Adhesive composition and adhesive sheet, and hardened article and semiconductor device using same
The purpose of the present invention is to provide an adhesive composition having high heat conductivity and excellent adhesion, in which the dispersibility of a heat-conductive filler is controlled, and in which thermal stress during cooling/heating cycle testing can be alleviated. An adhesive composition containing a soluble polyimide (A), an epoxy resin (B), and a heat-conductive filler (C), the adhesive composition characterized by containing three types of diamine residues having a specific structure, and in that the content of the epoxy resin (B) is 30-100 parts by weight with respect to 100 parts by weight of the soluble polyimide (A).
1. An adhesive composition containing an organic-solvent-soluble polyimide (A), an epoxy resin (B) and a thermally conductive filler (C),
wherein the organic-solvent-soluble polyimide (A) contains a diamine residue having a structure represented by the following general formula (1), a diamine residue represented by the following general formula (2) and a diamine residue represented by the following general formula (3), and
the content of the epoxy resin (B) is not less than 30 parts by weight and not more than 100 parts by weight with respect to 100 parts by weight of the organic-solvent-soluble polyimide (A):
in the general formula (1), X represents an integer of 1 to 10 and n represents an integer of 1 to 20;
in the general formula (2), m represents an integer of 1 to 30, and R 5 and R 6 may be the same or different and represent an alkylene group having 1 to 30 carbon atoms or a phenylene group, R 1 to R 4 each may be the same or different and represent an alkyl group having 1 to 30 carbon atoms, a phenyl group or a phenoxy group;
2. The adhesive composition according to claim 1 , wherein
the content of the diamine residue having a structure represented by the general formula (1) is 30% by mole or more in all the diamine residues,
the content of the diamine residue represented by the general formula (2) is 10% by mole or more in all the diamine residues, and
the content of the diamine residue represented by the general formula (3) is 5% by mole or more in all the diamine residues.
3. The adhesive composition according to claim 1 , wherein the epoxy resin (B) has a skeleton represented by the following general formula (4):
4. The adhesive composition according to claim 1 , wherein the content of the thermally conductive filler (C) is not less than 60% by volume and not more than 90% by volume in the adhesive composition.
5. The adhesive composition according to claim 1 , wherein the thermally conductive filler (C) contains three types of thermally conductive fillers differing in the average particle diameter, a thermally conductive filler (C-1), a thermally conductive filler (C-2) and a thermally conductive filler (C-3), and
when average particle diameters of the thermally conductive fillers (C-1), (C-2) and (C-3) are denoted by d1, d2 and d3, respectively, an average particle diameter ratio d1/d2 is not less than 1.5 and not more than 15 and an average particle diameter ratio d2/d3 is not less than 1.5 and not more than 15.
6. The adhesive composition according to claim 5 , wherein the average particle diameter d3 of the thermally conductive filler (C-3) is 2 μm or less.
7. The adhesive composition according to claim 5 , wherein the thermally conductive filler (C-1) is aluminum nitride.
8. The adhesive composition according to claim 5 , wherein the content of the thermally conductive filler (C-1) is not less than 40% by volume and not more than 80% by volume in the whole thermally conductive fillers (C).
9. A adhesive sheet obtained by forming the adhesive composition according to claim 1 into a sheet.
10. A layered product including an adhesive layer and a radiating fin made of a metallic substrate, wherein the adhesive layer is formed by adhering the adhesive sheet according to claim 9 to the radiating fin.
11. A power IC packaging which is obtained by bonding the layered product according to claim 10 by way of thermocompression to a lead frame, which is made of copper, of a semiconductor device having the power IC mounted thereon.
12. A layered product including an adhesive layer and a radiating fin made of a metallic substrate, wherein the adhesive layer is formed by applying a varnish of the adhesive composition according to claim 1 onto the radiating fin and drying the varnish.
13. A power IC packaging which is obtained by bonding the layered product according to claim 12 by way of thermocompression to a lead frame, which is made of copper, of a semiconductor device having the power IC mounted thereon.
14. The power IC packaging according to claim 13 , wherein the power IC is Si semiconductor or SiC semiconductor.
15. A hardened article obtained by hardening an adhesive composition containing an organic-solvent-soluble polyimide (A), an epoxy resin (B) and a thermally conductive filler (C),
wherein the organic-solvent-soluble polyimide (A) contains a diamine residue having a structure represented by the following general formula (1), a diamine residue represented by the following general formula (2) and a diamine residue represented by the following general formula (3), and
the content of the epoxy resin (B) is not less than 30 parts by weight and not more than 100 parts by weight with respect to 100 parts by weight of the organic-solvent-soluble polyimide (A):
in the general formula (1), X represents an integer of 1 to 10 and n represents an integer of 1 to 20;
in the general formula (2), m represents an integer of 1 to 30, and R 5 and R 6 may be the same or different and represent an alkylene group having 1 to 30 carbon atoms or a phenylene group, R 1 to R 4 each may be the same or different and represent an alkyl group having 1 to 30 carbon atoms, a phenyl group or a phenoxy group;
16. A semiconductor device including the hardened article according to claim 15 .