EP0102246A1 - Emballage et densification d'un matériau particulaire - Google Patents

Emballage et densification d'un matériau particulaire Download PDF

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Publication number
EP0102246A1
EP0102246A1 EP83304974A EP83304974A EP0102246A1 EP 0102246 A1 EP0102246 A1 EP 0102246A1 EP 83304974 A EP83304974 A EP 83304974A EP 83304974 A EP83304974 A EP 83304974A EP 0102246 A1 EP0102246 A1 EP 0102246A1
Authority
EP
European Patent Office
Prior art keywords
bellows
bellows container
container
cannister
refractory
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
EP83304974A
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German (de)
English (en)
Other versions
EP0102246B1 (fr
Inventor
Eric John Ramm
Alfred Edward Ringwood
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.)
Australian Atomic Energy Commission
Australian National University
Original Assignee
Australian Atomic Energy Commission
Australian National University
Australian Nuclear Science and Technology Organization
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
Priority claimed from AU18163/83A external-priority patent/AU552755B2/en
Application filed by Australian Atomic Energy Commission, Australian National University, Australian Nuclear Science and Technology Organization filed Critical Australian Atomic Energy Commission
Priority to AT83304974T priority Critical patent/ATE30649T1/de
Publication of EP0102246A1 publication Critical patent/EP0102246A1/fr
Application granted granted Critical
Publication of EP0102246B1 publication Critical patent/EP0102246B1/fr
Expired legal-status Critical Current

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    • G—PHYSICS
    • G21—NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21F—PROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00—Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/28—Treating solids
    • G21F9/34—Disposal of solid waste

