EP0383153B1 - Device for containers with radioactive waste for the reduction of internal pressure caused by the formation of hydrogen - Google Patents
Device for containers with radioactive waste for the reduction of internal pressure caused by the formation of hydrogen Download PDFInfo
- Publication number
- EP0383153B1 EP0383153B1 EP90102291A EP90102291A EP0383153B1 EP 0383153 B1 EP0383153 B1 EP 0383153B1 EP 90102291 A EP90102291 A EP 90102291A EP 90102291 A EP90102291 A EP 90102291A EP 0383153 B1 EP0383153 B1 EP 0383153B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- container
- hydrogen
- catalyst
- containers
- sintered metal
- 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 - Lifetime
Links
Images
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
- G21F5/00—Transportable or portable shielded containers
- G21F5/06—Details of, or accessories to, the containers
- G21F5/12—Closures for containers; Sealing arrangements
-
- 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
- G21F5/00—Transportable or portable shielded containers
Definitions
- the present invention relates to a device on containers with radioactive waste for reducing the internal pressure due to hydrogen generated in the waste and for reducing the release of hydrogen from the container.
- the formation of gases - in particular hydrogen - is possible on the one hand due to the reactions of metallic components with water, as well as through the formation of radiolysis gases from cement / bitumen matrix materials.
- the first formation mechanism is particularly important in the case of high-pressure compacted mixed waste. For intermediate and final storage, the formation / release rates per container and time are limited in order to be able to declare a container as suitable for final storage.
- a transport container for radioactive liquids is known from DD-A-34 878, which has a catalyst arrangement for recombining the decomposition products.
- the catalyst arrangement is arranged in the interior of the container below the lid.
- the object of the present invention on the one hand, to reduce the hydrogen pressure in the containers or containers or reduce it to zero, but at the same time to drastically reduce the hydrogen release rate.
- the boundary condition for this task is to change the state of the conditioning and container technology as little as possible, i.e. to make as much use as possible of the technical conditions of final storage.
- the present invention proposes on a device of the type described in the introduction that a catalyst for the oxidation of hydrogen with oxygen from the air to water at storage temperature at a predetermined throughput rate from the container interior into a passage opening in the wall of the container or its cover is introduced outside.
- a catalyst for the oxidation of hydrogen with oxygen from the air to water at storage temperature at a predetermined throughput rate from the container interior into a passage opening in the wall of the container or its cover is introduced outside.
- the device consists essentially of a cup-shaped pot or container 1, which is inserted into an opening 2 of the container wall, the lid 3 of a repository barrel for radioactive waste.
- a threaded ring 4 is expediently welded to the opening 2, into which the pot 1 is screwed from the outside by means of its external thread 5.
- the surface between the pot 1 and the lid 3 is sealed by the seal 6 in between.
- the interior of the pot 1, in which the catalyst or a catalyst pack 7 is inserted, has a connection opening 8 to the barrel interior 9, in which a gas-permeable sintered metal candle 10 is inserted.
- the catalyst 7 is covered by a wire mesh, a water vapor-permeable plate 11 or a sintered metal cover.
- This construction now allows gases to escape from the container or from the waste container shown.
- the hydrogen formed in the container is now passed through the opening 8 and the sintered metal candle 10 over the catalyst 7, on which the hydrogen is oxidized to water with the oxygen of the outside air at ambient temperature.
- Systems such as noble metals on an internal support, e.g. Palladium on alumina use.
- a palladium catalyst with 0.5 percent by weight palladium on an Al2O3 support matrix (catalyst E 221 P / D-0.5% PD) has proven to be suitable.
- the oxidation product of the hydrogen i.e. water
- the catalyst in conjunction with the oxygen present in the air in any case avoids the addition of expensive oxidizing agents which, moreover, can easily be consumed by reaction with other components and would therefore no longer be available for H2 oxidation.
- the new device can be easily integrated into existing or existing container and barrel systems, which is particularly favored by its compact design.
