EP0727243B1 - Mousse de décontamination à l'ozone, et procédé de décontamination utilisant cette mousse - Google Patents
Mousse de décontamination à l'ozone, et procédé de décontamination utilisant cette mousse Download PDFInfo
- Publication number
- EP0727243B1 EP0727243B1 EP96400331A EP96400331A EP0727243B1 EP 0727243 B1 EP0727243 B1 EP 0727243B1 EP 96400331 A EP96400331 A EP 96400331A EP 96400331 A EP96400331 A EP 96400331A EP 0727243 B1 EP0727243 B1 EP 0727243B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- decontamination
- foam
- ozone
- phase
- surfactant
- 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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Classifications
-
- 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
-
- A—HUMAN NECESSITIES
- A62—LIFE-SAVING; FIRE-FIGHTING
- A62D—CHEMICAL MEANS FOR EXTINGUISHING FIRES OR FOR COMBATING OR PROTECTING AGAINST HARMFUL CHEMICAL AGENTS; CHEMICAL MATERIALS FOR USE IN BREATHING APPARATUS
- A62D1/00—Fire-extinguishing compositions; Use of chemical substances in extinguishing fires
- A62D1/0071—Foams
Definitions
- the invention relates to a decontamination foam. with ozone, usable in particular for decontaminating or rinse the surface of objects, especially objects relatively large or complex in shape, more particularly hollow volumes.
- the invention also relates to a decontamination process using this foam.
- the foam according to the invention is particularly applicable to decontamination of equipment or circuits nuclear industry, chemical industry, food industry or sanitary. It no longer applies particularly to the decontamination of circuits or devices made of copper, copper alloy, ordinary steel, or an alloy of iron, chromium and nickel, such as stainless steel in particular austenitic stainless steel for example steel 304 L stainless steel, or the alloy known as Inconel brand.
- Chemical or radioactive decontamination of the surface of objects is usually done by means of wet chemical processes, using solutions containing decontamination reagents and generally having a stripping power.
- Decontamination techniques used with solutions may consist of washing, sprinkling or soaking but when the parts to decontaminate have large dimensions, these techniques are unsuitable because they have the disadvantage of require large volumes of reagents and by way of consequence of causing the formation of very large quantities significant liquid active effluents.
- the volume of the phase liquid may be weak because the foam contains usually 5 to 50 times more gas than liquid. In consequence, the active liquid effluents obtained after decontamination are significantly reduced.
- radioactive contamination is divides into two types, whether they are products of fission, activation products or actinides.
- This process is therefore selective in dissolving of the surface oxide but gives a very dissolving minimal, if any, of the metal surface. In in addition, it generates a large amount of effluents liquids.
- a method for decontaminating surfaces the primary circuit of pressurized water reactors in particular chromium-nickel-iron alloy surfaces.
- This method consists in bringing the surfaces to contact treat with acid decontamination solution containing cerium (IV) nitrate and acid chromic, in the presence of ozone as an oxidizing agent.
- Ozone is preferably present in the form of saturated solution. It can also be used under form of a two-phase gas / water mixture in which ozone is in gaseous form, or in the form oxygen enriched with ozone.
- the attack on the metal is very slow and very weak, (on the order of a few micrometers in 48 hours), but it is precisely erosion of the surface surface of the metal which allows obtain good decontamination.
- the volumes of reagent involved represent several times the volume of the circuit of the device to be decontaminated.
- the invention aims to remedy to the drawbacks of the aforementioned prior art.
- the invention relates to a foam of decontamination.
- the redox couple forming decontamination agent is chosen from the pairs Ce 4+ / Ce 3+ , Co 3+ / Co 2+ , Ag 2+ / Ag + , S 2 O 2- / 3 / SO 2- / 4, V 2+ / V 3+ or Cr 4+ / Cr 3+ and it is associated with at least one acid.
- This acid allows the solubilization of the redox couple. It can be chosen from HCl, HNO 3 , H 2 SO 4 , H 3 PO 4 or their mixtures or be a weak acid.
- This redox couple can also be MnO - / 4 / MnO 2 associated with at least one base, in particular a strong base.
- the oxidizing action of ozone is increased, due to the enormous increase in the liquid surface (in the form thin strips), found in the bubbles of foam and due to the significant dissolution of the ozone inside this foam, while ozone moreover has a very solubility limited in water.
