Abstract
Multicomponent heterogeneous catalysts present excellent catalytic performance attributed to the synergistic effect of multi-sites.Nevertheless,identifying the composition of the multi-sites and exploring the synergistic catalytic mechanisms for the multiple active sites in electrocatalytic CO2 reduction reaction(CO2RR)still lack intensive study.This work regulates the chemical composition of Cu-based nanoreactors readily by adjusting the geometrical morphology of metal-organic frameworks precursor.The obtained cuboctahedron nanoreactor containing CU-N4/Cu2O/CU multiple active sites exhibits excellent CO2RR selectivity towards deep reduction product(80%)with high current density.Moreover,the tandem catalytic mechanism of multicomponent active sites has been studied intensively.The CO2 molecule is firstly reduced in CU-N4 sites to form CO and then the CO is transfered to Cu2O/Cu sites for further deep reduction.The high concentration of CO provided by CU-N4 sites decreases the free energy of rate-determining step for CH4 products in Cu2O sites.This work provides a promising direction for designing and synthesizing multicomponent Cu-based tandem catalysts to access high efficiency and selectivity in the electrocatalytic CO2 reduction reaction.
NSTL