Benxiong Hu, Tao Yang, You Peng, Fushan Chen, Dongsheng Liu
{"title":"用于稀薄燃烧氮氧化物脱除的 Pt/Ba/CoxMg1-xAl2O4 催化剂的高温性能","authors":"Benxiong Hu, Tao Yang, You Peng, Fushan Chen, Dongsheng Liu","doi":"10.1007/s10562-024-04852-2","DOIUrl":null,"url":null,"abstract":"<div><p>A series of catalysts Pt/Ba/Co<sub><i>x</i></sub>Mg<sub>1-<i>x</i></sub>Al<sub>2</sub>O<sub>4</sub> supported by cobalt doped hydrotalcite materials were prepared by coprecipitation-impregnation method for NO<sub><i>x</i></sub> removal at 250–500 °C. The techniques of XRD, TEM, XPS, BET, H<sub>2</sub>-TPR, NO<sub><i>x</i></sub>-TPD, and FT-IR were employed to study the structure and properties of the catalysts. After Co doping, the specific surface area of the catalyst is significantly increased, while the number of surface reactive oxygen species is increased, making NO more easily oxidized to NO<sub>2</sub>, which is conducive to NO<sub><i>x</i></sub> storage. Meanwhile, XRD and TEM results show that Co doping also promotes the dispersion of BaCO<sub>3</sub>, which is the NO<sub><i>x</i></sub> storage site. In addition, the results of TEM and XPS before and after high temperature reaction showed that the active center Pt maintained good dispersion, no obvious sintering occurred, and the valence state of Co remained unchanged. The above characterization results show that the addition of Co significantly improves the storage capacity and thermal stability of the storage intermediates in the catalyst, that is, enhances the elimination performance of lean burn NO<sub><i>x</i></sub> at high temperatures. Co-doped catalysts Pt/Ba/Co<sub><i>x</i></sub>Mg<sub>1-<i>x</i></sub>Al<sub>2</sub>O<sub>4</sub> (<i>x</i> = 0.1, 0.3 and 0.5) showed better high-temperature activity than Pt/Ba/MgAl<sub>2</sub>O<sub>4</sub>. Pt/Ba/Co<sub>0.3</sub>Mg<sub>0.7</sub>Al<sub>2</sub>O<sub>4</sub> showed the highest De-NO<sub><i>x</i></sub> efficiency of 93.2% at 400 ºC and 88.7% at 450 ºC, respectively.</p><h3>Graphical Abstract</h3>\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>","PeriodicalId":508,"journal":{"name":"Catalysis Letters","volume":"155 1","pages":""},"PeriodicalIF":2.3000,"publicationDate":"2024-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"The High-Temperature Performance of Pt/Ba/CoxMg1-xAl2O4 Catalysts for Lean-Burn NOx Removal\",\"authors\":\"Benxiong Hu, Tao Yang, You Peng, Fushan Chen, Dongsheng Liu\",\"doi\":\"10.1007/s10562-024-04852-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>A series of catalysts Pt/Ba/Co<sub><i>x</i></sub>Mg<sub>1-<i>x</i></sub>Al<sub>2</sub>O<sub>4</sub> supported by cobalt doped hydrotalcite materials were prepared by coprecipitation-impregnation method for NO<sub><i>x</i></sub> removal at 250–500 °C. The techniques of XRD, TEM, XPS, BET, H<sub>2</sub>-TPR, NO<sub><i>x</i></sub>-TPD, and FT-IR were employed to study the structure and properties of the catalysts. After Co doping, the specific surface area of the catalyst is significantly increased, while the number of surface reactive oxygen species is increased, making NO more easily oxidized to NO<sub>2</sub>, which is conducive to NO<sub><i>x</i></sub> storage. Meanwhile, XRD and TEM results show that Co doping also promotes the dispersion of BaCO<sub>3</sub>, which is the NO<sub><i>x</i></sub> storage site. In addition, the results of TEM and XPS before and after high temperature reaction showed that the active center Pt maintained good dispersion, no obvious sintering occurred, and the valence state of Co remained unchanged. The above characterization