- the action of ozone foam is particularly remarkable for the decontamination of the first oxide layer which is deposited on the surface of copper alloys or alloys of iron, chromium and nickel, in particular of austenitic stainless steels.
- the layers of liquid in contact with the metal surfaces to be treated are quickly renewed due to the coalescence (degradation) of the bubbles and the drainage of the liquid phase on the surfaces, whereas if a liquid solution is used. decontamination and not foam, the boundary layers prevent the deep action of the liquid phase.
- the use of a foam makes it possible to remove deposits and metallic particles of several mm 3 which is not possible with a conventional liquid decontamination solution. Therefore, the foam of the present invention is particularly suitable in the case where a strong and rapid action is necessary, for example for dismantling and to "decategorize" the waste.
- this decontamination foam is also particularly suitable for the decontamination of the surface layer of a metal substrate.
- cerium (IV) for example
- brought initially in the foam tends to degrade in cerium (III), but it can then be transformed back into cerium (IV) by the action of ozone and can thus oxidize the chromium and make it soluble which facilitates decontamination. Therefore, the invention is very thrifty in cerium (respectively in another element redox) and there is no need to add of cerium during the use of the foam.
- the surfactant used in the liquid phase foam is preferably betaine, in especially a sulfobetaine or an alkyl ether oligosaccharide which have the advantage of being biodegradable. These two surfactants can also be used in admixture.
- sulfobetaine such as that sold by the Seppic Company under the trade name Amonyl®.
- alkyl ethers oligosaccharides we can cite the one sold by the Seppic company under the trade name Oramix CG 110® and the one sold by the Rohm and Hass Company under the name Triton CG60®.
- the combination of the two surfactants is also interesting because it remains surfactant whatever the pH and is therefore also suitable for neutral medium than in acidic or basic medium.
- the agent surfactant used in decontamination foam according to the invention destroys very slowly on contact of ozone. Therefore, it is sometimes necessary to add a little surfactant in the foam decontamination during its use.
- ozone has the great advantage of destroy the surfactants in the longer term, especially at the time of intermediate storage of the liquid effluent obtained after decontamination, before the discharge of this liquid effluent to the treatment station. The foaming power of this liquid effluent is then considerably weakened.
- the liquid phase consists of an aqueous solution comprising 0.1 to 3 mol / l of H 2 SO 4 (or better 1 mol / 1), 0.1 to 3 mol / l of HNO 3 ( or better 1 mol / l), 0.001 to 0.1 mol / l of ceric sulphate (or better 0.005 mol / l) and 0.2 to 1% by weight of surfactant (or better 0.5%) .
- the invention also relates to a method of decontamination consisting in bringing into contact surfaces contaminated with the above foam. This operation is generally carried out under pressure ambient and at a temperature between 10 and 70 ° C, preferably between 20 and 30 ° C. Indeed, the foam reactivity increases with temperature, but above 70 ° C, the foam tends to coalesce.
- At least one step of degreasing using a degreasing foam including the gas phase is air and whose liquid phase is an aqueous solution of at least one surfactant, a base and a viscosifier, and after having carried out the decontamination step, we carry out at least once a rinsing step using a rinsing foam whose gaseous phase is air and whose liquid phase is an aqueous solution of at least minus a surfactant.
- degreasing foams, decontamination and rinsing can be mixed to form a neutral effluent in which ozone residual oxidizes the surfactant.
- each decontamination foam used is recovered, filtered and recycled in the process of decontamination and the gas phase of the foam decontamination is treated on a catalyst to destroy the residual ozone before the phase is rejected gas in the atmosphere.
- the installation includes a tank of decontamination solution 1 connected to a foam generator 3 through a pipe 5 provided a filter 7 and a circulation pump 9.
- the foam generator 3 is supplied in phase gas from an ozone generator 11 by via a pipe 13.
- a pipe 15 connects the foam generator 3 to the exchanger 17 at clean. This will be described in more detail later.
- the foam is in contact with the walls to be decontaminated, then this foam comes out of the exchanger through an upper orifice 19 while the liquid (coalesced foam) flows to the bottom 21 of the exchanger and is evacuated via a pipe 23 provided a filter 25 and a recycling pump 27, towards the solution tank 1.
- the upper orifice 19 is connected by a pipe 29 to solution tank 1.
