EP1346373B1 - Procede pour eliminer des echangeurs d'ions charges radioactivement et devant etre stockes, tout en reduisant leur volume - Google Patents

Procede pour eliminer des echangeurs d'ions charges radioactivement et devant etre stockes, tout en reduisant leur volume Download PDF

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Publication number
EP1346373B1
EP1346373B1 EP01980359A EP01980359A EP1346373B1 EP 1346373 B1 EP1346373 B1 EP 1346373B1 EP 01980359 A EP01980359 A EP 01980359A EP 01980359 A EP01980359 A EP 01980359A EP 1346373 B1 EP1346373 B1 EP 1346373B1
Authority
EP
European Patent Office
Prior art keywords
biosorbents
ion exchangers
radionuclides
radioactive metals
radioactive
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
Application number
EP01980359A
Other languages
German (de)
English (en)
Other versions
EP1346373A2 (fr
Inventor
Andreas Wolf
Günther Mann
Manfred Kühn
Herwig Brunner
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
ATC Dr Mann eK
Original Assignee
Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
ATC Dr Mann eK
Priority date (The priority date 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 date listed.)
Filing date
Publication date
Application filed by Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV, ATC Dr Mann eK filed Critical Fraunhofer Gesellschaft zur Forderung der Angewandten Forschung eV
Publication of EP1346373A2 publication Critical patent/EP1346373A2/fr
Application granted granted Critical
Publication of EP1346373B1 publication Critical patent/EP1346373B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

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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
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • G21F9/32—Processing by incineration
    • 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
    • G21F9/04—Treating liquids
    • G21F9/06—Processing
    • G21F9/12—Processing by absorption; by adsorption; by ion-exchange
    • 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
    • G21F9/30—Processing
    • 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
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • 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
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/307—Processing by fixation in stable solid media in polymeric matrix, e.g. resins, tars

