Embedding void into condensed soft matter
Nature does not like a void. We challenge to introduce a void into condensed phase of soft matter like gels. Recently our group has been developing methods to synthesize porous soft matter. We build up from RhMOPs – these pre-assembled building blocks are stable in solution, and withstand activation processes for gas sorption. They can be linked together using ditopic ligands, and through exploration of assembly pathways we have synthesized coordination polymer particles or self-supporting gels based on these RhMOPs. The porous units remain intact when solvent is removed from the lattice, allowing us to demonstrate that the materials store gas molecules, and opening the door to applications in mass transport and catalysis.
In ongoing work, we are using dynamic, physical methods to trigger the supramolecular assembly of the polymers and investigating how to control the precise spatial distribution of the materials.
凝縮相に空間を埋め込み、新しいソフトマテリアルをつくる
自然は「何もない状態（真空）」を嫌います。私達は、分子がいっぱい集まった状態である凝縮相にその真空（空間）を埋め込むことに挑戦しています。特に、ゲルのようなソフトマテリアルに空間を埋め込むことで、その凝縮相での物質輸送を制御することを目的としています。私達が得意とする金属錯体多面体（MOP）をポーラスモノマーとして、超分子重合により連結していくことで、非周期的、異方的、非対称的ネットワークへと集積化することで多様な特性を持つソフトマテリアルを作り上げます。MOPのもつ安定空間によりどのような形で集積させても空間特性は失われることはありません。
現在は、分子集合過程のメカニズム解明、様々な外場による集合状態制御、異方性の導入、そしてこれまでになかった新しいアプリケーションを目指して研究を行っています。
<Original papers>
“Self-assembly of metal–organic polyhedra into supramolecular polymers with intrinsic microporosity”
Nat. Commun. 2018, 9, 2506.
“A Coordinative Solubilizer Method to Fabricate Soft Porous Materials from Insoluble Metal-Organic Polyhedra”
Angew. Chem. Int. Ed. 2019, 58, 6347-6350.
(Chemrixv. Preprint. https://doi.org/10.26434/chemrxiv.7460618.v1)
“Understanding of the multiscale self-assembly of metal-organic polyhedra towards functionally graded porous gels”
Chem. Sci. 2019, 10, 10833.
(Chemrixv Preprint https://doi.org/10.26434/chemrxiv.9746177.v1)
“Understanding the role of linker flexibility in soft porous coordination polymers”
Mol. Syst. Des. Eng. 2020, 5, 284.
“Spatiotemporal Control of Supramolecular Polymerization and Gelation of Metal-Organic Polyhedra”
J. Am. Chem. Soc. 2021, 143, 3562–3570.
(Chemrxiv Preprint https://doi.org/10.26434/chemrxiv.13414646.v1)
“Porous Colloidal Hydrogels Formed by Coordination-Driven Self-Assembly of Charged Metal-Organic Polyhedra”
Chem. Asian J. 2021, 16, 1092-1100.
(Chemrxiv Preprint https://doi.org/10.26434/chemrxiv.13621220.v1)
“Multiscale Structural Control of Linked Metal-Organic Polyhedra Gel by Aging-Induced Linkage-Reorganization”
Chem. Sci. 2021, 12, 12556-12563.
(Chemrxiv Preprint https://doi.org/10.26434/chemrxiv.14481855.v1)