WO2015174299A1 - Pâte conductrice, procédé de production d'une pâte conductrice, structure de connexion, et procédé de production de structure de connexion - Google Patents

Pâte conductrice, procédé de production d'une pâte conductrice, structure de connexion, et procédé de production de structure de connexion Download PDF

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Publication number
WO2015174299A1
WO2015174299A1 PCT/JP2015/063095 JP2015063095W WO2015174299A1 WO 2015174299 A1 WO2015174299 A1 WO 2015174299A1 JP 2015063095 W JP2015063095 W JP 2015063095W WO 2015174299 A1 WO2015174299 A1 WO 2015174299A1
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Prior art keywords
conductive paste
conductive
particles
electrode
thermosetting
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PCT/JP2015/063095
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English (en)
Japanese (ja)
Inventor
仁志 山際
敬士 久保田
石澤　英亮
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積水化学工業株式会社
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Application filed by 積水化学工業株式会社 filed Critical 積水化学工業株式会社
Priority to JP2015524523A priority Critical patent/JP6329144B2/ja
Priority to CN201580003105.5A priority patent/CN105849820B/zh
Priority to KR1020167012326A priority patent/KR102410173B1/ko
Publication of WO2015174299A1 publication Critical patent/WO2015174299A1/fr

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    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J9/00—Adhesives characterised by their physical nature or the effects produced, e.g. glue sticks
    • C09J9/02—Electrically-conducting adhesives
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J11/00—Features of adhesives not provided for in group C09J9/00, e.g. additives
    • C09J11/02—Non-macromolecular additives
    • C09J11/04—Non-macromolecular additives inorganic
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J163/00—Adhesives based on epoxy resins; Adhesives based on derivatives of epoxy resins
    • C—CHEMISTRY; METALLURGY
    • C09—DYES; PAINTS; POLISHES; NATURAL RESINS; ADHESIVES; COMPOSITIONS NOT OTHERWISE PROVIDED FOR; APPLICATIONS OF MATERIALS NOT OTHERWISE PROVIDED FOR
    • C09J—ADHESIVES; NON-MECHANICAL ASPECTS OF ADHESIVE PROCESSES IN GENERAL; ADHESIVE PROCESSES NOT PROVIDED FOR ELSEWHERE; USE OF MATERIALS AS ADHESIVES
    • C09J201/00—Adhesives based on unspecified macromolecular compounds
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B1/00—Conductors or conductive bodies characterised by the conductive materials; Selection of materials as conductors
    • H01B1/20—Conductive material dispersed in non-conductive organic material
    • H01B1/22—Conductive material dispersed in non-conductive organic material the conductive material comprising metals or alloys
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B13/00—Apparatus or processes specially adapted for manufacturing conductors or cables
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B7/00—Insulated conductors or cables characterised by their form
    • H01B7/04—Flexible cables, conductors, or cords, e.g. trailing cables
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01B—CABLES; CONDUCTORS; INSULATORS; SELECTION OF MATERIALS FOR THEIR CONDUCTIVE, INSULATING OR DIELECTRIC PROPERTIES
    • H01B7/00—Insulated conductors or cables characterised by their form
    • H01B7/08—Flat or ribbon cables
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01R—ELECTRICALLY-CONDUCTIVE CONNECTIONS; STRUCTURAL ASSOCIATIONS OF A PLURALITY OF MUTUALLY-INSULATED ELECTRICAL CONNECTING ELEMENTS; COUPLING DEVICES; CURRENT COLLECTORS
    • H01R11/00—Individual connecting elements providing two or more spaced connecting locations for conductive members which are, or may be, thereby interconnected, e.g. end pieces for wires or cables supported by the wire or cable and having means for facilitating electrical connection to some other wire, terminal, or conductive member, blocks of binding posts
    • H01R11/01—Individual connecting elements providing two or more spaced connecting locations for conductive members which are, or may be, thereby interconnected, e.g. end pieces for wires or cables supported by the wire or cable and having means for facilitating electrical connection to some other wire, terminal, or conductive member, blocks of binding posts characterised by the form or arrangement of the conductive interconnection between the connecting locations
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/14—Structural association of two or more printed circuits
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/22—Secondary treatment of printed circuits
    • H05K3/28—Applying non-metallic protective coatings
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/30—Assembling printed circuits with electric components, e.g. with resistor
    • H05K3/32—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits
    • H05K3/34—Assembling printed circuits with electric components, e.g. with resistor electrically connecting electric components or wires to printed circuits by soldering
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K3/00—Apparatus or processes for manufacturing printed circuits
    • H05K3/36—Assembling printed circuits with other printed circuits
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L2224/10—Bump connectors; Manufacturing methods related thereto
    • H01L2224/11—Manufacturing methods
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L2224/00—Indexing scheme for arrangements for connecting or disconnecting semiconductor or solid-state bodies and methods related thereto as covered by H01L24/00
    • H01L2224/01—Means for bonding being attached to, or being formed on, the surface to be connected, e.g. chip-to-package, die-attach, "first-level" interconnects; Manufacturing methods related thereto
    • H01L2224/10—Bump connectors; Manufacturing methods related thereto
    • H01L2224/11—Manufacturing methods
    • H01L2224/115—Manufacturing methods by chemical or physical modification of a pre-existing or pre-deposited material
    • H01L2224/1152—Self-assembly, e.g. self-agglomeration of the bump material in a fluid

Definitions

  • the present invention relates to a conductive paste containing conductive particles and a method for manufacturing the conductive paste.
  • the present invention also relates to a connection structure using the conductive paste and a method for manufacturing the connection structure.
  • Anisotropic conductive materials such as anisotropic conductive paste and anisotropic conductive film are widely known.
  • anisotropic conductive material conductive particles are dispersed in a binder resin.
  • the anisotropic conductive material may be connected between a flexible printed circuit board and a glass substrate (FOG (Film on Glass)), or connected between a semiconductor chip and a flexible printed circuit board (COF ( (Chip on Film)), connection between a semiconductor chip and a glass substrate (COG (Chip on Glass)), connection between a flexible printed circuit board and a glass epoxy substrate (FOB (Film on Board)), and the like.
  • FOG Glass
  • COF Chip on Film
  • an anisotropic conductive material containing conductive particles is disposed on the glass epoxy substrate. To do.
  • a flexible printed circuit board is laminated, and heated and pressurized. As a result, the anisotropic conductive material is cured, and the electrodes are electrically connected via the conductive particles to obtain a connection structure.
  • Patent Document 1 includes a resin layer containing a thermosetting resin, solder powder, and a curing agent, and the solder powder and the curing agent include the resin layer.
  • An adhesive tape present therein is disclosed. This adhesive tape is in the form of a film, not a paste.
  • Patent Document 1 discloses a bonding method using the above-mentioned adhesive tape. Specifically, a first substrate, an adhesive tape, a second substrate, an adhesive tape, and a third substrate are laminated in this order from the bottom to obtain a laminate. At this time, the first electrode provided on the surface of the first substrate is opposed to the second electrode provided on the surface of the second substrate. Moreover, the 2nd electrode provided in the surface of the 2nd board
  • Patent Document 2 listed below includes (A) a silica filler having an average particle diameter of 3 to 100 nm that has been subjected to a hydrophobization treatment, (B) an adhesive component, and (C) a conductive particle. An isotropic conductive material is disclosed. In Patent Document 2, the amount of the silica filler is 10 to 60% by mass with respect to the total amount of the adhesive component.
  • Patent Document 3 listed below includes (1) an epoxy resin having an average of 1.2 or more epoxy groups in one molecule, and (2) a rubber having a softening point temperature of 0 ° C. or less and a primary particle diameter of 5 ⁇ m or less. -Like polymer fine particles, (3) thermally active latent epoxy curing agent, and (4) anisotropic conductive material having high softening point polymer fine particles having a softening point temperature of 50 ° C. or higher and a primary particle diameter of 2 ⁇ m or less Is disclosed.
  • the adhesive tape described in Patent Document 1 is a film, not a paste. For this reason, it is difficult to efficiently arrange the solder powder on the electrodes (lines). For example, in the adhesive tape described in Patent Document 1, a part of the solder powder is easily placed in a region (space) where no electrode is formed. Solder powder disposed in a region where no electrode is formed does not contribute to conduction between the electrodes.
  • the anisotropic conductive paste contains solder powder, the solder powder may not be efficiently disposed on the electrodes (lines).
  • the anisotropic conductive material described in Patent Document 2 may have low coatability when applied by screen printing or the like.
  • the solder powder can easily move onto the electrode (line).
