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Title: Ion-Exchanged SAPO-34 membranes for Krypton-Xenon Separation: Control of Permeation Properties and Fabrication of Hollow Fiber Membranes

Abstract

Separation of radioisotope 85Kr from 136Xe is of importance in used nuclear fuel reprocessing. Membrane separation based on zeolite molecular sieves such as chabazite SAPO- 34 is an attractive alternative to energy-intensive cryogenic distillation. We report the synthesis of SAPO-34 membranes with considerably enhanced performance, via thickness reduction based upon control of a steam-assisted vapor-solid conversion technique followed by ion exchange with alkali metal cations. The reduction of membrane thickness leads to a large increase in Kr permeance from 7.5 gas permeation units (GPU) to 26.3 GPU with ideal Kr/Xe selectivities > 20 at 298 K. Cation-exchanged membranes show large (>50%) increases in selectivity at ambient or slight sub-ambient conditions. The adsorption, diffusion, and permeation characteristics of ionexchanged SAPO-34 materials and membranes are investigated in detail, with potassium exchanged SAPO-34 membranes showing particularly attractive performance. Lastly, we then demonstrate the fabrication of selective SAPO-34 membranes on α-alumina hollow fibers.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1]
  1. Georgia Inst. of Technology, Atlanta, GA (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Georgia Institute of Technology, Atlanta, GA (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1418424
Grant/Contract Number:  
NE0008298
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 10; Journal Issue: 7; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; fuel cycle; off-gas; membrane; krypton; separation; zeolite

Citation Formats

Kwon, Yeon Hye, Min, Byunghyun, Yang, Shaowei, Koh, Dong -Yeun, Bhave, Ramesh R., and Nair, Sankar. Ion-Exchanged SAPO-34 membranes for Krypton-Xenon Separation: Control of Permeation Properties and Fabrication of Hollow Fiber Membranes. United States: N. p., 2018. Web. https://doi.org/10.1021/acsami.7b18244.
Kwon, Yeon Hye, Min, Byunghyun, Yang, Shaowei, Koh, Dong -Yeun, Bhave, Ramesh R., & Nair, Sankar. Ion-Exchanged SAPO-34 membranes for Krypton-Xenon Separation: Control of Permeation Properties and Fabrication of Hollow Fiber Membranes. United States. https://doi.org/10.1021/acsami.7b18244
Kwon, Yeon Hye, Min, Byunghyun, Yang, Shaowei, Koh, Dong -Yeun, Bhave, Ramesh R., and Nair, Sankar. Mon . "Ion-Exchanged SAPO-34 membranes for Krypton-Xenon Separation: Control of Permeation Properties and Fabrication of Hollow Fiber Membranes". United States. https://doi.org/10.1021/acsami.7b18244. https://www.osti.gov/servlets/purl/1418424.
@article{osti_1418424,
title = {Ion-Exchanged SAPO-34 membranes for Krypton-Xenon Separation: Control of Permeation Properties and Fabrication of Hollow Fiber Membranes},
author = {Kwon, Yeon Hye and Min, Byunghyun and Yang, Shaowei and Koh, Dong -Yeun and Bhave, Ramesh R. and Nair, Sankar},
abstractNote = {Separation of radioisotope 85Kr from 136Xe is of importance in used nuclear fuel reprocessing. Membrane separation based on zeolite molecular sieves such as chabazite SAPO- 34 is an attractive alternative to energy-intensive cryogenic distillation. We report the synthesis of SAPO-34 membranes with considerably enhanced performance, via thickness reduction based upon control of a steam-assisted vapor-solid conversion technique followed by ion exchange with alkali metal cations. The reduction of membrane thickness leads to a large increase in Kr permeance from 7.5 gas permeation units (GPU) to 26.3 GPU with ideal Kr/Xe selectivities > 20 at 298 K. Cation-exchanged membranes show large (>50%) increases in selectivity at ambient or slight sub-ambient conditions. The adsorption, diffusion, and permeation characteristics of ionexchanged SAPO-34 materials and membranes are investigated in detail, with potassium exchanged SAPO-34 membranes showing particularly attractive performance. Lastly, we then demonstrate the fabrication of selective SAPO-34 membranes on α-alumina hollow fibers.},
doi = {10.1021/acsami.7b18244},
journal = {ACS Applied Materials and Interfaces},
number = 7,
volume = 10,
place = {United States},
year = {2018},
month = {1}
}

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Cited by: 4 works
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Figures / Tables:

Figure 1 Figure 1: Example surface and cross-sectional SEM images of M1 (a, c) and M2 (b, d) membranes, and (e,f) the corresponding cross-sectional P/Al ratio profiles of each membrane as determined by EDX analysis. The yellow lines define the thickness of the membrane.

