Activated-Carbon-Supported Clusters Consisting of Four Planarly Arranged Palladium Atoms as Highly Active and Alkene-Selective Hydrogenation Catalysts

IF 13.1 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-06-24 DOI:10.1021/acscatal.5c00339

Chikako Yanagisawa, Rinako Miyauchi, Risa Nishiura, Yoshimasa Wada, Seiji Yamazoe, Atsushi Tahara, Yusuke Sunada

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Abstract

The development of metal catalysts that require a minimum amount of precious metals is highly desirable due to the high cost and scarcity of noble metals. In this study, we synthesized a heterogeneous catalyst consisting of a cluster of four planarly arranged Pd atoms (Pd₄) immobilized onto activated carbon. The obtained catalyst exhibited high catalytic activity in the hydrogenation of various alkenes, whereby the highest TON was 455,556 per Pd atom. This catalyst is characterized by high alkene selectivity, while intramolecular −NO₂, −CN, −OCH₂Ph, epoxy, ester, ketone, and halogen groups remained intact. An X-ray absorption fine structure analysis revealed that the Pd₄ framework was maintained on activated carbon after catalysis. This heterogeneous catalyst structure provides a platform for the development of catalysts that combine good catalytic activity with high chemoselectivity, recyclability, and good substrate compatibility based on a minimum amount of palladium atoms.

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由四个平面排列的钯原子组成的活性炭负载簇作为高活性和烯烃选择性加氢催化剂

由于贵金属的高成本和稀缺性，开发需要最少贵金属的金属催化剂是非常可取的。在这项研究中，我们合成了一种由四个平面排列的钯原子（Pd4）组成的簇固定在活性炭上的多相催化剂。所制备的催化剂对多种烯烃的加氢反应表现出较高的催化活性，其中最高的TON为455,556 / Pd原子。该催化剂的特点是烯烃选择性高，而分子内的- NO2、- CN、- OCH2Ph、环氧、酯、酮和卤素基团保持完整。x射线吸收精细结构分析表明，催化作用后，活性炭上保持了Pd4骨架。这种非均相催化剂结构为开发基于最少钯原子量的催化剂提供了一个平台，该催化剂将良好的催化活性与高化学选择性、可回收性和良好的底物相容性结合起来。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.