EP0044692B1 - Arrangements for containing waste material - Google Patents

Arrangements for containing waste material Download PDF

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Publication number
EP0044692B1
EP0044692B1 EP81303221A EP81303221A EP0044692B1 EP 0044692 B1 EP0044692 B1 EP 0044692B1 EP 81303221 A EP81303221 A EP 81303221A EP 81303221 A EP81303221 A EP 81303221A EP 0044692 B1 EP0044692 B1 EP 0044692B1
Authority
EP
European Patent Office
Prior art keywords
canister
metal
supply material
synthetic rock
metal canister
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
Application number
EP81303221A
Other languages
German (de)
English (en)
French (fr)
Other versions
EP0044692A3 (en
EP0044692A2 (en
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
Application filed by Australian Atomic Energy Commission, Australian National University, Australian Nuclear Science and Technology Organization filed Critical Australian Atomic Energy Commission
Publication of EP0044692A2 publication Critical patent/EP0044692A2/en
Publication of EP0044692A3 publication Critical patent/EP0044692A3/en
Application granted granted Critical
Publication of EP0044692B1 publication Critical patent/EP0044692B1/en
Expired 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
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • 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
    • G21F9/008—Apparatus specially adapted for mixing or disposing radioactively contamined material
    • 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 arrangements for containing waste material for long term storage and the invention is particularly applicable to immobilisation of high level radioactive waste material such as that produced by nuclear reactors.
  • 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 application in some embodiments, is concerned with making use of the synthetic rock arrangements of A.
  • E. Ringwood et al and is concerned with an apparatus and method for producing disposable blocks of material which can include radioactive wastes in an immobilised form.
  • the present application is not necessarily restricted to the particular classes of synthetic rocks of A.
  • E. Ringwood et al and the apparatus and method described herein could be applied to other synthetic rocks in addition to those specifically described by A. E. Ringwood et al.
  • synthetic rock is defined as a material which consists chemically of one or more metal oxides (or compounds derived from metal oxides which have been formed into a rock-like structure by subjecting a mass of solid particles of the material to heat and pressure.
  • EP application 81103570.8 published after the filing data of this application as EP-A-0044381 of ASEA AB.
  • the conversion into a solid body involves isostatic pressing.
  • This invention relates to a method for forming solid blocks which include synthetic rock in which nuclear reactor waste is immobilised, the method comprising:-
  • the bellows-like wall structure of the metal canister allows it to collapse under axial pressure, the wall structure of the canister itself preventing gross outward deformation.
  • At least preferred embodiments of'the invention provide a simple and effective method which can readily be practised in a "hot cell" and a relatively safe and easily handled product ensues. It is considered that during very long term storage radiation damage within the synthetic rock is likely to cause a small expansion perhaps of the order of 2% to 3%. At least in preferred embodiments, such long term expansion can be accommodated without increased risk of contamination of the environment, for example through leaching with ground water.
  • the metal canister has a sealed bottom end wall and only the final step of welding or otherwise permanently fixing a metal cap to the top of the canister is required in the hot cell.
  • the present method is best implemented by including in the supply material or in contact therewith a suitable metal in a suitable quantity to provide a selected oxygen potential to facilitate the effective formation of the synthetic rock with radioactive waste immobilised therein.
  • suitable metals to consider for providing the desired oxygen potential are nickel, titanium and iron.
  • the metal could be provided in the form of a lining to the metal canister or as an inner can for the supply material or alternatively the metal could be provided in fine particulate form mixed with the supply material.
  • the present invention includes the additional step of initially forming the supply material into a granulated form which can be easily poured. This should minimise spillage and contamination in the hot cell.
  • the granules can be formed in a cold pressing operation, by disc granulation, by a spray drying/calcination or by fluidised bed/calcination process.
  • the supply material is initially charged into thin walled metal cans which will remain solid at the sintering temperatures used which are typically of the order of 1200°C.
  • the metal can may have a close fitting lid and the supply material could be poured or cold pressed into the can before the lid is fitted.
  • the lid is tight fitting so as largely to retain any components of the nuclear waste which are somewhat volatile at the high sintering temperatures. This step can be very high important to the economics of operation since contamination of the hot cell by such volatile components can be largely minimised.
  • the thin walled metal can could have a close fitting lid rather like a paint tin and can be made of nickel or iron and indeed the choice of such metals can provide the preferred oxygen potential.
  • One useful material for the metal canister is stainless steel which is sufficiently corrosion resistant and has sufficient high temperature strength to be readily used in the present method.
  • One such steel is that known as Sandvik 253MA.
  • heating to about 1260°C and the application of pressure of about 7MPA will be suitable sintering conditions.
  • the pressure could be increased, for example, up to 14 MPA.
  • a practical limit exists as to the maximum height of a column of supply material.
  • the method includes using an apparatus in which the refractory support element includes a series of separate electrical induction heating coils disposed to apply selectively heat to regions extending respective distances along the axis of the metal canister, whereby a series of densification steps occur commencing at one end of the canister, the induction coils being utilised in sequence after the densification and sintering of the previous section of the supply material.
