Amino‐Induced CO2 Spillover to Boost the Electrochemical Reduction Activity of CdS for CO Production

Abstract

AbstractA considerable challenge in CO2 reduction reaction (CO2RR) to produce high‐value‐added chemicals comes from the adsorption and activation of CO2 to form intermediates. Herein, an amino‐induced spillover strategy aimed at significantly enhancing the CO2 adsorption and activation capabilities of CdS supported on N‐doped mesoporous hollow carbon sphere (NH2−CdS/NMHCS) for highly efficient CO2RR is presented. The prepared NH2−CdS/NMHCS exhibits a high CO Faradaic efficiency (FECO) exceeding 90% from −0.8 to −1.1 V versus reversible hydrogen electrode (RHE) with the highest FECO of 95% at −0.9 V versus RHE in H cell. Additional experimental and theoretical investigations demonstrate that the alkaline −NH2 group functions as a potent trapping site, effectively adsorbing the acidic CO2, and subsequently triggering CO2 spillover to CdS. The amino modification‐induced CO2 spillover, combined with electron redistribution between CdS and NMHCS, not only readily achieves the spontaneous activation of CO2 to *COOH but also greatly reduces the energy required for the conversion of *COOH to *CO intermediate, thus endowing NH2−CdS/NMHCS with significantly improved reaction kinetics and reduced overpotential for CO2‐to‐CO conversion. It is believed that this research can provide valuable insights into the development of electrocatalysts with superior CO2 adsorption and activation capabilities for CO2RR application.