EP0522931A1 - Block kontaminierte Ionenaustauschharze enthaltend und Herstellung davon - Google Patents

Block kontaminierte Ionenaustauschharze enthaltend und Herstellung davon Download PDF

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Publication number
EP0522931A1
EP0522931A1 EP92401879A EP92401879A EP0522931A1 EP 0522931 A1 EP0522931 A1 EP 0522931A1 EP 92401879 A EP92401879 A EP 92401879A EP 92401879 A EP92401879 A EP 92401879A EP 0522931 A1 EP0522931 A1 EP 0522931A1
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EP
European Patent Office
Prior art keywords
exchange resins
cement
ion exchange
water
epoxy resin
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
EP92401879A
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English (en)
French (fr)
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EP0522931B1 (de
Inventor
Claude Kertesz
Patrice Da Silva
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.)
Commissariat a lEnergie Atomique et aux Energies Alternatives CEA
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Commissariat a lEnergie Atomique CEA
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Publication of EP0522931A1 publication Critical patent/EP0522931A1/de
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Publication of EP0522931B1 publication Critical patent/EP0522931B1/de
Anticipated expiration legal-status Critical
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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
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/302—Processing by fixation in stable solid media in an inorganic matrix
    • G21F9/304—Cement or cement-like 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
    • G21F9/28—Treating solids
    • G21F9/30—Processing
    • G21F9/301—Processing by fixation in stable solid media
    • G21F9/307—Processing by fixation in stable solid media in polymeric matrix, e.g. resins, tars

Definitions

  • the present invention relates to a block containing ion exchange resins contaminated, for example by toxic or radioactive elements, as well as a process for preparing such a block. It is particularly applicable in the field of storage of ion exchange resins contaminated by radioactive elements of low and medium activity.
  • the ion exchange resins used to purify water in nuclear installations undergo degradation phenomena after a certain time and consequently lose their effectiveness. It is then a question of storing these used ion exchange resins which, during their use, have fixed various radioelements giving them a certain radioactivity.
  • thermosetting resins such as those described in documents FR-A- 2 251 081, FR-A- 2 361 724 and EP-A- 0 127 490 are satisfactory because they allow to ensure good retention of radioactivity, but they nevertheless have certain drawbacks.
  • EP-A-0 127 490 also makes it possible to incorporate cationic resins which still have active sites into an epoxy resin, but it has the disadvantage of requiring the use of particular amine hardeners which are relatively expensive products. .
  • thermosetting resins are sensitive to the initial temperature which accelerates the polymerization and / or leads to a release of heat detrimental to the quality of the block formed.
  • radioactive waste consists of chemical co-precipitation sludge which may contain 20 to 40% of water, dry pulverulent waste such as the incineration ashes of combustible materials or technological, non-combustible waste such as glass and metals.
  • the present invention specifically relates to a block containing ion exchange resins contaminated for storage, which overcomes the drawbacks mentioned above of the known methods.
  • the block containing ion exchange resins contaminated for storage is characterized in that the ion exchange resins are incorporated in a composite matrix consisting of a hardened hydrophilic epoxy resin and a cement. hardened chosen from Clinker's slag cements and slag and ash cements.
  • the choice of a hydrophilic epoxy resin and a cement with a low heat of hydration constitutes by a clinker slag cement (CLK) and / or a slag cement and with fly ash ( CLC) provides a matrix compatible with ion exchange resins, even when these are saturated with water and contain, for example, 50 to 55% by weight of water, and / or contain active sites usually requiring pretreatment.
  • CLK clinker slag cement
  • CLC fly ash
  • this matrix makes it possible to obtain a high coating coefficient and a block having very interesting physical and mechanical properties, in particular better resistance to compression.
  • CLC and CLK cements have very different compositions from those of Portland cements and aluminous cements.
  • CLK and CLC cements have lower hydration heats than those of Portland and aluminous cements and a slower hydration kinetics.
  • the temperature can reach 120 ° C at the core, which causes the distillation of the water included in the exchange resins d 'ions and a degradation of the properties of the barrel.
  • the proportions by weight of hardened cement and epoxy resin used in the constitution of the matrix are chosen so as to obtain the desired characteristics of radioelement retention, resistance to leaching and mechanical resistance for storage. of the block with a high degree of safety.
  • ion exchange resins With this matrix, relatively large amounts of ion exchange resins can be included in the block; it can thus contain up to 45% by weight of contaminated ion exchange resins, saturated with water, whereas in the in the case of CLK cement alone, only 15 to 20% by weight of ion exchange resins could be coated.
  • ion exchange resins can be constituted by cationic exchange resins, anionic resins or mixtures of these resins, in the form of grains or particles obtained by grinding.
  • organic ion exchange resins such as polystyrene resins crosslinked with divinyl benzene which comprise, for example, sulfonic groups or hydroxyl groups.
  • a hydrophilic epoxy resin is used, compatible both with the cement used and with the ion exchange resin to be conditioned.
  • hydrophilic epoxy resins By way of example of such hydrophilic epoxy resins, mention may be made of the diglycidyl ether of bis-phenol-A and the diglycidyl ether of bis-phenol-F hardened by reaction with an amino hardener.
  • the diglycidyl ether of bis phenol A corresponds to the formula:
  • the bis-phenol F diglycidyl ether corresponds to the formula:
  • the use of a hydrophilic epoxy resin is advantageous because it facilitates obtaining a homogeneous mixture with the cement, in the presence of water.
  • the invention also relates to a process for the preparation of the block containing the contaminated ion exchange resins, described above.
  • the contaminated ion exchange resins are saturated with water, which is done by immersing these resins in water for a sufficient time, for example for 24 hours. After this operation, the ion exchange resins are drained until disappearance of the water flow in order to ensure that the ion exchange resins contain only their saturation water which generally represents approximately 50 to 55% by weight of the saturated ion exchange resins, but can go in certain case up to 65% by weight.
  • the water necessary for the hydration of the cement is then added to the resins by carrying out this operation with stirring.
  • the amount of water of hydration needed for curing Clinker's slag cements or slag and fly ash cements depends on the amount of cement that will be introduced into the block. It is generally such that the hydration water / cement weight ratio is from 0.25 to 0.35.
  • the cement After introduction of the water, the cement is added with stirring and this stirring is continued until a fluid paste is obtained, then the epoxy resin in the liquid state and its amine hardener are added, continuing the agitation.
  • the operations of adding water, cement and epoxy resin are carried out in a mixer.
  • the mixture After adding the epoxy resin and its hardener, the mixture can be emulsified by rotation at high speed, left to stand and poured into a mold having the dimensions of the block to be manufactured.
  • the block is allowed to harden in the mold, which can be obtained relatively quickly, for example in 12 hours.
  • the choice of the amine hardener is also important, because by choosing an appropriate amine hardener, the epoxy resin is allowed to harden in the presence of large amounts of water.
  • amine hardeners containing a combination of aromatic and aliphatic amines it is possible to use amine hardeners containing a combination of aromatic and aliphatic amines, and by varying the amounts of these different amines, an optimized hardener can be obtained, suitable for the preparation of an epoxy composite matrix. cement suitable for coating ion exchange resins saturated with water to be conditioned.
  • the proportion of amine hardener is such that the hardener / epoxy resin weight ratio is preferably from 0.5 to 0.6.
  • the contaminated water exchange resins are saturated with water by swelling them in water for 24 h and then subjected to a spin. 400 g of drained anionic resins are then weighed and the 78 g of water added to them, that is to say the amount sufficient to hydrate the 222 g of CLK 45 cement.
  • the resins are mixed with water, then the CLK 45 cement is added to the suspension and the mixture is kneaded so as to obtain a very fluid paste.
  • the block obtained is also subjected to a water absorption test by immersing it for one month in water. After this period, it can be seen that the mass coefficient of water absorption is of the order of 1 to 3%.
  • the block obtained therefore has very satisfactory characteristics for the storage of anion exchange resins.
  • Example 2 The same contaminated anion exchange resins and the same matrix constituents are used as in Example 1, except the hardener which in this example is the product sold by Spado Lassailly under the reference SL D 2005.
  • Example 2 The same procedure is followed as in Example 1, using the same proportions for coating 400 g of anion exchange resins in the composite matrix.
  • a solid block is thus obtained having properties practically identical to those of the block obtained in Example 1, except that its external appearance is more shiny.
  • Example 2 The same procedure is followed and the same matrix is used as in Example 1 to coat 400 g of cationic ion exchange resins of the Rohm and Haas IR 120 type.
  • the block obtained also has very good properties.
  • the coating of contaminated ion exchange resins is carried out using only as coating component an epoxy resin and its hardener.
  • an epoxy-cement composite matrix makes it possible, during polymerization, to limit the core temperature of the block to a value lower than that which is obtained with an epoxy resin alone.
  • the core temperature is limited to 58-63 ° C, while in the case of an epoxy resin alone, it can reach 78 ° C for a block of 0.5 l. Also, for blocks of larger volume, the core temperature can become higher than 100 ° C with an epoxy resin alone. However, at this temperature, the water contained in the ion-exchange resins saturated with water is brought to the boil and the water vapor generated in the block is the cause of more or less significant damage.
  • the enthalpy corresponding to the setting of the binder is very substantially lower than the enthalpy of polymerization of the epoxy part.
  • curve A corresponds to the average values of the two curves in FIG. 2
  • curve B corresponds to the average values of the two curves of FIG. 3.
  • the reduction of the peak of the polymerization exotherm is particularly sought after, because it increases the intrinsic safety of the process, in particular in the event of acceleration of the polymerization rate observed in hot weather: in this case, in Indeed, the polymerization kinetics is increased, and the temperature obtained at the core of the coating must imperatively be below the vaporization temperature of the REI water.
  • the lengthening of the hardening time is an interesting phenomenon at the industrial stage because it allows increased possibilities of intervention on the process.
  • Another important advantage of the process of the invention is that it allows the coating of anionic, cationic or mixed ion exchange resins without requiring pretreatment. Indeed, the use of a hydraulic binder which releases in the aqueous medium dissociated ions, avoids prior saturation of any active sites of cation exchange resins since the ions released by the cement are capable of achieving this saturation.

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  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Epoxy Resins (AREA)
  • Processing Of Solid Wastes (AREA)
  • Curing Cements, Concrete, And Artificial Stone (AREA)
EP19920401879 1991-07-03 1992-07-01 Block kontaminierte Ionenaustauschharze enthaltend und Herstellung davon Expired - Lifetime EP0522931B1 (de)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
FR9108309 1991-07-03
FR9108309A FR2678761B1 (fr) 1991-07-03 1991-07-03 Bloc contenant des resines echangeuses d'ions contaminees et son procede de preparation.

Publications (2)

Publication Number Publication Date
EP0522931A1 true EP0522931A1 (de) 1993-01-13
EP0522931B1 EP0522931B1 (de) 1997-04-02

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Family Applications (1)

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EP19920401879 Expired - Lifetime EP0522931B1 (de) 1991-07-03 1992-07-01 Block kontaminierte Ionenaustauschharze enthaltend und Herstellung davon

Country Status (4)

Country Link
EP (1) EP0522931B1 (de)
DE (1) DE69218680T2 (de)
ES (1) ES2102477T3 (de)
FR (1) FR2678761B1 (de)

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4324818A1 (de) * 1993-07-23 1995-01-26 Siemens Ag Verfahren zum Entsorgen von Ionenaustauscherharz
FR2742256A1 (fr) * 1995-12-11 1997-06-13 Korea Atomic Energy Res Methode de solidification de dechets radioactifs sans bore sous forme vitrifiee en utilisant des cendres volantes et des dechets radioactifs contenant du bore en tant que frittes de verre borosilicate
US6231664B1 (en) * 1998-06-30 2001-05-15 Halliburton Energy Services, Inc. Well sealing compositions and methods
US6234251B1 (en) 1999-02-22 2001-05-22 Halliburton Energy Services, Inc. Resilient well cement compositions and methods
US6244344B1 (en) 1999-02-09 2001-06-12 Halliburton Energy Services, Inc. Methods and compositions for cementing pipe strings in well bores
US6279652B1 (en) 1998-09-23 2001-08-28 Halliburton Energy Services, Inc. Heat insulation compositions and methods
US6287772B1 (en) 1998-04-29 2001-09-11 Boston Probes, Inc. Methods, kits and compositions for detecting and quantitating target sequences
FR2825182A1 (fr) * 2001-05-23 2002-11-29 Qualia Systeme matriciel pour l'enrobage et le stockage d'un produit dangereux, procede de preparation et utilisation notamment pour les resines echangeuses d'ions faiblement radioactives
WO2009090209A1 (de) * 2008-01-17 2009-07-23 Areva Np Gmbh Verfahren zur konditionierung radioaktiver ionenaustauscherharze

