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Oxygen Vacancies in ZnO Nanosheets Enhance CO2 Electrochemical Reduction to CO
Authors:Zhigang Geng  Xiangdong Kong  Weiwei Chen  Hongyang Su  Yan Liu  Fan Cai  Prof Guoxiong Wang  Prof Jie Zeng
Institution:1. Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, P. R. China;2. State Key Laboratory of Catalysis, CAS Center for Excellence in Nanoscience, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, China
Abstract:As electron transfer to CO2 is generally considered to be the critical step during the activation of CO2, it is important to develop approaches to engineer the electronic properties of catalysts to improve their performance in CO2 electrochemical reduction. Herein, we developed an efficient strategy to facilitate CO2 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 CO2. Mechanistic studies further revealed that the enhancement of CO production by introducing oxygen vacancies into ZnO nanosheets originated from the increased binding strength of CO2 and the eased CO2 activation.
Keywords:CO2 activation  CO2 electrochemical reduction  electronic properties  oxygen vacancies  ZnO nanosheets
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