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单原子催化与表面有机金属催化的比较

The Comparison between Single Atom Catalysis and Surface Organometallic Catalysis.

作者信息

Samantaray Manoja K, D'Elia Valerio, Pump Eva, Falivene Laura, Harb Moussab, Ould Chikh Samy, Cavallo Luigi, Basset Jean-Marie

机构信息

King Abdullah University of Science and Technology (KAUST) , Thuwal 23955-6900 , Saudi Arabia.

School of Molecular Science and Engineering (MSE) , Vidyasirimedhi Institute of Science and Technology (VISTEC) , Wang Chan, Payupnai , 21210 Rayong , Thailand.

出版信息

Chem Rev. 2020 Jan 22;120(2):734-813. doi: 10.1021/acs.chemrev.9b00238. Epub 2019 Oct 15.

Abstract

Single atom catalysis (SAC) is a recent discipline of heterogeneous catalysis for which a single atom on a surface is able to carry out various catalytic reactions. A kind of revolution in heterogeneous catalysis by metals for which it was assumed that specific sites or defects of a nanoparticle were necessary to activate substrates in catalytic reactions. In another extreme of the spectrum, surface organometallic chemistry (SOMC), and, by extension, surface organometallic catalysis (SOMCat), have demonstrated that single atoms on a surface, but this time with specific ligands, could lead to a more predictive approach in heterogeneous catalysis. The predictive character of SOMCat was just the result of intuitive mechanisms derived from the elementary steps of molecular chemistry. This review article will compare the aspects of single atom catalysis and surface organometallic catalysis by considering several specific catalytic reactions, some of which exist for both fields, whereas others might see mutual overlap in the future. After a definition of both domains, a detailed approach of the methods, mostly modeling and spectroscopy, will be followed by a detailed analysis of catalytic reactions: hydrogenation, dehydrogenation, hydrogenolysis, oxidative dehydrogenation, alkane and cycloalkane metathesis, methane activation, metathetic oxidation, CO activation to cyclic carbonates, imine metathesis, and selective catalytic reduction (SCR) reactions. A prospective resulting from present knowledge is showing the emergence of a new discipline from the overlap between the two areas.

摘要

单原子催化(SAC)是多相催化领域中一门新兴学科,在该领域中,表面上的单个原子能够进行各种催化反应。这是金属多相催化领域的一种变革,此前人们认为纳米颗粒的特定位点或缺陷对于催化反应中活化底物是必需的。在该领域的另一个极端,表面有机金属化学(SOMC),以及由此延伸出的表面有机金属催化(SOMCat),已经证明表面上的单个原子,但这次带有特定配体,能够在多相催化中带来更具预测性的方法。SOMCat的预测特性仅仅是源自分子化学基本步骤的直观机理的结果。这篇综述文章将通过考虑几个特定的催化反应来比较单原子催化和表面有机金属催化的各个方面,其中一些反应在两个领域都存在,而其他一些反应未来可能会有相互重叠。在对这两个领域进行定义之后,将详细介绍主要包括建模和光谱学在内的方法,随后对催化反应进行详细分析:氢化、脱氢、氢解、氧化脱氢、烷烃和环烷烃复分解、甲烷活化、复分解氧化、CO活化生成环状碳酸酯、亚胺复分解以及选择性催化还原(SCR)反应。基于现有知识的展望表明,这两个领域的重叠将催生出一门新学科。

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