Abstract
AbstractSelective electrochemical CO2 reduction reaction (CO2RR) into value‐added hydrocarbon products such as C2H4 provides a sustainable approach to producing carbon chemicals, which however remains a great challenge owing to the multi‐electron transfer process during CO2 electroreduction. Herein, a tandem catalyst a‐Ni/Cu‐NP@CMK is developed by encapsulating Cu nanoparticles (Cu NPs) into hydrophobic cubic mesoporous carbon with doped atomic Ni‐N4 moieties. Electrochemical tests demonstrate the outstanding C2H4 selectivity of a‐Ni/Cu‐NP@CMK with a high Faraday efficiency (FE) of 72.3% for C2H4 at a large current density of 406.1 mA cm−2 in a flow cell under a neutral medium. Moreover, when used as the cathode catalyst in membrane electrode assembly, a‐Ni/Cu‐NP@CMK stably delivers a current density of 200 mA cm−2 with a FEC2H4 of 63% at ‐2.8 V for 30 h, providing a full‐cell energy efficiency of 28.3% for C2H4 production. Comparative studies disclose that the hydrophobic microenvironment of the Cu NPs in a‐Ni/Cu‐NP@CMK successfully suppresses the competitive hydrogen evolution reaction and improves the CO2RR selectivity. Additionally, in situ spectroscopic investigations and theoretical calculations reveal that the efficient CO2‐to‐CO conversion on the Ni‐N4 moieties feeds Cu NPs with enriched adsorbed CO (*CO), which facilitates the C─C coupling between adjacent *CO to form C2H4.
Published Version
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