Efficient Conversion of Carbon Dioxide on Atomically Dispersed Metal-Nx Species-Anchored Porous Carbon with Embedded CuxCoy Nanoparticles by Accelerating Electron Separation

摘要

To promote methanol product selectivity in CO2 reduction through photoelectrochemical reactions, a novel hybrid electrocatalyst (CuCo/NC) was developed to enhance electron transfer from cobalt to copper atoms with coordinated nitrogen on a ZIF-derived carbon matrix. The binding energies of Co 2p3/2 in CuCo/NC exhibited a 0.2 eV shifting to lower values, whereas those of Cu 2p3/2 exhibited a lower value shift by 1.5 eV, both of which contributed to electron transfer from Co to Cu. DFT calculations showed that the C-Co bond length (1.808 A) between the CO* intermediate and CuCo/NC electrocatalyst was shorter than those in Cu/NC and Co/NC (1.946 and 1.870 A, respectively), indicating that CO* was easier to adsorb on the CuCo/NC electrocatalyst for further reduction. The CuCo/NC electrocatalyst with stable properties efficiently converted CO2 into methanol (FE > 60%) with a carbon atom conversion rate of 4098 nmol h(-1) cm(-2) .