Promoting Electrocatalytic Reduction of CO₂ to C₂H₄ Production by Inhibiting C₂H₅OH Desorption from Cu₂O/C Composite

Abstract

The electrochemical CO₂ reduction reaction (CO₂ RR) has great potential in realizing carbon recycling while storing sustainable electricity as hydrocarbon fuels. However, it is still a challenge to enhance the selectivity of the CO₂ RR to single multi-carbon (C₂₊ ) product, such as C₂ H₄ . Here, an effective method is proposed to improve C₂ H₄ selectivity by inhibiting the production of the other competitive C₂ products, namely C₂ H₅ OH, from Cu₂ O/C composite. Density functional theory indicates that the heterogeneous structure between Cu₂ O and carbon is expected to inhibit C₂ H₅ OH production and promote CC coupling, which facilitates C₂ H₄ production. To prove this, a composite electrode containing octahedral Cu₂ O nanoparticles (NPs) (o-Cu₂ O) with {111} facets and carbon NPs is constructed, which experimentally inhibits C₂ H₅ OH production while strongly enhancing C₂ H₄ selectivity compared with o-Cu₂ O electrode. Furthermore, the surface hydroxylation of carbon can further improve the C₂ H₄ production of o-Cu₂ O/C electrode, exhibiting a high C₂ H₄ Faradaic efficiency of 67% and a high C₂ H₄ current density of 45 mA cm^-2 at -1.1 V in a near-neutral electrolyte. This work provides a new idea to improve C₂₊ selectivity by controlling products desorption.