EP0082267B1 - Moulded body for encapsulating radioactive wastes, and process for manufacturing this body - Google Patents
Moulded body for encapsulating radioactive wastes, and process for manufacturing this body Download PDFInfo
- Publication number
- EP0082267B1 EP0082267B1 EP82109825A EP82109825A EP0082267B1 EP 0082267 B1 EP0082267 B1 EP 0082267B1 EP 82109825 A EP82109825 A EP 82109825A EP 82109825 A EP82109825 A EP 82109825A EP 0082267 B1 EP0082267 B1 EP 0082267B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- graphite
- nickel
- waste
- radioactive
- manufacturing
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Expired
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
- G21F9/34—Disposal of solid waste
- G21F9/36—Disposal of solid waste by packaging; by baling
Definitions
- the invention relates to a shaped body made of graphite with nickel sulfide as a binder for the safe long-term incorporation of radioactive and toxic waste and a method for producing such shaped bodies.
- Spent fuel elements from nuclear reactors have to be disposed of for a final disposal after a certain period of time.
- Two ways have been investigated worldwide, namely the reprocessing of the fuel elements with the return of the fuels to the fuel element production as well as the separation and final storage of the fission products (highly active waste) and alternatively the direct final storage of the spent elements. 1
- highly active waste is generated that must be safely stored in suitable geological formations for 1000 years and more.
- Other, highly radioactive and highly toxic waste must also be kept away from the biosphere.
- Nickel sulfide (DE-A No. 2917437) is preferably used as the binder.
- Such moldings are very dense and have good resistance to corrosion and leaching, in particular to salt solutions, which in some cases has not yet proven to be optimal.
- the nickel sulfide is predominantly in the form of Ni 3 S 2 . At least 80% of the introduced nickel sulfide is preferably present as defined Ni 3 S 2 in the graphite matrix.
- Molded graphite bodies containing radioactive or toxic waste and containing Ni 3 S 2 as binders have an extremely high resistance to corrosion and leaching out of salt solutions.
- the shaped articles contain, in addition to the embedded waste, 25 to 90% by weight of nickel sulfide (Ni 3 S 2 ), in particular 45 to 60% by weight of nickel sulfide (Ni s S z ), the rest of the graphite.
- Ni 3 S 2 nickel sulfide
- Ni s S z nickel sulfide
- These moldings are produced by pressing a mixture of radioactive and / or toxic waste, graphite, sulfur and nickel powder at temperatures above 100 ° C., 35 to 45 g of sulfur powder being added to 100 g of nickel powder and pressing at temperatures between 400 and 500 ° C because the sulfur can sublimate from the molding compound to a small extent, depending on the process.
- the graphite-Ni 3 S 2 matrix Because of the extremely high long-term stability of the graphite-Ni 3 S 2 matrix, it can also be used to integrate long-life a-lamps, such as plutonium.
Description
Die Erfindung betrifft einen Formkörper aus Graphit mit Nickelsulfid als Bindemittel zur sicheren Langzeiteinbindung von radioaktiven und toxischen Abfällen und ein Verfahren zur Herstellung solcher Formkörper.The invention relates to a shaped body made of graphite with nickel sulfide as a binder for the safe long-term incorporation of radioactive and toxic waste and a method for producing such shaped bodies.
Abgebrannte Brennelemente aus Kernreaktoren müssen nach einer gewissen Zeit der Zwischenlagerung einer Endbeseitigung zugeführt werden. Weltweit wurden dazu zwei Wege untersucht, nämlich die Wiederaufarbeitung der Brennelemente mit Rückführung der Brennstoffe in die Brennelementfertigung sowie Abtrennung und Endlagerung der Spaltprodukte (hochaktiver Abfall) und alternativ die direkte Endlagerung der abgebrannten Elemente. 1 jedem Fall entsteht hochaktiver Abfall, der 1000 Jahre und mehr sicher in geeignete geologische Formationen eingelagert werden muss. Auch sonstiger, hochradioaktiver und hochtoxischer Abfall muss sicher von der Biosphäre ferngehalten werden.Spent fuel elements from nuclear reactors have to be disposed of for a final disposal after a certain period of time. Two ways have been investigated worldwide, namely the reprocessing of the fuel elements with the return of the fuels to the fuel element production as well as the separation and final storage of the fission products (highly active waste) and alternatively the direct final storage of the spent elements. 1 In every case, highly active waste is generated that must be safely stored in suitable geological formations for 1000 years and more. Other, highly radioactive and highly toxic waste must also be kept away from the biosphere.
