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EP1430487A1 - Procede de mise au rebut d'un objet en ceramique, graphite et/ou charbon contamine par au moins une matiere toxique, en particulier radiotoxique - Google Patents

Procede de mise au rebut d'un objet en ceramique, graphite et/ou charbon contamine par au moins une matiere toxique, en particulier radiotoxique

Info

Publication number
EP1430487A1
EP1430487A1 EP02758142A EP02758142A EP1430487A1 EP 1430487 A1 EP1430487 A1 EP 1430487A1 EP 02758142 A EP02758142 A EP 02758142A EP 02758142 A EP02758142 A EP 02758142A EP 1430487 A1 EP1430487 A1 EP 1430487A1
Authority
EP
European Patent Office
Prior art keywords
ceramic
granules
container
coating material
granulate
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.)
Granted
Application number
EP02758142A
Other languages
German (de)
English (en)
Other versions
EP1430487B1 (fr
Inventor
Heinz BRÜCHER
Gerd Haag
Werner Von Lensa
Rainer Moormann
Reinhard Odoj
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.)
Forschungszentrum Juelich GmbH
Original Assignee
Forschungszentrum Juelich GmbH
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 Forschungszentrum Juelich GmbH filed Critical Forschungszentrum Juelich GmbH
Publication of EP1430487A1 publication Critical patent/EP1430487A1/fr
Application granted granted Critical
Publication of EP1430487B1 publication Critical patent/EP1430487B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

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
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • G21F9/305—Glass or glass like 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
    • G21F9/008—Apparatus specially adapted for mixing or disposing radioactively contamined material

