EP0216782A1 - Bande laminee d'alliage de plomb pour grilles d'accumulateurs; cellules electrochimiques utilisant celle-ci - Google Patents

Bande laminee d'alliage de plomb pour grilles d'accumulateurs; cellules electrochimiques utilisant celle-ci

Info

Publication number
EP0216782A1
EP0216782A1 EP85906009A EP85906009A EP0216782A1 EP 0216782 A1 EP0216782 A1 EP 0216782A1 EP 85906009 A EP85906009 A EP 85906009A EP 85906009 A EP85906009 A EP 85906009A EP 0216782 A1 EP0216782 A1 EP 0216782A1
Authority
EP
European Patent Office
Prior art keywords
lead
strip
calcium
alloy
tin
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.)
Withdrawn
Application number
EP85906009A
Other languages
German (de)
English (en)
Other versions
EP0216782A4 (fr
Inventor
Fu-Wen Ling
Frank E. Haas
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.)
Revere Copper and Brass Inc
Original Assignee
Revere Copper and Brass Inc
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 Revere Copper and Brass Inc filed Critical Revere Copper and Brass Inc
Publication of EP0216782A4 publication Critical patent/EP0216782A4/fr
Publication of EP0216782A1 publication Critical patent/EP0216782A1/fr
Withdrawn legal-status Critical Current

Links

Classifications

    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/66—Selection of materials
    • H01M4/68—Selection of materials for use in lead-acid accumulators
    • H01M4/685—Lead alloys
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B15/00—Layered products comprising a layer of metal
    • B32B15/01—Layered products comprising a layer of metal all layers being exclusively metallic
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/70—Carriers or collectors characterised by shape or form
    • H01M4/72—Grids
    • H01M4/74—Meshes or woven material; Expanded metal
    • H01M4/745—Expanded metal
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/64—Carriers or collectors
    • H01M4/82—Multi-step processes for manufacturing carriers for lead-acid accumulators
    • H01M4/84—Multi-step processes for manufacturing carriers for lead-acid accumulators involving casting
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries

Definitions

  • This invention relates to laminated lead alloy composite materials for use in fabricating battery ⁇ grids... More particularly, it relates to wrought strips of a lead- calcium-tin alloy laminated on each side with an antimonial lead alloy. The invention also relates to electrochemical cells with grids constructed from these laminated materials.
  • a lead alloy is melted and continuously cast into a slab, which is then rolled into a strip.
  • the wrought strip is then mechanically expanded into a grid.
  • the grid expansion process is more advantageous than the cast method because it is less labor intensive and minimizes the possibility of the occurrence of industrial pollution problems.
  • Battery grids produced by the grid expansion method have excellent functional characteristics. They are less vulnerable to failure by grid corrosion.
  • Grid material produced by the grid expansion method is devoid of the chemical segregation and structural inhomogeneity of cast grids. For this reason, batteries made from such material usually have a longer useful active life, especially when used as supplemental power source. grids. For this reason, batteries made from such material usually have a longer useful active life, especially when used as supplemental power source.
  • lead alloys of lead , calcium and tin are generally used as the material for most grids produced by the expanded grid process. These alloys recrystallize during rolling, however, and thus lack the hardness required for use as battery grid material.
  • lead-calcium-tin alloys are not suitable for batteries which undergo deep charge-discharge cycles, such as so called "traction" batteries for small electrically powered vehicles.
  • the cycle life of the lead- calcium-tin alloys is significantly inferior to the cycle life of the antimonial lead alloys which have conventionally been used in the fabrication of cast grids.
  • Traction batteries are typically made of cast antimonial lead due to the good past adherence of the cast material during deep charging-discharging cycles.
  • U.S. Patent 4 ,401 ,730 discloses sealed, deep cycle lead acid batteries constructed with positive grids formed from cast antimony-lead alloys containing no more than about 2 weight percent of antimony and negative grids formed from alloys that are essentially antimony- free. Furthermore, these batteries have a highly porous, easily wetted separator material between the plates and a sufficient void volume to permit oxygen gas transport therethrough.
  • This patent discloses the typical construction of sealed lead-acid batteries and its content is expressly incorporated by reference herein. '
  • These cast alloys have been subject to various drawbacks and also have not been manufactured by the expanded grid technology.
  • Various modifications to cast antimonial lead battery grids have been made to overcome problems such as antimony ion migration, contamination of the battery electrolyte, and deposition on the battery cathode.
  • Patent 2,952 ,726 discloses a method for reducing the content of chemically active antimony in batteries, the grids of which are fabricated of antimony- lead alloys. This method involves the reduction of the antimony content in the surface layer portions of the positive electrode plates and pasting the negative electrode plates with an active electrode mass mixed with additives which act against self discharge by binding metallic antimony deposited on the negative plates during operation.
  • the additives consist of about 0.1 weight percent of the electrode mass of polymers of isoprene or isoprene derivatives in liquid form.
  • the surface antimony content may be reduced either by acid treatment with concentrated sulfuric acid, electrolytic treatment to form hydrogen which reacts with antimony to form gaseous antimony hydride, or by glow discharge treatment which similarly results in hydrogen generation followed by gaseous antimony hydride formation.
  • U.S._ Patent.3,933,5_2 discloses the use of non- antimonial lead alloys or antimonial lead alloys with less than 0.5 weight percent of antimony, onto which a coating of pure antimony has been applied to a surface density of from 0.0002 to 0.00132 gm/cm 2 .
  • the alloys are used for the fabrication of the positive plates of a battery grid to increase the cycle life of the batteries.
  • Such coatings may ⁇ be applied in a number of ways including electroplating, spraying, vapor deposition, sputtering and chemical displacement.
  • Such solutions however cause other problems to occur in batteries so fabricated, namely, the grids show the same high charging potential as antimony-free grids under the same conditions.
  • the thin deposited coating contains porosity which detracts from its performance.
  • the coating composition is selected such that the resulting grid achieves charging potentials of the same magnitude as are achieved with grids formed of lead alloys containing 6 to 12 weight percent antimony, while minimizing the possibility of antimony poisoning of the cathode.
  • the surface alloy disclosed,there contains from 3 to 95 weight percent of one or more of the metals copper, silver, gold, zinc, cadmium, germanium, indium, thallium, gallium, tin, - arsenic, antimony, bismuth, selenium, tellurium, chromium, 1 molybdenum, nickel and cobalt.
  • the methods for applying the surface alloy there include electroplating, dipping in molten alloy, spray metallization and deposition of evaporated metal in a vacuum. These methods deposit very thin layers of surface alloy, and porosity is again a source of problems in the performance of the alloy.
  • U.S. Patent 4,125,690 discloses the use of lead-aluminum-calcium alloys alone or in conjunction with lead-tin-calcium alloys.
