WO2019203048A1 - 電子装置の製造方法 - Google Patents
電子装置の製造方法 Download PDFInfo
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- WO2019203048A1 WO2019203048A1 PCT/JP2019/015339 JP2019015339W WO2019203048A1 WO 2019203048 A1 WO2019203048 A1 WO 2019203048A1 JP 2019015339 W JP2019015339 W JP 2019015339W WO 2019203048 A1 WO2019203048 A1 WO 2019203048A1
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- Prior art keywords
- electronic device
- manufacturing
- flux
- resin composition
- resin
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Classifications
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- H01L24/12—Structure, shape, material or disposition of the bump connectors prior to the connecting process
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- B23—MACHINE TOOLS; METAL-WORKING NOT OTHERWISE PROVIDED FOR
- B23K—SOLDERING OR UNSOLDERING; WELDING; CLADDING OR PLATING BY SOLDERING OR WELDING; CUTTING BY APPLYING HEAT LOCALLY, e.g. FLAME CUTTING; WORKING BY LASER BEAM
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Definitions
- the present invention relates to a method for manufacturing an electronic device.
- a soldering agent is usually used to connect a semiconductor element and a substrate using a fluxing agent and then washed with a solvent.
- the semiconductor element was encapsulated with the semiconductor encapsulating resin composition.
- the step of washing the flux residue on the substrate with a solvent may reduce the productivity of the electronic device.
- the step of cleaning the flux residue is not performed, the flux residue remains between the cured product of the resin composition of the electronic device and the substrate.
- the base material provided with the copper circuit is sealed with the resin composition due to the residual flux residue, the adhesiveness between the cured resin composition and the base material is reduced, and as a result, the electrical characteristics of the electronic device Reliability may be reduced. Therefore, there is room for improvement in terms of either productivity or manufacturing stability of the electronic device, whether or not the step of washing the flux residue with a solvent is performed.
- the present inventors do not perform the step of washing the flux residue on the base material with a solvent, thereby increasing the productivity of the electronic device, and between the cured product of the resin composition and the base material.
- we studied a method for manufacturing electronic devices with reduced flux residue Specifically, a method for removing the flux residue was examined even when the flux residue was washed with a solvent.
- an average solubility parameter based on the Hansen method of a resin group consisting of an epoxy resin and a phenol resin curing agent which contains a specific amount of rosin and has a small mass change rate before and after heat treatment. It has been found that by using a resin composition in which SP1 and the number average molecular weight Mn1 satisfy a predetermined relationship, the flux residue can be removed by incorporating the resin composition into the resin composition. Although the detailed mechanism is not clear, use of the above flux and resin composition improves the compatibility of these, so that the flux residue is taken into the resin composition and the flux residue is removed. It is thought that.
- the present inventors can remove the flux residue by using the above-mentioned flux and the resin composition in combination, and thus the adhesion between the cured product of the resin composition and the substrate. As a result, it was found that the manufacturing stability of the electronic device can be improved.
- a manufacturing method of an electronic device comprising a base material having a metal exposed portion on a surface and an electronic component provided on the base material, A flux treatment step in which the metal exposed portion is brought into contact with the flux to flux-treat the metal exposed portion; An introducing step of introducing a resin composition so as to be in contact with the surface of the exposed metal portion subjected to the flux treatment; Including The flux includes rosin, an activator, and a solvent, The content of the rosin is 1 part by mass or more and 18 parts by mass or less with respect to 100 parts by mass of the flux, In the flux, the mass change rate of the flux before and after the heat treatment measured by the following procedure is 21% by mass or less, (procedure) When the flux was heat-treated in a nitrogen atmosphere at a heating rate of 10 ° C./min and heated from 25 ° C.
- the resin composition includes an epoxy resin and a phenol resin curing agent
- SP1 is an average solubility parameter based on the Hansen method of the resin group consisting of the epoxy resin and the phenol resin curing agent
- the number average molecular weight of the resin group consisting of the epoxy resin and the phenol resin curing agent is Mn1.
- SP1 and Mn1 satisfy Mn1 ⁇ 210 ⁇ SP1-4095.
- FIG. 6 is a plot showing the relationship between the average solubility parameter SP1 of a resin group consisting of an epoxy resin and a phenol resin curing agent and the number average molecular weight Mn for the resin compositions 1 to 14 according to Examples and Comparative Examples. It is a figure which shows an example of the electronic device which concerns on this embodiment. It is a figure for demonstrating the manufacturing method of the electronic device which concerns on this embodiment.
- the manufacturing method of the electronic device includes a base material having a metal exposed portion on the surface and an electronic component provided on the base material.
- a metal exposed portion and a flux are brought into contact with each other, and a flux treatment process for flux-treating the metal exposed portion, and a resin composition is introduced so as to be in contact with the surface of the flux-treated metal exposed portion. And an introduction step.
- the flux used in the flux treatment step includes rosin, an activator, and a solvent, and the content of the rosin in the flux is 1 part by mass or more and 18 parts by mass or less with respect to 100 parts by mass of the flux.
- the mass change rate of the flux before and after the heat treatment measured by the following procedure satisfies 21% by mass or less. (procedure) When the flux is heat-treated in a nitrogen atmosphere at a heating rate of 10 ° C./min and under a heating condition where the temperature is raised from 25 ° C. to 250 ° C., the mass M1 of the flux before the heat treatment using a thermogravimetric measuring device And the mass M2 of the flux after heat processing are measured. Then, the mass change rate of the flux before and after the heat treatment is calculated based on the formula: (M2 / M1) ⁇ 100 using the obtained M1 and M2.
- the resin composition used in the introduction step includes an epoxy resin and a phenol resin curing agent.
- the flux residue may remain between the cured product of the resin composition of the electronic device and the substrate.
- the flux is a resin flux containing rosin, an activator, and a solvent.
- a flux is applied to a metal member such as an electric circuit of an electronic device
- the rosin and the activator in the flux react with the oxide film formed on the surface of the metal member to remove the oxide film.
- the metal member from which the oxide film has been removed can improve the adhesion with the solder compared to the metal member in which the oxide film exists.
- rosin and activator that did not react with the oxide film remain on the surface of the metal member. The remaining rosin and activator form a flux residue.
- the rosin becomes heat-denatured rosin by heat treatment during soldering in the manufacturing process of the electronic device.
- the heat-denatured rosin is designed to have a low affinity with water and be insulative in order to suppress adverse effects such as corrosion and short circuits on the metal member.
- Such a heat-denatured rosin and a conventional resin composition have low chemical affinity.
- heat-denatured rosin has low affinity with water.
- the shape of the heat-denatured rosin is a porous shape.
- the conventional resin composition having low chemical affinity cannot penetrate into the heat-modified rosin having a porous shape. Therefore, it is estimated that the flux residue is not compatible with the conventional resin composition.
- the activator is decomposed by heat treatment during soldering in the manufacturing process of the electronic device.
- the lead-free solder used in recent years contains a metal such as tin (Sn).
- the decomposed activator reacts with a metal such as Sn contained in the solder or a metal such as Ag, Fe, or Ni derived from the metal member, and the crystal of the metal is converted. Presumed to form.
- the friction in a flux increases and the viscosity of a flux rises.
- the viscosity of the flux increases as described above, the molecular chain of the flux and the molecular chain of the resin composition are not entangled, and the physical affinity is lowered.
- the conventional resin composition having low physical affinity does not entangle with the molecular chain of the flux. Therefore, it is estimated that the flux residue is not compatible with the conventional resin composition.
- the present inventors examined a method for removing the flux residue on the premise that the step of washing the flux residue is not performed.
- a resin composition having a specific relationship between the average solubility parameter SP1 and the number average molecular weight Mn1 based on the Hansen method of the resin group composed of an epoxy resin and a phenol resin curing agent is combined with the flux described above. It was found that the use was effective. Thereby, it is estimated that compatibility, such as chemical affinity and physical affinity with a flux and a resin composition, improves. Therefore, by introducing the resin composition, the flux and the resin composition are compatible, and the flux residue can be removed without washing the flux residue.
- the electronic device according to the present embodiment is an electronic device in which no flux residue exists between the cured product of the resin composition and the base material on the assumption that the step of cleaning the flux residue on the base material is not performed.
- the manufacturing method can be provided. Thereby, the adhesiveness of the hardened
- the resin composition according to this embodiment is a thermosetting resin composition containing an epoxy resin and a phenol resin curing agent.
- the resin composition according to this embodiment includes an average solubility parameter SP1 based on the Hansen method of a resin group consisting of an epoxy resin and a phenol resin curing agent, and a number average molecular weight Mn1 of the resin group consisting of an epoxy resin and a phenol resin curing agent.
- SP1 average solubility parameter
- Mn1 number average molecular weight
- the Hansen method divides evaporation energy into dispersion energy dD (Dispersion Energy), polarization energy dP (Polar Energy), and hydrogen bond energy dH (Hydrogen Bonding Energy), and dD, dP, and dH are used as three-dimensional vectors. This is a method of calculating the length of a vector as a solubility parameter.
- the average solubility parameter SP1 can be calculated by the following formula 1.
- Average solubility parameter SP1 ⁇ (A (n) ⁇ Ca (n) ) + ⁇ (B (m) ⁇ Cb (m) ) (Formula 1)
- a (n) is a solubility parameter calculated based on the Hansen method for each of the n types of epoxy resins contained in the resin composition.
- Ca (n) is the resin.
- the content of each of the n types of epoxy resins with respect to the total content of all the epoxy resins and all the phenolic resin curing agents in the composition refers to B (m) , m types of phenols contained in the resin composition.
- the average solubility parameter SP1 of the resin group is calculated by the following formula 2.
- Average solubility parameter SP1 A 1 ⁇ Ca 1 + A 2 ⁇ Ca 2 + B 1 ⁇ Cb 1 + B 2 ⁇ Cb 2 (Formula 2) (In Formula 2, A 1 represents the value of the solubility parameter calculated based on the Hansen method for the first epoxy resin.
- a 2 represents the solubility calculated based on the Hansen method for the second epoxy resin.
- B 1 represents the value of the solubility parameter calculated based on the Hansen method for the first curing agent
- B 2 represents the solubility parameter calculated based on the Hansen method for the second curing agent
- Ca 1 represents the content of the first epoxy resin relative to the total amount of the resin group
- Ca 2 represents the content of the second epoxy resin relative to the total amount of the resin group
- Cb 1 represents the total amount of the resin group.
- the content of the first curing agent with respect to the Cb 2 represents the content of the second curing agent with respect to the total amount of the resin group.
- the upper limit value of the average solubility parameter SP1 of the resin group is preferably, for example, 30.0 [cal / cm 3 ] 0.5 or less, and 28.0 [cal / cm 3 ] 0.5 or less. Is more preferably 26.0 [cal / cm 3 ] 0.5 or less, and particularly preferably 24.0 [cal / cm 3 ] 0.5 or less.
- the SP1 value is equal to or less than the above upper limit value, the interaction between the molecular chains of the epoxy resin and the phenol resin curing agent is reduced, and is comparable to the interaction between the molecules of the flux residue. Furthermore, it is considered that the interaction between the two becomes stronger and the compatibility is improved.
- the lower limit of the average solubility parameter SP1 of the resin group is, for example, preferably 20.8 [cal / cm 3 ] 0.5 or more, and 21.0 [cal / cm 3 ] 0.5 or more. More preferably.
- the compatibility of the resin composition with respect to the flux residue can be improved.
- the SP1 value is equal to or greater than the above lower limit value
- the interaction between the molecular chains of the epoxy resin and the phenol resin curing agent is increased, and is comparable to the interaction between the molecules of the flux residue. It is considered that the interaction between the two becomes stronger and the compatibility is improved.
