JP2015138614A - Method for manufacturing battery electrode, battery electrode, and secondary battery - Google Patents

Method for manufacturing battery electrode, battery electrode, and secondary battery Download PDF

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JP2015138614A
JP2015138614A JP2014008534A JP2014008534A JP2015138614A JP 2015138614 A JP2015138614 A JP 2015138614A JP 2014008534 A JP2014008534 A JP 2014008534A JP 2014008534 A JP2014008534 A JP 2014008534A JP 2015138614 A JP2015138614 A JP 2015138614A
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electrode
electrode plate
active material
hole
manufacturing
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JP6369027B2 (en
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悠人 成澤
Haruto Narisawa
悠人 成澤
洋一 吉岡
Yoichi Yoshioka
洋一 吉岡
義貴 上原
Yoshitaka Uehara
義貴 上原
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Nissan Motor Co Ltd
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    • 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
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    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
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    • Y02E60/10—Energy storage using batteries

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Abstract

PROBLEM TO BE SOLVED: To provide a method for manufacturing a battery electrode which facilitates the manufacturing of an electrode with many micro holes having a diameter of several tens micrometers.SOLUTION: A method for manufacturing a battery electrode in which fine holes 4 are formed in an electrode plate 3 in a thickness direction thereof comprises: an electrode plate forming process in which the electrode plate 3 is formed by coating a current collector foil 1 with an active material 2; a hole forming step in which holes 4 are formed in the electrode plate 3; and a press step in which the electrode plate 3 with the holes 4 formed therein is pressed in the thickness direction. The holes 4 formed in the hole forming step are reduced in size in the press step, which makes possible to form many micro holes having a diameter of several tens micrometers.

Description

この発明は、リチウムイオン電池などの電極の製造に関する。   The present invention relates to the manufacture of electrodes such as lithium ion batteries.

リチウムイオン２次電池は電解質内において電気化学反応により発電を行なう発電要素として、リチウム金属酸化物からなる正極と、炭素材からなる負極とを交互に積層している。   Lithium ion secondary batteries alternately stack positive electrodes made of lithium metal oxides and negative electrodes made of carbon materials as power generation elements that generate power by an electrochemical reaction in an electrolyte.

こうしたリチウムイオン２次電池の電極に関して、特許文献１は正極、負極及び分離膜に電極面に垂直な複数の微細な孔部（マイクロホール）をレーザー加工により形成し、電極への電解液の浸透を促進することを提案している。   Regarding the electrode of such a lithium ion secondary battery, Patent Document 1 discloses that a plurality of fine holes (microholes) perpendicular to the electrode surface are formed in the positive electrode, the negative electrode, and the separation membrane by laser processing, and the electrolyte solution penetrates into the electrode. Propose to promote.

特許３６９０５２２号公報Japanese Patent No. 3690522

電極への電解液の均一な浸潤のためには、マイクロホールを高密度で数多く設ける必要がある。一方、電極の体積を確保するためには、各マイクロホールの径を小さくする必要がある。つまり、電極の性能を上げるためには、電極に径の小さなマイクロホールを数多く形成することが望ましい。   In order to uniformly infiltrate the electrolyte into the electrode, it is necessary to provide a large number of microholes at a high density. On the other hand, in order to ensure the volume of the electrode, it is necessary to reduce the diameter of each microhole. That is, in order to improve the performance of the electrode, it is desirable to form a large number of microholes having a small diameter in the electrode.

特許文献１には、レーザ加工によるマイクロホールの形成方法で形成されるマイクロホールの径は０．５ミリメートル（ｍｍ）と説明されている。一方、電極の体積損失を小さくするためには、マイクロホールの径を数十ミクロンメートル（μｍ）に抑えることが望ましい。   Patent Document 1 describes that the diameter of a microhole formed by a method of forming a microhole by laser processing is 0.5 millimeter (mm). On the other hand, in order to reduce the volume loss of the electrode, it is desirable to suppress the diameter of the microhole to several tens of micrometers (μm).

