DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface

Abstract

The control of membrane morphology and microstructure is crucial to improve the separation performance of molecular-sieve membranes. This can be enabled by making thin, dense, and uniform seed-crystal coatings, which are then intergrown into continuous membranes. Herein, we show a novel and simple floating particle coating method can give closely packed monolayers of zeolite nanosheets on nonporous or porous supports. The zeolite nanosheet monolayer is formed at the air–water interface in a conical Teflon trough. As the water in the trough is drained, the monolayer is deposited on a support placed below. Membranes prepared by gel-free secondary growth of the nanosheets deposited by this method show unprecedented ultra-selective performance for separation of para- from ortho-xylene (separation factor >10,000).

Authors:
ORCiD logo [1];  [1];  [2]; ORCiD logo [1]
  1. Univ. of Minnesota, Minneapolis, MN (United States). Dept. of Chemical Engineering and Materials Science
  2. Augsburg Univ., Minneapolis, MN (United States). Dept. of Physics
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1470070
Alternate Identifier(s):
OSTI ID: 1412943
Grant/Contract Number:  
SC0001015
Resource Type:
Accepted Manuscript
Journal Name:
Angewandte Chemie (International Edition)
Additional Journal Information:
Journal Name: Angewandte Chemie (International Edition); Journal Volume: 57; Journal Issue: 2; Related Information: CGS partners with University of California, Berkeley; University of California, Davis; Lawrence Berkeley National Laboratory; University of Minnesota; National Energy Technology Laboratory; Texas A&M University; Journal ID: ISSN 1433-7851
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 77 NANOSCIENCE AND NANOTECHNOLOGY; membrane; carbon capture; materials and chemistry by design; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)

Citation Formats

Kim, Donghun, Jeon, Mi Young, Stottrup, Benjamin L., and Tsapatsis, Michael. para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface. United States: N. p., 2017. Web. doi:10.1002/anie.201708835.
Kim, Donghun, Jeon, Mi Young, Stottrup, Benjamin L., & Tsapatsis, Michael. para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface. United States. https://doi.org/10.1002/anie.201708835
Kim, Donghun, Jeon, Mi Young, Stottrup, Benjamin L., and Tsapatsis, Michael. Thu . "para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface". United States. https://doi.org/10.1002/anie.201708835. https://www.osti.gov/servlets/purl/1470070.
@article{osti_1470070,
title = {para -Xylene Ultra-selective Zeolite MFI Membranes Fabricated from Nanosheet Monolayers at the Air-Water Interface},
author = {Kim, Donghun and Jeon, Mi Young and Stottrup, Benjamin L. and Tsapatsis, Michael},
abstractNote = {The control of membrane morphology and microstructure is crucial to improve the separation performance of molecular-sieve membranes. This can be enabled by making thin, dense, and uniform seed-crystal coatings, which are then intergrown into continuous membranes. Herein, we show a novel and simple floating particle coating method can give closely packed monolayers of zeolite nanosheets on nonporous or porous supports. The zeolite nanosheet monolayer is formed at the air–water interface in a conical Teflon trough. As the water in the trough is drained, the monolayer is deposited on a support placed below. Membranes prepared by gel-free secondary growth of the nanosheets deposited by this method show unprecedented ultra-selective performance for separation of para- from ortho-xylene (separation factor >10,000).},
doi = {10.1002/anie.201708835},
journal = {Angewandte Chemie (International Edition)},
number = 2,
volume = 57,
place = {United States},
year = {2017},
month = {11}
}

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

Citation Metrics:
Cited by: 17 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Oriented MFI Membranes by Gel-Less Secondary Growth of Sub-100 nm MFI-Nanosheet Seed Layers
journal, April 2015

  • Agrawal, Kumar Varoon; Topuz, Berna; Pham, Tung Cao Thanh
  • Advanced Materials, Vol. 27, Issue 21, p. 3243-3249
  • DOI: 10.1002/adma.201405893

2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets
journal, April 2015

  • Rangnekar, Neel; Shete, Meera; Agrawal, Kumar Varoon
  • Angewandte Chemie, Vol. 127, Issue 22
  • DOI: 10.1002/ange.201411791

Metal-organic framework nanosheets as building blocks for molecular sieving membranes
journal, December 2014


