EP0274138A1 - Agencement d'électrode, pour électrolyseurs produisant des gaz, présentant des plaques d'électrode disposées verticalement - Google Patents
Agencement d'électrode, pour électrolyseurs produisant des gaz, présentant des plaques d'électrode disposées verticalement Download PDFInfo
- Publication number
- EP0274138A1 EP0274138A1 EP87201843A EP87201843A EP0274138A1 EP 0274138 A1 EP0274138 A1 EP 0274138A1 EP 87201843 A EP87201843 A EP 87201843A EP 87201843 A EP87201843 A EP 87201843A EP 0274138 A1 EP0274138 A1 EP 0274138A1
- Authority
- EP
- European Patent Office
- Prior art keywords
- electrode
- electrodes
- membrane
- plate
- plate electrodes
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Granted
Links
- 239000012528 membrane Substances 0.000 claims abstract description 37
- 229910052751 metal Inorganic materials 0.000 claims description 13
- 239000002184 metal Substances 0.000 claims description 13
- 239000004744 fabric Substances 0.000 claims description 3
- 230000003247 decreasing effect Effects 0.000 abstract 1
- 238000005868 electrolysis reaction Methods 0.000 description 20
- 239000003792 electrolyte Substances 0.000 description 16
- 239000007789 gas Substances 0.000 description 11
- RTAQQCXQSZGOHL-UHFFFAOYSA-N Titanium Chemical compound [Ti] RTAQQCXQSZGOHL-UHFFFAOYSA-N 0.000 description 7
- 150000002500 ions Chemical class 0.000 description 7
- 229910052719 titanium Inorganic materials 0.000 description 7
- 239000010936 titanium Substances 0.000 description 7
- HEMHJVSKTPXQMS-UHFFFAOYSA-M Sodium hydroxide Chemical compound [OH-].[Na+] HEMHJVSKTPXQMS-UHFFFAOYSA-M 0.000 description 6
- WOCIAKWEIIZHES-UHFFFAOYSA-N ruthenium(iv) oxide Chemical compound O=[Ru]=O WOCIAKWEIIZHES-UHFFFAOYSA-N 0.000 description 6
- 238000000034 method Methods 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 4
- FAPWRFPIFSIZLT-UHFFFAOYSA-M Sodium chloride Chemical compound [Na+].[Cl-] FAPWRFPIFSIZLT-UHFFFAOYSA-M 0.000 description 4
- 239000000243 solution Substances 0.000 description 4
- NLXLAEXVIDQMFP-UHFFFAOYSA-N Ammonia chloride Chemical compound [NH4+].[Cl-] NLXLAEXVIDQMFP-UHFFFAOYSA-N 0.000 description 3
- 238000007872 degassing Methods 0.000 description 3
- 150000002739 metals Chemical class 0.000 description 3
- VEXZGXHMUGYJMC-UHFFFAOYSA-M Chloride anion Chemical compound [Cl-] VEXZGXHMUGYJMC-UHFFFAOYSA-M 0.000 description 2
- KDLHZDBZIXYQEI-UHFFFAOYSA-N Palladium Chemical compound [Pd] KDLHZDBZIXYQEI-UHFFFAOYSA-N 0.000 description 2
- 239000003513 alkali Substances 0.000 description 2
- 239000011248 coating agent Substances 0.000 description 2
- 238000000576 coating method Methods 0.000 description 2
- 230000005611 electricity Effects 0.000 description 2
- 239000000463 material Substances 0.000 description 2
- 229910052759 nickel Inorganic materials 0.000 description 2
- BASFCYQUMIYNBI-UHFFFAOYSA-N platinum Chemical compound [Pt] BASFCYQUMIYNBI-UHFFFAOYSA-N 0.000 description 2
- 239000011780 sodium chloride Substances 0.000 description 2
- 239000000725 suspension Substances 0.000 description 2
- 238000003466 welding Methods 0.000 description 2
- ZAMOUSCENKQFHK-UHFFFAOYSA-N Chlorine atom Chemical compound [Cl] ZAMOUSCENKQFHK-UHFFFAOYSA-N 0.000 description 1
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 description 1
- 229920000557 Nafion® Polymers 0.000 description 1
- 244000089486 Phragmites australis subsp australis Species 0.000 description 1
- KJTLSVCANCCWHF-UHFFFAOYSA-N Ruthenium Chemical group [Ru] KJTLSVCANCCWHF-UHFFFAOYSA-N 0.000 description 1
- 229910000831 Steel Inorganic materials 0.000 description 1
- QCWXUUIWCKQGHC-UHFFFAOYSA-N Zirconium Chemical compound [Zr] QCWXUUIWCKQGHC-UHFFFAOYSA-N 0.000 description 1
- 230000002378 acidificating effect Effects 0.000 description 1
- 230000003213 activating effect Effects 0.000 description 1
- 229910001854 alkali hydroxide Inorganic materials 0.000 description 1
- 229910001514 alkali metal chloride Inorganic materials 0.000 description 1
- 150000008044 alkali metal hydroxides Chemical class 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000005452 bending Methods 0.000 description 1
- 239000012267 brine Substances 0.000 description 1
- 238000005341 cation exchange Methods 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000000460 chlorine Substances 0.000 description 1
- 229910052801 chlorine Inorganic materials 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
- 239000004020 conductor Substances 0.000 description 1
- 239000004035 construction material Substances 0.000 description 1
- 230000006378 damage Effects 0.000 description 1
- 238000005265 energy consumption Methods 0.000 description 1
- 239000001257 hydrogen Substances 0.000 description 1
- 229910052739 hydrogen Inorganic materials 0.000 description 1
- 229910052741 iridium Inorganic materials 0.000 description 1
- GKOZUEZYRPOHIO-UHFFFAOYSA-N iridium atom Chemical compound [Ir] GKOZUEZYRPOHIO-UHFFFAOYSA-N 0.000 description 1
- 238000005259 measurement Methods 0.000 description 1
- 229910044991 metal oxide Inorganic materials 0.000 description 1
- 150000004706 metal oxides Chemical class 0.000 description 1
- 229910052758 niobium Inorganic materials 0.000 description 1
- 239000010955 niobium Substances 0.000 description 1
- GUCVJGMIXFAOAE-UHFFFAOYSA-N niobium atom Chemical compound [Nb] GUCVJGMIXFAOAE-UHFFFAOYSA-N 0.000 description 1
- 229910052762 osmium Inorganic materials 0.000 description 1
- SYQBFIAQOQZEGI-UHFFFAOYSA-N osmium atom Chemical compound [Os] SYQBFIAQOQZEGI-UHFFFAOYSA-N 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 229910052763 palladium Inorganic materials 0.000 description 1
- 229910052697 platinum Inorganic materials 0.000 description 1
- 239000000376 reactant Substances 0.000 description 1
- 229910052703 rhodium Inorganic materials 0.000 description 1
- 239000010948 rhodium Substances 0.000 description 1
- MHOVAHRLVXNVSD-UHFFFAOYSA-N rhodium atom Chemical compound [Rh] MHOVAHRLVXNVSD-UHFFFAOYSA-N 0.000 description 1
- 238000000926 separation method Methods 0.000 description 1
- HPALAKNZSZLMCH-UHFFFAOYSA-M sodium;chloride;hydrate Chemical compound O.[Na+].[Cl-] HPALAKNZSZLMCH-UHFFFAOYSA-M 0.000 description 1
- 239000010935 stainless steel Substances 0.000 description 1
- 229910001220 stainless steel Inorganic materials 0.000 description 1
- 239000010959 steel Substances 0.000 description 1
- 229910052715 tantalum Inorganic materials 0.000 description 1
- GUVRBAGPIYLISA-UHFFFAOYSA-N tantalum atom Chemical compound [Ta] GUVRBAGPIYLISA-UHFFFAOYSA-N 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
- 229910052726 zirconium Inorganic materials 0.000 description 1
Images
Classifications
-
- C—CHEMISTRY; METALLURGY
- C25—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES; APPARATUS THEREFOR
- C25B—ELECTROLYTIC OR ELECTROPHORETIC PROCESSES FOR THE PRODUCTION OF COMPOUNDS OR NON-METALS; APPARATUS THEREFOR
- C25B11/00—Electrodes; Manufacture thereof not otherwise provided for
- C25B11/02—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form
- C25B11/03—Electrodes; Manufacture thereof not otherwise provided for characterised by shape or form perforated or foraminous
Definitions
- the invention relates to an electrode arrangement for gas-forming electrolyzers, in particular monopolar membrane electrolysers with vertically arranged plate electrodes and counter electrodes.
- the uniform distribution is influenced by the scatterability of the electrolyte as well as by the homogeneity of the electrodes. A lack of scattering capacity can be compensated for by increasing the distance between the electrodes, but this increases the voltage drop in the cell. If there are inhomogeneities in the electrode surface, the current flow causes local warping. The parallel arrangement of the electrodes, ie the uniform distance between the anode and cathode, is therefore of great importance. Maintaining or setting a defined electrode spacing is extremely complex in gases such as chlorine, oxygen and hydrogen in technical membrane electrolysis cells.
- Electrodes with openings for the removal of the reaction gases are used, for example perforated electrodes, wire mesh or expanded metal.
- the disadvantages include in a reduced active surface, lack of mechanical stability and loss of high-quality coating material on the back of the electrode.
- an electrode plate consisting of individual plates in vertically arranged electrodes in gas-forming diaphragm cells, the individual plates having guide surfaces for the discharge of the generated gas.
- the electrodes are arranged in parallel with the smallest possible distance.
- the previously known electrodes are from one or several plates.
- the plates have horizontal slits, which are caused by bending the plate strips and provide the least resistance to the gas outlet. The bends face away from the counter electrode, there is no noticeable reduction in the active surface.
- the electrodes are ideally also to be used as conductors of the electrical current. This application does not cause problems in bipolar cells, since here the current is transported through the electrode in the direction of the electrolysis current, i.e. in any case, there is a sufficient cross-section for electricity transport. With monopolar cells, however, the current in the electrode must be transported across the electrolysis current. Flat electrodes can be used for this, but wire mesh and expanded metals cannot be used easily. This applies in particular to those electrolysis cells which, in contrast to the diaphragm cells, operate at current densities above 3 kA / m2. In this case, internal current line elements, such as line rods, are normally used, from which the current is distributed to the active surface of the electrodes (DE-OS 28 21 984).
- the invention has for its object to avoid or reduce such voltage losses and to enable high electrolysis currents.
- the invention is based on an electrode arrangement for gas-forming electrolyzers, in particular monopolar membrane electrolyzers with a vertically arranged plate electrode and counter electrode and a membrane between the plate electrode and counter electrode.
- the invention solves the problem in that an electrode arrangement of the type mentioned is designed and improved in accordance with the invention in such a way that perforated, electrically conductive and electrically conductively connected flat structures are attached as pre-electrodes to the surfaces of the plate electrodes facing the membrane, which run in parallel planes to the plate electrodes.
- the membrane is in a certain distance from the plate-shaped anode held and the filling of the space between the membrane and plate surface with electrolyte ensured.
- the pre-electrode made of openwork supports the ion-selective membrane, while the electrically highly conductive, plate-shaped electrode allows high electrolysis currents and at the same time participates in the electrolysis with its surface facing the openwork (front electrode).
- the surface of the membrane that is inactive in conventional arrangements due to the necessary perforation of the usual electrodes is also included in the electrolysis process. Furthermore, a particularly effective degassing of the electrolyte / gas suspension is brought about.