Zum sicheren Langzeiteinschluss solcher radioaktiver und toxischer Abfälle sind zahlreiche Behältertypen vorgeschlagen worden, die die geforderten Bedingungen, wie dichter Einschluss bei den auftretenden Drücken und Temperaturen oder Korrosionsfestigkeit gegen Salzlaugen, gut erfüllen. Als Behältermaterial werden vielerlei metallische und nichtmetallische Werkstoffe verwendet.For the safe long-term containment of such radioactive and toxic waste, numerous types of containers have been proposed which well meet the required conditions, such as tight containment at the pressures and temperatures that occur or corrosion resistance against brine. Various metallic and non-metallic materials are used as container material.
Da Graphit eine hervorragende Korrosionsbeständigkeit besitzt, ist vorgeschlagen worden (DE-A Nr. 2942092), Behälter mit einer Korrosionsschutzschicht aus Graphit zu versehen. Da Graphitformkörper der für die Aufnahme eines Brennelementes notwendigen Abmessungen weder gas- noch flüssigkeitsdicht herzustellen sind, ist eine anschliessende Beschichtung mit Pyrokohlenstoff oder Siliciumkarbid vorgesehen. Nach dem Einfüllen des Brennelements soll der beschichtete Behälter mit einem gleichermassen beschichteten Deckel gas- und flüssigkeitsdicht verschlossen werden. Hierbei sollen Graphitdichtungen bzw. geeignete Klebemittel zum Einsatz kommen. Ein wesentlicher Nachteil dieses Behälterkonzepts ist der ausserordentlich hohe technische Aufwand, der für die Herstellung und Beschichtung von Behältern mit grossen Abmessungen notwendig ist. Ausserdem lassen sich solche grossen Formkörper nicht in den geforderten Qualitätsansprüchen beschichten.Since graphite has excellent corrosion resistance, it has been proposed (DE-A No. 2942092) to provide containers with a corrosion protection layer made of graphite. Since graphite moldings of the dimensions required for accommodating a fuel assembly cannot be made gas-tight or liquid-tight, a subsequent coating with pyrocarbon or silicon carbide is provided. After the fuel element has been filled in, the coated container is to be closed in a gastight and liquid-tight manner with an equally coated lid. Here graphite seals or suitable adhesives should be used. A major disadvantage of this container concept is the extraordinarily high technical effort that is necessary for the production and coating of containers with large dimensions. In addition, such large moldings cannot be coated in the required quality requirements.
Es ist auch bekannt, zur Einbindung von radioaktiven und toxischen Abfällen Formkörper aus einer Kohlenstoffmatrix herzustellen, indem man Graphitpulver mit einem Bindemittel presst. Als Bindemittel verwendet man hierbei vorzugsweise Nickelsulfid (DE-A Nr. 2917437). Solche Formkörper sind sehr dicht und besitzen eine gute Korrosions- und Auslaugebeständigkeit, insbesondere gegenüber Salzlösungen, die sich allerdings in manchen Fällen als noch nicht optimal erwies.It is also known to produce molded articles from a carbon matrix for the incorporation of radioactive and toxic waste by pressing graphite powder with a binder. Nickel sulfide (DE-A No. 2917437) is preferably used as the binder. Such moldings are very dense and have good resistance to corrosion and leaching, in particular to salt solutions, which in some cases has not yet proven to be optimal.