Definitions

  • the present invention relates to the containment of waste material, and more particularly is concerned with arrangements for containing waste material which requires very reliable, very long term storage.
  • the nuclear reactor waste is incorporated into the crystal lattices of the synthetic rock in the form of a dilute solid solution and therefore should be safely immobilised.
  • a dense, compact, mechanically strong block of the synthetic rock incorporating the nuclear waste is produced by pressure and heat in a densification process and the block may then be safely disposed of in a suitable geological formation.
  • the present invention provides a method of containing and densifying particulate supply material comprising pouring the waste material into a bellows container of generally cylindrical form with side wall including a bellows-like formation and of heat and decay resistant material, closing the bellows container with a lid, placing the bellows container on an upwardly displaceable ram having a heat resistant surface portion, displacing the ram upwardly to press the bellows container against a fixed abutment, maintaining substantially axially pressure on the bellows container and maintaining a sufficiently elevated temperature in the bellows container for a sufficient length of time to cause densification of said particulate supply material in the bellows container and axial compression of the bellows container, the arrangement being such that deformation of the bellows container occurs in its axial direction and removing the bellows container after completion of the densification step.
  • the invention thus can provide a most effective and reliable process for use with supply material in the form of high level radioactive waste and capable of long term operation in a hot cell with ease of operation of the process and maintenance of equipment. Furthermore. the method characterised by the upward pressing technique permits considerable economy of capital equipment and the hot cell space required by virtue of the use of a single ram with a fixed abuttment. Since typically operating temperatures in the region of 1100 0 C will be used, a substantial refractory facing can readily be provided for the fixed abutment and also for the refractory ram.
  • the upward pressing method facilitates, in a preferred embodiment, a most easily serviced apparatus since the refractory facing for the ram can simply be a disc-like pad located by simple locating means such as a spiggot and socket with the pad essentially remaining in position under the force of gravity, Thus. using manipulators in a hot cell a worn refractory pad can readily be removed for disposal and a replacement pad fitted.
  • the high working temperatures for the densification step are best achieved by the use of induction heating and therefore typically it takes many hours for the contents of the bellows container to come to a uniform working temperature. Therefore preheating of the bellows container to bring the contents up to a uniform temperature suitable for the densification step is a major advantage. Not only can the production rate for given capital cost be maximized but furthermore a substantial further advantage is that bringing the contents of the bellows container to the uniform densification temperature aids reliable and uniform densification thereby ensuring reliable axial compression of the bellows container which facilitates its later handling and storage.
  • the bellows container is typically of a heat resistant steel and preferably a stainless steel. Inevitably the mechanical strength of the steel is reduced at the high densification temperatures in the region of 1100 to 12 00 0 C.
  • the broad method may be utilized in a surprisingly effective and synergistic combination of steps in which the bellows container is subjected to the densification step whilst in a cylindrical cannister in which the bellows container becomes a tight fit after the pressing operation thereby providing a most effective and convenient extra containment for long term safe storage of the waste material.
  • Such a method may be defined as consisting in a method for the containment of particulate waste material, the method comprising pouring the waste material into bellows containers of generally cylindrical form with a side wall including a bellows-like formation and of heat and decay resistant material, closing each bellows container with a lid, preheating in series the bellows containers to bring the contents thereof to a substantially uniform elevated temperature, placing each bellows container in turn on an upwardly displacable ram and displacing the ram upwardly to insert the bellows container into a cylindrical canister and applying pressure and maintaining a sufficiently elevated temperature for sufficient time to cause densification of the contents of the bellows container with axial compression of the bellows container and relatively slight outward expansion thereof to cause the bellows container to grip the interior wall of the cylindrical canister, and when the canister has been filled with a series of such bellows containers, sealing the canister and removing the canister for storage.
  • the invention is particularly useful in relation to the incorporation of high level radioactive waste in synthetic rock of the type described by A. E. Ringwood (and referred to above), the invention can also be applied to other synthetic rock arrangements and furthermore can also be applicable to other materials which require storage and are capable of compaction under heat and pressure.
  • One example of such other --material would be shredded-waste zirconium alloy nuclear fuel rod tubes and similar waste components.
  • the invention consists in a combination of steps which cooperate together in an advantageous relationship which permits efficient, economic, and convenient operations in a hot cell.
  • the apparatus used can be relatively simple, and this can contribute greatly to the reliability and acceptability of the system due to simplicity of servicing and intrinsic reliability.
  • the cylindrical canister will be of the order of 30 cm diameter and 2 metres long and each bellows container will be compressible from an initial height of about 40 cm to a final height of about 10 cm.
  • the use of induction heating coils is the preferred method of both preheating and maintaining the necessary elevated temperature during the densification step, and due to the fact that heating of the 5 particulate material is due to conduction from the bellows container (which is heated by the induction heating coils) a considerable time is required for the preheating step.
  • preheating for several hours can be effective whereas the final densification step will be much shorter, e.g. about one hour.
  • the bellows container is given a preliminary axial pressing which can be at ambient temperature or with advantage can be at a bellows container temperature of up to about 800 C to anneal the material of the bellows container. Since the bellows container will have a high degree of strength at ambient temperature and also at temperatures up to about 800 0 C, good control can be achieved in this preliminary axial pressing and, surprisingly, during the densification step at high temperature (typically 1200 0 C) excellent control of the axial pressing can be achieved thereby essentially minimizing the risk of the bellows container compressing with sideways shear rather than true axial compression.
  • a preliminary axial pressing which can be at ambient temperature or with advantage can be at a bellows container temperature of up to about 800 C to anneal the material of the bellows container. Since the bellows container will have a high degree of strength at ambient temperature and also at temperatures up to about 800 0 C, good control can be achieved in this preliminary axial pressing and, surprisingly, during the densification step at high temperature (typical
  • the pressure in the preliminary pressing is of at least 3000 Ibs/sq. inch.
  • the material is preferably provided in the form of well graded fine particles up to about 2 mm maximum dimension whereby a readily pourable material is provided which can be easily densified in the process.
  • Preferably synthetic rock is used to incorporate radioactive waste, a mixture of synthetic rock precursor and high level waste being sprayed into a rotary kiln to produce the intimately mixed materials.
  • the temperature at the region in which the material is introduced into the rotary kiln is preferably controlled in the range of about 400-600°C, and the maximum temperature in the kiln is about 700-800°C with the exit from the rotary kiln being at ambient temperature.
  • a preferred embodiment of the invention can also provide further means for safeguarding the cylindrical canister from outward deformation under the pressure of expanding bellows containers within the canister.