  • the viscosity of the anisotropic conductive paste is lowered, the thickness of the anisotropic conductive paste layer after coating becomes thin, and the anisotropic conductive paste flows excessively and is disposed in an unintended region. It becomes easy to be.
  • the (1) epoxy resin is (1-1) an epoxy resin that is liquid in the temperature range of 0 to 50 ° C. and (1-2) a solid epoxy resin in the temperature range of 0 to 50 ° C.
  • an anisotropic conductive paste for example, “Epicron EP-1004”, which is a bisphenol A type epoxy resin, is dissolved in 1,6-hexanediol diglycidyl ether in Examples. Only a specific example in which a solid epoxy resin is dissolved is shown. Thus, even if the epoxy resin is solid at 25 ° C. alone, the epoxy resin is not always in a solid state in an anisotropic conductive paste, and the epoxy resin is generally used in a dissolved state. It is.
  • An object of the present invention is to produce a conductive paste and a conductive paste that can improve the coating property, and further can efficiently dispose conductive particles on the electrodes, and can improve the conduction reliability between the electrodes. Is to provide a method. Moreover, this invention is providing the manufacturing method of the connection structure and connection structure using the said electrically conductive paste.
  • the thermosetting component includes a thermosetting component and a plurality of conductive particles, and the thermosetting component contains a thermosetting compound that is solid at 25 ° C. and a thermosetting agent.
  • the thermosetting component contains a thermosetting compound that is solid at 25 ° C. and a thermosetting agent.
  • the conductive paste there is provided a conductive paste in which the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles.
  • the conductive paste contains a thermosetting compound that is liquid at 25 ° C.
  • thermosetting compound that is solid at 25 ° C. is a thermosetting epoxy compound that is solid at 25 ° C.
  • the thermosetting compound that is solid at 25 ° C. includes a first thermosetting compound that is solid at 25 ° C., and the first thermosetting compound. And a second thermosetting compound that has a different melting point and is solid at 25 ° C.
  • the conductive particles have solder on a conductive outer surface, and more preferably solder particles.
  • the melting point of the solder in the conductive particles at ⁇ 5 ° C. and 5 rpm is higher than the melting point of the solder in the conductive particles at ⁇ 5 ° C. and the viscosity at 0.5 rpm.
  • the ratio is 1 or more and 2 or less.
  • the particle size of the particulate thermosetting compound is 1 ⁇ m or more and 40 ⁇ m or less.
  • the ratio of the viscosity at 25 ° C. and 5 rpm to the viscosity at 25 ° C. and 0.5 rpm is 2.5 or more and 7 or less, and other specific aspects Then, the ratio of the viscosity at 25 ° C. and 5 rpm to the viscosity at 25 ° C. and 0.5 rpm is 4 or more and 7 or less.
  • the conductive paste includes a flux.
  • the conductive paste does not contain a filler or contains 100% by weight of the conductive paste in an amount of 1% by weight or less.
  • thermosetting component containing a thermosetting compound that is solid at 25 ° C., and a thermosetting agent, and a plurality of conductive properties. Particles are mixed to obtain a mixture, and then the mixture is heated above the melting point of the thermosetting compound that is solid at 25 ° C. and below the curing temperature of the thermosetting component, and solid at 25 ° C. The thermosetting compound is melted and solidified to obtain a conductive paste in which the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, or heat that is solid at 25 ° C.
  • thermosetting compound that is particulate and solid at 25 ° C. a thermosetting component containing a thermosetting agent, and a plurality of conductive particles after the curable compound is made into particles.
  • thermosetting compound that is solid at 25 ° C. thermosetting compound that is solid at 25 ° C.
  • a first connection target member having at least one first electrode on the surface
  • a second connection target member having at least one second electrode on the surface
  • the first connection A connection portion connecting the target member and the second connection target member, wherein the connection portion is formed of the conductive paste described above, and the first electrode and the second electrode
  • a connection structure that is electrically connected by the conductive particles in the connection portion.
  • the first connection target member is arranged to be disposed so as to face each other, and by heating the conductive paste to a temperature equal to or higher than the melting point of the thermosetting compound that is solid at 25 ° C. and higher than the curing temperature of the thermosetting component. And connecting the second connection target member with the conductive paste, and connecting the first electrode and the second electrode to the conductive particles in the connection portion. Electrically connecting with Comprising, a manufacturing method of the connecting structure is provided.
  • connection portion in the step of arranging the second connection target member and the step of forming the connection portion, no pressure is applied, and the conductive paste includes The weight of the second connection target member is added.
  • the second connection target member is a resin film, a flexible printed board, a flexible flat cable, or a rigid flexible board.
  • the conductive paste according to the present invention includes a thermosetting component and a plurality of conductive particles, and the thermosetting component contains a thermosetting compound that is solid at 25 ° C. and a thermosetting agent, Furthermore, in the conductive paste according to the present invention, the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, so that the coating property of the conductive paste can be improved. Furthermore, when the electrodes are electrically connected using the conductive paste according to the present invention, the conductive particles can be efficiently disposed on the electrodes, and the conduction reliability between the electrodes can be improved.
  • FIG. 1 is a partially cutaway front sectional view schematically showing a connection structure obtained using a conductive paste according to an embodiment of the present invention.
  • 2A to 2C are cross-sectional views for explaining each step of an example of a method for manufacturing a connection structure using the conductive paste according to the embodiment of the present invention.
  • FIG. 3 is a partially cutaway front sectional view showing a modified example of the connection structure.
  • FIG. 4 is a cross-sectional view schematically showing conductive particles that can be used in the conductive paste according to an embodiment of the present invention.
  • FIG. 5 is a cross-sectional view showing a modification of the conductive particles.
  • FIG. 6 is a cross-sectional view showing another modified example of conductive particles.
  • FIG. 7 is an image showing the thermosetting compound dispersed in the form of particles in the conductive paste according to the embodiment of the present invention.
  • the conductive paste according to the present invention includes a thermosetting component and a plurality of conductive particles.
  • the thermosetting component contains a thermosetting compound that is solid at 25 ° C. and a thermosetting agent.
  • the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles.
  • the above configuration is adopted, so that the coating property can be improved.
  • the conductive paste according to the present invention can be satisfactorily coated by a coating method such as dispenser and screen printing. If the viscosity of the anisotropic conductive paste is lowered, the conductive particles easily move onto the electrodes (lines).
  • the dispersion of the thermosetting compound that is solid at 25 ° C. in the conductive paste in the form of particles greatly contributes to improving the coating property. For example, the viscosity of the conductive paste becomes moderately high, the thixotropy of the conductive paste is appropriately expressed, the thickness of the conductive paste layer after coating is difficult to be thinned, and the conductive paste is difficult to flow excessively.
  • thermosetting compound that is solid at 25 ° C. is less likely to hinder the movement of the conductive particles onto the electrode as compared with the filler. In particular, if the thermosetting compound becomes liquid during the movement of the conductive particles onto the electrode, the liquid thermosetting compound does not hinder the movement of the conductive particles onto the electrode.
  • the above-described configuration is adopted. Therefore, when the electrodes are electrically connected, a plurality of conductive particles are interposed between the first electrode and the second electrode. It is easy to gather and a plurality of conductive particles can be efficiently arranged on the electrode (line). Moreover, it is difficult for some of the plurality of conductive particles to be disposed in a region (space) where no electrode is formed, and the amount of conductive particles disposed in a region where no electrode is formed can be considerably reduced. . Therefore, the conduction reliability between the first electrode and the second electrode can be improved. In addition, it is possible to prevent electrical connection between laterally adjacent electrodes that should not be connected, and to improve insulation reliability. The reason why such an effect is obtained is considered that the thermosetting compound that is solid at 25 ° C. is less likely to hinder the movement of the conductive particles onto the electrode as compared with the filler.
  • the conductive paste according to the present invention it is possible to obtain both the effect of improving the coating property and the effect of improving the conduction reliability between the electrodes achieved by the efficient movement of the conductive particles onto the electrodes. Can do. Further, in the conductive paste according to the present invention, when the conductive particles have solder on the conductive outer surface, the configuration of the particulate thermosetting compound and the configuration of the conductive particles that easily move in the conductive paste Synergistically exert the effects of the present invention more effectively. Furthermore, in the conductive paste according to the present invention, when the conductive particles are solder particles, the configuration of the particulate thermosetting compound and the configuration of the conductive particles that are particularly easily moved in the conductive paste are synergistic. The effect of the present invention is further effectively exhibited.
