Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

doi:10.1016/j.cjche.2023.06.026

中国化学工程学报 ›› 2024, Vol. 65 ›› Issue (1): 130-144.DOI: 10.1016/j.cjche.2023.06.026

• Full Length Article • 上一篇下一篇

Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

Donghui Li¹, Wenzhe Wu¹, Xue Ren¹, Xixi Zhao¹, Hongbing Song¹, Meng Xiao¹, Quanhong Zhu¹, Hengjun Gai², Tingting Huang¹

1 College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China;
2 School of Chemical & Environmental Engineering, China University of Mining & Technology-Beijing, Beijing 100083, China

收稿日期:2023-02-19 修回日期:2023-06-14 出版日期:2024-01-28 发布日期:2024-04-17
通讯作者: Hengjun Gai,E-mail:hjgai@126.com;Tingting Huang,E-mail:huangtingting@qust.edu.cn
基金资助:
The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China (22108145 and 21978143), the Shandong Province Natural Science Foundation (ZR2020QB189), State Key Laboratory of Heavy Oil Processing (SKLHOP202203008) and the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering (STHGYX2201).

Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

Donghui Li¹, Wenzhe Wu¹, Xue Ren¹, Xixi Zhao¹, Hongbing Song¹, Meng Xiao¹, Quanhong Zhu¹, Hengjun Gai², Tingting Huang¹

1 College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, China;
2 School of Chemical & Environmental Engineering, China University of Mining & Technology-Beijing, Beijing 100083, China

Received:2023-02-19 Revised:2023-06-14 Online:2024-01-28 Published:2024-04-17
Contact: Hengjun Gai,E-mail:hjgai@126.com;Tingting Huang,E-mail:huangtingting@qust.edu.cn
Supported by:
The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China (22108145 and 21978143), the Shandong Province Natural Science Foundation (ZR2020QB189), State Key Laboratory of Heavy Oil Processing (SKLHOP202203008) and the Talent Foundation funded by Province and Ministry Co-construction Collaborative Innovation Center of Eco-chemical Engineering (STHGYX2201).

摘要/Abstract

摘要： The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method. During the preparation of the Fe-NC catalyst, the complexation of N elements in urea could anchor Fe, and the formation of C₃N₄ during urea pyrolysis could also prevent migration and aggregation of Fe species, which jointly improve the dispersion and stability of Fe. The FeN₄ sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation, while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process, which together promote catalytic degradation of m-cresol by PMS activation. Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO₄^-· and ·OH, and partially based on ·OH as the active components, and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed. This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.

关键词: Degradation, Peroxymonosulfate, Fe(II)/Fe(III)/FeN₄, Ordered mesopores carbon, Catalyst, Radical

Abstract: The novel Fe-N co-doped ordered mesoporous carbon with high catalytic activity in m-cresol removal was prepared by urea-assisted impregnation and simple pyrolysis method. During the preparation of the Fe-NC catalyst, the complexation of N elements in urea could anchor Fe, and the formation of C₃N₄ during urea pyrolysis could also prevent migration and aggregation of Fe species, which jointly improve the dispersion and stability of Fe. The FeN₄ sites and highly dispersed Fe nanoparticles synergistically trigger the dual-site peroxymonosulfate (PMS) activation for highly efficient m-cresol degradation, while the ordered mesoporous structure of the catalyst could improve the mass transfer rate of the catalytic process, which together promote catalytic degradation of m-cresol by PMS activation. Reactive oxygen species (ROS) analytic experiments demonstrate that the system degrades m-cresol by free radical pathway mainly based on SO₄^-· and ·OH, and partially based on ·OH as the active components, and a possible PMS activation mechanism by 5Fe-50 for m-cresol degradation was proposed. This study can provide theoretical guidance for the preparation of efficient and stable catalysts for the degradation of organic pollutants by activated PMS.

Key words: Degradation, Peroxymonosulfate, Fe(II)/Fe(III)/FeN₄, Ordered mesopores carbon, Catalyst, Radical

Donghui Li, Wenzhe Wu, Xue Ren, Xixi Zhao, Hongbing Song, Meng Xiao, Quanhong Zhu, Hengjun Gai, Tingting Huang. Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol[J]. 中国化学工程学报, 2024, 65(1): 130-144.

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Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

Enhanced activation of peroxymonosulfate by Fe/N co-doped ordered mesoporous carbon with dual active sites for efficient removal of m-cresol

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