Solid composition, circuit board, method for producing solid composition, and proposal device

Abstract

A solid composition comprising a fluororesin and a fibrous anisotropic filler, wherein the reduction rate of the linear expansion coefficient of the solid composition at 20-200°C with respect to the linear expansion coefficient of the fluororesin at 20-200°C is 50% or more.

Description

Solid composition, circuit board, method for producing solid composition, and proposed device

[0001] The present disclosure relates to a solid composition, a circuit board, a method for manufacturing the solid composition, and a proposed device.

[0002] As materials for high-frequency substrates, solid compositions containing fluororesins and fillers that combine a low dielectric loss tangent and a low linear expansion coefficient have been investigated (see, for example, Patent Document 1). Also, dispersions containing tetrafluoroethylene-based polymer powder, anisotropic fillers, and a liquid dispersion medium have been reported (see, for example, Patent Document 2). However, a low dielectric constant and a low linear expansion coefficient are generally in a trade-off relationship, making it difficult to achieve both. Therefore, a solid composition for high-frequency substrate materials that combines a low dielectric constant and a low linear expansion coefficient has not yet been found.

[0003] JP 2023-155181 A International Publication No. 2021 / 112164

[0004] An object of the present disclosure is to provide a solid composition that has both a low dielectric constant and a low coefficient of linear expansion.

[0005] <1> A solid composition containing a fluororesin and a fibrous anisotropic filler, wherein the linear expansion coefficient of the solid composition at 20°C to 200°C decreases by 50% or more relative to the linear expansion coefficient of the fluororesin at 20°C to 200°C. <2> The solid composition according to <1>, wherein the aspect ratio of the fibrous anisotropic filler is 100 or more. <3> The solid composition according to <1> or <2>, wherein the mass ratio (A / B) of the fibrous anisotropic filler (A) to the fluororesin (B) is 5 / 95 to 60 / 40. <4> The solid composition according to any one of <1> to <3>, wherein the fibrous anisotropic filler is silica. <5> The solid composition according to any one of <1> to <3>, wherein the unstable terminal group present at the end of the main chain of the fluororesin is 1×10 carbon atoms. ６ the unstable terminal groups are less than 50 per unit area, and the unstable terminal groups are -CF ２ H, -COF, -COOH, -COOCH ３ , -CONH ２ , and -CH ２The solid composition according to any one of <1> to <4>, wherein the fluororesin is at least one selected from the group consisting of polytetrafluoroethylene, tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer, and tetrafluoroethylene / hexafluoropropylene copolymer. <6> The solid composition according to any one of <1> to <5>, wherein the fluororesin is at least one selected from the group consisting of polytetrafluoroethylene, tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer, and tetrafluoroethylene / hexafluoropropylene copolymer. <7> The solid composition according to any one of <1> to <6>, wherein the dielectric loss tangent at 25°C and 10 GHz is 0.003 or less. <8> The solid composition according to any one of <1> to <7>, wherein the solid composition is a film or sheet. <9> The solid composition according to any one of <1> to <8>, wherein the solid composition is an insulating material for circuit boards. <10> The solid composition according to any one of <1> to <9>, wherein the relative dielectric constant at 25°C and 10 GHz is 2.6 or less. <11> A circuit board having an insulating layer containing the solid composition according to any one of <1> to <10> and a conductive layer. <12> The circuit board according to <11>, wherein the conductive layer is a metal. <13> The circuit board according to <12>, wherein the metal is copper. <14> The circuit board according to any one of <11> to <13>, wherein the surface roughness Rz of the conductive layer on the side of the solid composition is 2.0 μm or less. <15> The circuit board according to any one of <11> to <14>, which is a printed circuit board, a multilayer circuit board, or a high-frequency board. <16> A method for producing the solid composition according to any one of <1> to <10>, comprising melt-kneading the fluororesin and the anisotropic filler to obtain the solid composition.<17> A proposal device having a control unit that proposes kneading conditions for producing a solid composition containing a fluororesin and a filler, wherein the control unit: outputs a predicted index value by inputting the search kneading conditions into a trained model trained using training data including the training kneading conditions and index values ​​related to the linear expansion coefficient and dielectric properties of the solid composition produced under the training kneading conditions; optimizes the search kneading conditions based on the predicted index value and a target index value, and outputs the optimized kneading conditions. <18> The proposal device according to <17>, wherein the kneading conditions include information indicating the shape of the filler and information related to the blending ratio of the fluororesin and the filler. <19> The proposal device according to <18>, wherein the kneading conditions include a kneading rotation speed and a kneading time. <20> The proposed device according to <18> or <19>, wherein the information indicating the shape of the filler includes information indicating the shape of the fibrous filler, information indicating the shape of the spherical filler, and information indicating the shape of the plate-like filler. <21> The proposed device according to any one of <18> to <20>, wherein the information relating to the blending ratio includes a mass of the fibrous filler, a mass of the spherical filler, and a mass of the plate-like filler relative to a predetermined mass of the fluororesin.

[0006] According to the present disclosure, it is possible to provide a solid composition that has both a low dielectric constant and a low coefficient of linear expansion.

[0007] 1 is a diagram illustrating an example of a system configuration of a processing system including a proposed device in a learning phase. FIG. 2 is a diagram illustrating an example of a hardware configuration of the proposed device. FIG. 3 is a diagram illustrating an example of learning data. FIG. 4 is a diagram illustrating details of a method for calculating index values. FIG. 5 is a diagram illustrating an example of a functional configuration of the proposed device in a learning phase. FIG. 6 is an example of a flowchart illustrating a processing flow of the processing system in the learning phase. FIG. 7 is a diagram illustrating an example of a system configuration of a processing system including a proposed device in a proposal phase. FIG. 8 is a diagram illustrating an example of a functional configuration of the proposed device in the proposal phase. FIG. 9 is an example of a flowchart illustrating a processing flow of the processing system in the proposal phase.

[0008] (Solid Composition) The solid composition of the present disclosure contains a fluororesin and a fibrous anisotropic filler, and further contains other components as needed. The linear expansion coefficient of the solid composition at 20°C to 200°C is reduced by 50% or more relative to the linear expansion coefficient of the fluororesin at 20°C to 200°C.

[0009] According to the solid composition of the present disclosure, by including a fibrous anisotropic filler, the linear expansion coefficient can be reduced (improved) despite the inclusion of a fluororesin, and a low dielectric constant of 2.5 or less and a low linear expansion coefficient of 50 ppm / °C or less can both be achieved, resulting in good insulation properties and moldability. Furthermore, by incorporating a fibrous anisotropic filler, the amount of internal voids is reduced when the solid composition of the present disclosure is pelletized. This improves the mechanical properties of films and sheets formed from the pellets. Furthermore, by incorporating a fibrous anisotropic filler, the electrical properties can be improved. Furthermore, the solid composition of the present disclosure has the advantage of requiring fewer manufacturing steps and being easier to form thick films than the dispersion described in Patent Document 2, due to its solid nature.

[0010] <Fluororesin> The fluororesin is not particularly limited and can be appropriately selected depending on the purpose, but at least one selected from the group consisting of polytetrafluoroethylene, tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer, and tetrafluoroethylene / hexafluoropropylene copolymer is preferred in terms of being able to reduce deformation of the solid composition and reduce the linear expansion coefficient, and tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer is more preferred in terms of being able to suppress deformation of the solid composition during solder processing. These may be used alone or in combination of two or more.

[0011] The fluororesin has very few hydrogen atoms bonded to carbon atoms in the repeating units constituting the main chain, and may have hydrogen atoms bonded to carbon atoms in structures other than the repeating units constituting the main chain, such as terminal structures.

[0012] The content of the fluorine-containing monomer in the fluororesin may be copolymerized with other copolymerizable monomers as long as it is 90 mol % or more, preferably 95 mol % or more, more preferably 99 mol % or more, and may be 100 mol %.

[0013] -Perfluoro(alkyl vinyl ether)- Examples of the perfluoro(alkyl vinyl ether) copolymerization monomer for the tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer include fluoromonomers represented by the following general formula (10), fluoromonomers represented by the following general formula (20), fluoromonomers represented by the following general formula (30), fluoromonomers represented by the following general formula (40), and fluoromonomers represented by the following general formula (50). These may be used alone or in combination of two or more.

