EP2774155A1 - Verfahren zur behandlung einer verkleidung mit gesintertem calciumhydrid - Google Patents
Verfahren zur behandlung einer verkleidung mit gesintertem calciumhydridInfo
- Publication number
- EP2774155A1 EP2774155A1 EP12794429.6A EP12794429A EP2774155A1 EP 2774155 A1 EP2774155 A1 EP 2774155A1 EP 12794429 A EP12794429 A EP 12794429A EP 2774155 A1 EP2774155 A1 EP 2774155A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- sheath
- sintered
- treatment
- calcium hydride
- treatment according
- 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
Links
- CSDQQAQKBAQLLE-UHFFFAOYSA-N 4-(4-chlorophenyl)-4,5,6,7-tetrahydrothieno[3,2-c]pyridine Chemical compound C1=CC(Cl)=CC=C1C1C(C=CS2)=C2CCN1 CSDQQAQKBAQLLE-UHFFFAOYSA-N 0.000 title claims abstract description 40
- 238000000034 method Methods 0.000 title claims abstract description 35
- 238000005253 cladding Methods 0.000 title abstract description 3
- VTYYLEPIZMXCLO-UHFFFAOYSA-L Calcium carbonate Chemical compound [Ca+2].[O-]C([O-])=O VTYYLEPIZMXCLO-UHFFFAOYSA-L 0.000 claims abstract description 42
- 239000000463 material Substances 0.000 claims abstract description 29
- 239000000843 powder Substances 0.000 claims abstract description 28
- 229910000019 calcium carbonate Inorganic materials 0.000 claims abstract description 21
- 239000011541 reaction mixture Substances 0.000 claims abstract description 18
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 claims abstract description 16
- 239000001569 carbon dioxide Substances 0.000 claims abstract description 8
- 229910002092 carbon dioxide Inorganic materials 0.000 claims abstract description 8
- 239000011261 inert gas Substances 0.000 claims abstract description 8
- 239000012857 radioactive material Substances 0.000 claims description 22
- 238000006243 chemical reaction Methods 0.000 claims description 17
- 230000008569 process Effects 0.000 claims description 14
- 239000000203 mixture Substances 0.000 claims description 7
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 6
- YZCKVEUIGOORGS-NJFSPNSNSA-N Tritium Chemical compound [3H] YZCKVEUIGOORGS-NJFSPNSNSA-N 0.000 claims description 6
- 229910052722 tritium Inorganic materials 0.000 claims description 6
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 4
- 230000005484 gravity Effects 0.000 claims description 4
- 229910052751 metal Inorganic materials 0.000 claims description 3
- 239000002184 metal Substances 0.000 claims description 3
- 229910052757 nitrogen Inorganic materials 0.000 claims description 3
- 230000002285 radioactive effect Effects 0.000 claims description 3
- 229910052786 argon Inorganic materials 0.000 claims description 2
- 239000000919 ceramic Substances 0.000 claims description 2
- 238000000605 extraction Methods 0.000 claims description 2
- 239000004033 plastic Substances 0.000 claims description 2
- 239000002699 waste material Substances 0.000 abstract description 21
- 239000010804 inert waste Substances 0.000 abstract 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 11
- 229910052739 hydrogen Inorganic materials 0.000 description 11
- 239000001257 hydrogen Substances 0.000 description 11
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 8
- 239000011575 calcium Substances 0.000 description 6
- 239000007789 gas Substances 0.000 description 6
- 230000001464 adherent effect Effects 0.000 description 5
- 239000002901 radioactive waste Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- 230000009466 transformation Effects 0.000 description 4
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 3
- 229910000831 Steel Inorganic materials 0.000 description 3
- 229910052791 calcium Inorganic materials 0.000 description 3
- 150000004678 hydrides Chemical class 0.000 description 3
- 238000011084 recovery Methods 0.000 description 3
- 239000010959 steel Substances 0.000 description 3
- 239000012535 impurity Substances 0.000 description 2
- 235000012771 pancakes Nutrition 0.000 description 2
- 235000012431 wafers Nutrition 0.000 description 2
- FYYHWMGAXLPEAU-UHFFFAOYSA-N Magnesium Chemical compound [Mg] FYYHWMGAXLPEAU-UHFFFAOYSA-N 0.000 description 1
- 230000001133 acceleration Effects 0.000 description 1
- 239000002253 acid Substances 0.000 description 1
- 150000007513 acids Chemical class 0.000 description 1
- 230000004075 alteration Effects 0.000 description 1
- 229910052782 aluminium Inorganic materials 0.000 description 1
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 description 1
- 239000000920 calcium hydroxide Substances 0.000 description 1
