CO2-to-C2H5OH photoconversion by an amorphization-activated catalyst

Abstract

CO₂ photoconversion into value-added C₂ products with high selectivity and efficiency is formidably challenging due to highly energetic and kinetic restriction of C–C coupling. Designing catalysts to overcome those barriers is therefore crucial. Here, for the first time, we demonstrate an amorphization strategy to boost photocatalytic CO₂ ethanolization. By integrating amorphous Pd onto Cd_0.9Zn_0.1S nanorods (a-Pd/CZS), an activity of 412.1 μmol g⁻¹ h⁻¹ and a selectivity of 96.5% for CO₂-to-C₂H₅OH photoconversion were achieved without a sacrificial agent with an apparent quantum efficiency (AQE) of 0.87% at 420 nm. The superior performance results from rapid migration of photogenerated electrons to amorphous Pd via interfacial Ohmic junction. In situ characterization and theoretical calculation further reveal that amorphous Pd can optimize CO₂ adsorption/activation and reduce the C–C coupling energy barrier via intensified interaction and stabilization with a ^∗OCCO intermediate, thereby maximizing conversion efficiency and selectivity. This work highlights an efficient photocatalyst for a CO₂-to-C₂ product and inspires high-performance photocatalyst design.