  • the method for producing a conductive paste according to the present invention comprises (1) a mixture of a thermosetting compound that is solid at 25 ° C. and a thermosetting component containing a thermosetting agent, and a plurality of conductive particles. The mixture is then heated to a temperature above the melting point of the thermosetting compound that is solid at 25 ° C. and below the curing temperature of the thermosetting component, and the thermosetting compound that is solid at 25 ° C. Or a solidified thermosetting compound in which the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, or (2) the thermosetting compound that is solid at 25 ° C.
  • thermosetting component that is particulate and solid at 25 ° C.
  • thermosetting component containing a thermosetting agent e.g., a thermosetting component containing a thermosetting agent
  • a thermosetting thermosetting epoxy compound that is solid at 25 ° C.
  • a thermosetting agent may be already mixed, and at 25 ° C., which is blended as necessary.
  • a liquid thermosetting compound may already be mixed.
  • the conductive particles contained in the conductive paste preferably have solder on the outer surface of the conductive material, and more preferably are solder particles. If such preferable conductive particles are used, the conductive particles can be arranged more efficiently on the electrode.
  • the conductive paste according to the present invention can be suitably used for the following manufacturing method of the connection structure according to the present invention.
  • a conductive paste, a first connection target member, and a second connection target member are used.
  • the conductive material used in the method for manufacturing a connection structure according to the present invention is not a conductive film but a conductive paste.
  • the conductive paste includes a plurality of conductive particles and a thermosetting component.
  • the first connection target member has at least one first electrode on the surface.
  • the second connection target member has at least one second electrode on the surface.
  • the method for manufacturing a connection structure includes a step of disposing the conductive paste on a surface of the first connection target member, and a surface opposite to the first connection target member side of the conductive paste.
  • the step of arranging the second connection object member so that the first electrode and the second electrode face each other, the melting point of the thermosetting compound that is solid at 25 ° C. and above By heating the conductive paste to a temperature equal to or higher than the curing temperature of the thermosetting component, a connection portion connecting the first connection target member and the second connection target member is formed with the conductive paste, And a step of electrically connecting the first electrode and the second electrode with conductive particles in the connection portion.
  • connection structure in the step of arranging the second connection target member and the step of forming the connection portion, no pressure is applied, and the second connection is applied to the conductive paste.
  • the weight of the target member is preferably added.
  • the conductive paste in the step of arranging the second connection target member and the step of forming the connection portion, has a weight force of the second connection target member. It is preferable not to apply a pressure higher than.
  • the plurality of conductive particles are easily collected between the first electrode and the second electrode, and the plurality of conductive particles are collected. It can arrange
  • a conductive film is used instead of a conductive film.
  • the inventors have found that it is necessary to use a paste.
  • the connection portion is The conductive particles arranged in the region (space) where the electrode is not formed before the formation becomes easier to gather between the first electrode and the second electrode, and the plurality of conductive particles are separated from the electrode ( The present inventors have also found that it can be arranged efficiently on the line).
  • a configuration in which a conductive paste is used instead of a conductive film and a configuration in which the weight of the second connection target member is added to the conductive paste without applying pressure are used in combination. This has a great meaning in order to obtain the effects of the present invention at a higher level.
  • WO2008 / 023452A1 describes that it is preferable to pressurize with a predetermined pressure at the time of bonding from the viewpoint of efficiently moving the solder powder to the electrode surface, and the pressurizing pressure further ensures the solder area.
  • the pressure is set to 0 MPa or more, preferably 1 MPa or more.
  • a predetermined pressure may be applied to the adhesive tape by its own weight.
  • the pressure applied intentionally to the adhesive tape may be 0 MPa, but there is no difference between the effect when the pressure exceeding 0 MPa is applied and when the pressure is set to 0 MPa. Not listed.
  • the thickness of the connecting portion can be adjusted as appropriate depending on the amount of the conductive paste applied.
  • the conductive film in order to change or adjust the thickness of the connection portion, it is necessary to prepare a conductive film having a different thickness or to prepare a conductive film having a predetermined thickness. There is.
  • connection portion is formed.
  • the first electrode and the second electrode are more firmly bonded to each other by the solder portion solidified after being melted. As a result, the conduction reliability between the electrodes is further enhanced.
  • FIG. 1 schematically shows a connection structure obtained by using a conductive paste according to an embodiment of the present invention in a partially cutaway front sectional view.
  • connection structure 1 shown in FIG. 1 is a connection that connects a first connection target member 2, a second connection target member 3, and the first connection target member 2 and the second connection target member 3.
  • Part 4 is formed with the electrically conductive paste containing a thermosetting component and several electroconductive particle.
  • the thermosetting component contains a thermosetting compound that is solid at 25 ° C. and a thermosetting agent.
  • the thermosetting compound that is solid at 25 ° C. It is dispersed in the form of particles.
  • solder particles are used as the conductive particles.
  • the connecting portion 4 includes a solder portion 4A (conductive particles) in which a plurality of solder particles gather and are joined to each other, and a cured product portion 4B in which a thermosetting component is thermally cured.
  • solder portion 4A conductive particles
  • cured product portion 4B in which a thermosetting component is thermally cured.
  • the first connection object member 2 has a plurality of first electrodes 2a on the surface (upper surface).
  • the second connection target member 3 has a plurality of second electrodes 3a on the surface (lower surface).
  • the first electrode 2a and the second electrode 3a are electrically connected by the solder portion 4A. Therefore, the first connection target member 2 and the second connection target member 3 are electrically connected by the solder portion 4A.
  • no solder exists in a region (cured product portion 4B portion) different from the solder portion 4A gathered between the first electrode 2a and the second electrode 3a.
  • connection structure 1 As shown in FIG. 1, in the connection structure 1, after a plurality of solder particles are melted, the molten solder particles are wetted and spread on the surface of the electrode to solidify to form a solder portion 4 ⁇ / b> A. For this reason, the connection area of 4 A of solder parts and the 1st electrode 2a, and 4 A of solder parts, and the 2nd electrode 3a becomes large. That is, by using the solder particles, the solder portion 4A, the first electrode 2a, and the solder portion are compared with the case where the conductive outer surface is made of a metal such as nickel, gold or copper. The contact area between 4A and the second electrode 3a increases. For this reason, the conduction
  • the conductive paste may contain a flux. In general, the flux contained in the conductive paste is gradually deactivated by heating.
  • connection structure 1 shown in FIG. 1 all of the solder portions 4A are located in the facing region between the first and second electrodes 2a and 3a.
  • the connection structure 1X of the modification shown in FIG. 3 is different from the connection structure 1 shown in FIG. 1 only in the connection portion 4X.
  • the connection part 4X has the solder part 4XA and the hardened
  • most of the solder portions 4XA are located in regions where the first and second electrodes 2a and 3a are opposed to each other, and a part of the solder portion 4XA is first and second. You may protrude to the side from the area
  • the solder part 4XA protruding laterally from the region where the first and second electrodes 2a and 3a are opposed is a part of the solder part 4XA and is not a solder separated from the solder part 4XA.
  • the amount of solder away from the solder portion can be reduced, but the solder away from the solder portion may exist in the cured product portion.
  • connection structure 1 If the amount of solder particles used is reduced, the connection structure 1 can be easily obtained. If the amount of the solder particles used is increased, it becomes easy to obtain the connection structure 1X.
  • connection structure 1 using the conductive paste according to the embodiment of the present invention will be described.
  • the first connection target member 2 having the first electrode 2a on the surface (upper surface) is prepared.
  • a conductive paste 11 including a thermosetting component 11B and a plurality of solder particles 11A is disposed on the surface of the first connection target member 2 (first step).
  • the conductive paste 11 is disposed on the surface of the first connection target member 2 on which the first electrode 2a is provided.
  • the solder particles 11A are disposed both on the first electrode 2a (line) and on a region (space) where the first electrode 2a is not formed.
  • the arrangement method of the conductive paste 11 is not particularly limited, and examples thereof include application with a dispenser, screen printing, and ejection with an inkjet device. Of these, screen printing is preferable.
  • a dispenser screen printing
  • screen printing is preferable.
  • the conductive paste according to the present invention applicability by screen printing is considerably improved, and even when screen printing is performed, the conductive paste layer can be formed to a predetermined thickness, and excessive wetting and spreading of the conductive paste can be achieved. This makes it difficult to place the conductive paste in an unintended region.
  • the 2nd connection object member 3 which has the 2nd electrode 3a on the surface (lower surface) is prepared.
  • the 2nd connection object member 3 is arrange
  • the second connection target member 3 is disposed from the second electrode 3a side. At this time, the first electrode 2a and the second electrode 3a are opposed to each other.
  • the conductive paste 11 is heated above the melting point of the thermosetting compound that is solid at 25 ° C. and above the curing temperature of the thermosetting component 11B (third step). That is, the conductive paste 11 is heated to a temperature lower than the melting point of the thermosetting compound that is solid at 25 ° C. and the curing temperature of the thermosetting component 11B.
  • the conductive paste 11 is heated above the melting point of the solder, that is, above the melting point of the solder particles 11A. At the time of this heating, the solder particles 11A that existed in the region where no electrode is formed gather between the first electrode 2a and the second electrode 3a (self-aggregation effect).
  • the solder particles 11A are effectively collected between the first electrode 2a and the second electrode 3a. Also, the solder particles 11A are melted and joined together. Further, the thermosetting component 11B is thermoset. As a result, as shown in FIG. 2C, the connection portion 4 connecting the first connection target member 2 and the second connection target member 3 is formed with the conductive paste 11.
  • the connection part 4 is formed by the conductive paste 11, the solder part 4A is formed by joining a plurality of solder particles 11A, and the cured part 4B is formed by thermosetting the thermosetting component 11B.
  • the first electrode 2a and the second electrode are moved after the movement of the solder particles 3 that are not positioned between the first electrode 2a and the second electrode 3a starts. It is not necessary to keep the temperature constant until the movement of the solder particles 3 is completed.
  • a preheating step may be provided in the first half of the third step.
  • This preheating step is a temperature at which the thermosetting component 11B is not substantially thermally cured at a temperature equal to or higher than the melting temperature of the solder in a state where the weight of the second connection target member 3 is added to the conductive paste 11. This refers to the process of heating for 5 to 60 seconds.
  • connection structure 1 shown in FIG. 1 is obtained.
  • the second step and the third step may be performed continuously.
  • the laminated body of the obtained 1st connection object member 2, the electrically conductive paste 11, and the 2nd connection object member 3 is moved to a heating part, and said 3rd said You may perform a process.
  • the laminate In order to perform the heating, the laminate may be disposed on a heating member, or the laminate may be disposed in a heated space.
  • the heating temperature in the third step is preferably not less than the melting point of the thermosetting compound that is solid at 25 ° C. and not less than the curing temperature of the thermosetting component 11B, and more than the melting point of the solder and curing of the thermosetting component. It is preferable that the temperature is higher.
  • the heating temperature is preferably 130 ° C. or higher, more preferably 160 ° C. or higher, preferably 450 ° C. or lower, more preferably 250 ° C. or lower, and still more preferably 200 ° C. or lower.
  • the temperature of the preheating step is preferably 100 ° C. or higher, more preferably 120 ° C. or higher, still more preferably 140 ° C. or higher, preferably less than 160 ° C., more preferably 150 ° C. or lower.
  • the said 1st connection object member should just have at least 1 1st electrode.
  • the first connection target member preferably has a plurality of first electrodes.
  • the said 2nd connection object member should just have at least 1 2nd electrode.
  • the second connection target member preferably has a plurality of second electrodes.
  • the first and second connection target members are not particularly limited. Specific examples of the first and second connection target members include electronic components such as semiconductor chips, capacitors, and diodes, and resin films, printed boards, flexible printed boards, flexible flat cables, rigid flexible boards, glass epoxies. Examples thereof include electronic components such as circuit boards such as substrates and glass substrates.
  • the first and second connection target members are preferably electronic components.
  • At least one of the first connection target member and the second connection target member is a resin film, a flexible printed board, a flexible flat cable, or a rigid flexible board.
  • the second connection target member is preferably a resin film, a flexible printed board, a flexible flat cable, or a rigid flexible board. Resin films, flexible printed boards, flexible flat cables, and rigid flexible boards have the property of being highly flexible and relatively lightweight. When a conductive film is used for connection of such a connection object member, there exists a tendency for electroconductive particle to collect on an electrode easily.
  • the conductive paste according to the present invention is used, even when a resin film, a flexible printed board, a flexible flat cable, or a rigid flexible board is used, the conductive particles are efficiently collected on the electrode. And the conduction reliability between the electrodes can be sufficiently enhanced.
  • the reliability of conduction between electrodes by not applying pressure compared to the case of using other connection target members such as a semiconductor chip. The improvement effect can be obtained more effectively.
  • the electrode provided on the connection target member examples include metal electrodes such as a gold electrode, a nickel electrode, a tin electrode, an aluminum electrode, a copper electrode, a silver electrode, a molybdenum electrode, a SUS electrode, and a tungsten electrode.
  • the electrode is preferably a gold electrode, a nickel electrode, a tin electrode, a silver electrode, or a copper electrode.
  • the electrode is preferably an aluminum electrode, a copper electrode, a molybdenum electrode, a silver electrode, or a tungsten electrode.
  • the electrode formed only with aluminum may be sufficient and the electrode by which the aluminum layer was laminated
  • the material for the metal oxide layer include indium oxide doped with a trivalent metal element and zinc oxide doped with a trivalent metal element.
  • the trivalent metal element include Sn, Al, and Ga.
  • the distance D1 of the connecting portion at the position where the first electrode and the second electrode face each other is preferably 3 ⁇ m or more, more preferably 10 ⁇ m or more, preferably 100 ⁇ m or less, more preferably 75 ⁇ m or less.
  • the distance D1 is equal to or greater than the lower limit, the connection reliability between the connection portion and the connection target member is further increased.
  • the distance D1 is less than or equal to the above upper limit, the conductive particles are more likely to gather on the electrodes when the connection portion is formed, and the conduction reliability between the electrodes is further enhanced.
  • the particle size of the thermosetting compound which is solid at 25 ° C. is preferably 0.1 ⁇ m or more, more preferably 1 ⁇ m or more, preferably 40 ⁇ m or less, more preferably 30 ⁇ m or less. Preferably it is 20 micrometers or less, Most preferably, it is 10 micrometers or less.
  • the particle diameter of the thermosetting compound that is solid at 25 ° C. in the form of particles indicates a number average particle diameter.
  • the particle size of the thermosetting compound that is solid at 25 ° C. that is in the form of particles is, for example, that 50 thermosetting compounds that are solid at 25 ° C. that are in an arbitrary particle shape are observed with an electron microscope or an optical microscope. It is obtained by calculating an average value.
  • the viscosity ⁇ 1 at 25 ° C. and 5 rpm of the conductive paste is preferably 10 Pa ⁇ s or more, more preferably 50 Pa ⁇ s or more, still more preferably 100 Pa ⁇ s or more, preferably 800 Pa ⁇ s or less, more preferably 600 Pa ⁇ s or less. More preferably, it is 500 Pa ⁇ s or less.
  • the viscosity ⁇ 1 is not less than the above lower limit and not more than the above upper limit, the coating property of the conductive paste and the arrangement accuracy of the conductive particles are further enhanced.
  • the viscosity ⁇ 2 of the conductive paste at 25 ° C. and 0.5 rpm is preferably 1 Pa ⁇ s or more, and preferably 100 Pa ⁇ s or less.
  • the viscosity ⁇ 2 is not less than the above lower limit and not more than the above upper limit, the coating property of the conductive paste and the arrangement accuracy of the conductive particles are further enhanced.
  • the ratio ( ⁇ 1 / ⁇ 2) of the viscosity ⁇ 1 at 25 ° C. and 5 rpm to the viscosity ⁇ 2 at 25 ° C. and 0.5 rpm is preferably 1 or more, more preferably 2.5 or more, still more preferably 4 or more, preferably It is 7 or less, more preferably 6 or less, and still more preferably 5 or less.
  • the ratio ( ⁇ 1 / ⁇ 2) is not less than the above lower limit and not more than the above upper limit, the coating property of the conductive paste and the placement accuracy of the conductive particles are further increased, and the conduction reliability between the electrodes is effectively increased. .
  • the melting point of the solder in the conductive particles is T ° C.
  • the ratio ( ⁇ 1 ′ / ⁇ 2 ′) of the viscosity ⁇ 1 ′ at (T-5) ° C. and 5 rpm to the viscosity ⁇ 2 ′ at (T-5) ° C. and 0.5 rpm is preferably 1 or more, preferably 2 or less. It is.
  • the ratio ( ⁇ 1 ′ / ⁇ 2 ′) is not less than the above lower limit and not more than the above upper limit, the arrangement accuracy of the conductive particles is further increased, and the conduction reliability between the electrodes is effectively increased.
  • the viscosity can be appropriately adjusted depending on the type of blending component, the blending amount of the blending component, and particularly the dispersion state of the thermosetting compound that is solid at 25 ° C.
  • the viscosity is, for example, using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd.) or the like, at 25 ° C. and 5 rpm, at 25 ° C. and 0.5 rpm, (T-5) ° C. and 5 rpm, and ( T-5) Measurement is possible under the conditions of ° C and 0.5 rpm.
  • E-type viscometer manufactured by Toki Sangyo Co., Ltd.
  • the conductive paste includes a thermosetting component and a plurality of conductive particles.
  • the said thermosetting component contains the thermosetting compound (curable compound which can be hardened
  • the conductive paste preferably contains a thermosetting compound that is liquid at 25 ° C. (a curable compound that can be cured by heating).
  • the conductive paste preferably contains a flux.
  • the conductive paste may contain a filler.
  • the conductive particles electrically connect the electrodes of the connection target member.
  • the conductive particles are not particularly limited as long as they are conductive particles.
  • the said electroconductive particle should just have an electroconductive part on the electroconductive outer surface.
  • Examples of the conductive particles include organic particles, inorganic particles other than metal particles, organic-inorganic hybrid particles, or metal particles whose surfaces are covered with a conductive layer (metal layer), or substantially only metal. Examples thereof include metal particles.
  • the conductive particles contained in the conductive paste preferably have solder on the conductive outer surface, and more preferably are solder particles.
  • solder particles conductive particles having solder on a conductive outer surface will be described.
  • FIG. 4 is a sectional view showing conductive particles that can be used in the conductive paste according to one embodiment of the present invention.
  • the 4 has base particles 52 (resin particles and the like) and conductive portions 53 arranged on the outer surface 52a of the base particles 52.
  • the conductive part 53 is a conductive layer.
  • the conductive portion 53 covers the outer surface 52 a of the base particle 52.
  • the conductive particles 51 are coated particles in which the outer surface 52 a of the base particle 52 is coated with the conductive portion 53. Accordingly, the conductive particles 51 have the conductive portions 53 on the outer surface 51a.
  • the conductive portion 53 includes a first conductive portion 54 (first conductive layer) disposed on the outer surface 52 a of the base particle 52 and a solder disposed on the outer surface 54 a of the first conductive portion 54.
  • Part 55 solder layer, second conductive part (second conductive layer)).
  • the outer surface portion (surface layer) of the conductive portion 53 is a solder portion 55. Therefore, the conductive particle 51 has a solder part 55 as a part of the conductive part 53, and is further provided between the base particle 52 and the solder part 55 as a part of the conductive layer 53 separately from the solder part 55.
  • 1 conductive portion 54 As described above, the conductive portion 53 may have a multilayer structure or may have a laminated structure of two or more layers.
  • the conductive portion 53 has a two-layer structure.
  • the conductive particles 61 may have a solder portion 62 as a single-layer conductive portion (conductive layer).
  • the surface part (surface layer) at least the outer side of the electroconductive part in electroconductive particle should just be a solder part.
  • the conductive particles 51 are preferable among the conductive particles 51 and the conductive particles 61 because the conductive particles can be easily produced.
  • the solder particles 11A that do not have the base particles in the core and are not core-shell particles may be used. In the solder particles 11A, both the central portion and the conductive outer surface are formed of solder.
  • Conductive particles 51 and 61 and solder particles 11A can be used in the conductive paste. From the viewpoint of effectively increasing the conduction reliability between the electrodes and also improving the connection reliability, among the conductive particles 51 and 61 and the solder particles 11A, the solder particles 11A are particularly preferable.
  • the conductive part is not particularly limited. Gold, silver, copper, nickel, palladium, tin, etc. are mentioned as a metal which comprises the said electroconductive part.
  • Examples of the conductive layer include a gold layer, a silver layer, a copper layer, a nickel layer, a palladium layer, or a conductive layer containing tin.
  • the conductive particle is composed of a resin particle and a conductive layer (on the surface of the resin particle ( First conductive layer).
  • the conductive particles are preferably conductive particles having at least a conductive outer surface of a low melting point metal layer. More preferably, the conductive particles have base particles and a conductive layer disposed on the surface of the base particles, and at least the outer surface of the conductive layer is a low melting point metal layer. More preferably, the conductive particles include base particles and conductive portions arranged on the surfaces of the base particles, and at least the outer surface of the conductive portions is a low melting point metal layer.
  • the solder is preferably a low melting point metal having a melting point of 450 ° C. or lower.
  • the solder particles are preferably low melting point metal particles having a melting point of 450 ° C. or lower.
  • the low melting point metal particles are particles containing a low melting point metal.
  • the low melting point metal is a metal having a melting point of 450 ° C. or lower.
  • the melting point of the low melting point metal is preferably 300 ° C. or lower, more preferably 160 ° C. or lower.
  • the solder contains tin. In 100% by weight of the metal contained in the solder, the content of tin is preferably 30% by weight or more, more preferably 40% by weight or more, still more preferably 70% by weight or more, and particularly preferably 90% by weight or more. When the content of tin in the solder is not less than the above lower limit, the connection reliability between the solder portion and the electrode is further enhanced.
  • the tin content is determined using a high-frequency inductively coupled plasma emission spectrometer (“ICP-AES” manufactured by Horiba, Ltd.) or a fluorescent X-ray analyzer (“EDX-800HS” manufactured by Shimadzu). It can be measured.
  • ICP-AES high-frequency inductively coupled plasma emission spectrometer
  • EDX-800HS fluorescent X-ray analyzer
  • the solder is melted and joined to the electrodes, and the solder portion conducts between the electrodes. For example, since the solder portion and the electrode are not in point contact but in surface contact, the connection resistance is lowered.
  • the use of conductive particles having solder on the outer surface increases the bonding strength between the solder part and the electrode. As a result, peeling between the solder part and the electrode is further less likely to occur. Reliability is effectively increased.
  • the low melting point metal constituting the solder is not particularly limited.
  • the low melting point metal is preferably tin or an alloy containing tin.
  • the alloy include a tin-silver alloy, a tin-copper alloy, a tin-silver-copper alloy, a tin-bismuth alloy, a tin-zinc alloy, and a tin-indium alloy.
  • the low melting point metal is preferably tin, a tin-silver alloy, a tin-silver-copper alloy, a tin-bismuth alloy, or a tin-indium alloy because of its excellent wettability with respect to the electrode. More preferred are a tin-bismuth alloy and a tin-indium alloy.
  • the solder is preferably a filler material having a liquidus of 450 ° C. or lower based on JIS Z3001: Welding terminology.
  • the composition of the solder include a metal composition containing zinc, gold, silver, lead, copper, tin, bismuth, indium and the like. Of these, a tin-indium system (117 ° C. eutectic) or a tin-bismuth system (139 ° C. eutectic) which is low-melting and lead-free is preferable. That is, the solder preferably does not contain lead, and preferably contains tin and indium, or contains tin and bismuth.
  • the solder may contain phosphorus and tellurium, and nickel, copper, antimony, aluminum, zinc, iron, gold, titanium, germanium, cobalt, Metals such as bismuth, manganese, chromium, molybdenum, and palladium may be included.
  • the solder preferably contains nickel, copper, antimony, aluminum, or zinc.
  • the content of these metals for increasing the bonding strength is preferably 0.0001% by weight or more, preferably 1% by weight in 100% by weight of the solder. It is as follows.
  • the average particle diameter of the conductive particles is preferably 0.5 ⁇ m or more, more preferably 1 ⁇ m or more, still more preferably 3 ⁇ m or more, particularly preferably 5 ⁇ m or more, preferably 100 ⁇ m or less, more preferably 30 ⁇ m or less, still more preferably 20 ⁇ m. Hereinafter, it is particularly preferably 15 ⁇ m or less, most preferably 10 ⁇ m or less.
  • the average particle diameter of the conductive particles is particularly preferably 3 ⁇ m or more and 30 ⁇ m or less.
  • the “average particle size” of the conductive particles indicates a number average particle size.
  • the average particle diameter of the conductive particles is obtained, for example, by observing 50 arbitrary conductive particles with an electron microscope or an optical microscope and calculating an average value.
  • the content of the conductive particles is preferably 0.1% by weight or more, more preferably 1% by weight or more, still more preferably 2% by weight or more, and further preferably 10% by weight or more. It is particularly preferably 20% by weight or more, most preferably 30% by weight or more, preferably 80% by weight or less, more preferably 60% by weight or less, and further preferably 50% by weight or less.
  • the content of the conductive particles is not less than the above lower limit and not more than the above upper limit, the conductive particles can be arranged more efficiently on the electrodes, and it is easy to arrange many conductive particles between the electrodes. Therefore, the conduction reliability is further enhanced. From the viewpoint of further improving the conduction reliability, the content of the conductive particles is preferably large.
  • thermosetting component Compound curable by heating: thermosetting component
  • the thermosetting compound is not particularly limited as long as it is solid at 25 ° C. and can be dispersed in the form of particles in the conductive paste.
  • the thermosetting compound that is solid at 25 ° C. is dispersed in the conductive paste.
  • FIG. 7 shows an image of the thermosetting compound dispersed in the form of particles in the conductive paste according to one embodiment of the present invention.
  • thermosetting compound that is solid at 25 ° C. examples include oxetane compounds, epoxy compounds, episulfide compounds, (meth) acrylic compounds, phenolic compounds, amino compounds, unsaturated polyester compounds, polyurethane compounds, silicone compounds, polyimide compounds, and polythiols. Etc. As for the said thermosetting compound which is solid at 25 degreeC, only 1 type may be used and 2 or more types may be used together.
  • thermosetting compound that is solid at 25 ° C. is It is preferably a thermosetting epoxy compound that is solid at 25 ° C. Moreover, connection reliability becomes still higher by using an epoxy compound.
  • the melting point of the thermosetting compound that is solid at 25 ° C. is preferably 40 ° C. or higher, more preferably 70 ° C. or higher, still more preferably 90 ° C. or higher, Preferably it is 160 degrees C or less, More preferably, it is 140 degrees C or less, More preferably, it is 120 degrees C or less.
  • thermosetting compound which is solid at 25 ° C. has a melting point different from that of the first thermosetting compound which is solid at 25 ° C. and the first thermosetting compound and is solid at 25 ° C. It is preferable to contain the 2nd thermosetting compound which is.
  • the absolute value of the difference between the melting point of the first thermosetting compound and the melting point of the second thermosetting compound is preferably 1 ° C. or more. Preferably it is 5 degreeC or more, More preferably, it is 10 degreeC or more, Preferably it is 30 degrees C or less, More preferably, it is 20 degrees C or less.
  • the conductive paste contains a thermosetting compound that is liquid at 25 ° C. It is preferable to include.
  • the thermosetting compound that is liquid at 25 ° C. include oxetane compounds, epoxy compounds, episulfide compounds, (meth) acrylic compounds, phenolic compounds, amino compounds, unsaturated polyester compounds, polyurethane compounds, silicone compounds, polyimide compounds, and polythiols. Etc.
  • the thermosetting compound that is liquid at 25 ° C. only one type may be used, or two or more types may be used in combination.
  • thermosetting compound that is liquid at 25 ° C. is a thermosetting epoxy compound that is liquid at 25 ° C. Is preferred.
  • the total content of the thermosetting compound that is solid at 25 ° C. and the thermosetting compound that is liquid at 25 ° C. in 100% by weight of the conductive paste is preferably 20% by weight or more, more preferably 40%. % By weight or more, more preferably 50% by weight or more, preferably 99% by weight or less, more preferably 98% by weight or less, still more preferably 90% by weight or less, and particularly preferably 80% by weight or less. From the viewpoint of further improving the impact resistance, it is preferable that the content of the thermosetting component is large.
  • the content of the thermosetting compound that is solid at 25 ° C. and the thermosetting epoxy compound that is solid at 25 ° C. in the conductive paste of 100% by weight is preferably 5% by weight or more, and more preferably 10% by weight. % Or more, preferably 70% by weight or less, more preferably 50% by weight or less.
  • the content of the thermosetting compound that is solid at 25 ° C. and the content of the thermosetting epoxy compound that is solid at 25 ° C. is not less than the above lower limit and not more than the above upper limit, the coating properties of the conductive paste and the conductive particles The placement accuracy is further increased.
  • the content of the thermosetting compound that is liquid at 25 ° C. and the thermosetting epoxy compound that is liquid at 25 ° C. is preferably 5% by weight or more, and more preferably 10% by weight in 100% by weight of the conductive paste. % Or more, preferably 70% by weight or less, more preferably 50% by weight or less.
  • the content of the thermosetting compound that is liquid at 25 ° C. and the content of the thermosetting epoxy compound that is liquid at 25 ° C. is not less than the above lower limit and not more than the above upper limit, The placement accuracy is further increased.
  • the difference in SP value between the thermosetting compound which is solid at 25 ° C. and the thermosetting compound which is liquid at 25 ° C. is preferably 0.5 or more, more preferably 1 or more, preferably 3 or less, more preferably 2 or less.
  • the difference in SP value is not less than the above lower limit and not more than the above upper limit, it can stably exist as particles of a thermosetting compound that is solid at 25 ° C., and the arrangement accuracy of the conductive particles of the conductive paste is more It gets even higher.
  • thermosetting agent thermosetting component
  • the thermosetting agent thermosets the thermosetting compound.
  • examples of the thermosetting agent include an imidazole curing agent, an amine curing agent, a phenol curing agent, a polythiol curing agent, an acid anhydride, a thermal cation initiator, and a thermal radical generator.
  • the said thermosetting agent only 1 type may be used and 2 or more types may be used together.
  • an imidazole curing agent, a polythiol curing agent, or an amine curing agent is preferable because the conductive paste can be cured more rapidly at a low temperature.
  • a latent curing agent is preferable.
  • the latent curing agent is preferably a latent imidazole curing agent, a latent polythiol curing agent or a latent amine curing agent.
  • the said thermosetting agent may be coat
  • the imidazole curing agent is not particularly limited, and 2-methylimidazole, 2-ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2, 4-Diamino-6- [2'-methylimidazolyl- (1 ')]-ethyl-s-triazine and 2,4-diamino-6- [2'-methylimidazolyl- (1')]-ethyl-s- Examples include triazine isocyanuric acid adducts.
  • the polythiol curing agent is not particularly limited, and examples thereof include trimethylolpropane tris-3-mercaptopropionate, pentaerythritol tetrakis-3-mercaptopropionate, and dipentaerythritol hexa-3-mercaptopropionate. .
  • the amine curing agent is not particularly limited, and hexamethylenediamine, octamethylenediamine, decamethylenediamine, 3,9-bis (3-aminopropyl) -2,4,8,10-tetraspiro [5.5].
  • examples include undecane, bis (4-aminocyclohexyl) methane, metaphenylenediamine, and diaminodiphenylsulfone.
  • thermal cation curing agent examples include iodonium cation curing agents, oxonium cation curing agents, and sulfonium cation curing agents.
  • examples of the iodonium-based cationic curing agent include bis (4-tert-butylphenyl) iodonium hexafluorophosphate.
  • examples of the oxonium-based cationic curing agent include trimethyloxonium tetrafluoroborate.
  • the sulfonium-based cationic curing agent examples include tri-p-tolylsulfonium hexafluorophosphate.
  • the thermal radical generator is not particularly limited, and examples thereof include azo compounds and organic peroxides.
  • examples of the azo compound include azobisisobutyronitrile (AIBN).
  • examples of the organic peroxide include di-tert-butyl peroxide and methyl ethyl ketone peroxide.
  • the reaction initiation temperature (curing temperature) of the thermosetting agent is preferably 50 ° C. or higher, more preferably 70 ° C. or higher, still more preferably 80 ° C. or higher, preferably 250 ° C. or lower, more preferably 200 ° C. or lower, still more preferably. 150 ° C. or lower, particularly preferably 140 ° C. or lower.
  • the reaction initiation temperature of the thermosetting agent is particularly preferably 80 ° C. or higher and 140 ° C. or lower.
  • the reaction initiation temperature of the thermosetting agent is preferably lower than the melting point of the solder in the conductive particles, and more preferably 5 ° C. or lower. More preferably, it is 10 ° C. or lower.
  • the reaction start temperature of the thermosetting agent means the temperature at which the exothermic peak of DSC starts to rise.
  • the content of the thermosetting agent is not particularly limited.
  • the content of the thermosetting agent is preferably 0.01 parts by weight or more, more preferably 1 part by weight or more, preferably 200 parts by weight or less with respect to 100 parts by weight of the thermosetting compound that is solid at 25 ° C.
  • the amount is more preferably 100 parts by weight or less, still more preferably 75 parts by weight or less, still more preferably 50 parts by weight or less, and particularly preferably 37.5 parts by weight or less.
  • the content of the thermosetting agent is preferably 0.01 parts by weight or more with respect to a total of 100 parts by weight of the thermosetting compound that is solid at 25 ° C. and the thermosetting compound that is liquid at 25 ° C.
  • thermosetting agent is 1 part by weight or more, preferably 200 parts by weight or less, more preferably 100 parts by weight or less, still more preferably 75 parts by weight or less.
