担当区分：筆頭著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Advanced Science  

Cell migration plays a crucial role in the dynamic processes that guide tissue development, regeneration, and repair; yet, developing cell culture platforms that allow control over cell migration in 3D space and time remains a challenge. Here, a strategy is presented using chemically-responsive granular hydrogels to enable dynamic control over 3D cell migration. Dynamic microgels are fabricated via hyaluronic acid crosslinked via reversible guest–host interactions between adamantane (guest) and β-cyclodextrin (host), which swell in the presence of a cytocompatible competitive guest molecule (adamantane carboxylic acid, Ad-COOH) and de-swell when Ad-COOH is removed. When formed into granular hydrogels, the addition of Ad-COOH results in a dynamic porous material with reduced microgel stiffness and increased pore size. Ad-COOH addition also results in the reduction of mesenchymal stromal cell (MSC) migration from embedded aggregates (spheroids); however, MSC migration returns when Ad-COOH is removed. Furthermore, suspension bioprinting of jammed spheroids into dynamic granular hydrogels results in 4D printed constructs with patterned cellular regions (e.g., lines, zigzags, spirals) where cellular egress is controlled over time through the presence of Ad-COOH to create distinct spatiotemporal cellular patterns. This platform offers precise, on-demand modulation of cell migration, enabling new opportunities to fabricate dynamic, complex engineered tissues.

DOI： 10.1002/advs.202512971

Web of Science

Scopus

PubMed

担当区分：筆頭著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Advanced Materials  

4D printing of hydrogels is an emerging technology used to fabricate shape-morphing soft materials that are responsive to external stimuli for use in soft robotics and biomedical applications. Soft materials are technically challenging to process with current 4D printing methods, which limits the design and actuation potential of printed structures. Here, a simple multi-material 4D printing technique is developed that combines dynamic temperature-responsive granular hydrogel inks based on hyaluronic acid, whose actuation is modulated via poly(N-isopropylacrylamide) crosslinker design, with granular suspension bath printing that provides structural support during and after the printing process. Granular hydrogels are easily extruded upon jamming due to their shear-thinning properties and their porous structure enables rapid actuation kinetics (i.e., seconds). Granular suspension baths support responsive ink deposition into complex patterns due to shear-yielding to fabricate multi-material objects that can be post-crosslinked to obtain anisotropic shape transformations. Dynamic actuation is explored by varying printing patterns and bath shapes, achieving complex shape transformations such as ‘S’-shaped and hemisphere structures. Furthermore, stepwise actuation is programmed into multi-material structures by using microgels with varied transition temperatures. Overall, this approach offers a simple method to fabricate programmable soft actuators with rapid kinetics and precise control over shape morphing.

DOI： 10.1002/adma.202410661

Web of Science

Scopus

担当区分：筆頭著者   記述言語：英語   掲載種別：研究論文（学術雑誌）   出版者・発行元：Springer Nature  

Synthetic composite hydrogels comprising supramolecular fibers and covalent polymers have attracted considerable attention because their properties are similar to biological connective tissues. However, an in-depth analysis of the network structures has not been performed. In this study, we discovered the composite network can be categorized into four distinct patterns regarding morphology and colocalization of the components using in situ, real-time confocal imaging. Time-lapse imaging of the network formation process reveals that the patterns are governed by two factors, the order of the network formation and the interactions between the two different fibers. Additionally, the imaging studies revealed a unique composite hydrogel undergoing dynamic network remodeling on the scale of a hundred micrometers to more than one millimeter. Such dynamic properties allow for fracture-induced artificial patterning of a network three dimensionally. This study introduces a valuable guideline to the design of hierarchical composite soft materials.

DOI： 10.1038/s41467-023-37412-0

Web of Science

Scopus

PubMed

CiNii Research

担当区分：筆頭著者   記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： https://doi.org/10.1021/jacs.1c09172

記述言語：英語   掲載種別：研究論文（学術雑誌）  

DOI： https://doi.org/10.1038/s41467-020-17698-0

In a living system, myriad biomolecules, such as proteins/peptides, nucleic acids, lipids, saccharides, and other metabolites, undergo self-sorting through specific interactions, resulting in a well-organized structure with sophisticated functions. Self-sorting is the key to realizing life-like emergent functions of synthetic peptide self-assembly. This chapter focuses on how to analyze, design, and control purely synthetic supramolecules achieving self-sorting systems.

DOI： 10.1002/9783527841264.ch7

Scopus

記述言語：英語   掲載種別：記事・総説・解説・論説等（学術雑誌）  

DOI： https://doi.org/10.1002/open.201900328Digital Object Identifier (DOI)