WO2014172360A2 - Système à tritium avancé pour séparation de tritium à partir de déchets radioactifs et d'eau de réacteur dans des système à eau légère - Google Patents

Système à tritium avancé pour séparation de tritium à partir de déchets radioactifs et d'eau de réacteur dans des système à eau légère Download PDF

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Publication number
WO2014172360A2
WO2014172360A2 PCT/US2014/034182 US2014034182W WO2014172360A2 WO 2014172360 A2 WO2014172360 A2 WO 2014172360A2 US 2014034182 W US2014034182 W US 2014034182W WO 2014172360 A2 WO2014172360 A2 WO 2014172360A2
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WO
WIPO (PCT)
Prior art keywords
tritium
water
gas
catalyst
exchange column
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Application number
PCT/US2014/034182
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English (en)
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WO2014172360A3 (fr
Inventor
Mark S. Denton
Walter T. Shmayda
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Kurion, Inc.
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Filing date
Publication date
Priority claimed from US13/863,206 external-priority patent/US20130336870A1/en
Application filed by Kurion, Inc. filed Critical Kurion, Inc.
Publication of WO2014172360A2 publication Critical patent/WO2014172360A2/fr
Publication of WO2014172360A3 publication Critical patent/WO2014172360A3/fr

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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D59/00—Separation of different isotopes of the same chemical element
    • B01D59/28—Separation by chemical exchange

