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Title: Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets

Abstract

A zeolite with structure type MFI is an aluminosilicate or silicate material that has a three-dimensionally connected pore network, which enables molecular recognition in the size range 0.5-0.6 nm. These micropore dimensions are relevant for many valuable chemical intermediates, and therefore MFI-type zeolites are widely used in the chemical industry as selective catalysts or adsorbents. As with all zeolites, strategies to tailor them for specific applications include controlling their crystal size and shape. Nanometre-thick MFI crystals (nanosheets) have been introduced in pillared and self-pillared (intergrown) architectures, offering improved mass-transfer characteristics for certain adsorption and catalysis applications. Moreover, single (non-intergrown and nonlayered) nanosheets have been used to prepare thin membranes that could be used to improve the energy efficiency of separation processes. However, until now, single MFI nanosheets have been prepared using a multi-step approach based on the exfoliation of layered MFI9,15, followed by centrifugation to remove non-exfoliated particles. This top-down method is time-consuming, costly and low-yield and it produces fragmented nanosheets with submicrometre lateral dimensions. Alternatively, direct (bottom-up) synthesis could produce high-aspect-ratio zeolite nanosheets, with improved yield and at lower cost. Here we use a nanocrystal-seeded growth method triggered by a single rotational intergrowth to synthesize high-aspect-ratio MFI nanosheets withmore » a thickness of 5 nanometres (2.5 unit cells). These high-aspect-ratio nanosheets allow the fabrication of thin and defect-free coatings that effectively cover porous substrates. Finally, these coatings can be intergrown to produce high-flux and ultra-selective MFI membranes that compare favourably with other MFI membranes prepared from existing MFI materials (such as exfoliated nanosheets or nanocrystals).« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2];  [2];  [2];  [3];  [4];  [1];  [1];  [1];  [4];  [1];  [1] more »;  [1] « less
+ Show Author Affiliations
  1. Univ. of Minnesota, Minneapolis, MN (United States)
  2. King Abdulaziz Univ., Jeddah (Saudi Arabia)
  3. Argonne National Lab. (ANL), Lemont, IL (United States)
  4. Univ. of Massachusetts, Amherst, MA (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Scientific User Facilities Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; King Abdulaziz University; National Science Foundation (NSF); USDOE Advanced Research Projects Agency - Energy (ARPA-E)
OSTI Identifier:
1373573
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature (London)
Additional Journal Information:
Journal Name: Nature (London); Journal Volume: 543; Journal Issue: 7647; Journal ID: ISSN 0028-0836
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Jeon, Mi Young, Kim, Donghun, Kumar, Prashant, Lee, Pyung Soo, Rangnekar, Neel, Bai, Peng, Shete, Meera, Elyassi, Bahman, Lee, Han Seung, Narasimharao, Katabathini, Basahel, Sulaiman Nasir, Al-Thabaiti, Shaeel, Xu, Wenqian, Cho, Hong Je, Fetisov, Evgenii O., Thyagarajan, Raghuram, DeJaco, Robert F., Fan, Wei, Mkhoyan, K. Andre, Siepmann, J. Ilja, and Tsapatsis, Michael. Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets. United States: N. p., 2017. Web. doi:10.1038/nature21421.