[0014] General formula (10): CF ２ =CF-ORf １１ (wherein, Rf １１ represents a perfluoroorganic group.

[0015] General formula (20): CF ２ =CF-OCH ２ -Rf ２１ (wherein, Rf ２１ represents a perfluoroalkyl group having 1 to 5 carbon atoms.

[0016] General formula (30): CF ２ = CFOCF ２ ORf ３１ (wherein, Rf ３１ represents a linear or branched perfluoroalkyl group having 1 to 6 carbon atoms, a cyclic perfluoroalkyl group having 5 to 6 carbon atoms, or a linear or branched perfluorooxyalkyl group having 2 to 6 carbon atoms and containing 1 to 3 oxygen atoms.

[0017] General formula (40): CF ２ = CFO (CF ２ CF (Y ４１ ) O) ｍ (CF ２ ) ｎ F (wherein, Y ４１represents a fluorine atom or a trifluoromethyl group, m is an integer of 1 to 4, and n is an integer of 1 to 4.

[0018] General formula (50): CF ２ =CF-O-(CF ２ CFY ５１ -O) ｎ -(CFY ５２ ) ｍ -A ５１ (In the formula, Y ５１ represents a fluorine atom, a chlorine atom, -SO ２ It represents a F group or a perfluoroalkyl group. The perfluoroalkyl group is an etheric oxygen and -SO ２ The group n may contain an F group. n represents an integer of 0 to 3. １５１ may be the same or different. ５２ represents a fluorine atom, a chlorine atom, or —SO ２ represents an F group, and m represents an integer of 1 to 5. ５２ may be the same or different. ５１ is -SO ２ X ５１ , -COZ ５１ or -POZ ５２ Z ５３ represents. ５１ is F, Cl, Br, I, -OR ５１ or -NR ５２ R ５３ Represents Z. ５１ , Z ５２ and Z ５３ are each independently -NR ５４ R ５５ Or -OR ５６ Represents R ５１ , R ５２ , R ５３ , R ５４ , R ５５ and R ５６ each independently represents H, ammonium, an alkali metal, an alkyl group which may contain a fluorine atom, an aryl group, or a sulfonyl-containing group.

[0019] Here, the term "perfluoroorganic group" refers to an organic group in which all hydrogen atoms bonded to carbon atoms are substituted with fluorine atoms. The perfluoroorganic group is an organic group in which etheric oxygen and -SO ２ It may have an F group.

[0020] The term "organic group" refers to a group containing one or more carbon atoms or a group formed by removing one hydrogen atom from an organic compound. Examples of the organic group include an alkyl group which may have one or more substituents, an alkenyl group which may have one or more substituents, an alkynyl group which may have one or more substituents, a cycloalkyl group which may have one or more substituents, a cycloalkenyl group which may have one or more substituents, a cycloalkadienyl group which may have one or more substituents, an aryl group which may have one or more substituents, an aralkyl group which may have one or more substituents, a non-aromatic heterocyclic group which may have one or more substituents, a heteroaryl group which may have one or more substituents, a cyano group, a formyl group, RaO-, RaCO-, and RaSO. ２ -, RaCOO-, RaNRaCO-, RaCONRa-, RaOCO-, RaOSO ２ -, and RaNRbSO ２ (In the formula, Ra independently represents an alkyl group which may have one or more substituents, an alkenyl group which may have one or more substituents, an alkynyl group which may have one or more substituents, a cycloalkyl group which may have one or more substituents, a cycloalkenyl group which may have one or more substituents, a cycloalkadienyl group which may have one or more substituents, an aryl group which may have one or more substituents, an aralkyl group which may have one or more substituents, a non-aromatic heterocyclic group which may have one or more substituents, or a heteroaryl group which may have one or more substituents; and Rb independently represents H or an alkyl group which may have one or more substituents.) Of the above organic groups, an alkyl group which may have one or more substituents is preferable.

[0021] In the general formula (10), Rf １１represents a perfluoroorganic group, and examples thereof include a perfluoroalkyl group and a perfluoro(alkoxyalkyl) group. As the perfluoroalkyl group, a perfluoroalkyl group having 1 to 10 carbon atoms and a perfluoroalkyl group having 1 to 5 carbon atoms are more preferred. Examples of the perfluoroalkyl group having 1 to 10 carbon atoms include a perfluoromethyl group, a perfluoroethyl group, a perfluoropropyl group, a perfluorobutyl group, a perfluoropentyl group, and a perfluorohexyl group. As the perfluoro(alkoxyalkyl) group, examples thereof include a perfluoro(alkoxyalkyl) group having 4 to 9 carbon atoms, a group represented by the following general formula (10a), and a group represented by the following general formula (10b).

[0022] General formula (10a): (In the formula, m represents 0 or an integer of 1 to 4.)

[0023] General formula (10b): (In the formula, n represents an integer of 1 to 4.)

[0024] Among the fluoromonomers represented by the general formula (10), Rf １１ is a perfluoroalkyl group having 1 to 10 carbon atoms, and perfluoro(alkyl vinyl ether) [PAVE] is preferred, １１ More preferred are perfluoro(alkyl vinyl ethers) in which the alkyl group is a perfluoroalkyl group having 1 to 5 carbon atoms. Among these, at least one selected from the group consisting of perfluoro(methyl vinyl ether) [PMVE], perfluoro(ethyl vinyl ether) [PEVE], and perfluoro(propyl vinyl ether) [PPVE] is preferred, and at least one selected from the group consisting of perfluoro(methyl vinyl ether) and perfluoro(propyl vinyl ether) is more preferred.

[0025] The fluoromonomer represented by the general formula (30) is CF ２ = CFOCF ２ OCF ３ , C.F. ２ = CFOCF ２ OCF ２ CF ３, and CF ２ = CFOCF ２ OCF ２ CF ２ OCF ３ At least one selected from the group consisting of:

[0026] The fluoromonomer represented by the general formula (40) is CF ２ = CFOCF ２ CF (CF ３ ) O(CF ２ ) ３ F, CF ２ = CFO (CF ２ CF (CF ３ ) O) ２ (CF ２ ) ３ F and CF ２ = CFO (CF ２ CF (CF ３ ) O) ２ (CF ２ ) ２ At least one selected from the group consisting of F is preferred.

[0027] The fluoromonomer represented by the general formula (50) is CF ２ = CFOCF ２ CF ２ SO ２ F, CF ２ = CFOCF ２ CF (CF ３ ) OCF ２ CF ２ SO ２ F, CF ２ = CFOCF ２ CF (CF ２ CF ２ SO ２ F) OCF ２ CF ２ SO ２ F and CF ２ = CFOCF ２ CF (SO ２ F) ２ At least one selected from the group consisting of:

[0028] Among the perfluoro(alkyl vinyl ethers), those represented by the general formula (10) and Rf１１ is a perfluoroalkyl group having 1 to 5 carbon atoms, a fluoromonomer represented by the general formula (30), and at least one selected from the group consisting of a fluoromonomer represented by the general formula (40) are preferred.

[0029] -Other Copolymerizable Monomer- Examples of the other copolymerizable monomer include other fluorine-containing ethylenic monomers and monomers other than fluorine-containing monomers. The other copolymerizable monomers may be used alone or in combination of two or more. Examples of the other fluorine-containing ethylenic monomer include vinyl fluoride [VF], vinylidene fluoride [VdF], chlorotrifluoroethylene [CTFE], a fluoromonomer represented by the following general formula (60), a fluoroalkyl ethylene represented by the following general formula (70), and a fluoroalkyl allyl ether represented by the following general formula (80).

[0030] General formula (60): CH ２ = CFRf ６１ (wherein, Rf ６１ represents a linear or branched fluoroalkyl group having 1 to 12 carbon atoms.

[0031] General formula (70): CH ２ =CH-(CF ２ ) ｎ -X ７１ (In the formula, X ７１ is H or F, and n is an integer from 3 to 10.

[0032] General formula (80): CF ２ =CF-CF ２ -ORf ８１ (wherein, Rf ８１ represents a perfluoroorganic group.

