mg离子促进Cu/SSZ-13催化剂对磷中毒选择性催化还原NOx的抗性和再生能力

IF 11.3 1区 环境科学与生态学 Q1 ENGINEERING, ENVIRONMENTAL
Xuan Tang, Yanzhao Gao, Wenbo Li, Sheng Dai, Li Wang, Yun Guo, Yanglong Guo, Wangcheng Zhan and Aiyong Wang*, 
{"title":"mg离子促进Cu/SSZ-13催化剂对磷中毒选择性催化还原NOx的抗性和再生能力","authors":"Xuan Tang,&nbsp;Yanzhao Gao,&nbsp;Wenbo Li,&nbsp;Sheng Dai,&nbsp;Li Wang,&nbsp;Yun Guo,&nbsp;Yanglong Guo,&nbsp;Wangcheng Zhan and Aiyong Wang*,&nbsp;","doi":"10.1021/acs.est.5c01029","DOIUrl":null,"url":null,"abstract":"<p >The SSZ-13 zeolite-supported Cu (Cu/SSZ-13) is a commercial catalyst for ammonia selective catalytic reduction (NH<sub>3</sub>–SCR), but it faces challenges such as phosphorus poisoning in practical applications. Despite extensive investigations into how phosphorus poisoning leads to the deactivation of Cu/SSZ-13, effective strategies for regenerating catalysts with high phosphorus loading poisoned under practical conditions remain underdeveloped. In this study, we propose that incorporating Mg ions into Cu/SSZ-13 zeolites can significantly enhance their resistance and regeneration ability against phosphorus poisoning. After hydrothermal aging at 650 °C, the NH<sub>3</sub>–SCR activity of phosphorus-poisoned Cu/SSZ-13 catalysts with high phosphorus loading (0.6 mmol/g<sub>cat</sub>) cannot be effectively restored; however, the addition of Mg enables nearly complete recovery of their activity. Combining advanced microscopy evidence with complementary spectroscopy results, we reveal that Mg ions occupy the Brønsted acid sites in the six-membered rings (6-MRs) of SSZ-13, which regulates the distribution of subsequently introduced Cu ions while enhancing the stability of Cu<sup>2+</sup> and the framework Al of SSZ-13, inhibiting the aggregation of Cu species after phosphorus poisoning and thereby improving resistance. Furthermore, the preservation of the SSZ-13 framework also effectively facilitates the redispersion of Cu species after hydrothermal aging, significantly restoring NH<sub>3</sub>–SCR performance.</p>","PeriodicalId":36,"journal":{"name":"环境科学与技术","volume":"59 26","pages":"13447–13457"},"PeriodicalIF":11.3000,"publicationDate":"2025-06-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Mg-Ion-Promoted Resistance and Regeneration Ability of Cu/SSZ-13 Catalysts against Phosphorus Poisoning for Selective Catalytic Reduction of NOx\",\"authors\":\"Xuan Tang,&nbsp;Yanzhao Gao,&nbsp;Wenbo Li,&nbsp;Sheng Dai,&nbsp;Li Wang,&nbsp;Yun Guo,&nbsp;Yanglong Guo,&nbsp;Wangcheng Zhan and Aiyong Wang*,&nbsp;\",\"doi\":\"10.1021/acs.est.5c01029\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The SSZ-13 zeolite-supported Cu (Cu/SSZ-13) is a commercial catalyst for ammonia selective catalytic reduction (NH<sub>3</sub>–SCR), but it faces challenges such as phosphorus poisoning in practical applications. Despite extensive investigations into how phosphorus poisoning leads to the deactivation of Cu/SSZ-13, effective strategies for regenerating catalysts with high phosphorus loading poisoned under practical conditions remain underdeveloped. In this study, we propose that incorporating Mg ions into Cu/SSZ-13 zeolites can significantly enhance their resistance and regeneration ability against phosphorus poisoning. After hydrothermal aging at 650 °C, the NH<sub>3</sub>–SCR activity of phosphorus-poisoned Cu/SSZ-13 catalysts with high phosphorus loading (0.6 mmol/g<sub>cat</sub>) cannot be effectively restored; however, the addition of Mg enables nearly complete recovery of their activity. Combining advanced microscopy evidence with complementary spectroscopy results, we reveal that Mg ions occupy the Brønsted acid sites in the six-membered rings (6-MRs) of SSZ-13, which regulates the distribution of subsequently introduced Cu ions while enhancing the stability of Cu<sup>2+</sup> and the framework Al of SSZ-13, inhibiting the aggregation of Cu species after phosphorus poisoning and thereby improving resistance. Furthermore, the preservation of the SSZ-13 framework also effectively facilitates the redispersion of Cu species after hydrothermal aging, significantly restoring NH<sub>3</sub>–SCR performance.</p>\",\"PeriodicalId\":36,\"journal\":{\"name\":\"环境科学与技术\",\"volume\":\"59 26\",\"pages\":\"13447–13457\"},\"PeriodicalIF\":11.3000,\"publicationDate\":\"2025-06-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"环境科学与技术\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acs.est.5c01029\",\"RegionNum\":1,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, ENVIRONMENTAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"环境科学与技术","FirstCategoryId":"1","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.est.5c01029","RegionNum":1,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, ENVIRONMENTAL","Score":null,"Total":0}
引用次数: 0

