials. These ultrathin 1D AC materials demand substantive attention. They may bring opportunities to develop ultimate-scaled AC-based electronic, optoelectronic, thermoelectric, spintronic, memory devices, etc.

DOI： 10.1021/acsnano.2c06359

Scopus

出版者・発行元：Advanced Materials Interfaces  

Due to the tunable bandgaps, high quantum efficiency, and long carrier diffusion length, perovskites have attracted significant attention as active materials for solar cells, nanoscale lasers, photodetectors, and light-emitting diodes. Herein, laser-induced dual-wavelength emissions from the CsPbBr3xI3(1–x) perovskite alloy microcrystals are reported. Under a 375 nm laser illumination, the micro-photoluminescence (PL) emission spectra of these microcrystals exhibit two emission bands at 570 and 690 nm with gradually increased and decreased PL intensity, respectively. Moreover, the time-dependent emission wavelength of the two emission bands almost has no changes, while the PL intensity of both emission bands shows periodic fluctuations with the on–off switching of excitation light. This dual-wavelength emission phenomenon suggests that phase segregation occurs in these perovskite microcrystals during laser illumination. These results would provide valuable design guidelines for perovskites-based tunable nanophotonic devices and multi-color displays.

DOI： 10.1002/admi.202200680

Scopus

出版者・発行元：Advanced Functional Materials  

Design of efficient and robust electrocatalysts for hydrogen evolution reaction (HER) under all pH conditions has attracted significant attention. In particular, it is still a considerable challenge since the HER kinetics of Pt in alkaline solutions is about two to three orders of magnitude lower than that in acidic conditions. Herein, a heterogeneous yolk–shell nanostructure with Rh nanoparticles embedded in S, N co-doped carbon nanospheres prepared by a facile self-template method is reported. The optimized electrocatalyst can achieve an extremely small overpotential of 13.5 mV at 10 mA cm-2, low Tafel slope of 25.5 mV dec-1, high turnover frequency of 0.143 s-1 (at −75 mV vs. reversible hydrogen electrode), and long-term durability for 10 h, which is the record-high alkaline HER activity among the ever-reported noble metal based catalysts. These striking performances are ascribed to the optimized electronic structure and unique heterogeneous yolk–shell nanostructure. More importantly, it is also demonstrated that the obtained electrocatalyst exhibits superior activities in all pH range, which is better than commercial Pt/C and Rh/C catalysts. This work proves that Rh-based nanomaterials are promising superior electrocatalysts in a wide pH range and nanostructure design is a powerful tool to increase the mass/electron transfer during reaction.

DOI： 10.1002/adfm.202206006

Scopus

出版者・発行元：InfoMat  

Developing new methodologies to produce clean and renewable energy resources is pivotal for carbon-neutral initiatives. Hydrogen (H2) is considered as an ideal energy resource due to its nontoxic, pollution-free, high utilization rate, and high calorific combustion value. Electrolysis of water driven by the electricity generated from renewable and clean energy sources (e.g., solar energy, wind energy) to produce hydrogen attracts great efforts for hydrogen production with high purity. Recently, the breakthrough of the catalyst activity limit for the hydrogen evolution reaction (HER) catalysts has received extensive attention. Comparatively, fewer reviews have focused on the long-term stability of HER catalysts, which is indeed decisive for large-scale electrolytic industrialization. Therefore, a systematic summary concentrated on the durability of HER electrocatalysts would provide a fundamental understanding of the electrocatalytic performance for practical applications and offer new opportunities for the rational design of the highly performed HER electrocatalysts. This review summarizes the research progress toward the HER stability of precious metals, transition metals, and metal-free electrocatalysts in the past few years. It discusses the challenges in the stability of HER electrocatalysts and the future perspectives. We anticipate that it would provide a valuable basis for designing robust HER electrocatalysts. (Figure presented.).

