Mesoporous Copper‐Based Metal‐Organic Framework Flakes as a Promising Platform for Electrosynthesis of Ethylene from Carbon Dioxide

Developing practical electrocatalysts for carbon dioxide electroreduction (CO2RR) requires a synergy of sustainable synthesis and high performance. Here, we report a one-pot green synthesis of a flake-like, mesoporous copper-based metal-organic framework (Cu-MOF) optimized for CO2 conversion. Spectroscopic analysis confirms a coordination environment of Cu2+ centers tetragonally bonded to nitrogen atoms, characteristic of zeolitic imidazolate frameworks (ZIFs). This flake-like architecture and mesoporosity facilitate rapid mass transport and ensure maximum site accessibility. By maintaining optimally spaced Cu centers, the framework modulates the surface coverage of reaction intermediates, effectively promoting C–C dimerization toward multicarbon products. Operating in a zero-gap cell, the Cu-MOF achieves a Faradaic efficiency of 51.6% for ethylene at an industrially relevant current density of 200 mA cm–2. Furthermore in-situ X-ray absorption spectroscopy (XAS) reveals a reversible restructuring into metallic Cu active species with negligible dissolution, demonstrating the robust potential of this green-synthesized catalyst for scalable CO2 electrolysis.