期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 8, 期 1, 页码 210-222出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b05183
关键词
CO2 electrochemical reduction; Cu(211); bimetallic single-atom surface alloy; density functional theory; microkinetic modeling
资金
- National Natural Science Foundation of China [21673137]
- Science and Technology Commission of Shanghai Municipality [16ZR1413900]
- Scientific Data and Computing Center, a component of the Computational Science Initiative, at Brookhaven National Laboratory [DE-SC0012704]
Copper is a well-known metal for catalyzing electrochemical CO2 reduction reaction (CO2 RR) toward valuable hydrocarbons and alcohols. Here, using combined density-functional theory and microkinetic modeling approach, we systematically investigated eleven bimetallic [email protected](211) single-atom stepped surface alloys for their CO2 RR activity. It is revealed that the stepped M edge is most likely to be active sites for CO2 RR. The primary reaction pathway is identified as *COOH -> *CO -> *CHO with the potential determining step of *CO + H+ + e- -> *CHO, leading to either CH4 or CH3OH formation at more negative potential. Especially, [email protected](211) and [email protected](211) are both predicted to be most efficient in promoting CO2 RR toward CH4 owing to their breaking of the coupled scaling relations of key intermediates binding at active site. Furthermore, the binding strength of *CO and *OH can serve as good descriptor for differentiating various [email protected](211) for CO2 RR activity and selectivity and specifically, the moderate oxophilic and carbophilic elements of M are preferred. Our study highlights the utmost importance of breaking the linear scaling relations of key intermediates binding at active site for boosting CO2 RR performance.
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