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Catalysts (AREA)
- Processing Of Solid Wastes (AREA)
- Pressure Vessels And Lids Thereof (AREA)
Description
Die vorliegende Erfindung betrifft eine Vorrichtung an Behältern mit radioaktiven Abfällen zur Reduktion des Innendruckes durch in den Abfällen entstehenden Wasserstoff und zur Reduktion der Wasserstofffreisetzung aus dem Behälter.The present invention relates to a device on containers with radioactive waste for reducing the internal pressure due to hydrogen generated in the waste and for reducing the release of hydrogen from the container.
Bei einer großen Anzahl schwach- und mittelradioaktiver Abfallgebinde ist prinzipiell die Bildung von Gasen - insbesondere Wasserstoff - einerseits aufgrund der Reaktionen metallischer Komponenten mit Wasser, als auch durch die Bildung von Radiolysegasen aus Zement/Bitumenmatrixmaterialien möglich. Der erste Bildungsmechanismus ist insbesondere bei hochdruckkompaktierten Mischabfällen wichtig. Für die Zwischen- und Endlagerung sind die Bildungs-/Freisetzungsraten pro Behälter und Zeit limitiert um ein Gebinde als endlagerfähig deklarieren zu können.With a large number of low- and medium-level radioactive waste containers, the formation of gases - in particular hydrogen - is possible on the one hand due to the reactions of metallic components with water, as well as through the formation of radiolysis gases from cement / bitumen matrix materials. The first formation mechanism is particularly important in the case of high-pressure compacted mixed waste. For intermediate and final storage, the formation / release rates per container and time are limited in order to be able to declare a container as suitable for final storage.
Bisher bekannte Problemlösungen sind die Bregrenzung der spezifischen Aktivität, bzw. bei den kompaktierten Mischabfällen wird eine sorgfältige Sortierung der Rohabfälle, bzw. sogar eine langandauernde, und damit sehr kostenaufwendige Vakuumtrocknung vorgeschlagen.Previously known problem solutions are the limitation of the specific activity, or in the case of the compacted mixed waste, a careful sorting of the raw waste or even a long-lasting, and therefore very costly, vacuum drying is proposed.
Aus DD-A-34 878 ist ein Transportbehälter für radioaktive Flüssigkeiten bekannt, der eine Katalysatoranordnung zur Rekombination der Zersetzungsprodukte besitzt. Die Katalysatoranordnung ist dabei im Innenraum des Behälters unterhalb des Deckels angeordnet.A transport container for radioactive liquids is known from DD-A-34 878, which has a catalyst arrangement for recombining the decomposition products. The catalyst arrangement is arranged in the interior of the container below the lid.
Eine perfekte Sortierung der in die Behälter einzubringenden Abfälle, die zu einer vollständigen Vermeidung von Wasser führen soll, ist technisch nicht machbar, d.h. ein Feuchtigkeitsausschluß ist grundsätzlich nicht gewährleistet. Daher ist die Reaktion von vielen relevanten Metallen, wie z.B. Eisenbasislegierungen mit Wasser unter allen hier vorkommenden Temperatur- und Druckbedingungen thermodynamisch möglich: Z.B. - die sogen. Schikorr-Reaktion
3Fe + 4H₂O = Fe₃O₄ + 4H₂
Eine Trocknung des Behälterinhaltes z.B. eine Vakuumtrocknung wäre für hohe Durchsätze wegen der langen Trocknungszeiten von mehreren Tagen sehr kostspielig, da dafür sehr teure Anlagen Kapazität benötigt würde.A perfect sorting of the waste to be brought into the container, which should lead to a complete avoidance of water, is technically not feasible, ie a moisture exclusion is fundamentally not guaranteed. The reaction of many relevant metals, such as iron-based alloys with water, is therefore thermodynamically possible under all the temperature and pressure conditions that occur here: Eg - the so-called. Schikorr reaction
3Fe + 4H₂O = Fe₃O₄ + 4H₂
Drying the contents of the container, for example vacuum drying, would be very expensive for high throughputs because of the long drying times of several days, since very expensive systems would need capacity.
