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Oxidative homocoupling of arenes is a challenging but attractive method converting non-activated aromatics into biaryl compounds. Applications and mechanistic understanding of bimetallic nanocatalysts for arene C–H bond activation are lim-ited at present. In this study, we found that Pd-Ru bimetallic catalyst supported on Al2O3 showed remarkably high catalytic activity for the oxidative homocoupling of arenes owing to the synergistic effect between Pd and Ru. Structural analyses by high-angle annular dark-field scanning transmission electron microscopy with energy dispersive X-ray spectroscopy and X-ray absorption spectroscopy revealed that Pd nanoparticles were decorated by partially oxidized Ru clusters. Mechanistic studies indicated that the arene C–H bond cleavage was the rate-determining step and proceeded by concerted metalation deprotonation mechanism. It was proposed that the role of Ru is promoting the C–H activation step by generating electron deficient Pd sites, which was supported by DFT calculations. The Ru-decorated Pd nanoparticles showed large turnover numbers for simple arenes.

権利情報:

• In Copyright
  

  This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Catalysis, copyright © 2024 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acscatal.4c05551.

キーワード: Bimetallic catalyst, Palladium, Ruthenium, C-H bond activation, Oxidative coupling, Arene, Biaryl

刊行年月日: 2025-01-03

出版者: American Chemical Society (ACS)

掲載誌:

• ACS Catalysis (ISSN: 21555435) vol. 15 issue. 1 p. 487-493

研究助成金:

• Japan Society for the Promotion of Science JP22K20554
• Japan Society for the Promotion of Science JP23H04874
• Japan Society for the Promotion of Science JP23K13602
• Japan Society for the Promotion of Science JP23K23131
• Tokyo Ohka Foundation for The Promotion of Science and Technology

原稿種別: 著者最終稿 (Accepted manuscript)

MDR DOI: https://doi.org/10.48505/nims.5245

公開URL: https://doi.org/10.1021/acscatal.4c05551

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更新時刻: 2025-01-06 16:26:31 +0900

MDRでの公開時刻: 2025-12-19 14:11:42 +0900