Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

doi:10.1016/j.cjche.2023.04.004

中国化学工程学报 ›› 2023, Vol. 63 ›› Issue (11): 140-147.DOI: 10.1016/j.cjche.2023.04.004

• Full Length Article • 上一篇下一篇

Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

Chongfu Wu, Changsheng Chen, Zhaoyang Qi, Jie Chen, Qinglian Wang, Changshen Ye, Ting Qiu

1. College of Chemical Engineering, Fuzhou University, Fuzhou 350108, China;
2. Qingyuan Innovation Laboratory, Quanzhou 362801, China;
3. Engineering Research Center of Reactive Distillation, Fujian Province Higher Education Institutes, Fuzhou 350108, China

收稿日期:2022-10-27 修回日期:2023-04-06 出版日期:2023-11-28 发布日期:2024-01-08
通讯作者: Changshen Ye,E-mail:fzycsyrfyq@fzu.edu.cn;Ting Qiu,E-mail:tingqiu@fzu.edu.cn
基金资助:
This work was supported by the National Natural Science Foundation of China (22378065, 22278077) and the Fujian Province Department of Science & Technology, China (2019YZ017001).

Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

Chongfu Wu, Changsheng Chen, Zhaoyang Qi, Jie Chen, Qinglian Wang, Changshen Ye, Ting Qiu

1. College of Chemical Engineering, Fuzhou University, Fuzhou 350108, China;
2. Qingyuan Innovation Laboratory, Quanzhou 362801, China;
3. Engineering Research Center of Reactive Distillation, Fujian Province Higher Education Institutes, Fuzhou 350108, China

Received:2022-10-27 Revised:2023-04-06 Online:2023-11-28 Published:2024-01-08
Contact: Changshen Ye,E-mail:fzycsyrfyq@fzu.edu.cn;Ting Qiu,E-mail:tingqiu@fzu.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China (22378065, 22278077) and the Fujian Province Department of Science & Technology, China (2019YZ017001).

摘要/Abstract

摘要： The ultra-deep desulfurization of oil needs to be solved urgently due to various problems, including environmental pollution and environmental protection requirements. Oxidative desulfurization (ODS) was considered to be the most promising technology. The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task. In this paper, pentamethylene hexamine (PEHA) and phosphotungstic acid (HPW) were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil. The composite material exhibited excellent catalytic activity and high recyclability, which could reach a 100% dibenzothiophene (DBT) removal rate in 30 min and be recycled at least 5 times. Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW. It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role. This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.

关键词: Oxidation, Catalyst, Desulfurization, Fuel, Phosphotungstic acid, Amino

Abstract: The ultra-deep desulfurization of oil needs to be solved urgently due to various problems, including environmental pollution and environmental protection requirements. Oxidative desulfurization (ODS) was considered to be the most promising technology. The facile synthesis of highly efficient and stable HPW-based heterogeneous catalysts for oxidative desulfurization is still a challenging task. In this paper, pentamethylene hexamine (PEHA) and phosphotungstic acid (HPW) were combined by a simple one-step method to prepare a heterogeneous catalyst of PEHA-HPW for the production of ultra-deep desulfurization fuel oil. The composite material exhibited excellent catalytic activity and high recyclability, which could reach a 100% dibenzothiophene (DBT) removal rate in 30 min and be recycled at least 5 times. Experiments and DFT simulations were used to better examine the ODS mechanism of PEHA-HPW. It was proved that the rich amino groups on the surface of PEHA-HPW play a crucial role. This work provides a simple and feasible way for the manufacture of efficient HPW-based catalysts.

Key words: Oxidation, Catalyst, Desulfurization, Fuel, Phosphotungstic acid, Amino

Chongfu Wu, Changsheng Chen, Zhaoyang Qi, Jie Chen, Qinglian Wang, Changshen Ye, Ting Qiu. Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization[J]. 中国化学工程学报, 2023, 63(11): 140-147.

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Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

Facile synthesis of efficient pentaethylenehexamine-phosphotungstic acid heterogeneous catalysts for oxidative desulfurization

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