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Three Ru-based catalysts were synthesized using in-situ synthesis, impregnation, and deposition-precipitation methods in combination with MFI zeolites to investigate their catalytic oxidation activity toward propane (C3H8). The catalyst synthesized via the in-situ method, denoted as Ru@MFI, exhibited the highest low-temperature oxidation activity, achieving a 90% conversion rate at 270℃, along with remarkable thermal stability at high temperatures and hydrophobicity. Characterization techniques, including X-ray diffraction (XRD), N2 adsorption-desorption, high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM), and temperature-programmed desorption of CO (CO-TPD), revealed that Ru confined within the MFI zeolite channels possessed the smallest particle size and highest dispersion, thereby increasing the number of active Ru sites. Further characterization using Raman spectroscopy and hydrogen temperature-programmed reduction (H2-TPR) indicated that interactions between Ru and the MFI framework led to a redistribution of charge around Ru or oxygen, enhancing the reduction capabilities.Consequently, the Ru@MFI catalyst demonstrated superior propane oxidation activity. Additionally, the geometric confinement within the MFI channels maintained the stability and dispersion of Ru species during high-temperature calcination, effectively preventing Ru aggregation and further ensuring the catalyst's high-temperature thermal stability.
, correspAuthors=Yan-fei JIAN, Chi HE, authorNote=null, correspAuthorsNote=null, copyrightStatement=null, copyrightOwner=null, extLink=null, articleAbsUrl=null, sourceXml=null, magXml=null, pdfUrl=null, pdf=null, pdfFileSize=null, pdfExtLink=null, richHtmlUrl=null, mobilePdfUrl=null, reviewReport=null, pdfFirstPage=null, abstractGraph=null, abstractGraphContent=null, abstractVideo=null, citation=null, cebUrl=null, magXmlContent=null, mapNumber=null, authorCompany=null, fund=null, authors=null, authorsList=Jing-jing WANG, Liang-hui XIA, Ya-ni WU, Yu-jie LIU, He XU, Qi-yuan LIU, Ji-chen LIU, Yan-fei JIAN, Chi HE), CN=ArticleExt(id=1241049974587314593, articleId=1241049966513279278, tenantId=1146029695717560320, journalId=1234093305789726721, language=CN, title=MFI分子筛限域Ru催化剂的制备及其丙烷催化燃烧性能, columnId=1241049969449292093, journalTitle=中国环境科学, columnName=臭氧污染与控制, runingTitle=null, highlight=null, articleAbstract=
采用原位合成法、浸渍法和沉积沉淀法制备Ru与MFI分子筛结合的3种催化剂,用于丙烷(C3H8)的催化氧化活性研究.结果显示,通过原位合成法将Ru限域在MFI分子筛孔道内时,Ru@MFI催化剂展现出最佳的低温C3H8氧化活性,在270℃时达到90%转化率,并表现出卓越的高温热稳定性和抗水性.通过XRD、N2吸脱附、HAADF-STEM以及CO-TPD等表征技术发现,限域在MFI分子筛孔道内部的Ru具有最小的粒径和最高的分散度,增加了活性Ru位点的数量.拉曼和H2-TPR表征结果表明,孔道内的Ru与MFI之间相互作用导致电荷重新分布,增强了还原性能.因此,Ru@MFI催化剂呈现出最优异的C3H8氧化活性.此外,MFI孔道的几何限制作用在高温焙烧过程中维持Ru的稳定性和分散度,有效避免了Ru的聚集,进一步确保了催化剂的高温热稳定性.
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1.西安交通大学能源与动力工程学院,动力工程多相流国家重点实验室,陕西 西安 710049, bio={"content":"
王晶晶(1993-),女,甘肃定西人,西安交通大学博士研究生,主要从事挥发性有机污染物降解和分子筛封装贵金属研究.ijjwang@stu.xjtu.edu.cn.
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王晶晶(1993-),女,甘肃定西人,西安交通大学博士研究生,主要从事挥发性有机污染物降解和分子筛封装贵金属研究.ijjwang@stu.xjtu.edu.cn.