- the separated gas phase in the solution tank 1 is filtered on high efficiency filters 31 then treated on a catalyst 32 before being released into the atmosphere at by means of an extractor fan 33.
- the foam was formed in a mixer 3 using a hydropneumatic pump simultaneously injecting the liquid phase at the rate of 500 l / h and the gas phase, at the rate of 3 to 4 Nm 3 / h .
- the pressure of the gas allows the foam to fill the exchanger from the bottom.
- This foam has a humidity close to 15% by volume.
- the pressure of this foam also causes the foam to overflow at the top of the exchanger through the return connection to the tank of decontamination solution 1.
- the return foam is partially destroyed in the tank 1 by spraying with liquid and by centrifugation.
- the liquid from this foam after coalescence again serves to recreate a foam in the mixer 3. A portion of the foam can even be recycled as it is through the hydropneumatic pump. Liquids are kept at a temperature of 20 ° C.
- decontamination is carried out. of exchanger n ° 17 I, using foam with the air.
- Decontamination of exchanger No. 17 II is carried out using oxygen foam enriched with ozone (100 g of O 3 / Nm 3 of O 2 ), in the presence of cerium (IV).
- Example 1 the quantities of cerium (IV) added are regularly consumed by the oxidation of metals, which requires permanent additions, up to 16 kg. Decontamination is good to judge by the lower dose rates (16 ⁇ Gy / h), and the radioactivity extracted. The quantity of liquid effluent is small: 1.2 m 3 . The decontamination factor is 40.
- Example 2 better results are obtained than in Example 1.
- a smaller quantity of cerium (IV) is used (6 kg), but this product is expensive.
- Each of the two acid phases goes further in decontamination.
- the quantity of dissolved iron can exceed by 100% that dissolved in example 1.
- the residual dose rate of the exchanger is low ( ⁇ 6 ⁇ Gy / h).
- the quantity of liquid effluent is also low: 1.2 m 3 .
- the decontamination factor is 160.
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- Engineering & Computer Science (AREA)
- Chemical Kinetics & Catalysis (AREA)
- Chemical & Material Sciences (AREA)
- General Chemical & Material Sciences (AREA)
- Food Science & Technology (AREA)
- Life Sciences & Earth Sciences (AREA)
- Electrochemistry (AREA)
- Physics & Mathematics (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Business, Economics & Management (AREA)
- Emergency Management (AREA)
- Apparatus For Disinfection Or Sterilisation (AREA)
- Cleaning And De-Greasing Of Metallic Materials By Chemical Methods (AREA)
Description
- d'une phase liquide constituant le milieu de dispersion, qui renferme le(s) réactif(s) de décontamintion et le(s) additif(s) nécessaire(s) pour former la mousse, et
- d'une phase gazeuse constituant la phase dispersée, qui est généralement formée d'air, d'azote ou d'un gaz neutre tel que l'argon (EP 0526 305 A).
- une contamination radioactive de surface due à des éléments radioactifs qui se déposent sur les surfaces des appareils et des tuyauteries et qui sont piégés par les oxydes métalliques également présents sur ces surfaces, et
- une contamination radioactive en profondeur due à une petite fraction des éléments radioactifs qui pénètrent dans le métal des appareils et des tuyauteries, c'est-à-dire dans les microfissures et les joints intergranulaires.
- a) une phase liquide comprenant une solution d'au moins un agent tensio-actif et d'un couple oxydo-réducteur formant agent de décontamination, et
- b) une phase gazeuse dispersée dans la phase liquide et comprenant de l'air enrichi en ozone ou de l'oxygène enrichi en ozone, (de préférence entre 1 et 1000 g d'ozone/Nm3 d'oxygène, ou mieux entre 10 et 200 g d'ozone/Nm3 d'oxygène).
- matériau : acier inoxydable 304L,
- dimensions de la virole : longueur 6,5 m, diamètre 0,5 m,
- surface des tubes : 214 m2
- le fluide primaire circulait du côté de la calandre, sans chicanes. C'est donc l'espace entre les tubes qui a été contaminé en radioéléments béta et gamma et qui fait l'objet de la décontamination
- le fluide secondaire circulait côté tube en trois passes.
- première phase : il s'agit d'une phase de dégraissage réalisée à l'aide d'une mousse de dégraissage basique dont la phase liquide contient 250 l d'eau, 40 kg d'NaOH et 0,5% en poids d'agents tensio-actifs.
