Toyota Jidosha Kabushiki Kaisha

Kabushiki Kaisha Toyota Chuo Kenkyusho

Denso Corporation

Japan Advanced Institute of Science and Technology

Shingo Ohta

Masatsugu Kawakami

Takahiko Asaoka

Masaki Watanabe

Naohiro Hayashi

Shinji Nakanishi

Mitsuru Asai

Keita Takahashi

Tatsuya Shimoda

Hiroshi Suyama

Kazuyuki Nakanishi

Takashi Masuda

Chihiro Yada

Takashi Iseki

Hideyuki Yamamura

Tetsuro Kobayashi

Yuka Yamada

Toshiya Saito

Yasuhiro Ozawa

Ryohei Yamamoto

Tooru Saeki

Yuki Goto

Shogo Komagata

Yasutoshi Houjyou

Shunsuke Yamakawa

Ikuna Satou

A lithium-ion secondary battery includes: a single cell that includes a first electrode, a separator stacked on the first electrode, and a second electrode stacked on the separator. The first electrode includes a porous body that includes at least one LLZ-based solid electrolyte of a lithium lanthanum zirconate or the lithium lanthanum zirconate doped with an atom other than a Li atom, a La atom, and a Zr atom, and has a pore, and an active material held in the pore. The separator has a relative density of 80% or more, and includes the at least one LLZ-based solid electrolyte of the lithium lanthanum zirconate or the lithium lanthanum zirconate doped with the atom other than the Li atom, the La atom, and the Zr atom, and at least one of a B atom, a P atom, or a Si atom.

Lithium-ion secondary battery and manufacturing method thereof

The sintered body has an average particle size in the range of 0.1 &#x3bc;m or more and 5 &#x3bc;m or less, includes gamet-type oxide base material particles having at least Li, La, and Zr, has 8% by volume or more of voids, and has an ionic conductivity of 1.0&#xd7;10S/cm or more at temperature of 25&#xb0; C.

Sintered body and method for manufacturing thereof

There is provided a hydrogen-substituted garnet-type oxide containing at least Li, H, La and Zr and has an amount of hydrogen a (moll unit) per one unit of a garnet-type oxide in a range of &#x2264;1.85.

Hydrogen-substituted garnet-type oxide, manufacturing method of sintered body and manufacturing method of hydrogen-substituted garnet-type oxide

A garnet-type ion-conducting oxide configured to inhibit lithium carbonate formation on the surface of crystal particles thereof, and a method for producing an oxide electrolyte sintered body using the garnet-type ion-conducting oxide. The garnet-type ion-conducting oxide represented by a general formula (Li, E, H)LMO(where E is at least one kind of element selected from the group consisting of Al, Ga, Fe and Si; L is at least one kind of element selected from an alkaline-earth metal and a lanthanoid element: M is at least one kind of element selected from a transition element which be six-coordinated with oxygen and typical elements in groups 12 to 15 of the periodic table; 3&#x2264;x&#x2212;3y&#x2212;z&#x2264;; 0&#x2264;y&#x2264;0.22; C&#x2264;z&#x2264;2.8; 2.5&#x2264;&#x3b1;&#x2264;3.5; 1.5&#x2264;&#x2248;&#x2264;2.5; and 11&#x2264;&#x3b3;&#x2264;13), wherein a half-width of a diffraction peak which has a highest intensity and which is observed at a diffraction angle (2&#x3b8;) in a range of from 29&#xb0; to 32&#xb0; as a result of X-ray diffraction measurement using CuK&#x3b1; radiation, is 0.164&#xb0; or less.

Garnet-type ion-conducting oxide and method for producing oxide electrolyte sintered body

Provided are a battery separator with less voids, a lithium battery comprising the battery separator, and methods for producing them. A battery separator comprising an oxide electrolyte sintered body and a resin, wherein the oxide electrolyte sintered body has grain boundaries between crystal particles of a garnet-type ion-conducting oxide; wherein a number average particle diameter of the crystal particles is 3 &#x3bc;m or less; and wherein the oxide electrolyte sintered body satisfies the following formula 1:/()&#x2264;0.6&#x2003;&#x2003;Formula 1where Ris an intragranular resistance value that is an ion conductivity resistance inside the crystal particles, and Ris a grain boundary resistance value that is an ion conductivity resistance of the grain boundaries between the crystal particles.

Battery separator, lithium battery and methods for producing them

A method for producing an electrode comprising a porous garnet-type ion-conducting oxide sintered body with high ion conductivity, the electrode, and an electrode-electrolyte layer assembly comprising the electrode and an electrolyte layer comprising a dense garnet-type ion-conducting oxide sintered body with high ion conductivity. Disclosed is a method for producing an electrode, the method comprising: preparing crystal particles of a garnet-type ion-conducting oxide; preparing a lithium-containing flux; preparing the electrode active material; preparing an electrolyte material by mixing the crystal particles of the garnet-type ion-conducting oxide and the flux; and sintering the electrolyte material and the electrode active material by heating at a temperature of 650&#xb0; C. or less, wherein a number average particle diameter of the flux is larger than a number average particle diameter of the crystal particles of the garnet-type ion-conducting oxide.

Method for producing electrode, electrode, and electrode-electrolyte layer assembly

Disclosed is a cathode active material that can lower sintering temperature, the cathode active mated al including a particle of a lithium containing composite oxide having a layered rock-salt crystalline phase, wherein the layered rock-salt crystalline phase is partially deficient in lithium, a percentage of deficient lithium in the layered rock-salt crystalline phase in a surface portion of the particle is higher than that in the layered rock-salt crystalline phase inside the particle, and the particle includes two phases that are different in lattice constant as the layered rock-salt crystalline phase.

Cathode active material, cathode mixture, method for producing cathode active material, method for producing cathode, and method for producing oxide solid-state battery

A battery with excellent output characteristics and stability. The battery comprising a cathode, an anode and a separator disposed between the cathode and the anode, wherein the cathode comprises an aqueous electrolyte and a cathode active material; wherein the anode comprises an anode active material; wherein the separator comprises a first oxide electrolyte sintered body and a resin; wherein the first oxide electrolyte sintered body has grain boundaries between crystal particles of a garnet-type ion-conducting oxide represented by a general formula (A); wherein a number average particle diameter of the crystal particles is 3 &#x3bc;m or less; and wherein the first oxide electrolyte sintered body satisfies the following formula 1: R/(R+R)&#x2264;0.6 where Ris an intragranular resistance value that is an ion conductivity resistance inside the crystal particles, and Ris a grain boundary resistance value that is an ion conductivity resistance of the grain boundaries between the crystal particles.

Battery

A method for producing a cathode that can lower a sintering temperature is provided. The method comprises: acid-treating particles of a lithium containing composite oxide that has a layered rock-salt structure; obtaining a mixture by mixing the acid-treated particles with a lithium salt whose melting point is lower than that of the lithium containing composite oxide; and heating and sintering the mixture.

Method for producing cathode, and method for producing oxide solid-state battery

An oxide electrolyte sintered body with high lithium ion conductivity and a method for producing the same, which can obtain the oxide electrolyte sintered body with high lithium ion conductivity by sintering at lower temperature than ever before. The method for producing an oxide electrolyte sintered body may comprise the steps of: preparing crystal particles of a garnet-type ion-conducting oxide which comprises Li, H, at least one kind of element L selected from the group consisting of an alkaline-earth metal and a lanthanoid element, and at least one kind of element M selected from the group consisting of a transition element that can be 6-coordinated with oxygen and typical elements belonging to the Groups 12 to 15, and which is represented by a general formula (Li,E,H)LMO(where E is at least one kind of element selected from the group consisting of Al, Ga, Fe and Si, 3&#x2264;x&#x2212;3y&#x2212;z&#x2264;7, 0&#x2264;y&#x3c;0.22, 0&#x3c;z&#x2264;2.8, 2.5&#x2264;&#x3b1;&#x2264;3.5, 1.5&#x2264;&#x3b2;&#x2264;2.5, and 11&#x2264;&#x3b3;&#x2264;13); preparing a lithium-containing flux; and sintering a mixture of the crystal particles of the garnet-type ion-conducting oxide and the flux by heating at 400&#xb0; C. or more and 650&#xb0; C. or less.

