Zhang Jian, Wu Xi, Cheong Weng-Chon, Chen Wenxing, Lin Rui, Li Jia, Zheng Lirong, Yan Wensheng, Gu Lin, Chen Chen, Peng Qing, Wang Dingsheng, Li Yadong
Department of Chemistry, Tsinghua University, 100084, Beijing, China.
Laboratory for Computational Materials Engineering, Division of Energy and Environment, Graduate School at Shenzhen, Tsinghua University, 518055, Shenzhen, China.
Nat Commun. 2018 Mar 8;9(1):1002. doi: 10.1038/s41467-018-03380-z.
Development of single-atomic-site catalysts with high metal loading is highly desirable but proved to be very challenging. Although utilizing defects on supports to stabilize independent metal atoms has become a powerful method to fabricate single-atomic-site catalysts, little attention has been devoted to cation vacancy defects. Here we report a nickel hydroxide nanoboard with abundant Ni vacancy defects serving as the practical support to achieve a single-atomic-site Pt catalyst (Pt/Ni(OH)) containing Pt up to 2.3 wt% just by a simple wet impregnation method. The Ni vacancies are found to have strong stabilizing effect of single-atomic Pt species, which is determined by X-ray absorption spectrometry analyses and density functional theory calculations. This Pt/Ni(OH) catalyst shows a high catalytic efficiency in diboration of a variety of alkynes and alkenes, yielding an overall turnover frequency value upon reaction completion for phenylacetylene of ~3000 h, which is much higher than other reported heterogeneous catalysts.
开发具有高金属负载量的单原子位点催化剂是非常令人期待的，但事实证明极具挑战性。尽管利用载体上的缺陷来稳定独立的金属原子已成为制备单原子位点催化剂的一种有效方法，但阳离子空位缺陷却很少受到关注。在此，我们报道了一种具有丰富镍空位缺陷的氢氧化镍纳米板，作为一种实用载体，仅通过简单的湿浸渍法就可制备出单原子位点铂催化剂（Pt/Ni(OH)），其中铂含量高达2.3 wt%。通过X射线吸收光谱分析和密度泛函理论计算确定，镍空位对单原子铂物种具有很强的稳定作用。这种Pt/Ni(OH)催化剂在多种炔烃和烯烃的双硼化反应中表现出高催化效率，对于苯乙炔，反应完成时的总周转频率值约为3000 h⁻¹，远高于其他已报道的多相催化剂。
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