KR102467385B1 - Connection structure, circuit connection member and adhesive composition - Google Patents

Abstract

The present invention provides a first circuit member having a first circuit electrode, a second circuit member having a second circuit electrode, and provided between the first circuit member and the second circuit member, the first circuit electrode and the second circuit electrode. are provided with circuit connecting members electrically connecting them to each other, and the amount of linear thermal expansion L(t) at temperature t of the circuit connecting members is dL(t)/dt<0 at least in any one of t=30°C to 12°C. A connection structure that satisfies the condition is provided.

Description

Connection structure, circuit connection member and adhesive composition

The present invention relates to a connection structure, a circuit connection member, and an adhesive composition.

Conventionally, in semiconductor devices and display devices, various adhesives are used for the purpose of bonding various circuit members in the device to each other. Regarding adhesives, in addition to adhesiveness, various properties such as heat resistance and reliability in high temperature and high humidity conditions are required. Further, circuit members include, for example, printed wiring boards, organic substrates such as polyimide, metals such as titanium, copper, and aluminum, and members having various surface states such as ITO, IZO, IGZO, SiN, and SiO ₂ . Because it is used, the material used for the adhesive needs to be molecularly designed according to the circuit member.

In recent years, the use of amorphous (amorphous) ITO films, organic insulating films, and the like for circuit members has also increased for the purpose of simplifying and lowering the manufacturing process of semiconductor elements and display elements, and lowering the temperature. These film surfaces are often unfavorable to adhesion from the physical point of view of low surface irregularities or from the chemical point of view of low wettability of the surface.

On the other hand, in order to strengthen the adhesion between the circuit connecting member obtained by curing the adhesive and the circuit member, mutual bonding, hydrogen bonding, hydrophobic interaction by van der Waals force, etc. between the circuit connecting member and the surface of the circuit member. Additives such as coupling agents that generate action may be added to adhesives. As the coupling agent, a silane coupling agent, a coupling agent having a phosphoric acid group, a carboxyl group, or the like is used. For example, an organic functional group such as an epoxy group, an acryloyl group, or a vinyl group is present in a resin constituting the circuit connection member, and an alkoxysilane structure that causes an interaction between the circuit member surface and the circuit connection member, a phosphoric acid group, or the like is present. When a coupling agent is used, it becomes possible to further firmly bond the circuit member and the circuit connection member (see Patent Documents 1 to 3).

Japanese Unexamined Patent Publication No. 2003-282637 Japanese Unexamined Patent Publication No. 2003-277694 Japanese Unexamined Patent Publication No. 2013-191625

However, according to the study of the present inventors, when the additives described above are used, the interaction between the circuit connecting members and the circuit members does not function effectively depending on the type of circuit members under a high temperature and high humidity environment, and the circuit connecting members There exists a problem that it peels off from a circuit member.

Then, an object of this invention is to provide the connection structure which can suppress peeling of a circuit connection member from a circuit member, and the circuit connection member used for this connection structure, and adhesive composition even in a high-temperature, high-humidity environment.

In one aspect, the present invention provides a first circuit member having a first circuit electrode, a second circuit member having a second circuit electrode, and provided between the first circuit member and the second circuit member, and the first circuit electrode and a circuit connecting member electrically connecting the second circuit electrodes to each other, wherein the linear thermal expansion L(t) at temperature t of the circuit connecting member is dL(t) at least any temperature t between t=30°C and 120°C )/dt<0, a connection structure is provided.

In another aspect of the present invention, a circuit connecting member is provided, wherein the amount of linear thermal expansion L(t) at temperature t of the circuit connecting member is dL(t)/dt< A circuit connecting member that satisfies the condition of 0 is provided.

The average coefficient of linear thermal expansion of the circuit connecting member at 30°C to 120°C is preferably 500 ppm/°C or less.

In another aspect, the present invention is an adhesive composition, wherein the amount of linear thermal expansion l(t) at temperature t of a cured product of the adhesive composition is dl(t)/dt< An adhesive composition that satisfies the condition of 0 is provided.

The average linear thermal expansion coefficient of the cured product at 30°C to 120°C is preferably 500 ppm/°C or less.

ADVANTAGE OF THE INVENTION According to this invention, the connection structure which can suppress peeling of a circuit connection member from a circuit member even under a high-temperature, high-humidity environment, and the circuit connection member and adhesive composition used for this connection structure can be provided.

1 is a schematic cross-sectional view showing one embodiment of a connection structure.
2 is a graph showing an example of the relationship between temperature and linear thermal expansion amount.

EMBODIMENT OF THE INVENTION Hereinafter, embodiment of this invention is described in detail. However, this invention is not limited to the following embodiment. “(meth)acrylic acid” means acrylic acid or methacrylic acid, and the same applies to other similar expressions such as (meth)acrylate.

1 is a schematic cross-sectional view showing an embodiment of a connection structure. As shown in FIG. 1, the connection structure 1 is provided between the 1st circuit member 2, the 2nd circuit member 3, and the 1st circuit member 2 and the 2nd circuit member 3. A circuit connecting member 4 is provided.

The first circuit member 2 includes a first substrate 5 and a first circuit electrode 6 provided on a main surface of the first substrate 5 . The second circuit member 3 includes a second substrate 7 and a second circuit electrode 8 provided on the main surface of the second substrate 7 .

The first and second circuit members 2 and 3 may be the same or different, and may be chip components such as semiconductor chips, resistor chips, and capacitor chips, substrates such as printed circuit boards, and the like. The first and second substrates 5 and 7 may be formed of inorganic substances such as semiconductors, glass and ceramics, organic substances such as polyimide and polycarbonate, composites such as glass/epoxy, and the like. The first and second circuit electrodes 6 and 8 may be formed of gold, silver, tin, ruthenium, rhodium, palladium, osmium, iridium, platinum, crystalline or amorphous indium tin oxide (ITO), or the like.

On the substrates 5 and 7 of these circuit members 2 and 3, a plurality of circuit electrodes 6 and 8 are usually provided (single number may be sufficient depending on the case). The first and second circuit members 2 and 3 are arranged such that at least one pair of first circuit electrode 6 and second circuit electrode 8 face each other.

The circuit connecting member 4 contains the cured product 9 of the adhesive component and the conductive particles 10 dispersed in the cured product 9 of the adhesive component. When the conductive particles 10 in the circuit connection member 4 are interposed between the first circuit electrode 6 and the second circuit electrode 8 that face each other, the first circuit electrode 6 and the second circuit electrode ( 8) are electrically connected to each other.

