Resin composition, cured resin, sheet-like cured resin, laminated body, prepreg, electronic parts and multilayer boards

• US 20050003199A1
• Filed: 12/29/2003
• Published: 01/06/2005
• Est. Priority Date: 12/27/2002
• Status: Abandoned Application

• Current Assignee: TDK Corporation
• Original Assignee: TDK Corporation
• Inventors: Endo, Toshikazu, Kawabata, Kenichi, Takaya, Minoru
• Application Number:
  US10/745,587
• Publication Number:
  US 20050003199A1
• Time in Patent Office: Days
• US Class Current: 428/413
• CPC Class Codes: B32B 15/08 of synthetic resin
• CPC Class Codes: B32B 2305/076 Prepregs
• CPC Class Codes: B32B 2305/08 Reinforcements
• CPC Class Codes: B32B 2307/202 Conductive
• CPC Class Codes: B32B 2307/204 Di-electric
• CPC Class Codes: B32B 2307/206 Insulating
• CPC Class Codes: B32B 27/08 of synthetic resin
• CPC Class Codes: B32B 9/005 comprising one layer of ceramic material, e.g. porcelain, ceramic tile layered products with at least two ceramic layers composed mainly of ceramic B32B18/00
• CPC Class Codes: C08G 59/4223 aromatic
• CPC Class Codes: C08J 2363/00 Characterised by the use of epoxy resins; Derivatives of epoxy resins
• CPC Class Codes: C08J 5/10 characterised by the additives used in the polymer mixture
• CPC Class Codes: C08J 5/18 Manufacture of films or sheets
• CPC Class Codes: C08J 5/244 using glass fibres
• CPC Class Codes: C08J 5/249 characterised by the additives used in the prepolymer mixture
• CPC Class Codes: C08L 2666/18 Polyesters or polycarbonates according to C08L67/00 - C08L69/00; Derivatives thereof
• CPC Class Codes: C08L 63/00 Compositions of epoxy resins; Compositions of derivatives of epoxy resins
• CPC Class Codes: C08L 67/03 the dicarboxylic acids and dihydroxy compounds having the carboxyl- and the hydroxy groups directly linked to aromatic rings
• CPC Class Codes: H01F 17/0006 Printed inductances printed coils for dynamo-electric machines H02K3/26; printed circuits H05K
• CPC Class Codes: H01F 2017/048 with encapsulating core, e.g. made of resin and magnetic powder
• CPC Class Codes: H01F 27/323 Insulation between winding turns, between winding layers
• CPC Class Codes: H01F 27/327 : Encapsulating or impregnating encapsulating coil and core H01F27/022
• CPC Class Codes: H01L 2224/32225 : the item being non-metallic, e.g. insulating substrate with or without metallisation
• CPC Class Codes: H01L 2224/45015 : being circular
• CPC Class Codes: H01L 2224/45099 : Material
• CPC Class Codes: H01L 2224/48091 : Arched
• CPC Class Codes: H01L 2224/48227 : connecting the wire to a bond pad of the item
• CPC Class Codes: H01L 2224/73265 : Layer and wire connectors
• CPC Class Codes: H01L 23/49894 : Materials of the insulating layers or coatings
• CPC Class Codes: H01L 24/48 : of an individual wire connector
• CPC Class Codes: H01L 25/16 : the devices being of types provided for in two or more different main groups of groups H01L27/00 - H01L33/00, or in a single subclass of H10K, H10N, e.g. forming hybrid circuits
• CPC Class Codes: H01L 2924/00 : Indexing scheme for arrangements or methods for connecting or disconnecting semiconductor or solid-state bodies as covered by H01L24/00
• CPC Class Codes: H01L 2924/00012 : Relevant to the scope of the group, the symbol of which is combined with the symbol of this group
• CPC Class Codes: H01L 2924/00014 : the subject-matter covered by the group, the symbol of which is combined with the symbol of this group, being disclosed without further technical details
• CPC Class Codes: H01L 2924/01012 : Magnesium [Mg]
• CPC Class Codes: H01L 2924/01019 : Potassium [K]
• CPC Class Codes: H01L 2924/0102 : Calcium [Ca]
• CPC Class Codes: H01L 2924/01025 : Manganese [Mn]
• CPC Class Codes: H01L 2924/01046 : Palladium [Pd]
• CPC Class Codes: H01L 2924/01068 : Erbium [Er]
• CPC Class Codes: H01L 2924/01078 : Platinum [Pt]
• CPC Class Codes: H01L 2924/01079 : Gold [Au]
• CPC Class Codes: H01L 2924/12041 : LED
• CPC Class Codes: H01L 2924/12042 : LASER
• CPC Class Codes: H01L 2924/181 : Encapsulation
• CPC Class Codes: H01L 2924/19041 : being a capacitor
• CPC Class Codes: H01L 2924/19105 : in a side-by-side arrangement on a common die mounting substrate
• CPC Class Codes: H01L 2924/207 : Diameter ranges
• CPC Class Codes: H01L 2924/30107 : Inductance
• CPC Class Codes: H01L 2924/3011 : Impedance
• CPC Class Codes: H01L 2924/3025 : Electromagnetic shielding
• CPC Class Codes: H05K 1/0373 : containing additives, e.g. fillers H05K1/036 takes precedence
• CPC Class Codes: H05K 1/162 : incorporating printed capacitors
• CPC Class Codes: H05K 2201/0209 : Inorganic, non-metallic particles
• CPC Class Codes: H05K 2201/09672 : Superposed layout, i.e. in different planes parallel traces in one plane H05K2201/09236
• CPC Class Codes: H05K 3/4626 : characterised by the insulating layers or materials H05K3/4688 takes precedence
• CPC Class Codes: H05K 3/4676 : Single layer compositions
• CPC Class Codes: H05K 3/4688 : Composite multilayer circuits, i.e. comprising insulating layers having different properties having a special base or central core H05K3/4602
• CPC Class Codes: Y10T 428/2971 : Impregnation
• CPC Class Codes: Y10T 428/31511 : Of epoxy ether
• CPC Class Codes: Y10T 428/31515 : As intermediate layer
• CPC Class Codes: Y10T 428/31522 : Next to metal
• CPC Class Codes: Y10T 428/31529 : Next to metal

