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WO2006012830A2 - Procede pour traiter une ceramique contaminee par du radiocarbone, en particulier du graphite nucleaire - Google Patents

Procede pour traiter une ceramique contaminee par du radiocarbone, en particulier du graphite nucleaire Download PDF

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Publication number
WO2006012830A2
WO2006012830A2 PCT/DE2005/001222 DE2005001222W WO2006012830A2 WO 2006012830 A2 WO2006012830 A2 WO 2006012830A2 DE 2005001222 W DE2005001222 W DE 2005001222W WO 2006012830 A2 WO2006012830 A2 WO 2006012830A2
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WO
WIPO (PCT)
Prior art keywords
ceramic
radiocarbon
corrosion medium
corrosion
carbon
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.)
Ceased
Application number
PCT/DE2005/001222
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German (de)
English (en)
Other versions
WO2006012830A3 (fr
Inventor
Johannes Fachinger
Tatjana Podruzhina
Werner Von Lensa
Kerstin KÜHN
Reinhard Odoj
Heiner BRÜCHER
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
Priority to EP05766947.5A priority Critical patent/EP1771865B1/fr
Publication of WO2006012830A2 publication Critical patent/WO2006012830A2/fr
Publication of WO2006012830A3 publication Critical patent/WO2006012830A3/fr
Anticipated expiration legal-status Critical
Ceased 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
    • 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 treating a radio-carbon-contaminated ceramic, in particular reactor graphite.
  • Radiocarbon is the radioactive 14 carbon isotope of carbon. It is formed, except in a natural way, by cosmic radiation in neutron radiation fields of nuclear reactors in small amounts as a cleavage product or by activation of the isotope 13 C occurring in 1: 1% in natural carbon with an effective cross section of 0.0009 barn, but vor ⁇ predominantly by activation of nitrogen ( 14 N) in an n, p reaction with a cross section of 1.81 barn.
  • the isotope 17 O with only 0.038% of oxygen present in the air can be converted into radiocarbon via a n, ⁇ reaction with a lower cross-section of 0.235 barn.
  • radiocarbon Because of its long physical half-life of 5,730 years and its good mountability in biological systems due to a substitution of 12 C or 13 C radiocarbon in carbon compounds with high biological half-life is radiocarbon a problematic contamination in radioactive waste represents and requires special safety precautions. On the other hand, it is also a valuable indicator of biological research because it is built into biological systems like natural carbon and can easily be tracked for radioactive decay.
  • Ceramics include: reactor graphite, carbon, SiC, Al 2 O 3 , MgO and Verbundmate ⁇ materials containing ceramics, eg carbon fiber reinforced SiC.
  • MAGNOX reactor CO 2 -cooled reactor type
  • Natural uranium fuel assemblies with Magnox shell Advanced Gas-cooled Reactor (EGR), HTR (High-temperature reactor), RBMK (water-cooled nuclear reactor type Russian)), but also in the thermal columns of research reactors (eg MERLIN, see ATW, Street ⁇ gang 48, Issue 6, June 2003, pages 404-407) , The main part comes mostly from the activation of nitrogen and oxygen. Oxygen and nitrogen are stored z. B. by air access to thermal columns and adsorption. In the case of the thermal decomposition of nitrogen-containing plastics (for example hexamethylenetetramine as binder) in the production of graphites, incorporation into grain boundaries preferably takes place.
  • nitrogen-containing plastics for example hexamethylenetetramine as binder
  • DE 197 37 891 C2 discloses a method for disposing of a radiotoxic contaminated article from reactor graphite or coal rock, in which part of the radiotoxins is removed by heating the article therefrom and fed to a further removal step and at the at least a closed layer at the surface of the article by filling in pores with pyrolytic carbon by means Infiltra ⁇ tion of hydrocarbons above 1000 0 C and / or by chemical reaction with egg ner silicon compound to form silicon carbide in a sealing and / or diffusionshem- mend formed , It is disclosed that the heating takes place in a vacuum or under protective gas, in order to prevent the formation of carbon monoxide and carbon dioxide on heating by reactions with the atmo ⁇ spherical oxygen, which contain the existing radiocarbon and therefore may not escape uncontrolled.
  • This object is achieved in a method of the type mentioned in that in a process temperature range by means of chemical reaction of at least one Korrosi ⁇ onsmediums at least with the radiocarbon at least one volatile reaction gas is formed det, the amount of at least one corrosion medium, the process temperature and / or the duration of the process can be selected such that the chemical reaction takes place essentially only on the surface of the ceramic, including pore surfaces, and within areas close to the surface, and the at least one reaction gas is collected and fed to a separate treatment.
  • the process can be carried out at relatively low temperatures, so that a stronger involvement of the radio-carbon, z. B. is prevented by diffusing near-surface Ra ⁇ diocarbon into the crystal lattice or by a Nachgraphitmaschine.
  • the concentration of the radiocarbon contamination can be considerably reduced by the method. Although it is not possible to remove the entire radiocarbon from the treated ceramic by acting on the surfaces and the areas near the surface. However, even a distance of z. 50%, which are processed by the method achievable measurements could double the usability of waste storage because the (end) storage capacities are coupled to the total cumulative 14 C activity.
  • SectiondekontaminATORs graphite material can be supplied at sufficiently low residual contamination and a complete conversion to CO or CO 2 at higher temperatures of, for example, about 1000 ° C in air.
  • the concentration of the radiocarbon in the collected reaction gases is significantly enriched in comparison to the natural occurrence, which is a good prerequisite for a further use of the radio-carbon as valuable material.
  • the treated ceramic can be corroded on its surface metered so that the inner regions remain as stable as possible.
  • the process according to the invention can also be carried out in such a way that oxygen is used as the corrosion medium.
  • oxygen when used, it reacts with carbon to form carbon monoxide or carbon dioxide, ie volatile carbon compounds.
  • the inventive method can also be carried out so that air is used as an oxygen supplier.
  • air is used as an oxygen supplier.
  • the reaction schieht ge into the aforementioned volatile carbon compounds at temperatures of about 500 0 C. At these temperatures, the Sau ⁇ erstoff far into an existing pore system penetrate to the crystals on the inner O- ber Assembly partially oxidize. At higher temperatures, however, a strong oxidation on the outside of the ceramic to be treated, since the pore diffusion is accelerated less by increasing the temperature than the chemical reaction and thus to a depletion of corrosion oxygen in the interior of the pore system of korrodie ⁇ -generating ceramic Medium is coming.
  • 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 inert inert gases, and the dimensions of the ceramic material to be corroded.
