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

Abstract

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.