The electrochemical conversion of carbon dioxide(CO_(2))has been attracting increasingly research interest in the past decade,with the ultimate goal of utilizing electricity from renewable energy to realize carbon neu...The electrochemical conversion of carbon dioxide(CO_(2))has been attracting increasingly research interest in the past decade,with the ultimate goal of utilizing electricity from renewable energy to realize carbon neutrality,as well as economic and energy benefits.Nonetheless,the capture and concentrating of CO_(2) cost a substantial portion of energy,while almost all the reported researches showed CO_(2) electroreduction under high concentrations of(typically pure)CO_(2) reactants,and only very few recent studies have investigated the capability of applying low CO_(2) concentrations(such as~10%in flue gases).In this work,we first demonstrated the electroreduction of 0.03%CO_(2)(in helium)in a homemade gas‐phase electrochemical electrolyzer,using a low‐cost copper(Cu)or nanoscale copper(nano‐Cu)catalyst.Mixed with steam,the gas‐phase CO_(2) was directly delivered onto the gas‐solid interface with the Cu catalyst and reduced to CO,without the need/constraint of being adsorbed by aqueous solution or alkaline electrolytes.By tuning the catalyst and experi‐mental parameters,the conversion efficiency of CO_(2) reached as high as~95%.Furthermore,we demonstrated the direct electroreduction of 0.04%CO_(2) from real air sample with an optimized conversion efficiency of~79%,suggesting a promising perspective of the electroreduction ap‐proach toward direct CO_(2) conversion.展开更多
文摘The electrochemical conversion of carbon dioxide(CO_(2))has been attracting increasingly research interest in the past decade,with the ultimate goal of utilizing electricity from renewable energy to realize carbon neutrality,as well as economic and energy benefits.Nonetheless,the capture and concentrating of CO_(2) cost a substantial portion of energy,while almost all the reported researches showed CO_(2) electroreduction under high concentrations of(typically pure)CO_(2) reactants,and only very few recent studies have investigated the capability of applying low CO_(2) concentrations(such as~10%in flue gases).In this work,we first demonstrated the electroreduction of 0.03%CO_(2)(in helium)in a homemade gas‐phase electrochemical electrolyzer,using a low‐cost copper(Cu)or nanoscale copper(nano‐Cu)catalyst.Mixed with steam,the gas‐phase CO_(2) was directly delivered onto the gas‐solid interface with the Cu catalyst and reduced to CO,without the need/constraint of being adsorbed by aqueous solution or alkaline electrolytes.By tuning the catalyst and experi‐mental parameters,the conversion efficiency of CO_(2) reached as high as~95%.Furthermore,we demonstrated the direct electroreduction of 0.04%CO_(2) from real air sample with an optimized conversion efficiency of~79%,suggesting a promising perspective of the electroreduction ap‐proach toward direct CO_(2) conversion.
