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EP2368254B1 - Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire - Google Patents

Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire Download PDF

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Publication number
EP2368254B1
EP2368254B1 EP09804242A EP09804242A EP2368254B1 EP 2368254 B1 EP2368254 B1 EP 2368254B1 EP 09804242 A EP09804242 A EP 09804242A EP 09804242 A EP09804242 A EP 09804242A EP 2368254 B1 EP2368254 B1 EP 2368254B1
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EP
European Patent Office
Prior art keywords
plant
corrosion medium
medium
corrosion
radiotoxic
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.)
Not-in-force
Application number
EP09804242A
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German (de)
English (en)
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EP2368254A2 (fr
Inventor
Werner Von Lensa
Johannes Fachinger
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Forschungszentrum Juelich GmbH
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Forschungszentrum Juelich GmbH
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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
    • G21F9/28—Treating solids
    • 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

Definitions

  • the invention relates to a method for the at least partial removal of a radiotoxic or specific radiotoxic agents from a still operational nuclear facility before their final decommissioning.
  • a disadvantage when disassembling are the high technical complexity and the associated radiation exposure and costs.
  • the high local dose rate in the interior of a nuclear facility and the risk of incorporation, especially in the mechanical processing of plant components make it often necessary to perform the dismantling remote controlled and / or under water or behind shields.
  • Particularly problematic contaminants z. B. in the dismantling of graphite moderated nuclear reactors are in this context, for. B. 14 C because of its biocompatibility and 36 Cl because of its solubility.
  • these isotopes have relatively long half-lives, so that their dangerousness is only insignificantly reduced by a decades-long "safe enclosure" before the start of dismantling.
  • a better separation of the radiotoxic from the non-radiant base material of the plant should be done as in the prior art.
  • a method has been developed for the at least partial removal of at least one radiotoxic agent from a nuclear facility.
  • the nuclear part of this plant is flowed through by at least one operating medium, which is introduced into the plant through at least one flow and is carried out by at least one return from the plant. It can be heated advantageously in the nuclear part of the plant.
  • the operating means may be a cooling liquid or a cooling gas used in normal operation to transfer the thermal reactor power to heat exchangers.
  • At least one corrosion medium is introduced individually or in combination with the operating medium, preferably metered, through the flow into the system at a suitable temperature.
  • the nuclear part of the plant is thereby heated by nuclear fission, possibly additionally by externally introduced energy to a temperature that supports or accelerates the chemical reaction.
  • the corrosion medium is then in the system, advantageously controlled, brought into contact with the radiotoxic and transferred the radiotoxic by a chemical reaction, at least in part in a chemical compound.
  • this chemical compound may be volatile, such as a gas.
  • the chemical reaction takes place substantially only on outer and inner surfaces, with which the corrosion medium comes into contact, including inner surfaces of pores, in which the corrosion medium penetrates.
  • the chemical compound is at least partially carried out by the return from the plant. It can be advantageously removed from the circulation in the circuit for the equipment, for example in the cooling circuit, already existing cleaning devices during and after application of the method.
  • the corrosion process can be controlled by the prevailing nuclear temperature, which can be provided by nuclear fission or by the temperature of the corrosion medium, as well as by the dosage of the corrosion medium so that neither the safety nor the strength of the structures in the nuclear part (in particular Core structures) are at risk.
  • the choice of the corrosion medium can cause the reaction with the radiotoxic agents to produce a comparatively low-risk, for example gaseous, chemical compound for further processing, which can advantageously be converted into solid products capable of end-storage (eg carbonates, carbides or chlorides).
  • the method according to the invention also offers great advantages in terms of the approval capability.
  • the process is usually performed only while or after the nuclear facility is already operating or operating in an approved normal condition. It can be used in particular during the reactor operation or in the final phase of the operating time. This not only has the technical advantage that the operating temperatures can be advantageously used to assist or accelerate the chemical reaction. If the operating state deviates only slightly from this normal state when carrying out the method, then only this small deviation must be approved by nuclear law.
  • any overriding of a security system is associated with temporary or permanent decommissioning and to approve each breakthrough by a barrier due to the resulting increase in risk separately, which can take years and excludes re-commissioning.
  • the execution of the chemical reaction only on outer and inner surfaces can be controlled via the process parameters, in particular via the composition of the corrosion medium, via the amount and / or concentration of the corrosion medium and the temperature of the nuclear installation and / or the corrosion medium.
  • Even within the usual operating temperatures of gas-cooled graphite-moderated reactors MAGNOX / UNGG: 150-400 ° C, EGR: 250-650 ° C, HTR: 250-950 ° C
  • there is considerable room for control of the reaction Especially at the relatively low temperatures in the MAGNOX / UNGG and AGR is a stronger involvement of radiotoxic agents, eg. B. prevented by diffusing near-surface contamination in the crystal lattice or in the remaining core structures inside.