- 229910001861 calcium hydroxide Inorganic materials 0.000 description 1
- 239000004568 cement Substances 0.000 description 1
- 150000001875 compounds Chemical class 0.000 description 1
- 230000003750 conditioning effect Effects 0.000 description 1
- 238000011109 contamination Methods 0.000 description 1
- 238000005520 cutting process Methods 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000005553 drilling Methods 0.000 description 1
- 230000004992 fission Effects 0.000 description 1
- 238000004817 gas chromatography Methods 0.000 description 1
- 239000011521 glass Substances 0.000 description 1
- 229910052749 magnesium Inorganic materials 0.000 description 1
- 239000011777 magnesium Substances 0.000 description 1
- 230000014759 maintenance of location Effects 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 238000012544 monitoring process Methods 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 230000037361 pathway Effects 0.000 description 1
- 239000008188 pellet Substances 0.000 description 1
- 230000009257 reactivity Effects 0.000 description 1
- 230000001105 regulatory effect Effects 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- 238000005245 sintering Methods 0.000 description 1
- 239000007787 solid Substances 0.000 description 1
- 230000002269 spontaneous effect Effects 0.000 description 1
- 238000000844 transformation Methods 0.000 description 1
- 238000011144 upstream manufacturing Methods 0.000 description 1
- 239000002912 waste gas Substances 0.000 description 1
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 present invention is in the field of the treatment of nuclear waste.
- It relates in particular to the treatment of a sheath containing sintered calcium hydride (Ca3 ⁇ 4).
- This material is generally in the form of slabs which are stacked in a cylindrical sealed steel sheath.
- the nuclear waste treatment sector must neutralize the chemical risk while reducing the volume of waste as much as possible and optimizing their subsequent conditioning. In order to meet this double constraint, it would therefore be desirable to have a treatment at the end of which, on the one hand, the waste resulting from the sheath, and on the other hand the waste resulting from the hydride wafers.
- calcium irradiated are evacuated by ways adapted to the nature of each waste.
- One of the aims of the invention is to provide a process for treating a sheath containing sintered calcium hydride and optionally a radioactive material, which exhibits all or some of the aforementioned advantages.
- the present invention thus relates to a process for treating a sheath, in which there is a sintered material which consists wholly or partly of sintered calcium hydride which may optionally contain at least one radioactive material.
- the method comprises a step in which the sintered material is contacted with a reaction mixture containing 0.5% to 5% by weight of water vapor, 5% to 25% carbon dioxide and 74.5% by molar percentage. % to 94.5% of a chemically inert gas, i.e. a gas preventing a reaction between oxygen (possibly present in the reaction atmosphere) and hydrogen (produced by the carbonation reaction described hereinafter).
- a chemically inert gas i.e. a gas preventing a reaction between oxygen (possibly present in the reaction atmosphere) and hydrogen (produced by the carbonation reaction described hereinafter).
- the contacting is carried out for a time to transform all the sintered calcium hydride into a calcium carbonate powder.
- This transformation can be interrupted and resumed at the moment chosen by the operator, or its kinetics modulated depending on the amount of reaction mixture injected.
- the particular treatment method of the invention is to convert the sintered calcium hydride into a calcium carbonate powder which is non-adherent to the sheath walls and chemically inert.
- the non-adherent powder obtained at the end of the treatment process of the invention comprising calcium carbonate, is therefore naturally extracted from the sheath by simple gravity, with the radioactive material and / or any other material that may be present. 'it contains.
- This property of non-adhesion avoids at best the dissemination of radioactive material possibly present in the calcium carbonate powder, as well as the contamination of the cladding by retention of material.
- the calcium carbonate powder can be discharged to a conventional die or adapted to radioactive waste.
- waste gas such as for example hydrogen (3 ⁇ 4), optionally tritiated (HT) and / or tritium ( 2 ).