  • This patent further discloses that where cold-wrought procedures are 0 used, the alloy may either be continuously cast as a slab and then preferably immediately rolled to a sheet or be additionally cooled so that it is rolled at about ambient temperature. The sheet may be rolled to reduce its 5 thickness by a reduction ratio of. from 2 to 20.
  • This invention discloses the art of using laminated wrought strip for battery grid applications, especially for so called "traction" batteries used in electrically powered vehicles.
  • the strips of the grid material consist of a layer of antimonial lead alloy, laminated to each side of a lead-calcium-tin strip.
  • the laminated s.trip is produced by a roll bonding process at room temperature .
  • This invention involves a composite metallic allo strip fabricated from a center lead-calcium-tin alloy strip laminated on both sides with an outer layer of antimonial lead alloy.
  • the composite metallic alloy strip of the invention is ideally suited for use as a battery grid material, especially, for traction batteries with deep charge-discharge cycles as employed in electrically powered vehicles.
  • the composite metallic alloy strip is produced in either a batch or continuous process by roll bonding the individual center and two outer strips.
  • the batch process is generally used for smaller scale, lower volume applications.
  • the continuous process is preferred for the production of laminated strip material in large scale, high volume applications such as in the manufacture of conventional non-deep charge-discharge lead-acid automobile batteries.
  • the roll bonding process is carried out at room temperature. This process, as utilized in the invention, serves to increase the cycle life and deep discharge g characteristics of lead-acid batteries constructed from battery grid material as disclosed herein.
  • the preferred composition contains about 0.05 to about 0.15 0 percent calcium and about 0.01 to about 0.1 weight percent tin, with the balance being substantially lead. (Unless otherwise designated, all percentages in this application refer to weight percent.)
  • a number of 5 antimonial lead alloys may be utilized for the outer strip layer. It is difficult to roll antimonial lead alloys having greater than about 10% antimony.
  • An especially advantageous composition is' about 0.5 to about 2 percent antimony and about 0.05 to about 0.5 percent arsenic, with 0 the balance being substantially lead.
  • the components of the lead-calcium-tin alloy include the following: about 0.08 to about 0.10 percent calcium and about 0.1 to about 5 0.8 percent tin, preferably between about 0.3 to 0.7 percent tin. Minor amounts (less than about 0.1 percent) of other alloying elements such as aluminum, silicon, magnesium, etc. which do not detract from the desired strength, hardness, and corrosion resistance of these lead-calcium-tin alloys,
  • antimonial lead alloys include the following: about _b_ 0.2 to 0.5 percent arsenic and about 1.2 to 2 percent antimony and preferably about 1.6 to 2 oercent antimony. Minor amounts (less than about 0.5 percent) of other alloying elements such as cadmium, rare earth metals, aluminum, etc., which do not detract from the desired electrical properties of antimony arsenic-lead alloys, may also be present.
  • This invention also encompasses the electrochemical cells constructed with a qrid of positive plates fabricated from the composite metallic alloy strip material described above and a separator material intimately contacting the grid and separating the plates thereof from one another.
  • the negative plates of these cells may also be constructed from these composite metallic strip materials. From an economic standpoint, however, it is preferable to construct these negative plates from standard lead-calcium-tin alloys.
  • the separator material should be at least about 70% porous, easily wettable and capable of wicking the electrolyte;
  • the electrochemical cells of this invention also contain an electrolyte, such as sulfuric acid.
  • the electrochemical cells of this invention reach at least about 75% depth of discharge after 2 hours and have an overall charge-discharge cycle life of at least about 200 hours, a significant and surprising improvement over batteries constructed with conventional grid materials and/or grid constructions.
  • a laminated strip for use as a battery grid can be produced by either a batch or continuous process.
  • individual lead-calcium-tin and antimonial lead alloy strips are prepared by first separately melting the alloys and static casting to slabs -measuring 2 inches x 28 inches x 33 inches.
  • the lead-calcium-tin alloy slab is then rolled to a strip ranging in thickness from 1 inch down to 0.25 inches, and preferably 0.5 inch.
  • the antimonial lead alloy slab is rolled to a strip which can be as thin as can be practicably rolled, and preferably is 0.08 inches.
  • the final rolled thickness is 0.042", since this thickness is commonly utilized in the battery industry as a preferred expanded grid size.
  • the total thickness may vary widely over a range from about 0.001 to about 0.25. Strips having ' greater or lesser total thicknesses may also be utilized, if desired, withoput departing from this invention.
  • ⁇ It is preferred to provide outer- layers of antimonial lead alloys which are sufficiently thick to • improve the electrical properties of the grid but below that which will reduce the contribution of the lead-calcium-tin to the overall strength of the strip.
  • the preferred final thickness for each outer layer ranges from 0.0002 to 0.04".
  • the preferred thickness for each outer layer will be in the jange ⁇ of about 1:5 to 1:100 (i.e. , rjat o ⁇ of each outer layer to the inner layer) and most.preferably between about 1:20 toi 1:50.
  • Alt .ough each outer layer is usually the same thickness, outer layers of different thickness can be easily provided and utilized if desired.
