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

Abstract

To provide a solid composition which achieves both a low dielectric constant and a low coefficient of linear expansion.SOLUTION: A solid composition contains a fluorine resin, and a fibrous anisotropic filler, where a reduction rate of a coefficient of linear expansion at 20°C to 200°C of the solid composition to a coefficient of linear expansion at 20°C to 200°C of the fluorine resin is 50% or more.SELECTED DRAWING: None

Description

[Technical Field]

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

[0002] As materials for high frequency substrates, fluororesins that have both a low dielectric loss tangent and a low linear expansion coefficient, and solid compositions with fillers, have been investigated (see, for example, Patent Document 1). Furthermore, a dispersion containing a tetrafluoroethylene-based polymer powder, an anisotropic filler, and a liquid dispersion medium has 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, and it is difficult to achieve both, and no solid composition for use as a high-frequency substrate material that achieves both a low dielectric constant and a low linear expansion coefficient has been found. [Prior art documents] [Patent documents]

[0003] [Patent Document 1] Japanese Patent Application Publication No. 2023-155181 [Patent Document 2] International Publication No. 2021 / 112164 Summary of the Invention [Problem to be solved by the invention]

[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. [Means for solving the problem]

[0005] <1> A solid composition containing a fluororesin and a fibrous anisotropic filler, The solid composition has a linear expansion coefficient at 20 to 200°C, the coefficient of which decreases by 50% or more relative to the linear expansion coefficient at 20 to 200°C of the fluororesin. <2> The aspect ratio of the fibrous anisotropic filler is 100 or more. <1> 1. A solid composition according to claim 1. <3> The mass ratio (A / B) of the fibrous anisotropic filler (A) to the fluororesin (B) is 5 / 95 to 60 / 40. <1> or <2> The solid composition is as described in <4> The fibrous anisotropic filler is silica. <1> from <3> 1. A solid composition according to any one of claims 1 to 9. <5> The unstable terminal group present at the end of the main chain of the fluororesin is 1×10 6 There are less than 50 pieces per piece, The unstable terminal group is at least one selected from the group consisting of -CF2H, -COF, -COOH, -COOCH3, -CONH2, and -CH2OH. <1> from <4> 1. A solid composition according to any one of claims 1 to 9. <6> The fluororesin is at least one selected from the group consisting of polytetrafluoroethylene, tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer, and tetrafluoroethylene / hexafluoropropylene copolymer. <1> from <5> 1. A solid composition according to any one of claims 1 to 9. <7> The dielectric loss tangent at 25°C and 10GHz is 0.003 or less. <1> from <6> 1. A solid composition according to any one of claims 1 to 9. <8> The above-mentioned film or sheet <1> from <7> 1. A solid composition according to any one of claims 1 to 9. <9> The insulating material of the circuit board <1> from <8> 1. A solid composition according to any one of claims 1 to 9. <10> The dielectric constant at 25°C and 10GHz is 2.6 or less. <1> from <9> 1. A solid composition according to any one of claims 1 to 9. <11> The aforementioned <1> from <10> 1. A circuit board having an insulating layer containing the solid composition according to any one of claims 1 to 9 and a conductive layer. <12> The conductive layer is a metal. <11> 2. The circuit board according to claim 1 . <13> The metal is copper. <12> 2. The circuit board according to claim 1 . <14> The surface roughness Rz of the conductive layer on the side of the solid composition is 2.0 μm or less. <11> from <13> 10. The circuit board according to claim 9, wherein: <15> The above is a printed circuit board, a laminated circuit board, or a high-frequency board. <11> from <14> 10. The circuit board according to claim 9, wherein: <16> The aforementioned <1> from <10> A method for producing the solid composition according to any one of the preceding claims, comprising: The method for producing a solid composition includes 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, The control unit outputting a predicted index value by inputting the kneading conditions for search into a trained model 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; The proposal device optimizes the kneading conditions for search based on the predicted index value and the target index value, and outputs the optimized kneading conditions. <18> The kneading conditions include information indicating the shape of the filler and information regarding the compounding ratio of the fluororesin and the filler. The aforementioned <17> This is the proposed device described in <19> The kneading conditions include the kneading rotation speed and the kneading time. The aforementioned <18> This is the proposed device described in <20> 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. The aforementioned <18> or <19> This is the proposed device described in <21> 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-like filler relative to a predetermined mass of the fluororesin. The aforementioned <18> from <20> The proposed device is described in any one of the above. [Effects of the Invention]

