JP5247570B2 - Thin film lithium secondary battery manufacturing apparatus and thin film lithium secondary battery manufacturing method - Google Patents

Thin film lithium secondary battery manufacturing apparatus and thin film lithium secondary battery manufacturing method Download PDF

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JP5247570B2
JP5247570B2 JP2009098467A JP2009098467A JP5247570B2 JP 5247570 B2 JP5247570 B2 JP 5247570B2 JP 2009098467 A JP2009098467 A JP 2009098467A JP 2009098467 A JP2009098467 A JP 2009098467A JP 5247570 B2 JP5247570 B2 JP 5247570B2
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substrate
chamber
forming
layer
secondary battery
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JP2010251075A (en
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勲 木村
武人 神保
弘綱 鄒
鉄也 島田
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Ulvac Inc
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    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/05—Accumulators with non-aqueous electrolyte
    • H01M10/056—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes
    • H01M10/0561—Accumulators with non-aqueous electrolyte characterised by the materials used as electrolytes, e.g. mixed inorganic/organic electrolytes the electrolyte being constituted of inorganic materials only
    • H01M10/0562—Solid materials
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M10/00—Secondary cells; Manufacture thereof
    • H01M10/04—Construction or manufacture in general
    • H01M10/0404—Machines for assembling batteries
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M4/00—Electrodes
    • H01M4/02—Electrodes composed of, or comprising, active material
    • H01M4/04—Processes of manufacture in general
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M2300/00—Electrolytes
    • H01M2300/0017—Non-aqueous electrolytes
    • H01M2300/0065—Solid electrolytes
    • H01M2300/0068—Solid electrolytes inorganic
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/10—Energy storage using batteries
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

Description

本発明は、固体電解質を用いたリチウム二次電池を製造する技術に関し、特に真空中で薄膜によってリチウム二次電池を製造する技術に関する。   The present invention relates to a technique for manufacturing a lithium secondary battery using a solid electrolyte, and more particularly to a technique for manufacturing a lithium secondary battery using a thin film in a vacuum.

従来から、携帯電話やパーソナルコンピュータの電源として、リチウムイオン二次電池が広く知られている。
しかし、リチウムイオン二次電池は、液体電解質を用いているため、液漏れや発火等が発生する場合があり、安全性についての課題がある。
そこで、近年、電解質の材料として固体材料を用いた全固体型のリチウム二次電池が提案されており、その開発が進展している。
特に、固体材料を用いた全固体型のリチウム二次電池として、薄膜からなる全固体型のリチウム二次電池は、カード型の電子部品等の電源用として期待されている。
しかし、薄膜からなる全固体型のリチウム二次電池は、種々の工程を経て製造されるため、製造装置が大型複雑化するという課題がある。
なお、本発明に関連する先行技術文献としては、例えば以下のようなものがある。 Conventionally, lithium ion secondary batteries have been widely known as power sources for mobile phones and personal computers.
However, since a lithium ion secondary battery uses a liquid electrolyte, liquid leakage, ignition, etc. may occur, and there are safety issues.
Therefore, in recent years, an all-solid-state lithium secondary battery using a solid material as an electrolyte material has been proposed, and its development is progressing.
In particular, as an all-solid-state lithium secondary battery using a solid material, an all-solid-type lithium secondary battery including a thin film is expected as a power source for a card-type electronic component or the like.
However, an all-solid-state lithium secondary battery made of a thin film is manufactured through various processes, and thus there is a problem that the manufacturing apparatus becomes large and complicated.
In addition, as a prior art document relevant to this invention, there exist the following, for example.

特開２００２−４２８６３号公報JP 2002-42863 A

本発明は、このような従来の技術の課題に鑑みてなされたもので、その目的とするところは、小型で簡素な構成の真空装置で薄膜リチウム二次電池を製造する技術を提供することにある。   The present invention has been made in view of the problems of the conventional technology, and an object of the present invention is to provide a technology for manufacturing a thin film lithium secondary battery with a vacuum device having a small and simple configuration. is there.