Open-Pore Two-Dimensional MFI Zeolite Nanosheets for the Fabrication of Hydrocarbon-Isomer-Selective Membranes on Porous Polymer Supports
journal, April 2016

  • Zhang, Han; Xiao, Qiang; Guo, Xianghai
  • Angewandte Chemie International Edition, Vol. 55, Issue 25
  • DOI: 10.1002/anie.201601135

Zeolite membranes – Recent developments and progress
journal, November 2008


Surface nano-architecture of a metal–organic framework
journal, May 2010

  • Makiura, Rie; Motoyama, Soichiro; Umemura, Yasushi
  • Nature Materials, Vol. 9, Issue 7
  • DOI: 10.1038/nmat2769

Seven chemical separations to change the world
journal, April 2016

  • Sholl, David S.; Lively, Ryan P.
  • Nature, Vol. 532, Issue 7600
  • DOI: 10.1038/532435a

Hierarchical Nanomanufacturing: From Shaped Zeolite Nanoparticles to High-Performance Separation Membranes
journal, October 2007

  • Snyder, Mark A.; Tsapatsis, Michael
  • Angewandte Chemie International Edition, Vol. 46, Issue 40, p. 7560-7573
  • DOI: 10.1002/anie.200604910

Ultrathin, Molecular-Sieving Graphene Oxide Membranes for Selective Hydrogen Separation
journal, October 2013


Growth of Uniformly Oriented Silica MFI and BEA Zeolite Films on Substrates
journal, December 2011


Solution-processable exfoliated zeolite nanosheets purified by density gradient centrifugation
journal, May 2013

  • Agrawal, Kumar Varoon; Topuz, Berna; Jiang, Zheyu
  • AIChE Journal, Vol. 59, Issue 9, p. 3458-3467
  • DOI: 10.1002/aic.14099

Advances in nanosized zeolites
journal, January 2013

  • Mintova, Svetlana; Gilson, Jean-Pierre; Valtchev, Valentin
  • Nanoscale, Vol. 5, Issue 15
  • DOI: 10.1039/c3nr01629c

A highly crystalline layered silicate with three-dimensionally microporous layers
journal, December 2002

  • Jeong, Hae-Kwon; Nair, Sankar; Vogt, Thomas
  • Nature Materials, Vol. 2, Issue 1, p. 53-58
  • DOI: 10.1038/nmat795

Layer Structure Preservation during Swelling, Pillaring, and Exfoliation of a Zeolite Precursor
journal, January 2008

  • Maheshwari, Sudeep; Jordan, Edgar; Kumar, Sandeep
  • Journal of the American Chemical Society, Vol. 130, Issue 4, p. 1507-1516
  • DOI: 10.1021/ja077711i

Membranes containing selective flakes
journal, September 1990


Fabrication of Polymer/Selective-Flake Nanocomposite Membranes and Their Use in Gas Separation
journal, October 2004

  • Jeong, Hae-Kwon; Krych, Wojtek; Ramanan, Harikrishnan
  • Chemistry of Materials, Vol. 16, Issue 20
  • DOI: 10.1021/cm049154u

Stable single-unit-cell nanosheets of zeolite MFI as active and long-lived catalysts
journal, September 2009

  • Choi, Minkee; Na, Kyungsu; Kim, Jeongnam
  • Nature, Vol. 461, Issue 7261, p. 246-249
  • DOI: 10.1038/nature08288

Ultra-selective high-flux membranes from directly synthesized zeolite nanosheets
journal, March 2017

  • Jeon, Mi Young; Kim, Donghun; Kumar, Prashant
  • Nature, Vol. 543, Issue 7647
  • DOI: 10.1038/nature21421

Gel-Free Secondary Growth of Uniformly Oriented Silica MFI Zeolite Films and Application for Xylene Separation
journal, July 2013

  • Pham, Tung Cao Thanh; Nguyen, Thanh Huu; Yoon, Kyung Byung
  • Angewandte Chemie International Edition, Vol. 52, Issue 33, p. 8693-8698
  • DOI: 10.1002/anie.201301766

Ordered porous materials for emerging applications
journal, June 2002


Dispersible Exfoliated Zeolite Nanosheets and Their Application as a Selective Membrane
journal, October 2011


Layered zeolitic materials: an approach to designing versatile functional solids
journal, January 2014