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Works referenced in this record:

Evolution of nuclear fission reactors: Third generation and beyond
journal, September 2010


Advanced Technology Paths to Global Climate Stability: Energy for a Greenhouse Planet
journal, November 2002


Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes
journal, July 2016

  • Hye Kwon, Yeon; Kiang, Christine; Benjamin, Emily
  • AIChE Journal, Vol. 63, Issue 2
  • DOI: 10.1002/aic.15434

Separation of krypton and xenon by selective permeation
journal, November 1980


Kr/Xe Separation over a Chabazite Zeolite Membrane
journal, August 2016

  • Feng, Xuhui; Zong, Zhaowang; Elsaidi, Sameh K.
  • Journal of the American Chemical Society, Vol. 138, Issue 31
  • DOI: 10.1021/jacs.6b06515

Membrane Gas Separation: A Review/State of the Art
journal, May 2009

  • Bernardo, P.; Drioli, E.; Golemme, G.
  • Industrial & Engineering Chemistry Research, Vol. 48, Issue 10
  • DOI: 10.1021/ie8019032

Highly H 2 permeable SAPO-34 membranes by steam-assisted conversion seeding
journal, September 2014


Thin Hydrogen-Selective SAPO-34 Zeolite Membranes for Enhanced Conversion and Selectivity in Propane Dehydrogenation Membrane Reactors
journal, June 2016


Growth of High-Quality, Thickness-Reduced Zeolite Membranes towards N 2 /CH 4 Separation Using High-Aspect-Ratio Seeds
journal, August 2015

  • Huang, Yi; Wang, Lei; Song, Zhuonan
  • Angewandte Chemie International Edition, Vol. 54, Issue 37
  • DOI: 10.1002/anie.201503782

Highly permeable N2/CH4 separation SAPO-34 membranes synthesized by diluted gels and increased crystallization temperature
journal, April 2016


High flux high-silica SSZ-13 membrane for CO 2 separation
journal, January 2014

  • Kosinov, Nikolay; Auffret, Clement; Gücüyener, Canan
  • J. Mater. Chem. A, Vol. 2, Issue 32
  • DOI: 10.1039/C4TA02744B

Zeolite NaA membranes supported on alumina hollow fibers: Effect of support resistances on pervaporation performance
journal, February 2014


Ion-exchanged SAPO-34 membranes for light gas separations
journal, November 2007


Highly Tunable Molecular Sieving and Adsorption Properties of Mixed-Linker Zeolitic Imidazolate Frameworks
journal, March 2015

  • Eum, Kiwon; Jayachandrababu, Krishna C.; Rashidi, Fereshteh
  • Journal of the American Chemical Society, Vol. 137, Issue 12
  • DOI: 10.1021/jacs.5b00803

Cation Selectivity in Alkali-Exchanged Chabazite:  An ab Initio Periodic Study
journal, October 2003

  • Civalleri, B.; Ferrari, A. M.; Llunell, M.
  • Chemistry of Materials, Vol. 15, Issue 21
  • DOI: 10.1021/cm0342804

Cation-exchanged SAPO-34 for adsorption-based hydrocarbon separations: predictions from dispersion-corrected DFT calculations
journal, January 2014

  • Fischer, Michael; Bell, Robert G.
  • Phys. Chem. Chem. Phys., Vol. 16, Issue 39
  • DOI: 10.1039/C4CP01049C

Site Preferences in the Mixed Cation Zeolite, Li,Na-Chabazite:  A Combined Solid-State NMR and Neutron Diffraction Study
journal, March 2000

  • Smith, Luis J.; Eckert, Hellmut; Cheetham, Anthony K.
  • Journal of the American Chemical Society, Vol. 122, Issue 8
  • DOI: 10.1021/ja992882b

The Maxwell-Stefan description of mass transport across zeolite membranes
journal, April 1995

  • Krishna, R.; van den Broeke, L. J. P.
  • The Chemical Engineering Journal and the Biochemical Engineering Journal, Vol. 57, Issue 2
  • DOI: 10.1016/0923-0467(94)02951-2

Ba-SAPO-34 membrane synthesized from microwave heating and its performance for CO2/CH4 gas separation
journal, July 2011

  • Chew, Thiam Leng; Ahmad, Abdul Latif; Bhatia, Subhash
  • Chemical Engineering Journal, Vol. 171, Issue 3
  • DOI: 10.1016/j.cej.2011.05.001

    Works referencing / citing this record:

    Adsorption of Chelerythrine from Toddalia asiatica (L.) Lam. by ZSM-5
    journal, January 2020

    • Liu, Yunlong; Guo, Jie; Xiao, Zhuobing
    • Advances in Polymer Technology, Vol. 2020
    • DOI: 10.1155/2020/9408921

    Highly Selective SSZ-13 Zeolite Hollow Fiber Membranes by Ultraviolet Activation at Near-Ambient Temperature
    journal, August 2018


    Scalable One‐Step Gel Conversion Route to High‐Performance CHA Zeolite Hollow Fiber Membranes and Modules for CO 2 Separation
    journal, June 2019


    Xenon Recovery by DD3R Zeolite Membranes: Application in Anaesthetics
    journal, October 2019

    • Wang, Xuerui; Zhang, Yuting; Wang, Xiaoyu
    • Angewandte Chemie International Edition, Vol. 58, Issue 43
    • DOI: 10.1002/anie.201909544

    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