Artificial Enzymes base on Metalated Peptides

2019 Fiscal Year Final Research Report

• Project/Area Number: 17H03056
• Research Category: Grant-in-Aid for Scientific Research (B)
• Allocation Type: Single-year Grants
• Section: 一般
• Research Field: Synthetic chemistry
• Research Institution: Kyoto University
• Principal Investigator: Takaya HIkaru 京都大学, 化学研究所, 准教授 (50304035)
• Project Period (FY): 2017-04-01 – 2020-03-31
• Keywords: メタル化アミノ酸 / メタル化ペプチド / 金属配列制御 / 超分子錯体 / 人工酵素 / ペプチド中分子

Outline of Final Research Achievements

To investigate programmable metal array fabrication based on metalated amino acids and peptides, where various transition-metal complexes are covalently conjugated to the alpha-side chains of amino acids and peptides. We successfully achieved the syntheses of various transition-metal complex-bound glutamines and norvalines and their peptides and finally succeeded to find their unique catalysis and self-assembly properties with the applications of supramolecular aggregates of metalated amino acids in various organic transformations, such as the cyclization of alkynes and oxidations of alcohols and methoxybenzenes under aqueous conditions. A detailed research of the mechanism of the self-assembly process and the catalytic reactions have been also achieved to prove the effectiveness of metalated amino acid- and peptide-based metal array fabrication in the design of advanced smart materials based on bioorganometallic compounds.

Free Research Field

有機合成化学，有機金属化学，ペプチド科学，超分子科学，触媒科学

Academic Significance and Societal Importance of the Research Achievements

人類社会の物質生産基盤を担う様々な金属錯体触媒は，天然の酵素にない触媒機能を実現し，活性や耐久性は酵素のそれを遥かに凌駕する。しかし，多種多様な分子が高密度に混在する分子夾雑系における基質選択的反応については，酵素を凌駕する金属触媒は開発されていない。特に生体組織の様に夾雑な分子環境において，狙った基質から，必要な反応のみを引き起こし，所望の物質を生産できる人工酵素の開発は，有機合成化学における未踏領域の開拓につながる。本研究では木質夾雑系からリグニンを認識して精密分解できる人工酵素の開発に成功し，将来のSDGs達成に必要な未利用バイオマスからの触媒的な有用物質生産法に先鞭をつけた。