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单原子催化剂中的电子金属-载体相互作用。

Electronic metal-support interactions in single-atom catalysts.

机构信息

Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention (LAP3), Department of Environmental Science and Engineering, Fudan University, 220 Handan Road, Shanghai, 200433 (China).

出版信息

Angew Chem Int Ed Engl. 2014 Mar 24;53(13):3418-21. doi: 10.1002/anie.201309248. Epub 2014 Mar 5.

Abstract

The synthesis of single-atom catalysts and the control of the electronic properties of catalytic sites to arrive at superior catalysts is a major challenge in heterogeneous catalysis. A stable supported single-atom silver catalyst with a controllable electronic state was obtained by anti-Ostwald ripening. An electronic perturbation of the catalytic sites that is induced by a subtle change in the structure of the support has a strong influence on the intrinsic reactivity. The higher depletion of the 4d electronic state of the silver atoms causes stronger electronic metal-support interactions, which leads to easier reducibility and higher catalytic activity. These results may improve our understanding of the nature of electronic metal-support interactions and lead to structure-activity correlations.

摘要

合成单原子催化剂并控制催化位点的电子性质以获得更优异的催化剂,是多相催化领域的一个重大挑战。通过反奥斯特瓦尔德熟化法得到了一种稳定的负载型单原子银催化剂,其电子状态可控。载体结构的细微变化引起催化位点的电子微扰对本征反应性有很强的影响。银原子的 4d 电子态损耗越高,导致电子金属-载体相互作用越强,从而使催化剂更容易还原,活性更高。这些结果可能会增进我们对电子金属-载体相互作用本质的理解,并有助于建立结构-活性关系。

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