- the compatibility of the resin composition and the flux residue can be improved.
- curing agent is demonstrated.
- the number average molecular weight Mn1 of the resin group can be calculated by the following formula 3.
- Number average molecular weight Mn1 ⁇ (a (n) ⁇ Ca (n) ) + ⁇ (b (m) ⁇ Cb (m) ) (Formula 3)
- a (n) refers to the value of the number average molecular weight for each of the n types of epoxy resins contained in the resin composition.
- Ca (n) is the total number in the resin composition.
- each of the n types of epoxy resins relative to the total content of the epoxy resin and the total phenolic resin curing agent is indicated, and b (m) relates to each of the m types of phenolic resin curing agents contained in the resin composition.
- Cb (m) represents the content of each of the m types of phenol resin curing agents relative to the total content of all epoxy resins and all phenol resin curing agents in the resin composition.
- N and m are integers of 1 or more.
- the resin group included in the resin composition according to the present embodiment includes a first epoxy resin, a second epoxy resin, a first phenol resin curing agent, and a second phenol resin curing.
- the number average molecular weight Mn1 of the resin group is calculated by the following formula 4.
- Number average molecular weight Mn1 a 1 ⁇ Ca 1 + a 2 ⁇ Ca 2 + b 1 ⁇ Cb 1 + b 2 ⁇ Cb 2 (Formula 4)
- a 1 represents the number average molecular weight of the first epoxy resin.
- a 2 represents the number average molecular weight of the second epoxy resin.
- B 1 represents the first phenol resin curing agent.
- the .b 2 to refer to number average molecular weight, .ca 1 showing a number-average molecular weight of the second phenolic resin curing agent, .ca 2 showing the content of the first epoxy resin to the resin group the total amount, the resin group total amount Cb 1 indicates the content of the first phenol resin curing agent relative to the total amount of the resin group, and Cb 2 indicates the content of the second phenol resin curing agent relative to the total amount of the resin group. Indicates the amount.
- the lower limit of the number average molecular weight Mn1 of the resin group is, for example, preferably 250 or more, more preferably 260 or more, and further preferably 265 or more.
- the interaction between the rosin and active species contained in the flux residue and the main chain constituting the molecular structure of the epoxy resin or phenol resin curing agent is promoted. Compatibility can be improved.
- the number average molecular weight Mn1 is not less than the above lower limit, the entanglement between the molecular chains of the epoxy resin and the phenol resin curing agent increases. Thereby, the mobility of the molecular chains of the epoxy resin and the phenol resin curing agent is limited.
- the flux residue can easily interact with the epoxy resin and the phenol resin curing agent, and the compatibility can be improved.
- the upper limit value of the number average molecular weight Mn1 of the resin group is, for example, preferably 550 or less, and more preferably 520 or less. As a result, the interaction between the rosin and active species contained in the flux residue and the main chain constituting the molecular structure of the epoxy resin or phenol resin curing agent is promoted. Compatibility can be improved.
- the present inventors have studied a combination of an epoxy resin in the resin composition and a phenol resin curing agent. .
- SP1 which is the chemical compatibility of the molecular chain such as hydrogen bond, dispersion force, and dipole interaction
- Mn1 which is the physical compatibility such as the shape of the molecular chain
- the composition and the flux residue can be dissolved.
- the specific numerical range it is preferable that the number average molecular weight Mn1 is small and the average solubility parameter SP1 is large so as to satisfy the relationship of Mn1 ⁇ 210 ⁇ SP1-4095.
- Mn1 when Mn1 is plotted against SP1, Mn1 is equal to 210 ⁇ SP1-4095, or Mn1 becomes smaller than that or SP1 becomes larger. Show. In the relational expression of Mn1 ⁇ 210 ⁇ SP1-4095, the unit of Mn1 is dimensionless and the unit of SP1 is [cal / cm 3 ] 0.5 .
- curing agent and the molecular chain of a flux residue can be improved because the value of SP1 becomes large.
- the interaction between the molecular chains of the flux residue is far more than the interaction between the molecular chain of the epoxy resin and the phenol resin curing agent and the molecular chain of the flux residue. It was big.
- the molecular chains of the epoxy resin and the phenol resin curing agent and the molecular chains of the flux residue enhance the chemical affinity, so that the molecular chains of the epoxy resin and the phenol resin curing agent are included in the flux residue. Easy to take up molecular chains. From the above, it is presumed that the resin composition and the flux residue can be compatible with each other when both Mn1 and SP1 are in an appropriate numerical range.
- a relationship between SP1 and Mn1 for example, a relationship of 210 ⁇ SP1-5000 ⁇ Mn1 may further hold.
- the resin composition according to the present embodiment includes an epoxy resin and a phenol resin curing agent.
- epoxy resin As the epoxy resin according to the present embodiment, monomers, oligomers and polymers generally having two or more epoxy groups in one molecule can be used, and the molecular weight and molecular structure are not particularly limited. Specific examples of the epoxy resin include biphenyl type epoxy resins; bisphenol type epoxy resins such as bisphenol A type epoxy resins, bisphenol F type epoxy resins, and tetramethylbisphenol F type epoxy resins; stilbene type epoxy resins; phenol novolac type epoxies.
- novolak epoxy resin such as cresol novolac epoxy resin
- multifunctional such as triphenyl epoxy resin exemplified by triphenylmethane epoxy resin, triphenolmethane epoxy resin, alkyl-modified triphenolmethane epoxy resin, etc.
- Epoxy resin phenol aralkyl type epoxy resin having a phenylene skeleton, naphthol aralkyl type epoxy resin having a phenylene skeleton, phenol aralkyl type epoxy having a biphenylene skeleton
- Phenyl aralkyl type epoxy resins such as xylene resins (biphenyl aralkyl type epoxy resins) and biphenylene skeleton-containing naphthol aralkyl type epoxy resins
- dihydroxy naphthalene type epoxy resins, naphthols such as epoxy resins obtained by dihydroxy naphthalene dimerization Type epoxy resins
- triazine nucleus-containing epoxy resins such as triglycidyl isocyanurate and monoallyl diglycidyl isocyanurate
- bridged cyclic hydrocarbon compound-modified phenol type epoxy resins such as dicyclopentadiene-modified phenol type epoxy resins.
- an epoxy resin it can use 1 type or in combination of 2 or more types among the said specific examples.
- the epoxy resin it is preferable to use one or more selected from the group consisting of biphenyl type epoxy resin, polyfunctional epoxy resin, phenol aralkyl type epoxy resin, and bisphenol type epoxy resin among the above specific examples. . Thereby, average solubility parameter SP1 can be enlarged and the compatibility of a resin composition and a flux can be improved.
- the lower limit of the content of the epoxy resin in the resin composition is, for example, preferably 2 parts by mass or more and more preferably 4 parts by mass or more with respect to 100 parts by mass of the total solid content of the resin composition. Preferably, it is 6 parts by mass or more. Moreover, it is preferable that it is 20 mass parts or less with respect to 100 mass parts of total solids of a resin composition, for example, and the upper limit of content of the epoxy resin in a resin composition is 15 mass parts or less. Is more preferable, and it is still more preferable that it is 12 mass parts or less.
- the average solubility parameter SP1 can be set within a desired numerical range while satisfying the above-described number average molecular weight Mn1.
- the total solid content of the resin composition refers to the entire component excluding the solvent contained in the resin composition.
- the phenol resin curing agent includes all monomers, oligomers, and polymers having two or more phenolic hydroxyl groups in one molecule, and the molecular weight and molecular structure are not particularly limited.
- Specific examples of the phenol resin curing agent include phenol novolac resins, cresol novolac resins, trisphenol methane type phenol novolac resins, naphthol novolac resins and other novolac type phenol resins; triphenol methane type phenol resins and other polyfunctional phenols.
- Modified phenol resin such as terpene modified phenol resin, triphenylmethane phenol resin modified with formaldehyde, trihydroxyphenylmethane phenol resin modified with formaldehyde, dicyclopentadiene modified phenol resin; phenylene skeleton and / or biphenylene skeleton Phenol aralkyl resin, naphthol aralkyl resin having phenylene and / or biphenylene skeleton, phenyl aralkyl type phenol resin Aralkyl type phenol resins such as a biphenyl aralkyl type phenol resin; bisphenol A, and the like bisphenol compounds such as bisphenol F.
- Modified phenol resin such as terpene modified phenol resin, triphenylmethane phenol resin modified with formaldehyde, trihydroxyphenylmethane phenol resin modified with formaldehyde, dicyclopentadiene modified phenol resin; phenylene skeleton and /
- curing agent it can use 1 type or in combination of 2 or more types among the said specific examples.
- curing agent it is preferable to use 1 type (s) or 2 or more types selected from the group which consists of a novolak type phenol resin, a polyfunctional type phenol resin, and an aralkyl type phenol resin among the said specific examples, for example.
- average solubility parameter SP1 can be enlarged and the compatibility of a resin composition and a flux can be improved.
- the lower limit of the content of the phenol resin curing agent in the resin composition is, for example, preferably 2 parts by mass or more with respect to 100 parts by mass of the total solid content of the resin composition, and 3 parts by mass or more. Is more preferable. Moreover, it is preferable that it is 20 mass parts or less with respect to 100 mass parts of total solids of a resin composition, for example, and the upper limit of content of the phenol resin hardening
- the resin composition according to the present embodiment includes, as necessary, various additives such as a curing accelerator, a filler, a coupling agent, a release agent, a colorant, a flame retardant, an ion scavenger, and a low stress agent.
- various additives such as a curing accelerator, a filler, a coupling agent, a release agent, a colorant, a flame retardant, an ion scavenger, and a low stress agent.
- 1 type (s) or 2 or more types can be mix
- the curing accelerator is not limited as long as it accelerates the curing reaction of the epoxy resin and the curing agent, and can be selected according to the type of the epoxy resin and the curing agent.
- Specific examples of the curing accelerator include onium salt compounds, organic phosphines such as triphenylphosphine, tetra-substituted phosphonium compounds, phosphobetaine compounds, addition products of phosphine compounds and quinone compounds, addition of phosphonium compounds and silane compounds.
- Phosphorus-containing compounds such as 2-methylimidazole, 2-ethyl-4-methylimidazole (EMI24), 2-phenyl-4-methylimidazole (2P4MZ), 2-phenylimidazole (2PZ), 2-phenyl-4 -Imidazole compounds such as methyl-5-hydroxyimidazole (2P4MHZ) and 1-benzyl-2-phenylimidazole (1B2PZ); 1,8-diazabicyclo [5.4.0] undecene-7, benzyldimethylamine and the like Amidine and grade 3 Min; like the amidine or a nitrogen atom-containing compounds such as quaternary ammonium salts of the tertiary amines.
- EMI24 2-methylimidazole
- 2-phenylimidazole (2PZ) 2-phenyl-4 -Imidazole compounds
- the resin composition according to the present embodiment may further include, for example, a filler.
- the filler is not limited, and an appropriate filler can be selected according to the structure of the electronic device, the mechanical strength required for the electronic device, and the thermal characteristics.
- Specific examples of the filler include fused crushed silica, fused spherical silica, crystalline silica, secondary agglomerated silica, and spherical fine powder silica; alumina, silicon nitride, aluminum nitride, boron nitride, titanium oxide, silicon carbide And metal compounds such as aluminum hydroxide, magnesium hydroxide and titanium white; talc; clay; mica; glass fiber.
- a filler it can use 1 type or in combination of 2 or more types among the said specific examples.
- silica is preferably used as the filler.
- adherence adjuvant interact, and it can improve adhesiveness further.