Oxide electrolyte sintered body and method for producing the same

Provided are a slurry for a solid electrolyte, which can reduce the usage of a polymer binder, a method for producing a solid electrolyte layer, and a method for producing an all-solid-state battery. Disclosed is a slurry for a solid electrolyte, the slurry comprising a solvent, a lithium compound, and crystal particles of a garnet-type ion-conducting oxide represented by a general formula (Li,E,H)LMO(where E is at least one kind of element selected from the group consisting of Al, Ga, Fe and Si; L is at least one kind of element selected from an alkaline-earth metal and a lanthanoid element; M is at least one kind of element selected from a transition element that can be six-coordinated with oxygen and typical elements in groups 12 to 15 of the periodic table; 3&#x2264;x&#x2212;3y&#x2212;z&#x2264;7; 0&#x2264;y&#x2264;0.25; 0&#x3c;z&#x2264;2.8; 2.5&#x2264;&#x3b1;&#x2264;3.5; 1.5&#x2264;&#x3b2;&#x2264;2.5; and 11&#x2264;&#x3b3;&#x2264;13).

Slurry, method for producing solid electrolyte layer, and method for producing all-solid-state battery

A composite solid electrolyte with excellent formability and chemical stability and high lithium ion conductivity. The composite solid electrolyte may comprise an oxide-based solid electrolyte and a sulfide-based solid electrolyte, wherein the oxide-based solid electrolyte is (Li, Al)(La)(Zr, M)O(where M is at least one element selected from the group consisting of Nb and Ta; Y is a number in a range of 0&#x2264;Y&#x3c;0.22; and Z is a number in a range of 0&#x2264;Z&#x2264;2), and wherein the sulfide-based solid electrolyte is VLiX-(1&#x2212;V)((1&#x2212;W)LiS-WPS) (where X is a halogen element; V is a number in a range of 0&#x3c;V&#x3c;1; and W is a number in a range of 0.125&#x2264;W&#x2264;0.30).

Composite solid electrolyte

A method for producing a garnet type oxide solid electrolyte that is inhibited from a reaction of a flux and a crucible in heating and from a contamination with a crucible component produced by the reaction. The method for producing a garnet type oxide solid electrolyte represented by a general formula (Li, A)LaEZrMOmay comprise the steps of: preparing raw materials for the garnet type oxide solid electrolyte at a stoichiometric ratio of the above general formula; preparing flux raw materials by using NaCl and KCl at a molar ratio of NaCl:KCl=x:(1&#x2212;x) where x satisfies 0&#x2264;x&#x2264;1; mixing the solid electrolyte raw materials prepared in the above step and the flux raw materials prepared in the above step; and heating a mixture of the solid electrolyte raw materials and the flux raw materials at a temperature of less than 1100&#xb0; C.

Method for producing garnet type oxide solid electrolyte

A sintered electrode having a large cathode capacity is obtained. A method for producing a sintered electrode which uses a lithium containing composite oxide as a cathode active material, and lithium lanthanum zirconate as an oxide solid electrolyte comprises: mixing at least the lithium containing composite oxide and a hydroxide, to obtain a cathode mixture; mixing at least the lithium lanthanum zirconate and a lithium salt that has a melting point lower than the lithium lanthanum zirconate, to obtain a solid electrolyte mixture; laminating the cathode mixture and the solid electrolyte mixture, to obtain a laminate; and heating the laminate, to sinter at least the solid electrolyte mixture.

Method for producing sintered electrode

An all-solid-state lithium secondary battery includes a positive electrode; a negative electrode; and a solid electrolyte arranged between the positive and negative electrodes, to conduct lithium ions. In the all-solid-state lithium secondary battery, a mixed layer is in close contact with a surface of the solid electrolyte adjacent to the positive electrode, the mixed layer containing the positive-electrode active material and (Li, M)(B, A)O(wherein in the formula, M and A each represent at least one or more elements selected from C, Al, Si, Ga, Ge, In, and Sn, &#x3b1; satisfies 0&#x2264;&#x3b1;&#x3c;1, &#x3b2; represents the valence of M, &#x3b3; represents the average valence of (Li, M), y satisfies 0&#x2264;y&#x3c;1, z represents the average valence of (B, A) and x, &#x3b1;, &#x3b2;, &#x3b3;, z, and &#x3b3; satisfy the relational expression (x(1&#x2212;&#x3b1;)+x&#x3b1;/&#x3b2;)&#x3b3;+z=2&#x3b4;) serving as a matrix.

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Susono, Japan

Shingo Ohta