Definitions

  • the present invention relates generally to the treatment of radioactive waste and in particular to the separation of tritium from radioactive waste materials.
  • Tritium is a radioactive isotope of hydrogen with a half-life of approximately
  • Tritium is one of several radioactive isotopes that, over time, concentrate in organic systems and enter the food chain, possibly with adverse environmental and public health effects. Tritium contamination of the groundwater in the vicinity of nuclear power stations, including PWRs, has led to public outcry and negative publicity for the nuclear power industry. This could be particularly important, for example, at the site of a nuclear incident. Clearly, it would be advantageous to have methods, systems and apparatuses for the separation and concentration of tritium from light water used in PWRs and from water and liquids isolated from radioactive waste materials.
  • the present general inventive concept in some of its several embodiments, includes systems and processes for high throughput treatment of water from reactor systems to concentrate and separate tritium from the reactor water.
  • a high throughput, low concentration system for volume reduction as opposed to a low throughput, high concentration system for tritium product generation.
  • Some embodiments of the present general inventive concept involve the reaction of tritiated hydrogen gases with water in the presence of a catalyst (often a palladium catalyst) in a catalytic exchange column, yielding a more concentrated and purified tritiated water product.
  • the present general inventive concept includes an advanced tritium system (ATS) for the separation of tritium.
  • An ATS receives water from a light water reactor or from radioactive waste treatment system. When it enters the ATS, the water contains tritium isotopes, primarily in the form of tritiated water (e.g. HTO), where at least one of the protonic hydrogen atoms of the water molecule has been replaced by a tritium atom.
  • HTO tritiated water
  • the water with tritiated water passes into an electrolyzer— generally an alkaline electrolyzer, although other electrolyzers are contemplated— where the tritiated water is broken up by electrolysis into a combination of oxygen gas ((3 ⁇ 4) and hydrogen gas comprising a number of hydrogen isotopes and isotope combinations (e.g. H 2 , HT, T 2 ).
  • the oxygen gas is diverted and discharged from the ATS, while the hydrogen gas with tritium is directed to a gas purifier, where various contaminants entrained in the gas, such as KOH or another substance from the electrolyzer, are removed from the gas.
  • the hydrogen gas passes from the gas purifier into a catalytic exchange column; in some embodiments, the hydrogen gas leaving the gas purifier first passes through a heater or a humidifier, or both, before entering the catalytic exchange column.
  • tritium is separated from protonic hydrogen.
  • Hydrogen gas including gas molecules with tritium constituents, enters the bottom of the catalytic exchange column and rises through the height of the catalytic exchange column.
  • the hydrogen gas with tritium has been heated before it enters the catalytic exchange column.
  • purified (distilled or at least deionized) water from a purified water source is fed into the top of the catalytic exchange column and allowed to trickle down.
  • the catalytic exchange column is packed with granulated palladium or a similar catalyst.
  • the hydrogen gas with tritium and the purified water react to yield tritiated water (e.g., HTO) and hydrogen gas that is substantially free of tritium isotopes (i.e., "detritiated hydrogen").
  • the detritiated hydrogen is vented from the catalytic exchange column, while the tritiated water exits the catalytic exchange column and proceeds to a holding tank. This concentrated, substantially pure hydrogen can then be used as a fuel source.
  • the tritiated water in the holding tank is fed back into the electrolyzer in order to repeat the process of electrolysis and catalytic tritium separation, thereby yielding a tritiated water product with a higher concentration of tritium. Otherwise, the tritiated water proceeds from the holding tank to storage or other disposition (e.g., waste stabilization and disposal). Passing tritiated water from a nuclear reactor, or from radioactive waste, through an ATS such as the one illustrated in Figure 3 and outlined above results in a product of concentrated tritiated water. The ATS greatly reduces or eliminates the volume of water that includes tritium. In some embodiments of the present general inventive concept, tritiated water is passed through multiple catalytic exchange columns in series.
  • a system for high throughput separation and concentration of tritium from tritiated waste water in light water nuclear reactors includes an electrolysis system to electrolyze tritiated waste water to produce oxygen gas, hydrogen gas and tritium gas, a heater to heat water vapor, a liquid phase catalytic exchange column to receive a mixture of hydrogen gas and tritium gas from said electrolysis system and heated water vapor from said heater, said liquid phase catalytic exchange column including a catalyst to retain tritium gas from said mixture as said mixture passes through said liquid phase catalytic exchange column, a deionized water source to provide deionized wash water to said liquid phase catalytic exchange column in order to remove said tritium from said catalyst, so that said deionized wash water and said tritium emerge from said liquid phase catalytic exchange column as a concentrated tritium waste product a gaseous exhaust subsystem to carry away hydrogen gas and water vapor as gaseous exhaust from said liquid phase catalytic exchange column.