  • This is achievable by the use of a block of refractory material having a slightly tapered bore which at its narrowest diameter just fits over the canister, the refractory block being adapted to be moved downwardly in a series of steps corresponding to bellows container locations, the slightly tapered bore permitting release of the block even if some outward deformation of the canister has taken place in a step of densification and compression of the bellows container.
  • the refractory block is formed so as to embrace the induction heating coil for surrounding the canister.
  • the refractory block comprises a series of interlocking refractory segments arranged to be mounted inside a cylindrical containment shroud which absorbs any expansion forces applied from the canister.
  • apparatus for encapsulating particulate supply material in bellows containers within a cylindrical canister comprising means for pouring the particulate material into a bellows container, means for sealing the bellows container with a lid, means for moving bellows containers in sequence to a pressing station, a pressing station comprising an upwardly displaceable ram for receiving a bellows container, means for mounting a cylindrical container with an open end directed downwardly towards said ram, means for upwardly pressing a bellows container supported on the ram into the canister, upper refractory support means to act as an abutment, heating means for maintaining an elevated temperature in said bellows container whilst said pressure is applied to cause densification of said material in the bellows container and expand slightly the bellows container to cause it to jam in the canister, the heating means being adapted to provide heating in a series of zones within the container corresponding to a series of bellows containers inserted one below the other in series therein
  • the apparatus includes a preheating station adapted to bring the contents of the bellows containers to a substantially uniform elevated temperature, and means for transferring a preheated bellows container to said pressing station.
  • the process has a preliminary mixing stage 21 in which synthetic rock precursor from supply 20 is formed into a slurry with high level radioactive waste from waste supply 19 which is in the form of a nitrate solution, and the slurry is passed along line 22 to be sprayed into the elevated temperature end of a rotary kiln, at which a maximum temperature in the range 700-800° is maintained.
  • the spraying step immediately vaporises the water content of the slurry sprayed into the rotary kiln and causes chemical decomposition of the radioactive nitrates and will cause the mineral components of the synthetic rock to start to form with the radioactive elements starting to go into mineral phases.
  • a chemical reducing control gas (such as argon-hydrogen, nitrogen-hydrogen, or CO-C0 2 ) is passed through the rotary kiln.
  • the process could be operated so that synthetic rock particles incorporating the radioactive waste are completely formed in the rotary kiln but this is not essential.
  • the rotary kiln produces cold particulate material of well graded particle size up toabout 2 mm maximum dimension, whereas gases produced by the rotary kiln are fed back through a filter F to the preliminary mixing stage 21 since these gases will include some radioactive components.
  • the particulate material produced by the rotary kiln is fed into a titanium mixing stage 24 which receives metallic titanium powder from a hopper 25 whereby the mixture poured into a bellows container 20 has about 2% titanium metal powder by weight.
  • An example of a suitable synthetic rock composition is indicated in the table set out below and is produced using tetraisopropyl titanate and tetrabutyl zirconate as ultimate sources of TiO 2 and Zr0 2 .
  • the components are mixed with nitrate solutions of the other components, co-precipitated by addition of sodium hydroxide and then washed..to produce synthetic rock precursor.
  • the precursor material is a product which possesses a very high surface area and functions as an effective ion exchange medium, which is mixed with additives containing Ca, Ba. and Al in solution and mixed in a hot cell with high level nuclear waste (HLW) in the form of nitrate solution to form a thick homogeneous slurry at mixing stage 21.
  • HMW high level nuclear waste
  • up to about 20% by weight of the solid content of the slurry may comprise the high level wastes.
  • the bellows container 20 is of a heat resisting steel such as an austenitic stainless steel, for example Sandvik grade 253MA which retains reasonable mechanical strength even at the elevated temperatures used in the process, although at these temperatures the container is relatively ductile.
  • a thin perforated metal liner 26 is located within the bellows container and the space between the liner and bellows wall is filled with zirconium oxide powder 27.
  • a stainless steel cap 29 is used to seal the bellows container which is then placed between a pair of pistons 30 for a cold pressing operation which can increase the density of particulate material from about 25% of the theoretical maximum density to about 36%.
  • each bellows container 20 is fed in sequence into a vertical induction furnace 31, each bellows container being supported on a refractory disk 32. the lowermost refractory disk being supported by a retractable latch 33. Over a period of several hours the temperature gradually increases up to about 1200 0 C.
  • a first water cooled ram 34 having a top spiggot on which a refractory plate 35 is located is adapted to support and lower one at a time the bellows containers from the furnace for horizontal movement across a support table 36 to a pressing station having a second water cooled ram 37 of similar form.
  • Figure 2 shows the ram 37 both in the lower receiving position and also in the upwardly displaced pressing position inside a metal canister 38 mounted on a support 39 and having its top sealed and in abutment against a fixed refractory block 40, vertically displaceable induction heating coils 41 being provided outside the canister 38.
  • the left hand side of the section of a bellows container 20a is shown in its configuration before hot pressing and the right hand side of the section shows a bellows container 20b as it would be after pressing.
  • the bellows container slightly expands to become an interference fit within the canister 38 as shown by bellows 20c at the top of the canister 38.
  • the refractory plate 32 upon which each of the bellows containers is supported is removed after the pressing stage, the plate 32 being lowered on the water cooled ram 37 and then pushed onto a receiving table from which the plate can be recylced for further use.
  • Refractory plates will . wear in use and must be replaced and an important advantage of the design illustrated in Figure 2 is a very simple and easily . serviced arrangement made possible by the use of an upward pressing technique; this permits the replaceable refractory top plate 35 simply to sit on the head of each water cooled ram. Just a simple spiggot and socket engagement is provided so that manipulators can readily remove a worn refractory plate and insert a new one.
  • the apparatus further includes a base plate 42 with a set of upstanding tubular guides 43 on which sliding mounts for the support 39 and the induction furnace unit 41 are slidably mounted but adapted to be clamped at any selected position.
  • the canister 38 is urged upwardly against the refractory block 40 which is supported by a top cap 44 adapted to be bolted to a top plate 45.
  • Figure 3 shows the parts in slightly exploded view for clarity.
  • the induction heating coil 41 is shown embedded within a refractory block 46 having a tapered bore. the drawing showing a greatly exaggerated taper and clearance between the bore and the container 38.
  • the object of the tapered bore of the refractory block 46 is that any small expansion of the canister 38 causes the canister to be supported against further outward deformation by the refractory block but by virtue of the taper, the refractory block can be released by downward motion to the next location for the succeeding bellows container.
  • the refractory block is assembled from refractory segments comprising outer refractory segments 46a of cylindrical profile and inner refractory elements 46b having an inner profile adapted to cooperate to form a tapered bore with circumferentially extending grooves for accommodating the turns of the induction coil 41.
  • the refractory elements are contained within a steel outer support cylinder 47 which absorbs the forces of any outward expansion applied by the canister 38.
  • Figure 5 shows in isometric view the refractory blocks 46a and 46b each having a semi-circular rib 46c on one side thereof and a corresponding cavity 46d on the other side for interengagement purposes.

