CA1186169A - Low antimony alloy - Google Patents

Low antimony alloy

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Publication number
CA1186169A
CA1186169A CA000402809A CA402809A CA1186169A CA 1186169 A CA1186169 A CA 1186169A CA 000402809 A CA000402809 A CA 000402809A CA 402809 A CA402809 A CA 402809A CA 1186169 A CA1186169 A CA 1186169A
Authority
CA
Canada
Prior art keywords
antimony
weight percent
alloy
alloys
lead
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
Application number
CA000402809A
Other languages
French (fr)
Inventor
Raymond D. Prengaman
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.)
RSR Corp
Original Assignee
RSR Corp
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 RSR Corp filed Critical RSR Corp
Application granted granted Critical
Publication of CA1186169A publication Critical patent/CA1186169A/en
Expired legal-status Critical Current

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Classifications

    • CCHEMISTRY; METALLURGY
    • C22METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
    • C22CALLOYS
    • C22C11/00Alloys based on lead
    • C22C11/08Alloys based on lead with antimony or bismuth as the next major constituent
    • C22C11/10Alloys based on lead with antimony or bismuth as the next major constituent with tin
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00Electrodes
    • H01M4/02Electrodes composed of, or comprising, active material
    • H01M4/64Carriers or collectors
    • H01M4/66Selection of materials
    • H01M4/68Selection of materials for use in lead-acid accumulators
    • H01M4/685Lead alloys
    • YGENERAL 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
    • Y02TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02EREDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10Energy storage using batteries

Landscapes

  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Materials Engineering (AREA)
  • Organic Chemistry (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Mechanical Engineering (AREA)
  • Metallurgy (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Cell Electrode Carriers And Collectors (AREA)
  • Glass Compositions (AREA)
  • Sampling And Sample Adjustment (AREA)
  • Piezo-Electric Or Mechanical Vibrators, Or Delay Or Filter Circuits (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Superconductors And Manufacturing Methods Therefor (AREA)
  • Manufacture And Refinement Of Metals (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)
  • Connection Of Batteries Or Terminals (AREA)
  • Preventing Corrosion Or Incrustation Of Metals (AREA)

Abstract

LOW ANTIMONY ALLOY
Abstract of the Disclosure Low antimony lead alloys suitable for use as grid material in maintenance free high capacity lead acid batteries are disclosed. The alloys comprise 0.6 to 1.1 weight percent antimony, 0.06 to 0.25 weight percent arsenic, 0.1 to 0.4 weight percent tin, 0.06 to 0.11 weight percent copper and the balance lead. A preferred alloy contains 0.8 weight percent antimony, 0.15 weight percent arsenic, 0.02 weight percent tin and 0.08 weight percent copper.

Description

1~86~6~3?

a) Field of the Invention This invention relates to lead alloys having a low antimony content and containing arsenic, tin and copper~
The alloys have utility in high capacity, maintenance-free battery grids.
b~ State of the Art Lead-antimony alloys have been used as grid materials for lead acid batteries. Antimony is used to increase the strength and/~r other physical properties of lead, thereby faciliating various aspects of battery manufacture. In the case of lead-acid battery grids, this is particularly important in order for the grids to withstand normal handling during battery manufacturing and service.
The battery industry has begun produciny batteries which requlre little or no maintenance, such as addition of water to maintain the electrolyte level during the service ]ife of a battery. In such batteries it is the practice to either seal the battery or use vent plugs for the filling ports which are not easily removed by the ultimate battery user. Since the purpose of such batteries is to eliminate the need for filling, a lead alloy system must be selected in which the supply of electrolyte will not be significantly diminished over the intended life of the battery. The presence of antimony typically causes excessive gas generation in lead-acid batteries, especially during periods of charging or overcharging, which ultimately depletes the quantity of electrolyte. Such gassing is unacceptable in reduced or no maintenance batteries particularly if they are o~ the completely sealed type.
Alloys containing no antimony, such as leàd-calcium-tin, lead-strontium-tin-aluminum, and lead-calcium-,..~, --1-- ~

