期刊
ACS CATALYSIS
卷 9, 期 6, 页码 5011-5018出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00499
关键词
segregation; adsorption preference; surface modeling; scaling relations; density functional theory; DFT; global optimization; CO2 hydrogenation reaction
资金
- National Key R&D Program of China [2016YFB0600901]
- National Natural Science Foundation of China [21525626, 21761132023, 21676181]
- Program of Introducing Talents of Discipline to Universities [B06006]
- Spanish Grants [PGC2018-093863-B-C22, CTQ2015-64618-R, MDM-2017-0767]
- Generalitat de Catalunya [2017SGR13]
- Deutsche Forschungsgemeinschaft [STU 703/1-1]
A correct description of active sites is a precondition toward reaction mechanism study and catalyst screening. In many cases, high-symmetry and ideally ordered crystalline surfaces are used to represent the reactive sites. However, reaction-induced surface segregation and restructuring weaken the rationality of simply employing the suggested most stable surfaces. This paper describes establishment of the scaling relation between segregation energy and adsorption preference for a fast prediction of segregation over bimetallic surfaces with low computational cost, which helps the construction of more accurate active sites, especially for segregation-prone alloys. Based on this methodology, mechanisms of representative hydrogenation reactions are computationally explored on two surface models of a typical bimetallic alloy, CoCu. Our experiments performed in parallel demonstrate the reactivity of CoCu catalyst to be determined by surface Co/Cu composition, reflecting the limitation of one-and-only surface modeling in the description of complex reactions.
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