- deuxième phase : il s'agit d'une phase de dissolution des oxydes et d'attaque du métal, réalisée à l'aide d'une mousse acide dont la phase liquide comprend 250 l d'eau, 16 kg d'acide sulfurique à 92%, 46 kg d'acide nitrique à 62%, 6 kg de sulfate cérique et 0,5% en poids d'agents tensio-actifs ;
- troisième phase : elle est identique à la deuxième ;
- quatrième phase : il s'agit d'une phase de rinçage à l'aide d'une mousse de rinçage formée de 250 l d'eau et de 0,5% en poids d'agents tensio-actifs.
Claims (15)
- Mousse de décontamination à l'ozone, caractérisée en ce qu'elle comprend :a) une phase liquide comprenant une solution d'au moins un agent tensio-actif et un couple oxydo-réducteur formant agent de décontamination, etb) une phase gazeuse dispersée dans la phase liquide et comprenant de l'air enrichi en ozone ou de l'oxygène enrichi en ozone.
- Mousse de décontamination selon la revendication 1, caractérisée en ce que la phase gazeuse comprend entre 1 et 1000 g d'ozone/Nm3 d'oxygène, de préférence entre 10 et 200 g d'ozone/Nm3 d'oxygène.
- Mousse de décontamination selon la revendication 1, caractérisée en ce que le couple oxydo-réducteur formant agent de décontamination est choisi parmi les couples Ce4+/Ce3+, Co3+/Co2+, V2+/V3+, Ag2+/Ag+, S2O 2- / 3/SO 2- / 4 ou Cr4+/Cr3+ et en ce qu'il est associé à au moins un acide.
- Mousse de décontamination selon la revendication 3, caractérisée en ce que l'acide est choisi parmi HCl, HNO3, H2SO4, H3PO4 ou leurs mélanges.
- Mousse de décontamination selon la revendication 1, caractérisée en ce que le couple oxydo-réducteur formant agent de décontamination est MnO - / 4/MnO2 et en ce qu'il est associé à au moins une base forte.
- Mousse de décontamination selon la revendication 1, caractérisée en ce que l'agent tensio-actif est choisi parmi une bétaïne, un éther alkylique d'oligosaccharide ou leurs mélanges.
- Mousse de décontamination selon la revendication 3, caractérisée en ce que la phase liquide est constituée par une solution aqueuse comprenant :0,1 à 3 mol/l d'acide sulfurique,0,1 à 3 mol/l d'acide nitrique,0,001 à 0,1 mol/l de sulfate cérique,0,2 à 1 % en poids d'agent tensio-actif.
- Mousse de décontamination selon la revendication 7, caractérisée en ce que la phase liquide est constituée par une solution aqueuse comprenant environ 1 mol/l d'acide sulfurique, 1 mol/l d'acide nitrique, 0,005 mol/l de sulfate cérique et 0,5% en poids d'agent tensio-actif.
- Procédé de décontamination caractérisé en ce qu'il consiste à mettre une surface à décontaminer en contact avec la mousse de décontamination selon l'une quelconque des revendications précédentes à une température de décontamination comprise entre 10 et 70°C, de préférence entre 20 et 30°C.
- Procédé de décontamination selon la revendication 9, caractérisé en ce qu'après avoir réalisé l'étape de décontamination, on effectue au moins une fois une étape de rinçage à l'aide d'une mousse de rinçage dont la phase gazeuse est de l'air et dont la phase liquide est une solution aqueuse d'au moins un agent tensio-actif.
- Procédé de décontamination selon la revendication 9 ou 10, caractérisé en ce qu'avant l'étape de décontamination, on effectue au moins une étape de dégraissage à l'aide d'une mousse de dégraissage dont la phase gazeuse est de l'air et dont la phase liquide est une solution aqueuse d'au moins un agent tensio-actif, d'une base et d'un agent viscosant.
- Procédé de décontamination selon la revendication 11, caractérisé en ce qu'après la décontamination et lorsque la phase aqueuse de la mousse de décontamination contient un acide, les mousses de dégraissage, de décontamination et de rinçage sont mélangées pour former un effluent neutre dans lequel l'ozone résiduel oxyde l'agent tensio-actif.
- Procédé de décontamination selon la revendication 9, 10 ou 11, caractérisé en ce qu'après la décontamination, chaque mousse de décontamination utilisée est récupérée et recyclée dans le procédé de décontamination.
