Thermal storage composition

Abstract

A heat storage composition including a substance A and a polymer 2, wherein: the heat storage composition has a melting peak temperature between 10 and 60°C, and has melting enthalpy of 30 J / g or more between 10 and 60°C; the heat storage composition does not have a sea-island structure or has a sea-island structure; and the volume-average circle-equivalent particle diameter of the islands (dispersed phase) is 1.5 µm or less, or the area fraction of the islands (dispersed phase) is 15% or less.

Description

[Technical Field]

[0001] The present invention relates to a heat storage composition. [Background technology]

[0002] With the recent increase in the demand for comfort, various textile products and building materials using thermal functional materials have been developed.

[0003] Patent Document 1 describes a heat storage material obtained by kneading a phase transition material obtained by reacting an ethylene-methyl acrylate copolymer with n-eicosyl alcohol with polypropylene. [Prior art documents] [Patent documents]

[0004] [Patent Document 1] Japanese Patent Application Publication No. 2018-188752 Summary of the Invention [Problem to be solved by the invention]

[0005] However, improvements in heat storage materials are required from the viewpoints of heat storage capacity, spinnability, drawability, fiber texture, etc. Therefore, an object of the present application is to provide a novel composition and fiber having excellent heat storage capacity. [Means for solving the problem]

[0006] The present invention relates to, but is not limited to, the following: [Invention 1] A heat storage composition comprising a substance A and a polymer 2, The heat storage composition has a melting peak temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 30 J / g or more; The heat storage composition does not have a sea-island structure, or the heat storage composition has a sea-island structure, and the volume-average circle-equivalent particle diameter of the islands (dispersed phase) is 1.5 μm or less, or the area ratio of the islands (dispersed phase) is 15% or less. Heat storage composition. [Invention 2] The heat storage composition according to Invention 1, which has a plurality of melting peak temperatures, at least one of which is within the range of 60 to 120°C. [Invention 3] 3. The heat storage composition according to claim 1, wherein the gel fraction is 15% by weight or less. [Invention 4] 4. The heat storage composition according to any one of inventions 1 to 3, wherein substance A has a molecular weight of more than 2,000. [Invention 5] A fiber comprising the heat storage composition according to any one of inventions 1 to 4. [Invention 6] A heat storage fiber comprising a heat storage composition comprising substance A and polymer 2, The fiber has a peak melting temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 5 J / g or more; A heat storage fiber in which the heat storage composition of the fiber does not have an island-sea structure, or the heat storage composition of the fiber has an island-sea structure, and the circle-equivalent particle diameter of the islands (dispersed phase) is less than 0.1 μm, or the area ratio of the islands (dispersed phase) is 15% or less. [Invention 7] 7. The heat storage fiber according to claim 6, which has a plurality of melting peak temperatures, at least one of which is within the range of 60 to 120°C. [Invention 8] A heat storage fiber according to invention 6 or 7, wherein the gel fraction of the heat storage composition within the fiber is 15% by weight or less. [Invention 9] 9. The heat storage fiber according to any one of Inventions 6 to 8, wherein Substance A has a molecular weight of more than 2,000. [Effects of the Invention]

[0007] The composition of the present invention has excellent heat storage properties. In one embodiment, the composition of the present invention has excellent shape retention properties. In one embodiment, the composition of the present invention has excellent moldability. In one embodiment, the fiber of the present invention has excellent spinnability and drawability and a good feel. DETAILED DESCRIPTION OF THE INVENTION

[0008] definition All numbers disclosed herein are approximations, whether or not the word "about" or "approximately" is used in conjunction with them. They may vary by 1 percent, 2 percent, 5 percent, or sometimes 10-20 percent. The lower limit R L and upper limit R U Whenever a range of values ​​involving R = R is disclosed, any number falling within the range is specifically disclosed. Specifically, the following numbers within the range are specifically disclosed: R = R L +k * (R U -R L ) where k is a variable ranging from 1 percent to 100 percent in 1 percent increments, i.e., k is 1 percent, 2 percent, 3 percent, 4 percent, 5 percent, ..., 50 percent, 51 percent, 52 percent, ..., 95 percent, 96 percent, 97 percent, 98 percent, 99 percent, or 100 percent. Additionally, any numerical range defined by two R numbers as set forth above is also specifically disclosed.

[0009] The expression "lower limit to upper limit" representing a numerical range means "at least the lower limit, and at most the upper limit," and the expression "upper limit to lower limit" means "at most the upper limit, and at least the lower limit." In other words, these expressions represent a numerical range that includes the lower limit and the upper limit.

[0010] Gel fraction The gel fraction (wt %) can be obtained by the following procedure. Approximately 500 mg of a measurement sample (a crosslinked polymer or a composition containing the same) and an empty wire basket made of wire mesh (opening: 400 mesh) are weighed. The mesh basket containing the measurement sample and 50 mL of xylene (in this example, special-grade xylene (a mixture of o-, m-, p-xylene and ethylbenzene, with a total weight of o-, m-, and p-xylene of 85% or more) manufactured by Kanto Chemical Co., Inc.) are introduced into a 100 mL test tube, and extraction is carried out by heating at 110°C for 6 hours. After extraction, the wire basket containing the extraction residue is removed from the test tube and dried under reduced pressure at 80°C for 3 hours in a vacuum dryer. The dried wire basket containing the extraction residue is weighed. The gel weight is calculated from the difference in weight between the dried wire basket containing the extraction residue and the empty wire basket. The gel fraction (wt%) is calculated using the following formula: Gel fraction = (gel weight / measured sample weight) × 100

[0011] Melting Peak Temperature The melting peak temperature Tm (°C) can be obtained by the following procedure. The aluminum pan containing the sample was measured under a nitrogen atmosphere using a differential scanning calorimeter (DSC Q100 manufactured by TA Instruments was used in the examples) under any of the following measurement conditions. Measurement condition 1: An aluminum pan containing approximately 10 mg of sample is (1) held at 200°C for 5 minutes, then (2) cooled from 200°C to -80°C at a rate of 5°C / min, then (3) held at -80°C for 10 minutes, and then (4) heated from -80°C to approximately 200°C at a rate of 5°C / min. Measurement condition 2: An aluminum pan containing approximately 5 mg of sample is (1) held at 200°C for 5 minutes, then (2) cooled from 200°C to -80°C at a rate of 5°C / min, then (3) held at -80°C for 10 minutes, and then (4) heated from -80°C to approximately 200°C at a rate of 5°C / min. Measurement condition 3: An aluminum pan containing approximately 10 mg of sample is (1) held at 150°C for 5 minutes, then (2) cooled from 150°C to -80°C at a rate of 5°C / min, then (3) held at -80°C for 10 minutes, and then (4) heated from -80°C to approximately 150°C at a rate of 5°C / min. Measurement condition 4: An aluminum pan containing approximately 5 mg of sample is (1) held at 150°C for 5 minutes, then (2) cooled from 150°C to -80°C at a rate of 5°C / min, then (3) held at -80°C for 10 minutes, and then (4) heated from -80°C to approximately 150°C at a rate of 5°C / min. Measurement condition 5: An aluminum pan containing approximately 5 mg of sample is (1) held at 150°C for 5 minutes, then (2) cooled from 150°C to -50°C at a rate of 5°C / min, then (3) held at -50°C for 5 minutes, and then (4) heated from -50°C to approximately 150°C at a rate of 5°C / min. The differential scanning calorimetry curve obtained by the calorimetry in step (4) is taken as the melting curve. The melting curve is analyzed by a method in accordance with JIS K7121-1987 to obtain the melting peak temperature at which the melting endotherm is maximum.

[0012] The glass transition temperature (midpoint glass transition temperature) can be obtained by analyzing the melting curve measured according to the differential scanning calorimetry method described above, using a method in accordance with JIS K7121-1987.

[0013] enthalpy of fusion The fusion enthalpy ΔH (J / g) can be obtained by analyzing the portion of the melting curve within the temperature range of 10 to 60° C. or 60 to 120° C. by a method in accordance with JIS K7122-1987. In the examples, the multi-layered heat storage compositions were kneaded at 200°C using a kneader (Xplore manufactured by DSM) or a 20 mmφ single screw extruder before being used as samples.

[0014] Number of melting peaks between 60 and 120°C The number of melting peaks between 60 and 120°C can be obtained by analyzing the number of temperatures showing maximums when the endothermic direction of the differential scanning calorimetry curve is taken as positive in the range of 60 to 120°C. However, the intensity of 1% or less of the area of ​​the first peak observed between 10 and 60°C is noise and not a peak.

[0015] Circle-equivalent particle size and volume-average circle-equivalent particle size of the dispersed phase The circle-equivalent particle diameter Di (μm) and volume-average circle-equivalent particle diameter Dv (μm) of the dispersed phase (islands in the sea-island structure) contained in the composition and fiber of the present invention can be obtained by the following procedure. The heat storage compositions of the examples of the present invention or comparative examples were cut out using a microtome at -70°C, stained with ruthenium tetroxide vapor at room temperature for about 3 days, and then ultrathin sections with a thickness of about 1300 angstroms were prepared using a diamond knife at -70°C. Note that for the multilayer heat storage compositions in the examples (Examples A1 to A3 and Comparative Examples C1 to C2), the samples were prepared after kneading at 200°C for 5 minutes using a kneader (Xplore, manufactured by DSM). Using a transmission electron microscope (JEM-2100F manufactured by JEOL Ltd. was used in the examples), the ultrathin sections were observed at a magnification of 15,000x for Examples A1 to A6 and Comparative Examples C1 to C4, and at a magnification of 60,000x for Examples B1 to B4 and Comparative Example D1. Regarding the heat storage compositions (Examples A1 to A6 and Comparative Examples C1 to C4), any surface of the kneaded material was observed. Regarding the fibers (Examples B1 to B4 and Comparative Example D1), cross sections in the fiber diameter direction were observed. Using a transmission electron microscope, digital images taken with a CCD camera at a magnification of 15,000x or 60,000x were subjected to the image analysis process described below to determine the circular diameter (circular equivalent particle diameter) and volume-average circular equivalent particle diameter of the dispersed phase.

[0016] Image analysis processing The digital images (8-bit) obtained from the transmission electron microscope were imported into a computer, and the island phase was visually identified based on the intensity of the staining using image analysis software (Asahi Engineering Co., Ltd., A-Zou-kun, in this example). The analysis area of ​​one field of view was approximately 58-73 μm at 15,000x magnification. 2 At 60,000x magnification, it is in the range of approximately 4 to 5 μm2, and is calculated as the average value of two or three visual fields. Since the shape of the dispersed phase is irregular, the diameter of the circle (equivalent circular particle diameter Di (μm)) is found, and the volume-average equivalent circular particle diameter Dv (μm) is calculated using the following formula.

number

[0017] Area ratio of dispersed phase The area ratio (%) of the dispersed phase is calculated based on the following formula: Area ratio (%) = (total area of ​​dispersed phase / analysis area) x 100 Dispersed phases with different staining concentrations are analyzed as different components.

[0018] Melt flow rate (g / 10 min) The melt flow rate (MFR) is measured according to the method specified in JIS-K-7210. Unless otherwise specified, the measurement is performed at a temperature of 230°C and a load of 2.16 kg.

[0019] Shear viscosity (Pa·sec) Using the heat storage composition of the Examples of the present invention or Comparative Examples, a capillary with a diameter of 1 mm, a length of 40 mm, and an inlet angle of 90° was attached to a Capillograph 1B (a product manufactured by Toyo Seiki Seisakusho Co., Ltd. (barrel diameter: 9.55 mm) was used in the Examples), and the measurement temperature was 270°C, and the shear rate was 1.216 × 10 3 sec -1 The shear viscosity is measured.

[0020] Breaking elongation (%) A tensile test is performed on undrawn or drawn yarn under the conditions below in accordance with JIS L 1013:2010, and the breaking elongation is measured three times and averaged. The higher the breaking elongation value, the better the tensile properties (stretchability). Measurement temperature: Room temperature 23℃ Pulling speed: 10 mm / min Grip spacing: 10 mm

[0021] Spinnability When a sample is spun using a spinning device, three people perform a sensory evaluation of the spinnability and determine a consensus opinion (good or broken).

[0022] flexibility The flexibility (hardness) of the sample is evaluated by five examiners using the following method to determine a consensus (soft or hard). Method: The examiner places his / her hand inside 500g of the short fiber and gently squeezes it to determine its flexibility.

[0023] Hereinafter, several embodiments of the present invention will be described in detail, but the present invention is not limited to the following embodiments.

[0024] Heat storage composition E The heat storage composition of the present invention (hereinafter, sometimes referred to as "heat storage composition E") contains a substance A (hereinafter, sometimes referred to as "phase change substance A") and a polymer 2 (hereinafter, sometimes referred to as "base resin"), The heat storage composition E has a melting peak temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 30 J / g or more; The heat storage composition E does not have an island-sea structure, or has an island-sea structure in which the volume-average circle-equivalent particle diameter of the islands (dispersed phase) is 1.5 μm or less, or the area ratio of the islands (dispersed phase) is 15% or less.

[0025] The heat storage composition E has a peak melting temperature within the range of 10 to 60°C, more preferably within the range of 10 to 50°C, and even more preferably within the range of 10 to 40°C.

[0026] Preferably, the heat storage composition E has a plurality of melting peak temperatures, at least one of which is within the range of 60 to 120°C.