- the lower limit value of the volume-based cumulative 50% particle size (D 50 ) of the filler is, for example, preferably 0.1 ⁇ m or more, more preferably 0.3 ⁇ m or more, and The thickness is further preferably 5 ⁇ m or more, and more preferably 1 ⁇ m or more.
- the viscosity of a resin composition can be improved. Therefore, when the resin composition is introduced, the flux is more preferably taken into the resin composition.
- the upper limit value of the volume-based cumulative 50% particle size (D 50 ) of the filler is, for example, preferably 50 ⁇ m or less, more preferably 30 ⁇ m or less, and even more preferably 25 ⁇ m or less.
- the volume-based cumulative 50% particle size (D50) of the filler is determined using, for example, a commercially available laser diffraction particle size distribution measuring device (for example, SALD-7000, manufactured by Shimadzu Corporation). The particle size distribution can be measured and calculated on a volume basis.
- the lower limit of the content of the filler in the resin composition according to the present embodiment is, for example, preferably 70 parts by mass or more, and 75 parts by mass or more with respect to 100 parts by mass of the solid content of the resin composition. More preferably, it is preferably 80 parts by mass or more. Thereby, the intensity
- the upper limit of the content of the filler in the resin composition is preferably 95 parts by mass or less, more preferably 93 parts by mass or less, with respect to the solid content of the resin composition, It is preferable that it is 90 mass parts or less. Thereby, the viscosity of a resin composition can be improved. Therefore, when the resin composition is introduced, the flux is more preferably taken into the resin composition.
- the well-known coupling agent used for an electronic device can be used.
- Specific examples of the coupling agent include vinyl silanes such as vinyltrimethoxysilane and vinyltriethoxysilane; 2- (3,4-epoxycyclohexyl) ethyltrimethoxysilane, 3-glycidoxypropylmethyldimethoxysilane, 3 -Epoxy silanes such as glycidoxypropyltrimethoxysilane, 3-glycidoxypropylmethyldiethoxysilane, 3-glycidoxypropyltriethoxysilane; styryl silanes such as p-styryltrimethoxysilane; 3-methacryloxypropyl Methacrylic silanes such as methyldimethoxysilane, 3-methacryloxypropyltrimethoxysilane, 3-methacryloxypropylmethyldiethoxysilane, 3-methacryloxypropylmethyldiethoxysilane,
- 1 type (s) or 2 or more types can be mix
- aminosilane is preferably used among the above specific examples.
- aminosilane for example, N-phenyl ⁇ -aminopropyltrimethoxysilane is more preferably used.
- the well-known mold release agent used for the sealing material of an electronic device can be used.
- Specific examples of the release agent include natural waxes such as carnauba wax, synthetic waxes such as diethanolamine / dimantane ester, higher fatty acids such as zinc stearate and metal salts thereof, paraffin, and the like.
- 1 type (s) or 2 or more types can be mix
- coloring agent It does not limit as a coloring agent, The well-known coloring agent used for the sealing material of an electronic device can be used. Specific examples of the colorant include carbon black, bengara, and titanium oxide. As a coloring agent, 1 type (s) or 2 or more types can be mix
- flame retardants It does not limit as a flame retardant,
- the well-known flame retardant used for the sealing material of an electronic device can be used.
- Specific examples of the flame retardant include aluminum hydroxide, magnesium hydroxide, zinc borate, zinc molybdate, and phosphazene.
- 1 type (s) or 2 or more types can be mix
- Ion scavenger It does not limit as an ion trapping agent, The well-known ion trapping agent used for the sealing material of an electronic device can be used. Specific examples of the ion scavenger include hydrotalcite, zeolite, and bismuth hydroxide.
- Low stress agent It does not limit as a low stress agent,
- the well-known low stress agent used for the sealing material of an electronic device can be used.
- Specific examples of the low stress agent include silicone compounds such as silicone oil and silicone rubber; polybutadiene compounds; acrylonitrile butadiene copolymer.
- 1 type (s) or 2 or more types can be mix
- the method for producing a resin composition according to the present embodiment includes, for example, a mixing step in which the above-described raw material components are mixed to produce a mixture, and then a molding step in which the mixture is molded.
- the mixing process is a process for preparing a mixture by mixing raw material components.
- the method of mixing is not limited, and a known method can be used depending on the components used.
- the mixing step the raw material components contained in the above-described resin composition are uniformly mixed using a mixer or the like.
- the mixture is melt-kneaded with a kneader such as a roll, a kneader or an extruder to prepare a mixture.
- a forming step (S2) for forming the mixture is performed. It does not limit as a method to shape
- mold A well-known method can be used according to the shape of a resin composition.
- the shape of the resin composition is not limited, and examples thereof include granule shape, powder shape, tablet shape, and sheet shape.
- the shape of the resin composition can be selected depending on the molding method.
- Examples of the molding step for producing the resin composition in the form of granules include a step of pulverizing the cooled mixture after melt-kneading.
- a granule-shaped resin composition may be sieved to adjust the size of the granules.
- the resin composition in the form of granules may be processed by a method such as a centrifugal milling method or a hot cut method to prepare the degree of dispersion or fluidity.
- molding process which produces the resin composition made into the powder form the process of grind
- molding process which produces the resin composition made into the tablet shape after pulverizing a mixture and making it into a granule-shaped resin composition, the process of tablet-molding this granule-shaped resin composition is mentioned, for example.
- molding process which produces the resin composition made into the sheet shape the process of extruding or calendering the mixture after melt-kneading is mentioned, for example.
- the flux according to the present embodiment includes rosin, an activator, and a solvent.
- the flux according to this embodiment is preferably a low-residue type flux that has a small absolute amount of flux residue generated by solder reflow, for example. Thereby, the absolute amount of a flux residue can be reduced and it can disperse
- a low-residue type flux the flux is evaluated by thermogravimetry, before the temperature rise when the temperature is raised from 25 ° C. to 250 ° C. at a temperature rise rate of 10 ° C./min in a nitrogen atmosphere.
- the percentage (mass change rate) of the mass of the flux after heating is 21% by mass or less, for example, 15% by mass or less, preferably 10% by mass or less. Is more preferable, and 5 mass% or less is still more preferable. Thereby, the absolute amount of a flux residue can be reduced. Thereby, a flux residue can be disperse
- a lower limit of the said mass change rate it may be over 0 mass%, for example, may be 5 mass% or more, and may be 10 mass% or more.
- rosin pine resin
- raw material rosins such as gum rosin, wood rosin and tall oil rosin
- rosin derivatives derived from the above raw rosins.
- Specific examples of the rosin derivative include ⁇ -, ⁇ -unsaturated carboxylic acid-modified rosin such as acrylic acid-modified rosin, phenol-modified rosin, maleic acid-modified rosin, and fumaric acid-modified rosin; hydrogenated rosin; polymerized rosin; Rosin; and the above-mentioned ⁇ , ⁇ -unsaturated carboxylic acid-modified rosin, hydrogenated rosin, polymerized rosin, and purified rosin purified from disproportionated rosin.
- the rosin one or more of the above specific examples can be used in combination.
- ⁇ , ⁇ -unsaturated carboxylic acid-modified rosin is
- the upper limit of the content of rosin in the flux according to the present embodiment is 18 parts by mass or less, for example, 15 parts by mass or less, preferably 10 parts by mass or less with respect to 100 parts by mass of the flux. More preferably. Thereby, a flux residue can be reduced. Therefore, compatibility can be improved.
- the lower limit of the content of rosin in the flux according to the present embodiment is 1 part by mass or more with respect to 100 parts by mass of the flux, for example, preferably 2 parts by mass or more, and 3 parts by mass or more. More preferably. Thereby, soldering can be performed suitably.
- activator Specifically, amines, organic acids, and the like can be used as the activator. As the activator, one or a combination of two or more of the above specific examples can be used. Details will be described below.
- amines used as activators include aliphatic amines such as cyclohexylamine; aromatic amines such as aniline; heterocyclic amines such as imidazoles, benzotriazoles, and pyridines; Aromatic amine, heterocyclic amine hydrochloride, hydrobromide, tetrafluoroborate and the like can be mentioned.
- amine one or more of the above specific examples can be used in combination.
- imidazole or benzotriazole is preferably used among the above specific examples.
- imidazole examples include 2-methylimidazole, 2-undecylimidazole, 2-heptadecylimidazole, 1,2-dimethylimidazole, 2-ethyl-4-methylimidazole, 2-phenylimidazole, 2- Phenyl-4-methylimidazole, 1-benzyl-2-methylimidazole, 1-benzyl-2-phenylimidazole, 1-cyanoethyl-2-methylimidazole, 1-cyanoethyl-2-undecylimidazole, 1-cyanoethyl-2- Ethyl-4-methylimidazole, 1-cyanoethyl-2-phenylimidazole, 1-cyanoethyl-2-undecylimidazolium trimellitate, 1-cyanoethyl-2-phenylimidazolium trimellitate, 2,4-diamino-6 -[2 ' Methylimidazolyl- (1 ′
- benzotriazole examples include 2- (2′-hydroxy-5′-methylphenyl) benzotriazole, 2- (2′-hydroxy-3′-tert-butyl-5′-methylphenyl)- 5-chlorobenzotriazole, 2- (2′-hydroxy-3 ′, 5′-di-tert-amylphenyl) benzotriazole, 2- (2′-hydroxy-5′-tert-octylphenyl) benzotriazole, 2 , 2'-methylenebis [6- (2H-benzotriazol-2-yl) -4-tert-octylphenol], 6- (2-benzotriazolyl) -4-tert-octyl-6'-tert-butyl- 4'-methyl-2,2'-methylenebisphenol, 1,2,3-benzotriazole, 1- [N, N-bis (2- Tilhexyl) aminomethyl] benzotriazole, carboxybenzotriazole, 1- [N, N-bis (2-ethy
- organic acid used as the activator examples include adipic acid, azelaic acid, eicosane diacid, citric acid, glycolic acid, succinic acid, salicylic acid, diglycolic acid, dipicolinic acid, dibutylaniline diglycolic acid, and suberin.
- Acid sebacic acid, thioglycolic acid, terephthalic acid, dodecanedioic acid, parahydroxyphenylacetic acid, picolinic acid, phenylsuccinic acid, phthalic acid, fumaric acid, maleic acid, malonic acid, lauric acid, benzoic acid, p-tert- Butylbenzoic acid, tartaric acid, isocyanuric acid tris (2-carboxyethyl), glycine, 1,3-cyclohexanedicarboxylic acid, 2,2-bis (hydroxymethyl) propionic acid, 2,2-bis (hydroxymethyl) butanoic acid, 2,3-dihydroxybenzoic acid, 2,4-diethylglutar 2-quinolinecarboxylic acid, 3-hydroxybenzoic acid, malic acid, p-anisic acid, stearic acid, 12-hydroxystearic acid, oleic acid, linoleic acid, linolenic acid, dimer acid, hydrogen
- solvent used for the flux examples include water, alcohol solvents, glycol ether solvents, and terpineols.
- alcohol solvents include isopropyl alcohol, 1,2-butanediol, isobornylcyclohexanol, 2,4-diethyl-1,5-pentanediol, 2,2-dimethyl-1,3-propanediol, 2,5 -Dimethyl-2,5-hexanediol, 2,5-dimethyl-3-hexyne-2,5-diol, 2,3-dimethyl-2,3-butanediol, 1,1,1-tris (hydroxymethyl) Ethane, 2-ethyl-2-hydroxymethyl-1,3-propanediol, 2,2′-oxybis (methylene) bis (2-ethyl-1,3-propanediol), 2,2-bis (hydroxymethyl) 1,3-propanediol, 1,2,6-trihydroxyhex
- glycol ether solvents include diethylene glycol mono-2-ethylhexyl ether, ethylene glycol monophenyl ether, 2-methylpentane-2,4-diol, diethylene glycol monohexyl ether, diethylene glycol dibutyl ether, and triethylene glycol monobutyl ether.
