{"title":"通过改善Cu-Zn接触增强Cu-Zn相互作用:促进锌迁移以形成活性位点","authors":"Xuguang Wang, Yaxin Liu, Zihao Wang, Chonghao Chen, Zixin Song, Yuanxiang Xu, Dianhua Liu","doi":"10.1021/acs.iecr.5c01767","DOIUrl":null,"url":null,"abstract":"The complexity and limited understanding of the modulation processes and mechanisms of conventional Cu–Zn–Al catalysts have hindered their widespread implementation. Here, we prepared Cu–Zn/γ-Al<sub>2</sub>O<sub>3</sub> catalysts via the deposition–precipitation method to investigate the relationship among Cu–Zn content, contact, and interaction. We found that excessive Cu–Zn content leads to the aggregation of Cu and Zn species, while insufficient Cu–Zn content prevents effective separation of Cu by Zn. Additionally, the reduction and reaction processes of Cu–Zn/γ-Al<sub>2</sub>O<sub>3</sub> were visualized. During the reduction process, ZnO (0 0 2) migrated to the catalyst surface, forming the ZnO (0 0 2)@Cu active site, where CO<sub>2</sub> readily generates methanol via HCOO*. Therefore, enhanced Cu–Zn contact facilitates Zn migration, leading to the formation of active sites for methanol synthesis. The content-optimized 0.06Cu0.03Zn/Al<sub>2</sub>O<sub>3</sub> exhibits 65.77% CO<sub>2</sub> conversion and 88.32% methanol selectivity and displays better thermal stability than commercial CZA catalysts. We believe that our findings provide significant guidance and practical value for the industrialization of Cu–Zn catalysts in methanol synthesis.","PeriodicalId":39,"journal":{"name":"Industrial & Engineering Chemistry Research","volume":"24 1","pages":""},"PeriodicalIF":3.9000,"publicationDate":"2025-07-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhancement of Cu–Zn Interaction via Improved Cu–Zn Contact: Promoting Zinc Migration for Active Site Formation\",\"authors\":\"Xuguang Wang, Yaxin Liu, Zihao Wang, Chonghao Chen, Zixin Song, Yuanxiang Xu, Dianhua Liu\",\"doi\":\"10.1021/acs.iecr.5c01767\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The complexity and limited understanding of the modulation processes and mechanisms of conventional Cu–Zn–Al catalysts have hindered their widespread implementation. Here, we prepared Cu–Zn/γ-Al<sub>2</sub>O<sub>3</sub> catalysts via the deposition–precipitation method to investigate the relationship among Cu–Zn content, contact, and interaction. We found that excessive Cu–Zn content leads to the aggregation of Cu and Zn species, while insufficient Cu–Zn content prevents effective separation of Cu by Zn. Additionally, the reduction and reaction processes of Cu–Zn/γ-Al<sub>2</sub>O<sub>3</sub> were visualized. During the reduction process, ZnO (0 0 2) migrated to the catalyst surface, forming the ZnO (0 0 2)@Cu active site, where CO<sub>2</sub> readily generates methanol via HCOO*. Therefore, enhanced Cu–Zn contact facilitates Zn migration, leading to the formation of active sites for methanol synthesis. The content-optimized 0.06Cu0.03Zn/Al<sub>2</sub>O<sub>3</sub> exhibits 65.77% CO<sub>2</sub> conversion and 88.32% methanol selectivity and displays better thermal stability than commercial CZA catalysts. We believe that our findings provide significant guidance and practical value for the industrialization of Cu–Zn catalysts in methanol synthesis.\",\"PeriodicalId\":39,\"journal\":{\"name\":\"Industrial & Engineering Chemistry Research\",\"volume\":\"24 1\",\"pages\":\"\"},\"PeriodicalIF\":3.9000,\"publicationDate\":\"2025-07-12\",\"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://doi.org/10.1021/acs.iecr.5c01767\",\"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://doi.org/10.1021/acs.iecr.5c01767","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}
Enhancement of Cu–Zn Interaction via Improved Cu–Zn Contact: Promoting Zinc Migration for Active Site Formation
The complexity and limited understanding of the modulation processes and mechanisms of conventional Cu–Zn–Al catalysts have hindered their widespread implementation. Here, we prepared Cu–Zn/γ-Al2O3 catalysts via the deposition–precipitation method to investigate the relationship among Cu–Zn content, contact, and interaction. We found that excessive Cu–Zn content leads to the aggregation of Cu and Zn species, while insufficient Cu–Zn content prevents effective separation of Cu by Zn. Additionally, the reduction and reaction processes of Cu–Zn/γ-Al2O3 were visualized. During the reduction process, ZnO (0 0 2) migrated to the catalyst surface, forming the ZnO (0 0 2)@Cu active site, where CO2 readily generates methanol via HCOO*. Therefore, enhanced Cu–Zn contact facilitates Zn migration, leading to the formation of active sites for methanol synthesis. The content-optimized 0.06Cu0.03Zn/Al2O3 exhibits 65.77% CO2 conversion and 88.32% methanol selectivity and displays better thermal stability than commercial CZA catalysts. We believe that our findings provide significant guidance and practical value for the industrialization of Cu–Zn catalysts in methanol synthesis.
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.