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题名: Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst
作者: Li, Junjie1;  Liu, Min1;  Guo, Xinwen1;  Xu, Shutao2;  Wei, Yingxu2;  Liu, Zhongmin2;  Song, Chunshan1, 3
关键词: Al-zoned ZSM-5 ;  enclosed hollow structure ;  distorted tetrahedral Al ;  dealumination-realumination process ;  reinserted Al ;  interconnected mesopore structure ;  MTP
刊名: ACS APPLIED MATERIALS & INTERFACES
发表日期: 2017-08-09
DOI: 10.1021/acsami.7b07806
卷: 9, 期:31, 页:26096-26106
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Technology
类目[WOS]: Nanoscience & Nanotechnology ;  Materials Science, Multidisciplinary
研究领域[WOS]: Science & Technology - Other Topics ;  Materials Science
英文摘要: ZSM-5 that uses TPAOH as a template has an Al-rich exterior and defective Si-rich interior; thus, a simple base leaching selectively removed the Si-rich interior while the Al-rich exterior was protected. This catalyst showed no change in stability comparing with parent ZSM-5 during the MTP reaction that was attributed to the enclosed hollow structure and richly acidic outer shell. A preliminary fluorination, however, both removed defective Si-sites and caused distortion in tetrahedral aluminum that made the outer shell susceptible to alkaline treatment. These distorted tetrahedral Al were mostly leached out by NaOH in 1 min. Furthermore, aluminum in the filtrate was slowly redeposited onto the zeolite, serving as external pore-directing agents to control silicon dissolution from the Si-rich interior. This dealumination-realumination alkaline treatment process led to a higher solid yield and a uniform opened-mesopore structure with mesopores around 13 nm in diameter. This material was characterized by SEM, TEM, N-2 adsorption, and mercury porosimetry.In addition, NH3-TPD, OH-IR, Al-27 MAS NMR, and H-1 MAS NMR results demonstrated that the reinserted Al were unlike the framework Al, contributing less to acidity. The dealumination-realumination process, therefore, was also capable of tuning the acidity of the mesoporous ZSM-5. This mesoporous catalyst exhibited a longer lifetime and a higher propylene selectivity than other catalysts with an enclosed mesopore structure.
关键词[WOS]: METHANOL-TO-HYDROCARBONS ;  CONTROLLED DESILICATION ;  FRAMEWORK DEFECTS ;  ZEOLITE CATALYSTS ;  MFI ZEOLITES ;  CONVERSION ;  H-ZSM-5 ;  SELECTIVITY ;  ALUMINUM ;  MESOPOROSITY
语种: 英语
WOS记录号: WOS:000407540400048
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/149819
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China
2.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
3.Penn State Univ, Dept Energy & Mineral Engn, EMS Energy Inst, PSU DUT Joint Ctr Energy Res, University Pk, PA 16802 USA

Recommended Citation:
Li, Junjie,Liu, Min,Guo, Xinwen,et al. Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst[J]. ACS APPLIED MATERIALS & INTERFACES,2017,9(31):26096-26106.
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