Computational Design of a Two-Dimensional Copper Carbide Monolayer as a Highly Efficient Catalyst for Carbon Monoxide...

Rationally designing stable and low-cost electrocatalysts with high efficiency is of great significance for the large-scale electrochemical reduction of carbon monoxide (eCOR) to high-value-added multicarbon products. Inspired by the tunable atomic structures, abundant active sites, and excellent properties of two-dimensional (2D) materials, in this work, we designed several novel 2D C-rich copper carbide materials as eCOR electrocatalysts by performing an extensive structural search and comprehensive first-principles computations. According to the computed phonon spectra, formation energies, and ab initio molecular dynamics simulations, we screened out two highly stable candidates, i.e., CuC₂ and CuC₅ monolayers with metallic features. Interestingly, the predicted 2D CuC₅ monolayer exhibits superior eCOR performance for C₂H₅OH synthesis with high catalytic activity (low limiting potential of -0.29 V and small activation energy for C-C coupling of 0.35 eV) and high selectivity (significant suppressing effect on the side reactions). Thus, we predicted that the CuC₅ monolayer holds great potential as an eligible electrocatalyst for CO conversion to multicarbon products, which could motivate more study to develop highly efficient electrocatalysts in similar binary noble-metal compounds.