Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO2 into glycerol carbonate

doi:10.1016/j.cjche.2024.05.014

中国化学工程学报 ›› 2024, Vol. 72 ›› Issue (8): 153-163.DOI: 10.1016/j.cjche.2024.05.014

Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO₂ into glycerol carbonate

Xufang Chen¹, Xin Shu¹, Yanru Zhu^1,2, Jian Zhang^1,2, Zhigang Chai¹, Hongyan Song¹, Zhe An^1,2, Jing He^1,2

1 State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2 Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China

收稿日期:2023-12-22 修回日期:2024-05-20 出版日期:2024-08-28 发布日期:2024-10-17
通讯作者: Xin Shu,E-mail:shuxin@mail.buct.edu.cn;Zhe An,E-mail:anzhe@mail.buct.edu.cn.Tel.:+86-10-64425280;fax:+86-10-64425385
基金资助:
Financial support from the National Key Research and Development Program of China (2022YFB3805602), the National Natural Science Foundation of China (22138001, 22288102), and the Fundamental Research Funds for the Central Universities is acknowledged.

Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO₂ into glycerol carbonate

Xufang Chen¹, Xin Shu¹, Yanru Zhu^1,2, Jian Zhang^1,2, Zhigang Chai¹, Hongyan Song¹, Zhe An^1,2, Jing He^1,2

1 State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2 Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China

Received:2023-12-22 Revised:2024-05-20 Online:2024-08-28 Published:2024-10-17
Contact: Xin Shu,E-mail:shuxin@mail.buct.edu.cn;Zhe An,E-mail:anzhe@mail.buct.edu.cn.Tel.:+86-10-64425280;fax:+86-10-64425385
Supported by:
Financial support from the National Key Research and Development Program of China (2022YFB3805602), the National Natural Science Foundation of China (22138001, 22288102), and the Fundamental Research Funds for the Central Universities is acknowledged.

摘要/Abstract

摘要： Glycerol carbonate, an important glycerol value-added product, has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics, detergents, chemical intermediates, polymers, and so on. The direct carbonylation from glycerol with CO₂ is considered a promising route, but still tough work due to the thermodynamic stability and the kinetic inertness of CO₂. In this work, highly-selective direct carbonylation of glycerol and CO₂ into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides (MgInCe-MMO), which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides (MgInCe-LDHs). By precisely modulating the surface basic-acidic properties and the oxygen vacancies, an efficient carbonylation of glycerol with CO₂ has been achieved with a selectivity of up to >99% to glycerol carbonate. Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.

关键词: Catalytic reaction engineering, Glycerol carbonate, Direct carbonylation from glycerol, Carbon dioxide, Mixed metal oxides, Synergistic catalysis

Abstract: Glycerol carbonate, an important glycerol value-added product, has been widely used as an active intermediate and inert solvent in the synthesis of cosmetics, detergents, chemical intermediates, polymers, and so on. The direct carbonylation from glycerol with CO₂ is considered a promising route, but still tough work due to the thermodynamic stability and the kinetic inertness of CO₂. In this work, highly-selective direct carbonylation of glycerol and CO₂ into glycerol carbonate has been achieved over highly dispersed MgInCe-mixed metal oxides (MgInCe-MMO), which were prepared through the topological transformation derived from the MgInCe-layered double hydroxides (MgInCe-LDHs). By precisely modulating the surface basic-acidic properties and the oxygen vacancies, an efficient carbonylation of glycerol with CO₂ has been achieved with a selectivity of up to >99% to glycerol carbonate. Deep investigation into the synergistic catalysis of base-acid sites and oxygen vacancies has been clarified.

Key words: Catalytic reaction engineering, Glycerol carbonate, Direct carbonylation from glycerol, Carbon dioxide, Mixed metal oxides, Synergistic catalysis

Xufang Chen, Xin Shu, Yanru Zhu, Jian Zhang, Zhigang Chai, Hongyan Song, Zhe An, Jing He. Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO₂ into glycerol carbonate[J]. 中国化学工程学报, 2024, 72(8): 153-163.

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Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO₂ into glycerol carbonate

Highly dispersed MgInCe-mixed metal oxides catalyzed direct carbonylation of glycerol and CO₂ into glycerol carbonate

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