Aufgabe der vorliegenden Erfindung ist es nun, zum einen den durch Wasserstoff entstehenden Überdruck in den Behältern bzw. Gebinden zu reduzieren bzw. auf Null zurückzuführen und dabei aber jedoch die Wasserstofffreisetzungsrate gleichzeitig drastisch zu reduzieren. Randbedingung für diese Aufgabenstellung ist jedoch den Stand der Konditionierungs- und Behältertechnik möglichst wenig zu verändern, d.h. von den technischen Begebenheiten der Endlagerung möglichst weitgehenst Gebrauch zu machen.It is the object of the present invention, on the one hand, to reduce the hydrogen pressure in the containers or containers or reduce it to zero, but at the same time to drastically reduce the hydrogen release rate. However, the boundary condition for this task is to change the state of the conditioning and container technology as little as possible, i.e. to make as much use as possible of the technical conditions of final storage.
Zur Lösung dieser Aufgabe schlägt nun die vorligende Erfindung an einer Vorrichtung der eingangsbeschriebenen Art vor, daß in eine Durchlaßöffnung der Wandung des Behälters oder seines Deckels ein Katalysator zur Oxidation von Wasserstoff mit Sauerstoff aus der Luft zu Wasser bei Lagertemperatur mit einer vorbestimmten Durchsatzrate vom Behälterinnenraum nach außen eingebracht ist. Eine besonders vorteilhafte Ausbildung dieser Katalysatoranordnung ist aus den Merkmalen zu entnehmen, die in den Merkmalen der Patentansprüche 2 und 3 angegeben sind.To achieve this object, the present invention proposes on a device of the type described in the introduction that a catalyst for the oxidation of hydrogen with oxygen from the air to water at storage temperature at a predetermined throughput rate from the container interior into a passage opening in the wall of the container or its cover is introduced outside. A particularly advantageous embodiment of this catalytic converter arrangement can be gathered from the features specified in the features of
Weitere Einzelheiten der vorligenden Erfindung werden im folgenden anhand der Figur näher erläutert:
Gemäß der Figur besteht die Vorrichtung im wesentlichen aus einem napfförmigen Topf bzw. Behälter 1, der in eine Öffnung 2 der Behälterwandung, dem Deckel 3 eines Endlagerfasses für radioaktive Abfälle eingesetzt ist. Zweckmäßigerweise ist dazu an die Öffnung 2 von innen her ein Gewindering 4 angeschweißt, in den der Topf 1 von außen her mittels seines Außengewindes 5 eingeschraubt ist. Die Abdichtung der Fläche zwischen Topf 1 und Deckel 3 erfolgt durch die dazwischenliegende Dichtung 6.Further details of the present invention are explained in more detail below with reference to the figure:
According to the figure, the device consists essentially of a cup-shaped pot or container 1, which is inserted into an
Der Innenraum des Topfes 1, in den der Katalysator bzw. eine Katalysatorpackung 7 eingesetzt ist, weist eine Verbindungsöffnung 8 zum Faßinnenraum 9 auf, in welche eine gasdurchlässige Sintermetallkerze 10 eingesetzt ist. Zu dem Außenraum 12 hin ist der Katalysator 7 durch ein Drahtnetz, eine wasserdampfdurchlässige Platte 11 oder einen Sintermetalldeckel gedeckt.The interior of the pot 1, in which the catalyst or a catalyst pack 7 is inserted, has a connection opening 8 to the
Diese Konstruktion ermöglicht nun das Entweichen von Gasen aus dem Behälter bzw. aus dem dargestellten Abfallfaß. Der im Behälter gebildete Wasserstoff wird nun durch die Öffnung 8 und die Sintermetallkerze 10 über den Katalysator 7 geleitet, an welchem der Wasserstoff mit dem Sauerstoff der Außenluft bei Umgebungstemperatur zu Wasser oxidiert wird. Verwendung als Katalysator finden Systeme wie Edelmetalle auf inentem Träger, z.B. Palladium auf Aluminiumoxyd Verwendung. Bei Versuchen hat sich dabei ein Palladiumkatalysator mit 0,5 Gewichtsprozent Palladium auf einer Al₂O₃-Trägermatrix (Katalysator E 221 P/D-0,5 % PD) als geeignet erwiesen.This construction now allows gases to escape from the container or from the waste container shown. The hydrogen formed in the container is now passed through the
Durch die Oxidation außerhalb des Behälters wird nun das Oxidationsprodukt des Wasserstoffs d.h Wasser, von einer erneuten Reaktion ausgeschlossen. Der Katalysator in Verbindung mit dem ohnehin vorhandenen Sauerstoff in der Luft vermeidet die Zugabe von teuren Oxidationsmitteln die sich im übrigen leicht durch Reaktion mit anderen Komponenten verbrauchen können und damit nicht mehr für die H₂-Oxidation verfügbar wären.The oxidation product of the hydrogen, i.e. water, is now excluded from a renewed reaction by the oxidation outside the container. The catalyst in conjunction with the oxygen present in the air in any case avoids the addition of expensive oxidizing agents which, moreover, can easily be consumed by reaction with other components and would therefore no longer be available for H₂ oxidation.
