EP0082061B1 - Procédé et dispositif de traitement de solutions contenant de l'eau tritiée, électrode utilisable dans un tel dispositif et son procédé de préparation - Google Patents
Procédé et dispositif de traitement de solutions contenant de l'eau tritiée, électrode utilisable dans un tel dispositif et son procédé de préparation Download PDFInfo
- Publication number
- EP0082061B1 EP0082061B1 EP82402226A EP82402226A EP0082061B1 EP 0082061 B1 EP0082061 B1 EP 0082061B1 EP 82402226 A EP82402226 A EP 82402226A EP 82402226 A EP82402226 A EP 82402226A EP 0082061 B1 EP0082061 B1 EP 0082061B1
- Authority
- EP
- European Patent Office
- Prior art keywords
- cathode
- solution
- palladium
- tritium
- cell
- 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
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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
- G21F9/04—Treating liquids
- G21F9/06—Processing
Definitions
- the subject of the present invention is a method and a device for the treatment by electrolysis of solutions containing tritiated water such as effluents from plants for reprocessing irradiated nuclear fuels, water for cooling light water or water reactors. heavy and effluents from laboratories where tritium is handled.
- solutions containing tritiated water such as effluents from plants for reprocessing irradiated nuclear fuels, water for cooling light water or water reactors. heavy and effluents from laboratories where tritium is handled.
- aqueous solutions containing a large quantity of tritiated water for example a content of approximately 40 Ci / m 3 , are obtained at certain stages of reprocessing. These solutions are generally obtained during the concentration by evaporation of uranium, plutonium or fission product solutions, or during the regeneration treatment of nitric acid with a view to its recycling at the dissolving stage of irradiated fuel elements. . In the latter case, these solutions are obtained during the concentration of the nitric acid which has been formed by regenerating by means of water vapor the nitrogen oxides originating from the step of destruction of the nitric acid by the formalin. It is also possible to envisage higher concentrations, either by recycling the nitric solutions, or by isotopic concentration of the effluents.
- the present invention specifically relates to a process for treating solutions containing water formed from an isotope of hydrogen, which is suitable for the treatment of tritiated water and makes it possible to solve the problems of recovery of tritium in satisfactory conditions.
- this process for treating a solution containing water formed from an isotope of hydrogen consists in adding to the solution an electrolyte chosen in such a way that the solution obtained can liberate by electrolysis the isotope of hydrogen in the gaseous state, to subject the solution thus obtained to electrolysis so as to obtain a release of the isotope of hydrogen, by operating in an electrolysis cell comprising a metal cathode capable of promoting the diffusion of the hydrogen isotope, said cathode forming a sealed separation wall between the solution to be electrolyzed and a compartment for receiving the hydrogen isotope, and the isotope is recovered in said compartment hydrogen desorbed from said cathode, and it is characterized in that said isotope of hydrogen is tritium and the cathode is coated with a deposit of porous palladium black on its surface in contact with the solution to be electrolyzed.
- the cathode coated with porous palladium black thanks to the structure and the nature of the cathode coated with porous palladium black, it is possible to recover directly in the gaseous state, with good yields, the tritium released during the electrolysis, after its diffusion through the electrode wall and its desorption on the other side of the electrode.
- the choice of a cathode of non-porous material, permeable to hydrogen and impermeable to other gases makes it possible to obtain, after release of the tritium at the cathode, an adsorption of the tritium by the cathode, then a diffusion of this in the cathode and its desorption on the other side of the cathode in the receiving compartment.
- a slight depression is established in the receiving compartment, for example when the tritium is collected by pumping.
- the first step constitutes the most important step because it determines the amount of tritium which could be adsorbed then diffused by the wall of the cathode in contact with the electrolyte.
- a cathode coated on its surface is used in contact with the solution to be electrolyzed from a deposit of porous palladium black.
- this deposit makes it possible to increase the specific surface of the cathode and to give it a higher adsorption capacity with respect to tritium.
- a second deposit on the desorption side is also favorable but in lesser proportions.
- tritium can also be recovered in the form of solid metal tritiide by reacting it directly in the reception compartment with a compound capable of forming a metal tritiide. Mention may be made, as compounds capable of being used, of La-Ni s compounds, Fe-Ti compounds and palladium, alloyed or not.
- a cathode covered with porous palladium black is used on its adsorption face and, preferably, also on its desorption face. Furthermore, the presence of traces of ferric oxide on the adsorption face of the cathode is favorable and the use of annealing to restore the cathode also makes it possible to improve the results obtained.
- the cathode is advantageously made of palladium or a palladium alloy such as a palladium-silver alloy because these metals have the property of adsorbing very large quantities of tritium.
- a palladium alloy such as a palladium-silver alloy
- an alloy of palladium and silver with 25% silver is used because it has a permeability substantially equal to that of pure palladium and the property of not deteriorating after repeated cycles of heating and hydrogenation.
- metals capable of adsorbing tritium can be used, for example, pure iron, nickel, platinum and their alloys.
- T tritium
- the secondary reactions to avoid are: because in this case, the tritium would be discharged directly into the electrolysis cell, instead of diffusing through the wall of the electrode.
- the adsorption of tritium by palladium is improved by subjecting the palladium or palladium alloy electrode to an activation treatment comprising a step of coating the surface of the electrode which will be in contact with the solution to be electrolyzed, a layer of finely divided and porous palladium black.
- the porous palladium black coating is formed by electrolysis of a solution of palladium chloride in dilute hydrochloric acid. This electrolysis can be carried out at a current density of 150 mA / cm 2 for 4 min. Thus, a deposit of palladium black with a thickness of 6 I lm is obtained.
- the annealing heat treatment makes it possible to increase the size of the meshes of the metal network of the cathode and thus to improve the diffusion of the tritium in the cathode.
- the palladium electrodes are generally obtained by rolling and are therefore strongly hardened.
- the grains appear little and are oriented in the direction of rolling.
- recrystallization annealing is possible since the germs necessary for the growth of the crystals have been produced by work hardening, the most disturbed regions where the dislocation energy is concentrated playing the role of germs.
- the metal is heated to a suitable temperature, the germs start to grow and the grain gets bigger; after a certain heating time which corresponds to the incubation period, the recrystallization actually begins.
- time and temperature play an important role and temperature intervenes in a rather complex way.
- the temperature is not high enough during the incubation period, the number of germs decreases and recrystallization can be suppressed, which corresponds to the phenomenon of restoration.
- palladium electrodes good results are obtained by annealing at a temperature of around 650 ° C for one hour under vacuum.
- the hardness decreases, the mechanical tensions are reduced and the dislocations or other imperfections of the metallic network can move towards the surface of the electrode, from where a better diffusion of the tritium in the metallic network of palladium.
- the mechanical abrasion treatment using ferric oxide as a hydrogenation accelerator makes it possible to modify the energy required to pass the chemisorbed hydrogen into hydrogen absorbed in the interstitial sites directly below the cathode surface.
- Iron occupies a number of sites by lending electrons to the 4d band of palladium. This model of iron adsorption which covers the cathode surface increases the permeability of hydrogen in palladium with decrease in potential and increase in current.
- This treatment acts on the amount of tritium released over time.
- the deposition of a thin layer of finely divided and porous palladium black on the surface of the cathode in contact with the solution to be electrolyzed makes it possible to improve the adsorption and the diffusion of tritium.
- the existence on the surface of a very finely divided deposit of palladium black promotes and multiplies the reactions which occur at the solid-solution interface to be electrolyzed.
- a deposit of palladium black on the desorption face improves the diffusion.
- the electrolyte added to the solution containing the tritiated water preferably consists of an alkali metal hydroxide such as sodium hydroxide or potassium hydroxide, which makes it possible to avoid as much as possible the formation of complex ions resulting from radiolysis phenomena and the presence of solvated electrons due to tritium.
- an alkali metal hydroxide such as sodium hydroxide or potassium hydroxide
- the electrolyte concentration of this solution is advantageously from 1 ml-1 to 20 ml-1.
- electrolysis is carried out at a temperature higher than ambient temperature, for example at a temperature of 50 to 160 ° C. because, it is thus possible to increase the current density and cell yield without bubbles forming on the cathode.
- the operation is carried out at a temperature of 80 ° C. since this avoids the technological constraints due to the use of high temperatures as well as the appearance of unfavorable phenomena such as corrosion or secondary reactions of radiolysis.
- the cathode when the cathode is constituted by a wall of palladium or of palladium alloy having a thickness of 50 to 250 ⁇ m, electrolysis is carried out with a current density of between 60 and 150 milliamperes / cm 2 , at a temperature 80 ° C.
- the cathode is constituted by a hollow tube closed at one of its ends and arranged in the cell so as to be partially immersed in the electrolytic solution, the space defined at the interior of the tube constituting the tritium receiving compartment.
- the device comprises means for extracting hydrogen and / or isotopes of hydrogen in the gaseous state, which have diffused in said receiving compartment, these means being constituted either by a suitable pump, or by a trap. based on metals and alloys such as LaNi 5 , Fe-Ti, palladium, alloyed or not, forming hydrides.
- the device preferably comprises means for heating the solution electrolytic present in said cell.
- the cathode is preferably made of palladium or a palladium alloy, for example a palladium and silver alloy.
- a palladium alloy for example a palladium and silver alloy.
- this tube is covered externally and possibly internally with porous palladium black.
- the anode is advantageously constituted by the wall of the electrolysis cell and it is made of stainless steel.
- the palladium-silver alloy tube which constitutes the cathode is subjected to an annealing heat treatment, then its external surface is treated by mechanical abrasion using ferric oxide before being coated with palladium black by electrolysis. .
- the device comprises an electrolysis cell 1 made, for example, of ceramic which is not soluble in an alkaline medium, of metal or of a non-corrodable metal alloy such as steel 316L 22 CND 17-13. Preferably, it is made of passivated stainless steel.
- the cell 1 is closed in leaktight manner at its upper part by a cover 3. Inside the cell is disposed a cathode 5 constituted by a tube closed at its lower end, and the wall of the cell constitutes the anode 7 .
- the device comprises a condenser 15 and an electrolytic solution supply line 17 provided with a valve 18 controlled by an electrical relay associated with the probes 11 and 13, as well as a line 19 for introducing an inert gas. Furthermore, the device comprises heating means 21 of the electrolysis cell constituted by electrical resistances controlled from a thermostat which ensures thermal regulation.
- the cathode 5 is constituted by a hollow tube 5a of circular section having a thickness of 50 to 250 ⁇ m closed at its lower end which delimits the compartment 23 for receiving tritium connected at its upper part to a device for recovery of tritium.
- This tritium recovery device must be sealed to maintain the high purity of the diffused tritium and it can be maintained under vacuum by means of a primary vane pump.
- this device comprises a vacuum gauge and a pressure gauge to control the vacuum, an intermediate enclosure for storing tritium, a test tube for taking gaseous samples and a trap used for storing tritium in the form of tritiide.
- the vacuum can be obtained by a pumping group.
- the tube constituting the cathode 5 is made of a non-porous palladium-silver alloy, permeable to hydrogen and impermeable to other gases, and it has been annealed at a temperature of 650 ° C. for one hour under a vacuum of order of 1.35 Pa to remove the orientation of the grains due to rolling.
- the external surface of the tube intended to be in contact with the solution to be electrolyzed has undergone a mechanical abrasion treatment by means of a ferric oxide powder Fe 2 0 3 moistened, with water , for a few minutes, as an accelerator for the hydrogenation of palladium, then a layer of finely divided and porous palladium black with a thickness of 7 ⁇ m was deposited on this surface thus treated, in order to increase the active surface of palladium on contact with electrically discharged tritium.
- This deposit of finely divided and porous palladium black was produced by electrolysis of a solution of palladium chloride containing 4 g of PdC1 2 dissolved in 20 cm3 of HCl at 12 mol / l., Then diluted to 500 cm 3 distilled water, operating at a cathode current density of 150 mA / cm 2 at a temperature of 20 ° C, for 4 min.
- the anode 7 is formed by the wall of the cell 1 and it is connected to the positive pole of the electric current generator.
- Such an arrangement of the anode and the cathode makes it possible to obtain a good distribution of the current over the surface of the cathode and the formation of regular equipotentials.
- the electrolysis current is programmed using a potentiostat operating in intensiostatic mode.
- solutions containing tritiated water can be treated in the following way: the solution to be electrolyzed which is constituted by tritiated water containing from 1 to 20 mol. 1-1 of sodium hydroxide.
- This tritiated water was obtained by catalytic oxidation of gaseous effluents containing tritium.
- the introduction of solution stops automatically.
- the heating device is then switched on to bring the temperature of the solution to around 80 ° C.
- argon is introduced via line 19 and the electrodes 5 and 7 are connected to the electric current generator to electrolyze the solution with a cathode current density of 60 mA.cm- 2 and obtain a release of gaseous tritium on the cathode 5.
- the tritium is adsorbed by the cathode 5, then it diffuses inside the tube 5 normally under vacuum by pumping, but the process can work when the gas pressure inside the tube is much higher than the pressure of the electrolysis cell. Under these conditions, we can obtain a tritium flow rate of the order of 1 cm.min- 1 .
- the gases released during electrolysis i.e.
- oxygen as well as the tritium which has not diffused in the tube 5 and the water vapor, are evacuated from the cell by the current d argon to the condenser 15 in which the water vapor is condensed and then recycled inside the cell 1.
- the gases leaving the condenser will be sent in a catalytic recombination assembly to reform tritiated water which can then be recycled inside the cell.
- the gas evacuation pipe leaving the condenser 15 can lead to a catalytic oxidation element for residual tritium, this element consisting of palladium black fixed on alumina.
- the tritium recombined with oxygen in the form of heavy water is then condensed in a heat exchanger and optionally recycled in cell 1. It is possible to connect a sampling bulb to the gas outlet pipe so as to analyze the gases extracted. , either at the outlet of the electrolysis cell, or after the catalytic oxidation element.
- a device of this type has made it possible to obtain satisfactory results after operating periods of approximately six weeks without any disassembly of the cathode. At the end of this time, the latter showed no failure and the diffusion of tritium through its wall was carried out under good conditions.
- electrolysis can be carried out at 160 ° C, at a current density of 670 mA / cm 2 , and the diffusion rate of hydrogen and tritium is under these conditions of 3.9 CM 3 . CM - 2 . M in-1.
- the method and the device of the invention make it possible to solve the safety problems posed by the handling of tritiated water, the rejection of contaminated effluents, in particular as regards the hydrogen-tritium fraction released in the electrolysis tank. , as well as the problems of resistance of materials to tritiated water, radiolysis of tritiated water and interaction with nitrogen in the air which leads to corrosive compounds.
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- Physics & Mathematics (AREA)
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- High Energy & Nuclear Physics (AREA)
- Electrolytic Production Of Metals (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
- Electrolytic Production Of Non-Metals, Compounds, Apparatuses Therefor (AREA)
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
FR8123033A FR2517663B1 (fr) | 1981-12-09 | 1981-12-09 | Procede et dispositif de traitement d'effluents aqueux contenant de l'eau tritiee, electrode utilisable dans un tel dispositif et son procede de preparation |
FR8123033 | 1981-12-09 |
Publications (3)
Publication Number | Publication Date |