From the viewpoint of suppressing separation of the circuit connecting member 4 from the circuit members 2 and 3 and the circuit electrodes 6 and 8, the circuit connecting member 4 has a temperature of t ° C. A circuit connecting member in which the amount of linear thermal expansion L(t) µm satisfies the condition of dL(t)/dt<0 at at least a certain temperature t between t=30°C and 120°C.

The amount of linear thermal expansion L(t) of the circuit connecting member 4 was measured using a thermomechanical analyzer, with a length of 10 mm, a width of 4 mm and a thickness of 0.1 mm, a load of 5 gf (per sectional area of 0.4 mm), and a heating rate of 5°C/min. Under the condition of t = 0 ° C to 200 ° C, every 0.1 ° C, as the linear thermal expansion (μm) at the temperature t ° C when the linear thermal expansion at the temperature t = 0 ° C L (0) = 0 μm It is measured. The amount of linear thermal expansion here means the amount of linear thermal expansion in the longitudinal direction of the sample.

The amount of linear thermal expansion L(t) of the circuit connecting member 4 is t = 30°C from the viewpoint of suppressing separation of the circuit connecting member 4 from the circuit members 2, 3 and the circuit electrodes 6, 8. At at least a certain temperature t of 120°C to 120°C, the condition of dL(t)/dt<0 is satisfied, preferably dL(t)/dt≤-0.01, more preferably dL(t)/dt≤-0.1 , more preferably satisfies the condition of dL(t)/dt≤-0.5.

The amount of linear thermal expansion L(t) of the circuit connecting member 4 is preferably t from the viewpoint of suppressing separation of the circuit connecting member 4 from the circuit members 2, 3 and the circuit electrodes 6, 8. At least any temperature t of = 30°C to 100°C, more preferably t = 30°C to 90°C, even more preferably t = 30°C to 80°C, the above condition of dL(t)/dt is satisfied.

The average coefficient of linear thermal expansion of the circuit connecting member 4 at 30°C to 120°C is from the viewpoint of suppressing peeling of the circuit connecting member 4 from the circuit members 2, 3 and the circuit electrodes 6, 8. , It is preferably 500 ppm/°C or less, more preferably 250 ppm/°C or less, and still more preferably 150 ppm/°C or less.

The coefficient of linear thermal expansion (ppm/°C) of the circuit connecting member 4 is defined as the amount of linear thermal expansion (μm) per 1°C of temperature rise in a length of 1 m of the circuit connecting member 4. The average linear thermal expansion coefficient α _L of the circuit connecting member 4 at 30° C. to 120° C. is the linear thermal expansion amount L at t = 30° C. to 120° C. of the circuit connecting member 4 measured according to the method described above ( t) The amount of change in [unit: μm/10 mm] is converted into the amount of linear thermal expansion (μm) in the length of 1 m of the circuit connecting member 4, and from the converted value as an average value per 1 ° C. of temperature rise (that is, in the following formula Therefore) is calculated.

α _L = {L(t=120°C)-L(t=30°C)}×100/(120-30)

The cured material 9 of the adhesive component constituting the circuit connecting member 4 and the conductive particles 10 are selected so that the circuit connecting member 4 has the above characteristics. The circuit connection member 4 is obtained by hardening the adhesive composition containing the adhesive component and the electroconductive particle 10, for example. From the viewpoint of suppressing peeling of the circuit connecting member 4 from the circuit members 2 and 3 and the circuit electrodes 6 and 8, such an adhesive composition is preferably a line at the temperature t of the cured product of the adhesive composition. An adhesive composition in which the amount of thermal expansion l(t) satisfies the condition of dl(t)/dt<0 at least at any temperature t of t=30°C to 120°C. The cured product of the adhesive composition may be, for example, a cured product obtained by molding the adhesive composition into a film adhesive having a thickness of 100±20 μm and heating the film adhesive at 180° C. for 1 hour.

The amount of linear thermal expansion l(t) of the cured product of the adhesive composition was measured using a thermomechanical analysis device, at a sample length of 10 mm, a width of 4 mm and a thickness of 0.1 mm, a load of 5 gf (per 0.4 mm2 of cross-sectional area of the sample), and a heating rate of 5 °C/min. Under the condition of t = 0 ° C to 200 ° C, every 0.1 ° C, as the linear thermal expansion (μm) at the temperature t ° C when the linear thermal expansion at the temperature t = 0 ° C is l (0) = 0 μm It is measured. The amount of linear thermal expansion here means the amount of linear thermal expansion in the longitudinal direction of the sample.

The amount of linear thermal expansion 1 (t) of the cured product of the adhesive composition is determined from the viewpoint of suppressing peeling of the cured product of the adhesive composition (circuit connecting member 4) from the circuit members 2, 3 and circuit electrodes 6, 8. , at least any temperature t between t = 30 ° C and 120 ° C, dl (t) / dt ≤ -0.01, more preferably dl (t) / dt ≤ -0.1, more preferably dl (t) / dt ≤ It satisfies the condition of -0.5.

The amount of linear thermal expansion 1 (t) of the cured product of the adhesive composition is determined from the viewpoint of suppressing peeling of the cured product of the adhesive composition (circuit connecting member 4) from the circuit members 2, 3 and circuit electrodes 6, 8. , at least any temperature t, preferably t = 30 ° C to 100 ° C, more preferably t = 30 ° C to 90 ° C, still more preferably t = 30 ° C to 80 ° C, the above dl (t) / dt Satisfy the condition.

The mean linear thermal expansion coefficient at 30°C to 120°C of the cured adhesive composition is the peeling of the cured adhesive composition (circuit connecting member 4) from the circuit members 2, 3 and the circuit electrodes 6, 8. From the viewpoint of suppressing, it is preferably 500 ppm/°C or less, more preferably 250 ppm/°C or less, and still more preferably 150 ppm/°C or less.

The coefficient of linear thermal expansion (ppm/°C) of the cured product of the adhesive composition is defined as the amount of linear thermal expansion (μm) per 1°C of temperature increase per 1 m in length of the cured product of the adhesive composition. The average linear thermal expansion coefficient α _l at 30 ° C. to 120 ° C. of the cured adhesive composition is the amount of linear thermal expansion l (t) [unit of t = 30 ° C. to 120 ° C. : μm / 10 mm] is converted into the amount of linear thermal expansion (μm) in the length of 1 m of the cured product of the adhesive composition, and from the converted value as an average value per 1 ° C. of temperature rise (ie, according to the following formula). Calculated.

α _l = {l(t=120°C)-l(t=30°C)}×100/(120-30)

Adhesive compositions having such properties include, for example, two or more resin components having different glass transition points (Tg), components that easily cause phase separation from each other, components that have skeletons that are easy to orient, and fillers that have a negative linear thermal expansion coefficient. contains ingredients, etc. Examples of combinations of components that easily cause phase separation from each other include combinations of components with a large difference in molecular weight and combinations of components with a large difference in polarity. Specifically, the combination of components that easily cause phase separation with each other may be a combination of an acrylic resin and an epoxy resin, a combination of a urethane resin and a phenoxy resin, a combination of an acrylic rubber and a phenoxy resin, a combination of an acrylic rubber and an epoxy resin, and the like. . Examples of components having skeletons that are easily oriented include components containing an alkyl chain, components containing a phenyl group, and the like. In the cured product (circuit connection member 4) of the adhesive composition obtained by the adhesive composition containing the above components, reduction of minute voids due to temperature rise, reorientation of molecular chains, rearrangement of filler components, etc. The present inventors believe that shrinkage (volume phenomenon) accompanying the temperature rise has occurred.

The adhesive composition, in one embodiment, preferably includes (a) a thermoplastic resin (hereinafter also referred to as "component (a)") and (b) a radically polymerizable compound (hereinafter also referred to as "component (b)") and (c) a radical polymerization initiator (hereinafter also referred to as "component (c)").

The component (a) is not particularly limited, and examples thereof include polyimide resins, polyamide resins, phenoxy resins, poly(meth)acrylic resins, polyester resins, polyurethane resins, polyesterurethane resins, and polyvinylbutyresins. One or two or more resins selected from ral resins are exemplified.

From the viewpoint of easiness of obtaining a cured product of the adhesive composition (circuit connecting member 4) having a desired amount of linear thermal expansion, the adhesive composition preferably contains two or more of the above thermoplastic resins, and more preferably has a mutually Tg of 2 or more. It contains 2 or more types of other thermoplastic resins. Preferable resin combinations include, for example, a combination of a phenoxy resin and a poly(meth)acrylic resin, a combination of a phenoxy resin and a polyester resin, a combination of a phenoxy resin and a polyester urethane resin, and a combination of a phenoxy resin and a poly(meth)acrylic resin. A combination of mid-resin may be mentioned.

When the adhesive composition contains two or more types of thermoplastic resins having different Tg, the ratio of the contents of the thermoplastic resin with the higher Tg and the thermoplastic resin with the lower Tg (mass ratio: high Tg/low Tg) is the desired amount of linear thermal expansion. From the viewpoint of easiness of obtaining a cured product of the adhesive composition (circuit connection member 4) having, the ratio is preferably 90/10 to 10/90, more preferably 90/10 to 20/80, still more preferably 90/10. 10 to 30/70. When the adhesive composition contains three or more types of thermoplastic resins having different Tg, the adhesive composition preferably contains such that the ratio of the contents of the thermoplastic resin having the highest Tg and the thermoplastic resin having the lowest Tg is the above ratio. do.

The weight average molecular weight of the thermoplastic resin is preferably 5000 or more, more preferably 10000 or more, and is preferably 400000 or less, more preferably 200000 or less, still more preferably 150000 or less. When the weight average molecular weight of the thermoplastic resin is 5000 or more, the adhesive strength of the adhesive composition tends to be improved. When the weight average molecular weight of the thermoplastic resin is 400000 or less, compatibility with other components is excellent, and the fluidity of the adhesive tends to be improved. The weight average molecular weight in the present invention means a weight average molecular weight (standard polystyrene equivalent) measured by GPC (Gel Permeation Chromatography).

The adhesive composition may contain a rubber component as a thermoplastic resin from the viewpoint of further improving stress relaxation and adhesiveness. The rubber component is, for example, silicone rubber, acrylic rubber, polyisoprene rubber, polybutadiene rubber, carboxyl group terminal polybutadiene rubber, hydroxyl group terminal polybutadiene rubber, 1,2-polybutadiene rubber, carboxyl group terminal 1,2-polybutadiene Rubber, hydroxyl terminal 1,2-polybutadiene rubber, styrene-butadiene rubber, hydroxyl terminal styrene-butadiene rubber, acrylonitrile-butadiene rubber, carboxylated nitrile rubber, hydroxyl terminal poly(oxypropylene) rubber, alkoxysilyl terminal poly(oxypropylene) rubber, poly(oxytetramethylene) glycol rubber, polyolefin glycol rubber, and poly-ε-caprolactone rubber. The rubber component preferably has a cyano group or carboxyl group, which is a highly polar group, as a side chain group or terminal group, from the viewpoint of further improving adhesiveness. These rubber components can be used individually by 1 type or in combination of 2 or more types.

The rubber component may form particulates. The average particle diameter of the rubber particles is preferably 2 times or less of the average particle diameter of the conductive particles 10, and is, for example, 0.01 μm to 100 μm. The storage elastic modulus of the rubber particles at room temperature (25°C) is preferably 1/2 or less of the storage elastic modulus of the conductive particles 10 and the adhesive composition at room temperature, and is, for example, 0.1 MPa to 100 MPa. The rubber particles are excellent in solvent resistance and are preferably three-dimensionally crosslinked rubber particles from the viewpoint of being easily dispersed in the adhesive composition.

The content of component (a) is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, still more preferably 35 parts by mass or more, based on 100 parts by mass of the total amount of component (a) and component (b). Further, it is preferably 80 parts by mass or less, more preferably 70 parts by mass or less, and still more preferably 65 parts by mass or less. When the content of the component (a) is 20 parts by mass or more, the adhesive strength is further improved and the film formability of the adhesive composition tends to be improved, and when it is 80 parts by mass or less, the fluidity of the adhesive tends to be improved.

The component (b) is not particularly limited, and may be, for example, a compound (monomer) described below, may be an oligomer of the compound, or may contain both.

Component (b) is preferably a polyfunctional (meth)acrylate compound having two or more (meth)acryloyloxy groups. As such a (meth)acrylate compound, epoxy (meth)acrylate, urethane (meth)acrylate, polyether (meth)acrylate, polyester (meth)acrylate, trimethylolpropane tri(meth)acrylate, polyethylene Polyalkylene glycol di(meth)acrylates such as glycol di(meth)acrylate, dicyclopentenyl(meth)acrylate, dicyclopentenyloxyethyl(meth)acrylate, neopentyl glycol di(meth)acrylate rate, dipentaerythritol hexa(meth)acrylate, isocyanuric acid-modified bifunctional (meth)acrylate, isocyanuric acid-modified trifunctional (meth)acrylate, and the like. As the epoxy (meth) acrylate, epoxy (meth) acrylate obtained by adding (meth) acrylic acid to two glycidyl groups of bisphenol fluorene diglycidyl ether, and two glycidyl groups of bisphenol fluorene diglycidyl ether and compounds in which a (meth)acryloyloxy group is introduced into a compound obtained by adding ethylene glycol and/or propylene glycol to a dil group. Among these (meth)acrylate compounds, urethane (meth)acrylate is preferably used from the viewpoint of obtaining better adhesiveness by having a urethane bond. These compounds are used individually by 1 type or in combination of 2 or more types.

