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Atomically Defined Undercoordinated Active Sites for Highly Efficient CO 2 Electroreduction
Author(s) -
Zheng Wanzhen,
Yang Jian,
Chen Hengquan,
Hou Yang,
Wang Qi,
Gu Meng,
He Feng,
Xia Ying,
Xia Zheng,
Li Zhongjian,
Yang Bin,
Lei Lecheng,
Yuan Chris,
He Qinggang,
Qiu Ming,
Feng Xinliang
Publication year - 2020
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201907658
Subject(s) - materials science , faraday efficiency , electrocatalyst , graphene , selectivity , copper , carbon fibers , atom (system on chip) , adsorption , molecule , nanotechnology , chemical engineering , catalysis , electrode , chemistry , electrochemistry , composite number , organic chemistry , composite material , computer science , engineering , metallurgy , embedded system
Electrocatalytic reduction of carbon dioxide (CO 2 ER) in rechargeable Zn–CO 2 battery still remains a great challenge. Herein, a highly efficient CO 2 ER 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 CO 2 ER 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 CO 2 promote the adsorption of CO 2 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 *CO 2 , thus efficiently boosting the *COOH generation and CO 2 ER performance. A designed rechargeable Zn–CO 2 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.