Rational Design of Artificial Metalloenzymes toward On-demand Functionalization of C-H Bond

2023 Fiscal Year Final Research Report

• Project/Area Number: 20H02755
• 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: Osaka University
• Principal Investigator: Oohora Koji 大阪大学, 大学院工学研究科, 准教授 (10631202)
• Project Period (FY): 2020-04-01 – 2023-03-31
• Keywords: 再構成ミオグロビン / 水酸化 / アミノ化 / 分子動力学計算 / 合理的設計

Outline of Final Research Achievements

In this study, we prepared an artificial metalloenzyme by substituting the active center heme in myoglobin, an oxygen-storing heme protein, with an artificial metal complex, and evaluated its catalytic activity. It was found to be useful for hydroxylation and amination of carbon-hydrogen bonds. Additionally, the introduction of mutations into the protein improved selectivity and activity. Notably, we established a method for designing artificial metalloenzymes using molecular dynamics calculations toward enantioselective C-H hydroxylation. In the future, this could indicate new directions for substance transformation reactions that contribute to the realization of a sustainable society.

Free Research Field

生物無機化学

Academic Significance and Societal Importance of the Research Achievements

有用な化学物質を生産するためには優れた触媒が必要になる。しかしながら現代の生産プロセスでは様々な多段階合成とともに毒性の高い化学物質を経由する場合が多い。本研究では、次世代型の物質変換として金属イオンを含むタンパク質から構成される人工金属酵素を合理的に設計し、その性能を評価した。将来的には、必要な化学反応を水中、常圧、常温の温和な条件で自在な物質生産を担うコア技術を確立するための知見を得ることができた。