[0033] In general formula (60), Rf ６１ Rf is a linear or branched fluoroalkyl group having 1 to 12 carbon atoms, preferably a linear fluoroalkyl group having 1 to 12 carbon atoms, and more preferably a linear perfluoroalkyl group having 1 to 12 carbon atoms. ６１The number of carbon atoms is preferably 1 to 6. Examples of the fluoromonomer represented by the general formula (60) include CH ２ =CFCF ３ , C.H. ２ =CFCF ２ CF ３ , C.H. ２ =CFCF ２ CF ２ CF ３ , C.H. ２ =CFCF ２ CF ２ CF ２ H, CH ２ =CFCF ２ CF ２ CF ２ CF ３ , CHF=CHCF ３ (E form), CHF=CHCF ３ Among these, CH ２ =CFCF ３ Preferred is 2,3,3,3-tetrafluoropropylene represented by the following formula:

[0034] The fluoroalkylethylene represented by the general formula (70) is CH ２ =CH-C ４ F ９ , and C.H. ２ =CH-C ６ F １３ At least one selected from the group consisting of:

[0035] In the general formula (80), Rf ８１ is Rf in the general formula (10). １１ Although the matters explained in the above can be appropriately selected, a perfluoroalkyl group having 1 to 10 carbon atoms or a perfluoroalkoxyalkyl group having 1 to 10 carbon atoms is preferred. The fluoroalkyl allyl ether represented by the general formula (80) is preferably CF ２ =CF-CF ２ -O-CF ３ , C.F. ２ =CF-CF ２ -O-C ２ F ５ , C.F. ２ =CF-CF ２-O-C ３ F ７ , and CF ２ =CF-CF ２ -O-C ４ F ９ At least one selected from the group consisting of CF ２ =CF-CF ２ -O-C ２ F ５ , C.F. ２ =CF-CF ２ -O-C ３ F ７ , and CF ２ =CF-CF ２ -O-C ４ F ９ More preferably, at least one selected from the group consisting of CF ２ =CF-CF ２ -O-CF ２ CF ２ CF ３ is more preferred.

[0036] The monomer other than the fluorine-containing monomer is not particularly limited as long as it is a monomer unit copolymerizable with TFE, HFP, and PAVE, and can be appropriately selected depending on the purpose. Examples thereof include non-fluorinated ethylenic monomers such as ethylene, propylene, and alkyl vinyl ether; itaconic anhydride, citraconic anhydride, 5-norbornene-2,3-dicarboxylic anhydride, and maleic anhydride.

[0037] The content of perfluoro(alkyl vinyl ether) (PAVE) units in the tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer (also referred to as perfluoroalkoxyalkane (PFA)) is preferably 0.1% by mass or more, more preferably 0.3% by mass or more, even more preferably 0.7% by mass or more, even more preferably 1.0% by mass or more, particularly preferably 1.1% by mass or more, and is preferably 12% by mass or less, more preferably 8.0% by mass or less, even more preferably 6.5% by mass or less, particularly preferably 6.0% by mass or less, based on the total polymerized units. The content of PAVE units is １９ It can be measured by F-NMR.

[0038] In the tetrafluoroethylene / hexafluoropropylene copolymer (also referred to as fluorinated ethylene propylene (FEP)), the mass ratio (TFE / HFP) of tetrafluoroethylene (TFE) units to hexafluoropropylene (HFP) units is preferably 70 / 30 to 99 / 1, more preferably 85 / 15 to 95 / 5. The content of HFP units in the FEP is preferably 1 mass% or more, more preferably 1.1 mass% or more, based on the total monomer units.

[0039] The FEP preferably contains PAVE units in addition to TFE units and HFP units. Examples of the PAVE units contained in the FEP include the same PAVE units as those constituting the PFA, and among these, PPVE is preferred.

[0040] When the FEP contains TFE units, HFP units, and PAVE units, the mass ratio (TFE:HFP:PAVE) is preferably 70-99.8:0.1-25:0.1-25, and more preferably 75-98:1.0-15:1.0-10, in terms of excellent heat resistance and chemical resistance. The content of HFP units and PAVE units in the FEP is preferably 1% by mass or more, more preferably 1.1% by mass or more, based on the total monomer units. The content of HFP units in the FEP is preferably 25% by mass or less, more preferably 20% by mass or less, even more preferably 18% by mass or less, particularly preferably 15% by mass or less, based on the total monomer units, in terms of obtaining a solid composition with excellent heat resistance. Also, preferably 0.1% by mass or more, more preferably 1% by mass or more, and even more preferably 2% by mass or more.

[0041] When the FEP contains TFE units, HFP units, PAVE units, and other copolymerizable monomers, the mass ratio (TFE:HFP:PAVE:other copolymerizable monomers) is preferably 70-98:0.1-25:0.1-25:0.1-10. The content of the monomer units other than the TFE units in the FEP is preferably 1 mass% or more, more preferably 1.1 mass% or more, based on the total monomer units.

[0042] The fluororesin is also preferably a mixture of the PFA and the FEP. In other words, the PFA and the FEP can be used in combination. The mass ratio of the PFA to the FEP (PFA / FEP) is preferably 90 / 10 to 30 / 70, and more preferably 90 / 10 to 50 / 50.

[0043] The fluororesin can be produced by a conventionally known method, for example, by appropriately mixing monomers that form the constituent units thereof and additives such as a polymerization initiator, followed by emulsion polymerization or suspension polymerization.

[0044] [Unstable Terminal Groups Present at the Terminals of the Main Chain of Fluororesin] From the viewpoint of electrical properties, it is preferable that the number of unstable terminal groups present at the terminals of the main chain of the fluororesin is small. ６ The number of unstable terminal groups per unit is preferably less than 700, more preferably less than 100, and even more preferably less than 50. The lower limit is not particularly limited. ２ H, -COF, -COOH, -COOCH ３ , -CONH ２ , and -CH ２ It is preferably at least one selected from the group consisting of OH, which may be associated with water.

[0045] -CF present at the main chain terminal of the tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer (PFA) ２ As the H-terminal, the number of carbon atoms of the PFA is 1×10, in that the electrical properties (particularly, the dielectric tangent) are better. ６ The number per unit is preferably less than 600, more preferably less than 200, even more preferably less than 100, and particularly preferably less than 30. There is no particular lower limit.

[0046] The number of unstable terminal groups can be reduced by, for example, subjecting the fluororesin to a fluorination treatment. The fluorination treatment can be carried out by a known method, for example, by contacting an unfluorinated fluororesin with a fluorine-containing compound. As the fluorine-containing compound, a fluorine radical source that generates fluorine radicals under fluorination treatment conditions can be used, for example, F ２ Gas, CoF ３ , AgF ２ , U.F. ６ , OF ２ , N ２ F ２ , C.F. ３ OF, halogen fluorides (e.g., IF ５ , ClF ３ etc.)

[0047] [Method for Identifying Fluororesin] The fluororesin can be identified and the number of unstable terminal groups can be determined by, for example, analyzing the fluororesin by infrared attenuated total reflection (IR-ATR) using a Fourier transform infrared spectrometer (FT-IR) to identify the constituent components. FT-IR measurements can be performed using, for example, a Nicolet 6700 (manufactured by Thermo Fisher Scientific K.K.).

[0048] Specifically, the method for identifying the number of unstable terminal groups involves first preparing a film-like sample having an average thickness of 0.25 mm to 0.3 mm using the fluororesin. This sample is analyzed by Fourier transform infrared spectroscopy to obtain an infrared absorption spectrum of the fluororesin, and a difference spectrum is obtained from the base spectrum of a standard sample formed using a fluororesin that has been completely fluorinated and has no unstable terminal groups. From the absorption peaks of specific unstable terminal groups that appear in this difference spectrum, the number of carbon atoms in the fluororesin can be determined according to the following formula (A): ６ The number of unstable terminal groups per unit, N, can be calculated. The sample can be prepared by cutting out a pellet or sheet obtained by molding the fluororesin. N = I × K / t (A), where I is absorbance, K is correction coefficient, and t is the average thickness (mm) of the film (sample).

[0049] The melting point of the fluororesin is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 240° C. to 340° C. in terms of facilitating melt-kneading. The upper limit of the melting point is more preferably 318° C. or lower, and even more preferably 315° C. or lower, and the lower limit is more preferably 245° C. or higher, and even more preferably 250° C. or higher. The melting point of the fluororesin can be measured as the temperature corresponding to the maximum value on the heat of fusion curve when the temperature is increased at a rate of 10° C. / min using a differential scanning calorimeter (DSC).