  • said catalyst includes palladium.
  • said catalyst includes palladium coated with a hydrophobic material.
  • said catalyst includes palladium coated with a hydrophobic polymer.
  • said catalyst includes palladium coated with a fluoropolymer.
  • said catalyst includes palladium coated with a polytetrafluoroethylene.
  • Some embodiments further include a tritium monitor to monitor the tritium content of the gaseous exhaust within said gaseous exhaust subsystem.
  • Some embodiments further include a condenser to condense at least some of the gaseous exhaust.
  • Some embodiments further include a stabilization subsystem for treating said concentrated tritium waste product.
  • a method for high throughput separation and concentration of tritium from tritiated waste water in light water nuclear reactors includes electrolyzing tritiated water to produce hydrogen and tritium gas, combining hydrogen and tritium gas produced by electrolysis with heated water vapor to produce a mixture, passing the mixture through a liquid phase catalytic exchange column that includes a catalyst configured to retain tritium from the mixture, passing deionized wash water through said liquid phase catalytic exchange column to remove the tritium from said catalyst, collecting the tritium and the deionized wash water as a high activity tritium waste product, and expelling water vapor and hydrogen gas as effluent.
  • said catalyst includes palladium.
  • said catalyst includes palladium coated with a hydrophobic material.
  • said catalyst includes palladium coated with a hydrophobic polymer.
  • said catalyst includes palladium coated with a fluoropolymer.
  • said catalyst includes palladium coated with a polytetrafluoroethylene.
  • a method further includes monitoring the tritium content of the effluent with a tritium monitor. [0022] In some embodiments, a method further includes condensing at least some of the effluent.
  • a method further includes stabilizing the high activity tritium waste product.
  • Figure 1 is a block diagram illustrating an example of a system for processing radioactive waste materials that includes an ATS for separating tritium from liquid radioactive waste material;
  • FIG. 2 is a block diagram illustrating an example embodiment of the present general inventive concept in which an ATS is used for separating tritium from the water used to cool a nuclear reactor;
  • FIG. 3 is a block diagram illustrating an example embodiment of an ATS according to the present general inventive concept, including a catalytic exchange column;
  • FIG. 4 is a block diagram illustrating an example embodiment of the present general inventive concept in which an ATS includes an electrolysis system, a column, and a monitor to monitor the expulsion of di-tritiated hydrogen; and
  • FIG. 5 is a block diagram illustrating an example embodiment of the present general inventive including a system to recover tritium gas from concentrated tritiated water.
  • the present general inventive concept in some of its embodiments, includes processes and methods for the separation, isolation, or removal (collectively “separation") of tritium from radioactive waste.
  • the present general inventive concept in some of its several embodiments, includes systems and processes for high throughput treatment of water from reactor systems to concentrate and separate tritium from the reactor water.
  • Figure 1 illustrates an example embodiment of a larger system within which an advanced tritium system (ATS) for tritium separation is a component.
  • ATS advanced tritium system
  • radioactive waste material from a nuclear reactor 10 is conveyed 15 first to waste tanks 20, where the waste material is kept submerged in water; as a result of storing radioactive waste, the water itself comes to contain a concentration of radioactive isotopes.
  • the waste material which at this stage includes both liquid and solid wastes, is conveyed 25 from the waste tanks 20 to a liquid/solid separation system 30 where liquid wastes (including the water from the waste tanks 20) are separated from the solid wastes. From the liquid/solid separation system 30, the solid wastes proceed 32 to stabilization 34 and storage 36. It is possible that, in some instances, not all of the moisture or liquid mixed with the solid wastes will be separated from the solid wastes by the liquid/solid separation system 30, in which case the stabilization and storage of those wastes will proceed differently.
  • liquid wastes that are substantially free of solid waste material proceed 38 to a liquid processing system 40.
  • the liquid processing system 40 comprises an isotope-specific-media-based system 42 for the separation of specific isotopes and an ATS 44 for the separation or removal of tritium from the liquid wastes.
  • Separated isotopes 52 removed by isotope-specific media (ISM) from the liquid wastes are stabilized 54 and moved to storage 56 or other disposition (with the final disposition or storage conditions often dependent upon the specific isotope involved).
