WO1981002027A1 - Cellules avec anodes en cermet pour l'electrolyse de sels fondus - Google Patents

Cellules avec anodes en cermet pour l'electrolyse de sels fondus Download PDF

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Publication number
WO1981002027A1
WO1981002027A1 PCT/US1981/000064 US8100064W WO8102027A1 WO 1981002027 A1 WO1981002027 A1 WO 1981002027A1 US 8100064 W US8100064 W US 8100064W WO 8102027 A1 WO8102027 A1 WO 8102027A1
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WO
WIPO (PCT)
Prior art keywords
anode
cermet
metallic phase
nickel
oxide
Prior art date
Application number
PCT/US1981/000064
Other languages
English (en)
Inventor
J Duruz
J Derivaz
Original Assignee
Diamond Shamrock Corp
J Duruz
J Derivaz
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 Diamond Shamrock Corp, J Duruz, J Derivaz filed Critical Diamond Shamrock Corp
Priority to BR8106067A priority Critical patent/BR8106067A/pt
Publication of WO1981002027A1 publication Critical patent/WO1981002027A1/fr
Priority to NO813015A priority patent/NO155401C/no

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Classifications

    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C3/00—Electrolytic production, recovery or refining of metals by electrolysis of melts
    • C25C3/06—Electrolytic production, recovery or refining of metals by electrolysis of melts of aluminium
    • C25C3/08—Cell construction, e.g. bottoms, walls, cathodes
    • C25C3/12—Anodes
    • C—CHEMISTRY; METALLURGY
    • C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
    • C25C—PROCESSES FOR THE ELECTROLYTIC PRODUCTION, RECOVERY OR REFINING OF METALS; APPARATUS THEREFOR
    • C25C7/00—Constructional parts, or assemblies thereof, of cells; Servicing or operating of cells
    • C25C7/02—Electrodes; Connections thereof
    • C25C7/025—Electrodes; Connections thereof used in cells for the electrolysis of melts

