A carbon-based single-atom Cu electrocatalyst for efficient conversion of CO2 to carbon products

Abstract

The simultaneous and efficient electroreduction of CO₂ to C₁ and C₂ different phase products is an extremely challenging task due to the competitive reaction of hydrogen evolution, high energy barrier of CO₂ activation and C–C coupling. Herein, an N-doped carbon-based single-atom Cu-based electrocatalyst (Cu–N₄/C) was designed, which can efficiently reduce CO₂ to carbon products with a total Faraday efficiency (CO and ethanol) of 94.67%. Among them, the selectivity of ethanol reached 53.11%. And Cu–N₄/C could also maintain excellent stability within 16 h. In situ infrared spectroscopy showed that the intermediates, such as *CO_B, *OCH₂, *CO–*OCH₂, and OC₂H₅, which appeared during the electrocatalytic reaction of Cu–N₄/C, promoted the generation of both CO and ethanol, leading to an extremely high carbon product efficiency. This work elucidates the active center of the Cu–N₄/C electrocatalyst as well as the reason for the highly selective generation of carbon products, and provides a new perspective for subsequent in-depth exploration of the rational design of CO₂RR electrocatalysts.