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`Japanese Patent Application Laid-Open No. 05-
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`062712
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`(19) [Country of issue] Japan Patent Office (JP)
`
`(12) [Type of publication] Published patent publication (A)
`
`(11) [Publication number] JP-A-5-62712
`
`(43) [Published date] 1993 ( 1993) March 12
`
`(54) [Title of invention] Non-aqueous electrolyte secondary battery
`
`(51) [International Patent Classification 5th edition]
`
`H01M 10/40 Z 8939-4K
`
`[Request for examination] Unclaimed
`
`[Claim Number] 1
`
`[Total number of pages] 4
`
`(21) [Application number] Japanese Patent Application Hei 3-220200
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`https://www.j-platpat.inpit.go.jp/p0200
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`APPLE-1021
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`Patent/utility model document display(cid:955)J-PlatPat [JPP]
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`(22) [Filing date] August 30, 1991
`
`(71) [Applicant]
`
`[Identification number] 000001889
`
`[Name] SANYO Electric Co., Ltd.
`
`(72) [Inventor]
`
`[Name] Satoshi Ikukawa
`
`(72) [Inventor] [
`
`Name] Toru Amazutsumi
`
`(72) [Inventor]
`
`[Name] Keisaku Nakanishi
`
`( 74) [Agent]
`
`[Patent Attorney]
`
`[Name] Yasuhiro Toyosu
`
`wrap up
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`(57) [Summary]
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`close
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`[Objective] To minimize the decrease in cycle life under normal use conditions
`
`and to minimize the decrease in discharge capacity due to overdischarge.
`
`A non-aqueous electrolyte secondary battery includes a positive electrode mai
`
`nly composed of a rechargeable active material and a negative electrode cont
`
`aining lithium as an active material. In particular, in the secondary battery of
`
`the present invention, the theoretical capacity ratio between the positive elect
`
`rode and the negative electrode is set within the range of 1:1 to 1.3.
`
`[Effect] By setting the theoretical capacity ratio between the positive electrod
`
`e and the negative electrode within an extremely limited range, during overdi
`
`scharge, the positive electrode is consumed and a large amount of the negati
`
`ve electrode active material remains, and the discharge reaction proceeds, ca
`
`using the electrolyte to decompose and conduct electricity. It is possible to eff
`
`ectively prevent deterioration of battery performance due to side reactions su
`
`ch as reactions between the agent and the negative electrode active material.
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`The scope of the claims
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`open
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`[Scope of Claims]
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`[Claim 1] A non-aqueous electrolyte secondary battery comprising a positive
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`electrode mainly composed of a rechargeable active material and a negative
`
`electrode containing lithium as the active material, wherein the theoretical ca
`
`pacities of the positive electrode and the negative electrode
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`are A non-aqueous electrolyte secondary battery, characterized in that the rat
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`io is designed to be in the range of 1:1 to 1.3.
`
`detailed description
`
`open
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`Description: BACKGROUND OF THE INVENTION
`
`1.
`
`Field of the Invention The present invention relates to a positive electrode ma
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`inly composed of a rechargeable active material such as manganese oxide, an
`
`d a negative electrode composed of metallic lithium, lithium-aluminum alloy o
`
`r the like. It relates to a non-aqueous electrolyte secondary battery.
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`2.
`
`Description of the Related Art In a non-aqueous electrolyte secondary battery
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`in which the positive electrode active material is manganese dioxide and the
`
`negative electrode is lithium, the following reaction occurs between the positi
`
`ve electrode and the negative electrode during charging and discharging.
`+
`−
`
`Negative electrode during discharge: Li→Li
`
` +e
`+
`
`−
`
`Positive electrode during discharge: MnO 2 +xLi
`
` +e
`
` →Li x MnO 2
`
`Negative electrode and positive electrode during charge: Li x MnO 2 →xLi+Mn
`
`O 2
`
`Li is eluted as Li
`
` ions are deposited on the surface
`
`+ ions, and when charged, the Li +
`
`as metal Li. A non-aqueous electrolyte secondary battery that is charged and
`
`discharged by this reaction decreases the amount of lithium as it is charged a
`
`nd discharged. The reason for this is that lithium deposited on the surface of t
`
`he negative electrode during charging gradually reacts with the electrolyte to
`
`form a negatively active product. That is, the following reactions proceed duri
`
`ng charging and discharging.