Die neue Vorrichtung kann leicht in bestehende bzw. vorhandene Container- und Faßsysteme integriert werden, was insbesondere durch ihre kompakte Bauweise begünstigt wird.The new device can be easily integrated into existing or existing container and barrel systems, which is particularly favored by its compact design.
- 11
- Topfpot
- 22nd
- Öffnungopening
- 33rd
- FaßdeckelDrum lid
- 44th
- GewinderingThreaded ring
- 55
- AußengewindeExternal thread
- 66
- Dichtungpoetry
- 77
- KatalysatorpackungCatalyst pack
- 88th
- VerbindungsöffnungConnection opening
- 99
- FaßinnenraumBarrel interior
- 1010th
- SintermetallkerzeSintered metal candle
- 1111
- durchlässige Plattepermeable plate
- 1212th
- AußenraumOutside space
Claims (3)
- Apparatus for containers (1) containing radioactive waste and having a discharge aperture (8) for reducing the internal pressure caused by hydrogen produced in the waste and for reducing the release of hydrogen from the container, characterized in that a catalyst (7) is applied to the wall of the container or its cover above the discharge aperture (8) externally of the container interior in order to oxidise hydrogen with oxygen to form water at storage temperature, the discharge aperture itself being sealed in a gas-permeable manner.
- Apparatus according to claim 1, characterized by the following features:a) the catalyst pack (7) sits in a cup-shaped vessel (1), which is screw-connected in, or screw-mounted on, an externally sealed opening (2) in the container cover;b) the base of the vessel (1) facing the container interior (9) has a through-aperture (8);c) a gas-permeable sintered metal candle (10) is inserted in the through-aperture (8);d) at the end situated opposite the sintered metal candle (10), the catalyst pack (7) in the vessel (1) is covered by means of wire netting or a sintered metal plate (11), which is permeable to water vapour.
- Apparatus according to claim 1, characterised by a palladium catalyst with 0.5 per cent by weight PD on an Al₂O₃ carrier matrix.
Applications Claiming Priority (2)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| DE3904149 | 1989-02-11 | ||
| DE3904149A DE3904149C2 (en) | 1989-02-11 | 1989-02-11 | Device on containers with radioactive waste to reduce the internal pressure due to hydrogen formation |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| EP0383153A1 EP0383153A1 (en) | 1990-08-22 |
| EP0383153B1 true EP0383153B1 (en) | 1994-02-23 |
Family
ID=6373903
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| EP90102291A Expired - Lifetime EP0383153B1 (en) | 1989-02-11 | 1990-02-06 | Device for containers with radioactive waste for the reduction of internal pressure caused by the formation of hydrogen |
Country Status (4)
| Country | Link |
|---|---|
| EP (1) | EP0383153B1 (en) |
| JP (1) | JP2930644B2 (en) |
| KR (1) | KR930001952B1 (en) |
| DE (1) | DE3904149C2 (en) |
Families Citing this family (11)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| GB8901738D0 (en) * | 1989-01-26 | 1989-03-15 | Atomic Energy Authority Uk | Recombination catalyst |
| DE4343500A1 (en) * | 1993-12-20 | 1995-06-22 | Forschungszentrum Juelich Gmbh | Device for avoiding overpressures in storage containers with hydrogen-developing content |
