Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

Peng Lu; Supriya Ghosh; Matheus Dorneles de Mello; Huda Sharbini Kamaluddin; Xinyu Li; Gaurav Kumar; Xuekui Duan; Milinda Abeykoon; J. Anibal Boscoboinik; Liang Qi; Heng Dai; Tianyi Luo; Shaeel Al-Thabaiti; Katabathini Narasimharao; Zaheer Khan; Jeffrey D. Rimer; Alexis T. Bell; Paul Dauenhauer; K. Andre Mkhoyan; Michael Tsapatsis

doi:10.1002/anie.202104574

Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

Peng Lu
, Supriya Ghosh
, Matheus Dorneles de Mello
, Huda Sharbini Kamaluddin
, Xinyu Li
, Gaurav Kumar
, Xuekui Duan
, Milinda Abeykoon
, J. Anibal Boscoboinik
, Liang Qi
, Heng Dai
, Tianyi Luo
, Shaeel Al-Thabaiti
, Katabathini Narasimharao
, Zaheer Khan
, Jeffrey D. Rimer
, Alexis T. Bell
, Paul Dauenhauer
, K. Andre Mkhoyan
, Michael Tsapatsis

Research output: Contribution to journal › Article › peer-review

35 Scopus citations

Abstract

Synthesis of a pentasil-type zeolite with ultra-small few-unit-cell crystalline domains, which we call FDP (few-unit-cell crystalline domain pentasil), is reported. FDP is made using bis-1,5(tributyl ammonium) pentamethylene cations as structure directing agent (SDA). This di-quaternary ammonium SDA combines butyl ammonium, in place of the one commonly used for MFI synthesis, propyl ammonium, and a five-carbon nitrogen-connecting chain, in place of the six-carbon connecting chain SDAs that are known to fit well within the MFI pores. X-ray diffraction analysis and electron microscopy imaging of FDP indicate ca. 10 nm crystalline domains organized in hierarchical micro-/meso-porous aggregates exhibiting mesoscopic order with an aggregate particle size up to ca. 5 μm. Al and Sn can be incorporated into the FDP zeolite framework to produce active and selective methanol-to-hydrocarbon and glucose isomerization catalysts, respectively.

Original language	English (US)
Pages (from-to)	19214-19221
Number of pages	8
Journal	Angewandte Chemie - International Edition
Volume	60
Issue number	35
DOIs	https://doi.org/10.1002/anie.202104574
State	Published - Aug 23 2021

Bibliographical note

Funding Information:
The authors extend their appreciation to the Deputyship for Research & Innovation, Ministry of Education in Saudi Arabia for funding this research work through the project number (721). Partial support for this work (certain catalysis experiments and characterizations) was also provided by the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award No. DE‐SC0001004. Parts of this work were carried out in the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC (Award Number DMR‐2011401) and the NNCI (Award Number ECCS‐2025124) programs. S.G. and K.A.M. were supported by the NSF through the University of Minnesota MRSEC under award number DMR‐2011401. The authors are grateful for Dr. Renato N. Sampaio and Dr. Javier Concepcion, Chemistry Division of Brookhaven National Laboratory, for providing the experimental setup for glucose isomerization catalysis experiments. J.D.R. acknowledges support primarily from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award DE‐SC0014468) and additional support from the Welch Foundation (Award E‐1794). A.T.B. and L.Q. acknowledge support from the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231, L.Q. also acknowledges support from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, People's Republic of China.

Publisher Copyright:
© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

Keywords

adsorption
catalysis
di-quaternary structure directing agents
pentasil
ultrasmall crystalline domain

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Lu, P., Ghosh, S., Dorneles de Mello, M., Kamaluddin, H. S., Li, X., Kumar, G., Duan, X., Abeykoon, M., Boscoboinik, J. A., Qi, L., Dai, H., Luo, T., Al-Thabaiti, S., Narasimharao, K., Khan, Z., Rimer, J. D., Bell, A. T., Dauenhauer, P., Mkhoyan, K. A., & Tsapatsis, M. (2021). Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent. Angewandte Chemie - International Edition, 60(35), 19214-19221. https://doi.org/10.1002/anie.202104574