~6~6g tin-aluminum alloys have been introduced as maintenance-free battery grid alloys and to meet the requirements of cold cranking performance of the batteries. Lead-antimony alloys having abov~ 2.5% antlmony are not adequate for high capacity, maintenance-free battery grid alloys; rather the antimony content must be further reduced to reduce water loss or gassing in batteries during charging and increase the conductivity of the grid alloy, thus increasing the cold cranking performance of the battery. However, elimination of antimony from the battery can result in formation of non-conducting layers at the grid-active material interface, thereby reducing battery performance.
~ ccording to the lead-antimony phase diagram, the freeæing range becomes a maximum at about 3.5% antimony and antimony alloys containing less than 3.5% antimony should have reduced freezing range and no eutectic liquid. In fact, the amount of eutectic liquid is greatly reduced.
However, because of segregation effects during solidification, some eutectic may be present in alloys of l~ antimony or less indica ing that the freezing range, instead of becoming narrower, becomes wider as the antimony content is decreased.
~he combination of increased freezing range and reduced eutectic liquid make alloys in the 1-2% antimony content range very difficult to cast without cracking. To permit the use of alloys in this range, resort has been made to addition of nucleants, such as selenium, sulphur, copper, phosphorous, or aluminum, to prevent cracking. In these alloys, problems of temperature control, loss of nucleants and adverse reactions may occur and lead to loss of the alloying elements in use and produce cracking.

It has now been discovered that by restricting the antimony content of alloys to less than 1.1%, both the ~reezing range and amount of eutectic material are reduced.
However, where such alloys are cast as battery grids, at the grid intersec-tions or points where there are large differences in cross section which can cause soliclification at different r-ates some cracking can still occur due to concentration of eutectic liquid. It has further been discovered that such crac~ing can be eliminated by the addition of copper to the alloy. The low antimony alloys of the invention are suitable ror use as battery grids in maintenance-free, high capacity batteries.
c~ Summary of the Invention This invention provides a low antimony alloy which comprises 0.6 to 1.1 weight percent antimony, preferably 0.8 weight percent antimony, 0.06 to 0.25 weight percent arsenic, preferably 0.15 weight percent arsenic, 0.1 to 0.4 weight percent tin, preferably 0.20 weight percent tin, 0.06 to 0.11 weight percent copper, preferably 0.08 weight percent copper and the balance lead. The alloys are suitable for use in the grids of maintenance-free high capacity lead acid batteries.
d) Detailed Description of the Invention The present invention provides low antimony lead alloys for acid battery grids. The alloy comprises 0.6 to 1.1 weight percent antimony, preferably 0.8 weight percent antimony, 0.06 to 0.25 weight percent arsenic, preferably 0.15 weight percent arsenic, 0.1 to 0.4 weight percent tin, preferahly 0.20 weight percent tin, 0.06 to 0.11 weight percent copper, preferably 0.08 weight percent copper and the balance of lead.

-~8~

Because the alloy contains some antimony, the formation of non conducting layers at the grid-active material interface is avoided. However, because the antimony level is reduced, relatively little ~assing is observed, thus rendering the alloy suitable for use in maintenance-free batteries. Further the reduced antintony content increases the conductivity of the alloy thus increasing cold cranking performance of batteries employing the alloy as grid material.
The alloys of the invention are very fluid and can be cast into fine grain, crack and corrosion resistant battery grids which are as thin as any commercially available.
Casting can be effected by conventional grid casting techniques or by continuous grid casting processes.
A comparison was made of ~.055 inch thick grids cast from alloys of the following compositions:

Alloy A Alloy B
(Weight Percent)tWeight Percent) Antimony0.75 0.75 Tin 0.20 0.20 Arsenic0.16 0.16 Copper 0.03 0.083 Lead Balance Balance Visual inspection of the grids using 80x magnification inaicated that Alloy ~ had a large grain size with so~e cracking at grid wire intersections. In contrast ~lloy B, which is within the scope of the present invention, had a markedly reduced grain size and was very resistant to cracking and resultant penetrating corrosion.
Reduction of the antimony content of an alloy for use in battery grids results in an increase in conductivity.