DOI： 10.1002/inf2.12357

Scopus

出版者・発行元：ACS Nano  

Wavelength-tunable semiconductor nanolasers have attracted tremendous attention for their tunable emissions and robust stability, bringing possibilities for various applications, including nanophotonic circuits, solid-state white-light sources, wavelength-converted devices, and on-chip optical communications. Here, we report on the demonstration of broadband-tunable, single-mode nanolasers based on high-quality alloyed single crystalline CdS1-xSex(x = 0-1) nanotripods with well-formed facets fabricated using a conventional CVD approach. Microstructural characterization and optical investigations reveal that these structures are crystalline with composition-tunable CdS1-xSexalloys. Microphotoluminescence spectra and mapping of these nanotripods exhibit emissions with continuous wavelengths from 509 to 712 nm, further demonstrating that the CdS1-xSexalloys have tunable bandgaps due to the composition gradient. Additionally, under a pulse laser illumination, room-temperature single-mode lasing is clearly observed from these nanotripods cavities, which shows almost identical emission lines with a high-quality factor of ∼1231. More importantly, wavelength continuously tunable nanolasers from 520 to 738 nm are successfully constructed using these bandgap gradient nanotripods. The capability to fabricate high-quality tunable nanolasers represents a significant step toward high-integration optical circuits and photonics communications.

DOI： 10.1021/acsnano.2c04632

Scopus

出版者・発行元：Advanced Materials Interfaces  

Although the recent advance of ultra-thin 2D nanosheets for hydrogen evolution reaction (HER) is remarkable, there are still substantial challenges to reliably control their physioelectric and electrochemical properties to employ as highly-efficient electrocatalysts. Herein, based on complementary theoretical and experimental studies, the d-band center position of ultra-thin 2D Ni5P4 nanosheets can be manipulated by simple heteroatom doping. Interestingly, the Fe-doped nanosheets yield the lowest d-band center position, but they do not display the optimal Gibbs free energy of adsorbed H atoms due to the imbalance of adsorption and desorption of adsorbed H atoms. With the proper Co doping (i.e., 20%), the nanosheets exhibit the best electrocatalytic performance along with an excellent stability. The overpotential is only 100.5 mV at 10 mA cm−2 with a Tafel slope of 65.8 mV dec−1, which is superior than those of Fe-doped, Cu-doped, and pristine Ni5P4 nanosheets. Ultraviolet photoelectron and X-ray photoelectron spectroscopy further verify the downshift of d-band centers of nanosheets by optimal doping, illustrating that Ni with the lower binding energy mainly dominates the active sites. All these results provide a valuable design scheme of dopants to control the d-band center position of nanosheets for next-generation highly-efficient HER electrocatalysts.

DOI： 10.1002/admi.202200739

Scopus

出版者・発行元：ACS Nano  

The incapability of modulating the photoresponse of assembled heterostructure devices has remained a challenge for the development of optoelectronics with multifunctionality. Here, a gate-tunable and anti-ambipolar phototransistor is reported based on 1D GaAsSb nanowire/2D MoS2 nanoflake mixed-dimensional van der Waals heterojunctions. The resulting heterojunction shows apparently asymmetric control over the anti-ambipolar transfer characteristics, possessing potential to implement electronic functions in logic circuits. Meanwhile, such an anti-ambipolar device allows the synchronous adjustment of band slope and depletion regions by gating in both components, thereby giving rise to the gate-tunability of the photoresponse. Coupled with the synergistic effect of the materials in different dimensionality, the hybrid heterojunction can be readily modulated by the external gate to achieve a high-performance photodetector exhibiting a large on/off current ratio of 4 × 104, fast response of 50 μs, and high detectivity of 1.64 × 1011 Jones. Due to the formation of type-II band alignment and strong interfacial coupling, a prominent photovoltaic response is explored in the heterojunction as well. Finally, a visible image sensor based on this hybrid device is demonstrated with good imaging capability, suggesting the promising application prospect in future optoelectronic systems.

