Au/Co3O4-ZnO催化剂上CO2-丙三醇羰基化合成丙三醇碳酸酯

引用本文: 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): 230800. doi: 10.3866/PKU.WHXB202308005 shu

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

Au/Co₃O₄-ZnO催化剂上CO₂-丙三醇羰基化合成丙三醇碳酸酯

李亚晋 ^1, ,
刘会敏 ^{2,
,} ,
马兰 ^3, ,
刘佳雄 ^1, ,
贺德华 ^{1,
,}

1.
清华大学化学系, 北京 100084;
2.
辽宁工业大学化学与环境工程学院, 辽宁锦州 121001;
3.
防化学院, 北京 102205

通讯作者: 刘会敏,Email:liuhuimin08@tsinghua.org.cn; 贺德华,Email:hedeh@mail.tsinghua.edu.cn

基金项目:
国家自然科学基金(21573120)及辽宁省教育厅基金(JQL202015401)资助项目

摘要: CO₂与丙三醇羰基化合成丙三醇碳酸酯是一项前景广阔的CO₂利用途径。尽管该反应可以通过热驱动的催化途径实现，但受热力学平衡的限制。在本研究中，我们开发了xAu/20Co₃O₄-ZnO系列催化剂，并引入太阳光辐射能量来实现光热协同催化反应，以突破热力学限制。由p型半导体Co₃O₄和n型半导体ZnO复合而成的Co₃O₄-ZnO氧化物具有异质结构，而负载于Co₃O₄-ZnO表面的Au纳米粒子具有局域表面等离子体共振(LSPR)效应。我们研究了xAu/20Co₃O₄-ZnO的可见光吸收性能、光生电子-空穴对分离效率以及Au添加对xAu/20Co₃O₄-ZnO催化剂光热协同催化性能的影响。此外，我们还研究了Au掺杂对xAu/20Co₃O₄-ZnO的体相和表面性质(晶相结构、形貌、比表面积、元素结合能、表面酸碱性、还原行为)的影响。研究结果显示，Au/20Co₃O₄-ZnO的异质结构有助于吸收可见光并提高电子-空穴对的分离效率。负载于Co₃O₄-ZnO表面的Au纳米颗粒约为50 nm，Au的加入改变了Zn和Co的电子密度，增强了Co物种的还原性，并增加了Co₃O₄-ZnO表面的氧空位。此外，Au纳米粒子的LSPR进一步提高了Au/20Co₃O₄-ZnO的可见光吸收能力，并改善了光生电子-空穴对的分离，从而提高了光热协同催化性能。在优化的条件下(150 °C、5 MPa、6 h、25 W可见光照射)，2%Au/20Co₃O₄-ZnO表现出良好的光热协同催化性能，丙三醇碳酸酯的产率为6.5%。这项工作有望为合理设计更好的CO₂-丙三醇羰基化制丙三醇碳酸酯光热催化剂提供参考。

关键词:

English

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, ; Dehua He,

Received Date: 03 August 2023
Accepted Date: 10 October 2023
Revised Date: 06 October 2023
Available Online: 16 October 2023
Fund Project:
The project was supported by the National Natural Science Foundation of China (21573120) and Education Department of Liaoning Province (JQL202015401).

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 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 °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.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

Au/Co₃O₄-ZnO催化剂上CO₂-丙三醇羰基化合成丙三醇碳酸酯

通讯作者: 刘会敏,Email:liuhuimin08@tsinghua.org.cn; 贺德华,Email:hedeh@mail.tsinghua.edu.cn

English

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

Corresponding author: Huimin Liu, ; Dehua He,

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