JP5668636B2 - Method for manufacturing circuit connection structure - Google Patents

Method for manufacturing circuit connection structure Download PDF

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Publication number
JP5668636B2
JP5668636B2 JP2011173136A JP2011173136A JP5668636B2 JP 5668636 B2 JP5668636 B2 JP 5668636B2 JP 2011173136 A JP2011173136 A JP 2011173136A JP 2011173136 A JP2011173136 A JP 2011173136A JP 5668636 B2 JP5668636 B2 JP 5668636B2
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Japan
Prior art keywords
circuit
connection
circuit connection
mass
film
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JP2011173136A
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JP2012067281A (en
Inventor
立澤　貴
貴 立澤
小林　宏治
宏治 小林
雅英 久米
雅英 久米
耕太郎 関
耕太郎 関
陽介 相澤
陽介 相澤
伊藤　彰浩
彰浩 伊藤
藤縄　貢
貢 藤縄
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Showa Denko Materials Co Ltd
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Hitachi Chemical Co Ltd
Showa Denko Materials Co Ltd
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Application filed by Hitachi Chemical Co Ltd, Showa Denko Materials Co Ltd filed Critical Hitachi Chemical Co Ltd
Priority to JP2011173136A priority Critical patent/JP5668636B2/en
Priority to KR1020110083861A priority patent/KR101227358B1/en
Priority to PCT/JP2011/068982 priority patent/WO2012026470A1/en
Priority to CN2011102511296A priority patent/CN102417794B/en
Priority to TW100130042A priority patent/TWI436709B/en
Publication of JP2012067281A publication Critical patent/JP2012067281A/en
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Publication of JP5668636B2 publication Critical patent/JP5668636B2/en
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    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/06—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances
    • H01B1/12—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors mainly consisting of other non-metallic substances organic substances
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  • Engineering & Computer Science (AREA)
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  • Chemical & Material Sciences (AREA)
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  • Spectroscopy & Molecular Physics (AREA)
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  • Physics & Mathematics (AREA)
  • Combinations Of Printed Boards (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Electric Connection Of Electric Components To Printed Circuits (AREA)
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  • Adhesive Tapes (AREA)
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Description

本発明は、回路接続材料、これを用いた回路部材の接続方法、回路接続構造体、及び、回路接続構造体の製造方法に関する。   The present invention relates to a circuit connection material, a method for connecting circuit members using the same, a circuit connection structure, and a method for manufacturing the circuit connection structure.

従来、相対向する回路を加熱、加圧し加圧方向の電極間を電気的に接続する回路接続材料として、異方導電性接着フィルムが知られている。例えば、エポキシ系接着剤やアクリル系接着剤に導電粒子を分散させた異方導電性接着フィルムが知られている。かかる異方導電性接着フィルムは、主に液晶ディスプレイ（以下、「ＬＣＤ」とする。）を駆動させる半導体が搭載されたＴＣＰ（Ｔａｐｅ Ｃａｒｒｉｅｒ Ｐａｃｋａｇｅ）又はＣＯＦ（Ｃｈｉｐ Ｏｎ Ｆｌｅｘ）とＬＣＤパネルとの電気的接続、あるいは、ＴＣＰ又はＣＯＦとプリント配線板との電気的接続に広く使用されている。   Conventionally, anisotropic conductive adhesive films are known as circuit connection materials for heating and pressurizing opposing circuits to electrically connect electrodes in the pressurizing direction. For example, an anisotropic conductive adhesive film in which conductive particles are dispersed in an epoxy adhesive or an acrylic adhesive is known. Such an anisotropic conductive adhesive film is mainly composed of a TCP (Tape Carrier Package) or COF (Chip On Flex) on which a semiconductor for driving a liquid crystal display (hereinafter referred to as “LCD”) is mounted and the LCD panel. Widely used for electrical connection or electrical connection between a TCP or COF and a printed wiring board.

また、最近では、半導体をフェイスダウンで直接ＬＣＤパネルやプリント配線板に実装する場合でも、従来のワイヤーボンディング法ではなく、薄型化や狭ピッチ接続に有利なフリップチップ実装が採用されている。フリップチップ実装においても、異方導電性接着フィルムが回路接続材料として用いられている（例えば、特許文献１〜４参照）。   Recently, even when a semiconductor is directly mounted on an LCD panel or a printed wiring board face down, flip chip mounting, which is advantageous for thinning and narrow pitch connection, has been adopted instead of the conventional wire bonding method. Also in flip chip mounting, anisotropic conductive adhesive films are used as circuit connection materials (see, for example, Patent Documents 1 to 4).

特開昭５９−１２０４３６号公報JP 59-120436 A 特開昭６０−１９１２２８号公報JP-A-60-191228 特開平０１−２５１７８７号公報Japanese Patent Laid-Open No. 01-251787 特開平０７−０９０２３７号公報Japanese Patent Laid-Open No. 07-090237

異方導電性接着フィルムを用いた回路部材の接続では、加熱及び加圧により、対向配置された電極の間に導電粒子が挟まれ、電極間の導通が確保される。回路部材の接続工程では、接着剤成分を流動させるための十分な熱と、導電粒子を電極に密着させるための十分な圧力とが必要となる。熱硬化樹脂系の回路接続材料では、硬化剤が十分に反応するための温度まで加熱するために、比較的高い接続温度が必要である。また、回路部材の接続には、接着剤成分の硬化に必要な熱的ストレスと、粒子を電極間で押し潰すための圧力ストレスとを要する。そのため、回路接続材料の接続は、通常３ＭＰａ以上の圧力で行われる。これらのストレスは、被着体にダメージを与え、表示不良や信頼性の低下の原因となりやすい。特に、被着体にＰＥＴフィルムを用いるタッチパネル用途等では、圧力ストレスを低減することが求められている。   In connection of circuit members using an anisotropic conductive adhesive film, conductive particles are sandwiched between opposed electrodes by heating and pressurization, and conduction between the electrodes is ensured. In the circuit member connecting step, sufficient heat for flowing the adhesive component and sufficient pressure for bringing the conductive particles into close contact with the electrode are required. In a thermosetting resin-based circuit connection material, a relatively high connection temperature is required to heat the thermosetting resin to a temperature at which the curing agent sufficiently reacts. Further, the connection of the circuit members requires thermal stress necessary for curing the adhesive component and pressure stress for crushing the particles between the electrodes. Therefore, the connection of the circuit connection material is usually performed at a pressure of 3 MPa or more. These stresses tend to cause damage to the adherend, resulting in poor display and reduced reliability. In particular, in touch panel applications using a PET film as an adherend, it is required to reduce pressure stress.

ラジカル硬化系の回路接続材料の登場により、低温・短時間での接続が可能となりつつある。しかし、従来のラジカル硬化系の回路接続材料では、１．５ＭＰａ以下の低圧条件で接続した場合に、接着剤成分の流動性が不足し、導通不良や圧痕不良が起こりやすい。   With the advent of radical-curing circuit connection materials, low-temperature and short-time connections are becoming possible. However, in a conventional radical curing system circuit connecting material, when connected under a low pressure condition of 1.5 MPa or less, the fluidity of the adhesive component is insufficient, and continuity failure and indentation failure are likely to occur.

そこで本発明は、上記事情に鑑み、回路接続時の圧力を従来よりも低くした場合でも、圧痕の形成及び接続抵抗が良好である接続を可能とする回路接続材料、その回路接続材料を用いた回路部材の接続方法、回路接続構造体、及び、回路接続構造体の製造方法を提供することを目的とする。   Therefore, in view of the above circumstances, the present invention uses a circuit connection material that enables connection with formation of indentations and good connection resistance, even when the pressure at the time of circuit connection is lower than conventional pressure, and the circuit connection material. It aims at providing the connection method of a circuit member, a circuit connection structure, and the manufacturing method of a circuit connection structure.

回路接続材料を用いた回路接続では、接続を行う回路電極で回路接続材料を挟み、被着材の側から高温に加熱した圧着棒を押し当てる。圧着棒により加熱された回路接続材料は、流動性を示し、接続回路間における不要な接着剤成分が接続部外に押し出される。そして、対向する電極間のスペースが、導電粒子の直径よりも狭くなると、導電粒子が対抗する電極に押し潰され、電極間の導通が確保される。したがって、より低い圧力条件で回路接続を行う場合、十分に高い流動性を示す回路接続材料を選択する必要がある。   In the circuit connection using the circuit connection material, the circuit connection material is sandwiched between the circuit electrodes to be connected, and a crimping rod heated to a high temperature is pressed from the side of the adherend. The circuit connection material heated by the crimping rod exhibits fluidity, and unnecessary adhesive components between the connection circuits are pushed out of the connection portion. When the space between the opposing electrodes becomes narrower than the diameter of the conductive particles, the conductive particles are crushed by the opposing electrodes, and conduction between the electrodes is ensured. Therefore, when circuit connection is performed under a lower pressure condition, it is necessary to select a circuit connection material that exhibits sufficiently high fluidity.

本発明者らは、ラジカル重合系の回路接続材料の構成成分であるフィルム性付与ポリマーに着目し、鋭意検討を重ねた結果、回路接続時の圧力が低くとも圧痕の形成及び接続抵抗が良好である接続を可能とする回路接続材料を見出した。   The inventors of the present invention focused on the film property-imparting polymer, which is a component of the radical polymerization system circuit connection material, and as a result of intensive studies, the formation of indentation and connection resistance were good even when the pressure during circuit connection was low. The circuit connection material which enables a certain connection was discovered.

すなわち本発明は、第一の基板の主面上に第一の回路電極が形成された第一の回路部材と、第二の基板の主面上に第二の回路電極が形成された第二の回路部材との間に介在させ、加熱及び加圧により第一の回路電極及び第二の回路電極を対向配置された状態で電気的に接続するための回路接続材料であって、加圧は１．５ＭＰａ以下で行われ、フィルム性付与ポリマー、ラジカル重合性物質、ラジカル重合開始剤及び導電粒子を含有し、フィルム性付与ポリマーは、ガラス転移温度７０℃未満のポリマーを含み、ガラス転移温度７０℃未満のポリマーの配合量がフィルム性付与ポリマー及びラジカル重合性物質の総量を基準として３０〜７０質量％である、回路接続材料を提供する。   That is, the present invention provides a first circuit member in which a first circuit electrode is formed on a main surface of a first substrate, and a second circuit member in which a second circuit electrode is formed on a main surface of a second substrate. A circuit connecting material for electrically connecting the first circuit electrode and the second circuit electrode in a state of being opposed to each other by heating and pressurizing, The process is performed at 1.5 MPa or less and contains a film property-imparting polymer, a radical polymerizable substance, a radical polymerization initiator, and conductive particles. The film property-imparting polymer includes a polymer having a glass transition temperature of less than 70 ° C. Provided is a circuit connecting material in which the blending amount of the polymer having a temperature lower than 0 ° C. is 30 to 70% by mass based on the total amount of the film-imparting polymer and the radical polymerizable substance.

ここで、フィルム性付与ポリマーは、ガラス転移温度５０℃以上７０℃未満のポリマーを、フィルム性付与ポリマーの全量を基準として５０質量％以上含むことが好ましい。これにより、上記接続を一層良好に行うことができる。   Here, the film property-imparting polymer preferably contains a polymer having a glass transition temperature of 50 ° C. or more and less than 70 ° C. in an amount of 50% by mass or more based on the total amount of the film property imparting polymer. Thereby, the said connection can be performed still more favorably.

更に、ラジカル重合性物質は、２官能以下のラジカル重合性物質を含み、該２官能以下のラジカル重合性物質の配合量が、ラジカル重合性物質の全量を基準として５０質量％以上であることが好ましい。これにより、上記回路接続材料の流動性をより向上することができる。   Furthermore, the radically polymerizable substance includes a bifunctional or lower radical polymerizable substance, and the blending amount of the bifunctional or lower radical polymerizable substance is 50% by mass or more based on the total amount of the radical polymerizable substance. preferable. Thereby, the fluidity | liquidity of the said circuit connection material can be improved more.