[0027] The fusion enthalpy (ΔH) of the heat storage composition E of the present invention between 10 and 60° C. is 30 J / g or more, preferably 40 J / g or more, and more preferably 50 J / g or more.

[0028] The heat storage composition E does not have an island-in-a-sea structure, or it has an island-in-a-sea structure, and the volume-average circle-equivalent particle diameter Dv of the islands (dispersed phase) is 1.5 μm or less, or the area ratio of the islands (dispersed phase) is 15% or less. Preferably, the volume-average circle-equivalent particle diameter Dv of the islands (dispersed phase) is 1.5 μm or less, and the area ratio of the islands (dispersed phase) is 15% or less. When the heat storage composition E has an island-in-a-sea structure, the islands (dispersed phase) have a higher content of polymer 2 than the sea (continuous phase). Dv is preferably 1.3 μm or less, more preferably 1.0 μm or less. When multiple types of dispersed phases are present, the Dv calculated without distinguishing between all types of dispersed phase satisfies the above.

[0029] When the heat storage composition E has an island-sea structure, the area ratio of the islands (dispersed phase) in the cross section of the heat storage composition E is preferably 15% or less, more preferably 13% or less, and even more preferably 10% or less. When multiple types of dispersed phases are present, the total area calculated without distinguishing between all the types of dispersed phases satisfies the above.

[0030] The number of melting peaks between 60 and 120°C of the heat storage composition E is preferably 3 or less, more preferably 2 or less, and even more preferably 1.

[0031] The contents of substance A and polymer 2 in the thermal storage composition E are preferably such that, with the total amount of substance A and polymer 2 being 100% by weight, the content of substance A is 30 to 99% by weight and the content of polymer 2 is 70 to 1% by weight. More preferably, the content of substance A is 50 to 90% by weight and the content of polymer 2 is 50 to 10% by weight. Even more preferably, the content of substance A is 60 to 90% by weight and the content of polymer 2 is 40 to 10% by weight. When the thermal storage composition E is mainly composed of polymers, it may be referred to as a "resin composition". Furthermore, the thermal storage composition E may be referred to as a "thermal storage material" or "thermal storage substance".

[0032] Heat storage fiber F The heat storage composition E contained in the heat storage fiber of the present invention (hereinafter also referred to as "heat storage fiber F") contains a substance A (also referred to as "phase change substance A") described below and a polymer 2 (also referred to as "base resin") described below, The heat storage fiber F has a melting peak temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 5 J / g or more, The heat storage composition E contained in the heat storage fiber F does not have an island-in-a-sea structure, or has an island-in-a-sea structure in which the circle-equivalent particle diameter of the islands (dispersed phase) is less than 0.1 μm, or the area ratio of the islands (dispersed phase) is 15% or less.

[0033] The heat storage fiber F has a melting peak temperature within the range of 10 to 60°C, more preferably within the range of 10 to 50°C, and even more preferably within the range of 10 to 40°C.

[0034] Preferably, the heat storage fiber F has a plurality of melting peak temperatures, at least one of which is in the range of 60 to 120°C.

[0035] The heat storage fiber F of the present invention has a melting enthalpy (ΔH) between 10 and 60°C of 5 J / g or more, preferably 10 J / g or more, and more preferably 15 J / g or more. In one embodiment, the heat storage fiber F has a peak melting temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 20 J / g or more.

[0036] The heat storage composition E of the heat storage fiber F does not have an island-in-a-sea structure, or has an island-in-a-sea structure, and the circle-equivalent particle diameter Di of the islands (dispersed phase) is less than 0.1 μm, or the area ratio of the islands (dispersed phase) is 15% or less. Preferably, the circle-equivalent particle diameter Di of the islands (dispersed phase) is less than 0.1 μm, and the area ratio of the islands (dispersed phase) is 15% or less. When the heat storage composition E has an island-in-a-sea structure, the islands (dispersed phase) have a higher content of polymer 2 than the sea (continuous phase). Di is preferably less than 0.1 μm, more preferably 0.09 μm or less. When multiple types of dispersed phases are present, Di calculated without distinguishing between all types of dispersed phase satisfies the above.

[0037] When the heat storage composition E of the heat storage fiber F has an island-sea structure, the area ratio of the islands (dispersed phase) in the cross section of the heat storage composition E is preferably 15% or less, more preferably 13% or less, and even more preferably 10% or less. When multiple types of dispersed phases are present, the total area calculated without distinguishing between all the types of dispersed phases satisfies the above.

[0038] Preferably, the heat storage fiber F has a plurality of melting peak temperatures, at least one of which is in the range of 60 to 120°C.

[0039] The number of melting peaks between 60 and 120°C of the heat storage fiber F is preferably 3 or less, more preferably 2 or less, and even more preferably 1.

[0040] Substance A Heat storage composition E contains a substance (sometimes referred to as "substance A" or "phase change substance A") that has a peak melting temperature between 10 and 60°C and a melting enthalpy of 30 J / g or more between 10 and 60°C. In this specification, a phase change substance is a material that has heat storage properties due to a phase change.

[0041] Substance A has a peak melting temperature within the range of 10 to 60°C, and the peak melting temperature is preferably within the range of 10 to 50°C, more preferably 10 to 40°C.

[0042] In one embodiment, the substance A has a melting enthalpy ΔH observed within a temperature range of 10 to 60° C. of 30 J / g or more, preferably 40 J / g or more, more preferably 50 J / g or more, and even more preferably 60 J / g or more. The ΔH is usually 200 J / g or less.

[0043] From the viewpoint of shape retention, the gel fraction of the heat storage composition E and the heat storage fiber F is preferably 15% by weight or more, more preferably 20% by weight or more, even more preferably 40% by weight or more, and even more preferably 60% by weight or more. The gel fraction is calculated based on the total weight of the heat storage composition E being 100% by weight. The gel fraction indicates the degree of crosslinking of the crosslinked polymer, and a high gel fraction means that the polymer contained in the composition or fiber has a more crosslinked structure and a stronger network structure is formed. A high gel fraction means that the composition or fiber has high shape retention and is less likely to deform.

[0044] On the other hand, from the viewpoint of spinnability, the gel fraction of the heat storage composition E is preferably 15% by weight or less, more preferably 12% by weight or less, and even more preferably 10% by weight or less. When the gel fraction is low, the composition or fiber tends to have high spinnability.

[0045] The substance A may be a high molecular weight substance (sometimes referred to as polymer 1) or a low molecular weight substance (sometimes referred to as compound L). The heat storage composition E may contain two or more types of substance A, and in this case, it may contain two or more types of polymer 1 only, two or more types of compound L only, or both polymer 1 and compound L.

[0046] Polymer 1 Polymer 1 meets the requirements of substance A and has a molecular weight of greater than 2000.

[0047] The polymer 1 has a melting peak temperature in the range of 10 to 60°C, and the melting peak temperature is preferably in the range of 10 to 50°C, and more preferably in the range of 10 to 40°C.

[0048] For example, the number of structural units B in polymer 1, which will be described later, and the L 6 By adjusting the number of carbon atoms, it is possible to adjust the melting peak temperature of polymer 1. As a result, it is possible to adjust the heat storage performance and the like of a composition containing polymer 1.

[0049] Polymer 1 has a melting enthalpy ΔH between 10 and 60° C. of 30 J / g or more, preferably 40 J / g or more, more preferably 50 J / g or more, and even more preferably 60 J / g or more. ΔH is usually 200 J / g or less.

[0050] For example, when the number of structural units B described later in polymer 1 and L in the following formula (1) of structural units B are 6 By adjusting the number of carbon atoms in the polymer 1, ΔH can be adjusted to fall within the above range, and as a result, the heat storage performance and other properties of the composition containing the polymer 1 can be adjusted.

[0051] The activation energy E of the flow of the polymer 1 a From the viewpoint of further reducing the extrusion load during molding, the extrusion energy is preferably 40 kJ / mol or more, more preferably 50 kJ / mol or more, and even more preferably 60 kJ / mol or more. In addition, in order to ensure that the molded article obtained by extrusion molding has a good appearance, the extrusion energy is preferably 100 kJ / mol or less, more preferably 90 kJ / mol or less, and even more preferably 80 kJ / mol or less. a The magnitude of E depends mainly on the number of long chain branches in the polymer. Polymers with more long chain branches have a higher E a is higher.

[0052] Activation energy of flow E a is obtained by the following method. First, the melt complex viscosity-angular frequency curve of polymer 1 is measured at each temperature T (unit: °C) for three or more temperatures including 170°C from among temperatures of 90°C, 110°C, 130°C, 150°C, and 170°C. The melt complex viscosity-angular frequency curve is a double logarithmic curve with the logarithm of the melt complex viscosity (unit: Pa·sec) on the vertical axis and the logarithm of the angular frequency (unit: rad / sec) on the horizontal axis. Next, for the melt complex viscosity-angular frequency curves measured at each temperature other than 170°C, the angular frequency is adjusted to a T times the melt complex viscosity to 1 / a T Double. a Tis a value that is appropriately determined so that the melt complex viscosity-angular frequency curve measured at each temperature other than 170°C overlaps with the melt complex viscosity-angular frequency curve measured at 170°C.

[0053] The above a T is generally called the shift factor, and is a value that varies depending on the measurement temperature of the melt complex viscosity-angular frequency curve.

[0054] Next, at each temperature T, [ln(a T )] and [1 / (T+273.16)], and then [ln(a T )] and [1 / (T+273.16)] are approximated by the least squares method using the following formula (ii), and the slope m of the line representing formula (ii) is determined. a Ask for. ln(a T )=m(1 / (T+273.16))+n (ii) E a =|0.008314×m| (iii) a T :Shift factor E a : Activation energy of flow (unit: kJ / mol) T: Temperature (unit: ℃)

[0055] The above calculation may be performed using commercially available calculation software, such as Ochestrator manufactured by TA Instruments.

[0056] The above method is based on the following principle. It is known that melt complex viscosity-angular frequency curves (double logarithmic curves) measured at different temperatures can be superimposed on a single parent curve (sometimes called a master curve) by horizontally shifting each temperature curve by a predetermined amount, and this is called the "temperature-time superposition principle." The amount of horizontal shift is called the shift factor, and the shift factor is a value that depends on temperature. It is known that the temperature dependence of the shift factor is expressed by the above formulas (II) and (III), and formulas (II) and (III) are called Arrhenius equations.

[0057] [ln(a T )] and [1 / (T+273.16)] using the least squares method in the above formula (II), the correlation coefficient is set to 0.9 or more.

[0058] The melt complex viscosity-angular frequency curve is measured using a viscoelasticity measuring device (e.g., ARES manufactured by TA Instruments) under the following conditions: geometry: parallel plate, plate diameter: 25 mm, plate spacing: 1.2 to 2 mm, strain: 5%, and angular frequency: 0.1 to 100 rad / sec. The measurement is carried out in a nitrogen atmosphere. It is also preferable to preliminarily blend an appropriate amount of antioxidant (e.g., 1000 ppm by weight) into the measurement sample.

[0059] The extensional viscosity nonlinear index k, which represents the strength of strain hardening of the polymer 1, is preferably 0.85 or more, more preferably 0.90 or more, and even more preferably 0.95 or more, from the viewpoint of excellent moldability, such as small neck-in during T-die film processing, small thickness variations in the resulting film, and resistance to cell breakage during foam molding. Strain hardening of a polymer means that when strain is applied to the polymer, the extensional viscosity increases rapidly above a certain strain. Furthermore, from the viewpoint of ease of molding the polymer 1 or the heat storage composition of the present invention containing the polymer 1 into a desired shape, the index k is preferably 2.00 or less, more preferably 1.50 or less, even more preferably 1.40 or less, even more preferably 1.30 or less, and particularly preferably 1.20 or less.

[0060] The extensional viscosity nonlinearity index k can be calculated using the following method. 110℃ temperature and 1 second -1 Viscosity η at the extension time t when a polymer is uniaxially stretched at a strain rate of E 1(t), a temperature of 110°C and 0.1 seconds -1 Viscosity η at the extension time t when a polymer is uniaxially stretched at a strain rate of E 0.1(t). The η E 1(t) and the aforementioned η E Substitute 0.1(t) into the formula below to find α(t). α(t)=η E 1(t) / η E 0.1(t) The logarithm of α(t) (ln(α(t))) is plotted against the extension time t, and ln(α(t)) and t are approximated by the following formula using the least squares method within the range of t from 2.0 to 2.5 seconds. The slope of the line representing the following formula is k. ln(α(t))=kt The k is adopted when the correlation function r2 used for the least squares approximation in the above formula is 0.9 or more.

[0061] The viscosity when stretched uniaxially is measured using a viscoelasticity measuring device (for example, ARES manufactured by TA Instruments) in a nitrogen atmosphere.

[0062] In extensional viscosity measurements, polymers with long chain branches exhibit a property known as strain hardening, in which the extensional viscosity deviates from the linear region and increases sharply in the high strain region. For polymers with strain hardening, the logarithm of α(t) (ln(α(t))) is known to increase in proportion to ln(l / l0) (where l0 and l are the sample lengths at extension times 0 and t, respectively) [Reference: Koyama Kiyoto, Ishizuka Osamu; Sen'i Gakkaishi Journal, 37, T-258 (1981)]. For polymers without strain hardening, α(t) is 1 for any extension time, and the slope k of the line plotting the logarithm of α(t) (ln(α(t))) against extension time is 0. For polymers with strain hardening, the slope k of the line plot is not 0, especially in the high strain region. In the present invention, the slope of the line obtained by plotting the logarithm (ln(α(t))) of the nonlinear parameter α(t), which is a parameter representing the degree of strain hardening, against the elongation time is defined as k.