  • the process according to the invention can also be carried out so that water vapor is used as an oxygen supplier. It has proved to be advantageous, an inert gas To saturate at room temperature with water and then heat the water-inert gas mixture to process temperature.
  • the process according to the invention can also be carried out in such a way that hydrogen is used as the corrosion medium.
  • substantially CH 4 is formed as the reaction product with carbon.
  • the inventive method can also be carried out so that the ceramic is in a container, wherein the at least one corrosion medium at a suitable process temperature supplied controlled and the reaction gas is withdrawn.
  • the method according to the invention such that the at least one corrosion medium is adsorbed by the surface of the ceramic, including the pore surfaces, and then the ceramic is brought to process temperature. It may be advantageous to heat the ceramic under vacuum or in an inert gas atmosphere.
  • the extent to which the surfaces are loaded with the corrosion medium can be controlled, for example, by the chosen partial pressure and the loading time. The degree of loading should be chosen so that the amount of corrosion medium present is just sufficient to achieve the desired level of corrosion during heating.
  • the inventive method can also be carried out so that in a further step, the container is evacuated or the ceramic is purged with inert gas to withdraw the reaction gases, and then the process, starting with the adsorbing of at least one corrosion medium on the surface , at least one more timeteur ⁇ is performed.
  • the container is evacuated or the ceramic is purged with inert gas to withdraw the reaction gases, and then the process, starting with the adsorbing of at least one corrosion medium on the surface , at least one more timeteur ⁇ is performed.
  • a batch process with several cycles is given, which, on the one hand, leads to longer treatment times compared to the continuous process, but on the other hand can entail increased proportions of radiocarbon in the reaction gases.
  • the method according to the invention can also be carried out such that, before adsorbing the at least one corrosion medium, metered corrosion is carried out by controlled addition of the at least one corrosion medium at process temperature such that at least a portion of closed pores is opened.
  • the first step in this process primarily serves to open the closed pores, it also already leads to a removal of a portion of the radio-carbon.
  • the opening of the closed pores can, for example, be carried out under a medium of corrosive medium, wherein this treatment step can be carried out at elevated temperatures in a relatively short time, which is just sufficient to open the pores.
  • pore opening can also be carried out with the aid of a previously adsorbed corrosion medium in vacuo or in an inert gas atmosphere.
  • the process according to the invention can also be carried out in such a way that the remaining residual ceramic is recycled after the final removal of the reaction gases, for example as nuclear graphite.
  • the method according to the invention can be carried out in such a way that the radiocarbon contained in the collected reaction gases is enriched. Subsequently, the radiocarbon can be recycled as a valuable material. If from the extracted radiocarbon again a solid, e.g. In the form of graphite, which were ⁇ should be, especially when using steam as an oxygen supplier, a cycle for the corrosion medium be advantageous.
  • the cyclic process might look like this: During the corrosion process, carbon monoxide and hydrogen are formed under appropriate process conditions with the endothermic reaction of graphite with water vapor as reaction products. In the extracted and collected carbon monoxide, a significantly increased proportion of radiocarbon is now present compared to the original ceramic. This proportion can now be further increased by enrichment processes. In a further step, solid carbon and water (steam) can be generated from the carbon monoxide in reaction with the hydrogen. The water can then again serve as a supplier for the corrosion medium oxygen.
  • 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 an enrichment of the radiocarbon.
  • the production of leach-resistant, non-combustible storage containers makes sense. This can e.g. by reaction of the radiocarbon-rich material to carbides, e.g. SiC, or ge ⁇ stone-like carbonates happen.
  • carbides e.g. SiC
  • ge ⁇ stone-like carbonates happen.
  • the corrosion medium should be chosen so that the reaction gases are as directly as possible suitable for the further treatment steps.
  • FIG. 1 shows a diagram of the result of a treatment of one of the AVR reactor (first high-temperature experimental reactor in Anlagenstechnik Anlagenlich, see VD / report 729, AVR 20 years of operation, ISBN 3-18-090720-0, VDI -Verlag, Dusseldorf, 1989)) originating graphite powder.
  • AVR reactor first high-temperature experimental reactor in Anlagenstechnik GmbH, see VD / report 729, AVR 20 years of operation, ISBN 3-18-090720-0, VDI -Verlag, Dusseldorf, 1989
  • oxygen was used as a constituent of water.
  • first argon was saturated with water vapor at room temperature.
  • the graphite powder was heated in the steam-argon atmosphere to 1057 0 C and held at this temperature for 16 hours.
  • FIG. 1 shows the release of the carbon during the treatment period.
  • Curve 1 shows the total mass loss of the graphite powder. This mass loss is expressed in percent by the left scale.
  • Curve 2 represents the percent release of radiocarbon with respect to the original radiocarbon content. Thus, after 16 hours, about 46% of the radiocarbon originally present in the graphite powder is released.
  • Curve 3 shows the ratio between the percent release of carbon monoxide and the release of stable carbon isotopes in percent. As an example, the ratio after about 16 hours of treatment is shown below. As mentioned earlier, about 46% of the radiocarbon is removed. At the same time, the treatment released a little more than 16% of the stable carbon isotopes. The ratio of the percentages 46/16 gives a ratio of about 2.85. The relationship is shown on the right-hand scale of the diagram in FIG. The diagram makes it clear that at the beginning of the
  • the ratio of the yield of radiocarbon is higher than at later time points. This confirms the predominant deposition of the radiocarbon on the surface, including the pore surfaces.
  • graphite powder from the experimental reactor MERLIN was first stored in air so that the surfaces of the powder, including the pore surfaces, could adsorb oxygen. This material was then placed in a pure argon atmosphere, heated to 1057 0 C and held at this temperature for about 13.5 hours.
  • FIG. 2 shows the result of this treatment in a diagram corresponding to FIG. It can be seen that, on the whole, a substantially lower absolute release rate was achieved with respect both to the radiocarbon (curve 5) and also to the stable carbon isotopes (curve 4). However, according to curve 6, the ratio of the percentage release of the radiocarbon to the percentage release of the stable carbon isotopes is higher by more than a factor of 10. Accordingly, the percentage is also the radiocarbon-containing molecules in reaction gases significantly higher than in the treatment under the water-argon atmosphere.
  • the corrosion solely by means of the adsorbed oxygen is particularly suitable when high proportions of radiocarbon are to be achieved in the reaction gases, for example for the recycling of the radiocarbon.