Definitions

  • the invention relates to a method for reducing the volume of stored, radioactively charged ion exchangers.
  • the inventive method can be radioactively contaminated ion exchangers, which are used in particular in the nuclear area as Adsorbermaterialien dispose of the radioactive metals and / or radionuclides are eluted from the ion exchangers, the eluate is decontaminated with Biosorbentiea, the biosorbents with the bound radioactive metals and or radionuclides are burned and the solid combustion residues are trapped in glass powder, cement or bitumen.
  • the process of the invention has significance for the disposal and disposal of radioactive constituents from ion exchangers used in industrial plants, such as e.g. in nuclear power plants and in radioactive metal and / or radionuclide scientific and hospital facilities.
  • the object of the present invention was therefore to provide a cost-effective, easy to carry out and effective method for the volume-reducing disposal of radioactively charged ion exchangers to be stored, which are e.g. To provide in huge quantities in the decontamination of water from nuclear power plants to provide, especially those based on polystyrene.
  • the object is achieved by eluting radioactively loaded ion exchangers and the eluates are brought into contact with the radioactive metals and / or radionuclides with biosorbents, which are bound in the solutions contained radioactive metals and / or radionuclides to the biosorbents, the loaded Biosorbents are separated from solutions liberated to the tolerable limits of radioactive metals and / or radionuclides, which are subjected to a combustion process involving the bound radioactive metals and / or radionuclides, which reduced to a very small volume, solid burn residues of the loaded biosorbents in be enclosed in a material such as glass, cement or bitumen and so volume-reduced and stable storable a radioactive waste disposal or disposal are fed.
  • the invention relates to organic-synthetic ion exchangers, in particular polystyrene-based ion exchangers, more particularly to spherical resin ion exchangers.
  • the elution of the radioactive metals and / or radionuclides from the ion exchangers is carried out under suitable and technically known conditions, as a rule and therefore preferably under acidic pH conditions at pH values of less than 7, preferably between 1 and 3.
  • the elution is of course also with aqueous solutions of complexing agents, eg EDTA (ethylenediaminetetraacetic acid) or NTE (nitrilotriacetic acid) possible.
  • biosorbents for the purposes of the present invention, all insoluble materials of biological origin can be used, which are capable of biosorbing radioactive metals and / or radionuclides.
  • the biosorbing process which can be carried out with biosorbents is a relatively new and very economical possibility for removing toxic metals from the environment (Biotechnol Prog., 1995, 11, 235-250 and Appl. Microbiol. Biotechnol., 1997, 48, 577-587), since biosorbents different origin and structure can bind toxic metals with sometimes very high binding rates. Biosorbents are in cheap and easily accessible in most cases. Biosorbents are known materials that can be obtained, inter alia, from the biomass of mosses, algae, fungi or bacteria.
  • biosorbents All previously mentioned modified and unmodified biosorbents, but also from biological material isolated and purified and optionally also chemically and / or biologically modified Biomakromolelcüle such as celluloses, starch, xylans, agarose, dextranes, lignins, humic acids, chitin, chitosan and co- Macromolecules of the abovementioned biomacromolecules are understood as bioadsorbers in connection with their use in this patent.
  • Biomakromolelcüle such as celluloses, starch, xylans, agarose, dextranes, lignins, humic acids, chitin, chitosan and co- Macromolecules of the abovementioned biomacromolecules are understood as bioadsorbers in connection with their use in this patent.
  • biosorbents according to DE 197 184 52 A1 are used.
  • the biosorbents Before the radioactively charged eluates of ion exchangers of any origin are brought into contact with the listed biosorbents, the biosorbents must be brought to a pH suitable for the binding of the radioactive metals and / or radionuclides.
  • the pH range at which a connection of radioactive metals and / or radionuclides to Biosorbentien is at pH values between 2.0 to 14, especially between 4.0 and 8.0.
  • the contacting of the radioactively loaded liquid sample with the biosorbent is carried out in two ways, either by the batch process or by the column method.
  • the radioactive metals and radionuclide-binding biosorbents are added to the reactor in a radioactively loaded eluate and the resulting suspension is different times at temperatures of 5 ° C to 50 ° C, preferably at a temperature of 15 ° C to 30 ° C stirred.
  • the stirring times are from 5 minutes to 10 hours, preferably from 1 hour to 3 hours.
  • the biosorbents are filled in a column suitable for chromatography in a suitable amount for the application, through which the radioactive metals and / or radionuclides containing eluate is passed.
  • Flow through the filled chromatography column binds the radioactive metals and / or radionuclides to the biosorbents.
  • the operating temperatures apply as in the batch process.
  • the conditions for binding are selected in the specific application case within the given and above-mentioned general binding conditions so that the prescribed release values for radioactive effluents (eluate residue) in the receiving waters, which must be less than or 25 Bq / l.
  • Influencing factors for this are, for example, the amount of radioactive metals and / or radionuclides to be bound, the amount of biosorbents, the pH of the eluate solutions to be purified, the working temperatures and stirring or throughput times.
  • the biosorbents are separated from the purified radioactive eluate solutions, advantageously by filtration through suitable barrier layers or by suitable membrane modules, optionally after addition of combustible and thereby no soot-producing filter aids. In some cases, where the properties of the loaded biosorbents do not permit filtration, the separation may also be by centrifugation. Residues of this process step then remain the biosorbents loaded according to the invention and still to be disposed of, as well as the eluate solutions which can be released from the effluents and freed of radioactivity, and ion exchangers which can be used again.
  • biosorbents loaded with radioactive metals and / or radionuclides are subsequently burned.