[0063] When the polystyrene-equivalent weight average molecular weight Mw of the polymer 1 according to the present invention is measured by gel permeation chromatography (GPC), the mobile phase is usually orthodichlorobenzene and the measurement temperature is 140°C.

[0064] It is preferable that polymer 1 contains structural unit A derived from ethylene, as this improves the moldability of polymer 1.

[0065] With respect to Polymer 1, the ratio A defined by the following formula (I) is preferably 0.95 or less, more preferably 0.90 or less, and even more preferably 0.80 or less. A=α1 / α0(I) In formula (I), α1 is a value obtained by measuring the absolute molecular weight and intrinsic viscosity of a polymer by gel permeation chromatography using an apparatus equipped with a light scattering detector and a viscosity detector, plotting the measured data with the logarithm of the absolute molecular weight on the horizontal axis and the logarithm of the intrinsic viscosity on the vertical axis, and fitting the logarithm of the absolute molecular weight and the logarithm of the intrinsic viscosity by the least squares method using formula (II) within the range where the horizontal axis is equal to or greater than the logarithm of the weight-average molecular weight of the polymer and equal to or less than the logarithm of the z-average molecular weight, to determine the value α1 of the slope of the straight line expressed by formula (II). log[η1]=α1logM1+logK1(II) In formula (II), [η1] represents the intrinsic viscosity of the polymer (unit: dl / g), M1 represents the absolute molecular weight of the polymer, and K1 is a constant. α0 is a value obtained by measuring the absolute molecular weight and intrinsic viscosity of polyethylene standard substance 1475a (manufactured by the National Institute of Standards and Technology) by gel permeation chromatography using an apparatus equipped with a light scattering detector and a viscosity detector, plotting the measured data with the logarithm of the absolute molecular weight on the horizontal axis and the logarithm of the intrinsic viscosity on the vertical axis, and fitting the logarithm of the absolute molecular weight and the logarithm of the intrinsic viscosity by the least squares method using equation (I-II) within the range where the horizontal axis is equal to or greater than the logarithm of the weight-average molecular weight of polyethylene standard substance 1475a and equal to or less than the logarithm of the z-average molecular weight, and determining the value α0 of the slope of the straight line expressed by equation (I-II). log[η0]=α0logM0+logK0(I-II) In formula (I-II), [η0] represents the intrinsic viscosity (unit: dl / g) of polyethylene standard substance 1475a, M0 represents the absolute molecular weight of polyethylene standard substance 1475a, and K0 is a constant.

[0066] In measuring the absolute molecular weight and intrinsic viscosity of the polymer and polyethylene standard substance 1475a by gel permeation chromatography, the mobile phase was orthodichlorobenzene and the measurement temperature was 155°C.

[0067] The absolute molecular weight is determined from the data obtained by the light scattering detector, and the intrinsic viscosity ([η]) is determined by the viscosity detector. Malvern's data processing software OmniSEC (registered trademark) (version 4.7) is used, and calculations are performed based on the literature "Size Exclusion Chromatography, Springer (1999)."

[0068] The polyethylene standard 1475a (manufactured by the National Institute of Standards and Technology) is a non-branched high density polyethylene.

[0069] The formulas (II) and (I-II) are called the Mark-Hauwink-Sakurada formula, which expresses the correlation between the intrinsic viscosity and molecular weight of a polymer. The smaller α1, the greater the number of entanglements of polymer chains due to branched structures. Since the polyethylene reference material 1475a does not form a branched structure, entanglements of polymer chains due to branched structures do not occur. The smaller A, which is the ratio of α1 to α0 for the polyethylene reference material 1475a, the greater the amount of long-chain branched structures formed by the structural unit A described below in the polymer.

[0070] The weight average molecular weight of the polymer 1 measured by gel permeation chromatography using an apparatus equipped with a light scattering detector is preferably 10,000 to 1,000,000, more preferably 50,000 to 750,000, and even more preferably 100,000 to 500,000.

[0071] In measuring the weight-average molecular weight of polymer 1 by gel permeation chromatography, the mobile phase was orthodichlorobenzene and the measurement temperature was 155°C.

[0072] Examples of polymer 1 include polymers having a long-chain alkyl group or a long-chain ether group on the side chain, which may be branched and optionally substituted with a functional group. The polymer is not particularly limited, but examples include polymers primarily composed of (meth)acrylate having a long-chain alkyl group or a long-chain ether group on the side chain, which may be branched and optionally substituted with a functional group; polymers primarily composed of a vinyl ester main chain having a long-chain alkyl group or a long-chain ether group on the side chain, which may be branched and optionally substituted with a functional group; polymers primarily composed of a vinyl ether main chain having a long-chain alkyl group or a long-chain ether group on the side chain, which may be branched and optionally substituted with a functional group; and polymers primarily composed of a polyolefin main chain having a long-chain alkyl group or a long-chain ether group on the side chain, which may be branched and optionally substituted with a functional group. The side chain is preferably a long-chain alkyl group, which may be branched and optionally substituted with a functional group, and polymers primarily composed of a (meth)acrylate or polyolefin main chain are preferred. Examples of polymer 1 include polymers described in JP-A-2015-091903, WO2016 / 098674, and WO2017 / 217419.

[0073] Two or more types of the polymer 1 may be used in combination. The heat storage composition E and the composite of the present invention described below may contain a sensible heat storage material. Examples of the sensible heat storage material include concrete, crushed stone, iron, copper, steel, and polyethylene.

[0074] As one embodiment of the polymer 1, C 14~30 Examples of suitable polymers include those containing structural units having an alkyl group such as the above.

[0075] The polymer 1 preferably has a structural unit represented by the following formula (1) (sometimes referred to as structural unit B). [ka] In formula (1), R 1 represents a hydrogen atom or a methyl group, L 11represents a single bond, -CO-O-, -O-CO-, or -O-; L 12 represents a single bond, -CH-, -CH-CH-, -CH-CH-CH-, -CH-CH(OH)-CH-, or -CH-CH(CHOH)-; L 13 represents a single bond, —CO—O—, —O—CO—, —O—, —CO—NH—, —NH—CO—, —CO—NH—CO—NH—, —NH—, or —N(CH3)—; L 16 is C 14~30 It should be noted that L 11 , L 12 , and L 13 In each of the horizontally written chemical formulas, the left side corresponds to the upper side of formula (1) (the main chain side of the polymer), and the right side corresponds to the lower side of formula (1) (the terminal side of the side chain of the polymer).

[0076] R 1 is preferably a hydrogen atom.

[0077] L 11 is preferably —CO—O—, —O—CO—, or —O—, more preferably —CO—O— or —O—CO—, and even more preferably —CO—O—.

[0078] L 12 is preferably a single bond, -CH2-, -CH2-CH2-, or -CH2-CH2-CH2-, more preferably a single bond.

[0079] L 13 is preferably a single bond, —O—CO—, —O—, —NH—, or —N(CH 3 )—, and more preferably a single bond.

[0080] L in Equation (1) 16 is C so that the composition containing the polymer 1 has good moldability. 14~30 C is an alkyl group. 14~30 The alkyl group of C 14~30 and C14~30 Examples of branched alkyl groups include: L 6 is preferably C 14~30 and more preferably a straight chain alkyl group of C 14~24 and more preferably C 16~22 is a straight chain alkyl group.

[0081] Said C 14~30 Examples of the straight-chain alkyl group include an n-tetradecyl group, an n-pentadecyl group, an n-hexadecyl group, an n-heptadecyl group, an n-octadecyl group, an n-nonadecyl group, an n-eicosyl group, an n-heneicosyl group, an n-docosyl group, an n-tricosyl group, an n-tetracosyl group, an n-pentacosyl group, an n-hexacosyl group, an n-heptacosyl group, an n-octacosyl group, an n-nonacosyl group, and an n-triacontyl group.

[0082] Said C 14~30 Examples of the branched alkyl group include an isotetradecyl group, an isopentadecyl group, an isohexadecyl group, an isoheptadecyl group, an isooctadecyl group, an isononadecyl group, an isoeicosyl group, an isoheneicosyl group, an isodocosyl group, an isotricosyl group, an isotetracosyl group, an isopentacosyl group, an isohexacosyl group, an isoheptacosyl group, an isooctacosyl group, an isononacosyl group, and an isotriacontyl group.

[0083] R in Equation (1) 1 , L 11 , L 12 , L 13 Examples of the combination include the following: [ka] [ka] [ka] [ka] [ka] [ka] [ka] [ka] [ka] [ka]

[0084] R in Equation (1) 1 , L 11 , L 12 , L 13 The combination is preferably: [ka] [ka] [ka]

[0085] R in Equation (1) 1 , L 11 , L 12 , L 13 The following combinations are also preferred: R 1 is a hydrogen atom, and L 11 , L 12 , and L 13 is a single bond, and L16 C 14~30 and a combination of the alkyl groups R 1 is a hydrogen atom or a methyl group, and L 11 is -CO-O-, and L 2 and L 3 is a single bond, and L 16 C 14~30 A combination of alkyl groups.

[0086] R in Equation (1) 1 , L 11 , L 12 , and L 13 The combination is more preferably: [ka]

[0087] R in Equation (1) 1 , L 11 , L 12 , and L 13 The combinations are more preferably as follows: [ka]

[0088] The structural unit B is preferably n-hexadecene, n-octadecene, n-eicosene, n-docosene, n-tetracosene, n-hexacosene, n-octacosene, n-triacontene, n-dotriacontene, n-tetradecyl acrylate, n-pentadecyl acrylate, n-hexadecyl acrylate, n-heptadecyl acrylate, n-octadecyl acrylate, n-nonadecyl acrylate, or n-eicosene. acrylate, n-heneicosyl acrylate, n-docosyl acrylate, n-tricosyl acrylate, n-tetracosyl acrylate, n-pentacosyl acrylate, n-hexacosyl acrylate, n-heptacosyl acrylate, n-octacosyl acrylate, n-nonacosyl acrylate, n-triacontyl acrylate, n-tetradecyl methacrylate, n-pentadecyl methacrylate, n-hexacosyl acrylate n-Heptadecyl methacrylate, n-Octadecyl methacrylate, n-Nonadecyl methacrylate, n-Eicosyl methacrylate, n-Heneicosyl methacrylate, n-Docosyl methacrylate, n-Tricosyl methacrylate, n-Tetracosyl methacrylate, n-Pentacosyl methacrylate, n-Hexacosyl methacrylate, n-Heptacosyl methacrylate, n-Octacosyl methacrylate, n-Nonacosyl methacrylate, n-Triacontyl methacrylate, n-Vinyltetradecylate, n-Vinylhexadecylate, n-Vinyloctadecylate, n-Vinyleicosylate, n-Vinyldocosylate, n-Tetradecyl vinyl ether, n-Hexadecyl vinyl ether, n-Octadecyl vinyl ether, n-Eicosyl vinyl ether, or n-Docosyl vinyl ether.

[0089] The polymer 1 may have two or more types of the structural unit B, and may be, for example, a polymer having a structural unit derived from n-hexadecyl acrylate and a structural unit derived from n-octadecyl acrylate.

[0090] The polymer 1 is preferably a polymer having a structural unit derived from ethylene (sometimes referred to as structural unit A) so that a molded article containing a composition containing the polymer 1 has good shape retention at or above the melting peak temperature of the polymer 1, and the composition containing the polymer 1 has good moldability. The structural unit A is a structural unit obtained by polymerizing ethylene, and the structural unit A may form a branched structure in the polymer.

[0091] The polymer 1 is preferably a polymer having a structural unit B represented by formula (1) and a structural unit A derived from ethylene.

[0092] The polymer 1 may have at least one structural unit (sometimes referred to as structural unit C) selected from the group consisting of structural units represented by the following formula (2) and structural units represented by the following formula (3). [ka] [ka] In formula (2), R 2 represents a hydrogen atom or a methyl group, L 21 represents a single bond, -CO-O-, -O-CO-, or -O-; L 24 is C 1~8 represents an alkylene group represented by the formula: L 25 is a hydrogen atom, an epoxy group, -CH(OH)-CHOH, a carboxy group, a hydroxy group, an amino group, or C 1~4 It is to be noted that L represents an alkylamino group. 1 In each of the horizontally written chemical formulas in the explanation of the chemical structure, the left side corresponds to the upper side of formula (2) (the main chain side of the polymer), and the right side corresponds to the lower side of formula (2) (the terminal side of the side chain of the polymer).

[0093] In equation (2), R 2 is preferably a hydrogen atom.

[0094] In equation (2), L 21 is preferably —CO—O—, —O—CO—, or —O—, more preferably —CO—O— or —O—CO—, and even more preferably —CO—O—.

[0095] In equation (2), L 24 C as 1~8 Examples of the alkylene group include a methylene group, an ethylene group, an n-propylene group, a 1-methylethylene group, an n-butylene group, a 1,2-dimethylethylene group, a 1,1-dimethylethylene group, a 2,2-dimethylethylene group, an n-pentylene group, an n-hexylene group, an n-heptalene group, an n-octylene group, and a 2-ethyl-n-hexylene group.

[0096] In equation (2), L 24 is preferably a methylene group, an ethylene group, or an n-propylene group, more preferably a methylene group.