この発明は、電極へのマイクロホールの形成に関わる以上の問題を解決すべくなされたもので、数十μｍの径の多数のマイクロホールを備えた電極を容易に製造できるようにすることを目的とする。   The present invention has been made to solve the above problems related to the formation of microholes in electrodes, and an object thereof is to make it possible to easily manufacture an electrode having a large number of microholes with a diameter of several tens of μm. And

以上の目的を達成するために、この発明のある実施形態は、電極板に厚さ方向の複数の微細な孔部を形成する電極の製造方法に適用される。製造方法は、集電箔に活物質を塗布して電極板を形成する電極板形成工程と、電極板に孔部を形成する孔部形成工程と、孔部を形成した電極板を厚さ方向にプレスするプレス工程と、を含んで構成される。   In order to achieve the above object, an embodiment of the present invention is applied to an electrode manufacturing method in which a plurality of fine holes in the thickness direction are formed in an electrode plate. The manufacturing method includes an electrode plate forming step of forming an electrode plate by applying an active material to a current collector foil, a hole forming step of forming a hole in the electrode plate, and a thickness direction of the electrode plate in which the hole is formed And a pressing step for pressing.

孔部を形成した電極板を厚さ方向にプレスすることで、電極板の活物質が圧縮される。圧縮された活物質は厚さ方向と直交する方向へ膨出し、孔部を収縮させる。結果として、孔部が小径化し、活物質の体積密度がプレス工程以前と比べて増加する。また、プレス工程で電極板を厚さ方向にプレスすることで活物質の表面の凹凸が均され、均一な平面となる。   By pressing the electrode plate in which the hole is formed in the thickness direction, the active material of the electrode plate is compressed. The compressed active material swells in a direction perpendicular to the thickness direction and contracts the hole. As a result, the diameter of the hole is reduced, and the volume density of the active material is increased as compared with that before the pressing step. Moreover, the unevenness | corrugation of the surface of an active material is leveled by pressing an electrode plate in the thickness direction at a press process, and it becomes a uniform plane.

この発明の第１の実施形態による電極の製造方法を工程順に説明する、電極板の断面図である。It is sectional drawing of the electrode plate explaining the manufacturing method of the electrode by 1st Embodiment of this invention to process order. この発明の第１の実施形態による孔部形成工程を説明する、電極板と治具の斜視図である。It is a perspective view of an electrode plate and a jig explaining a hole part formation process by a 1st embodiment of this invention. この発明の第１の実施形態によるプレス工程を説明する、電極板とプレス治具の断面図である。It is sectional drawing of an electrode plate and a press jig explaining the press process by 1st Embodiment of this invention. この発明の第２の実施形態によるプレス工程を説明する、電極板とプレス治具の断面図である。It is sectional drawing of an electrode plate and a press jig explaining the press process by 2nd Embodiment of this invention.

図１−３を参照して、この発明の第１の実施形態を説明する。   A first embodiment of the present invention will be described with reference to FIGS.

この実施形態はリチウムイオン２次電池の電極の製造方法に関する。リチウムイオン２次電池は電解質内において電気化学反応により発電を行なう発電要素として、リチウム金属酸化物からなる正極と、炭素材からなる負極と、を備える。正極と負極は交互に積層される。正極と負極はいずれも、集電箔の上に活物質を塗布することで形成される。正極と負極は塗布される活物質が異なるのみで、他の仕様は同じであるため、以下の説明では正極と負極を電極と総称する。   This embodiment relates to a method for manufacturing an electrode of a lithium ion secondary battery. A lithium ion secondary battery includes a positive electrode made of a lithium metal oxide and a negative electrode made of a carbon material as a power generation element that generates power by an electrochemical reaction in an electrolyte. The positive electrode and the negative electrode are alternately stacked. Both the positive electrode and the negative electrode are formed by applying an active material on a current collector foil. Since the positive electrode and the negative electrode differ only in the applied active material and other specifications are the same, in the following description, the positive electrode and the negative electrode are collectively referred to as electrodes.

この実施形態による電極の製造方法は、次の３つの工程からなる。   The electrode manufacturing method according to this embodiment includes the following three steps.

すなわち、電極板形成工程と、孔部形成工程と、プレス工程である。   That is, an electrode plate forming process, a hole forming process, and a pressing process.