This is evidenced by the data in Table I which shows the 6316~

electrical resistivity of various lead alloys.
Table Electrical Resistivity of Various lead Alloys Electrical Resistivity _1~ at 2noc OHM-cm Pure lead .00002065 Pure lead & As & Sn & Cu . 0000212 0.8% Sb Alloy .00002185 1.0~; Sb-Lead .0000220
2.0~s Sb Lead . O000227
3.0% Sb-Lead .0000234
4.0% Sb-Lead .000024 0
5.09~ Sb-Lead .0000246 Pb-0.1 Ca-0.3 Sn .0000219 The data indicate that the 0.8% antimony alloy is 11% more conductive than conventional 5% antimony and 6%
more conductive than 2.75% low antimony alloys and equal in conductivi ty to the Pb-Ca-Sn alloy.
Since corrosion of the antimony from the positive grid and transfer to the negative is the major cause of gassing in batteries, the reduced amount of antimony and the dispersed nature of the antimony particles due to the copper additive will reduce antimony corrosion from the positive grid and concomitant transfer to the negative grid where alloys of the present invention are employed.
A major problem with low antimony alloys has been sufficient strenyth and rate of strengthening for processing after casting. The presence of arsenic and copper in the alloy of the invention gives the alloy initial hardness and adequate handling strength due to precipitation of the copper and arsenic throughout the alloy.
Table II below shows the rate of aging and ultimate hardness levels of the 0.8% antimony alloy compared to conventional low antimony alloy and an alloy of 0. 09% Ca-0.3% tin. The alloys were cast into 1/4" thick plates andcooled by blowing air over the surface. The hardness was ~ ~L8~

measured by the R~ckwell ~R" scale (1/2" D Ball with an applied load of 60 Kg). The duration of the test was 30 seconds.
Table II

Rate of ~ardening of Various Alloys After Casting Rockwell "R" Hardness of Alloys ~ging Time New fter Castin~2. 75~o Sb Pb-0.09 Ca-0.3 Sn 0.8~ Sb Alloy l Minute 40 ~ 10 5 Minutes 69 22 60 15 Minutes 80 40 7Q
l Hour 82 6~ 76 24 Hours 86 76 79 4 Days 88 78 79 7 Days 30 79 79 14 Days 92 80 79 30 Days 92 83 80 The first -test was conducted one minute after casting. The samples were still hot at this time and this represents the hardening condition of a much thinner battery grid soon aEter ejection Erom the mold as it would be handled for trimming. The new 0.8% antimony alloy is slightly stronger than the 0.09% Calcium-0.3% tin alloy due to the slight amount of eutectic and copper second phase particles in the structure. The 0.8% Sb alloy, however, is weaker than the conventional low antimony alloy ~2.75~ Sb) which contains more strengthening antimony eutectic network.
The 0.8~ antimony alloy strengthens rapidly as it cools, reaches 95~ of its strength in one hour and is virtually fully aged in one day. The 2.75~ antimony and the lead-calcium alloys continue to slowly harden. ~fter seven days, the lea~-calcium and the 0.8% antimony alloy are at the same hardness with b~th alloys softer than the 2.75% antimony alloy. The mechanical properties of the fully aged (30 days) alloys are shown in Table III.

