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Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction

delete2019-11-04
delete271
PRE
AI
W
Wanzhen Zheng
杨健 封面图
杨健 (Jian Yang)
H
Hengquan Chen
侯
侯阳 (Yang Hou) *
Q
Qi Wang
谷
谷猛 (Meng Gu)
何
何锋 (Feng He)
夏
夏螢 (Ying Xia)
X
Xia Zheng
李
李中坚 (Zhongjian Li)
B
Bin Yang
雷乐成 封面图
雷乐成 (Lecheng Lei)
C
Chris Yuan
Q
Qinggang He *
M
Ming Qiu *
Prof. Dr. Xinliang Feng 封面图
Prof. Dr. Xinliang Feng (Xinliang Feng) *
DOI:10.1002/adfm.201907658delete
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摘要

摘要

En 中文
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.
Keyword:
active sites
atomic dispersion Cu-N-2
CO2 electroreduction
unsaturated coordination
Zn-CO2 battery
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期刊

Advanced Functional Materials 封面图
Advanced Functional Materials
IF:
19
论文数:
3.5W
被引数:
32.1W

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University System of Ohio
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zhejiang university of technology
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Central China Normal University
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Case Western Reserve University
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zhejiang university
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