- FIG. 2 is a diagram illustrating an example of the electronic apparatus according to the present embodiment.
- the electronic device 100 according to the present embodiment includes, for example, a base material 10 and an electronic component 20, and includes a sealing material 50 that seals the electronic component 20.
- the sealing material 50 consists of the hardened
- the electronic component 20 and the base material 10 are electrically connected via the solder bumps 30, but the electrical connection method is not limited to this. Absent.
- the substrate 10 according to the present embodiment is not limited as long as it has a metal exposed portion on the surface.
- the metal exposed portion includes an electric circuit such as a copper circuit; metal plating such as silver and gold.
- the base material 10 may be, for example, an organic substrate made of an epoxy resin, a cyanate resin, a maleimide resin, or a ceramic substrate.
- the electronic component 20 according to this embodiment is not limited as long as the solder bump 30 is provided, but a semiconductor element is preferable, for example.
- the semiconductor element include, but are not limited to, an integrated circuit, a large-scale integrated circuit, a transistor, a thyristor, a diode, and a solid-state imaging element.
- the electronic device is not limited, but a semiconductor device obtained by molding a semiconductor element is preferable.
- the types of semiconductor devices include MAP (Mold Array Package), QFP (Quad Flat Package), SOP (Small Outline Package), CSP (Chip Size Package), QFN (Quad Flat Package), and QFN (Quad Flat Package).
- MAP Mold Array Package
- QFP Quant Flat Package
- SOP Small Outline Package
- CSP Chip Size Package
- QFN Quad Flat Package
- QFN Quad Flat Package
- QFN Quadraturethane
- SON Small Outline Non-leaded Package
- BGA Ball Grid Array
- LF-BGA Lead Frame BGA
- FCBGA Felip Chip BGAe
- MAPBGA Molded Array Process BGA
- MAPBGA Molded Array Process BGA
- Examples include Fan-In type eWLB and Fan-Out type eWLB. It is.
- the manufacturing method of the electronic device according to the present embodiment includes, for example, bringing the metal exposed portion of the base material into contact with the flux and flux-treating the metal exposed portion, and reflowing the electronic component and the base material. Then, a solder reflow process for electrically connecting the electronic component and the metal exposed part of the base material via the solder bump, and an introduction process for introducing the resin composition so as to be in contact with the surface of the metal exposed part subjected to the flux treatment And including.
- the step of cleaning the flux is not performed.
- the metal exposed portion of the base material is brought into contact with the flux, and the metal exposed portion is flux-treated.
- the flux processing step first, an electronic component 20 having solder bumps 30 is prepared as shown in FIG. Next, as shown in FIG. 3B, a flux 200 is applied to the solder bumps 30 provided on the electronic component 20. Specifically, the surface of the prepared electronic component 20 on which the solder bump 30 is provided is brought into contact with a stand on which the flux 200 is applied, whereby the solder bump 30 provided on the electronic component 20 is fluxed. 200 is deposited. Next, as shown in FIG. 3C, the electronic component 20 is disposed directly on the base material 10. Thereby, the metal exposure part with which the base material 10 is provided, and the flux 200 are made to contact, and the flux process which makes the flux 200 adhere to a metal exposure part is performed.
- solder reflow process In the solder reflow process, the electronic component and the base material are reflowed to electrically connect the electronic component and the metal exposed portion of the base material via the solder bump. Specifically, by reflowing the structure composed of the electronic component and the base material shown in FIG. 3C, the electronic component and the metal exposed portion of the base material are electrically connected through the solder bumps. 3D is obtained.
- the flux is applied to the exposed metal portion of the base material 10, the electronic component 20 mounted on the base material 10, and the solder bump 30 provided in the electronic component 20. Residue 300 is attached.
- the resin composition is introduced so as to be in contact with the surface of the exposed metal portion subjected to the flux treatment.
- the sealing material 50 is formed by introducing and curing the resin composition.
- the method for introducing the resin composition is not limited, and specifically, methods such as a transfer molding method, a compression molding method, and an injection molding method can be used.
- Epoxy resin (Epoxy resin) ⁇
- Epoxy resin 1 Mixture of triphenylmethane type epoxy resin and biphenyl type epoxy resin (Made by Mitsubishi Chemical, EPIKOTE YL6677) -Epoxy resin 2: phenol aralkyl type epoxy resin containing biphenylene skeleton (Nippon Kayaku Co., Ltd., NC-3000)
- Epoxy resin 3 phenol aralkyl type epoxy resin containing biphenylene skeleton (Nippon Kayaku Co., Ltd., NC-3000-L)
- Epoxy resin 4 triphenylmethane type epoxy resin (manufactured by Mitsubishi Chemical Corporation, 1032H60)
- Epoxy resin 5 bisphenol A type epoxy resin (Mitsubishi Chemical Corporation YL6810) -Epoxy resin 6: biphenyl type epoxy resin (Mitsubishi Chemical Corporation, YX4000K)
- Epoxy resin 7 Mixture of biphenylene skeleton-containing phenol aralkyl type
- Phenolic resin curing agent 1 Triphenylmethane type phenolic resin (Maywa Kasei Co., Ltd., MEH-7500)
- Phenolic resin curing agent 2 phenol aralkyl resin containing biphenylene skeleton (Maywa Kasei Co., Ltd., MEH-7851SS)
- Phenolic resin curing agent 3 Biphenylene skeleton-containing phenol aralkyl resin (MEH-7851M, manufactured by Meiwa Kasei Co., Ltd.)
- Phenolic resin curing agent 4 Biphenylene skeleton-containing phenol aralkyl resin (MEH-7851H, manufactured by Meiwa Kasei Co., Ltd.)
- Phenolic resin curing agent 5 Biphenylene skeleton-containing phenol aralkyl resin (manufactured by Nippon Kayaku Co., Ltd., GPH-
- solubility parameters were calculated based on the Hansen method. Table 1 shows the calculated SP values.
- the Hansen method divides evaporation energy into dispersion energy dD (Dispersion Energy), polarization energy dP (Polar Energy), and hydrogen bond energy dH (Hydrogen Bonding Energy), and dD, dP and dH are three-dimensional vectors. This is a method of calculating the length of the vector as an SP value.
- Curing accelerator 1 Triphenylphosphine (manufactured by Hokuko Chemical Co., Ltd., TPP)
- Filler 1 spherical fused silica (manufactured by Denki Kagaku Kogyo Co., Ltd., FB-950FC, D 50 : 24 ⁇ m, coarse particle content exceeding 75 ⁇ m in particle size: 0.5% by weight or less)
- Colorant 1 Carbon black (Mitsubishi Chemical Corporation MA-600)
- Coupling agent 1 N-phenyl ⁇ -aminopropyltrimethoxysilane (manufactured by Shin-Etsu Chemical, KBM-573) Release agent 1: Carnauba wax (Nikko Fine Co., Nikko Carnauba)
- the average solubility parameter SP1 and the number average molecular weight Mn1 of the resin group consisting of each epoxy resin and phenol resin curing agent are shown in Table 2 below.
- the average solubility parameter SP1 was calculated by the following formula 1.
- Average solubility parameter SP1 ⁇ (A (n) ⁇ Ca (n) ) + ⁇ (B (m) ⁇ Cb (m) ) (Formula 1)
- a (n) represents a solubility parameter calculated based on the Hansen method for each of the n types of epoxy resins contained in the resin composition.
- Ca (n) represents the resin composition.
- B (m) is the m types of phenol resin curing agents contained in the resin composition.
- the number average molecular weight Mn1 was calculated by the following formula 3.
- Number average molecular weight Mn1 ⁇ (a (n) ⁇ Ca (n) ) + ⁇ (b (m) ⁇ Cb (m) ) (Formula 3)
- a (n) indicates the value of the number average molecular weight for each of the n types of epoxy resins contained in the resin composition.
- Ca (n) is the total epoxy resin in the resin composition.
- b (m) is the number average molecular weight for each of the m types of phenol resin curing agents contained in the resin composition.
- Cb (m) indicates the content of each of the m types of phenol resin curing agents relative to the total content of all epoxy resins and all phenol resin curing agents in the resin composition.
- Rosin 1 Acrylic acid-modified hydrogenated rosin Organic acid 1: Glutaric acid Amine 1: 2-Undecylimidazole Solvent: Isobornylcyclohexanol (87.5 wt%) and 1,3-butylene glycol (12. 5 wt%) mixed solvent
- Fluxes 1 to 5 were prepared by mixing the raw material components at the mixing ratios shown in Table 3 below.
- Mass change rate of flux With respect to the obtained fluxes 1 to 5, the mass change rate before and after the heat treatment was measured based on the following procedure. First, each of the fluxes 1 to 5 was heat-treated in a nitrogen atmosphere at a heating rate of 10 ° C./min and under heating conditions in which the temperature was raised from 25 ° C. to 250 ° C. At this time, the mass M1 of the flux before the heat treatment and the mass M2 of the flux after the heat treatment were measured using a thermogravimetry apparatus. Using the obtained M1 and M2, the mass change rate (mass%) of the flux before and after heat treatment was calculated based on the formula: (M2 / M1) ⁇ 100. The mass change rate of the flux before and after the heat treatment is expressed as a percentage of the mass of the flux after the temperature rise with respect to the mass of the flux before the temperature rise. The measurement results are shown in Table 3 below.
- an electronic device was produced according to the following procedure. First, a printed wiring board provided with a copper circuit on one surface having a length of 15 mm and a width of 15 mm was prepared. Next, flux was applied to one surface of the printed wiring board. Next, a flip chip type package having a solder bump and having a length of 10 mm, a width of 10 mm, and a thickness of 250 ⁇ m was prepared. Next, the surface having the solder bumps of the flip chip type package is placed oppositely on one surface of the printed wiring board, and the solder bumps are melted by performing reflow treatment in a nitrogen atmosphere at a peak temperature of 240 ° C. and a peak temperature time of 10 seconds.
- the flip chip type package and the copper circuit of the printed circuit board were soldered.
- the reflow process was performed twice.
- the printed wiring board on which the flip chip type package is mounted is placed in the mold, and the resin composition is placed in the mold at a mold temperature of 175 ° C. and an injection pressure of 9.8 MPa using a transfer molding machine. And molded.
- the resin composition was introduced so as to contact the surface of the copper circuit and the surface of the solder bump and to cover the periphery of the flip chip package.
- a heat treatment at 175 ° C. for 120 seconds was performed at the time of molding, and the resin composition was cured to form a sealing material.
- an electronic device was manufactured.
- the resin compositions 1 to 14 described above as the resin composition and the fluxes 1 to 5 as the flux were used in combinations shown in Table 4.
- the conditions of Examples 1 to 24 and Comparative Examples 1 to 46 were set according to the combinations of the resin compositions 1 to 14 and the fluxes 1 to 5 shown in Table 4.
- electronic devices were produced in the same manner as described above.
- Examples 1 to 24 were all “good” and one of Comparative Examples 1 to 46 was “x”. Thereby, it was confirmed that the electronic device of each Example was excellent in the compatibility of a flux and a resin composition compared with the electronic device of each comparative example. In addition, Examples 1 to 24 were superior in adhesion between the cured product of the resin composition and the printed wiring substrate as compared with Comparative Examples 1 to 46. From the above, it is possible to improve the productivity and the manufacturing stability of the electronic device by the method for manufacturing the electronic device of Examples 1 to 24.
