WO2003107461A1 - Secondary cell - Google Patents

Secondary cell Download PDF

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Publication number
WO2003107461A1
WO2003107461A1 PCT/US2002/015157 US0215157W WO03107461A1 WO 2003107461 A1 WO2003107461 A1 WO 2003107461A1 US 0215157 W US0215157 W US 0215157W WO 03107461 A1 WO03107461 A1 WO 03107461A1
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WO
WIPO (PCT)
Prior art keywords
complex
secondary cell
negative electrode
chromium
positive
Prior art date
Application number
PCT/US2002/015157
Other languages
French (fr)
Inventor
Show-Jong Yeh
Yu-Ta Tu
Original Assignee
Sunyen Co., 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
Priority claimed from US10/170,716 external-priority patent/US20030228514A1/en
Application filed by Sunyen Co., Ltd. filed Critical Sunyen Co., Ltd.
Priority to AU2002343324A priority Critical patent/AU2002343324A1/en
Publication of WO2003107461A1 publication Critical patent/WO2003107461A1/en

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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
    • H01M4/36—Selection of substances as active materials, active masses, active liquids
    • H01M4/58—Selection of substances as active materials, active masses, active liquids of inorganic compounds other than oxides or hydroxides, e.g. sulfides, selenides, tellurides, halogenides or LiCoFy; of polyanionic structures, e.g. phosphates, silicates or borates
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/06—Lead-acid accumulators
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/24—Alkaline accumulators
    • 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
    • H01M4/661—Metal or alloys, e.g. alloy coatings
    • 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