---|---|
EP0082061A2 EP0082061A2 (fr) | 1983-06-22 |
EP0082061A3 EP0082061A3 (en) | 1983-07-20 |
EP0082061B1 true EP0082061B1 (fr) | 1988-06-29 |
Family
ID=9264846
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP82402226A Expired EP0082061B1 (fr) | 1981-12-09 | 1982-12-06 | Procédé et dispositif de traitement de solutions contenant de l'eau tritiée, électrode utilisable dans un tel dispositif et son procédé de préparation |
Country Status (6)
Country | Link |
---|---|
US (1) | US4487670A (ja) |
EP (1) | EP0082061B1 (ja) |
JP (1) | JPS58113797A (ja) |
CA (1) | CA1215020A (ja) |
DE (1) | DE3278714D1 (ja) |
FR (1) | FR2517663B1 (ja) |
Families Citing this family (36)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4861555A (en) * | 1985-03-11 | 1989-08-29 | Applied Automation, Inc. | Apparatus for chromatographic analysis of ionic species |
BE902271A (nl) * | 1985-04-25 | 1985-08-16 | Studiecentrum Kernenergi | Elektrolyseur voor hoogactief-getritieerd water. |
DE3606316A1 (de) * | 1986-02-27 | 1987-09-03 | Kernforschungsz Karlsruhe | Verfahren und vorrichtung zur dekontamination des abgases des brennstoffkreislaufs eines fusionsreaktors von tritium und/oder deuterium in chemisch gebundener form enthaltenden abgas-bestandteilen |
JPS6450998A (en) * | 1987-08-21 | 1989-02-27 | Power Reactor & Nuclear Fuel | Electrolysis treating method of radioactive waste liquid |
WO1992022906A1 (en) * | 1991-06-11 | 1992-12-23 | Electric Power Research Institute, Inc. | Methods for cleaning cathodes |
AU2257392A (en) * | 1991-06-11 | 1993-01-12 | Electric Power Research Institute, Inc. | Methods for forming films on cathodes |
AU2336192A (en) * | 1991-06-11 | 1993-01-12 | Electric Power Research Institute, Inc. | Apparatus for producing heat from deuterated palladium |
US20020090047A1 (en) * | 1991-10-25 | 2002-07-11 | Roger Stringham | Apparatus for producing ecologically clean energy |
FR2690270A1 (fr) * | 1992-04-21 | 1993-10-22 | Framatome Sa | Enceinte de séparation et de confinement de produits radioactifs contenus dans des effluents liquides et installation et procédé pour le traitement de ces effluents. |
WO1994014163A1 (en) * | 1992-12-10 | 1994-06-23 | Electric Power Research Institute, Inc. | Methods for forming films on cathodes |
EP0914668A2 (en) * | 1995-06-06 | 1999-05-12 | André Jouanneau | Method and apparatus for producing and using plasma |
US6024935A (en) * | 1996-01-26 | 2000-02-15 | Blacklight Power, Inc. | Lower-energy hydrogen methods and structures |
US20090142257A1 (en) * | 1997-07-22 | 2009-06-04 | Blacklight Power, Inc. | Inorganic hydrogen compounds and applications thereof |
US20090129992A1 (en) * | 1997-07-22 | 2009-05-21 | Blacklight Power, Inc. | Reactor for Preparing Hydrogen Compounds |
EP1031169A4 (en) * | 1997-07-22 | 2000-10-18 | Blacklight Power Inc | INORGANIC HYDROGEN COMPOUNDS, SEPARATION METHODS AND FUEL APPLICATIONS |
US20090123356A1 (en) * | 1997-07-22 | 2009-05-14 | Blacklight Power, Inc. | Inorganic hydrogen compounds |
CA2466953A1 (en) * | 2001-11-14 | 2003-08-14 | Blacklight Power, Inc. | Hydrogen power, plasma, and reactor for lasing, and power conversion |
US20040095705A1 (en) * | 2001-11-28 | 2004-05-20 | Mills Randell L. | Plasma-to-electric power conversion |
US20030129117A1 (en) * | 2002-01-02 | 2003-07-10 | Mills Randell L. | Synthesis and characterization of a highly stable amorphous silicon hydride as the product of a catalytic hydrogen plasma reaction |
US20040118348A1 (en) * | 2002-03-07 | 2004-06-24 | Mills Randell L.. | Microwave power cell, chemical reactor, and power converter |
AU2003234301A1 (en) * | 2002-05-01 | 2003-11-17 | Blacklight Power, Inc. | Diamond synthesis |
