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Oxygen Vacancies in ZnO Nanosheets Enhance CO 2 Electrochemical Reduction to CO

2018; Wiley; Volume: 57; Issue: 21 Linguagem: Inglês

10.1002/anie.201711255

1521-3773

Zhigang Geng, Xiangdong Kong, Weiwei Chen, Hongyang Su, Yan Liu, Fan Cai, Guoxiong Wang, Jie Zeng,

Advanced battery technologies research

Abstract As electron transfer to CO 2 is generally considered to be the critical step during the activation of CO 2 , it is important to develop approaches to engineer the electronic properties of catalysts to improve their performance in CO 2 electrochemical reduction. Herein, we developed an efficient strategy to facilitate CO 2 activation by introducing oxygen vacancies into electrocatalysts with electronic‐rich surface. ZnO nanosheets rich in oxygen vacancies exhibited a current density of −16.1 mA cm −2 with a Faradaic efficiency of 83 % for CO production. Based on density functional theory (DFT) calculations, the introduction of oxygen vacancies increased the charge density of ZnO around the valence band maximum, resulting in the enhanced activation of CO 2 . Mechanistic studies further revealed that the enhancement of CO production by introducing oxygen vacancies into ZnO nanosheets originated from the increased binding strength of CO 2 and the eased CO 2 activation.