Es war daher Aufgabe der vorliegenden Erfindung, einen Formkörper aus Graphit mit Nickelsulfid als Bindemittel zur sicheren Langzeiteinbindung von radioaktiven und toxischen Abfällen zu schaffen, der eine möglichst hohe Korrosions- und Auslaugebeständigkeit aufweist.It was therefore an object of the present invention to provide a shaped body made of graphite with nickel sulfide as a binder for the safe long-term incorporation of radioactive and toxic waste, which has the highest possible resistance to corrosion and leaching.
Diese Aufgabe wurde erfindungsgemäss dadurch gelöst, dass das Nickelsulfid überwiegend als Ni3S2 vorliegt. Vorzugsweise liegen mindestens 80% des eingebrachten Nickelsulfids als definiertes Ni3S2 in der Graphitmatrix vor.This object was achieved according to the invention in that the nickel sulfide is predominantly in the form of Ni 3 S 2 . At least 80% of the introduced nickel sulfide is preferably present as defined Ni 3 S 2 in the graphite matrix.
Mit radioaktiven oder toxischen Abfällen versetzte Graphitformkörper, die als Bindemittel Ni3S2 enthalten, besitzen eine extrem hohe Korrosions- und Auslaugebeständigkeit gegenüber Salzlösungen.Molded graphite bodies containing radioactive or toxic waste and containing Ni 3 S 2 as binders have an extremely high resistance to corrosion and leaching out of salt solutions.
Als günstig hat es sich herausgestellt, wenn die Formkörper neben den eingebetteten Abfällen 25 bis 90 Gew.-% Nickelsulfid (Ni3S2), insbesondere 45 bis 60 Gew.-% Nickelsulfid (NisSz), Rest Graphit enthalten. Die Sicherheit der Einbindung von Abfällen gegen chemisches oder mechanisches Herauslösen lässt sich weiterhin verbessern, wenn man die Abfälle in einem Kern einbettet, der von einer abfallfreien Schale aus dem gleichen Material umgeben ist.It has proven to be advantageous if the shaped articles contain, in addition to the embedded waste, 25 to 90% by weight of nickel sulfide (Ni 3 S 2 ), in particular 45 to 60% by weight of nickel sulfide (Ni s S z ), the rest of the graphite. The security of the integration of waste against chemical or mechanical extraction can be further improved if the waste is embedded in a core which is surrounded by a waste-free shell made of the same material.
Die Herstellung dieser Formkörper erfolgt durch Pressen eines Gemisches aus radioaktiven und/ oder toxischen Abfällen, Graphit-, Schwefel- und Nickelpulver bei Temperaturen oberhalb 100° C, wobei auf 100 g Nickelpulver 35 bis 45 g Schwefelpulver zugesetzt werden und das Pressen bei Temperaturen zwischen 400 und 500° C erfolgt, da der Schwefel je nach Verfahrensführung zu einem geringen Teil aus der Pressmasse absublimieren kann.These moldings are produced by pressing a mixture of radioactive and / or toxic waste, graphite, sulfur and nickel powder at temperatures above 100 ° C., 35 to 45 g of sulfur powder being added to 100 g of nickel powder and pressing at temperatures between 400 and 500 ° C because the sulfur can sublimate from the molding compound to a small extent, depending on the process.
Wegen der extrem hohen Langzeitbeständigkeit der Graphit-Ni3S2-Matrix kann diese auch zum Einbinden langlebiger a-Strahler, wie beispielsweise Plutonium, verwendet werden.Because of the extremely high long-term stability of the graphite-Ni 3 S 2 matrix, it can also be used to integrate long-life a-lamps, such as plutonium.
Folgendes Beispiel soll die Erfindung näher erläutern:
- Als Ausgangspulver wurde eine Mischung aus 43,7 Gew.-% Feinpudernaturgraphit, 15 Gew.-% feingemahlenem Schwefel und 41,3 Gew.-% Nikkelmetallpulver durch Trockenmischen hergestellt. In diese Mischung wurden aktive Abfälle eingebettet.
- A mixture of 43.7% by weight of fine powder natural graphite, 15% by weight of finely ground sulfur and 41.3% by weight of nickel metal powder was prepared as the starting powder by dry mixing. Active waste was embedded in this mixture.