  • the refractory support element includes a series of separate electrical induction heating coils disposed to apply selectively heat to regions extending respective distances along the axis of the metal canister, whereby a series of densification steps occur commencing at one end of the canister, the induction coils being utilised in sequence after the densification and sintering of the previous section of the supply material.
  • water cooled induction coils in partially overlapping relationship are provided.
  • a constant pressure is applied to the supply material by means of a refractory faced plunger inserted into the open end of the canister and gradual densification occurs.
  • An additional quantity of supply material or an additional small can of supply material may be inserted before the final step.
  • a close fitting refractory spacer is then inserted on top of the supply material to prevent the refractory faced plunger from entering the final heat zone.
  • the pressure most conveniently is applied from a lower supporting hydraulic ram and from a refractory faced metal ram in contact with the supply material.
  • the refractory facing protects the metal ram from overheating. Water cooling of the metal ram may also be desirable.
  • the invention is best implemented in a manner which carefully minimises outward deformation of the metal canister and yet provides a long working life for the apparatus.
  • the apparatus includes induction heating coils which are water cooled.
  • the apparatus is adapted to handle a relatively long canister which might be up to approximately 3.6 metres long and up to approximately 375 mm in diameter; the apparatus in this embodiment should include a series of separate induction coils to permit densification and sintering of the supply material zone by zone from one end of the metal canister in separate steps thereby ensuring effective densification and sintering along the entire mass of supply material in the metal canister.
  • the zones overlap to ensure a continuous mass of properly densified material in the canister at the end of the process.
  • a disposable element comprising a sealed metal canister containing a densified synthetic rock mass including, in the crystal structure, a minor proportion of nuclear reactor waste, the element being produced by the method of the invention.
  • Figure 2 The embodiment shown in Figure 2 is characterized by the use of a metal canister 20 formed of stainless steel and having a bellows-like structure, the bellows-like structure preventing gross outward deformation of the canister during the pressing step.
  • Figure 2 illustrates schematically the overall process and the apparatus which is to be used.
  • non-radioactive synthetic rock precursor is produced as indicated by the step shown in Figure 2 labelled "SYNROC precursor".
  • the synthetic rock has a composition as indicated in the table set out below and is produced using tetraisopropyl titanate and tetrabutyl zirconate as ultimate sources of Ti0 2 and Zr0 2 .
  • the components are mixed with nitrate solutions of the other components, coprecipitated by addition of sodium hydroxide and then washed.
  • 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 and high level nuclear waste (HLW) in the form of nitrate solution to form a thick homogeneous slurry at mixing stage 21 which is located in a hot cell.
  • HMW high level nuclear waste
  • the slurry is then fed by line 22 to a rotary kiln 23 operating at about 850°C in which the slurry is heated, devolatilised and calcined.
  • the resulting calcine is mixed in mixer 24 with 2% by weight of metallic titanium powder supplied from hopper 25.
  • the mixer 24 then supplies the powder to a primary canister 20 of stainless steel and of bellows-like form as illustrated. It will be noted from the drawings that the canister can be compressed by a factor of about 3 and does not have gross outward deformation.
  • a thin perforated metal liner 26 is located within the canister and the space between the liner and the canister wall is filled with zirconium oxide powder 27 or alternatively any other powder possessing low thermal conductivity properties may be used.
  • the canister can then be filled with powder 28 from the mixer 24.
  • a stainless steel plug or cap 29 is then used to seal the canister and the canister placed between a pair of pistons 30 which are of molybdenum- based alloy and capable of operation at temperatures up to 1200°C.
  • a radio frequency induction coil 31 is then used to raise the temperature of the ends of the pistons 30 and the canister and its contents to about 1150°C.
  • the resultant sealed compressed canisters containing the synthetic rock structure are then removed and stacked in a disposable cylinder 31a which is fabricated from highly corrosion resistant alloy such as that based on Ni 3 Fe.
  • the space between the primary canisters 20 and the internal wall of the cylinder 31a is filled with molten lead 32 and the cylinder finally is sealed for disposal.
  • the embodiment of Figures 3 and 4 is a variation on the embodiment of Figure 2, the steps up to the mixer 24 of Figure 2 being the same.
  • the outer cylinder 40 and the bellows-like canister 41 are respectively dimensioned so that the clearance between the envelope of the canister 41 and the interior of the cylinder 40 is substantially taken up after the compression step, thus obviating the need for handling of the canister after compression to insert it into the cylinder and the pouring of lead to fill the cavity around the canister in the embodiment of Figure 2.
  • the cylinder 40 is supported on a base 43 and the canister 41 inserted with an open-ended metal cylinder 41a located within the canister.
  • Mix from mixer 24 is then poured into the canister to fill the zone within the cylinder 41a and a top cap 44 secured in position.
  • the whole mass is then heated by a radio frequency induction coil 45 which surrounds the outer cylinder and after sufficient time has elapsed for a uniform temperature to be reached, a ram 46 having a piston-like face 47 is used to apply compression to the canister 41.
  • the canister collapses with slight outward expansion of the canister but the arrangement is such that the walls of the cylinder 40 do not have any significant constraining effect on outward expansion of the bellows-like canister 41.
  • the cylinder 41a crinkles somewhat but prevents substantial ingress of synthetic rock material into the zone of the bellows, thereby obviating the risk of insufficient compression in the bellows zone and improperly formed synthetic rock occurring between the bellows corrugations.
  • the adjacent corrugations of the bellows will come together in the compression step.
  • Figure 4 also illustrates how the induction coil 45 can be moved upwardly to the next location ready for treating the next canister which is to be inserted on top of the canister 41.