Abstract

The invention provides electronic parts which comprise a composite dielectric layer composed of an organic insulating material and a dielectric ceramic powder having a larger relative dielectric constant than the organic insulating material, and which also comprise conductive element sections forming inductor elements, etc., wherein the organic insulating material comprises a cured resin obtained by curing reaction of an epoxy resin with an active ester compound obtained by reaction between a compound with two or more carboxyl groups and a compound with a phenolic hydroxyl group. The dielectric ceramic powders of the described electronic parts have larger relative dielectric constants than the organic insulating materials, and the organic insulating materials have low dielectric loss tangents. It is possible to adequately reduce time-dependent dielectric constant changes in the high-frequency range of 100 MHz and above even with prolonged use at high temperatures of 100° C. and higher, while it is also possible to satisfactorily prevent deformation and other damage to the electronic parts during their handling.

Claims

1. A resin composition comprising a curable mixture containing an epoxy resin and an active ester compound obtained by reaction between a compound with a phenolic hydroxyl group and a compound with two or more groups which form ester bonds by reaction with said phenolic hydroxyl group,

with a dielectric ceramic powder distributed in said curable mixture.

2. A resin composition according to claim 1, wherein said active ester compound is an aromatic active ester compound represented by the following general formula (1).

3. A resin composition according to claim 1, wherein said dielectric ceramic powder is a metal oxide powder comprising at least one metal selected from the group consisting of magnesium, silicon, aluminum, titanium, zinc, calcium, strontium, zirconium, barium, tin, neodymium, bismuth, lithium, samarium and tantalum, and it is metal oxide powder having a dielectric constant of 3.7-300 and a Q value of 500-100,000.

4. A resin composition according to claim 1, wherein the content of said dielectric ceramic powder is 5-185 parts by volume with respect to 100 parts by volume as the total of said epoxy resin and said active ester compound.

