Silicon oxide powder and making method

Chemistry: electrical current producing apparatus – product – and – Current producing cell – elements – subcombinations and... – Electrode or plural tablets – pellets or discs

Reexamination Certificate

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C423S335000, C423S336000, C423S337000

Reexamination Certificate

active

06759160

ABSTRACT:

This invention relates to a silicon oxide powder for use as a negative electrode active material in lithium ion secondary cells, and a method for preparing the same.
BACKGROUND OF THE INVENTION
Silicon oxide represented by SiO is a well-know material. By taking advantage of its chemical activity, it is used, for example, in the synthesis of industrially useful alkylhalosilanes (Gary N. Bokerman et al., U.S. Pat. No. 5,051,247) and the direct synthesis of siloxanes (Peter L. Timms and William N. Rowlands, EPA 0406000A2 “Polysiloxane oils and process for their preparation”). It is also reported that magnesium silicide is prepared by reacting silicon oxide with magnesium at low temperatures (E. Fuglein and U. Schubert, Chem. Mater., 1999, 11, 865-866).
Meanwhile, JP-A 9-7638 corresponding to EP 840386A discloses that the use of SiOx as a negative electrode active material in lithium ion secondary cells facilitates occlusion and release of lithium ions. Silicon oxide is thus expected to find an extra application as the negative electrode active material in lithium ion secondary batteries.
The use of silicon oxide (SiOx) powder as the negative electrode material in lithium ion secondary cells leads to a drastically increased initial capacity, but poor cycle performance.
SUMMARY OF THE INVENTION
An object of the invention is to provide a silicon oxide powder which is used as the negative electrode material to construct a lithium ion secondary cell capable of maintaining a high capacity without detracting from cycle performance. Another object is to provide a method for preparing the silicon oxide powder.
We have found that when a silicon oxide powder of the formula: SiOx wherein x has a value within a certain range and having a certain specific surface area is used as the negative electrode material in a lithium ion secondary cell, the cell has a high capacity and excellent cycle performance. The conditions under which a silicon oxide powder of a specific composition having physical properties in the desired range can be prepared have been empirically established.
The invention provides a silicon oxide powder represented by the formula: SiOx wherein x is a number from 1.05 to 1.5 and having a BET specific surface area of 5 to 300 m
2
/g.
According to another aspect of the invention, the silicon oxide powder is prepared by heating a raw material powder mixture containing at least a silicon dioxide powder in an inert gas atmosphere or in vacuum at a temperature of 1,100 to 1,600° C. to generate SiO gas, continuously or intermittently feeding oxygen gas to the SiO gas to form a gas mixture, and depositing the gas mixture on a surface of a cooled substrate.


REFERENCES:
patent: 5051247 (1991-09-01), Bokerman et al.
patent: 5834378 (1998-11-01), Kurtz et al.
patent: 2001/0012503 (2001-08-01), Fukuoka et al.
patent: 2003/0143834 (2003-07-01), Morisaki et al.
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patent: 0 840 386 (1998-05-01), None
patent: 9-7638 (1997-10-01), None
patent: 2001348656 (2001-12-01), None
Database WPI, Section Ch, Week 200207 Derwent Publications Ltd., London, GB; AN 2002-051162 XP002201123& JP 2001 226112 A (Shinetsu Chem Ind Co Ltd), Aug. 21, 2001 *abstract*.
Database WPI, Section Ch, Week 200163 Derwent Publications Ltd., London, GB; AN 2001-560341 XP002201124 & JP 2001 158613 A (Denki Kagaku Kogyo KK), Jun. 12, 2001 *abstract*.
Database WPI, Section Ch, Week 200158 Derwent Publications Ltd., London, GB; An 2001-524965 XP002201125 & JP 2001 118568 A (Denki Kagaku Kogyo KK), Apr. 27, 2001 *abstract*.
Patent Abstracts of Japan, vol. 2000, No. 24, May 11, 2001 & JP 2001 185125 A (Denki Kagaku Kogyo KK), Jul. 6, 2001 *abstract*.
Patent Abstracts of Japan, vol. 2000, No. 24, May 11, 2001 & JP 2001 199716 A (Denki Kagaku Kogyo KK), Jul. 24, 2001 *abstract*.
Database CA Online! Chemical Abstracts Service, Columbus, Ohio, US; Eckert, Hans J. et al.: “Studies on silicon oxides” retrieved from STN database accession No. 86:46630 CA XP002201140 *abstract* & Wiss. Z., Tech. Hochsch., Karl-Marx Stadt (1976), 18(1), 103-12, 1976.
Fuglein, Ekkehard et al., “Formation of Mg2Si from Solid Silicon Monoxide, and Solid-State Comproportionation between Mg2Si and SiO”, Chem. Mater, 1999, 11, pp. 865-866.

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