EP1070266B1 - Verfahren zur messung der tritium-aktivität in einem behälter für radioaktiven abfall - Google Patents

Verfahren zur messung der tritium-aktivität in einem behälter für radioaktiven abfall Download PDF

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Publication number
EP1070266B1
EP1070266B1 EP99911877A EP99911877A EP1070266B1 EP 1070266 B1 EP1070266 B1 EP 1070266B1 EP 99911877 A EP99911877 A EP 99911877A EP 99911877 A EP99911877 A EP 99911877A EP 1070266 B1 EP1070266 B1 EP 1070266B1
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EP
European Patent Office
Prior art keywords
drum
tritium
sample
partial pressure
contained
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Expired - Lifetime
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EP99911877A
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English (en)
French (fr)
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EP1070266A1 (de
Inventor
Philippe Bugeon
Bernard Bachet
Didier Devillard
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Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique CEA
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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/02—Treating gases

Definitions

  • the present invention relates to a method for measuring the tritium activity of a waste drum radioactive.
  • Tritium is a radionuclide present in radioactive waste. It is an unstable isotope of hydrogen. Its disintegration into 3 helium is accompanied by the emission of a particle ⁇ with a negative charge which corresponds to an electron. The pathways of these ⁇ particles are extremely reduced. They do not exceed 6 ⁇ m in water and 5.7 mm in air. This property excludes any possibility of detection of tritium radiation through drum walls or in solid or liquid waste.
  • Tritium is also present in organic solid waste, for example poly (ethylene / vinyl acetate) or EVA or poly (vinyl chloride) or PCV, from overboots, gloves, variable regulator, etc ...
  • organic solid waste for example poly (ethylene / vinyl acetate) or EVA or poly (vinyl chloride) or PCV.
  • EVA poly (ethylene / vinyl acetate)
  • poly (vinyl chloride) or PCV from overboots, gloves, controlgants, etc ...
  • the diversity of nature of this waste reinforces the difficulty of characterization.
  • Experience shows a strong heterogeneity of activity distribution. When all these types of products are mixed, the representativeness of a few grams of samples is very random. However, a sample burner (weighing from 0.1 to 1 g) under an oxygen stream allows to estimate the activity of some samples to levels of some Bq / g.
  • Tritiated waste with little contamination is very difficult to characterize, especially organic waste each sample is marked by a very high degree of uncertainty important as to its representativeness.
  • the problem can be solved by homogenizing waste by grinding. The lack of sensitivity of the calorimetry does not allow it to be used. Point analytical checks an important gap remains. The solution is to achieve control overall, non-destructive and without generating waste.
  • the principle adopted is to measure the amount of helium 3 resulting from the decay of tritium from a sample of the gaseous atmosphere surrounding the waste. This amount of helium formed is proportional to the tritium activity present.
  • waste with an activity of 10 9 Bq (0.027 Ci) causes in one year a release of 3 helium leading to a concentration of 0.0055 ppm of this gas in a volume of 200 liters.
  • Tritium is radioactive ⁇ - . it disintegrates by giving 3 helium, an electron and an antineutrino according to the reaction: T ⁇ 3 He + e - + ⁇
  • the subject of the invention is therefore a method for measuring the tritium activity of a radioactive waste drum containing a quantity of radioactive waste and a free volume, consisting in measuring the amount of 3 He produced by the disintegration of the tritium contained in it. in said radioactive waste for a determined period of time and to deduce therefrom the corresponding activity of the tritium contained in said radioactive waste.
  • the amount of 3 He produced can advantageously be evaluated by a leak detector.
  • the tritiated waste contained in the bags behave globally as a single source of 3 helium which discharges into the free volume of the drum.
  • the partial pressure of the gas present is a function of the 3 helium flow rate of the tritium source (thus the activity), the free volume and the tightness of the barrel (a part of the gas created is escaping from it), the confinement time.