| DE19531498C2 (en) * | 1995-08-26 | 2001-06-13 | Nuklear Service Gmbh Gns | Metal drum, in particular steel drum, for radioactive waste with pressure relief devices |
| DE19733283C2 (en) * | 1997-08-01 | 1999-08-05 | Gnb Gmbh | Shielding container for the transport and / or storage of spent fuel elements |
| JP4615749B2 (en) * | 2001-03-22 | 2011-01-19 | 日揮株式会社 | Radioactive waste treatment method and apparatus |
| FR2874120B1 (en) * | 2004-08-09 | 2006-11-24 | Cogema Logistics Sa | METHOD AND DEVICE FOR REMOVING FLAMMABLE GASES IN A CLOSED ENCLOSURE AND ENCLOSURE EQUIPPED WITH SUCH A DEVICE |
| FR2925752B1 (en) * | 2007-12-21 | 2012-03-09 | Tn Int | DEVICE FOR TRANSPORTING AND / OR STORING RADIOACTIVE MATERIALS TO ENABLE CONTROLLED RELEASE OF OXYGEN IN A CLOSED ENCLOSURE |
| FR2971614A1 (en) | 2011-02-11 | 2012-08-17 | Tn Int | DEVICE FOR TRAPPING FLAMMABLE GASES PRODUCED BY RADIOLYSIS OR THERMOLYSIS IN A CONTAINMENT ENCLOSURE |
| JP6242263B2 (en) * | 2014-03-27 | 2017-12-06 | 日立Ｇｅニュークリア・エナジー株式会社 | Radioactive material storage container |
| JP6746922B2 (en) * | 2016-01-20 | 2020-08-26 | 株式会社Ihi | Method and device for storing radioactive waste |
| US12084238B2 (en) | 2021-08-19 | 2024-09-10 | Battelle Savannah River Alliance, Llc | Compact augmented permeation system (CAPS) assemblies and related systems and methods |
Family Cites Families (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| DD34878A (en) * | ||||
| US2847284A (en) * | 1955-03-10 | 1958-08-12 | Harold M Busey | Apparatus for catalytically combining gases |
| US3369121A (en) * | 1966-04-06 | 1968-02-13 | Squibb & Sons Inc | Radioactive package and container therefor |
| US3755075A (en) * | 1970-03-25 | 1973-08-28 | North American Rockwell | Condenser-type gas combiner |
| DE2922717C2 (en) * | 1979-06-05 | 1983-01-27 | Brown Boveri Reaktor GmbH, 6800 Mannheim | Process and device for the catalytic recombination of hydrogen that is enclosed in the containment of a nuclear reactor plant |
| DE3227512C2 (en) * | 1982-07-23 | 1996-03-28 | Nuklear Service Gmbh Gns | Lost shielding container for radioactive waste |
| JPS62265600A (en) * | 1986-05-12 | 1987-11-18 | 秩父セメント株式会社 | Pressure regulator for storage-transport-disposal vessel |
| DE3730743A1 (en) * | 1987-09-12 | 1989-03-30 | Nuklear Service Gmbh Gns | Method for reducing the internal pressure build-up in a storage container for radioactive wastes |
-
1989
- 1989-02-11 DE DE3904149A patent/DE3904149C2/en not_active Expired - Fee Related
-
1990
- 1990-02-06 EP EP90102291A patent/EP0383153B1/en not_active Expired - Lifetime
- 1990-02-07 KR KR1019900001477A patent/KR930001952B1/en not_active IP Right Cessation
- 1990-02-09 JP JP2028607A patent/JP2930644B2/en not_active Expired - Lifetime
Also Published As
| Publication number | Publication date |
|---|---|
| KR900013526A (en) | 1990-09-06 |
| DE3904149A1 (en) | 1990-08-23 |
| DE3904149C2 (en) | 1994-01-20 |
| KR930001952B1 (en) | 1993-03-20 |
| EP0383153A1 (en) | 1990-08-22 |
| JPH03200000A (en) | 1991-08-30 |
| JP2930644B2 (en) | 1999-08-03 |
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