[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. [Brief explanation of the drawings]

[0007] [Figure 1] FIG. 1 is a diagram illustrating an example of a system configuration of a processing system including a proposed device in a learning phase. [Figure 2] FIG. 2 is a diagram illustrating an example of a hardware configuration of the proposed device. [Figure 3] FIG. 10 is a diagram illustrating an example of learning data. [Figure 4] FIG. 10 is a diagram illustrating details of a method for calculating an index value. [Figure 5] FIG. 10 is a diagram illustrating an example of a functional configuration of the proposed device in a learning phase. [Figure 6] 10 is an example of a flowchart showing a processing flow in a learning phase of the processing system. [Figure 7] FIG. 1 is a diagram illustrating an example of a system configuration of a processing system including a proposed device in a proposal phase. [Figure 8] FIG. 10 is a diagram illustrating an example of a functional configuration of a proposing device in a proposal phase. [Figure 9] 10 is an example of a flowchart showing a processing flow in a proposal phase of a processing system. DETAILED DESCRIPTION OF THE INVENTION

[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 decreases 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, it is possible to reduce (improve) the linear expansion coefficient despite the inclusion of a fluororesin, and it is possible to achieve both a low dielectric constant of 2.5 or less and a low linear expansion coefficient of 50 ppm / °C or less, thereby improving insulation properties and moldability. Furthermore, by incorporating a fibrous anisotropic filler, the solid composition of the present disclosure has fewer internal voids when pelletized, which improves the mechanical properties of films and sheets formed from the pellets. Furthermore, by blending a fibrous anisotropic filler, the electrical properties can be improved. Furthermore, the solid composition of the present disclosure has the advantage that, compared to the dispersion described in Patent Document 2, it has fewer production steps and is easier to form a thick film, because it is a solid.

[0010] <Fluoropolymer> 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 that it can reduce deformation of the solid composition and reduce the linear expansion coefficient, and tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer is more preferred in that it can 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) that is a copolymerization monomer for the tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer include a fluoromonomer represented by the following general formula (10), a fluoromonomer represented by the following general formula (20), a fluoromonomer represented by the following general formula (30), a fluoromonomer represented by the following general formula (40), and a fluoromonomer represented by the following general formula (50). These may be used alone or in combination of two or more.

[0014] General formula (10): CF2=CF-ORf 11 (In the formula, Rf 11 represents a perfluoroorganic group.

[0015] General formula (20): CF2=CF-OCH2-Rf 21 (In the formula, Rf 21 represents a perfluoroalkyl group having 1 to 5 carbon atoms.

[0016] General formula (30): CF2=CFOCF2ORf 31 (In the formula, 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): CF2=CFO(CF2CF(Y 41)O) m (CF2) n F (In the formula, Y 41 represents 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): CF2=CF-O-(CF2CFY 51 -O) n -(CFY 52 ) m -A 51 (In the formula, Y 51 represents a fluorine atom, a chlorine atom, a -SO2F group, or a perfluoroalkyl group. The perfluoroalkyl group may contain an etheric oxygen and a -SO2F group. n represents an integer of 0 to 3. n Y 151 may be the same or different. 52 represents a fluorine atom, a chlorine atom, or a -SO2F group. m represents an integer of 1 to 5. m Y 52 may be the same or different. 51 -SO2X 51 , -COZ 51 or -POZ 52 Z 53 represents X 51 are 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 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 may have an etheric oxygen and a -SOF group.

