在V2O5-WO3/TiO2催化剂中,WO3通过形成V-W双核位选择性还原NO的意外氧化还原作用

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Zhuocan Li, Rucheng Duan, Xin Wang, Yu Fu, Meng Gao, Hongwei Li, Guangzhi He, Hong He
{"title":"在V2O5-WO3/TiO2催化剂中,WO3通过形成V-W双核位选择性还原NO的意外氧化还原作用","authors":"Zhuocan Li,&nbsp;Rucheng Duan,&nbsp;Xin Wang,&nbsp;Yu Fu,&nbsp;Meng Gao,&nbsp;Hongwei Li,&nbsp;Guangzhi He,&nbsp;Hong He","doi":"10.1002/anie.202501957","DOIUrl":null,"url":null,"abstract":"<p>Promoters can greatly improve the activity of catalysts; however, the mechanism by which they interact with the primary catalyst to enhance catalytic activity is not always clear. It has been widely demonstrated that WO<sub>3</sub> in V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts acts as a promoter to enhance the surface acidity and regulate the dispersion of active V<sub>2</sub>O<sub>5</sub> species, while it is believed that the redox process takes place entirely at the V sites in the selective catalytic reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> (NH<sub>3</sub>-SCR). Here, by combining in situ spectroscopic measurements and density functional theory (DFT) calculations, we validate that the WO<sub>3</sub> directly participates in the oxidative activation of NH<sub>3</sub>, and hence explicitly exerts a redox effect in NH<sub>3</sub>-SCR by forming V–W dinuclear sites with V<sub>2</sub>O<sub>5</sub>. This study sheds new light on a long-standing puzzle regarding the role of WO<sub>3</sub> as a promoter and hence advances the understanding of the working principle of V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts.</p>","PeriodicalId":125,"journal":{"name":"Angewandte Chemie International Edition","volume":"64 28","pages":""},"PeriodicalIF":16.9000,"publicationDate":"2025-05-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unexpected Redox Role of WO3 in V2O5-WO3/TiO2 Catalysts for Selective Reduction of NO by Forming V–W Dinuclear Sites\",\"authors\":\"Zhuocan Li,&nbsp;Rucheng Duan,&nbsp;Xin Wang,&nbsp;Yu Fu,&nbsp;Meng Gao,&nbsp;Hongwei Li,&nbsp;Guangzhi He,&nbsp;Hong He\",\"doi\":\"10.1002/anie.202501957\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>Promoters can greatly improve the activity of catalysts; however, the mechanism by which they interact with the primary catalyst to enhance catalytic activity is not always clear. It has been widely demonstrated that WO<sub>3</sub> in V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts acts as a promoter to enhance the surface acidity and regulate the dispersion of active V<sub>2</sub>O<sub>5</sub> species, while it is believed that the redox process takes place entirely at the V sites in the selective catalytic reduction of NO<i><sub>x</sub></i> with NH<sub>3</sub> (NH<sub>3</sub>-SCR). Here, by combining in situ spectroscopic measurements and density functional theory (DFT) calculations, we validate that the WO<sub>3</sub> directly participates in the oxidative activation of NH<sub>3</sub>, and hence explicitly exerts a redox effect in NH<sub>3</sub>-SCR by forming V–W dinuclear sites with V<sub>2</sub>O<sub>5</sub>. This study sheds new light on a long-standing puzzle regarding the role of WO<sub>3</sub> as a promoter and hence advances the understanding of the working principle of V<sub>2</sub>O<sub>5</sub>-WO<sub>3</sub>/TiO<sub>2</sub> catalysts.</p>\",\"PeriodicalId\":125,\"journal\":{\"name\":\"Angewandte Chemie International Edition\",\"volume\":\"64 28\",\"pages\":\"\"},\"PeriodicalIF\":16.9000,\"publicationDate\":\"2025-05-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Angewandte Chemie International Edition\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/anie.202501957\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Angewandte Chemie International Edition","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/anie.202501957","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0

摘要

促进剂能大大提高催化剂的活性;然而,它们与一级催化剂相互作用以增强催化活性的机制并不总是很清楚。研究表明,在V2O5-WO3/TiO2催化剂中,WO3作为促进剂增强了表面酸度,调节了活性V2O5的分散,而在NH3选择性催化还原NOx (NH3- scr)过程中,氧化还原过程完全发生在V位点。本研究通过原位光谱测量和密度泛函理论(DFT)计算相结合,验证了WO3直接参与NH3的氧化活化,从而通过与V2O5形成V-W双核位在NH3- scr中明显发挥氧化还原作用。该研究揭示了长期以来关于WO3作为促进剂的作用的新谜团,从而促进了对V2O5-WO3/TiO2催化剂工作原理的理解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Unexpected Redox Role of WO3 in V2O5-WO3/TiO2 Catalysts for Selective Reduction of NO by Forming V–W Dinuclear Sites

Unexpected Redox Role of WO3 in V2O5-WO3/TiO2 Catalysts for Selective Reduction of NO by Forming V–W Dinuclear Sites

Promoters can greatly improve the activity of catalysts; however, the mechanism by which they interact with the primary catalyst to enhance catalytic activity is not always clear. It has been widely demonstrated that WO3 in V2O5-WO3/TiO2 catalysts acts as a promoter to enhance the surface acidity and regulate the dispersion of active V2O5 species, while it is believed that the redox process takes place entirely at the V sites in the selective catalytic reduction of NOx with NH3 (NH3-SCR). Here, by combining in situ spectroscopic measurements and density functional theory (DFT) calculations, we validate that the WO3 directly participates in the oxidative activation of NH3, and hence explicitly exerts a redox effect in NH3-SCR by forming V–W dinuclear sites with V2O5. This study sheds new light on a long-standing puzzle regarding the role of WO3 as a promoter and hence advances the understanding of the working principle of V2O5-WO3/TiO2 catalysts.

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
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
×
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