また、本発明は、第一の基板の主面上に第一の回路電極が形成された第一の回路部材と、第二の基板の主面上に第二の回路電極が形成された第二の回路部材と、第一の回路部材及び第二の回路部材の間に配置された上記回路接続材料とを第一の回路電極と第二の回路電極とが対向配置された状態で加熱及び加圧して、第一の回路電極と第二の回路電極とを電気的に接続する回路部材の接続方法であって、加圧が１．５ＭＰａ以下で行われる回路部材の接続方法を提供する。このような方法で接続された接続構造は、圧痕及び接続抵抗が良好である。   The present invention also provides a first circuit member in which a first circuit electrode is formed on a main surface of a first substrate, and a second circuit electrode in which a second circuit electrode is formed on a main surface of a second substrate. Heating the second circuit member and the circuit connecting material disposed between the first circuit member and the second circuit member in a state where the first circuit electrode and the second circuit electrode are opposed to each other. A circuit member connection method for applying pressure and electrically connecting a first circuit electrode and a second circuit electrode, wherein the circuit member is connected at a pressure of 1.5 MPa or less. The connection structure connected by such a method has good indentation and connection resistance.

また、本発明は、第一の基板の主面上に第一の回路電極が形成された第一の回路部材、及び、第二の基板の主面上に第二の回路電極が形成された第二の回路部材の間に上記回路接続材料を配置する工程と、第一の回路電極と第二の回路電極とが対向配置された状態で加熱及び加圧して、第一の回路電極と第二の回路電極とを電気的に接続する工程と、を備え、加圧が１．５ＭＰａ以下で行われる、回路接続構造体の製造方法を提供する。このような製造方法によれば、圧痕の形成及び接続抵抗が良好な回路接続構造体を得ることができる。   Further, according to the present invention, the first circuit member in which the first circuit electrode is formed on the main surface of the first substrate, and the second circuit electrode is formed on the main surface of the second substrate. The step of disposing the circuit connecting material between the second circuit members, and heating and pressurizing the first circuit electrode and the second circuit electrode in a state where the first circuit electrode and the second circuit electrode are opposed to each other. And a step of electrically connecting the two circuit electrodes, and a method for producing a circuit connection structure is provided, wherein the pressurization is performed at 1.5 MPa or less. According to such a manufacturing method, it is possible to obtain a circuit connection structure with good indentation formation and connection resistance.

また、本発明は、上記製造方法により製造された回路接続構造体を提供する。このような回路接続構造体は、圧痕の形成及び接続抵抗が良好である。   Moreover, this invention provides the circuit connection structure manufactured by the said manufacturing method. Such a circuit connection structure has good indentation and connection resistance.

本発明によれば、回路接続時の圧力を従来よりも低くした場合でも、圧痕の形成及び接続抵抗が良好である接続を可能とする回路接続材料、その回路接続材料用いた回路部材の接続方法、回路接続構造体、及び、回路接続構造体の製造方法を提供することができる。   According to the present invention, even when the pressure at the time of circuit connection is lower than that of the prior art, the circuit connection material that enables the formation of the indentation and the connection resistance is good, and the circuit member connection method using the circuit connection material The circuit connection structure and the method for manufacturing the circuit connection structure can be provided.

フィルム状の回路接続材料の一実施形態を示す断面図である。It is sectional drawing which shows one Embodiment of a film-form circuit connection material. 本発明に係る回路接続材料で接続された接続構造の好適な一実施形態を示す模式断面図である。It is a schematic cross section which shows suitable one Embodiment of the connection structure connected with the circuit connection material which concerns on this invention. 本発明の回路部材の接続方法の一実施形態を概略断面図により示す工程図である。It is process drawing which shows one Embodiment of the connection method of the circuit member of this invention with a schematic sectional drawing. 実施例で観察した回路接続構造体の圧痕の写真である。It is the photograph of the indentation of the circuit connection structure observed in the Example. フィルム状回路接続材料を用いて回路部材を接続する前の状態を示す平面図である。It is a top view which shows the state before connecting a circuit member using a film-form circuit connection material.

以下、必要に応じて図面を参照しつつ、本発明の好適な実施形態について詳細に説明する。ただし、本発明は以下の実施形態に限定されるものではない。なお、図面中、同一要素には同一符号を付すこととし、重複する説明は省略する。また、上下左右等の位置関係は、特に断らない限り、図面に示す位置関係に基づくものとする。さらに、図面の寸法比率は図示の比率に限られるものではない。また、本明細書における「（メタ）アクリレート」とは、「アクリレート」及びそれに対応する「メタクリレート」を意味し、「（メタ）アクリロキシ」とは、「アクリロキシ」及びそれに対応する「メタクリロキシ」を意味する。   Hereinafter, preferred embodiments of the present invention will be described in detail with reference to the drawings as necessary. However, the present invention is not limited to the following embodiments. In the drawings, the same elements are denoted by the same reference numerals, and redundant description is omitted. Further, the positional relationship such as up, down, left and right is based on the positional relationship shown in the drawings unless otherwise specified. Further, the dimensional ratios in the drawings are not limited to the illustrated ratios. In the present specification, “(meth) acrylate” means “acrylate” and its corresponding “methacrylate”, and “(meth) acryloxy” means “acryloxy” and its corresponding “methacryloxy”. To do.

（回路接続材料）
本発明の回路接続材料は、接着剤成分と、導電粒子とを含有するものである。本発明において接着剤成分とは、回路接続材料の構成材料のうち、導電粒子以外の全ての材料を含むものを意味する。本発明の回路接続材料は、接着剤成分として、フィルム性付与ポリマー、ラジカル重合性物質及びラジカル重合開始剤を含む。また、接着剤成分は、必要に応じて、ハイドロキノン、メチルエーテルハイドロキノン類等の重合禁止剤を含んでもよい。 (Circuit connection material)
The circuit connection material of the present invention contains an adhesive component and conductive particles. In the present invention, the adhesive component means a constituent material of the circuit connection material that includes all materials other than the conductive particles. The circuit connection material of this invention contains a film property provision polymer, a radically polymerizable substance, and a radical polymerization initiator as an adhesive component. Further, the adhesive component may contain a polymerization inhibitor such as hydroquinone or methyl ether hydroquinone as necessary.

フィルム性付与ポリマーは、ガラス転移温度（以下、「Ｔｇ」と略記する。）が７０℃未満のポリマーを含む。このようなポリマーとしては、例えば、ポリイミド樹脂、ポリアミド樹脂、（メタ）アクリル樹脂、ポリエステルウレタン樹脂、ポリウレタン樹脂、フェノキシ樹脂、ポリビニルブチラール樹脂が挙げられる。これらの中でも、好ましい例としては、ポリエステルウレタン樹脂、ポリウレタン樹脂、フェノキシ樹脂が挙げられる。これらは１種を単独で又は２種以上を混合して用いることができる。   The film property-imparting polymer includes a polymer having a glass transition temperature (hereinafter abbreviated as “Tg”) of less than 70 ° C. Examples of such polymers include polyimide resins, polyamide resins, (meth) acrylic resins, polyester urethane resins, polyurethane resins, phenoxy resins, and polyvinyl butyral resins. Among these, preferable examples include polyester urethane resins, polyurethane resins, and phenoxy resins. These can be used individually by 1 type or in mixture of 2 or more types.

ポリマーのＴｇは、構成するモノマーの構造や共重合するモノマーのモル比を調整することで目的の範囲のものを合成することができる。Ｔｇを上げるためにはベンゼン環やナフタレン環等の剛直な骨格を持つモノマーをモノマー成分として導入することができる。Ｔｇを下げるためには、脂肪族系のモノマーをモノマー成分として導入することができる。   The Tg of the polymer can be synthesized within the target range by adjusting the structure of the constituent monomers and the molar ratio of the monomers to be copolymerized. In order to increase Tg, a monomer having a rigid skeleton such as a benzene ring or a naphthalene ring can be introduced as a monomer component. In order to lower Tg, an aliphatic monomer can be introduced as a monomer component.

ポリエステルウレタン樹脂は、例えば、ポリエステルポリオールと、ジイソシアネートとの反応により得られる。ジイソシアネートとしては、２，４−トリレンジイソシアネート（ＴＤＩ）、４，４’−ジフェニルメタンジイソシアネート（ＭＤＩ）、１，６−ヘキサメチレンジイソシアネート（ＨＤＩ）、イソホロンジイソシアネート（ＩＰＤＩ）等の芳香族、脂環族、又は脂肪族のジイソシアネートが好適に用いられる。   Polyester urethane resin is obtained by reaction of polyester polyol and diisocyanate, for example. Diisocyanates include 2,4-tolylene diisocyanate (TDI), 4,4′-diphenylmethane diisocyanate (MDI), 1,6-hexamethylene diisocyanate (HDI), isophorone diisocyanate (IPDI), and other aromatic and alicyclic groups. Or aliphatic diisocyanates are preferably used.

ポリエステルポリオールは、例えば、ジカルボン酸とジオールとの反応により得られる。ジカルボン酸としては、テレフタル酸、イソフタル酸、アジピン酸、セバチン酸等の芳香族や脂肪族ジカルボン酸が好ましい。ジオールとしては、エチレングリコール、プロピレングリコール、１，４−ブタンジオール、ヘキサンジオール、ネオペンチルグリコール、ジエチレングリコール、トリエチレングリコールのようなグリコール類が好ましい。   The polyester polyol is obtained, for example, by a reaction between a dicarboxylic acid and a diol. As the dicarboxylic acid, aromatic or aliphatic dicarboxylic acids such as terephthalic acid, isophthalic acid, adipic acid, and sebacic acid are preferable. As the diol, glycols such as ethylene glycol, propylene glycol, 1,4-butanediol, hexanediol, neopentyl glycol, diethylene glycol, and triethylene glycol are preferable.

ポリエステルウレタン樹脂は、接着強度を向上させるためにアニオン性を有してもよい。アニオン性を有するポリエステルウレタン樹脂は、ポリエステルポリオールとジイソシアネートとの反応の際に、側鎖にスルホン酸基やカルボキシル基を有するジオールやジアミン類を共重合することにより得られる。   The polyester urethane resin may have an anionic property in order to improve the adhesive strength. The polyester urethane resin having an anionic property is obtained by copolymerizing a diol or diamine having a sulfonic acid group or a carboxyl group in the side chain in the reaction of the polyester polyol and the diisocyanate.

ポリエステルウレタン樹脂は、ベンゼン環等を含む芳香族基や、シクロヘキサン環等を含む環状脂肪族基を有することが好ましい。   The polyester urethane resin preferably has an aromatic group containing a benzene ring or the like, or a cyclic aliphatic group containing a cyclohexane ring or the like.

ポリエステルウレタン樹脂は、ラジカル重合性を有する不飽和二重結合及び／又はエポキシ基を有していてもよい。これにより、回路接続材料を硬化するときに、接着剤組成物中のエポキシ樹脂やラジカル重合性化合物と反応して、回路接続材料の硬化物の弾性率や耐熱性が向上する。   The polyester urethane resin may have an unsaturated double bond and / or an epoxy group having radical polymerizability. Thereby, when hardening a circuit connection material, it reacts with the epoxy resin and radically polymerizable compound in an adhesive composition, and the elasticity modulus and heat resistance of the hardened | cured material of a circuit connection material improve.

ポリエステルウレタン樹脂は、２種類以上を混合して使用することができる。例えば、芳香族ポリエステルポリオールと脂肪族ジイソシアネートとの反応により得られるものと、脂肪族ポリエステルポリオールと芳香族ジイソシアネートとの反応により得られるものとを組み合せて用いてもよい。   Two or more types of polyester urethane resins can be mixed and used. For example, you may use combining what is obtained by reaction of aromatic polyester polyol and aliphatic diisocyanate, and what is obtained by reaction of aliphatic polyester polyol and aromatic diisocyanate.