図１を参照すると、電極板形成工程では、図の（ａ）に示すように、集電箔１の一面に活物質２を塗布することで、集電箔１と活物質２が一体化された電極板３を形成する。   Referring to FIG. 1, in the electrode plate forming step, as shown in FIG. 1A, the current collector foil 1 and the active material 2 are integrated by applying the active material 2 to one surface of the current collector foil 1. An electrode plate 3 is formed.

図２を参照すると、孔部形成工程では、ラジアル方向に数多くのピン７を突出させたローラ状の治具５を用いる。治具５を所定圧力Ｐ１で電極板３の活物質２の表面に押しつけて転動させることで、活物質２にピン７の密度に応じた多数の孔部４が等間隔で規則的に形成される。 Referring to FIG. 2, in the hole forming step, a roller-shaped jig 5 having a large number of pins 7 protruding in the radial direction is used. By pressing and rolling the jig 5 against the surface of the active material 2 of the electrode plate 3 at a predetermined pressure P 1 , a large number of holes 4 corresponding to the density of the pins 7 are regularly formed in the active material 2 at equal intervals. It is formed.

再び図１を参照すると、孔部形成工程においては、治具５の個々のピン７が図の（ｂ）に示すように活物質２に貫入し、活物質２の塑性変形により活物質２に多数の孔部４が形成される。孔部形成工程は好ましくは電極板形成工程で集電箔１に塗布された活物質２が塑性変形しやすい状態、すなわち活物質２が硬化する前に実施する。孔部形成工程により、図の（ｅ）に示すようにピン７の径に略等しい径ＷＡの孔部４が活物質２に多数形成される。 Referring to FIG. 1 again, in the hole forming step, individual pins 7 of the jig 5 penetrate into the active material 2 as shown in FIG. A large number of holes 4 are formed. The hole forming step is preferably carried out in a state where the active material 2 applied to the current collector foil 1 in the electrode plate forming step is easily plastically deformed, that is, before the active material 2 is cured. The hole forming step is substantially equal diameter W A of the hole 4 to the diameter of the pin 7 as shown in (e) in the figure is a large number in the active material 2.

このように、ラジアル方向に数多くのピン７を突出させたローラ状の治具５を用いることで孔部４を容易に形成することができる。しかしながら、この発明は孔部形成工程における孔部４の形成方法には限定されない。例えば、表面に数多くのピン７を突設した板状の治具を上方から活物質２に押しつけて孔部４を形成することも可能である。あるいは、前記従来技術が提案するレーザ加工により孔部４を形成しても良い。   As described above, the hole 4 can be easily formed by using the roller-shaped jig 5 in which a large number of pins 7 protrude in the radial direction. However, the present invention is not limited to the method of forming the hole 4 in the hole forming process. For example, it is also possible to form the hole 4 by pressing a plate-like jig having a large number of pins 7 protruding on the surface against the active material 2 from above. Or you may form the hole 4 by the laser processing which the said prior art proposes.

図３を参照すると、プレス工程では、多数の孔部４を形成した活物質２に、平面状の押圧面を有するプレス治具６を用いて上方から垂直方向に圧力Ｐ２を加える。 Referring to FIG. 3, in the pressing step, pressure P 2 is applied to the active material 2 having a large number of holes 4 in the vertical direction from above using a pressing jig 6 having a flat pressing surface.

再び図１を参照すると、図の（ｃ）に示すように、上方から垂直方向の圧力Ｐ２を加えられた活物質２は圧縮変形し、上下方向の寸法、すなわち厚さをＨＡからＨＢへと減じる一方、圧縮により減じた体積相当分の活物質２を孔部４の内側に進出させる。その結果、孔部４は図の（ｄ）に示すように、図の（ｅ）に示すプレス工程以前の径ＷＡより小さな径ＷＢへと収縮する。このときプレス治具６が活物質２に加える圧力Ｐ２は、孔部形成工程でローラ状の治具５が活物質２に加える圧力Ｐ１より小さな値に設定される。 Referring again to FIG. 1, as shown in (c) of FIG, active material 2 applied pressure P 2 in the vertical direction from above is compressed and deformed, H indicates vertical direction, i.e. the thickness of the H A While reducing to B , the active material 2 corresponding to the volume reduced by the compression is advanced inside the hole 4. As a result, the hole 4, as shown in (d) of FIG, shrinks into a small diameter W B from the pressing process earlier diameter W A shown in (e) of FIG. At this time, the pressure P 2 applied to the active material 2 by the pressing jig 6 is set to a value smaller than the pressure P 1 applied to the active material 2 by the roller-shaped jig 5 in the hole forming step.