  • content of the thermosetting agent is at least the above lower limit, it is easy to sufficiently cure the conductive paste.
  • content of the thermosetting agent is not more than the above upper limit, it is difficult for an excess thermosetting agent that did not participate in curing after curing to remain, and the heat resistance of the cured product is further enhanced.
  • the conductive paste preferably contains a flux.
  • the conductive particles are conductive particles having solder on a conductive surface, it is preferable to use a flux.
  • the flux is not particularly limited.
  • a flux generally used for soldering or the like can be used.
  • the flux include zinc chloride, a mixture of zinc chloride and an inorganic halide, a mixture of zinc chloride and an inorganic acid, a molten salt, phosphoric acid, a derivative of phosphoric acid, an organic halide, hydrazine, an organic acid, and pine resin.
  • Etc As for the said flux, only 1 type may be used and 2 or more types may be used together.
  • Examples of the molten salt include ammonium chloride.
  • Examples of the organic acid include lactic acid, citric acid, stearic acid, glutamic acid, and glutaric acid.
  • Examples of the pine resin include activated pine resin and non-activated pine resin.
  • the flux is preferably an organic acid having two or more carboxyl groups, pine resin.
  • the flux may be an organic acid having two or more carboxyl groups, or pine resin.
  • the above rosins are rosins whose main component is abietic acid.
  • the flux is preferably rosins, and more preferably abietic acid. By using this preferable flux, the conduction reliability between the electrodes is further enhanced.
  • the melting point of the flux is preferably 50 ° C. or higher, more preferably 70 ° C. or higher, still more preferably 80 ° C. or higher, preferably 200 ° C. or lower, more preferably 160 ° C. or lower, even more preferably 150 ° C. or lower, still more preferably. 140 ° C. or lower.
  • the melting point of the flux is preferably 80 ° C. or higher and 190 ° C. or lower.
  • the melting point of the flux is particularly preferably 80 ° C. or higher and 140 ° C. or lower.
  • Examples of the flux having a melting point of 80 ° C. or higher and 190 ° C. or lower include succinic acid (melting point 186 ° C.), glutaric acid (melting point 96 ° C.), adipic acid (melting point 152 ° C.), pimelic acid (melting point 104 ° C.), suberic acid
  • Examples thereof include dicarboxylic acids such as (melting point 142 ° C.), benzoic acid (melting point 122 ° C.), and malic acid (melting point 130 ° C.).
  • the boiling point of the flux is preferably 200 ° C. or lower.
  • the melting point of the flux is preferably lower than the melting point of the solder in the solder particles, more preferably 5 ° C. or more, more preferably 10 ° C. or more. Is more preferable.
  • the melting point of the flux is preferably lower than the reaction start temperature of the thermosetting agent, more preferably 5 ° C. or more, and more preferably 10 ° C. or less. More preferably.
  • the flux may be dispersed in the conductive paste or may be adhered on the surface of the conductive particles.
  • the content of the flux is preferably 0.5% by weight or more, preferably 30% by weight or less, more preferably 25% by weight or less.
  • the conductive paste may not contain a flux.
  • the flux content is not less than the above lower limit and not more than the above upper limit, it becomes more difficult to form an oxide film on the surface of the solder and the electrode, and the oxide film formed on the surface of the solder and the electrode is more effective. Can be removed.
  • the conductive paste may contain a filler.
  • the filler By using the filler, the latent heat expansion of the cured product of the conductive paste can be suppressed.
  • it is better not to use a filler and in the case of using a filler, the smaller the filler content is, the better.
  • the conductive paste does not contain a filler or contains a filler in an amount of 1% by weight or less in 100% by weight of the conductive paste.
  • the filler content is more preferably 0.5% by weight or less.
  • the filler examples include inorganic fillers such as silica, talc, aluminum nitride, and alumina.
  • the filler may be an organic filler or an organic-inorganic composite filler. As for the said filler, only 1 type may be used and 2 or more types may be used together.
  • the conductive paste is, for example, a filler, an extender, a softener, a plasticizer, a polymerization catalyst, a curing catalyst, a colorant, an antioxidant, a heat stabilizer, a light stabilizer, an ultraviolet absorber, and a lubricant.
  • various additives such as an antistatic agent and a flame retardant may be included.
  • the polymer A is a structural unit in which a hydroxyl group derived from bisphenol F and 1,6-hexanediol diglycidyl ether and an epoxy group of a bisphenol F-type epoxy resin are bonded. In the main chain and having an epoxy group at both ends.
  • Polymer A obtained by GPC had a weight average molecular weight of 10,000 and a number average molecular weight of 3,500.
  • Polymer B both ends epoxy group rigid skeleton phenoxy resin, “YX6900BH45” manufactured by Mitsubishi Chemical Corporation, weight average molecular weight 16000
  • thermosetting compound 1 solid at 25 ° C, thermosetting epoxy compound, “EX-201” manufactured by Nagase ChemteX Corporation, crystallized at ⁇ 5 ° C., washed with hexane, and hexane removed by vacuum drying use
  • thermosetting compound 2 solid at 25 ° C, thermosetting epoxy compound, “HP-4032D” manufactured by DIC is crystallized at ⁇ 5 ° C., washed with hexane, and used after removing hexane by vacuum drying)
  • thermosetting compound 3 liquid at 25 ° C., thermosetting epoxy compound, “1,6-hexanediol glycidyl ether” manufactured by Yokkaichi Gosei Co., Ltd.
  • thermosetting compound 4 liquid at 25 ° C, thermosetting polythiol compound, Showa Denko "Karenz MT PE1"
  • thermosetting compound 5 solid at 25 ° C, thermosetting epoxy compound, ADEKA “EP-3300” crystallized at -5 ° C, washed with hexane, hexane removed by vacuum drying
  • thermosetting compound 6 solid at 25 ° C, thermosetting epoxy compound, "TEPIC-SS” manufactured by Nissan Chemical Co., Ltd. crystallized at -5 ° C, washed with hexane, hexane removed by vacuum drying and used )
  • thermosetting compound 7 solid at 25 ° C, thermosetting epoxy compound, "TEP-G” manufactured by Asahi Organic Materials Co., Ltd. is crystallized at -5 ° C, washed with hexane, and hexane removed by vacuum drying. After use)
  • Conductive particles 1 (SnBi solder particles, melting point 139 ° C., “ST-5” manufactured by Mitsui Kinzoku Co., Ltd., average particle size 5.4 ⁇ m)
  • Conductive particles 2 (SnBi solder particles, melting point 139 ° C., Mitsui Kinzoku “DS-10”, average particle size 12 ⁇ m)
  • Conductive particles 3 (resin core solder coated particles, prepared by the following procedure) Divinylbenzene resin particles (“Micropearl SP-207” manufactured by Sekisui Chemical Co., Ltd., average particle diameter: 7 ⁇ m) were subjected to electroless nickel plating to form a base nickel plating layer having a thickness of 0.1 ⁇ m on the surface of the resin particles. Next, the resin particles on which the base nickel plating layer was formed were subjected to electrolytic copper plating to form a 1 ⁇ m thick copper layer. Furthermore, electrolytic plating was performed using an electrolytic plating solution containing tin and bismuth to form a solder layer having a thickness of 1 ⁇ m.
  • Conductive particles (average particle diameter 14 ⁇ m, resin core solder-coated particles) were prepared.
  • Conductive particles 4 Au plated particles of divinylbenzene resin particles (“Au-210” manufactured by Sekisui Chemical Co., Ltd., average particle size 10 ⁇ m)
  • Phenoxy resin (“YP-50S” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.)
  • FR-4 substrate having a copper electrode pattern (copper electrode thickness 10 ⁇ m) having an L / S of 50 ⁇ m / 50 ⁇ m on the upper surface
  • Second connection object member the flexible printed circuit board (2nd connection object member) which has a copper electrode pattern (copper electrode thickness 10 micrometers) whose L / S is 50 micrometers / 50 micrometers on the lower surface was prepared.
  • the overlapping area of the glass epoxy substrate and the flexible printed board was 1.5 cm ⁇ 4 mm, and the number of connected electrodes was 75 pairs.
  • the anisotropic conductive paste immediately after fabrication was applied to the upper surface of the glass epoxy substrate so as to have a thickness of 50 ⁇ m by screen printing to form an anisotropic conductive paste layer.
  • the flexible printed circuit board was laminated on the upper surface of the anisotropic conductive paste layer so that the electrodes face each other. At this time, no pressure was applied.
  • the weight of the flexible printed board is added to the anisotropic conductive paste layer. Thereafter, while heating the anisotropic conductive paste layer to a temperature of 185 ° C., the solder was melted and the anisotropic conductive paste layer was cured at 185 ° C. to obtain a first connection structure.
