增强用于氮氧化物 NH3-SCR 的 Ce-Mn Oxide 改性 Cu-SSZ-39 催化剂的低温活性和水热稳定性

IF 3.8 3区 化学 Q2 CHEMISTRY, PHYSICAL
Catalysts Pub Date : 2023-12-21 DOI:10.3390/catal14010010
Ahui Tang, Fuzhen Yang, Ying Xin, Xiaoli Zhu, Long Yu, Shuai Liu, Dongxu Han, Junxiu Jia, Yaning Lu, Zhenguo Li, Zhaoliang Zhang
{"title":"增强用于氮氧化物 NH3-SCR 的 Ce-Mn Oxide 改性 Cu-SSZ-39 催化剂的低温活性和水热稳定性","authors":"Ahui Tang, Fuzhen Yang, Ying Xin, Xiaoli Zhu, Long Yu, Shuai Liu, Dongxu Han, Junxiu Jia, Yaning Lu, Zhenguo Li, Zhaoliang Zhang","doi":"10.3390/catal14010010","DOIUrl":null,"url":null,"abstract":"Cu-SSZ-39 zeolite with an AEI structure exhibits excellent hydrothermal stability and can be a potential alternative to Cu-SSZ-13 zeolite SCR catalysts for NOx removal in diesel vehicles. However, the inferior low-temperature performance of Cu-SSZ-39 leads to substantial NOx emissions during the cold-start period, impeding its practical application. In this study, Ce-Mn oxide-modified Cu-SSZ-39 catalysts (CeMnOx/Cu-SSZ-39) and references (CeO2/Cu-SSZ-39 and MnOx/Cu-SSZ-39) were prepared by the ion-exchange of Cu ions followed by impregnation of the oxide precursors, with the aim of enhancing the NH3-SCR performance at low temperatures. The modified catalysts exhibited improved low-temperature activity and hydrothermal stability compared to the unmodified counterpart. In particular, CeMnOx/Cu-SSZ-39 showed the highest activity among the three catalysts and achieved NOx conversions above 90% within the temperature range of 180 °C to 600 °C, even after undergoing hydrothermal aging at 800 °C. Experimental results indicated that the synergistic effect between Ce and Mn in CeMnOx improves the redox properties and acidity of the catalyst due to the presence of Ce3+, Mn4+, and abundant adsorbed oxygen species, which facilitate low-temperature SCR reactions. Furthermore, the interaction of CeMnOx with Cu-SSZ-39 stabilizes the zeolite framework and hinders the agglomeration of Cu species during the hydrothermal aging process, contributing to its exceptional hydrothermal stability. The kinetics and NO oxidation experiments demonstrated that CeMnOx provides access to fast SCR reaction pathways by oxidizing NO to NO2, resulting in a significant increase in low-temperature activity. This study provides novel guidelines for the design and preparation of Cu-SSZ-39 zeolite with outstanding SCR performance over a wide temperature range.","PeriodicalId":9794,"journal":{"name":"Catalysts","volume":"38 25","pages":""},"PeriodicalIF":3.8000,"publicationDate":"2023-12-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Enhanced Low-Temperature Activity and Hydrothermal Stability of Ce-Mn Oxide-Modified Cu-SSZ-39 Catalysts for NH3-SCR of NOx\",\"authors\":\"Ahui Tang, Fuzhen Yang, Ying Xin, Xiaoli Zhu, Long Yu, Shuai Liu, Dongxu Han, Junxiu Jia, Yaning Lu, Zhenguo Li, Zhaoliang Zhang\",\"doi\":\"10.3390/catal14010010\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Cu-SSZ-39 zeolite with an AEI structure exhibits excellent hydrothermal stability and can be a potential alternative to Cu-SSZ-13 zeolite SCR catalysts for NOx removal in diesel vehicles. However, the inferior low-temperature performance of Cu-SSZ-39 leads to substantial NOx emissions during the cold-start period, impeding its practical application. In this study, Ce-Mn oxide-modified Cu-SSZ-39 catalysts (CeMnOx/Cu-SSZ-39) and references (CeO2/Cu-SSZ-39 and MnOx/Cu-SSZ-39) were prepared by the ion-exchange of Cu ions followed by impregnation of the oxide precursors, with the aim of enhancing the NH3-SCR performance at low temperatures. The modified catalysts exhibited improved low-temperature activity and hydrothermal stability compared to the unmodified counterpart. In particular, CeMnOx/Cu-SSZ-39 showed the highest activity among the three catalysts and achieved NOx conversions above 90% within the temperature range of 180 °C to 600 °C, even after undergoing hydrothermal aging at 800 °C. Experimental results indicated that the synergistic effect between Ce and Mn in CeMnOx improves the redox properties and acidity of the catalyst due to the presence of Ce3+, Mn4+, and abundant adsorbed oxygen species, which facilitate low-temperature SCR reactions. Furthermore, the interaction of CeMnOx with Cu-SSZ-39 stabilizes the zeolite framework and hinders the agglomeration of Cu species during the hydrothermal aging process, contributing to its exceptional hydrothermal stability. The kinetics and NO oxidation experiments demonstrated that CeMnOx provides access to fast SCR reaction pathways by oxidizing NO to NO2, resulting in a significant increase in low-temperature activity. This study provides novel guidelines for the design and preparation of Cu-SSZ-39 zeolite with outstanding SCR performance over a wide temperature range.