The adhesive composition may contain a monofunctional (meth)acrylate compound as component (b) from the viewpoint of control of fluidity or the like. Examples of the monofunctional (meth)acrylate compound include pentaerythritol (meth)acrylate, 2-cyanoethyl (meth)acrylate, cyclohexyl (meth)acrylate, and dicyclopentenyl (meth)acrylate. Rate, dicyclopentenyloxyethyl (meth)acrylate, 2-(2-ethoxyethoxy)ethyl (meth)acrylate, 2-ethoxyethyl (meth)acrylate, 2-ethylhexyl (meth)acrylate Rate, n-hexyl (meth)acrylate, 2-hydroxyethyl (meth)acrylate, hydroxypropyl (meth)acrylate, isobornyl (meth)acrylate, isodecyl (meth)acrylate, isooctyl (meth)acrylate, n-lauryl (meth)acrylate, 2-methoxyethyl (meth)acrylate, 2-phenoxyethyl (meth)acrylate, tetrahydrofurfuryl (meth)acrylate, 2- (meth)acryloyloxyethyl phosphate, N,N-dimethylaminoethyl (meth)acrylate, N,N-dimethylaminopropyl (meth)acrylate, one glycidyl group of an epoxy resin having a plurality of glycidyl groups glycidyl group-containing (meth)acrylate obtained by reacting (meth)acrylic acid and (meth)acryloylmorpholine. These compounds are used individually by 1 type or in combination of 2 or more types.

The adhesive composition may contain a compound having a radically polymerizable functional group such as an allyl group, a maleimide group, or a vinyl group as the component (b) from the viewpoint of improving the crosslinking rate or the like. Examples of such compounds include N-vinylimidazole, N-vinylpyridine, N-vinylpyrrolidone, N-vinylformamide, N-vinylcaprolactam, 4,4'-vinylidenebis(N, N-dimethylaniline), N-vinylacetamide, N,N-dimethylacrylamide, N-isopropylacrylamide and N,N-diethylacrylamide.

The adhesive composition preferably contains a radically polymerizable compound having a phosphoric acid ester structure as component (b) for the purpose of improving adhesive strength. The radically polymerizable compound having a phosphoric acid ester structure may be a compound represented by the following formula (1), (2) or (3), for example.

In Formula (1), R ¹ represents a hydrogen atom or a methyl group, R ² represents a (meth)acryloyloxy group, and a and b each independently represent an integer of 1 to 8. A plurality of R ¹ , R ² , a and b in the same molecule may be the same as or different from each other.

In Formula (2), R ³ represents a (meth)acryloyloxy group, and c and d each independently represent an integer of 1 to 8. A plurality of R ³ s, c and d in the same molecule may be the same as or different from each other.

In formula (3), R ⁴ represents a hydrogen atom or a methyl group, R ⁵ represents a (meth)acryloyloxy group, and e and f each independently represents an integer of 1 to 8. A plurality of R ⁴ , R ⁴ , e and f in the same molecule may be the same as or different from each other.

As a radically polymerizable compound having a phosphoric acid ester structure, for example, acid phosphooxyethyl (meth)acrylate, acid phosphooxypropyl (meth)acrylate, acid phosphooxypolyoxyethylene glycol mono(meth)acryl Rate, acid phosphooxypolyoxypropylene glycol mono(meth)acrylate, 2,2'-di(meth)acryloyloxydiethyl phosphate, EO(ethylene oxide) modified phosphoric acid di(meth)acrylate, phosphoric acid modified epoxy (meth)acrylates and vinyl phosphates.

The content of component (b) in the adhesive composition is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, and still more preferably based on 100 parts by mass of the total amount of component (a) and component (b). It is 35 parts by mass or more, and is preferably 80 parts by mass or less, more preferably 70 parts by mass or less, and even more preferably 65 parts by mass or less. When the content of the component (b) is 20 parts by mass or more, the heat resistance of the cured product (circuit connecting member 4) of the adhesive composition tends to improve, and when it is 80 parts by mass or less, the circuit connecting member 4 under a high temperature, high humidity environment. It tends to be able to further suppress the peeling of.

When the adhesive composition contains a radical polymerizable compound having a phosphoric acid ester structure as component (b), the content of the radical polymerizable compound having a phosphoric acid ester structure is 100 parts by mass of the total amount of component (a) and component (b). It is preferably 0.1 part by mass or more, more preferably 0.5 part by mass or more, and preferably 15 parts by mass or less, more preferably 10 parts by mass or less. When the content of the radical polymerizable compound having a phosphoric acid ester structure is 0.1 part by mass or more, the adhesive strength of the adhesive composition tends to be higher, and when it is 15 parts by mass or less, the physical properties of the cured product (circuit connecting member 4) of the adhesive composition. Deterioration is less likely to occur, and reliability tends to improve.

(c) As a component, it can select arbitrarily from compounds, such as a peroxide and an azo compound, for example. As the component (c), a peroxide having a half-life temperature of 90°C to 175°C for one minute and a molecular weight of 180 to 1000 is preferably used from the viewpoint of excellent stability, reactivity, and compatibility. "1-minute half-life temperature" means the temperature at which the half-life of peroxide is 1 minute. "Half-life" refers to the time until the concentration of a compound decreases to half of the initial value at a predetermined temperature.

