共 54 条
Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO2 over Au/Co3O4-ZnO Catalyst
被引:2
作者:
Li, Yajin
[1
]
Liu, Huimin
[2
]
Ma, Lan
[3
]
Liu, Jiaxiong
[1
]
He, Dehua
[1
]
机构:
[1] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[2] Liaoning Univ Technol, Sch Chem & Environm Engn, Jinzhou 121001, Liaoning, Peoples R China
[3] Inst NBC Def, Beijing 102205, Peoples R China
基金:
中国国家自然科学基金;
关键词:
CO;
2;
utilization;
Glycerol carbonylation;
Glycerol carbonate;
Plasmonic metal;
Photo-thermal catalysis;
PHOTOCATALYTIC ACTIVITY;
ELECTROCHEMICAL SENSOR;
NONRENEWABLE ENERGY;
CONVERSION;
ADSORPTION;
DIOXIDE;
FTIR;
HYDROGENATION;
NANOCATALYST;
PERFORMANCE;
D O I:
10.3866/PKU.WHXB202308005
中图分类号:
O64 [物理化学(理论化学)、化学物理学];
学科分类号:
070304 ;
081704 ;
摘要:
Glycerol carbonylation with CO 2 to synthesize glycerol carbonate is a promising approach for CO 2 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/20Co 3 O 4 -ZnO catalysts, where Co 3 O 4 -ZnO, a composite of p -type semiconductor Co 3 O 4 and n -type semi -conductor ZnO, exhibited a heterojunction structure, and Au nanoparticles loaded onto the surface of Co 3 O 4 -ZnO revealed the localized surface plasmon resonance (LSPR). We investigated the ability of x Au/Co 3 O 4 -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/Co 3 O 4 -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 x Au/Co 3 O 4 -ZnO. Our findings revealed that the heterojunction structure of Au/20Co 3 O 4 -ZnO facilitated visible light absorption and hole -electron pair separation. The size of Au nano -particles (NPs) loaded on Co 3 O 4 -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 Co 3 O 4 -ZnO surface. The LSPR of Au NPs further enhanced the visible light absorption capacity of Au/20Co 3 O 4 -ZnO, and improved the separating of photogenerated hole -electron pairs, thus enhancing the photothermal catalytic performances. With the optimizing conditions (150 degrees C, 5 MPa, 6 h, and 225 W visible light irradiation), the 2%Au/20Co 3 O 4 -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 CO 2 to produce glycerol carbonate in the future.
引用
收藏
页数:12
相关论文