  • the present invention relates to a rechargeabjle secondary cell and, more particularly, to a secondary ell which has relatively high capacitance and stable charge/discharge current',) which can b6 charged/discharged with reduced risk of explosion, and which can be manufactured at low cost.
  • the positive electrode complex and the negative electrode complex' are in a combination selected from the group consisting of lead/chromium complex, chromium complex /aluminum complex, and manganese complex/zinc complex.
  • a secondary cell As compared with a primary cell, a secondary cell is rechargeable and thus is environn entally friendly.
  • a sepondary cell can be recharged, for example, more than 500 times. Therefore, when the total service life is considered, a secondary cell would benefit the user.
  • nickel-cadmium cell has been widely used in portable radios, remote controls, flash lights and the Jike.
  • the nickel-hydrogen hydride cell cto be used for replacing the nickel-cadmium cell and has a capacitance higher than that of the latter. Accordingly, the nickel-hydrogen cell has been widely used in cameras, mobile phones, portable computers and the like.
  • the lithiunl ion cell has a capacitance higher than that of the nickel ⁇ hydrogen cetf.
  • a lithium ion cell of standard size used for a mobile phone has a capacitance in the range of from 500 mAh to 700 mAh.
  • the object of the present invention is, therefore, to provide a secondary cell which may generate a direct current when the positive electrode compound and the negative electrode compound thereof conduct a reversible redox reaction in the presence of an electrolyte, wherein the positive electrode complex and the negative electrode pomplex are in a combination (represented by positive electrode complex/the negative electrode complex) selected from the group consisting of lead/chromium complex, chromium complex/aluminum complex, and manganese complex/zinc complex.
  • the secondary cell according to the present invention has relatively high capacitance, and more stable chemical reactio ⁇ s So that it can be stably charged/discharged without risk of explosion, with large current, and yet can be manufactured at low cost.
  • Fig. 1 is a schematic drawing of the lead-chromium secondary poll according to one preferred embodiment of the present invention
  • Fig. 2 is a schematic drawing qf the aluminum-chromium sepondary cell according to another preferred embodiment of the present invention.
  • Fig. 3 is a schematic drawing of the manganese-zinc secondary cell according to still another preferred embodiment of the present invention. Detailed Description of Preferred Embodiments
  • the lead-chromium secondary cell comprises l ⁇ ad -as the positive electrode 1, a cliromium complex as the negative electrode 2, a lead foil or lead alloy fpil as the positive plate 3, a copper fojl as the negative plate 4, a diluted sulfbric, acid as the electrolyte 5, and a spacer (not shown) disposed between thp positive and negative electrodes.
  • the positive electrode consists essentially of PbOz(0.1 to 0.5 mole) and, a chelating agent (0.05-0.3 mole) and' the negative electrode is chrorn im complex (0.05 to 0.3 mole).
  • the electrolyte consists essentially of H2SO4 having a eonpentration of 10-50% and may inelude HC1.
  • the reaction scheme of the charge/discharge thereof is as follows;
  • the chromium forms a chromium complex during the charge, it does not react and combine with the sulfate radical and thus the capacitanpe of the secondary cell can be significantly increased.
  • the acid decreases in concentration until any one of the sulfate radical and chromium is exhausted or the chromium complex has a saturated concentration.
  • an aluminum-chromium secondary cell comprises a chroririum complex as the positive electrode 6, an aluminum complex as the negative electrode 7, an aluminum foil as the positive plate 8, a cpppef foil as the negative pt ⁇ te S, a diluted potassium hydroxide as the electrolyte 10, an a spacer (not shown) disposed between the positive and negative jelectrodes.
  • the positive electrode of' this embodiment consists of Cr 2 + (0.1-0.4 mole) and the negative electrode consists essentially of aluminum complex (0.1-0.4 mole);
  • the KOH electrolyte has a preferred concentration of 5-40% .
  • a chelating agent in an amount suph as 0.05-0,3 mole may be included.
  • the reaction scheme of the charge/discharge thereof is as follows:
  • hydroxide ion is formed, sp that the electrolyte increases in hydroxide ipn concentration until it reaches the original concentration.
  • the electrolyte decreases in hydroxide ion concentration until any one of the lead and ch omate is completely reacted.
  • overcharge should be avoided because it will result in the depletion of the water in the eleptrolyte and catuse a short circuit
  • the manganese-zinc secondary cell comprises a manganese complex as the positive electrode 11, a zinc complex as the negative electrode 12, a lead foil as the positive plate 13, a copper foil as the negative plate 14, a diluted potassium hydroxide as the electrolyte 15, and a spacer (not shown) disposed -between the positive and negative Electrodes.
  • the positive electrode preferably consists essentially of Mn ⁇ 2 (0 * 05-0.2 mole) and negative eleqtfode preferably consists essentially of Zinc complex (Oil -0.4 mole).
  • a chelating agent in an amount suph as 0,05 to 0.3 mole is preferably included.
  • the KOH electrolyte m y have a concentration of 5 to 30%. The reaption scheme of the charge/discharge thereof is as follows:
  • the zinc will result in the occurrence of a- hydrated ion or combine with hydrogen to form a zinp-hydrogen complex.
  • a lead-phromium secondary cell comprising lead as the positive electrode, a chromium complex as the negative eleotrode, a lead foil as the positive plate, a copffer foil as the negative plate, spacer disposed between the positive and negative electrodes, and a diluted sulfurie acid as the electrolyte was prepared.
  • the secon r cpll was, made into a standard battery for an ordinary mobile phone- The resulting standard battery as fully charged. Thereafter, the capacitance and the discharge voltage thereof at room temperature were measured and had 800 mAh and 2.4 volts, respeptively.
  • An aluminum-rebj'omium seeondary cell comprising a chromium complex as the positive electrpde, an aluminum complex as the negative electrode, an aluminum foil as the positive plate, a copper foil as the negative plate, a spacer, disposed between the positive and negative electrodes, and a diluted potassium hydroxide as the electrolyte was prepared.
  • the secondary pell was made into a standard battery for an ordinary mobile phone, The resulting standard battery was fully charged. Thereafter, the capacitance and the discharge voltage thereof at room tempera,ture were measured and had 20 0 mAh and 3.0 volts, respe ⁇ tively.
  • a manganese-zinc sepondary celi comprising a manganese complex as the positive electrqd ⁇ , a zinc complex as the negative electrode, a lead foil as the positive plate, arid a copper foil as the negative plate, a spacer disposed between the positive and negative electrodes, and a diluted potassium hydroxide as the electrolyte was prepared.
  • the secondary cell was made into a standard battery for an ordinary mobile phone. The resulting standard battery was fully charged, thereafter, the capacitance and the discharge voltage thereof at room temperature were measured and had 2000 mAh and 2.4 volts, respectively It can be seen from the results of the above examples and descriptions that a secondary cell, according to the present invention has relatively high capacitance and can be ⁇ anufactured at low cost. Moreover, it is used safely and can be stably charged/discharged with large current.

Abstract

In a secondary cell which generates a direct current when the positive electrode complex and the negative electrode complex thereof conduct a reversible redox reaction in the presence of an electrolyte, the positive electrode complex and the negative electrode complex are in a combination (represented by positive electrode complex/negative electrode complex) selected from the group consisting of lead/chromium complex, chromium complex/aluminium complex, and manganese complex/zinc complex. The secondary cell has relatively high capacitance and can be manufactured at low cost. Moreover, it provides more stable chemical reactions and can therefore be stably charged/discharged with large current and without risk of explosion.

Description

SECONDARY CELL
Background of the Preseh Invention
1. Field of the invention
The present invention relates to a rechargeabjle secondary cell and, more particularly, to a secondary ell which has relatively high capacitance and stable charge/discharge current',) which can b6 charged/discharged with reduced risk of explosion, and which can be manufactured at low cost. The positive electrode complex and the negative electrode complex' are in a combination selected from the group consisting of lead/chromium complex, chromium complex /aluminum complex, and manganese complex/zinc complex.
2. Description of the Related Art
As compared with a primary cell, a secondary cell is rechargeable and thus is environn entally friendly. A sepondary cell can be recharged, for example, more than 500 times. Therefore, when the total service life is considered, a secondary cell would benefit the user.
Conventional secondary cells (or batteries), sμch as a nickel-cadmium cell, nickel-hydrogen; hydride cell, Kthium ion cell, etc, are weU-knowri. The nickel-cadmium cell has been widely used in portable radios, remote controls, flash lights and the Jike. The nickel-hydrogen hydride cell cto be used for replacing the nickel-cadmium cell and has a capacitance higher than that of the latter. Accordingly, the nickel-hydrogen cell has been widely used in cameras, mobile phones, portable computers and the like. The lithiunl ion cell has a capacitance higher than that of the nickelτhydrogen cetf. Therefore, for pxample, an increasing number of mobile phones and portable computers, use a lithium ion cell as the power supply. A Uthium ion cell of standard size" used for a mobile phone has a capacitance in the range of from 500 mAh to 700 mAh. Summary of the Invention
The object of the present invention is, therefore, to provide a secondary cell which may generate a direct current when the positive electrode compound and the negative electrode compound thereof conduct a reversible redox reaction in the presence of an electrolyte, wherein the positive electrode complex and the negative electrode pomplex are in a combination (represented by positive electrode complex/the negative electrode complex) selected from the group consisting of lead/chromium complex, chromium complex/aluminum complex, and manganese complex/zinc complex. The secondary cell according to the present invention has relatively high capacitance, and more stable chemical reactioηs So that it can be stably charged/discharged without risk of explosion, with large current, and yet can be manufactured at low cost.
Other objects, features and advantages of the present invention will become apparent to those skilled in the art from the following detailed description. It should b understood, however, that the detailed description and specific examples, while indicating preferred embodiments pf the present invention, are given by way Of illustration and not limitation. Many changes and modifications within the scope of the present invention may be made without departing from the spirit thereof.
Brief Description of Drawings
Fig. 1 is a schematic drawing of the lead-chromium secondary poll according to one preferred embodiment of the present invention;
Fig. 2 is a schematic drawing qf the aluminum-chromium sepondary cell according to another preferred embodiment of the present invention; and
Fig. 3 is a schematic drawing of the manganese-zinc secondary cell according to still another preferred embodiment of the present invention. Detailed Description of Preferred Embodiments
According to one embodiment of the present invention, a lead-chrόmium secondary cell is provided. Referring to Fig, 1, the lead-chromium secondary cell comprises lέad -as the positive electrode 1, a cliromium complex as the negative electrode 2, a lead foil or lead alloy fpil as the positive plate 3, a copper fojl as the negative plate 4, a diluted sulfbric, acid as the electrolyte 5, and a spacer (not shown) disposed between thp positive and negative electrodes. By may of example, the positive electrode consists essentially of PbOz(0.1 to 0.5 mole) and, a chelating agent (0.05-0.3 mole) and' the negative electrode is chrorn im complex (0.05 to 0.3 mole). The electrolyte consists essentially of H2SO4 having a eonpentration of 10-50% and may inelude HC1. The reaction scheme of the charge/discharge thereof is as follows;
(Charge) 3PbSO + 6H2O+2Cr3+→ 3PbO2 + 12H+ + 3SO4 2" + 2Cr
(Positive electrode) PbS O4 + 2H2 O → Pb02 + 4H+ + S O 2 "+2e"
(Negative electrode) Cr3 ++3 e"-» Cr
During the charge, water is being cpnsumed and, the acid increases in concentration until tile reaction is complete. Since the chromium forms a chromium complex during the charge, it does not react and combine with the sulfate radical and thus the capacitanpe of the secondary cell can be significantly increased.
(Discharge) 3PbO2 + 12H+ + 3SO4 21 + 2Cr→ 3PbSO4 + 6H2O+2Cr +3
(Positive electrode) PbO2 + 4 H+ + S O " → PbS O4 + 2H2O
(Negative electrode) Cr"-^ Cr+3+3 e'
During the discharge of the lead-chromium -cell, the acid decreases in concentration until any one of the sulfate radical and chromium is exhausted or the chromium complex has a saturated concentration.