Definitions

  • the invention relates to a method for disposing of an object made of ceramic, graphite and / or coal stone contaminated with at least one toxic, in particular radiotoxic.
  • DE 197 37 891 A1 discloses a method of the type mentioned at the outset in which the object to be disposed of is first heated in order to remove some of the toxicants by outgassing or thermal decomposition. The removed portion of the toxicant is collected and the partially decontaminated article and the collected toxicant are then separately passed on to further disposal steps.
  • the captured toxicants in high concentration are disposed of in a way that is already used for more radioactive waste, e.g. B. filters from nuclear plants, is known. Due to the reduced concentration of the radiotoxics, the partially decontaminated article can be handled under less stringent requirements and can be stored temporarily or temporarily. To protect against fire and leaching, the surface of the object can be treated, e.g. B.
  • any stored energy generated by radiation-induced interference with the crystal lattice (Wigner energy) and the associated risk of self-heating are eliminated in a controlled manner.
  • the objects to be disposed of come from nuclear facilities, these are usually solid blocks with dimensions of approx. 0.5 to 1 m in height and width and up to approx. 2 m Length that contain significant amounts of different radiotoxics. They fall, for example, when decommissioning graphite-moderated nuclear reactors or during normal operation of gas-cooled reactors by exchanging ceramic components, e.g. B. fuel element casings or in the form of moderator columns in material test reactors (MTR) or in the form of ceramic or carbon-containing adsorbent from cleaning systems of all kinds.
  • MTR material test reactors
  • reactor graphite and coal stone are particularly susceptible to chemical attack and leaching.
  • Reactor graphite is a graphite form with extremely high porosity that is used especially for nuclear facilities.
  • Coal stone is also highly porous.
  • the object of the invention concerned here is to provide a method of the type mentioned at the outset with which the utilization of given storage capacities can be optimized and at the same time efficient protection against combustion and leaching is provided.
  • the object is achieved in a method of the type mentioned at the outset, in which the object is comminuted into granules, the object is heated before, during and / or after the comminution in order to reduce its contamination, and the granules are either poured over with a liquefied coating material is, or mixed with the coating composition in powder or granular form and then heated until the coating composition liquefies, the liquefied coating composition either solidifying itself into a ceramic or chemically reacting with the granulate to form a ceramic.
  • the comminution of the object enables the material to be disposed of to be adapted to predetermined shapes, e.g. B. the shape of transport containers or the geometry of the deposit, and thus optimizing the use of space. Crushing to granulate with grain sizes of at most a few cm allows almost any shape. In the case of a liquefied coating mass which reacts chemically with the material of the granulate, the granulate can react completely under the appropriate conditions. As a rule, at least the larger granules of the granulate will react to form a ceramic only in the area of a surface layer from a few ⁇ m to approximately 1 mm thick.
  • the granules are mixed with the powdery or granular coating, it can also be mixed with liquefied coating before, during or after heating.
  • the comminution and the coating of the granules with the coating compound also have the effect that the contamination remaining after baking out is essentially distributed in the volume of the container.
  • This is particularly advantageous in the case of objects to be disposed of which have a high surface contamination and little or no volume contamination.
  • the conversion into volume contamination can lead to significantly lower demands on the handling of the containers due to the lower surface dose rate and the given self-shielding.
  • Another advantage of shredding is when the granules themselves are baked out, since more efficient baking can be achieved due to the shorter diffusion paths.
  • the parameters to be used in the process according to the invention are each dependent on the type of the original concentrations of the toxicants and the desired properties of the container. Should a toxic due to the high stability of its binding to the object or can only be expelled to the required extent by heating the object over uneconomically long periods of time, the corresponding toxic by chemical reaction with a suitable substance, for. B. a halogen, in a thermally removable from the object chemical compound, for. B. a halide.
  • the heated toxicants are - as is already known from the prior art - collected and disposed of separately.
  • the mixture produced from the granulate and the coating material can be filled into a suitable container to produce a container that can be stored in an interim or final storage facility. This can be done in the flowable or mouldable state of the batch in order to completely fill the container with the batch.
  • the use of metallic containers is known. However, these have the disadvantage that hydrogen can form due to oxidation of the metal in aqueous solution and can collect in the repository.
  • the method according to the invention can be carried out in such a way that, after the mixture has been poured, the container is completely filled with an uncontaminated, liquid filling compound which solidifies to form ceramic.
  • the loading container closed in such a way that the mixture has no contact with the environment.
  • the filler mass, the z. B. can solidify to the same ceramic, of which the container consists, so closes the latter.