Table III
Mechanical Properties of Various Alloys ~ged 30 Days 2.75% Sb O.O9Ca-0.3 Sn 0.8% Sb UTS (psi) 7000 6500 5500 YS (psi) 5800 4B00 3750 Elongation 10% 30% 30~
Based on the hardness tests of Table II, the alloy hardens sufficiently after seven days to be processed through casting, trimming, and pasting comparably to the Pb - 0.09 Ca -0.3 Sn alloy. After 3~ days, the alloy is slightly weaker than the Pb-Ca-Sn alloy and significantly weaker than the conventional low (2.75%) antimony alloy. The reduced strength is due to the reduced antimony content.
Overall -the low antimony alloy of the inven-tion would be significantly more conductive than conventional low antimony alloys containing greater amounts of antimony.
Thus cold cranking performance comparable to Pb-Ca-Sn alloy batteries could be achieved. Further gassing rate can b~
greatly reduced compared to conventional low antimony alloys because of the reduced antimony eutectic content and increased distribution of the antimony. The alloy has suEficient hot str~ngth and aged mechanical properties to be handled in casting and pasting. The reduced antimony content, and the addition of copper produce a reduced freezing range and uniform fine grained crack-resistant grain structure.
Finally, the a~loy is very Eluid and can be easily cast into -the thinnest commercially available grids.
The alloy of the invention may contain nucleating agents such as are present in conventional low antimony alloys. For example, sulfur, selenium, tellurium, phosphorous and/or aluminum may be incorporated into the alloy of the
6~

invention in amounts which do not destroy its mechanical or operational characteristics. However, such additives are not necessary for achieving the above~described beneficial characteristics oE the alloy of the invention.

Claims (2)

The embodiments of the invention in which an exclusive property or privilege is claimed are defined as follows:
1. A lead alloy for use in lead-acid batteries comprising 0.6 to 1.1 weight percent antimony, 0.06 to 0.25 weight percent arsenic, 0.1 to 0.4 weight percent tin, 0.06 to 0.11 weight percent copper and the balance lead.
2. The alloy of Claim 1 containing 0.8 weight percent antimony, 0.15 weight percent arsenic, 0.20 weight percent tin and 0.08 weight percent copper.
CA000402809A 1981-06-03 1982-05-12 Low antimony alloy Expired CA1186169A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US06/270,134 US4376093A (en) 1981-06-03 1981-06-03 Low antimony alloy
US270,134 1981-06-03

Publications (1)

Publication Number Publication Date
CA1186169A true CA1186169A (en) 1985-04-30

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ID=23030046

Family Applications (1)

Application Number Title Priority Date Filing Date
CA000402809A Expired CA1186169A (en) 1981-06-03 1982-05-12 Low antimony alloy

Country Status (10)

Country Link
US (1) US4376093A (en)
EP (1) EP0071001B1 (en)
JP (1) JPS6020455B2 (en)
AT (1) ATE19794T1 (en)
AU (1) AU530569B2 (en)
BR (1) BR8203214A (en)
CA (1) CA1186169A (en)
DE (1) DE3271120D1 (en)
MX (1) MX164793B (en)
PH (1) PH19538A (en)

Families Citing this family (12)

* Cited by examiner, † Cited by third party
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JPS6229063A (en) * 1985-07-29 1987-02-07 Shin Kobe Electric Mach Co Ltd Positive electrode plate for lead storage battery
US5120429A (en) * 1987-07-10 1992-06-09 Lummus Crest Inc. Co-processing of carbonaceous solids and petroleum oil
JP2748126B2 (en) * 1988-08-15 1998-05-06 日本製箔株式会社 Lead alloy rolled foil
NL9101376A (en) * 1990-08-16 1992-03-16 Digital Equipment Corp AN IMPROVED ERROR DETECTION CODING SYSTEM.
US5352549A (en) * 1992-08-19 1994-10-04 Gnb Battery Technologies Inc. Lead oxide composition for use in lead-acid batteries
US5508125A (en) * 1994-03-21 1996-04-16 Globe-Union Inc. Battery straps made of a lead-based alloy containing antimony, arsenic, tin and selenium
US6114067A (en) * 1998-04-08 2000-09-05 East Penn Manufacturing Company, Inc. Corrosion resistant lead alloy for lead-acid batteries
US20050112470A1 (en) * 1998-06-26 2005-05-26 Johnson Controls Technology Company Alloy for battery grids
US20040110067A1 (en) * 2002-12-06 2004-06-10 Johnson Controls Technology Company Alloy for battery grids
CN100385720C (en) * 2006-01-05 2008-04-30 赵恒祥 Alloy material of battery positive grid and preparation method thereof
US9168647B2 (en) * 2008-10-21 2015-10-27 Michael A. Logan Automobile rim hammer
CN114284583A (en) * 2021-12-27 2022-04-05 河南超威正效电源有限公司 Method for reducing EFB power-on and power-off pool water loss