According to another embodiment of the present invention, an aluminum-chromium secondary cell is provided. Referring to Fig. 2, the aluminum-chrpmium secondary cell comprises a chroririum complex as the positive electrode 6, an aluminum complex as the negative electrode 7, an aluminum foil as the positive plate 8, a cpppef foil as the negative ptøte S, a diluted potassium hydroxide as the electrolyte 10, an a spacer (not shown) disposed between the positive and negative jelectrodes. By may of example, the positive electrode of' this embodiment consists of Cr2 + (0.1-0.4 mole) and the negative electrode consists essentially of aluminum complex (0.1-0.4 mole); The KOH electrolyte has a preferred concentration of 5-40% . Those skilled in the art wh appreciate that a chelating agent in an amount suph as 0.05-0,3 mole may be included. The reaction scheme of the charge/discharge thereof is as follows:
(Charge) 2Cr2 + + 7H2O +A13 + complex-* Cr2 O7 2 ' + 14 H+ + 2A1
(Positive electrode) 2Cr2+ + 7H2O → Cr207 2- + 14H+ + 6e"
(NegatiVe electrode) Al3 + cpmpiex + 3 e"→ Al
During the charge of the aluminum-chromium cell, hydroxide ion is formed, sp that the electrolyte increases in hydroxide ipn concentration until it reaches the original concentration.
(Discharge) Cr2 O7 2'+ 14H++2Al-→ 2Cr2++7H2 O+Al3 + compιex
(Positive electrode) Cr2O7 2" + 14H+ + 6e'^ Cr2+ + 7H2O (Negative eleptrode) Al→ Al3+ com lex + 3 e"
During the discharge of the aluminum-chromium cell, the electrolyte decreases in hydroxide ion concentration until any one of the lead and ch omate is completely reacted. When charged, overcharge should be avoided because it will result in the depletion of the water in the eleptrolyte and catuse a short circuit
According to still another embodiment pf the present invention, a manganes,e-zhic sepondary cell is provided. Referring to Fig. 3, the manganese-zinc secondary cell comprises a manganese complex as the positive electrode 11, a zinc complex as the negative electrode 12, a lead foil as the positive plate 13, a copper foil as the negative plate 14, a diluted potassium hydroxide as the electrolyte 15, and a spacer (not shown) disposed -between the positive and negative Electrodes. The positive electrode preferably consists essentially of Mnθ2 (0*05-0.2 mole) and negative eleqtfode preferably consists essentially of Zinc complex (Oil -0.4 mole). A chelating agent in an amount suph as 0,05 to 0.3 mole is preferably included. The KOH electrolyte m y have a concentration of 5 to 30%. The reaption scheme of the charge/discharge thereof is as follows:
(Charge) 2Mn 2+ +5Zn 2+ compϊex + 8H2O→ 2Mn O4 " + 16H+ + 5Zn
(Positive electrode) Mn 2+ + 4H2O → Mn O4 " + 8H++ 5 e"
(Negative electrode) Zn com lex + 2e"→ Zn
During the pharge, the hydrogen ion and hydroxide ion ionized from the water will pombine wjth zinc to form a hydrated zinc ion. The hydroxide ion concentration in the electrolyte should be controlled in order to avoid the occurrence of overcharge. (Discharge) 2Mn O " + 16H+ + 5Zn→ 2Mn 2+ +Zn2+ complex + 8H2O
(Positive electrode) Mn O4 " + 8H++ 5e → Mn1+ + 4H2O
(Negative electrode) Zn→ Zn2 + complex + 2e"
During the discharge of the
Figure imgf000007_0001
cell, the zinc will result in the occurrence of a- hydrated ion or combine with hydrogen to form a zinp-hydrogen complex.
the jnvention is illustrated by the following examples.
Examples
Example; 1
A lead-phromium secondary cell comprising lead as the positive electrode, a chromium complex as the negative eleotrode, a lead foil as the positive plate, a copffer foil as the negative plate, spacer disposed between the positive and negative electrodes, and a diluted sulfurie acid as the electrolyte was prepared. The secon r cpll Was, made into a standard battery for an ordinary mobile phone- The resulting standard battery as fully charged. Thereafter, the capacitance and the discharge voltage thereof at room temperature were measured and had 800 mAh and 2.4 volts, respeptively.
Example 2
An aluminum-rebj'omium seeondary cell comprising a chromium complex as the positive electrpde, an aluminum complex as the negative electrode, an aluminum foil as the positive plate, a copper foil as the negative plate, a spacer, disposed between the positive and negative electrodes, and a diluted potassium hydroxide as the electrolyte was prepared. The secondary pell was made into a standard battery for an ordinary mobile phone, The resulting standard battery was fully charged. Thereafter, the capacitance and the discharge voltage thereof at room tempera,ture were measured and had 20 0 mAh and 3.0 volts, respeόtively.
Example 3
A manganese-zinc sepondary celi comprising a manganese complex as the positive electrqd^, a zinc complex as the negative electrode, a lead foil as the positive plate, arid a copper foil as the negative plate, a spacer disposed between the positive and negative electrodes, and a diluted potassium hydroxide as the electrolyte was prepared. The secondary cell was made into a standard battery for an ordinary mobile phone. The resulting standard battery was fully charged, thereafter, the capacitance and the discharge voltage thereof at room temperature were measured and had 2000 mAh and 2.4 volts, respectively It can be seen from the results of the above examples and descriptions that a secondary cell, according to the present invention has relatively high capacitance and can be ώanufactured at low cost. Moreover, it is used safely and can be stably charged/discharged with large current.

