Citation: Yajin Li, Huimin Liu, Lan Ma, Jiaxiong Liu, Dehua He. Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO₂ over Au/Co₃O₄-ZnO Catalyst[J]. Acta Physico-Chimica Sinica, ;2024, 40(9): 230800. doi: 10.3866/PKU.WHXB202308005 shu

Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO₂ over Au/Co₃O₄-ZnO Catalyst

Yajin Li ¹ ,
Huimin Liu ^2,, ,
Lan Ma ³ ,
Jiaxiong Liu ¹ ,
Dehua He ^1,,

1.
Department of Chemistry, Tsinghua University, Beijing 100084, China
2.
School of Chemical and Environmental Engineering, Liaoning University of Technology, Jinzhou 121001, Liaoning Province, China
3.
Institute of NBC Defense, Beijing 102205, China

Corresponding author: Huimin Liu, liuhuimin08@tsinghua.org.cn Dehua He, hedeh@mail.tsinghua.edu.cn
Received Date: 3 August 2023
Revised Date: 6 October 2023
Accepted Date: 10 October 2023
Available Online: 16 October 2023
Fund Project: the National Natural Science Foundation of China 21573120Education Department of Liaoning Province JQL202015401

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 xAu/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 ℃, 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.
- CO₂ utilization,
- Glycerol carbonylation,
- Glycerol carbonate,
- Plasmonic metal,
- Photo-thermal catalysis
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Photothermal Synthesis of Glycerol Carbonate via Glycerol Carbonylation with CO₂ over Au/Co₃O₄-ZnO Catalyst