  • Tritium removed from the liquid wastes proceeds 64 to its own disposition 66.
  • the liquid (mostly water), now substantially free of specified radioactive isotopes and tritium, usually is recycled 70 into the reactor 10, where it is combined with other water 72 fed into the reactor 10.
  • liquid emerging from the liquid processing system 40 proceeds, not to the reactor 10 to be recycled, but to storage for low-classification waste.
  • FIG. 2 illustrates another way in which an ATS according to the present general inventive concept is used with a nuclear reactor.
  • cooling water 17 supplied to the reactor 18 emerges 19 from the reactor 18 and is passed through an ATS 84 in order to remove tritium contaminants from the water.
  • the separated tritium is diverted to disposal 86, either on-site or off-site, or made into a concentrated product.
  • FIG. 3 illustrates a tritium separation system according to an example embodiment of the present general inventive concept.
  • water enters the ATS 101 through an input 110; at this stage in the treatment of the water, the water contains tritium isotopes primarily in the form of tritiated water (e.g. HTO), where at least one of the protonic hydrogen atoms of the water molecule has been replaced by a tritium atom.
  • HTO tritiated water
  • the water with tritiated water passes into an electrolyzer 120— generally an alkaline electrolyzer, although other electrolyzers are contemplated— where the tritiated water is broken up by electrolysis into a combination of oxygen gas (0 2 ) and hydrogen gas comprising a number of hydrogen isotopes and isotope combinations (e.g. H 2 , HT, T 2 ).
  • the electrolysis of water generates heat, and therefore a cooling system 160 is connected to the electrolyzer 120 for maintaining the temperature of the electrolyzer 120 and other components of the ATS 101 within acceptable limits.
  • the oxygen gas is diverted and discharged 122 from the ATS 101, while the hydrogen gas is directed to a gas purifier 125, where various contaminants entrained in the gas, such as KOH or another substance from the electrolyzer 120, are removed from the gas.
  • the hydrogen gas passes from the gas purifier 125 into a catalytic exchange column 130; in some embodiments, the hydrogen gas leaving the gas purifier 125 first passes through a heater 140 or a humidifier 145, or both, before entering the catalytic exchange column 130.
  • tritium is separated from protonic hydrogen.
  • Hydrogen gas including gas molecules with tritium constituents (i.e., tritiated hydrogen gas), enters the bottom of the catalytic exchange column 130 and rises through the height of the catalytic exchange column 130.
  • the hydrogen gas with tritium has been heated before it enters the catalytic exchange column 130.
  • purified water— distilled or at least deionized— from a purified water source 150 is fed into the top of the catalytic exchange column 130 and allowed to trickle down; this purified water is also called “reagent water” because it reacts with the hydrogen gas with tritium.
  • the catalytic exchange column is packed with granulated palladium 135 or a similar catalyst (shown in the cutaway in the inset view in Figure 3).
  • the falling reagent water in the presence of the catalyst 135 within the catalytic exchange column 130 reacts with the retained tritium to yield tritiated water (e.g., HTO) and hydrogen gas that is substantially free of tritium isotopes (i.e., "detritiated hydrogen").
  • tritiated water e.g., HTO
  • detritiated hydrogen hydrogen gas that is substantially free of tritium isotopes
  • the tritiated water in the holding tank 136 is fed back 138 into the electrolyzer 120 in order to repeat the process of electrolysis and catalytic tritium separation, thereby yielding a tritiated water product with a higher concentration of tritium. Otherwise, the tritiated water proceeds from the holding tank 136 to storage or other disposition (e.g., stabilization and disposal).
  • Some embodiments of the present general inventive concept include using an
  • a water feed 210 delivers low activity water containing HTO (and other tritiated water compounds, like T 2 O) to an electrolysis system 220— generally an alkaline electrolyzer, although other electrolyzers are contemplated— which electrolyzes the tritiated water to produce a combination of oxygen gas (O 2 ) and hydrogen gas comprising a number of hydrogen isotopes and isotope combinations (e.g. H 2 , HT, T 2 ).
  • HTO tritiated water compounds
  • electrolysis system 220 generally an alkaline electrolyzer, although other electrolyzers are contemplated— which electrolyzes the tritiated water to produce a combination of oxygen gas (O 2 ) and hydrogen gas comprising a number of hydrogen isotopes and isotope combinations (e.g. H 2 , HT, T 2 ).
  • the oxygen gas is diverted and discharged from the ATS, while the hydrogen gas is combined with heated water vapor within a heater 225; the mixture of hydrogen gas and water vapor is then directed into the bottom of a liquid phase catalytic exchange column 230 (hereinafter "LPCE column”).
  • LPCE column liquid phase catalytic exchange column 230
  • a water source 250 delivers deionized water (or, in some embodiments, distilled water, or some other liquid) to the top of the LPCE column 230.