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`+
`
`[0004]
`
` In the charging process, Li
`
` ions are converted into Li and deposit
`
`ed on the surface of the negative electrode.
`
` Part of the Li deposited on the
`
`surface of the negative electrode reacts with the solvent to form a chemically
`+ .
`
`inactive reaction product.
`
` During discharge, Li is eluted and becomes Li
`
`However, in this step, not all Li deposited on the surface of the negative electr
`
`ode is eluted. This is because an inert reaction product produced by the reacti
`+ and does not elute.
`
`on of Li with the solvent becomes Li
`
`[0005] Therefore, all of the Li deposited on the negative electrode in the st
`+ ions in the step (3).
`
`ep (2) cannot be eluted as Li
`
`Therefore, as charging and d
`
`ischarging progress, the amount of lithium that can be eluted from the negati
`
`ve electrode decreases, shortening the cycle life. In order to overcome this dr
`
`awback, conventional non-aqueous electrolyte secondary batteries have a ne
`
`gative electrode capacity that is at least twice the positive electrode capacity.
`
`[0006]
`
`However, a non-aqueous electrolyte secondary battery in which the negative
`
`electrode capacity is at least twice the positive electrode capacity is discharge
`
`d to 0 V, that is, when it is overdischarged, it cannot be recharged. The perfor
`
`mance of the battery deteriorated such that it became impossible to discharg
`
`e even when the battery was charged, and the capacity decreased significantl
`
`y. It means that the negative electrode capacity is the positive electrodeIn a
`
`non-aqueous electrolyte secondary battery with a capacity of more than twice
`
`the capacity, when overdischarged to 0 V, the negative electrode active mater
`
`ial and the negative electrode active material react, that is, even after the po
`
`sitive electrode capacity is exhausted. This is because the remaining substanc
`
`e promotes the discharge reaction, causing side reactions such as the decom
`
`position of the electrolyte and the reaction between the conductive agent and
`
`the negative electrode active material, thereby deteriorating the battery perfo
`
`rmance.
`
`[0007] The present invention was developed with the object of further solving
`
`this drawback. An object of the present invention is to provide a non-aqueous
`
`electrolyte secondary battery capable of extremely reducing the decrease in d
`
`ischarge capacity due to discharge.
`
`[0008]
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`The non-aqueous electrolyte secondary battery of the present invention has t
`
`he following constitutions in order to achieve the above objects. That is, the n
`
`on-aqueous electrolyte secondary battery of the present invention includes a
`
`positive electrode mainly composed of a rechargeable active material and a n
`
`egative electrode containing lithium as the active material, and the theoretica
`
`l capacity ratio between the positive electrode and the negative electrode is It
`
`is characterized by being set in the range of 1:1 to 1.3.
`
`[0009] For the active material of the positive electrode, for example, a compo
`
`site compound of MnO 2 , TiS 2 , chromium oxide, vanadium compound and th
`
`e like can be used. Li-Al alloy and Li-Wood's metal alloy can be used for the n
`
`egative electrode.
`
`In the non-aqueous electrolyte secondary battery of the present invention, th
`
`e active material of the positive electrode is preferably a composite compoun
`
`d of MnO 2 such as Li(OH)--MnO 2 sintered body, and the negative electrode i
`
`s a Li--Al alloy or the like. Li-Wood metal alloy.
