Au/Co3O4-ZnO催化剂上CO2-丙三醇羰基化合成丙三醇碳酸酯OA北大核心CSTPCD

Glycerol carbonylation with CO2 to synthesize glycerol carbonate is a promising approach for CO2 utilization.This reaction can be achieved through a thermally-driven catalytic pathway,but it is constrained by thermodynamic equilibrium.In the present study,we introduced solar energy into the reaction system to enable a photo-thermal synergistic catalytic reaction,breaking through the thermodynamic limitations.We developed a series of x Au/20Co3O4-ZnO catalysts,where Co3O4-ZnO,a composite of p-type semi-conductor Co3O4 and n-type semi-conductor ZnO,exhibited a heterojunction structure,and Au nanoparticles loaded onto the surface of Co3O4-ZnO revealed the localized surface plasmon resonance(LSPR).We investigated the ability of xAu/Co3O4-ZnO to absorb visible light absorption,the efficiency of separating photo-generated hole-electron pairs,and the impact of Au on the photothermal synergistic catalytic performances of Au/Co3O4-ZnO catalysts.We also examined the effects of Au doping on the bulk and surface properties,including crystalline structures,morphologies,specific surface areas and pore structures,the binding energies of the elements,surface acid-base sites,and reduction behaviors of xAu/Co3O4-ZnO.Our findings revealed that the heterojunction structure of Au/20Co3O4-ZnO facilitated visible light absorption and hole-electron pair separation.The size of Au nano-particles(NPs)loaded on Co3O4-ZnO surface was approximately 50 nm.The loading of Au altered the electron density of Co and Zn,improved the reducibility of Co species,and enhanced the presence of oxygen vacancies on Co3O4-ZnO surface.The LSPR of Au NPs further enhanced the visible light absorption capacity of Au/20Co3O4-ZnO,and improved the separating of photogenerated hole-electron pairs,thus enhancing the photothermal catalytic performances.With the optimizing conditions(150 °C,5 MPa,6 h,and 225 W visible light irradiation),the 2%Au/20Co3O4-ZnO catalyst demonstrated excellent performances,yielding a glycerol carbonate yield of 6.5%.This study is expected to serve as a reference for the rational design of improved photothermal catalysts for glycerol carbonylation with CO2 to produce glycerol carbonate in the future.