No abstract

The electrochemical CO 2 reduction reaction (CO 2 RR) over Cu-based catalysts shows great potential for converting CO 2 into multicarbon (C 2 + ) fuels and chemicals. Herein, we introduce an A 2 M 2 O 7 structure into a Cu-based catalyst through a solid-state reaction synthesis method. The Cu 2 P 2 O 7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO 2 RR conditions. The reconstructed Cu 2 P 2 O 7 catalyst achieves a Faradaic efficiency of 73.6 % for C 2 + products at an applied current density of 350 mA cm À 2 , remarkably higher than the CuO counterparts. The reconstructed Cu 2 P 2 O 7 catalyst has a high electrochemically active surface area, abundant defects, and low-coordinated sites. In situ Raman spectroscopy and density functional theory calculations reveal that CO adsorption with bridge and atop configurations is largely improved on Cu with defects and low-coordinated sites, which decreased the energy barrier of the CÀ C coupling reaction for C 2 + products.