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

IF 3.9 3区 工程技术 Q2 ENGINEERING, CHEMICAL
Xuguang Wang, Yaxin Liu, Zihao Wang, Chonghao Chen, Zixin Song, Yuanxiang Xu, Dianhua Liu
{"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}
引用次数: 0

摘要

传统Cu-Zn-Al催化剂的调制过程和机理的复杂性和有限的认识阻碍了它们的广泛应用。本文采用沉积-沉淀法制备了Cu-Zn /γ-Al2O3催化剂,研究了Cu-Zn含量、接触和相互作用之间的关系。我们发现Cu - Zn含量过高会导致Cu和Zn的聚集,而Cu - Zn含量不足则会阻碍Zn对Cu的有效分离。并对Cu-Zn /γ-Al2O3的还原反应过程进行了可视化研究。在还原过程中,ZnO(0 0 2)迁移到催化剂表面,形成ZnO (0 0 2)@Cu活性位点,CO2容易通过HCOO*生成甲醇。因此,Cu-Zn接触增强有利于Zn的迁移,从而形成甲醇合成的活性位点。优化后的0.06Cu0.03Zn/Al2O3催化剂的CO2转化率为65.77%,甲醇选择性为88.32%,热稳定性优于CZA催化剂。我们相信我们的发现对甲醇合成中Cu-Zn催化剂的工业化具有重要的指导意义和实用价值。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
Industrial & Engineering Chemistry Research
Industrial & Engineering Chemistry Research 工程技术-工程:化工
CiteScore
7.40
自引率
7.10%
发文量
1467
审稿时长
2.8 months
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.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信