Lu, P, Ghosh, S, Dorneles de Mello, M, Kamaluddin, HS, Li, X, Kumar, G, Duan, X, Abeykoon, M, Boscoboinik, JA, Qi, L, Dai, H, Luo, T, Al-Thabaiti, S, Narasimharao, K, Khan, Z, Rimer, JD, Bell, AT, Dauenhauer, P , Mkhoyan, KA & Tsapatsis, M 2021, 'Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent', Angewandte Chemie - International Edition, vol. 60, no. 35, pp. 19214-19221. https://doi.org/10.1002/anie.202104574

@article{f13cda2e96554fcfb6c9d566e9ea4712,

title = "Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent",

abstract = "Synthesis of a pentasil-type zeolite with ultra-small few-unit-cell crystalline domains, which we call FDP (few-unit-cell crystalline domain pentasil), is reported. FDP is made using bis-1,5(tributyl ammonium) pentamethylene cations as structure directing agent (SDA). This di-quaternary ammonium SDA combines butyl ammonium, in place of the one commonly used for MFI synthesis, propyl ammonium, and a five-carbon nitrogen-connecting chain, in place of the six-carbon connecting chain SDAs that are known to fit well within the MFI pores. X-ray diffraction analysis and electron microscopy imaging of FDP indicate ca. 10 nm crystalline domains organized in hierarchical micro-/meso-porous aggregates exhibiting mesoscopic order with an aggregate particle size up to ca. 5 μm. Al and Sn can be incorporated into the FDP zeolite framework to produce active and selective methanol-to-hydrocarbon and glucose isomerization catalysts, respectively.",

keywords = "adsorption, catalysis, di-quaternary structure directing agents, pentasil, ultrasmall crystalline domain",

author = "Peng Lu and Supriya Ghosh and \{Dorneles de Mello\}, Matheus and Kamaluddin, \{Huda Sharbini\} and Xinyu Li and Gaurav Kumar and Xuekui Duan and Milinda Abeykoon and Boscoboinik, \{J. Anibal\} and Liang Qi and Heng Dai and Tianyi Luo and Shaeel Al-Thabaiti and Katabathini Narasimharao and Zaheer Khan and Rimer, \{Jeffrey D.\} and Bell, \{Alexis T.\} and Paul Dauenhauer and Mkhoyan, \{K. Andre\} and Michael Tsapatsis",

note = "Funding Information: The authors extend their appreciation to the Deputyship for Research \& Innovation, Ministry of Education in Saudi Arabia for funding this research work through the project number (721). Partial support for this work (certain catalysis experiments and characterizations) was also provided by the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award No. DE‐SC0001004. Parts of this work were carried out in the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC (Award Number DMR‐2011401) and the NNCI (Award Number ECCS‐2025124) programs. S.G. and K.A.M. were supported by the NSF through the University of Minnesota MRSEC under award number DMR‐2011401. The authors are grateful for Dr. Renato N. Sampaio and Dr. Javier Concepcion, Chemistry Division of Brookhaven National Laboratory, for providing the experimental setup for glucose isomerization catalysis experiments. J.D.R. acknowledges support primarily from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award DE‐SC0014468) and additional support from the Welch Foundation (Award E‐1794). A.T.B. and L.Q. acknowledge support from the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231, L.Q. also acknowledges support from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, People's Republic of China. Publisher Copyright: {\textcopyright} 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH",

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month = aug,

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doi = "10.1002/anie.202104574",

language = "English (US)",

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T1 - Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

AU - Lu, Peng

AU - Ghosh, Supriya

AU - Dorneles de Mello, Matheus

AU - Kamaluddin, Huda Sharbini

AU - Li, Xinyu

AU - Kumar, Gaurav

AU - Duan, Xuekui

AU - Abeykoon, Milinda

AU - Boscoboinik, J. Anibal

AU - Qi, Liang

AU - Dai, Heng

AU - Luo, Tianyi

AU - Al-Thabaiti, Shaeel

AU - Narasimharao, Katabathini

AU - Khan, Zaheer

AU - Rimer, Jeffrey D.

