Gege Qu, Xiaohong Xue, Ning Wei, Weiping Zhang, Guiqiu Wang*, Peidong Li*, Jiaxu Liu* and Shengjun Huang,
{"title":"ZSM-5/氧化铝复合材料交叉复分解反应中Mo负载与煅烧温度的相互作用","authors":"Gege Qu, Xiaohong Xue, Ning Wei, Weiping Zhang, Guiqiu Wang*, Peidong Li*, Jiaxu Liu* and Shengjun Huang, ","doi":"10.1021/acs.iecr.5c01473","DOIUrl":null,"url":null,"abstract":"<p >Thermal treatment and metal loading levels are key factors impacting the distribution and transformation of active sites in supported catalysts. Zeolite-alumina extrudate-derived catalysts receive limited attention due to the complexity arising from the competition in the anchoring and transformation of supported metal/metallic species. In this work, we investigated the intersecting impacts of Mo loading and calcination temperature on the performance of hierarchical MFI zeolite-alumina extruded catalysts in the cross-metathesis reaction between ethene and 2-butene. The response of metathesis activity to alterations in calcination temperature significantly depended on the Mo loading. At the lower Mo loading level, enhanced performance in the cross-metathesis reaction was achieved as the elevated calcination temperature stimulated the thermally driven migration of the dispersed Mo-oxo species from Al<sub>2</sub>O<sub>3</sub> component toward zeolite micropores. Nevertheless, the metathesis activity suffered from rapid decay at a higher Mo loading level, especially at elevated temperatures, on account of the formation of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species. The negative role of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species in the metathesis reaction was further corroborated by a designed experiment, wherein the stability and durability of the catalyst were restored after the removal of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species through acid leaching.</p>","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"64 34","pages":"16544–16552"},"PeriodicalIF":3.9000,"publicationDate":"2025-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The Interplay between Mo Loading and Calcination Temperature over the Hierarchical ZSM-5/Alumina Composite for the Cross-Metathesis Reaction\",\"authors\":\"Gege Qu, Xiaohong Xue, Ning Wei, Weiping Zhang, Guiqiu Wang*, Peidong Li*, Jiaxu Liu* and Shengjun Huang, \",\"doi\":\"10.1021/acs.iecr.5c01473\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >Thermal treatment and metal loading levels are key factors impacting the distribution and transformation of active sites in supported catalysts. Zeolite-alumina extrudate-derived catalysts receive limited attention due to the complexity arising from the competition in the anchoring and transformation of supported metal/metallic species. In this work, we investigated the intersecting impacts of Mo loading and calcination temperature on the performance of hierarchical MFI zeolite-alumina extruded catalysts in the cross-metathesis reaction between ethene and 2-butene. The response of metathesis activity to alterations in calcination temperature significantly depended on the Mo loading. At the lower Mo loading level, enhanced performance in the cross-metathesis reaction was achieved as the elevated calcination temperature stimulated the thermally driven migration of the dispersed Mo-oxo species from Al<sub>2</sub>O<sub>3</sub> component toward zeolite micropores. Nevertheless, the metathesis activity suffered from rapid decay at a higher Mo loading level, especially at elevated temperatures, on account of the formation of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species. The negative role of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species in the metathesis reaction was further corroborated by a designed experiment, wherein the stability and durability of the catalyst were restored after the removal of Al<sub>2</sub>(MoO<sub>4</sub>)<sub>3</sub> species through acid leaching.</p>\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"64 34\",\"pages\":\"16544–16552\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-08-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Industrial & Engineering Chemistry Research\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.iecr.5c01473\",\"RegionNum\":3,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Industrial & Engineering Chemistry Research","FirstCategoryId":"5","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.iecr.5c01473","RegionNum":3,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
The Interplay between Mo Loading and Calcination Temperature over the Hierarchical ZSM-5/Alumina Composite for the Cross-Metathesis Reaction
Thermal treatment and metal loading levels are key factors impacting the distribution and transformation of active sites in supported catalysts. Zeolite-alumina extrudate-derived catalysts receive limited attention due to the complexity arising from the competition in the anchoring and transformation of supported metal/metallic species. In this work, we investigated the intersecting impacts of Mo loading and calcination temperature on the performance of hierarchical MFI zeolite-alumina extruded catalysts in the cross-metathesis reaction between ethene and 2-butene. The response of metathesis activity to alterations in calcination temperature significantly depended on the Mo loading. At the lower Mo loading level, enhanced performance in the cross-metathesis reaction was achieved as the elevated calcination temperature stimulated the thermally driven migration of the dispersed Mo-oxo species from Al2O3 component toward zeolite micropores. Nevertheless, the metathesis activity suffered from rapid decay at a higher Mo loading level, especially at elevated temperatures, on account of the formation of Al2(MoO4)3 species. The negative role of Al2(MoO4)3 species in the metathesis reaction was further corroborated by a designed experiment, wherein the stability and durability of the catalyst were restored after the removal of Al2(MoO4)3 species through acid leaching.
期刊介绍:
ndustrial & Engineering Chemistry, with variations in title and format, has been published since 1909 by the American Chemical Society. Industrial & Engineering Chemistry Research is a weekly publication that reports industrial and academic research in the broad fields of applied chemistry and chemical engineering with special focus on fundamentals, processes, and products.