上記課題を解決するためになされた本発明は、真空中で、基板上に、正極層、負極層、固体電解質層、正極集電層、負極集電層、保護層を有する薄膜リチウム二次電池を製造するための薄膜リチウム二次電池製造装置であって、前記基板を搬入し且つ搬出するための仕込取出室と、前記基板上に分子中にリチウムを含む正極層をスパッタリングによって形成する正極層形成室と、前記基板上に真空蒸着によって負極層を形成する負極層形成室と、前記基板上に分子中にリチウムを含む固体電解質層をスパッタリングによって形成する固体電解質層形成室と、前記基板上に正極集電層と負極集電層をスパッタリングによって形成する集電体層形成室と、前記基板上に保護層を形成する保護層形成室とが、基板搬送機構を有する搬送室の周囲にそれぞれ配置されるとともに当該搬送室にそれぞれ接続され、前記仕込取出室内に、前記基板上に形成された正極層をアニール処理するための基板加熱手段が設けられている薄膜リチウム二次電池製造装置である。
本発明において、前記負極層形成室に、真空中で前記基板の上下関係を反転させる基板反転機構が設けられている場合にも効果的である。
本発明において、前記集電体層形成室に、成膜用マスクを交換するマスク交換機構が設けられている場合にも効果的である。
一方、本発明は、上述のいずれかの薄膜リチウム二次電池製造装置を用いて薄膜リチウム二次電池を製造する方法であって、前記集電体層形成室内に、集電体層形成用のターゲット及び保護層形成用のターゲットを含む複数のターゲットを配置し、前記仕込取出室から搬入した基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上に前記正極集電層をスパッタリングによって形成する工程と、前記基板を前記搬送室を介して前記仕込取出室内に搬入して当該基板上の正極集電層をアニール処理する工程と、前記基板を前記搬送室を介して前記正極層形成室内に搬入して当該基板上に前記正極層をスパッタリングによって形成する工程と、前記基板を前記搬送室を介して前記固体電解質層形成室内に搬入して当該基板上に前記固体電解質層をスパッタリングによって形成する工程と、前記基板を前記搬送室を介して前記負極層形成室内に搬入して当該基板上に前記負極層を真空蒸着によって形成する工程と、前記基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上に前記負極集電層をスパッタリングによって形成する工程と、前記基板を前記搬送室を介して前記保護層形成室内に搬入して当該基板上に第１の保護層を蒸着重合によって形成する工程と、前記基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上の第１の保護層上に第２の保護層をスパッタリングによって積層形成する工程とを有する薄膜リチウム二次電池製造方法である。
本発明において、前記負極層を形成する際に、前記基板反転機構によって前記基板の上下関係を反転させる工程を有する場合にも効果的である。
本発明において、前記正極集電層、前記負極集電層、前記第２の保護層を形成する際に、前記マスク交換機構によって前記成膜用マスクを交換する工程を有する場合にも効果的である。
本発明において、前記正極層が、コバルト酸リチウムからなる場合に特に効果的である。
本発明において、前記固体電解質層が、リン酸リチウムオキシナイトライドからなる場合に特に効果的である。 The present invention has been made to solve the above-described problems. A thin film lithium secondary battery having a positive electrode layer, a negative electrode layer, a solid electrolyte layer, a positive electrode current collecting layer, a negative electrode current collecting layer, and a protective layer on a substrate in a vacuum. A thin-film lithium secondary battery manufacturing apparatus for manufacturing a substrate, a loading / unloading chamber for loading and unloading the substrate, and a positive electrode layer for forming a positive electrode layer containing lithium in the molecule on the substrate by sputtering A forming chamber, a negative electrode layer forming chamber for forming a negative electrode layer on the substrate by vacuum deposition, a solid electrolyte layer forming chamber for forming a solid electrolyte layer containing lithium in the molecule on the substrate by sputtering, and the substrate A current collector layer forming chamber for forming a positive electrode current collecting layer and a negative electrode current collecting layer by sputtering and a protective layer forming chamber for forming a protective layer on the substrate are arranged around a transport chamber having a substrate transport mechanism. Thin-film lithium secondary battery manufacturing apparatus, each of which is arranged and connected to the transfer chamber, and is provided with substrate heating means for annealing the positive electrode layer formed on the substrate in the charging / unloading chamber It is.
In the present invention, the negative electrode layer forming chamber is also effective when a substrate reversing mechanism for reversing the vertical relationship of the substrates in a vacuum is provided.
The present invention is also effective when a mask exchange mechanism for exchanging the film forming mask is provided in the current collector layer forming chamber.
On the other hand, the present invention is a method of manufacturing a thin film lithium secondary battery using any one of the above-described thin film lithium secondary battery manufacturing apparatuses, wherein the current collector layer forming chamber is provided for forming a current collector layer. A plurality of targets including a target and a target for forming a protective layer are arranged, and the substrate carried in from the charging / unloading chamber is carried into the current collector layer forming chamber via the transfer chamber, and the positive electrode collector is placed on the substrate. A step of forming an electric layer by sputtering, a step of carrying the substrate into the charging / unloading chamber through the transfer chamber, and annealing the positive electrode current collecting layer on the substrate; and the substrate through the transfer chamber. Carrying the positive electrode layer forming chamber into the positive electrode layer forming chamber and forming the positive electrode layer on the substrate by sputtering; and carrying the substrate into the solid electrolyte layer forming chamber through the transfer chamber and placing the substrate on the substrate. A step of forming a body electrolyte layer by sputtering, a step of carrying the substrate into the negative electrode layer forming chamber via the transfer chamber, and forming the negative electrode layer on the substrate by vacuum deposition; and the transfer of the substrate Carrying the current collector layer forming chamber through a chamber and forming the negative electrode current collecting layer on the substrate by sputtering; and carrying the substrate into the protective layer forming chamber through the transfer chamber. Forming a first protective layer on the substrate by vapor deposition polymerization; carrying the substrate into the current collector layer forming chamber through the transfer chamber; and forming a first protective layer on the first protective layer on the substrate. A method for producing a thin film lithium secondary battery comprising: a step of laminating and forming two protective layers by sputtering.
In the present invention, when forming the negative electrode layer, it is also effective in the case of having a step of inverting the vertical relation of the substrate by the substrate inverting mechanism.
In the present invention, when forming the positive electrode current collecting layer, the negative electrode current collecting layer, and the second protective layer, it is also effective in the case of having a step of replacing the film forming mask by the mask replacing mechanism. is there.
In the present invention, it is particularly effective when the positive electrode layer is made of lithium cobalt oxide.
In the present invention, it is particularly effective when the solid electrolyte layer is made of lithium phosphate oxynitride.

本発明装置の場合、仕込取出室と、正極層形成室と、負極層形成室と、固体電解質層形成室と、集電体層形成室と、保護層形成室とが、基板搬送機構を有する搬送室の周囲にそれぞれ配置されるとともに当該搬送室にそれぞれ接続され、さらに仕込取出室内に基板加熱手段が設けられていることから、少ない成膜室及び処理室を有する真空装置で薄膜リチウム二次電池を製造することができる。
また、本発明によれば、仕込取出室を使用しない時間においてアニール処理を行うことができるので、効率良く各工程を行うことができる。
本発明において、負極層形成室に真空中で基板の上下関係を反転させる基板反転機構が設けられている場合には、この基板反転機構によって基板を反転させることによって、所謂フェイスアップで真空蒸着を行う特殊な構成の装置を用いる必要がなく、その結果、一般の真空蒸着装置を用いてコストダウンを図ることができる。
また、集電体層形成室に成膜用マスクを交換するマスク交換機構が設けられている場合には、このマスク交換機構によって成膜用マスクを交換することにより、異なる材料を用いて容易に集電体層を積層形成することができる。
さらに、保護層の材料として例えばアルミニウム等の金属を含むものを用いる場合に、集電体層形成室においてスパッタリングによって当該保護層を形成することができるので、成膜室を増やすことなく簡素な構成の薄膜リチウム二次電池製造装置を得ることができる。 In the case of the apparatus of the present invention, the charging / unloading chamber, the positive electrode layer forming chamber, the negative electrode layer forming chamber, the solid electrolyte layer forming chamber, the current collector layer forming chamber, and the protective layer forming chamber have a substrate transport mechanism. Since the substrate heating means is disposed in the periphery of the transfer chamber and connected to the transfer chamber, and the substrate heating means is provided in the charging / unloading chamber, the thin film lithium secondary can be used in a vacuum apparatus having a small number of film forming chambers and processing chambers. A battery can be manufactured.
Further, according to the present invention, since the annealing process can be performed in a time during which the preparation / extraction chamber is not used, each process can be performed efficiently.
In the present invention, when a substrate reversing mechanism for reversing the vertical relationship of the substrate in a vacuum is provided in the negative electrode layer forming chamber, the substrate is reversed by this substrate reversing mechanism, so that vacuum deposition is performed with a so-called face up. There is no need to use a specially configured apparatus, and as a result, the cost can be reduced by using a general vacuum deposition apparatus.
In addition, in the case where a mask exchange mechanism for exchanging the film formation mask is provided in the current collector layer forming chamber, the film formation mask is exchanged by this mask exchange mechanism, so that different materials can be used easily. A current collector layer can be stacked.
Further, when a material containing a metal such as aluminum is used as the material of the protective layer, the protective layer can be formed by sputtering in the current collector layer forming chamber, so that a simple configuration without increasing the film forming chamber is possible. A thin film lithium secondary battery manufacturing apparatus can be obtained.