  • the measurement can be carried out in three phases: calibration and measurement of the concentration of helium 3, measurement of the free volume in the barrel, measuring the tightness of the drum.
  • step a parasitic gases are removed from the sample taken before evaluating the amount of 3 He.
  • said evaluation may comprise the comparison of the sample taken with a gas at the same pressure and known 3 He concentration.
  • the operation b) can be carried out by injecting a known amount of 4 He into the drum, then measuring the partial pressure of 4 He in the drum, and finally by determining the free volume of said drum from the known amount of 4 He and the measurement of the partial pressure of 4 He.
  • This 4 He partial pressure measurement can be obtained by taking a sample of the gas contained in the drum and evaluating the amount of 4 He contained in this sample by a leak detector.
  • the operation c) can be carried out by injecting a known quantity of 4 He into the drum, then by measuring a first time the partial pressure of 4 He in the drum, then, after a determined duration with respect to said first time , by measuring a second time the partial pressure of 4 He in the drum, the leakage rate of the drum being calculated from these values of partial pressure of 4 He and of the determined duration between these partial pressure measurements.
  • the measurement of the said quantity of 3 He produced can simply be obtained by placing the barrel in a chamber designed to collect the 3 He fleeing the barrel and evaluating this amount of 3 He by the leak detector.
  • the attached figure shows a closed barrel 1 by a lid 6 and containing radioactive waste 2 arranged in PVC bags and leaving a free volume 3 in the drum.
  • Reference 4 designates a leak detector provided with a spectrometer of mass.
  • a test-tube 5, with a capacity of about 2 liters, allows to take a sample of gas in the free volume 3 of the barrel, through the lid 6.
  • the signal delivered by a leak detector depends, among other things, on the value of the gas flow tracer and tracer gas pressure being in upstream of this leak.
  • the 3 He concentration of the test specimens is deduced after calibration under the same conditions of specimens with a known 3 He concentration.
  • the 3 He concentration of the sample specimens is low, of the order of one part per trillion. However, after the elimination of the gases other than 3 He, 4 He and Ne of the test piece by means of an activated carbon trap, a pressure of the order of 10 millibars can be reached in the test specimen. Under these conditions, the concentration of 3 He in the test tube is multiplied by a factor of 100.
  • the sampling specimen 5 disconnected from the barrel 1 and connected to an activated carbon trap 7 soaked in liquid nitrogen. After the trap 7 has exerted its action by attracting gases other than 3 He, 4 He and Ne, the test piece 5 is connected to the leak detector via a micrometer valve 8. The sample to be tested is is then placed upstream of the calibrated leak of the detector 4.
  • the calibration is performed by replacing the sample gas by a gas at the same pressure and of known 3 He concentration.
  • a calculation program makes it possible to obtain the value of the flow rate of the source 3 He as a function of the concentration in 3 He, the free volume, the tightness of the drum and the duration of confinement of the waste.
  • the tritium activity is deduced from the value of the flow rate of the 3 He source.
  • the partial pressure of 3 He inside the drum is such that the system stabilizes.
  • the apparent leak of the barrel (the 3 He coming out of the barrel) is equal to the flow of the tritium source (the 3 He that is created). Under these conditions, sampling in the drum is no longer necessary. It is sufficient to measure the apparent leakage of the drum to know its tritium activity. This measurement can be done by placing for about 20 hours the barrel of 200 liters in a slightly larger enclosure, to limit the dead volume to about twenty liters, and measuring as previously the concentration of 3 He.
  • this method was used to measure the tritium activity of two steel containers containing a tritium source (consisting of 0.1 liter of tritiated water) and having a free volume of 12.7 liters. .
  • the activities of the sources enclosed in these containers were 0.455.10 9 Bq (12.3 mCi) for the first container and 4.55.10 9 Bq (123 mCi) for the second container.
  • the ambient gas contained in these containers was analyzed at regular time intervals in accordance with the process of the present invention.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Measurement Of Radiation (AREA)

Claims (9)

