A Reconstructed Cu2P2O7 Catalyst for Selective CO2 Electroreduction to Multicarbon Products

The electrochemical CO2 reduction reaction (CO2RR) over Cu-based catalysts shows great potential for converting CO2 into multicarbon (C2+) 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 Cu2P2O7 catalyst is electrochemically reduced to metallic Cu with a significant structure evolution from grain aggregates to highly porous structure under CO2RR conditions. The reconstructed Cu2P2O7 catalyst achieves a Faradaic efficiency of 73.6 % for C2+ products at an applied current density of 350 mA cm(-2), remarkably higher than the CuO counterparts. The reconstructed Cu2P2O7 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 C-C coupling reaction for C2+ products.