Der fertiggepresste Formkörper hatte folgende Eigenschaften:
- Matrixdichte: 3,36 g/cm3
- Dichte: 97% der theoretischen Dichte
- Wärmeleitfähigkeit: 0,8 W/cm - ° K
- Linear thermischer Ausdehnungskoeffizient: 9,2µm/m·°K
- Druckfestigkeit: 107 MN/m2
- Matrix density: 3.36 g / cm 3
- Density: 97% of the theoretical density
- Thermal conductivity: 0.8 W / cm - ° K
- Linear coefficient of thermal expansion: 9.2µm / m · ° K
- Compressive strength: 107 MN / m 2
Die Auslaugebeständigkeit in Salzlösungen war sehr gut.The resistance to leaching in salt solutions was very good.
Claims (5)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE3144764 | 1981-11-11 | ||
DE19813144764 DE3144764A1 (en) | 1981-11-11 | 1981-11-11 | MOLDED BODY FOR INCLUDING RADIOACTIVE WASTE AND METHOD FOR THE PRODUCTION THEREOF (II) |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0082267A1 EP0082267A1 (en) | 1983-06-29 |
EP0082267B1 true EP0082267B1 (en) | 1985-04-10 |
Family
ID=6146116
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP82109825A Expired EP0082267B1 (en) | 1981-11-11 | 1982-10-23 | Moulded body for encapsulating radioactive wastes, and process for manufacturing this body |
Country Status (8)
Country | Link |
---|---|
US (1) | US4560502A (en) |
EP (1) | EP0082267B1 (en) |
JP (1) | JPS5887500A (en) |
BR (1) | BR8206479A (en) |
CA (1) | CA1170824A (en) |
DE (2) | DE3144764A1 (en) |
ES (1) | ES8402672A1 (en) |
FI (1) | FI74835C (en) |
Families Citing this family (8)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
AT385435B (en) * | 1986-03-07 | 1988-03-25 | Oesterr Forsch Seibersdorf | METHOD AND DEVICE FOR EMBEDDING AND, IF NECESSARY, REACTIVATING, IN PARTICULAR, TOXIC AND / OR RADIOACTIVE SUBSTANCES OR. DISEASE |
US5360632A (en) * | 1993-08-10 | 1994-11-01 | Phillips Petroleum Company | Reduced leaching of arsenic and/or mercury from solid wastes |
GB0415335D0 (en) * | 2004-07-08 | 2004-08-11 | British Nuclear Fuels Plc | Method for the handling and minimisation of waste |
EA021732B1 (en) | 2008-11-10 | 2015-08-31 | Алд Вакуум Текнолоджиз Гмбх | Matrix material composed of graphite and inorganic binders and suitable for final storage of radioactive waste, method for the manufacture thereof, and processing and use thereof |
US8502009B2 (en) | 2008-11-26 | 2013-08-06 | Ald Vacuum Technologies Gmbh | Matrix material comprising graphite and an inorganic binder suited for final disposal of radioactive waste, a process for producing the same and its processing and use |
DE102012112643A1 (en) | 2012-12-19 | 2014-06-26 | Ald Vacuum Technologies Gmbh | Graphite matrix, useful for the preparation of a molded body to store radioactive waste, comprises graphite and a metallic binder |
DE102012112642A1 (en) | 2012-12-19 | 2014-06-26 | Ald Vacuum Technologies Gmbh | Graphite matrix, useful for manufacturing a molded body to store radioactive waste, comprises graphite and glass ceramic |
DE102012112648B4 (en) | 2012-12-19 | 2016-08-04 | Ald Vacuum Technologies Gmbh | Graphite matrix with crystalline binder |
Family Cites Families (15)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US2990352A (en) * | 1950-02-21 | 1961-06-27 | Finniston Harold Montague | Metal sheathed bodies |