フィルム性付与ポリマーは、重量平均分子量が５０００〜１０００００であることが好ましい。重量平均分子量が５０００未満であると、フィルム状に成形する際のフィルム形成性が低下する傾向にあり、重量平均分子量が１０００００を超えると、溶剤への溶解性や相溶性が低下して、フィルム状に成形するための塗工液を調製することが困難となる傾向にある。   The film property-imparting polymer preferably has a weight average molecular weight of 5,000 to 100,000. If the weight average molecular weight is less than 5,000, the film formability when formed into a film tends to be reduced, and if the weight average molecular weight exceeds 100,000, the solubility in the solvent and the compatibility are reduced. It tends to be difficult to prepare a coating liquid for forming into a shape.

本実施形態において、重量平均分子量とは、下記表１に示す条件に従ってゲル浸透クロマトグラフ（ＧＰＣ）より標準ポリスチレンによる検量線を用いて測定した値をいう。   In the present embodiment, the weight average molecular weight refers to a value measured from a gel permeation chromatograph (GPC) using a standard polystyrene calibration curve according to the conditions shown in Table 1 below.

Ｔｇ７０℃未満のポリマーの配合量は、フィルム性付与ポリマーとラジカル重合性物質との総量を基準として、３０〜７０質量％であり、５０〜７０質量％であることが好ましく、４０〜７０質量％であることがより好ましく、５５〜６５重量％であることが更に好ましい。   The blending amount of the polymer having a Tg of less than 70 ° C. is 30 to 70% by mass, preferably 50 to 70% by mass, and preferably 40 to 70% by mass based on the total amount of the film-imparting polymer and the radical polymerizable substance. More preferably, it is more preferably 55 to 65% by weight.

上記フィルム性付与ポリマーは、Ｔｇ５０℃以上７０℃未満のポリマーを含むことが好ましい。該Ｔｇ５０℃以上７０℃未満のポリマーが、フィルム性付与ポリマーの全量を基準として５０質量％以上含まれることが好ましく、６０質量％以上がより好ましく、７５質量％以上含まれることが更に好ましい。また、フィルム性付与ポリマーは、Ｔｇが異なる２種類以上のポリマーを混合して使用することができる。例えば、Ｔｇが５０℃以上７０℃未満のポリマーと、Ｔｇが１０℃以上３０℃未満のポリマーとを混合して使用することができる。   The film property-imparting polymer preferably contains a polymer having a Tg of 50 ° C. or more and less than 70 ° C. The polymer having a Tg of 50 ° C. or more and less than 70 ° C. is preferably contained in an amount of 50% by mass or more, more preferably 60% by mass or more, and still more preferably 75% by mass or more based on the total amount of the film-imparting polymer. The film property-imparting polymer can be used by mixing two or more kinds of polymers having different Tg. For example, a polymer having a Tg of 50 ° C. or more and less than 70 ° C. and a polymer having a Tg of 10 ° C. or more and less than 30 ° C. can be mixed and used.

本実施形態の回路接続材料は、本発明の奏する効果を逸脱しない範囲で、フィルム性付与ポリマーとしてＴｇ７０℃以上のポリマーを併用することができる。この場合、その配合量は、フィルム性付与ポリマーとラジカル重合性物質との総量を基準として１５質量％以下であることが好ましい。   In the circuit connection material of the present embodiment, a polymer having a Tg of 70 ° C. or more can be used in combination as a film-imparting polymer without departing from the effects of the present invention. In this case, the blending amount is preferably 15% by mass or less based on the total amount of the film-imparting polymer and the radical polymerizable substance.

ラジカル重合性物質は、ラジカルにより重合する官能基を有する物質であり、例えば、（メタ）アクリレート、マレイミド化合物等が挙げられる。   The radically polymerizable substance is a substance having a functional group that is polymerized by radicals, and examples thereof include (meth) acrylates and maleimide compounds.

ラジカル重合性物質としては、２官能以下（すなわち単官能又は２官能）のラジカル重合性物質を含むことが好ましい。その具体例として、（メタ）アクリレートとしては、例えば、ウレタン（メタ）アクリレート、メチル（メタ）アクリレート、エチル（メタ）アクリレート、イソプロピル（メタ）アクリレート、イソブチル（メタ）アクリレート、エチレングリコールジ（メタ）アクリレート、ジエチレングリコールジ（メタ）アクリレート、トリエチレングリコールジ（メタ）アクリレート、２−ヒドロキシ−１，３−ジ（メタ）アクリロキシプロパン、２，２−ビス〔４−（（メタ）アクリロキシメトキシ）フェニル〕プロパン、２，２−ビス〔４−（（メタ）アクリロキシポリエトキシ）フェニル〕プロパン、ジシクロペンテニル（メタ）アクリレート、トリシクロデカニル（メタ）アクリレート、ビス（（メタ）アクリロキシエチル）イソシアヌレートが挙げられる。   The radical polymerizable substance preferably includes a bifunctional or lower (ie monofunctional or bifunctional) radical polymerizable substance. Specific examples thereof include (meth) acrylates such as urethane (meth) acrylate, methyl (meth) acrylate, ethyl (meth) acrylate, isopropyl (meth) acrylate, isobutyl (meth) acrylate, and ethylene glycol di (meth). Acrylate, diethylene glycol di (meth) acrylate, triethylene glycol di (meth) acrylate, 2-hydroxy-1,3-di (meth) acryloxypropane, 2,2-bis [4-((meth) acryloxymethoxy) Phenyl] propane, 2,2-bis [4-((meth) acryloxypolyethoxy) phenyl] propane, dicyclopentenyl (meth) acrylate, tricyclodecanyl (meth) acrylate, bis ((meth) acryloxyethyl) ) Isocyanurate Door and the like.

マレイミド化合物としては、分子中にマレイミド基を少なくとも２個以上含有するものが好ましく、例えば、１−メチル−２，４−ビスマレイミドベンゼン、Ｎ，Ｎ’−ｍ−フェニレンビスマレイミド、Ｎ，Ｎ’−ｐ−フェニレンビスマレイミド、Ｎ，Ｎ’−ｍ−トルイレンビスマレイミド、Ｎ，Ｎ’−４，４−ビフェニレンビスマレイミド、Ｎ，Ｎ’−４，４−（３，３’−ジメチル−ビフェニレン）ビスマレイミド、Ｎ，Ｎ’−４，４−（３，３’−ジメチルジフェニルメタン）ビスマレイミド、Ｎ，Ｎ’−４，４−（３，３−ジエチルジフェニルメタン）ビスマレイミド、Ｎ，Ｎ’−４，４−ジフェニルメタンビスマレイミド、Ｎ，Ｎ’−４，４−ジフェニルプロパンビスマレイミド、Ｎ，Ｎ’−４，４−ジフェニルエーテルビスマレイミド、Ｎ，Ｎ’−３，３’−ジフェニルスルホンビスマレイミド、２，２−ビス［４−（４−マレイミドフェノキシ）フェニル］プロパン、２，２−ビス［３−ｓ−ブチル−４，８−（４−マレイミドフェノキシ）フェニル］プロパン、１，１−ビス［４−（４−マレイミドフェノキシ）フェニル］デカン、４，４’−シクロヘキシリデン−ビス［１−（４−マレイミドフェノキシ）−２−シクロヘキシル］ベンゼン、２，２−ビス［４−（４−マレイミドフェノキシ）フェニル］ヘキサフルオロプロパンが挙げられる。これらはアリルフェノール、アリルフェニルエーテル、安息香酸アリル等のアリル化合物と組み合わせて用いてもよい。   As the maleimide compound, those containing at least two maleimide groups in the molecule are preferable. For example, 1-methyl-2,4-bismaleimidebenzene, N, N′-m-phenylenebismaleimide, N, N ′ -P-phenylene bismaleimide, N, N'-m-toluylene bismaleimide, N, N'-4,4-biphenylene bismaleimide, N, N'-4,4- (3,3'-dimethyl-biphenylene ) Bismaleimide, N, N′-4,4- (3,3′-dimethyldiphenylmethane) bismaleimide, N, N′-4,4- (3,3-diethyldiphenylmethane) bismaleimide, N, N′— 4,4-diphenylmethane bismaleimide, N, N′-4,4-diphenylpropane bismaleimide, N, N′-4,4-diphenyl ether bismale N, N'-3,3'-diphenylsulfone bismaleimide, 2,2-bis [4- (4-maleimidophenoxy) phenyl] propane, 2,2-bis [3-s-butyl-4,8 -(4-maleimidophenoxy) phenyl] propane, 1,1-bis [4- (4-maleimidophenoxy) phenyl] decane, 4,4'-cyclohexylidene-bis [1- (4-maleimidophenoxy) -2 -Cyclohexyl] benzene, 2,2-bis [4- (4-maleimidophenoxy) phenyl] hexafluoropropane. These may be used in combination with allyl compounds such as allylphenol, allylphenyl ether, and allyl benzoate.

２官能以下のラジカル重合性物質の中でも、ウレタン（メタ）アクリレートが接着性の観点から好ましい。また、耐熱性を向上させるために、後述する有機過酸化物（ラジカル重合開始剤の１種）との橋かけ後の重合物のガラス転移温度（Ｔｇ）が、単独で１００℃以上となるようなラジカル重合性物質を併用することが好ましい。このようなラジカル重合性物質としては、ジシクロペンテニル基、トリシクロデカニル基及び／又はトリアジン環を有するものを用いることができる。特に、トリシクロデカニル基やトリアジン環を有するラジカル重合性物質が好適に用いられる。   Of the bifunctional or lower radical polymerizable substances, urethane (meth) acrylate is preferable from the viewpoint of adhesiveness. Moreover, in order to improve heat resistance, the glass transition temperature (Tg) of the polymer after crosslinking with an organic peroxide (one kind of radical polymerization initiator) described later is 100 ° C. or more alone. It is preferable to use a radically polymerizable substance in combination. As such a radically polymerizable substance, a substance having a dicyclopentenyl group, a tricyclodecanyl group and / or a triazine ring can be used. In particular, a radical polymerizable substance having a tricyclodecanyl group or a triazine ring is preferably used.

ラジカル重合性物質としては、本発明の効果を阻害しない範囲で、３官能以上のラジカル重合性物質を含有させてもよい。そのようなラジカル重合性物質として、例えば、トリメチロールプロパントリ（メタ）アクリレート、テトラメチロールメタンテトラ（メタ）アクリレート、ε−カプロラクトン変性トリス（（メタ）アクリロキシエチル）イソシアヌレート、トリス（（メタ）アクリロキシエチル）イソシアヌレートが挙げられる。   As the radically polymerizable substance, a radically polymerizable substance having three or more functional groups may be contained as long as the effects of the present invention are not impaired. Examples of such radically polymerizable substances include trimethylolpropane tri (meth) acrylate, tetramethylolmethanetetra (meth) acrylate, ε-caprolactone-modified tris ((meth) acryloxyethyl) isocyanurate, tris ((meth)) Acryloxyethyl) isocyanurate.

また、ラジカル重合性物質はリン酸エステル構造を有したものでもよい。具体的には、２−メタクリロイロキシエチルアッシドフォスフェート、２−アクリロイロキシエチルアッシドフォスフェート等が挙げられる。なお、リン酸エステル構造を有するラジカル重合性物質は、無水リン酸と２−ヒドロキシル（メタ）アクリレートとの反応物として得られる。   Further, the radical polymerizable substance may have a phosphate structure. Specific examples include 2-methacryloyloxyethyl acid phosphate and 2-acryloyloxyethyl acid phosphate. In addition, the radically polymerizable substance having a phosphoric ester structure is obtained as a reaction product of phosphoric anhydride and 2-hydroxyl (meth) acrylate.

さらに、リン酸エステル構造を有するラジカル重合性物質を、接着剤成分の固形分全量を基準（１００質量％）として０．１〜１０質量％用いた場合、金属等の無機物表面での接着強度が向上するので好ましく、０．５〜５質量％用いるとより好ましい。   Furthermore, when the radically polymerizable substance having a phosphate ester structure is used in an amount of 0.1 to 10% by mass based on the total solid content of the adhesive component (100% by mass), the adhesive strength on the surface of an inorganic substance such as a metal is reduced. Since it improves, it is preferable and it is more preferable to use 0.5-5 mass%.

