{"title":"揭示酸性位点在确定 WO3 催化剂上 NH3-SCR 机制中的重要作用:实验与计算相结合的研究","authors":"Zheng Yan, Yang Liu, Haiting Zhao, Xin Ke","doi":"10.1016/j.jallcom.2024.175373","DOIUrl":null,"url":null,"abstract":"With regard to the catalysts for NH selective catalytic reduction (NH-SCR), the acid sites distribution can affect the adsorption of reactants and formation of intermediates, thus determining the reaction routines. In this work, a representative acidic component, monoclinic-WO (m-WO), was used to probe the combination strategy of experimental and theoretical research, aiming at systematic understanding on the full-process mechanisms. Macro-scale characterizations, Temperature Programmed Desorption (TPD) and Temperature Programmed Reduction (TPR), are associated with the Density Functional Theory (DFT) calculations, by which W ion (Lewis acid site) is affirmed as the active sites. By comparing the energy barriers of possible pathways with DFT calculations, we identify that NHNO and NHNOH are responsible active intermediates. Both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) pathways may take place on acid sites and the former on Lewis acid site is optimal, which agrees well the in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) analysis. This study offers a reasonable prototype for precisely examining the correlation between the catalyst and mechanisms of NH-SCR catalysts.","PeriodicalId":344,"journal":{"name":"Journal of Alloys and Compounds","volume":null,"pages":null},"PeriodicalIF":5.8000,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Unraveling the significance of acid sites in determining NH3-SCR mechanisms over WO3 catalyst: A combined experimental and computational study\",\"authors\":\"Zheng Yan, Yang Liu, Haiting Zhao, Xin Ke\",\"doi\":\"10.1016/j.jallcom.2024.175373\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"With regard to the catalysts for NH selective catalytic reduction (NH-SCR), the acid sites distribution can affect the adsorption of reactants and formation of intermediates, thus determining the reaction routines. In this work, a representative acidic component, monoclinic-WO (m-WO), was used to probe the combination strategy of experimental and theoretical research, aiming at systematic understanding on the full-process mechanisms. Macro-scale characterizations, Temperature Programmed Desorption (TPD) and Temperature Programmed Reduction (TPR), are associated with the Density Functional Theory (DFT) calculations, by which W ion (Lewis acid site) is affirmed as the active sites. By comparing the energy barriers of possible pathways with DFT calculations, we identify that NHNO and NHNOH are responsible active intermediates. Both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) pathways may take place on acid sites and the former on Lewis acid site is optimal, which agrees well the in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) analysis. This study offers a reasonable prototype for precisely examining the correlation between the catalyst and mechanisms of NH-SCR catalysts.\",\"PeriodicalId\":344,\"journal\":{\"name\":\"Journal of Alloys and Compounds\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2024-06-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Alloys and Compounds\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jallcom.2024.175373\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Alloys and Compounds","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1016/j.jallcom.2024.175373","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Unraveling the significance of acid sites in determining NH3-SCR mechanisms over WO3 catalyst: A combined experimental and computational study
With regard to the catalysts for NH selective catalytic reduction (NH-SCR), the acid sites distribution can affect the adsorption of reactants and formation of intermediates, thus determining the reaction routines. In this work, a representative acidic component, monoclinic-WO (m-WO), was used to probe the combination strategy of experimental and theoretical research, aiming at systematic understanding on the full-process mechanisms. Macro-scale characterizations, Temperature Programmed Desorption (TPD) and Temperature Programmed Reduction (TPR), are associated with the Density Functional Theory (DFT) calculations, by which W ion (Lewis acid site) is affirmed as the active sites. By comparing the energy barriers of possible pathways with DFT calculations, we identify that NHNO and NHNOH are responsible active intermediates. Both Langmuir-Hinshelwood (L-H) and Eley-Rideal (E-R) pathways may take place on acid sites and the former on Lewis acid site is optimal, which agrees well the in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) analysis. This study offers a reasonable prototype for precisely examining the correlation between the catalyst and mechanisms of NH-SCR catalysts.
期刊介绍:
The Journal of Alloys and Compounds is intended to serve as an international medium for the publication of work on solid materials comprising compounds as well as alloys. Its great strength lies in the diversity of discipline which it encompasses, drawing together results from materials science, solid-state chemistry and physics.