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Jeon, Mi Young, Kim, Donghun, Kumar, Prashant, Lee, Pyung Soo, Rangnekar, Neel, Bai, Peng, Shete, Meera, Elyassi, Bahman, Lee, Han Seung, Narasimharao, Katabathini, Basahel, Sulaiman Nasir, Al-Thabaiti, Shaeel, Xu, Wenqian, Cho, Hong Je, Fetisov, Evgenii O., Thyagarajan, Raghuram, DeJaco, Robert F., Fan, Wei, Mkhoyan, K. Andre, Siepmann, J. Ilja, & Tsapatsis, Michael. Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets. United States. https://doi.org/10.1038/nature21421
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Jeon, Mi Young, Kim, Donghun, Kumar, Prashant, Lee, Pyung Soo, Rangnekar, Neel, Bai, Peng, Shete, Meera, Elyassi, Bahman, Lee, Han Seung, Narasimharao, Katabathini, Basahel, Sulaiman Nasir, Al-Thabaiti, Shaeel, Xu, Wenqian, Cho, Hong Je, Fetisov, Evgenii O., Thyagarajan, Raghuram, DeJaco, Robert F., Fan, Wei, Mkhoyan, K. Andre, Siepmann, J. Ilja, and Tsapatsis, Michael. Wed . "Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets". United States. https://doi.org/10.1038/nature21421. https://www.osti.gov/servlets/purl/1373573.
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@article{osti_1373573,
title = {Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets},
author = {Jeon, Mi Young and Kim, Donghun and Kumar, Prashant and Lee, Pyung Soo and Rangnekar, Neel and Bai, Peng and Shete, Meera and Elyassi, Bahman and Lee, Han Seung and Narasimharao, Katabathini and Basahel, Sulaiman Nasir and Al-Thabaiti, Shaeel and Xu, Wenqian and Cho, Hong Je and Fetisov, Evgenii O. and Thyagarajan, Raghuram and DeJaco, Robert F. and Fan, Wei and Mkhoyan, K. Andre and Siepmann, J. Ilja and Tsapatsis, Michael},
abstractNote = {A zeolite with structure type MFI is an aluminosilicate or silicate material that has a three-dimensionally connected pore network, which enables molecular recognition in the size range 0.5-0.6 nm. These micropore dimensions are relevant for many valuable chemical intermediates, and therefore MFI-type zeolites are widely used in the chemical industry as selective catalysts or adsorbents. As with all zeolites, strategies to tailor them for specific applications include controlling their crystal size and shape. Nanometre-thick MFI crystals (nanosheets) have been introduced in pillared and self-pillared (intergrown) architectures, offering improved mass-transfer characteristics for certain adsorption and catalysis applications. Moreover, single (non-intergrown and nonlayered) nanosheets have been used to prepare thin membranes that could be used to improve the energy efficiency of separation processes. However, until now, single MFI nanosheets have been prepared using a multi-step approach based on the exfoliation of layered MFI9,15, followed by centrifugation to remove non-exfoliated particles. This top-down method is time-consuming, costly and low-yield and it produces fragmented nanosheets with submicrometre lateral dimensions. Alternatively, direct (bottom-up) synthesis could produce high-aspect-ratio zeolite nanosheets, with improved yield and at lower cost. Here we use a nanocrystal-seeded growth method triggered by a single rotational intergrowth to synthesize high-aspect-ratio MFI nanosheets with a thickness of 5 nanometres (2.5 unit cells). These high-aspect-ratio nanosheets allow the fabrication of thin and defect-free coatings that effectively cover porous substrates. Finally, these coatings can be intergrown to produce high-flux and ultra-selective MFI membranes that compare favourably with other MFI membranes prepared from existing MFI materials (such as exfoliated nanosheets or nanocrystals).},
doi = {10.1038/nature21421},
journal = {Nature (London)},
number = 7647,
volume = 543,
place = {United States},
year = {Wed Mar 15 00:00:00 EDT 2017},
month = {Wed Mar 15 00:00:00 EDT 2017}
}
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    • Angewandte Chemie, Vol. 130, Issue 45
    • DOI: 10.1002/ange.201808991