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Abstract
Description
しかしながら、フラックス残渣を洗浄する工程を行わない場合、電子装置の樹脂組成物の硬化物と、基材との間にフラックス残渣が残存することになる。フラックス残渣が残存することで、樹脂組成物によって銅回路を備える基材を封止する場合、樹脂組成物の硬化物と、基材との密着性が低下し、その結果、電子装置の電気的信頼性が低下することがあった。
よって、フラックス残渣を溶剤で洗浄する工程を行っても、行わなくても、電子装置の生産性及び製造安定性のいずれかの点で改善の余地を有していた。
詳細なメカニズムは定かではないが、上記のフラックスと樹脂組成物とを使用することで、こられの相溶性が向上すため、フラックス残渣が樹脂組成物中に取り込まれて、フラックス残渣が除去される、と考えられる。
本発明者らは、このような知見に基づいて、上記のフラックスと樹脂組成物とを併用することによって、フラックス残渣を取り除くことができるため、樹脂組成物の硬化物と基材との密着性の低下を抑制でき、電子装置の製造安定性を高められることを見出し、本発明を完成した。
表面に金属露出部を有する基材と、前記基材上に設けられた電子部品とを備える電子装置の製造方法であって、
前記金属露出部と、フラックスとを接触させて、前記金属露出部をフラックス処理するフラックス処理工程と、
前記フラックス処理した前記金属露出部の表面に接するように樹脂組成物を導入する導入工程と、
を含み、
前記フラックスは、ロジンと、活性剤と、溶剤と、を含み、
前記ロジンの含有量が、前記フラックス100質量部に対して、1質量部以上18質量部以下であり、
前記フラックスにおいて、下記の手順で測定される、加熱処理前後の前記フラックスの質量変化率が21質量%以下であり、
(手順)
窒素雰囲気下、昇温速度10℃/minで、温度25℃から250℃に昇温する加熱条件で、前記フラックスを加熱処理したとき、熱重量測定装置を用いて、加熱処理前の前記フラックスの質量M1と、加熱処理後の前記フラックスの質量M2とを測定する。そして、加熱処理前後の前記フラックスの質量変化率を、得られたM1、M2を用いて、式:(M2/M1)×100に基づいて算出する。
前記樹脂組成物は、エポキシ樹脂と、フェノール樹脂硬化剤と、を含み、
前記樹脂組成物において、前記エポキシ樹脂および前記フェノール樹脂硬化剤からなる樹脂群のHansen法に基づく平均溶解度パラメーターをSP1とし、前記エポキシ樹脂および前記フェノール樹脂硬化剤からなる樹脂群の数平均分子量をMn1としたとき、SP1とMn1とが、Mn1≦210×SP1-4095を満たすものである、
電子装置の製造方法が提供される。
(手順)
窒素雰囲気下、昇温速度10℃/minで、温度25℃から250℃に昇温する加熱条件で、フラックスを加熱処理したとき、熱重量測定装置を用いて、加熱処理前のフラックスの質量M1と、加熱処理後のフラックスの質量M2とを測定する。そして、加熱処理前後のフラックスの質量変化率を、得られたM1、M2を用いて、式:(M2/M1)×100に基づいて算出する。
フラックスは、ロジンと、活性剤と、溶剤と、を含む樹脂系フラックスである。
電子装置の電気回路などの金属部材にフラックスを塗工する場合、フラックス中のロジン及び活性剤が、金属部材の表面に形成される酸化膜と反応し、酸化膜を除去する。これにより、酸化膜が除去された金属部材は、酸化膜が存在する金属部材と比べて、はんだとの密着性を向上することができる。
ここで、金属部材の表面には、酸化膜と反応しなかったロジン及び活性剤が残存する。そして、残存するロジン及び活性剤が、フラックス残渣を形成する。
以上より、化学的親和性の低い従来の樹脂組成物は、多孔質形状の熱変性ロジン内部に侵入できない。したがって、フラックス残渣が従来の樹脂組成物と相溶しないと推測される。
ところで、近年使用される鉛フリーのはんだには、スズ(Sn)などの金属が含有される。詳細なメカニズムは定かではないが、分解された活性剤は、はんだ中に含まれるSnなどの金属、または、金属部材に由来するAg、Fe、Niなどの金属と反応し、該金属の結晶を形成すると推測される。これにより、フラックス中の摩擦が増加し、フラックスの粘度が上昇する。このようにフラックスの粘度が上昇してしまうと、フラックスの分子鎖と、樹脂組成物の分子鎖とが絡み合わなくなり、物理的親和性が低くなる。
以上より、物理的親和性の低い従来の樹脂組成物はフラックスの分子鎖と絡み合わない。したがって、フラックス残渣が従来の樹脂組成物と相溶しないと推測される。
以上より、本実施形態に係る電子装置は、基材上のフラックス残渣を洗浄する工程を行わないことを前提に、樹脂組成物の硬化物と、基材と間にフラックス残渣が存在しない電子装置の製造方法を提供できるものである。これにより、樹脂組成物の硬化物と、基材との密着性を向上し、電子装置の電気的信頼性といった性能を向上できる。よって、生産性および製造安定性に優れた電子装置の製造方法を実現できる。
本実施形態に係る樹脂組成物は、エポキシ樹脂とフェノール樹脂硬化剤とを含む熱硬化性樹脂組成物である。
本実施形態に係る樹脂組成物は、エポキシ樹脂およびフェノール樹脂硬化剤からなる樹脂群のHansen法に基づく平均溶解度パラメーターSP1と、エポキシ樹脂およびフェノール樹脂硬化剤からなる樹脂群の数平均分子量Mn1との間に、Mn1≦210×SP1-4095の関係が成り立つものである。これにより、フラックスと相溶性を示し、フラックス残渣を取り除くことができるものである。
Hansen法とは、蒸発エネルギーを分散エネルギーdD(Dispersion Energy)と、分極エネルギーdP(Polar Energy)と、水素結合エネルギーdH(Hydrogen Bonding Energy)とに分け、dD、dP及びdHを三次元ベクトルとしたときのベクトルの長さを溶解度パラメーターとして算出する方法である。
平均溶解度パラメーターSP1=Σ(A(n)×Ca(n))+Σ(B(m)×Cb(m)) (式1)
(上記式1において、A(n)は、本樹脂組成物中に含まれているn種のエポキシ樹脂それぞれに関するHansen法に基づいて算出された溶解度パラメーターを指す。Ca(n)は、本樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するn種のエポキシ樹脂それぞれの含有量を指す。B(m)は、本樹脂組成物中に含まれているm種のフェノール樹脂硬化剤それぞれに関するHansen法に基づいて算出された溶解度パラメーターを指す。Cb(m)は、本樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するm種のフェノール樹脂硬化剤それぞれの含有量を指す。なお、上記n、mは、1以上の整数である。)
平均溶解度パラメーターSP1=A1×Ca1+A2×Ca2+B1×Cb1+B2×Cb2 (式2)
(上記式2において、A1は、第1のエポキシ樹脂に関するHansen法に基づいて算出された溶解度パラメーターの値を示す。A2は、第2のエポキシ樹脂に関するHansen法に基づいて算出された溶解度パラメーターの値を示す。B1は、第1の硬化剤に関するHansen法に基づいて算出された溶解度パラメーターの値を示す。B2は、第2の硬化剤に関するHansen法に基づいて算出された溶解度パラメーターの値を示す。Ca1は、樹脂群全量に対する第1のエポキシ樹脂の含有量を示す。Ca2は、樹脂群全量に対する第2のエポキシ樹脂の含有量を示す。Cb1は、樹脂群全量に対する第1の硬化剤の含有量を示す。Cb2は、樹脂群全量に対する第2の硬化剤の含有量を示す。)
また、樹脂群の平均溶解度パラメーターSP1の下限値としては、例えば、20.8[cal/cm3]0.5以上であることが好ましく、21.0[cal/cm3]0.5以上であることがより好ましい。これにより、フラックス残渣中に含まれているロジン、活性種と、エポキシ樹脂やフェノール樹脂硬化剤の分子構造中に含まれている官能基との間に生じる水素結合、双極子相互作用などの相互作用が促進され、フラックス残渣に対する樹脂組成物の相溶性を向上させることができる。具体的には、SP1の値が上記下限値以上となることで、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖同士の相互作用が大きくなり、フラックス残渣の分子の相互作用と同程度となるために、両者の相互作用が強くなり、相溶性が向上すると考えられる。
以上より、上述した平均溶解度パラメーターSP1の値が上記数値範囲内となるように制御した場合には、樹脂組成物及びフラックス残渣の相溶性を向上させることができる。
樹脂群の数平均分子量Mn1は、具体的には、以下の式3により算出することができる。
数平均分子量Mn1=Σ(a(n)×Ca(n))+Σ(b(m)×Cb(m)) (式3)
(上記式3において、a(n)は、本樹脂組成物中に含まれているn種のエポキシ樹脂それぞれに関する数平均分子量の値を指す。Ca(n)は、本樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するn種のエポキシ樹脂それぞれの含有量を指す。b(m)は、本樹脂組成物中に含まれているm種のフェノール樹脂硬化剤それぞれに関する数平均分子量の値を指す。Cb(m)は、本樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するm種のフェノール樹脂硬化剤それぞれの含有量を指す。なお、上記n,mは、1以上の整数である。)
数平均分子量Mn1=a1×Ca1+a2×Ca2+b1×Cb1+b2×Cb2 (式4)
(上記式4において、a1は、第1のエポキシ樹脂の数平均分子量を示す。a2は、第2のエポキシ樹脂の数平均分子量を示す。b1は、第1のフェノール樹脂硬化剤の数平均分子量を指す。b2は、第2のフェノール樹脂硬化剤の数平均分子量を示す。Ca1は、樹脂群全量に対する第1のエポキシ樹脂の含有量を示す。Ca2は、樹脂群全量に対する第2のエポキシ樹脂の含有量を示す。Cb1は、樹脂群全量に対する第1のフェノール樹脂硬化剤の含有量を示す。Cb2は、樹脂群全量に対する第2のフェノール樹脂硬化剤の含有量を示す。)
樹脂群の数平均分子量Mn1の上限値は、例えば、550以下であることが好ましく、520以下であることがより好ましい。これにより、フラックス残渣中に含まれているロジン、活性種と、エポキシ樹脂やフェノール樹脂硬化剤の分子構造を構成する主鎖との間に生じる相互作用が促進され、フラックス残渣に対する樹脂組成物の相溶性を向上させることができる。
特定の数値範囲としては、具体的には、Mn1≦210×SP1-4095の関係を満たすように、数平均分子量Mn1が小さく、平均溶解度パラメーターSP1が大きくなることが好ましい。これは、図1にも示すように、SP1に対してMn1をプロットした時に、Mn1=210×SP1-4095の直線上、あるいは、それよりもMn1が小さくなる、または、SP1が大きくなることを示す。なお、Mn1≦210×SP1-4095の関係式において、Mn1の単位は無次元であり、SP1の単位は[cal/cm3]0.5である。
まず、Mn1の値が小さくなることで、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖の絡み合いが適切に制御されると推測される。これにより、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖と、フラックス残渣中に含まれているロジン、活性種の分子鎖との物理的親和性が向上し、相溶性が向上する。