プレス工程の結果、電極板３の面積に関して活物質２が占めする面積が増大し、孔部４が占める面積が減少する。３次元的にも電極板３に占める活物質２の体積割合が増大し、孔部４の体積割合が減少する。活物質２の体積割合の増大は２次電池の蓄電容量を増大させる効果をもたらす。一方、プレス治具６の圧力Ｐ２を治具５の圧力Ｐ１より小さく設定しているので、プレス工程によって電極板３の厚さが過度に薄くなったり、活物質２の密度が過度に上昇したりするのを抑制することができる。 As a result of the pressing step, the area occupied by the active material 2 with respect to the area of the electrode plate 3 increases, and the area occupied by the hole 4 decreases. Also in three dimensions, the volume ratio of the active material 2 occupying the electrode plate 3 is increased, and the volume ratio of the hole 4 is decreased. An increase in the volume ratio of the active material 2 brings about an effect of increasing the storage capacity of the secondary battery. On the other hand, since the pressure P 2 of the press jig 6 is set to be smaller than the pressure P 1 of the jig 5, or become excessively thin thickness of the electrode plate 3 by the pressing process, is excessively density of the active material 2 It can suppress rising.

このようにして径を縮小した孔部４が、リチウムイオン２次電池の稼働時には、電解液を活物質に浸透させるマイクロホールとして機能する。発明者らの実験によれば、以上のプレス工程により孔部４の体積を約５０％減少させることができた。このように、この電極製造方法によれば孔部４の径を効率良く減少させることができる。   The hole 4 with the diameter reduced in this manner functions as a microhole that allows the electrolytic solution to permeate the active material when the lithium ion secondary battery is in operation. According to the inventors' experiment, the volume of the hole 4 could be reduced by about 50% by the above pressing process. Thus, according to this electrode manufacturing method, the diameter of the hole 4 can be reduced efficiently.

径ＷＢの孔部４をピン７による活物質２の塑性変形のみで形成しようとすれば、ピン７の径をＷＢに等しく設定しなければならない。しかしながら、ピン７の径を小さくするとピン７の折れやすさが二次関数的に増加する。孔部形成工程の後にプレス工程を行なうこの製造方法によれば、孔部形成工程で使用する治具５のピン７の径を小さくせずに、数十μｍという好ましい径の多数のマイクロホールを活物質２に容易に形成することができる。 If an attempt is made to form a hole portion 4 of the diameter W B pin 7 only plastic deformation of the active material 2 in accordance with, must equally set the diameter of the pin 7 to W B. However, if the diameter of the pin 7 is reduced, the ease with which the pin 7 is broken increases in a quadratic function. According to this manufacturing method in which the pressing step is performed after the hole forming step, a large number of microholes having a preferable diameter of several tens of μm are formed without reducing the diameter of the pin 7 of the jig 5 used in the hole forming step. It can be easily formed on the active material 2.

この製造方法により製造された電極板３は、プレス工程でプレス治具６を用いて活物質２を圧縮した結果、孔部４の開口部の周囲の活物質２の密度が集電箔１に近い部位の孔部４の周囲の活物質２の密度より高くなる。これは、プレス治具６の押圧面に近い位置ほど、活物質２が押しつぶされるからである。   The electrode plate 3 manufactured by this manufacturing method compresses the active material 2 by using the pressing jig 6 in the pressing process. As a result, the density of the active material 2 around the opening of the hole 4 becomes the current collecting foil 1. The density becomes higher than the density of the active material 2 around the hole 4 in the near portion. This is because the active material 2 is crushed closer to the pressing surface of the pressing jig 6.

また、プレス工程を実行することで、活物質２の凹凸が平らに均される。したがって、電極板３の活物質２の厚さを均一にすることができる。   Moreover, the unevenness | corrugation of the active material 2 is leveled flat by performing a press process. Therefore, the thickness of the active material 2 of the electrode plate 3 can be made uniform.

