Thermal and solvent effects on catalytic reactions over heterogeneous catalysis
| Project/Area Number |
15K06563
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| Research Category |
Grant-in-Aid for Scientific Research (C)
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| Allocation Type | Multi-year Fund |
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| Section | 一般 |
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| Research Field |
Catalyst/Resource chemical process
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| Research Institution | Hokkaido University |
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Principal Investigator |
NAKAYAMA AKIRA 北海道大学, 触媒科学研究所, 准教授 (10422007)
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| Research Collaborator |
Nisanth Nair N.
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| Project Period (FY) |
2015-04-01 – 2019-03-31
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| Project Status |
Completed (Fiscal Year 2018)
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| Budget Amount *help |
¥4,810,000 (Direct Cost: ¥3,700,000、Indirect Cost: ¥1,110,000)
Fiscal Year 2017: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2016: ¥1,430,000 (Direct Cost: ¥1,100,000、Indirect Cost: ¥330,000)
Fiscal Year 2015: ¥1,950,000 (Direct Cost: ¥1,500,000、Indirect Cost: ¥450,000)
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| Keywords | 第一原理計算 / 不均一系触媒 / 第一原理分子動力学法 / 酸化セリウム / 第一原理シミュレーション |
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| Outline of Final Research Achievements |
We aimed to understand the thermal and solvent effects on catalytic reactions occurring at the liquid/solid-oxide interface. First-principle MD simulations were performed to provide microscopic insights into structures and dynamics at the interface. We primarily focused on reactions over CeO2 and the following two topics were investigated. First one involved the formation of strong base site by unique adsorption of 2-cyanopyridine over CeO2. We identified the adsorption structure and reaction mechanism of hydromethoxylation of acrylonitrile in methanol were elucidated by the first-principle MD simulations. Second topic is related to the reaction mechanism of the direct synthesis of dimethyl carbonate from CO2 and methanol over CeO2. Based on the free energy profiles, we found that intermediate with an oxygen vacancy is formed during the reaction, and the stability of this intermediate is a key factor that makes CeO2 an efficient catalyst for this reaction.
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| Academic Significance and Societal Importance of the Research Achievements |
これまでの不均一触媒反応の理論計算の多くは、実験的に報告（仮定）された各中間種や活性種において、気相中または簡素にモデル化された溶媒（例えば連続体モデル）中での安定構造と遷移状態を求める研究がほとんどであった。本研究の特色は、これまでの静的なポテンシャル曲面の議論だけでは得ることのできなかった動的な反応機構（熱揺らぎやエントロピーの効果）に着目し、不均一系触媒における触媒反応のシンプルな原理抽出を目指し、さらにその揺らぎや溶媒効果を制御した合理的触媒設計への指針を与えるものである。
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Report
(5 results)
Research Products
(54 results)
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[Journal Article] Synthesis of yellow and red fluorescent 1,3a,6a-triazapentalenes and the theoretical investigation of their optical properties2015
Author(s)
Kosuke Namba, Ayumi Osawa, Akira Nakayama, Akane Mera, Fumi Tano, Yoshiro Chuman, Eri Sakuda, Tetsuya Taketsugu, Kazuyasu Sakaguchi, Noboru Kitamura, Keiji Tanino
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Journal Title
Chemical Science
Volume: 6
Issue: 2
Pages: 1083-1093
DOI
Related Report
Peer Reviewed / Open Access / Acknowledgement Compliant
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[Journal Article] Total Synthesis of Palau’amine2015
Author(s)
K. Namba, K. Takeuchi, Y. Kaihara, M. Oda, A. Nakayama, A. Nakayama, M. Yoshida, and K. Tanino
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Journal Title
Nature Communications
Volume: 6
Issue: 1
Pages: 8731-8731
DOI
NAID
Related Report
Peer Reviewed / Open Access / Int'l Joint Research / Acknowledgement Compliant
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