CA2522506A1 (en) * | 2003-04-15 | 2004-10-28 | Blacklight Power, Inc. | Plasma reactor and process for producing lower-energy hydrogen species |
US7188033B2 (en) * | 2003-07-21 | 2007-03-06 | Blacklight Power Incorporated | Method and system of computing and rendering the nature of the chemical bond of hydrogen-type molecules and molecular ions |
US7773656B1 (en) | 2003-10-24 | 2010-08-10 | Blacklight Power, Inc. | Molecular hydrogen laser |
AU2005204618A1 (en) * | 2004-01-05 | 2005-07-28 | Blacklight Power, Inc. | Method and system of computing and rendering the nature of atoms and atomic ions |
US20060088138A1 (en) * | 2004-04-07 | 2006-04-27 | Andre Jouanneau | Method and apparatus for the generation and the utilization of plasma solid |
US7689367B2 (en) | 2004-05-17 | 2010-03-30 | Blacklight Power, Inc. | Method and system of computing and rendering the nature of the excited electronic states of atoms and atomic ions |
US20070198199A1 (en) * | 2004-07-19 | 2007-08-23 | Mills Randell L | Method and system of computing and rendering the nature of the chemical bond of hydrogen-type molecules and molecular ions |
US20080304522A1 (en) * | 2006-04-04 | 2008-12-11 | Mills Randell L | Catalyst laser |
US8597471B2 (en) | 2010-08-19 | 2013-12-03 | Industrial Idea Partners, Inc. | Heat driven concentrator with alternate condensers |
JP6549372B2 (ja) * | 2014-12-16 | 2019-07-24 | 吉田 英夫 | トリチウム水による汚染土壌および汚染水の除染方法および除染システム |
US10385468B2 (en) | 2016-06-06 | 2019-08-20 | Ih Ip Holdings Limited | Plasma frequency trigger |
US11268202B2 (en) | 2019-02-13 | 2022-03-08 | Industrial Heat, Llc | Methods for enhanced electrolytic loading of hydrogen |
US10767273B2 (en) * | 2019-02-13 | 2020-09-08 | Ih Ip Holdings Limited | Methods for enhanced electrolytic loading of hydrogen |
CN112489847B (zh) * | 2020-12-01 | 2023-05-05 | 中国工程物理研究院核物理与化学研究所 | 一种活化石墨减容处理方法 |
CN115240884A (zh) * | 2022-07-04 | 2022-10-25 | 中核核电运行管理有限公司 | 一种验证基于精馏的高氚重水自辐照分解的方法 |
Family Cites Families (7)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US2863526A (en) * | 1956-10-17 | 1958-12-09 | Oliver N Salmon | Method of separating hydrogen isotopes |
US3620844A (en) * | 1963-03-04 | 1971-11-16 | Varta Ag | System for the activation of hydrogen |
GB1289309A (ja) * | 1968-12-31 | 1972-09-13 | ||
US4000048A (en) * | 1973-06-25 | 1976-12-28 | Diamond Shamrock Technologies S.A. | Novel cathode |
DE2711366A1 (de) * | 1977-03-16 | 1978-09-21 | Hoechst Ag | Verfahren zum anreichern und abtrennen von tritium und/oder tritiumhydrid von tritiumwasser |
CA1095848A (en) * | 1978-03-30 | 1981-02-17 | Electrolyser Corporation Ltd. (The) | Heavy-water extraction from non-electrolytic hydrogen streams |
US4331522A (en) * | 1981-01-12 | 1982-05-25 | European Atomic Energy Commission (Euratom) | Reprocessing of spent plasma |
-
1981
- 1981-12-09 FR FR8123033A patent/FR2517663B1/fr not_active Expired
-
1982
- 1982-12-06 EP EP82402226A patent/EP0082061B1/fr not_active Expired
- 1982-12-06 DE DE8282402226T patent/DE3278714D1/de not_active Expired
- 1982-12-08 US US06/447,801 patent/US4487670A/en not_active Expired - Lifetime
- 1982-12-08 CA CA000417276A patent/CA1215020A/en not_active Expired
- 1982-12-09 JP JP57216248A patent/JPS58113797A/ja active Granted
Also Published As
Publication number | Publication date |
---|---|
JPH0129439B2 (ja) | 1989-06-09 |
JPS58113797A (ja) | 1983-07-06 |
DE3278714D1 (en) | 1988-08-04 |
EP0082061A2 (fr) | 1983-06-22 |
EP0082061A3 (en) | 1983-07-20 |
FR2517663B1 (fr) | 1985-08-09 |
FR2517663A1 (fr) | 1983-06-10 |
CA1215020A (en) | 1986-12-09 |
US4487670A (en) | 1984-12-11 |
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