  • the operating temperature profiles can also be adjusted as necessary by modifying the gas flow rate, reducing system performance, and optimizing the power distribution (changing the trip bar settings) to achieve sufficient conversion of 14 C and other radiotoxic agents in all parts of the reactor core.
  • the optimum temperature for the metered corrosion thus depends on the chemical reactivity of the corrosion medium, the diffusion rate in the pore system, which can be increased or controlled, for example by reducing the pressure or by adding light inert gases, and the dimensions of the material to be corroded.
  • the corrosion products eg, carbon monoxide enriched with carbon monoxide or carbon dioxide
  • the corrosion products can be more easily removed from the coolant loop. This could be z. B. by temporary replacement of CO 2 in MAGNOX, UNGG and AGR against noble gases done with metered corrosion media.
  • the process parameters are not limited to the range intended for normal operation.
  • the temperature in the decommissioning phase, for example, can certainly be increased to a range beyond the design limit for normal operation, and it can be accepted that the durability of parts of the system may be irreversibly weakened.
  • gas-cooled graphite-moderated reactors usually have a gas purification system, which can optionally be adapted in their performance and selectivity. If now about 14 C oxidized in the reactor by the inventive method, the resulting reaction products CO and CO 2 can be removed using the gas cleaning system from the cooling gas, such as helium at HTR. If the reactor uses CO 2 as the cooling gas, the gas purification system can be equipped with an isotope separation device for this purpose
  • the process parameters are chosen so that the corrosion medium can penetrate far into an existing pore system, so that it converts at least a portion of the radiotoxic there located by a chemical reaction in a chemical compound.
  • This is particularly advantageous when a gas-cooled graphite moderated reactor is to be decontaminated.
  • Reactor graphite and coal are extremely porous, so have a very large internal surface area.
  • a contamination with radiocarbon ( 14 C) is present in these media in two main forms: on the one hand as only loosely bound to the inner surface contamination, on the other hand stably bound to regular places in the crystal lattice.
  • a gaseous corrosion medium This may for example contain oxygen, air, water vapor, hydrogen, a halogen or a halogenated hydrocarbon.
  • a gaseous corrosion medium is particularly advantageous when the system is flowed through during operation of a gaseous coolant as the operating medium. Then, the corrosion medium can be metered into this coolant, and gaseous reaction products exit with the coolant from the return.
  • the radiotoxic agent is at least partially converted by the corrosion medium into a gaseous chemical compound.
  • a gaseous chemical compound for example, CO, CO 2 , a hydrocarbon (in particular CH 4 ), a halogenated hydrocarbon, HTO or an acid (in particular HCl) can be formed.
  • a gaseous compound is best removed from the plant, for example, by conventional or retrofitted gas cleaning systems in the cooling circuit, but also by flushing the system with an inert medium, such as by replacing the cooling medium, or by evacuating the system.
  • the radiotoxic agent can be converted by the corrosion medium alternatively or in combination thereto but also at least partially into a solid chemical compound which precipitates, for example, from said liquid phase.
  • the chemical compound is advantageously collected and fed to a separate treatment. It can then be enriched, for example, the remote from the plant radiotoxic, so that much of the contamination initially present in the system can be disposed of using a minimum repository volume.
  • the enriched radiotoxic, and here in particular 14 C can also be used as a valuable material, as this, like other radioisotopes, finds applications in medicine or in technology.
  • the process according to the invention can be carried out in particular on gas-cooled graphite-moderated reactors in such a way that the radiocarbon ( 14 C) removed from the reactor is enriched. Subsequently, the remaining graphite can also be recycled for nuclear engineering or disposal. From the extracted radiocarbon is advantageous again a solid, z. As in the form of graphite, hydrocarbons (eg., Bitumen), carbides or carbonates produced to condition it for disposal. If the radiocarbon is to be used in high concentration, a cyclic process for the corrosion medium may be advantageous, especially when using hydrogen or water vapor as the oxygen supplier.
  • hydrocarbons eg., Bitumen
  • the cyclic process could look like this: During the corrosion process, under appropriate process conditions, the endothermic reaction of graphite with, for example, hydrogen or water vapor as reaction products occurs Methane or carbon monoxide and hydrogen. Extracted and collected methane or carbon monoxide now contain a significantly higher proportion of radiocarbon than the original ceramic. This proportion can now be further increased by enrichment processes. In a further step, solid carbon can be generated from the methane or carbon monoxide by pyrolysis or reduction. The reaction products can be reused in the circulation.
  • carbon monoxide or CH 4 is preferably produced as the reaction gas.
  • Carbon monoxide and CH 4 have a lower weight than carbon dioxide. With these reaction gases, therefore, the given weight difference between radiocarbon and the stable isotopes of the carbon can be better utilized for enrichment of the radiocarbon.
  • the production of leach-resistant, non-combustible storage containers makes sense.
  • This can be z. B. by reaction of the radiocarbon-rich material to carbides, z. B. SiC, or rock-like carbonates, or bitumen happen.
  • the corrosion medium should be chosen so that the reaction gases are as directly as possible suitable for the further treatment steps.
  • the corrosion medium attacks on the way through the system at least one component thereof. This favors the replacement of the radiotoxicum from external and internal surfaces and leaves the plant components with only a small residual contamination, so that they can be disposed of as near-surface "low-level waste” or even released immediately or after further decontamination.