以上のラジカル重合性物質は、１種を単独で又は２種以上を組み合わせて用いることができる。   The above radical polymerizable substances can be used singly or in combination of two or more.

ラジカル重合性物質としては、回路接続材料を硬化する前の回路部材の仮固定を容易にする観点から、２５℃での粘度が１０００００〜１００００００ｍＰａ・ｓであるラジカル重合性物質を少なくとも１種含有することが好ましく、１０００００〜５０００００ｍＰａ・ｓの粘度（２５℃）を有するラジカル重合性物質を含有することがより好ましい。ラジカル重合性物質の粘度は、市販のＥ型粘度計を用いて測定することができる。   The radically polymerizable substance contains at least one radically polymerizable substance having a viscosity at 25 ° C. of 100,000 to 1,000,000 mPa · s from the viewpoint of facilitating temporary fixing of the circuit member before curing the circuit connecting material. It is preferable to contain a radical polymerizable substance having a viscosity (25 ° C.) of 100,000 to 500,000 mPa · s. The viscosity of the radical polymerizable substance can be measured using a commercially available E-type viscometer.

本実施形態の回路接続材料は、２官能以下のラジカル重合性物質を含む場合、ラジカル重合性物質の全量を基準として５０〜１００質量％含むことが好ましく、６５〜１００質量％含むことがより好ましく、８０〜１００質量％含むことが更に好ましい。これにより、回路接続時の圧着において、樹脂の流動性が高まる。   When the circuit connection material of the present embodiment includes a bifunctional or lower radical polymerizable substance, the circuit connecting material preferably includes 50 to 100% by mass, more preferably 65 to 100% by mass based on the total amount of the radical polymerizable substance. 80 to 100% by mass is more preferable. Thereby, the fluidity | liquidity of resin increases in the crimping | compression-bonding at the time of circuit connection.

ラジカル重合開始剤（遊離ラジカル発生剤）としては、過酸化化合物、アゾ系化合物等の加熱又は光により分解して遊離ラジカルを発生するものが挙げられる。ラジカル重合開始剤は、目的とする接続温度、接続時間、ポットライフ等に応じて適宜選定されるが、高反応性とポットライフの観点から、半減期１０時間の温度が４０℃以上、かつ半減期１分の温度が１８０℃以下の有機過酸化物が好ましい。   Examples of the radical polymerization initiator (free radical generator) include those that decompose by heating or light, such as peroxide compounds and azo compounds, to generate free radicals. The radical polymerization initiator is appropriately selected according to the intended connection temperature, connection time, pot life, etc. From the viewpoint of high reactivity and pot life, the temperature of the half-life of 10 hours is 40 ° C. or more and half. An organic peroxide having a period of 1 minute at a temperature of 180 ° C. or less is preferred.

ラジカル重合開始剤の配合量は、接着剤成分の固形分全量を基準として０．０５〜１０質量％程度であることが好ましく、０．１〜５質量％であることがより好ましい。   The blending amount of the radical polymerization initiator is preferably about 0.05 to 10% by mass and more preferably 0.1 to 5% by mass based on the total solid content of the adhesive component.

ラジカル重合開始剤としては、具体的には、ジアシルパーオキサイド類、パーオキシジカーボネート類、パーオキシエステル類、パーオキシケタール類、ジアルキルパーオキサイド類、ハイドロパーオキサイド類等が挙げられる。これらの中でも、回路部材の回路電極の腐食を抑える観点から、パーオキシエステル類、ジアルキルパーオキサイド類、ハイドロパーオキサイド類が好ましい。また、高反応性が得られる観点から、パーオキシエステル類がより好ましい。   Specific examples of the radical polymerization initiator include diacyl peroxides, peroxydicarbonates, peroxyesters, peroxyketals, dialkyl peroxides, hydroperoxides, and the like. Among these, peroxyesters, dialkyl peroxides, and hydroperoxides are preferable from the viewpoint of suppressing corrosion of the circuit electrode of the circuit member. Moreover, peroxyesters are more preferable from the viewpoint of obtaining high reactivity.

ジアシルパーオキサイド類としては、例えば、イソブチルパーオキサイド、２，４−ジクロロベンゾイルパーオキサイド、３，５，５−トリメチルヘキサノイルパーオキサイド、オクタノイルパーオキサイド、ラウロイルパーオキサイド、ステアロイルパーオキサイド、スクシニックパーオキサイド、ベンゾイルパーオキシトルエン、ベンゾイルパーオキサイドが挙げられる。   Examples of diacyl peroxides include isobutyl peroxide, 2,4-dichlorobenzoyl peroxide, 3,5,5-trimethylhexanoyl peroxide, octanoyl peroxide, lauroyl peroxide, stearoyl peroxide, and succinic peroxide. Examples thereof include oxide, benzoylperoxytoluene, and benzoyl peroxide.

パーオキシジカーボネート類としては、例えば、ジ−ｎ−プロピルパーオキシジカーボネート、ジイソプロピルパーオキシジカーボネート、ビス（４−ｔ−ブチルシクロヘキシル）パーオキシジカーボネート、ジ−２−エトキシメトキシパーオキシジカーボネート、ジ（２−エチルヘキシルパーオキシ）ジカーボネート、ジメトキシブチルパーオキシジカーボネート、ジ（３−メチル−３−メトキシブチルパーオキシ）ジカーボネートが挙げられる。   Examples of peroxydicarbonates include di-n-propyl peroxydicarbonate, diisopropyl peroxydicarbonate, bis (4-t-butylcyclohexyl) peroxydicarbonate, and di-2-ethoxymethoxyperoxydicarbonate. , Di (2-ethylhexylperoxy) dicarbonate, dimethoxybutylperoxydicarbonate, and di (3-methyl-3-methoxybutylperoxy) dicarbonate.

パーオキシエステル類としては、例えば、クミルパーオキシネオデカノエート、１，１，３，３−テトラメチルブチルパーオキシネオデカノエート、１−シクロヘキシル−１−メチルエチルパーオキシネオデカノエート、ｔ−ヘキシルパーオキシネオデカノエート、ｔ−ブチルパーオキシピバレート、１，１，３，３−テトラメチルブチルパーオキシ−２−エチルヘキサノエート、２，５−ジメチル−２，５−ビス（２−エチルヘキサノイルパーオキシ）ヘキサン、１−シクロヘキシル−１−メチルエチルパーオキシ−２−エチルヘキサノエート、ｔ−ヘキシルパーオキシ−２−エチルヘキサノエート、ｔ−ブチルパーオキシ−２−エチルヘキサノエート、ｔ−ブチルパーオキシイソブチレート、１，１−ビス（ｔ−ブチルパーオキシ）シクロヘキサン、ｔ−ヘキシルパーオキシイソプロピルモノカーボネート、ｔ−ブチルパーオキシ−３，５，５−トリメチルヘキサノエート、ｔ−ブチルパーオキシラウレート、２，５−ジメチル−２，５−ビス（ｍ−トルオイルパーオキシ）ヘキサン、ｔ−ブチルパーオキシイソプロピルモノカーボネート、ｔ−ブチルパーオキシ−２−エチルヘキシルモノカーボネート、ｔ−ヘキシルパーオキシベンゾエート、ｔ−ブチルパーオキシアセテートが挙げられる。   Examples of peroxyesters include cumyl peroxyneodecanoate, 1,1,3,3-tetramethylbutylperoxyneodecanoate, 1-cyclohexyl-1-methylethylperoxyneodecanoate, t-hexylperoxyneodecanoate, t-butylperoxypivalate, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexanoate, 2,5-dimethyl-2,5-bis (2-ethylhexanoylperoxy) hexane, 1-cyclohexyl-1-methylethylperoxy-2-ethylhexanoate, t-hexylperoxy-2-ethylhexanoate, t-butylperoxy-2- Ethylhexanoate, t-butyl peroxyisobutyrate, 1,1-bis (t-butylperoxy) cycle Hexane, t-hexylperoxyisopropyl monocarbonate, t-butylperoxy-3,5,5-trimethylhexanoate, t-butylperoxylaurate, 2,5-dimethyl-2,5-bis (m- Toluoyl peroxy) hexane, t-butyl peroxyisopropyl monocarbonate, t-butyl peroxy-2-ethylhexyl monocarbonate, t-hexyl peroxybenzoate, t-butyl peroxyacetate.

パーオキシケタール類としては、例えば、１，１−ビス（ｔ−ヘキシルパーオキシ）−３，５，５−トリメチルシクロヘキサン、１，１−ビス（ｔ−ヘキシルパーオキシ）シクロヘキサン、１，１−ビス（ｔ−ブチルパーオキシ）−３，５，５−トリメチルシクロヘキサン、１，１−（ｔ−ブチルパーオキシ）シクロドデカン、２，２−ビス（ｔ−ブチルパーオキシ）デカンが挙げられる。   Examples of peroxyketals include 1,1-bis (t-hexylperoxy) -3,5,5-trimethylcyclohexane, 1,1-bis (t-hexylperoxy) cyclohexane, 1,1-bis. (T-Butylperoxy) -3,5,5-trimethylcyclohexane, 1,1- (t-butylperoxy) cyclododecane, 2,2-bis (t-butylperoxy) decane.

ジアルキルパーオキサイド類としては、例えば、α，α’−ビス（ｔ−ブチルパーオキシ）ジイソプロピルベンゼン、ジクミルパーオキサイド、２，５−ジメチル−２，５−ジ（ｔ−ブチルパーオキシ）ヘキサン、ｔ−ブチルクミルパーオキサイドが挙げられる。   Examples of dialkyl peroxides include α, α'-bis (t-butylperoxy) diisopropylbenzene, dicumyl peroxide, 2,5-dimethyl-2,5-di (t-butylperoxy) hexane, A t-butyl cumyl peroxide is mentioned.

ハイドロパーオキサイド類としては、例えば、ジイソプロピルベンゼンハイドロパーオキサイド、クメンハイドロパーオキサイドが挙げられる。   Examples of hydroperoxides include diisopropylbenzene hydroperoxide and cumene hydroperoxide.

以上のラジカル重合開始剤は、１種を単独で又は２種以上を混合して使用することができる。また、ラジカル重合開始剤は、分解促進剤や抑制剤等を混合して用いてもよい。   The above radical polymerization initiator can be used individually by 1 type or in mixture of 2 or more types. In addition, the radical polymerization initiator may be used by mixing a decomposition accelerator, an inhibitor or the like.

本実施形態の回路接続材料は、導電粒子を含有する。導電粒子としては、Ａｕ、Ａｇ、Ｎｉ、Ｃｕ、はんだ等の金属粒子やカーボン等が挙げられる。また、非導電性のガラス、セラミック、プラスチック等を核とし、この核に上記金属、金属粒子やカーボンを被覆したものでもよい。導電粒子が、プラスチックを核としてこの核に上記金属、金属粒子やカーボンを被覆したものである場合、又ははんだ等の熱溶融金属粒子である場合は、加熱加圧による変形性を有するため回路接続時に電極の厚みバラツキを吸収したり、電極との接触面積が増加したりして信頼性が向上するので好ましい。   The circuit connection material of this embodiment contains conductive particles. Examples of the conductive particles include metal particles such as Au, Ag, Ni, Cu, and solder, and carbon. Further, non-conductive glass, ceramic, plastic or the like may be used as a core, and the core may be coated with the metal, metal particles, or carbon. If the conductive particles are made of plastic as a core and the core is coated with the above metal, metal particles or carbon, or if it is a hot-melt metal particle such as solder, circuit connection is possible because it has deformability due to heat and pressure. This is preferable because it sometimes improves the reliability by absorbing variations in electrode thickness or increasing the contact area with the electrode.