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CA542499A (en) 1957-06-18 National Lead Company Grid metal alloy
US682330A (en) * 1901-04-10 1901-09-10 Hans Leyendecker Alloy.
US1021997A (en) * 1912-02-24 1912-04-02 William Morrison Storage-battery conductor or support.
US1674958A (en) * 1924-06-21 1928-06-26 Western Electric Co Alloy
GB473911A (en) 1936-06-04 1937-10-22 Goodlass Wall & Lead Ind Ltd Improvements in the manufacture of lead alloys
US2446996A (en) * 1942-06-06 1948-08-17 Bell Telephone Labor Inc Metal objects coated with lead alloys
US2694628A (en) * 1951-07-14 1954-11-16 Nat Lead Co Grid metal alloy
US2841491A (en) * 1955-12-16 1958-07-01 Gould National Batteries Inc Battery grid alloy
DE1113579B (en) * 1959-03-11 1961-09-07 Accumulatoren Fabrik Ag Lead-antimony alloy for the grid of the plates of electrical accumulators
US3287165A (en) * 1964-12-03 1966-11-22 Eltra Corp High capacity lead acid battery with lead calcium negative grids
GB1461260A (en) * 1973-03-15 1977-01-13 Electric Power Storage Ltd Electric storage battery grids
US3912537A (en) * 1974-03-07 1975-10-14 Electric Power Storage Ltd Electric storage battery grids
GB1461266A (en) * 1973-03-15 1977-01-13 Electric Power Storage Ltd Electric storage battery grids
DE2319711A1 (en) * 1973-04-18 1974-10-31 Metallgesellschaft Ag Lead-antimony-arsenic alloys - used for constructional elements requiring high creep strength
DE2337708C2 (en) * 1973-07-25 1983-03-24 Accumulatorenfabriken Wilhelm Hagen Ag Soest-Kassel-Berlin, 4770 Soest Lead-antimony alloy
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US3990893A (en) * 1974-08-19 1976-11-09 Varta Batterie Aktiengesellschaft Lead alloy for battery grid
US4113476A (en) * 1976-10-20 1978-09-12 General Battery Corporation Method of treating low antimony alloy battery grid material with phosphorus
US4158563A (en) * 1977-10-11 1979-06-19 N L Industries, Inc. Low antimonial lead alloy for making grids for use in maintenance free batteries
DE2826590A1 (en) 1978-06-19 1980-01-03 Metallgesellschaft Ag Lead alloy for mfg. accumulator grids - contains tin pref. together with arsenic and selenium and has relatively low antimony content to reduce cost
US4159908A (en) * 1978-08-14 1979-07-03 N L Industries, Inc. Alkali metal containing battery grid lead alloy
DE2907227C2 (en) * 1979-02-23 1985-05-09 Metallgesellschaft Ag, 6000 Frankfurt Use of a lead alloy

Also Published As

Publication number Publication date
PH19538A (en) 1986-05-20
JPS6020455B2 (en) 1985-05-22
US4376093A (en) 1983-03-08
EP0071001A1 (en) 1983-02-09
DE3271120D1 (en) 1986-06-19
MX164793B (en) 1992-09-24
BR8203214A (en) 1983-04-12
ATE19794T1 (en) 1986-05-15
AU530569B2 (en) 1983-07-21
JPS581039A (en) 1983-01-06
EP0071001B1 (en) 1986-05-14
AU8386482A (en) 1982-12-09

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