Atomic level dispersed nickel coupled with silver nanoparticle to boost the efficiency of CO2 conversion to CO via spin electrons regulation

Modulating the electronic configuration by coupling multi-scale active sites for electrocatalytic conversion of CO 2 to CO is extremely challenging in terms of structural analysis and mechanism elucidation. Herein, a catalyst NiAD/AgNPs@CN with both atomic-level dispersed Ni and Ag nanoparticles on N-doped carbon substrate has been designed to reveal the true active sites and catalytic mechanism in complex materials. NiAD/AgNPs@CN exhibits CO Faraday efficiency (FE CO ) of 99.97% at −0.88 V (vs. RHE) in H-type cell and 91.77% FE CO with a high current density of 79.70 mA/cm 2 in flow cell. DFT calculations show that the tiny change in the energy level of spin electrons at atomic sites has a significant impact on the CO 2 activation. The regulation of atomic Ni on Ag sites is the main reason for improving CO 2 RR performance. This work gives a new understanding on the catalytic mechanism of composite materials structured by atomic-level dispersed metal and nanoparticles.