5. A resin composition according to claim 1, which further comprises a polyarylate.

6. A resin composition according to claim 5, wherein said polyarylate comprises a plurality of repeating units represented by —

X—

Y composed of structural unit X and structural unit Y (The plurality of each of the structural units X and structural units Y may be the same or different.),

wherein said structural unit X is a phthaloyl group, isophthaloyl group or terephthaloyl group represented by the following formula (2) (wherein the number of moles of terephthaloyl groups constitutes less than 40 mole percent of the total moles of the phthaloyl, isophthaloyl and terephthaloyl groups),

and said structural unit Y is a divalent group represented by the following general formula (3).

[wherein R¹¹ and R¹² each independently represent C1-4 alkyl, alkoxy or a halogen, Z represents a single bond, ether bond, thioether bond, sulfone bond or carbonyl bond, and p and q each independently represent an integer of 0-4, with the proviso that when more than one R¹¹, R¹² and Z are present in the polyarylate, R¹¹, R¹² and Z may be the same or different.]

7. A resin composition according to claim 6, wherein R ¹¹ and R¹² are both methyl and Z is a single bond.

8. A resin composition according to claim 5, wherein the content of said dielectric ceramic powder is 5-185 parts by volume with respect to 100 parts by volume as the total of said epoxy resin, said active ester compound and said polyarylate.

9. A resin composition according to claim 1, which further comprises one or more additives selected from the group consisting of coupling agents, curing accelerators, flame retardants, flexibilizers and organic solvents.

10. A resin composition according to claim 9, wherein at least a portion of the coupling agent is bonded or adsorbed onto the surface of the dielectric ceramic powder.

11. A cured resin obtained by partially completing the curing reaction between said epoxy resin and said active ester compound in a resin composition according to claim 1.

12. A cured resin obtained by fully completing the curing reaction between said epoxy resin and said active ester compound in a resin composition according to claim 1.

13. A sheet-like cured resin comprising a cured resin according to claim 11 shaped into the form of a sheet.

14. A sheet-like cured resin according to claim 13, which has a thickness of 5-200 μ

m.

15. A sheet-like cured resin comprising a cured resin according to claim 12 shaped into the form of a sheet.

16. A sheet-like cured resin according to claim 15, which has a thickness of 5-1000 μ

m.

17. A laminated body comprising a sheet-like cured resin according to claim 13 and a metal foil bonded on one or both sides of said sheet-like cured resin.

18. A laminated body comprising a sheet-like cured resin according to claim 15 and a metal foil bonded on one or both sides of said sheet-like cured resin.

19. A prepreg obtained by semi-curing of a resin composition comprising a curable mixture containing an epoxy resin and an active ester compound obtained by reaction between a compound with a phenolic hydroxyl group and a compound with two or more groups which form ester bonds by reaction with said phenolic hydroxyl group, with a dielectric ceramic powder and reinforcing fibers distributed in said curable mixture.

23. A prepreg according to claim 19, wherein said active ester compound is an aromatic active ester compound represented by the following general formula (1).

24. A prepreg according to claim 19, wherein said dielectric ceramic powder is a metal oxide powder comprising at least one metal selected from the group consisting of magnesium, silicon, aluminum, titanium, zinc, calcium, strontium, zirconium, barium, tin, neodymium, bismuth, lithium, samarium and tantalum, and it is metal oxide powder having a dielectric constant of 3.7-300 and a Q value of 500-100,000.

25. A prepreg according to claim 19, wherein the content of said dielectric ceramic powder is 5-100 parts by volume with respect to 100 parts by volume as the total of said epoxy resin and said active ester compound.

26. A prepreg according to claim 19, wherein said resin composition further comprises a polyarylate.

27. A prepreg according to claim 26, wherein said polyarylate comprises a plurality of repeating units represented by —

X—

Y composed of structural unit X and structural unit Y (The plurality of each of the structural units X and structural units Y may be the same or different.),

wherein said structural unit X is a phthaloyl group, isophthaloyl group or terephthaloyl group represented by the following formula (2) (wherein the number of moles of terephthaloyl groups constitutes less than 40 mole percent of the total moles of the phthaloyl, isophthaloyl and terephthaloyl groups),

and said structural unit Y is a divalent group represented by the following general formula (3).

