物理化学学报2024，Vol.40Issue(9)：84-86,3.DOI:10.3866/PKU.WHXB202308005
Au/Co3O4-ZnO催化剂上CO2-丙三醇羰基化合成丙三醇碳酸酯
Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO2 over Au/Co3O4-ZnO Catalyst
摘要
Abstract
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.关键词
CO2利用/丙三醇羰基化/丙三醇碳酸酯/等离子体金属/光热催化Key words
CO2 utilization/Glycerol carbonylation/Glycerol carbonate/Plasmonic metal/Photo-thermal catalysis分类
化学化工引用本文复制引用
李亚晋,刘会敏,马兰,刘佳雄,贺德华..Au/Co3O4-ZnO催化剂上CO2-丙三醇羰基化合成丙三醇碳酸酯[J].物理化学学报,2024,40(9):84-86,3.基金项目
The project was supported by the National Natural Science Foundation of China(21573120)and Education Department of Liaoning Province(JQL202015401).国家自然科学基金(21573120)及辽宁省教育厅基金(JQL202015401)资助项目 （21573120）
