Source: http://www.google.com/patents/US7682747?dq=7,453,150
Timestamp: 2015-07-31 13:45:13
Document Index: 365768494

Matched Legal Cases: ['Application No. 2006', 'Application No. 2002', 'Application No. 2003', 'Application No. 2002', 'Application No. 2003', 'Application No. 2002', 'Application No. 10', 'Application No. 2000', 'application No. 2002']

Patent US7682747 - Positive electrode active material and non-aqueous electrolyte secondary ... - Google PatentsSearch Images Maps Play YouTube News Gmail Drive More »Sign inAdvanced Patent SearchPatentsThe present invention provides a high-capacity and low-cost non-aqueous electrolyte secondary battery, comprising: a negative electrode containing, as a negative electrode active material, a substance capable of absorbing/desorbing lithium ions and/or metal lithium; a separator; a positive electrode;...http://www.google.com/patents/US7682747?utm_source=gb-gplus-sharePatent US7682747 - Positive electrode active material and non-aqueous electrolyte secondary battery containing the sameAdvanced Patent SearchPublication numberUS7682747 B2Publication typeGrantApplication numberUS 11/976,491Publication dateMar 23, 2010Filing dateOct 25, 2007Priority dateMar 22, 2001Fee statusPaidAlso published asCN1287474C, CN1430795A, EP1296391A1, EP1296391A4, US7592100, US7718318, US20030170540, US20080096111, US20080193844, WO2002078105A1Publication number11976491, 976491, US 7682747 B2, US 7682747B2, US-B2-7682747, US7682747 B2, US7682747B2InventorsTsutomu Ohzuku, Hiroshi Yoshizawa, Masatoshi NagayamaOriginal AssigneePanasonic CorporationExport CitationBiBTeX, EndNote, RefManPatent Citations (96), Non-Patent Citations (57), Classifications (39), Legal Events (2) External Links: USPTO, USPTO Assignment, EspacenetPositive electrode active material and non-aqueous electrolyte secondary battery containing the same
US 7682747 B2Abstract
The present invention provides a high-capacity and low-cost non-aqueous electrolyte secondary battery, comprising: a negative electrode containing, as a negative electrode active material, a substance capable of absorbing/desorbing lithium ions and/or metal lithium; a separator; a positive electrode; and an electrolyte, wherein the positive electrode active material contained in the positive electrode is composed of crystalline particles of an oxide containing two kinds of transition metal elements, the crystalline particles having a layered crystal structure, and oxygen atoms constituting the oxide forming a cubic closest packing structure.
1. A method for producing a positive electrode active material for a non-aqueous electrolyte battery comprising the steps of:
introducing an aqueous alkaline solution comprising sodium hydroxide and ammonia and an aqueous solution containing a nickel sulfate, a manganese sulfate and a cobalt sulfate simultaneously into a reactor;
coprecipitating said nickel, said manganese and said cobalt while passing an inert gas therethrough to obtain a nickel manganese cobalt hydroxide and/or a nickel manganese cobalt oxide;
mixing said nickel manganese cobalt hydroxide and/or said nickel manganese cobalt oxide with a lithium compound to obtain a mixture; and
heating said mixture at a temperature not lower than 900� C. to obtain a positive electrode material.
2. The method for producing a positive electrode active material for a non-aqueous electrolyte battery in accordance with claim 1,
wherein the temperature of said reactor is 30 to 50� C.
3. The method for producing a positive electrode active material for a non-aqueous electrolyte battery in accordance with, claim 1,
wherein said lithium compound is lithium carbonate and/or lithium hydroxide.
4. The method for producing a positive electrode active material for a non-aqueous electrolyte battery in accordance with claim 1,
further comprising heating said mixture at a temperature of 700 to 800� C. after said step of heating at a temperature not lower than 900� C.
5. The method for producing a positive electrode active material for a non-aqueous electrolyte battery in accordance with claim 1,
wherein said coprecipitating step comprises: a step of flowing the mixed solution upward from a bottom of the reactor and colliding microcrystals precipitating by coprecipitation.