DOI： 10.1021/acsnano.2c03673

Scopus

出版者・発行元：Nano Energy  

Electrochemical conversion of nitrate to ammonia is widely considered a “two birds with one stone” approach to alleviate the nitrate pollution in water and simultaneously to generate the valuable green NH3 fuels. However, it remains challenging due to the lack of efficient electrocatalysts for practical utilization. Herein, we investigate the synergistic effect between asymmetric Cu-Ov-W sites (Ov represents oxygen vacancy) and adjacent Mo clusters in tuning the local electronic environment around active sites of catalysts for substantially enhanced nitrate reduction. The dynamic balance between the adsorption and desorption of O in NO3- caused by asymmetric Ov and the promoted protonation process due to Mo clusters are responsible for boosting the entire process. Such synergistic effect modulates the local electronic environment for binding the reaction intermediates and dramatically facilitates the intermediate formation in rate-determining steps (*NO→*NOH and *NOH→*N), leading to the high NH3 Faradaic efficiency and yield rate of 94.60% and 5.84 mg h−1 mgcat.−1 at − 0.7 V vs. RHE, respectively.

DOI： 10.1016/j.nanoen.2022.107338

Scopus

出版者・発行元：Chemical Engineering Journal  

Designing highly efficient and stable electrocatalysts for hydrogen evolution reaction (HER), particularly in seawater, still remains a challenging task. Herein, the unique heterostructures composed of 1D NiMo cores and 2D C3N5 shells (NiMo@C3N5) are rationally designed and demonstrated as the robust HER catalysts in both alkaline electrolytes and natural seawater, where the carbon-based shell can effectively protect the catalyst core from seawater poisoning. Based on the experimental investigation and density functional theory calculation, multiple electronic transmission channels were found to establish at the interface between NiMo cores and C3N5 shells, thus providing efficiently optimized HER pathways to achieve minimized overpotential with a reduced energy barrier of the rate-determining step. More importantly, the NiMo@C3N5 hybrids exhibit stable HER performance with a high Faradaic efficiency of 94.8% in seawater, which is superior to that of commercial Pt/C. All these results can evidently highlight a feasible strategy to develop high-performance HER electrocatalysts via interface engineering.

DOI： 10.1016/j.cej.2022.135379

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adfm.202203003

記述言語：英語  

Halide perovskites have attracted significant recent attention due to their remarkable photoelectric properties; however, the poor structural and moisture stability limit their use for practical utilization. Interestingly, binary halides, such as BiI3 and PbI2, are the typical constituents of halide perovskites, where they do not only have the similar outstanding properties of perovskites but also the superior stability. Herein, the synthesis of layered BiI3 and PbI2 microcrystals by simple drop-casting is investigated and their enhanced photoelectric performance compared to the thin-film counterparts obtained by conventional spin-coating is demonstrated. For the formation of high-quality layered microcrystals, the keys are adopting glycol as a green solvent and appropriate temperature during processing. Once configured into photodetectors, the BiI3 and PbI2 microcrystals exhibit a higher photocurrent, on/off current ratio, responsivity, and other performance parameters than their thin-film devices. These improved performances of microcrystals can be attributed to their superior crystallinity, thanks to the excellent solvent properties of glycol and the optimal growth temperature chosen. This work proposes a more simple and effective solution processing technique to fabricate layered binary halides with higher quality than the conventional spin-coating method, enabling the further development of halides-based optoelectronic devices.

CiNii Research

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1021/acsnano.2c01455

出版者・発行元：APL Materials  

CsPb2Br5/CsPbBr3 composite systems have received considerable attention among numerous lead halide perovskite materials due to their significantly enhanced photoluminescence intensity and stability against moisture. However, the luminescence mechanism of CsPb2Br5 based materials remains controversial, which significantly hinders the further material design and utilization for optoelectronic devices. In this work, to deconvolute their luminescent mechanisms, high-quality CsPb2Br5 crystals without any undesired by-products and impurities have been first prepared by a microwave-assisted synthesis method. The luminescence-inactive characteristics of the material are then confirmed by the steady-state absorption, photoluminescence, transient absorption spectra, and time-resolved terahertz spectroscopy. The prepared CsPb2Br5 crystals exhibit excellent crystallinity and enhanced thermal stability, particularly that they can maintain their crystalline structures in polar organic solvents. By simply manipulating the ratios of different precursor materials, it is witnessed that the green emission comes from the CsPbBr3 adhered, nucleated, and grown on the CsPb2Br5 crystals. Ultrafast transient absorption measurements in visible and terahertz spectral regions reveal that with the help of phonon scattering-assisted hopping at interfacial states, intersystem crossing dominates the electron transfer process in the composite crystals. As a result, the CsPb2Br5 and CsPbBr3 interact extensively with each other. Meanwhile, the Auger recombination rate and the defect-related non-radiative process are suppressed in the composite crystals, thereby enhancing the fluorescence of composite crystals. This work has not only deconvoluted the controversial and unclear luminescent mechanisms of CsPb2Br5 materials but also established a pathway to design and enhance the fluorescence of materials for technological applications.