The radical polymerization initiator is, for example, 1,1,3,3-tetramethylbutylperoxyneodecanoate, di(4-t-butylcyclohexyl)peroxydicarbonate, di(2-ethylhexyl) Peroxydicarbonate, cumylperoxyneodecanoate, 1,1,3,3-tetramethylbutylperoxyneodecanoate, dilauroylperoxide, 1-cyclohexyl-1-methylethylperoxyneo Decanoate, t-hexylperoxyneodecanoate, t-butylperoxyneodecanoate, t-butylperoxypivalate, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexa Noate, 2,5-dimethyl-2,5-di(2-ethylhexanoylperoxy)hexane, t-hexylperoxy-2-ethylhexanoate, t-butylperoxy-2-ethylhexanoate , t-butylperoxyneoheptanoate, t-amylperoxy-2-ethylhexanoate, di-t-butylperoxyhexahydroterephthalate, t-amylperoxy-3,5,5-trimethylhexanoate Noate, 3-hydroxy-1,1-dimethylbutylperoxyneodecanoate, 1,1,3,3-tetramethylbutylperoxy-2-ethylhexanoate, t-amylperoxyneodecano Eight, t-amylperoxy-2-ethylhexanoate, 3-methylbenzoyl peroxide, 4-methylbenzoyl peroxide, di(3-methylbenzoyl) peroxide, dibenzoyl peroxide, di(4-methylbenzoyl ) Peroxide, 2,2'-azobis-2,4-dimethylvaleronitrile, 1,1'-azobis (1-acetoxy-1-phenylethane), 2,2'-azobisisobutyro Nitrile, 2,2'-azobis (2-methylbutyronitrile), dimethyl-2,2'-azobisisobutyronitrile, 4,4'-azobis (4-cyanovaleric acid), 1, 1'-azobis(1-cyclohexanecarbonitrile), t-hexylperoxyisopropylmonocarbonate, t-butylperoxymaleic acid, t-butylperoxy-3,5,5-trimethylhexanoate , t-butylperoxylaurate, 2,5-dimethyl-2,5-di(3-methylbenzoylperoxy)hexane, t-butylperoxy-2-ethylhexylmonocarbonate, t-hexylperoxy Benzoate, 2,5-dimethyl-2,5-di(benzoylperoxy)hexane, t-butylperoxybenzoate, dibutylperoxytrimethyladipate, t-amylperoxynormaloctoate, t-amylfer 1 selected from oxyisononanoate and t-amylperoxybenzoate Any of the above compounds may be used.

From the viewpoint of suppressing corrosion of the circuit electrodes 6 and 8, the content of chlorine ions or organic acids in the radical polymerization initiator is preferably 5000 ppm or less, and a radical polymerization initiator with less organic acid generated after decomposition is more preferably used. . From the viewpoint of improving the stability of the adhesive composition, a radical polymerization initiator having a mass retention rate of 20% by mass or more after being left in the atmosphere at room temperature (25°C) and atmospheric pressure for 24 hours is preferably used.

The content of component (c) in the adhesive composition is preferably 1 part by mass or more, more preferably 2.5 parts by mass or more, based on 100 parts by mass of the total amount of component (a) and component (b). It is preferably 15 parts by mass or less, more preferably 10 parts by mass or less.

The adhesive composition, in another embodiment, preferably includes (a) a thermoplastic resin, (d) an epoxy resin (hereinafter also referred to as "(d) component"), and (e) a curing agent (hereinafter referred to as "( e) component”)). The component (a) in this embodiment is the same component as the component (a) described in the above-mentioned embodiment.

(d) The epoxy resin is a resin having at least one epoxy group in its molecule. As the epoxy resin, bisphenol A type epoxy resin, bisphenol F type epoxy resin, bisphenol S type epoxy resin, phenol novolak type epoxy resin, cresol novolak type epoxy resin, bisphenol A novolak type epoxy resin, bisphenol F novolak type epoxy resins, alicyclic epoxy resins, glycidyl ester type epoxy resins, glycidylamine type epoxy resins, hydantoin type epoxy resins, isocyanurate type epoxy resins, aliphatic chain epoxy resins and the like. (d) The epoxy resin may be a halogenated epoxy resin obtained by halogenating the epoxy resin or a hydrogenated epoxy resin obtained by adding hydrogen to the epoxy resin. These epoxy resins, halogenated epoxy resins, and hydrogenated epoxy resins are used alone or in combination of two or more.

The content of component (d) in the adhesive composition is preferably 10 parts by mass or more, more preferably 20 parts by mass or more, and still more preferably based on 100 parts by mass of the total amount of component (a) and component (d). It is 30 parts by mass or more, and is preferably 90 parts by mass or less, more preferably 80 parts by mass or less, and still more preferably 70 parts by mass or less. When the content of component (d) is 10 parts by mass or more, better adhesiveness tends to be obtained, and when it is 90 parts by mass or less, stickiness tends to be low and workability tends to be good.

(e) The curing agent (also referred to as "epoxy polymerization initiator" or "latent type curing agent") only needs to be a curing agent capable of curing the (d) epoxy resin. Examples of the curing agent include anionic polymerizable catalyst type curing agents, cationically polymerizable catalyst type curing agents, and polyaddition type curing agents. These are used individually by 1 type or in combination of 2 or more types. (e) The curing agent is preferably anionic polymerizable or cationic polymerizable catalyst-type curing agent from the viewpoint of excellent fast curing property and unnecessary chemical equivalent considerations.

Examples of the anionic polymerizable or cationic polymerizable catalytic curing agent include imidazole-based curing agents, hydrazide-based curing agents, boron trifluoride-amine complexes, sulfonium salts, onium salts such as diazonium salts, amineimides, diaminomaleonitriles, melamine and derivatives thereof, polyamine salts, dicyandiamide, and the like, and modified products thereof may also be used.

When a compound having a tertiary amino group, an imidazole compound, or the like is used as an anionically polymerizable catalytic curing agent, the epoxy resin is cured by heating at a temperature of about 160°C to 200°C for several 10 seconds to several hours. For this reason, the pot life (pot life) of adhesive composition can be made comparatively long. As the cationic polymerizable catalytic curing agent, for example, photosensitive onium salts (aromatic diazonium salts, aromatic sulfonium salts, etc.) that cure epoxy resins by irradiation with energy rays are preferably used. Aliphatic sulfonium salts etc. are mentioned as a cationic polymerizable catalyst type hardening agent which activates by heating and hardens an epoxy resin. These anionic polymerizable or cationic polymerizable catalytic curing agents are preferably used because they have fast curing properties.

Polyamines, polymer captans, polyphenols, acid anhydrides, and the like are exemplified as polyaddition type curing agents.

These curing agents (latent curing agents) are coated with a polymer compound such as polyurethane or polyester, a metal film such as nickel or copper, or an inorganic material such as calcium silicate to microencapsulate the microencapsulated curing agent. It is preferably used in this respect.

The content of component (e) in the adhesive composition is preferably 20 parts by mass or more, more preferably 30 parts by mass or more, based on 100 parts by mass of the total amount of component (a) and component (d). It is preferably 80 parts by mass or less, more preferably 70 parts by mass or less.

