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    Solid electrolyte with low-symmetry garnet-related structure and lithium-ion secondary battery
    1.
    发明授权
    Solid electrolyte with low-symmetry garnet-related structure and lithium-ion secondary battery 有权

    公开(公告)号：US10763544B1

    公开(公告)日：2020-09-01

    申请号：US16304231

    申请日：2017-05-02

    申请人： National Institute of Advanced Industrial Science and Technology

    发明人： Naoki Hamao ,  Kunimitsu Kataoka ,  Junji Akimoto

    IPC分类号： H01M10/0562 ,  H01M10/0525 ,  C30B13/28 ,  C30B29/30 ,  C01G35/00

    摘要： A solid electrolyte material having high ion conductivity and a all-solid-state lithium-ion secondary battery using this solid electrolyte material are provided. The solid electrolyte material has a garnet-related structure crystal represented by the chemical composition Li7−x−yLa3Zr2−x−yTaxNbyO12 (0.05≤x+y≤0.2, x≥0, y≥0), which belongs to an orthorhombic system and a space group belonging to Ibca. The solid electrolyte material has lithium-ion conductivity at 25° C. of at least 1.0×10−4 S/cm. Also, in this solid electrolyte material, the lattice constants are 1.29 nm≤a≤1.32 nm, 1.26 nm≤b≤1.29 nm, and 1.29 nm≤c≤1.32 nm, and three 16f sites and one 8d site in the crystal structure are occupied by lithium-ions. The all-solid-state lithium-ion secondary battery has a positive electrode, a negative electrode, and a solid electrolyte, the solid electrolyte comprising this solid electrolyte material.

    Lithium-containing garnet crystal body, method for producing same, and all-solid-state lithium ion secondary battery
    3.
    发明授权
    Lithium-containing garnet crystal body, method for producing same, and all-solid-state lithium ion secondary battery 有权

    公开(公告)号：US10693184B2

    公开(公告)日：2020-06-23

    申请号：US15329750

    申请日：2015-07-30

    申请人： NATIONAL INSTITUTE OF ADVANCED INDUSTRIAL SCIENCE AND TECHNOLOGY

    发明人： Kunimitsu Kataoka ,  Junji Akimoto

    IPC分类号： H01M10/0562 ,  H01M10/0525 ,  C01G25/00 ,  C30B13/28 ,  C30B29/22 ,  C30B15/20

    摘要： Provided is a high-density lithium-containing garnet crystal body. The lithium-containing garnet crystal body has a relative density of 99% or more, belongs to a tetragonal system, and has a garnet-related type structure. A method of producing a Li7La3Zr2O12 crystal, which is one example of this lithium-containing garnet crystal body, includes melting a portion of a rod-like raw material composed of polycrystalline Li7La3Zr2O12 belonging to a tetragonal system while rotating it on a plane perpendicular to the longer direction and moving the melted portion in the longer direction. The moving rate of the melted portion is preferably 8 mm/h or more but not more than 19 mm/h. The rotational speed of the raw material is preferably 30 rpm or more but not more than 60 rpm. By increasing the moving rate of the melted portion, decomposition of the raw material due to evaporation of lithium can be prevented and by increasing the rotational speed of the raw material, air bubbles can be removed.

    Polycrystalline material and production method therefor
    7.
    发明授权
    Polycrystalline material and production method therefor 有权

    公开(公告)号：US10347912B2

    公开(公告)日：2019-07-09

    申请号：US15502452

    申请日：2015-08-06

    申请人： NATIONAL INSTITUTE OF ADVANCED INDUSTRIAL SCIENCE AND TECHNOLOGY

    发明人： Kunimitsu Kataoka ,  Junji Akimoto

    IPC分类号： C01G23/00 ,  H01M4/485 ,  H01M10/054 ,  H01M10/0525

    摘要： Provided are a sodium ion secondary battery and a lithium ion secondary battery capable of undergoing a reversible large-capacity charge/discharge reaction. The sodium and lithium ion secondary batteries each have a positive electrode, a negative electrode, and an electrolyte. The active substance of the positive or negative electrode of these secondary batteries is a single-phase polycrystal represented by the following chemical formula: NaxTi4O9 (2≤x≤3), preferably Na2Ti4O9, having a one-dimensional tunnel type structure, and belonging to a monoclinic crystal system. This polycrystal is obtained by filling a container made of molybdenum or the like with a raw material containing a sodium compound and at least one of a titanium compound and metal titanium, and firing at 800° C. or more but 1600° C. or less.

    Lithium ion conductive crystal body and all-solid state lithium ion secondary battery
    8.
    发明授权
    Lithium ion conductive crystal body and all-solid state lithium ion secondary battery 有权

    公开(公告)号：US11139504B2

    公开(公告)日：2021-10-05

    申请号：US16897119

    申请日：2020-06-09

    申请人： NATIONAL INSTITUTE OF ADVANCED INDUSTRIAL SCIENCE AND TECHNOLOGY

    发明人： Kunimitsu Kataoka ,  Junji Akimoto

    IPC分类号： H01M10/0562 ,  H01M10/0525 ,  H01M10/0585 ,  H01B1/08 ,  H01B1/12 ,  C01G25/00 ,  C01G35/00

    摘要： To provide a lithium ion conductive crystal body having a high density and a large length and an all-solid state lithium ion secondary battery containing the lithium ion conductive crystal body. A Li5La3Ta2O12 crystal body, which is one example of the lithium ion conductive crystal body, has a relative density of 99% or more, belongs to a cubic system, has a garnet-related type structure, and has a length of 2 cm or more. The Li5La3Ta2O12 crystal body is grown by a melting method employing a Li5La3Ta2O12 polycrystal body as a raw material. With the growing method, a Li5La3Ta2O12 crystal body having a relative density of 100% can also be obtained. In addition, the all-solid state lithium ion secondary battery has a positive electrode, a negative electrode, and a solid electrolyte, in which the solid electrolyte contains the lithium ion conductive crystal body.

    Solid electrolyte material and all solid lithium ion secondary battery
    9.
    发明授权
    Solid electrolyte material and all solid lithium ion secondary battery 有权

    公开(公告)号：US10566655B2

    公开(公告)日：2020-02-18

    申请号：US15776229

    申请日：2016-12-26

    申请人： National Institute of Advanced Industrial Science and Technology

    发明人： Kunimitsu Kataoka ,  Chika Takamori ,  Haruo Ishizaki ,  Junji Akimoto

    IPC分类号： H01M10/0525 ,  H01M10/0562 ,  C01G35/00 ,  C01G33/00

    摘要： There are provided a solid electrolyte material having high density and ion conductivity, and an all solid lithium ion secondary battery using the solid electrolyte material. The solid electrolyte material has a garnet-related structure which has a chemical composition represented by Li7-x-yLa3Zr2-x-yTaxNbyO12 (0≤x≤0.8, 0.2≤y≤1, and 0.2≤x+y≤1) and relative density of 99% or greater, and belongs to a cubic system. The solid electrolyte material has lithium ion conductivity which is equal to or greater than 1.0×10−3 S/cm. The solid electrolyte material has a lattice constant a which satisfies 1.28 nm≤a≤1.30 nm, and has a lithium ion which occupies only two or more 96h sites in a crystal structure. The all solid lithium ion secondary battery includes a positive electrode, a negative electrode, and a solid electrolyte. The solid electrolyte includes the solid electrolyte material.