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

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":"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}
引用次数: 0

Abstract

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.

Abstract Image

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
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。
求助全文
约1分钟内获得全文 求助全文
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