本発明によれば、小型で簡素な構成の真空装置で薄膜リチウム二次電池を製造する技術を提供することができる。   ADVANTAGE OF THE INVENTION According to this invention, the technique which manufactures a thin film lithium secondary battery with the vacuum apparatus of a small and simple structure can be provided.

本発明に係る薄膜リチウム二次電池製造装置の実施の形態の概略構成平面図Schematic configuration plan view of an embodiment of a thin-film lithium secondary battery manufacturing apparatus according to the present invention 同実施の形態における仕込取出室及び搬送室の内部構成を示す縦断面図The longitudinal cross-sectional view which shows the internal structure of the preparation taking-out chamber and transfer chamber in the embodiment （ａ）（ｂ）：同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その１）(A) (b): Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 1) （ａ）（ｂ）：同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その２）(A) (b): Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 2) （ａ）（ｂ）：同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その３）(A) (b): Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 3) （ａ）（ｂ）：同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その４）(A) (b): Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 4) （ａ）（ｂ）：同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その５）(A) (b): Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 5) 同実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図（その６）Explanatory drawing which shows the conveyance operation of the board | substrate in the manufacturing process of the thin film lithium secondary battery of the embodiment (the 6)

以下、本発明の好ましい実施の形態を図面を参照して詳細に説明する。
図１は、本発明に係る薄膜リチウム二次電池製造装置の実施の形態の概略構成平面図である。
図１に示すように、本実施の形態の薄膜リチウム二次電池製造装置１は、図示しない真空排気系に接続された断面六角形状の搬送室２を有し、この搬送室２内には、基板１０を搬送するための搬送ロボット３が配置されている。
この搬送ロボット３は、伸縮旋回自在のアーム３０を有し、このアーム３０の先端部に、基板１０を支持して搬送するためのキャリア３１が取り付けられている。
搬送室２の周囲には、アニール処理室を兼ねる仕込取出室４、第１〜第３のスパッタリング室５、６、７、負極層形成室８、保護層形成室９が設けられている。
ここで、仕込取出室４、第１〜第３のスパッタリング室５〜７、負極層形成室８、保護層形成室９は、図示しない真空排気系に接続されるとともに、それぞれゲートバルブ４０、５０、６０、７０、８０、９０を介して搬送室２に接続されている。
本実施の形態では、仕込取出室４はアニール処理室を兼ねるもので、仕込取出室４内には、後述するように、例えばランプ加熱方式の加熱ヒータ（基板加熱手段）４６が設けられている。 Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the drawings.
FIG. 1 is a schematic configuration plan view of an embodiment of a thin-film lithium secondary battery manufacturing apparatus according to the present invention.
As shown in FIG. 1, the thin-film lithium secondary battery manufacturing apparatus 1 of the present embodiment includes a transfer chamber 2 having a hexagonal cross section connected to a vacuum exhaust system (not shown). A transfer robot 3 for transferring the substrate 10 is disposed.
This transfer robot 3 has an arm 30 that can be freely extended and retracted, and a carrier 31 for supporting and transferring the substrate 10 is attached to the tip of the arm 30.
Around the transfer chamber 2, a charging / unloading chamber 4 that also serves as an annealing chamber, first to third sputtering chambers 5, 6, 7, a negative electrode layer forming chamber 8, and a protective layer forming chamber 9 are provided.
Here, the charging / unloading chamber 4, the first to third sputtering chambers 5 to 7, the negative electrode layer forming chamber 8, and the protective layer forming chamber 9 are connected to a vacuum exhaust system (not shown) and gate valves 40 and 50, respectively. , 60, 70, 80, 90 are connected to the transfer chamber 2.
In the present embodiment, the charging / unloading chamber 4 also serves as an annealing chamber. In the charging / unloading chamber 4, as will be described later, for example, a lamp-heating heater (substrate heating means) 46 is provided. .

一方、本実施の形態の第１のスパッタリング室５は、集電体層形成室と保護層形成室の機能を兼ねるもので、その内部には、複数（本実施の形態の場合は４個）のターゲット５１〜５４が配置されている。
第１のターゲット５１としては、例えば、正極集電体層形成用のクロム（Ｃｒ）ターゲット、第２のターゲット５２としては、例えば、正極集電体層形成用の白金（Ｐｔ）ターゲット、第３のターゲット５３としては、例えば、負極集電体層形成用の銅（Ｃｕ）ターゲット、第４のターゲット５４としては、例えば、保護層形成用のアルミニウム（Ａｌ）ターゲットが配置されている。
そして、第１のスパッタリング室５には、例えばその側部に、各スパッタリングプロセスに応じて成膜用マスク５６（５６Ａ、５６Ｂ、５６Ｃ）を交換して所定の位置に装着するためのマスク交換機構５５が設けられている。 On the other hand, the first sputtering chamber 5 of the present embodiment also functions as a current collector layer forming chamber and a protective layer forming chamber, and there are a plurality of (four in the case of the present embodiment) inside. Targets 51 to 54 are arranged.
Examples of the first target 51 include a chromium (Cr) target for forming a positive electrode current collector layer, and examples of the second target 52 include a platinum (Pt) target for forming a positive electrode current collector layer, and a third target. As the target 53, for example, a copper (Cu) target for forming the negative electrode current collector layer is arranged, and as the fourth target 54, for example, an aluminum (Al) target for forming the protective layer is arranged.
In the first sputtering chamber 5, for example, a mask exchange mechanism for exchanging the film formation masks 56 (56 </ b> A, 56 </ b> B, 56 </ b> C) on the side thereof according to each sputtering process and mounting them at predetermined positions. 55 is provided.