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0124825A2 (de) * 1983-04-29 1984-11-14 W.R. Grace & Co. Einkapseln von radioaktiven Abfällen
EP0127490A1 (de) * 1983-04-21 1984-12-05 Commissariat A L'energie Atomique Verfahren zur Konditionierung von in saurem Medium kontaminierten Abfällen, insbesondere von Kationenaustauschermaterialien
FR2607957A1 (fr) * 1986-12-05 1988-06-10 Commissariat Energie Atomique Bloc contenant des dechets en vue de leur stockage et procede de realisation d'un tel bloc
EP0318367A1 (de) * 1987-11-23 1989-05-31 Commissariat A L'energie Atomique Verfahren zur Konditionierung von radioaktiven oder toxischen Abfällen in wärmehärtbaren Harzen

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0127490A1 (de) * 1983-04-21 1984-12-05 Commissariat A L'energie Atomique Verfahren zur Konditionierung von in saurem Medium kontaminierten Abfällen, insbesondere von Kationenaustauschermaterialien
EP0124825A2 (de) * 1983-04-29 1984-11-14 W.R. Grace & Co. Einkapseln von radioaktiven Abfällen
FR2607957A1 (fr) * 1986-12-05 1988-06-10 Commissariat Energie Atomique Bloc contenant des dechets en vue de leur stockage et procede de realisation d'un tel bloc
EP0318367A1 (de) * 1987-11-23 1989-05-31 Commissariat A L'energie Atomique Verfahren zur Konditionierung von radioaktiven oder toxischen Abfällen in wärmehärtbaren Harzen

Cited By (11)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE4324818A1 (de) * 1993-07-23 1995-01-26 Siemens Ag Verfahren zum Entsorgen von Ionenaustauscherharz
DE4324818C2 (de) * 1993-07-23 2002-06-27 Framatome Anp Gmbh Verfahren zum Entsorgen von Ionenaustauscherharz
FR2742256A1 (fr) * 1995-12-11 1997-06-13 Korea Atomic Energy Res Methode de solidification de dechets radioactifs sans bore sous forme vitrifiee en utilisant des cendres volantes et des dechets radioactifs contenant du bore en tant que frittes de verre borosilicate
US6287772B1 (en) 1998-04-29 2001-09-11 Boston Probes, Inc. Methods, kits and compositions for detecting and quantitating target sequences
US6231664B1 (en) * 1998-06-30 2001-05-15 Halliburton Energy Services, Inc. Well sealing compositions and methods
US6279652B1 (en) 1998-09-23 2001-08-28 Halliburton Energy Services, Inc. Heat insulation compositions and methods
US6244344B1 (en) 1999-02-09 2001-06-12 Halliburton Energy Services, Inc. Methods and compositions for cementing pipe strings in well bores
US6234251B1 (en) 1999-02-22 2001-05-22 Halliburton Energy Services, Inc. Resilient well cement compositions and methods
FR2825182A1 (fr) * 2001-05-23 2002-11-29 Qualia Systeme matriciel pour l'enrobage et le stockage d'un produit dangereux, procede de preparation et utilisation notamment pour les resines echangeuses d'ions faiblement radioactives
WO2009090209A1 (de) * 2008-01-17 2009-07-23 Areva Np Gmbh Verfahren zur konditionierung radioaktiver ionenaustauscherharze
US8372289B2 (en) 2008-01-17 2013-02-12 Areva Np Gmbh Method for conditioning radioactive ion exchange resins

Also Published As

Publication number Publication date
DE69218680T2 (de) 1997-10-23
EP0522931B1 (de) 1997-04-02
FR2678761A1 (fr) 1993-01-08
ES2102477T3 (es) 1997-08-01
FR2678761B1 (fr) 1994-07-01
DE69218680D1 (de) 1997-05-07

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