また、これらの導電粒子の表面を、さらに高分子樹脂等で被覆した微粒子は、導電粒子の配合量を増加した場合の粒子同士の接触による短絡を抑制し、電極回路間の絶縁性が向上できることから、適宜これを単独あるいは導電粒子と混合して用いてもよい。   In addition, fine particles with the surface of these conductive particles coated with a polymer resin or the like can suppress short-circuiting due to contact between particles when the amount of conductive particles is increased, and can improve insulation between electrode circuits. Therefore, they may be used alone or mixed with conductive particles as appropriate.

この導電粒子の平均粒径は、分散性、導電性の点から１〜１８μｍであることが好ましい。このような導電粒子を含有する場合、回路部材同士の接続に本実施形態の回路接続材料をより好適に用いることができる。   The average particle diameter of the conductive particles is preferably 1 to 18 μm from the viewpoint of dispersibility and conductivity. When such a conductive particle is contained, the circuit connection material of this embodiment can be used more suitably for connection between circuit members.

以上に示した回路接続材料により、第一の基板の主面上に第一の回路電極が形成された第一の回路部材と、第二の基板の主面上に第二の回路電極が形成された第二の回路部材とを電気的に接続することができる。より具体的には、上記二つの電極が対向配置された状態で本実施形態の回路接続材料を介在させ、加熱及び加圧して、上記二つの回路電極同士を電気的に接続する。このときの加圧は、１．５ＭＰａ以下である。本実施形態の回路接続材料によれば、加圧時の圧力が１．５ＭＰａ以下と低い場合であっても、接続構造における圧痕及び接続抵抗は良好である。   With the circuit connection material shown above, the first circuit member having the first circuit electrode formed on the main surface of the first substrate and the second circuit electrode formed on the main surface of the second substrate The second circuit member thus made can be electrically connected. More specifically, the two circuit electrodes are electrically connected to each other by heating and pressurizing the circuit connection material of the present embodiment with the two electrodes facing each other. The pressurization at this time is 1.5 MPa or less. According to the circuit connection material of this embodiment, even if the pressure at the time of pressurization is as low as 1.5 MPa or less, the indentation and connection resistance in the connection structure are good.

また、本発明の回路接続材料は、フィルム状とすることができる。図１は、回路接続材料及び支持基材を備える接着シートの一実施形態を示す断面図である。図１に示す接着シート１００は、支持基材８と、支持基材８上に剥離可能に積層されたフィルム状の回路接続材料１０とを備える。回路接続材料１０は、絶縁性の接着剤成分５と、接着剤成分５内に分散した導電粒子７とを含む。   Moreover, the circuit connection material of this invention can be made into a film form. Drawing 1 is a sectional view showing one embodiment of an adhesive sheet provided with circuit connection material and a support substrate. An adhesive sheet 100 shown in FIG. 1 includes a support base 8 and a film-like circuit connection material 10 that is detachably laminated on the support base 8. The circuit connecting material 10 includes an insulating adhesive component 5 and conductive particles 7 dispersed in the adhesive component 5.

支持基材８は、回路接続材料１０フィルム状に保つことができるものであれば、その形状や素材は任意である。具体的には、フッ素樹脂フィルム、ポリエチレンテレフタレートフィルム（ＰＥＴ）、二軸延伸ポリプロピレンフィルム（ＯＰＰ）又は不織布等を支持基材として用いることができる。   As long as the support base material 8 can be kept in a film shape of the circuit connection material 10, its shape and material are arbitrary. Specifically, a fluororesin film, a polyethylene terephthalate film (PET), a biaxially stretched polypropylene film (OPP), a nonwoven fabric, or the like can be used as a supporting substrate.

（回路部材の接続構造）
図２は、本発明に係る回路部材の接続構造（回路接続構造体）の一実施形態を示す概略断面図である。図２に示す回路部材の接続構造（回路接続構造体）１は、相互に対向する第一の回路部材２０及び第二の回路部材３０を備えており、第一の回路部材２０と第二の回路部材３０との間には、これらを接続する回路接続材料１０が設けられている。 (Circuit member connection structure)
FIG. 2 is a schematic cross-sectional view showing an embodiment of a circuit member connection structure (circuit connection structure) according to the present invention. A circuit member connection structure (circuit connection structure) 1 shown in FIG. 2 includes a first circuit member 20 and a second circuit member 30 that face each other. Between the circuit members 30, a circuit connection material 10 for connecting them is provided.

第一の回路部材２０は、第一の基板２１と、第一の基板２１の主面２１ａ上に形成された第一の接続端子２２とを有する。第二の回路部材３０は、第二の基板３１と、第二の基板３１の主面３１ａ上に形成された第二の接続端子３２とを有する。第一の基板２１の主面２１ａ上、及び／又は第二の基板３１の主面３１ａ上には、場合により絶縁層（図示せず）が形成されていてもよい。つまり、必要に応じて形成される絶縁層は、第一の回路部材２０及び第二の回路部材３０のうち少なくとも一方と回路接続材料１０との間に形成される。   The first circuit member 20 includes a first substrate 21 and first connection terminals 22 formed on the main surface 21 a of the first substrate 21. The second circuit member 30 includes a second substrate 31 and second connection terminals 32 formed on the main surface 31 a of the second substrate 31. An insulating layer (not shown) may be formed on the main surface 21a of the first substrate 21 and / or the main surface 31a of the second substrate 31, as the case may be. That is, the insulating layer formed as necessary is formed between at least one of the first circuit member 20 and the second circuit member 30 and the circuit connection material 10.

第一及び第二の基板２１，３１としては、半導体、ガラス、セラミック等の無機物、ＴＣＰ、ＣＯＦ等のフレキシブルプリント配線板に代表されるポリイミド樹脂、ポリカーボネート、ポリエチレンテレフタレート等のポリエステルテレフタレート、ポリエーテルサルフォン、エポキシ樹脂、アクリル樹脂等の有機物、これらの無機物や有機物を複合化した材料からなる基板が挙げられる。回路接続材料１０との接着強度を更に高める観点から、第一及び第二の基板のうちの少なくとも一方は、ポリエステルテレフタレート、ポリエーテルサルフォン、エポキシ樹脂、アクリル樹脂、ポリイミド樹脂及びガラスからなる群より選ばれる少なくとも１種の樹脂を含む材料からなる基板であることが好ましい。   As the first and second substrates 21 and 31, inorganic materials such as semiconductors, glass and ceramics, polyimide resins typified by flexible printed wiring boards such as TCP and COF, polyester terephthalates such as polycarbonate and polyethylene terephthalate, polyethersal Examples thereof include substrates made of organic materials such as phon, epoxy resin, and acrylic resin, and materials obtained by combining these inorganic materials and organic materials. From the viewpoint of further increasing the adhesive strength with the circuit connection material 10, at least one of the first and second substrates is selected from the group consisting of polyester terephthalate, polyethersulfone, epoxy resin, acrylic resin, polyimide resin, and glass. A substrate made of a material containing at least one selected resin is preferable.

また、回路部材の、回路接続材料１０と接する面に絶縁層がコーティングされている場合又は付着している場合、絶縁層はシリコーン樹脂、アクリル樹脂及びポリイミド樹脂からなる群より選ばれる少なくとも１種の樹脂を含む層であることが好ましい。これにより、上記絶縁層が形成されていないものに比べて、第一の基板２１及び／又は第二の基板３１と回路接続材料１０との接着強度がより一層向上する。   Further, when the insulating layer is coated on or attached to the surface of the circuit member that contacts the circuit connecting material 10, the insulating layer is at least one selected from the group consisting of silicone resin, acrylic resin, and polyimide resin. A layer containing a resin is preferred. Thereby, compared with the thing in which the said insulating layer is not formed, the adhesive strength of the 1st board | substrate 21 and / or the 2nd board | substrate 31, and the circuit connection material 10 improves further.

第一の接続端子２２及び第二の接続端子３２のうち少なくとも一方は、その表面が金、銀、錫、白金族の金属及びインジウム−錫酸化物（ＩＴＯ）からなる群より選ばれる少なくとも１種を含む材料からなることが好ましい。これにより、同一回路部材２０又は３０上で隣り合う接続端子２２又は３２同士の間で絶縁性を維持しつつ、対向する接続端子２２及び３２間の抵抗値をより一層低減させることができる。   At least one of the first connection terminal 22 and the second connection terminal 32 has at least one surface selected from the group consisting of gold, silver, tin, a platinum group metal, and indium-tin oxide (ITO). It is preferable to consist of a material containing. Thereby, the resistance value between the opposing connection terminals 22 and 32 can be further reduced while maintaining insulation between the connection terminals 22 or 32 adjacent on the same circuit member 20 or 30.

第一及び第二の回路部材２０，３０の具体例としては、液晶ディスプレイに用いられている、ＩＴＯ等で接続端子が形成されたガラス基板又はプラスチック基板や、プリント配線板、セラミック配線板、フレキシブルプリント配線板、半導体シリコンチップ等が挙げられる。これらのうちプラスチック基板は、例えば、ポリエチレンテレフタレート（ＰＥＴ）、ポリカーボネート（ＰＣ）、ポリエチレンナフタレート（ＰＥＮ）に代表されるものであり、タッチパネルや電子ペーパー等に用いられる。特にこのようなプラスチック基板は機械的強度が比較的低い材質であるため低圧条件での接続が効果的である。これらは必要に応じて組み合わせて使用される。   Specific examples of the first and second circuit members 20 and 30 include a glass substrate or a plastic substrate, a printed circuit board, a ceramic circuit board, and a flexible circuit board, which are used in a liquid crystal display and have connection terminals formed of ITO or the like. Examples thereof include a printed wiring board and a semiconductor silicon chip. Among these, plastic substrates are represented by, for example, polyethylene terephthalate (PET), polycarbonate (PC), and polyethylene naphthalate (PEN), and are used for touch panels and electronic paper. In particular, since such a plastic substrate is a material having a relatively low mechanical strength, connection under low pressure conditions is effective. These are used in combination as necessary.

本実施形態において効果的な回路部材の組み合わせとしては、例えば、
ＴＣＰ、ＣＯＦ等のフレキシブルプリント配線板とガラス基板との接続、
ＴＣＰ、ＣＯＦ等のフレキシブルプリント配線板とプラスチック基板との接続、
ＴＣＰ、ＣＯＦ等のフレキシブルプリント配線板とプリント配線板との接続、及び、
ＴＣＰ、ＣＯＦ等のフレキシブルプリント配線板とセラミック配線板との接続が挙げられる。 As an effective combination of circuit members in the present embodiment, for example,
Connection between flexible printed wiring boards such as TCP and COF and glass substrates,
Connection between flexible printed wiring boards such as TCP and COF and plastic substrates,
Connection between flexible printed wiring boards such as TCP and COF and printed wiring boards, and
Examples include connection between a flexible printed wiring board such as TCP and COF and a ceramic wiring board.

回路接続材料１０は、導電粒子７を含有する上記本実施形態の回路接続材料の硬化物から形成されている。回路接続材料１０は、接着剤成分１１と、該接着剤成分１１内に分散している導電粒子７とから構成される。回路接続材料１０中の導電粒子７は、対向する第一の接続端子２２と第二の接続端子３２との間のみならず、主面２１ａ，３１ａ同士間にも配置されている。回路部材の接続構造１においては、導電粒子７が第一及び第二の接続端子２２，３２の双方に直接接触しているとともに、第一及び第二の接続端子２２，３２間で扁平状に圧縮されている。これにより、第一及び第二の接続端子２２，３２が、導電粒子７を介して電気的に接続されている。このため、第一の接続端子２２及び第二の接続端子３２間の接続抵抗が十分に低減される。したがって、第一及び第二の接続端子２２，３２の間の電流の流れを円滑にすることができ、回路の持つ機能を十分に発揮することができる。   The circuit connection material 10 is formed from a cured product of the circuit connection material of the present embodiment containing the conductive particles 7. The circuit connection material 10 includes an adhesive component 11 and conductive particles 7 dispersed in the adhesive component 11. The conductive particles 7 in the circuit connection material 10 are arranged not only between the first connection terminal 22 and the second connection terminal 32 facing each other but also between the main surfaces 21a and 31a. In the circuit member connection structure 1, the conductive particles 7 are in direct contact with both the first and second connection terminals 22, 32 and are flat between the first and second connection terminals 22, 32. It is compressed. Thereby, the first and second connection terminals 22 and 32 are electrically connected via the conductive particles 7. For this reason, the connection resistance between the first connection terminal 22 and the second connection terminal 32 is sufficiently reduced. Therefore, the flow of current between the first and second connection terminals 22 and 32 can be made smooth, and the functions of the circuit can be fully exhibited.