  • Díaz, Urbano; Corma, Avelino
  • Dalton Transactions, Vol. 43, Issue 27
  • DOI: 10.1039/c3dt53181c

Recent progress in polycrystalline zeolite membrane research
journal, May 2013


Zeolite Thin Films: From Computer Chips to Space Stations
journal, February 2010

  • Lew, Christopher M.; Cai, Rui; Yan, Yushan
  • Accounts of Chemical Research, Vol. 43, Issue 2, p. 210-219
  • DOI: 10.1021/ar900146w

Metal–organic framework nanosheets in polymer composite materials for gas separation
journal, November 2014

  • Rodenas, Tania; Luz, Ignacio; Prieto, Gonzalo
  • Nature Materials, Vol. 14, Issue 1
  • DOI: 10.1038/nmat4113

2D Zeolite Coatings: Langmuir-Schaefer Deposition of 3 nm Thick MFI Zeolite Nanosheets
journal, April 2015

  • Rangnekar, Neel; Shete, Meera; Agrawal, Kumar Varoon
  • Angewandte Chemie International Edition, Vol. 54, Issue 22
  • DOI: 10.1002/anie.201411791

Highly conducting graphene sheets and Langmuir–Blodgett films
journal, August 2008

  • Li, Xiaolin; Zhang, Guangyu; Bai, Xuedong
  • Nature Nanotechnology, Vol. 3, Issue 9, p. 538-542
  • DOI: 10.1038/nnano.2008.210

Langmuir−Blodgett Assembly of Graphite Oxide Single Layers
journal, January 2009

  • Cote, Laura J.; Kim, Franklin; Huang, Jiaxing
  • Journal of the American Chemical Society, Vol. 131, Issue 3
  • DOI: 10.1021/ja806262m

Open-Pore Two-Dimensional MFI Zeolite Nanosheets for the Fabrication of Hydrocarbon-Isomer-Selective Membranes on Porous Polymer Supports
journal, April 2016


Reverse osmosis molecular differentiation of organic liquids using carbon molecular sieve membranes
journal, August 2016


High-flux MFI membranes
journal, May 2002


Membranes from nanoporous 1D and 2D materials: A review of opportunities, developments, and challenges
journal, December 2013


Diffusion of Aromatics in Silicalite-1: Experimental and Theoretical Evidence of Entropic Barriers
journal, September 2016

  • Kolokathis, Panagiotis D.; Káli, György; Jobic, Hervé
  • The Journal of Physical Chemistry C, Vol. 120, Issue 38
  • DOI: 10.1021/acs.jpcc.6b05462

Two-Dimensional Zeolites: Current Status and Perspectives
journal, February 2014

  • Roth, Wieslaw J.; Nachtigall, Petr; Morris, Russell E.
  • Chemical Reviews, Vol. 114, Issue 9
  • DOI: 10.1021/cr400600f

Molecular Sieving MFI-Type Zeolite Membranes for Pervaporation Separation of Xylene Isomers
journal, April 2004

  • Yuan, Wenhui; Lin, Y. S.; Yang, Weishen
  • Journal of the American Chemical Society, Vol. 126, Issue 15
  • DOI: 10.1021/ja031653t

Hierarchische Nanofertigung: von geformten Zeolithnanopartikeln zu hochleistungsfähigen Trennmembranen
journal, October 2007


2-dimensional zeolites
journal, May 2014


Gel-Free Secondary Growth of Uniformly Oriented Silica MFI Zeolite Films and Application for Xylene Separation
journal, July 2013

  • Pham, Tung Cao Thanh; Nguyen, Thanh Huu; Yoon, Kyung Byung
  • Angewandte Chemie, Vol. 125, Issue 33
  • DOI: 10.1002/ange.201301766

Progress in manipulating zeolite morphology and related applications
journal, December 2005

  • Drews, Timothy O.; Tsapatsis, Michael
  • Current Opinion in Colloid & Interface Science, Vol. 10, Issue 5-6
  • DOI: 10.1016/j.cocis.2005.09.013

Zeolite films and membranes. Emerging applications
journal, October 2011


Zeolite films prepared via the Langmuir–Blodgett technique
journal, February 2002

  • Morawetz, K.; Reiche, J.; Kamusewitz, H.
  • Colloids and Surfaces A: Physicochemical and Engineering Aspects, Vol. 198-200
  • DOI: 10.1016/S0927-7757(01)00987-6