[0050] The melt flow rate (MFR) of the fluororesin at 372°C is not particularly limited and can be appropriately selected depending on the purpose, but in terms of facilitating melt-kneading, it is preferably 0.1 g / 10 min to 100 g / 10 min, more preferably 0.5 g / 10 min or more, even more preferably 1.5 g / 10 min or more, and more preferably 80 g / 10 min or less, even more preferably 40 g / 10 min or less. The MFR is a value obtained in accordance with ASTM D1238, for example, using a melt indexer (manufactured by Yasuda Seiki Seisakusho Co., Ltd.), as the mass (g / 10 min) of polymer flowing out of a nozzle with an inner diameter of 2 mm and a length of 8 mm under a load of 5 kg at 372°C.

[0051] The relative dielectric constant of the fluororesin is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 4.5 or less, more preferably 4.0 or less, even more preferably 3.5 or less, and particularly preferably 2.5 or less, in terms of the relative dielectric constant at 25° C. and a frequency of 10 GHz. The lower limit is not particularly limited, but may be, for example, 1.0 or more.

[0052] The dielectric loss tangent of the fluororesin is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 0.01 or less, more preferably 0.008 or less, and even more preferably 0.005 or less, in terms of dielectric loss tangent at 25° C. and 10 GHz. The lower limit is not particularly limited, but may be, for example, 0.0001 or more.

[0053] The content of the fluororesin is not particularly limited and can be appropriately selected depending on the purpose. However, it is preferably 40% by mass to 95% by mass, more preferably 45% by mass or more, and even more preferably 50% by mass or more, and more preferably 90% by mass or less, and even more preferably 80% by mass or less, based on the total amount of the solid composition.

[0054] <Fibrous Anisotropic Filler> The fibrous anisotropic filler is a particle having an anisotropic shape (the diameter varies depending on the direction) and has a fibrous shape. The aspect ratio of the anisotropic filler, which is the ratio of the longest diameter to the shortest diameter of the anisotropic filler or the ratio of the fiber length to the fiber diameter of the anisotropic filler, is preferably 100 or more, more preferably 200 or more, and even more preferably 500 or more. The upper limit of the aspect ratio is preferably 2000 or less, more preferably 1000.

[0055] The fibrous anisotropic filler is not particularly limited and can be appropriately selected depending on the purpose. Examples include inorganic compounds such as zinc oxide, silica, titanium oxide, zirconium oxide, tin oxide, silicon nitride, silicon carbide, boron nitride, calcium carbonate, calcium silicate, potassium titanate, aluminum nitride, indium oxide, alumina, antimony oxide, cerium oxide, magnesium oxide, iron oxide, and tin-doped indium oxide (ITO); minerals such as montmorillonite, talc, mica, boehmite, kaolin, smectite, zonolite, vermiculite, and sericite; carbon compounds such as carbon nanotubes; and various glasses such as glass fibers. The fibrous anisotropic filler may be used alone or in combination of two or more. The fibrous anisotropic filler may also include a fibrous anisotropic filler that has been surface-functionalized. Among these, silica is preferred.

[0056] The content of the fibrous anisotropic filler is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 5% by mass to 60% by mass, more preferably 10% by mass or more, even more preferably 20% by mass or more, and more preferably 55% by mass or less, even more preferably 50% by mass or less, relative to the total amount of the solid composition.

[0057] The mass ratio (A / B) of the fibrous anisotropic filler (A) to the fluororesin (B) is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 5 / 95 to 60 / 40, more preferably 10 / 90 to 55 / 45, and even more preferably 20 / 80 to 50 / 50.

[0058] [Method for identifying fibrous anisotropic filler] Examples of a method for identifying the fibrous anisotropic filler include a method for identifying the fibrous anisotropic filler by observing the cross section of the solid composition under a microscope (e.g., measuring the aspect ratio of the anisotropic filler) or by observing the cross section using X-ray CT.

[0059] <Other Components> The solid composition of the present disclosure may contain other components as needed, such as fillers, crosslinking agents, antistatic agents, heat stabilizers, foaming agents, foam nucleating agents, antioxidants, surfactants, photopolymerization initiators, anti-wear agents, surface modifiers, resins other than the fluororesins, fillers other than the fibrous anisotropic fillers, and liquid crystal polymers.

[0060] The filler is not particularly limited and can be appropriately selected depending on the purpose, and examples thereof include inorganic compounds such as zinc oxide, silica, titanium oxide, zirconium oxide, tin oxide, silicon nitride, silicon carbide, boron nitride, calcium carbonate, calcium silicate, potassium titanate, aluminum nitride, indium oxide, alumina, antimony oxide, cerium oxide, magnesium oxide, iron oxide, and tin-doped indium oxide (ITO); minerals such as montmorillonite, talc, mica, boehmite, kaolin, smectite, zonolite, vermiculite, and sericite; carbon compounds such as carbon black, acetylene black, ketjen black, and carbon nanotubes; metal hydroxides such as aluminum hydroxide and magnesium hydroxide; and various glasses such as glass beads, glass flakes, and glass balloons. The fillers may be used alone or in combination of two or more.

[0061] The filler is preferably one that has ultraviolet absorption properties, and examples thereof include zinc oxide and titanium oxide, with zinc oxide being preferred. Having ultraviolet absorption properties means that the absorbance of light having a wavelength of 355 nm is 0.1 or more. The absorbance of light having a wavelength of 355 nm is a value measured in a reflection configuration using an ultraviolet-visible-near-infrared spectrophotometer (for example, "V-770" manufactured by JASCO Corporation) on filler powder packed to a thickness of 100 μm.

[0062] The shape of the filler is not particularly limited, and a shape other than a fiber shape can be appropriately selected depending on the purpose. Examples of the shape of the filler include scale-like, plate-like, needle-like, granular, spherical, columnar, cone-like, frustum-like, polyhedral, and hollow shapes.

[0063] The average particle size of the filler is preferably 0.01 μm to 20 μm, more preferably 0.02 μm or more, even more preferably 0.03 μm or more, and more preferably 5 μm or less, even more preferably 2 μm or less, in terms of reducing aggregation and achieving good surface roughness. The average particle size can be measured by a laser diffraction / scattering method.

[0064] The filler may be surface-functionalized, for example, with a silicone compound. By surface-functionalizing with the silicone compound, the relative dielectric constant of the filler can be reduced. The silicone compound is not particularly limited and can be appropriately selected depending on the purpose, but it preferably contains at least one selected from the group consisting of a silane coupling agent and an organosilazane. The amount of surface functionalization of the silicone compound is determined by the unit surface area (nm ) of the filler. ２ The reaction amount of the surface treatment agent per 1000 carbon atoms is preferably 0.1 to 10, more preferably 0.3 to 7.

[0065] From the viewpoint of enhancing affinity with the resin, the functional group of the silane coupling agent is preferably at least one selected from the group consisting of a fluorine-containing group, an amino group, a vinyl group, and an epoxy group, more preferably at least one selected from the group consisting of a fluorine-containing group, an amino group, and a vinyl group, and even more preferably a fluorine-containing group or an amino group.

[0066] [Characteristics of Solid Composition] - Linear Expansion Coefficient - The linear expansion coefficient of the solid composition at 20°C to 200°C is preferably 50 ppm / °C or less, and more preferably 40 ppm / °C or less, in terms of the average linear expansion coefficient in the temperature range of 20°C to 200°C. The lower limit is not particularly limited, and may be, for example, 10 ppm / °C.

[0067] - Reduction rate of linear expansion coefficient- The reduction rate of the linear expansion coefficient of the solid composition at 20°C to 200°C relative to the linear expansion coefficient of the fluororesin at 20°C to 200°C is 50% or more, preferably 55% or more, more preferably 60%, and most preferably 65%. When the reduction rate of the linear expansion coefficient is 50% or more, the linear expansion coefficient of the resulting solid composition can be sufficiently reduced below the linear expansion coefficient of the fluororesin used, and a solid composition with excellent moldability can be obtained.

