skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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
  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 Lab. (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) (SC-22). 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:
Journal Article: 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.
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. doi:10.1038/nature21421.
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. doi:10.1038/nature21421. https://www.osti.gov/servlets/purl/1373573.
@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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 16works
Citation information provided by
Web of Science

Save / Share: