CA1122273A - DRY CELL CATHODE OF .beta.-MNO.SUB.2 AND HETAEROLITE - Google Patents

DRY CELL CATHODE OF .beta.-MNO.SUB.2 AND HETAEROLITE

Info

Publication number
CA1122273A
CA1122273A CA000322643A CA322643A CA1122273A CA 1122273 A CA1122273 A CA 1122273A CA 000322643 A CA000322643 A CA 000322643A CA 322643 A CA322643 A CA 322643A CA 1122273 A CA1122273 A CA 1122273A
Authority
CA
Canada
Prior art keywords
hetaerolite
mno2
beta
ore
cells
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
CA000322643A
Other languages
French (fr)
Inventor
Frank L. Tye
John E.A. Shaw
Andrzej K. Agopsowicz
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.)
Berec Group Ltd
Original Assignee
Berec Group Ltd
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 Berec Group Ltd filed Critical Berec Group Ltd
Application granted granted Critical
Publication of CA1122273A publication Critical patent/CA1122273A/en
Expired legal-status Critical Current

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Classifications

    • 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
    • H01M4/36Selection of substances as active materials, active masses, active liquids
    • H01M4/48Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides
    • H01M4/50Selection of substances as active materials, active masses, active liquids of inorganic oxides or hydroxides of manganese
    • HELECTRICITY
    • H01ELECTRIC ELEMENTS
    • H01MPROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M6/00Primary cells; Manufacture thereof
    • H01M6/04Cells with aqueous electrolyte
    • H01M6/06Dry cells, i.e. cells wherein the electrolyte is rendered non-fluid

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  • Chemical & Material Sciences (AREA)
  • Inorganic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Electrochemistry (AREA)
  • General Chemical & Material Sciences (AREA)
  • Battery Electrode And Active Subsutance (AREA)
  • Inorganic Compounds Of Heavy Metals (AREA)

Abstract

ABSTRACT

A dry electric cell of the Leclanche type having a cathode mix which includes (i) MnO2 having a .beta.-crystal structure, and (ii) either hetaerolite (Zno.Mn2O3) or materials which enable hetaerolite to be generated in situ at a sufficiently rapid rate so that it constitutes the major discharge product even at moderate to high rates of discharge.

Description

ll;~Z273 The present invention relates to dry electric cells of the Leclanche type.
Cathode mixes of dry cells of the Leclanché type usually contain manganese dioxide, zinc oxide, carbon black, zinc chloride, ammonium chloride and sometimes graphite.
The best cell capacities are achieved by using chemically or electrolytically manufactured manganese dioxides. Such manganese dioxides usually have an~ or~ crystal structure and usually contain about 90% MnO2.
Naturally occurring manganese dioxides can also be used in cathode mixes for Leclanché cells because they are much cheaper although they give somewhat poorer cell capacities. The naturally occurring ores which are generally preferred for use in cathode mixes for such cells also have the~ orP crystal structure and after appropriate refining generally contain up to 82% MnO2. Deposits of this type of ore are scarce and in some case nearing exhaustion.
The moxt common naturally occurring type of manganese ore is pyrolusite in which the manganese dioxide has a ~- crystal structure (~-MnO2). Although grades of pyrolu-site containing up to 92% MnO2 are available, the pyrolu-site ores are generally known to give very poor results when used in cathode mixes for cells of Leclanché type.
The superior capacity of cells containing ~andp crystalline manganese dioxides has been ascri~e~ to tile fact that they undergo electrochemical reduction in the homogeneous phase down to a composition rep-ll;~ZZ73 resented by MnOl 5.
The overall cell reaction is 2MnO2 + Zn + 2NH4 C1 - 2Mn OOH + Zn (NH3)2 C12 In contrast, in cells containing B-MnO2, the electro-chemical reduction proceeds in the heterogeneous phase. In such cells, the overall cell reaction predominantly is MnO2 + Zn + 4NH4Cl + Zn C12 Mn C 2 ( 3) 2 2 results in consumption of the electrolyte salts NH4Cl and ZnC12 in the cell. The working life of cells of this type is thus limited by the exhaustion of these electrolyte salts.
We have now found that in certain circumstances high capacity cells in which the manganese dioxide in the cathode mix is all or predominantly ,B-MnO2 can be obtained.
Accordingly, the present invention provides a dry electric cell of the Leclanché type having a cathode mix which includes (i) MnO2 having a ,B-crystal structure, and (ii) hetaerolite (ZnO.Mn2O3).

In this specification the terms "moderate" and "high"
rates of discharge are used to mean discharge rates for Leclanche cells of the order given in the International Electrotechnical Commission's (IEC) publication No. 86-2 (Primary Batteries) for a given size of battery as suitable for application in "portable lighting", "transistor radios"
and "pocket calculators".

We have found that ,B-MnO2 can be utilized efficiently in dry electric cells provided that hetaerolite is the discharge product of the cell. Under typical discharge ll;~ZZ73 conditions hetaerolite does not appear to nucleate spontan-eously when untreated ~-MnO2 ore is used alone. However, if hetaerolite nuclei are provided by appropriate pretreat-ment of the ~-MnO2 ore, or by addition of hetaerolite to the cathode mix, the main overall discharge product formed in the cell will be hetaerolite. The result of the pre-treatment of the ore or the use of the additives which include or generate hetaerolite at a sufficiently rapid rate is that the ~-MnO2 is reduced with high efficiency in the cell. Furthermore, when the main discharge product is hetaerolite, little or no ammonium chloride or zinc chloride are consumed when the cell is in operation. Thus less ammonium chloride and more manganese dioxide can therefore be included in the cell to improve its capacity.
The ~-MnO2 is preferably obtained as a naturally-occurring ore such as pyrolusite.
Preferably 40 - 100~ of the total weight of the MnO2 in the cathode mix of the cell of the present invention is ~-MnO2.
Synthetically prepared hetaerolite is an example of a type of hetaerolite which can be added to the cathode mix as a separate ingredient. An alternative source of hetaerolite is ~-MnO2 containing ore pretreated in the presence of zinc or a compound of zinc so as to produce some hetaerolite phase in the ore.
It has been found that in the cells of the present invention optimum efficiency can be obtained even though an amount of ammonium chloride which is smaller than the amount usually found necessary in corresponding cells containing~ and~ manganese dioxides is used. Therefore, ~' il;~Z273 cathode mixes can contain a greater proportion of manganese dioxides and this results in the cells having excellent capacities.
The invention also provides a battery including one or more cells according to the present invention.
The following Examples illustrate the invention.
In the accompanying drawings, referred to in the Examples, Figures l and 2 are graphs relating discharge time to closed circuit voltage.

Example l. Pretreatment of 3-MnO2 to produce hetaerolite A solution was prepared by mixing equal volumes of aqueous zinc chloride solution (S.G. 1.45) and water. The solution was then saturated at 25C with respect to ammon-ium chloride and zinc oxide.
To 100ml of this solution was added:
92% grade ~-MnO2 ore of Moroccan origin. 50g Hydrated manganous chloride MnC12.4H2O 3.25g Zinc oxide 3g Ammonium chloride 4g The slurry was stirred for 4 days at temperatures in the range 80 - 90C. The solids were then filtered off, washed and dried. X-Ray diffraction analysis of the resultant treated ore showed, in addition to the phases originally present in the ore, a trace of hetaerolite ZnO.
Mn203 .
Two separate cathode mixes were prepared using treated and untreated ore according to the formulation:

i~ZZ~73 Manganese dioxide (treated or untreated) 23.08g Zinc oxide 0.25g Ammonium chloride 11.36g Acetylene black 3.55g Zinc chloride solution (S.G. 1.45)7.47g Water 4.25g Two paper lined R20 size cells containing 48.1 g cathode mix per cell were made. Each cell was subjected to a dis-charge test through a 5 ohm resistance for 30 minutes per day, 7 days per week at 20C. The discharge curves and the open circuit voltages measured immediately before each discharge cycle are plotted in Figure 1 as curve a for untreated ore and curve _ for treated ore. It can be seen that the cell which had been made with the untreated ore give a steeply falling discharge curve. Its on load volt-age fell below 0.75v. after 8.5 hours total discharge. On the other hand the cell which had been made with treated ore gave a flatter discharge curve and sustained an on load voltage above 0.75v for 21.5 hours of discharge.
After discharge the cells were opened, the discharged cathode mixes extracted and subjected to X-ray diffraction analysis. No hetaerolite could be detected in the mix made with untreated ore while a strong diffraction pattern corresponding to hetaerolite was recorded on the mix made with treated ore.
Example 2. Addition of Hetaerolite A cell with 92% ~-MnO2 ore gave a discharge life of 58 hours when subjected by a discharge test through a 40 ohm resistance 4 hours per day, 7 days per week at 20C

to an end point of 0.9v. The discharge curve and open ilZ2Zt73 circuit voltage for this cell are shown on Figure 2 as curve c. A similar cell in which a 4:1 mixture of 92% ~-MnO2 ore and laboratory synthesized hetaerolite was substituted for the manganese dioxide gave 203 hours discharge life on the same discharge test. The discharge curve and open circuit voltage for this cell are shown on Figure 2 as curve d.
The present invention thus enables one to use sources of manganese dioxide previously considered unsuitable for use in cathode mixes and to achieve greater cell and battery capacities using natural ore than has been possible in the past.

Claims (6)

The embodiments of the invention in which an exclusive property or privilege is claimed are defined as follows:
1. A dry electric cell of the Leclanché type having a cathode mix which includes (i) MnO2 having a .beta.-crystal structure, and (ii) hetaerolite (ZnO.Mn2O3).
2. An electric cell according to claim 1 in which hetaerolite has been added as a separate ingredient to the cathode mix.
3. An electric cell according to claim 1, wherein the .beta.-MnO2 is one which has been subjected to a chemical or thermal pre-treatment in the presence of zinc or a compound of zinc so as to produce some hetaerolite there-in.
4. An electric cell according to claim 1, wherein the .beta.-MnO2 is obtained from a naturally-occurring ore.
5. An electric cell according to claim 4, wherein the naturally-occurring ore is pyrolusite.
6. A battery including one or more cells, each of which cells is a dry electric cell of the Leclanché type having a cathode mix which includes (i) MnO2 having a .beta.-crystal structure, and (ii) hetaerolite (ZnO.Mn2O3).
CA000322643A 1978-03-02 1979-03-02 DRY CELL CATHODE OF .beta.-MNO.SUB.2 AND HETAEROLITE Expired CA1122273A (en)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
GB8356/78 1978-03-02
GB8356/78A GB1557754A (en) 1978-03-02 1978-03-02 Dry electric cells

Publications (1)

Publication Number Publication Date
CA1122273A true CA1122273A (en) 1982-04-20

Family

ID=9850963

Family Applications (1)

Application Number Title Priority Date Filing Date
CA000322643A Expired CA1122273A (en) 1978-03-02 1979-03-02 DRY CELL CATHODE OF .beta.-MNO.SUB.2 AND HETAEROLITE

Country Status (15)

Country Link
US (1) US4221853A (en)
JP (1) JPS54135322A (en)
BE (1) BE874581A (en)
CA (1) CA1122273A (en)
DE (1) DE2908052A1 (en)
DK (1) DK89879A (en)
EG (1) EG13620A (en)
ES (1) ES478218A1 (en)
FR (1) FR2418965A1 (en)
GB (1) GB1557754A (en)
GR (1) GR66974B (en)
HK (1) HK25080A (en)
IT (1) IT1120951B (en)
NL (1) NL7901490A (en)
ZA (1) ZA79760B (en)

Families Citing this family (10)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
AT321494B (en) * 1973-07-02 1975-04-10 Mag Pharm Horst Hrovat Device for subdividing store or the like.
US4312930A (en) * 1978-09-29 1982-01-26 Union Carbide Corporation MnO2 Derived from LiMn2 O4
DE3123100A1 (en) * 1981-06-11 1983-01-05 Varta Batterie Ag, 3000 Hannover MANGANE DIOXIDE ELECTRODE FOR LITHIUM BATTERIES
DE3242139C2 (en) * 1982-11-13 1984-09-06 Accumulatorenwerke Hoppecke Carl Zoellner & Sohn GmbH & Co KG, 5790 Brilon Process for the production of positive electrodes for electrochemical elements, in particular Li / Mn0 2 cells and electrodes produced by this process
JPS60189163A (en) * 1984-03-06 1985-09-26 Sony Corp Lithium-manganese dioxide battery
DK0931362T3 (en) * 1996-10-10 2001-08-27 Merck Patent Gmbh Modified electrode material and its use
EP0960445A1 (en) 1997-01-31 1999-12-01 MERCK PATENT GmbH New manganese dioxide electrodes, process for producing the same and their use
DE10016024A1 (en) 2000-03-31 2001-10-04 Merck Patent Gmbh Active anode material in electrochemical cells and process for their manufacture
EP1337600A2 (en) 2000-11-30 2003-08-27 MERCK PATENT GmbH Particles with opalescent effect
US7718319B2 (en) 2006-09-25 2010-05-18 Board Of Regents, The University Of Texas System Cation-substituted spinel oxide and oxyfluoride cathodes for lithium ion batteries

Family Cites Families (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US1173965A (en) * 1911-05-10 1916-02-29 Griesheim Elektron Chem Fab Galvanic battery.
US1430726A (en) * 1920-02-24 1922-10-03 Winchester Repeating Arms Co Manufacture of dry cells
GB551471A (en) * 1941-08-20 1943-02-24 John William Smith Improvements in depolarising materials
GB569217A (en) * 1943-04-30 1945-05-14 Boots Pure Drug Co Ltd Improvements relating to the production of depolarising materials for use in primaryelectrical cells
FR1336429A (en) * 1961-08-19 1963-08-30 Knapsack Ag Process for the treatment of synthetic manganese dioxide, in particular for use as a depolarizing agent in dry cells
US3242013A (en) * 1961-08-19 1966-03-22 Knapsack Ag Dry cell batteries with a pyrolusite depolarizing agent
FR1519624A (en) * 1966-12-23 1968-04-05 Wonder Piles Improvements in the manufacture of manganese dioxide, in particular for electrochemical generators, and manganese dioxide thus obtained

Also Published As

Publication number Publication date
JPS54135322A (en) 1979-10-20
IT7967444A0 (en) 1979-03-01
FR2418965A1 (en) 1979-09-28
ZA79760B (en) 1980-02-27
IT1120951B (en) 1986-03-26
US4221853A (en) 1980-09-09
GR66974B (en) 1981-05-15
GB1557754A (en) 1979-12-12
DK89879A (en) 1979-09-03
BE874581A (en) 1979-07-02
HK25080A (en) 1980-05-16
EG13620A (en) 1982-03-31
NL7901490A (en) 1979-09-04
ES478218A1 (en) 1979-08-01
DE2908052A1 (en) 1979-09-13

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