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Title: Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes

Abstract

Separation of the radioisotope 85Kr from 136Xe is an important target during used nuclear fuel recycling. In this paper, we report a detailed study on the Kr and Xe adsorption, diffusion, and membrane permeation properties of the silicoaluminophosphate zeolite SAPO-34. Adsorption and diffusion measurements on SAPO-34 crystals indicate their potential for use in Kr-Xe separation membranes, but also highlight competing effects of adsorption and diffusion selectivity. SAPO-34 membranes are synthesized on α$-$alumina disk and tubular substrates via steam assisted conversion seeding and hydrothermal growth, and are characterized in detail. Membrane transport measurements reveal that SAPO-34 membranes can separate Kr from Xe by molecular sieving, with Kr permeabilities around 50 Barrer and mixture selectivity of 25–30 for Kr at ambient or slight sub-ambient conditions. Finally, the membrane transport characteristics are modeled by the Maxwell-Stefan equations, whose predictions are in very good agreement with experiment and confirm the minimal competing effects of adsorption and diffusion.

Authors:
 [1];  [1];  [1];  [1];  [1];  [2]
  1. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemical & Biomolecular Engineering
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1356958
Alternate Identifier(s):
OSTI ID: 1400772
Grant/Contract Number:  
AC05-00OR22725; NE0008298
Resource Type:
Accepted Manuscript
Journal Name:
AIChE Journal
Additional Journal Information:
Journal Volume: 63; Journal Issue: 2; Journal ID: ISSN 0001-1541
Publisher:
American Institute of Chemical Engineers
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS; zeolite membranes; gas separation

Citation Formats

Hye Kwon, Yeon, Kiang, Christine, Benjamin, Emily, Crawford, Phillip, Nair, Sankar, and Bhave, Ramesh. Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes. United States: N. p., 2016. Web. https://doi.org/10.1002/aic.15434.
Hye Kwon, Yeon, Kiang, Christine, Benjamin, Emily, Crawford, Phillip, Nair, Sankar, & Bhave, Ramesh. Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes. United States. https://doi.org/10.1002/aic.15434
Hye Kwon, Yeon, Kiang, Christine, Benjamin, Emily, Crawford, Phillip, Nair, Sankar, and Bhave, Ramesh. Wed . "Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes". United States. https://doi.org/10.1002/aic.15434. https://www.osti.gov/servlets/purl/1356958.
@article{osti_1356958,
title = {Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes},
author = {Hye Kwon, Yeon and Kiang, Christine and Benjamin, Emily and Crawford, Phillip and Nair, Sankar and Bhave, Ramesh},
abstractNote = {Separation of the radioisotope 85Kr from 136Xe is an important target during used nuclear fuel recycling. In this paper, we report a detailed study on the Kr and Xe adsorption, diffusion, and membrane permeation properties of the silicoaluminophosphate zeolite SAPO-34. Adsorption and diffusion measurements on SAPO-34 crystals indicate their potential for use in Kr-Xe separation membranes, but also highlight competing effects of adsorption and diffusion selectivity. SAPO-34 membranes are synthesized on α$-$alumina disk and tubular substrates via steam assisted conversion seeding and hydrothermal growth, and are characterized in detail. Membrane transport measurements reveal that SAPO-34 membranes can separate Kr from Xe by molecular sieving, with Kr permeabilities around 50 Barrer and mixture selectivity of 25–30 for Kr at ambient or slight sub-ambient conditions. Finally, the membrane transport characteristics are modeled by the Maxwell-Stefan equations, whose predictions are in very good agreement with experiment and confirm the minimal competing effects of adsorption and diffusion.},
doi = {10.1002/aic.15434},
journal = {AIChE Journal},
number = 2,
volume = 63,
place = {United States},
year = {2016},
month = {7}
}

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Works referenced in this record:

Preparation and Gas Adsorption Characteristics of Zeolite MFI Crystals with Organic-Functionalized Interiors
journal, September 2011

  • Kassaee, Mohamad H.; Sholl, David S.; Nair, Sankar
  • The Journal of Physical Chemistry C, Vol. 115, Issue 40
  • DOI: 10.1021/jp206822b

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

Membrane purification in radioactive waste management: a short review
journal, February 2012


Diffusion in gas separation membrane materials: A comparison and analysis of experimental characterization techniques
journal, July 1998


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


Atomically Detailed Modeling of Metal Organic Frameworks for Adsorption, Diffusion, and Separation of Noble Gas Mixtures
journal, May 2012

  • Gurdal, Yeliz; Keskin, Seda
  • Industrial & Engineering Chemistry Research, Vol. 51, Issue 21
  • DOI: 10.1021/ie300766s

