Tailoring Solvent-Mediated CO 2 Reservoirs at Heterointerfaces for Enhanced Electrochemical CO 2 -to-C 2 H 4 Conversion

作者：Jing Yang, Chengkai Jin, Si Di, Fusong Kang, Fen Qiao, Junfeng Wang, Dongjing Liu, Lilin Zhang, Tian Tian, Xunhua Zhao, Yu Zhou, Kang Chen, H.L. Chen, Xiao‐Shun Zhou · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c06799 · 被引用次数：49 · 研究领域：CO2 Reduction Techniques and Catalysts、Ionic liquids properties and applications、Carbon dioxide utilization in catalysis

Transforming waste CO 2 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 C 2+ products remains challenging, primarily due to the low CO 2 concentration at the catalyst surface in aqueous environments. Herein, we addressed this issue by designing Cu 2 O-MgO catalysts with abundant nanointerfaces serving as effective CO 2 reservoirs under aqueous conditions. Ab initio molecular dynamics simulations demonstrated that these interfaces substantially enhanced the CO 2 stabilization at the surface, effectively inhibiting their displacement by interfacial water molecules. This localized CO 2 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 Cu 2 O-MgO nanointerfaces and evaluated its performance in aqueous media. Remarkably, flowing electrolyzer tests demonstrated a Faradaic efficiency of 67% for ethylene at a current density of ∼ 240 mA·cm –2 . Subsequent mechanistic investigations combining spectroscopy experiments and theoretical calculation simulations demonstrated that the surface-enriched CO 2 enhanced the CO* coverage at the Cu active sites, thereby promoting ethylene production through facilitated C–C coupling. This study pioneers the rational design of heterogeneous catalysts for selective CO ...