`
`[0011]
`
`The non-aqueous electrolyte secondary battery of the present invention is des
`
`igned so that the theoretical capacity ratio between the positive electrode and
`
`the negative electrode is in the range of 1:1 to 1.3. In this secondary battery,
`
`unlike conventional non-aqueous electrolyte secondary batteries, the capacity
`
`of the negative electrode is not significantly larger than that of the positive el
`
`ectrode, and the capacity is set within a specific range. This secondary batter
`
`y is designed such that when over-discharged, the positive and negative elect
`
`rodes are approximately the same, or the positive electrode is more or less c
`
`onsumed first. Therefore, as in the conventional non-aqueous electrolyte seco
`
`ndary battery, after the positive electrode is consumed, a large amount of the
`
`negative electrode active material remains and the discharge reaction procee
`
`ds, causing decomposition of the electrolyte, reaction between the conductive
`
`agent and the negative electrode active material, and the like. It is possible t
`
`o prevent a side reaction from occurring and deteriorating the battery perfor
`
`mance. After the positive electrode is consumed, side reactions do not occur
`
`at all, but they can be suppressed to a low level, and there is almost no deter
`
`ioration in battery performance. Also, the decrease in cycle life due to the dec
`
`rease in negative electrode capacity can be suppressed.
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`DETAILED
`
`DESCRIPTION OF THE PREFERRED EMBODIMENTS Embodiments of the prese
`
`nt invention will now be described with reference to the drawings. However, t
`
`he examples shown below are illustrative of non-aqueous electrolyte seconda
`
`ry batteries for embodying the technical idea of the present invention, and th
`
`e non-aqueous electrolyte secondary batteries of the present invention are co
`
`mposed of The material, shape, structure, arrangement, etc. are not specified
`
`as follows. The non-aqueous electrolyte secondary battery of the present inve
`
`ntion isVarious changes can be made within the range of .
`
`[0013] Further, in this specification, to facilitate understanding of the claims,
`
`the numbers corresponding to the members shown in the examples are referr
`
`ed to as "claims" and "means for solving the problems". column” is added to t
`
`he member shown. However, the members shown in the claims are by no me
`
`ans specified as the members of the embodiments.
`
`FIG. 1 shows a half sectional view of a flat type non-aqueous electrolyte seco
`
`ndary battery according to an embodiment of the present invention. In this fi
`
`gure, reference numeral 1 denotes a positive electrode can, and a positive ele
`
`ctrode 2 is press-contacted to the inner bottom surface thereof with a positiv
`
`e electrode current collector 3 interposed therebetween.
`
`For the positive electrode, an active material obtained by heat-treating lithiu
`
`m hydroxide and manganese dioxide at 400.degree. A predetermined amount
`
`of the positive electrode mixture mixed at a weight ratio is sampled and mold
`
`ed.
`
`A negative electrode 4 made of a lithium-aluminum alloy plate is crimped to t
`
`he inner bottom surface of a negative electrode can 6 with a negative electro
`
`de current collector 5 interposed therebetween.
`
`7 is a separator made of polypropylene. This separator is impregnated with a
`
`non-aqueous electrolytic solution prepared by dissolving 1 mol of LiClO 4 in a m
`
`ixed solvent of propylene carbonate and dimethoxyethane. 8 is an insulating packing.
`
`The battery has an outer diameter of 24.0 mmφ and a thickness of 3.0 mm.
`
`The theoretical capacity of the positive electrode is 100 mAh, and the theoreti
`
`cal capacity of the negative electrode is 100 mAh and 130 mAh. was fabricate
`
`d as described above to fabricate a non-aqueous electrolyte secondary batter
`
`y of the present invention.
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`As a comparative example, a nonaqueous electrolyte secondary battery B1 ha
`
`ving a positive electrode capacity of 100 mAh and a negative electrode capaci
`
`ty of 50 mAh, that is, a theoretical capacity ratio of 1:0.5, has a positive elect
`
`rode of 100 mAh and a negative electrode capacity of 50 mAh. A non-aqueou
`
`s electrolyte secondary battery B2 with a capacity ratio of 1:2, which is twice
`
`as large as 200 mAh, was also prototyped.
