EP2056302B1 - Dekontaminierungsverfahren für eine durch radioaktive Elemente kontaminierte Metalloberfläche - Google Patents

Dekontaminierungsverfahren für eine durch radioaktive Elemente kontaminierte Metalloberfläche Download PDF

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Publication number
EP2056302B1
EP2056302B1 EP07119543A EP07119543A EP2056302B1 EP 2056302 B1 EP2056302 B1 EP 2056302B1 EP 07119543 A EP07119543 A EP 07119543A EP 07119543 A EP07119543 A EP 07119543A EP 2056302 B1 EP2056302 B1 EP 2056302B1
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EP
European Patent Office
Prior art keywords
decontamination
gel
group
film
acid
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Not-in-force
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EP07119543A
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English (en)
French (fr)
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EP2056302A1 (de
Inventor
Jen-Chieh Chung
Che-Nan Chen
Kou-Min Lin
Tsong-Yang Wei
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Institute of Nuclear Energy Research
Atomic Energy Council
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Institute of Nuclear Energy Research
Atomic Energy Council
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Priority to EP07119543A priority Critical patent/EP2056302B1/de
Priority to AT07119543T priority patent/ATE538478T1/de
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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
    • G21F9/001—Decontamination of contaminated objects, apparatus, clothes, food; Preventing contamination thereof
    • G21F9/002—Decontamination of the surface of objects with chemical or electrochemical processes
    • G21F9/004—Decontamination of the surface of objects with chemical or electrochemical processes of metallic surfaces
    • 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
    • G21F9/28—Treating solids

