Effect of ionic radius and valence state of alkali and alkaline earth metals on promoting the catalytic performance of La2O3 catalysts for glycerol carbonate production

Jialin Yu; Ke Wang; Shibo Shao; Wei Li; Shangfeng Du; Xianfeng Chen; Cong Chao; Xianfeng Fan

doi:10.1016/j.cej.2023.141486

Effect of ionic radius and valence state of alkali and alkaline earth metals on promoting the catalytic performance of La₂O₃ catalysts for glycerol carbonate production

Jialin Yu, Ke Wang, Shibo Shao, Wei Li, Shangfeng Du, Xianfeng Chen, Cong Chao^*, Xianfeng Fan^*

^*Corresponding author for this work

Chemical Engineering

Research output: Contribution to journal › Article › peer-review

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Abstract

Alkali metals and alkaline earth metals have been used to promote the catalytic performance of metal oxides in transesterification of glycerol and dimethyl carbonate, however, the promotional roles of the dopants in influencing the catalytic performance of the metal oxides have not been fully investigated which hinder the development of low-cost and high-efficiency catalysts in transesterification of glycerol and dimethyl carbonate. This paper, for the first time, systematically studied the influence of ionic radius and valence state of dopants, surface concentration of dopants and the basicity of the catalysts on the catalytic performance of La₂O₃ in transesterification of glycerol and dimethyl carbonate. Our results suggest that the ionic radius and valence state of the dopants are the determining factors, while the basic site density is not a crucial factor, although the basicity of catalyst surface is important in activating glycerol and dimethyl carbonate. Among alkali and alkaline earth metals, 25 mol% Na/La₂O₃ catalyst achieved the highest glycerol conversion (85 %) and glycerol carbonate yield (60 %) in the 70 °C and 2-hour reaction. After the detailed investigation, a plausible mechanism of glycerol and dimethyl carbonate transesterification on Na/La₂O₃ catalyst has been proposed. This research could help understand the promotional role of alkali metals and alkaline earth metals and the results may guide future design of metal oxide catalysts.

Original language	English
Article number	141486
Number of pages	12
Journal	Chemical Engineering Journal
Volume	458
Early online date	18 Jan 2023
DOIs	https://doi.org/10.1016/j.cej.2023.141486
Publication status	Published - 15 Feb 2023

Bibliographical note

Funding Information:
Thanks to the financial support from the UK research council EPSRC (EP/V041665/1). The authors appreciate Mr Fergus Dingwall from School of Engineering in The University of Edinburgh for all his technical support; Dr. Laetitia Pichevin and Dr. Nicola Cayzer from School of Geoscience in The University of Edinburgh for their kind help on ICP-OES and SEM analysis; and Dr. Gary Nichol from School of Chemistry in The University of Edinburgh for providing XRD facility and valuable advice.

Publisher Copyright:
© 2023 The Authors

Keywords

Alkali metal
La2O3
Ionic radius
Catalysis
Glycerol
glycerol carbonate

ASJC Scopus subject areas

General Chemistry
Environmental Chemistry
General Chemical Engineering
Industrial and Manufacturing Engineering

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Heat Accumulation from Renewables with Valid Energy Storage and Transformation - HARVEST
Li, Y.
Engineering & Physical Science Research Council
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Project: Research Councils

Cite this

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title = "Effect of ionic radius and valence state of alkali and alkaline earth metals on promoting the catalytic performance of La2O3 catalysts for glycerol carbonate production",

abstract = "Alkali metals and alkaline earth metals have been used to promote the catalytic performance of metal oxides in transesterification of glycerol and dimethyl carbonate, however, the promotional roles of the dopants in influencing the catalytic performance of the metal oxides have not been fully investigated which hinder the development of low-cost and high-efficiency catalysts in transesterification of glycerol and dimethyl carbonate. This paper, for the first time, systematically studied the influence of ionic radius and valence state of dopants, surface concentration of dopants and the basicity of the catalysts on the catalytic performance of La2O3 in transesterification of glycerol and dimethyl carbonate. Our results suggest that the ionic radius and valence state of the dopants are the determining factors, while the basic site density is not a crucial factor, although the basicity of catalyst surface is important in activating glycerol and dimethyl carbonate. Among alkali and alkaline earth metals, 25 mol% Na/La2O3 catalyst achieved the highest glycerol conversion (85 %) and glycerol carbonate yield (60 %) in the 70 °C and 2-hour reaction. After the detailed investigation, a plausible mechanism of glycerol and dimethyl carbonate transesterification on Na/La2O3 catalyst has been proposed. This research could help understand the promotional role of alkali metals and alkaline earth metals and the results may guide future design of metal oxide catalysts.",

