Tensile-Strained Cu Penetration Electrode Boosts Asymmetric C-C Coupling for Ampere-Level CO2-to-C2+ Reduction in Acid

Angew Chem Int Ed Engl. 2024 Oct 7;63(41):e202407612. doi: 10.1002/anie.202407612. Epub 2024 Sep 6.

Abstract

The synthesis of multicarbon (C2+) products remains a substantial challenge in sustainable CO2 electroreduction owing to the need for sufficient current density and faradaic efficiency alongside carbon efficiency. Herein, we demonstrate ampere-level high-efficiency CO2 electroreduction to C2+ products in both neutral and strongly acidic (pH=1) electrolytes using a hierarchical Cu hollow-fiber penetration electrode (HPE). High concentration of K+ could concurrently suppress hydrogen evolution reaction and facilitate C-C coupling, thereby promoting C2+ production in strong acid. By optimizing the K+ and H+ concentration and CO2 flow rate, a faradaic efficiency of 84.5 % and a partial current density as high as 3.1 A cm-2 for C2+ products, alongside a single-pass carbon efficiency of 81.5 % and stable electrolysis for 240 h were demonstrated in a strong acidic solution of H2SO4 and KCl (pH=1). Experimental measurements and density functional theory simulations suggested that tensile-strained Cu HPE enhances the asymmetric C-C coupling to steer the selectivity and activity of C2+ products.

Keywords: Acidic CO2 Electroreduction; Ampere-Level; Asymmetric C−C Coupling; Cu Penetration Electrode; Tensile-Strain.