Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism

doi:10.1016/j.cjche.2024.02.002

中国化学工程学报 ›› 2024, Vol. 69 ›› Issue (5): 101-111.DOI: 10.1016/j.cjche.2024.02.002

Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism

Chenchao Hu¹, Suhang Xun^1,3, Desheng Liu¹, Junjie Zhang¹, Minqiang He², Wei Jiang², Huaming Li², Wenshuai Zhu²

1. Institute of Environmental Health and Ecological Security, School of Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, China;
2. School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;
3. Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, China

收稿日期:2023-11-25 修回日期:2024-02-07 出版日期:2024-05-28 发布日期:2024-07-01
通讯作者: Suhang Xun,E-mail:xunsuhang@ujs.edu.cn
基金资助:
We thank the financial supports from National Natural Science Foundation of China (22172066, 22378176). This work was also supported by State Key Laboratory of Heavy Oil Processing. Supported by Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology.

Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism

Chenchao Hu¹, Suhang Xun^1,3, Desheng Liu¹, Junjie Zhang¹, Minqiang He², Wei Jiang², Huaming Li², Wenshuai Zhu²

1. Institute of Environmental Health and Ecological Security, School of Environment and Safety Engineering, Jiangsu University, Zhenjiang 212013, China;
2. School of Chemistry and Chemical Engineering, Institute for Energy Research, Jiangsu University, Zhenjiang 212013, China;
3. Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology, Suzhou 215009, China

Received:2023-11-25 Revised:2024-02-07 Online:2024-05-28 Published:2024-07-01
Contact: Suhang Xun,E-mail:xunsuhang@ujs.edu.cn
Supported by:
We thank the financial supports from National Natural Science Foundation of China (22172066, 22378176). This work was also supported by State Key Laboratory of Heavy Oil Processing. Supported by Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment, Suzhou University of Science and Technology.

摘要/Abstract

摘要： An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system. Herein, a phosphotungstic acid (HPW) active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid (CTAC-HPW) by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide. The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene (DBT) with the excitation of visible light. The deep desulfurization (<10 mg·kg^-1) is attained within 30 min, and well stability is demonstrated within 25 cycles. Moreover, the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes, for example, 4-methyldibenzothiophene (4-MDBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT). Ultimately, a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry (GC-MS), proving that the final product is the corresponding sulfone. The trapping experiment and electron spin resonance (ESR) analysis confirmed that h⁺ and ·COOH played critical roles in the oxidation process. The work offers a practicable strategy for efficiently converting DBT to DBTO₂ with added value.

关键词: Photocatalytic desulfurization, Extraction, Ionic liquid, CTAC-HPW

Abstract: An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system. Herein, a phosphotungstic acid (HPW) active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid (CTAC-HPW) by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide. The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene (DBT) with the excitation of visible light. The deep desulfurization (<10 mg·kg^-1) is attained within 30 min, and well stability is demonstrated within 25 cycles. Moreover, the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes, for example, 4-methyldibenzothiophene (4-MDBT) and 4,6-dimethyldibenzothiophene (4,6-DMDBT). Ultimately, a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry (GC-MS), proving that the final product is the corresponding sulfone. The trapping experiment and electron spin resonance (ESR) analysis confirmed that h⁺ and ·COOH played critical roles in the oxidation process. The work offers a practicable strategy for efficiently converting DBT to DBTO₂ with added value.

Key words: Photocatalytic desulfurization, Extraction, Ionic liquid, CTAC-HPW

Chenchao Hu, Suhang Xun, Desheng Liu, Junjie Zhang, Minqiang He, Wei Jiang, Huaming Li, Wenshuai Zhu. Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism[J]. 中国化学工程学报, 2024, 69(5): 101-111.

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Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism

Phosphotungstic acid ionic liquid for efficient photocatalytic desulfurization: Synthesis, application and mechanism

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