Definitions

  • the invention relates to electrolytic cells for electrowinning metals from fused salt baths, especially aluminium from a fused cryolite-alumina bath.
  • a fused salt baths especially aluminium from a fused cryolite-alumina bath.
  • consumption of the carbon anodes entails signifi ⁇ cant costs.
  • metal oxides as anodes instead of consumable carbon anodes was investigated by A. I. Belyaev more than forty years ago (see, e.g., Chem. Abstr. 31, 1937, 8384 and 32, 1938, 6553).
  • the state of the art relating to metal oxide anodes proposed for aluminium electrowinning may be illustrated for example by U.S.
  • Patents 4,039,401, 4,057,480, 4,098,669, 4,146,438, 3,718,550 The use of inconsumable anodes for aluminium electrowinning would eliminate the significant costs of carbon replacement required for the carbon anodes currently used, as well as emissions from the cell, while allowing closer control of the anode-cathode gap.
  • the oxygen evolution potential on an inconsumable anode would be higher than for the evolution of C0 tent on the carbon anode.
  • the electrical energy consumption for aluminium production would thus be increased accordingly, unless other modifications are made in the design and mode of operation of the electrolytic cell.
  • inconsumable anodes for aluminium electrowinning from fused cryolite-alumina is particularly difficult due to the fact that they must meet extremely strict requirements with regard to stability and conductivity under severe operating conditions.
  • Such anodes must firstly be substantially insoluble and able to resist attack by both the cryolite-alumina bath at high temperature (about 1000 C) and anodically generated oxygen. This first requirement is essential since contamination of the molten aluminium recovered at the cathode above the tolerated impurity levels would be undesirable.
  • the electronic conductivity of the anode should be greater than 4 ohm cm at 1000 C.
  • Pure non noble metals have high conductivity but are unstable as anodes in fused cryolite-alumina.
  • the use of noble metals having adequate stability is restricted by their high cost.
  • the metal oxides which have been proposed as anode materials generally have inadequate electronic conductivity.
  • an object of the invention is to provide an anode material, which is substantially resistant to attack by cryolite-alumina melts and anodically generated oxygen, has a high electronic conductivity, and can meet the tech ⁇ nical and economic requirements of anodes for electro ⁇ winning aluminium from cryolite-alumina melts.
  • more particular object of the invention is to provide such an anode material in the form of a cermet wherein a small amount of noble metal is incorporated, in a ceramic phase so as to provide adequate conductivity in an economical manner.
  • the invention provides cermet anodes which are suitable for electrowinning metals from fused salt baths, especially aluminium from fused cryolite-alumina and are composed of a ceramic phase and a metallic phase which are respectively selected from a limited number of oxides and metals.
  • the ceramic phase of the cermet according to the invention is selected from the group of oxides consisting of nickeL copper and zinc; ferrites or chromites of iron, nickel, copper and zinc; ferric oxide; chromic oxide; nickel oxide; cupric oxide; and zinc oxide.
  • the metallic phase of the cermet according to the invention is selected from the group consisting of palladium, platinum, iridium, rhodium, gold, and alloys thereof.
  • Such alloys may consist of noble metals of this group in suitable combinations with each other, or with iron, cobalt, nickel or copper whereby to reduce the cost of the metallic phase.
  • Ceramics selected from said group of oxides ac- cording to the invention have been found to have relatively high stability under the severe anodic conditions of alumin ⁇ ium electrowinning from cryolite-alumina melts, whereas their electrical conductivity is inadequate. It has also been found that when these ceramics are properly combined with metals according to the invention, a cermet can be obtained which has satisfactory stability and conductivity under said anodic conditions.
  • the oxide of the ceramic phase is thermodynamically more stable than oxides which may be formed by the metallic phase, so that reduction of the ceramic phase by the metallic phase is avoided in the cermet according to the invention.
  • the density of a cermet material according to the invention should be in ⁇ creased as far as possible towards 100% of the theoretical density, in order to provide maximum resistance to attack under anodic conditions in a cryolite-alumina melt; namely at least 90%, and preferably greater than 95%.
  • the cermet material of the anode according to the invention should contain a uniformly distributed metallic phase in an amount sufficient to provide the cermet with an electronic conductivity greater than 4 ohm cm at 1000 C.
  • the electronic conductivity of the cermets according to the invention may preferably be greater than 20 ohm -1cm-1 at
  • the proportion of the noble metal or noble metai alloy phase incorporated in the cermet should generally be limited so as to decrease the cost of the cermet as far as possible while ensuring adequate conductiv- ity and stability.
  • the amount of the metallic phase incor ⁇ porated in the cermet may lie between 2% and about 30% by volume of the cermet, preferably between 5 and 15 vol. %.
  • This program included theomme ⁇ gation of on one hand a broad range of base metals compris ⁇ ing chromium, iron, cobalt, nickel, copper, tugsten, molybdenum, and on the other hand noble metals comprising rhodium, palladium, iridium, platinum, gold.
  • base metals comprising chromium, iron, cobalt, nickel, copper, tugsten, molybdenum, and on the other hand noble metals comprising rhodium, palladium, iridium, platinum, gold.
  • palladium is particularly advantageous due to its high stability, low density, and relatively low cost.
  • the elctronic conductivity provided by the metallic phase depends essentially on its volume in the cermet, palladium may be used in smaller amounts to provide a continuous metallic phase, and that at a lower cost than with other noble metals.
  • an anode for aluminium electrowinning may consist either entirely or partly of a cermet material according to the invention.