また、SP1の値が大きくなることで、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖と、フラックス残渣との分子鎖との化学的親和性を向上できると推測される。従来の電子装置の封止に用いられる樹脂組成物では、フラックス残渣の分子鎖同士の相互作用が、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖と、フラックス残渣の分子鎖との相互作用より遥かに大きかった。しかしながら、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖と、フラックス残渣の分子鎖とが化学的親和性を強めることによって、エポキシ樹脂及びフェノール樹脂硬化剤の分子鎖が、フラックス残渣中に含まれている分子鎖を取り込みやすくなる。
以上より、Mn1及びSP1が、共に適切な数値範囲となることで、樹脂組成物と、フラックス残渣とを相溶させることができると推測される。
本実施形態に係る樹脂組成物は、エポキシ樹脂と、フェノール樹脂硬化剤とを含む。
本実施形態に係るエポキシ樹脂としては、1分子内にエポキシ基を2個以上有するモノマー、オリゴマー、ポリマー全般を用いることができ、その分子量や分子構造は特に限定されない。
エポキシ樹脂としては、具体的には、ビフェニル型エポキシ樹脂;ビスフェノールA型エポキシ樹脂、ビスフェノールF型エポキシ樹脂、テトラメチルビスフェノールF型エポキシ樹脂等のビスフェノール型エポキシ樹脂;スチルベン型エポキシ樹脂;フェノールノボラック型エポキシ樹脂、クレゾールノボラック型エポキシ樹脂等のノボラック型エポキシ樹脂;トリフェニルメタン型エポキシ樹脂、トリフェノールメタン型エポキシ樹脂、アルキル変性トリフェノールメタン型エポキシ樹脂等に例示されるトリフェニル型エポキシ樹脂等の多官能エポキシ樹脂;フェニレン骨格を有するフェノールアラルキル型エポキシ樹脂、フェニレン骨格を有するナフトールアラルキル型エポキシ樹脂、ビフェニレン骨格含有フェノールアラルキル型エポキシ樹脂(ビフェニルアラルキル型エポキシ樹脂)、ビフェニレン骨格含有ナフトールアラルキル型エポキシ樹脂等のフェノールアラルキル型エポキシ樹脂;ジヒドロキシナフタレン型エポキシ樹脂、ジヒドロキシナフタレンの2量体をグリシジルエーテル化して得られるエポキシ樹脂等のナフトール型エポキシ樹脂;トリグリシジルイソシアヌレート、モノアリルジグリシジルイソシアヌレート等のトリアジン核含有エポキシ樹脂;ジシクロペンタジエン変性フェノール型エポキシ樹脂等の有橋環状炭化水素化合物変性フェノール型エポキシ樹脂などが挙げられる。エポキシ樹脂としては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。エポキシ樹脂としては、上記具体例のうち例えば、ビフェニル型エポキシ樹脂、多官能エポキシ樹脂、フェノールアラルキル型エポキシ樹脂、ビスフェノール型エポキシ樹脂からなる群より選択される1種または2種以上を用いることが好ましい。これにより、平均溶解度パラメーターSP1を大きくすることができ、樹脂組成物及びフラックスの相溶性を向上できる。
また、樹脂組成物中のエポキシ樹脂の含有量の上限値は、樹脂組成物の全固形分100質量部に対して、例えば、20質量部以下であることが好ましく、15質量部以下であることがより好ましく、12質量部以下であることが更に好ましい。
エポキシ樹脂の含有量が上記数値範囲内であることにより、上述した数平均分子量Mn1を満たしつつ、平均溶解度パラメーターSP1を所望の数値範囲内とすることができる。
なお、本実施形態において、樹脂組成物の全固形分とは、樹脂組成物に含まれる溶剤を除く成分全体を示す。
本実施形態に係るフェノール樹脂硬化剤は、一分子内にフェノール性水酸基を2個以上有するモノマー、オリゴマー、ポリマー全般であり、その分子量、分子構造については特に限定されるものではない。
フェノール樹脂硬化剤としては、具体的には、フェノールノボラック樹脂、クレゾールノボラック樹脂、トリスフェノールメタン型フェノールノボラック樹脂、ナフトールノボラック樹脂等のノボラック型フェノール樹脂;トリフェノールメタン型フェノール樹脂等の多官能型フェノール樹脂;テルペン変性フェノール樹脂、ホルムアルデヒドで変性したトリフェニルメタン型フェノール樹脂、ホルムアルデヒドで変性したトリヒドロキシフェニルメタン型フェノール樹脂、ジシクロペンタジエン変性フェノール樹脂等の変性フェノール樹脂;フェニレン骨格及び/又はビフェニレン骨格を有するフェノールアラルキル樹脂、フェニレン及び/又はビフェニレン骨格を有するナフトールアラルキル樹脂、フェニルアラルキル型フェノール樹脂、ビフェニルアラルキル型フェノール樹脂等のアラルキル型フェノール樹脂;ビスフェノールA、ビスフェノールF等のビスフェノール化合物などが挙げられる。フェノール樹脂硬化剤としては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。フェノール樹脂硬化剤としては、上記具体例のうち例えば、ノボラック型フェノール樹脂、多官能型フェノール樹脂、アラルキル型フェノール樹脂からなる群より選択される1種または2種以上を用いることが好ましい。これにより、平均溶解度パラメーターSP1を大きくすることができ、樹脂組成物及びフラックスの相溶性を向上できる。
また、樹脂組成物中のフェノール樹脂硬化剤の含有量の上限値は、樹脂組成物の全固形分100質量部に対して、例えば、20質量部以下であることが好ましく、15質量部以下であることがより好ましく、12質量部以下であることが更に好ましく、10質量部以下であることが一層好ましい。
フェノール樹脂硬化剤の含有量が上記数値範囲内であることで、上述した数平均分子量Mn1を満たしつつ、平均溶解度パラメーターSP1を所望の数値範囲内とすることができる。
本実施形態に係る樹脂組成物は、必要に応じて、硬化促進剤、充填材、カップリング剤、離型剤、着色剤、難燃剤、イオン捕捉剤、低応力剤等の各種添加剤のうち1種または2種以上を適宜配合することができる。
以下に、代表成分について説明する。
硬化促進剤は、エポキシ樹脂及び硬化剤の硬化反応を促進させるものであれば限定されず、エポキシ樹脂及び硬化剤の種類に応じて選択できる。
硬化促進剤としては、具体的には、オニウム塩化合物、トリフェニルホスフィンなどの有機ホスフィン、テトラ置換ホスホニウム化合物、ホスホベタイン化合物、ホスフィン化合物とキノン化合物との付加物、ホスホニウム化合物とシラン化合物との付加物等のリン原子含有化合物;2-メチルイミダゾール、2-エチル-4-メチルイミダゾール(EMI24)、2-フェニル-4-メチルイミダゾール(2P4MZ)、2-フェニルイミダゾール(2PZ)、2-フェニル-4-メチル-5-ヒドロキシイミダゾール(2P4MHZ)、1-ベンジル-2-フェニルイミダゾール(1B2PZ)などのイミダゾール化合物;1,8-ジアザビシクロ[5.4.0]ウンデセン-7、ベンジルジメチルアミン等が例示されるアミジンや3級アミン;上記アミジンまたは上記3級アミンの4級アンモニウム塩等の窒素原子含有化合物などが挙げられる。硬化促進剤としては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。
本実施形態に係る樹脂組成物は、例えば、充填材を更に含んでもよい。充填材としては限定されず、電子装置の構造、電子装置に要求される機械的強度、熱的特性に応じて適切な充填材を選択できる。
充填材としては、具体的には、溶融破砕シリカ、溶融球状シリカ、結晶性シリカ、2次凝集シリカ、球状微粉シリカなどのシリカ;アルミナ、窒化ケイ素、窒化アルミニウム、窒化ホウ素、酸化チタン、炭化ケイ素、水酸化アルミニウム、水酸化マグネシウム、チタンホワイトなどの金属化合物;タルク;クレー;マイカ;ガラス繊維などが挙げられる。充填材としては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。充填材としては、上記具体例のうち、例えば、シリカを用いることが好ましい。これにより、充填材と、密着助剤とが相互作用し、さらに密着性を向上できる。
また、充填材の体積基準の累積50%粒径(D50)の上限値は、例えば、50μm以下であることが好ましく、30μm以下であることがより好ましく、25μm以下であることが更に好ましい。これにより、粗大な充填材が、樹脂組成物と、フラックスとの接触を妨げることを抑制できる。したがって、樹脂組成物と、フラックスとの相溶性を向上できる。
なお、本実施形態において、充填材の体積基準の累積50%粒径(D50)は、例えば、市販のレーザー回折式粒度分布測定装置(例えば、島津製作所社製、SALD-7000)を用いて粒子の粒度分布を体積基準で測定し、算出することができる。
また、樹脂組成物中の充填材の含有量の上限値は、樹脂組成物の固形分に対して、例えば、95質量部以下であることが好ましく、93質量部以下であることがより好ましく、90質量部以下であることが好ましい。これにより、樹脂組成物の粘度を向上できる。したがって、樹脂組成物が導入される際に、フラックスが、樹脂組成物中により好適に取り込まれる。
カップリング剤としては限定されず、電子装置に用いられる公知のカップリング剤を用いることができる。
カップリング剤としては、具体的には、ビニルトリメトキシシラン、ビニルトリエトキシシランなどのビニルシラン;2-(3,4-エポキシシクロヘキシル)エチルトリメトキシシラン、3-グリシドキシプロピルメチルジメトキシシラン、3-グリシドキシプロピルトリメトキシシラン、3-グリシドキシプロピルメチルジエトキシシラン、3-グリシドキシプロピルトリエトキシシランなどのエポキシシラン;p-スチリルトリメトキシシランなどのスチリルシラン;3-メタクリロキシプロピルメチルジメトキシシラン、3-メタクリロキシプロピルトリメトキシシラン、3-メタクリロキシプロピルメチルジエトキシシラン、3-メタクリロキシプロピルトリエトキシシランなどのメタクリルシラン;3-アクリロキシプロピルトリメトキシシランなどのアクリルシラン;N-2-(アミノエチル)-3-アミノプロピルメチルジメトキシシラン、N-2-(アミノエチル)-3-アミノプロピルトリメトキシシラン、3-アミノプロピルトリメトキシシラン、3-アミノプロピルトリエトキシシラン、3-トリエトキシシリル-N-(1,3-ジメチル-ブチリデン)プロピルアミン、N-フェニルγ-アミノプロピルトリメトキシシラン、フェニルアミノプロピルトリメトキシシランなどのアミノシラン;イソシアヌレートシラン;アルキルシラン;3-ウレイドプロピルトリアルコキシシランなどのウレイドシラン;3-メルカプトプロピルメチルジメトキシシラン、3-メルカプトプロピルトリメトキシシランなどのメルカプトシラン;3-イソシアネートプロピルトリエトキシシランなどのイソシアネートシラン;チタン系化合物;アルミニウムキレート類;アルミニウム/ジルコニウム系化合物などが挙げられる。カップリング剤としては、上記具体例のうち1種または2種以上を配合することができる。カップリング剤としては、上記具体例のうち例えば、アミノシランを用いることが好ましい。また、アミノシランとしては、例えば、N-フェニルγ-アミノプロピルトリメトキシシランを用いることがより好ましい。これにより、樹脂組成物中におけるフラックス残渣の分散性をさらに向上させることができる。したがって、フラックス残渣の残存をより高度に抑制できる。
離型剤としては限定されず、電子装置の封止材に用いられる公知の離型剤を用いることができる。
離型剤としては、具体的には、カルナバワックスなどの天然ワックス、ジエタノールアミン・ジモンタンエステルなどの合成ワックス、ステアリン酸亜鉛などの高級脂肪酸及びその金属塩、パラフィンなどが挙げられる。離型剤としては、上記具体例のうち1種または2種以上を配合することができる。
着色剤としては限定されず、電子装置の封止材に用いられる公知の着色剤を用いることができる。
着色剤としては、具体的には、カーボンブラック、ベンガラ、酸化チタンなどを挙げることができる。着色剤としては、上記具体例のうち1種または2種以上を配合することができる。
難燃剤としては限定されず、電子装置の封止材に用いられる公知の難燃剤を用いることができる。
難燃剤としては、具体的には、水酸化アルミニウム、水酸化マグネシウム、ホウ酸亜鉛、モリブデン酸亜鉛、ホスファゼンなどを挙げることができる。難燃剤としては、上記具体例のうち1種または2種以上を配合することができる。