[0068] The linear expansion coefficient of the solid composition at 20°C to 200°C can be measured using a thermomechanical analyzer (e.g., EXSTAR6000TMA / SS6000, manufactured by SII NanoTechnology Inc.) on a sheet having an average thickness of 25 μm formed from the solid composition under the following measurement conditions. --Measurement Conditions-- Stage 1: The sample is heated to 150°C at a heating rate of 5°C / min to remove absorbed water from the sample. Stage 2: The sample is air-cooled to room temperature at a heating rate of 5°C / min. Stage 3: The main measurement is performed at a heating rate of 5°C / min. The average value of the linear expansion coefficients in the temperature range of 20°C to 200°C measured in this measurement is calculated and used as the linear expansion coefficient of the target solid composition. The linear expansion coefficient of the fluororesin at 20°C to 200°C can also be measured in the same manner by using a fluororesin instead of the solid composition.

[0069] The dielectric constant of the solid composition at 25°C and 10 GHz is preferably 2.5 or less, and more preferably 2.4 or less. There is no particular lower limit, but it may be, for example, 1.0. If the dielectric constant is within the above range, the solid composition can be suitably used for circuit boards.

[0070] The relative dielectric constant of the solid composition at 25°C and 10 GHz can be measured by the SPDR method (resonator method) using a vector network analyzer (e.g., E5063A, manufactured by Keysight) on a sheet having an average thickness of 2.5 µm formed from the solid composition.

[0071] -Dielectric loss tangent- The dielectric loss tangent of the solid composition at 25°C and 10 GHz is preferably 0.003 or less, more preferably 0.002 or less, and even more preferably 0.0015 or less. The lower limit is not particularly limited, but may be, for example, 0.0001. If it is within the above range, it can be suitably used for circuit boards.

[0072] The dielectric loss tangent of the solid composition at 25°C and 10 GHz can be measured by the SPDR method (resonator method) using a vector network analyzer (e.g., E5063A, manufactured by Keysight) on a sheet having an average thickness of 2.5 µm formed from the solid composition.

[0073] The form of the solid composition is not particularly limited and can be appropriately selected depending on the purpose, and examples thereof include pellets, films, sheets, etc. When used for circuit boards, films or sheets are preferred, and when used as a molding material, pellets are preferred.

[0074] The number of voids in the solid composition is determined by the number of voids per 1 mm of an observed image in image analysis of a laser microscope. ２ The number of voids having a width of 30 μm or more per area is preferably 30 or less, more preferably 25 or less, even more preferably 20 or less, and may be 0. Within the above range, moldability (particularly, sheet moldability and strand take-up stability) is improved. Note that the image analysis under laser microscope observation was performed on a cross section of a pellet formed from the solid composition.

[0075] [Uses] The solid composition can reduce (improve) the linear expansion coefficient and can simultaneously achieve a low dielectric constant of 2.5 or less and a low linear expansion coefficient of 50 ppm / °C or less, and therefore can be suitably used as an insulating material (particularly, a low dielectric material) for circuit boards and a thermal conductive material.

[0076] (Circuit Board) The circuit board of the present disclosure has an insulating layer containing the solid composition of the present disclosure, a conductive layer, and may further have other layers as necessary.

[0077] <Insulating Layer> The insulating layer is a layer containing the solid composition, and is preferably a layer made of the solid composition.

[0078] The average thickness of the insulating layer is not particularly limited and can be appropriately selected depending on the purpose, and may be, for example, 1 μm to 1 mm, preferably 20 μm or more, more preferably 30 μm or more, and even more preferably 50 μm or more, and preferably 800 μm or less, more preferably 600 μm or less. The average thickness can be calculated by measuring the thickness at any 10 or more points and averaging these values.

[0079] When forming a film from the dispersion liquid described in Patent Document 2, it is usually difficult to achieve a thickness of 50 μm or more. However, when forming a film from the solid composition, it is easy to achieve a thickness of 50 μm or more.

[0080] <Conductive Layer> The conductive layer is a layer containing a metal, and is preferably a layer made of a metal. The conductive layer may be provided on only one side of the insulating layer, or on both sides. Examples of the metal include copper, stainless steel, aluminum, iron, silver, gold, ruthenium, and alloys thereof. Among these, copper is preferred. Examples of the copper include rolled copper and electrolytic copper.

[0081] The surface roughness Rz of the conductive layer on the side facing the solid composition is preferably 2.0 μm or less, more preferably 1.8 μm or less, and even more preferably 1.5 μm or less. This results in good transmission loss when the insulating layer and the conductive layer are joined. Furthermore, the surface roughness Rz is preferably 0.3 μm or more, more preferably 0.5 μm or more. The surface roughness Rz is a value (maximum height roughness) calculated using the method of JIS C 6515-1998.

[0082] The average thickness of the conductive layer is not particularly limited and can be appropriately selected depending on the purpose, but is preferably 2 μm to 200 μm, more preferably 5 μm to 50 μm.

[0083] <Other Layers> In addition to the insulating layer and the conductive layer, the circuit board of the present disclosure may further include other layers formed from resins other than the fluororesin. Examples of the resins other than the fluororesin include thermosetting resins and resins other than thermosetting resins. Among these, thermosetting resins are preferred.

[0084] The thermosetting resin is preferably at least one selected from the group consisting of polyimide, modified polyimide, epoxy resin, and thermosetting modified polyphenylene ether, more preferably epoxy resin, modified polyimide, or thermosetting modified polyphenylene ether, and even more preferably epoxy resin or thermosetting modified polyphenylene ether.

[0085] The resin other than the thermosetting resin is preferably at least one selected from the group consisting of liquid crystal polymers, polyphenylene ethers, thermoplastic modified polyphenylene ethers, cycloolefin polymers, cycloolefin copolymers, polystyrene, and syndiotactic polystyrene.

[0086] The average thickness of the other layers is preferably 5 μm or more, more preferably 10 μm or more, and is preferably 2000 μm or less, more preferably 1500 μm or less.

[0087] The circuit board is preferably a sheet, and the average thickness of the circuit board is preferably 20 μm or more, more preferably 30 μm or more, and is preferably 5000 μm or less, more preferably 3000 μm or less.

[0088] The circuit board can be suitably used as a printed circuit board, a laminated circuit board (multilayer board), or a high-frequency board.

[0089] The high-frequency circuit board is a circuit board that can operate in a high-frequency band. The high-frequency band may be a band of 1 GHz or higher, preferably a band of 3 GHz or higher, and more preferably a band of 5 GHz or higher. There is no particular upper limit, but it may be a band of 100 GHz or lower.

[0090] (Method for producing solid composition) The method for producing the solid composition of the present disclosure is not particularly limited and can be appropriately selected depending on the purpose, and examples thereof include melt-kneading, injection molding, blow molding, inflation molding, vacuum / pressure molding; paste extrusion in a state where the composition is dispersed or dissolved in a solvent, or a casting method; etc. Among these, the melt-kneading method is preferred. The method for producing the solid composition of the present disclosure is a method for melt-kneading the fluororesin and the anisotropic filler to obtain the solid composition.

[0091] The apparatus used for the melt-kneading is not particularly limited and can be appropriately selected depending on the purpose. Examples thereof include a twin-screw extruder, a single-screw extruder, a multi-screw extruder, and a tandem extruder.

[0092] The melt-kneading time is preferably 10 seconds to 1800 seconds, more preferably 60 seconds to 1200 seconds, and can be, for example, 300 seconds (5 minutes). If the time is too long, the fluororesin may deteriorate, and if the time is too short, the fibrous anisotropic filler may not be sufficiently dispersed. The rotation speed of the melt-kneading is preferably 5 rpm to 200 rpm, more preferably 10 rpm to 100 rpm, and can be, for example, 50 rpm.

[0093] The melt-kneading temperature may be any temperature as long as it is equal to or higher than the melting point of the fluororesin, but is preferably 240°C to 450°C, and more preferably 260°C to 400°C.

[0094] (Proposal Device) The proposal device of the present disclosure is a proposal device having a control unit that proposes kneading conditions for producing a solid composition containing a fluororesin and a filler, wherein the control unit: outputs a predicted index value by inputting the search kneading conditions into a trained model that is trained using training data including the training kneading conditions and index values ​​related to the linear expansion coefficient and dielectric properties of the solid composition produced under the training kneading conditions, optimizes the search kneading conditions based on the predicted index value and a target index value, and outputs the optimized kneading conditions. The proposal device of the present disclosure can propose kneading conditions that satisfy predetermined conditions for the linear expansion coefficient and dielectric properties when producing a solid composition containing a fluororesin and a filler.