Definitions

  • the present invention relates to a decontamination method of a metal surface contaminated by radioactive element; more particularly, relates to mixing a blend of polymers, characteristic additives and a decontamination reagent to obtain a decontamination gel for indicating contaminations of Co, Cs and Sr and to obtain good decontamination effect by cleaning the contaminations by removing a film of the decontamination gel dried-up
  • Different decontamination reagents are used for cleansing.
  • distilled products from petroleum are used to clean contaminations on surfaces of tire, break, etc.
  • These reagents usually contain hydrocarbon solvents like methylbenzene and xylene.
  • environmental-friendly products are developed and widely used in the modern time.
  • D-limonene is used to cleanse oil and earth on mechanical facilities.
  • 2 to 8 weight percents (wt%) of terpene, or 5 to 25 wt% of anionic or nonionic surfactant is used to effectively remove grease or tar on a surface.
  • a surface having a pollution of radionuclides is not effectively cleansed.
  • a solution obtained after cleansing the surface may need further treatment.
  • the chemical decontamination technologies use chemical reagents, such as organic acids having reduction property, chelating agents, oxidants, reductive agent, etc. These chemical reagents are soft and are used for precision machines such as reactor coolant pump (RCP). But its decontamination factor is usually small.
  • RCP reactor coolant pump
  • the later non-chemical technologies are more widely used, such as electrochemical decontamination, abrading decontamination, high pressure water-jet decontamination, mechanical decontamination, etc. These methods are usually severe and may even ruin machine; though the decontamination factors may reach 103 to 104.
  • Traditional decontamination reagent for radioactive waste usually contains strong acid or alkali to improve decontamination effect, like phosphoric acid, sulfuric acid, nitric acid, fluorboric acid, potassium permanganate or sodium hydroxide. And the operation is usually processed under a high temperature.
  • contaminations are gradually accumulated in the decontamination reagent, its decontamination effect decreases while radioactive activity of the accumulated contaminations increases.
  • the decontamination reagent needs further treatment or becomes a waste. But, the treatment may not be easy owing to the complex components contained in the used decontamination reagent. And, the waste may be a great amount. All these may greatly heighten the cost.
  • surface protective films are developed. They are usually used as protective layers on industrial objects to prevent from contamination and collision, and thus are soft.
  • US 5,891,261 discloses (meth)acrylic acid ester combined with other polymer monomers, like less than 5%wt of carbonyl group, to form a gel. And the gel is pasted on a surface to be dried for obtaining a film. Then cold or hot water (even vapor) are spayed on the dried film to remove it.
  • US 2003/172959 A1 discloses a method for removing a wide variety of radioactive contaminats from a contaminated surface.
  • US 5,763,734 discloses another method of deconatminating devices in nuclear power plants.
  • US 6,689,226 B1 discloses a decontamination gel including a decontamination agent, two organic polymers and water.
  • US 6,203,624 B1 discloses a decontamination gel that can be used to decontaminate metal surfaces, while decontamination is understood to be related to the removal of radioactive elements.
  • Conventional decontaminations gels comprise a viscosing agent that is generally mineral and a decontamination agent choosen in relation to the type of the surface. Because of the viscosing agent spraying of the gel is difficult.
  • US 6,203,624 B1 therefore suggests combining a mineral viscosing agent and an organic viscosing agent choosen from hydosoluble organic polymenrs and surfactants.
  • the present invention provides a decontamination method comprising the steps of claim 1.
  • Advantageous embodiments of the claimed method are laid down in further claims.
  • the present invention provides a decontamination gel according to claim 15.
  • the decontamination reagent contains at least one polymer to be sprayed on a contaminated material for forming a film for cleaning contamination.
  • Evaporable organic solvent is added to increase fluidity of gel and to control time for obtaining the film.
  • a colorimetric indicator is added in the decontamination gel to be sprayed on the contaminated material to show places of contaminations.
  • the decontamination reagent has abilities of physical absorbing or chemical chelating to Co, Cs and Sr.
  • FIG.1 is a flow view showing a preferred embodiment according to the present invention.
  • the present invention is a decontamination method of a metal surface contaminated by radioactive element, comprising the following steps:
  • FIG.2 is a flow view showing fabricating a gel fluid.
  • a mixed solution with a physical ratio of water to an evaporable organic solution [21] between 1 and 5 is obtained in a reactor.
  • a first polymer [22] such as methylcellulose
  • the methylcellulose is blended to be fully solved with temperature heated up.
  • a condenser is then further used to prevent an evaporation of the organic solution and water.