イオン捕捉剤としては限定されず、電子装置の封止材に用いられる公知のイオン捕捉剤を用いることができる。
イオン捕捉剤としては、具体的には、ハイドロタルサイト、ゼオライト、水酸化ビスマスなどを挙げることができる。
低応力剤としては限定されず、電子装置の封止材に用いられる公知の低応力剤を用いることができる。
低応力剤としては、具体的には、シリコーンオイル、シリコーンゴム等のシリコーン化合物;ポリブタジエン化合物;アクリロニトリルブタジエン共重合などを挙げることができる。低応力剤としては、上記具体例のうち1種または2種以上を配合することができる。
次に、本実施形態に係る樹脂組成物の製造方法について説明する。
本実施形態に係る樹脂組成物の製造方法は、例えば、上述した原料成分を混合して混合物を作製する混合工程と、次いで、混合物を成形する成形工程とを含む。
混合工程は、原料成分を混合し、混合物を作製工程である。混合する方法は限定されず、用いられる成分に応じて、公知の方法を用いることができる。
混合工程としては、具体的には、上述した樹脂組成物が含む原料成分を、ミキサーなどを用いて均一に混合する。次いで、ロール、ニーダーまたは押出機等の混練機で溶融混練し、混合物を作製する。
上述した混合工程に、次いで、混合物を成形する成形工程(S2)を行う。
成形する方法としては限定されず、樹脂組成物の形状に応じて、公知の方法を用いることができる。樹脂組成物の形状としては限定されず、例えば、顆粒形状、粉末形状、タブレット形状、シート形状などが挙げられる。樹脂組成物の形状は、成形方法に応じて選択できる。
また、粉末形状とした樹脂組成物を作製する成形工程としては、例えば、混合物を粉砕し顆粒形状の樹脂組成物とした後、該顆粒形状の樹脂組成物をさらに粉砕する工程が挙げられる。
また、タブレット形状とした樹脂組成物を作製する成形工程としては、例えば、混合物を粉砕し顆粒形状の樹脂組成物とした後、該顆粒形状の樹脂組成物を打錠成型する工程が挙げられる。
また、シート形状とした樹脂組成物を作製する成形工程としては、例えば、溶融混練後、混合物を押出成形またはカレンダー成形する工程が挙げられる。
本実施形態に係るフラックスは、ロジンと、活性剤と、溶剤と、を含む。
本実施形態に係るフラックスは、例えば、半田のリフローにより生じるフラックス残渣の絶対量が少ない、低残渣タイプのフラックスであることが好ましい。これにより、フラックス残渣の絶対量を低減することができ、樹脂組成物中により分散することができる。ここで、低残渣タイプのフラックスとしては、フラックスについて、熱重量測定で評価される、窒素雰囲気下、昇温速度10℃/minで温度25℃から250℃に昇温した時の、昇温前の前記フラックスの質量に対する、昇温後の前記フラックスの質量の百分率(質量変化率)は、21質量%以下のものであり、例えば、15質量%以下のものが好ましく、10質量%以下のものがより好ましく、5質量%以下のものがさらに好ましい。これにより、フラックス残渣の絶対量を低減することができる。これにより、樹脂組成物中にフラックス残渣をより分散でき、相溶性を向上できる。
なお、上記質量変化率の下限値としては、例えば、0質量%超としてもよく、5質量%以上としてもよく、10質量%以上としてもよい。
ロジン(松脂)としては、具体的には、ガムロジン、ウッドロジン及びトール油ロジンなどの原料ロジン;上記原料ロジンから誘導されるロジン誘導体などが挙げられる。
ロジン誘導体としては、具体的には、アクリル酸変性ロジン、フェノール変性ロジン、マレイン酸変性ロジン、フマル酸変性ロジンなどのα,β不飽和カルボン酸変性ロジン;水添ロジン;重合ロジン;不均化ロジン;上記α,β不飽和カルボン酸変性ロジン、水添ロジン、重合ロジン、不均化ロジンを精製した精製ロジンなどが挙げられる。ロジンとしては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。ロジンとしては、上記具体例のうち例えば、α,β不飽和カルボン酸変性ロジンを用いることが好ましい。
本実施形態に係るフラックス中のロジンの含有量の下限値としては、フラックス100質量部に対して、1質量部以上であり、例えば、2質量部以上であることが好ましく、3質量部以上であることがより好ましい。これにより、半田付けを好適に行うことができる。
活性剤としては、具体的には、アミン、有機酸などを用いることができる。活性剤としては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。
以下、詳細を説明する。
活性剤として用いられるアミンとしては、具体的には、シクロへキシルアミンなどの脂肪族アミン;アニリンなどの芳香族アミン;イミダゾール類、ベンゾトリアゾール類、ピリジン類などの複素環アミン;上記脂肪族アミン、芳香族アミン、複素環アミンの塩酸塩、臭化水素酸塩、テトラフルオロホウ酸塩などが挙げられる。アミンとしては、上記具体例のうち、1種または2種以上を組み合わせて用いることができる。アミンとしては、上記具体例のうち例えば、イミダゾール、ベンゾトリアゾールを用いることが好ましい。
次に、本実施形態に係る電子装置について説明する。
図2は、本実施形態に係る電子装置の一例を示す図である。
図2に示すように、本実施形態に係る電子装置100は、例えば、基材10と、電子部品20とを備えるものであり、電子部品20を封止する封止材50を備えるものである。ここで、封止材50は、例えば、上述した樹脂組成物の硬化物によってなる。
なお、図2に示す電子装置100は、電子部品20と基材10とが半田バンプ30を介して電気的に接続されたものであるが、電気的な接続方法はこれに限定されるものではない。
基材10は、例えば、エポキシ樹脂、シアネート樹脂、マレイミド樹脂等によって構成される有機基板や、セラミック基板であってもよい。
半導体素子としては、限定されるものではないが、たとえば、集積回路、大規模集積回路、トランジスタ、サイリスタ、ダイオード、固体撮像素子が挙げられる。
半導体装置の種類としては、具体的には、MAP(Mold Array Package)、QFP(Quad Flat Package)、SOP(Small Outline Package)、CSP(Chip Size Package)、QFN(Quad Flat Non-leaded Package)、SON(Small Outline Non-leaded Package)、BGA(Ball Grid Array)、LF-BGA(Lead Flame BGA)、FCBGA(Flip Chip BGA)、MAPBGA(Molded Array Process BGA)、eWLB(Embedded Wafer-Level BGA)、Fan-In型eWLB、Fan-Out型eWLBなどの種類が挙げられる。
本実施形態に係る電子装置の製造方法は、例えば、基材の金属露出部と、フラックスとを接触させて、金属露出部をフラックス処理するフラックス処理工程と、電子部品及び基材をリフローすることで、半田バンプを介して、電子部品と、基材の金属露出部とを電気的に接続させる半田リフロー工程と、フラックス処理した金属露出部の表面に接するように樹脂組成物を導入する導入工程と、を含む。
なお、本実施形態に係る電子装置の製造方法においては、フラックスを洗浄する工程を行わない。
以下、各工程について、図3を用いて詳細を説明する。
フラックス処理工程では、基材の金属露出部と、フラックスとを接触させて、金属露出部をフラックス処理する。
フラックス処理工程では、まず、図3(a)に示すように半田バンプ30を有する電子部品20を準備する。
次に、図3(b)に示すように電子部品20に設けられた半田バンプ30にフラックス200を塗布する。具体的には、準備した電子部品20における半田バンプ30が設けられている側の面を、フラックス200が塗布された台上に接触させることにより、電子部品20に設けられた半田バンプ30にフラックス200を付着させる。
次いで、図3(c)に示すように、電子部品20を基材10の上に直接配置する。これにより、基材10が備える金属露出部と、フラックス200とを接触させ、金属露出部にフラックス200を付着させるフラックス処理をする。
半田リフロー工程では、電子部品及び基材をリフローすることで、半田バンプを介して、電子部品と、基材の金属露出部とを電気的に接続させる。
具体的には、図3(c)に示す電子部品及び基材からなる構造体をリフローすることで、半田バンプを介して、電子部品と、基材の金属露出部とを電気的に接続させ、図3(d)に示す構造体を得る。ここで、図3(d)に示す構造体においては、例えば、基材10の金属露出部と、基材10上に搭載される電子部品20と、電子部品20が備える半田バンプ30とにフラックス残渣300が付着している。
導入工程では、フラックス処理した金属露出部の表面に接するように樹脂組成物を導入する。
具体的には、図3(e)に示すように、樹脂組成物を導入し、硬化させることで封止材50を成形する。
樹脂組成物を導入する方法としては限定されず、具体的には、トランスファー成形法、圧縮成形法、インジェクション成形法といった方法を用いることができる。
各実施例、各比較例に用いた樹脂組成物の原料成分の詳細について以下に示す。
・エポキシ樹脂1:トリフェニルメタン型エポキシ樹脂とビフェニル型エポキシ樹脂の混合物(三菱化学社製、EPIKOTE YL6677)
・エポキシ樹脂2:ビフェニレン骨格含有フェノールアラルキル型エポキシ樹脂(日本化薬社製、NC-3000)
・エポキシ樹脂3:ビフェニレン骨格含有フェノールアラルキル型エポキシ樹脂(日本化薬社製、NC-3000-L)
・エポキシ樹脂4:トリフェニルメタン型エポキシ樹脂(三菱化学社製、1032H60)
・エポキシ樹脂5:ビスフェノールA型エポキシ樹脂(三菱化学社製、YL6810)
・エポキシ樹脂6:ビフェニル型エポキシ樹脂(三菱化学社製、YX4000K)
・エポキシ樹脂7:ビフェニレン骨格含有フェノールアラルキル型エポキシ樹脂とビフェノールグリシジルエーテルの混合物(日本化薬社製、CER-3000-L)
・フェノール樹脂硬化剤1:トリフェニルメタン型フェノール樹脂(明和化成社製、MEH-7500)
・フェノール樹脂硬化剤2:ビフェニレン骨格含有フェノールアラルキル樹脂(明和化成社製、MEH-7851SS)
・フェノール樹脂硬化剤3:ビフェニレン骨格含有フェノールアラルキル樹脂(明和化成社製、MEH-7851M)
・フェノール樹脂硬化剤4:ビフェニレン骨格含有フェノールアラルキル樹脂(明和化成社製、MEH-7851H)
・フェノール樹脂硬化剤5:ビフェニレン骨格含有フェノールアラルキル樹脂(日本化薬社製、GPH-65)
・フェノール樹脂硬化剤6:ホルムアルデヒドで変性したトリヒドロキシフェニルメタン型フェノール樹脂(エアウォーターケミカル社製、SK Resin HE910-20)
・フェノール樹脂硬化剤7:ノボラック型フェノール樹脂(住友ベークライト社製、Sumilite Resin PR-51470)
なお、Hansen法とは、蒸発エネルギーを分散エネルギーdD(Dispersion Energy)と、分極エネルギーdP(Polar Energy)と、水素結合エネルギーdH(Hydrogen Bonding Energy)とに分け、dD、dP及びdHを三次元ベクトルとしたときのベクトルの長さをSP値として算出する方法である。
測定条件:カラム温度 40℃
溶媒:テトラヒドロフラン
流速:0.6ml/分
検出:RI(示差屈折計)
測定した数平均分子量を下記表1に示す。
・硬化促進剤1:トリフェニルホスフィン(北興化学工業社製、TPP)
・充填材1:球状溶融シリカ(電気化学工業社製、FB-950FC、D50:24μm、粒径75μmを超える粗大粒子の含有量:0.5重量%以下)
・着色剤1:カーボンブラック(三菱化学社製、MA-600)
・カップリング剤1:N-フェニルγ-アミノプロピルトリメトキシシラン(信越化学社製、KBM-573)
・離型剤1:カルナバワックス(日興ファイン社製、ニッコウカルナバ)