[0097] In equation (2), L 25 C as 1~4 Examples of the alkylamino group include a methylamino group, an ethylamino group, a propylamino group, a butylamino group, a dimethylamino group, and a diethylamino group.

[0098] In equation (2), L 25 is preferably a hydrogen atom, an epoxy group, or CH(OH)—CHOH, and more preferably a hydrogen atom.

[0099] R in Equation (2) 2 , L 21 , L 24 , L 25 Examples of the combination include the following: [ka] [ka] [ka] [ka]

[0100] R in Equation (2) 2 , L 21 , L 24 , L 25 The combination is preferably: [ka] [ka] [ka]

[0101] R in Equation (2) 2 , L 21 , L 24 , L 25 The combination is more preferably: [ka]

[0102] R in Equation (2) 2 , L 21 , L 24 , L 25 The combinations are more preferably as follows: [ka]

[0103] Examples of the structural unit represented by formula (2) include propylene, butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, acrylic acid, methacrylic acid, vinyl alcohol, methyl acrylate, ethyl acrylate, n-propyl acrylate, isopropyl acrylate, n-butyl acrylate, isobutyl acrylate, sec-butyl acrylate, tert-butyl acrylate, methyl methacrylate, ethyl methacrylate, n-propyl methacrylate, isopropyl methacrylate, n-butyl methacrylate, isobutyl methacrylate, sec-butyl methacrylate, and tert-butyl methacrylate. The alkyl acrylates are derived from vinyl formate, vinyl acetate, vinyl propionate, vinyl(n-butylate), vinyl(isobutyrate), methyl vinyl ether, ethyl vinyl ether, n-propyl vinyl ether, isopropyl vinyl ether, n-butyl vinyl ether, isobutyl vinyl ether, sec-butyl vinyl ether, tert-butyl vinyl ether, glycidyl acrylate, glycidyl methacrylate, 2,3-dihydroxypropyl acrylate, 2,3-dihydroxypropyl methacrylate, 3-(dimethylamino)propyl acrylate, and 3-(dimethylamino)propyl methacrylate.

[0104] When polymer 1 contains structural unit C and structural unit C is represented by formula (3), the structural unit may be derived from maleic anhydride. Alternatively, structural unit C may be formed by a condensation reaction of two structural units that may be selected in combination from structural unit B and structural unit C represented by formula 2.

[0105] The polymer 1 may have two or more types of the structural unit C, and may be, for example, a polymer having a structural unit derived from methyl acrylate, a structural unit derived from ethyl acrylate, and a structural unit derived from glycidyl methacrylate.

[0106] The polymer 1 is preferably a polymer having a structural unit B represented by formula (1). Examples of the polymer 1 having the structural unit B represented by formula (1) include the following: Polymer 1 consisting of structural unit B, Polymer 1 having structural unit B and structural unit A; Polymer 1 having structural units B and C, and Polymer 1 has structural unit B, structural unit A, and structural unit C.

[0107] Examples of the "polymer 1 composed of structural unit B" include the following: L 11 , L 12 , and L 13 is a single bond, and L 16 C 14~30 A polymer comprising a structural unit B represented by formula (1), which is an alkyl group represented by the formula: L 11 -CO-O-, L 12 and L 13 is a single bond, L 16 C 14~30 A polymer comprising a structural unit B represented by formula (1), which is an alkyl group.

[0108] Examples of the "polymer 1 having structural unit B and structural unit A" include the following: R 1 is a hydrogen atom, and L 11 , L 12 , and L 13 is a single bond, and L 16 C 14~30 a polymer having a structural unit B represented by formula (1), which is an alkyl group represented by the formula: and the structural unit A, wherein the total number of the structural units A and the structural units B is 90% or more, relative to 100% of the total number of all structural units contained in the polymer; and R 1 is a hydrogen atom or a methyl group, and L 1 is -CO-O-, and L 12 and L 13 is a single bond, and L 16 C 14~30Polymer 1 has a structural unit B represented by formula (1), which is an alkyl group represented by the formula (1), and a structural unit A, and may further have the structural unit C, wherein the total number of the structural units A and the structural units B is 90% or more, relative to 100% of the total number of all structural units contained in the polymer.

[0109] From the viewpoint of increasing ΔH, polymer 1 is preferably a polymer in which the number of the structural units B accounts for 50 to 80% relative to 100% in total number of the structural units B and A contained in the polymer.

[0110] From the viewpoint of moldability, polymer 1 is preferably a polymer in which the number of structural units B is 10 to 50% relative to 100% of the total number of structural units B and A contained in the polymer.

[0111] The "polymer 1 having the structural unit B and the structural unit C" includes R 1 is a hydrogen atom or a methyl group, and L 11 is -CO-O-, and L 12 and L 13 is a single bond, and L 16 C 14~30 A structural unit B represented by formula (1) which is an alkyl group, and R 2 is a hydrogen atom or a methyl group, and L 21 is -CO-O-, and L 24 is a methylene group, and L 25 and a structural unit C represented by formula (2) in which is a hydrogen atom. In this case, the number of structural units B is preferably 80% or more relative to 100% of the total number of structural units B and C contained in the polymer.

[0112] In one embodiment of polymer 1, relative to 100% of the total number of structural units A, B, and C, the number of structural units A is typically 0 to 99%, the total number of structural units B and C is typically 1 to 100%, and relative to 100% of the total number of structural units B and C, the number of structural units B is typically 1 to 100%, and the number of structural units C is typically 0 to 99%.

[0113] In one embodiment, the number of structural units A in polymer 1 is 1 to 99% relative to the total number of structural units A, B, and C (100%), and is preferably 70 to 99%, more preferably 80 to 97.5%, and even more preferably 85 to 92.5%, so that a molded article containing the heat storage composition of the present invention has good shape retention. The total number of structural units B and C in polymer 1 is preferably 1 to 30%, more preferably 2.5 to 20%, and even more preferably 7.5 to 15%, relative to the total number of structural units A, B, and C (100%), so that a molded article containing the heat storage composition of the present invention has good shape retention.

[0114] In one embodiment, the number of structural units B in polymer 1 is typically 1 to 100%, relative to the total number of structural units B and C (100%), and is preferably 60 to 100%, and more preferably 80 to 100%, so that a composition containing polymer 1 has good heat storage performance.

[0115] In one embodiment, the number of structural units C in polymer 1 is typically 0 to 99%, relative to the total number of structural units B and C (100%), and is preferably 0 to 40%, and more preferably 0 to 20%, so that a composition containing polymer 1 has good heat storage performance.

[0116] The number of structural units A, the number of structural units B, and the number of structural units C were measured by a well-known method. 13 C nuclear magnetic resonance spectrum (hereinafter, 13 C-NMR spectrum) or 1 H nuclear magnetic resonance spectrum (hereinafter, 1 It is calculated from the integral values ​​of the signals assigned to each structural unit of the H-NMR spectrum.

[0117] When polymer 1 is produced by a method of reacting a precursor polymer P described below with a compound α described below, the number of structural units A, the number of structural units B, and the number of structural units C can be determined, for example, by the following method.

[0118] <Number of structural units A1 derived from ethylene and structural units C1 derived from methyl acrylate when precursor polymer P is an ethylene-methyl acrylate copolymer> (unit: %) When the precursor polymer P contains a structural unit A derived from ethylene, first, the number of structural units A1 and structural units C1 contained in the precursor polymer P is determined. 13 When determining from a C-NMR spectrum, for example, the integral value in the ranges of a1, b1, c1, d1, and e1 below is determined, and the number of dyads (AA, AC, CC) of structural unit A and structural unit C is determined from the formula below, and the number is determined by substituting into the formula below. Here, AA is a structural unit A-structural unit A dyad, AC is a structural unit A-structural unit C dyad, and CC is a structural unit C-structural unit C dyad.

[0119] a1:28.1-30.5ppm b1:31.9-32.6ppm c1: 41.7 ppm d1: 43.1-44.2 ppm e1:45.0-46.5ppm

[0120] AA=a1 / 4+b1 / 2 AC=e1 CC=c1+d1

[0121] <Conversion rate X of the structural unit C1 derived from methyl acrylate to the structural unit B represented by formula (1) B > (unit: %) The structural unit C contained in the precursor polymer P reacts with the compound α described below to form the structural unit B in the polymer 1, and the conversion rate X of the structural unit C1 to the structural unit B by the reaction is B is calculated by the following method.

[0122] The conversion rate is calculated by substituting the integral value (hereinafter, integral value F1) of the signal (range f1) attributed to a specific carbon contained in the side chain of structural unit C of precursor polymer P and the integral value (hereinafter, integral value G1) of the signal (range g1) attributed to a specific carbon contained in the side chain of structural unit B of polymer 1 into the following equation.

[0123] f1:50.0-51.2ppm g1: 55.0-56.8 ppm

[0124] <Number of structural units A derived from ethylene, structural units B represented by formula (1), and structural units C derived from methyl acrylate contained in polymer 1> (unit: %) In the reaction of precursor polymer P with compound α described later, the structural unit A contained in precursor polymer P does not change, so the number of structural units A contained in polymer 1 and the number of structural units A1 contained in precursor polymer P are the same (number of structural units A = number of structural units A1). The number of structural units B contained in polymer 1 is determined by multiplying the number of structural units C1 contained in precursor polymer P by the conversion rate X B (Number of constituent units B = Number of constituent units C1 × Pass-through rate X B / 100). The number of structural units C contained in polymer 1 is calculated as the difference between the number of structural units C1 contained in precursor polymer P and the number of structural units B contained in polymer 1 (number of structural units C = number of structural units C1 - number of structural units B).

[0125] The contents (% by weight) of the structural unit A, the structural unit B, and the structural unit C contained in the polymer 1 according to the present invention can each be calculated using the following formula.

[0126] Weight % of structural unit A = (Number of structural units A × Molecular weight of structural unit A) / (Number of structural units A × Molecular weight of structural unit A + Number of structural units B × Molecular weight of structural unit B + Number of structural units C × Molecular weight of structural unit C)

[0127] Weight % of structural unit B = (number of structural units B × molecular weight of structural unit B) / (number of structural units A × molecular weight of structural unit A + number of structural units B × molecular weight of structural unit B + number of structural units C × molecular weight of structural unit C)

[0128] Weight % of structural unit C = (number of structural units C × molecular weight of structural unit C) / (number of structural units A × molecular weight of structural unit A + number of structural units B × molecular weight of structural unit B + number of structural units C × molecular weight of structural unit C)

[0129] In one example, the precursor polymer P is a polymer having at least one structural unit C selected from the group consisting of structural units represented by the above formula (2) and structural units represented by the above formula (3) (wherein, in formula (2), L 21 may be —CO—O—, —O—CO—, or O—).

[0130] Compound α The compound (sometimes referred to as compound α) that reacts with the structural unit C in the precursor polymer P to form the structural unit B is at least one compound selected from the group consisting of: C 14~30 an alcohol having an alkyl group represented by the formula: C 14~30 an amine having an alkyl group represented by the formula: C 14~30 an alkyl halide having an alkyl group represented by the formula: C 14~30 a carboxylic acid having an alkyl group represented by the formula: C 14~30 a carboxylic acid amide having an alkyl group represented by the formula: C 14~30 a carboxylic acid halide having an alkyl group represented by the formula: C 14~30 Carbamic acids having an alkyl group of the formula: C 14~30 and alkyl ureas having an alkyl group of C 14~30 Isocyanates having alkyl groups of the formula:

[0131] Examples of methods for producing the polymer 1 include a method of reacting a precursor polymer P with a compound α, and a method of polymerizing each monomer corresponding to a structural unit of the polymer 1. The alkyl group of the compound α may be, for example, a linear alkyl group or a branched alkyl group, but a linear alkyl group is preferred.

[0132] The precursor polymer P is a raw material for producing polymer 1, and the precursor polymer P does not substantially contain the structural unit B represented by formula (1). The precursor polymer P may contain a structural unit that does not fall into any of structural units A, B, and C.

[0133] The precursor polymer P is preferably a polymer in which the number of structural units A is 0 to 99% and the total number of structural units C is 1 to 100%, relative to 100% in total of the structural units A and C, and more preferably a polymer in which the number of structural units A is 70 to 99% and the total number of structural units C is 1 to 30%.

[0134] Examples of methods for forming the structural unit B in the polymer 1 include reacting the structural unit C contained in the precursor polymer P with a compound α, polymerizing a monomer that serves as a raw material for the structural unit B, or copolymerizing ethylene with a monomer that serves as a raw material for the structural unit B. The alkyl group in the compound α is preferably a linear alkyl group. A polymerization initiator such as an azo compound may be used in the method of polymerizing the monomer. Examples of the azo compound include azobisisobutyronitrile.