    Paralyzed membrane: Current-driven synthesis of a metal-organic framework with sharpened propene/propane separation
    journal, October 2018

    Continuous Zeolite MFI Membranes Fabricated from 2D MFI Nanosheets on Ceramic Hollow Fibers
    journal, May 2019

    • Min, Byunghyun; Yang, Shaowei; Korde, Akshay
    • Angewandte Chemie, Vol. 131, Issue 24
    • DOI: 10.1002/ange.201903554

    Liquid dispersions of zeolite monolayers with high catalytic activity prepared by soft-chemical exfoliation
    journal, March 2020

    • Roth, Wieslaw J.; Sasaki, Takayoshi; Wolski, Karol
    • Science Advances, Vol. 6, Issue 12
    • DOI: 10.1126/sciadv.aay8163

    Metal-induced ordered microporous polymers for fabricating large-area gas separation membranes
    journal, November 2018

    Molecularly Mixed Composite Membranes for Advanced Separation Processes
    journal, January 2019

    • Zhu, Guanghui; Zhang, Fengyi; Rivera, Matthew P.
    • Angewandte Chemie International Edition, Vol. 58, Issue 9
    • DOI: 10.1002/anie.201811341

    Template‐Free, Surfactant‐Mediated Orientation of Self‐Assembled Supercrystals of Metal–Organic Framework Particles
    journal, June 2019

    Sol–gel asynchronous crystallization of ultra-selective metal–organic framework membranes for gas separation
    journal, January 2018

    • Li, Wanbin; Wu, Wufeng; Li, Zhanjun
    • Journal of Materials Chemistry A, Vol. 6, Issue 34
    • DOI: 10.1039/c8ta06083e

    Membrane Filtration with Liquids: A Global Approach with Prior Successes, New Developments and Unresolved Challenges
    journal, December 2018

    IDM‐1: A Zeolite with Intersecting Medium and Extra‐Large Pores Built as an Expansion of Zeolite MFI
    journal, May 2020

    • Villaescusa, Luis A.; Li, Jian; Gao, Zihao
    • Angewandte Chemie, Vol. 132, Issue 28
    • DOI: 10.1002/ange.202001740

    MXene molecular sieving membranes for highly efficient gas separation
    journal, January 2018

    Anticorrosion Behavior of Zeolite Coatings Obtained by In Situ Crystallization: A Critical Review
    journal, December 2018

    Highly Oriented Growth of Catalytically Active Zeolite ZSM-5 Films with a Broad Range of Si/Al Ratios
    journal, July 2017

    • Fu, Donglong; Schmidt, Joel E.; Ristanović, Zoran
    • Angewandte Chemie, Vol. 129, Issue 37
    • DOI: 10.1002/ange.201704846

    Polycrystalline Advanced Microporous Framework Membranes for Efficient Separation of Small Molecules and Ions
    journal, July 2019

    An Hetero‐Epitaxially Grown Zeolite Membrane
    journal, October 2019

    • Jeong, Yanghwan; Hong, Sungwon; Jang, Eunhee
    • Angewandte Chemie, Vol. 131, Issue 51
    • DOI: 10.1002/ange.201911164

    Interfacial barriers to gas transport: probing solid-gas interfaces at the atomistic level
    journal, July 2019

    Controlled release of siliceous species for the fabrication of highly b -oriented MFI zeolite films
    journal, January 2019

    • Peng, Yong; Xu, Ruilan; Lu, Xiaofei
    • CrystEngComm, Vol. 21, Issue 28
    • DOI: 10.1039/c9ce00817a

    Bridging the Gap between Structurally Distinct 2D Lamellar Zeolitic Precursors through a 3D Germanosilicate Intermediate
    journal, September 2019

    • Xu, Le; Choudhary, Madhuresh K.; Muraoka, Koki
    • Angewandte Chemie International Edition, Vol. 58, Issue 41
    • DOI: 10.1002/anie.201907857

    Ultrafast synthesis of zeolites: breakthrough, progress and perspective
    journal, January 2019

    • Liu, Zhendong; Zhu, Jie; Wakihara, Toru
    • Inorganic Chemistry Frontiers, Vol. 6, Issue 1
    • DOI: 10.1039/c8qi00939b

    Zeolitic Imidazolate Framework Membranes for Light Olefin/Paraffin Separation
    journal, December 2018

    Ultra‐thin skin carbon hollow fiber membranes for sustainable molecular separations
    journal, April 2019

    • Zhang, Chen; Kumar, Rachana; Koros, William J.
    • AIChE Journal, Vol. 65, Issue 8
    • DOI: 10.1002/aic.16611