また、本実施の形態の第１のスパッタリング室５は、図示しない反応ガス源に接続され、第１のスパッタリング室５内に、酸素（Ｏ2）ガスを導入するように構成されている。
第２のスパッタリング室６内には、正極層形成用のターゲット６１として、例えばコバルト酸リチウム（ＬｉＣｏＯ2）ターゲットが配置されている。
第３のスパッタリング室７内には、固体電解質層形成用のターゲット７１として、例えばリン酸リチウム（Ｌｉ3ＰＯ4）ターゲットが配置されている。
本実施の形態の第３のスパッタリング室７は、図示しない反応ガス源に接続され、酸素（Ｏ2）ガスを導入するように構成されている。
本実施の形態の負極層形成室８には、その底部に、例えば金属リチウム（Ｌｉ）からなる蒸発材料を加熱蒸発させるための蒸発源８１が配置されている。
そして、負極層形成室８には、真空中で例えば基板１０を回転させてその上下関係を反転させる基板反転機構８２が設けられている。 The first sputtering chamber 5 of the present embodiment is connected to a reaction gas source (not shown), and is configured to introduce oxygen (O 2 ) gas into the first sputtering chamber 5.
In the second sputtering chamber 6, for example, a lithium cobaltate (LiCoO 2 ) target is disposed as the target 61 for forming the positive electrode layer.
In the third sputtering chamber 7, for example, a lithium phosphate (Li 3 PO 4 ) target is disposed as the target 71 for forming the solid electrolyte layer.
The third sputtering chamber 7 of the present embodiment is connected to a reaction gas source (not shown) and configured to introduce oxygen (O 2 ) gas.
In the negative electrode layer forming chamber 8 of the present embodiment, an evaporation source 81 for heating and evaporating an evaporation material made of, for example, metallic lithium (Li) is disposed at the bottom.
The negative electrode layer forming chamber 8 is provided with a substrate reversing mechanism 82 that rotates, for example, the substrate 10 in a vacuum to reverse its vertical relationship.

保護層形成室９内には、例えばポリ尿素層を蒸着重合によって形成するための２種類の原料モノマー用の蒸発源９１、９２が配置されている。
本発明の場合、蒸着重合用の原料モノマーとしては、ジアミンモノマーとして、例えば、１，１２−ジアミノドデカン、イソシアネートモノマーとして、例えば、１，３−ビス（イソシアネートメチル）シクロヘキサンを好適に用いることができる。 In the protective layer forming chamber 9, for example, two types of raw material monomer evaporation sources 91 and 92 for forming a polyurea layer by vapor deposition polymerization are arranged.
In the case of the present invention, as a raw material monomer for vapor deposition polymerization, for example, 1,12-diaminododecane can be suitably used as a diamine monomer, and for example, 1,3-bis (isocyanatomethyl) cyclohexane can be suitably used as an isocyanate monomer. .

図２は、本実施の形態における仕込取出室及び搬送室の内部構成を示す縦断面図である。
図２に示すように、本実施の形態の仕込取出室４は、真空槽本体４１の一の側部に、基板１０を搬入又は搬出するための仕込取出口４２が設けられ、この仕込取出口４２は、開閉自在の真空扉４３を閉じた状態でＯリング４４によって密閉されるように構成されている。
一方、真空槽本体４１の下部には基板昇降機構１１が設けられている。
この基板昇降機構１１は、真空槽本体４１の下方に設けられた基部１２上に昇降ピン１３が複数設けられ、これら昇降ピン１３が真空槽本体４１内に挿入され、それぞれの上端部に設けられた支持部１４によって基板１０を支持するように構成されている。
ここで、基板昇降機構１１は、例えばモータ１５によって駆動されるボールねじ１６を有し、このボールねじ１６の動作によって基部１２が上下方向に移動されるようになっている。
一方、真空槽本体４１の上部には、例えば石英ガラスからなる窓部４５が設けられ、この窓部４５の上方の空間に、例えばランプ加熱方式の加熱ヒータ４６が設けられている。
また、加熱ヒータ４６の上方の天井部分には、加熱ヒータ４６からの赤外線を反射するための反射面４７が形成されている。 FIG. 2 is a longitudinal cross-sectional view showing the internal configuration of the charging / unloading chamber and the transfer chamber in the present embodiment.
As shown in FIG. 2, the charging / unloading chamber 4 of the present embodiment is provided with a charging / unloading port 42 for loading or unloading the substrate 10 at one side of the vacuum chamber body 41. 42 is configured to be sealed by an O-ring 44 with the openable / closable vacuum door 43 closed.
On the other hand, a substrate elevating mechanism 11 is provided in the lower part of the vacuum chamber body 41.
In the substrate lifting mechanism 11, a plurality of lifting pins 13 are provided on a base portion 12 provided below the vacuum chamber body 41, and these lifting pins 13 are inserted into the vacuum chamber body 41 and provided at respective upper ends. The substrate 10 is supported by the support portion 14.
Here, the substrate raising / lowering mechanism 11 has, for example, a ball screw 16 driven by a motor 15, and the base 12 is moved in the vertical direction by the operation of the ball screw 16.
On the other hand, a window portion 45 made of, for example, quartz glass is provided on the upper portion of the vacuum chamber body 41, and a lamp heater heater 46 is provided in a space above the window portion 45, for example.
In addition, a reflective surface 47 for reflecting infrared rays from the heater 46 is formed on the ceiling portion above the heater 46.