  • the combustion process has already been tried for radioactively loaded polystyrene-based organic ion exchangers, it has hitherto not been technically possible due to the difficulties described.
  • biosorbents loaded with radioactive metals and / or radionuclides are very well suited for their disposal by incineration and a concomitant dramatic reduction in the volume of radioactive waste because they burn only to form gaseous products, water and a very low inorganic material ashes.
  • no soot is formed, which has hitherto made the use of combustion technology in the disposal of radioactive material on the basis of polystyrene so difficult or completely prevented.
  • This combustion plant with a throughput of about 50 kg / hour consists of a combustion furnace, a post-combustion chamber and downstream equipment for particle separation and flue gas scrubbing.
  • a built-in suction filter keeps the entire incinerator to the feed system under vacuum, so that before they are cleaned to remove radioactive particles and gases, no exhaust gases leave the incinerator and can reach the environment untreated. After their purification and analytical control, the exhaust gases are fed through a chimney to the environment.
  • the feeding of the incinerator is automatic and discontinuous depending on the temperature and pressure conditions in the incinerators and the concentrations of added oxygen and combustion of resulting carbon monoxide or carbon dioxide in the flue gases.
  • the ashes obtained after the combustion are automatically discharged from the plant and, according to the invention, fed to a further preparation by inclusion in glass powder, cement or bitumen.
  • Biosorbents are burned in the oven at ⁇ 1100 ° C.
  • the minimum temperature shall be 850 ° C and the minimum oxygen content 6%.
  • the small residual residue after incineration is ashes consisting of inorganic material which give only a negligible fraction of the volume of radioactive biosorbents and still much less of the liquid radioactive eluate solutions used to load the biosorbents. According to the method described so far for the reduction of radioactively contaminated waste, a previously unachieved volume reduction effect on radioactively contaminated waste occurs.
  • the volumes decrease in the disposal of the radioactively loaded polystyrene-based ion exchangers and, depending on the type of burned bioadsorber and the amount of bound radioactive metals and / or radionuclides, to 0.05 to 5% of the initial volume of the decontaminated ion exchanger Polystyrene base, wherein the ion exchanger itself is operational again.
  • the inclusion products according to the invention produced for the intermediate or final disposal according to the method of the invention are easy to handle during transport and storage, as they can be shaped and packed according to their type of storage during the manufacturing process. So they can be stored in the intermediate or final storage, saving space. The previously low storage capacities for radioactive waste can thus be used much more effectively.
  • the achieved according to the invention volume reduction effect of the radioactive waste produced contributes significantly to a more economical intermediate or final disposal of radioactive waste.
  • the biosorbents used according to the invention are obtained from renewable raw materials. They are cheap and easily accessible. Upon their incineration, significantly lower levels of radioactive waste pollute the storage capacities than in the current state of the art. As main combustion residue only as much carbon dioxide is formed, as was consumed for the biological synthesis of biosorbents from the atmosphere. The combustion process is advantageously CO 2 neutral. Combustion does not require the addition of additional combustion promoting materials. The combustion of biosorbents loaded with radioactive metals and / or with radionuclides only requires low temperatures, so that the risk of contamination of the environment with radioactive material via the combustion products is technically minimized or eliminated altogether by simpler means.
  • radioactive residues occupy only a small volume, are dry and can be easily processed into mixtures with glass powder, cement or bitumen. There are no problems of segregation of individual components of the materials used for inclusion, especially when mixing bitumen with aqueous radioactively contaminated wastewater concentrates.
  • special cements can be omitted in the process of the invention.
  • the filled column is then eluted with 0.1 molar hydrochloric acid, with a flow rate of about 20 ml / min is set. After a flow of about 5000 ml, the elution is complete, the residual activity of the ion exchanger is then at about 2.0 x 10 1 Bq / l. With this residual activity, it can be sent to normal waste recycling or reuse.
  • the recovered eluate containing the radioactivity becomes adjusted to pH 7.0 by adding 5 molar sodium hydroxide solution.
  • 200 ml of pre-swollen bioadsorber (prepared according to DE 197 18 452 A1) are now filled into a second chromatography column with identical dimensions as above. Thereafter, the neutralized eluate is also run at a flow rate of about 20 ml / min over this second column, which is also behind a shield made of lead bricks.
  • the eluate obtained in this case still has a radioactive residual activity of about 5.0 x 10 ° Bq / l and is fed to the normal wastewater.
  • the column with the loaded bio-adsorber remains on site for 24 hours to dry thoroughly.
  • the loaded Bioadsorber is removed from the column, filtered off over a ceramic frit, sucked dry and fed to the combustion. This is done in the described and nuclear approved incinerator. The residues of the waste gas purification are again bound to Bioadsorbern, which can be burned again. As a residue of the combustion incurred inorganic ash, which now occupies only a volume of 1.5 ml, is disposed of according to the prior art, ie either glazed or cemented.
  • Example 2 An identical test setup as described in Example 1 is created. For the elution of the ion exchanger but instead of hydrochloric acid 0.1 molar sulfuric acid is used. The neutralization of the eluate is now carried out with solid calcium hydroxide (about 70 g). The suspension is allowed to stand overnight and then filtered from precipitated calcium sulfate. This has bound about 90% of the initial activity and is concreted or glazed together with the resulting ashes of the Bioadsorbers. The bond of the water in the Eluates remaining residual activity is analogous to the above, except in this case the binding to 40 ml of an ion exchanger of phosphorylated cellulose.

