EP2368254A2 - 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

Info

Publication number
EP2368254A2
EP2368254A2 EP09804242A EP09804242A EP2368254A2 EP 2368254 A2 EP2368254 A2 EP 2368254A2 EP 09804242 A EP09804242 A EP 09804242A EP 09804242 A EP09804242 A EP 09804242A EP 2368254 A2 EP2368254 A2 EP 2368254A2
Authority
EP
European Patent Office
Prior art keywords
corrosion medium
radiotoxic
plant
corrosion
chemical compound
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
EP09804242A
Other languages
German (de)
English (en)
Other versions
EP2368254B1 (fr
Inventor
Werner Von Lensa
Johannes Fachinger
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 Jülich
Original Assignee
Forschungszentrum Jülich
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 Jülich filed Critical Forschungszentrum Jülich
Publication of EP2368254A2 publication Critical patent/EP2368254A2/fr
Application granted granted Critical
Publication of EP2368254B1 publication Critical patent/EP2368254B1/fr
Not-in-force legal-status Critical Current
Anticipated expiration legal-status Critical

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
    • 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.
  • the resulting hydrogen and carbon monoxide can form highly explosive gas mixtures if oxygen enters the work zone in an uncontrolled manner. Furthermore, it is disadvantageous that this process has no selective effect on the removal of specific radiotoxic agents and can only be used after completion of the reactor operation.
  • 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.
  • Erflndungsloom at least one corrosion medium is introduced individually or in combination with the equipment, preferably metered, through the flow in the system located at a suitable temperature.
  • the nuclear part of the plant can be heated in particular by nuclear fission or 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 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 may take years and excludes re-commissioning.
  • the chemical reaction used according to the invention finds essentially only at outer and inner surfaces, with which the corrosion medium comes into contact, including inner surfaces of pores, in which the corrosion medium - depending on the temperature profile in the nuclear part and here in particular in the reactor core advantageously in relatively low concentrations - penetrates, instead. This has a double effect:
  • a gas-cooled graphite moderated reactor consists of a large number of graphite blocks, some of which are joined together in the tongue and groove system. These blocks are in particular contaminated with the radiotoxic agent 14 C, which is at least partially removed by the method according to the invention. Each individual block also contributes to the mechanical See stability of the plant. A massive chemical reaction that attacks 14 C is likely to attack 12 C and thus the structure of the reactor core. Conducting the reaction only on outer and inner surfaces prevents the blocks from structurally weakening and collapsing the core structures.
  • a certain amount of 14 C and other radiotoxic agents are bound in the form of fine dusts in the reactor circuit.
  • a large part of the fine dust is converted into gaseous corrosion products and can advantageously also be removed via the cleaning systems of the coolant circuit.
  • This process can be favorably influenced by sudden changes in the coolant velocity, such as by recurring switching on and off of the circulation devices (such as cooling gas blower), since this can cause the dusts to be stirred up and reacted.
  • the circulation devices such as cooling gas blower
  • the remaining graphite in the reactor has only a small residual contamination, which is also stable bound to regular lattice sites.
  • the method becomes a method for in-situ decontamination of the reactor. It is the fundamental goal of any decontamination to separate contaminated material from non-contaminated or only slightly contaminated material, so that the majority of the total contamination in a nem least possible Endlagervolun ⁇ en can be accommodated. If the residual contamination in the plant components is stably bound, this can also be decisive for the fact that plant components can be classified as "low-level waste” instead of "intermediate-level waste” and thus disposed of in a much simpler and cheaper way or even recycled after further treatment ,
  • the inventive method solves most of the existing mobilizable during decommissioning or repository activity from the graphite and also simplifies the handling of the residual contamination in the very large amount of graphite.
  • contaminated graphite falls in a gas-cooled graphite moderated reactor in addition to a large amount of fiber material, with which the hot gas lines are isolated.
  • This material can also advantageously be decontaminated in situ with the method according to the invention.
  • 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 0 C, HTR: 250-950 ° C), there is considerable scope for controlling the reaction.
  • MAGNOX / UNGG gas-cooled graphite-moderated reactors
  • EGR 250-650 0 C
  • HTR 250-950 ° C
  • 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 conversion of 14 C into volatile carbon compounds already occurs at temperatures below about 500 ° C. At these temperatures, the oxygen can penetrate far into an existing pore system to partially oxidize the crystals on the inner surface. At higher temperatures, however, a strong oxidation on the outside of the graphite blocks, since the pore diffusion is accelerated less by increasing the temperature as the chemical reaction and thus to a depletion of the corrosion oxygen in the interior of the pore system of the graphite blocks to be corroded.
  • 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 radiocarbon 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 (Pressure swing, gas centrifuges, etc.) are extended, if not used by the above described exchange of the cooling medium.
  • 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.
  • 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.
  • 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:
  • 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.
  • 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 detachment of the radiotoxicum from external and internal surfaces and leaves the plant components with only a small residual contamination so that they can either be disposed as "low-level waste" near the surface 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 such media support the safe dismantling. This applies in particular if the corrosion medium in the plant is covered 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 corrosion medium can also be injected locally into certain areas of 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 method according to the invention can also be applied to already shut down systems. Any necessary process heat can be provided even in the absence of nuclear fuel elements, for example by the core structures of gas-cooled reactors are heated by the operation of the cooling gas blower or the remaining heat exchangers are supplied for example with secondary steam.
  • 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. The inventive method, however, 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.
  • Figure 1 Release of 14 C and 12 C in the simulated implementation of an embodiment of the method according to the invention.
  • i-graphite irradiated graphite
  • An exemplary 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 shows an example of 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 0 C.
  • the release of 14 C increases much faster than the release of 12 C, since the am 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 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 promotes or accelerates the chemical reaction can be produced by further nuclear fission, by utilizing the residual heat from the decomposition of the fission products after the nuclear fission has been switched off, or by additional 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)

Abstract

L'invention concerne un procédé d'élimination au moins partielle d'une substance radiotoxique dans une installation nucléaire. En fonctionnement, cette installation est traversée par au moins un agent de fonctionnement qui est introduit dans l'installation par au moins une conduite d'entrée et qui est évacué de l'installation par au moins une conduite de retour, l'agent de fonctionnement pouvant notamment être un liquide de refroidissement ou un gaz de refroidissement. L'invention est caractérisée en ce qu'au moins un agent corrosif, seul ou combiné à l'agent de fonctionnement, est introduit dans l'installation par la conduite d'entrée. Ainsi, l'agent corrosif entre en contact, dans l'installation, avec la substance radiotoxique qu'il transforme au moins partiellement en un composé chimique par une réaction chimique. Cette réaction chimique a lieu sensiblement seulement sur les surfaces internes et externes avec lesquelles l'agent corrosif entre en contact, y compris sur les surfaces internes de pores dans lesquelles l'agent corrosif pénètre. Le composé chimique est au moins partiellement évacué de l'installation par la conduite de retour.
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 true EP2368254A2 (fr) 2011-09-28
EP2368254B1 EP2368254B1 (fr) 2012-10-03

Family

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Family Applications (1)

Application Number Title Priority Date Filing Date
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

Country Status (3)

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

Families Citing this family (3)

* 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
CN121148769B (zh) * 2025-09-08 2026-07-28 中国核电工程有限公司 一种自动调料系统、方法、装置、设备及介质

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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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Also Published As

Publication number Publication date
WO2010069290A3 (fr) 2010-08-26
EP2368254B1 (fr) 2012-10-03
DE102008063941A1 (de) 2010-07-01
WO2010069290A2 (fr) 2010-06-24

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