  • an electrode support body of any suitable shape and material may be covered with said cermet material.
  • cermets as anode materials according to the invention provides a particular combination of advan- tages, namely:
  • Said experimental program carried out within the framework of the invention also covered a broad range of refractory ceramic materials which seemed of potential in ⁇ terest as anodes to be used for aluminium electrowinning from cryolite-alumina melts.
  • ceramic samples intended for preliminary corrosion resis ⁇ tance tests were prepared by isostatic cold-pressing of powders of about 40 * J particle size, followed by sintering at temperatures lying in the range between 1300°C and 1600°C in air, or in argon when oxidizable components were con ⁇ tained in the samples.
  • the invention further provides an electrolytic cell for electrowinning aluminium from a fused cryolite- alumina bath.
  • This cell comprises at least one anode con- sisting essentially of a cermet material according to the invention, as set forth in the claims.
  • Said cell may fur ⁇ ther advantageously comprise a substantially inert solid cathode structure disposed at a predetermined distance be ⁇ low said anode, so as to thereby obviate the drawbacks of the conventional liquid metal cathode pool.
  • the described cell assembly was enclosed in a container made of Inconel 600TM and heated in a verticle electrical re ⁇ sistance furnace. Before each test, some pure aluminium (about 5g of Merck pro analysi Al) was placed on the bot- torn of said small crucible and electrically contacted with the cathode feeder rod. The electrolysis crucible was heated to form an electrolysis melt. A cermet anode sample (5 x 5 x 30mm) suspended from a platinum wire was partly immersed in the melt having reached thermal equilibrium at 1000°C. Each test run was carried out at a given constant electrolysis current for a given period, as indicated in the examples.
  • Anode samples consisting of a cermet of nickel ferrite and palladium (Ref. 79/18/1, Table 1) were fabri ⁇ cated by hot-pressing and electrolytically tested as anodes in a laboratory experiment simulating the conditions of aluminium electrowinning from molten cryolite-alumina at 1000°C.
  • the cermet material (79/18/1) was fabricated by mixing powdered NiO and Fe-O.. with 20. vol.% Pd and sinter ⁇ ing the resulting powder mixture (325 mesh, about 40 ⁇ ) by
  • Table 1 shows the test conditions (anode/cathode current densities) and results for electrolytic test runs 187 and 206 which were carried out on these anode samples 79/18/1, for 6 and 18 hours, respectively.
  • the cell volt ⁇ age remained at about 3.5 V throughout these test runs, while the aluminium current efficiency was 55% and 81%, re ⁇ spectively.
  • Table 1 also indicates the level of impurities found in the aluminium pool, said levels being corrected for an assumed aluminium current efficiency of 90%, which can be achieved industrially.
  • the aluminum produced in Run 187 was analyzed by a method having a detection level of 90 ppm Pd and no palladium was detected. A more precise method of analysis used for Run 206 allowed the detection of 20 ppm Pd.
  • Anode samples (Ref. 79/18/2) consisting of a cermet of nickel ferrite and palladium were fabricated and tested in the manner generally described in Example I.
  • Anode sample (Ref. 79/29/1) consisting of a cer ⁇ met of hematite and 20 vol. % palladium was fabricated and tested in the manner described in Example II, the corre- sponding electrolytic test data of Run 259/7 h being in ⁇ dicated in Table 1.
  • Anode sample (Ref. 79/29/2) consisting of a cer ⁇ met of hematite and 20 vol. % palladium was fabricated by cold-pressing a powder mixture of Fe,0., with 20 vol. % Pd at 1000 kg/cm 2 and then sintering at 1400°C for 6 hours in air. It had a density of 88% and a conductivity of 70 ohm cm at room temperature. Electrolytic test data for* Run 321/6 is given in Table 1, as in the preceding examples.
  • Anode sample 79/31/1 of a cermet composed of nickel ferrite and 15% palladium was fabricated and tested in the manner described in Example I.
  • the relative density of sample 79/31/1 was 95%, and Table 1 shows the data of electrolytic test run 247/6.
  • Example 1 Anode sample 79/32/1 of a cermet composed sub ⁇ stantially of nickel ferrite and 10 vol. % palladium was fabricated and tested as described in Example I. The relative density of this cermet was 93% and its conduc ⁇ tivity at room temperature was 80 ohm " cm- . Table 1 also shows the data of test run 241 carried out on anode sample 79/32/1. TABLE 1
  • the described results may be improved by modifying the composition and manufacture of the cermets according to the invention with respect to the above examples.
  • the stability of the cermet may be considerably improved by increasing its density as far as possible up to 100% of theoretical. This might be achieved by optimizing " the manufacturing conditions (temperature, pressure, duration) , or by using a different method of manufacturing the cermet.
  • optimization of the relative proportions of the ceramic oxide and the metallic phases of the cermet may allow its noble metal content to be reduced while providing satis ⁇ factory conductivity.
  • Other oxide-metal combinations than those described in the examples may likewise improve re- suits.
  • the aluminium contamination levels given in Table 1 with reference to the above examples may be significantly higher than may be expected in industrial operation.
  • the reason for this is that the impurities detected in the laboratory experi ⁇ ments may at least partly originate from the cryolite bath itself, from the aluminium initially present, or from the cell assembly (outer container and heat shields made of Inconel®) • As a matter of fact, that this seems to be the case is indicated by further control test runs wherein electrolysis was carried out under similar operating con ⁇ ditions with the same cell assembly equipped with a pure carbon anode (instead of a cermet anode) and also resulted in nonnegligible contamination of the aluminium produced.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • Materials Engineering (AREA)
  • Metallurgy (AREA)
  • Organic Chemistry (AREA)
  • Electrolytic Production Of Metals (AREA)

Abstract

Une cellule electrolytique et une anode sont utilisees pour l'electro-extraction de metal en fusion d'un bain de sels fondus, par exemple de l'aluminium extrait de cryolite-alumine, ladite anode consistant en un materiau de cermet (ceramique-metal) forme a partir d'un oxyde ceramique par exemple, ferrite ou chromite, et un metal par exemple un metal noble ou un alliage d'un metal noble.
PCT/US1981/000064 1980-01-17 1981-01-16 Cellules avec anodes en cermet pour l'electrolyse de sels fondus WO1981002027A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
BR8106067A BR8106067A (pt) 1980-01-17 1981-01-16 Pilha provida de anodo de metal ceramico para eletrolise em sal em fusao
NO813015A NO155401C (no) 1980-01-17 1981-09-04 Anode for elektroutvinning av smeltet metall fra et smeltet salt i en elektrolysecelle, og anvendelse av anoden.

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB8001550 1980-01-17
GB8001550A GB2069529A (en) 1980-01-17 1980-01-17 Cermet anode for electrowinning metals from fused salts

Publications (1)

Publication Number Publication Date
WO1981002027A1 true WO1981002027A1 (fr) 1981-07-23

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Application Number Title Priority Date Filing Date
PCT/US1981/000064 WO1981002027A1 (fr) 1980-01-17 1981-01-16 Cellules avec anodes en cermet pour l'electrolyse de sels fondus

Country Status (7)

Country Link
US (1) US4397729A (fr)
AU (1) AU552201B2 (fr)
BR (1) BR8106067A (fr)
CA (1) CA1175388A (fr)
FR (1) FR2474061B1 (fr)
GB (2) GB2069529A (fr)
WO (1) WO1981002027A1 (fr)

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4443314A (en) * 1983-03-16 1984-04-17 Great Lakes Carbon Corporation Anode assembly for molten salt electrolysis
US4472258A (en) * 1983-05-03 1984-09-18 Great Lakes Carbon Corporation Anode for molten salt electrolysis
EP0122160A2 (fr) * 1983-04-11 1984-10-17 Aluminum Company Of America Composition appropriée pour électrode inerte
EP0306099A1 (fr) * 1987-09-02 1989-03-08 MOLTECH Invent S.A. Matériau composite céramique/métal
WO2000044952A1 (fr) * 1997-06-26 2000-08-03 Alcoa Inc. Electrode inerte contenant des oxydes metalliques, du cuivre et un metal noble

Families Citing this family (27)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0109164A1 (fr) * 1982-11-15 1984-05-23 Texasgulf Inc. Production de sodium métallique à partir de carbonate de sodium par électrolyse en bains fondus
US4462889A (en) * 1983-10-11 1984-07-31 Great Lakes Carbon Corporation Non-consumable electrode for molten salt electrolysis
DE3687072T2 (de) * 1985-02-18 1993-03-18 Moltech Invent Sa Aluminiumoxid-elektrolyse bei niedriger temperatur.
US4620905A (en) * 1985-04-25 1986-11-04 Aluminum Company Of America Electrolytic production of metals using a resistant anode
US4626333A (en) * 1986-01-28 1986-12-02 Great Lakes Carbon Corporation Anode assembly for molten salt electrolysis
US4871438A (en) * 1987-11-03 1989-10-03 Battelle Memorial Institute Cermet anode compositions with high content alloy phase
AU625225B2 (en) * 1987-11-03 1992-07-02 Battelle Memorial Institute Cermet anode with continuously dispersed alloy phase and process for making
US5368702A (en) * 1990-11-28 1994-11-29 Moltech Invent S.A. Electrode assemblies and mutimonopolar cells for aluminium electrowinning
US5362366A (en) * 1992-04-27 1994-11-08 Moltech Invent S.A. Anode-cathode arrangement for aluminum production cells
US6821312B2 (en) * 1997-06-26 2004-11-23 Alcoa Inc. Cermet inert anode materials and method of making same
US6372119B1 (en) 1997-06-26 2002-04-16 Alcoa Inc. Inert anode containing oxides of nickel iron and cobalt useful for the electrolytic production of metals
US6416649B1 (en) 1997-06-26 2002-07-09 Alcoa Inc. Electrolytic production of high purity aluminum using ceramic inert anodes
US6217739B1 (en) 1997-06-26 2001-04-17 Alcoa Inc. Electrolytic production of high purity aluminum using inert anodes
US6162334A (en) * 1997-06-26 2000-12-19 Alcoa Inc. Inert anode containing base metal and noble metal useful for the electrolytic production of aluminum
US6423195B1 (en) 1997-06-26 2002-07-23 Alcoa Inc. Inert anode containing oxides of nickel, iron and zinc useful for the electrolytic production of metals
US6423204B1 (en) 1997-06-26 2002-07-23 Alcoa Inc. For cermet inert anode containing oxide and metal phases useful for the electrolytic production of metals
US5942097A (en) * 1997-12-05 1999-08-24 The Ohio State University Method and apparatus featuring a non-consumable anode for the electrowinning of aluminum
US6372099B1 (en) * 1998-07-30 2002-04-16 Moltech Invent S.A. Cells for the electrowinning of aluminium having dimensionally stable metal-based anodes
ATE276384T1 (de) * 1999-10-26 2004-10-15 Moltech Invent Sa Bei niedriger temperatur betriebene elektrolysezelle zur herstellung von aluminium
NO20010928D0 (no) * 2001-02-23 2001-02-23 Norsk Hydro As Materiale for benyttelse i produksjon
US6837982B2 (en) * 2002-01-25 2005-01-04 Northwest Aluminum Technologies Maintaining molten salt electrolyte concentration in aluminum-producing electrolytic cell
US6758991B2 (en) 2002-11-08 2004-07-06 Alcoa Inc. Stable inert anodes including a single-phase oxide of nickel and iron
US7033469B2 (en) * 2002-11-08 2006-04-25 Alcoa Inc. Stable inert anodes including an oxide of nickel, iron and aluminum
US9206516B2 (en) 2011-08-22 2015-12-08 Infinium, Inc. Liquid anodes and fuels for production of metals from their oxides by molten salt electrolysis with a solid electrolyte
JP2014526611A (ja) 2011-09-01 2014-10-06 インフィニウム，インク． 酸素および液体金属環境における高温で高電流の導体
FR3034433B1 (fr) * 2015-04-03 2019-06-07 Rio Tinto Alcan International Limited Materiau cermet d'electrode
US11154816B2 (en) * 2019-05-30 2021-10-26 Toyota Motor Engineering & Manufacturing North America, Inc. Palladium oxide supported on spinels for NOx storage

Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3718550A (en) * 1969-12-05 1973-02-27 Alusuisse Process for the electrolytic production of aluminum
US3960678A (en) * 1973-05-25 1976-06-01 Swiss Aluminium Ltd. Electrolysis of a molten charge using incomsumable electrodes
US4173518A (en) * 1974-10-23 1979-11-06 Sumitomo Aluminum Smelting Company, Limited Electrodes for aluminum reduction cells
US4187155A (en) * 1977-03-07 1980-02-05 Diamond Shamrock Technologies S.A. Molten salt electrolysis
US4233148A (en) * 1979-10-01 1980-11-11 Great Lakes Carbon Corporation Electrode composition