このような回路部材の接続構造（回路接続構造体）１は、次の工程を経て製造することができる。すなわち、第一の基板２１の主面２１ａ上に第一の接続端子（第一の回路電極）２２が形成された第一の回路部材２０、及び、第二の基板３１の主面３１ａ上に第二の接続端子（第二の回路電極）３２が形成された第二の回路部材３０の間に、上記回路接続材料１０を配置する工程と、第一の接続端子２２と第二の接続端子３２とが対向配置された状態で加熱及び加圧して、第一の接続端子２２と第二の接続端子３２とを電気的に接続する工程と、を備え、加圧が１．５ＭＰａ以下で行われる製造方法により製造することができる。   Such a circuit member connection structure (circuit connection structure) 1 can be manufactured through the following steps. That is, on the first circuit member 20 in which the first connection terminal (first circuit electrode) 22 is formed on the main surface 21 a of the first substrate 21 and on the main surface 31 a of the second substrate 31. A step of arranging the circuit connection material 10 between the second circuit members 30 on which the second connection terminals (second circuit electrodes) 32 are formed, and the first connection terminals 22 and the second connection terminals. And a step of electrically connecting the first connection terminal 22 and the second connection terminal 32 with the pressure being 1.5 MPa or less. Can be manufactured by a manufacturing method.

（回路部材の接続方法）
図３（ａ）〜（ｃ）は、本発明に係る回路部材の接続方法の一実施形態を概略断面図により示す工程図である。 (Circuit member connection method)
FIG. 3A to FIG. 3C are process diagrams showing an embodiment of a circuit member connection method according to the present invention in schematic cross-sectional views.

本実施形態では、まず、上述した第一の回路部材２０と、フィルム状回路接続材料４０とを用意する。   In this embodiment, first, the first circuit member 20 and the film-like circuit connection material 40 described above are prepared.

フィルム状回路接続材料４０の厚さは、５〜５０μｍであることが好ましい。回路接続材料４０の厚さが５μｍ未満では、第一及び第二の接続端子２２，３２間への回路接続材料４０の充填が不十分となる傾向がある。他方、５０μｍを超えると、第一及び第二の接続端子２２，３２間の導通の確保が困難となる傾向がある。   The thickness of the film-like circuit connecting material 40 is preferably 5 to 50 μm. If the thickness of the circuit connection material 40 is less than 5 μm, the filling of the circuit connection material 40 between the first and second connection terminals 22 and 32 tends to be insufficient. On the other hand, if it exceeds 50 μm, it tends to be difficult to ensure conduction between the first and second connection terminals 22 and 32.

次に、フィルム状回路接続材料４０を第一の回路部材２０の接続端子２２が形成されている面上に載せる。そして、フィルム状回路接続材料４０を、図３（ａ）の矢印Ａ及びＢ方向に加圧し、フィルム状回路接続材料４０を第一の回路部材２０に仮接着する（図３（ｂ））。   Next, the film-like circuit connection material 40 is placed on the surface of the first circuit member 20 on which the connection terminals 22 are formed. And the film-form circuit connection material 40 is pressurized to the arrow A and B direction of Fig.3 (a), and the film-form circuit connection material 40 is temporarily bonded to the 1st circuit member 20 (FIG.3 (b)).

このときの圧力は、回路部材に損傷を与えない範囲であれば特に制限されないが、一般的には０．１〜３０ＭＰａとすることが好ましく、０．５〜１．５ＭＰａとすることがより好ましい。また、加熱しながら加圧してもよく、加熱温度は回路接続材料４０が実質的に硬化しない温度とする。加熱温度は、一般的には５０〜１９０℃にするのが好ましい。これらの加熱及び加圧は０．５〜１２０秒間の範囲で行うことが好ましい。   The pressure at this time is not particularly limited as long as it does not damage the circuit member, but is generally preferably 0.1 to 30 MPa, more preferably 0.5 to 1.5 MPa. . Moreover, you may pressurize, heating, and let heating temperature be the temperature which the circuit connection material 40 does not harden | cure substantially. In general, the heating temperature is preferably 50 to 190 ° C. These heating and pressurization are preferably performed in the range of 0.5 to 120 seconds.

次いで、図３（ｃ）に示すように、第二の回路部材３０を、第二の接続端子３２を第一の回路部材２０の側に向けるようにしてフィルム状回路接続材料４０上に載せる。なお、フィルム状回路接続材料４０が支持基材（図示せず）上に密着して設けられている場合には、支持基材を剥離してから第二の回路部材３０をフィルム状回路接続材料４０上に載せる。そして、回路接続材料４０を加熱しながら、図３（ｃ）の矢印Ａ及びＢ方向に全体を加圧する。   Next, as shown in FIG. 3C, the second circuit member 30 is placed on the film-like circuit connection material 40 so that the second connection terminal 32 faces the first circuit member 20. When the film-like circuit connection material 40 is provided in close contact with a support base (not shown), the second circuit member 30 is removed from the support base after the second base member 30 is peeled off. 40. And the whole is pressurized in the arrow A and B directions of FIG.3 (c), heating the circuit connection material 40. FIG.

加熱温度は、例えば、９０〜２００℃とし、接続時間は例えば１秒〜１０分とする。圧力は１．５ＭＰａ以下とする。加熱温度及び接続時間は、使用する用途、回路接続材料、回路部材によって適宜選択され、必要に応じて、後硬化を行ってもよい。例えば、回路接続材料がラジカル重合性物質を含有する場合の加熱温度は、ラジカル重合開始剤がラジカルを発生可能な温度とする。これにより、ラジカル重合開始剤においてラジカルが発生し、ラジカル重合性物質の重合が開始される。   The heating temperature is, for example, 90 to 200 ° C., and the connection time is, for example, 1 second to 10 minutes. The pressure is 1.5 MPa or less. The heating temperature and the connection time are appropriately selected depending on the intended use, circuit connection material, and circuit member, and post-curing may be performed as necessary. For example, the heating temperature when the circuit connecting material contains a radical polymerizable substance is set to a temperature at which the radical polymerization initiator can generate radicals. As a result, radicals are generated in the radical polymerization initiator, and polymerization of the radical polymerizable substance is started.

本実施形態の回路接続材料を用いることにより、前述した１．５ＭＰａ以下という低圧条件での接続が可能である。この圧力の下限は０．５ＭＰａ程度であり、０．８ＭＰａ程度であることが好ましく、０．９ＭＰａ程度であることがより好ましい。量産性の観点からは、０．８〜１．５ＭＰａの圧力であることが好ましく、０．９〜１．３ＭＰａであることがより好ましく、０．９〜１．２ＭＰａであることが特に好ましい。   By using the circuit connection material of this embodiment, the connection under the low pressure condition of 1.5 MPa or less is possible. The lower limit of this pressure is about 0.5 MPa, preferably about 0.8 MPa, and more preferably about 0.9 MPa. From the viewpoint of mass productivity, the pressure is preferably 0.8 to 1.5 MPa, more preferably 0.9 to 1.3 MPa, and particularly preferably 0.9 to 1.2 MPa.

図５は、フィルム状回路接続材料を用いて回路部材（ＦＰＣ、ＴＣＰ、ＣＯＦ等のフレキシブル基板プリント配線板）を接続する前の状態を示す平面図である。上述した接続時の加圧力は、接続部の総面積に対する圧力を意味する。「接続部の総面積」とは、回路接続材料により接続される接続端子２２及び接続端子２２間の隙間を含む領域の面積の合計を意味し、図５（ａ）及び（ｂ）に示されるように、接続端子２２が並設された幅ｘと、その幅に垂直な方向の接続端子の長さｙとの積により求められる。この計算方法は、接続部とフィルム状回路接続材料４０の大きさがほぼ等しい場合（図５（ａ））も、フィルム状回路接続材料４０が接続部よりも広い領域にわたる場合（図５（ｂ））も同様である。   FIG. 5 is a plan view showing a state before a circuit member (a flexible printed circuit board such as FPC, TCP, COF) is connected using a film-like circuit connecting material. The applied pressure at the time of connection mentioned above means the pressure with respect to the total area of a connection part. The “total area of the connection portion” means the total area of the connection terminal 22 connected by the circuit connection material and the area including the gap between the connection terminals 22, and is shown in FIGS. 5 (a) and 5 (b). Thus, it is obtained by the product of the width x in which the connection terminals 22 are arranged in parallel and the length y of the connection terminal in the direction perpendicular to the width. In this calculation method, when the size of the connection portion and the film-like circuit connection material 40 are substantially equal (FIG. 5A), the case where the film-like circuit connection material 40 covers a wider area than the connection portion (FIG. 5B). The same applies to)).

加圧力は、具体的には次のようにして求めることができる。例えば、接続部の幅が３０ｍｍ、この幅に垂直な方向の接続端子の長さが２ｍｍである場合に、接続部における圧力を１．０ＭＰａ（≒１０ｋｇｆ／ｃｍ２）とするには、加圧装置に設定する加圧力は次に示す計算により求めることができる。対応する圧着ヘッドに下記の加圧力がかかるようにすればよい。
目標圧力＝１．０ＭＰａ（１０ｋｇｆ／ｃｍ２）
接続部の総面積＝０．２ｃｍ×３．０ｃｍ＝０．６ｃｍ２
加圧力＝（接続部の総面積）×（目標圧力）＝０．６ｃｍ２×１０ｋｇｆ／ｃｍ２＝６ｋｇｆ Specifically, the applied pressure can be obtained as follows. For example, when the width of the connection portion is 30 mm and the length of the connection terminal in the direction perpendicular to the width is 2 mm, the pressure at the connection portion is 1.0 MPa (≈10 kgf / cm 2 ). The pressure applied to the apparatus can be obtained by the following calculation. The following pressure may be applied to the corresponding crimping head.
Target pressure = 1.0 MPa (10 kgf / cm 2 )
Total area of connection part = 0.2 cm × 3.0 cm = 0.6 cm 2
Applied pressure = (total area of connection part) × (target pressure) = 0.6 cm 2 × 10 kgf / cm 2 = 6 kgf

なお、上記例において、接続部が複数（例えば１０個）存在し、各部分を同時に加圧する場合、加圧力は次のようになる。
目標圧力＝１．０ＭＰａ（１０ｋｇｆ／ｃｍ２）
接続部の総面積＝０．２ｃｍ×３．０ｃｍ×１０＝６ｃｍ２
加圧力＝（接続部の総面積）×（目標圧力）＝６ｃｍ２×１０ｋｇｆ／ｃｍ２＝６０ｋｇｆ In the above example, when there are a plurality of (for example, 10) connecting portions and each portion is pressurized simultaneously, the applied pressure is as follows.
Target pressure = 1.0 MPa (10 kgf / cm 2 )
Total area of connection part = 0.2 cm × 3.0 cm × 10 = 6 cm 2
Applied pressure = (total area of connection part) × (target pressure) = 6 cm 2 × 10 kgf / cm 2 = 60 kgf

フィルム状回路接続材料４０の加熱により、第一の接続端子２２と第二の接続端子３２との間の距離を十分に小さくした状態でフィルム状回路接続材料４０が硬化して、第一の回路部材２０と第二の回路部材３０とが回路接続材料１０を介して強固に接続される。   By heating the film-like circuit connection material 40, the film-like circuit connection material 40 is cured in a state where the distance between the first connection terminal 22 and the second connection terminal 32 is sufficiently small, and the first circuit. The member 20 and the second circuit member 30 are firmly connected via the circuit connection material 10.

