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Title: Final Project Report (Oct 2014-Dec 2017): Zeolite Membranes for Krypton/Xenon Separation from Spent Nuclear Fuel Reprocessing Off-Gas

Abstract

The overall focus of this project is to develop and understand SAPO-34 zeolitic membranes that can separate mixtures of radioisotope krypton-85 and xenon released as off-gases during used nuclear fuel recycling. The primary advantage of separating 85Kr from Xe is to reduce the volume of radioactive waste for storage. The second advantage is the revenue generated from the sale of high-purity Xe. Zeolite membranes are attractive because of their much lower energy requirements relative to cryogenic distillation, and their high resistance to radiation degradation. We report the detailed study of silicoaluminophosphate zeolite SAPO-34 materials and membranes for this application, due to hypothesized favorable molecular sieving properties. In the 3-year Mission Support project, we developed a novel, high-performance, low-energy intensity, lower-cost zeolite membrane process for Kr/Xe separation during SNF processing; and investigated the underlying molecular adsorption and transport processes in both ‘idealized’ and ‘realistic’ operating conditions to develop reliable synthesis-structure-property relationships for such membranes. 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 synthesized on α-alumina substrates via steam-assisted conversion seeding and hydrothermal growth are characterized in detail, with Kr permeances 26more » GPU and ideal Kr/Xe selectivities >20 at 298 K after thickness reduction. Post-synthesis cation exchange shows large (>50%) increases in selectivity at ambient or slight sub-ambient conditions. In addition, we confirm that SAPO-34 membrane is stable under radiation exposure and the impact of radiation exposure on membrane performance would not be substantial. We also successfully synthesized hollow-fiber SAPO-34 membranes with the same performance levels as the disk-type and tubular membranes. This important development will allow a very compact and low-cost Kr/Xe separation system. Finally, a detailed process calculation for techno-economic analysis was performed by integrating Maxwell-Stefan model into cross-flow membrane system, in order to estimate the required number of membrane stages and the total cost.« less

Authors:
 [1];  [1];  [2];  [2]
  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:
1433074
Report Number(s):
14-6309
14-6309
DOE Contract Number:  
NE0008298
Resource Type:
Technical Report
Country of Publication:
United States
Language:
English
Subject:
11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS

Citation Formats

Kwon, Yeon Hye, Nair, Sankar, Bhave, Ramesh, and Spencer, Barry. Final Project Report (Oct 2014-Dec 2017): Zeolite Membranes for Krypton/Xenon Separation from Spent Nuclear Fuel Reprocessing Off-Gas. United States: N. p., 2018. Web.
Kwon, Yeon Hye, Nair, Sankar, Bhave, Ramesh, & Spencer, Barry. Final Project Report (Oct 2014-Dec 2017): Zeolite Membranes for Krypton/Xenon Separation from Spent Nuclear Fuel Reprocessing Off-Gas. United States.
Kwon, Yeon Hye, Nair, Sankar, Bhave, Ramesh, and Spencer, Barry. Sun . "Final Project Report (Oct 2014-Dec 2017): Zeolite Membranes for Krypton/Xenon Separation from Spent Nuclear Fuel Reprocessing Off-Gas". United States.
@article{osti_1433074,
title = {Final Project Report (Oct 2014-Dec 2017): Zeolite Membranes for Krypton/Xenon Separation from Spent Nuclear Fuel Reprocessing Off-Gas},
author = {Kwon, Yeon Hye and Nair, Sankar and Bhave, Ramesh and Spencer, Barry},
abstractNote = {The overall focus of this project is to develop and understand SAPO-34 zeolitic membranes that can separate mixtures of radioisotope krypton-85 and xenon released as off-gases during used nuclear fuel recycling. The primary advantage of separating 85Kr from Xe is to reduce the volume of radioactive waste for storage. The second advantage is the revenue generated from the sale of high-purity Xe. Zeolite membranes are attractive because of their much lower energy requirements relative to cryogenic distillation, and their high resistance to radiation degradation. We report the detailed study of silicoaluminophosphate zeolite SAPO-34 materials and membranes for this application, due to hypothesized favorable molecular sieving properties. In the 3-year Mission Support project, we developed a novel, high-performance, low-energy intensity, lower-cost zeolite membrane process for Kr/Xe separation during SNF processing; and investigated the underlying molecular adsorption and transport processes in both ‘idealized’ and ‘realistic’ operating conditions to develop reliable synthesis-structure-property relationships for such membranes. 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 synthesized on α-alumina substrates via steam-assisted conversion seeding and hydrothermal growth are characterized in detail, with Kr permeances 26 GPU and ideal Kr/Xe selectivities >20 at 298 K after thickness reduction. Post-synthesis cation exchange shows large (>50%) increases in selectivity at ambient or slight sub-ambient conditions. In addition, we confirm that SAPO-34 membrane is stable under radiation exposure and the impact of radiation exposure on membrane performance would not be substantial. We also successfully synthesized hollow-fiber SAPO-34 membranes with the same performance levels as the disk-type and tubular membranes. This important development will allow a very compact and low-cost Kr/Xe separation system. Finally, a detailed process calculation for techno-economic analysis was performed by integrating Maxwell-Stefan model into cross-flow membrane system, in order to estimate the required number of membrane stages and the total cost.},
doi = {},
url = {https://www.osti.gov/biblio/1433074}, journal = {},
number = ,
volume = ,
place = {United States},
year = {2018},
month = {4}
}

Technical Report:
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