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Title: Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water

Abstract

Highly tritiated water (HTW) may be generated at ITER by various processes and, due to the excessive radio toxicity, the self-radiolysis and the exceedingly corrosive property of HTW, a potential hazard is associated with its storage and process. Therefore, the capture and exchange method for HTW utilizing Molecular Sieve Beds (MSB) was investigated in view of adsorption capacity, isotopic exchange performance and process parameters. For the MSB, different types of zeolite were selected. All zeolite materials were additionally coated with platinum. The following work comprised the selection of the most efficient zeolite candidate based on detailed parametric studies during the H{sub 2}/D{sub 2}O laboratory scale exchange experiments (about 25 g zeolite per bed) at the Tritium Laboratory Karlsruhe (TLK). For the zeolite, characterization analytical techniques such as Infrared Spectroscopy, Thermogravimetry and online mass spectrometry were implemented. Followed by further investigation of the selected zeolite catalyst under full technical operation, a MSB (about 22 kg zeolite) was processed with hydrogen flow rates up to 60 mol*h{sup -1} and deuterated water loads up to 1.6 kg in view of later ITER processing of arising HTW. (authors)

Authors:
; ; ; ; ;  [1]; ; ;  [2]
  1. Karlsruhe Institute of Technology, Eggenstein-Leopoldshafen (Germany)
  2. ITER Organization, Saint-Paul-lez-Durance (France)
Publication Date:
OSTI Identifier:
22429747
Resource Type:
Journal Article
Resource Relation:
Journal Name: Fusion Science and Technology; Journal Volume: 67; Journal Issue: 3; Conference: TRITIUM 2013: 10. International Conference on Tritium Science and Technology, Nice Acropolis (France), 21-25 Oct 2013; Other Information: Country of input: France; 6 refs.
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 70 PLASMA PHYSICS AND FUSION TECHNOLOGY; ABSORPTION SPECTROSCOPY; ADSORPTION; AUTORADIOLYSIS; DEUTERIUM; HEAVY WATER; HYDROGEN; INFRARED SPECTRA; ISOTOPIC EXCHANGE; ITER TOKAMAK; MASS SPECTROSCOPY; MOLECULAR SIEVES; PARAMETRIC ANALYSIS; PLATINUM; THERMAL GRAVIMETRIC ANALYSIS; TRITIUM; TRITIUM OXIDES; ZEOLITES

Citation Formats

Michling, R., Braun, A., Cristescu, I., Dittrich, H., Gramlich, N., Lohr, N., Glugla, M., Shu, W., and Willms, S.. Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water. United States: N. p., 2015. Web. doi:10.13182/FST14-T60.
Michling, R., Braun, A., Cristescu, I., Dittrich, H., Gramlich, N., Lohr, N., Glugla, M., Shu, W., & Willms, S.. Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water. United States. doi:10.13182/FST14-T60.
Michling, R., Braun, A., Cristescu, I., Dittrich, H., Gramlich, N., Lohr, N., Glugla, M., Shu, W., and Willms, S.. Sun . "Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water". United States. doi:10.13182/FST14-T60.
@article{osti_22429747,
title = {Capture and isotopic exchange method for water and hydrogen isotopes on zeolite catalysts up to technical scale for pre-study of processing highly tritiated water},
author = {Michling, R. and Braun, A. and Cristescu, I. and Dittrich, H. and Gramlich, N. and Lohr, N. and Glugla, M. and Shu, W. and Willms, S.},
abstractNote = {Highly tritiated water (HTW) may be generated at ITER by various processes and, due to the excessive radio toxicity, the self-radiolysis and the exceedingly corrosive property of HTW, a potential hazard is associated with its storage and process. Therefore, the capture and exchange method for HTW utilizing Molecular Sieve Beds (MSB) was investigated in view of adsorption capacity, isotopic exchange performance and process parameters. For the MSB, different types of zeolite were selected. All zeolite materials were additionally coated with platinum. The following work comprised the selection of the most efficient zeolite candidate based on detailed parametric studies during the H{sub 2}/D{sub 2}O laboratory scale exchange experiments (about 25 g zeolite per bed) at the Tritium Laboratory Karlsruhe (TLK). For the zeolite, characterization analytical techniques such as Infrared Spectroscopy, Thermogravimetry and online mass spectrometry were implemented. Followed by further investigation of the selected zeolite catalyst under full technical operation, a MSB (about 22 kg zeolite) was processed with hydrogen flow rates up to 60 mol*h{sup -1} and deuterated water loads up to 1.6 kg in view of later ITER processing of arising HTW. (authors)},
doi = {10.13182/FST14-T60},
journal = {Fusion Science and Technology},
number = 3,
volume = 67,
place = {United States},
year = {Sun Mar 15 00:00:00 EDT 2015},
month = {Sun Mar 15 00:00:00 EDT 2015}
}
  • Highly tritiated water (HTW) is produced in fusion machines and one of the promising technologies to process it is isotopic exchange. 3 kinds of Pt-catalyzed zeolite (13X-APG, CBV-100-CY and HiSiv-1000) were tested as candidates for isotopic exchange of highly tritiated water (HTW), and CBV-100-CY (Na-Y type with a SiO{sub 2}/Al{sub 2}O{sub 3} ratio of ∼ 5.0) shows the best performance. Small-scale tritium testing indicates that this method is efficient for reaching an exchange factor (EF) of 100. Full-scale non-tritium testing implies that an EF of 300 can be achieved in 24 hours of operation if a temperature gradient is appliedmore » along the column. For the isotopic exchange, deuterium recycled from the Isotope Separation System (deuterium with 1% T and/or 200 ppm T) should be employed, and the tritiated water regenerated from the Pt-catalyzed zeolite bed after isotopic exchange should be transferred to Water Detritiation System (WDS) for further processing.« less
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  • The behavior of hydrophobic catalyst in the isotopic exchange reactions H/D/T was analyzing by quantum chemical methods.The primary radiolytic effect was evaluated using a two-step radiolytic mechanism: a) the ionization of molecule and spatial redistribution of atoms in order to reach a minimum value of energy, characteristic to the new quantum state; b) the neutralization of molecule by capture of an electron and its rapid dissociation in free radicals. Chemical bonds suspected to break are located in the distribution region of LUMO orbital and have minimal bond energy.Evaluation of secondary effects taking place in polymeric structure in the presence ofmore » water was carried out through the study of the transition state resulted after the attack of HO. radicals formed in the radiolysis of tritiated water.« less
  • Methods of preparation of Ni, Pt, Cu, and Fe catalysts are presented. The apparatus for experiments with these catalysts is diagramed for rapid measurements in pyrex and brass and for high temperature reactions. Results are tabulated. (M.H.R.)