[0020] "Organic group" means 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-, RaSO2-, RaCOO-, RaNRaCO-, RaCONRa-, RaOCO-, RaOSO2-, and RaNRbSO2-. (wherein, 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.) Among the above organic groups, alkyl groups which may have one or more substituents are preferred.

[0021] In the general formula (10), Rf 11represents a perfluoroorganic group, and examples thereof include a perfluoroalkyl group and a perfluoro(alkoxyalkyl) group. The perfluoroalkyl group is preferably a perfluoroalkyl group having 1 to 10 carbon atoms, more preferably a perfluoroalkyl group having 1 to 5 carbon atoms. 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. Examples of the perfluoro(alkoxyalkyl) group include perfluoro(alkoxyalkyl) groups having 4 to 9 carbon atoms, groups represented by the following general formula (10a), and groups represented by the following general formula (10b).

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

[0023] General formula (10b): [ka] (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, and Rf 11 More preferred is perfluoro(alkyl vinyl ether), which 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 preferably at least one selected from the group consisting of CF2=CFOCF2OCF3, CF2=CFOCF2OCF2CF3, and CF2=CFOCF2OCF2CF2OCF3.

[0026] The fluoromonomer represented by the general formula (40) is preferably at least one selected from the group consisting of CF2=CFOCF2CF(CF3)O(CF2)3F, CF2=CFO(CF2CF(CF3)O)2(CF2)3F, and CF2=CFO(CF2CF(CF3)O)2(CF2)2F.

[0027] The fluoromonomer represented by the general formula (50) is preferably at least one selected from the group consisting of CF2=CFOCF2CF2SO2F, CF2=CFOCF2CF(CF3)OCF2CF2SO2F, CF2=CFOCF2CF(CF2CF2SO2F)OCF2CF2SO2F and CF2=CFOCF2CF(SO2F)2.

[0028] Among the perfluoro(alkyl vinyl ethers), those represented by the general formula (10) and Rf 11 is a perfluoroalkyl group having 1 to 5 carbon atoms, a fluoromonomer represented by the general formula (30), and a fluoromonomer represented by the general formula (40).

[0029] -Other copolymerizable monomers- 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 monomers 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): CH2=CFRf 61 (In the formula, Rf 61 represents a linear or branched fluoroalkyl group having 1 to 12 carbon atoms.

[0031] General formula (70): CH2=CH-(CF2) n -X 71 (In the formula, X 71 is H or F, and n is an integer of 3 to 10.

[0032] General formula (80): CF2=CF-CF2-ORf 81 (In the formula, 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. 61 The number of carbon atoms is preferably 1 to 6. Examples of fluoromonomers represented by general formula (60) include CH2=CFCF3, CH2=CFCF2CF3, CH2=CFCF2CF2CF3, CH2=CFCF2CF2CF2H, CH2=CFCF2CF2CF2CF3, CHF=CHCF3 (E-form), CHF=CHCF3 (Z-form), and the like. Among these, 2,3,3,3-tetrafluoropropylene represented by CH2=CFCF3 is preferred.

[0034] The fluoroalkylethylene represented by the general formula (70) includes CH2=CH-C4F9 and CH2=CH-C6F 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 at least one selected from the group consisting of CF2=CF-CF2-O-CF3, CF2=CF-CF2-O-C2F5, CF2=CF-CF2-O-C3F7, and CF2=CF-CF2-O-C4F9, more preferably at least one selected from the group consisting of CF2=CF-CF2-O-C2F5, CF2=CF-CF2-O-C3F7, and CF2=CF-CF2-O-C4F9, and even more preferably CF2=CF-CF2-O-CF2CF2CF3.

