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Springer Science and Business Media LLC Nano-Micro Letters 16(1)
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    초록·키워드

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

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