  • the rolling of the strip produces a multi-layer structure wherein the outer layers are relatively porosity free and are metallurgically bonded to the inner layer. This also enables the strip to provide the improved I
  • the cost of a rolled laminate is signi icantly lower in comparison to providing such outer layers by electrodeposition, coating, or otherwise depositing antimonial lead alloys on lead- calcium-tin substrates.
  • the starting thickness of the individual strips can be selected to obtain the desired final thickness for each layer as well as the total thickness. For example,- to obtain a preferred grid structure, two pieces of 0.08" antimonial lead alloy are sandwiched around an inner piece of a 0.5" lead-calcium-tin alloy. As one skilled in the rolling art would realize, however, these thicknesses can be varied to obtained different final thicknesses. Thus, by selecting different layer thicknesses before rolling, different ratios of layer thicknesses can be easily obtained. J. lmi -
  • lead-calcium-tin alloy slabs are continuously cast, to a thickness of 3/4 inch . ' The slabs are then directed to a rolling mill where they can be cold rolled to the desired thickness.
  • the antimonial lead slabs for use in the continuous lamination process are also initially rolled to a thinner desired thickness before laminating. This thinner gauqe is required for continuous processing so that the antimonial lead strips may be coiled easily.
  • One or two pieces of lead-calcium-tin strip are sandwiched between two pieces of antimonial lead strip and pack rolled to a final desired thickness of the laminate.
  • the roll b.Q&dlxiCL.operation is accomplished using a rolling mill having a 20 inch diameter roll and capable of handling a 30 inch wide strip. Such machines are well known in the industry as "Two-Hi" rolling mills.
  • a reduct on ⁇ of at least about 30% and preferably J50% or more is required to achieve the appropriate bonding between the layers. Typically, an 80 to 95% reduction is utilized.
  • Rolling ⁇ is performed "c_oldT_, at ambient temperature, however, the rolled strip experiences. a temperature rise due to frictional heat generated during the rolling operation and attains a maximum temperature of about 185°F at the end of the rolling operation.
  • the cast grid was produced using a conventional grid caster.
  • the alloys were melted and static cast to slabs of 2 inches x 28 inches x 33 inches. Slabs were then rolled to a finished gauge of 0.042 inch for grid expansion.
  • the antimonial lead was rolled to 0.08 inch strip and the lead-calcium-tin alloy was rolled to 0.5 inch strip. Two pieces of lead-calcium-tin strip were then sandwiched between two pieces of antimonial lead strip and pack rolled to 0.042 inch.
  • the finished rolled strip exhibited a thickness distribution of 0.037 inch versus 0.0025 inch for the center layer of the lead- calcium-tin alloy and the outer layers of the antimonial lead alloy, respectively.
  • Tensile strength of this laminated strip was found to be 7.5 ksi with an elongation of 15 percent. All the 0.042 inch strip was slit and then expanded into a grid having a width of about 2.68 inches.
  • the cells were constructed using, as far as possible, methods and procedures similar to those employed in commercial battery fabrication.
  • each of the batteries was approximately 6 inches x 4 inches.
  • the grids were pasted with a conventional high density formula. Efforts were made to keep the weight of paste per unit area of positive plate constant regardless of grid type.
  • Each test cell consisted of three plates. Commercially available separators of the type used in the manufacture of traction type batteries (such as armor-rib with 0.020 glass mat, manufactured by W.R. Grace) were used between the plates.
  • the cells were formed conventionally using a sulfuric acid electrolyte with a specific gravity of about 1.11 and constant current. After formation, the cells were dumped and refilled with acid having a specific gravity of about 1.32. Adjustment of the specific gravity of the electrolyte in the individual cells was then made to bring the final value to within the range 1.265 to 1.275.
  • the cells were charged for 9.5 hours through current limiting resistors from a regulated 2.6 volt bus.
  • the current was limited to a 2 hour rate at the beginning of the charge phase of the cycle. Following the charge phase there was a one-half hour rest period before commencement of the discharge phase.
  • the discharge phase was carried out to yield a 75% depth of discharge after 2 hours. As the cells progressed toward the end of the discharge phase, the voltage dropped below 1.75 volts before the end of the 2 hour discharge period. When that occurred, and automatic cell cut-off circuit terminated the discharge at 1.75 volts in order to avoid an unrealistically deep discharge cycle. Cell failure was defined to have occurred when cell capacity fell below 50 percent of the capacity of the 10th cycle. Base capacity was defined as the 10th cycle value in order to avoid initial transients. Cells were cycled at room temperature, separated from each other, to minimize heating effects.
  • antimonial lead alloy strips were sandwiched around different thicknesses of lead- calcium-tin alloy strips. These multi-layer strips were then rolled as described in the specification to a desired final dimension. The various thickness of the initial and final strips are illustrated below in Table II.
  • the antimonial-lead alloy strip comprises 2% Sb, 0.3% As, 0.2% Sn , balance Pb, while the lead-calcium-tin alloy strip comprises 0.07% Ca, 0.05% Sn, balance Pb .
  • Example layer 3 4 5 6 outer layer (top) 0.08 0.16 0.04 0.16 0.16 0.008 inner layer 0.5 ' 0.5 0.5 0.5 0.5 0.5 0.5 outer layer (bottom) 0.08 0.16 0.4 0.08 0.01 0.04 B. Laminate Thickness (in.)