DOI： 10.1063/5.0083022

Scopus

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1038/s41467-022-28380-y

記述言語：英語   掲載種別：研究論文（学術雑誌）  

Surface self-reconstruction processes in alkaline hydrogen evolution reaction (HER), especially regarding the explicit structure–activity relationships, remain elusive. Here, we first design a hierarchical Co@NCNT/CoMoOx precatalyst constituted by defective CoMoOx nanosheets grafted with flexible Co@NCNT arrays, followed by a delicate anodic treatment for fast dissolution balance. Benefiting from the multi-level Co@NCNT arrays as a stable micro-environment, the resultant Co@NCNT/CoMoyOx displays excellent electrocatalytic activity with a low overpotential of 195 mV at −100 mA cm−2 and stable 600 h operation for the HER in alkaline media, including natural seawater, which is better than most reported carbon/transition metal-based catalysts. In situ Raman analyses disclose a local high-resolution self-reconstruction evolution of localized Mo species at controllable negative potentials. Density functional theory calculations further demonstrate that the ultimate Mo–Mo surface state accelerates reaction kinetics to promote H2 generation in alkaline media. Our findings provide a unique insight into the mechanism of the structural evolution in the alkaline HER process to pave a new avenue guiding the design of durable and efficient catalysts.

DOI： 10.1039/d1ta09010k

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/anie.202111826

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.mattod.2021.09.023

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1007/s12274-021-3907-9

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/anie.202111826

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1007/s40843-021-1900-7

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adfm.202111970

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.nanoen.2021.106778

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.apmt.2021.101234

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.nanoen.2021.106654

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.202101523

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.mtener.2021.100883

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.202101289

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/qute.202100072

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/smll.202102323

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1021/acsami.1c07839

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/smll.202100442

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1007/s12274-021-3351-x

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1007/s12274-021-3332-0

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/d1tc00077b

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/smll.202006860

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.202101289

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/d0ta11287a

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.202001991

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/D0NR06788A

記述言語：英語   掲載種別：研究論文（学術雑誌）  

Rapid development of artificial intelligence techniques ignites the emerging demand on accurate perception
and understanding of optical signals from external environments via brain-like visual systems. Here, enabled by
quasi–two-dimensional electron gases (quasi-2DEGs) in InGaO3(ZnO)3 superlattice nanowires (NWs), an artificial
visual system was built to mimic the human ones. This system is based on an unreported device concept
combining coexistence of oxygen adsorption-desorption kinetics on NW surface and strong carrier quantumconfinement effects in superlattice core, to resemble the biological Ca2+ ion flux and neurotransmitter release
dynamics. Given outstanding mobility and sensitivity of superlattice NWs, an ultralow energy consumption down
to subfemtojoule per synaptic event is realized in quasi-2DEG synapses, which rivals that of biological synapses
and now available synapse-inspired electronics. A flexible quasi-2DEG artificial visual system is demonstrated to
simultaneously perform high-performance light detection, brain-like information processing, nonvolatile charge
retention, in situ multibit-level memory, orientation selectivity, and image memorizing.

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/d0tc04330c

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： org/10.1016/j.apmt.2020.100820

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1016/j.apsusc.2020.147977

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.202001201

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： org/10.1021/acsami.0c09651

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： org/10.1038/s43246-020-00063-5

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1039/d0nr03740k

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： org/10.1007/s12274-020-2983-6

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： org/10.1007/s12274-020-3003-6

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/aenm.202001059

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adom.201901626

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： 10.1002/adma.201907527

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   掲載種別：研究論文（学術雑誌）  

記述言語：英語   会議種別：口頭発表（一般）  

国名：デンマーク王国  

記述言語：英語