Theoretically Designed Cu₁₀Sn₃-Cu-SnO_x as Three-Component Electrocatalyst for Efficient and Tunable CO₂ Reduction to...

Electrocatalytic 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-SnO_x 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.