[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 called 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% by mass or more, more preferably 1.1% by 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 that constitute 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 order to obtain a solid composition with excellent heat resistance, and is 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% by mass or more, more preferably 1.1% by 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, it is possible to use a mixture of the PFA and the FEP. 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 ends of the main chain of fluororesin] It is preferable that the unstable terminal groups present at the end of the main chain of the fluororesin are few in terms of electrical properties. Specifically, it is preferable that the number of carbon atoms of the fluororesin is 1×10 6 The number per unit is preferably less than 700, more preferably less than 100, and even more preferably less than 50. There is no particular lower limit. The unstable terminal group is preferably at least one selected from the group consisting of -CF2H, -COF, -COOH, -COOCH3, -CONH2, and -CH2OH, and may be associated with water.

[0045] The -CF2H terminal present at the end of the main chain of the tetrafluoroethylene / perfluoro(alkyl vinyl ether) copolymer (PFA) is preferably 1×10 carbon atoms in the PFA in order to improve the electrical properties (particularly, the dielectric loss tangent). 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 the unstable terminal groups can be reduced, for example, by subjecting the fluororesin to a fluorination treatment. The fluorination treatment can be carried out by a known method, for example, by contacting a fluorine-containing compound with a fluororesin that has not been fluorinated. Furthermore, as the fluorine-containing compound, a fluorine radical source that generates fluorine radicals under fluorination treatment conditions can be used, and examples thereof include F2 gas, CoF3, AgF2, UF6, OF2, N2F2, CF3OF, and halogen fluorides (e.g., IF5, ClF3, etc.).

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

[0048] Specifically, the method for identifying the number of unstable terminal groups is as follows: first, a film-like sample having an average thickness of 0.25 mm to 0.3 mm is prepared 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) I: Absorbance K: Correction coefficient t: average thickness of film (sample) (mm)

[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 order to facilitate 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. In terms of facilitating melt-kneading, the MFR 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, more preferably 80 g / 10 min or less, and 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.), and is 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 per 10 min.

[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, but is preferably 40% by mass to 95% by mass, more preferably 45% by mass or more, even more preferably 50% by mass or more, and more preferably 90% by mass or less, even more preferably 80% by mass or less, based on the total amount of the solid composition.

[0054] <Anisotropic fibrous filler> The fibrous anisotropic filler is a particle having an anisotropic shape (having a different diameter 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, and more preferably 1000 or less.

[0055] The fibrous anisotropic filler is not particularly limited and can be appropriately selected depending on the purpose. 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, verculite, 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 kinds. The fibrous anisotropic filler may 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 selected appropriately 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 fillers] Methods for identifying the fibrous anisotropic filler include, for example, shape observation by microscopic observation of the cross section of the solid composition (e.g., measurement of the aspect ratio of the anisotropic filler) or shape observation by X-ray CT.

[0059] <Other ingredients> The solid composition of the present disclosure may optionally contain other ingredients. Examples of other components include 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. Examples of the filler 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, sericite, etc.; Carbon compounds such as carbon black, acetylene black, ketjen black, and carbon nanotubes; Metal hydroxides such as aluminum hydroxide and magnesium hydroxide; Examples include various types of glass 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 having ultraviolet absorbing 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) for 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 that aggregation is reduced and good surface roughness can be obtained. 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 the filler 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 is preferable that the silicone compound contains at least one selected from the group consisting of a silane coupling agent and an organosilazane. The amount of the silicone compound used for surface functionalization is determined based on the unit surface area (nm 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 the 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, 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, but may be, for example, 10 ppm / ° C.

[0067] -Decrease in coefficient of linear expansion- 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 for a sheet having an average thickness of 25 μm formed from the solid composition using a thermomechanical analyzer (e.g., EXSTAR6000TMA / SS6000, manufactured by SII NanoTechnology Inc.) under the following measurement conditions: --Measurement conditions-- First stage: The temperature is increased to 150°C at a rate of 5°C / min to remove adsorbed water from the sample. Second stage: Air-cool to room temperature at a rate of 5°C / min. Third step: The actual measurement is carried out at a temperature increase rate of 5°C / min. The average value of the linear expansion coefficients measured in the temperature range of 20°C to 200°C is determined and is taken 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 the fluororesin instead of the solid composition.