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

Abstract

L'invention concerne un procédé pour traiter une céramique contaminée par du radiocarbone, en particulier du graphite nucléaire, ce procédé consistant à corroder, de manière dosée, la surface de la céramique, y compris la surface des pores de la céramique. Fait surprenant, le radiocarbone se dépose de préférence dans des zones proches de la surface, ce qui va à l'encontre des hypothèses antérieures. Ainsi, il est possible d'effectuer une décontamination partielle efficace qui permet, de réutiliser la matière partiellement décontaminée, par exemple en tant que graphite nucléaire, ou de procéder à un stockage définitif, et/ou d'enrichir le radiocarbone éliminé, dans les gaz de réaction de la corrosion et de le revaloriser.
PCT/DE2005/001222 2004-07-28 2005-07-12 Procede pour traiter une ceramique contaminee par du radiocarbone, en particulier du graphite nucleaire Ceased WO2006012830A2 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
EP05766947.5A EP1771865B1 (fr) 2004-07-28 2005-07-12 Procede pour traiter une ceramique contaminee par du radiocarbone, en particulier du graphite nucleaire

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Application Number Priority Date Filing Date Title
DE200410036631 DE102004036631B4 (de) 2004-07-28 2004-07-28 Verfahren zur Behandlung einer mit Radiokarbon kontaminierten Keramik, insbesondere Reaktorgraphit
DE102004036631.4 2004-07-28

