期刊
ADVANCED FUNCTIONAL MATERIALS
卷 30, 期 4, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/adfm.201907658
关键词
active sites; atomic dispersion Cu-N-2; CO2 electroreduction; unsaturated coordination; Zn-CO2 battery
类别
资金
- National Natural Science Foundation of China [21922811, 21878270, 51702284]
- Zhejiang Provincial Natural Science Foundation of China [LR19B060002]
- Startup Foundation for Hundred-Talent Program of Zhejiang University
- CCNU [CCNU18TS048]
- Hubei Natural Science Foundation of China [2018CFB531]
Electrocatalytic reduction of carbon dioxide (CO2ER) in rechargeable Zn-CO2 battery still remains a great challenge. Herein, a highly efficient CO2ER electrocatalyst composed of coordinatively unsaturated single-atom copper coordinated with nitrogen sites anchored into graphene matrix (Cu-N-2/GN) is reported. Benefitting from the unsaturated coordination environment and atomic dispersion, the ultrathin Cu-N-2/GN nanosheets exhibit a high CO2ER activity and selectivity for CO production with an onset potential of -0.33 V and the maximum Faradaic efficiency of 81% at a low potential of -0.50 V, superior to the previously reported atomically dispersed Cu-N anchored on carbon materials. Experimental results manifest the highly exposed and atomically dispersed Cu-N-2 active sites in graphene framework where the Cu species are coordinated by two N atoms. Theoretical calculations demonstrate that the optimized reaction free energy for Cu-N-2 sites to capture CO2 promote the adsorption of CO2 molecules on Cu-N-2 sites; meanwhile, the short bond lengths of Cu-N-2 sites accelerate the electron transfer from Cu-N-2 sites to *CO2, thus efficiently boosting the *COOH generation and CO2ER performance. A designed rechargeable Zn-CO2 battery with Cu-N-2/GN nanosheets deliver a peak power density of 0.6 mW cm(-2), and the charge process of battery can be driven by natural solar energy.
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