Interconnected Hierarchical ZSM-5 with Tunable Acidity Prepared by a Dealumination-Realumination Process: A Superior MTP Catalyst | |
Guo, Xinwen3; Li, Junjie3; Liu, Min3; Xu, Shutao1; Wei, Yingxu1; Liu, Zhongmin1; Song, Chunshan2,3 | |
刊名 | ACS APPLIED MATERIALS & INTERFACES |
2017-08-09 | |
卷号 | 9期号:31页码:26096-26106 |
关键词 | Al-zoned ZSM-5 enclosed hollow structure distorted tetrahedral Al dealumination-realumination process reinserted Al interconnected mesopore structure MTP |
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. |
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 |
关键词[WOS] | METHANOL-TO-HYDROCARBONS ; CONTROLLED DESILICATION ; FRAMEWORK DEFECTS ; ZEOLITE CATALYSTS ; MFI ZEOLITES ; CONVERSION ; H-ZSM-5 ; SELECTIVITY ; ALUMINUM ; MESOPOROSITY |
收录类别 | SCI |
语种 | 英语 |
WOS记录号 | WOS:000407540400048 |
内容类型 | 期刊论文 |
源URL | [http://cas-ir.dicp.ac.cn/handle/321008/149819] |
专题 | 大连化学物理研究所_中国科学院大连化学物理研究所 |
作者单位 | 1.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China 2.Penn State Univ, Dept Energy & Mineral Engn, EMS Energy Inst, PSU DUT Joint Ctr Energy Res, University Pk, PA 16802 USA 3.Dalian Univ Technol, Sch Chem Engn, PSU DUT Joint Ctr Energy Res, State Key Lab Fine Chem, Dalian 116024, Peoples R China |
推荐引用方式 GB/T 7714 | Guo, Xinwen,Li, Junjie,Liu, Min,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 | Guo, Xinwen.,Li, Junjie.,Liu, Min.,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 | Guo, Xinwen,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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