Preparation of Cu single atoms on N-doped carbon materials with supercritical CO2 deposition

Cu single atoms dispersed on N-doped carbon materials (Cu-NC) were obtained after supercritical CO 2 deposition and decompression, without further post-treatment. AC-HAADF-STEM, STEM , XRD , ICP-OES, and XPS results confirmed that the Cu atoms were equably dispersed over the N-doped carbon (NC) support with the loading of 0.80 wt%. The catalytic performance of Cu-NC in solvent-free oxidation of phenylcarbinol to benzaldehyde was investigated, and the conversion of 73.9% and selectivity of 85.7% were obtained at 50 °C for 1 h. A high-pressure view cell was used to observe the dissolution and diffusion for Cu(acac) 2 in scCO 2 . The stability of Cu-NC structures and the formation path of active oxygen species (O*) on different configurations were predicted by density functional theory (DFT) calculations, and CuN 3 C 1 was found to be more conducive to the activation of tert-butyl hydroperoxide (TBHP).