US3142648A - Process for the production of solid products containing radioactive waste material and products obtained by this process - Google Patents

Process for the production of solid products containing radioactive waste material and products obtained by this process Download PDF

Info

Publication number
US3142648A
US3142648A US242800A US24280062A US3142648A US 3142648 A US3142648 A US 3142648A US 242800 A US242800 A US 242800A US 24280062 A US24280062 A US 24280062A US 3142648 A US3142648 A US 3142648A
Authority
US
United States
Prior art keywords
bitumen
water
mud
temperature
mixing
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
Application number
US242800A
Other languages
English (en)
Inventor
Lefillatre Guy
Rodier Jean
Scheidhauer Jean
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
Original Assignee
Commissariat a lEnergie Atomique CEA
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 Commissariat a lEnergie Atomique CEA filed Critical Commissariat a lEnergie Atomique CEA
Application granted granted Critical
Publication of US3142648A publication Critical patent/US3142648A/en
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • GPHYSICS
    • G21NUCLEAR PHYSICS; NUCLEAR ENGINEERING
    • G21FPROTECTION AGAINST X-RADIATION, GAMMA RADIATION, CORPUSCULAR RADIATION OR PARTICLE BOMBARDMENT; TREATING RADIOACTIVELY CONTAMINATED MATERIAL; DECONTAMINATION ARRANGEMENTS THEREFOR
    • G21F9/00Treating radioactively contaminated material; Decontamination arrangements therefor
    • G21F9/04Treating liquids
    • G21F9/06Processing
    • G21F9/16Processing by fixation in stable solid media
    • G21F9/167Processing by fixation in stable solid media in polymeric matrix, e.g. resins, tars