Examples of the conductive particles 10 include metal particles such as Au, Ag, Ni, Cu, and solder, and conductive particles such as conductive carbon particles. The conductive particles 10 may be coated conductive particles provided with a nucleus made of non-conductive particles of glass, ceramic, plastic, etc., and a layer composed of the metal, metal particles, conductive carbon particles, etc. covering the nucleus. . When the conductive particles 10 are coated conductive particles or metal particles that melt with heat (heat-melting metal particles), the conductive particles 10 are deformed by heating and pressing during circuit connection, so that the circuit electrodes 6 and 8 Even if the height fluctuates, the contact area between the conductive particles 10 and the circuit electrodes 6 and 8 increases and good reliability is obtained. The conductive particles 10 prevent short circuit between the conductive particles 10, especially when the compounding amount of the conductive particles 10 is increased, and between the adjacent first circuit electrodes 6, 6 or the second circuit electrode 8 , 8) from the viewpoint of improving the insulation between the conductive particles described above and the insulating coating layer formed of an insulating material such as a polymer resin that covers the surface of the conductive particles may be insulated-coated conductive particles. These electroconductive particles, coated electroconductive particles, and insulated-coated electroconductive particles are used individually by 1 type or in combination of 2 or more types.

The average particle diameter of the conductive particles 10 is preferably 1 μm to 50 μm from the viewpoint of excellent dispersibility and conductivity. The content of the conductive particles is preferably 0.1% by volume or more, and preferably 30% by volume or less, more preferably 10% by volume or less, based on the total amount of the adhesive composition. When the content is 0.1 vol% or more, the conductivity tends to be further improved, and when the content is 30 vol% or less, short circuit between adjacent first circuit electrodes 6, 6 or between second circuit electrodes 8, 8 can be suppressed. tend to have The content of the conductive particles 10 is determined based on the volume of each component of the adhesive composition (before curing) at 23°C. The volume of each component can use, for example, a value converted into a volume from a weight using specific gravity. In addition, for example, the volume increased by introducing the component into a measuring cylinder or the like into which an appropriate solvent (water, alcohol, etc.) that wets the component well without dissolving or swelling the component is found as its volume. may be

In addition to the adhesive composition, component (a), component (b), component (c) and conductive particles 10, or component (a), component (d), component (e) and conductive particles 10 , other resins such as phenol resins and melamine resins, fillers (fillers), softeners, hardening accelerators, anti-aging agents, colorants, flame retardants, thixotropic agents, adhesion improvers such as coupling agents, thickeners, leveling agents, weather resistance improvers, isocyanates You may further contain a compound etc.

The filler (filler) may be particles composed of silicon, calcium, zirconium, titanium, aluminum, carbon, bismuth, cobalt, copper, iron, indium, manganese, tin, yttrium, zinc, or the like, or a compound containing them, an organic compound, or the like. . The average particle diameter of the particles is preferably 1/2 or less of the average particle diameter of the conductive particles 10, and is, for example, 0.005 μm to 25 μm. When the adhesive composition contains non-conductive particles (for example, the rubber particles), the average particle diameter of the particles used as the filler may be equal to or less than the average particle diameter of the non-conductive particles.

From the viewpoint of further improving the electrical properties such as connection reliability between the circuit electrodes 6 and 8 with the cured product (circuit connection member 4) of the adhesive composition having a desired amount of linear thermal expansion, the filler is preferably A filler having a negative mean coefficient of linear thermal expansion between 30°C and 120°C. Examples of the filler having a negative average linear thermal expansion coefficient between 30°C and 120°C include particles composed of zirconium-based compounds.

The content of the filler is preferably 5 parts by mass or more, and preferably 60 parts by mass or less with respect to 100 parts by mass of the adhesive composition. When the content is 60 parts by mass or less, the effect of improving connection reliability tends to be more sufficiently obtained, and when the content is 5 parts by mass or more, the effect of adding a filler tends to be sufficiently obtained.

The coupling agent may be, for example, a silane coupling agent. By using a coupling agent such as a silane coupling agent, the adhesion of the adhesive composition can be further improved. Examples of the silane coupling agent include vinyltrimethoxysilane, vinyltriethoxysilane, 3-glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, and 3-(meth)acryloxy. Propylmethyldimethoxysilane, 3-(meth)acryloxypropyltrimethoxysilane, 3-(meth)acryloxypropylmethyldiethoxysilane, 3-(meth)acryloxypropyltriethoxysilane, N-2-( Aminoethyl)-3-aminopropylmethyldimethoxysilane, N-phenyl-3-aminopropyltrimethoxysilane, 3-ureidpropyltriethoxysilane, 3-mercaptopropyltrimethoxysilane, 3-isocyanate propyl triethoxysilane, and condensates thereof.

The content of the coupling agent is preferably 0.1 part by mass or more, more preferably 0.25 part by mass or more, based on 100 parts by mass of the adhesive components (for example, components (a) to (e)) of the adhesive composition. It is preferably 10 parts by mass or less, more preferably 5 parts by mass or less. When the content of the coupling agent is 0.1 part by mass or more, the occurrence of peeling between the circuit member and the circuit connection member tends to be further suppressed, and when the content of the coupling agent is 10 parts by mass or less, the pot life of the adhesive composition tends to be longer there is

When the adhesive composition is liquid at 15°C to 25°C, it can be used as a paste adhesive composition. When the adhesive composition is solid at room temperature (25°C), it can be used as a paste adhesive composition by heating, or can be used as a paste adhesive composition after being dissolved in a solvent. The solvent is not particularly limited as long as it is not reactive with the components contained in the adhesive composition and exhibits sufficient solubility in the components contained in the adhesive composition, but a solvent having a boiling point under atmospheric pressure of 50°C to 150°C is preferably used. When the boiling point is 50 ° C. or higher, volatilization of the solvent at room temperature (25 ° C.) can be suppressed, and use in an open system becomes easy. When the boiling point is 150°C or lower, the solvent is easily volatilized after applying the adhesive composition to the circuit members 2 and 3, and reliability after adhesion can be ensured.

The adhesive composition can also be used as a film adhesive. For the adhesive composition, for example, a solution in which a solvent or the like is added to the adhesive composition as necessary is applied onto a peelable substrate such as a fluororesin film, a polyethylene terephthalate film, or a release paper, or a solution is applied to a substrate such as a nonwoven fabric. It is impregnated and mounted on a peelable base material, and thereafter, the solvent or the like is removed and molded into a film shape. A film adhesive is used suitably from viewpoints, such as handleability.

The adhesive composition can be used as a circuit connection material represented by an anisotropic conductive adhesive, silver paste, silver film, etc., a semiconductor element adhesive material represented by an elastomer for CSP, an underfill material for CSP, and a LOC tape.

The connection structure 1 arranges, for example, the first circuit member 2 and the second circuit member 3 so that the first circuit electrode 6 and the second circuit electrode 8 are opposed to each other, Obtained by interposing a film adhesive between the circuit member 2 and the second circuit member 3, heating and pressurizing them to electrically connect the first circuit electrode 6 and the second circuit electrode 8 to each other. .