[0069] -Dielectric constant- The dielectric constant of the solid composition at 25°C and 10 GHz is preferably 2.5 or less, 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 Corporation) for 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. Within this range, the solid composition 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 Corporation) 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. Examples thereof include pellets, films, and sheets. When used for circuit boards, a film or sheet is preferred, and when used as a molding material, pellets are preferred.

[0074] The number of voids in the solid composition was determined by the number of voids per mm of the observed image in image analysis of laser microscope observation. 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 this range, formability (particularly, sheet formability and strand take-up stability) will be better. The image analysis by the laser microscope observation was carried out on a cross section of a pellet made from the solid composition.

[0075] [Application] The solid composition can reduce (improve) the linear expansion coefficient and can achieve both 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. For example, it may be 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 is 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.

[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 preferable. Examples of the copper include rolled copper and electrolytic copper.

[0081] The surface roughness Rz of the conductive layer on the side of 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, which results in good transmission loss when the insulating layer and the conductive layer are joined. The surface roughness Rz is preferably 0.3 μm or more, and more preferably 0.5 μm or more. The surface roughness Rz is a value (maximum height roughness) calculated by 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> The circuit board of the present disclosure may be one in which, in addition to the insulating layer and the conductive layer, other layers formed from resins other than the fluororesin are further laminated. Examples of the resin other than the fluororesin include thermosetting resins and resins other than thermosetting resins, among which 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 of 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. Examples 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; and casting. Among these, the melt-kneading method is preferred. The method for producing a solid composition according to the present disclosure is a method for producing the solid composition by melt-kneading the fluororesin and the anisotropic filler.

[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, and is preferably 240°C to 450°C, and more preferably 260°C to 400°C.

[0094] (Proposed device) The proposed apparatus of the present disclosure is a proposed apparatus having a control unit that proposes kneading conditions when producing a solid composition containing a fluororesin and a filler, The control unit outputting a predicted index value by inputting the kneading conditions for search into a trained model 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; The kneading conditions for search are optimized based on the predicted index value and the target index value, and the optimized kneading conditions are output. According to the proposed device of the present disclosure, when producing a solid composition containing a fluororesin and a filler, it is possible to propose kneading conditions under which the linear expansion coefficient and dielectric properties satisfy predetermined conditions.

[0095] <System configuration including the proposed device (learning phase)> Next, the system configuration of the entire processing system including the proposal device according to the first embodiment will be described. Fig. 1 is a diagram showing an example of the system configuration of the processing system including the proposal device in the learning phase. As shown in Fig. 1, the processing system 100 has a kneader 130, evaluation devices 151 and 152, and a proposal device 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 reference numeral 110_2). Filler (see reference numeral 120) having a shape (see reference numeral 110_1) defined under each kneading condition, in an amount corresponding to the blending ratio (see reference numeral 110_1) defined under each kneading condition; A specific fluororesin (see reference numeral 120) in an amount corresponding to a blending ratio (see reference numeral 110_1) defined under each kneading condition; The kneader 130 is The kneading rotation speed (see symbol 110_2) defined under each kneading condition, The mixing time defined for each mixing condition (see reference numeral 110_2), It operates based on the

[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 to generate 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 conversion process to a predetermined index value and the generation process of 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 the proposed device> Next, the hardware configuration of the proposal device 180 will be described. Fig. 2 is a diagram showing an example of the hardware configuration of the proposal device. As shown in Fig. 2, the proposal 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 proposal device 180 are connected to each other via a bus 207.