- Procédé de décontamination selon la revendication 9, 10 ou 11, caractérisé en ce qu'après l'étape de décontamination, la phase gazeuse de la mousse de décontamination est traitée sur un catalyseur pour détruire l'ozone résiduel avant le rejet de la phase gazeuse dans l'atmosphère.
- Procédé de décontamination selon l'une quelconque des revendications 9 à 14, caractérisé en ce qu'il est appliqué au nettoyage de surfaces contaminées réalisées en cuivre, en alliage de cuivre, en acier, ou en alliage de fer, de chrome et de nickel tel que l'acier inoxydable.
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR9501921A FR2730641B1 (fr) | 1995-02-20 | 1995-02-20 | Mousse de decontamination a l'ozone, et procede de decontamination utilisant cette mousse |
FR9501921 | 1995-02-20 |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0727243A1 EP0727243A1 (fr) | 1996-08-21 |
EP0727243B1 true EP0727243B1 (fr) | 2001-06-27 |
Family
ID=9476311
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP96400331A Expired - Lifetime EP0727243B1 (fr) | 1995-02-20 | 1996-02-16 | Mousse de décontamination à l'ozone, et procédé de décontamination utilisant cette mousse |
Country Status (3)
Country | Link |
---|---|
EP (1) | EP0727243B1 (fr) |
DE (1) | DE69613496T2 (fr) |
FR (1) | FR2730641B1 (fr) |
Families Citing this family (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1998044960A1 (fr) * | 1997-04-04 | 1998-10-15 | Toyota Jidosha Kabushiki Kaisha | Agent purifiant, appareil et procede permettant de former un agent purifiant, et procede de purification utilisant l'agent |
FR2775606B1 (fr) * | 1998-03-09 | 2000-03-31 | Commissariat Energie Atomique | Mousse de decontamination comprenant un agent oxydant tel que le cerium (iv) |
GB0014189D0 (en) * | 2000-06-09 | 2000-08-02 | Bradtec Decon Technologies Ltd | Method of applying foam reagents for radioactive decontamination |
CN101199026B (zh) * | 2005-11-29 | 2012-02-22 | 阿利发Np有限公司 | 对核技术设施的部件或系统的含氧化层表面去污的方法 |
FR2994427B1 (fr) * | 2012-08-10 | 2014-08-22 | Technavox | Catalyseur solide pour ozonation catalytique de composes organiques en milieu aqueux |
Citations (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1985004279A1 (fr) * | 1984-03-09 | 1985-09-26 | Studsvik Energiteknik Ab | Decontamination de reacteurs a eau sous pression |
Family Cites Families (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
SE435329B (sv) * | 1983-02-09 | 1984-09-17 | Studsvik Energiteknik Ab | Dekontaminering av tryckvattenreaktorer |
CH673545A5 (fr) * | 1987-10-02 | 1990-03-15 | Industrieorientierte Forsch | |
FR2679458A1 (fr) * | 1991-07-23 | 1993-01-29 | Commissariat Energie Atomique | Mousse de decontamination a duree de vie controlee et installation de decontamination d'objets utilisant une telle mousse. |
FR2687005B1 (fr) * | 1992-02-03 | 1994-10-21 | Framatome Sa | Procede et installation de decontamination de la partie primaire d'un generateur de vapeur usage d'un reacteur nucleaire a eau ordinaire sous pression. |
-
1995
- 1995-02-20 FR FR9501921A patent/FR2730641B1/fr not_active Expired - Lifetime
-
1996
- 1996-02-16 DE DE1996613496 patent/DE69613496T2/de not_active Expired - Lifetime
- 1996-02-16 EP EP96400331A patent/EP0727243B1/fr not_active Expired - Lifetime
Patent Citations (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
WO1985004279A1 (fr) * | 1984-03-09 | 1985-09-26 | Studsvik Energiteknik Ab | Decontamination de reacteurs a eau sous pression |
Also Published As
Publication number | Publication date |
---|---|
DE69613496T2 (de) | 2002-04-25 |
FR2730641A1 (fr) | 1996-08-23 |
EP0727243A1 (fr) | 1996-08-21 |
FR2730641B1 (fr) | 1997-03-14 |
DE69613496D1 (de) | 2001-08-02 |
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