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Graphite particles and lithium secondary battery using the same as negative electrode

a lithium secondary battery and graphite technology, applied in the direction of cell components, final product manufacturing, sustainable manufacturing/processing, etc., can solve the problems of deteriorating cycle characteristics, internal breakage of electrodes, and affecting the quality of lithium secondary batteries, etc., to achieve excellent rapid charge-discharge characteristics and cycle characteristics, excellent in cycle characteristics, and small irreversible capacity of the first cycle

Inactive Publication Date: 2001-10-25
HITACHI CHEM CO LTD
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Benefits of technology

[0007] This invention further provides graphite particles suitable for use as a negative electrode of lithium secondary battery small in the irreversible capacity of the first cycle and excellent in cycle characteristics.
[0087] The use of the above-mentioned graphite particles of this invention as the graphite particle of the third negative electrode for lithium secondary battery of this invention is preferable because, when the negative electrode of the lithium secondary battery prepared therefrom is made to have a high density, discharge capacity, rapid charge-discharge characteristics and cycle characteristics can be improved thereby.

Problems solved by technology

As its result, due to repeated occlusion of lithium into graphite crystal and its release, a strain arises in the direction of c-axis, which causes an internal breakage of electrode.
Thus, the cycle characteristics are deteriorated and, in addition, the rapid charge-discharge characteristics tend to become worse.
Further, prior art graphite particles having a large crystallite size in the face direction requires a long period of time for occlusion and release of lithium.
Thus, the lithium secondary battery obtained therefrom has a large irreversible capacity in the first cycle and, in addition, such graphite particles are poor in adhesiveness to current collector so that a large quantity of binder is needed.
If the adhesiveness to current collector is not good, the current-collecting effect is not good and discharge capacity, rapid charge-discharge characteristics and cycle characteristics are deteriorated.

Method used

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  • Graphite particles and lithium secondary battery using the same as negative electrode
  • Graphite particles and lithium secondary battery using the same as negative electrode
  • Graphite particles and lithium secondary battery using the same as negative electrode

Examples

Experimental program
Comparison scheme
Effect test

example 1

[0096] (1) Preparation of Graphite Particles

[0097] Seventy parts by weight of coke powder having a mean particle diameter of 10 .mu.m, 20 parts by weight of tar pitch, 10 parts by weight of iron oxide and 20 parts by weight of coal tar were mixed together and stirred at 100.degree. C. for one hour. The mixture was calcined at 2,800.degree. C. in an atmosphere of nitrogen and then pulverized to obtain graphite particles having a mean particle diameter of 20 .mu.m. According to a scanning electron microscopic photograph (SEM photograph) of the graphite particles thus obtained, the graphite particles had a structure in which a plurality of flat-shaped particles were bound together so that the planes of orientation were not parallel to one another. One hundred particles were selected at random from the graphite particles thus obtained, and a mean value of their aspect ratios was measured. As a result, the mean value was 1.8. In a X ray broad angle diffraction of the graphite particles t...

example 2

[0104] Seventy parts by weight of coke powder having a mean particle diameter of 10 .mu.m, 10 parts by weight of tar-pitch, 2 parts by weight of iron oxide and 20 parts by weight of coal tar were mixed together and stirred at 100.degree. C. for one hour. Subsequently, the mixture was calcined in an atmosphere of nitrogen at 2,800.degree. C. and then pulverized to obtain graphite particles having a mean particle diameter of 20 .mu.m. An examination of the graphite particles thus obtained under an electron microscope revealed that a plurality of flat-shaped particles were assembled or bound together so that the planes of orientation thereof were not parallel to one another to form a graphite particle. One hundred particles were at random selected from the graphite particles, and mean value of aspect ratios thereof was determined to obtain a result of 4.8. X ray broad angle diffraction of the graphite particle thus obtained revealed that the interlaminar distance d (002) of the crystal...

example 3

[0106] A coke powder having a mean particle diameter of 20 .mu.m was calcined in an atmosphere of nitrogen at 2,800.degree. C. to obtain graphite particles having a mean particle diameter of 20 .mu.m. The graphite particles thus obtained constituted a flaky graphite having a mean aspect ratio of 6, a specific surface area of 11 m.sup.2 / g, an interlaminar distance d (002) in crystal of 3.365 .ANG. and a crystallite size Lc (002) of 800 .ANG..

[0107] The flaky graphite thus obtained was made into a lithium secondary battery via the same processes as in Example 1, and the battery characteristics thereof were examined in the same manner as in Example 1. The results are shown in FIG. 3 and FIG. 4.

[0108] The lithium secondary batteries obtained in Examples 1, 2 and 3 of this invention were compared with one another on occlusion and release of lithium. The results were as mentioned below. FIG. 3 is a graph illustrating the relation between discharge capacity and charge-discharge cycle numbe...

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Abstract

A graphite particle obtained by assembling or binding together a plurality of flat-shaped particles so that the planes of orientation are not parallel to one another, or a graphite particle in which aspect ratio is 5 or less or specific surface area is 8 m2 / g or less or the size of crystallite in the direction of c-axis of the crystal is 500 Å or more and the size of crystallite in the direction of plane is 1,000 Å or less as measured by X ray broad angle diffraction, or a graphite particle in which pore volume of the pores having a size falling in a range of 102 to 106 Å is 0.4 to 2.0 cc / g per weight of graphite particle or pore volume of the pores having a size falling in a range of 1x102 to 2x104 Å is 0.08 to 0.4 cc / g per weight of graphite particle is suitable for production of negative electrode of lithium secondary battery, and a lithium secondary battery obtained therefrom is excellent in rapid charge-discharge characteristics, cycle characteristics, etc.

Description

[0001] This application is a Divisional app lication of application Serial No. 09 / 230,889, filed Febr. 2, 1999, which is an Application under 35 USC 371 of International application Serial No. PCT / JP97 / 02762, filed Aug. 7, 1997.[0002] This invention relates to a novel graphite particle, a process for producing the same, a graphite paste using the graphite particle, a negative electrode for lithium secondary battery using the graphite paste, a process for producing the negative electrode, and a lithium secondary battery. More particularly, this invention relates to a lithium secondary battery suitable for use in portable instruments, electric cars, electric power storage, etc. and excellent in the rapid charge-discharge characteristics, the cycle characteristics, etc., and to graphite particle for use as a negative electrode thereof, a process for producing the graphite particle, a graphite paste using the graphite particle, a negative electrode for lithium secondary battery using th...

Claims

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Application Information

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Patent Type & Authority Applications(United States)
IPC IPC(8): H01M4/36C01B31/04H01M4/02H01M4/133H01M4/1393H01M4/58H01M4/583H01M4/587H01M10/052H01M10/0525H01M10/058H01M10/36
CPCC01B31/04Y10T29/49115C01P2002/72C01P2004/54C01P2004/61C01P2006/12C01P2006/14H01M4/0404H01M4/133H01M4/1393H01M4/583H01M4/587H01M4/621H01M10/052H01M10/0525H01M10/058H01M2004/021H01M2004/027Y02E60/122Y02T10/7011H01M4/0433Y10T428/2982C01P2002/60C01B32/20C01B32/205Y02E60/10Y02P70/50H01M4/139Y02T10/70
Inventor ISHII, YOSHITONISHIDA, TATSUYAFUJITA, ATSUSHIYAMADA, KAZUO
Owner HITACHI CHEM CO LTD
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