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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
Grant/Contract Number:
AC05-00OR22725; NE0008298; NE 0008298
Resource Type:
Journal Article: 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. doi: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. doi:10.1002/aic.15434.
Hye Kwon, Yeon, Kiang, Christine, Benjamin, Emily, Crawford, Phillip, Nair, Sankar, and Bhave, Ramesh. 2016. "Krypton-xenon separation properties of SAPO-34 zeolite materials and membranes". United States. doi: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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  • Cited by 1
  • 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 largemore » (>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.« less
  • SAPO-34 membranes were synthesized by several routes towards N-2/CH4 separation. Membrane synthesis parameters including water content in the gel, crystallization time, support pore size, and aluminum source were investigated. High performance N-2-selective membranes were obtained on 100-nm-pore alumina tubes by using Al(i-C3H7O)(3) as aluminum source with a crystallization time of 6 h. These membranes separated N-2 from CH, with N-2 permeance as high as 500 GPU with separation selectivity of 8 at 24 degrees C. for a 50/50 N-2/CH4 mixture. Nitrogen and CH, adsorption isotherms were measured on SAPO-34 crystals. The N-2 and CH, heats of adsorption were 11 andmore » 15 kJ/mol, respectively, which lead to a preferential adsorption of CE-H-4 over N-2 in the N-2/CH4 mixture. Despite this, the SAPO-34 membranes were selective for N-2 over CH4 in the mixture because N-2 diffuses much faster than CH4 and differences in diffusivity played a more critical role than the competitive adsorption. Preliminary economic evaluation indicates that the required N-2/CH4 selectivity would be 15 in order to maintain a CH4 loss below 10%. For small nitrogen-contaminated gas wells, our current SAPO-34 membranes have potential to compete with the benchmark technology cryogenic distillation for N-2 rejection. (C) 2015 Elsevier B.V. All rights reserved,« less
  • Cited by 10