  • a second polymer [23] such as PVA, is gradually added with blending under 85°C during 4 to 5hrs to be fully solved into water for obtaining a proper weight ratio of the first polymer to the second polymer.
  • a plasticizer [24] such as glycerin
  • glycerin a plasticizer added at a temperature between 80°C and 95°C to obtain a proper volume ratio of glycerin to water.
  • a gel fluid [26] is obtained after a continuous blending [25].
  • FIG.3 is a flow view showing a decontamination gel.
  • a decontamination reagent [27] such as DTPA
  • DTPA a decontamination reagent
  • a solution of phosphoric acid and water [28] is solved into a solution of phosphoric acid and water [28] to be fully blended for obtaining a molar ratio of 1:8:175 for DTPA to phosphoric acid to water in the decontamination reagent solution [29].
  • 6500 volumes of gel fluid [26] is added with 200 volumes of the decontamination reagent solution [29] to obtain a ratio of 33 to 1.
  • the solution is blended [31] under 85°C [30] in the reactor.
  • the decontamination reagent solution [34] is obtained after being placed still [32] for 1hr to be cooled down [33] to room temperature.
  • FIG.4 is a flow view showing a colorimetric decontamination gel.
  • a colorimetric indicator [35] such as alizarin
  • ethanol solution [36] is added into an ethanol solution [36] to obtain a colorimetric indicator solution [37] with a ratio of alizarin to the ethanol solution between 0.01 and 0.03.
  • 50 volumes of the colorimetric indicator solution [37] are mixed with 4800 volumes of a decontamination reagent [34] to obtain a proper ratio.
  • the solution is blended [38] and then is placed still [39] to obtain a colorimetric decontamination gel [40].
  • the decontamination gel is sprayed on a surface of a material.
  • a film is formed and radioactive substances like cobalum (Co), cesium (Cs) and strontium (Sr) are soaked in the film and are shown by the colorimetric indicator with different colors. In this way, positions of the contaminations are observed and are cleaned by removing the film. In addition, densities of the contamination are recognized by the colors.
  • FIG.5 is a view showing colors of a first state of use.
  • different colorimetric indicators have different color reactions.
  • decontamination gels separately having colorimetric indicators are obtained.
  • materials of stainless steel are used to be sunk in a cleanser.
  • the materials are cleansed with ultrasound before being hot-dried in an oven.
  • solutions separately having contaminations of Co, Cs and Sr are obtained and dropped on glasses to be hot-dried.
  • the decontamination gels separately having colorimetric indicators are sprayed on the glasses having contaminations of Co, Cs and Sr to show different colors.
  • the glasses having the contaminations of Co show obvious colors by the decontamination gels having alizarin and BrPADAP; and the glasses having the contaminations of Cs and Sr show obvious colors by the decontamination gels having alizarin and arsenazo III.
  • different decontamination gels separately having different colorimetric indicators detect materials separately having contaminations of Co, Cs and Sr for preventing pollution dispersion and protecting environment.
  • FIG.6 is a view showing colors of a second state of use.
  • a decontamination gel having more than two colorimetric indicators is used to show colors of materials having contaminations of Co, Cs and Sr.
  • two different colorimetric indicators are solved in an ethanol solution.
  • the mixed colorimetric indicators are added to a decontamination gel.
  • solutions separately having contaminations of Co, Cs and Sr are obtained and the mixed colorimetric indicators are dropped on glasses to be hot-dried to show different colors.
  • the colorimetric indicators are BrPADAP and arsenazo III; PR and alizarin; PR and arsenazo III; or alizarin and arsenazo III.
  • the glasses having the contaminations of Co, Cs and Sr show obvious colors by the decontamination gel having the colorimetric indicators.
  • the decontamination gel having the colorimetric indicators detects materials having contaminations of Co, Cs and Sr for preventing pollution dispersion and protecting environment.
  • a decontamination gel according to the present invention is obtained. Solutions having contaminations of Co, Cs and Sr are obtained and dropped on a glass to be hot-dried. After the temperature is cooled down to room temperature, the decontamination gel is sprayed on a glass having contaminations of Co, Cs and Sr to form a film after being dried up naturally. Thus, the contaminations of Co, Cs and Sr are cleaned by removing the film. By sinking the glass in an acid solution and analyze the acid solution afterward, a decontamination effect of the decontamination gel to materials having contaminations of Co, Cs and Sr is shown. As a result, it is shown that the decontamination gel has decontamination effects of 99%, 96% and 97% to Co, Cs and Sr separately.
  • the present invention is a decontamination method of a metal surface contaminated by radioactive element, where a blend of polymers, characteristic additives and a decontamination reagent are mixed to obtain a decontamination gel for indicating contaminations of Co, Cs and Sr and to obtain good decontamination effect by cleaning the contaminations by removing a film of the decontamination gel dried-up.

