Plasmon-Enhanced C₂H₄ Generation in the CO₂ Electroreduction Reaction on a CuPd Tandem Catalyst

Abstract

High Resolution Image Download MS PowerPoint Slide Electrocatalysis enables the conversion of CO 2 into value-added fuels and chemicals, offering a sustainable solution for greenhouse gas mitigation. However, achieving high selectivity for C2 products like ethylene (C 2 H 4 ) remains challenging due to competing C1 pathways and complex multielectron processes. Here, we demonstrate that plasmon resonances can selectively enhance the electroreduction of CO 2 to C 2 H 4 by 27.0% on a CuPd catalyst under LED illumination (625 nm) at −1.3 V RHE . Photocurrent response, in situ FTIR spectroscopy, and COMSOL simulations reveal that plasmon-derived hot electrons and heating greatly facilitate *CO formation at the CuPd interface, which diffuses to the Cu surface for subsequent C–C coupling. DFT calculations show that the increased *CO coverage on the Cu sites reduces the energy barrier for C–C coupling, ultimately enhancing C 2 H 4 generation. This work offers valuable mechanistic insights into plasmon-mediated electrocatalysis, guiding the development of more efficient plasmonic tandem electrocatalysts for future carbon recycling technologies.