- the vertically arranged plate anode can consist, in a manner known per se, of strip-shaped titanium sheets which are bent in a certain way and have gas discharge lines corresponding to the type described in EP-OS 102 099.
- the individual strip-shaped sheets are completely separated from one another by a horizontally continuous gap.
- the plate electrode carrying the perforated flat structure can also be separated into a plurality of units which are completely separate from one another vertically or vertically and horizontally.
- Membrane electrolysis cells of such an electrode structure in which the electrode of one polarity is horizontally divided into several separate units and the electrode of the opposite polarity is divided vertically into several separate units, are known from EP-OS 97 991.
- the openwork fabrics or pre-electrodes are attached to the plate electrode at a distance of 1 to 5 mm. A distance of 1.5 to 2.5 mm is preferably maintained.
- the perforated flat structures are usually connected to cams or bosses of the plate electrode via spot welds. The distances or number of hump or spot welds are adapted to the requirements with regard to the current load. Of course, all other common connection techniques can also be used.
- the openwork, electrically conductive metallic fabric which is generally resilient and flexible and has a thickness of about 0.5 to 2 mm, can be, for example, a perforated plate (screen plate), expanded metal or wire mesh, such as wire mesh or wire mesh.
- the openwork structure can also be formed by a system of individual wires which are aligned in a plane essentially parallel to the electrode plate and are connected to the plate electrode by spot welding on the latter. The individual wires can be arranged in parallel or at an angle to one another, so that square or diamond-like structures arise.
- the construction material for the electrode arrangement according to the invention for monopolar electrolyzers depends in a manner known per se on the use of the electrode arrangement as an anode or cathode. If the electrode arrangement consisting of plate electrodes and a perforated sheet (pre-electrode) connected to it is used as an anode in the electrolysis of aqueous alkali chloride solutions, the plate and pre-electrodes consist, for example, of titanium, zirconium, niobium, Tantalum or its alloys. When used as a cathode, the material of the front and plate electrodes is, for example, stainless steel, nickel or steel plated with these metals.
- the electrode arrangement of the invention is firmly installed in a manner known per se in a frame which has connection elements for the supply of the electric current.
- the plate electrode is only provided with an activating coating on its surface facing the counterelectrode, in a known manner from e.g. Metal oxides and metals from the platinum, iridium, osmium, palladium, rhodium, ruthenium group.
- the electrode arrangement according to the invention is used in monopolar electrolyzers with membranes.
- membrane cells are only to be understood as those cells which have ion-selective membranes, such as perfluorinated cation exchange membranes.
- ion-selective membranes such as perfluorinated cation exchange membranes.
- Such membranes allow the separation of cathodic and anodic products of an electrolysis from one another or from the reactants supplied to the counterelectrode.
- the electrode arrangement according to the invention has a number of advantages.
- the ion-selective membrane is kept at the desired constant distance from the plate electrode in a simple and safe manner. Due to the fact that both the perforated pre-electrode works on the flanks of the openings and the plate electrode works on the projected areas of the openings, the current in the membrane is distributed more evenly than when only using perforated electrodes. In the space between the perforated electrode and the plate electrode is due to the geometric arrangement better degassing of the gas / electrolyte suspension and a better electrolyte exchange. Due to the arrangement of the invention, it is also possible to reduce the voltage drop.
- the K number can be reduced by values of up to 0.05 V ⁇ m2 / kA, which corresponds to a voltage gain of 200 mV at a current of 4 kA / m2.
- the gap between the front and plate electrodes was kept at a distance of 3 mm by vertical titanium wires, which simultaneously made the electrical contact between the front and plate electrodes.
- the counter electrode consisted of non-activated expanded metal made of nickel.
- the electrode gap between The front electrode and counter electrode were 4 mm.
- the membrane was in contact with the pre-electrode.
- the electrolyte temperature was 70 to 80 ° C.
- the catholyte consisted of 32% sodium hydroxide solution.
