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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]
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  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. doi:10.1021/acsami.7b18244.
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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
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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.
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@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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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acsami.7b18244
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Citation Metrics:
Cited by: 26 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
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Advanced Technology Paths to Global Climate Stability: Energy for a Greenhouse Planet
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Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes
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Kr/Xe Separation over a Chabazite Zeolite Membrane
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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
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High flux high-silica SSZ-13 membrane for CO 2 separation
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Highly Tunable Molecular Sieving and Adsorption Properties of Mixed-Linker Zeolitic Imidazolate Frameworks
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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
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Cation-exchanged SAPO-34 for adsorption-based hydrocarbon separations: predictions from dispersion-corrected DFT calculations
journal, January 2014

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

    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

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

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      Figures / Tables found in this record:

      Figure 1 (p. 11)figure
      Figure 2 (p. 12)figure
      Figure 3 (p. 14)figure
      Figure 4 (p. 15)figure
      Table 1 (p. 16)table
      Figure 5 (p. 17)figure
      Figure 6 (p. 20)figure
      Figure 7 (p. 21)figure
      Table 2 (p. 21)table
      Figure 8 (p. 23)figure
      Figure 9 (p. 24)figure
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