Electrocatalytic CO2 reduction to ethylene in an acid-fed membrane electrode assembly at 10 A

Abstract

Abstract Electrocatalytic CO 2 reduction reaction (CO 2 RR) using membrane electrode assembly (MEA) systems requires complex regulation of protons, hydroxyls, carbonate ions and alkali-metal ions across both electrodes to efficiently produce multicarbon products. In acid-fed CO₂RR MEAs, excessive proton migration and accumulation on the catalyst surface suppress CO₂ adsorption and promote hydrogen evolution, leading to low Faradaic and energy efficiencies. Sluggish hydroxide transport further triggers carbonate precipitation, undermining system stability. Here we report an acid-fed membrane electrode assembly system for highly efficient CO 2 RR by integrating hydrazone-linked covalent organic framework (COF) and catalyst on the anion-exchange membrane to enable bidirectional pathway for hydroxide and potassium ions diffusion, while enhancing transport of CO 2 to the catalyst surface. As a result, the scaled-up MEA operates at a full-cell voltage of ~4.5 V under a total current of 10 A (current density of 204 mA cm⁻²), delivering a Faradaic efficiency of ~50% for CO₂-to-C₂H₄ conversion and maintaining stability for over 300 hours.