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126:459-469., articleTitle=Component regulation in novel La-Co-O-C composite catalyst for boosted redox reactions and enhanced thermal stability in methane combustion, refAbstract=null)], funds=[Fund(id=1241049994732556576, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, awardId=2022YFB4101500, language=CN, fundingSource=国家重点研发计划(2022YFB4101500), fundOrder=null, country=null), Fund(id=1241049994849997101, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, awardId=22276145, language=CN, fundingSource=国家自然科学基金资助项目(22276145), fundOrder=null, country=null), Fund(id=1241049996548690240, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, awardId=21922606, language=CN, fundingSource=国家自然科学基金资助项目(21922606), fundOrder=null, country=null)], companyList=[AuthorCompany(id=1241049975065465264, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, xref=1., ext=[AuthorCompanyExt(id=1241049975073853873, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, companyId=1241049975065465264, language=EN, country=null, province=null, city=null, postcode=null, companyName=null, departmentName=null, remark=
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催化剂的性能测试, figureFileSmall=6Vhu41I8+9p/2kQ0DfGx8g==, figureFileBig=6bp3OzbBaMs/qWdShiRMGQ==, tableContent=null), ArticleFig(id=1241049989586145291, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.2, caption=
XRD pattern of catalysts, figureFileSmall=qbqiPcwNiaZ1xmym0b/A5Q==, figureFileBig=6mrhsMbiZUZHKQJBm7bKqg==, tableContent=null), ArticleFig(id=1241049989812637717, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=CN, label=图2, caption=
催化剂的XRD谱图, figureFileSmall=qbqiPcwNiaZ1xmym0b/A5Q==, figureFileBig=6mrhsMbiZUZHKQJBm7bKqg==, tableContent=null), ArticleFig(id=1241049990001381408, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.3, caption=
N2 adsorption and desorption curve of catalysts, figureFileSmall=C5y326OluzIg2DU9pzJYaQ==, figureFileBig=P6r15g+vDD93rNWCa3H/wQ==, tableContent=null), ArticleFig(id=1241049990181736495, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=CN, label=图3, caption=
催化剂的N2吸脱附曲线, figureFileSmall=C5y326OluzIg2DU9pzJYaQ==, figureFileBig=P6r15g+vDD93rNWCa3H/wQ==, tableContent=null), ArticleFig(id=1241049990466949186, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.4, caption=
(a-c) High-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM) images and (d-f)high-resolution transmission electron microscopy (HRTEM) images, figureFileSmall=VuY1E1eB60B+eHW923zTog==, figureFileBig=wLuMJsrvxMsGjEZrL3ra6w==, tableContent=null), ArticleFig(id=1241049992241139810, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=CN, label=图4, caption=
(a-c)高角环形暗场扫描透射(HAADF-STEM)图像和(d-f)高分辨透射电子显微镜(HRTEM)图像, figureFileSmall=VuY1E1eB60B+eHW923zTog==, figureFileBig=wLuMJsrvxMsGjEZrL3ra6w==, tableContent=null), ArticleFig(id=1241049992576684149, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.5, caption=
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催化剂的CO脱附曲线, figureFileSmall=hHNKaEux9gV6Udy8j3lbaA==, figureFileBig=SolPs/PdsoKxJbasgQyadw==, tableContent=null), ArticleFig(id=1241049993075806357, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.6, caption=
Raman spectra of catalysts, figureFileSmall=YCn17MSrJPrpNcP9xrucLg==, figureFileBig=PPzzuyTZmJEv1IKkMi6hPQ==, tableContent=null), ArticleFig(id=1241049993197441188, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=CN, label=图6, caption=
催化剂的拉曼光谱, figureFileSmall=YCn17MSrJPrpNcP9xrucLg==, figureFileBig=PPzzuyTZmJEv1IKkMi6hPQ==, tableContent=null), ArticleFig(id=1241049993491042489, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Fig.7, caption=
H2-TPR spectra of catalysts, figureFileSmall=E5w7Nv1OWk4IWfv5O0f66Q==, figureFileBig=ICaDALXblb98eJUWyhKTLw==, tableContent=null), ArticleFig(id=1241049993654620365, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=CN, label=图7, caption=
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T50, T90, and T100 for C3H8 oxidation over fresh and high-temperature calcined catalysts
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| 催化剂 | 新鲜 | 700℃高温 |
|---|
| T50 | T90 | T100 | T50 | T90 | T100 |
|---|
| Ru@MFI | 245 | 270 | 300 | 262 | 293 | 320 |
| Ru/MFI-IM | 258 | 300 | 340 | 316 | 445 | 590 |
| Ru/MFI-DP | 316 | 390 | 500 | >500 | - | - |
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新鲜催化剂与高温焙烧后催化剂的C3H8氧化的T50,T90及T100
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| 催化剂 | 新鲜 | 700℃高温 |
|---|
| T50 | T90 | T100 | T50 | T90 | T100 |
|---|
| Ru@MFI | 245 | 270 | 300 | 262 | 293 | 320 |
| Ru/MFI-IM | 258 | 300 | 340 | 316 | 445 | 590 |
| Ru/MFI-DP | 316 | 390 | 500 | >500 | - | - |
), ArticleFig(id=1241049994220851455, tenantId=1146029695717560320, journalId=1234093305789726721, articleId=1241049966513279278, language=EN, label=Table 2, caption=
Structural properties of catalysts
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| 催化剂 | 比表面积(m2/g)a | 微孔面积(m2/g)b | 总孔容(cm3/g)b | 微孔孔容(cm3/g)b | Ru含量(wt%)c |
|---|
| Ru@MFI | 399.32 | 157.08 | 0.662 | 0.182 | 0.60 |
| Ru/MFI-IM | 340.05 | 183.33 | 0.495 | 0.157 | 0.59 |
| Ru/MFI-DP | 329.74 | 177.36 | 0.484 | 0.152 | 0.60 |
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催化剂的结构性质
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| 催化剂 | 比表面积(m2/g)a | 微孔面积(m2/g)b | 总孔容(cm3/g)b | 微孔孔容(cm3/g)b | Ru含量(wt%)c |
|---|
| Ru@MFI | 399.32 | 157.08 | 0.662 | 0.182 | 0.60 |
| Ru/MFI-IM | 340.05 | 183.33 | 0.495 | 0.157 | 0.59 |
| Ru/MFI-DP | 329.74 | 177.36 | 0.484 | 0.152 | 0.60 |
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