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MULTILAYER BODY AND METHOD FOR PRODUCING SAME UPDATE_EN meetings

Foreign code F190009825
Posted date Jun 27, 2019
Country WIPO
International application number 2019JP006898
International publication number WO 2019163967
Date of international filing Feb 22, 2019
Date of international publication Aug 29, 2019
Priority data
  • P2018-031293 (Feb 23, 2018) JP
Title MULTILAYER BODY AND METHOD FOR PRODUCING SAME UPDATE_EN meetings
Abstract Provided is a multilayer body which is used for a negative electrode of a lithium ion secondary battery that has high capacity, while having excellent safety, economic efficiency and cycle characteristics. This multilayer body comprises a conductive base material and a composite layer that is provided on the conductive base material. The composite layer comprises a plurality of silicon oxide particles and a conductive substance that is present in the spaces among the plurality of silicon oxide particles. The silicon oxide particles have an average particle diameter of 1.0 μm or less. This multilayer body additionally comprises a conductive layer that is provided on the composite layer and contains the conductive substance. The conductive layer has a thickness of 20 μm or less.
Outline of related art and contending technology BACKGROUND ART
Is a lithium ion secondary battery, a positive electrode including a positive electrode active material, and a negative electrode including a negative electrode active material, an electrolyte interposed between them are mainly composed of. The performance of the lithium ion secondary battery, the positive and negative electrodes largely depends on the characteristics of the electrode active material. Such as hard carbon or graphite carbon-based material of the lithium ion secondary battery are widely used as an anode active material. Carbon-based material is used as a negative electrode active material of the lithium ion secondary battery in the charging capacity is the theoretical 372mAh/g. An automobile or a portable telephone or the like is widely used as the lithium ion secondary battery, and the growing needs of the increased charge capacity.
The negative electrode active material a lithium ion secondary battery using silicon as the theoretical charge capacity in approximately 4200mAh/g. Therefore, it is expected that the silicon is a next-generation active material, negative electrode active material using silicon has been developed. However, the volume expansion of silicon, also referred to as a shrinkage rate is 400%, the charging and discharging of the expansion and contraction at the time of insertion and desorption of lithium occurs. Therefore, silicon is used as a negative electrode is a lithium ion secondary battery, it is possible to perform reversible charge-discharge reaction is very difficult. As one large expansion and contraction of the solution 1, including silicon monoxide and silicon oxide is used as a negative electrode active material is attempted.
Is the charging reaction of silicon monoxide according to the following reaction occurs. 4SiO+17.2Li++7.2e -→3Li4.4Si+Li4SiO4Li4SiO4 since the material is stable, and the irreversible capacity in charge and discharge of the element. On the other hand, only Li4.4Si is used as a negative electrode active material theoretical capacity of the lithium ion secondary battery and 2011mAh/g, carbon-based material is used as a negative electrode active material of the theoretical charge capacity of the lithium ion secondary battery exceeds 5 times. However, since the insulating silicon oxide, to serve as the electrode is necessary for imparting electrical conductivity.
In general, is an electrode for secondary battery, the active material on a current collector and conductive auxiliary agent and binder are prepared with the adhesive. In accordance with this prior art method, the auxiliary conductive agent is coated with a powder of SiO or SiOx, graphite, a mixture of the binder is coated on the copper foil, dried and compression-molded into a negative electrode can be manufactured by known (Patent Document 1). Using the negative electrode charging capacity of the lithium ion secondary battery, except that the initial irreversible capacity in the about 1500mAh/g, the theoretical value is about 75%. In this way, a high charge capacity of the negative electrode active material of the lithium ion secondary battery is promising as a silicon oxide SiOx is known, silicon oxide is used as a negative electrode active material in lithium ion secondary battery, the charging capacity close to the theoretical charge capacity and charge and discharge has not been developed.
Scope of claims (In Japanese)[請求項1]
 導電性基材と、
 前記導電性基材上に設けられ、平均粒径1.0μm以下の複数の酸化ケイ素の粒子と、前記複数の酸化ケイ素の粒子の隙間に存在する導電性物質とを備える複合層と、
 を有する積層体。

