Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction

Zheng W, Yang J, Chen H, Hou Y, Wang Q, Gu M, He F, Xia Y, Xia Z, Li Z, Yang B, Lei L, Yuan C, He Q, Qiu M, Feng X (2020)

Publication Type: Journal article

Publication year: 2020

Journal

Advanced Functional Materials Wiley-VCH Verlag

Book Volume: 30

Article Number: 1907658

Journal Issue: 4

DOI: 10.1002/adfm.201907658

Abstract

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–N2/GN) is reported. Benefitting from the unsaturated coordination environment and atomic dispersion, the ultrathin Cu–N2/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–N2 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–N2 sites to capture CO2 promote the adsorption of CO2 molecules on Cu–N2 sites; meanwhile, the short bond lengths of Cu–N2 sites accelerate the electron transfer from Cu–N2 sites to *CO2, thus efficiently boosting the *COOH generation and CO2ER performance. A designed rechargeable Zn–CO2 battery with Cu–N2/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.

Involved external institutions

Zhejiang University CN China (CN) Southern University of Science and Technology CN China (CN) Zhejiang University of Technology (ZJUT) / 浙江工业大学 CN China (CN) Central China Normal University (CCNU) / Huazhong Normal University / 华中师范大学 CN China (CN) Case Western Reserve University US United States (USA) (US) Technische Universität Dresden DE Germany (DE)

How to cite

APA:

Zheng, W., Yang, J., Chen, H., Hou, Y., Wang, Q., Gu, M.,... Feng, X. (2020). Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction. Advanced Functional Materials, 30(4). https://doi.org/10.1002/adfm.201907658

MLA:

Zheng, Wanzhen, et al. "Atomically Defined Undercoordinated Active Sites for Highly Efficient CO2 Electroreduction." Advanced Functional Materials 30.4 (2020).

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