- This gaseous effluent can be extracted during or after the treatment process.
- radioactive material possibly present is found at the end of the treatment in gaseous form (such as tritiated hydrogen or tritium), it is discharged as a radioactive gaseous effluent.
- gaseous form such as tritiated hydrogen or tritium
- radioactive material there is no longer any radioactive material in the calcium carbonate powder.
- the possible initial presence of radioactive material nevertheless requires the evacuation of this powder to a simplified pathway adapted to radioactive waste, which is however less restrictive than that which would be imposed by the actual presence of a radioactive material in the waste to be discharged.
- the sheath is not altered or destroyed during the treatment of the invention, because the calcium carbonate is a relatively chemically inert compound and its formation is accompanied by a limited expansion.
- the sheath is not or only slightly contaminated with traces of calcium carbonate or any other radioactive material it contains.
- the sheath can then be evacuated to a simplified stream adapted to radioactive waste to be scrapped or recycled in the nuclear industry.
- This separation of the dies reduces the volume of waste, since obtaining a powder makes it possible to obtain a compact package and the sheath can optionally be recycled.
- the method of the invention makes it possible to treat with a minimum of manipulation a sheath containing a sintered material, which is particularly advantageous when this material contains at least one radioactive material.
- the sintered material comprises sintered calcium hydride and optionally at least one radioactive material.
- the radioactive material is for example a material containing the tritium element (T).
- the treatment method of the invention comprises a step in which the sintered material is contacted with a reaction mixture containing 0.5 mol% of steam at 25% carbon dioxide and 74.5% at 25% carbon dioxide. 94.5% of an inert gas.
- any gas that is chemically inert to calcium hydride may be suitable.
- the inert gas is for example selected from nitrogen, argon, or mixtures thereof.
- the nature and the proportion of the components of the reaction mixture allow a controlled and complete treatment of the sintered calcium hydride according to the following overall carbonation reaction:
- the time of contacting the reaction mixture with the sintered calcium hydride depends on the amount of calcium hydride and the composition of the reaction mixture. Those skilled in the art can easily adapt this duration, in particular by prolonging it until the total treatment of the sheath is obtained, which results, for example, in the end of the evolution of a gas such as hydrogen.
- the duration of contacting is for example at least
- 1 day typically between 1 day and 15 days for amounts of sintered calcium hydride to be treated of the order of one hectogram.
- the contacting is preferably carried out at a temperature of between 40 ° C. and 55 ° C. in order in particular to adjust the molar percentage of water vapor to prevent the water from condensing and reacting violently with the hydride. of calcium.
- the treatment according to the invention is most often carried out in a confinement enclosure such as a glove box or a shielded cell.
- the reaction mixture is then generally introduced into the confinement chamber at a rate allowing its continuous renewal at least once an hour.
- the propagation mode of the reaction by successive transformations in powder form of the sintered material, makes it possible to treat a sheath in which this material is relatively inaccessible, for example a sheath of complex geometry or large size.
- the sintered calcium hydride is converted into a calcium carbonate powder, but obtaining this powder does not limit the kinetics of the reaction, which makes it possible to treat the entire sintered calcium hydride present in the sheath.
- the sintered material can be in contact with the reaction mixture. Moreover, this contacting allows the calcium hydride powder to be removed from the sheath. When the sheath is sealed, it is then necessary to make at least one opening, for example by drilling or cutting the sheath.
- the sheath can be in an inclined or vertical position, in order to promote the extraction by gravity of the calcium carbonate powder (and if necessary of any material that it contains).
- the sintered calcium hydride is converted into a calcium carbonate powder containing the radioactive material (s), if appropriate, and / or any other material present initially in the sintered material or resulting from its treatment.
- This powder has no chemical reactivity with respect to water and air. In the absence of radioactive material, it can be evacuated as such to a conventional die.
- radioactive material In the presence of radioactive material, it can be incorporated in glass or cement, or dissolved in the form of Ca (HC03) 2 in most of the acids used in the nuclear waste treatment sector.
- the gases produced during the treatment process of the invention may be extracted as gaseous effluents and discharged into a specific stream in order to to be treated,
- the sheath is most often intact or has not undergone any major alteration.
- it may consist of metal (preferably a steel), plastic or ceramic.