  • Glass epoxy substrate (FR-4 substrate) having a copper electrode pattern (copper electrode thickness 10 ⁇ m) having L / S of 75 ⁇ m / 75 ⁇ m on the upper surface (First connection object member) was prepared.
  • the flexible printed circuit board (2nd connection object member) which has a copper electrode pattern (copper electrode thickness 10 micrometers) whose L / S is 75 micrometers / 75 micrometers on the lower surface was prepared.
  • 2nd connection structure was obtained like manufacture of the 1st connection structure except having used the above-mentioned glass epoxy board and flexible printed circuit board from which L / S differs.
  • 3rd connection structure was obtained like manufacture of the 1st connection structure except having used the above-mentioned glass epoxy board and flexible printed circuit board from which L / S differs.
  • the flexible printed circuit board (second connection target member) for obtaining the first connection structure was stored at 120 ° C. and a humidity of 20% for 1 hour.
  • a fourth connection structure was obtained in the same manner as the first connection structure except that the first and second connection target members after storage were used.
  • the flexible printed circuit board (second connection target member) for obtaining the second connection structure was stored at 120 ° C. and a humidity of 20% for 1 hour.
  • a fifth connection structure was obtained in the same manner as the production of the second connection structure except that the first and second connection target members after storage were used.
  • the flexible printed circuit board (second connection target member) for obtaining the third connection structure was stored at 120 ° C. and a humidity of 20% for 1 hour. Except having used the 1st, 2nd connection object member after storage, it carried out similarly to preparation of the 3rd connection structure, and obtained the 6th connection structure.
  • the electrode size / inter-electrode space is 50 ⁇ m / 50 ⁇ m (for the first and fourth connection structures), 75 ⁇ m / 75 ⁇ m (for the second and fifth connection structures), 100 ⁇ m / 100 ⁇ m (the third and sixth A glass epoxy substrate (size 30 ⁇ 30 mm, thickness 0.4 mm) having a 5 mm square semiconductor chip (thickness 400 ⁇ m) and an electrode facing it is used for the connection structure. 4th, 5th and 6th connection structures were obtained.
  • phenoxy resin (“YP-50S” manufactured by Nippon Steel & Sumikin Chemical Co., Ltd.) was dissolved in methyl ethyl ketone (MEK) so that the solid content was 50% by weight to obtain a solution.
  • MEK methyl ethyl ketone
  • Ingredients other than the phenoxy resin shown in Table 2 below were blended with the blending amounts shown in Table 2 below and the total amount of the above solution, and after stirring for 5 minutes at 2000 rpm using a planetary stirrer, a bar coater was used. It was coated on a release PET (polyethylene terephthalate) film so that the thickness after drying was 30 ⁇ m.
  • An anisotropic conductive film was obtained by removing MEK by vacuum drying at room temperature.
  • the 1st, 2nd, 3rd, 4th, 5th, 6th connection structure was obtained like Example 1 except having used the anisotropic conductive film.
  • Viscosity The viscosity ⁇ 1 at 25 ° C. and 5 rpm of the anisotropic conductive paste was measured using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd.). Further, the viscosity ⁇ 2 at 25 ° C. and 0.5 rpm of the anisotropic conductive paste was measured using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd.). The ratio ( ⁇ 1 / ⁇ 2) was determined from the measured values obtained.
  • the melting point of the solder in the conductive particles of the anisotropic conductive paste was measured at ⁇ 5 ° C. and the viscosity ⁇ 1 ′ at 5 rpm using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd.). Further, the melting point of the solder in the conductive particles of the anisotropic conductive paste was measured at ⁇ 5 ° C. and the viscosity ⁇ 2 ′ at 0.5 rpm using an E-type viscometer (manufactured by Toki Sangyo Co., Ltd.). The ratio ( ⁇ 1 ′ / ⁇ 2 ′) was determined from the obtained measured values. The ratio ( ⁇ 1 ′ / ⁇ 2 ′) was determined according to the following criteria.
  • thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, and the particle size of the particulate thermosetting compound is 1 ⁇ m or more and 10 ⁇ m or less.
  • the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, and the particle size of the particulate thermosetting compound is more than 10 ⁇ m and not more than 40 ⁇ m ⁇ :
  • the thermosetting compound that is solid at 25 ° C. is dispersed in the form of particles, and the particle size of the particulate thermosetting compound exceeds 40 ⁇ m.
  • X Solid at 25 ° C. in the conductive paste Some thermosetting compounds are not dispersed in particulate form
  • ⁇ Can be applied with a thickness variation of less than 5 ⁇ m, and the anisotropic conductive paste does not wet and spread in unintended areas.
  • ⁇ Can be applied with a thickness variation of 5 ⁇ m or more and less than 10 ⁇ m, and intended. The anisotropic conductive paste does not wet and spread in the areas where it does not.
  • X Thickness variation of 10 ⁇ m or more occurs after coating, or the anisotropic conductive paste wets and spreads in unintended areas
  • ⁇ Average value of connection resistance is 10 7 ⁇ or more ⁇ : Average value of connection resistance is 10 6 ⁇ or more, less than 10 7 ⁇ ⁇ : Average value of connection resistance is 10 5 ⁇ or more, less than 10 6 ⁇ ⁇ : Connection The average resistance is less than 10 5 ⁇
  • the second connection target member is a flexible printed circuit board
  • the second connection target member is It can be seen that the effect of improving the conduction reliability by using the conductive paste of the present invention can be obtained more effectively than in the case of a semiconductor chip.
  • the evaluation of conduction reliability (results OO) of Examples 16 and 17 since a plurality of thermosetting compounds that are solid at 25 ° C. having different melting points are used, the evaluation of other examples (results ⁇ ) The specific value of the connection resistance was lower than (including ⁇ ). In Examples 16 and 17, the conduction reliability was particularly excellent as compared with the other examples.

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  • Engineering & Computer Science (AREA)
  • Chemical & Material Sciences (AREA)
  • Manufacturing & Machinery (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Organic Chemistry (AREA)
  • Dispersion Chemistry (AREA)
  • Physics & Mathematics (AREA)
  • Spectroscopy & Molecular Physics (AREA)
  • Inorganic Chemistry (AREA)
  • Conductive Materials (AREA)
  • Non-Insulated Conductors (AREA)
  • Adhesives Or Adhesive Processes (AREA)
  • Combinations Of Printed Boards (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Manufacturing Of Electrical Connectors (AREA)

Abstract

Cette invention concerne une pâte conductrice permettant d'améliorer les propriétés de revêtement, d'assurer une disposition efficace des particules conductrices sur des électrodes, et d'améliorer la fiabilité de la conduction entre des électrodes. Ladite pâte conductrice comprend un composant thermodurcissable et une pluralité de particules conductrices. Ledit composant thermodurcissable contient un composé thermodurcissable qui est solide à 25 °C et un agent thermodurcissable. Ledit composé thermodurcissable qui est solide à 25 °C est diffusé sous forme de particules dans la pâte conductrice.
PCT/JP2015/063095 2014-05-14 2015-05-01 Pâte conductrice, procédé de production d'une pâte conductrice, structure de connexion, et procédé de production de structure de connexion WO2015174299A1 (fr)

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CN201580003105.5A CN105849820B (zh) 2014-05-14 2015-05-01 导电糊剂、导电糊剂的制造方法、连接结构体及连接结构体的制造方法
KR1020167012326A KR102410173B1 (ko) 2014-05-14 2015-05-01 도전 페이스트, 도전 페이스트의 제조 방법, 접속 구조체 및 접속 구조체의 제조 방법

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JP6849374B2 (ja) * 2016-10-06 2021-03-24 イー・アイ・デュポン・ドウ・ヌムール・アンド・カンパニーＥ．Ｉ．Ｄｕ Ｐｏｎｔ Ｄｅ Ｎｅｍｏｕｒｓ Ａｎｄ Ｃｏｍｐａｎｙ 接合用の導電性ペースト
KR20190098709A (ko) 2018-02-14 2019-08-22 에피스타 코포레이션 발광 장치, 그 제조 방법 및 디스플레이 모듈
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JP7400926B2 (ja) 2018-08-06 2023-12-19 株式会社レゾナック 伸縮性樹脂形成用熱硬化性組成物、伸縮性樹脂、及び半導体装置
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TWI672710B (zh) 2019-09-21
KR102410173B1 (ko) 2022-06-20
JPWO2015174299A1 (ja) 2017-04-20
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JP6329144B2 (ja) 2018-05-23

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