`
`FIG. 2 shows a characteristic diagram of the overdischarge cycle of these non
`
`-aqueous electrolyte secondary batteries. As for the charging condition, the b
`
`attery was charged for 100 hours by connecting a protection resistance of 10
`
`0Ω in series to a constant-voltage power supply with an output voltage of 3.5
`
`V. Discharge was performed by connecting a load of 1 kΩ and discharging unt
`
`il the battery voltage became 0V. However, FIG. 2 plots the capacity up to a v
`
`oltage of 2 volts, which is commonly used in practical equipment. From this fi
`
`gure, it is clear that the overdischarge cycle characteristics of the batteries A
`
`1 and A2 of the present invention are significantly improved. As shown in this
`
`figure, the conventional comparative battery B2, in which the capacity of the
`
`negative electrode is twice that of the positive electrode, has the drawback of
`
`significant deterioration due to overdischarge.be.
`
`Further, FIG. 3 shows charge-discharge cycle characteristics of a non-aqueous
`
`electrolyte secondary battery tested under conditions different from those in
`
`FIG. This characteristic was tested by charging and discharging at a constant
`
`current of 5 mA. Charging stopped when the battery voltage increased to 3.5
`
`V. Discharge stopped when the voltage dropped to 2.0V. As shown in this figu
`
`re, the non-aqueous electrolyte secondary batteries A1 and A2 of the present
`
`invention achieved a cycle life substantially equal to that of the comparative b
`
`attery B2 in which the negative electrode capacity was twice the positive elect
`
`rode capacity.
`
`As is clear from FIGS. 2 and 3, the non-aqueous electrolyte secondary batter
`
`y of the present invention, in which the theoretical capacity ratio between the
`
`positive electrode and the negative electrode is restricted to a specific range,
`
`has a long cycle life under normal use conditions. The cycle life of overdischar
`
`ge to 0V could be remarkably extended with almost no deterioration.
`
`[0023] In the embodiments, a flat battery is shown as an example, but the s
`
`ame effect can be obtained with a rectangular battery or a cylindrical battery.
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`INDUSTRIAL APPLICABILITY The non-aqueous electrolyte secondary battery o
`
`f the present invention comprises a positive electrode mainly composed of a r
`
`echargeable active material and a negative electrode containing lithium as th
`
`e active material
`
`. T
`
`he capacity ratio is specified in the range of 1:1 to 1:1.3. The non-aqueous
`
`electrolyte secondary battery having this configuration can extremely effectiv
`
`ely prevent the deterioration of battery performance due to overdischarge, an
`
`d can extremely reduce the deterioration of the cycle life under normal use co
`
`nditions, and has industrial value. extremely large. In this way, the reduction
`
`in cycle life due to overdischarge can be prevented by setting the theoretical
`
`capacity ratio between the negative electrode and the positive electrode withi
`
`n an extremely limited range, so that the positive electrode and the negative
`
`electrode are consumed in the same manner. This is because it is possible to
`
`prevent the deterioration of battery performance due to the occurrence of sid
`
`e reactions.
`
`Brief description of the drawing
`
`open
`
`BRIEF DESCRIPTION OF THE DRAWINGS FIG. 1 is a cross-sectional view of a
`
`non-aqueous electrolyte secondary battery
`
`showing one embodiment of the present invention; [Fig. 3] A
`
`graph
`
`showing the cycle life of the battery of the present invention and a convention
`
`al non-aqueous electrolyte secondary battery
`
`[Explanation of symbols]
`
`1... Positive electrode can 2... Positive electrode
`
`3... Positive electrode current collector 4... Negative electrode
`
`5... Negative electrode current collector 6 Negative electrode can
`
`7 Separator 8 Insulating packing
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`open
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`drawing
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`[Fig. 1]
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`[Figure 2]
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`[Figure 3]
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`drawing
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`open
`
`Representative drawing
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`1
`
`2
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`3
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`Magnify and Rotate
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`Representative drawing
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