Family Cites Families (1)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0022921B1 (fr) * 1979-07-20 1983-10-26 C. CONRADTY NÜRNBERG GmbH & Co. KG Electrode régénérable à stabilité de forme pour l'emploi à haute température

Patent Citations (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3718550A (en) * 1969-12-05 1973-02-27 Alusuisse Process for the electrolytic production of aluminum
US3960678A (en) * 1973-05-25 1976-06-01 Swiss Aluminium Ltd. Electrolysis of a molten charge using incomsumable electrodes
US4173518A (en) * 1974-10-23 1979-11-06 Sumitomo Aluminum Smelting Company, Limited Electrodes for aluminum reduction cells
US4187155A (en) * 1977-03-07 1980-02-05 Diamond Shamrock Technologies S.A. Molten salt electrolysis
US4233148A (en) * 1979-10-01 1980-11-11 Great Lakes Carbon Corporation Electrode composition

Cited By (17)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4443314A (en) * 1983-03-16 1984-04-17 Great Lakes Carbon Corporation Anode assembly for molten salt electrolysis
WO1984003721A1 (fr) * 1983-03-16 1984-09-27 Great Lakes Carbon Corp Assemblage d'anode pour l'electrolyse de sels en fusion
EP0122160A2 (fr) * 1983-04-11 1984-10-17 Aluminum Company Of America Composition appropriée pour électrode inerte
EP0122160A3 (fr) * 1983-04-11 1986-11-26 Aluminum Company Of America Composition appropriée pour électrode inerte
US4472258A (en) * 1983-05-03 1984-09-18 Great Lakes Carbon Corporation Anode for molten salt electrolysis
EP0306100A1 (fr) * 1987-09-02 1989-03-08 MOLTECH Invent S.A. Matériau composite céramique/métal
EP0306102A1 (fr) * 1987-09-02 1989-03-08 MOLTECH Invent S.A. Electrolyse de sel fondu avec anode inconsumable
EP0306101A1 (fr) * 1987-09-02 1989-03-08 MOLTECH Invent S.A. Anode inconsumable pour l'électrolyse du sel fondu
EP0306099A1 (fr) * 1987-09-02 1989-03-08 MOLTECH Invent S.A. Matériau composite céramique/métal
WO1989001994A1 (fr) * 1987-09-02 1989-03-09 Moltech Invent S.A. Electrolyse dans des sels fondus avec une anode non fusible
WO1989001991A1 (fr) * 1987-09-02 1989-03-09 Moltech Invent S.A. Matiere composite en ceramique et metal
WO1989001992A1 (fr) * 1987-09-02 1989-03-09 Moltech Invent S.A. Matiere composite en ceramique et metal
WO1989001993A1 (fr) * 1987-09-02 1989-03-09 Moltech Invent S.A. Anode non fusible pour electrolyse dans des sels fondus
US4956068A (en) * 1987-09-02 1990-09-11 Moltech Invent S.A. Non-consumable anode for molten salt electrolysis
US4960494A (en) * 1987-09-02 1990-10-02 Moltech Invent S.A. Ceramic/metal composite material
US5069771A (en) * 1987-09-02 1991-12-03 Moltech Invent S.A. Molten salt electrolysis with non-consumable anode
WO2000044952A1 (fr) * 1997-06-26 2000-08-03 Alcoa Inc. Electrode inerte contenant des oxydes metalliques, du cuivre et un metal noble

Also Published As

Publication number Publication date
CA1175388A (fr) 1984-10-02
GB2069529A (en) 1981-08-26
US4397729A (en) 1983-08-09
GB2078259B (en) 1983-03-09
AU6772881A (en) 1981-08-07
AU552201B2 (en) 1986-05-22
GB2078259A (en) 1982-01-06
FR2474061B1 (fr) 1986-02-21
FR2474061A1 (fr) 1981-07-24
BR8106067A (pt) 1981-11-24

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