This application is a Divisional of U.S. application Ser. No. 10/333,269, filed Jan. 17, 2003, which is a 371 under International Application No. PCT/JP01/09756, filed Nov. 7, 2001, which claims priority of Japanese Application No. JP 2001-083610, filed Mar. 22, 2001, the entire contents of which are hereby incorporated by reference.
Furthermore, U.S. Pat. No. 5,629,110 proposes a dry mixing synthesis method which uses β-Ni(OH)2 to obtain an active material represented by the formula LiNi1-xMnxO2 wherein 0<x≦0.2, y≦0.2.
Further, Japanese Laid-Open Patent Publication No. Hei 10-69910 proposes an active material synthesized by a coprecipitation synthesis method, represented by the formula Liy-xNi1-x2MxO2 wherein M is Co, Al, Mg, Fe, Mg or Mn, 0<x2≦0.5, 0≦x1<0.2, x=x1+x2, and 0.9≦y≦1.3. This patent publication describes that the discharge capacity is inherently small if M is Mn, and the essential function of the positive electrode active material for a lithium secondary battery intended to achieve a high capacity is dismissed if X2 is more than 0.5. LiNi0.6Mn0.4O2 is exemplified as a material having the highest proportion of Mn.
The dry mixing synthesis method as described above is described in U.S. Pat. Nos. 5,393,622, 5,370,948 and 5264201 and each of these publications describes that the dry synthesis method is adequate since the content of Mn is small.
Composition Ni(%)
The second difference is that in (a) and (b), the peak half-width observed in the range of 15 to 20�is small compared with that in the others. In addition, in the analysis of (a) to (j) in FIG. 6, it is found that the height H1 of the peak observed in the range of 15 to 20�is extremely high compared with the height H2 of the peak observed in the range of 30 to 40�, satisfying the relation:
H 1≧2�H 2 The difference described above indicates that in (a) and (b) the crystallinity has already developed to some extent in the precursor. This is easily recognized by comparing (a) and (b) with (i) and (j). In (i) and (j), although there is no evident Mn2O3 peak, the peak intensity ratio and the half-width are clearly different from those in (a) and (b).
As an example, three kinds of lithium-containing oxides expressed by formula (2) in which x was 0.1, 0.2 and 0.3, respectively were synthesized. In the synthesis, the amount of lithium hydroxide was adjusted to attain each of the above ratios when a nickel-manganese composite hydroxide as the precursor prepared by the coprecipitation method and lithium hydroxide were mixed sufficiently in the dry state. The resultant oxide was subjected to primary sintering at 500� C. for 8 hours, pulverization with Masscolloider, secondary sintering at 950� C. for 10 hours, and tertiary sintering at 700% for 5 hours, to have the specific crystal structure described above. It is possible to confirm that the crystal structure of crystalline particles of the oxide is a layered structure and that oxygen atoms constituting the oxide form a cubic closest packing structure, by analyzing the pattern of the powder X-ray diffraction image with the Rietveld method.
The same results were obtained for the active material expressed by Li[Li0.1(Ni1/2Mn1/2)0.9]O2 and the active material expressed by Li[Li0.3(Ni1/2Mn1/2)0.7]O2. Therefore, from the results for Li[Lix(Ni1/2Mn1/2)1-x]O2 (X=0.1˜0.3) containing lithium excessively as described above, there is found a merit that the thermal stability of the active material at an overcharge can be improved by the mechanism described above. No prior art discloses or suggests this idea, and thus the present invention presents a guideline for entirely novel material design.
As the inorganic solid electrolyte, nitrides of Li, halides of Li, and oxysalt of Li are well known. Among them, Li4SiO4, Li4SiO4—LiI—LiOH, xLi3PO4-(1-x)Li4SiO4, Li2SiS3, Li3PO4—Li2S—SiS2 and phosphorus sulfide compounds are effectively used.
The pressing temperature is preferably between room temperature and 200%. The ratio of the width of the positive electrode sheet to the width of the negative electrode sheet is preferably at 0.9 to 1.1, and more preferably at 0.95 to 1.0. The ratio of the content of the positive electrode active material to the content of the negative electrode material cannot be specified because it differs according to the kind of the compound used and the formulation of the mixture, but those skilled in the art can set an optimum value considering the capacity, cycle characteristics and safety.
