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DOE OSTI · 1981663

Dual-atom active sites embedded in two-dimensional C 2 N for efficient CO 2 electroreduction: A computational study

Liu, Haimei·Huang, Qingliang·An, Wei·Wang, Yuanqiang·Men, Yong·Liu, Shuang
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Abstract

Double-atom catalysts (DACs) have emerged as an enhanced platform of single-atom catalyst for promoting electrocatalytic CO 2 reduction reaction (CO 2 RR). Herein, we present a density-functional theory study on CO 2 RR performance of seven C 2 N-supported homo- and heteronuclear DACs, denoted as M 2 @C 2 N. Our results demonstrate that there exists substantial synergistic effect of dual-metal-atom N 2 M 2 N 2 active site and C 2 N matrix on O&#x2550 C &#x2550O bond activation. The dual-atom M 2 sites are able to drive CO 2 RR beyond C 1 products with low limiting potential (U L ). Specifically, C 2 H 4 formation is preferred on FeM@C 2 N (M = Fe, Co, Ni, Cu) versus CH 4 formation on CuM@C 2 N (M = Co, Ni, Cu). Furthermore, *CO+*CO co-binding strength can serve as a descriptor for CO 2 RR activity for making C 2 products such that the moderate binding results in the lowest U L . Remarkably, C-affinity matters most to C—C bond coupling and C 2 H 4 formation while both C- and O-affinity control CH 4 formation. Furthermore, our results provide theoretical insight into rational design of DACs for efficient CO 2 RR.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYC2NCO2 electroreductionChemistryDensity functional theoryDouble-atom catalystEnergy & FuelsEngineeringGraphene

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Liu, Haimei, Huang, Qingliang, An, Wei, Wang, Yuanqiang, Men, Yong, Liu, Shuang. 2021-02-25. Dual-atom active sites embedded in two-dimensional C 2 N for efficient CO 2 electroreduction: A computational study. https://doi.org/10.1016/j.jechem.2021.02.007

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