期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 122, 期 34, 页码 19712-19721出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcc.8b06494
关键词
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资金
- China by the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province [JC2018004]
- Excellent Young Foundation of Harbin Normal University [XKYQ201304]
- National Natural Science Foundation of China [11704203]
- United States by NSF-CREST Center for Innovation, Research and Education in Environmental Nanotechnology (CIRE2N) [HRD-1736093]
The carbon dioxide electrochemical reduction (CO2RR) to useful fuels and chemicals with renewable electricity offers a promising strategy for resolving energy security and environmental issues. Searching for low-cost catalysts with high efficiency and high selectivity is crucial to achieve this goal. Here, by means of comprehensive density functional theory computations, we systematically investigated the potential of several transition metal dimers supported on a porous C2N layer (Cu-2@C2N) as the CO2RR electrocatalysts. Our results revealed that the Cu dimer can be stably embedded in the porous C2N monolayer because of the strong hybridization between Cu 3d orbitals and N 2p orbitals, thus ensuring its high stability. On the basis of the computed free energy changes, we found that Cu-2@C2N exhibits superior performance for the CO2RR with a small limiting potential of -0.23 V and the CO2 -> HCOO* -> HCOOH* -> H2COOH* -> H2CO* -> H2COH* -> CH2* -> CH3* -> CH4 route is the most favorable, among which the hydrogenation of HCOO* to HCOOH* is the potential-determining step. In addition, C2H4 can also be yielded, as the formed CO* provides active sites for the coupling with another CO species with the limiting potential of -0.76 V. Therefore, Cu-2@C2N layer is a quite promising bi-atom catalyst for the electrochemical reduction of CO2 to hydrocarbons.
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