図３（ａ）（ｂ）〜図８は、本実施の形態の薄膜リチウム二次電池の製造工程における基板の搬送動作を示す説明図である。
本実施の形態において薄膜リチウム二次電池を製造するには、図２及び図３（ａ）に示すように、仕込取出室４の真空扉４３を開いて基板１０を仕込取出室４内に搬入し、基板昇降機構１１の支持部１４上に載置する。
そして、基板昇降機構１１を動作させて基板１０を所定の高さ位置に配置するとともに、仕込取出室４の真空扉４３を閉じて真空排気を行う。
仕込取出室４内の圧力が所定の値に到達した後、搬送室２との間のゲートバルブ４０を開き、搬送ロボット３を動作させてキャリア３１を仕込取出室４内に挿入し、基板昇降機構１１を下降させてキャリア３１上に基板１０を載置して、第１のスパッタリング室５との間のゲートバルブ５０を開き、図３（ｂ）に示すように、基板１０を第１のスパッタリング室５内に搬入する。 FIGS. 3A and 3B to 8 are explanatory views showing the substrate transport operation in the manufacturing process of the thin film lithium secondary battery of the present embodiment.
In order to manufacture the thin film lithium secondary battery in the present embodiment, as shown in FIGS. 2 and 3A, the vacuum door 43 of the charging / unloading chamber 4 is opened and the substrate 10 is loaded into the charging / unloading chamber 4. Then, it is placed on the support portion 14 of the substrate lifting mechanism 11.
Then, the substrate raising / lowering mechanism 11 is operated to place the substrate 10 at a predetermined height, and the vacuum door 43 of the loading / unloading chamber 4 is closed to perform evacuation.
After the pressure in the loading / unloading chamber 4 reaches a predetermined value, the gate valve 40 with the transfer chamber 2 is opened, and the transfer robot 3 is operated to insert the carrier 31 into the loading / unloading chamber 4 and lift the substrate. The mechanism 11 is lowered to place the substrate 10 on the carrier 31, and the gate valve 50 between the first sputtering chamber 5 and the first valve is opened. As shown in FIG. It is carried into the sputtering chamber 5.

第１のスパッタリング室５においては、正極集電体層形成用の成膜用マスク５６Ａを用い、基板１０と、第１のターゲット５１（例えばＣｒ）との間に高周波電力を印加することにより、スパッタリングによって基板１０上にＣｒ層を形成する。
その後、第２のターゲット５２（例えばＰｔ）との間に高周波電力を印加することにより、スパッタリングによって基板１０上に正極集電層（Ｐｔ／Ｃｒ）を形成する。 In the first sputtering chamber 5, by applying a high frequency power between the substrate 10 and the first target 51 (for example, Cr) using the film formation mask 56 </ b> A for forming the positive electrode current collector layer, A Cr layer is formed on the substrate 10 by sputtering.
Thereafter, a positive current collecting layer (Pt / Cr) is formed on the substrate 10 by sputtering by applying high-frequency power to the second target 52 (for example, Pt).

次に、搬送ロボット３を動作させ、図４（ａ）に示すように、搬送室２を介して基板１０を第２のスパッタリング室６内に搬入する。そして、第２のスパッタリング室６内にアルゴン（Ａｒ）ガスを導入し、基板１０と、正極層形成用のターゲット６１（ＬｉＣｏＯ2）との間に高周波電力を印加することにより、基板１０の正極集電体層上にＬｉＣｏＯ2からなる正極層を形成する。
本工程では、基板ステージに設けられたヒータ（図示せず）を動作させ、基板１０を加熱しながらスパッタリングを行う。
その後、搬送ロボット３を動作させ、図４（ｂ）に示すように、搬送室２を介して基板１０を仕込取出室４内に搬入する。そして、図２に示す加熱ヒータ４６を動作させ、基板１０上に形成された正極層に対してアニール処理を行う（例えば、６００℃、１０分程度）。これにより、基板１０上に形成された正極層が結晶化される。 Next, the transfer robot 3 is operated to load the substrate 10 into the second sputtering chamber 6 through the transfer chamber 2 as shown in FIG. Then, argon (Ar) gas is introduced into the second sputtering chamber 6, and high frequency power is applied between the substrate 10 and the target 61 (LiCoO 2 ) for forming the positive electrode layer, whereby the positive electrode of the substrate 10. A positive electrode layer made of LiCoO 2 is formed on the current collector layer.
In this step, sputtering is performed while the substrate 10 is heated by operating a heater (not shown) provided on the substrate stage.
Thereafter, the transfer robot 3 is operated, and the substrate 10 is carried into the preparation / extraction chamber 4 through the transfer chamber 2 as shown in FIG. Then, the heater 46 shown in FIG. 2 is operated to perform an annealing process on the positive electrode layer formed on the substrate 10 (for example, 600 ° C., about 10 minutes). Thereby, the positive electrode layer formed on the substrate 10 is crystallized.

次に、搬送ロボット３を動作させ、図５（ａ）に示すように、搬送室２を介して基板１０を第３のスパッタリング室７内に搬入する。そして、第３のスパッタリング室７内に例えば窒素（Ｎ2）ガスを導入し、基板１０と、固体電解質層形成用のターゲット７１（Ｌｉ3ＰＯ4）との間に高周波電力を印加することにより、基板１０の正極層上にＬｉＰＯＮ（リン酸リチウムオキシナイトライド）からなる固体電解質層を形成する。
本工程では、基板ステージに設けられた冷却機構（図示せず）を動作させ、基板１０を冷却しながらスパッタリングを行う。 Next, the transfer robot 3 is operated, and the substrate 10 is carried into the third sputtering chamber 7 through the transfer chamber 2 as shown in FIG. Then, for example, nitrogen (N 2 ) gas is introduced into the third sputtering chamber 7 and high frequency power is applied between the substrate 10 and the solid electrolyte layer forming target 71 (Li 3 PO 4 ). A solid electrolyte layer made of LiPON (lithium phosphate oxynitride) is formed on the positive electrode layer of the substrate 10.
In this step, sputtering is performed while the substrate 10 is cooled by operating a cooling mechanism (not shown) provided on the substrate stage.

次に、搬送ロボット３を動作させ、図５（ｂ）に示すように、搬送室２を介して基板１０を第１のスパッタリング室５内に搬入する。そして、基板１０と、第３のターゲット５３（例えばＣｕ）との間に高周波電力を印加することにより、基板１０上にＣｕからなる負極集電体層をスパッタリングによって形成する。
この工程においては、マスク交換機構５５を動作させて正極集電体層形成用の成膜用マスク５６Ａを第１のスパッタリング室５から取り出し、負極集電体層形成用の成膜用マスク５６Ｂを所定の位置に装着してスパッタリングを行う。 Next, the transfer robot 3 is operated, and the substrate 10 is carried into the first sputtering chamber 5 through the transfer chamber 2 as shown in FIG. Then, by applying high frequency power between the substrate 10 and the third target 53 (for example, Cu), a negative electrode current collector layer made of Cu is formed on the substrate 10 by sputtering.
In this step, the mask exchange mechanism 55 is operated to take out the film forming mask 56A for forming the positive electrode current collector layer from the first sputtering chamber 5, and the film forming mask 56B for forming the negative electrode current collector layer is removed. Sputtering is performed at a predetermined position.