results show that the addition of Co significantly improves the storage capacity and thermal stability of the storage intermediates in the catalyst, that is, enhances the elimination performance of lean burn NO<sub><i>x</i></sub> at high temperatures. Co-doped catalysts Pt/Ba/Co<sub><i>x</i></sub>Mg<sub>1-<i>x</i></sub>Al<sub>2</sub>O<sub>4</sub> (<i>x</i> = 0.1, 0.3 and 0.5) showed better high-temperature activity than Pt/Ba/MgAl<sub>2</sub>O<sub>4</sub>. Pt/Ba/Co<sub>0.3</sub>Mg<sub>0.7</sub>Al<sub>2</sub>O<sub>4</sub> showed the highest De-NO<sub><i>x</i></sub> efficiency of 93.2% at 400 ºC and 88.7% at 450 ºC, respectively.</p><h3>Graphical Abstract</h3>\\n<div><figure><div><div><picture><source><img></source></picture></div></div></figure></div></div>\",\"PeriodicalId\":508,\"journal\":{\"name\":\"Catalysis Letters\",\"volume\":\"155 1\",\"pages\":\"\"},\"PeriodicalIF\":2.3000,\"publicationDate\":\"2024-11-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Letters\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10562-024-04852-2\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Letters","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10562-024-04852-2","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
采用共沉淀-浸渍法制备了一系列以掺钴氢铝土矿材料为支撑的 Pt/Ba/CoxMg1-xAl2O4 催化剂，用于在 250-500 ℃ 下脱除氮氧化物。采用 XRD、TEM、XPS、BET、H2-TPR、NOx-TPD 和 FT-IR 等技术研究了催化剂的结构和性质。掺杂 Co 后，催化剂的比表面积显著增加，表面活性氧的数量增加，使 NO 更容易氧化成 NO2，有利于 NOx 的储存。同时，XRD 和 TEM 结果表明，Co 掺杂也促进了作为 NOx 储存位点的 BaCO3 的分散。此外，高温反应前后的 TEM 和 XPS 结果表明，活性中心铂保持了良好的分散性，没有发生明显的烧结，Co 的价态保持不变。上述表征结果表明，Co 的加入明显提高了催化剂中储存中间体的储存能力和热稳定性，即提高了高温下贫烧氮氧化物的消除性能。掺杂 Co 的催化剂 Pt/Ba/CoxMg1-xAl2O4（x = 0.1、0.3 和 0.5）显示出比 Pt/Ba/MgAl2O4 更好的高温活性。Pt/Ba/Co0.3Mg0.7Al2O4 的脱氮效率最高，在 400 ºC 时为 93.2%，在 450 ºC 时为 88.7%。
The High-Temperature Performance of Pt/Ba/CoxMg1-xAl2O4 Catalysts for Lean-Burn NOx Removal
A series of catalysts Pt/Ba/CoxMg1-xAl2O4 supported by cobalt doped hydrotalcite materials were prepared by coprecipitation-impregnation method for NOx removal at 250–500 °C. The techniques of XRD, TEM, XPS, BET, H2-TPR, NOx-TPD, and FT-IR were employed to study the structure and properties of the catalysts. After Co doping, the specific surface area of the catalyst is significantly increased, while the number of surface reactive oxygen species is increased, making NO more easily oxidized to NO2, which is conducive to NOx storage. Meanwhile, XRD and TEM results show that Co doping also promotes the dispersion of BaCO3, which is the NOx storage site. In addition, the results of TEM and XPS before and after high temperature reaction showed that the active center Pt maintained good dispersion, no obvious sintering occurred, and the valence state of Co remained unchanged. The above characterization results show that the addition of Co significantly improves the storage capacity and thermal stability of the storage intermediates in the catalyst, that is, enhances the elimination performance of lean burn NOx at high temperatures. Co-doped catalysts Pt/Ba/CoxMg1-xAl2O4 (x = 0.1, 0.3 and 0.5) showed better high-temperature activity than Pt/Ba/MgAl2O4. Pt/Ba/Co0.3Mg0.7Al2O4 showed the highest De-NOx efficiency of 93.2% at 400 ºC and 88.7% at 450 ºC, respectively.
期刊介绍：
Catalysis Letters aim is the rapid publication of outstanding and high-impact original research articles in catalysis. The scope of the journal covers a broad range of topics in all fields of both applied and theoretical catalysis, including heterogeneous, homogeneous and biocatalysis.
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