Definitions

  • the first treatment envisaged generally has the effect of obtaining a mud which is as thick as possible, that is to say containing as little liquid as possible (generally water).
  • This treatment usually involves evaporation, absorption of radioactive ions on ion-exchange resins and/ or co-precipitation.
  • a subsequent treatment has the purpose of trans-. forming the mud into a generally solid product in the form of blocks, which may or may not be enclosed in receptacles, and which are stored under the ground or in the sea.
  • such blocks can also be obtained from solid radioactive waste materials (earths, constructional materials, ash, etc.) for example by coating with cement.
  • This treatment generally consists in directly passing to the solid state, without any drying step, however, which is not economic, because of the appreciable waste of heat and the necessity for a subsequent agglomeration stage in a moist medium, the treatment also giving rise to a considerable problem as to the trapping of radioactive dust formed during the agglomeration.
  • the present invention has the object of providing a process for the manufacture of solid products containing radio-active waste materials which overcomes these disadvantages; these solid products are obtained in a form which does not involve any risk of contamination.
  • the process consists essentially in that, at a temperature between the ambient temperature and 95 C., the mud is mixed with a fiuidified atent ice bitumen, in the presence of a surface-active or wetting agent which serves to permit coating of the mud and to facilitate separation of water contained therein, the greater part of this water then being eliminated by decantation and/ or by means of a mechanical device and the bituminous mastic thus obtained then being further mixed at a temperature such that it becomes sufficiently fluid and is finally poured in order to obtain, on cooling, solid blocks of suitable plasticity.
  • bituminous mastic After elimination of the larger part of the water, and before the second mixing, the bituminous mastic can be raised to a temperature of approximately 100 C. in order to distil off completely the residual water.
  • the products obtained according to this process are also included in the present invention in the form of novel industrial products.
  • the addition of one (or more) wetting agents has the object of facilitating, with agitation, the production of a water/mud solids/bitumen mixture, as a result of its emollient or softening properties. Also, when the agitation is stopped, this addition permits separation of the larger part of the water of the mud, the quantity of water separating being greatly superior to that obtained by the process referred to above.
  • the surfactant or wetting agent also has the object of improving the adhesion of the bitumen with respect to the particles in suspension in the mud, which facilitates coating of these particles with the bitumen.
  • Separation of the water can occur, when the agitation ends, at the temperature at which the mixing has taken place. It can also be carried out more rapidly or can be completed by passing through a suitable mechanical device (for example, a mixer).
  • a suitable mechanical device for example, a mixer
  • the total proportion of the wetting agent with respect to the bitumen added preferably lies between 1 and 20%.
  • the wetting agent can, for example, be mixed with the mud before addition of the bitumen. It can also be incorporated in the bitumen before contacting it with the mud.
  • the bitumen can be fluidified, for example, by elevation of the temperature or by admixture with a certain proportion of non-polar solvents. In the latter case, the thus-fluidified bitumen contains preferably 6080% bitumen per se, 15-33% of non-polar solvents and 17% of wetting agents.
  • the quantity of water eliminated without using distillation can comprise of the total water in the mud. It can be taken that, if distillation of the residual water is begun when the bituminous mastic still contains 40% of the water from the mud, the process is no longer economic. It is thus important for the elimination of the water before distillation to be at least 60% of the total water of the mud, which can readily be obtained in any case.
  • the present invention allows the use of bitumens which have softening points higher than those of the bitumens utilised in prior art processes, which allows final products of suitable plasticity to be obtained.
  • the introduction of the bitumen can take place in a single stage, before separation of the water, or in two stages, a first stage before separation of the Water and a second stage after distilling off the residual water.
  • the bitumen added after distilling off the water preferably has a softening point which is higher than that added before separation of the water.
  • a product is then obtained which has a suitable plasticity and is resistant to shock.
  • the temperature at which the first mixing takes place then being from 60 to 90 C. If all the water is eliminated, the residual water is distilled off in the vicinity of 100 C. and, during the second mixing, the temperature rises to 100 to 160 C. If total elimination of the water by distillation is not effected, the temperature during the second mixing is maintained at 60 to 90 C. A final product is then obtained which contains about 5-10% of water. Depending upon the storage conditions envisaged, the products can ensure the desired retention of the radio elements, despite its water content. In certain cases, this allows simplification of the process and apparatus and thus also ensures a more rapid treatment of the radioactive mud.
  • bitumen is preferably used before separation of the water which has a lower softening point than that in the preceding case, for example of 3045 C.
  • This bitumen is fluidified by addition of a non-polar solvent, which allows mixing to occur at the ambient temperature.
  • a second bitumen preferably having a softening point of 80130 C., is added during the second mixing stage after elimination of the residual Water by distillation, the temperature then being 120160 C.
  • the coating obtained according to the process of the invention ensures, in the best conditions, retention of the radio-elements in the final product and perfect cohesion of this product. Economic and total elimination of the water can, if desired, readily be obtained. In all cases, as the various starting materials are inexpensive, the process of the invention is thus very economic.
  • the bituminous mastic obtained after completion of the coating step is poured hot or cast in order to obtain on cooling a final product in the form of blocks; this operation can be effected in receptacles which can be the subsequent storage receptacles. These blocks can also be stored, after removal from the moulds, without protective receptacles or introduced into other storage receptacles.
  • this mastic can be poured in any suitable form and, if desired, can be subjected to an agglomeration operation, for example, formed into briquettes.
  • the total quantities of bitumen added are variable and depend upon the initial proportion of water in the mud. These quantities generally correspond however to a weight proportion of 2842 in the product, which corresponds to a weight proportion of bitumen with respect to the dry mud between 40 and 70%.
  • the ratio weight of final product/Weight of mud treated can thusbe of the order of 0.38-0.75, while the ratio volume of final product/volume of mud treated can be between 0.35 and 0.60 (for mud containing initially 50-75% of water).
  • Example I 100 kg. of a radioactive mud, containing about 60% of water and having an activity of the order of 4 curies per metric ton, were introduced into a double-jacketed mixer heated by circulation of a hot fiuid. A special surface-active or wetting agent soluble in the water constituting the mud was then added, comprising potassium naphthenate. The amount of Wetting agent depended upon the quantity of bitumen which was to be added later, namely 15% by weight with respect to the bitumen.
  • the bitumen was introduced at its pumping temperature, namelyl10-l30 C.
  • the quantity of bitumen added was determined as a function of the water content of the mud and its particle size range (by weight, 4.5%, 55%, 28% and 12.5% of the particles had dimensions greater than 34 1., from 12 to 34 from 5.5. to 1 2 and from 1.4 to 5.5,u respectively).
  • the bituminous mastic thus obtained having a weight of about 64 kg, was subjected to distillation with agitation. All the water still contained in the mastic (about 6.5% by weight of the mastic) was distilled off and condensed. This water was less radioactive than the former (about 1000 times less) and could be put into the drain without danger. The temperature was then taken above C. and mixing was carried out to obtain a suitable viscosity, which was obtained at a temperature of C.
  • Coating was thus suitably effected and the product (about 60 kg.) was poured hot into special receptacles.
  • the mixer used for mixing before separation of the water was also employed after distillation of the residual water, so that up to the pouring step, the process can be carried out in the same apparatus.
  • This mixture employs simultaneous contrary kneading, two vertical interfitting supports causing the kneading having different speeds of rotation. Also, a scraper operates against the vertical wall of the casing of the mixture.
  • the pouring orifice was provided with a hinged cover or with a flow recorder at the base of the casing, which allows total recovery of the final product.
  • Example 11 17 kg. of a fluidified bitumen comprising by Weight 70% of bitumen per se, 6% of a wetting agent constituted by calcium naphthenate and 24% of non-polar solvents (for example of the kerosene type) were introduced into a mixer. 100 kg. of radioactive mud containing 50% of water were then introduced into the mixture at a rate of 100 litres/hour. The mixture was slowly kneaded at the ambient temperature. When about half the mud had been added, the clear water exuded from the mud separated from the bituminous mastic being formed. When all the mud had been added, the decanted water was pumped off. The mixer was emptied and separation of the mastic and water was completed by means of a special screw or cylinder system (the total amount of water this eliminated represents 80% of the water contained in the mud).
  • a special screw or cylinder system the total amount of water this eliminated represents 80% of the water contained in the mud.
  • the bitumen used had the following characteristics: Direct distillation bitumen- Penetration at 25 C. (NFT standard 66.004), 180 to 220 (in tenths of a millimetre);
  • the bituminous mastic thus obtained had a Weight of about 75 kg. and was forwarded under gravity to a second double-jacketed mixer heated by circulation of a heating fluid. It was subjected to distillation under agitation. All the water in the mastic was distilled off, as well as the major part of the non-polar solvents contained in the fiuidified bitumen.
  • the mixers used can be of the same type as those referred to in Example I.
  • Average pumping temperature in C. 150-195 C.
  • the ratio of the mass of the product obtained (density 1.47) to the mass of the initial mud (density 1.58) was about 0.8 and the corresponding volume ratio was about 0.7.
  • a process for the production of solid products containing radioactive waste material which comprises mixing an aqueous radioactive mud with a fluidified bitumen in the presence of a wetting agent for a time sufiicient to eliminate a major proportion of the water and so form a bituminous mastic containing the mud solids in a coated form.
  • a process for the production of solid products of low activity containing radio-elements present in radioactive waste material, previously put into the form of radioactive muds, by the addition of bitumen to the mud comprising the steps of admixing a fiuidified bitumen with the mud in the presence of a surface-active agent at a [temperature between the ambient temperature and C. to permit coating of the mud and to facilitate separation of water contained in the mud, eliminating the major part of such water and working the bituminous mastic thus obtained at a temperature such that it becomes sufficiently fluid and is finally poured in order to obtain, on cooling, solid blocks of suitable plasticity.
  • bitumen is fluidified by elevation of its temperature.
  • bitumen is fluidified by addition of non-polar solvents.
  • bitumen is a direct distilled bitumen with a softening point of 40 to 65 C., the temperature before separation of the water being 60 to 90 C.

Landscapes

  • Physics & Mathematics (AREA)
  • Engineering & Computer Science (AREA)
  • General Engineering & Computer Science (AREA)
  • High Energy & Nuclear Physics (AREA)
  • Treatment Of Sludge (AREA)
  • Processing Of Solid Wastes (AREA)
  • Removal Of Floating Material (AREA)
US242800A 1961-12-06 1962-12-06 Process for the production of solid products containing radioactive waste material and products obtained by this process Expired - Lifetime US3142648A (en)

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
FR881196A FR1315162A (fr) 1961-12-06 1961-12-06 Procédé de fabrication de produits solides renfermant des déchets radioactifs et produits obtenus selon ce procédé

Publications (1)

Publication Number Publication Date
US3142648A true US3142648A (en) 1964-07-28

Family

ID=8768216

Family Applications (1)

Application Number Title Priority Date Filing Date
US242800A Expired - Lifetime US3142648A (en) 1961-12-06 1962-12-06 Process for the production of solid products containing radioactive waste material and products obtained by this process

Country Status (12)

Country Link
US (1) US3142648A (de)
AT (1) AT245695B (de)
BE (1) BE625756A (de)
CH (1) CH413142A (de)
DE (1) DE1464476A1 (de)
DK (1) DK113509B (de)
ES (1) ES283165A1 (de)
FR (1) FR1315162A (de)
GB (1) GB959751A (de)
LU (1) LU42815A1 (de)
NL (1) NL286324A (de)
YU (1) YU32070B (de)

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3298961A (en) * 1965-08-26 1967-01-17 George D Davis Concentration and containment of radioactivity from radioactive waste solutions in asphalt
US3883441A (en) * 1970-07-20 1975-05-13 Atcor Inc Apparatus for fixing radioactive waste
US3966175A (en) * 1971-09-20 1976-06-29 Stock Equipment Company Apparatus for introducing particulate material into a container
US3986977A (en) * 1975-02-03 1976-10-19 Nuclear Engineering Company, Inc. Methods of disposing of radioactive waste
US4009116A (en) * 1973-12-20 1977-02-22 Bayer Aktiengesellschaft Process of preparing substantially organic waste liquids containing radioactive or toxic substances for safe, non-pollutive handling, transportation and permanent storage
US4010108A (en) * 1972-01-24 1977-03-01 Nuclear Engineering Company, Inc. Radioactive waste disposal of water containing waste using urea-formaldehyde resin
US4139488A (en) * 1975-06-26 1979-02-13 Vereinigte Edelstahlwerke Aktiengesellschaft Method of preparing solid radioactive or toxic waste for long-term storage
EP0005902A1 (de) * 1978-05-18 1979-12-12 Imperial Chemical Industries Plc Selbst- oder mit Wasser abbindende Isocyanat-Zusammensetzungen und Verfahren zu ihrer Herstellung
US4196169A (en) * 1974-06-27 1980-04-01 Nuclear Engineering Company, Inc. System for disposing of radioactive waste
US4235737A (en) * 1977-12-29 1980-11-25 Komrow Robert R Method for treating radioactive liquids
US4440673A (en) * 1979-03-22 1984-04-03 Rheinisch-Westfalisches Elektrizitatswerk Ag Method of and apparatus for the treatment of radioactive waste water from nuclear power plants
US4513205A (en) * 1982-07-28 1985-04-23 Peckson Usa Corp. Inner and outer waste storage vaults with leak-testing accessibility
US4832874A (en) * 1986-07-04 1989-05-23 Ebara Corporation Method of solidifying radioactive waste and solidified product thereof
US4847006A (en) * 1985-08-30 1989-07-11 Hoeglund Lars O Encapsulated ion-exchange resin and a method for its manufacture

Families Citing this family (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4056362A (en) * 1972-01-24 1977-11-01 Nuclear Engineering Co., Inc. System for disposing of radioactive waste
DE2238694C2 (de) * 1972-08-05 1983-12-22 Kernforschungszentrum Karlsruhe Gmbh, 7500 Karlsruhe Verfahren zur Aufbereitung einer bei der Wiederaufarbeitung bestrahlter Kernbrenn- und/oder Brutstoffe verwendeten Phosphorsäureester und Kohlenwasserstoffe enthaltenden Abfallflüssigkeit
DE2714672A1 (de) * 1976-04-02 1977-11-10 Bofors Ab Verfahren zum abtrennen von festen, radioaktiven bestandteilen aus fluessigem abfall und ueberfuehren in einheiten fuer die langzeitlagerung
DE3048543C2 (de) * 1980-12-22 1983-03-17 Werner & Pfleiderer, 7000 Stuttgart Verfahren zur Verfestigung radioaktiver Abfallkonzentrate in Bitumen

Non-Patent Citations (1)

* Cited by examiner, † Cited by third party
Title
None *

Cited By (14)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3298961A (en) * 1965-08-26 1967-01-17 George D Davis Concentration and containment of radioactivity from radioactive waste solutions in asphalt
US3883441A (en) * 1970-07-20 1975-05-13 Atcor Inc Apparatus for fixing radioactive waste
US3966175A (en) * 1971-09-20 1976-06-29 Stock Equipment Company Apparatus for introducing particulate material into a container
US4010108A (en) * 1972-01-24 1977-03-01 Nuclear Engineering Company, Inc. Radioactive waste disposal of water containing waste using urea-formaldehyde resin
US4009116A (en) * 1973-12-20 1977-02-22 Bayer Aktiengesellschaft Process of preparing substantially organic waste liquids containing radioactive or toxic substances for safe, non-pollutive handling, transportation and permanent storage
US4196169A (en) * 1974-06-27 1980-04-01 Nuclear Engineering Company, Inc. System for disposing of radioactive waste
US3986977A (en) * 1975-02-03 1976-10-19 Nuclear Engineering Company, Inc. Methods of disposing of radioactive waste
US4139488A (en) * 1975-06-26 1979-02-13 Vereinigte Edelstahlwerke Aktiengesellschaft Method of preparing solid radioactive or toxic waste for long-term storage
US4235737A (en) * 1977-12-29 1980-11-25 Komrow Robert R Method for treating radioactive liquids
EP0005902A1 (de) * 1978-05-18 1979-12-12 Imperial Chemical Industries Plc Selbst- oder mit Wasser abbindende Isocyanat-Zusammensetzungen und Verfahren zu ihrer Herstellung
US4440673A (en) * 1979-03-22 1984-04-03 Rheinisch-Westfalisches Elektrizitatswerk Ag Method of and apparatus for the treatment of radioactive waste water from nuclear power plants
US4513205A (en) * 1982-07-28 1985-04-23 Peckson Usa Corp. Inner and outer waste storage vaults with leak-testing accessibility
US4847006A (en) * 1985-08-30 1989-07-11 Hoeglund Lars O Encapsulated ion-exchange resin and a method for its manufacture
US4832874A (en) * 1986-07-04 1989-05-23 Ebara Corporation Method of solidifying radioactive waste and solidified product thereof

Also Published As

Publication number Publication date
ES283165A1 (es) 1963-02-01
GB959751A (en) 1964-06-03
BE625756A (de)
DE1464476B2 (de) 1970-10-29
NL286324A (de)
YU32070B (en) 1974-04-30
DK113509B (da) 1969-03-31
FR1315162A (fr) 1963-01-18
LU42815A1 (de) 1963-02-05
YU163162A (en) 1973-10-31
DE1464476A1 (de) 1969-03-06
AT245695B (de) 1966-03-10
CH413142A (fr) 1966-05-15

Similar Documents

Publication Publication Date Title
US3142648A (en) Process for the production of solid products containing radioactive waste material and products obtained by this process
US2390860A (en) Purification of plant rubbers
US2829982A (en) Process of coating granules with a thermosetting resin
Kampouris et al. Solvent recycling of rigid poly (vinyl chloride) bottles
CA1169737A (en) Method of treating water-in-oil dispersions
DE2549195A1 (de) Verfahren, um verbrauchte, kornfoermige, organische ionenaustauschmasse in zement einzubetten
DE3630132C2 (de) Verfahren zur Herstellung einer elastischen bituminösen Isolier- und Dichtungsmasse
US2807556A (en) Process for producing dry, free-flowing, thermosetting resin-coated sand granules
US4432837A (en) Solvent recovery process
US3043785A (en) Depigmenting polymeric compositions with aliphatic carboxylic acid settling aids
EP0168638B1 (de) Verfahren zur Herstellung deponierbarer Produkte aus umweltgefährdeten Salzgemischen
EP0240983A3 (de) Kompaktes Agglomerat von Polymerlatexpartikeln
DE2714672A1 (de) Verfahren zum abtrennen von festen, radioaktiven bestandteilen aus fluessigem abfall und ueberfuehren in einheiten fuer die langzeitlagerung
WO1995009196A1 (en) Method for compacting expanded polystyrene, and compacted mass thus obtained
US5298128A (en) Process for recovering polyurethane from polyurethane waste pastes
DE3529264A1 (de) Verfahren und vorrichtung zur neutralisierung von schadstoffhaltigen rueckstaenden
Franz et al. Immobilization of sodium nitrate waste with polymers: Topical report
JPS62112100A (ja) 付加重合可能な基を持つ物体の容積を減少させる方法
JPS5815756B2 (ja) スラリ状廃液物または放射性廃液物の固化体製造方法
US2243700A (en) Molding composition and method of making
AT379250B (de) Einbettungsmasse und verfahren zum einbetten von anionenaustauscherharzen bzw. diese enthaltenden gemischen
CA1171022A (en) Solvent recovery process
JP3136297B2 (ja) 粒状瀝青物の製造法
Ham et al. The development of a leaching test for industrial wastes
Pordes et al. Encapsulation of radioactive waste