  1. Verfahren zur Messung der Tritium-Aktivität eines Behälters (1) für radioaktiven Abfall, der eine Menge an radioaktivem Abfall (2) und ein Leervolumen aufweist, das darin besteht, dass man die durch den Zerfall des in dem radioaktiven Abfall (2) enthaltenen Tritiums während einer festgelegten Zeitspanne gebildete 3He-Menge misst und daraus die entsprechende Aktivität des in dem radioaktiven Abfall (2) enthaltenen Tritiums ableitet.
  2. Verfahren nach Anspruch 1, dadurch gekennzeichnet, dass die Menge des gebildeten 3He mittels eines Leckage-Detektors (4) bestimmt wird.
  3. Verfahren nach Anspruch 2, dadurch gekennzeichnet, dass es die folgenden Arbeitsgänge umfasst:
    a) Entnahme einer Probe des in dem Behälter (1) enthaltenen Gases und Bestimmung der in der Probe enthaltenen 3He-Menge mittels des Leckage-Detektors (4),
    b) Bestimmung des Leervolumens des Behälters (1),
    c) Bestimmung der Dichtheit des Behälters (1), um daraus den Umfang der Leckage zu ermitteln,
    d) Berechnung der 3He-Durchflussmenge aus den Angaben, die bei den Arbeitsgängen (a), (b) und (c) erhalten werden,
    e) Bestimmung der Tritium-Aktivität des Behälters (1) als Funktion der in dem Arbeitsgang (d) errechneten 3He-Durchflussmenge.
  4. Verfahren nach Anspruch 3, dadurch gekennzeichnet, dass in dem Arbeitsgang (a) störende Gase aus der Probe entfernt werden, bevor die 3He-Menge bestimmt wird.
  5. Verfahren nach einem der Ansprüche 3 oder 4, dadurch gekennzeichnet, dass in dem Arbeitsgang (a) die Bestimmung umfasst den Vergleich der entnommenen Probe mit einem Gas, das unter dem gleichen Druck steht und eine bekannte 3He-Konzentration aufweist.
  6. Verfahren nach einem der Ansprüche 3 bis 5, dadurch gekennzeichnet, dass der Arbeitsgang (b) durchgeführt wird durch Injizieren einer bekannten Menge 4He in den Behälter (1), anschließendes Messen des 4He-Partialdruckes in dem Behälter (1) und schließlich Bestimmung des Leervolumens des Behälters (1) aus der bekannten 4He-Menge und der Messung des 4He-Partialdruckes.
  7. Verfahren nach Anspruch 6, dadurch gekennzeichnet, dass die Messung des 4He-Partialdruckes durchgeführt wird durch Entnahme einer Probe des in dem Behälter (1) enthaltenen Gases und Bestimmung der in dieser Probe enthaltenen 4He-Menge mit einem Leckage-Detektor (4).
  8. Verfahren nach einem der Ansprüche 3 bis 7, dadurch gekennzeichnet, dass der Arbeitsgang (3) durchgeführt wird durch Injizieren einer bekannten 4He-Menge in den Behälter (1), anschließendes erstes Messen des 4He-Partialdruckes in dem Behälter (1) und danach, nach einer festgelegten Zeitspanne nach der ersten Messung, zweites Messen des 4He-Partialdruckes in dem Behälter (1), wobei der Grad der Leckage des Behälters (1) errechnet wird aus diesen 4He-Partialdruckwerten und der festgelegten Zeitspanne zwischen diesen Partialdruck-Messungen.
  9. Verfahren nach Anspruch 2, dadurch gekennzeichnet, dass die 3He-Leckage aus dem Behälter (1) angenommen wird als gleich der 3He-Menge, die durch den Zerfall des in dem radioaktiven Abfall (2) enthaltenen Tritiums gebildet wird, wobei die Messung dieser gebildeten 3He-Menge dadurch erhalten wird, dass man den Behälter (1) in einem Behälter für die Aufnahme des aus dem Behälter (1) entweichenden 3He anordnet und diese 3He-Menge mit dem Leckage-Detektor (4) bestimmt.
EP99911877A 1998-04-07 1999-04-06 Verfahren zur messung der tritium-aktivität in einem behälter für radioaktiven abfall Expired - Lifetime EP1070266B1 (de)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
FR9804302A FR2777090B1 (fr) 1998-04-07 1998-04-07 Procede de msesure de l'activite tritium d'un fut de dechets radioactifs
FR9804302 1998-04-07
PCT/FR1999/000785 WO1999051997A1 (fr) 1998-04-07 1999-04-06 Procede de mesure de l'activite tritium d'un fut de dechets radioactifs

Publications (2)

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EP1070266A1 EP1070266A1 (de) 2001-01-24
EP1070266B1 true EP1070266B1 (de) 2003-06-25

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EP99911877A Expired - Lifetime EP1070266B1 (de) 1998-04-07 1999-04-06 Verfahren zur messung der tritium-aktivität in einem behälter für radioaktiven abfall

