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Electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) is an attractive approach to deal with the emission of CO2 and to produce valuable fuels and chemicals in a carbon‐neutral way. Many efforts have been devoted to boost the activity and selectivity of high‐value multicarbon products (C2+) on Cu‐based electrocatalysts. However, Cu‐based CO2RR electrocatalysts suffer from poor catalytic stability mainly due to the structural degradation and loss of active species under CO2RR condition. To date, most reported Cu‐based electrocatalysts present stabilities over dozens of hours, which limits the advance of Cu‐based electrocatalysts for CO2RR. Herein, a porous chlorine‐doped Cu electrocatalyst exhibits high C2+ Faradaic efficiency (FE) of 53.8 % at −1.00 V versus reversible hydrogen electrode (VRHE). Importantly, the catalyst exhibited an outstanding catalytic stability in long‐term electrocatalysis over 240 h. Experimental results show that the chlorine‐induced stable cationic Cu0/Cu+ species and the well‐preserved structure with abundant active sites are critical to the high FE of C2+ in the long‐term run of electrochemical CO2 reduction. [ABSTRACT FROM AUTHOR]

Electrochemical carbon dioxide (CO2) reduction reaction (CO2RR) is an attractive approach to deal with the emission of CO2 and to produce valuable fuels and chemicals in a carbon‐neutral way. Many efforts have been devoted to boost the activity and selectivity of high‐value multicarbon products (C2+) on Cu‐based electrocatalysts. However, Cu‐based CO2RR electrocatalysts suffer from poor catalytic stability mainly due to the structural degradation and loss of active species under CO2RR condition. To date, most reported Cu‐based electrocatalysts present stabilities over dozens of hours, which limits the advance of Cu‐based electrocatalysts for CO2RR. Herein, a porous chlorine‐doped Cu electrocatalyst exhibits high C2+ Faradaic efficiency (FE) of 53.8 % at −1.00 V versus reversible hydrogen electrode (VRHE). Importantly, the catalyst exhibited an outstanding catalytic stability in long‐term electrocatalysis over 240 h. Experimental results show that the chlorine‐induced stable cationic Cu0/Cu+ species and the well‐preserved structure with abundant active sites are critical to the high FE of C2+ in the long‐term run of electrochemical CO2 reduction. [ABSTRACT FROM AUTHOR]