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  • High Energy & Nuclear Physics (AREA)
  • General Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Chemical & Material Sciences (AREA)
  • Life Sciences & Earth Sciences (AREA)
  • Food Science & Technology (AREA)
  • Chemical & Material Sciences (AREA)
  • Electrochemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Detergent Compositions (AREA)
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Claims (15)

  1. Dekontaminationsverfahren zur Dekontamination einer mit radioaktiven Elementen kontaminierten Metalloberfläche, das folgende Schritte umfasst:
    (a) Mischen von einem organischen Lösungsmittel, mehr als einem Polymer und Wasser, um ein Gelfluid zu erhalten;
    (b) Hinzufügen eines Dekontaminations-Reagens und eines Weichmachers in das Gelfluid bis zur vollständigen Vermischung und anschließendes Hinzufügen einer Lösung aus mindestens einem kolorimetrischen Indikator, um ein kolorimetrisches Dekontaminationsgel zu erhalten; und
    (c) Aufbringen des Dekontaminationsgels auf eine kontaminierte Oberfläche eines Materials, damit ein Film entsteht, und Entfernen des Films, so dass die Oberfläche dekontaminiert wird;
    wobei
    das organische Lösungsmittel aus einer Gruppe gewählt wird, die aus Acetylaceton, Acetonitril und Ethanol besteht;
    der Weichmacher aus einer Gruppe gewählt wird, die aus Tetrahydrofuran, N-Methylformamid, N,N-Dimethylformamid, Glycerin und Phthalatsäureester besteht; und der kolorimetrische Indikator eine Mischung aus einer Ethanollösung und mindestens einem Stoff ist, der aus einer Gruppe gewählt wird, die aus Alizarin, Phenolrot, Arsenazo III und 2-(5-Bromo-2-Pyridylazo)-5-Dimethylaminophenol besteht.
  2. Verfahren nach Anspruch 1, wobei das Gelfluid eine Temperatur zwischen 80°C und 95°C aufweist.
  3. Verfahren nach Anspruch 1 oder 2,
    wobei das Wasser und das organische Lösungsmittel ein physikalisches Verhältnis zwischen 1 und 5 haben.
  4. Verfahren nach einem der Ansprüche 1 bis 3,
    wobei das Polymer aus einer Gruppe gewählt wird, die aus Polyäthylenoxid, Polyacrylnitirl, Polyvinylalkohol, Polyvinylpyrrolidon, Polyvinylacetat, Carboxymethylcellulose, Polyäthylenoxid, Polyäthylenglycol, Gelatine, Apfelpektin und Gummi arabicum besteht.
  5. Verfahren nach einem der Ansprüche 1 bis 4,
    wobei der Weichmacher bei einer Temperatur von 80°C bis 95°C mit dem Polymer gemischt wird.
  6. Verfahren nach einem der Ansprüche 1 bis 5,
    wobei das Dekontaminationsreagens eine Mischung aus mindestens einer ersten Verbindung, einer anorganischen Säure und Wasser ist; und
    wobei die erste Verbindung aus einer Gruppe gewählt wird, die aus Diäthylentriaminpentanessigsäure, Äthylendiamintetraessigsäure, Apfelpektin, Preußisch-Blau, Ammoniumphosphomolybdat, Ce4+/Ce3+, Wasserstoffperoxid und Ferrocyanid besteht.
  7. Verfahren nach einem der Ansprüche 1 bis 6,
    wobei die anorganische Säure aus einer Gruppe gewählt wird, die aus Phosphorsäure, Chlorwasserstoffsäure, Ameisensäure und Schwefelsäure besteht.
  8. Verfahren nach Anspruch 6,
    wobei ein Molverhältnis des Dekontaminationsreagens zu der anorganischen Säure zu Wasser 1 zu 8 zu 175 beträgt.
  9. Verfahren nach einem der Ansprüche 1 bis 8,
    wobei der kolorimetrische Indikator und die Ethanollösung zu einem Verhältnis zwischen 0,01 und 0,03 gemischt werden.
  10. Verfahren nach einem der Ansprüche 1 bis 9,
    wobei das Dekontaminationsgel 24 Stunden lang bei einer Temperatur zwischen 10°C und 40°C der Luft ausgesetzt wird, damit der Film gebildet wird.
  11. Verfahren nach einem der Ansprüche 1 bis 10,
    wobei der Film eine Dekontaminationseffizienz größer 96% bei einer Kontamination aufweist, die ein Element aus der Gruppe Kobalt, Cäsium und Strontium enthält.
  12. Verfahren nach einem der Ansprüche 1 bis 11,
    wobei das Material aus einer Gruppe gewählt wird, die aus Edelstahl, Kohlenstoffstahl, Aluminium, Kupfer, Kunststoff und Glas besteht.
  13. Verfahren nach einem der Ansprüche 1 bis 12,
    wobei der kolorimetrische Indikator Kontaminationen an der Oberfläche des Materials färbt und so die kontaminierten Stellen anzeigt.
  14. Verfahren nach einem der Ansprüche 1 bis 13,
    wobei ein physikalisches Verhältnis des Dekontaminationsreagens zu dem Gelfluid in einer Lösungsmischung 1 bis 33 beträgt.
  15. Dekontaminationsgel zur Dekontamination einer mit radioaktiven Elementen kontaminierten Metalloberfläche, das aus Folgendem besteht:
    (a) einem organischen Lösungsmittel, mehr als einem Polymer und Wasser, die zu einem Gelfluid gemischt werden; und
    (b) einem Dekontaminationsreagens, einem Weichmacher und mindestens einem kolorimetrischen Indikator in dem Gel, damit ein kolorimetrisches Dekontaminationsgel entsteht; und
    (c) das dazu geeignet ist, auf eine kontaminierte Oberfläche eines Materials aufgebracht zu werden, damit ein Film gebildet wird, der zum Zwecke der Dekontamination von der Oberfläche entfernt wird, wobei
    das organische Lösungsmittel aus einer Gruppe gewählt wird, die aus Acetylaceton, Acetonitril und Ethanol besteht;
    der Weichmacher aus einer Gruppe gewählt wird, die aus Tetrahydrofuran, N-Methylformamid, N,N-Dimethylformamid, Glycerin und Phthalatsäureester besteht; und der kolorimetrische Indikator eine Mischung aus einer Ethanollösung und mindestens einem Stoff ist, der aus einer Gruppe gewählt wird, die aus Alizarin, Phenolrot, Arsenazo III und 2-(5-Bromo-2-Pyridylazo)-5-Dimethylaminophenol besteht.
EP07119543A 2007-10-29 2007-10-29 Dekontaminierungsverfahren für eine durch radioaktive Elemente kontaminierte Metalloberfläche Not-in-force EP2056302B1 (de)