keywords = "Alkali metal, La2O3, Ionic radius, Catalysis, Glycerol, glycerol carbonate",

author = "Jialin Yu and Ke Wang and Shibo Shao and Wei Li and Shangfeng Du and Xianfeng Chen and Cong Chao and Xianfeng Fan",

note = "Funding Information: Thanks to the financial support from the UK research council EPSRC (EP/V041665/1). The authors appreciate Mr Fergus Dingwall from School of Engineering in The University of Edinburgh for all his technical support; Dr. Laetitia Pichevin and Dr. Nicola Cayzer from School of Geoscience in The University of Edinburgh for their kind help on ICP-OES and SEM analysis; and Dr. Gary Nichol from School of Chemistry in The University of Edinburgh for providing XRD facility and valuable advice. Publisher Copyright: {\textcopyright} 2023 The Authors",

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AU - Shao, Shibo

AU - Li, Wei

AU - Du, Shangfeng

AU - Chen, Xianfeng

AU - Chao, Cong

AU - Fan, Xianfeng

N1 - Funding Information: Thanks to the financial support from the UK research council EPSRC (EP/V041665/1). The authors appreciate Mr Fergus Dingwall from School of Engineering in The University of Edinburgh for all his technical support; Dr. Laetitia Pichevin and Dr. Nicola Cayzer from School of Geoscience in The University of Edinburgh for their kind help on ICP-OES and SEM analysis; and Dr. Gary Nichol from School of Chemistry in The University of Edinburgh for providing XRD facility and valuable advice. Publisher Copyright: © 2023 The Authors

PY - 2023/2/15

Y1 - 2023/2/15

N2 - Alkali metals and alkaline earth metals have been used to promote the catalytic performance of metal oxides in transesterification of glycerol and dimethyl carbonate, however, the promotional roles of the dopants in influencing the catalytic performance of the metal oxides have not been fully investigated which hinder the development of low-cost and high-efficiency catalysts in transesterification of glycerol and dimethyl carbonate. This paper, for the first time, systematically studied the influence of ionic radius and valence state of dopants, surface concentration of dopants and the basicity of the catalysts on the catalytic performance of La2O3 in transesterification of glycerol and dimethyl carbonate. Our results suggest that the ionic radius and valence state of the dopants are the determining factors, while the basic site density is not a crucial factor, although the basicity of catalyst surface is important in activating glycerol and dimethyl carbonate. Among alkali and alkaline earth metals, 25 mol% Na/La2O3 catalyst achieved the highest glycerol conversion (85 %) and glycerol carbonate yield (60 %) in the 70 °C and 2-hour reaction. After the detailed investigation, a plausible mechanism of glycerol and dimethyl carbonate transesterification on Na/La2O3 catalyst has been proposed. This research could help understand the promotional role of alkali metals and alkaline earth metals and the results may guide future design of metal oxide catalysts.

AB - Alkali metals and alkaline earth metals have been used to promote the catalytic performance of metal oxides in transesterification of glycerol and dimethyl carbonate, however, the promotional roles of the dopants in influencing the catalytic performance of the metal oxides have not been fully investigated which hinder the development of low-cost and high-efficiency catalysts in transesterification of glycerol and dimethyl carbonate. This paper, for the first time, systematically studied the influence of ionic radius and valence state of dopants, surface concentration of dopants and the basicity of the catalysts on the catalytic performance of La2O3 in transesterification of glycerol and dimethyl carbonate. Our results suggest that the ionic radius and valence state of the dopants are the determining factors, while the basic site density is not a crucial factor, although the basicity of catalyst surface is important in activating glycerol and dimethyl carbonate. Among alkali and alkaline earth metals, 25 mol% Na/La2O3 catalyst achieved the highest glycerol conversion (85 %) and glycerol carbonate yield (60 %) in the 70 °C and 2-hour reaction. After the detailed investigation, a plausible mechanism of glycerol and dimethyl carbonate transesterification on Na/La2O3 catalyst has been proposed. This research could help understand the promotional role of alkali metals and alkaline earth metals and the results may guide future design of metal oxide catalysts.

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