Electrochemical CO 2 reduction to multicarbon products with CuAg catalysts Preetam K. Sharma 1,2 , Santhosh Matam 3 , Ye Ma 1 , Da Li 1,4 , Alberto Roldan 5 , M. Danish Khan 1 , C. Richard A. Catlow 3,5,6 , Bhavin Siritanaratkul 7 , Alexander J. Cowan 7 , Eileen Hao Yu 1,8 * 1 Department of Chemical Engineering, Loughborough University, Loughborough, LE11 3TU, UK, 2 Institute for Materials Discovery, University College London, Malet Place, London, WC1E 7JE UK, 3 UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Oxford, OX11 0FA, UK, 4 State Key Laboratory of Urban Water Resource and Environment, School of Environment, Harbin Institute of Technology, Harbin, 150090, China, 5 Cardiff Catalysis Institute, School of Chemistry, Cardiff University, Park Place, Cardiff, CF10 3AT, UK, 6 Dept of Chemistry University College London, 20 Gordon St., London WC1 HOAJ, UK, 7 Department of Chemistry, University of Liverpool, Liverpool, L69 7ZX, 8 School of Chemistry and Chemical Engineering, University of Southampton, Southampton, SO17 1BJ The production of multicarbon chemicals from electrochemical CO2 reduction can provide fuels and feedstock for the chemical industry. In this work, we modified the surface of CuOx gas diffusion electrodes (GDEs) with Ag using a simple electrochemical method. The prepared catalysts were tested in a three-chamber flow GDE reactor to determine their electrochemical performance and product distribution resulting from the CO2 reduction reaction. Several products were obtained, including carbon monoxide, ethylene, ehtanol, 1-propanol, and hydrogen. The addition of Ag on the surface of Cu-GDE promoted the formation of C2+ carbon products and suppressed hydrogen evolution. CuOx GDE electrode with 8 min Ag deposition resulted in the highest C2+ faradaic efficiency of >60% with 130 mA cm-2 current density at -1.15 V vs RHE. The in-situ X-ray photoelectron and Raman spectroscopic investigations indicate that the reduction of copper oxide is slower in CuOx-Ag GDE compared to CuOx GDE. Furthermore, from the density functional theory analysis, Ag promotes Cu atoms migration towards the surface of the electrode, which seems to adsorb generated CO for the further reduction process to produce higher carbonaceous products.
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