Boosting hydrocarbon conversion via Cu-doping induced oxygen vacancies on CeO_(2) in CO_(2)electroreduction  

作　　者：Lei Xue Tong Shi Chenhui Han Heng Zhang Fenrong Liu Haorun Li Yan Wang Xiaojun Gu Shanghong Zeng 

机构地区：[1]Inner Mongolia Key Laboratory of Chemistry and Physics of Rare Earth Materials,School of Chemistry and Chemical Engineering,Inner Mongolia University,Hohhot 010021,Inner Mongolia,China [2]State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,Shanxi,China [3]Institute of Catalysis,Department of Chemistry,Zhejiang University,Hangzhou 310058,Zhejiang,China [4]National Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization,Baotou Research Institute of Rare Earths,Baotou 014030,Inner Mongolia,China

出　　处：《Journal of Energy Chemistry》2025年第1期66-76,共11页能源化学(英文版)

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)。

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.

关 键 词：Cu/CeO_(2)-x Oxygen vacancy Hydrocarbon production Reaction mechanism 

分 类 号：O64[理学—物理化学]