Dynamic Restructuring of Cu₇S₄/Cu for Efficient CO₂ Electro-reduction to Formate

Optimized catalytic properties and reactant adsorption energy played a crucial role in promoting CO₂ electrocatalysis. Herein, Cu₇S₄/Cu underwent in situ dynamic restructuring to generate S-Cu₂O/Cu hybrid catalyst for effective electrochemical CO₂ reduction to formate that outperformed Cu₂O/Cu and Cu₇S₄. Thermodynamic and in situ Raman spectra revealed that the optimized adsorption of the HCOO* intermediate on S-Cu₂O/Cu was regulated and the H₂ pathway (surface H) was suppressed by S-doping. Meanwhile, Cu₇S₄/Cu nanoflowers created abundant boundaries for ECR and strengthened the CO₂ adsorption by inducing Cu. These findings provide a new perspective on synthetic methods for various electrocatalytic reduction processes.