図４を参照して、この発明による電極の製造方法の第２の実施形態を説明する。   A second embodiment of the electrode manufacturing method according to the present invention will be described with reference to FIG.

この実施形態では、プレス工程で使用するプレス治具６の代わりにローラ状のプレス治具８を用いてプレス工程を実施する。なお、プレス治具８には、治具５のようなピン７は設けられない。プレス治具８の表面は滑らかな曲面である。   In this embodiment, the pressing process is performed using a roller-shaped pressing jig 8 instead of the pressing jig 6 used in the pressing process. Note that the press jig 8 is not provided with the pin 7 like the jig 5. The surface of the pressing jig 8 is a smooth curved surface.

プレス治具８は図に示すように、転動しつつ活物質２を押圧する。プレス治具８は第１の実施形態のプレス治具６と同じく上方から垂直に圧力Ｐ２を活物質２に加える。 As shown in the drawing, the pressing jig 8 presses the active material 2 while rolling. Add press jig 8 is a pressure P 2 perpendicularly from same upwardly press jig 6 in the first embodiment the active material 2.

この実施形態によっても、第１の実施形態と同様に、プレス工程によって孔部４を縮小させ、格別に細いピン７を用いることなく、数十μｍという好ましい径の多数のマイクロホールを活物質２に容易に形成することができる。また、ローラ状のプレス治具８によって活物質２の表面の凹凸が均されるので、電極板３の活物質２の厚さを均一にすることができる。   Also in this embodiment, as in the first embodiment, the hole 4 is reduced by a pressing process, and a large number of microholes having a preferable diameter of several tens of μm are formed without using the extremely thin pins 7 in the active material 2. Can be easily formed. Moreover, since the unevenness of the surface of the active material 2 is leveled by the roller-shaped press jig 8, the thickness of the active material 2 of the electrode plate 3 can be made uniform.

以上のように、この発明の第１の実施形態及び第２の実施形態による電池用電極の製造方法は、数十μｍの径の数多くのマイクロホールを有する、活物質の体積密度の高い電極板３の製造を可能とする。このようにして製造された電極板３を所定の寸法に切断することで、高性能の電極を製造することができる。製造された電極は孔部４の開口部の周囲の活物質２の密度が、集電箔１に近い部位の孔部４の周囲の活物質２の密度より高いのが特徴である。この特徴は、孔部４の深部においてリチウムイオンの活物質２への高い浸透性を確保するうえで好ましい。   As described above, the battery electrode manufacturing method according to the first embodiment and the second embodiment of the present invention is an electrode plate having a large volume of active material having a large number of microholes with a diameter of several tens of μm. 3 can be manufactured. A high-performance electrode can be manufactured by cutting the electrode plate 3 thus manufactured into a predetermined size. The manufactured electrode is characterized in that the density of the active material 2 around the opening of the hole 4 is higher than the density of the active material 2 around the hole 4 near the current collector foil 1. This feature is preferable for ensuring high penetration of lithium ions into the active material 2 in the deep part of the hole 4.

さらに、この電極を用いてリチウムイオン２次電池を製造することで、リチウムイオン２次電池の蓄電性能や放電性能を強化することができる。   Furthermore, by manufacturing a lithium ion secondary battery using this electrode, the storage performance and discharge performance of the lithium ion secondary battery can be enhanced.

以上の実施形態において、ピン７が孔部４に対応する突起を構成する。   In the above embodiment, the pin 7 constitutes a protrusion corresponding to the hole 4.

以上のように、この発明をいくつかの特定の実施形態を通じて説明して来たが、この発明は上記の各実施形態に限定されるものではない。当業者にとっては、特許請求の範囲でこれらの実施形態にさまざまな修正あるいは変更を加えることが可能である。   As described above, the present invention has been described through some specific embodiments, but the present invention is not limited to the above embodiments. Those skilled in the art can make various modifications or changes to these embodiments within the scope of the claims.

