Selective CO₂ Electroreduction to Multi-Carbon Products on Organic-Functionalized CuO Nanoparticles by Local Micro-Environment Modulation.

ABSTRACT: Surface functionalization of Cu-based catalysts has demonstrated promising potential for enhancing the electrochemical CO₂ reduction reaction (CO₂RR) toward multi-carbon (C₂₊) products, primarily by suppressing the parasitic hydrogen evolution reaction and facilitating a localized CO₂/CO concentration at the electrode. Building upon this approach, we developed surface-functionalized catalysts with exceptional activity and selectivity for electrocatalytic CO₂RR to C₂₊ in a neutral electrolyte. Employing CuO nanoparticles coated with hexaethynylbenzene organic molecules (HEB-CuO NPs), a remarkable C₂₊ Faradaic efficiency of nearly 90% was achieved at an unprecedented current density of 300 mA cm^-2, and a high FE (> 80%) was maintained at a wide range of current densities (100-600 mA cm^-2) in neutral environments using a flow cell. Furthermore, in a membrane electrode assembly (MEA) electrolyzer, 86.14% FE_C2+ was achieved at a partial current density of 387.6 mA cm^-2 while maintaining continuous operation for over 50 h at a current density of 200 mA cm^-2. In-situ spectroscopy studies and molecular dynamics simulations reveal that reducing the coverage of coordinated K⋅H₂O water increased the probability of intermediate reactants (CO) interacting with the surface, thereby promoting efficient C-C coupling and enhancing the yield of C₂₊ products. This advancement offers significant potential for optimizing local micro-environments for sustainable and highly efficient C₂₊ production.

SUBMITTER: Ren S 

PROVIDER: S-EPMC11310183 | biostudies-literature | 2024 Aug

REPOSITORIES: biostudies-literature