The first example of commensurate adsorption of atomic gas in a MOF and effective separation of xenon from other noble gases
journal, January 2014

  • Wang, Hao; Yao, Kexin; Zhang, Zhijuan
  • Chemical Science, Vol. 5, Issue 2, p. 620-624
  • DOI: 10.1039/C3SC52348A

Nuclear waste treatment by zeolites
journal, July 1984


Membrane processes in nuclear technology-application for liquid radioactive waste treatment
journal, March 2001


Adsorption equilibria of O2, Ar, Kr and Xe on activated carbon and zeolites: single component and mixture data
journal, February 2011


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


Nanoporous metal formates for krypton/xenon separation
journal, January 2013

  • Lawler, Keith V.; Hulvey, Zeric; Forster, Paul M.
  • Chemical Communications, Vol. 49, Issue 93, p. 10959-10961
  • DOI: 10.1039/c3cc44374d

Investigating the influence of diffusional coupling on mixture permeation across porous membranes
journal, March 2013


Scale-up of SAPO-34 membranes for CO2/CH4 separation
journal, April 2010


High-Pressure CO 2 /CH 4 Separation Using SAPO-34 Membranes
journal, April 2005

  • Li, Shiguang; Martinek, Janna G.; Falconer, John L.
  • Industrial & Engineering Chemistry Research, Vol. 44, Issue 9
  • DOI: 10.1021/ie0490177

Adsorption of Noble Gases on H-Mordenite
journal, November 2002

  • Ianovski, Dmitri; Munakata, Kenzo; Kanjo, Seigo
  • Journal of Nuclear Science and Technology, Vol. 39, Issue 11
  • DOI: 10.1080/18811248.2002.9715313

Permeation of single gases in thin zeolite MFI membranes
journal, June 1998


Synthesis and properties of A-type zeolite membranes by secondary growth method with vacuum seeding
journal, December 2004


Modelling issues in zeolite based separation processes
journal, November 2003


The generalized Maxwell–Stefan model for diffusion in zeolites:
journal, August 2000


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


SAPO-34 membranes for CO2/CH4 separation
journal, September 2004


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


Novel Long-Term Immobilization Method for Radioactive Iodine-129 Using a Zeolite/Apatite Composite Sintered Body
journal, June 2009

  • Watanabe, Yujiro; Ikoma, Toshiyuki; Yamada, Hirohisa
  • ACS Applied Materials & Interfaces, Vol. 1, Issue 7
  • DOI: 10.1021/am900251m

Blocking defects in SAPO-34 membranes with cyclodextrin
journal, August 2010

  • Zhang, Yanfeng; Avila, Adolfo M.; Tokay, Begum
  • Journal of Membrane Science, Vol. 358, Issue 1-2, p. 7-12
  • DOI: 10.1016/j.memsci.2010.04.006

Separation of hydrocarbon mixtures using zeolite membranes: a modelling approach combining molecular simulations with the Maxwell–Stefan theory
journal, November 2000


Effects of Molecular Siting and Adsorbent Heterogeneity on the Ideality of Adsorption Equilibria
journal, March 2004

  • Murthi, Manohar; Snurr, Randall Q.
  • Langmuir, Vol. 20, Issue 6
  • DOI: 10.1021/la035556p

Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation
journal, February 2013

  • Nugent, Patrick; Belmabkhout, Youssef; Burd, Stephen D.
  • Nature, Vol. 495, Issue 7439, p. 80-84
  • DOI: 10.1038/nature11893

Hydrogen purification using a SAPO-34 membrane
journal, January 2008


Potential of Metal–Organic Frameworks for Separation of Xenon and Krypton
journal, December 2014

  • Banerjee, Debasis; Cairns, Amy J.; Liu, Jian
  • Accounts of Chemical Research, Vol. 48, Issue 2
  • DOI: 10.1021/ar5003126

Unexpected Molecular Sieving Properties of Zeolitic Imidazolate Framework-8
journal, July 2012

  • Zhang, Chen; Lively, Ryan P.; Zhang, Ke
  • The Journal of Physical Chemistry Letters, Vol. 3, Issue 16
  • DOI: 10.1021/jz300855a

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

Improving SAPO-34 membrane synthesis
journal, October 2013


Switching Kr/Xe Selectivity with Temperature in a Metal–Organic Framework
journal, May 2012

  • Fernandez, Carlos A.; Liu, Jian; Thallapally, Praveen K.
  • Journal of the American Chemical Society, Vol. 134, Issue 22, p. 9046-9049
  • DOI: 10.1021/ja302071t

    Works referencing / citing this record:

    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

    Noble gas separation by a MOF with one-dimensional channels
    journal, January 2019


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