The heating temperature at the time of heating is not particularly limited, but is preferably 50°C to 250°C. The pressure at the time of pressing is not particularly limited as long as it does not damage the adherend (circuit member 2, 3), but is preferably 0.1 MPa to 10 MPa. Heating and pressurization are preferably performed for 0.5 second to 3 hours.

When connecting the circuit members 2 and 3, light irradiation may be performed simultaneously with heating and pressurization from the viewpoint of connecting at a lower temperature and in a shorter time. For light irradiation, irradiation light in a wavelength range of 150 nm to 750 nm is preferably used. Light irradiation may be performed at an irradiation amount of 0.1 J/cm 2 to 10 J/cm 2 using, for example, a low-pressure mercury-vapor lamp, a medium-pressure mercury-vapor lamp, a high-pressure mercury-vapor lamp, an ultra-high pressure mercury lamp, a xenon lamp, or a metal halide lamp.

As described above, the cured product of the adhesive composition (circuit connection member 4) is dl(t)/dt<0( Since it is a cured product (circuit connecting member) in which t satisfies dL(t)/dt<0), the amount of thermal expansion of the circuit connecting member 4 itself accompanying the temperature rise can be reduced, and the circuit connecting member ( 4) and the interface stress of peeling generated at the interface between the substrates 5 and 7 and the circuit electrodes 6 and 8 (circuit connecting member 4 from the substrates 5 and 7 and the circuit electrodes 6 and 8) stress to be released) can be reduced.

On the other hand, the cured product (circuit connection member) of the conventional adhesive composition is always dl (t) / dt ≥ 0 (dL ( Since it is a cured product (circuit connecting member) of an adhesive composition that satisfies t)/dt ≥ 0), the circuit connecting member 4 itself easily thermally expands as the temperature rises, and the circuit connecting member 4 and the substrates 5 and 7 ) and the interface stress of large peeling occurs at the interface with the circuit electrodes 6 and 8.

Therefore, compared to the cured product (circuit connecting member) of the conventional adhesive composition, the cured product of the adhesive composition (circuit connecting member 4) according to the present embodiment is more suitable for circuit connecting member 4 even when placed in a high-temperature, high-humidity environment. Separation from the substrates 5 and 7 and the circuit electrodes 6 and 8 can be suppressed. These effects are exhibited even when circuit electrodes formed of amorphous ITO or the like, which are unfavorable to adhesion, are used as the circuit electrodes 6 and 8 .

Example

Hereinafter, the present invention will be described in more detail based on examples, but the present invention is not limited to the examples.

<Synthesis of Polyurethane Resin>

To a separable flask equipped with a reflux condenser, a thermometer, and a stirrer, 1000 parts by mass of polypropylene glycol (number average molecular weight: 2000), which is a diol having an ether bond, and 4000 parts by mass of methyl ethyl ketone as a solvent were added, and the mixture was maintained at 40° C. for 30 minutes. Stir. After heating up this solution to 70 degreeC, 0.127 mass part of dimethyl tin laurate as a catalyst was added. Next, a solution prepared by dissolving 125 parts by mass of 4,4'-diphenylmethane diisocyanate in 125 parts by mass of methyl ethyl ketone was added dropwise to this solution over 1 hour. Then, stirring was continued at 70 degreeC until the absorption peak derived from NCO group was not observed with the infrared spectrophotometer, and the polyurethane resin methyl ethyl ketone solution was obtained. And the quantity of methyl ethyl ketone was adjusted so that the solid content concentration (concentration of polyurethane resin) of this solution might become 30 mass %.

The glass transition temperature (Tg) of the obtained polyurethane resin was -20°C. The glass transition temperature (Tg) was measured using a thermomechanical analyzer.

The weight average molecular weight of the obtained polyurethane resin was 320000. A weight average molecular weight is a standard polystyrene conversion value measured by GPC (Gel Permeation Chromatography). The analysis conditions of GPC are shown in Table 1 below.

<Synthesis of urethane acrylate>

In a 2-liter four-necked flask equipped with a thermometer, stirrer, inert gas inlet, and reflux condenser, 4000 parts by mass of polycarbonate diol (manufactured by Aldrich, number average molecular weight: 2000) and 2-hydroxyethyl acrylate A reaction solution was prepared by introducing 238 parts by mass, 0.49 parts by mass of hydroquinone monomethyl ether, and 4.9 parts by mass of a tin-based catalyst. 666 parts by mass of isophorone diisocyanate (IPDI) was uniformly added dropwise over 3 hours to the reaction solution heated to 70°C and reacted. After completion of the dropping, the reaction was continued for 15 hours, and the reaction was terminated at the time when it was confirmed that the content of NCO groups became 0.2% by mass or less with a potentiometric automatic titration device (product name AT-510, manufactured by Kyoto Denshi Industries Co., Ltd.), Urethane acrylate was obtained. The weight average molecular weight of urethane acrylate was 8500. In addition, the weight average molecular weight of urethane acrylate was measured similarly to the weight average molecular weight of the polyurethane resin mentioned above.

<Production of film adhesive>

The components shown below were mixed in the mass ratio shown in Tables 2 and 3 to obtain an adhesive composition.

(thermoplastic resin)

A1: phenoxy resin (product name: PKHC, manufactured by Union Carbide Co., Ltd., weight average molecular weight 45000, Tg: 90 ° C., bisphenol A skeleton)

A2: Phenoxy resin (product name: YD-6020, manufactured by Nippon Steel & Chemical Co., Ltd., weight average molecular weight: 5000, Tg: 70°C, bisphenol A/bisphenol F skeleton)

A3: Phenoxy resin (product name: FX-316, manufactured by Nippon Steel & Chemical Co., Ltd., weight average molecular weight: 50000, Tg: 70°C, bisphenol F skeleton)

A4: Phenoxy resin (product name: FX-293AT40, manufactured by Nippon Steel & Chemical Co., Ltd., Tg: 160°C, highly heat-resistant skeleton)

A5: polyurethane resin synthesized as described above

A6: Polyester resin (product name: UE-3400, manufactured by Unitica Co., Ltd., Tg: -20°C)

A7: Polyester resin (product name: UE-3200, manufactured by Unitica Co., Ltd., Tg: 70°C)

(radical polymerizable compound)

B1: urethane acrylate synthesized as described above

B2: isocyanuric acid EO modified diacrylate (product name: M-215, manufactured by Toagosei Co., Ltd.)

B3: 2-methacryloyloxyethyl acid phosphate (product name: Light Ester P-2M, manufactured by Kyoeisha Chemical Co., Ltd.)

In addition, about the solid component among the above components, it was used after setting it as a 40 mass % solution prepared by dissolving 40 g of the solid component in 60 g of methyl ethyl ketone.

