抄録
Aerobic oxidation of cyclohexane, propane, ethane, and methane to the corresponding alcohols was investigated over an Au55 gold nanoparticle with icosahedron symmetry using density functional theory. Reaction mechanisms were elucidated and activation barriers for catalytic C–H bond cleavage and corresponding alcohols’ formation were estimated. Furthermore, on the basis of the reaction rate constants calculated for realistic reaction temperatures, the relative reaction rates for each alkane hydroxylation were discussed. The catalyst selectivity was investigated for the formation of primary and secondary alcohols. All reaction mechanisms for alkane hydroxylation are compared with the catalytic dissociation of dioxygen molecule over gold nanoparticle surface, which is an important precursor reaction for aerobic oxidation. We have further investigated overoxidation reaction mechanisms leading to formation of ketones. Our results are compared with experimental findings to provide important guidelines for the tuning of catalytic reactions towards the desired products and reaction conditions.
| 元の言語 | 英語 |
|---|---|
| ページ（範囲） | 141-153 |
| ページ数 | 13 |
| ジャーナル | Journal of Catalysis |
| 巻 | 364 |
| DOI | |
| 出版物ステータス | 出版済み - 8 1 2018 |
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All Science Journal Classification (ASJC) codes
- Catalysis
- Physical and Theoretical Chemistry
これを引用
Aerobic oxidation of alkanes on icosahedron gold nanoparticle Au55. / Staykov, Aleksandar Tsekov; Miwa, Tetsuya; Yoshizawa, Kazunari.
：: Journal of Catalysis, 巻 364, 01.08.2018, p. 141-153.研究成果: ジャーナルへの寄稿 › 記事
}
TY - JOUR
T1 - Aerobic oxidation of alkanes on icosahedron gold nanoparticle Au55
AU - Staykov, Aleksandar Tsekov
AU - Miwa, Tetsuya
AU - Yoshizawa, Kazunari
PY - 2018/8/1
Y1 - 2018/8/1
N2 - Aerobic oxidation of cyclohexane, propane, ethane, and methane to the corresponding alcohols was investigated over an Au55 gold nanoparticle with icosahedron symmetry using density functional theory. Reaction mechanisms were elucidated and activation barriers for catalytic C–H bond cleavage and corresponding alcohols’ formation were estimated. Furthermore, on the basis of the reaction rate constants calculated for realistic reaction temperatures, the relative reaction rates for each alkane hydroxylation were discussed. The catalyst selectivity was investigated for the formation of primary and secondary alcohols. All reaction mechanisms for alkane hydroxylation are compared with the catalytic dissociation of dioxygen molecule over gold nanoparticle surface, which is an important precursor reaction for aerobic oxidation. We have further investigated overoxidation reaction mechanisms leading to formation of ketones. Our results are compared with experimental findings to provide important guidelines for the tuning of catalytic reactions towards the desired products and reaction conditions.
AB - Aerobic oxidation of cyclohexane, propane, ethane, and methane to the corresponding alcohols was investigated over an Au55 gold nanoparticle with icosahedron symmetry using density functional theory. Reaction mechanisms were elucidated and activation barriers for catalytic C–H bond cleavage and corresponding alcohols’ formation were estimated. Furthermore, on the basis of the reaction rate constants calculated for realistic reaction temperatures, the relative reaction rates for each alkane hydroxylation were discussed. The catalyst selectivity was investigated for the formation of primary and secondary alcohols. All reaction mechanisms for alkane hydroxylation are compared with the catalytic dissociation of dioxygen molecule over gold nanoparticle surface, which is an important precursor reaction for aerobic oxidation. We have further investigated overoxidation reaction mechanisms leading to formation of ketones. Our results are compared with experimental findings to provide important guidelines for the tuning of catalytic reactions towards the desired products and reaction conditions.
UR - http://www.scopus.com/inward/record.url?scp=85047905690&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=85047905690&partnerID=8YFLogxK
U2 - 10.1016/j.jcat.2018.05.017
DO - 10.1016/j.jcat.2018.05.017
M3 - Article
VL - 364
SP - 141
EP - 153
JO - Journal of Catalysis
JF - Journal of Catalysis
SN - 0021-9517
ER -