Zeolite Membranes: Microstructure Characterization and Permeation Mechanisms
journal, November 2011

  • Yu, Miao; Noble, Richard D.; Falconer, John L.
  • Accounts of Chemical Research, Vol. 44, Issue 11
  • DOI: 10.1021/ar200083e

Organization of Zeolite Microcrystals for Production of Functional Materials
journal, January 2007

  • Yoon, Kyung Byung
  • Accounts of Chemical Research, Vol. 40, Issue 1
  • DOI: 10.1021/ar000119c

Organization of Zeolite Microcrystals for Production of Functional Materials
journal, May 2007


Hierarchical Nanomanufacturing: From Shaped Zeolite Nanoparticles to High-Performance Separation Membranes
journal, December 2007


Highly Conducting Graphene Sheets and Langmuir-Blodgett Films
text, January 2008


Works referencing / citing this record:

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


Hochfluss‐Hochselektivitäts‐MOF‐Membran: Geträgerte MIL‐160‐Schicht für die Trennung der Xylolisomere durch Pervaporation
journal, November 2018


Separation of Aromatics/Cyclic Aliphatics by Nonporous Adaptive Pillararene Crystals
journal, August 2018


Template-Free Synthesis of Highly b-Oriented MFI-Type Zeolite Thin Films by Seeded Secondary Growth
journal, January 2019

  • Banihashemi, Fateme; Ibrahim, Amr F. M.; Babaluo, Ali Akbar
  • Angewandte Chemie, Vol. 131, Issue 8
  • DOI: 10.1002/ange.201814248

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


Efficient Separation of cis ‐ and trans ‐1,2‐Dichloroethene Isomers by Adaptive Biphen[3]arene Crystals
journal, June 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

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

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

High‐Flux High‐Selectivity Metal–Organic Framework MIL‐160 Membrane for Xylene Isomer Separation by Pervaporation
journal, November 2018

  • Wu, Xiaocao; Wei, Wan; Jiang, Jianwen
  • Angewandte Chemie International Edition, Vol. 57, Issue 47
  • DOI: 10.1002/anie.201807935

Template‐Free Synthesis of Highly b‐Oriented MFI‐Type Zeolite Thin Films by Seeded Secondary Growth
journal, February 2019

  • Banihashemi, Fateme; Ibrahim, Amr F. M.; Babaluo, Ali Akbar
  • Angewandte Chemie International Edition, Vol. 58, Issue 8
  • DOI: 10.1002/anie.201814248

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

  • Ma, Yao; Jue, Melinda L.; Zhang, Fengyi
  • Angewandte Chemie International Edition, Vol. 58, Issue 38
  • DOI: 10.1002/anie.201903105

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

Efficient Separation of cis - and trans -1,2-Dichloroethene Isomers by Adaptive Biphen[3]arene Crystals
journal, June 2019

  • Wang, Yiliang; Xu, Kaidi; Li, Bin
  • Angewandte Chemie International Edition, Vol. 58, Issue 30
  • DOI: 10.1002/anie.201905563

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

The rapid emergence of two-dimensional nanomaterials for high-performance separation membranes
journal, January 2018

  • Zhu, Junyong; Hou, Jingwei; Uliana, Adam
  • Journal of Materials Chemistry A, Vol. 6, Issue 9
  • DOI: 10.1039/c7ta10814a

Strategies to control zeolite particle morphology
journal, January 2019

  • Li, Shiying; Li, Junfen; Dong, Mei
  • Chemical Society Reviews, Vol. 48, Issue 3
  • DOI: 10.1039/c8cs00774h

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

Self-crystallization of uniformly oriented zeolitic imidazolate framework films at air–water interfaces
journal, January 2019

  • Su, Jingyi; Wu, Wufeng; Li, Zhanjun
  • Dalton Transactions, Vol. 48, Issue 30
  • DOI: 10.1039/c9dt02359c

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

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


2D-enabled membranes: materials and beyond
journal, May 2019


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

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

Separation of Aromatics/Cyclic Aliphatics by Nonporous Adaptive Pillararene Crystals
journal, August 2018

  • Jie, Kecheng; Zhou, Yujuan; Li, Errui
  • Angewandte Chemie International Edition, Vol. 57, Issue 39
  • DOI: 10.1002/anie.201808998