Construction of Supramolecular Structures to Manipulate Protons and Electrons toward Multiple Proton-Coupled Electron Transfer

2022 Fiscal Year Final Research Report

• Project/Area Number: 19H02732
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Review Section: Basic Section 34010:Inorganic/coordination chemistry-related
• Research Institution: Ritsumeikan University (2022); Tokyo Institute of Technology (2019-2021)
• Principal Investigator: Kuwata Shigeki 立命館大学, 生命科学部, 教授 (10292781)
• Project Period (FY): 2019-04-01 – 2023-03-31
• Keywords: 超分子化学 / プロトン共役電子移動 / ホスフィン / 窒素 / ヒドラジン / ルテニウム

Outline of Final Research Achievements

This study aimed at construction of supramolecular structures with accumulated proton-responsive sites and redox active metal centers to realize multiple proton-coupled electron transfer for reduction of dinitrogen and carbon dioxide. As the result, we obtained a series of dinuclear complexes, wherein metal fragments furnished with proton-responsive ligands are connected by a non-chelate diphosphine, 1,3-bis(diphenylphosphino)benzene. We also found that these complexes are effective in uptake and stabilization of diazene, a possible intermediate in nitrogen fixation, and in structural deformation triggered by anion exchange.

Free Research Field

錯体化学

Academic Significance and Societal Importance of the Research Achievements

化学的に不活性な窒素や二酸化炭素の還元、あるいは光合成における鍵反応の一つである水の酸化による電子の獲得は、地球上に豊富に存在する元素資源の有効活用や効率的なエネルギー変換に広く応用可能である。本研究の結果は、その実現のための基礎的な知見を与えるものである。また、超分子化学や、金属ー配位子協働作用に基づく均一系錯体触媒化学、生物無機化学など、関連分野の進展にもつながる成果である。