  • This embodiment is the furthest away from the teachings hitherto prevalent in the art. With regard to the long operating times of nuclear installations and the inaccessibility of contaminated areas for repairs, it was precisely the access of media that attack the substance of the installation that was reduced to a minimum. It is the merit of the inventors to have recognized that just such media supported the safe dismantling. This applies in particular when the corrosion medium in the plant with graphite, in particular Reactor graphite or coal or insulating materials, which is contaminated with one or more radiotoxic agents. In particular, radiocarbon ( 14 C) behaves chemically as well as the carbon in the graphite, so that there are hardly any means that convert the radiocarbon and leave the base material graphite unchanged.
  • radioactive chloroisotope 36 which arises as an activated residue from the production of graphite by neutron irradiation.
  • Injections z. B. of water vapor and / or hydrogen, the bound chlorine can be converted into more volatile gaseous compounds and similar to radiocarbon peel from the graphite structure.
  • the process according to the invention can generally also be carried out, for example, in several stages, wherein the aggressiveness of the corrosion medium is increased from stage to stage or else the corrosion medium is changed. For example, different fractions of radiotoxic agents can be removed separately from the plant.
  • the corrosion medium can also be injected locally into certain areas of the system.
  • the corrosion medium in the system of outer and inner surfaces including inner surfaces of pores, z. B. adsorbed during the Anlagenstilistands and then produced the process temperature. This will help to control the amount of corrosion medium used to load the surfaces. This can in turn be achieved that in addition to the radiotoxic as little non-radioactive material is attacked and removed from the system.
  • metered corrosion prior to adsorbing the corrosion medium, metered corrosion can be carried out by controlled addition of the corrosion medium at process temperature such that at least a portion of closed pores is opened. This ensures that during the adsorption, the corrosion medium reaches the largest possible area proportion of the inner surfaces of the pore system. The decontamination of these inner surfaces becomes more complete.
  • the cooling gas blower can advantageously be operated so that in the reactor existing contaminated dusts and in particular particulate matter are specifically mobilized. Then these dusts are primarily converted by the chemical reaction and removed from the plant. Fine particles are the most dangerous type of contamination for the personnel and therefore require special protective measures according to the state of the art. If these dusts are eliminated or reduced by the method according to the invention, the further handling is considerably simplified.
  • the inventive method pre-purifies the graphite so far that a simplified removal of the graphite blocks from the reactor core and a safer disposal are possible. It can be expected that the inventive method is an essential part of remove all existing surface contamination. Specifically, the performance of the chemical reaction with the corrosion medium only in near-surface areas here has the effect that the graphite blocks are not structurally weakened and not break when manipulated by manipulators. If the handling of the graphite blocks for shielding the radiation and binding of fine dusts under water, there is the advantage of a lower conversion of radiotoxic agents in the introduced liquid. However, the method according to the invention makes a contribution to the fact that possibly a handling under water can be omitted. This is a decisive advantage, especially in installations in which flooding with water is not possible for static reasons.
  • i-graphite irradiated graphite
  • An embodiment of the invention provides that surface-selective oxidation processes with oxygen, water vapor or halogens or surface-selective reduction processes with hydrogen, hydrocarbons or halogenated hydrocarbons are carried out in a first process step.
  • These corrosion media can be introduced, for example, as an admixture to an inert gas atmosphere at temperatures in the range of the reactor operating temperature.
  • FIG. 1 is shown by way of example how a separation of 14 C can be carried out in this way.
  • Plotted are the release ⁇ C-14 of 14 C and ⁇ C-12 of 12 C over time t at a process temperature of 900 ° C.
  • the release of 14 C increases much faster than the release of 12 C, since the fastest mobilisable portion of the total existing carbon contains a high proportion of 14 C.
  • the factor by which the release of 14 C is above that of 12 C decreases with time.
  • about 70% of 14 C is released, about 2% of 12 C is also released. The factor has dropped from over 100 to about 35. For lower process temperatures, similar results are expected while extending the process time.
  • metallic radionuclides are converted into more volatile metal halides with higher concentrations of halogens and optionally also higher temperatures, so that they likewise pass into the gas phase. Since significantly lower temperatures are generally used in this process than in prior art processes in which the graphite is treated ex situ after removal from the reactor core in a separate furnace system, the expected reaction rate is significantly lower than in the case of ex situ treatment. Therefore, cyclic gas routing is advantageous. The extra work required for this purpose is more than offset by a significant reduction in the total cost of dismantling.
  • a temperature which supports or accelerates the chemical reaction is produced by further operation of the nuclear fission, by utilizing the residual heat from the decomposition of the fission products after switching off the nuclear fission, optionally additionally by internal or external heating elements.
  • the use of the residual heat can be advantageously supported by a reduction in the circulation rate, a reduction in the refrigerant pressure or a reduction in heat dissipation via the heat exchangers.
  • An external heater has the advantage that no colder zones occur near the feed of the corrosion medium.
  • the cooling gas systems already present in the reactor can continue to be used. To separate the radionuclides, it then suffices to modify the gas purification system. If this is not possible, a gas bypass can be used to install a new gas cleaning system adapted to the temperatures and gas composition.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Physical Or Chemical Processes And Apparatus (AREA)