    2D MXene Nanofilms with Tunable Gas Transport Channels
    journal, June 2018

    • Shen, Jie; Liu, Guozhen; Ji, Yufan
    • Advanced Functional Materials, Vol. 28, Issue 31
    • DOI: 10.1002/adfm.201801511

    Molecularly Mixed Composite Membranes for Advanced Separation Processes
    journal, January 2019

    • Zhu, Guanghui; Zhang, Fengyi; Rivera, Matthew P.
    • Angewandte Chemie, Vol. 131, Issue 9
    • DOI: 10.1002/ange.201811341

    An Hetero‐Epitaxially Grown Zeolite Membrane
    journal, October 2019

    • Jeong, Yanghwan; Hong, Sungwon; Jang, Eunhee
    • Angewandte Chemie International Edition, Vol. 58, Issue 51
    • DOI: 10.1002/anie.201911164

    IDM‐1: A Zeolite with Intersecting Medium and Extra‐Large Pores Built as an Expansion of Zeolite MFI
    journal, May 2020

    • Villaescusa, Luis A.; Li, Jian; Gao, Zihao
    • Angewandte Chemie International Edition, Vol. 59, Issue 28
    • DOI: 10.1002/anie.202001740

    Ultrathin ZSM-5 zeolite nanosheet laminated membrane for high-flux desalination of concentrated brines
    journal, November 2018

    Morphology‐Reserved Synthesis of Discrete Nanosheets of CuO@SAPO‐34 and Pore Mouth Catalysis for One‐Pot Oxidation of Cyclohexane
    journal, January 2020

    Thermal processing of zeolite seed layers for the fabrication of compact oriented MFI zeolite films
    journal, January 2018

    • Peng, Yong; Xu, Ruilan; Jiang, Xinde
    • CrystEngComm, Vol. 20, Issue 32
    • DOI: 10.1039/c8ce00943k

    Two-dimensional nanosheet-based gas separation membranes
    journal, January 2018

    • Liu, Min; Gurr, Paul A.; Fu, Qiang
    • Journal of Materials Chemistry A, Vol. 6, Issue 46
    • DOI: 10.1039/c8ta09070j

    Sandwich membranes through a two-dimensional confinement strategy for gas separation
    journal, January 2018

    • Kang, Zixi; Wang, Sasa; Wang, Rongming
    • Materials Chemistry Frontiers, Vol. 2, Issue 10
    • DOI: 10.1039/c8qm00351c

    Uniformly Oriented Zeolite ZSM-5 Membranes with Tunable Wettability on a Porous Ceramic
    journal, August 2018

    • Fu, Donglong; Schmidt, Joel E.; Pletcher, Paul
    • Angewandte Chemie International Edition, Vol. 57, Issue 38
    • DOI: 10.1002/anie.201806361

    Intrinsically Microporous Polymer Nanosheets for High‐Performance Gas Separation Membranes
    journal, December 2019

    • Tamaddondar, Marzieh; Foster, Andrew B.; Luque‐Alled, Jose M.
    • Macromolecular Rapid Communications, Vol. 41, Issue 2
    • DOI: 10.1002/marc.201900572

    Multifunctional nanocomposite hollow fiber membranes by solvent transfer induced phase separation
    journal, November 2017

    Ultrathin ZSM-5 zeolite nanosheet laminated membrane for high-flux desalination of concentrated brines
    journal, November 2018

    Metal-Organic Frameworks for Separation
    journal, March 2018

    • Zhao, Xiang; Wang, Yanxiang; Li, Dong-Sheng
    • Advanced Materials, Vol. 30, Issue 37
    • DOI: 10.1002/adma.201705189

    One-dimensional intergrowths in two-dimensional zeolite nanosheets and their effect on ultra-selective transport
    journal, February 2020

    Continuous Zeolite MFI Membranes Fabricated from 2D MFI Nanosheets on Ceramic Hollow Fibers
    journal, June 2019

    • Min, Byunghyun; Yang, Shaowei; Korde, Akshay
    • Angewandte Chemie International Edition, Vol. 58, Issue 24
    • DOI: 10.1002/anie.201903554

