Tailoring Solvent-Mediated CO₂ Reservoirs at Heterointerfaces for Enhanced Electrochemical CO₂-to-C₂H₄ Conversion

Transforming waste CO2 into value-added fuels and chemicals, while simultaneously enabling renewable electricity storage, presents a viable strategy for achieving a sustainable energy economy. However, efficient conversion to C2+ products remains challenging, primarily due to the low CO2 concentration at the catalyst surface in aqueous environments. Herein, we addressed this issue by designing Cu2O-MgO catalysts with abundant nanointerfaces serving as effective CO2 reservoirs under aqueous conditions. Ab initio molecular dynamics simulations demonstrated that these interfaces substantially enhanced the CO2 stabilization at the surface, effectively inhibiting their displacement by interfacial water molecules. This localized CO2 enrichment facilitated C–C coupling kinetics and selectively promoted the formation of target products. Building on these findings, we synthesized a model catalyst featuring abundant Cu2O-MgO nanointerfaces…