Claims (16)

  1. Procédé de retrait au moins partiel d'au moins un radiotoxique d'une installation de technique nucléaire, dont la partie nucléaire est traversée en service par au moins un agent d'exploitation, où l'agent d'exploitation est introduit dans l'installation par au moins un conduit d'alimentation et est évacué de l'installation par au moins un conduit de recirculation, caractérisé par les étapes suivantes :
    a. au moins un milieu de corrosion est introduit dans l'installation, seul ou en combinaison avec l'agent d'exploitation, par le conduit d'alimentation ;
    b. le milieu de corrosion est mis en contact dans l'installation avec le radiotoxique et convertit au moins partiellement le radiotoxique par une réaction chimique en un composé chimique, où la réaction chimique se produit essentiellement uniquement sur des surfaces extérieures et intérieures avec lesquelles le milieu de corrosion entre en contact, y compris les surfaces intérieures de pores, dans lesquels pénètre le milieu de corrosion, et où la partie nucléaire de l'installation est chauffée par fission nucléaire ou par réchauffage à partir de la décomposition des produits de fission à une température qui favorise ou accélère la réaction chimique ;
    c. ce composé chimique est au moins partiellement évacué de l'installation par le conduit de recirculation.
  2. Procédé selon la revendication 1, caractérisé en ce que les poussières présentes dans l'installation de technique nucléaire sont mobilisées par des fluctuations soudaines de la vitesse du liquide de refroidissement.
  3. Procédé selon l'une des revendications 1 à 2, caractérisé en ce que les paramètres de procédé sont choisis de manière que le milieu de corrosion puisse pénétrer profondément dans un système de pores présent, de manière à convertir en un composé chimique au moins une partie du radiotoxique s'y trouvant par le biais d'une réaction chimique.
  4. Procédé selon l'une des revendications 1 à 3, caractérisé en ce que le radiotoxique est converti au moins partiellement en un composé chimique gazeux par le biais du milieu de corrosion.
  5. Procédé selon la revendication 4, caractérisé en ce qu'un ou plusieurs des composants suivants sont formés en tant que composé chimique gazeux :
    a. CO
    b. CO2
    c. hydrocarbure, en particulier CH4
    d. hydrocarbure halogéné
    e. HTO
    f. acide, en particulier HCl
  6. Procédé selon l'une des revendications 1 à 5, caractérisé en ce que le composé chimique formé à partir du milieu de corrosion et du radiotoxique est piégé et conduit vers un traitement séparé.
  7. Procédé selon l'une des revendications 1 à 6, caractérisé en ce que le milieu de corrosion, sur le chemin qu'il prend à travers l'installation, attaque au moins un composant de celle-ci.
  8. Procédé selon l'une des revendications 1 à 7, caractérisé en ce qu'un milieu de corrosion gazeux est choisi.
  9. Procédé selon la revendication 8, caractérisé en ce qu'un milieu qui comprend un ou plusieurs des composants suivants :
    a. oxygène
    b. air
    c. vapeur d'eau
    d. hydrogène
    e. halogène
    f. hydrocarbure halogéné
    est choisi.
  10. Procédé selon l'une des revendications 1 à 9, caractérisé en ce que l'installation est traversée en service par un liquide de refroidissement sous forme gazeuse en tant qu'agent d'exploitation.
  11. Procédé selon l'une des revendications 1 à 10, caractérisé en ce que le milieu de corrosion est mis en contact dans l'installation avec du graphite, en particulier du graphite de réacteur ou de la brique de carbone, qui est contaminé(e) par au moins un radiotoxique.
  12. Procédé selon l'une des revendications 1 à 11, caractérisé en ce que le milieu de corrosion est mis en contact dans l'installation avec 14C, 36Cl, 129I, 60Co, 3H ou 99Tc à titre de radiotoxique.
  13. Procédé selon l'une des revendications 1 à 12, caractérisé en ce que le milieu de corrosion est adsorbé dans l'installation par des surfaces extérieures et intérieures, y compris des surfaces intérieures de pores, et qu'ensuite la température de procédé est produite.
  14. Procédé selon la revendication 13, caractérisé en ce que, avant l'adsorption du milieu de corrosion, une corrosion dosée au moyen de l'addition contrôlée du milieu de corrosion est réalisée à la température de procédé de sorte qu'au moins une partie des pores fermés s'ouvre.
  15. Procédé selon l'une des revendications 1 à 14, caractérisé en ce que l'installation est évacuée ou rincée avec un milieu inerte pour éliminer de l'installation le composé chimique formé à partir du milieu de corrosion et du radiotoxique.
  16. Procédé selon l'une des revendications 1 à 15, caractérisé en ce que le radiotoxique éliminé de l'installation est enrichi.
EP09804242A 2008-12-19 2009-12-09 Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire Not-in-force EP2368254B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE102008063941A DE102008063941A1 (de) 2008-12-19 2008-12-19 Verfahren zur Reduzierung oder zumindest teilweisen Entfernung spezifischer Radiotoxika aus einer kerntechnischen Anlage
PCT/DE2009/001735 WO2010069290A2 (fr) 2008-12-19 2009-12-09 Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire

Publications (2)

Publication Number Publication Date
EP2368254A2 EP2368254A2 (fr) 2011-09-28
EP2368254B1 true EP2368254B1 (fr) 2012-10-03

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EP09804242A Not-in-force EP2368254B1 (fr) 2008-12-19 2009-12-09 Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire

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EP (1) EP2368254B1 (fr)
DE (1) DE102008063941A1 (fr)
WO (1) WO2010069290A2 (fr)

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE102010026936A1 (de) * 2010-07-12 2012-01-12 Forschungszentrum Jülich GmbH Verfahren zur Teildekontamination radioaktiver Abfälle
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 (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2333516C3 (de) * 1973-07-02 1979-05-03 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Dekontaminationsmittel für metallische Oberflächen und Verfahren zum Dekontaminieren unter Verwendung derselben
DE3345782A1 (de) * 1983-12-17 1985-06-27 BBC Aktiengesellschaft Brown, Boveri & Cie., Baden, Aargau Verfahren zur primaerkreis-dekontamination von reaktoren
DE3413868A1 (de) * 1984-04-12 1985-10-17 Kraftwerk Union AG, 4330 Mülheim Verfahren zur chemischen dekontamination von metallischen bauteilen von kernreaktoranlagen
JP3051859B2 (ja) * 1998-10-30 2000-06-12 原電事業株式会社 原子炉で使用された黒鉛の処理方法
UA57884C2 (uk) * 1999-10-14 2003-07-15 Дейвід БРЕДБЕРІ Спосіб обробки радіоактивного графіту
DE102004036631B4 (de) * 2004-07-28 2013-02-21 Forschungszentrum Jülich GmbH Verfahren zur Behandlung einer mit Radiokarbon kontaminierten Keramik, insbesondere Reaktorgraphit

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WO2010069290A3 (fr) 2010-08-26
EP2368254A2 (fr) 2011-09-28
WO2010069290A2 (fr) 2010-06-24
DE102008063941A1 (de) 2010-07-01

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