[0095] <System Configuration of System Including Proposed Apparatus (Learning Phase)> Next, the system configuration of the entire processing system including the proposed apparatus according to the first embodiment will be described. Fig. 1 is a diagram showing an example of the system configuration of a processing system including the proposed apparatus in the learning phase. As shown in Fig. 1, the processing system 100 has a kneader 130, evaluation devices 151 and 152, and a proposed apparatus 180.

[0096] In the learning phase, the kneader 130 kneads the fluororesin and the filler under various kneading conditions to produce a solid composition. In Fig. 1, kneading condition 1 to kneading condition n (see reference numeral 110) indicate that n patterns of kneading conditions were used to produce the solid composition (see reference numeral 140) in the learning phase.

[0097] In the processing system 100, the kneading conditions include the shape of the filler (fibrous, spherical, plate-like) and the blending ratio (see symbol 110_2). The kneader 130 kneads: a filler (see symbol 120) having a shape (see symbol 110_1) defined in each kneading condition, in an amount corresponding to the blending ratio (see symbol 110_1) defined in each kneading condition; and a specific fluororesin (see symbol 120) in an amount corresponding to the blending ratio (see symbol 110_1) defined in each kneading condition. The kneader 130 operates based on the kneading rotation speed (see symbol 110_2) defined in each kneading condition, and the kneading time (see symbol 110_2) defined in each kneading condition.

[0098] In the processing system 100, the properties of the solid composition (see reference numeral 140) produced under each kneading condition are evaluated in the evaluation device 151 and the evaluation device 152. The evaluation device 151 is a device that evaluates the linear expansion coefficient of the solid composition, and the evaluation device 152 is a device that evaluates the dielectric properties (dielectric loss tangent, relative dielectric constant, dielectric loss, etc.) of the solid composition.

[0099] In the processing system 100, the linear expansion coefficient and dielectric properties (see reference numeral 161) of the solid composition produced under each kneading condition are converted into predetermined index values ​​(values ​​calculated based on a predetermined FOM (Figure of Merit) formula, details of which will be described later) (see reference numeral 162). The index values ​​for the solid compositions produced under each kneading condition are associated with each kneading condition, thereby generating training data 170.

[0100] In the processing system 100, the generated training data is processed by the proposal device 180. In the training phase, the proposal device 180 performs a training process on the training model using the training data to generate a trained model.

[0101] 1 does not mention an entity that performs the process of converting into a predetermined index value and the process of generating the learning data 170, but the conversion process and the generation process may be performed, for example, in the proposal device 180. Alternatively, the conversion process and the generation process may be performed in a device other than the proposal device 180.

[0102] <Hardware Configuration of Proposed Device> Next, the hardware configuration of the proposed device 180 will be described. Fig. 2 is a diagram showing an example of the hardware configuration of the proposed device. As shown in Fig. 2, the proposed device 180 has a processor 201, a memory 202, an auxiliary storage device 203, a connection device 204, a communication device 205, and a drive device 206. Note that the respective hardware components included in the proposed device 180 are connected to each other via a bus 207.

[0103] The processor 201 has various computing devices such as a CPU (Central Processing Unit), a GPU (Graphics Processing Unit), etc. The processor 201 reads various programs (for example, a proposal program, etc.) into the memory 202 and executes them.

[0104] The memory 202 has a main storage device such as a read-only memory (ROM) or a random access memory (RAM). The processor 201 and the memory 202 form a so-called computer (also called a "control unit"), and the processor 201 executes various programs read onto the memory 202, causing the computer to realize various functions.

[0105] The auxiliary storage device 203 stores various programs and various information used when the various programs are executed by the processor 201 .

[0106] The connection device 204 is a connection device that connects to external devices (such as an operation device 211 and a display device 212).

[0107] The communication device 205 is connected to a network (not shown) and is a communication device for transmitting and receiving information to and from each device on the network.

[0108] The drive device 206 is a device for loading the recording medium 213. The recording medium 213 here includes media that record information optically, electrically, or magnetically, such as CD-ROMs, flexible disks, magneto-optical disks, etc. The recording medium 213 may also include semiconductor memories that record information electrically, such as ROMs, flash memories, etc.

[0109] The various programs to be installed in the auxiliary storage device 203 are installed, for example, by setting the distributed recording medium 213 in the drive device 206 and reading the various programs recorded on the recording medium 213 by the drive device 206. Alternatively, the various programs to be installed in the auxiliary storage device 203 may be installed by being downloaded from a network (not shown) via the communication device 205.

[0110] <Specific Example of Learning Data> Next, a description will be given of a specific example of the learning data 170. Fig. 3 is a diagram showing an example of the learning data.

[0111] 3, the learning data 170 includes information items such as "kneading conditions" and "index value." The "kneading conditions" further include detailed information items such as "filler shape," "mixing ratio," "kneading rotation speed," and "kneading time." The "index value" further includes detailed information items such as "FOM calculation result."

[0112] "Filler shape" includes "fibrous" and "spherical." "Fibrous" refers to a fibrous filler, and "spherical" refers to a spherical filler. As shown in FIG. 3 , in the column corresponding to the "fibrous" or "spherical" item, the following is entered: - If the fibrous filler or spherical filler is not surface-functionalized and has a small particle size, "0" is entered; - If the fibrous filler or spherical filler is surface-functionalized and has a small particle size, "1" is entered; - If the fibrous filler or spherical filler is not surface-functionalized and has a large particle size, "2" is entered; - If the fibrous filler or spherical filler is surface-functionalized and has a large particle size, "3" is entered.

[0113] Furthermore, "filler shape" includes "plate-like." "Plate-like" refers to a plate-like filler. As shown in FIG. 3 , in the field corresponding to the item "plate-like," if the plate-like filler is not surface-modified, "0" is entered, and if the plate-like filler is surface-modified, "1" is entered.

[0114] The "blending ratio" includes "fibrous," "spherical," and "plate-like." As described above, "fibrous" refers to fibrous filler, "spherical" refers to spherical filler, and "plate-like" refers to plate-like filler. As shown in FIG. 3 , the mass of fibrous filler relative to a predetermined mass of a specific fluororesin is input into the field corresponding to the "fibrous" item. The mass of spherical filler relative to a predetermined mass of a specific fluororesin is input into the field corresponding to the "spherical" item. The mass of plate-like filler relative to a predetermined mass of a specific fluororesin is input into the field corresponding to the "plate-like" item.

[0115] In the field corresponding to the item "Kneading rotation speed", the rotor rotation speed (rpm) during kneading by the kneader 130 is input. In the field corresponding to the item "Kneading time", the kneading time (min) during kneading by the kneader 130 is input. In the field corresponding to the item "FOM calculation result", index values ​​related to the linear expansion coefficient and dielectric properties are input.

[0116] <Explanation of Index Value> Next, a predetermined formula for FOM used when calculating an index value relating to the linear expansion coefficient and the dielectric property will be described. FIG. 4 is a diagram showing details of the method for calculating the index value. Assuming that the linear expansion coefficient of the solid composition is x and the dielectric property of the solid composition is y (here, y is the product of the dielectric loss tangent and the square root of the relative dielectric constant), as shown in FIG. 4, the formula for FOM used to calculate the index value can be expressed as follows: (Formula) FOM=(x ｍａｘ -x) / x ＿ｒａｎｇｅ -(y-y ｍｉｎ ) / y ＿ｒａｎｇｅ In the above formula, x ｍａｘ is the linear expansion coefficient of the fluororesin, y ｍｉｎ represents the dielectric properties of the fluororesin. ＿ｒａｎｇｅ is, for example, the range of variation of the linear expansion coefficient of a solid composition analyzed in the past, y ＿ｒａｎｇｅ represents, for example, the range of variation in the dielectric properties of solid compositions analyzed in the past. According to the above formula for FOM, the lower the linear expansion coefficient of the solid composition and the lower the dielectric properties, the larger the index value.

[0117] <Functional Configuration of Proposal Device (Learning Phase)> Next, the functional configuration of the proposal device 180 in the learning phase will be described. Fig. 5 is a diagram showing an example of the functional configuration of the proposal device in the learning phase. As described above, a proposal program is installed in the proposal device 180, and by executing the proposal program in the learning phase, the proposal device 180 functions as a learning unit 500.