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

[0104] The memory 202 has a main storage device such as a ROM (Read Only Memory), a RAM (Random Access Memory), etc. 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 processor 201 executes the various programs.

[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 setting the recording medium 213. The recording medium 213 here includes media that record information optically, electrically, or magnetically, such as a CD-ROM, a flexible disk, a magneto-optical disk, 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] <Examples 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] As shown in Fig. 3, the learning data 170 includes information items such as "kneading conditions" and "index value." Furthermore, the "kneading conditions" further include detailed information items such as "filler shape," "mixing ratio," "kneading rotation speed," and "kneading time." Furthermore, 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 Figure 3, the column corresponding to "fibrous" or "spherical" contains the following: If the fibrous filler or spherical filler is not surface-functionalized and has a small particle size, enter "0". If the fibrous filler or spherical filler is surface-functionalized and has a small particle size, enter "1"; If the fibrous filler or spherical filler is not surface-functionalized and has a large particle size, enter "2"; If the fibrous or spherical filler is surface-functionalized and has a large particle size, enter "3".

[0113] Furthermore, "filler shape" includes "plate-like." "Plate-like" refers to a plate-like filler. As shown in Figure 3, the column corresponding to the "plate-like" item includes the following: If the plate-shaped filler is not surface-modified, enter "0" If the plate-shaped filler is surface-modified, enter "1".

[0114] The "blending ratio" includes "fibrous," "spherical," and "plate-like." As described above, "fibrous" refers to a fibrous filler, "spherical" refers to a spherical filler, and "plate-like" refers to a plate-like filler. As shown in FIG. 3 , the mass of the fibrous filler relative to a predetermined mass of a specific fluororesin is input in the field corresponding to the "fibrous" item. The mass of the spherical filler relative to a predetermined mass of a specific fluororesin is input in the field corresponding to the "spherical" item. The mass of the plate-like filler relative to a predetermined mass of a specific fluororesin is input in 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 values> Next, a predetermined formula for FOM used when calculating an index value related to the linear expansion coefficient and the dielectric properties will be described. Fig. 4 is a diagram showing details of a 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 -(yy 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 the range of variation in the dielectric properties of, for example, previously analyzed solid compositions. 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 the proposed 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 field corresponding to each item of the "mixing conditions" of 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 field corresponding to the item of the "index value" of 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 the 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 also 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 including the proposed device (proposal phase)> Next, a description will be given of a system configuration in the proposal phase of a processing system including the proposal device 180. Fig. 7 is a diagram showing an example of a system configuration in the proposal phase of a processing system including the proposal device. As shown in Fig. 7, the processing system 700 has the proposal device 180, a kneader 130, and evaluation devices 151 and 152.

[0126] In the proposal phase, the target linear expansion coefficient and the 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 the target dielectric properties. A filler (see symbol 720) having a shape (see symbol 710_1) defined in the searched kneading conditions (see symbol 710) and in an amount according to the blending ratio (see symbol 710_1) defined in the searched kneading conditions; A specific fluororesin (see symbol 720) in an amount corresponding to a blending ratio (see symbol 710_1) defined under the searched kneading conditions (see symbol 710); The kneader 130 is The kneading rotation speed (see reference numeral 710_2) defined in the searched kneading conditions (see reference numeral 710), The kneading time (see reference numeral 710_2) defined in the searched kneading conditions (see reference numeral 710), It operates based on.

[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 proposal 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 proposal device 180.

[0129] <Functional configuration of the proposed 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 formula of FOM shown in FIG. 5 based on the input target linear expansion coefficient and target dielectric property.

[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 it 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] <Proposal phase process flow> Next, a description will be given of the flow of processing in the proposal phase of the processing system 700. Fig. 9 is an example of a flowchart showing the flow of processing 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 proposing device 180 predicts a prediction index value by inputting the kneading conditions for search into the trained model.

