Classifications

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Definitions

• the present disclosure includes the following aspects.
• a polymer film containing a polymer and a filler having a phase-separated structure containing at least two phases, and each of the at least two phases having an elastic modulus of 0.01 GPa or more.
• Ar 4 and Ar 5 each independently represent a phenylene group or a naphthylene group, and Z represents an oxygen atom, a sulfur atom, a carbonyl group, a sulfonyl group, or an alkylene group.
• Z represents an oxygen atom, a sulfur atom, a carbonyl group, a sulfonyl group, or an alkylene group.
• the term "to" indicating a numerical range is used to include the numerical values before and after it as lower and upper limits.
• the upper limit or lower limit of one numerical range may be replaced with the upper or lower limit of another numerical range described step by step.
• the upper or lower limits of the numerical ranges may be replaced with the values shown in the examples.
• alkyl group includes not only alkyl groups having no substituents (unsubstituted alkyl groups) but also alkyl groups having substituents (substituted alkyl groups).
• step in this specification is not only an independent step, but even if it cannot be clearly distinguished from other steps, if the intended purpose of the step is achieved included.
• % by mass and % by weight are synonymous, and “parts by mass” and “parts by weight” are synonymous.
• the weight average molecular weight (Mw) and number average molecular weight (Mn) in the present disclosure use columns of TSKgel GMHxL, TSKgel G4000HxL, and TSKgel G2000HxL (all trade names manufactured by Tosoh Corporation). It is a molecular weight converted using polystyrene as a standard substance detected with a solvent THF (tetrahydrofuran) and a differential refractometer using a gel permeation chromatography (GPC) analyzer.
• THF tetrahydrofuran
• the phase separation structure includes, for example, a sea-island structure, a co-continuous structure, a cylinder structure, and a lamellar structure.
• the sea-island structure means a structure in which one of at least two phases forms a continuous phase and the other phases are dispersed discontinuously.
• a co-continuous structure means a structure in which at least two phases both form a continuous phase.
• a cylindrical structure means a structure having a plurality of rod-like phases in at least one of at least two phases.
• a lamellar structure means a layered structure in which at least two phases are alternately stacked. Both the cylindrical structure and the lamellar structure are structures in which at least two phases form a continuous phase. .
• the polymer film according to the present disclosure preferably has a phase-separated structure in which at least two phases form continuous phases.
• the phase-separated structure in the polymer film according to the present disclosure is preferably a co-continuous structure, a cylindrical structure, or a lamellar structure.
• the organic filler may be nanofiber cellulose.
• the filler is at least selected from the group consisting of boron nitride, aluminum nitride, graphite, silicon carbide, silica, alumina, and beryllium oxide, from the viewpoint of improving heat conductivity.
• the filler is at least selected from the group consisting of boron nitride, aluminum nitride, graphite, silicon carbide, silica, alumina, and beryllium oxide, from the viewpoint of improving heat conductivity.
• One type is preferred.
• the phase separation structure includes two phases, the volume of the filler present in one phase is a, and the volume of the filler present in the other phase is b.
• the ratio a/b is preferably 100/0 to 60/40, more preferably 100/0 to 70/30, and particularly preferably 100/0. That is, it is particularly preferred that only one of the two phases contains fillers.
• the type of polymer is not particularly limited, and known polymers can be used.
• the polymer film has a phase-separated structure containing two phases, for example, embodiments in which both phases contain liquid crystalline polymer; embodiments in which both phases contain polysulfone; and liquid crystal in one phase.
• embodiments in which a polymer is included and the other phase includes polysulfone are included.
• the liquid crystal polymer is preferably a polymer having an aromatic ring, more preferably an aromatic polyester or an aromatic polyesteramide, and even more preferably an aromatic polyesteramide.
• Unit (1) is a structural unit derived from a predetermined aromatic hydroxycarboxylic acid.
• Unit (1) includes those in which Ar 1 is a p-phenylene group (structural unit derived from p-hydroxybenzoic acid) and those in which Ar 1 is a 2,6-naphthylene group (6-hydroxy-2 - structural unit derived from naphthoic acid) or a 4,4'-biphenylylene group (structural unit derived from 4'-hydroxy-4-biphenylcarboxylic acid).
• Unit (2) is a structural unit derived from a predetermined aromatic dicarboxylic acid.
• Unit (2) includes those in which Ar 2 is a p-phenylene group (structural unit derived from terephthalic acid), those in which Ar 2 is an m-phenylene group (structural unit derived from isophthalic acid), and those in which Ar 2 is 2,6-naphthylene group (structural unit derived from 2,6-naphthalene dicarboxylic acid), or Ar 2 is diphenyl ether-4,4'-diyl group (diphenyl ether-4,4'-dicarboxylic acid Structural units derived from acids) are preferred.
• the flow initiation temperature is also called flow temperature or flow temperature, and melts the liquid crystal polymer while increasing the temperature at a rate of 4 ° C./min under a load of 9.8 MPa (100 kg/cm 2 ) using a capillary rheometer. It is the temperature at which a viscosity of 4,800 Pa s (48,000 poise) is exhibited when extruded from a nozzle with an inner diameter of 1 mm and a length of 10 mm, and is a measure of the molecular weight of a liquid crystal polymer (edited by Naoyuki Koide). , "Liquid Crystal Polymer -Synthesis/Molding/Application-", CMC Co., Ltd., June 5, 1987, p.95).