[wherein R¹¹ and R¹² each independently represent C1-4 alkyl, alkoxy or a halogen, Z represents a single bond, ether bond, thioether bond, sulfone bond or carbonyl bond, and p and q each independently represent an integer of 0-4, with the proviso that when more than one R¹¹, R¹² and Z are present in the polyarylate, R¹¹, R¹² and Z may be the same or different.]

28. A prepreg according to claim 27, wherein R¹¹ and R¹² are both methyl and Z is a single bond.

29. A prepreg according to claim 26, wherein the content of said dielectric ceramic powder is 5-100 parts by volume with respect to 100 parts by volume as the total of said epoxy resin, said active ester compound and said polyarylate.

30. A prepreg according to claim 19, wherein said resin composition further comprises one or more additives selected from the group consisting of coupling agents, curing accelerators, flame retardants and flexibilizers.

31. A prepreg according to claim 30, wherein at least a portion of said coupling agent is bonded or adsorbed onto the surface of said dielectric ceramic powder.

32. A prepreg according to claim 19, wherein said reinforcing fibers are at least one type of reinforcing fibers selected from the group consisting of E glass fibers, D glass fibers, NE glass fibers, H glass fibers, T glass fibers and aramid fibers.

33. A sheet-like cured resin comprising a cured prepreg according to claim 19 shaped into the form of a sheet.

34. A sheet-like cured resin according to claim 33, which has a thickness of 30-10,000 μ

m.

35. A laminated body comprising a sheet-like cured resin according to claim 33 and a metal foil bonded on one or both sides of said sheet-like cured resin.

20. A prepreg comprising a reinforcing fiber fabric consisting of woven reinforcing fibers, and a resin layer formed on both sides of said reinforcing fiber fabric,

wherein said resin layer is a resin layer obtained by semi-curing of a resin composition comprising a curable mixture containing an epoxy resin and an active ester compound obtained by reaction between a compound with a phenolic hydroxyl group and a compound with two or more groups which form ester bonds by reaction with said phenolic hydroxyl group,

with a dielectric ceramic powder distributed in said curable mixture.

21. A prepreg according to claim 20, wherein said resin layer has a thickness of 5-100 μ

m.

22. A prepreg according to claim 20, wherein said reinforcing fiber fabric has a thickness of 20-300 μ

m.

36. An electronic part provided with at least one composite dielectric layer containing an organic insulating material and a dielectric ceramic powder having a larger relative dielectric constant than said organic insulating material,

and at least one conductive element section formed on said composite dielectric layer and constituting a capacitor element or inductor element,

wherein said organic insulating material comprises a cured resin obtained by curing reaction between an epoxy resin and an active ester compound which is itself obtained by reaction between a compound having two or more carboxyl groups and a compound having a phenolic hydroxyl group.

37. An electronic part according to claim 36, wherein said active ester compound is an aromatic active ester compound represented by the following general formula (1).

38. An electronic part according to claim 36, wherein said dielectric ceramic powder is a metal oxide powder comprising at least one metal selected from the group consisting of magnesium, silicon, aluminum, titanium, zinc, calcium, strontium, zirconium, barium, tin, neodymium, bismuth, lithium, samarium and tantalum, and it is metal oxide powder having a dielectric constant of 3.7-300 and a Q value of 500-100,000.

39. An electronic part according to claim 36, wherein said organic insulating material further comprises a polyarylate.

40. An electronic part according to claim 39, wherein said polyarylate comprises a plurality of repeating units represented by —

X—

Y composed of structural unit X and structural unit Y (The plurality of each of the structural units X and structural units Y may be the same or different.),

wherein said structural unit X is a phthaloyl group, isophthaloyl group or terephthaloyl group represented by the following formula (2) (wherein the number of moles of terephthaloyl groups constitutes less than 40 mole percent of the total moles of the phthaloyl, isophthaloyl and terephthaloyl groups),

and said structural unit Y is a divalent group represented by the following general formula (3).

