Theoretically Designed Cu10Sn3‐Cu‐SnOx as Three‐Component Electrocatalyst for Efficient and Tunable CO2 Reduction to Syngas

Abstract

AbstractElectrocatalytic transformation of CO2 to various syngas compositions is an exceedingly attractive approach to carbon‐neutral recycling. Meanwhile, the achievement of selectivity, stability, and tunability of product ratios using single‐component electrocatalysts is challenging. Herein, the theoretically‐assisted design of the triple‐component nanocomposite electrocatalyst Cu10Sn3‐Cu‐SnOx that addresses this challenge is presented. It is shown that Cu10Sn3 is a valuable electrocatalyst for suitable CO2 reduction to CO, SnO2 for CO2 reduction to formate at large overpotentials, and that the Cu–SnO2 interface facilitates H2 evolution. Accordingly, the interaction between the three functional components affords tunable CO/H2 ratios, from 1:2 to 2:1, of the produced syngas by controlling the applied potentials and relative contents of functional components. The syngas generation is selective (Faradaic efficiency, FE = 100%) at relatively lower cathodic potentials, whereas formate is the only liquid product detected at relatively higher cathodic potentials. The theoretically guided design approach therefore provides a new opportunity to boost the selectivity and stability of CO2 reduction to tunable syngas.