フィルム状回路接続材料４０の硬化により回路接続材料１０が形成されて、図２に示すような回路部材の接続構造１が得られる。   The circuit connection material 10 is formed by curing the film-like circuit connection material 40, and the circuit member connection structure 1 as shown in FIG. 2 is obtained.

本実施形態によれば、得られる回路部材の接続構造１において、導電粒子７を対向する第一及び第二の接続端子２２，３２の双方に接触させることが可能となり、第一及び第二の接続端子２２，３２間の接続抵抗を十分に低減することができるとともに、隣接する第一又は第二の接続端子２２，３２間の絶縁性を十分に確保することができる。また、回路接続材料１０が上記回路接続材料の硬化物により構成されていることから、第一及び第二の回路部材２０又は３０に対する回路接続材料１０の接着力が十分に高いものとなる。   According to the present embodiment, in the obtained circuit member connection structure 1, the conductive particles 7 can be brought into contact with both the first and second connection terminals 22 and 32 facing each other. The connection resistance between the connection terminals 22 and 32 can be sufficiently reduced, and the insulation between the adjacent first or second connection terminals 22 and 32 can be sufficiently ensured. Moreover, since the circuit connection material 10 is comprised by the hardened | cured material of the said circuit connection material, the adhesive force of the circuit connection material 10 with respect to the 1st and 2nd circuit members 20 or 30 becomes a thing sufficiently high.

以下、実施例及び比較例を挙げて本発明の内容をより具体的に説明する。なお、本発明は下記実施例に限定されるものではない。   Hereinafter, the contents of the present invention will be described more specifically with reference to examples and comparative examples. In addition, this invention is not limited to the following Example.

（ウレタンアクリレートの合成）
平均分子量８００のポリカプロラクトンジオール４００質量部と、２−ヒドロキシプロピルアクリレート１３１質量部と、触媒としてのジブチル錫ジラウレート０．５質量部と、重合禁止剤としてのハイドロキノンモノメチルエーテル１．０質量部とを攪拌しながら５０℃に加熱して混合した。次いで、イソホロンジイソシアネート２２２質量部を滴下し、更に攪拌しながら８０℃に昇温してウレタン化反応を行った。イソシアネート基の反応率が９９％以上になったことを確認後、反応温度を下げてウレタンアクリレートを得た。 (Synthesis of urethane acrylate)
400 parts by mass of polycaprolactone diol having an average molecular weight of 800, 131 parts by mass of 2-hydroxypropyl acrylate, 0.5 parts by mass of dibutyltin dilaurate as a catalyst, and 1.0 part by mass of hydroquinone monomethyl ether as a polymerization inhibitor The mixture was heated to 50 ° C. with stirring. Next, 222 parts by mass of isophorone diisocyanate was added dropwise, and the mixture was further heated to 80 ° C. with stirring to conduct a urethanization reaction. After confirming that the reaction rate of the isocyanate group was 99% or more, the reaction temperature was lowered to obtain urethane acrylate.

（ポリエステルウレタン樹脂Ａの合成）
ジカルボン酸としてテレフタル酸を、ジオールとしてプロピレングリコールを、イソシアネートとして４，４’−ジフェニルメタンジイソシアネートを用い、テレフタル酸／プロピレングリコール／４，４’−ジフェニルメタンジイソシアネートのモル比が１．０／２．０／０．２５となるポリエステルウレタン樹脂Ａを合成した。上記ポリエステルウレタン樹脂Ａをメチルエチルケトン（以下、「ＭＥＫ」と略記する。）に２０質量％となるように溶解した。このポリエステルウレタン樹脂Ａの２０質量％ＭＥＫ溶液を、厚み８０μｍの片面を表面処理したＰＥＴフィルムに塗工装置を用いて塗布し、７０℃、１０分間の熱風乾燥により、厚みが３５μｍのフィルムを作製した。このフィルムの弾性率の温度依存性を、広域動的粘弾性測定装置（測定条件：引っ張り荷重５ｇ、周波数１０Ｈｚ）を用いて測定した。弾性率の温度依存性から算出されるポリエステルウレタン樹脂Ａのガラス転移温度は６５℃であった。なお、ポリエステルウレタン樹脂Ａの重量平均分子量は、２４０００であった。 (Synthesis of polyester urethane resin A)
Using terephthalic acid as the dicarboxylic acid, propylene glycol as the diol, and 4,4′-diphenylmethane diisocyanate as the isocyanate, the molar ratio of terephthalic acid / propylene glycol / 4,4′-diphenylmethane diisocyanate is 1.0 / 2.0 / A polyester urethane resin A of 0.25 was synthesized. The polyester urethane resin A was dissolved in methyl ethyl ketone (hereinafter abbreviated as “MEK”) so as to be 20 mass%. A 20% by mass MEK solution of this polyester urethane resin A is applied to a PET film having a surface treated on one side of 80 μm thickness using a coating device, and hot air drying at 70 ° C. for 10 minutes produces a film having a thickness of 35 μm. did. The temperature dependence of the elastic modulus of this film was measured using a wide-range dynamic viscoelasticity measuring device (measurement conditions: tensile load 5 g, frequency 10 Hz). The glass transition temperature of the polyester urethane resin A calculated from the temperature dependence of the elastic modulus was 65 ° C. In addition, the weight average molecular weight of the polyester urethane resin A was 24000.

（ポリエステルウレタン樹脂Ｂの合成）
テレフタル酸／プロピレングリコール／４，４’−ジフェニルメタンジイソシアネートのモル比を１．０／１．３／０．２５に変更した以外は、ポリエステルウレタン樹脂Ａの合成と同様に操作して、ポリエステルウレタン樹脂Ｂの２０質量％ＭＥＫ溶液を調製した。このポリエステルウレタン樹脂Ｂの２０質量％ＭＥＫ溶液を、厚み８０μｍの片面を表面処理したＰＥＴフィルムに塗工装置を用いて塗布し、７０℃、１０分間の熱風乾燥により、厚みが３５μｍのフィルムを作製した。このフィルムの弾性率の温度依存性を、広域動的粘弾性測定装置（測定条件：引っ張り荷重５ｇ、周波数１０Ｈｚ）を用いて測定した。弾性率の温度依存性から算出されるポリエステルウレタン樹脂Ｂのガラス転移温度は１０５℃であった。なお、ポリエステルウレタン樹脂Ｂの重量平均分子量は、２６０００であった。 (Synthesis of polyester urethane resin B)
The polyester urethane resin was operated in the same manner as the synthesis of the polyester urethane resin A except that the molar ratio of terephthalic acid / propylene glycol / 4,4′-diphenylmethane diisocyanate was changed to 1.0 / 1.3 / 0.25. A 20% by mass MEK solution of B was prepared. A 20% by mass MEK solution of this polyester urethane resin B is applied to a PET film having a surface treated on one side of 80 μm thickness using a coating apparatus, and a film having a thickness of 35 μm is produced by drying with hot air at 70 ° C. for 10 minutes. did. The temperature dependence of the elastic modulus of this film was measured using a wide-range dynamic viscoelasticity measuring device (measurement conditions: tensile load 5 g, frequency 10 Hz). The glass transition temperature of the polyester urethane resin B calculated from the temperature dependence of the elastic modulus was 105 ° C. The weight average molecular weight of the polyester urethane resin B was 26000.

［実施例１］
（接着シートの作製）
ラジカル重合性物質として、上記ウレタンアクリレート２５質量部、イソシアヌレート型アクリレート（製品名：Ｍ−３２５、東亞合成社製）２０質量部、及び、２−メタクリロイロキシエチルアッシドフォスヘート（製品名：Ｐ−２Ｍ、共栄社化学社製）１質量部、並びに、ラジカル重合開始剤としてベンゾイルパーオキサイド（製品名：ナイパーＢＭＴ−Ｋ４０、日本油脂製）４質量部を、フィルム性付与ポリマーであるポリエステルウレタン樹脂Ａの２０質量％ＭＥＫ溶液２７５質量部（ポリエステルウレタン樹脂Ａ：５５質量部）と混合し、攪拌してバインダ樹脂を調製した。次いで、導電粒子として、ポリスチレンを核とし、最外層がＡｕで覆われた導電粒子を上記バインダ樹脂に対して２．０体積％を分散させ、接着剤ワニスを調製した。このワニスを、厚み５０μｍの片面を表面処理したＰＥＴフィルム（支持基材）に塗工装置を用いて塗布し、７０℃、１０分の熱風乾燥により、接着シート（幅１５ｃｍ、長さ７０ｍ）を得た。支持基材上に形成されたフィルム状回路接続材料の厚みは１６μｍであった。 [Example 1]
(Preparation of adhesive sheet)
As the radical polymerizable substance, 25 parts by mass of the urethane acrylate, 20 parts by mass of isocyanurate type acrylate (product name: M-325, manufactured by Toagosei Co., Ltd.), and 2-methacryloyloxyethyl acid phosphate (product name: 1 part by mass of P-2M (manufactured by Kyoeisha Chemical Co., Ltd.) and 4 parts by mass of benzoyl peroxide (product name: Nyper BMT-K40, manufactured by NOF Corporation) as a radical polymerization initiator, a polyester urethane resin which is a film property-imparting polymer A binder resin was prepared by mixing with 275 parts by mass of a 20% by mass MEK solution of A (polyester urethane resin A: 55 parts by mass) and stirring. Next, as the conductive particles, 2.0% by volume of conductive particles having polystyrene as a core and the outermost layer covered with Au was dispersed in the binder resin to prepare an adhesive varnish. This varnish is applied to a PET film (support base material) having a surface treated on one side having a thickness of 50 μm using a coating apparatus, and dried with hot air at 70 ° C. for 10 minutes to form an adhesive sheet (width 15 cm, length 70 m). Obtained. The thickness of the film-like circuit connecting material formed on the support substrate was 16 μm.

（回路接続構造体の作製）
上記接着シートを幅１．５ｍｍのサイズに切り出し、フィルム状回路接続材料面をＩＴＯ電極及びＡｌ電極が形成されたガラス基板に、７０℃、１ＭＰａ、２秒間の条件で仮接着した。次いで、支持基材を剥離した後、ＣＯＦ（電極間ピッチ：５０μｍ、電極幅２５μｍ、スペース２５μｍ）を積層し、１７０℃、１ＭＰａ、５秒間の条件で本接続を行い、回路接続構造体を得た。また、比較のため、本接続の条件を１７０℃、３ＭＰａ、５秒間に変更した以外は同様に操作して、回路接続構造体を得た。 (Production of circuit connection structure)
The adhesive sheet was cut into a size of 1.5 mm in width, and the film-like circuit connecting material surface was temporarily bonded to a glass substrate on which an ITO electrode and an Al electrode were formed under conditions of 70 ° C., 1 MPa, and 2 seconds. Next, after peeling off the supporting substrate, COF (interelectrode pitch: 50 μm, electrode width 25 μm, space 25 μm) is laminated, and main connection is performed under the conditions of 170 ° C., 1 MPa, 5 seconds to obtain a circuit connection structure. It was. For comparison, a circuit connection structure was obtained in the same manner except that the conditions for this connection were changed to 170 ° C., 3 MPa, and 5 seconds.

［実施例２］
ラジカル重合性物質としてウレタンアクリレートを３５質量部、Ｍ−３２５を２５質量部及びＰ−２Ｍを１質量部配合し、フィルム性付与ポリマーとしてポリエステルウレタン樹脂Ａを３０質量部及びポリエステルウレタン樹脂Ｃ（製品名：ＵＲ８３００、東洋紡社製、ガラス転移温度２０℃、重量平均分子量３００００）を１０質量部配合したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Example 2]
35 parts by mass of urethane acrylate, 25 parts by mass of M-325 and 1 part by mass of P-2M are blended as radically polymerizable substances, 30 parts by mass of polyester urethane resin A and polyester urethane resin C (product) Name: UR8300, manufactured by Toyobo Co., Ltd., glass transition temperature 20 ° C., weight average molecular weight 30000) was mixed in the same manner as in Example 1 to obtain a circuit connection structure.