A battery case 11 houses an electrode plate group 14 composed of a positive electrode plate and a negative electrode plate wound in a helical shape with a separator therebetween forming a plurality of windings. A positive electrode lead 15 is drawn out from the positive electrode plate and connected to a sealing plate 12, while a negative electrode lead 16 is drawn out from the negative electrode plate and connected to the bottom of the battery case 11. The battery case and the lead plates may be made of a metal or an alloy that is resistant to an organic electrolyte and has electron conductivity. Examples of such a metal and alloy include metals such as iron, nickel, titanium, chromium, molybdenum, copper and aluminum and alloys of these metals.
In particular, one machined from a stainless steel plate or an Al—Mn alloy plate is most suitable for the battery case, aluminum for the positive electrode lead, and nickel for the negative electrode lead. Also, for the battery case, various engineering plastics and these in combination with metals may be used for reduction in weight.
Insulating rings 17 are placed on the top and bottom of the electrode plate group 14. After an electrolyte is injected, the battery case is sealed with the sealing plate. A safety valve may be placed at the sealing plate. In addition to the safety valve, various conventionally known safety elements may be placed. For example, as the overcurrent prevention element, a fuse, bimetal, a-PTC element or the like may be used. As measures against rise of the internal pressure of the battery case other than placement of the safety valve, the following methods may be employed: forming a slit through the battery case, cracking a gasket, cracking the sealing plate, and disconnecting the lead plate. A protection circuit incorporating a measure against overcharge and overdischarge may be connected to a charger.
x in Li[Lix(Ni1/2Mn1/2)1−x]O2 (mAh)
(� C.) of DSC
x in Li[Lix(Ni1/2Mn1/2)1−x]O2 measurement
The coin-shaped batteries were produced in the following manner. The positive electrode active materials “a” to “J” obtained at various sintering temperatures, acetylene black as the conductive material, and a polyvinylidene fluoride resin (PVDF) as the binder were mixed at a weight ratio of 80:10:10, to obtain a sheet-shaped molded article. The molded article was stamped into a disk shape and dried under vacuum at 80′ for about 15 hours, to obtain a positive electrode. Also, a sheet-shaped lithium metal was stamped into a disk shape, to obtain a negative electrode. A polyethylene microporous film was used as a separator. One mol of LiPF6 was dissolved in a mixed solvent of ethylene carbonate (EC) and ethyl methyl carbonate (EMC) in 1:3 (volume ratio) to prepare an electrolyte.
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No. 10/629,815 dated on Jul. 10, 2008.55West et al., "Introduction for Solid-State Chemistry," Kodansha-Scientific, Mar. 20, 1996, with partial translation.56Yoshio et al., "Lithium-ion Secondary Battery," Nikkan Kogyo Shinbunsha, Mar. 29, 1996, with partial translation.57Yoshio, M. et al., "Preparation and properties of LiCoyMnxNi1-x-yO2 as a chathode for lithium ion batteries," Journal of Power Sources, Aug. 17, 1998, p. 176-181, vol. 90, Elsevier.Classifications U.S. Classification429/231.1, 423/594.6, 429/231.3, 429/223, 423/594.3, 423/594.4, 429/231.95, 423/599, 252/182.1, 429/224, 429/218.1, 423/594.5, 429/209, 423/593.1International ClassificationH01M10/05, H01M4/505, H01M4/525, H01M2/34, H01M10/42, H01M4/58, H01M4/36Cooperative ClassificationH01M4/485, H01M4/13, H01M2004/021, H01M4/525, H01M4/505, H01M10/052, H01M10/42, H01M2/34, H01M2004/028, Y02E60/122, H01M2010/4292, H01M4/362, H01M10/0525, H01M4/0471European ClassificationH01M4/13, H01M4/36K, H01M4/505, H01M4/525Legal EventsDateCodeEventDescriptionOct 18, 2011CCCertificate of correctionAug 28, 2013FPAYFee paymentYear of fee payment: 4RotateOriginal ImageGoogle Home - Sitemap - USPTO Bulk Downloads - Privacy Policy - Terms of Service - About Google Patents - Send FeedbackData provided by IFI CLAIMS Patent Services