- FIGS. 1, 2, 3 and 4 show photographic photographs taken during treatment of a sheath according to the process of the invention, the sheath containing fried pellets of calcium hydride.
- the following example deals with the treatment of a steel sheath. It is representative of a section of a sheath from a nuclear reactor type RNR that would be cut in the upper and lower part.
- the treated sheath consists of an inner tube positioned along the axis of an outer tube. It contains four pancakes obtained after the sintering of calcium hydride.
- the purity of the calcium hydride is 99% by mass. Trace impurities consist essentially of aluminum and magnesium.
- the dimensions of the sheath and a slab are as follows:
- the assembly is maintained by placing the lower part of the sheath on a removable grid disposed above a recovery tank.
- calcium hydride slabs do not contain radioactive material.
- the sheath is placed in a glove box with a volume of 550 liters serving as a reaction chamber.
- the temperature is regulated at 43 ° C.
- a reaction mixture is continuously introduced at a rate of 12 liters per minute.
- This mixture consists, in percentage by volume, of 2.5% of water vapor, 10% of carbon dioxide, the remainder being nitrogen as an inert gas.
- composition is analyzed upstream and downstream of the glove box by gas chromatography to determine the content of the following gases: N 2 , CO 2 , O 2 , H 2 .
- the amount of water vapor introduced is measured with a Peltier-type mirror hygrometer.
- the hydrogen content produced is also constantly monitored by an explosimeter.
- the carbonation reaction can be stopped by stopping the introduction of the reaction mixture. and replacing it entirely with inert gas.
- the carbonation reaction can be resumed according to its initial regime by reintroduction of steam and carbon dioxide in the glove box without this affecting the overall efficiency of the treatment process.
- the method of the invention thus allows a controlled and secure treatment.
- the reaction mixture is brought into contact with the sintered calcium hydride mainly at the outer face of the first and the last slab, but also, to a lesser extent, on the inner and outer perimeter of the slabs, which is spaced 0.5 mm from the facing surfaces of the sheath.
- Figures 1, 2, 3 and 4 reproduce the photographs taken respectively at the following times: introduction in the glove box of the reaction mixture (time to), to + 2 days, to + 4 days, to + 14 days.
- the vertical position of the sheath allows the spontaneous fall of the calcium carbonate powder and any other material it contains, such as the impurities initially present in the patties.
- the monitoring of the hydrogen content evolved during the carbonation reaction makes it possible, from the stoichiometric coefficients of the carbonation reaction, to calculate the mass of sintered calcium hydride which is converted.
- the residual mass of calcium hydride is in the recovery tank. It can be transformed in turn by extending the duration of treatment.
- the metal sheath emptied of its contents, the calcium carbonate powder and the hydrogen are evacuated according to separate channels.
- the treatment method of the invention makes it possible to completely treat a sheath, in which there is a sintered material which consists wholly or partly of sintered calcium hydride and which optionally contains at least one radioactive material, while limiting the volume of waste obtained, and by authorizing the evacuation see the valorization of this waste by adapted channels.
