Baichao Li , Jiabei Shao , Shiying Li , Qi Li , Pengcheng Feng , Zhangfeng Qin , Jianguo Wang , Weibin Fan , Mei Dong
{"title":"新型含锌HZSM-5型乙烯芳构化催化剂的研究","authors":"Baichao Li , Jiabei Shao , Shiying Li , Qi Li , Pengcheng Feng , Zhangfeng Qin , Jianguo Wang , Weibin Fan , Mei Dong","doi":"10.1016/j.fuel.2025.135383","DOIUrl":null,"url":null,"abstract":"<div><div>The Zn-modified HZSM-5 catalyst has been predominantly utilized in the aromatization reaction of light olefins, a crucial step in the conversion of coal-based methanol to aromatics (MTA). Nonetheless, the catalyst encounters a challenge wherein Zn species undergo migration, transformation, and subsequent loss, ultimately resulting in irreversible deactivation. To address this concern, we have developed a stable catalyst, ZnAl<sub>1.5</sub>O/HZSM-5, which incorporates both spinel-structured ZnAl<sub>2</sub>O<sub>4</sub> and ZnO species in HZSM-5 zeolite. The results demonstrate that the ZnAl<sub>1.5</sub>O/HZSM-5 catalyst, with ZnO content of 0.69 wt.%, exhibits exceptional catalytic performance characterized by a significantly higher aromatization selectivity of 67.8 %, remarkable stability spanning 174.5 h, and a substantially lower Zn loss rate of 0.15 wt.%/h, when compared to other Zn-based catalysts. Despite the absence of aromatization catalytic activity in the pure spinel sample (ZnAl<sub>2</sub>O<sub>4</sub>-pure), it effectively aids in improving the dispersion of ZnO and facilitates reversible migration, which promotes ethylene aromatization (ETA) and enhances catalytic stability. Furthermore, the migration and capture mechanisms of Zn on the ZnAl<sub>1.5</sub>O/HZSM-5 catalyst are also discussed.</div></div>","PeriodicalId":325,"journal":{"name":"Fuel","volume":"397 ","pages":"Article 135383"},"PeriodicalIF":6.7000,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Study on a novel Zn-containing HZSM-5 catalyst for ethylene aromatization\",\"authors\":\"Baichao Li , Jiabei Shao , Shiying Li , Qi Li , Pengcheng Feng , Zhangfeng Qin , Jianguo Wang , Weibin Fan , Mei Dong\",\"doi\":\"10.1016/j.fuel.2025.135383\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>The Zn-modified HZSM-5 catalyst has been predominantly utilized in the aromatization reaction of light olefins, a crucial step in the conversion of coal-based methanol to aromatics (MTA). Nonetheless, the catalyst encounters a challenge wherein Zn species undergo migration, transformation, and subsequent loss, ultimately resulting in irreversible deactivation. To address this concern, we have developed a stable catalyst, ZnAl<sub>1.5</sub>O/HZSM-5, which incorporates both spinel-structured ZnAl<sub>2</sub>O<sub>4</sub> and ZnO species in HZSM-5 zeolite. The results demonstrate that the ZnAl<sub>1.5</sub>O/HZSM-5 catalyst, with ZnO content of 0.69 wt.%, exhibits exceptional catalytic performance characterized by a significantly higher aromatization selectivity of 67.8 %, remarkable stability spanning 174.5 h, and a substantially lower Zn loss rate of 0.15 wt.%/h, when compared to other Zn-based catalysts. Despite the absence of aromatization catalytic activity in the pure spinel sample (ZnAl<sub>2</sub>O<sub>4</sub>-pure), it effectively aids in improving the dispersion of ZnO and facilitates reversible migration, which promotes ethylene aromatization (ETA) and enhances catalytic stability. Furthermore, the migration and capture mechanisms of Zn on the ZnAl<sub>1.5</sub>O/HZSM-5 catalyst are also discussed.</div></div>\",\"PeriodicalId\":325,\"journal\":{\"name\":\"Fuel\",\"volume\":\"397 \",\"pages\":\"Article 135383\"},\"PeriodicalIF\":6.7000,\"publicationDate\":\"2025-04-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Fuel\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0016236125011081\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Fuel","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0016236125011081","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Study on a novel Zn-containing HZSM-5 catalyst for ethylene aromatization
The Zn-modified HZSM-5 catalyst has been predominantly utilized in the aromatization reaction of light olefins, a crucial step in the conversion of coal-based methanol to aromatics (MTA). Nonetheless, the catalyst encounters a challenge wherein Zn species undergo migration, transformation, and subsequent loss, ultimately resulting in irreversible deactivation. To address this concern, we have developed a stable catalyst, ZnAl1.5O/HZSM-5, which incorporates both spinel-structured ZnAl2O4 and ZnO species in HZSM-5 zeolite. The results demonstrate that the ZnAl1.5O/HZSM-5 catalyst, with ZnO content of 0.69 wt.%, exhibits exceptional catalytic performance characterized by a significantly higher aromatization selectivity of 67.8 %, remarkable stability spanning 174.5 h, and a substantially lower Zn loss rate of 0.15 wt.%/h, when compared to other Zn-based catalysts. Despite the absence of aromatization catalytic activity in the pure spinel sample (ZnAl2O4-pure), it effectively aids in improving the dispersion of ZnO and facilitates reversible migration, which promotes ethylene aromatization (ETA) and enhances catalytic stability. Furthermore, the migration and capture mechanisms of Zn on the ZnAl1.5O/HZSM-5 catalyst are also discussed.
期刊介绍:
The exploration of energy sources remains a critical matter of study. For the past nine decades, fuel has consistently held the forefront in primary research efforts within the field of energy science. This area of investigation encompasses a wide range of subjects, with a particular emphasis on emerging concerns like environmental factors and pollution.