Simple “Directional Trimming” Strategy Engineered Platinum Atomic Clusters with Controllable Coordination Numbers for Efficient Hydrogen Evolution

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2025-03-25 DOI:10.1002/anie.202504828
Fengkun Hao, Jing Zhong, Fengqian Hao, Shaorou Ke, Yanghong Li, Zhengyi Mao, Yunhu He, Tengshijie Gao, Linlin Wang, Shuohan Li, Minghao Fang, Zhaohui Huang, Xiaoxue Chang, Ruiwen Shao, Jian Lu, Xin Min
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Abstract

The coordination number (CN) in atomic cluster (AC) catalysts endows their catalytic performance with flexible tunability. However, the quantitative relationship between the CN and catalytic activity of atomic cluster catalysts remains ambiguity. Herein, inspired by the gardeners trimming plants branches to obtain ornamental value shape, we propose a “directional trimming” strategy to obtain a series of AC catalysts with wide range of Cl CN and establish an inverted volcano curve to explain the effect of CN on hydrogen evolution reaction (HER). Moreover, Pt/CB-90 (moderate Cl CN of 3.7) exhibits the lowest overpotential of 22.94 mV at 10 mA cm−2 and outstanding mass activity (25 times to commercial Pt/C). This proposed synthesis strategy fully utilizes the precursor atoms and is widely applicable. The reaction liquid can be reused up to 20 times to obtain 1130 mg catalysts without introducing any other chemicals. Additionally, theoretical calculations highlight the appropriate Cl CN benefits the HER on Pt2 ACs. This fundamental understanding of the role of CN in catalytic activity offers valuable guidance to promote performance in various catalytic reactions.

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简单的“定向修剪”策略设计了具有可控配位数的铂原子簇,用于有效的析氢
原子簇催化剂的配位数(CN)使其催化性能具有灵活的可调性。然而,原子簇催化剂的配位数(CN)与催化活性之间的定量关系尚不明确。在此,灵感来自园丁修剪植物的枝干,以获得观赏价值的形状。我们提出了一种“定向修剪”策略,以获得一系列具有宽范围Cl - CN的AC催化剂,并建立了倒火山曲线来解释CN对析氢反应(HER)的影响。此外,Pt/CB‐90(中等Cl CN为3.7)在10 mA cm‐2时的过电位最低,为22.94 mV,质量活性是商用Pt/C的25倍。该合成策略充分利用了前驱体原子,具有广泛的应用前景。该反应液最多可重复使用20次,在不引入任何其他化学物质的情况下获得1130毫克的催化剂。此外,理论计算强调了适当的Cl CN有利于Pt2 ACs上的HER。这种对CN在催化活性中的作用的基本理解为提高各种催化反应的性能提供了有价值的指导。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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