  • the method according to the invention can also be carried out in such a way that the mixture produced from the granulate and the coating composition is used in the flowable or moldable state for filling up the interstices in other containers containing intermediate, repository or repository-capable waste.
  • the method according to the invention can be carried out in such a way that, in order to produce a container that can be stored temporarily or permanently, another contaminated waste is completely encased with the mixture produced from the granulate and the coating composition in the flowable or moldable state.
  • the batch can enclose the other contaminated objects without any space and thus form an optimally adapted container. If the residual contamination is sufficiently low, particularly in the area of the surface of the batch, the container can be stored temporarily or without further coating.
  • a suitable form e.g. B. a cuboid or cylinder.
  • the other waste is completely enclosed by the batch, it can also be one that is itself considerably more contaminated than the batch, e.g. B. to highly radioactive waste, e.g. B. fuel assemblies.
  • the shielding by the ceramic covering can be completely sufficient for final storage. Otherwise, further shielding measures must be taken according to the state of the art.
  • Both the filling of the gaps and the covering of waste with the batch can advantageously be carried out before it has completely solidified. However, it is also possible to provide this in a later process step after heating the batch separately.
  • the method according to the invention can be carried out in such a way that the mixture produced from the granules and the coating composition is shaped into a container, the container is filled with further contaminated waste, sealed and temporarily or finally stored with this content.
  • the batch is thus processed into a commodity that can be suitable for wrapping even highly radioactive waste.
  • the container can e.g. B. be pot-shaped. Cover elements such as lids can also be formed.
  • a container made of two or more parts can e.g. B. by means of silicon, which is deposited from the gas phase of a silicon-containing compound, or by applying silicon carbide, which e.g. is produced from uncontaminated raw materials. It is also possible to thread the container parts.
  • the method according to the invention can also be carried out in such a way that a carbide former is used as the coating material for objects containing carbon.
  • Liquid silicon which forms SiC with carbon, is particularly suitable for this.
  • the ceramic SiC forms a refractory, leach-resistant and abrasion-resistant protective layer around the granules.
  • Other suitable carbide formers are e.g. B. boron and zircon.
  • the method according to the invention can also be designed in such a way that reinforcing ceramic fibers are added to the coating composition or to the mixture produced from the granules and the coating composition.
  • the fibers can e.g. B. used as wound fibers, fiber mats or pieces of fiber from a few mm to a few cm in length. They increase the ductility and thus the resistance of the container to crack formation and brittleness if it is present in the container, in the ceramic casing or in the container contents.
  • Phenolic resins can also be added. When they are heated, they are decomposed, and the resulting carbon can be mixed with the coating material, e.g. B. silicon to SiC react.
  • metal structures for reinforcing the ceramic are also conceivable.
  • the method according to the invention can be carried out such that the comminution takes place under an inert gas atmosphere. This reduces the risk of ignition and deflagration and, in the case of carbon-containing objects, the reaction with atmospheric oxygen to form CO or CO 2 avoided, which would normally contain C 14 and therefore must not escape.
  • Suitable atmospheres are e.g. B. nitrogen and argon.
  • the method according to the invention can also be carried out in such a way that the liquefied coating composition is poured around or the mixture of coating composition and granules is heated in a vacuum. This can in particular prevent gas inclusions from hindering the complete wetting of the granulate surface by the liquefied coating compound. Furthermore, the vacuum can already be generated during the comminution of the object in order to reduce the risk of deflagration and that of CO or CO 2 formation.
  • the method according to the invention can be carried out in such a way that the object and the resulting granulate are moistened with a non-combustible liquid during comminution.
  • the method according to the invention can also be carried out in such a way that the object is immersed in a non-flammable liquid for comminution.
  • Water is particularly suitable for both moistening and comminution in liquid. If the material of the object to be disposed of is not wetted by water, a suitable solvent can be added to it.
  • the method according to the invention can also be carried out in such a way that dust which arises during the comminution of the object and which floats in the liquid is collected and cast with the granulate together with the coating. The dust can be collected by means of filters and / or by evaporating the liquid. The dust is thus effectively disposed of.
  • the method according to the invention can be carried out in such a way that the liquid is collected and fed to the method again.
  • the liquid is thus circulated, which relieves the burden on the environment.
  • the method according to the invention can also be carried out in such a way that the surface of the batch is oxidized.
  • the shell mass unless it is already itself a liquefied ceramic, will not continuously form a chemical compound with the formation of a ceramic in the method according to the invention.