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WO2006012830A2 true WO2006012830A2 (fr) 2006-02-09
WO2006012830A3 WO2006012830A3 (fr) 2006-05-11

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EP (1) EP1771865B1 (fr)
DE (1) DE102004036631B4 (fr)
WO (1) WO2006012830A2 (fr)

Cited By (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010069290A3 (fr) * 2008-12-19 2010-08-26 Forschungszentrum Jülich GmbH Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire
DE102011016273A1 (de) * 2011-04-06 2012-10-11 Forschungszentrum Jülich GmbH Verfahren zur Herstellung von Kohlenstoff- und Graphitwerkstoffen sowie dadurch hergestellte Kohlenstoff- und Graphitwerkstoffe
WO2012136191A1 (fr) * 2011-04-06 2012-10-11 Forschungszentrum Jülich GmbH Procédé de décontamination de radionucléides présents dans des matériaux carbonés et/ou graphitiques irradiés avec des neutrons
DE102013003847B3 (de) * 2013-03-07 2014-09-04 Forschungszentrum Jülich GmbH Fachbereich Patente Verfahren zur Dekontamination von Radionukliden aus neutronenbestrahlten Kohlenstoff- und/ oder Graphitwerkstoffen
RU2546981C1 (ru) * 2013-10-16 2015-04-10 Открытое акционерное общество "Ордена Ленина Научно-исследовательский и конструкторский институт энерготехники им. Н.А. Доллежаля" (ОАО "НИКИЭТ") Способ обработки облученного реакторного графита
RU2603015C1 (ru) * 2015-10-29 2016-11-20 Федеральное государственное автономное образовательное учреждение высшего образования "Национальный исследовательский Томский политехнический университет" Способ очистки облученных графитовых втулок уран-графитового реактора и устройство для его осуществления
RU2660804C1 (ru) * 2017-07-03 2018-07-10 Российская Федерация, от лица которой выступает Государственная корпорация по атомной энергии "Росатом" Способ подготовки графитовых радиоактивных отходов к захоронению

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DE102010026936A1 (de) 2010-07-12 2012-01-12 Forschungszentrum Jülich GmbH Verfahren zur Teildekontamination radioaktiver Abfälle
RU2711292C1 (ru) 2018-11-21 2020-01-16 Акционерное Общество "Российский Концерн По Производству Электрической И Тепловой Энергии На Атомных Станциях" (Ао "Концерн Росэнергоатом") Способ дезактивации элемента конструкции ядерного реактора

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Cited By (8)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2010069290A3 (fr) * 2008-12-19 2010-08-26 Forschungszentrum Jülich GmbH Procédé de réduction ou d'élimination au moins partielle de substances radiotoxiques spécifiques dans une installation nucléaire
DE102011016273A1 (de) * 2011-04-06 2012-10-11 Forschungszentrum Jülich GmbH Verfahren zur Herstellung von Kohlenstoff- und Graphitwerkstoffen sowie dadurch hergestellte Kohlenstoff- und Graphitwerkstoffe
WO2012136191A1 (fr) * 2011-04-06 2012-10-11 Forschungszentrum Jülich GmbH Procédé de décontamination de radionucléides présents dans des matériaux carbonés et/ou graphitiques irradiés avec des neutrons
DE102013003847B3 (de) * 2013-03-07 2014-09-04 Forschungszentrum Jülich GmbH Fachbereich Patente Verfahren zur Dekontamination von Radionukliden aus neutronenbestrahlten Kohlenstoff- und/ oder Graphitwerkstoffen
WO2014135138A2 (fr) 2013-03-07 2014-09-12 Forschungszentrum Jülich GmbH Procédé pour décontaminer des radionucléides provenant de matériaux carbonés et/ou graphitiques irradiés aux neutrons
RU2546981C1 (ru) * 2013-10-16 2015-04-10 Открытое акционерное общество "Ордена Ленина Научно-исследовательский и конструкторский институт энерготехники им. Н.А. Доллежаля" (ОАО "НИКИЭТ") Способ обработки облученного реакторного графита
RU2603015C1 (ru) * 2015-10-29 2016-11-20 Федеральное государственное автономное образовательное учреждение высшего образования "Национальный исследовательский Томский политехнический университет" Способ очистки облученных графитовых втулок уран-графитового реактора и устройство для его осуществления
RU2660804C1 (ru) * 2017-07-03 2018-07-10 Российская Федерация, от лица которой выступает Государственная корпорация по атомной энергии "Росатом" Способ подготовки графитовых радиоактивных отходов к захоронению

Also Published As

Publication number Publication date
WO2006012830A3 (fr) 2006-05-11
DE102004036631A1 (de) 2006-03-23
EP1771865B1 (fr) 2013-07-10
EP1771865A2 (fr) 2007-04-11
DE102004036631B4 (de) 2013-02-21

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