2023 Fiscal Year Final Research Report
Development of Reaction Concepts and Computational Methods for Chemical Reactions under Mechanochemical Stimulations
| Project/Area Number |
20H02685
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Review Section |
Basic Section 32010:Fundamental physical chemistry-related
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| Research Institution | Hokkaido University |
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Principal Investigator |
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| Project Period (FY) |
2020-04-01 – 2024-03-31
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| Keywords | メカノケミストリ / 反応原理 / 電子状態 / ポテンシャル面 |
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| Outline of Final Research Achievements |
We have developed a computational method that introduces externally induced forces and studied the principle of unique chemical reactions in mechanochemistry. Although there has been a rapid increase in the number of experimental reports showing that mechanical stimuli change the selectivity of chemical reactions, the theoretical understanding of this phenomenon has not yet progressed. The experimental results that depolymerization is prioritized over side chain hydrolysis in the hydrolysis of chitin using a ball mill, the computational results showing that the Fischer-Tropsch reaction activity can deviate from the BEP rule in response to external force stimulation of a high-index interface, and the computational results showing that a narrow reaction field changes selectivity in cyclopropanation reactions using a ball mill were reported. The reaction mechanism under mechanical stimuli was elucidated. The developed program is available on GitHub.
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| Free Research Field |
理論・計算化学
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| Academic Significance and Societal Importance of the Research Achievements |
力学的刺激による化学反応の促進は，局所加熱による反応性の向上と理解されている。これに対し，反応選択性の変化については単なる熱的な解釈を越えた理解が必要であった。このような実験事実に対して，様々な解釈が行われてきたが，これを裏付ける理論的研究が必要とされてきた。本研究では，力学的刺激を露わに導入した計算を行うことで，反応機構を提案することで提案されてきた解釈を理論的に検証し，力学的刺激による活性促進効果を予測した。また，使用した計算プログラムはGaussian16など各種の電子状態計算プログラムと接続して使用でき，研究成果のオープンリソース化による社会での活用が期待できる。
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