次に、搬送ロボット３を動作させ、図６（ａ）に示すように、搬送室２を介して基板１０を負極層形成室８内に搬入し、蒸発源８１の蒸発材料（Ｌｉ）を加熱することにより、真空蒸着によって基板１０上にＬｉからなる負極層を形成する。
本工程では、基板反転機構８２を動作させ、例えば基板１０を回転させることにより、基板１０の上下関係を反転させる（所謂フェイスダウン）。
そして、基板ステージに設けられた冷却機構（図示せず）を動作させ、基板１０を冷却しながら蒸着を行う。
その後、基板反転機構８２を動作させ、基板１０を回転させることにより、基板１０の上下関係を反転させる（所謂フェイスアップ）。 Next, the transfer robot 3 is operated to carry the substrate 10 into the negative electrode layer forming chamber 8 through the transfer chamber 2 and heat the evaporation material (Li) of the evaporation source 81 as shown in FIG. Thus, a negative electrode layer made of Li is formed on the substrate 10 by vacuum deposition.
In this step, the substrate reversing mechanism 82 is operated to rotate the substrate 10, for example, thereby reversing the vertical relationship of the substrate 10 (so-called face down).
Then, a cooling mechanism (not shown) provided on the substrate stage is operated to perform vapor deposition while cooling the substrate 10.
Thereafter, the substrate reversing mechanism 82 is operated to rotate the substrate 10, thereby reversing the vertical relationship of the substrate 10 (so-called face up).

次に、搬送ロボット３を動作させ、図６（ｂ）に示すように、基板１０を保護層形成室９内に搬入し、蒸発源９１、９２の原料モノマーを加熱することにより、蒸着重合によって基板１０上にポリ尿素からなる第１の保護層を形成する。
この蒸着重合によって形成した、ポリ尿素からなる第１の保護層は、段差被覆性に優れた性質を有するものである。
本工程では、基板ステージに設けられた温度調整機構（図示せず）を動作させ、基板１０を一定温度に保持しながら蒸着重合を行う。 Next, the transport robot 3 is operated, and as shown in FIG. 6B, the substrate 10 is carried into the protective layer forming chamber 9, and the raw material monomers of the evaporation sources 91 and 92 are heated, thereby performing vapor deposition polymerization. A first protective layer made of polyurea is formed on the substrate 10.
The first protective layer made of polyurea formed by this vapor deposition polymerization has a property excellent in step coverage.
In this step, a temperature adjustment mechanism (not shown) provided on the substrate stage is operated to perform vapor deposition polymerization while maintaining the substrate 10 at a constant temperature.

次に、搬送ロボット３を動作させ、図７（ａ）に示すように、搬送室２を介して基板１０を第１のスパッタリング室５内に搬入し、第１のスパッタリング室５内に例えば酸素（Ｏ2）ガスを導入し、基板１０と、保護層形成用の第４のターゲット５４（例えばＡｌ）との間にそれぞれ高周波電力を印加することにより、基板１０の第１の保護層上に二酸化アルミニウム（Ａｌ2Ｏ3）からなる第２の保護層をスパッタリングによって形成する。
この工程においては、マスク交換機構５５を動作させて正極集電体層形成用の成膜用マスク５６Ｂを第１のスパッタリング室５から取り出し、保護層形成用の成膜用マスク５６Ｃを所定の位置に装着してスパッタリングを行う。
これにより、目的とする全固体型の薄膜リチウム二次電池が得られる。
その後、薄膜リチウム二次電池が形成された基板１０Ａを、図７（ｂ）及び図８に示すように、仕込取出室４を介して薄膜リチウム二次電池製造装置１の外部へ搬出する。 Next, the transfer robot 3 is operated, and as shown in FIG. 7A, the substrate 10 is carried into the first sputtering chamber 5 through the transfer chamber 2, and oxygen, for example, is introduced into the first sputtering chamber 5. (O 2 ) gas is introduced, and high frequency power is applied between the substrate 10 and the fourth target 54 (for example, Al) for forming the protective layer, whereby the first protective layer of the substrate 10 is applied. A second protective layer made of aluminum dioxide (Al 2 O 3 ) is formed by sputtering.
In this step, the mask exchange mechanism 55 is operated to take out the film-forming mask 56B for forming the positive electrode current collector layer from the first sputtering chamber 5, and the film-forming mask 56C for forming the protective layer is placed at a predetermined position. Sputtering is performed by attaching to the surface.
Thereby, the target all-solid-state thin film lithium secondary battery is obtained.
Thereafter, the substrate 10A on which the thin-film lithium secondary battery is formed is carried out of the thin-film lithium secondary battery manufacturing apparatus 1 through the loading / unloading chamber 4, as shown in FIGS.

以上述べたように本実施の形態の場合、仕込取出室４と、第１〜第３のスパッタリング室５、６、７と、負極層形成室８と、保護層形成室９とが、搬送ロボット３を有する搬送室２の周囲にそれぞれ配置されるとともに当該搬送室２にそれぞれ接続され、さらに仕込取出室４内に加熱ヒータ４６が設けられていることから、少ない成膜室及び処理室を有する真空装置で薄膜リチウム二次電池を製造することができる。
また、本実施の形態によれば、仕込取出室４を使用しない時間においてアニール処理を行うことができるので、効率良く各工程を行うことができる。
さらに、本実施の形態では、負極層形成室８に真空中で基板１０の上下関係を反転させる基板反転機構８２が設けられていることから、この基板反転機構８２によって基板１０を反転させることによって、所謂フェイスアップで真空蒸着を行う特殊な構成の装置を用いる必要がなく、その結果、一般の真空蒸着装置を用いてコストダウンを図ることができる。 As described above, in the case of the present embodiment, the loading / unloading chamber 4, the first to third sputtering chambers 5, 6, 7, the negative electrode layer forming chamber 8, and the protective layer forming chamber 9 are transport robots. Since the heater 46 is provided in each of the transfer chambers 2 and connected to the respective transfer chambers 2 and further in the charging / unloading chamber 4, there are few film forming chambers and processing chambers. A thin film lithium secondary battery can be manufactured with a vacuum apparatus.
Moreover, according to this Embodiment, since annealing treatment can be performed in the time which does not use the preparation taking-out chamber 4, each process can be performed efficiently.
Further, in the present embodiment, since the substrate reversing mechanism 82 for reversing the vertical relationship of the substrate 10 in the vacuum is provided in the negative electrode layer forming chamber 8, the substrate 10 is reversed by the substrate reversing mechanism 82. Therefore, it is not necessary to use an apparatus having a special configuration for performing vacuum deposition by so-called face-up, and as a result, the cost can be reduced by using a general vacuum deposition apparatus.

