Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents

doi:10.1016/j.cjche.2021.04.031

Chinese Journal of Chemical Engineering ›› 2022, Vol. 44 ›› Issue (4): 205-211.DOI: 10.1016/j.cjche.2021.04.031

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Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents

Linlan Wu¹, Zhengxin Jiao², Suhang Xun², Minqiang He¹, Lei Fan³, Chao Wang², Wenshu Yang¹, Wenshuai Zhu¹, Huaming Li¹

1 School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;
2 School of Environment and Safety Engineering, Institute of Environmental Health and Ecological Security, Jiangsu University, Zhenjiang 212013, China;
3 School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China

Received:2021-01-29 Revised:2021-04-18 Online:2022-06-18 Published:2022-04-28
Contact: Minqiang He,E-mail:hemq@ujs.edu.cn;Wenshuai Zhu,E-mail:zhuws@ujs.edu.cn
Supported by:
This work was financially supported by the National Natural Science Foundation of China (No. 21808091), Natural Science Foundation of Jiangsu Province (Nos. BK20200896, BK20190243), Key Laboratory of Tropical Medicinal Plant Chemistry of Ministry of Education, Hainan Normal University (20150376), China Postdoctoral Foundation (No. 2020M671365), and the Student Innovation and Entrepreneurship Training Program (202010299457X).

Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents

Linlan Wu¹, Zhengxin Jiao², Suhang Xun², Minqiang He¹, Lei Fan³, Chao Wang², Wenshu Yang¹, Wenshuai Zhu¹, Huaming Li¹

1 School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;
2 School of Environment and Safety Engineering, Institute of Environmental Health and Ecological Security, Jiangsu University, Zhenjiang 212013, China;
3 School of Chemistry and Chemical Engineering, Yangzhou University, Yangzhou 225002, China

通讯作者: Minqiang He,E-mail:hemq@ujs.edu.cn;Wenshuai Zhu,E-mail:zhuws@ujs.edu.cn
基金资助:
This work was financially supported by the National Natural Science Foundation of China (No. 21808091), Natural Science Foundation of Jiangsu Province (Nos. BK20200896, BK20190243), Key Laboratory of Tropical Medicinal Plant Chemistry of Ministry of Education, Hainan Normal University (20150376), China Postdoctoral Foundation (No. 2020M671365), and the Student Innovation and Entrepreneurship Training Program (202010299457X).

Abstract

Abstract: A series of novel binary deep eutectic solvents (DESs) composed of choline chloride (ChCl) and formic acid (HCOOH) with different molar ratios have been successfully synthesized and applied in extractive desulfurization (EDS). Keggin-type polyoxometallate ionic liquid [TTPh]₃PW₁₂O₄₀ was prepared and used as catalyst to enhance the EDS capacity by means of photocatalytic oxidative process. Both of the DESs and [TTPh]₃PW₁₂O₄₀ ionic liquid catalyst were characterized in detail by Fourier transform infrared spectroscopy spectra (FT-IR), elemental analysis, and X-ray photoelectron spectroscopy (XPS). It was found that the molar ratios of ChCl:HCOOH had a major impact on desulfurization performance, and the optimal desulfurization capacity 96.5% was obtained by ChCl/5HCOOH. Besides dibenzothiophene (DBT), the desulfurization efficiencies of 4-methylbenzothiophene (4-MDBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT), two kinds of DBT derivatives, were also investigated under the same experimental conditions. Moreover, the free radical scavenging experiments manifested that superoxide radical (·O₂^-) and hole (h⁺) played important roles in the desulfurization system. After further analysis of the oxidation products by gas chromatography-mass spectrometry (GC–MS), the possible reaction mechanism was proposed. Thus, photocatalytic oxidative has been proved to be one of the efficient approaches for enhancing the extractive desulfurization performance in DES.

Key words: Deep eutectic solvents, Extractive desulfurization, Ionic liquid, Photocatalytic oxidative, Aerobic, Fuel

摘要： A series of novel binary deep eutectic solvents (DESs) composed of choline chloride (ChCl) and formic acid (HCOOH) with different molar ratios have been successfully synthesized and applied in extractive desulfurization (EDS). Keggin-type polyoxometallate ionic liquid [TTPh]₃PW₁₂O₄₀ was prepared and used as catalyst to enhance the EDS capacity by means of photocatalytic oxidative process. Both of the DESs and [TTPh]₃PW₁₂O₄₀ ionic liquid catalyst were characterized in detail by Fourier transform infrared spectroscopy spectra (FT-IR), elemental analysis, and X-ray photoelectron spectroscopy (XPS). It was found that the molar ratios of ChCl:HCOOH had a major impact on desulfurization performance, and the optimal desulfurization capacity 96.5% was obtained by ChCl/5HCOOH. Besides dibenzothiophene (DBT), the desulfurization efficiencies of 4-methylbenzothiophene (4-MDBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT), two kinds of DBT derivatives, were also investigated under the same experimental conditions. Moreover, the free radical scavenging experiments manifested that superoxide radical (·O₂^-) and hole (h⁺) played important roles in the desulfurization system. After further analysis of the oxidation products by gas chromatography-mass spectrometry (GC–MS), the possible reaction mechanism was proposed. Thus, photocatalytic oxidative has been proved to be one of the efficient approaches for enhancing the extractive desulfurization performance in DES.

关键词: Deep eutectic solvents, Extractive desulfurization, Ionic liquid, Photocatalytic oxidative, Aerobic, Fuel

Linlan Wu, Zhengxin Jiao, Suhang Xun, Minqiang He, Lei Fan, Chao Wang, Wenshu Yang, Wenshuai Zhu, Huaming Li. Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents[J]. Chinese Journal of Chemical Engineering, 2022, 44(4): 205-211.

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Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents

Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents

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