AU - Bell, Alexis T.

AU - Dauenhauer, Paul

AU - Mkhoyan, K. Andre

AU - Tsapatsis, Michael

N1 - Funding Information: The authors extend their appreciation to the Deputyship for Research & Innovation, Ministry of Education in Saudi Arabia for funding this research work through the project number (721). Partial support for this work (certain catalysis experiments and characterizations) was also provided by the Catalysis Center for Energy Innovation, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences under Award No. DE‐SC0001004. Parts of this work were carried out in the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC (Award Number DMR‐2011401) and the NNCI (Award Number ECCS‐2025124) programs. S.G. and K.A.M. were supported by the NSF through the University of Minnesota MRSEC under award number DMR‐2011401. The authors are grateful for Dr. Renato N. Sampaio and Dr. Javier Concepcion, Chemistry Division of Brookhaven National Laboratory, for providing the experimental setup for glucose isomerization catalysis experiments. J.D.R. acknowledges support primarily from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (Award DE‐SC0014468) and additional support from the Welch Foundation (Award E‐1794). A.T.B. and L.Q. acknowledge support from the Office of Science, Office of Basic Energy Sciences, of the U.S. Department of Energy under Contract No. DE‐AC02‐05CH11231, L.Q. also acknowledges support from the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, People's Republic of China. Publisher Copyright: © 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH

PY - 2021/8/23

Y1 - 2021/8/23

N2 - Synthesis of a pentasil-type zeolite with ultra-small few-unit-cell crystalline domains, which we call FDP (few-unit-cell crystalline domain pentasil), is reported. FDP is made using bis-1,5(tributyl ammonium) pentamethylene cations as structure directing agent (SDA). This di-quaternary ammonium SDA combines butyl ammonium, in place of the one commonly used for MFI synthesis, propyl ammonium, and a five-carbon nitrogen-connecting chain, in place of the six-carbon connecting chain SDAs that are known to fit well within the MFI pores. X-ray diffraction analysis and electron microscopy imaging of FDP indicate ca. 10 nm crystalline domains organized in hierarchical micro-/meso-porous aggregates exhibiting mesoscopic order with an aggregate particle size up to ca. 5 μm. Al and Sn can be incorporated into the FDP zeolite framework to produce active and selective methanol-to-hydrocarbon and glucose isomerization catalysts, respectively.

AB - Synthesis of a pentasil-type zeolite with ultra-small few-unit-cell crystalline domains, which we call FDP (few-unit-cell crystalline domain pentasil), is reported. FDP is made using bis-1,5(tributyl ammonium) pentamethylene cations as structure directing agent (SDA). This di-quaternary ammonium SDA combines butyl ammonium, in place of the one commonly used for MFI synthesis, propyl ammonium, and a five-carbon nitrogen-connecting chain, in place of the six-carbon connecting chain SDAs that are known to fit well within the MFI pores. X-ray diffraction analysis and electron microscopy imaging of FDP indicate ca. 10 nm crystalline domains organized in hierarchical micro-/meso-porous aggregates exhibiting mesoscopic order with an aggregate particle size up to ca. 5 μm. Al and Sn can be incorporated into the FDP zeolite framework to produce active and selective methanol-to-hydrocarbon and glucose isomerization catalysts, respectively.

KW - adsorption

KW - catalysis

KW - di-quaternary structure directing agents

KW - pentasil

KW - ultrasmall crystalline domain

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UR - https://www.scopus.com/pages/publications/85111876423#tab=citedBy

U2 - 10.1002/anie.202104574

DO - 10.1002/anie.202104574

M3 - Article

C2 - 34189811

AN - SCOPUS:85111876423

SN - 1433-7851

VL - 60

SP - 19214

EP - 19221

JO - Angewandte Chemie - International Edition

JF - Angewandte Chemie - International Edition

IS - 35

ER -

Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

Abstract

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Few-Unit-Cell MFI Zeolite Synthesized using a Simple Di-quaternary Ammonium Structure-Directing Agent

Abstract

Bibliographical note

Keywords

MRSEC Support

PubMed: MeSH publication types

Publisher link

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University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

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