Landscapes

  • Engineering & Computer Science (AREA)
  • Physics & Mathematics (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Environmental & Geological Engineering (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Processing Of Solid Wastes (AREA)
EP81303221A 1980-07-15 1981-07-14 Arrangements for containing waste material Expired EP0044692B1 (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
AU4534/80 1980-07-15
AUPE453480 1980-07-15

Publications (3)

Publication Number Publication Date
EP0044692A2 EP0044692A2 (en) 1982-01-27
EP0044692A3 EP0044692A3 (en) 1982-02-03
EP0044692B1 true EP0044692B1 (en) 1986-10-08

Family

ID=3768603

Family Applications (1)

Application Number Title Priority Date Filing Date
EP81303221A Expired EP0044692B1 (en) 1980-07-15 1981-07-14 Arrangements for containing waste material

Country Status (3)

Country Link
EP (1) EP0044692B1 (GUID-C5D7CC26-194C-43D0-91A1-9AE8C70A9BFF.html)
JP (1) JPS57118200A (GUID-C5D7CC26-194C-43D0-91A1-9AE8C70A9BFF.html)
DE (1) DE3175445D1 (GUID-C5D7CC26-194C-43D0-91A1-9AE8C70A9BFF.html)

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7078581B1 (en) 1999-11-12 2006-07-18 British Nuclear Fuels Plc Encapsulation of waste