    A Brief Overview on the Anticorrosion Performances of Sol-Gel Zeolite Coatings
    journal, June 2019

    Creation of Well‐Defined “Mid‐Sized” Micropores in Carbon Molecular Sieve Membranes
    journal, August 2019

    para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface
    journal, December 2017

    • Kim, Donghun; Jeon, Mi Young; Stottrup, Benjamin L.
    • Angewandte Chemie International Edition, Vol. 57, Issue 2
    • DOI: 10.1002/anie.201708835

    2D Metal‐Organic Framework Materials for Membrane‐Based Separation
    journal, November 2019

    Zeolitic imidazolate framework membranes made by ligand-induced permselectivation
    journal, September 2018

    Facile Preparation of Hydrophobic Colloidal MFI and CHA Crystals and Oriented Ultrathin Films
    journal, July 2018

    • Zhou, Ming; Hedlund, Jonas
    • Angewandte Chemie International Edition, Vol. 57, Issue 34
    • DOI: 10.1002/anie.201806502

    Melamine‐Based Microporous Organic Framework Thin Films on an Alumina Membrane for High‐Flux Organic Solvent Nanofiltration
    journal, October 2019

    • Amirilargani, Mohammad; Yokota, Giovana N.; Vermeij, Gijs H.
    • ChemSusChem, Vol. 13, Issue 1
    • DOI: 10.1002/cssc.201902341

    Formation of two-dimensional transition metal oxide nanosheets with nanoparticles as intermediates
    journal, July 2019

    In Situ Transmission Electron Microscopy Study of Nanocrystal Formation for Electrocatalysis
    journal, October 2019

    Engineered Transport in Microporous Materials and Membranes for Clean Energy Technologies
    journal, January 2018

    • Li, Changyi; Meckler, Stephen M.; Smith, Zachary P.
    • Advanced Materials, Vol. 30, Issue 8
    • DOI: 10.1002/adma.201704953

    In situ synthesis of ultrathin metal–organic framework nanosheets: a new method for 2D metal-based nanoporous carbon electrocatalysts
    journal, January 2017

    • Huang, Liang; Zhang, Xueping; Han, Yujie
    • Journal of Materials Chemistry A, Vol. 5, Issue 35
    • DOI: 10.1039/c7ta05821g

    A solution-processable and ultra-permeable conjugated microporous thermoset for selective hydrogen separation
    journal, April 2020

    Highly permeable and oriented AlPO-18 membranes prepared using directly synthesized nanosheets for CO 2 /CH 4 separation
    journal, January 2019

    • Wang, Bin; Gao, Feng; Zhang, Feng
    • Journal of Materials Chemistry A, Vol. 7, Issue 21
    • DOI: 10.1039/c9ta01233h

    Two‐Dimensional Metal–Organic Framework Nanosheets for Membrane‐Based Gas Separation
    journal, July 2017

    Morphology‐Reserved Synthesis of Discrete Nanosheets of CuO@SAPO‐34 and Pore Mouth Catalysis for One‐Pot Oxidation of Cyclohexane
    journal, February 2020

    • Guo, Xiangke; Xu, Mengxia; She, Minyi
    • Angewandte Chemie International Edition, Vol. 59, Issue 7
    • DOI: 10.1002/anie.201911749

    Uniformly Oriented Zeolite ZSM-5 Membranes with Tunable Wettability on a Porous Ceramic
    journal, August 2018

    • Fu, Donglong; Schmidt, Joel E.; Pletcher, Paul
    • Angewandte Chemie, Vol. 130, Issue 38
    • DOI: 10.1002/ange.201806361

    Uniformly Oriented Zeolite ZSM-5 Membranes with Tunable Wettability on a Porous Ceramic
    journal, August 2018

    • Fu, Donglong; Schmidt, Joel E.; Pletcher, Paul
    • Angewandte Chemie International Edition, Vol. 57, Issue 38
    • DOI: 10.1002/anie.201806361
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