\",\"PeriodicalId\":9794,\"journal\":{\"name\":\"Catalysts\",\"volume\":\"38 25\",\"pages\":\"\"},\"PeriodicalIF\":3.8000,\"publicationDate\":\"2023-12-21\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysts\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.3390/catal14010010\",\"RegionNum\":3,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysts","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.3390/catal14010010","RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

具有 AEI 结构的 Cu-SSZ-39 沸石具有出色的水热稳定性,可以替代 Cu-SSZ-13 沸石 SCR 催化剂,用于去除柴油车中的氮氧化物。然而,Cu-SSZ-39 的低温性能较差,导致其在冷启动期间排放大量氮氧化物,阻碍了其实际应用。本研究通过离子交换铜离子,然后浸渍氧化物前驱体,制备了铈锰氧化物改性的 Cu-SSZ-39 催化剂(CeMnOx/Cu-SSZ-39)和参照物(CeO2/Cu-SSZ-39 和 MnOx/Cu-SSZ-39),旨在提高低温下的 NH3-SCR 性能。与未改性的催化剂相比,改性催化剂具有更高的低温活性和水热稳定性。其中,CeMnOx/Cu-SSZ-39 在三种催化剂中表现出最高的活性,在 180 °C 至 600 °C 的温度范围内,即使经过 800 °C 的水热老化,其氮氧化物转化率也能达到 90% 以上。实验结果表明,CeMnOx 中 Ce 和 Mn 的协同作用改善了催化剂的氧化还原特性和酸性,这是因为 Ce3+、Mn4+ 和丰富的吸附氧物种的存在促进了低温 SCR 反应的进行。此外,CeMnOx 与 Cu-SSZ-39 的相互作用稳定了沸石框架,阻碍了水热老化过程中 Cu 物种的团聚,使其具有优异的水热稳定性。动力学和 NO 氧化实验表明,CeMnOx 通过将 NO 氧化为 NO2,提供了快速 SCR 反应途径,从而显著提高了低温活性。这项研究为设计和制备在宽温度范围内具有出色 SCR 性能的 Cu-SSZ-39 沸石提供了新的指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Enhanced Low-Temperature Activity and Hydrothermal Stability of Ce-Mn Oxide-Modified Cu-SSZ-39 Catalysts for NH3-SCR of NOx
Cu-SSZ-39 zeolite with an AEI structure exhibits excellent hydrothermal stability and can be a potential alternative to Cu-SSZ-13 zeolite SCR catalysts for NOx removal in diesel vehicles. However, the inferior low-temperature performance of Cu-SSZ-39 leads to substantial NOx emissions during the cold-start period, impeding its practical application. In this study, Ce-Mn oxide-modified Cu-SSZ-39 catalysts (CeMnOx/Cu-SSZ-39) and references (CeO2/Cu-SSZ-39 and MnOx/Cu-SSZ-39) were prepared by the ion-exchange of Cu ions followed by impregnation of the oxide precursors, with the aim of enhancing the NH3-SCR performance at low temperatures. The modified catalysts exhibited improved low-temperature activity and hydrothermal stability compared to the unmodified counterpart. In particular, CeMnOx/Cu-SSZ-39 showed the highest activity among the three catalysts and achieved NOx conversions above 90% within the temperature range of 180 °C to 600 °C, even after undergoing hydrothermal aging at 800 °C. Experimental results indicated that the synergistic effect between Ce and Mn in CeMnOx improves the redox properties and acidity of the catalyst due to the presence of Ce3+, Mn4+, and abundant adsorbed oxygen species, which facilitate low-temperature SCR reactions. Furthermore, the interaction of CeMnOx with Cu-SSZ-39 stabilizes the zeolite framework and hinders the agglomeration of Cu species during the hydrothermal aging process, contributing to its exceptional hydrothermal stability. The kinetics and NO oxidation experiments demonstrated that CeMnOx provides access to fast SCR reaction pathways by oxidizing NO to NO2, resulting in a significant increase in low-temperature activity. This study provides novel guidelines for the design and preparation of Cu-SSZ-39 zeolite with outstanding SCR performance over a wide temperature range.
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
Catalysts
Catalysts CHEMISTRY, PHYSICAL-
CiteScore
6.80
自引率
7.70%
发文量
1330
审稿时长
3 months
期刊介绍: Catalysts (ISSN 2073-4344) is an international open access journal of catalysts and catalyzed reactions. Catalysts publishes reviews, regular research papers (articles) and short communications. Our aim is to encourage scientists to publish their experimental and theoretical results in as much detail as possible. Therefore, there is no restriction on the length of the papers. The full experimental details must be provided so that the results can be reproduced.
×
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:481959085
Book学术官方微信