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RhRu Bimetallic Oxide Cluster Catalysts for Cross-Dehydrogenative Coupling of Arenes and Carboxylic Acids
http://hdl.handle.net/10131/0002001048
http://hdl.handle.net/10131/0002001048a5b3e4cd-029e-4123-a52c-080f0fb29901
名前 / ファイル | ライセンス | アクション |
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Item type | 学術雑誌論文 / Journal Article(1) | |||||||||||
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公開日 | 2024-07-26 | |||||||||||
タイトル | ||||||||||||
言語 | en | |||||||||||
タイトル | RhRu Bimetallic Oxide Cluster Catalysts for Cross-Dehydrogenative Coupling of Arenes and Carboxylic Acids | |||||||||||
言語 | ||||||||||||
言語 | eng | |||||||||||
キーワード | ||||||||||||
主題 | Aromatic Compounds, Bimetals, Catalysts, Hydrocarbons, Organic Acids(en) | |||||||||||
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資源タイプ識別子 | http://purl.org/coar/resource_type/c_6501 | |||||||||||
資源タイプ | journal article | |||||||||||
アクセス権 | ||||||||||||
アクセス権 | embargoed access | |||||||||||
アクセス権URI | http://purl.org/coar/access_right/c_f1cf | |||||||||||
著者 |
Hasegawa, Shingo
× Hasegawa, Shingo
ORCID
0000-0001-5295-017X
× Harano, Koji
ORCID
0000-0001-6800-8023
× Motokura, Ken
ORCID
0000-0002-0066-5139
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抄録 | ||||||||||||
内容記述タイプ | Abstract | |||||||||||
内容記述 | Noble-metal-based bimetallic oxide clusters are promising novel catalysts. In this study, we developed carbon-supported RhRu bimetallic oxide clusters (RhRuOx/C) with a mean diameter of 1.2 nm, which showed remarkable catalytic activity for the cross-dehydrogenative coupling (CDC) of arenes and carboxylic acids with O2 as the sole oxidant. RhRu bimetallic oxide cluster formation was confirmed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy with energy-dispersive X-ray spectroscopy and synchrotron X-ray absorption spectroscopy. Kinetic isotope and substituent effects indicated that arene C–H bond cleavage was the rate-determining step and proceeded via electrophilic concerted metalation–deprotonation mechanism, with a carboxylate as an internal base. Density functional theory calculations supported the proposed mechanism and indicated that the active center for C–H bond activation was Rh(V) rather than Rh(III), while Ru enhanced the electrophilicity of the Rh(V) site by decreasing the negative charge of the surrounding oxygen atoms. Electron-rich arenes showed relatively high reactivity for the RhRuOx/C-catalyzed CDC reaction, and both aliphatic and aromatic carboxylic acids were applicable to the reaction. The RhRuOx/C catalyst is promising for the CDC reaction of arenes and carboxylic acids to produce aryl esters. This work promotes the development of noble-metal-based bimetallic oxide clusters for C–H bond activation reactions. | |||||||||||
言語 | en | |||||||||||
書誌情報 |
en : Journal of the American Chemical Society 巻 146, 号 28, p. 19059-19069, ページ数 11, 発行日 2024-06-06 |
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収録物識別子タイプ | PISSN | |||||||||||
収録物識別子 | 00027863 | |||||||||||
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収録物識別子タイプ | NCID | |||||||||||
収録物識別子 | AA00692602 | |||||||||||
DOI | ||||||||||||
関連タイプ | isVersionOf | |||||||||||
識別子タイプ | DOI | |||||||||||
関連識別子 | https://doi.org/10.1021/jacs.4c03467 | |||||||||||
権利 | ||||||||||||
言語 | en | |||||||||||
権利情報Resource | https://pubs.acs.org/page/copyright/journals/posting_policies.html | |||||||||||
権利情報 | This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see [http://pubs.acs.org/articlesonrequest/AOR-KBKQW9JBFDRH5SGGQURG]. | |||||||||||
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出版タイプ | AM | |||||||||||
出版タイプResource | http://purl.org/coar/version/c_ab4af688f83e57aa | |||||||||||
出版者 | ||||||||||||
出版者 | American Chemical Society |