また、第１のスパッタリング室５に成膜用マスク５６を交換するマスク交換機構５５が設けられていることから、このマスク交換機構５５によって成膜用マスク５６を交換することにより、異なる材料を用いて容易に集電体層を積層形成することができる。
さらに、本実施の形態では、第２の保護層の材料として二酸化アルミニウム（Ａｌ2Ｏ3）を用いることから、第１のスパッタリング室５において第２の保護層をスパッタリングによって形成することができ、その結果、成膜室を増やすことなく簡素な構成の薄膜リチウム二次電池製造装置１を得ることができる。 Further, since a mask exchange mechanism 55 for exchanging the film formation mask 56 is provided in the first sputtering chamber 5, a different material is used by exchanging the film formation mask 56 by the mask exchange mechanism 55. Thus, the current collector layer can be easily laminated.
Furthermore, in this embodiment, since aluminum dioxide (Al 2 O 3 ) is used as the material of the second protective layer, the second protective layer can be formed by sputtering in the first sputtering chamber 5, As a result, the thin film lithium secondary battery manufacturing apparatus 1 having a simple configuration can be obtained without increasing the number of film forming chambers.

なお、本発明は上述の実施の形態に限られることなく、種々の変更を行うことができる。
例えば、上述の実施の形態においては、保護層として、蒸着重合によって第１の保護層形成し、さらに、第１の保護層の上にスパッタリングによって第２の保護層を形成するようにしたが、本発明はこれに限られず、スパッタリングのみによって保護層を形成することもできる。
この場合、ターゲットとしては、Ａｌ（又はＡｌ2Ｏ3）からなるものを用い、保護層として、例えば、Ａｌ2Ｏ3／Ａｌ／Ａｌ2Ｏ3が積層された膜を形成することもできる。このような保護層を形成すれば、真空槽内の室の数を減らすことができるとともに、水分のバリア性を向上させることが可能になる。
さらに、上記実施の形態における各室の配置構成は一例であり、必要とするプロセスに応じて適宜変更することができる。
さらにまた、本発明は、種々の材料、形状、大きさの基板、例えば、シリコン基板、セラミックス基板、耐熱樹脂基板、雲母基板等に適用することができるものである。 The present invention is not limited to the above-described embodiment, and various changes can be made.
For example, in the above-described embodiment, as the protective layer, the first protective layer is formed by vapor deposition polymerization, and further, the second protective layer is formed on the first protective layer by sputtering. The present invention is not limited to this, and the protective layer can be formed only by sputtering.
In this case, a target made of Al (or Al 2 O 3 ) is used as the target, and a film in which, for example, Al 2 O 3 / Al / Al 2 O 3 is laminated can be formed as the protective layer. If such a protective layer is formed, the number of chambers in the vacuum chamber can be reduced and the moisture barrier property can be improved.
Furthermore, the arrangement configuration of each chamber in the above embodiment is merely an example, and can be appropriately changed according to a required process.
Furthermore, the present invention can be applied to substrates of various materials, shapes, and sizes, such as silicon substrates, ceramic substrates, heat resistant resin substrates, mica substrates, and the like.

１…薄膜リチウム二次電池製造装置、２…搬送室、３…搬送ロボット（基板搬送機構）、４…仕込取出室、５…第１のスパッタリング室（集電体層形成室、保護層形成室）、６…第２のスパッタリング室（正極層形成室）、７…第３のスパッタリング室（固体電解質層形成室）、８…負極層形成室、９…保護層形成室、１０…基板、１１…基板昇降機構、４６…加熱ヒータ（基板加熱手段）、５１〜５４…第１〜第４のターゲット、６１…正極層形成用のターゲット、７１…固体電解質層形成用のターゲット、８１…蒸発源、９１、９２…原料モノマー用の蒸発源 DESCRIPTION OF SYMBOLS 1 ... Thin-film lithium secondary battery manufacturing apparatus, 2 ... Transfer chamber, 3 ... Transfer robot (substrate transfer mechanism), 4 ... Preparation taking-out chamber, 5 ... 1st sputtering chamber (collector layer formation chamber, protective layer formation chamber) ), 6 ... 2nd sputtering chamber (positive electrode layer forming chamber), 7 ... 3rd sputtering chamber (solid electrolyte layer forming chamber), 8 ... Negative electrode layer forming chamber, 9 ... Protective layer forming chamber, 10 ... Substrate, 11 DESCRIPTION OF SYMBOLS ... Substrate raising / lowering mechanism 46 ... Heater (substrate heating means) 51-54 ... 1st-4th target, 61 ... Target for positive electrode layer formation, 71 ... Target for solid electrolyte layer formation, 81 ... Evaporation source 91, 92... Evaporation source for raw material monomer

Claims (8)