Claims

What is planned is:
1. A secondary cell, comprising a positive electrode complex, a negatiVe electrode complex and an electrolyte, wherein said positive electrode Complex and negative electrode complex are in a combination selected from the group consisting of lead/chromium complex, chromium cpmplex/aluminum complex, and manganese complex /zinc complex.
2. The secondary pell according to claim 1, wherein the positive electrode complex /negative electrode complex are lead/ chromium complex.
3. The secondary cell according to claim 1 further comprising a lead foil as the positive plate, and a Copper foil as the negative plate.
4. The secondary cell according to claim 2 or 3, wherein the electrolyte is a sulfuric acid.
5. The secondary cell according to claim 1, wherein the positive electrode complex/negative electrode complex are chromium complex/ aluminum complex.
6. TJie secondary cell according to claim 1 further eomprising an alurninum fpil as the positive plate and a eopper foil as tib negative plate.
7. The secondary cell accprding o plaim 5 or 6, wherein the electrolyte is a potassium hydroxide.
8. The secondary cell according to, claim 1, wheSrein the positive eleetrode complex/negative electrode complex are manganese complex /zinc complex.
9. The secondary cell according to claim 1 further comprising a lead foil as the positive plate and a copper foil as the negative plate.
10. the secondary cell according to claim 8 or 9, wherein the electrolyte is a potassium hydroxide.
PCT/US2002/015157 2002-06-14 2002-07-19 Secondary cell WO2003107461A1 (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
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Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
US10/170,716 2002-06-14
US10/170,716 US20030228514A1 (en) 2002-06-07 2002-06-14 Secondary cell

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Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3993508A (en) * 1975-06-20 1976-11-23 Polaroid Corporation Method for manufacturing flat batteries
US5677084A (en) * 1992-12-25 1997-10-14 Toray Industries, Inc. Electrode and secondary battery using the same
US5932372A (en) * 1997-01-02 1999-08-03 Lightyear Technologies Inc. Composite materials, processes for manufacturing the composites, composite electrode, hydrogen occluding composite, and electrochemical cell utilizing the composite
US6242135B1 (en) * 1996-09-13 2001-06-05 Japan Gore-Tex, Inc. Solid electrolyte composite for electrochemical reaction apparatus

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US3993508A (en) * 1975-06-20 1976-11-23 Polaroid Corporation Method for manufacturing flat batteries
US5677084A (en) * 1992-12-25 1997-10-14 Toray Industries, Inc. Electrode and secondary battery using the same
US6242135B1 (en) * 1996-09-13 2001-06-05 Japan Gore-Tex, Inc. Solid electrolyte composite for electrochemical reaction apparatus
US5932372A (en) * 1997-01-02 1999-08-03 Lightyear Technologies Inc. Composite materials, processes for manufacturing the composites, composite electrode, hydrogen occluding composite, and electrochemical cell utilizing the composite

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