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US (1) US6731714B1 (de)
EP (1) EP1070266B1 (de)
JP (1) JP2002510800A (de)
CA (1) CA2324890C (de)
DE (1) DE69909074T2 (de)
FR (1) FR2777090B1 (de)
RU (1) RU2225016C2 (de)
UA (1) UA57136C2 (de)
WO (1) WO1999051997A1 (de)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US8597471B2 (en) 2010-08-19 2013-12-03 Industrial Idea Partners, Inc. Heat driven concentrator with alternate condensers
TWI460460B (zh) * 2013-03-18 2014-11-11 Inst Nuclear Energy Res Atomic Energy Council 用過核子燃料貯存桶頂部輻射偵檢裝置
RU2696811C1 (ru) * 2018-08-09 2019-08-06 Федеральное государственное бюджетное учреждение науки Институт геологии и минералогии им. В.С. Соболева Сибирского отделения Российской академии наук (Институт геологии и минералогии СО РАН, ИГМ СО РАН) Способ определения объемной активности трития в горючем природном газе или попутном нефтяном газе скважин нефтяных и газовых месторождений

Family Cites Families (15)

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DE2331209A1 (de) * 1973-06-19 1975-01-16 Kraftwerk Union Ag Einrichtung zur aktivitaetsueberwachung
US4075312A (en) * 1977-06-06 1978-02-21 The United States Of America As Represented By The United States Department Of Energy Process for recovering evolved hydrogen enriched with at least one heavy hydrogen isotope
US4196176A (en) * 1978-08-03 1980-04-01 The United States Of America As Represented By The United States Department Of Energy Method and apparatus for controlling accidental releases of tritium
DE2905094C2 (de) * 1979-02-10 1982-03-18 GNS Gesellschaft für Nuklear-Service mbH, 4300 Essen Abschirmtransport- und/oder Abschirmlagerbehälter
DE2950198A1 (de) * 1979-12-13 1981-06-19 Kraftwerk Union AG, 4330 Mülheim Einrichtung und verfahren zur lagerung von verbrauchten brennelementen
DE3025795C2 (de) * 1980-07-08 1986-08-28 GNS Gesellschaft für Nuklear-Service mbH, 4300 Essen Verfahren zur kontinuierlichen Überwachung von zwei Dichtungsbarrieren bei Abschirmtransport- und Lagerbehältern für radioaktive Substanzen
DE3214825C2 (de) * 1982-04-21 1986-09-11 Kernforschungsanlage Jülich GmbH, 5170 Jülich Verfahren zum Abtrennen von Krypton aus einem radioaktiven Abgas und Vorrichtung zur Durchführung des Verfahrens
US4808831A (en) * 1987-03-25 1989-02-28 Bioscan, Inc. Container for wet and dry radioactive samples
FR2620262B1 (fr) * 1987-09-09 1989-11-17 Commissariat Energie Atomique Procede et installation de traitement de dechets organiques solides contamines par du tritium
JPH0424583A (ja) * 1990-05-18 1992-01-28 Toshiba Corp トリチウム計測装置
US5089214A (en) * 1990-07-26 1992-02-18 Westinghouse Electric Corp. Apparatus for monitoring the pressure within a cask containing radioactive material
US5080693A (en) * 1991-03-26 1992-01-14 The United States Of America As Represented By The United States Department Of Energy Tritium monitor and collection system
JPH07151879A (ja) * 1993-12-01 1995-06-16 Toshiba Corp トリチウム燃料サイクルシステム
US5473643A (en) * 1994-08-19 1995-12-05 Westinghouse Idaho Nuclear Company Corrosion testing using isotopes
US5464988A (en) * 1994-11-23 1995-11-07 The United States Of America As Represented By The Department Of Energy Tritium waste package

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Publication number Publication date
CA2324890A1 (fr) 1999-10-14
FR2777090A1 (fr) 1999-10-08
UA57136C2 (uk) 2003-06-16
DE69909074D1 (de) 2003-07-31
CA2324890C (fr) 2006-12-05
JP2002510800A (ja) 2002-04-09
WO1999051997A1 (fr) 1999-10-14
RU2225016C2 (ru) 2004-02-27
US6731714B1 (en) 2004-05-04
EP1070266A1 (de) 2001-01-24
DE69909074T2 (de) 2004-05-06
FR2777090B1 (fr) 2000-05-05

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