  • silicon as a coating, a resistant surface made of ceramic, abrasion-resistant Si0 2 is produced.
  • the oxidation takes place by heating the container in an oxidizing atmosphere, e.g. B. 0 2 or air.
  • the separate heating of the container can be saved if the oxidizing atmosphere is generated as soon as possible after the granulate has been poured around it.
  • a high level of abrasion resistance is desirable in order to keep the uncontrolled loss of packaging material as low as possible. Mohs hardness greater than or equal to 4 would be advantageous.
  • the method according to the invention can be designed in such a way that containers which are made up of the granulate and the casing mass Contain generated batches are formed so that they can be placed together with surface contact.
  • Exemplary shapes are those with a rectangular or hexagonal cross section. They allow a seamless line-up and thus an optimized use of space.
  • the two-dimensional interaction also prevents a rock pressure in the repositories that acts against one another in the direction of the side surfaces and does not lead to cracks or brittleness in the container as quickly as is the case with cylindrical containers, which are only on the side have a linear contact with each other.
  • the method according to the invention can be carried out in such a way that it is carried out at the place where the object is used.
  • a carbon moderator element used in a nuclear power plant is assumed.
  • Such moderators have a ceramic structure composed of high-purity and porous graphite (reactor graphite) and coal stone.
  • a moderator is usually contaminated with different toxic substances.
  • the moderator element is placed in a high-temperature furnace heated by direct current passage.
  • heating can also be carried out inductively or using separate heating elements. The heating takes place in vacuum or under protective gas in order to prevent carbon monoxide and carbon dioxide, which contain the radioactive C 14 which is usually present in the irradiated carbon, and which therefore must not escape uncontrollably, when reacting with the atmospheric oxygen.
  • This method is already described in detail in DE 197 37 891 AI.
  • the object is crushed after it has been baked out, or even before or during the process.
  • This comminution can either take place outside the reactor pressure vessel or inside. In the latter case, large blocks and opening of the enclosure are avoided.
  • the comminution device would have to be introduced into the reactor vessel. With appropriate attachment to a manipulator arm, it is possible to disassemble and shred the blocks in-situ and then only remove the piece goods or granules. If the thermal treatment is only carried out afterwards, this can also be carried out within the reactor pressure vessel, since the heating devices required can be very compact.
  • the comminution is carried out under inert gas to avoid deflagration.
  • the piece goods can be moistened or completely in liquid, e.g. B. be immersed in water. A prior thermal expulsion of tritium should take place in order not to dislodge the liquid with it.
  • the dried sludge containing the dust can be returned to the disposal process and the liquid can be recycled after condensation. If the granules are heated, this can be carried out continuously or batchwise under inert gas.
  • the level of the temperature depends on the type of toxic substances and the desired decontamination factors. Essentially, the graphite cleaning procedure known in the graphite industry can be used here. Highly volatile toxic substances, such as B.
  • tritium or cesium are driven off at relatively low temperatures.
  • Toxic substances chemically bound to carbon must be detached from the ceramic structure by pyrolysis at higher temperatures. If individual toxic substances cannot be removed from the moderator material, e.g. B. difficult to decompose carbides, these can be converted into volatile halides by adding and infiltrating gaseous halogen compounds.
  • the toxic substances removed from the moderator material are separated on condensation plates or caught by traps or filters (e.g. for tritium), where they are then present in a considerably higher concentration than in moderator material.
  • the partially decontaminated moderator material now only contains toxic substances that could not be removed with thermal and / or thermochemical treatment. It follows from this that diffusion or leaching out of these toxic substances would not take place even over extremely long periods of time.
  • the thermally and / or chemically pretreated comminuted moderator material is permeated with liquid silicon, the surfaces of the carbon-containing granules reacting to SiC at a correspondingly high temperature, and a container made of Si and SiC with embedded granulate pieces can be poured off or extruded.
  • the shape, e.g. B. cylinders, cuboids or flat Cylinder segments that can be arranged next to each other are based on the transport and storage container geometries for the best possible use of space.
  • silicon dioxide being formed at the points accessible to the oxygen, which provides additional protection against oxidation, which also withstands long-term corrosion attacks.
  • the material can also be poured into small containers, which in turn can hold other hazardous substances and protect against corrosion and leaching. Furthermore, the still liquid mixture can be used for pouring out gaps or for enveloping whole or disassembled reactor fuel elements.
  • silicon carbide is also characterized by good heat conduction.
  • a coating made of SiC is much more resistant than metal.
  • Another disadvantage of the metal compared to the SiC is that the oxidation of metals in aqueous solution generates large amounts of hydrogen, which accumulate in the repository and can be a source of danger.