［実施例３］
ラジカル重合性物質としてウレタンアクリレートを４５質量部及びＰ−２Ｍを１質量部を配合し、フィルム性付与ポリマーとしてポリエステルウレタン樹脂Ａを５５質量部に配合したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Example 3]
In the same manner as in Example 1 except that 45 parts by mass of urethane acrylate and 1 part by mass of P-2M were blended as radical polymerizable substances, and polyester urethane resin A was blended in 55 parts by mass as a film-imparting polymer. A circuit connection structure was obtained.

［実施例４］
ラジカル重合性物質としてウレタンアクリレートを２０質量部、Ｍ−３２５を１５質量部及びＰ−２Ｍを１質量部配合し、フィルム性付与ポリマーとしてポリエステルウレタン樹脂Ａを６５質量部配合したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Example 4]
Example except that 20 parts by mass of urethane acrylate as a radical polymerizable substance, 15 parts by mass of M-325, and 1 part by mass of P-2M were blended, and 65 parts by mass of polyester urethane resin A was blended as a film-imparting polymer. In the same manner as in Example 1, a circuit connection structure was obtained.

［比較例１］
ポリエステルウレタン樹脂Ａをポリエステルウレタン樹脂Ｂに変更したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Comparative Example 1]
A circuit connection structure was obtained in the same manner as in Example 1 except that the polyester urethane resin A was changed to the polyester urethane resin B.

［比較例２］
ポリエステルウレタン樹脂Ａをポリエステルウレタン樹脂Ｄ（製品名：ＵＲ１４００、東洋紡社製、ガラス転移温度８３℃、重量平均分子量５００００）に変更したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Comparative Example 2]
A circuit connection structure was obtained in the same manner as in Example 1 except that the polyester urethane resin A was changed to the polyester urethane resin D (product name: UR1400, manufactured by Toyobo Co., Ltd., glass transition temperature 83 ° C., weight average molecular weight 50000). It was.

［比較例３］
ラジカル重合性物質としてウレタンアクリレートを２５質量部、Ｍ−３２５を２５質量部及びＰ−２Ｍを１質量部配合し、フィルム性付与ポリマーとしてポリエステルウレタン樹脂Ａを１０質量部、ポリエステルウレタン樹脂Ｂを３０質量部及びポリエステルウレタン樹脂Ｃを１０質量部配合したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Comparative Example 3]
25 parts by mass of urethane acrylate as a radical polymerizable substance, 25 parts by mass of M-325 and 1 part by mass of P-2M are blended, and 10 parts by mass of polyester urethane resin A and 30 parts of polyester urethane resin B as film-forming polymers. A circuit connection structure was obtained in the same manner as in Example 1 except that 10 parts by mass of the mass part and the polyester urethane resin C were blended.

［比較例４］
ラジカル重合性物質としてウレタンアクリレートを１０質量部、Ｍ−３２５を１５質量部及びＰ−２Ｍを１質量部配合し、フィルム性付与ポリマーとしてポリエステルウレタン樹脂Ａを７５質量部配合したこと以外は実施例１と同様にして、回路接続構造体を得た。 [Comparative Example 4]
Example except that 10 parts by mass of urethane acrylate as a radical polymerizable substance, 15 parts by mass of M-325, and 1 part by mass of P-2M were blended, and 75 parts by mass of polyester urethane resin A was blended as a film-imparting polymer. In the same manner as in Example 1, a circuit connection structure was obtained.

（接続抵抗の測定）
得られた回路接続構造体について、デジタルマルチメータ（アドバンテスト社製、商品名：ＴＲ−６８４５）を用い、測定電流１ｍＡの定電流下での隣接電極間の抵抗を３７点測定した。測定の平均値が３Ω未満の場合「Ａ」、３Ω以上場合「Ｂ」とした。 (Measurement of connection resistance)
About the obtained circuit connection structure, 37 points | pieces measured the resistance between the adjacent electrodes under the constant current of 1 mA of measurement currents using the digital multimeter (The product name: TR-6845 by Advantest Corporation). When the average value of measurement was less than 3Ω, “A” was assigned, and when it was 3Ω or more, “B” was given.

（圧痕の評価）
回路接続部の圧痕の形状を、オリンパス者製ＢＨ３−ＭＪＬ液晶パネル検査用顕微鏡を用い、ガラス基板側からノマルスキー微分干渉観察により評価した。図４に、観察した圧痕の写真の一例を示す。図４（ａ）は、圧痕の強度が十分に強くむらがない状態を示す写真である。図４（ｂ）は圧痕の強度が弱い場合やむらがある状態を示す写真である。図４（ａ）に示すように圧痕の強度が十分に強くむらがなく場合には「Ａ」、図４（ｂ）に示すように圧痕の強度が弱い場合やむらがある場合には「Ｂ」とした。 (Evaluation of indentation)
The shape of the indentation in the circuit connection portion was evaluated by Nomarski differential interference observation from the glass substrate side using an Olympus BH3-MJL liquid crystal panel inspection microscope. FIG. 4 shows an example of a photograph of the observed indentation. FIG. 4A is a photograph showing a state where the indentation is sufficiently strong and has no unevenness. FIG. 4B is a photograph showing a case where the indentation is weak or uneven. As shown in FIG. 4A, when the indentation strength is sufficiently strong and uneven, “A”, and when the indentation strength is weak or uneven as shown in FIG. 4B, “B” "

上記実施例及び比較例で得られた回路接続材料を構成するフィルム性付与ポリマー及びラジカル重合性物質の配合割合、及び、回路接続構造体の評価結果を表２に示す。   Table 2 shows the blending ratios of the film property-imparting polymer and the radical polymerizable substance constituting the circuit connection materials obtained in the above Examples and Comparative Examples, and the evaluation results of the circuit connection structures.

１ＭＰａで圧着を行った場合、実施例１〜４で作製した回路接続材料は、圧痕の形成及び接続抵抗ともに良好な結果を示した。これに対し、Ｔｇ７０℃以上のフィルム性付与ポリマーのみを含有する比較例１及び２、Ｔｇ７０℃未満のフィルム性付与ポリマーの含有量が少ない比較例３では、回路接続材料の流動性が不足し、圧痕の形成が不十分であり、接続抵抗も高かった。また、Ｔｇ７０℃未満のフィルム性付与ポリマーの含有量が多い比較例４では接着性が十分ではないため、圧痕の形成が不十分であり、接続抵抗も高かった。加えて、３ＭＰａで圧着を行った場合でも、比較例１、２及び４では接続抵抗が高く、比較例４では、圧痕の形成も不十分であった。   When pressure bonding was performed at 1 MPa, the circuit connection materials produced in Examples 1 to 4 showed good results in both formation of indentations and connection resistance. On the other hand, in Comparative Examples 1 and 2 containing only a film property-imparting polymer having a Tg of 70 ° C. or higher, and in Comparative Example 3 having a small film property-imparting polymer having a Tg of less than 70 ° C., the fluidity of the circuit connecting material is insufficient. Indentation was insufficiently formed and the connection resistance was high. Further, in Comparative Example 4 in which the content of the film property-imparting polymer having a Tg of less than 70 ° C. was large, the adhesiveness was not sufficient, so that the formation of indentation was insufficient and the connection resistance was also high. In addition, even when pressure bonding was performed at 3 MPa, in Comparative Examples 1, 2, and 4, the connection resistance was high, and in Comparative Example 4, formation of indentations was insufficient.

本発明の回路接続材料は、従来達成が困難であった１．５ＭＰａ以下の低い圧力条件における回路接続を良好に達成することができ、圧着時に被着体への負荷を低減することが可能である。   The circuit connection material of the present invention can satisfactorily achieve circuit connection under a low pressure condition of 1.5 MPa or less, which has been difficult to achieve in the past, and can reduce the load on the adherend during crimping. is there.

１…回路部材の接続構造、５，１１…接着剤成分、７…導電粒子、８…支持基材、１０…回路接続材料、２０…第一の回路部材、２１…第一の基板、２１ａ…第一の基板主面、２２…第一の接続端子、３０…第二の回路部材、３１…第二の基板、３１ａ…第二の基板主面、３２…第二の接続端子、４０…フィルム状回路接続材料、１００…接着シート。   DESCRIPTION OF SYMBOLS 1 ... Circuit member connection structure, 5, 11 ... Adhesive component, 7 ... Conductive particle, 8 ... Support base material, 10 ... Circuit connection material, 20 ... First circuit member, 21 ... First substrate, 21a ... 1st board | substrate main surface, 22 ... 1st connection terminal, 30 ... 2nd circuit member, 31 ... 2nd board | substrate, 31a ... 2nd board | substrate main surface, 32 ... 2nd connection terminal, 40 ... film Circuit connection material, 100 ... adhesive sheet.

Claims (4)

第一の基板の主面上に第一の回路電極が形成された第一の回路部材、及び、第二の基板の主面上に第二の回路電極が形成された第二の回路部材の間に、回路接続材料を配置する工程と、
前記第一の回路電極と前記第二の回路電極とが対向配置された状態で加熱及び加圧して、前記第一の回路電極と前記第二の回路電極とを電気的に接続する工程と、を備え、
前記加圧が０．５ＭＰａ以上１．５ＭＰａ以下で行われ、
前記回路接続材料が、フィルム性付与ポリマー、ラジカル重合性物質、ラジカル重合開始剤及び導電粒子を含有し、
前記フィルム性付与ポリマーが、ガラス転移温度７０℃未満のポリマーを含み、該ガラス転移温度７０℃未満のポリマーの配合量が、前記フィルム性付与ポリマー及び前記ラジカル重合性物質の総量を基準として３０〜７０質量％である、回路接続構造体の製造方法。 A first circuit member having a first circuit electrode formed on the main surface of the first substrate, and a second circuit member having a second circuit electrode formed on the main surface of the second substrate. A step of arranging a circuit connecting material therebetween,
Heating and pressurizing the first circuit electrode and the second circuit electrode facing each other to electrically connect the first circuit electrode and the second circuit electrode; With
The pressurization is performed at 0.5 MPa or more and 1.5 MPa or less,
The circuit connecting material contains a film-imparting polymer, a radical polymerizable substance, a radical polymerization initiator and conductive particles,
The film property-imparting polymer contains a polymer having a glass transition temperature of less than 70 ° C., and the blending amount of the polymer having a glass transition temperature of less than 70 ° C. is 30 to 30 based on the total amount of the film property-imparting polymer and the radical polymerizable substance. The manufacturing method of the circuit connection structure which is 70 mass%. 前記フィルム性付与ポリマーが、ガラス転移温度５０℃以上７０℃未満のポリマーを、前記フィルム性付与ポリマーの全量を基準として５０質量％以上含む、請求項１記載の回路接続構造体の製造方法。   The method for producing a circuit connection structure according to claim 1, wherein the film property-imparting polymer contains 50% by mass or more of a polymer having a glass transition temperature of 50 ° C or higher and lower than 70 ° C based on the total amount of the film property-imparting polymer. 前記ラジカル重合性物質が、２官能以下のラジカル重合性物質を含み、該２官能以下のラジカル重合性物質の配合量が、前記ラジカル重合性物質の全量を基準として５０質量％以上である、請求項１又は２記載の回路接続構造体の製造方法。   The radical polymerizable substance includes a radical polymerizable substance having a bifunctional or lower functionality, and a blending amount of the bifunctional or lower radical polymerizable substance is 50% by mass or more based on the total amount of the radical polymerizable substance. Item 3. A method for producing a circuit connection structure according to Item 1 or 2. 前記第一及び第二の基板のうち少なくとも一方がポリエチレンテレフタレートを含む材料からなる基板である、請求項１〜３のいずれか一項に記載の回路接続構造体の製造方法。   The method for manufacturing a circuit connection structure according to any one of claims 1 to 3, wherein at least one of the first and second substrates is a substrate made of a material containing polyethylene terephthalate.
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