US2969294A (en) * | 1954-03-18 | 1961-01-24 | James J Shyne | Method of impregnating uranium in graphite |
GB1051776A (en) * | 1963-10-17 | |||
US3361638A (en) * | 1967-04-07 | 1968-01-02 | Atomic Energy Commission Usa | Pyrolytic graphite and nuclear fuel particles coated therewith |
US3753854A (en) * | 1969-07-04 | 1973-08-21 | Nukem Gmbh | Production of a fuel carbide with a jacket of fuel nitride,sulfide orphosphide |
US3866043A (en) * | 1970-04-20 | 1975-02-11 | Central Electr Generat Board | Coated particle fuel for nuclear reactors and to the manufacture of such fuel |
DE2362088A1 (en) * | 1973-12-14 | 1975-06-26 | Hobeg Hochtemperaturreaktor | GRAPHITE BALL BURNER FOR HIGH-TEMPERATURE REACTORS AND PROCESS FOR ITS PROCESSING AFTER RADIATION |
US4134941A (en) * | 1973-12-14 | 1979-01-16 | Hobeg Hochtemperaturreaktor-Brennelement Gmbh | Spherical fuel elements made of graphite for temperature reactors and process for reworking it after the irradiation |
GB1468233A (en) * | 1974-02-08 | 1977-03-23 | Atomic Energy Authority Uk | Preparation for storage of fission products |
SU571143A1 (en) * | 1976-03-24 | 1980-01-25 | Предприятие П/Я Р-6575 | Method of manufacturing matrix for radioactive sources |
DE2654536C2 (en) * | 1976-12-02 | 1978-10-19 | Hobeg Hochtemperaturreaktor-Brennelement Gmbh, 6450 Hanau | Process for the production of spherical fuel elements for high-temperature reactors |
US4257912A (en) * | 1978-06-12 | 1981-03-24 | Westinghouse Electric Corp. | Concrete encapsulation for spent nuclear fuel storage |
DE2917437C2 (en) * | 1979-04-28 | 1983-11-17 | Nukem Gmbh, 6450 Hanau | Procedure for incorporating radioactive and toxic waste |
DE2942092C2 (en) * | 1979-10-18 | 1985-01-17 | Steag Kernenergie Gmbh, 4300 Essen | Final storage containers for radioactive waste, in particular irradiated nuclear reactor fuel elements |
DE3103557A1 (en) * | 1981-02-03 | 1982-12-09 | Deutsche Gesellschaft für Wiederaufarbeitung von Kernbrennstoffen mbH, 3000 Hannover | "TRANSPORT AND STORAGE CONTAINERS FOR RADIOACTIVE WASTE" |
-
1981
- 1981-11-11 DE DE19813144764 patent/DE3144764A1/en not_active Ceased
-
1982
- 1982-09-29 FI FI823334A patent/FI74835C/en not_active IP Right Cessation
- 1982-10-23 EP EP82109825A patent/EP0082267B1/en not_active Expired
- 1982-10-23 DE DE8282109825T patent/DE3263020D1/en not_active Expired
- 1982-11-09 BR BR8206479A patent/BR8206479A/en unknown
- 1982-11-09 US US06/440,344 patent/US4560502A/en not_active Expired - Fee Related
- 1982-11-09 CA CA000415145A patent/CA1170824A/en not_active Expired
- 1982-11-09 JP JP57195398A patent/JPS5887500A/en active Pending
- 1982-11-10 ES ES517239A patent/ES8402672A1/en not_active Expired
Also Published As
Publication number | Publication date |
---|---|
DE3144764A1 (en) | 1983-05-26 |
BR8206479A (en) | 1983-09-27 |
ES517239A0 (en) | 1984-02-01 |
JPS5887500A (en) | 1983-05-25 |
CA1170824A (en) | 1984-07-17 |
FI74835B (en) | 1987-11-30 |
EP0082267A1 (en) | 1983-06-29 |
ES8402672A1 (en) | 1984-02-01 |
FI823334L (en) | 1983-05-12 |
DE3263020D1 (en) | 1985-05-15 |
FI74835C (en) | 1988-03-10 |
US4560502A (en) | 1985-12-24 |
FI823334A0 (en) | 1982-09-29 |
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