[0139] In step S904, the proposing 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 process proceeds to step S905. Alternatively, if the proposing device 180 determines that the predetermined condition is satisfied but determines that searches have not been performed a predetermined number of times, the process 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 met (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 are kneading conditions 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 are kneading conditions 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 proposing 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: A predicted index value is output by inputting the kneading conditions for search into a trained model that has been 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. The kneading conditions for search are optimized based on the predicted index value and the target index value, and the optimized kneading conditions are output.

[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. [Example]

[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 A sheet-like solid composition of Example 1 was produced by melt-kneading 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 using a benchtop kneader (device name: MC15, manufactured by Xplore Instrument) under conditions of a kneading speed of 50 rpm, a kneading temperature of 360°C, and a kneading time of 5 minutes.

[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 "reduction rate of linear expansion coefficient") were evaluated according to the following procedure. First, the obtained solid composition was formed into a sheet with an average thickness of 25 μm 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 stage: The temperature is increased to 150°C at a rate of 5°C / min to remove adsorbed water from the sample. Second stage: Air-cool to room temperature at a rate of 5°C / min. Third step: The actual measurement is carried out at a temperature increase 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] Using a sheet having an average thickness of 25 μm formed using the fluororesin as a sample, the linear expansion coefficient of the fluororesin at 20° C. to 200° C. was similarly measured. 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 "decrease 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 the linear expansion coefficient" was evaluated based on the following evaluation criteria. -Evaluation criteria- ◯: The reduction rate of the linear expansion coefficient is 50% or more. ×: The reduction rate of the 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 using 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 relative dielectric constant of the solid composition is 2.5 or less. ×: The relative dielectric constant of the solid composition is more than 2.5.

[0157] (Comparative Example 1) In Example 1, instead of fibrous silica, spherical silica (spherical silica HS-311, manufactured by Nippon Steel Chemical & Material Co., Ltd., median diameter D 50A 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] [Table 1] [Explanation of symbols]

[0159] 100: Processing system 130: Mixing machine 151, 152: Evaluation device 170: Training data 180: Proposed device 500: Learning Department 810: Prediction Department 820: Evaluation Department 830: Optimization Department

Claims

1. A solid composition containing a fluororesin and a fibrous anisotropic filler, A solid composition in which 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. 2. The solid composition according to claim 1, wherein the aspect ratio of the fibrous anisotropic filler is 100 or more.

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

4. 3. The solid composition according to claim 1, 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 less than 50 per piece, The unstable terminal group is —CF ２ H, -COF, -COOH, -COOCH ３ , -CONH ２ , and -CH ２ 3. The solid composition according to claim 1, wherein the solid composition is at least one selected from the group consisting of OH.

6. 3. The solid composition according to claim 1, 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. 3. The solid composition according to claim 1, wherein the dielectric loss tangent at 25°C and 10 GHz is 0.003 or less.

8. 10. The solid composition of claim 1, which is a film or sheet.

9. 10. The solid composition according to claim 1, which is an insulating material for a circuit board.

10. 2. The solid composition according to claim 1, 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 of claim 1 and a conductive layer.

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

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

14. The circuit board according to claim 11, 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 claim 11, which is a printed circuit board, a multilayer circuit board or a high frequency board.

16. 2. A method for producing the solid composition of claim 1, comprising: A method for producing a solid composition, 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, The control unit outputting a predicted index value by inputting the kneading conditions for search into a trained model 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; optimizing the kneading conditions for search based on the predicted index value and the target index value, and outputting the optimized kneading conditions; Proposed device (180).

18. The kneading conditions include information indicating the shape of the filler and information regarding the compounding ratio of the fluororesin and the filler.

18. The proposed device (180) of claim 17.

19. The kneading conditions include the kneading rotation speed and the kneading time.

20. The proposed device (180) of claim 18.

20. 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.

20. The proposed device (180) of claim 18.

21. 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-like filler relative to a predetermined mass of the fluororesin.

20. The proposed device (180) of claim 18.

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