期刊
ELECTROCHIMICA ACTA
卷 426, 期 -, 页码 -出版社
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.electacta.2022.140764
关键词
PC 6 monolayer; Dual atom catalyst; Electrochemical CO 2 reduction; First principle calculations; Electrocatalyst
资金
- National Natural Science Foundation of China [21403003, 21403004]
The study designs 36 dual-atom catalysts to break the linear scaling relationship of adsorption energy between reaction intermediates in CO2 electrochemical reduction reaction. After several rounds of screening, Mn2@PC6 catalyst is identified as a promising candidate for deep reduction of CO2 to CH4.
The catalytic activity of the CO2 electrochemical reduction reaction (CO2RR), which is regarded as one of the most promising approach to tackle the current excess carbon emissions problem, is significantly restricted by the scaling relationship between adsorption energy of reaction intermediates. Here, inspired by the concept of multiple active centers, we designed 36 dual-atom catalysts in PC6 monolayer, including 8 homonuclear (M2@PC6, M=Cr, Mn, Fe, Co, Ni, Cu, Pd, and Ag) and 28 heteronuclear (M1M2@PC6) catalysts, to obtain efficient CO2RR catalysts by breaking the inherent limitation of linear scaling relations. After several rounds of screening for catalysts with stability, activity, selectivity through density functional theory (DFT) study, Mn2@PC6 was identified as a promising candidate for deep reduction of CO2 to CH4 with a low limiting potential of -0.31V (vs RHE). The projected density of states analysis demonstrates that the candidates break the linear scaling relationship stemming from the apparent mixing of the O-2p states and metal-3d states. The apparent change of spin polarization and asymmetric charge distribution on the active site of Mn2@PC6 play a crucial role in its superior CO2RR catalytic performance. This work provides a potential strategy from the theoretical perspective for rational design of efficient electrocatalyst by introduction of dual active centers to break the scaling relationship of intermediates.
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