真空中で、基板上に、正極層、負極層、固体電解質層、正極集電層、負極集電層、保護層を有する薄膜リチウム二次電池を製造するための薄膜リチウム二次電池製造装置であって、
前記基板を搬入し且つ搬出するための仕込取出室と、前記基板上に分子中にリチウムを含む正極層をスパッタリングによって形成する正極層形成室と、前記基板上に真空蒸着によって負極層を形成する負極層形成室と、前記基板上に分子中にリチウムを含む固体電解質層をスパッタリングによって形成する固体電解質層形成室と、前記基板上に正極集電層と負極集電層をスパッタリングによって形成する集電体層形成室と、前記基板上に保護層を形成する保護層形成室とが、基板搬送機構を有する搬送室の周囲にそれぞれ配置されるとともに当該搬送室にそれぞれ接続され、
前記仕込取出室内に、前記基板上に形成された正極層をアニール処理するための基板加熱手段が設けられている薄膜リチウム二次電池製造装置。 A thin film lithium secondary battery manufacturing apparatus for manufacturing a thin film lithium secondary battery having a positive electrode layer, a negative electrode layer, a solid electrolyte layer, a positive electrode current collector layer, a negative electrode current collector layer, and a protective layer on a substrate in a vacuum. There,
A loading / unloading chamber for loading and unloading the substrate, a positive electrode layer forming chamber for forming a positive electrode layer containing lithium in the molecule on the substrate by sputtering, and forming a negative electrode layer on the substrate by vacuum deposition. A negative electrode layer forming chamber, a solid electrolyte layer forming chamber for forming a solid electrolyte layer containing lithium in the molecule on the substrate by sputtering, and a collector for forming a positive electrode current collecting layer and a negative electrode current collecting layer on the substrate by sputtering. An electric body layer forming chamber and a protective layer forming chamber for forming a protective layer on the substrate are respectively arranged around a transfer chamber having a substrate transfer mechanism and connected to the transfer chamber,
An apparatus for manufacturing a thin film lithium secondary battery, wherein a substrate heating means for annealing the positive electrode layer formed on the substrate is provided in the charging / unloading chamber. 前記負極層形成室には、真空中で前記基板の上下関係を反転させる基板反転機構が設けられている請求項１記載の薄膜リチウム二次電池製造装置。   The thin-film lithium secondary battery manufacturing apparatus according to claim 1, wherein the negative electrode layer forming chamber is provided with a substrate reversing mechanism for reversing the vertical relationship of the substrates in a vacuum. 前記集電体層形成室には、成膜用マスクを交換するマスク交換機構が設けられている請求項１乃至２のいずれか１項記載の薄膜リチウム二次電池製造装置。   The thin film lithium secondary battery manufacturing apparatus according to claim 1, wherein the current collector layer forming chamber is provided with a mask exchange mechanism for exchanging a film forming mask. 請求項１乃至３のいずれか１項記載の薄膜リチウム二次電池製造装置を用いて薄膜リチウム二次電池を製造する方法であって、
前記集電体層形成室内に、集電体層形成用のターゲット及び保護層形成用のターゲットを含む複数のターゲットを配置し、
前記仕込取出室から搬入した基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上に前記正極集電層をスパッタリングによって形成する工程と、
前記基板を前記搬送室を介して前記仕込取出室内に搬入して当該基板上の正極集電層をアニール処理する工程と、
前記基板を前記搬送室を介して前記正極層形成室内に搬入して当該基板上に前記正極層をスパッタリングによって形成する工程と、
前記基板を前記搬送室を介して前記固体電解質層形成室内に搬入して当該基板上に前記固体電解質層をスパッタリングによって形成する工程と、
前記基板を前記搬送室を介して前記負極層形成室内に搬入して当該基板上に前記負極層を真空蒸着によって形成する工程と、
前記基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上に前記負極集電層をスパッタリングによって形成する工程と、
前記基板を前記搬送室を介して前記保護層形成室内に搬入して当該基板上に第１の保護層を蒸着重合によって形成する工程と、
前記基板を前記搬送室を介して前記集電体層形成室内に搬入して当該基板上の第１の保護層上に第２の保護層をスパッタリングによって積層形成する工程とを有する薄膜リチウム二次電池製造方法。 A method of manufacturing a thin film lithium secondary battery using the thin film lithium secondary battery manufacturing apparatus according to any one of claims 1 to 3,
A plurality of targets including a current collector layer forming target and a protective layer forming target are disposed in the current collector layer forming chamber,
A step of carrying the substrate carried in from the charging / unloading chamber into the current collector layer forming chamber via the transfer chamber and forming the positive electrode current collecting layer on the substrate by sputtering;
Carrying the substrate into the charging / unloading chamber through the transfer chamber and annealing the positive electrode current collecting layer on the substrate;
Carrying the substrate into the positive electrode layer forming chamber through the transfer chamber and forming the positive electrode layer on the substrate by sputtering;
Carrying the substrate into the solid electrolyte layer forming chamber through the transfer chamber and forming the solid electrolyte layer on the substrate by sputtering;
Carrying the substrate into the negative electrode layer forming chamber through the transfer chamber and forming the negative electrode layer on the substrate by vacuum deposition;
Carrying the substrate into the current collector layer forming chamber through the transfer chamber and forming the negative electrode current collecting layer on the substrate by sputtering;
Carrying the substrate into the protective layer forming chamber via the transfer chamber and forming a first protective layer on the substrate by vapor deposition polymerization;
Carrying the substrate into the current collector layer forming chamber through the transfer chamber and forming a second protective layer on the first protective layer on the substrate by sputtering to form a thin film lithium secondary Battery manufacturing method. 前記負極層を形成する際に、前記基板反転機構によって前記基板の上下関係を反転させる工程を有する請求項４記載の薄膜リチウム二次電池製造方法。   The method for producing a thin film lithium secondary battery according to claim 4, further comprising a step of inverting the vertical relation of the substrate by the substrate inverting mechanism when forming the negative electrode layer. 前記正極集電層、前記負極集電層、前記第２の保護層を形成する際に、前記マスク交換機構によって前記成膜用マスクを交換する工程を有する請求項４又は５のいずれか１項記載の薄膜リチウム二次電池製造方法。   6. The method according to claim 4, further comprising a step of exchanging the film-forming mask by the mask exchanging mechanism when forming the positive electrode current collecting layer, the negative electrode current collecting layer, and the second protective layer. The manufacturing method of the thin film lithium secondary battery of description. 前記正極層は、コバルト酸リチウムからなる請求項４乃至６のいずれか１項記載の薄膜リチウム二次電池製造方法。   The method of manufacturing a thin film lithium secondary battery according to claim 4, wherein the positive electrode layer is made of lithium cobalt oxide. 前記固体電解質層は、リン酸リチウムオキシナイトライドからなる請求項４乃至７のいずれか１項記載の薄膜リチウム二次電池製造方法。   The method for producing a thin film lithium secondary battery according to claim 4, wherein the solid electrolyte layer is made of lithium phosphate oxynitride.
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