Landscapes
- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Processing Of Solid Wastes (AREA)
- Separation, Recovery Or Treatment Of Waste Materials Containing Plastics (AREA)
- Solid-Sorbent Or Filter-Aiding Compositions (AREA)
- Silver Salt Photography Or Processing Solution Therefor (AREA)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR1159939A FR2982407B1 (fr) | 2011-11-03 | 2011-11-03 | Procede de traitement d'une gaine contenant de l'hydrure de calcium fritte. |
PCT/FR2012/052541 WO2013064785A1 (fr) | 2011-11-03 | 2012-11-02 | Procede de traitement d'une gaine contenant de l'hydrure de calcium fritte. |
Publications (2)
Publication Number | Publication Date |
---|---|
EP2774155A1 true EP2774155A1 (de) | 2014-09-10 |
EP2774155B1 EP2774155B1 (de) | 2015-12-30 |
Family
ID=47263463
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP12794429.6A Active EP2774155B1 (de) | 2011-11-03 | 2012-11-02 | Verfahren zur behandlung einer verkleidung mit gesintertem calciumhydrid |
Country Status (8)
Country | Link |
---|---|
US (1) | US9123448B2 (de) |
EP (1) | EP2774155B1 (de) |
JP (1) | JP5745728B2 (de) |
CN (1) | CN104025205B (de) |
ES (1) | ES2566183T3 (de) |
FR (1) | FR2982407B1 (de) |
RU (1) | RU2622500C2 (de) |
WO (1) | WO2013064785A1 (de) |
Families Citing this family (2)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
FR3008222B1 (fr) | 2013-07-08 | 2015-07-31 | Commissariat Energie Atomique | Procede de traitement d'une aiguille absorbante contenant du carbure de bore contamine et du sodium. |
US11961547B2 (en) * | 2022-02-09 | 2024-04-16 | Micron Technology, Inc. | Techniques for memory system refresh |
Family Cites Families (11)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
BE572172A (de) * | 1957-10-28 | |||
US3803043A (en) * | 1966-11-15 | 1974-04-09 | Teledyne Inc | Porous metal hydride bodies |
DE3209605A1 (de) * | 1982-03-17 | 1983-09-29 | Deutsche Gesellschaft für Wiederaufarbeitung von Kernbrennstoffen mbH, 3000 Hannover | Neutronen-moderator fuer behaelter zur lagerung von abgebrannten kernbrennstoffen |
UA57884C2 (uk) * | 1999-10-14 | 2003-07-15 | Дейвід БРЕДБЕРІ | Спосіб обробки радіоактивного графіту |
FR2859042B1 (fr) * | 2003-08-19 | 2005-11-18 | Framatome Anp | Procede et installation de traitement de metaux alcalins charges en tritium ou de composants souilles par des metaux alcalins charges en tritium |
CN100364017C (zh) * | 2005-08-06 | 2008-01-23 | 西南科技大学 | 一种高放射性废物固化处理基材的制备方法 |
JP4102400B2 (ja) * | 2005-09-30 | 2008-06-18 | 独立行政法人 日本原子力研究開発機構 | 機器の除染方法及び機器の除染装置 |
WO2007055146A1 (ja) * | 2005-11-10 | 2007-05-18 | Hiromaito Co., Ltd. | 水素発生剤及びその用途 |
WO2008071215A1 (de) * | 2006-12-14 | 2008-06-19 | Horst Grochowski | Verfahren und vorrichtung zum reinigen von abgasen eines sinterprozesses von erzen und/oder anderen metallhaltigen materialien in der metallerzeugung |
FR2933227B1 (fr) | 2008-06-25 | 2010-07-30 | Commissariat Energie Atomique | Procede de traitement d'une structure contenant du sodium et une matiere radioactive |
US20110080986A1 (en) * | 2009-10-05 | 2011-04-07 | Schenter Robert E | Method of transmuting very long lived isotopes |
-
2011
- 2011-11-03 FR FR1159939A patent/FR2982407B1/fr not_active Expired - Fee Related
-
2012
- 2012-11-02 ES ES12794429.6T patent/ES2566183T3/es active Active
- 2012-11-02 WO PCT/FR2012/052541 patent/WO2013064785A1/fr active Application Filing
- 2012-11-02 CN CN201280053795.1A patent/CN104025205B/zh active Active
- 2012-11-02 RU RU2014122053A patent/RU2622500C2/ru active
- 2012-11-02 EP EP12794429.6A patent/EP2774155B1/de active Active
- 2012-11-02 JP JP2014539389A patent/JP5745728B2/ja active Active
- 2012-11-11 US US14/356,207 patent/US9123448B2/en active Active
Non-Patent Citations (1)
Title |
---|
See references of WO2013064785A1 * |
Also Published As
Publication number | Publication date |
---|---|
WO2013064785A1 (fr) | 2013-05-10 |
RU2014122053A (ru) | 2015-12-10 |
US20140309473A1 (en) | 2014-10-16 |
EP2774155B1 (de) | 2015-12-30 |
US9123448B2 (en) | 2015-09-01 |
CN104025205B (zh) | 2015-08-19 |
JP5745728B2 (ja) | 2015-07-08 |
RU2622500C2 (ru) | 2017-06-16 |
FR2982407B1 (fr) | 2013-12-27 |
FR2982407A1 (fr) | 2013-05-10 |
ES2566183T3 (es) | 2016-04-11 |
JP2015502526A (ja) | 2015-01-22 |
CN104025205A (zh) | 2014-09-03 |
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