单原子催化的最新进展（英文）

发布时间：2018-02-26 15:48

本文关键词： 单原子催化催化剂合成一氧化碳氧化加氢反应电催化　出处：《催化学报》2017年09期 　论文类型：期刊论文

【摘要】：单原子催化剂由于其自身兼具均相催化剂的"孤立活性位点"和多相催化剂易于循环使用的特点,近年来受到了广泛关注.本综述概括了2015至2016年单原子催化领域的重要进展,重点介绍了新的催化剂制备方法、单原子金催化剂在CO氧化中的进展、单原子钯/铂催化的选择性加氢反应以及铂或非贵金属单原子催化剂在电化学中的应用等.在催化剂的合成方面,用传统的湿化学方法制备的单原子催化剂通常金属负载量较低,使得催化剂的常规表征比较困难.最近发展的一系列新型合成方法例如原子层沉积法、高温蒸汽转移法、光介还原法以及热解法等制备M-N-C等非贵金属催化剂等,尽管有不同程度的局限性,但均可以成功制备高负载量的单原子催化剂.单原子催化剂的载体得到了拓展,除传统的金属氧化物外,金属有机框架材料和二维材料等均被用于单原子催化剂的制备.在单原子催化剂的应用方面,金由于较高的电负性和与氧的弱相互作用能力,因而与氧化物载体作用较弱,不易形成单原子催化剂.但近期报道了成功制备的单原子金催化剂,在CO氧化反应、乙醇脱氢和二烯加氢反应中都有不错的进展.本文还介绍了铂和钯单原子(合金)催化剂在加氢反应中的优异活性及选择性,表明了单原子催化剂在选择性上的优势.将一种金属掺杂到另一种金属基底中制备的单原子合金催化剂也因其特异的性能备受关注.此外,对于化工生产中典型的均相催化反应,如氢甲酰化,单原子催化剂在无外加膦配体的情况下表现出高活性的同时还能很好地控制化学选择性,甚至达到令人满意的区域选择性,从实验上证明了单原子催化剂有望作为沟通均相催化和多相催化的桥梁.单原子催化剂在电催化和光催化中也得到了快速发展.铂单原子催化剂因其高原子利用率和高稳定性,在析氢反应和氧还原反应中有着良好的应用前景.另一方面,非贵金属特别是Co单原子催化剂在光电催化中因其优异的活性和巨大潜力得到了较深入的研究.除了上述进展,单原子催化领域还有许多基本问题需要继续深入研究,对单原子催化剂更加全面透彻的认识将为设计发展新型催化体系,扩展单原子催化领域提供指导和借鉴.
[Abstract]:Monatomic catalysts have attracted much attention in recent years because of their own "isolated active sites" of homogeneous catalysts and the characteristics of heterogeneous catalysts being easy to recycle. In this review, the important advances in monoatomic catalysis from 2015 to 2016 are summarized. The preparation method of monatomic gold catalyst and the progress of monatomic gold catalyst in CO oxidation are introduced. Selective hydrogenation of monoatomic palladium / platinum catalyst and application of platinum or non-noble metal monoatomic catalyst in electrochemistry. Monatomic catalysts prepared by traditional wet chemical methods usually have low metal loading, which makes the conventional characterization of catalysts more difficult. Recently, a series of new synthesis methods, such as atomic layer deposition, high temperature vapor transfer method, have been developed. Although there are some limitations in preparing non-noble metal catalysts such as M-N-C by photocatalytic reduction and pyrolysis, monatomic catalysts with high amount of loading can be successfully prepared, and the support of monatomic catalysts has been expanded. In addition to traditional metal oxides, metal-organic framework materials and two-dimensional materials are used in the preparation of monatomic catalysts. In the application of monatomic catalysts, gold is due to its high electronegativity and weak interaction with oxygen. Therefore, the reaction with oxide support is weak and it is not easy to form monatomic catalyst. However, the successful preparation of monatomic gold catalyst in CO oxidation reaction has been reported recently. Good progress has been made in the dehydrogenation of ethanol and the hydrogenation of diene. The excellent activity and selectivity of platinum and palladium monatomic (alloy) catalysts for hydrogenation are also introduced. The results show that monatomic catalysts have advantages in selectivity. Monatomic alloy catalysts prepared by doping one metal into another metal substrate have attracted much attention due to their specific properties. For typical homogeneous catalytic reactions in chemical production, such as hydroformylation, monatomic catalysts exhibit high activity without addition of phosphine ligands, but also can control chemical selectivity well, and even achieve satisfactory regioselectivity. It has been proved experimentally that monatomic catalyst can be used as a bridge between homogeneous catalysis and heterogeneous catalysis. Monoatomic catalyst has also been developed rapidly in electrocatalysis and photocatalysis. On the other hand, non-noble metals, especially Co monatomic catalysts, have been studied deeply in photocatalysis due to their excellent activity and great potential. There are still many basic problems in the field of monatomic catalysis that need to be further studied. A more comprehensive and thorough understanding of monatomic catalysts will provide guidance and reference for the design and development of new catalytic systems and the expansion of monatomic catalytic fields.
【作者单位】：中国科学院大连化学物理研究所催化基础国家重点实验室;中国科学院大学;
【基金】：supported by the National Natural Science Foundation of China(21606222,21303184,21573232) China Postdoctoral Science Foundation(2016M601350) Strategic Priority Research Program of the Chinese Academy of Sciences(XDB17020100) National Key Projects for Fundamental Research and Development of China(2016YFA0202801) Department of Science and Technology of Liaoning Province(2015020086-101)~~
【分类号】：O643.36

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