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Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst
Li, Junjie1; Liu, Min1; Guo, Xinwen1; Xu, Shutao2; Wei, Yingxu2; Liu, Zhongmin2; Song, Chunshan1,3
KeywordAl-zoned Zsm-5 Enclosed Hollow Structure Distorted TetrahedrAl Al Dealumination-realumination Process Reinserted Al Interconnected Mesopore Structure Mtp
Source PublicationACS APPLIED MATERIALS & INTERFACES
2017-08-09
DOI10.1021/acsami.7b07806
Volume9Issue:31Pages:26096-26106
Indexed BySCI
SubtypeArticle
WOS HeadingsScience & Technology ; Technology
WOS SubjectNanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS Research AreaScience & Technology - Other Topics ; Materials Science
WOS KeywordMETHANOL-TO-HYDROCARBONS ; CONTROLLED DESILICATION ; FRAMEWORK DEFECTS ; ZEOLITE CATALYSTS ; MFI ZEOLITES ; CONVERSION ; H-ZSM-5 ; SELECTIVITY ; ALUMINUM ; MESOPOROSITY
AbstractZSM-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.
Language英语
WOS IDWOS:000407540400048
Citation statistics
Document Type期刊论文
Identifierhttp://cas-ir.dicp.ac.cn/handle/321008/149819
Collection中国科学院大连化学物理研究所
Affiliation1.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
GB/T 7714
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.
APA Li, Junjie.,Liu, Min.,Guo, Xinwen.,Xu, Shutao.,Wei, Yingxu.,...&Song, Chunshan.(2017).Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst.ACS APPLIED MATERIALS & INTERFACES,9(31),26096-26106.
MLA Li, Junjie,et al."Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst".ACS APPLIED MATERIALS & INTERFACES 9.31(2017):26096-26106.
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