例えば、上記の各実施異形態では電極板形成工程に引き続いて孔部形成工程を実行している。これは、孔部４の形成を容易にするうえで好ましい。一方、集電箔１に活物質２を塗布した後に治具を用いて圧縮することで電極板３を得る場合もある。このようにして既に圧縮力を加えられた電極板３にマイクロホールを形成する場合も、この発明による電極の形成方法を適用することで、マイクロホールの小径化に関して相応の好ましい効果を得ることができる。言い換えれば、既成の電極板３にマイクロホールを形成して電極を製造する場合にも、この発明は有効である。   For example, in each of the above embodiments, the hole forming step is executed subsequent to the electrode plate forming step. This is preferable for facilitating the formation of the hole 4. On the other hand, the electrode plate 3 may be obtained by applying the active material 2 to the current collector foil 1 and then compressing it using a jig. Even in the case where microholes are formed in the electrode plate 3 to which a compressive force has already been applied in this way, by applying the electrode forming method according to the present invention, it is possible to obtain a correspondingly favorable effect with respect to the reduction in the diameter of the microholes. it can. In other words, the present invention is also effective when an electrode is manufactured by forming a microhole in the existing electrode plate 3.

１ 集電箔
２ 活物質
３ 電極板
４ 孔部
５ 治具
６ プレス治具
７ ピン
８ プレス治具 DESCRIPTION OF SYMBOLS 1 Current collector foil 2 Active material 3 Electrode plate 4 Hole part 5 Jig 6 Press jig 7 Pin 8 Press jig

Claims (7)

電極板に厚さ方向の複数の微細な孔部を形成する電極の製造方法において、
集電箔に活物質を塗布して電極板を形成する電極板形成工程と、
前記電極板に孔部を形成する孔部形成工程と、
前記孔部を形成した前記電極板を厚さ方向に圧縮するプレス工程と、
を含むことを特徴とする、電池用電極の製造方法。 In the electrode manufacturing method for forming a plurality of fine holes in the thickness direction in the electrode plate,
An electrode plate forming step of forming an electrode plate by applying an active material to a current collector foil;
A hole forming step of forming a hole in the electrode plate;
A pressing step of compressing the electrode plate in which the hole is formed in a thickness direction;
The manufacturing method of the electrode for batteries characterized by including. 前記孔部形成工程は、前記集電箔に塗布された前記活物質に前記孔部に対応する突起を所定圧力でプレスする工程を含むことを特徴とする、請求項１に記載の電池用電極の製造方法。   2. The battery electrode according to claim 1, wherein the hole forming step includes a step of pressing a protrusion corresponding to the hole on the active material applied to the current collector foil with a predetermined pressure. Manufacturing method. 前記プレス工程で電極板に加えられる圧力は前記所定圧力より低いことを特徴とする請求項２に記載の電池用電極の製造方法。   The method for manufacturing a battery electrode according to claim 2, wherein the pressure applied to the electrode plate in the pressing step is lower than the predetermined pressure. 前記プレス工程により、前記孔部の径が５０％以下に縮小することを特徴とする、請求項１から３のいずれかに記載の電池用電極の製造方法。   The method for manufacturing a battery electrode according to any one of claims 1 to 3, wherein the diameter of the hole portion is reduced to 50% or less by the pressing step. 前記電極板形成工程は、前記集電箔に塗布された前記活物質を圧縮する工程を含むことを特徴とする、請求項１から４のいずれかに記載の電池用電極の製造方法。   The method for manufacturing a battery electrode according to claim 1, wherein the electrode plate forming step includes a step of compressing the active material applied to the current collector foil. 電極板に厚さ方向の複数の微細な孔部を形成した電極において、
集電箔に活物質を塗布して形成された電極板と、
前記電極板に厚さ方向に形成された複数の微細な孔部と、
を備えるとともに、
前記複数の微細な孔部の開口側の活物質の密度が、前記集電箔側の活物質の密度より高いことを特徴とする、電池用電極。 In the electrode formed with a plurality of fine holes in the thickness direction on the electrode plate,
An electrode plate formed by applying an active material to a current collector foil;
A plurality of fine holes formed in the electrode plate in the thickness direction;
With
The battery electrode, wherein the density of the active material on the opening side of the plurality of fine holes is higher than the density of the active material on the current collector foil side. 請求項６に記載の電池用電極を用いて構成されることを特徴とする、二次電池。   A secondary battery comprising the battery electrode according to claim 6.
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