期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 7, 期 23, 页码 19113-19121出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.9b05042
关键词
CO2 reduction; electrocatalysis; C2N-gaphene; dimer; density functional theory
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]
Gaining mechanistic insights into the active site is essential to rational design of a high-performance cathode catalyst for the electrochemical CO2 reduction reaction (CO2 RR). Here, by means of density functional theory and computational hydrogen electrode methods, we investigated synergy of a metallic NiCo dimer anchored on a C2N graphene matrix for promoting the CO2 RR. It is found that heterometallic NiCo@C2N (U-L = -0.25 V) outperforms homometallic Co-2@C2N (U-L = -0.30 V) and Ni-2@C2N (U-L = -0.67 V) for catalyzing the CO2 RR toward CH4 formation owing to its synergy within the dimer. We emphasize the impact of co-adsorbed *H, *OH, and *CO intermediates on the CO2 RR, revealing that multiple competing reaction channels are accessible from viable co-adsorbates. Moreover, strongly-bound *H, *OH, and *CO intermediates are predicted not to deactivate metallic dimer sites for a continuous cycle of the CO2 RR Our study could provide a theoretical basis for optimizing a metallic dimer anchored on a N-doped graphene matrix for achieving a more advanced CO2 RR cathode with enhanced activity and selectivity.
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