Dianhui Chen , Zhongyi Sheng , Shuo Huang , Hexiao Huang , Yuqin Zhong , Ke Zhuang , Yaoyu Zhang , Liu Yang
{"title":"负载锰沸石催化剂臭氧氧化甲苯的失活和再生过程表征","authors":"Dianhui Chen , Zhongyi Sheng , Shuo Huang , Hexiao Huang , Yuqin Zhong , Ke Zhuang , Yaoyu Zhang , Liu Yang","doi":"10.1016/j.mcat.2025.115274","DOIUrl":null,"url":null,"abstract":"<div><div>Catalytic oxidation of toluene by ozone at ambient temperature is a promising, energy-efficient method. However, challenges such as catalyst poisoning and deactivation remain significant obstacles. As such, understanding the deactivation mechanisms and the regeneration of catalysts is crucial for optimizing catalytic oxidation processes. This study investigates the deactivation and regeneration processes of Mn/MOR catalysts in the ozone-mediated oxidation of toluene. The highest toluene removal efficiency achieved was 92.3 % with a manganese loading of 1 wt. %, but after eight experimental cycles, the catalytic performance declined to 24.3 %. The deactivation of the catalyst was primarily attributed to the accumulation of by-products during toluene degradation, the loss of Mn<sup>3+</sup>, and the reduction in oxygen vacancies. Regeneration experiments demonstrated that exposure to hot air effectively oxidized intermediate products and restored the active sites, recovering 94.2 % of the initial catalytic performance. Additionally, the possible reaction pathway for toluene degradation was deduced through GC–MS analysis. This work demonstrates the possibility of recovery of this deactivated catalyst and provides ideas for whole-life catalyst management.</div></div>","PeriodicalId":393,"journal":{"name":"Molecular Catalysis","volume":"584 ","pages":"Article 115274"},"PeriodicalIF":4.9000,"publicationDate":"2025-06-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Characterization of catalytic deactivation and regeneration processes in Mn-loaded zeolite catalysts for ozone oxidation of toluene\",\"authors\":\"Dianhui Chen , Zhongyi Sheng , Shuo Huang , Hexiao Huang , Yuqin Zhong , Ke Zhuang , Yaoyu Zhang , Liu Yang\",\"doi\":\"10.1016/j.mcat.2025.115274\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Catalytic oxidation of toluene by ozone at ambient temperature is a promising, energy-efficient method. However, challenges such as catalyst poisoning and deactivation remain significant obstacles. As such, understanding the deactivation mechanisms and the regeneration of catalysts is crucial for optimizing catalytic oxidation processes. This study investigates the deactivation and regeneration processes of Mn/MOR catalysts in the ozone-mediated oxidation of toluene. The highest toluene removal efficiency achieved was 92.3 % with a manganese loading of 1 wt. %, but after eight experimental cycles, the catalytic performance declined to 24.3 %. The deactivation of the catalyst was primarily attributed to the accumulation of by-products during toluene degradation, the loss of Mn<sup>3+</sup>, and the reduction in oxygen vacancies. Regeneration experiments demonstrated that exposure to hot air effectively oxidized intermediate products and restored the active sites, recovering 94.2 % of the initial catalytic performance. Additionally, the possible reaction pathway for toluene degradation was deduced through GC–MS analysis. This work demonstrates the possibility of recovery of this deactivated catalyst and provides ideas for whole-life catalyst management.</div></div>\",\"PeriodicalId\":393,\"journal\":{\"name\":\"Molecular Catalysis\",\"volume\":\"584 \",\"pages\":\"Article 115274\"},\"PeriodicalIF\":4.9000,\"publicationDate\":\"2025-06-12\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Molecular Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2468823125004602\",\"RegionNum\":2,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Molecular Catalysis","FirstCategoryId":"92","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2468823125004602","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Characterization of catalytic deactivation and regeneration processes in Mn-loaded zeolite catalysts for ozone oxidation of toluene
Catalytic oxidation of toluene by ozone at ambient temperature is a promising, energy-efficient method. However, challenges such as catalyst poisoning and deactivation remain significant obstacles. As such, understanding the deactivation mechanisms and the regeneration of catalysts is crucial for optimizing catalytic oxidation processes. This study investigates the deactivation and regeneration processes of Mn/MOR catalysts in the ozone-mediated oxidation of toluene. The highest toluene removal efficiency achieved was 92.3 % with a manganese loading of 1 wt. %, but after eight experimental cycles, the catalytic performance declined to 24.3 %. The deactivation of the catalyst was primarily attributed to the accumulation of by-products during toluene degradation, the loss of Mn3+, and the reduction in oxygen vacancies. Regeneration experiments demonstrated that exposure to hot air effectively oxidized intermediate products and restored the active sites, recovering 94.2 % of the initial catalytic performance. Additionally, the possible reaction pathway for toluene degradation was deduced through GC–MS analysis. This work demonstrates the possibility of recovery of this deactivated catalyst and provides ideas for whole-life catalyst management.
期刊介绍:
Molecular Catalysis publishes full papers that are original, rigorous, and scholarly contributions examining the molecular and atomic aspects of catalytic activation and reaction mechanisms. The fields covered are:
Heterogeneous catalysis including immobilized molecular catalysts
Homogeneous catalysis including organocatalysis, organometallic catalysis and biocatalysis
Photo- and electrochemistry
Theoretical aspects of catalysis analyzed by computational methods