Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction
Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction
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DOI：
10.1016/j.isci.2019.02.016
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发表时间：
2019-03-29
期刊：
影响因子：
5.8
通讯作者：
Liu, Jingyue
中科院分区：
文献类型：
--
作者：
Lou, Yang;Wu, Honglu;Liu, Jingyue
强金属-载体相互作用（SMSI）被广泛用于提高催化性能和确定反应机理。我们报道了锚定在空心纳米碳（h-NC）边缘上的单个Pt原子具有强的金属-碳相互作用，这显着改变了锚定Pt原子对选择性加氢反应的催化行为。强Pt- c键不仅稳定了单个Pt原子，而且改变了它们的电子结构，调整了它们的吸附性质，增强了反应物的活化。所制备的Pt-1/h- nc单原子催化剂（SACS）具有优异的3-硝基苯乙烯加氢成3-乙烯基苯胺的活性，其周转率为31000 /h，是目前文献报道的该类选择性加氢反应最佳催化剂的20倍。通过h-NCs的边缘碳原子强锚定Pt原子的策略是通用的，并且可以扩展到通过SMSI在各种支持材料的表面上构建强锚定的金属原子，以开发稳健的SACS。
Strong metal-support interaction (SMSI) has been widely used to improve catalytic performance and to identify reaction mechanisms. We report that single Pt atoms anchored onto hollow nanocarbon (h-NC) edges possess strong metal-carbon interaction, which significantly modifies the catalytic behavior of the anchored Pt atoms for selective hydrogenation reactions. The strong Pt-C bonding not only stabilizes single Pt atoms but also modifies their electronic structure, tunes their adsorption properties, and enhances activation of reactants. The fabricated Pt-1/h-NC single-atom catalysts (SACS) demonstrated excellent activity for hydrogenation of 3-nitrostyrene to 3-vinylaniline with a turnover number >31,000/h, 20 times higher than that of the best catalyst for such selective hydrogenation reactions reported in the literature. The strategy to strongly anchor Pt atoms by edge carbon atoms of h-NCs is general and can be extended to construct strongly anchored metal atoms, via SMSI, onto surfaces of various types of support materials to develop robust SACS.