[0118] As shown in FIG. 5 , the learning unit 500 includes a learning model 510 and a comparison / modification unit 520. Data in each column corresponding to each item of the "mixing conditions" in the learning data 170 is input as input data to the learning model 510. When the input data is input to the learning model 510, the learning model 510 outputs output data. Data in a column corresponding to the "index value" item in the learning data 170 is input as correct answer data to the comparison / modification unit 520. The comparison / modification unit 520 calculates an error based on the output data output from the learning model 510 and the correct answer data, and updates the model parameters of the learning model 510 according to the calculated error. In this way, the learning unit 500 generates a trained model by performing a learning process on the learning model 510 using the learning data 170.

[0119] <Processing Flow in Learning Phase> Next, a description will be given of the processing flow in the learning phase of the processing system 100. Fig. 6 is an example of a flowchart showing the processing flow in the learning phase of the processing system.

[0120] In step S601, the kneader 130 kneads the fluororesin and the filler under various kneading conditions to produce a solid composition.

[0121] In step S602, the evaluation devices 151 and 152 evaluate the linear expansion coefficient and dielectric properties of the produced solid composition, respectively. The proposal device 180 calculates an index value using a predetermined formula for FOM.

[0122] In step S603, the proposing device 180 generates learning data by associating the kneading conditions with the index values.

[0123] In step S604, the proposal device 180 performs a learning process on the learning model 510 using the learning data to generate a trained model.

[0124] In step S605, the proposal device 180 stores the generated trained model.

[0125] <System Configuration (Proposal Phase) of a System Including a Proposed Apparatus> Next, a system configuration in the proposal phase of a processing system including a proposed apparatus 180 will be described. Fig. 7 is a diagram showing an example of the system configuration in the proposal phase of a processing system including a proposed apparatus. As shown in Fig. 7, a processing system 700 has the proposed apparatus 180, a kneader 130, and evaluation devices 151 and 152.

[0126] In the proposal phase, a target linear expansion coefficient and target dielectric properties are input to the proposal device 180. The proposal device 180 searches for kneading conditions that satisfy the target linear expansion coefficient and target dielectric properties. The kneader 130 kneads: a filler (see reference symbol 720) having a shape (see reference symbol 710_1) defined in the searched kneading conditions (see reference symbol 710), in an amount corresponding to the blending ratio (see reference symbol 710_1) defined in the searched kneading conditions; and a specific fluororesin (see reference symbol 720) in an amount corresponding to the blending ratio (see reference symbol 710_1) defined in the searched kneading conditions (see reference symbol 710). The kneader 130 operates based on: - the kneading rotation speed (see symbol 710_2) defined in the searched kneading conditions (see symbol 710); and - the kneading time (see symbol 710_2) defined in the searched kneading conditions (see symbol 710).

[0127] 7, the properties of a solid composition (see reference numeral 740) produced under the searched kneading conditions are evaluated in evaluation devices 151 and 152. Specifically, the evaluation device 151 evaluates the linear expansion coefficient of the produced solid composition, and the evaluation device 152 evaluates the dielectric properties of the produced solid composition (see reference numeral 760).

[0128] This makes it possible to confirm that the linear expansion coefficient and dielectric properties of the solid composition produced under the kneading conditions searched for by the proposing device 180 satisfy the target linear expansion coefficient and target dielectric properties. If the linear expansion coefficient of the produced solid composition does not satisfy the target linear expansion coefficient, or if the dielectric properties of the produced solid composition do not satisfy the target dielectric properties, the solid composition is produced under other kneading conditions searched for by the proposing device 180.

[0129] <Functional Configuration of Proposal Device (Proposal Phase)> Next, the functional configuration of the proposal device 180 in the proposal phase will be described. Fig. 8 is a diagram showing an example of the functional configuration of the proposal device in the proposal phase. As described above, a proposal program is installed in the proposal device 180, and by executing the proposal program in the proposal phase, the proposal device 180 functions as a prediction unit 810, a target index value calculation unit 820, an evaluation unit 830, and an optimization unit 840.

[0130] 8 , the prediction unit 810 has a trained model 811. The training model 811 receives the blending conditions for search output from the optimization unit 830. By receiving the blending conditions for search, the trained model 811 predicts a prediction index value.

[0131] The target index value calculation unit 820 calculates the target index value using the predetermined FOM formula shown in FIG. 5 based on the input target linear expansion coefficient and target dielectric properties.

[0132] The evaluation unit 830 calculates the error between the predicted index value predicted by the trained model 811 and the target index value. The evaluation unit 830 notifies the optimization unit 840 of the calculated error.

[0133] The optimization unit 840 determines whether the error notified by the evaluation unit 830 satisfies a predetermined condition (whether the error is equal to or less than a predetermined threshold). If it is determined that the error is not equal to or less than the predetermined threshold, the optimization unit 840 generates mixing conditions for search and inputs them to the trained model 811. Note that the optimization unit 840 searches for mixing conditions for search that will make the error equal to or less than the predetermined threshold, for example, by Bayesian optimization.

[0134] If the optimization unit 840 determines that the error notified by the evaluation unit 830 is equal to or smaller than a predetermined threshold, it outputs the corresponding kneading conditions for search as the searched kneading conditions.

[0135] <Processing Flow in Proposal Phase> Next, a description will be given of the processing flow in the proposal phase of the processing system 700. Fig. 9 is an example of a flowchart showing the processing flow in the proposal phase of the processing system.

[0136] In step S901, the proposing device 180 receives input of a target linear expansion coefficient and a target dielectric property.

[0137] In step S902, the proposing device 180 calculates a target index value based on the target linear expansion coefficient and the target dielectric property.

[0138] In step S903, the proposal device 180 predicts a prediction index value by inputting the kneading conditions for search into the trained model.

[0139] In step S904, the proposal device 180 determines whether the error between the predicted index value and the target index value satisfies a predetermined condition. If it is determined that the predetermined condition is not satisfied (NO in step S904), the proposal device 180 proceeds to step S905. Alternatively, if the proposal device 180 determines that the predetermined condition is satisfied but determines that the predetermined number of searches has not been performed, the proposal device 180 proceeds to step S905.

[0140] In step S905, the proposing device 180 changes the kneading conditions for search based on Bayesian optimization, and returns to step S903.

[0141] On the other hand, if it is determined in step S904 that the predetermined condition is satisfied (YES in step S904), the process proceeds to step S906. Alternatively, if it is determined that the search has been performed a predetermined number of times, the process proceeds to step S906.

[0142] In step S906, the proposing device 180 outputs the kneading conditions for search when it is determined that the predetermined conditions are satisfied, as the searched kneading conditions.

[0143] In step S907, if a plurality of kneading conditions are found, the proposing device 180 selects one kneading condition.

[0144] In step S908, the kneader 130 kneads the fluororesin and the filler under the searched kneading conditions to produce a solid composition.

[0145] In step S909, the evaluation devices 151 and 152 evaluate the linear expansion coefficient and the dielectric properties of the produced solid composition, respectively.

[0146] In step S910, the proposal device 180 determines whether the linear expansion coefficient and dielectric properties of the generated solid composition satisfy the target linear expansion coefficient and target dielectric properties, respectively. If it is determined in step S910 that the linear expansion coefficient of the generated solid composition does not satisfy the target linear expansion coefficient, and if there are multiple kneading conditions that have been searched for and there is a kneading condition under which a solid composition has not yet been generated, the process returns to step S907. Alternatively, if it is determined in step S910 that the dielectric properties of the generated solid composition do not satisfy the target dielectric properties, and if there are multiple kneading conditions that have been searched for and there is a kneading condition under which a solid composition has not yet been generated, the process returns to step S907.

[0147] On the other hand, if it is determined in step S910 that the linear expansion coefficient and the dielectric properties of the generated solid composition satisfy the target linear expansion coefficient and the target dielectric properties, respectively, the process ends. Alternatively, if there are multiple kneading conditions searched and it is determined that solid compositions have been generated for all of the kneading conditions, the process ends.