- the brine contained 310 g NaCl / l; the anolyte contained 200 g NaCl / l.
Landscapes
- 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 Non-Metals, Compounds, Apparatuses Therefor (AREA)
- Electrodes For Compound Or Non-Metal Manufacture (AREA)
- Physical Or Chemical Processes And Apparatus (AREA)
- Electroluminescent Light Sources (AREA)
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
AT87201843T ATE71672T1 (de) | 1986-11-27 | 1987-09-25 | Elektrodenanordnung fuer gasbildende elektrolyseure mit vertikal angeordneten plattenelektroden. |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE19863640584 DE3640584A1 (de) | 1986-11-27 | 1986-11-27 | Elektrodenanordnung fuer gasbildende elektrolyseure mit vertikal angeordneten plattenelektroden |
DE3640584 | 1986-11-27 |
Publications (2)
Publication Number | Publication Date |
---|---|
EP0274138A1 true EP0274138A1 (fr) | 1988-07-13 |
EP0274138B1 EP0274138B1 (fr) | 1992-01-15 |
Family
ID=6314934
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
EP87201843A Expired - Lifetime EP0274138B1 (fr) | 1986-11-27 | 1987-09-25 | Agencement d'électrode, pour électrolyseurs produisant des gaz, présentant des plaques d'électrode disposées verticalement |
Country Status (12)
Country | Link |
---|---|
US (1) | US4839013A (fr) |
EP (1) | EP0274138B1 (fr) |
JP (1) | JPS63140093A (fr) |
AT (1) | ATE71672T1 (fr) |
AU (1) | AU594214B2 (fr) |
BR (1) | BR8706360A (fr) |
CA (1) | CA1312844C (fr) |
DE (2) | DE3640584A1 (fr) |
ES (1) | ES2029683T3 (fr) |
FI (1) | FI82488C (fr) |
IN (1) | IN165046B (fr) |
ZA (1) | ZA878895B (fr) |
Families Citing this family (11)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US5221452A (en) * | 1990-02-15 | 1993-06-22 | Asahi Glass Company Ltd. | Monopolar ion exchange membrane electrolytic cell assembly |
US5254233A (en) * | 1990-02-15 | 1993-10-19 | Asahi Glass Company Ltd. | Monopolar ion exchange membrane electrolytic cell assembly |
CN1019590B (zh) * | 1990-09-03 | 1992-12-23 | 张学明 | 高效水电解制氢氧装置 |
DE4306889C1 (de) * | 1993-03-05 | 1994-08-18 | Heraeus Elektrochemie | Elektrodenanordnung für gasbildende elektrolytische Prozesse in Membran-Zellen und deren Verwendung |
IT1279069B1 (it) * | 1995-11-22 | 1997-12-04 | Permelec Spa Nora | Migliorato tipo di elettrodo per elettrolizzatori a membrana a scambio ionico |
US20030112916A1 (en) * | 2000-02-25 | 2003-06-19 | Keeney Franklin W. | Cold nuclear fusion under non-equilibrium conditions |
US6924049B2 (en) * | 2000-09-11 | 2005-08-02 | Joe G. Rich, Sr. | Electrolysis fuel cell energy plant |
WO2003095705A1 (fr) * | 2002-05-13 | 2003-11-20 | Kirk Donald W | Electrode divisee s'utilisant dans des cellules electrolytiques |
CN102196940B (zh) * | 2008-10-31 | 2013-09-25 | 丰田自动车株式会社 | 电动车辆的电源系统及其控制方法 |
CN114990603B (zh) | 2014-01-15 | 2024-02-06 | 蒂森克虏伯新纪元氯氢有限公司 | 离子交换膜电解槽 |
NL2032717B1 (en) * | 2022-08-10 | 2024-02-16 | Itrec Bv | Electrolyser and method for performing electrolysis |
Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE3123665A1 (de) * | 1981-06-15 | 1982-12-30 | Metallgesellschaft Ag, 6000 Frankfurt | Vertikal angeordnete plattenelektrode fuer gasbildende elektrolyseure |
EP0076747A1 (fr) * | 1981-09-30 | 1983-04-13 | Creusot-Loire | Electrolyseur du type filtre-presse |
EP0170419A2 (fr) * | 1984-07-02 | 1986-02-05 | Olin Corporation | Cellule à densité de courant élevée |
Family Cites Families (4)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
CH288156A (de) * | 1949-11-03 | 1953-01-15 | Montedison Spa | Elektrodensystem für Bipolarelektrolyseure. |
US4236989A (en) * | 1978-07-07 | 1980-12-02 | Ppg Industries, Inc. | Electrolytic cell |
DE3228884A1 (de) * | 1982-08-03 | 1984-02-09 | Metallgesellschaft Ag, 6000 Frankfurt | Vertikal angeordnete plattenelektrode fuer gasbildende elektrolyseure |
GB8420873D0 (en) * | 1984-08-16 | 1984-09-19 | Ici Plc | Electrode for electrolytic cell |
-
1986
- 1986-11-27 DE DE19863640584 patent/DE3640584A1/de not_active Withdrawn
-
1987
- 1987-03-24 IN IN228/CAL/87A patent/IN165046B/en unknown
- 1987-09-25 ES ES198787201843T patent/ES2029683T3/es not_active Expired - Lifetime
- 1987-09-25 DE DE8787201843T patent/DE3776122D1/de not_active Expired - Lifetime
- 1987-09-25 EP EP87201843A patent/EP0274138B1/fr not_active Expired - Lifetime
- 1987-09-25 AT AT87201843T patent/ATE71672T1/de not_active IP Right Cessation
- 1987-09-28 CA CA000547986A patent/CA1312844C/fr not_active Expired - Fee Related
- 1987-10-06 FI FI874376A patent/FI82488C/fi not_active IP Right Cessation
- 1987-10-09 US US07/107,181 patent/US4839013A/en not_active Expired - Fee Related
- 1987-11-25 BR BR8706360A patent/BR8706360A/pt not_active IP Right Cessation
- 1987-11-26 AU AU81820/87A patent/AU594214B2/en not_active Ceased
- 1987-11-26 ZA ZA878895A patent/ZA878895B/xx unknown
- 1987-11-27 JP JP62299621A patent/JPS63140093A/ja active Pending
Patent Citations (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
DE3123665A1 (de) * | 1981-06-15 | 1982-12-30 | Metallgesellschaft Ag, 6000 Frankfurt | Vertikal angeordnete plattenelektrode fuer gasbildende elektrolyseure |
EP0076747A1 (fr) * | 1981-09-30 | 1983-04-13 | Creusot-Loire | Electrolyseur du type filtre-presse |
EP0170419A2 (fr) * | 1984-07-02 | 1986-02-05 | Olin Corporation | Cellule à densité de courant élevée |
Also Published As
Publication number | Publication date |
---|---|
CA1312844C (fr) | 1993-01-19 |
FI82488B (fi) | 1990-11-30 |
ZA878895B (en) | 1989-07-26 |
ES2029683T3 (es) | 1992-09-01 |
BR8706360A (pt) | 1988-07-26 |
ATE71672T1 (de) | 1992-02-15 |
AU594214B2 (en) | 1990-03-01 |
FI82488C (fi) | 1991-03-11 |
EP0274138B1 (fr) | 1992-01-15 |
JPS63140093A (ja) | 1988-06-11 |
FI874376A (fi) | 1988-05-28 |
FI874376A0 (fi) | 1987-10-06 |
IN165046B (fr) | 1989-08-05 |
AU8182087A (en) | 1988-06-02 |
DE3776122D1 (de) | 1992-02-27 |
DE3640584A1 (de) | 1988-06-09 |
US4839013A (en) | 1989-06-13 |
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