摘要
Conversion of CO_(2)back to hydrocarbons is the most direct way of closing the“carbon cycle”,and its significance is further enlarged if this process is driven by renewable energies such as electricity.However,precisely controlling the product selectivity towards hydrocarbons against the competitive hydrogen evolution remains challenging,especially for Cu-based catalysts.Herein,we report a novel defect engineering strategy,by which Cu-doping-induced oxygen vacancies on CeO_(2)nanorods were effectively created,with adjustable vacancy/Cu ratio.The resulting optimum catalyst shows up to 79%catalytic current density to hydrocarbons(excluding CO),with 49%faradaic efficiency to CH4.Experiments and density functional theory unveil that the ratio between oxygen vacancy and Cu affects significantly the formation of*CHO and activation of H2O,which leads to the following deep hydrogenation to hydrocarbons.These findings may spur new insights for designing and developing more controllable chemical process relevant to CO_(2)utilization.
基金
National Natural Science Foundation of China(21968020,22302222)
Natural Science Foundation of Inner Mongolia(2022MS02011)
China Postdoctoral Science Foundation under Grant Number(2024T170965,2023M743641)
Science and Technology Projects of China Northern Rare Earth(BFXT-2022-D-0023)
Science and Technology Department of Shanxi Province(202303021222409)
Education Department of Inner Mongolia Autonomous Region(NJZZ23094,NJYT23039)。
作者简介
Lei Xue,contributed equally to this work;Tong Shi,contributed equally to this work;Corresponding author:Chenhui Han,E-mail address:hanchenhui@imu.edu.cn;Corresponding author:Fenrong Liu,E-mail address:fenrongl@163.com;Corresponding author:Xiaojun Gu,E-mail address:xiaojun.gu@imu.edu.cn;Corresponding author:Shanghong Zeng,E-mail address:zengshanghong@imu.edu.cn。