[0148] As is clear from the above description, the proposal device 180 according to the first embodiment has a control unit that proposes kneading conditions for producing a solid composition containing a fluororesin and a filler, and the control unit: outputs a predicted index value by inputting the search kneading conditions into a trained model that has been trained using training data that includes training kneading conditions and index values ​​related to the linear expansion coefficient and dielectric properties of the solid composition produced under the training kneading conditions; optimizes the search kneading conditions based on the predicted index value and the target index value, and outputs the optimized kneading conditions.

[0149] As a result, the proposing device 180 according to the first embodiment can search for kneading conditions that satisfy the target linear expansion coefficient and target dielectric properties.

[0150] The present invention will be described in more detail below based on examples, but the present invention is not limited to the following examples.

[0151] Example 1 53 parts by mass of tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer (PFA) (Neoflon PFA AP series, product number: AP-230SH, manufactured by Daikin Industries, Ltd., linear expansion coefficient at 20°C to 200°C: 200 ppm / °C) as a fluororesin and fibrous silica (Silica Chopped Fiber KSF-3N, manufactured by Kowa Co., Ltd., fiber diameter: 7.5 μm, fiber length: 3 mm, aspect ratio: 400) as a fibrous anisotropic filler were melt-kneaded using a benchtop kneader (device name: MC15, manufactured by Xplore Instrument) under conditions of a kneading rotation speed of 50 rpm, a kneading temperature of 360°C, and a kneading time of 5 minutes, to produce a sheet-like solid composition of Example 1.

[0152] <Evaluation> <<Linear Expansion Coefficient and Reduction Rate of Linear Expansion Coefficient>> The linear expansion coefficient of the obtained solid composition at 20°C to 200°C and the reduction rate of the linear expansion coefficient of the solid composition at 20°C to 200°C relative to the linear expansion coefficient of the fluororesin at 20°C to 200°C (hereinafter sometimes referred to as the "reduction rate of linear expansion coefficient") were evaluated according to the following procedure. First, a sheet having an average thickness of 25 μm was formed from the obtained solid composition as a sample, and the linear expansion coefficient of the solid composition at 20°C to 200°C was measured and evaluated using a thermomechanical analyzer (EXSTAR6000TMA / SS6000, manufactured by SII NanoTechnology Inc.) under the following measurement conditions. The results are shown in Table 1. --Measurement Conditions-- First step: The sample was heated to 150°C at a heating rate of 5°C / min to remove adsorbed water. Second step: The sample was air-cooled to room temperature at a heating rate of 5°C / min. Third step: The main measurement was performed at a heating rate of 5°C / min. The average value of the linear expansion coefficients in the temperature range of 20°C to 200°C in this measurement was determined and used as the linear expansion coefficient of the target solid composition.

[0153] Similarly, a sheet having an average thickness of 25 μm formed using the fluororesin was used as a sample, and the linear expansion coefficient of the fluororesin was measured at 20° C. to 200° C. Next, the "linear expansion coefficient of the solid composition at 20° C. to 200° C." was divided by the "linear expansion coefficient of the fluororesin at 20° C. to 200° C.," to determine the "reduction rate of the linear expansion coefficient."

[0154] The "linear expansion coefficient of the solid composition at 20°C to 200°C" was evaluated based on the following evaluation criteria: -Evaluation criteria- ◯: The linear expansion coefficient of the solid composition is 50 ppm / °C or less. ×: The linear expansion coefficient of the solid composition is more than 50 ppm / °C.

[0155] The "reduction rate of linear expansion coefficient" was evaluated based on the following evaluation criteria: -Evaluation criteria- ◯: The reduction rate of linear expansion coefficient is 50% or more. ×: The reduction rate of linear expansion coefficient is less than 50%.

[0156] <<Dielectric Constant>> The dielectric constant of the obtained solid composition was measured by the SPDR method (resonator method) using a sheet having an average thickness of 25 μm formed from the solid composition as a sample at 25° C. and 10 GHz with a vector network analyzer (E5063A, manufactured by Keysight Corporation), and evaluated based on the following evaluation criteria. The results are shown in Table 1. -Evaluation Criteria- ◯: The dielectric constant of the solid composition is 2.5 or less. ×: The dielectric constant of the solid composition is more than 2.5.

[0157] Comparative Example 1 In Example 1, spherical silica (spherical silica HS-311, manufactured by Nippon Steel Chemical & Material Co., Ltd., median diameter D ５０ A solid composition of Comparative Example 1 was produced and evaluated in the same manner as in Example 1, except that the particle diameter was 2.2 μm and the aspect ratio was 1. The results are shown in Table 1.

[0158]

[0159] This application claims priority based on Japanese Patent Application No. 2024-070591, filed on April 24, 2024, the entire contents of which are incorporated herein by reference.

[0160] 100: Processing system 130: Kneader 151, 152: Evaluation device 170: Learning data 180: Proposal device 500: Learning unit 810: Prediction unit 820: Evaluation unit 830: Optimization unit

Claims

1. A solid composition containing a fluororesin and a fibrous anisotropic filler, wherein the linear expansion coefficient of the solid composition at 20°C to 200°C is reduced by 50% or more relative to the linear expansion coefficient of the fluororesin at 20°C to 200°C.

2. The solid composition according to claim 1, wherein the aspect ratio of the fibrous anisotropic filler is 100 or more.

3. The solid composition according to claim 1 or 2, wherein the mass ratio (A / B) of the fibrous anisotropic filler (A) to the fluororesin (B) is 5 / 95 to 60 / 40.

4. A solid composition according to any one of claims 1 to 3, wherein the fibrous anisotropic filler is silica.

5. The unstable terminal group present at the end of the main chain of the fluororesin is 1×10 carbon atoms. ６ the unstable terminal groups are less than 50 per unit area, and the unstable terminal groups are -CF ２ H, -COF, -COOH, -COOCH ３ , -CONH ２ , and -CH ２ 5. The solid composition according to claim 1, wherein the solid composition is at least one selected from the group consisting of OH.

6. A solid composition according to any one of claims 1 to 5, wherein the fluororesin is at least one selected from the group consisting of polytetrafluoroethylene, tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer, and tetrafluoroethylene / hexafluoropropylene copolymer.

7. A solid composition according to any one of claims 1 to 6, having a dielectric loss tangent at 25°C and 10 GHz of 0.003 or less.

8. A solid composition according to any one of claims 1 to 7, which is in the form of a film or sheet.

9. The solid composition according to any one of claims 1 to 8, which is an insulating material for circuit boards.

10. A solid composition according to any one of claims 1 to 9, which has a relative dielectric constant of 2.6 or less at 25°C and 10 GHz.

11. A circuit board having an insulating layer containing the solid composition according to any one of claims 1 to 10 and a conductive layer.

12. The circuit board of claim 11, wherein the conductive layer is a metal.

13. The circuit board of claim 12, wherein the metal is copper.

14. The circuit board according to any one of claims 11 to 13, wherein the surface roughness Rz of the surface of the conductive layer facing the solid composition is 2.0 µm or less.

15. The circuit board according to any one of claims 11 to 14, which is a printed circuit board, a laminated circuit board or a high-frequency board.

16. A method for producing a solid composition according to any one of claims 1 to 10, comprising melt-kneading the fluororesin and the anisotropic filler to obtain the solid composition.

17. A proposal device (180) having a control unit that proposes kneading conditions for producing a solid composition containing a fluororesin and a filler, wherein the control unit: outputs a predicted index value by inputting the kneading conditions for search into a trained model that has been trained using training data including the kneading conditions for learning and index values ​​related to the linear expansion coefficient and dielectric properties of the solid composition produced under the kneading conditions for learning; optimizes the kneading conditions for search based on the predicted index value and a target index value, and outputs the optimized kneading conditions.

18. The proposed device (180) according to claim 17, wherein the kneading conditions include information indicating the shape of the filler and information relating to the compounding ratio of the fluororesin and the filler.

19. The proposed device (180) according to claim 18, wherein the kneading conditions include a kneading rotation speed and a kneading time.

20. The proposed device (180) according to claim 18 or 19, wherein the information indicating the shape of the filler includes information indicating the shape of the fibrous filler, information indicating the shape of the spherical filler, and information indicating the shape of the plate-like filler.

21. A proposed device (180) according to any one of claims 18 to 20, wherein the information relating to the blending ratio includes the mass of the fibrous filler, the mass of the spherical filler, and the mass of the plate-shaped filler relative to a predetermined mass of the fluororesin.

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