Enhancing local K+ adsorption by high-density cube corners for efficient electroreduction of CO2 to C2+ products.

Abstract

Reducing carbon dioxide (CO2) to high value-added chemicals using renewable electricity is a promising approach to reducing CO2 levels in the air and mitigating the greenhouse effect, which depends on high-efficiency electrocatalysts. Copper-based catalysts can be used for electroreduction of CO2 to produce C2+ products with high added value, but suffer from poor stability and low selectivity. Herein, we propose a strategy to enhance the field effect by varying the cubic corner density on the surface of Cu2O microspheres for improving the electrocatalytic performance of CO2 reduction to C2+ products. Finite element method (FEM) simulation results show that the high density of cubic corners helps to enhance the local electric field, which increases the K+ concentration on the catalyst surface. The results of CO2 electroreduction tests show that the FEC2+ of the Cu2O catalyst with high-density cubic corners is 71% at a partial current density of 497 mA cm-2. Density functional theory (DFT) calculations reveal that Cu2O (111) and Cu2O (110) can effectively reduce the energy barrier of C-C coupling and improve the FEC2+ at high K+ concentrations relative to Cu2O (100). This study provides a new perspective for the design and development of efficient CO2RR catalysts.