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  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
  • Solid-Sorbent Or Filter-Aiding Compositions (AREA)
  • Electrical Discharge Machining, Electrochemical Machining, And Combined Machining (AREA)
  • Treatment Of Water By Ion Exchange (AREA)

Claims (8)

  1. Procédé d'élimination, réduisant le volume, d'échangeurs d'ions à stocker, contaminés par de la radioactivité,
    caractérisé en ce
    qu'on élue les métaux radioactifs et/ou les radionucléides des échangeurs d'ions, on décontamine l'éluat avec des sorbants biologiques, on brûle les sorbants biologiques contenant les métaux radioactifs et/ou les radionucléides liés et on incorpore les résidus de combustion solides dans du verre pulvérisé, du ciment ou du bitume.
  2. Procédé selon la revendication 1,
    caractérisé en ce
    qu'il s'agit d'échangeurs d'ions à base de polystyrène.
  3. Procédé selon la revendication 1 ou 2,
    caractérisé en ce
    qu'on effectue l'élution des métaux radioactifs et/ou des radionucléides des échangeurs d'ions avec des solutions aqueuses à des conditions de pH acide, à un pH < 7, de préférence à un pH compris entre 1 et 3.
  4. Procédé selon la revendication 1 ou 2,
    caractérisé en ce
    qu'on effectue l'élution des métaux radioactifs et/ou des radionucléides des échangeurs d'ions avec des agents complexants en solutions aqueuses.
  5. Procédé selon une des revendications 1 à 4,
    caractérisé en ce
    qu'en tant que sorbants biologiques, on utilise des matières premières biologiques d'origine végétale, notamment des matières premières et des sous-produits contenant de la cellulose et de la lignocellulose issus de l'agriculture, l'exploitation forestière, l'exploitation du papier, l'industrie alimentaire et du secteur économique de la pêche.
  6. Procédé selon la revendication 5,
    caractérisé en ce
    qu'en tant que sorbants biologiques, on utilise des biomacromolécules, de préférence des celluloses, de l'amidon, du xylane, de l'agarose, du dextrane, de la lignine, des acides humiques, de la chitine, du chitosane ou des comacromolécules des biomacromolécules mentionnées auparavant.
  7. Procédé selon la revendication 5 ou 6
    caractérisé en ce
    qu'on modifie chimiquement et/ou biologiquement les sorbants biologiques.
  8. Procédé selon une des revendications 5 à 7,
    caractérisé en ce
    qu'on effectue la décontamination des éluats d'échangeurs d'ions avec les sorbants biologiques dans des procédés sur colonnes ou par batch à des températures de 5°C à 50°C, de préférence de 15°C à 30°C, et à un pH compris entre 2 et 14, de préférence entre 4 et 8.
EP01980359A 2000-09-07 2001-09-07 Procede pour eliminer des echangeurs d'ions charges radioactivement et devant etre stockes, tout en reduisant leur volume Expired - Lifetime EP1346373B1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10045788 2000-09-07
DE10045788A DE10045788A1 (de) 2000-09-07 2000-09-07 Verfahren zur Volumenreduzierung von radioaktiv belasteten Abfällen
PCT/EP2001/010404 WO2002021538A2 (fr) 2000-09-07 2001-09-07 Procede pour eliminer des echangeurs d'ions charges radioactivement et devant etre stockes, tout en reduisant leur volume