[0135] Examples of the precursor polymer P include the following: Acrylic acid polymers, methacrylic acid polymers, vinyl alcohol polymers, methyl acrylate polymers, ethyl acrylate polymers, n-propyl acrylate polymers, n-butyl acrylate polymers, methyl methacrylate polymers, ethyl methacrylate polymers, n-propyl methacrylate polymers, n-butyl methacrylate polymers, vinyl formate polymers, vinyl acetate polymers, vinyl propionate polymers, vinyl (n-butylate) polymers, methyl vinyl ether polymers, ethyl vinyl ether polymers, n-propyl vinyl ether polymers, n-butyl vinyl ether polymers, maleic anhydride polymers, glycidyl acrylate polymers, glycidyl methacrylate polymers, 3-(dimethylamino)propyl acrylate polymers, 3-(dimethylamino)propyl methacrylate polymers, ethylene-acrylic acid copolymers, ethylene-methacrylic acid copolymers, ethylene-vinyl alcohol copolymers, ethylene-methyl acrylate copolymers, ethylene- Ethyl acrylate copolymer, ethylene-n-propyl acrylate copolymer, ethylene-n-butyl acrylate copolymer, ethylene-methyl methacrylate copolymer, ethylene-ethyl methacrylate copolymer, ethylene-n-propyl methacrylate copolymer, ethylene-n-butyl methacrylate copolymer, ethylene-vinyl formate copolymer, ethylene-vinyl acetate copolymer, ethylene-vinyl propionate copolymer, ethylene-vinyl (n-butylate) copolymer, ethylene-methyl vinyl ether copolymer, ethylene-ethyl vinyl ether copolymer, ethylene-n-propyl vinyl ether copolymer, ethylene-n-butyl vinyl ether copolymer, ethylene-maleic anhydride copolymer, ethylene-glycidyl acrylate copolymer, ethylene-glycidyl methacrylate copolymer, ethylene-3-(dimethylamino)propyl acrylate copolymer, and ethylene-3-(dimethylamino)propyl methacrylate copolymer.

[0136] Said C 14~30Examples of alcohols having a straight-chain alkyl group include n-tetradecyl alcohol, n-pentadecyl alcohol, n-hexadecyl alcohol, n-heptadecyl alcohol, n-octadecyl alcohol, n-nonadecyl alcohol, n-eicosyl alcohol, n-heneicosyl alcohol, n-docosyl alcohol, n-tricosyl alcohol, n-tetracosyl alcohol, n-pentacosyl alcohol, n-hexacosyl alcohol, n-heptacosyl alcohol, n-octacosyl alcohol, n-nonacosyl alcohol, and n-triacontyl alcohol.

[0137] Said C 14~30 Examples of alcohols having a branched alkyl group include isotetradecyl alcohol, isopentadecyl alcohol, isohexadecyl alcohol, isoheptadecyl alcohol, isooctadecyl alcohol, isononadecyl alcohol, isoeicosyl alcohol, isoheneicosyl alcohol, isodocosyl alcohol, isotricosyl alcohol, isotetracosyl alcohol, isopentacosyl alcohol, isohexacosyl alcohol, isoheptacosyl alcohol, isooctacosyl alcohol, isononacosyl alcohol, and isotriacontyl alcohol.

[0138] Said C 14~30 Examples of amines having a linear alkyl group include n-tetradecylamine, n-pentadecylamine, n-hexadecylamine, n-heptadecylamine, n-octadecylamine, n-nonadecylamine, n-eicosylamine, n-heneicosylamine, n-docosylamine, n-tricosylamine, n-tetracosylamine, n-pentacosylamine, n-hexacosylamine, n-heptacosylamine, n-octacosylamine, n-nonacosylamine, and n-triacontylamine.

[0139] Said C 14~30Examples of amines having a branched alkyl group include isotetradecylamine, isopentadecylamine, isohexadecylamine, isoheptadecylamine, isooctadecylamine, isononadecylamine, isoeicosylamine, isoheneicosylamine, isodocosylamine, isotricosylamine, isotetracosylamine, isopentacosylamine, isohexacosylamine, isoheptacosylamine, isooctacosylamine, isononacosylamine, and isotriacontylamine.

[0140] Said C 14~30 Examples of alkyl halides having a straight-chain alkyl group include n-tetradecyl iodide, n-pentadecyl iodide, n-hexadecyl iodide, n-heptadecyl iodide, n-octadecyl iodide, n-nonadecyl iodide, n-eicosyl iodide, n-heneicosyl iodide, n-docosyl iodide, n-tricosyl iodide, n-tetracosyl iodide, n-pentacosyl iodide, n-hexacosyl iodide, n-heptacosyl iodide, n-octacosyl iodide, n-nonacosyl iodide, and n-triacontyl iodide.

[0141] Said C 14~30 Examples of alkyl halides having a branched alkyl group include isotetradecyl iodide, isopentadecyl iodide, isohexadecyl iodide, isoheptadecyl iodide, isooctadecyl iodide, isononadecyl iodide, isoeicosyl iodide, isoheneicosyl iodide, isodocosyl iodide, isotricosyl iodide, isotetracosyl iodide, isopentacosyl iodide, isohexacosyl iodide, isoheptacosyl iodide, isooctacosyl iodide, isononacosyl iodide, and isotriacontyl iodide.

[0142] Said C 14~30Examples of carboxylic acids having a linear alkyl group include n-tetradecanoic acid, n-pentadecanoic acid, n-hexadecanoic acid, n-heptadecanoic acid, n-octadecanoic acid, n-nonadecanoic acid, n-eicosanoic acid, n-heneicosanoic acid, n-docosanoic acid, n-tricosanoic acid, n-tetracosanoic acid, n-pentacosanoic acid, n-hexacosanoic acid, n-heptacosanoic acid, n-octacosanoic acid, n-nonacosanoic acid, and n-triacontanoic acid.

[0143] Said C 14~30 Examples of carboxylic acids having a branched alkyl group include isotetradecanoic acid, isopentadecanoic acid, isohexadecanoic acid, isoheptadecanoic acid, isooctadecanoic acid, isononadecanoic acid, isoeicosanoic acid, isoheneicosanoic acid, isodocosanoic acid, isotricosanoic acid, isotetracosanoic acid, isopentacosanoic acid, isohexacosanoic acid, isoheptacosanoic acid, isooctacosanoic acid, isononacosanoic acid, and isotriacontanoic acid.

[0144] Said C 14~30 Examples of carboxylic acid amides having a linear alkyl group include n-tetradecanoic acid amide, n-pentadecanoic acid amide, n-hexadecanoic acid amide, n-heptadecanoic acid amide, n-octadecanoic acid amide, n-nonadecanoic acid amide, n-eicosanoic acid amide, n-heneicosanoic acid amide, n-docosanoic acid amide, n-tricosanoic acid amide, n-tetracosanoic acid amide, n-pentacosanoic acid amide, n-hexacosanoic acid amide, n-heptacosanoic acid amide, n-octacosanoic acid amide, n-nonacosanoic acid amide, and n-triacontanoic acid amide.

[0145] Said C 14~30Examples of carboxylic acid amides having a branched alkyl group include isotetradecanoic acid amide, isopentadecanoic acid amide, isohexadecanoic acid amide, isoheptadecanoic acid amide, isooctadecanoic acid amide, isononadecanoic acid amide, isoeicosanoic acid amide, isoheneicosanoic acid amide, isodocosanoic acid amide, isotricosanoic acid amide, isotetracosanoic acid amide, isopentacosanoic acid amide, isohexacosanoic acid amide, isoheptacosanoic acid amide, isooctacosanoic acid amide, isononacosanoic acid amide, and isotriacontanoic acid amide.

[0146] Said C 14~30 Examples of carboxylic acid halides having a linear alkyl group include n-tetradecanoic acid chloride, n-pentadecanoic acid chloride, n-hexadecanoic acid chloride, n-heptadecanoic acid chloride, n-octadecanoic acid chloride, n-nonadecanoic acid chloride, n-eicosanoic acid chloride, n-heneicosanoic acid chloride, n-docosanoic acid chloride, n-tricosanoic acid chloride, n-tetracosanoic acid chloride, n-pentacosanoic acid chloride, n-hexacosanoic acid chloride, n-heptacosanoic acid chloride, n-octacosanoic acid chloride, n-nonacosanoic acid chloride, and n-triacontanoic acid chloride.

[0147] Said C 14~30 Examples of carboxylic acid halides having a branched alkyl group include isotetradecanoic acid chloride, isopentadecanoic acid chloride, isohexadecanoic acid chloride, isoheptadecanoic acid chloride, isooctadecanoic acid chloride, isononadecanoic acid chloride, isoeicosanoic acid chloride, isoheneicosanoic acid chloride, isodocosanoic acid chloride, isotricosanoic acid chloride, isotetracosanoic acid chloride, isopentacosanoic acid chloride, isohexacosanoic acid chloride, isoheptacosanoic acid chloride, isooctacosanoic acid chloride, isononacosanoic acid chloride, and isotriacontanoic acid chloride.

[0148] Said C 14~30Examples of carbamic acids having a straight-chain alkyl group include n-tetradecylcarbamic acid, n-pentadecylcarbamic acid, n-hexadecylcarbamic acid, n-heptadecylcarbamic acid, n-octadecylcarbamic acid, n-nonadecylcarbamic acid, n-eicosylcarbamic acid, n-heneicosylcarbamic acid, n-docosylcarbamic acid, n-tricosylcarbamic acid, n-tetracosylcarbamic acid, n-pentacosylcarbamic acid, n-hexacosylcarbamic acid, n-heptacosylcarbamic acid, n-octacosylcarbamic acid, n-nonacosylcarbamic acid, and n-triacontylcarbamic acid.

[0149] Said C 14~30 Examples of carbamic acids having a branched alkyl group include isotetradecylcarbamic acid, isopentadecylcarbamic acid, isohexadecylcarbamic acid, isoheptadecylcarbamic acid, isooctadecylcarbamic acid, isononadecylcarbamic acid, isoeicosylcarbamic acid, isoheneicosylcarbamic acid, isodocosylcarbamic acid, isotricosylcarbamic acid, isotetracosylcarbamic acid, isopentacosylcarbamic acid, isohexacosylcarbamic acid, isoheptacosylcarbamic acid, isooctacosylcarbamic acid, isononacosylcarbamic acid, and isotriacontylcarbamic acid.

[0150] Said C 14~30 Examples of alkyl ureas having a linear alkyl group include n-tetradecyl urea, n-pentadecyl urea, n-hexadecyl urea, n-heptadecyl urea, n-octadecyl urea, n-nonadecyl urea, n-eicosyl urea, n-heneicosyl urea, n-docosyl urea, n-tricosyl urea, n-tetracosyl urea, n-pentacosyl urea, n-hexacosyl urea, n-heptacosyl urea, n-octacosyl urea, n-nonacosyl urea, and n-triacontyl urea.

[0151] Said C 14~30Examples of alkyl ureas having a branched alkyl group include isotetradecyl urea, isopentadecyl urea, isohexadecyl urea, isoheptadecyl urea, isooctadecyl urea, isononadecyl urea, isoeicosyl urea, isoheneicosyl urea, isodocosyl urea, isotricosyl urea, isotetracosyl urea, isopentacosyl urea, isohexacosyl urea, isoheptacosyl urea, isooctacosyl urea, isononacosyl urea, and isotriacontyl urea.

[0152] Said C 14~30 Examples of isocyanates having a linear alkyl group include n-tetradecyl isocyanate, n-pentadecyl isocyanate, n-hexadecyl isocyanate, n-heptadecyl isocyanate, n-octadecyl isocyanate, n-nonadecyl isocyanate, n-eicosyl isocyanate, n-heneicosyl isocyanate, n-docosyl isocyanate, n-tricosyl isocyanate, n-tetracosyl isocyanate, n-pentacosyl isocyanate, n-hexacosyl isocyanate, n-heptacosyl isocyanate, n-octacosyl isocyanate, n-nonacosyl isocyanate, and n-triacontyl isocyanate.

[0153] Said C 14~30 Examples of isocyanates having a branched alkyl group include isotetradecyl isocyanate, isopentadecyl isocyanate, isohexadecyl isocyanate, isoheptadecyl isocyanate, isooctadecyl isocyanate, isononadecyl isocyanate, isoeicosyl isocyanate, isoheneicosyl isocyanate, isodocosyl isocyanate, isotricosyl isocyanate, isotetracosyl isocyanate, isopentacosyl isocyanate, isohexacosyl isocyanate, isoheptacosyl isocyanate, isooctacosyl isocyanate, isononacosyl isocyanate, and isotriacontyl isocyanate.

[0154] When the precursor polymer P contains a structural unit A derived from ethylene, the product of the reactivity ratios r1×r2, where r1 is the reactivity ratio of ethylene used as a raw material in the production of the precursor polymer P and r2 is the reactivity ratio of the monomer that forms the structural unit C, is preferably 0.5 to 5.0, and more preferably 0.5 to 3.0, since this improves the shape retention of a molded article containing polymer 1 derived from the precursor polymer P.

[0155] The reactivity ratio r1 of ethylene is a value defined as r1 = k11 / k12, where k11 is the reaction rate at which ethylene bonds to a polymer terminated with structural unit A, and k12 is the reaction rate at which a monomer forming structural unit C bonds to a polymer terminated with structural unit A, during copolymerization of ethylene with a monomer forming structural unit C. This reactivity ratio r1 is an index that indicates whether a polymer terminated with structural unit A reacts more readily with ethylene or with the monomer forming structural unit C, during copolymerization of ethylene with a monomer forming structural unit C. The larger r1 is, the more readily a polymer terminated with structural unit A reacts with ethylene, and therefore the more easily a chain of structural unit A is formed.

[0156] The reactivity ratio r2 of the monomer that forms the structural unit C is a value defined as r2 = k22 / k21, where k21 is the reaction rate at which ethylene bonds to a polymer that has the structural unit C at its terminal, and k22 is the reaction rate at which the monomer that forms the structural unit C bonds to a polymer that has the structural unit C at its terminal, during copolymerization of ethylene with the monomer that forms the structural unit C. This reactivity ratio r2 is an index that indicates whether a polymer that has the structural unit C at its terminal reacts more readily with ethylene or the monomer that forms the structural unit C during copolymerization of ethylene with the monomer that forms the structural unit C. The larger r2 is, the more easily a polymer that has the structural unit C at its terminal reacts with the monomer that forms the structural unit C, and therefore the more easily a chain of structural units C is formed.

