SCI和EI收录∣中国化工学会会刊

Chinese Journal of Chemical Engineering ›› 2025, Vol. 78 ›› Issue (2): 187-195.DOI: 10.1016/j.cjche.2024.10.023

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Study on sulfur resistance of MnO2/Beta zeolite in toluene catalytic combustion: The effect of increased acidity on catalytic performance

Zhuo Wang1,2, Zetao Jin1, Hanqi Ning1, Baishun Jiang1, Kaiyuan Xie1, Shufeng Zuo1, Qiuyan Wang3   

  1. 1. Zhejiang Key Laboratory of Alternative Technologies for Fine Chemicals Process, College of Chemistry and Chemical Engineering, Shaoxing University, Shaoxing 312000, China;
    2. College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China;
    3. State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
  • Received:2024-08-04 Revised:2024-10-04 Accepted:2024-10-08 Online:2024-12-10 Published:2025-02-08
  • Supported by:
    This work was supported by the National Natural Science Foundation of China (21577094); the Zhejiang Public Welfare Technology Research Project (LGG19B070003).

Study on sulfur resistance of MnO2/Beta zeolite in toluene catalytic combustion: The effect of increased acidity on catalytic performance

Zhuo Wang1,2, Zetao Jin1, Hanqi Ning1, Baishun Jiang1, Kaiyuan Xie1, Shufeng Zuo1, Qiuyan Wang3   

  1. 1. Zhejiang Key Laboratory of Alternative Technologies for Fine Chemicals Process, College of Chemistry and Chemical Engineering, Shaoxing University, Shaoxing 312000, China;
    2. College of Materials Science and Engineering, Beijing University of Technology, Beijing 100124, China;
    3. State Key Laboratory of Elemento-Organic Chemistry, Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China
  • 通讯作者: Shufeng Zuo,E-mail:sfzuo@usx.edu.cn;Qiuyan Wang,E-mail:qywang@nankai.edu.cn
  • 基金资助:
    This work was supported by the National Natural Science Foundation of China (21577094); the Zhejiang Public Welfare Technology Research Project (LGG19B070003).

Abstract: Sulfur dioxide (SO2) frequently coexist with volatile organic compounds (VOCs) in exhaust gas. The competitive adsorption of SO2 and VOCs can adversely affect the efficiency of catalytic combustion, leading to catalyst poisoning and irreversible loss of activity. To investigate the impact of sulfur poisoning on the catalysts, we prepared the MnO2/Beta zeolite, and a corresponding series of sulfur-poisoned catalysts through in-situ thermal decomposition of (NH4)2SO4. The decrease in toluene catalytic activity of poisoned MnO2/Beta zeolite primarily results from the conversion of the active species MnO2 to MnSO4. However, the crystal structure and the porous structure of MnO2/Beta zeolite were stable, and original structure was still maintained when 1.6% (mass) sulfur species were introduced. Furthermore, the extra-framework Al of Beta zeolite could capture sulfur species to generate Al2(SO4)3, thereby reducing sulfur species from reacting with Mn4+ active sites. The combination of sulfur and Beta zeolite was found to directly produce new strong-acid sites, thus effectively compensating for the effect of reduced Mn4+ active species on the catalytic activity.

Key words: Sulfur-resistant mechanism, VOCs catalytic oxidation, Beta zeolite, In-situ thermal decomposition, (NH4)2SO4

摘要: Sulfur dioxide (SO2) frequently coexist with volatile organic compounds (VOCs) in exhaust gas. The competitive adsorption of SO2 and VOCs can adversely affect the efficiency of catalytic combustion, leading to catalyst poisoning and irreversible loss of activity. To investigate the impact of sulfur poisoning on the catalysts, we prepared the MnO2/Beta zeolite, and a corresponding series of sulfur-poisoned catalysts through in-situ thermal decomposition of (NH4)2SO4. The decrease in toluene catalytic activity of poisoned MnO2/Beta zeolite primarily results from the conversion of the active species MnO2 to MnSO4. However, the crystal structure and the porous structure of MnO2/Beta zeolite were stable, and original structure was still maintained when 1.6% (mass) sulfur species were introduced. Furthermore, the extra-framework Al of Beta zeolite could capture sulfur species to generate Al2(SO4)3, thereby reducing sulfur species from reacting with Mn4+ active sites. The combination of sulfur and Beta zeolite was found to directly produce new strong-acid sites, thus effectively compensating for the effect of reduced Mn4+ active species on the catalytic activity.

关键词: Sulfur-resistant mechanism, VOCs catalytic oxidation, Beta zeolite, In-situ thermal decomposition, (NH4)2SO4