Families Citing this family (15)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE3104366C2 (de) * 1981-02-07 1986-12-04 Deutsche Gesellschaft für Wiederaufarbeitung von Kernbrennstoffen mbH, 3000 Hannover Vorrichtung zum Evakuieren und Befüllen von Endlagerbehältern für radioaktives Material
DE3214242A1 (de) * 1982-04-17 1983-10-20 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur verbesserung der fuer eine langzeitlagerung erforderlichen eigenschaften von verfestigungen radioaktiver abfaelle
EP0102246B1 (en) * 1982-08-30 1987-11-04 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Containment and densification of particulate material
US4645624A (en) * 1982-08-30 1987-02-24 Australian Atomic Energy Commission Containment and densification of particulate material
SE442562B (sv) * 1983-01-26 1986-01-13 Asea Ab Sett att innesluta radioaktivt eller annat farligt avfall och en behallare for sadant avfall
JPS59201000A (ja) * 1983-04-28 1984-11-14 株式会社日立製作所 放射性固体廃棄物の収納方法
JPS60186800A (ja) * 1984-03-06 1985-09-24 日本碍子株式会社 放射性廃棄物の焼却固化方法および装置
JPS60198498A (ja) * 1984-03-21 1985-10-07 動力炉・核燃料開発事業団 使用済燃料被覆管等の処理方法
FR2575319B1 (fr) * 1984-12-21 1987-03-20 Sgn Soc Gen Tech Nouvelle Procede d'emballage etanche de conteneur renfermant des matieres toxiques
FR2584854B1 (fr) * 1985-07-09 1987-09-25 Commissariat Energie Atomique Procede et installation de compactage et de conditionnement de dechets solides radio-actifs de faible ou moyenne activite.
EP0209339A3 (en) * 1985-07-16 1988-06-08 AUSTRALIAN NUCLEAR SCIENCE & TECHNOLOGY ORGANISATION Inductive heating apparatus and process
US4778626A (en) * 1985-11-04 1988-10-18 Australian Nat'l Univ. of Acton Preparation of particulate radioactive waste mixtures
WO1990003648A1 (en) * 1988-09-27 1990-04-05 Australian Nuclear Science & Technology Organisation Hot pressing of particulate materials
US5414208A (en) * 1990-10-18 1995-05-09 Australian Nuclear Science & Technology Organisation Formation of densified material
CA2520813C (en) * 2003-04-25 2009-10-27 Mitsubishi Pharma Corporation Sustained release formulations of alkylene dioxybenzene derivatives useful as 5-ht1a agonists

Citations (1)

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US3160502A (en) * 1960-10-10 1964-12-08 American Beryllium Company Inc Method of making beryllium billets

Family Cites Families (8)

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US3000072A (en) * 1959-08-20 1961-09-19 Ca Atomic Energy Ltd Process of containing and fixing fission products
FR2369659A1 (fr) * 1976-11-02 1978-05-26 Asea Ab Pr
DE2659691C2 (de) * 1976-12-31 1985-11-14 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Anlage zum Verpressen von radioaktiven Abfällen in einem Faß
JPS54116600A (en) * 1978-03-01 1979-09-10 Gakei Denki Seisakusho:Kk Waste disposal method and container
JPS54130799A (en) * 1978-03-31 1979-10-11 Toshiba Corp Radioactive waste solidifying method
JPS54130800A (en) * 1978-03-31 1979-10-11 Toshiba Corp Radioactive waste solidifying method
JPS6044640B2 (ja) * 1978-07-14 1985-10-04 ジ・オ−ストラリアン・ナシヨナル・ユニバ−シテイ 高レベル放射性廃棄物か焼物を不動態化する方法および不動態化した高レベル放射性廃棄物を含有する鉱物集合体
JPS5572899A (en) * 1978-11-27 1980-06-02 Kobe Steel Ltd Volume decrease and solidification method of spent fuel cladding tube

Patent Citations (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3160502A (en) * 1960-10-10 1964-12-08 American Beryllium Company Inc Method of making beryllium billets

Cited By (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US7078581B1 (en) 1999-11-12 2006-07-18 British Nuclear Fuels Plc Encapsulation of waste

Also Published As

Publication number Publication date
EP0044692A3 (en) 1982-02-03
JPH0219920B2 (GUID-C5D7CC26-194C-43D0-91A1-9AE8C70A9BFF.html) 1990-05-07
EP0044692A2 (en) 1982-01-27
DE3175445D1 (en) 1986-11-13
JPS57118200A (en) 1982-07-22

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