  • tritiated gases from the electrolysis system 220 are retained on the catalyst, while protonic hydrogen gas passes through the LPCE column 230 and is expelled as gaseous exhaust 232.
  • the deionized water trickles down the LPCE column 230 and reacts with the retained tritiated gas molecules to form HTO (and, sometimes, T 2 O).
  • HTO and, sometimes, T 2 O.
  • the newly formed tritiated water product then emerges from the bottom of the LPCE column 230 as a concentrated high activity tritium product 235.
  • the concentrated high activity tritium product 235 is passed through the electrolysis system 220 and LPCE column 230 multiple times to enhance the concentration of tritium in the concentrated high activity tritium product— i.e., to separate more protonic hydrogen from tritiated hydrogen so as to yield a higher ratio of tritium to protium in the concentrated high activity tritiated water product or waste.
  • the concentrated high activity tritium product 235 exits the system for storage, stabilization, or disposal 260.
  • the catalyst is generally a TEFLON®-coated palladium catalyst, or a catalyst that includes palladium coated with or mixed with a fluorinated polymer, or a catalyst that includes palladium coated with or mixed with a hydrophobic polymer, or a similar catalyst.
  • Other catalysts are contemplated by the present general inventive concept, and the present general inventive concept is not limited to the illustrated example
  • the protonic hydrogen gas produced by electrolysis and passed through the LPCE column 230 generally is expelled along with water vapor as gaseous exhaust 232, as shown in Figure 4.
  • a tritium monitor 275 measures the tritium content of the exhaust gas as it leaves the LPCE column 230, thus monitoring whether tritium is being retained within the LPCE column 230 by the catalyst.
  • the hydrogen gas and water vapor optionally are passed through a condenser 236 and then into a storage tank 238.
  • the hydrogen gas is used as fuel.
  • the hydrogen gas is recombined with oxygen to form water.
  • the hydrogen gas is burned.
  • FIG. 4 illustrates one example embodiment of an ATS combined with a system to recover tritium gas from concentrated tritiated water.
  • a water feed 410 delivers low activity water containing HTO (and other tritiated water compounds, like T 2 0) to a distribution pump 415 and then to an electrolysis system 420, which electrolyzes the tritiated water to produce a combination of oxygen gas ((3 ⁇ 4) and hydrogen gas comprising a number of hydrogen isotopes and isotope combinations (e.g. EL, HT, T 2 ).
  • the oxygen gas is diverted and discharged from the ATS 442, while the hydrogen gas generally is combined with heated water vapor and directed into the bottom of a LPCE column 430.
  • a water source 450 delivers deionized water (or "purge water") to the top of the LPCE column 430.
  • tritiated gases are retained on the catalyst, while protonic hydrogen gas passes through the LPCE column 430 and is expelled as gaseous exhaust 432.
  • the hydrogen gas and water vapor optionally are passed through a condenser 436 and then into a storage tank 438.
  • the purge water trickles down the LPCE column 430 and reacts with the retained tritiated gas molecules to form HTO (and, sometimes, T 2 O).
  • HTO and, sometimes, T 2 O
  • the newly formed tritiated water product then emerges from the bottom of the LPCE column 430 as a concentrated high activity tritiated water product 435.
  • the concentrated high activity tritiated water product 435 is passed through the distribution pump 415 and electrolysis system 420 to again separate the oxygen atoms from the protium and tritium atoms.
  • the electrolytically separated oxygen gas is expelled 442, and the protium and tritium are directed toward an isotope separation system 482, where protonic hydrogen gas 484 and tritium gas 486 are separated for further disposition.
  • Concentrated tritium gas has numerous applications, as will be known to those in the art.
  • systems, methods, and processes for a high throughput, low concentration processing of low activity tritiated light water include the electrolysis of at least some of the tritiated water to produce hydrogen and tritium gas.
  • the hydrogen and tritium gas produced by electrolysis are combined with heated water vapor and passed through a LPCE column, which generally includes a catalyst that includes palladium coated with a hydrophobic polymer. As the hydrogen and tritium gas, along with heated water vapor, rise through the LPCE column, the tritium is retained on the catalyst.
  • Deionized wash water passes down the column (i.e., in the opposite direction of the flow of the hydrogen gas and heated water vapor) and carries the retained tritium out of the LPCE column.
  • the tritium combined with the deionized wash water, is thereby collected as a high activity tritium waste product with substantially less volume than the original volume of low activity tritiated light water.
  • the water vapor and hydrogen gas, substantially free of tritium, are exhausted as effluent.
  • the molar gas flow rate of the hydrogen and tritium gas, along with heated water vapor, rising through the LPCE column is greater than the molar liquid flow rate of the dionized wash water travelling down through the LPCE column.
  • composition or component ratio of the mixture of hydrogen gas and water vapor is adjusted to comply with emission guidelines while still maximizing throughput.