[0157] The product of the reactivity ratios r1 × r2 is calculated by the method described in the literature "Kakugo, M.; Naito, Y.; Mizunuma, K.; Miyatake, T. Macromolecules, 1982, 15, 1150." In the present invention, the product of the reactivity ratios r1 × r2 is calculated by the method described in the literature "Kakugo, M.; Naito, Y.; Mizunuma, K.; Miyatake, T. Macromolecules, 1982, 15, 1150." 13 It can be obtained by substituting the fractions of each of the dyads AA, AC, and CC of the structural unit A and the structural unit C calculated from the C nuclear magnetic resonance spectrum into the following formula. r1×r2=AA[CC / (AC / 2) 2 ]

[0158] The product of reactivity ratios r1 × r2 is an index that represents the monomer sequence distribution of a copolymer. The closer the product of reactivity ratios r1 × r2 is to 1, the more random the monomer sequence distribution of the copolymer. The closer the product of reactivity ratios r1 × r2 is to 0, the more alternating the monomer sequence distribution of the copolymer. The greater the product of reactivity ratios r1 × r2 is to 1, the more block the monomer sequence distribution of the copolymer.

[0159] The melt flow rate (MFR) of the precursor polymer P, measured in accordance with JIS K7210 at a temperature of 190°C and a load of 21 N, is preferably 0.1 to 500 g / 10 min or less, more preferably 1 to 100 g / 10 min or less, and even more preferably 5 to 50 g / 10 min or less.

[0160] Examples of methods for producing the precursor polymer P include coordination polymerization, cationic polymerization, anionic polymerization, and radical polymerization, with radical polymerization being preferred, and radical polymerization under high pressure being more preferred.

[0161] The temperature at which the precursor polymer P and the compound α are reacted is usually 40 to 250°C. This reaction may be carried out in the presence of a solvent. Examples of solvents include hexane, heptane, octane, nonane, decane, toluene, and xylene. If by-products are produced in this reaction, the reaction may be carried out while distilling off the by-products under reduced pressure to promote the reaction. Alternatively, the by-products may be azeotroped with the solvent, the vaporized by-products and the solvent may be cooled, the distillate containing the by-products and the solvent may be separated into a by-product layer and a solvent layer, and only the recovered solvent layer may be returned to the reaction system as a reflux liquid.

[0162] Furthermore, the reaction of the precursor polymer P with the compound α may be carried out while melt-kneading the precursor polymer P with the compound α. If by-products are generated when the precursor polymer P and the compound α are reacted while melt-kneading, the reaction may be carried out while distilling off the by-products under reduced pressure in order to promote the reaction. Examples of melt-kneading devices used for melt-kneading include single-screw extruders, twin-screw extruders, and Banbury mixers. The temperature of the melt-kneading device is preferably 100 to 250°C.

[0163] When reacting the precursor polymer P with the compound α, a catalyst may be added to promote the reaction. Examples of the catalyst include alkali metal salts and Group 4 metal complexes. Examples of alkali metal salts include alkali metal hydroxides such as lithium hydroxide, sodium hydroxide, and potassium hydroxide, and alkali metal alkoxides such as lithium methoxide and sodium methoxide. Examples of Group 4 metal complexes include tetra(isopropyl) orthotitanate, tetra(n-butyl) orthotitanate, and tetraoctadecyl orthotitanate. The amount of catalyst added is preferably 0.01 to 50 parts by weight, more preferably 0.01 to 5 parts by weight, per 100 parts by weight of the total amount of the precursor polymer P and the compound α used in the reaction.

[0164] The polymer 1 preferably contains a structural unit A derived from ethylene so that the molded article of the present invention has good shape retention at or above the peak melting temperature of the polymer 1 and the composition containing the polymer 1 has good moldability.

[0165] The polymer 1 may form a mixture with unreacted compound α or a catalyst added to promote the reaction. The content of unreacted compound α in the mixture is preferably less than 3 parts by weight based on 100 parts by weight of the polymer 1.

[0166] The polymer 1 may be a crosslinked polymer or a non-crosslinked polymer.

[0167] In one embodiment, the polymer 1 is a non-crosslinked polymer (hereinafter, also referred to as polymer α).

[0168] In one embodiment, the gel fraction of polymer α is less than 20% by weight.

[0169] Polymer α is a polymer in which the total number of the structural units A, B, and C is preferably 90% or more, more preferably 95% or more, and even more preferably 100%, relative to the total number of all structural units contained in the polymer (100%).

[0170] Crosslinking In one embodiment, the polymer 1 and / or the polymer 2 described below are crosslinked. That is, at least a portion of the molecules of the polymer 1 and the polymer 2 are linked by a covalent bond between the molecules. Note that "the polymer 1 is crosslinked" refers to either or both of the following: polymer 1 molecules are linked by a covalent bond between the molecules of the polymer 1, and polymer 1 and a polymer different from the polymer 1 (which may be polymer 2 or a polymer other than polymers 1 and 2) are linked by a covalent bond between the molecules of the polymer 1 and a polymer different from the polymer 1 (which may be polymer 2 or a polymer other than polymers 1 and 2).

[0171] Examples of methods for crosslinking a polymer include a method of crosslinking by irradiation with ionizing radiation and a method of crosslinking by using an organic peroxide.

[0172] When a polymer is irradiated with ionizing radiation to crosslink it, the polymer α, which has been previously molded into a desired shape, is usually irradiated with ionizing radiation. A known method is used for molding, and extrusion molding, injection molding, and press molding are preferred. The molded article to be irradiated with ionizing radiation may be a molded article containing only polymer 1 and polymer 2 as polymer components, or may be a molded article of a composition containing polymer 1, polymer 2, and a polymer other than these. In the latter case, examples of the polymer other than polymer 1 include the base resin described below. When the molded article contains the uncrosslinked polymer of the present invention and a base resin, the content of the uncrosslinked polymer of the present invention is preferably 1 to 99% by weight, assuming that the total amount of the uncrosslinked polymer of the present invention and the base resin is 100% by weight.

[0173] Examples of ionizing radiation include α-rays, β-rays, γ-rays, electron beams, neutron beams, and X-rays, and cobalt-60 γ-rays or electron beams are preferred. When the polymer-containing molded article is in the form of a sheet, the ionizing radiation may be irradiated from at least one side of the sheet-shaped molded article.

[0174] The irradiation with ionizing radiation is carried out using an ionizing radiation irradiation device, and the irradiation dose is usually 5 to 300 kGy, preferably 10 to 150 kGy. The polymer 1 can be obtained with a higher degree of crosslinking at a lower irradiation dose than usual.

[0175] When obtaining a polymer 1 crosslinked by irradiation with ionizing radiation, a crosslinked polymer 1 with a higher degree of crosslinking can be obtained by including a crosslinking aid in the molded article irradiated with ionizing radiation. The crosslinking aid increases the degree of crosslinking of polymer 1 and improves its mechanical properties, and a compound having multiple double bonds in the molecule is preferably used. Examples of crosslinking aids include N,N'-m-phenylene bismaleimide, toluylene bismaleimide, triallyl isocyanurate, triallyl cyanurate, p-quinone dioxime, nitrobenzene, diphenyl guanidine, divinylbenzene, ethylene glycol dimethacrylate, polyethylene glycol dimethacrylate, trimethylolpropane trimethacrylate, trimethylolpropane triacrylate, and allyl methacrylate. Furthermore, a combination of these crosslinking aids may be used.

[0176] The amount of the crosslinking aid added is preferably 0.01 to 4.0 parts by weight, more preferably 0.05 to 2.0 parts by weight, per 100 parts by weight of the total weight of the polymers contained in the molded article to be irradiated with ionizing radiation.

[0177] Examples of the crosslinking method using an organic peroxide include a method in which a composition containing the polymer α, polymer 2, and an organic peroxide is subjected to a known molding method involving heating to crosslink the polymer α. Known molding methods involving heating include extrusion molding, injection molding, and press molding.

[0178] When crosslinking is performed using an organic peroxide, an organic peroxide having a decomposition temperature equal to or higher than the flow initiation temperature of the resin component contained in the heat storage composition E is preferably used. Preferred organic peroxides include, for example, dicumyl peroxide, 2,5-dimethyl-2,5-di-tert-butylperoxyhexane, 2,5-dimethyl-2,5-di-tert-butylperoxyhexyne, α,α-di-tert-butylperoxyisopropylbenzene, and tert-butylperoxy-2-ethylhexyl carbonate.

[0179] The heat storage composition E and the composite of the present invention described below may contain known additives as needed. Examples of such additives include inorganic fillers, organic fillers, flame retardants, antioxidants, weathering agents, ultraviolet absorbers, heat stabilizers, light stabilizers, lubricants, antiblocking agents, antistatic agents, antifogging agents, anti-dripping agents, crystal nucleating agents, pigments, dyes, adsorbents, metal chlorides, hydrotalcites, aluminates, silicone compounds, antibacterial agents, deodorizers, light-absorbing heat-generating materials, moisture-absorbing heat-generating materials, and far-infrared heat-generating materials.

[0180] Compound L Compound L meets the requirements of substance A and has a molecular weight of 2000 or less.

[0181] Compound L has a melting peak temperature (highest crystalline transition temperature) within the range of 10 to 60°C, more preferably within the range of 10 to 50°C, and even more preferably within the range of 10 to 40°C.

[0182] The compound L has a melting enthalpy ΔH at 10 to 60° C. of 30 J / g or more, preferably 100 J / g or more, and more preferably 150 J / g or more.

[0183] The molecular weight of compound L is 2000 or less. Compound L may be a compound containing one or more structural units (repeating units) in the molecule, so long as the molecular weight is 2000 or less. The molecular weight of compound L is preferably 150 to 500, more preferably 150 to 400, and even more preferably 150 to 300. Compound L may be a "polymer" such as a dimer.

[0184] In one embodiment, the heat storage composition E may also contain both the polymer 1 and the compound L. In this case, the difference in temperature between the melting peak temperature of compound L and the melting peak temperature of polymer 1 contained in the composition is preferably 15°C or less, more preferably 10°C or less, and even more preferably 5°C or less.

[0185] The offset temperature of the melting curve (the intersection of the tangent to the inflection point of the melting curve on the melting end side and the baseline) is preferably 10 to 110° C., more preferably 20 to 50° C., and even more preferably 20 to 40° C. The larger the difference between the offset temperature of the melting curve and the melting peak temperature, the wider the temperature range over which the substance exhibits a heat storage effect.

[0186] Examples of the compound L include organic low-molecular-weight substances. Examples of the organic low-molecular-weight substances include paraffin, long-chain fatty acids, long-chain alcohols, long-chain fatty acid esters, and sugar alcohols. These may be encapsulated in organic microcapsules, fixed with a gelling agent, or encapsulated in a container such as a plastic.

[0187] The compound L is preferably C 14~30 C 14~30 The alkyl group of C 14~30 and C 14~30 Preferably, the branched alkyl group is C 14~30 and more preferably a straight chain alkyl group of C 14~24 and more preferably C 16~22 is a straight chain alkyl group.

[0188] Said C 14~30 Examples of the straight-chain alkyl group include an n-tetradecyl group, an n-pentadecyl group, an n-hexadecyl group, an n-heptadecyl group, an n-octadecyl group, an n-nonadecyl group, an n-eicosyl group, an n-heneicosyl group, an n-docosyl group, an n-tricosyl group, an n-tetracosyl group, an n-pentacosyl group, an n-hexacosyl group, an n-heptacosyl group, an n-octacosyl group, an n-nonacosyl group, and an n-triacontyl group.

[0189] Said C 14~30Examples of the branched alkyl group include an isotetradecyl group, an isopentadecyl group, an isohexadecyl group, an isoheptadecyl group, an isooctadecyl group, an isononadecyl group, an isoeicosyl group, an isoheneicosyl group, an isodocosyl group, an isotricosyl group, an isotetracosyl group, an isopentacosyl group, an isohexacosyl group, an isoheptacosyl group, an isooctacosyl group, an isononacosyl group, and an isotriacontyl group.

[0190] Compound L may be at least one heat storage material selected from the group consisting of hydrocarbons, fatty acids, fatty acid salts, fatty acid esters, aliphatic ethers, aliphatic ketones, aliphatic alcohols, and aliphatic amides. Furthermore, compound L may be a mixture of two or more compounds (which may be the same or different) selected from the above compounds.

[0191] The hydrocarbon is preferably a linear saturated hydrocarbon, a linear unsaturated hydrocarbon, a branched saturated hydrocarbon, or a branched unsaturated hydrocarbon, and is particularly preferably a linear saturated hydrocarbon. Examples of linear saturated hydrocarbons include n-tetradecane, n-pentadecane, n-hexadecane, n-heptadecane, n-octadecane, n-nonadecane, n-eicosane, n-heneicosane, n-docosane, n-tricosane, n-tetracosane, n-pentacosane, n-hexacosane, n-peptacosane, n-octacosane, n-nonacosane, and n-triacontane. Hydrocarbons also include various paraffin compounds.