[請求項2]
 請求項1において、
 前記酸化ケイ素が一酸化ケイ素である積層体。

[請求項3]
 請求項1において、
 前記複数の酸化ケイ素の粒子が、非晶質酸化ケイ素の粒子とケイ素の粒子の混合物である積層体。

[請求項4]
 請求項1において、
 前記酸化ケイ素が非晶質酸化ケイ素である積層体。

[請求項5]
 請求項1から4のいずれかにおいて、
 前記複合層上に設けられ、前記導電性物質を含有する導電層をさらに有する積層体。

[請求項6]
 請求項5において、
 前記導電層の厚さが20μm以下である積層体。

[請求項7]
 蒸着またはスパッタリングによって、複数の酸化ケイ素の粒子を含む酸化ケイ素層を導電性基材上に形成する成膜工程と、
 導電性物質と結着剤とを含有する混合物を前記酸化ケイ素層上に塗布し、前記酸化ケイ素層に前記導電性物質を浸透させるとともに、前記酸化ケイ素層上に前記導電性物質を含有する導電層を形成する塗布工程と、
 を有する積層体の製造方法。

[請求項8]
 蒸着またはスパッタリングによって、複数の酸化ケイ素の粒子を含む酸化ケイ素層を導電性基材上に形成する成膜工程と、
 前記酸化ケイ素層を酸化して非晶質酸化ケイ素層に変換する酸化工程と、
 導電性物質と結着剤とを含有する混合物を前記非晶質酸化ケイ素層上に塗布し、前記非晶質酸化ケイ素層に前記導電性物質を浸透させるとともに、前記非晶質酸化ケイ素層上に前記導電性物質を含有する導電層を形成する塗布工程と、
 を有する積層体の製造方法。

[請求項9]
 蒸着またはスパッタリングによって、複数の酸化ケイ素の粒子を含む酸化ケイ素層を導電性基材上に形成する成膜工程と、
 前記酸化ケイ素層を加熱して非晶質酸化ケイ素およびケイ素から構成される混合層に変換する加熱工程と、
 導電性物質と結着剤とを含有する混合物を前記混合層上に塗布し、前記混合層に前記導電性物質を浸透させるとともに、前記混合層上に前記導電性物質を含有する導電層を形成する塗布工程と、
 を有する積層体の製造方法。

[請求項10]
 請求項7から9のいずれかにおいて、
 前記酸化ケイ素が一酸化ケイ素である積層体の製造方法。

[請求項11]
 正極と、請求項1から6のいずれかの積層体を備える負極と、電解質とを有するリチウムイオン二次電池。
  • Applicant
  • ※All designated countries except for US in the data before July 2012
  • NATIONAL INSTITUTE OF ADVANCED INDUSTRIAL SCIENCE AND TECHNOLOGY
  • Inventor
  • MAMIYA Mikito
  • AKIMOTO Junji
IPC(International Patent Classification)
Specified countries National States: AE AG AL AM AO AT AU AZ BA BB BG BH BN BR BW BY BZ CA CH CL CN CO CR CU CZ DE DJ DK DM DO DZ EC EE EG ES FI GB GD GE GH GM GT HN HR HU ID IL IN IR IS JO KE KG KH KN KP KR KW KZ LA LC LK LR LS LU LY MA MD ME MG MK MN MW MX MY MZ NA NG NI NO NZ OM PA PE PG PH PL PT QA RO RS RU RW SA SC SD SE SG SK SL SM ST SV SY TH TJ TM TN TR TT TZ UA UG US UZ VC VN ZA ZM ZW
ARIPO: BW GH GM KE LR LS MW MZ NA RW SD SL SZ TZ UG ZM ZW
EAPO: AM AZ BY KG KZ RU TJ TM
EPO: AL AT BE BG CH CY CZ DE DK EE ES FI FR GB GR HR HU IE IS IT LT LU LV MC MK MT NL NO PL PT RO RS SE SI SK SM TR
OAPI: BF BJ CF CG CI CM GA GN GQ GW KM ML MR NE SN ST TD TG
Reference ( R and D project ) Advances Coating Technology Research Center,AIST

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