Synergized Cu/Pb Core/Shell Electrocatalyst for High-Efficiency CO₂ Reduction to C₂₊ Liquids.

Abstract

The design of efficient copper-based (Cu-based) carbon dioxide reduction (CO₂RR) electrocatalysts is crucial for converting CO₂ to value-added liquid products. In this work, we demonstrate that the strong synergy between Cu core and ultrathin lead (Pb) shell (0.7 nm) in the Cu/Pb core/shell nanocrystals (NCs, CuPb-0.7/C) significantly boosts the electrocatalytic reduction of CO₂ toward C₂₊ products (products with at least two carbon atoms). Specifically, when applying in a flow cell system, the Faradaic efficiency (FE) of total C₂₊ products and the selectivity of C₂₊ liquid products are as high as 81.6% and 49.5%, respectively. Moreover, the current density of C₂₊ liquid products reaches 196.8 mA cm^-2, outperforming most of the reported Cu-based catalysts for CO₂RR toward the production of C₂₊ liquid products. Density functional theory calculations indicate that the synergized Cu/Pb core/shell NCs reduce the formation energies of *COOH and *OCCOH intermediates, as the two critical intermediates for the reduction of CO₂ to CO and the formation of C₂₊ products, respectively, and leads to the significant increase in the selectivity of C₂₊ liquid products. This study provides a efficient Cu-based catalyst for the reduction of CO₂, highlighting the importance of synergistic effect for the design of electrocatalysts in catalysis.