Publications (2)

Publication Number Publication Date
EP1346373A2 EP1346373A2 (fr) 2003-09-24
EP1346373B1 true EP1346373B1 (fr) 2006-08-23

Family

ID=7656401

Family Applications (1)

Application Number Title Priority Date Filing Date
EP01980359A Expired - Lifetime EP1346373B1 (fr) 2000-09-07 2001-09-07 Procede pour eliminer des echangeurs d'ions charges radioactivement et devant etre stockes, tout en reduisant leur volume

Country Status (5)

Country Link
EP (1) EP1346373B1 (fr)
AT (1) ATE337603T1 (fr)
AU (1) AU2002212220A1 (fr)
DE (2) DE10045788A1 (fr)
WO (1) WO2002021538A2 (fr)

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
UA78704C2 (en) * 2003-12-22 2007-04-25 Oleksandr Oleksandro Kapitonov Method for cleaning liquid radioactive waste and wastewater
FR2943167B1 (fr) * 2009-03-11 2011-03-25 Electricite De France Traitement de dechets radioactifs carbones.
FR2956517B1 (fr) * 2010-02-17 2012-03-09 Commissariat Energie Atomique Procede de traitement avant calcination d'une solution aqueuse nitrique comprenant au moins un radionucleide et eventuellement du ruthenium

Family Cites Families (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE1564656A1 (de) * 1966-07-11 1970-02-12 Sartorius Membranfilter Gmbh Verfahren zur Dekontaminierung von Fluessigkeiten,die radioaktive Ionen enthalten
FR2068158A5 (en) * 1969-11-28 1971-08-20 Commissariat Energie Atomique Strontium-90 removal from irradiated fuel effluent - using carboxylic acid cation exchange resin
US4120933A (en) * 1977-09-27 1978-10-17 The United States Of America As Represented By The Unites States Department Of Energy Decontamination of plutonium from water with chitin
JPS6113195A (ja) * 1984-06-28 1986-01-21 住友化学工業株式会社 放射性排水の処理法
US4800024A (en) * 1986-04-07 1989-01-24 Iso-Clear Systems Corporation Removal of heavy metals and heavy metal radioactive isotopes from liquids
DE4117234A1 (de) * 1991-05-27 1992-12-03 Winfried Prof Dr Ing Hartmeier Praeparat zur biosorption von schwermetallen sowie dessen herstellung und anwendung
DE4138544A1 (de) * 1991-11-23 1993-05-27 Winfried Prof Dr Ing Hartmeier Mittel zur biosorption von schwermetallen sowie dessen herstellung und anwendung
JP2726375B2 (ja) * 1993-08-13 1998-03-11 動力炉・核燃料開発事業団 ＰｕおよびＮｐ含有硝酸溶液からのＰｕとＮｐの分離回収方法
JPH0868893A (ja) * 1994-08-29 1996-03-12 Sumitomo Metal Mining Co Ltd 種々の放射性物質及び重金属元素を含む廃液の処理方法
DE19718452C2 (de) * 1997-04-30 2001-09-13 Mann Guenther Biosorbentien für Metallionen und Verfahren zu ihrer Herstellung
DE19844171A1 (de) * 1998-09-25 2000-03-30 Koeckritz Tim Biosorptionsverfahren zur Entfernung von Metallen aus citronensaurer und gluconsaurer Lösung mit Schimmelpilzen

Also Published As

Publication number Publication date
DE10045788A1 (de) 2002-04-04
WO2002021538A3 (fr) 2002-11-07
AU2002212220A1 (en) 2002-03-22
WO2002021538A2 (fr) 2002-03-14
EP1346373A2 (fr) 2003-09-24
ATE337603T1 (de) 2006-09-15
DE50110833D1 (de) 2006-10-05

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