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EP07119543A EP2056302B1 (de) 2007-10-29 2007-10-29 Dekontaminierungsverfahren für eine durch radioaktive Elemente kontaminierte Metalloberfläche
AT07119543T ATE538478T1 (de) 2007-10-29 2007-10-29 Dekontaminierungsverfahren für eine durch radioaktive elemente kontaminierte metalloberfläche

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EP07119543A EP2056302B1 (de) 2007-10-29 2007-10-29 Dekontaminierungsverfahren für eine durch radioaktive Elemente kontaminierte Metalloberfläche

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EP2056302B1 true EP2056302B1 (de) 2011-12-21

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TWI457948B (zh) * 2011-09-29 2014-10-21 Atomic Energy Council 化學及電化學除污裝置及其方法
KR20140095266A (ko) 2013-01-24 2014-08-01 한국원자력연구원 금속 표면 고착성 방사능 오염 산화막 제거를 위한 무착화성 화학 제염제 및 이를 이용한 화학 제염방법
KR101601201B1 (ko) * 2015-04-15 2016-03-09 한국원자력연구원 금속 표면 고착성 방사능 오염 산화막 제거를 위한 무착화성 화학 제염제 및 이를 이용한 화학 제염방법
IT201800004473A1 (it) * 2018-04-13 2019-10-13 Composizione detergente per la decontaminazione di superfici, in particolare di superfici radioattive, e relativo metodo di decontaminazione
CN116504432B (zh) * 2023-03-29 2026-04-21 中国原子能科学研究院 一种去污复合溶液及其凝胶膜的制备方法、应用

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US4511488A (en) 1983-12-05 1985-04-16 Penetone Corporation D-Limonene based aqueous cleaning compositions
US5494611A (en) 1993-11-24 1996-02-27 Armor All Products Corporation Dual-purpose cleaning composition for painted and waxed surfaces
US5763734A (en) 1995-10-19 1998-06-09 Nachtman; Thomas J. Method for containing or removing contaminants from a substrate
JPH105684A (ja) 1996-04-23 1998-01-13 Fuji Heavy Ind Ltd ストリッパブル塗膜の剥離方法
FR2798603B1 (fr) 1999-09-20 2002-03-01 Tech En Milieu Ionisant Stmi S Gel organique de decontamination et son utilisation pour la decontamination de surfaces
US6652661B2 (en) 2001-10-12 2003-11-25 Bobolink, Inc. Radioactive decontamination and translocation method

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