[0192] The fatty acid is preferably a linear saturated fatty acid, a linear unsaturated fatty acid, a branched saturated fatty acid, or a branched unsaturated fatty acid, and particularly preferably a linear saturated fatty acid. Examples of linear saturated fatty acids include n-tetradecanoic acid, n-hexadecanoic acid, n-octadecanoic acid, n-eicosanoic acid, n-heneicosanoic acid, n-docosanoic acid, n-tricosanoic acid, n-tetracosanoic acid, n-pentacosanoic acid, n-hexacosanoic acid, n-heptacosanoic acid, n-octacosanoic acid, n-nonacosanoic acid, and n-triacontanoic acid.

[0193] Examples of the fatty acid salts include sodium salts, potassium salts, and ammonium salts of the fatty acids.

[0194] The fatty acid ester is preferably a linear saturated fatty acid ester, a linear unsaturated fatty acid ester, a branched saturated fatty acid ester, or a branched unsaturated fatty acid ester, and particularly preferably a linear saturated fatty acid ester. Examples of linear saturated fatty acid esters include the following: Tetradecyl n-methanoate, hexadecyl n-methanoate, octadecyl n-methanoate, eicosyl n-methanoate, docosyl n-methanoate, tetracosyl n-methanoate, hexacosyl n-methanoate, octacosyl n-methanoate, triacontyl n-methanoate; Tetradecyl n-ethanoate, hexadecyl n-ethanoate, octadecyl n-ethanoate, eicosyl n-ethanoate, docosyl n-ethanoate, tetracosyl n-ethanoate, hexacosyl n-ethanoate, octacosyl n-ethanoate, triacontyl n-ethanoate; Tetradecyl n-propanoate, hexadecyl n-propanoate, octadecyl n-propanoate, eicosyl n-propanoate, docosyl n-propanoate, tetracosyl n-propanoate, hexacosyl n-propanoate, octacosyl n-propanoate, triacontyl n-propanoate; Tetradecyl n-butanoate, hexadecyl n-butanoate, octadecyl n-butanoate, eicosyl n-butanoate, docosyl n-butanoate, tetracosyl n-butanoate, hexacosyl n-butanoate, octacosyl n-butanoate, triacontyl n-butanoate; Tetradecyl n-pentanoate, hexadecyl n-pentanoate, octadecyl n-pentanoate, eicosyl n-pentanoate, docosyl n-pentanoate, tetracosyl n-pentanoate, hexacosyl n-pentanoate, octacosyl n-pentanoate, triacontyl n-pentanoate; Tetradecyl n-hexanoate, hexadecyl n-hexanoate, octadecyl n-hexanoate, eicosyl n-hexanoate, docosyl n-hexanoate, tetracosyl n-hexanoate, hexacosyl n-hexanoate, octacosyl n-hexanoate, triacontyl n-hexanoate; Tetradecyl n-heptanoate, hexadecyl n-heptanoate, octadecyl n-heptanoate, eicosyl n-heptanoate, docosyl n-heptanoate, tetracosyl n-heptanoate, hexacosyl n-heptanoate, octacosyl n-heptanoate, triacontyl n-heptanoate; Tetradecyl n-octanoate, hexadecyl n-octanoate, octadecyl n-octanoate, eicosyl n-octanoate, docosyl n-octanoate, tetracosyl n-octanoate, hexacosyl n-octanoate, octacosyl n-octanoate, triacontyl n-octanoate; Tetradecyl n-nonanoate, hexadecyl n-nonanoate, octadecyl n-nonanoate, eicosyl n-nonanoate, docosyl n-nonanoate, tetracosyl n-nonanoate, hexacosyl n-nonanoate, octacosyl n-nonanoate, triacontyl n-nonanoate; Tetradecyl n-decanoate, hexadecyl n-decanoate, octadecyl n-decanoate, eicosyl n-decanoate, docosyl n-decanoate, tetracosyl n-decanoate, hexacosyl n-decanoate, octacosyl n-decanoate, triacontyl n-decanoate; Tetradecyl n-dodecanoate, hexadecyl n-dodecanoate, octadecyl n-dodecanoate, eicosyl n-dodecanoate, docosyl n-dodecanoate, tetracosyl n-dodecanoate, hexacosyl n-dodecanoate, octacosyl n-dodecanoate, triacontyl n-dodecanoate; Methyl n-tetradecanoate, ethyl n-tetradecanoate, propyl n-tetradecanoate, butyl n-tetradecanoate, pentyl n-tetradecanoate, hexyl n-tetradecanoate, heptyl n-tetradecanoate, octyl n-tetradecanoate, nonyl n-tetradecanoate, decyl n-tetradecanoate, dodecyl n-tetradecanoate, tetradecyl n-hexadecanoate, hexadecyl n-tetradecanoate, octadecyl n-tetradecanoate, eicosyl n-tetradecanoate, docosyl n-tetradecanoate, tetracosyl n-tetradecanoate, hexacosyl n-tetradecanoate, octacosyl n-tetradecanoate, triacontyl n-tetradecanoate; Methyl n-hexadecanoate, ethyl n-hexadecanoate, propyl n-hexadecanoate, butyl n-hexadecanoate, pentyl n-hexadecanoate, hexyl n-hexadecanoate, heptyl n-hexadecanoate, octyl n-hexadecanoate, nonyl n-hexadecanoate, decyl n-hexadecanoate, dodecyl n-hexadecanoate, tetradecyl n-hexadecanoate, hexadecyl n-hexadecanoate, octadecyl n-hexadecanoate, eicosyl n-hexadecanoate, docosyl n-hexadecanoate, tetracosyl n-hexadecanoate, hexacosyl n-hexadecanoate, octacosyl n-hexadecanoate, triacontyl n-hexadecanoate; Methyl n-octadecanoate, ethyl n-octadecanoate, propyl n-octadecanoate, butyl n-octadecanoate, pentyl n-octadecanoate, hexyl n-octadecanoate, heptyl n-octadecanoate, octyl n-octadecanoate, nonyl n-octadecanoate, decyl n-octadecanoate, dodecyl n-octadecanoate, tetradecyl n-octadecanoate, hexadecyl n-octadecanoate, octadecyl n-octadecanoate, eicosyl n-octadecanoate, docosyl n-octadecanoate, tetracosyl n-octadecanoate, hexacosyl n-octadecanoate, octacosyl n-octadecanoate, triacontyl n-octadecanoate; Methyl n-eicosanoate, ethyl n-eicosanoate, propyl n-eicosanoate, butyl n-eicosanoate, pentyl n-eicosanoate, hexyl n-eicosanoate, heptyl n-eicosanoate, octyl n-eicosanoate, nonyl n-eicosanoate, decyl n-eicosanoate, dodecyl n-eicosanoate, tetradecyl n-eicosanoate, hexadecyl n-eicosanoate, octadecyl n-eicosanoate, eicosyl n-eicosanoate, docosyl n-eicosanoate, tetracosyl n-eicosanoate, hexacosyl n-eicosanoate, octacosyl n-eicosanoate, triacontyl n-eicosanoate; Methyl n-docosanoate, ethyl n-docosanoate, propyl n-docosanoate, butyl n-docosanoate, pentyl n-docosanoate, hexyl n-docosanoate, heptyl n-docosanoate, octyl n-docosanoate, nonyl n-docosanoate, decyl n-docosanoate, dodecyl n-docosanoate, tetradecyl n-docosanoate, hexadecyl n-docosanoate, octadecyl n-docosanoate, eicosyl n-docosanoate, docosyl n-docosanoate, tetracosyl n-docosanoate, hexacosyl n-docosanoate, octacosyl n-docosanoate, triacontyl n-docosanoate; Methyl n-tetracosanoate, ethyl n-tetracosanoate, propyl n-tetracosanoate, butyl n-tetracosanoate, pentyl n-tetracosanoate, hexyl n-tetracosanoate, heptyl n-tetracosanoate, octyl n-tetracosanoate, nonyl n-tetracosanoate, decyl n-tetracosanoate, dodecyl n-tetracosanoate, tetradecyl n-tetracosanoate, hexadecyl n-tetracosanoate, octadecyl n-tetracosanoate, eicosyl n-tetracosanoate, docosyl n-tetracosanoate, tetracosyl n-tetracosanoate, hexacosyl n-tetracosanoate, octacosyl n-tetracosanoate, triacontyl n-tetracosanoate; Methyl n-hexacosanoate, ethyl n-hexacosanoate, propyl n-hexacosanoate, butyl n-hexacosanoate, pentyl n-hexacosanoate, hexyl n-hexacosanoate, heptyl n-hexacosanoate, octyl n-hexacosanoate, nonyl n-hexacosanoate, decyl n-hexacosanoate, dodecyl n-hexacosanoate, tetradecyl n-hexacosanoate, hexadecyl n-hexacosanoate, octadecyl n-hexacosanoate, eicosyl n-hexacosanoate, docosyl n-hexacosanoate, tetracosyl n-hexacosanoate, hexacosyl n-hexacosanoate, octacosyl n-hexacosanoate, triacontyl n-hexacosanoate; Methyl n-octacosanoate, ethyl n-octacosanoate, propyl n-octacosanoate, butyl n-octacosanoate, pentyl n-octacosanoate, hexyl n-octacosanoate, heptyl n-octacosanoate, octyl n-octacosanoate, nonyl n-octacosanoate, decyl n-octacosanoate, dodecyl n-octacosanoate, tetradecyl n-octacosanoate, hexadecyl n-octacosanoate, octadecyl n-octacosanoate, eicosyl n-octacosanoate, docosyl n-octacosanoate, tetracosyl n-octacosanoate, hexacosyl n-octacosanoate, octacosyl n-octacosanoate, triacontyl n-octacosanoate; Methyl n-triacontanoate, ethyl n-triacontanoate, propyl n-triacontanoate, butyl n-triacontanoate, pentyl n-triacontanoate, hexyl n-triacontanoate, heptyl n-triacontanoate, octyl n-triacontanoate, nonyl n-triacontanoate, decyl n-triacontanoate, dodecyl n-triacontanoate, tetradecyl n-triacontanoate, hexadecyl n-triacontanoate, octadecyl n-triacontanoate, eicosyl n-triacontanoate, docosyl n-triacontanoate, tetracosyl n-triacontanoate, hexacosyl n-triacontanoate, octacosyl n-triacontanoate, triacontyl n-triacontanoate.

[0195] Furthermore, compounds in which multiple fatty acid esters are bonded, such as triacylglycerol, may also be used.

[0196] The aliphatic ether is preferably a linear saturated aliphatic ether, a linear unsaturated aliphatic ether, a branched saturated aliphatic ether, or a branched unsaturated aliphatic ether, and particularly preferably a linear saturated aliphatic ether. Examples of linear saturated aliphatic ethers include: n-tetradecyl methyl ether, n-tetradecyl ethyl ether, n-tetradecyl propyl ether, n-tetradecyl butyl ether, n-tetradecyl pentyl ether, n-tetradecyl hexyl ether, n-tetradecyl heptyl ether, n-tetradecyl octyl ether, n-tetradecyl nonyl ether, n-tetradecyl decyl ether, n-tetradecyl dodecyl ether, n-ditetradecyl ether, n-tetradecyl hexadecyl ether, n-tetradecyl octadecyl ether, n-tetradecyl eicosyl ether, n-tetradecyl docosyl ether, n-tetradecyl tetracosyl ether, n-tetradecyl hexacosyl ether, n-tetradecyl octacosyl ether, n-tetradecyl triacontyl ether; n-Hexadecyl methyl ether, n-hexadecyl ethyl ether, n-hexadecyl propyl ether, n-hexadecyl butyl ether, n-hexadecyl pentyl ether, n-hexadecyl hexyl ether, n-hexadecyl heptyl ether, n-hexadecyl octyl ether, n-hexadecyl nonyl ether, n-hexadecyl decyl ether, n-hexadecyl dodecyl ether, n-dihexadecyl ether, n-hexadecyl octadecyl ether, n-hexadecyl eicosyl ether, n-hexadecyl docosyl ether, n-hexadecyl tetracosyl ether, n-hexadecyl hexacosyl ether, n-hexadecyl octacosyl ether, n-hexadecyl triacontyl ether: n-Octadecyl methyl ether, n-octadecyl ethyl ether, n-octadecyl propyl ether, n-octadecyl butyl ether, n-octadecyl pentyl ether, n-octadecyl hexyl ether, n-octadecyl heptyl ether, n-octadecyl octyl ether, n-octadecyl nonyl ether, n-octadecyl decyl ether, n-octadecyl dodecyl ether, n-dioctadecyl ether, n-octadecyl eicosyl ether, n-octadecyl docosyl ether, n-octadecyl tetracosyl ether, n-octadecyl hexacosyl ether, n-octadecyl octacosyl ether, n-octadecyl triacontyl ether; n-eicosyl methyl ether, n-eicosyl ethyl ether, n-eicosyl propyl ether, n-eicosyl butyl ether, n-eicosyl pentyl ether, n-eicosyl hexyl ether, n-eicosyl heptyl ether, n-eicosyl octyl ether, n-eicosyl nonyl ether, n-eicosyl decyl ether, n-eicosyl dodecyl ether, n-dieicosyl ether, n-eicosyl docosyl ether, n-eicosyl tetracosyl ether, n-eicosyl hexacosyl ether, n-eicosyl octacosyl ether, n-eicosyl triacontyl ether; n-docosyl methyl ether, n-docosyl ethyl ether, n-docosyl propyl ether, n-docosyl butyl ether, n-docosyl pentyl ether, n-docosyl hexyl ether, n-docosyl heptyl ether, n-docosyl octyl ether, n-docosyl nonyl ether, n-docosyl decyl ether, n-docosyl dodecyl ether, n-didocosyl ether, n-docosyl tetracosyl ether, n-docosyl hexacosyl ether, n-docosyl octacosyl ether, n-docosyl triacontyl ether; n-tetracosyl methyl ether, n-tetracosyl ethyl ether, n-tetracosyl propyl ether, n-tetracosyl butyl ether, n-tetracosyl pentyl ether, n-tetracosyl hexyl ether, n-tetracosyl heptyl ether, n-tetracosyl octyl ether, n-tetracosyl nonyl ether, n-tetracosyl decyl ether, n-tetracosyl dodecyl ether, n-ditetracosyl ether, n-tetracosyl hexacosyl ether, n-tetracosyl octacosyl ether, n-tetracosyl triacontyl ether; n-Hexacosyl methyl ether, n-hexacosyl ethyl ether, n-hexacosyl propyl ether, n-hexacosyl butyl ether, n-hexacosyl pentyl ether, n-hexacosyl hexyl ether, n-hexacosyl heptyl ether, n-hexacosyl octyl ether, n-hexacosyl nonyl ether, n-hexacosyl decyl ether, n-hexacosyl dodecyl ether, n-dihexacosyl ether, n-hexacosyl octacosyl ether, n-hexacosyl triacontyl ether; n-Octacosyl methyl ether, n-Octacosyl ethyl ether, n-Octacosyl propyl ether, n-Octacosyl butyl ether, n-Octacosyl pentyl ether, n-Octacosyl hexyl ether, n-Octacosyl heptyl ether, n-Octacosyl octyl ether, n-Octacosyl nonyl ether, n-Octacosyl decyl ether, n-Octacosyl dodecyl ether, n-Dioctacosyl ether, n-Octacosyl triacontyl ether; n-triacontyl methyl ether, n-triacontyl ethyl ether, n-triacontyl propyl ether, n-triacontyl butyl ether, n-triacontyl pentyl ether, n-triacontyl hexyl ether, n-triacontyl heptyl ether, n-triacontyl octyl ether, n-triacontyl nonyl ether, n-triacontyl decyl ether, n-triacontyl dodecyl ether, n-ditriacontyl ether.