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  • Engineering & Computer Science (AREA)
  • Environmental & Geological Engineering (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Processing Of Solid Wastes (AREA)
EP19830304974 1982-08-30 1983-08-30 Emballage et densification d'un matériau particulaire Expired EP0102246B1 (fr)

Priority Applications (1)

Application Number Priority Date Filing Date Title
AT83304974T ATE30649T1 (de) 1982-08-30 1983-08-30 Verpackung und verdichtung eines teilchenfoermigen materials.

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
AUPF567082 1982-08-30
AU5670/82 1982-08-30
AU18163/83A AU552755B2 (en) 1982-08-30 1982-08-30 Containment of waste material

Publications (2)

Publication Number Publication Date
EP0102246A1 true EP0102246A1 (fr) 1984-03-07
EP0102246B1 EP0102246B1 (fr) 1987-11-04

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EP19830304974 Expired EP0102246B1 (fr) 1982-08-30 1983-08-30 Emballage et densification d'un matériau particulaire

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2163893A (en) * 1984-07-31 1986-03-05 Agip Spa Immobilising the fission product and transuranic element content of liquid high level radioactive waste
EP0209339A2 (fr) * 1985-07-16 1987-01-21 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Appareil de chauffage par induction et procédé
EP0211533A1 (fr) * 1985-07-16 1987-02-25 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Bloc de pression pour soufflets à chaude pression
EP0228816A1 (fr) * 1985-11-29 1987-07-15 Australian Nuclear Science And Technology Organisation Dispositifs de traitement par vibrations
EP0230732A1 (fr) * 1985-11-29 1987-08-05 Australian Nuclear Science And Technology Organisation Formation de céramiques

Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0044692A2 (fr) * 1980-07-15 1982-01-27 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Dispositifs pour l'encapsulation de déchets
EP0044381A1 (fr) * 1980-05-19 1982-01-27 Asea Ab Méthode pour traiter les matériaux radioactifs et récipient pour enfermer de tels matériaux
DE3129852A1 (de) * 1981-07-29 1983-02-17 GNS Gesellschaft für Nuklear-Service mbH, 4300 Essen "verfahren zur lagerung von verdichtbaren radioaktiven abfallstoffen"

Patent Citations (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0044381A1 (fr) * 1980-05-19 1982-01-27 Asea Ab Méthode pour traiter les matériaux radioactifs et récipient pour enfermer de tels matériaux
EP0044692A2 (fr) * 1980-07-15 1982-01-27 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Dispositifs pour l'encapsulation de déchets
DE3129852A1 (de) * 1981-07-29 1983-02-17 GNS Gesellschaft für Nuklear-Service mbH, 4300 Essen "verfahren zur lagerung von verdichtbaren radioaktiven abfallstoffen"

Cited By (6)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
GB2163893A (en) * 1984-07-31 1986-03-05 Agip Spa Immobilising the fission product and transuranic element content of liquid high level radioactive waste
EP0209339A2 (fr) * 1985-07-16 1987-01-21 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Appareil de chauffage par induction et procédé
EP0211533A1 (fr) * 1985-07-16 1987-02-25 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Bloc de pression pour soufflets à chaude pression
EP0209339A3 (fr) * 1985-07-16 1988-06-08 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Appareil de chauffage par induction et procédé
EP0228816A1 (fr) * 1985-11-29 1987-07-15 Australian Nuclear Science And Technology Organisation Dispositifs de traitement par vibrations
EP0230732A1 (fr) * 1985-11-29 1987-08-05 Australian Nuclear Science And Technology Organisation Formation de céramiques

Also Published As

Publication number Publication date
EP0102246B1 (fr) 1987-11-04

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