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  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Physical Water Treatments (AREA)

Abstract

La présente invention concerne des systèmes, des procédés, et des processus pour un traitement à faible concentration et à haut débit d'eau légère tritiée à faible activité. Lesdits systèmes, procédés et processus comprennent l'électrolyse d'au moins une certaine partie de l'eau tritiée pour produire de l'hydrogène et du tritium gazeux. L'hydrogène et le tritium gazeux produits par électrolyse dans certains cas sont combinés à de la vapeur d'eau chauffée pour augmenter le débit et passent à travers une colonne d'échange catalytique en phase liquide, qui comprend généralement un catalyseur qui comprend du palladium enduit d'un polymère hydrophobe. Lorsque l'hydrogène et le tritium gazeux, conjointement avec la vapeur d'eau chauffée, s'élèvent à travers la colonne LPCE, le tritium est retenu sur le catalyseur. De l'eau de lavage déionisée passe vers le bas de la colonne (à savoir, dans la direction opposée à l'écoulement de l'hydrogène gazeux et de la vapeur d'eau chauffée) et transporte le tritium retenu hors de la colonne LPCE.
PCT/US2014/034182 2013-04-15 2014-04-15 Système à tritium avancé pour séparation de tritium à partir de déchets radioactifs et d'eau de réacteur dans des système à eau légère WO2014172360A2 (fr)

Applications Claiming Priority (2)

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US13/863,206 2013-04-15
US13/863,206 US20130336870A1 (en) 2010-04-02 2013-04-15 Advanced Tritium System for Separation of Tritium from Radioactive Wastes and Reactor Water in Light Water Systems

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WO2014172360A3 WO2014172360A3 (fr) 2015-04-30

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Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP3053638A1 (fr) * 2015-02-09 2016-08-10 Karlsruher Institut für Technologie Procédé perfectionné pour le traitement et la récupération de tritium d'eau tritiée
US9714457B2 (en) 2012-03-26 2017-07-25 Kurion, Inc. Submersible filters for use in separating radioactive isotopes from radioactive waste materials
US9981868B2 (en) 2010-04-02 2018-05-29 Kurion, Inc. Mobile processing system for hazardous and radioactive isotope removal
US10689281B2 (en) 2014-06-24 2020-06-23 Kurion, Inc. Mobile processing system for hazardous and radioactive isotope removal
CN112380703A (zh) * 2020-11-16 2021-02-19 中国科学技术大学 一种催化交换塔中氚浓度分布的计算方法
US10940437B2 (en) 2010-04-02 2021-03-09 Veolia Nuclear Solutions, Inc. Advanced tritium system and advanced permeation system for separation of tritium from radioactive wastes

Family Cites Families (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US6332914B1 (en) * 2000-02-28 2001-12-25 The United States Of America As Represented By The Department Of Energy Method and apparatus for separation of heavy and tritiated water
WO2011123851A1 (fr) * 2010-04-02 2011-10-06 Kurion, Inc. Système au tritium avancé et système de perméation avancé pour séparer le tritium de déchets radioactifs et de l'eau du réacteur
US20130336870A1 (en) * 2010-04-02 2013-12-19 Kurion, Inc. Advanced Tritium System for Separation of Tritium from Radioactive Wastes and Reactor Water in Light Water Systems

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US9981868B2 (en) 2010-04-02 2018-05-29 Kurion, Inc. Mobile processing system for hazardous and radioactive isotope removal
US10940437B2 (en) 2010-04-02 2021-03-09 Veolia Nuclear Solutions, Inc. Advanced tritium system and advanced permeation system for separation of tritium from radioactive wastes
US9714457B2 (en) 2012-03-26 2017-07-25 Kurion, Inc. Submersible filters for use in separating radioactive isotopes from radioactive waste materials
US10480045B2 (en) 2012-03-26 2019-11-19 Kurion, Inc. Selective regeneration of isotope-specific media resins in systems for separation of radioactive isotopes from liquid waste materials
US10689281B2 (en) 2014-06-24 2020-06-23 Kurion, Inc. Mobile processing system for hazardous and radioactive isotope removal
US11807549B2 (en) 2014-06-24 2023-11-07 Veolia Nuclear Solutions, Inc. Mobile processing system for hazardous and radioactive isotope removal
EP3053638A1 (fr) * 2015-02-09 2016-08-10 Karlsruher Institut für Technologie Procédé perfectionné pour le traitement et la récupération de tritium d'eau tritiée
CN112380703A (zh) * 2020-11-16 2021-02-19 中国科学技术大学 一种催化交换塔中氚浓度分布的计算方法
CN112380703B (zh) * 2020-11-16 2024-03-29 中国科学技术大学 一种催化交换塔中氚浓度分布的计算方法

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