(radical polymerization initiator)

C1: lauroyl peroxide (product name: Peroyl L, manufactured by Nichiyu Co., Ltd., molecular weight 398.6)

(filler (filler))

D1: Silica fine particles (product name: R104, manufactured by Nippon Aerosil Co., Ltd., primary particle diameter: 12 nm)

(Silane coupling agent)

E1: 3-methacryloxypropyltrimethoxysilane (product name: KBM-503, manufactured by Shin-Etsu Chemical Industry Co., Ltd.)

In addition, about silica fine particles, it was used after making it into the 10 mass % dispersion liquid prepared by dispersing 10 g of silica fine particles in the mixed solvent of 45 g of toluene and 45 g of ethyl acetate.

Subsequently, conductive particles having an average particle diameter of 5 μm and a specific gravity of 2.5 having a nickel layer having a thickness of 0.2 μm were formed on the surface of the polystyrene particles (nuclei). These conductive particles were dispersed in each adhesive composition at a ratio of 1.5% by volume to obtain a coating solution. This coating solution was applied to a polyethylene terephthalate (PET) film having a thickness of 50 μm using a coating device. The coating film was dried with hot air at 70°C for 10 minutes to obtain a film adhesive having a thickness of 18 µm.

<Production of Connection Structure>

A flexible circuit board (FPC) having about 2200 copper circuit electrodes with a line width of 75 μm, a pitch of 150 μm, and a thickness of 18 μm, and a glass (SiO ₂ ) substrate (product name: Pre-Clean Slide S7224, Matsunami Glass Kogyo Co., Ltd.) ), or a glass substrate with a thin film of amorphous indium tin oxide (ITO) (manufactured by Geomatech), and each of the above film adhesives was disposed, and the FPC was connected to the glass substrate or the glass substrate with amorphous ITO. The connection was performed by heating and pressurizing at 160°C and 3 MPa for 5 seconds using a thermocompression bonding device (heating method: constant heat type, manufactured by Toray Engineering Co., Ltd.). The pressure at the time of pressurization was calculated assuming that the compression area was 0.495 cm 2 . As a result, a connected structure in which the FPC and the glass substrate or the glass substrate with amorphous ITO were connected over a width of 1.5 mm by the cured product of the film adhesive was obtained.

<Measurement of linear thermal expansion amount>

A cured product sample was produced by bonding the prepared film adhesive to a thickness of 100 ± 20 µm using a laminator, and then heating in an oven at 180°C for 1 hour. Regarding the cured product sample, using a thermomechanical analyzer (manufactured by Shimadzu Seisakusho Co., Ltd.), the conditions of a sample length of 10 mm and a width of 4 mm, a load of 5 gf (per 0.4 mm 2 of the cross-sectional area of the sample), and a heating rate of 5 ° C./min. In , the amount of linear thermal expansion l(t) μm at a temperature t = 0 ° C to 200 ° C was measured every 0.1 ° C. The amount of linear thermal expansion 1(t) was measured assuming that the amount of linear thermal expansion 1(0) at a temperature t=0°C was 0 μm. From the measurement results, the presence or absence of a temperature range in which dl(t)/dt <0 was observed at a temperature of t = 30°C to 120°C (if present, the minimum value of the temperature range and dl(t)/dt) was confirmed. Also, from the measurement results, the average coefficient of linear thermal expansion (ppm/°C) between 30°C and 120°C was calculated. The results are shown in Tables 2 and 3.

<Evaluation of the presence or absence of peeling>

For the bonded structure produced as described above, the appearance of the connection immediately after connection and after a high-temperature, high-humidity test left in a constant temperature and humidity chamber at 85 ° C. and 85% RH for 250 hours was observed using an optical microscope, and the space portion (electrode of FPC The portion between the terminal and the electrode terminal) of the substrate-resin interface peeling area was measured. The case where the peeling generation area in the entire space exceeded 30% was evaluated as "existence" of peeling, and the case of 30% or less was evaluated as "absence of peeling". The results are shown in Tables 2 and 3.

From the above, it was confirmed that the circuit connecting members of Examples 1 to 7 could suppress the occurrence of peeling even under high temperature and high humidity conditions compared to the circuit connecting members of Comparative Examples 1 to 8.

1: connection structure
2: First circuit member
3: Second circuit member
4: circuit connection member
6: first circuit electrode
8: second circuit electrode
10: conductive particles

Claims (6)

a first circuit member having a first circuit electrode;
a second circuit member having a second circuit electrode;
a circuit connection member provided between the first circuit member and the second circuit member and electrically connecting the first circuit electrode and the second circuit electrode to each other;
The circuit connection member contains two or more types of thermoplastic resins,
A connection structure in which the amount of linear thermal expansion L(t) at temperature t of the circuit connecting member satisfies the condition of dL(t)/dt<0 at at least any temperature t of t=30°C to 120°C.
However, this excludes the case where the circuit connecting member contains particles of crystallized phosphate glass composed of P ₂ O ₅ and one or more cations selected from the group consisting of magnesium, cobalt, arsenic, zinc, iron, aluminum and zirconium. do. The connected structure according to claim 1, wherein the circuit connecting member has an average linear thermal expansion coefficient at 30°C to 120°C of 500 ppm/°C or less. As a circuit connecting member,
The circuit connection member contains two or more types of thermoplastic resins,
The circuit connecting member, wherein the linear thermal expansion L(t) at temperature t of the circuit connecting member satisfies the condition of dL(t)/dt<0 at at least any temperature t of t=30°C to 120°C.
However, this excludes cases where the circuit connecting member contains particles of crystallized phosphate glass composed of P ₂ O ₅ and one or more cations selected from the group consisting of magnesium, cobalt, arsenic, zinc, iron, aluminum and zirconium. do. The circuit connecting member according to claim 3, wherein the average linear thermal expansion coefficient at 30°C to 120°C of the circuit connecting member is 500 ppm/°C or less. As an adhesive composition,
The adhesive composition includes two or more thermoplastic resins,
The amount of linear thermal expansion l (t) at the temperature t of the cured product of the adhesive composition satisfies the condition of dl (t) / dt <0 at at least any temperature t of t = 30 ° C to 120 ° C, adhesive composition.
However, this excludes cases where the adhesive composition contains particles of crystallized phosphate glass composed of P ₂ O ₅ and one or more cations selected from the group consisting of magnesium, cobalt, arsenic, zinc, iron, aluminum and zirconium. . The adhesive composition according to claim 5, wherein the cured product has an average coefficient of linear thermal expansion at 30°C to 120°C of 500 ppm/°C or less.

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