[wherein R¹¹ and R¹² each independently represent C1-4 alkyl, alkoxy or a halogen, Z represents a single bond, ether bond, thioether bond, sulfone bond or carbonyl bond, and p and q each independently represent an integer of 0-4, with the proviso that when more than one R¹¹, R¹² and Z are present in the polyarylate, R¹¹, R¹² and Z may be the same or different.]

41. An electronic part according to claim 40, wherein R¹¹ and R¹² are both methyl and Z is a single bond.

42. An electronic part according to claim 36, wherein said dielectric ceramic powder is added at 5-185 parts by volume with respect to 100 parts by volume of said organic insulating material.

43. An electronic part according to claim 36, wherein said cured resin is obtained by curing reaction between said epoxy resin and said active ester compound in the presence of an additive, and said additive is at least one additive selected from the group consisting of curing accelerators, surface treatment agents, flame retardants and flexibilizers.

44. An electronic part according to claim 36, wherein said composite dielectric layer further comprises a magnetic powder dispersed in said organic insulating material.

45. An electronic part according to claim 36, wherein said composite dielectric layer further comprises a cloth made of reinforcing fibers.

46. A multilayer board constructed by laminating

at least one resin-containing first dielectric layer,

at least one resin-containing second dielectric layer

and at least one conductor layer,

wherein the dielectric loss tangent tan δ

of said second dielectric layer is no greater than 0.01,

and the critical flexure of said first dielectric layer is at least 1.3 times that of said second dielectric layer.

47. A multilayer board according to claim 46, wherein said second dielectric layer further comprises a ceramic powder having a larger relative dielectric constant than said resin.

48. A multilayer board according to claim 46, having two outermost layers, with at least one of said two outermost layers being composed of said first dielectric layer and at least one of said second dielectric layers being situated between said two outermost layers.

49. A multilayer board according to claim 46, wherein the peel strength of said first dielectric layer is at least 1.5 times the peel strength of said second dielectric layer.

51. A multilayer board according to claim 49, wherein the peel strengths of said first dielectric layers are at least 8 N/cm.

58. An electronic part comprising

a multilayer board according to claim 46,

and an electrical element formed on said multilayer board.

50. A multilayer board constructed by laminating two resin-containing first dielectric layers,

at least one resin-containing second dielectric layer situated between said two first dielectric layers,

and at least one conductor layer,

wherein at least one of said two first dielectric layers constitutes the outermost layer,

the dielectric loss tangent tan δ

of said second dielectric layer is no greater than 0.01,

and the peel strengths of said first dielectric layers are at least 1.5 times the peel strength of said second dielectric layer.

52. An electronic part constructed by laminating at least one resin-containing first dielectric layer,

at least one resin-containing second dielectric layer,

and at least one conductor layer,

wherein the dielectric loss tangent tan δ

of said second dielectric layer is no greater than 0.01,

and the critical flexure of said first dielectric layer is at least 1.3 times that of said second dielectric layer.

53. An electronic part according to claim 52, wherein said second dielectric layer further comprises a ceramic powder having a larger relative dielectric constant than said resin.

54. An electronic part according to claim 52, having two outermost layers, with at least one of said two outermost layers being composed of said first dielectric layer and at least one of said second dielectric layers being situated between said two outermost layers.

55. An electronic part according to claim 52, wherein the peel strength of said first dielectric layer is at least 1.5 times the peel strength of said second dielectric layer.

57. An electronic part according to claim 55, wherein the peel strengths of said first dielectric layers are at least 8 N/cm.

56. An electronic part constructed by laminating two resin-containing first dielectric layers,

at least one resin-containing second dielectric layer situated between said two first dielectric layers,

and at least one conductor layer,

wherein at least one of said two first dielectric layers constitutes the outermost layer,

the dielectric loss tangent tan δ

of said second dielectric layer is no greater than 0.01,

and the peel strengths of said first dielectric layers are at least 1.5 times the peel strength of said second dielectric layer.