Landscapes

  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
  • Compositions Of Oxide Ceramics (AREA)

Abstract

L'invention concerne un procédé de mise au rebut d'un objet en céramique, graphite ou charbon contaminé par au moins une matière toxique, en particulier radiotoxique. En vue de réaliser la décontamination partielle de l'objet, l'invention est caractérisée en ce que cet objet est chauffé et, en même temps, les fractions éliminées des matières toxiques sont recueillies, et en ce qu'ensuite, l'objet décontaminé et les matières toxiques recueillies sont amenés séparément à d'autres étapes de mise au rebut. L'objet est avant, pendant ou après le traitement thermique, fragmenté en granulats puis coulé avec une matière formant une gaine, de telle façon que le granulat soit muni d'une gaine en céramique. Après refroidissement du mélange constitué par la gaine et le granulat, il se forme un emballage en fût compact, non combustible, résistant à la lixivation et à l'usure par frottement. L'emballage également être réalisé sous la forme d'un conteneur pour matière dangereuse ou être utilisé comme enveloppe de déchets contaminés ou pour le remplissage d'espaces intermédiaires ayant une excellente tenue sur une longue durée et une haute résistance aux fuites.
EP02758142A 2001-09-28 2002-08-10 Procede de mise au rebut d'un objet en ceramique, graphite et/ou charbon contamine par au moins une matiere toxique, en particulier radiotoxique Expired - Lifetime EP1430487B1 (fr)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
DE10148146 2001-09-28
DE10148146A DE10148146B4 (de) 2001-09-28 2001-09-28 Verfahren zur Entsorgung eines mit mindestens einem Radiotoxikum kontaminierten Gegenstandes aus Reaktorgraphit und/oder Kohlestein
PCT/DE2002/002951 WO2003032328A1 (fr) 2001-09-28 2002-08-10 Procede de mise au rebut d'un objet en ceramique, graphite et/ou charbon contamine par au moins une matiere toxique, en particulier radiotoxique

Publications (2)

Publication Number Publication Date
EP1430487A1 true EP1430487A1 (fr) 2004-06-23
EP1430487B1 EP1430487B1 (fr) 2010-03-17

Family

ID=7700803

Family Applications (1)

Application Number Title Priority Date Filing Date
EP02758142A Expired - Lifetime EP1430487B1 (fr) 2001-09-28 2002-08-10 Procede de mise au rebut d'un objet en ceramique, graphite et/ou charbon contamine par au moins une matiere toxique, en particulier radiotoxique

Country Status (4)

Country Link
EP (1) EP1430487B1 (fr)
DE (2) DE10148146B4 (fr)
ES (1) ES2343003T3 (fr)
WO (1) WO2003032328A1 (fr)

Families Citing this family (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102004036631B4 (de) * 2004-07-28 2013-02-21 Forschungszentrum Jülich GmbH Verfahren zur Behandlung einer mit Radiokarbon kontaminierten Keramik, insbesondere Reaktorgraphit
DE102013003847B3 (de) * 2013-03-07 2014-09-04 Forschungszentrum Jülich GmbH Fachbereich Patente Verfahren zur Dekontamination von Radionukliden aus neutronenbestrahlten Kohlenstoff- und/ oder Graphitwerkstoffen

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3001629A1 (de) * 1980-01-17 1981-09-24 Alkem Gmbh, 6450 Hanau Verfahren zur endkonditionierung fester radioaktiverabfaelle
US4834914A (en) * 1987-06-09 1989-05-30 Jackson O L Radioactive waste disposal system and method
US5265545A (en) * 1989-04-12 1993-11-30 Miltox Holdings Pte, Limited Method and apparatus for waste treatment
FR2659876B1 (fr) * 1990-03-23 1992-08-21 Tanari Rene Procede et four de traitement de dechets fusibles.
FR2659877B1 (fr) * 1990-03-23 1992-11-27 Tanari Rene Procede et four de traitement de dechets incinerables.
US5424042A (en) * 1993-09-13 1995-06-13 Mason; J. Bradley Apparatus and method for processing wastes
DE19737891C2 (de) * 1997-08-29 2002-08-01 Forschungszentrum Juelich Gmbh Verfahren zur Entsorgung eines mit Radiotoxika kontaminierten Gegenstandes aus Reaktorgraphit oder Kohlestein

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
See references of WO03032328A1 *

Also Published As

Publication number Publication date
DE10148146B4 (de) 2009-08-27
DE10148146A1 (de) 2003-05-15
EP1430487B1 (fr) 2010-03-17
DE50214295D1 (de) 2010-04-29
WO2003032328A1 (fr) 2003-04-17
ES2343003T3 (es) 2010-07-21

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