摘要

SSZ-13沸石负载Cu (Cu/SSZ-13)是一种用于氨选择性催化还原(NH3-SCR)的商业催化剂,但在实际应用中面临着磷中毒等挑战。尽管对磷中毒如何导致Cu/SSZ-13失活进行了广泛的研究,但在实际条件下对高载磷中毒催化剂的有效再生策略尚不成熟。在本研究中,我们提出在Cu/SSZ-13沸石中加入Mg离子可以显著增强其对磷中毒的抗性和再生能力。650℃水热老化后,高载磷量(0.6 mmol/gcat)的磷中毒Cu/SSZ-13催化剂NH3-SCR活性不能有效恢复;然而,Mg的加入使它们的活性几乎完全恢复。结合先进的显微镜证据和互补光谱结果,我们发现Mg离子占据了SSZ-13六元环(6-MRs)中的Brønsted酸位点,这调节了随后引入的Cu离子的分布,同时增强了SSZ-13的Cu2+和框架Al的稳定性,抑制了磷中毒后Cu物种的聚集,从而提高了抗性。此外,SSZ-13框架的保存也有效地促进了热液老化后Cu物种的再分散,显著恢复了NH3-SCR性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mg-Ion-Promoted Resistance and Regeneration Ability of Cu/SSZ-13 Catalysts against Phosphorus Poisoning for Selective Catalytic Reduction of NOx

Mg-Ion-Promoted Resistance and Regeneration Ability of Cu/SSZ-13 Catalysts against Phosphorus Poisoning for Selective Catalytic Reduction of NOx

The SSZ-13 zeolite-supported Cu (Cu/SSZ-13) is a commercial catalyst for ammonia selective catalytic reduction (NH3–SCR), but it faces challenges such as phosphorus poisoning in practical applications. Despite extensive investigations into how phosphorus poisoning leads to the deactivation of Cu/SSZ-13, effective strategies for regenerating catalysts with high phosphorus loading poisoned under practical conditions remain underdeveloped. In this study, we propose that incorporating Mg ions into Cu/SSZ-13 zeolites can significantly enhance their resistance and regeneration ability against phosphorus poisoning. After hydrothermal aging at 650 °C, the NH3–SCR activity of phosphorus-poisoned Cu/SSZ-13 catalysts with high phosphorus loading (0.6 mmol/gcat) cannot be effectively restored; however, the addition of Mg enables nearly complete recovery of their activity. Combining advanced microscopy evidence with complementary spectroscopy results, we reveal that Mg ions occupy the Brønsted acid sites in the six-membered rings (6-MRs) of SSZ-13, which regulates the distribution of subsequently introduced Cu ions while enhancing the stability of Cu2+ and the framework Al of SSZ-13, inhibiting the aggregation of Cu species after phosphorus poisoning and thereby improving resistance. Furthermore, the preservation of the SSZ-13 framework also effectively facilitates the redispersion of Cu species after hydrothermal aging, significantly restoring NH3–SCR performance.

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
环境科学与技术
环境科学与技术 环境科学-工程:环境
CiteScore
17.50
自引率
9.60%
发文量
12359
审稿时长
2.8 months
期刊介绍: Environmental Science & Technology (ES&T) is a co-sponsored academic and technical magazine by the Hubei Provincial Environmental Protection Bureau and the Hubei Provincial Academy of Environmental Sciences. Environmental Science & Technology (ES&T) holds the status of Chinese core journals, scientific papers source journals of China, Chinese Science Citation Database source journals, and Chinese Academic Journal Comprehensive Evaluation Database source journals. This publication focuses on the academic field of environmental protection, featuring articles related to environmental protection and technical advancements.
×
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