2019 Fiscal Year Final Research Report
Development and application of computational methods toward controlling the active site of bio-catalysts
| Project Area | Precise Formation of a Catalyst Having a Specified Field for Use in Extremely Difficult Substrate Conversion Reactions |
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| Project/Area Number |
15H05805
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| Research Category |
Grant-in-Aid for Scientific Research on Innovative Areas (Research in a proposed research area)
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| Allocation Type | Single-year Grants |
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| Review Section |
Science and Engineering
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| Research Institution | Hokkaido University |
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Principal Investigator |
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| Project Period (FY) |
2015-06-29 – 2020-03-31
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| Keywords | 生体触媒 / 系間交差 / ポテンシャルエネルギー面 / 触媒設計 |
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| Outline of Final Research Achievements |
The purpose of this project is to contribute to the construction of a precisly controlled reaction field through the analysis of catalytic mechanisms in biocatalysts and similar reaction fields. We have developed a method for determining the reaction pathways through inter-system crossings in biocatalytic reactions, applied to the reaction mechanism of molecular adsorption in some metal complexes, and proposed guidelines for the ligand design. We also studied the inter-system crossing mechanisms of the catalytic reactions exhibited by myoglobin and, together with an experimental group, elucidated the origin of the catalytic activity exhibited by reconstituted myoglobin. In addition, we have collaborated on the analysis of reaction mechanisms through the collaborative researches and have clarified the physicochemical characteristics of a number of excellent catalytic systems. As a result, we were able to publish 38 original papers (including 13 in the area).
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| Free Research Field |
触媒理論化学
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| Academic Significance and Societal Importance of the Research Achievements |
精密制御反応場の代表的な例である生体触媒を理解する上で、活性中心を構成する鉄イオンなどの遷移金属元素が示す系間交差を含む反応の機構を明らかにする計算手法を開発する必要があった。この課題を解決し、ミオグロビンを含む幾つかの系に応用して反応機構を明らかにするとともに、配位子設計の指針を明らかにした。また、柔らかい生体分子に特徴的な構造ゆらぎの問題について、系間交差を経由する自由エネルギー面の計算を試み成果を得た。さらに、領域内の実験グループと協力し、二酸化炭素から高分子を合成する触媒反応をはじめとする多くの優れた触媒反応の反応機構を明らかにし、反応場の精密制御に貢献した。
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