Landscapes

  • Chemical & Material Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Cell Electrode Carriers And Collectors (AREA)

Abstract

Une bande laminée d'alliage de plomb convient pour des grilles d'accumulaterus à cycle complet de charge/décharge, de même que pour des grilles d'accumulateurs conventionnels au plomb. Une fine couche d'un alliage de plomb antimonial est laminée au rouleau sur les côtés d'une bande d'alliage de plomb-calcium-étain. La couche intérieure fournit une bonne résistance mécanique, alors que les couches extérieures fournissent les propriétés électrochimiques nécessaires pour une longue durée de décharge dans des accumulateurs à cycle complet de charge/décharge. L'invention concerne des procédés de fabrication et d'utilisation de cette bande comme matériau déployé de grille dans des cellules ou accumulateurs électrochimiques.
EP85906009A 1984-11-19 1985-11-18 Bande laminee d'alliage de plomb pour grilles d'accumulateurs; cellules electrochimiques utilisant celle-ci Withdrawn EP0216782A1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US67323984A 1984-11-19 1984-11-19
US673239 1984-11-19

Publications (2)

Publication Number Publication Date
EP0216782A4 EP0216782A4 (fr) 1987-03-26
EP0216782A1 true EP0216782A1 (fr) 1987-04-08

Family

ID=24701844

Family Applications (1)

Application Number Title Priority Date Filing Date
EP85906009A Withdrawn EP0216782A1 (fr) 1984-11-19 1985-11-18 Bande laminee d'alliage de plomb pour grilles d'accumulateurs; cellules electrochimiques utilisant celle-ci

Country Status (3)

Country Link
EP (1) EP0216782A1 (fr)
JP (1) JPS62501318A (fr)
WO (1) WO1986003343A1 (fr)

Families Citing this family (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JPS61124064A (ja) * 1984-11-20 1986-06-11 Matsushita Electric Ind Co Ltd 鉛蓄電池用格子体及びその製造法
US4761356A (en) * 1985-02-26 1988-08-02 Matsushita Electric Industrial Co., Ltd. Grid for lead storage batteries
IT1241001B (it) * 1990-10-31 1993-12-27 Magneti Marelli Spa Procedimento per la produzione di una griglia per elettrodi di accumulatori al piombo
JPH04286866A (ja) * 1991-03-18 1992-10-12 Matsushita Electric Ind Co Ltd シール形鉛蓄電池
JP3358508B2 (ja) * 1997-09-09 2002-12-24 松下電器産業株式会社 鉛蓄電池用エキスパンド格子体
US6096145A (en) 1997-12-18 2000-08-01 Texas Instruments Incorporated Method of making clad materials using lead alloys and composite strips made by such method
US7658774B2 (en) 2003-03-18 2010-02-09 Panasonic Corporation Method of producing lattice body for lead storage battery, and lead storage battery

Family Cites Families (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2011613A (en) * 1934-10-06 1935-08-20 Magnesium Dev Corp Magnesium duplex metal
FR1294005A (fr) * 1960-07-05 1962-05-18 Stolberger Zink A G Fuer Bergb Alliage ternaire de plomb, contenant de l'antimoine et de l'arsenic
US3867200A (en) * 1973-09-20 1975-02-18 Gen Motors Corp Method and apparatus for making oxidized expanded lead battery grids
DE2425375A1 (de) * 1974-05-25 1975-12-04 Varta Batterie Elektrodengitter fuer bleiakkumulatoren
US4166155A (en) * 1974-10-11 1979-08-28 Gould Inc. Maintenance-free battery
SE397155B (sv) * 1976-02-27 1977-10-17 Tudor Ab Galler for positiv elektrod till elektrisk blyackumulator
DE2721560A1 (de) * 1977-05-13 1978-11-16 Metallgesellschaft Ag Gitter fuer bleiakkumulatoren
US4279977A (en) * 1978-09-11 1981-07-21 General Motors Corporation Lead-calcium-tin battery grid
US4262412A (en) * 1979-05-29 1981-04-21 Teledyne Industries, Inc. Composite construction process and superconductor produced thereby

Also Published As

Publication number Publication date
JPS62501318A (ja) 1987-05-21
EP0216782A4 (fr) 1987-03-26
WO1986003343A1 (fr) 1986-06-05

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