下記表2に記載した配合比率にて、各原料成分を、常温でミキサーを用いて混合し、次に70℃以上100℃以下の温度で2軸混練した。次いで、常温まで冷却後、粉砕して、樹脂組成物1~14を作製した。
平均溶解度パラメーターSP1=Σ(A(n)×Ca(n))+Σ(B(m)×Cb(m)) (式1)
(上記式1において、A(n)は、樹脂組成物中に含まれているn種のエポキシ樹脂それぞれに関するHansen法に基づいて算出された溶解度パラメーターを指す。Ca(n)は、樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するn種のエポキシ樹脂それぞれの含有量を指す。B(m)は、樹脂組成物中に含まれているm種のフェノール樹脂硬化剤それぞれに関するHansen法に基づいて算出された溶解度パラメーターを指す。Cb(m)は、樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するm種のフェノール樹脂硬化剤それぞれの含有量を指す。)
数平均分子量Mn1=Σ(a(n)×Ca(n))+Σ(b(m)×Cb(m)) (式3)
(上記式3において、a(n)は、樹脂組成物中に含まれているn種のエポキシ樹脂それぞれに関する数平均分子量の値を指す。Ca(n)は、樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するn種のエポキシ樹脂それぞれの含有量を指す。b(m)は、樹脂組成物中に含まれているm種のフェノール樹脂硬化剤それぞれに関する数平均分子量の値を指す。Cb(m)は、樹脂組成物中における全エポキシ樹脂と全フェノール樹脂硬化剤の合計含有量に対するm種のフェノール樹脂硬化剤それぞれの含有量を指す。)
各実施例、各比較例に用いたフラックスの原料成分の詳細について以下に示す。
・有機酸1:グルタル酸
・アミン1:2-ウンデシルイミダゾール
・溶媒:イソボルニルシクロヘキサノール(87.5wt%)と1,3-ブチレングリコール(12.5wt%)の混合溶媒
下記表3に記載した配合比率にて、各原料成分を、混合することで、フラックス1~5を作製した。
得られたフラックス1~5について、下記の手順に基づいて、加熱処理前後の質量変化率を測定した。
まず、窒素雰囲気下、昇温速度10℃/minで、温度25℃から250℃に昇温する加熱条件で、フラックス1~5のそれぞれを加熱処理した。このとき、熱重量測定装置を用いて、加熱処理前のフラックスの質量M1と、加熱処理後のフラックスの質量M2とを測定した。得られたM1、M2を用いて、式:(M2/M1)×100に基づいて、加熱処理前後のフラックスの質量変化率(質量%)を算出した。
加熱処理前後のフラックスの質量変化率は、昇温前のフラックスの質量に対する、昇温後のフラックスの質量の百分率で表される。測定結果を下記表3に示す。
得られた樹脂組成物およびフラックスを用いて、以下の手順に従って、電子装置を作製した。
まず、長さ15mm×幅15mmの一面に銅回路を備えるプリント配線基板を用意した。
次いで、該プリント配線基板の一面にフラックスを塗工した。
次いで、半田バンプ有する、長さ10mm×幅10mm×厚さ250μmのフリップチップ型パッケージを準備した。
次いで、プリント配線基板の一面上に、フリップチップ型パッケージの半田バンプを有する面を対向配置し、ピーク温度240℃、ピーク温度時間10秒、窒素雰囲気下でリフロー処理することによって、半田バンプを溶融させて、フリップチップ型パッケージと、プリント配線基板の銅回路とを半田接合させた。なお、リフロー処理は2回行った。
次いで、フリップチップ型パッケージが搭載されたプリント配線基板を金型内に配置し、トランスファー成形機を用いて、金型温度175℃、注入圧力9.8MPaの条件で、樹脂組成物を金型内に注入し、成形した。このとき、銅回路の表面、半田バンプの表面に接触させるとともに、フリップチップ型パッケージの周囲を覆うように、樹脂組成物を導入した。成形時に175℃、120秒間の加熱処理を行い、樹脂組成物を硬化させて、封止材を形成した。
以上より、電子装置を作製した。
ここで、上記の電子装置の作製において、樹脂組成物として、上述の樹脂組成物1~14と、フラックスとして、フラックス1~5とを、表4に示す組み合わせで用いた。
表4の樹脂組成物1~14とフラックス1~5の組み合わせに応じて、実施例1~24、比較例1~46の条件を設定した。実施例1~24、比較例1~46のそれぞれにおいて、上記の手順と同様にして、電子装置を作製した。
得られた実施例1~24、比較例1~46の電子装置について、フラックス残渣を洗浄しない場合において、フラックスと樹脂組成物との相溶性を、下記のようにして評価した。
まず、電子装置のプリント配線基板の一面から、フリップチップ型パッケージを含む樹脂組成物の硬化物(封止材)を剥離した。
次いで、プリント配線基板の一面と密着していた硬化物の表面、プリント配線基板の一面のうち硬化物と密着していた表面を目視で観察し、以下の評価基準に基づいて評価した。
○:目視で観察した結果、樹脂組成物の硬化物の表面、プリント配線基板の表面にフラックス残渣が存在しておらず、フラックス残渣が樹脂組成物中に取り込まれたことが確認された。
×:目視で観察した結果樹脂組成物の硬化物の表面、プリント配線基板の表面にフラックス残渣が存在しており、フラックス残渣が樹脂組成物中に取り込まれず残存することが確認された。
これにより、各実施例の電子装置は、各比較例の電子装置と比べて、フラックスと、樹脂組成物との相溶性に優れることが確認された。また、実施例1~24は、比較例1~46と比べて、樹脂組成物の硬化物とプリント配線基材との密着性に優れていた。
以上より、実施例1~24の電子装置の製造方法によって、電子装置の生産性および製造安定性を向上できる。
Claims (19)
- 表面に金属露出部を有する基材と、前記基材上に設けられた電子部品とを備える電子装置の製造方法であって、
前記金属露出部と、フラックスとを接触させて、前記金属露出部をフラックス処理するフラックス処理工程と、
前記フラックス処理した前記金属露出部の表面に接するように樹脂組成物を導入する導入工程と、
を含み、
前記フラックスは、ロジンと、活性剤と、溶剤と、を含み、
前記ロジンの含有量が、前記フラックス100質量部に対して、1質量部以上18質量部以下であり、
前記フラックスにおいて、下記の手順で測定される、加熱処理前後の前記フラックスの質量変化率が21質量%以下であり、
(手順)
窒素雰囲気下、昇温速度10℃/minで、温度25℃から250℃に昇温する加熱条件で、前記フラックスを加熱処理したとき、熱重量測定装置を用いて、加熱処理前の前記フラックスの質量M1と、加熱処理後の前記フラックスの質量M2とを測定する。そして、加熱処理前後の前記フラックスの質量変化率を、得られたM1、M2を用いて、式:(M2/M1)×100に基づいて算出する。
前記樹脂組成物は、エポキシ樹脂と、フェノール樹脂硬化剤と、を含み、
前記樹脂組成物において、前記エポキシ樹脂および前記フェノール樹脂硬化剤からなる樹脂群のHansen法に基づく平均溶解度パラメーターをSP1とし、前記エポキシ樹脂および前記フェノール樹脂硬化剤からなる樹脂群の数平均分子量をMn1としたとき、SP1とMn1とが、Mn1≦210×SP1-4095を満たすものである、
電子装置の製造方法。 - 請求項1に記載の電子装置の製造方法であって、
前記樹脂組成物において、SP1が20.8[cal/cm3]0.5以上30.0[cal/cm3]0.5以下を満たす、電子装置の製造方法。 - 請求項1又は2に記載の電子装置の製造方法であって、
前記樹脂組成物において、Mn1が250以上550以下を満たす、電子装置の製造方法。 - 請求項1から3のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物において、SP1とMn1とが、210×SP1-5000≦Mn1を満たすものである、
電子装置の製造方法。 - 請求項1から4のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物において、前記エポキシ樹脂の含有量が、前記樹脂組成物の全固形分100質量部に対して、2質量部以上20質量部以下である、電子装置の製造方法。 - 請求項1から5のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物において、前記フェノール樹脂硬化剤の含有量が、前記樹脂組成物の全固形分100質量部に対して、2質量部以上20質量部以下である、電子装置の製造方法。 - 請求項1から6のいずれか1項に記載の電子装置の製造方法であって、
前記エポキシ樹脂が、ビフェニル型エポキシ樹脂、多官能エポキシ樹脂、フェノールアラルキル型エポキシ樹脂、ビスフェノール型エポキシ樹脂からなる群より選択される1種または2種以上を含む、電子装置の製造方法。 - 請求項1から7のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物は充填材を更に含む、電子装置の製造方法。 - 請求項8に記載の電子装置の製造方法であって、
前記樹脂組成物において、前記充填材の体積基準粒度分布の累積頻度が50%となる粒径D50が0.1μm以上50μm以下である、電子装置の製造方法。 - 請求項8または9に記載の電子装置の製造方法であって、
前記樹脂組成物において、前記充填材の含有量が、前記樹脂組成物の全固形分100質量部に対して、70質量部以上95質量部以下である、電子装置の製造方法。 - 請求項1から10のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物はカップリング剤を更に含む、電子装置の製造方法。 - 請求項11に記載の電子装置の製造方法であって、
前記カップリング剤が、アミノシランを含む、電子装置の製造方法。 - 請求項1から12のいずれか1項に記載の電子装置の製造方法であって、
前記フラックスにおいて、前記活性剤が、有機酸またはアミンを含む、電子装置の製造方法。 - 請求項13に記載の電子装置の製造方法であって、
前記アミンが、イミダゾールまたはベンゾトリアゾールを含む、電子装置の製造方法。 - 請求項1から13のいずれか1項に記載の電子装置の製造方法であって、
半田バンプを有する前記電子部品を準備し、
続いて、前記フラックス処理工程において、前記半田バンプに前記フラックスを付着させ、
続いて、前記半田バンプを介して、前記電子部品と前記基材の前記金属露出部とを電気的に接続させ、
その後、前記導入工程において、前記基材と前記電子部品との間、及び前記電子部品の周囲に、前記樹脂組成物を導入し、加熱処理する、
電子装置の製造方法。 - 請求項15に記載の電子装置の製造方法であって、
前記フラックス処理工程の後、前記導入工程の前に、前記半田バンプに付着した前記フラックスを溶剤で洗浄する工程を含まない、電子装置の製造方法。 - 請求項1から16のいずれか1項に記載の電子装置の製造方法であって、
前記金属露出部が、金属回路部である、電子装置の製造方法。 - 請求項1から17のいずれか1項に記載の電子装置の製造方法であって、
前記基材が、無機基板または有機基板で構成される、電子装置の製造方法。 - 請求項1から18のいずれか1項に記載の電子装置の製造方法であって、
前記樹脂組成物が熱硬化性樹脂組成物である、電子装置の製造方法。
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KR20200136485A (ko) | 2020-12-07 |
CN111989769B (zh) | 2021-07-13 |
TWI772637B (zh) | 2022-08-01 |
US11158599B2 (en) | 2021-10-26 |
CN111989769A (zh) | 2020-11-24 |
US20210143122A1 (en) | 2021-05-13 |
KR102307666B1 (ko) | 2021-10-05 |
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