• the polymer content is preferably 20% to 90% by volume, more preferably 30% to 80% by volume, relative to the total volume of the polymer film.
• the method for measuring the dielectric loss tangent in the present disclosure shall be measured by the following method. Loss tangent measurements are performed by the resonance perturbation method at a frequency of 10 GHz. A 10 GHz cavity resonator (Kanto Electronics Applied Development Co., Ltd. CP531) is connected to a network analyzer (Agilent Technology "E8363B"), and a measurement sample (width: 2.0 mm x length: 80 mm) is inserted into the cavity resonator. Then, the dielectric loss tangent of the measurement sample is measured from the change in resonance frequency before and after insertion for 96 hours under an environment of temperature 25° C. and humidity 60% RH.
• the polymer film according to the present disclosure preferably has a thermal conductivity of 1 W/(m ⁇ K) or more, more preferably 3 W/(m ⁇ K) or more.
• the upper limit of thermal conductivity is not particularly limited, and is, for example, 20 W/(m ⁇ K).
• the compound incompatible with the first polymer may be a low-molecular-weight compound having a molecular weight of less than 1,000, or a high-molecular-weight compound having a weight-average molecular weight Mw of 1,000 or more. From the viewpoint of ease of dissolution, it is preferably a polymer compound having a weight average molecular weight Mw of 1,000 or more, and more preferably a water-soluble resin.
• Water-soluble resins include, for example, polyvinyl alcohol, polyacrylamide, polyvinylpyrrolidone, poly(N-vinylacetamide), water-soluble polyesters, and water-soluble polyurethanes.
• the compound incompatible with the first polymer is preferably polyvinylpyrrolidone.
• the solvent is not particularly limited as long as it can dissolve the first polymer and the compound incompatible with the first polymer.
• the immersion step is a step of forming a film B by immersing the film A in a coagulation bath.
• Polar solvents used in the coagulation bath include dioxane, tetrahydrofuran, dimethylformamide, dimethylacetamide, N-methylpyrrolidone, cellosolves, methanol, ethanol, propanol, acetone, tetrahydrofuran, polyethylene glycol, and glycerin.
• the temperature of the coagulation bath is preferably 0°C to 50°C, more preferably 10°C to 35°C, and particularly preferably 20°C to 30°C, from the viewpoint of coagulability.
• the eluent may be a compound that does not dissolve the first polymer but dissolves a compound incompatible with the first polymer at a certain temperature. From the viewpoint of selective dissolution, a water-soluble solvent is preferable. .
• water-soluble solvents include glycerin, 1,2,6-hexanetriol, trimethylolpropane, alkanediols (e.g., ethylene glycol, propylene glycol (1,2-propanediol), 1,3-propanediol, 1 ,3-butanediol, 1,4-butanediol, 2-butene-1,4-diol, 2-ethyl-1,3-hexanediol, 2-methyl-2,4-pentanediol, 1,2-octane diol, 1,2-hexanediol, 1,2-pentanediol, 4-methyl-1,2-pentanediol, etc.), polyalkylene glycol (e.g., diethylene glycol, triethylene glycol, tetraethylene glycol, pentaethylene glycol, di Polyhydric alcohols such as propylene glycol, polyoxyethylene polyoxypropan
• the water-soluble solvent is preferably polyhydric alcohol or polyhydric alcohol ether, more preferably polyhydric alcohol, still more preferably polyalkylene glycol, and particularly preferably diethylene glycol.
• the firing temperature is not particularly limited, it is preferably 200°C to 400°C, more preferably 250°C to 300°C.
• the laminate according to the present disclosure may be a laminate including the polymer film according to the present disclosure.
• the laminate according to the present disclosure preferably has the polymer film according to the present disclosure and a layer arranged on at least one surface of the polymer film.
• the layer arranged on at least one surface of the polymer film is not particularly limited, and examples thereof include a polymer layer and a metal layer.
• the layer arranged on at least one surface of the polymer film may be a coating layer.
• the metal layer is preferably a copper layer.
• the copper layer is preferably a rolled copper foil formed by a rolling method or an electrolytic copper foil formed by an electrolytic method, and more preferably a rolled copper foil from the viewpoint of bending resistance.
• LC-A liquid crystal polymer produced according to the following production method
• LC-B liquid crystal polymer produced according to the following production method
• A-1 Low dielectric loss tangent filler with an average particle size of 600 nm (specially treated fused spherical silica, manufactured by Denka Co., Ltd., dielectric loss tangent 0.0001)
• B-1 Aluminum nitride particles (particle size 1 ⁇ m type, manufactured by Tokuyama Co., Ltd.)
• C-1 Silica particles with an average particle size of 0.5 ⁇ m (product name “SO-C2”, manufactured by Admatechs Co., Ltd.)
• D-1 Hollow powder with an average particle size of 16 ⁇ m (product name “Glass Bubbles iM30K”, manufactured by 3M Japan Co., Ltd.)
• E-1 Boron nitride particles (product name “HP40MF100”, manufactured by Mizushima Ferroalloy Co., Ltd.)
• Table 1 shows the elongation at break of the polymer films obtained in Examples and Comparative Examples. Further, as the filler ratio, a value represented by a/b is described, where a is the volume of the filler present in the first phase and b is the volume of the filler present in the second phase.
• Examples 1 to 10 contain a polymer and a filler, have a phase separation structure containing at least two phases, and both of the at least two phases have an elastic modulus of 0.01 GPa or more. Therefore, it was found that the breaking elongation of the polymer film is large and the toughness is high.
• the thermal conductivity of the polymer films of Examples 3, 4, and 5 was 4 W/(m K), 2 W/(m K), and 0.5 W/(m K), respectively. there were.

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