Controllable selective anchoring of subnanometric Ru clusters or single-atoms/clusters on tungsten nitride for the hydrogen oxidation

IF 10.4 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Qijiao Sun, Chuanqiang Wu, Yiqiang Sun, Yuan Shen, Lei Zhao, Xiaodong Yang, Li Yang, Yunxiang Lin, Keke Mao, Kun Xu
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Abstract

The impregnation method in the preparation of metal cluster catalysts typically inadvertently introduces single atoms (SAs) into the substrate. However, the question of whether the introduction of SAs will further improve the catalytic activity of cluster systems for specific reactions such as the hydrogen oxidation reaction (HOR) remains unraveled. Herein, we demonstrate Ru clusters anchored on WN nanowires (RuC/WN) show a higher alkaline HOR catalytic activity in comparison with Ru SAs and nanoclusters (NCs)-coupled catalyst anchored on WN nanowires system (RuC,S/WN). Notably, the RuC/WN exhibits superb intrinsic catalytic activity with a mass-normalized exchange current density of 890 mA mg−1PGM, which is among the top level of well developed Ru-based HOR catalysts. Both theoretical simulation and experimental investigation suggest that RuC/WN owns an optimized H* and OH* reaction intermediates for the alkaline HOR, therefore resulting in the excellent intrinsic HOR catalytic performance.

在氮化钨上可控地选择性锚定亚纳米级 Ru 簇或单原子/簇,以实现氢氧化
制备金属簇催化剂的浸渍法通常会无意中将单原子(SA)引入基质中。然而,引入单原子是否会进一步提高簇簇系统对氢氧化反应(HOR)等特定反应的催化活性,这个问题仍未解决。在此,我们证明了锚定在 WN 纳米线上的 Ru 簇(RuC/WN)与锚定在 WN 纳米线系统上的 Ru SAs 和纳米簇(NCs)耦合催化剂(RuC,S/WN)相比,具有更高的碱性氢氧化反应催化活性。值得注意的是,RuC/WN 表现出了极高的内在催化活性,其质量归一化交换电流密度为 890 mA mg-1PGM,是目前开发成熟的 Ru 基 HOR 催化剂中的最高水平。理论模拟和实验研究均表明,RuC/WN 具有优化的 H* 和 OH* 反应中间体,可用于碱性 HOR,因此具有优异的内在 HOR 催化性能。
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来源期刊
Science China Chemistry
Science China Chemistry CHEMISTRY, MULTIDISCIPLINARY-
CiteScore
14.40
自引率
7.30%
发文量
3787
审稿时长
2.2 months
期刊介绍: Science China Chemistry, co-sponsored by the Chinese Academy of Sciences and the National Natural Science Foundation of China and published by Science China Press, publishes high-quality original research in both basic and applied chemistry. Indexed by Science Citation Index, it is a premier academic journal in the field. Categories of articles include: Highlights. Brief summaries and scholarly comments on recent research achievements in any field of chemistry. Perspectives. Concise reports on thelatest chemistry trends of interest to scientists worldwide, including discussions of research breakthroughs and interpretations of important science and funding policies. Reviews. In-depth summaries of representative results and achievements of the past 5–10 years in selected topics based on or closely related to the research expertise of the authors, providing a thorough assessment of the significance, current status, and future research directions of the field.
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