[0197] The aliphatic ketone is preferably a linear saturated aliphatic ketone, a linear unsaturated aliphatic ketone, a branched saturated aliphatic ketone, or a branched unsaturated aliphatic ketone, and particularly preferably a linear saturated aliphatic ketone. Examples of linear saturated aliphatic ketones include: n-Tetradecyl methyl ketone, n-tetradecyl ethyl ketone, n-tetradecyl propyl ketone, n-tetradecyl butyl ketone, n-tetradecyl pentyl ketone, n-tetradecyl hexyl ketone, n-tetradecyl heptyl ketone, n-tetradecyl octyl ketone, n-tetradecyl nonyl ketone, n-tetradecyl decyl ketone, n-tetradecyl dodecyl ketone, n-ditetradecyl ketone, n-tetradecyl hexadecyl ketone, n-tetradecyl octadecyl ketone, n-tetradecyl eicosyl ketone, n-tetradecyl docosyl ketone, n-tetradecyl tetracosyl ketone, n-tetradecyl hexacosyl ketone, n-tetradecyl octacosyl ketone, n-tetradecyl triacontyl ketone; n-Hexadecyl methyl ketone, n-hexadecyl ethyl ketone, n-hexadecyl propyl ketone, n-hexadecyl butyl ketone, n-hexadecyl pentyl ketone, n-hexadecyl hexyl ketone, n-hexadecyl heptyl ketone, n-hexadecyl octyl ketone, n-hexadecyl nonyl ketone, n-hexadecyl decyl ketone, n-hexadecyl dodecyl ketone, n-dihexadecyl ketone, n-hexadecyl octadecyl ketone, n-hexadecyl eicosyl ketone, n-hexadecyl docosyl ketone, n-hexadecyl tetracosyl ketone, n-hexadecyl hexacosyl ketone, n-hexadecyl octacosyl ketone, n-hexadecyl triacontyl ketone; n-Octadecyl methyl ketone, n-octadecyl ethyl ketone, n-octadecyl propyl ketone, n-octadecyl butyl ketone, n-octadecyl pentyl ketone, n-octadecyl hexyl ketone, n-octadecyl heptyl ketone, n-octadecyl octyl ketone, n-octadecyl nonyl ketone, n-octadecyl decyl ketone, n-octadecyl dodecyl ketone, n-dioctadecyl ketone, n-octadecyl eicosyl ketone, n-octadecyl docosyl ketone, n-octadecyl tetracosyl ketone, n-octadecyl hexacosyl ketone, n-octadecyl octacosyl ketone, n-octadecyl triacontyl ketone; n-Eicosyl methyl ketone, n-Eicosyl ethyl ketone, n-Eicosyl propyl ketone, n-Eicosyl butyl ketone, n-Eicosyl pentyl ketone, n-Eicosyl hexyl ketone, n-Eicosyl heptyl ketone, n-Eicosyl octyl ketone, n-Eicosyl nonyl ketone, n-Eicosyl decyl ketone, n-Eicosyl dodecyl ketone, n-Diicosyl ketone, n-Eicosyl docosyl ketone, n-Eicosyl tetracosyl ketone, n-Eicosyl hexacosyl ketone, n-Eicosyl octacosyl ketone, n-Eicosyl triacontyl ketone; n-docosyl methyl ketone, n-docosyl ethyl ketone, n-docosyl propyl ketone, n-docosyl butyl ketone, n-docosyl pentyl ketone, n-docosyl hexyl ketone, n-docosyl heptyl ketone, n-docosyl octyl ketone, n-docosyl nonyl ketone, n-docosyl decyl ketone, n-docosyl dodecyl ketone, n-didocosyl ketone, n-docosyl tetracosyl ketone, n-docosyl hexacosyl ketone, n-docosyl octacosyl ketone, n-docosyl triacontyl ketone; n-Tetracosyl methyl ketone, n-tetracosyl ethyl ketone, n-tetracosyl propyl ketone, n-tetracosyl butyl ketone, n-tetracosyl pentyl ketone, n-tetracosyl hexyl ketone, n-tetracosyl heptyl ketone, n-tetracosyl octyl ketone, n-tetracosyl nonyl ketone, n-tetracosyl decyl ketone, n-tetracosyl dodecyl ketone, n-ditetracosyl ketone, n-tetracosyl hexacosyl ketone, n-tetracosyl octacosyl ketone, n-tetracosyl triacontyl ketone; n-Hexacosyl methyl ketone, n-hexacosyl ethyl ketone, n-hexacosyl propyl ketone, n-hexacosyl butyl ketone, n-hexacosyl pentyl ketone, n-hexacosyl hexyl ketone, n-hexacosyl heptyl ketone, n-hexacosyl octyl ketone, n-hexacosyl nonyl ketone, n-hexacosyl decyl ketone, n-hexacosyl dodecyl ketone, n-dihexacosyl ketone, n-hexacosyl octacosyl ketone, n-hexacosyl triacontyl ketone; n-Octacosyl methyl ketone, n-Octacosyl ethyl ketone, n-Octacosyl propyl ketone, n-Octacosyl butyl ketone, n-Octacosyl pentyl ketone, n-Octacosyl hexyl ketone, n-Octacosyl heptyl ketone, n-Octacosyl octyl ketone, n-Octacosyl nonyl ketone, n-Octacosyl decyl ketone, n-Octacosyl dodecyl ketone, n-Dioctacosyl ketone, n-Octacosyl triacontyl ketone; n-triacontyl methyl ketone, n-triacontyl ethyl ketone, n-triacontyl propyl ketone, n-triacontyl butyl ketone, n-triacontyl pentyl ketone, n-triacontyl hexyl ketone, n-triacontyl heptyl ketone, n-triacontyl octyl ketone, n-triacontyl nonyl ketone, n-triacontyl decyl ketone, n-triacontyl dodecyl ketone, n-ditriacontyl ketone.

[0198] The aliphatic alcohol is preferably a linear saturated aliphatic alcohol, a linear unsaturated aliphatic alcohol, a branched saturated aliphatic alcohol, or a branched unsaturated aliphatic alcohol, and particularly preferably a linear saturated aliphatic alcohol. Examples of linear saturated aliphatic alcohols include n-tetradecyl alcohol, n-pentadecyl alcohol, n-hexadecyl alcohol, n-heptadecyl alcohol, n-octadecyl alcohol, n-nonadecyl alcohol, n-eicosyl alcohol, n-heneicosyl alcohol, n-docosyl alcohol, n-tricosyl alcohol, n-tetracosyl alcohol, n-pentacosyl alcohol, n-hexacosyl alcohol, n-heptacosyl alcohol, n-octacosyl alcohol, n-nonacosyl alcohol, and n-triacontyl alcohol.

[0199] The aliphatic amide is preferably a linear saturated aliphatic amide, a linear unsaturated aliphatic amide, a branched saturated aliphatic amide, or a branched unsaturated aliphatic amide, and particularly preferably a linear saturated aliphatic amide. Examples of linear saturated aliphatic amides include n-tetradecylamine, n-pentadecylamine, n-hexadecylamine, n-heptadecylamine, n-octadecylamine, n-nonadecylamine, n-eicosylamine, n-heneicosylamine, n-docosylamine, n-tricosylamine, n-tetracosylamine, n-pentacosylamine, n-hexacosylamine, n-heptacosylamine, n-octacosylamine, n-nonacosylamine, and n-triacontylamine.

[0200] In one embodiment, in order to further suppress bleeding of compound L, compound L may be contained in heat storage composition E in a form encapsulated in microcapsules, or may be contained in heat storage composition E in a form filled in porous microparticles.

[0201] In one embodiment, the microcapsules containing compound L encapsulate compound L and have a coating containing a resin as an outer shell. Examples of materials for forming the coating include thermoplastic resins and thermosetting resins. Specific examples of resins for forming the coating include melamine resins, acrylic resins, urethane resins, nylon resins, and olefin resins. The material for forming the coating is preferably a resin that is not destroyed when producing the thermal storage composition E containing microcapsules containing compound L and polymer 1, or when producing a molded article containing the thermal storage composition E. In one embodiment, the average primary particle diameter of the microcapsules containing compound L (hereinafter sometimes referred to as primary particles) is preferably 0.2 to about 1000 μm, more preferably 0.2 to 500 μm. In another embodiment, the microcapsules having an average primary particle diameter of 0.2 to 50 μm, more preferably 0.2 to 10 μm, aggregate to form secondary particles, and the average particle diameter (average secondary particle diameter) of the secondary particles is preferably 10 to about 1000 μm, more preferably 50 to 500 μm. Examples of microcapsules containing paraffins as compound L include Micronal 5001 X (manufactured by BASF) and Rikenresin PMCD-25SP (manufactured by Miki Riken Kogyo Co., Ltd.).

[0202] As used herein, "porous microparticles" refers to microparticles containing an inorganic or organic substance and having pores penetrating from the surface to the interior. The porous microparticles may be hollow microparticles having internal cavities, or may be microparticles without cavities. Examples of porous microparticles containing inorganic substances include those containing metal oxides such as silica and alumina, silicates such as calcium silicate and magnesium silicate, carbonates such as calcium carbonate and magnesium carbonate, and phosphates such as magnesium phosphate and apatite. Examples of porous microparticles containing organic substances include foams containing various resins such as polyethylene and polyurethane, and expanded graphite. From the viewpoints of mechanical strength and chemical stability, porous microparticles containing inorganic substances are preferred. Furthermore, porous silica is more preferred because many microparticles with uniform particle sizes are commercially available and easily available. The particle size of the porous microparticles is preferably 0.2 μm to 500 μm, more preferably 0.2 μm to 300 μm.

[0203] When the porous fine particles contain an inorganic substance, the surfaces of the porous fine particles may be coated with a resin layer, for example, reactive resins such as melamine resin, acrylic resin, and urethane resin, and thermoplastic resins such as nylon resin and polyolefin resin.

[0204] The porous microparticles filled with compound L may be those in which a component that acts as a capture substance for compound L has been introduced into the porous microparticles, and compound L has been captured by the capture substance. For example, when compound L is paraffin and the porous microparticles are silica, examples of the capture substance include substances having affinity for paraffin, such as oligomers or polymers of polyisobutylene, polyoxypropylene, polyacrylate, polyether polyol, and polymethacrylate, to which reactive silyl groups that have affinity and reactivity with silica and are reactive groups that bond to each other are bonded.

[0205] Polymer 2 The heat storage composition E contains the substance A and a base resin (sometimes referred to as polymer 2) having a melting peak temperature or glass transition temperature between 60 and 120°C.

[0206] In one embodiment, the melting peak temperature or glass transition temperature of polymer 2 is preferably 60 to 120°C, more preferably 70 to 110°C.

[0207] The heat storage composition E may contain two or more types of polymers 2.

[0208] Examples of polymer 2 having a melting peak temperature in the range of 60 to 120°C include high-pressure low-density polyethylene (LDPE), ethylene-α-olefin copolymer, and ethylene-vinyl acetate copolymer (EVA).

[0209] Examples of polymer 2 having a glass transition temperature in the range of 60 to 120°C include cyclic olefin polymer (COP), cyclic olefin copolymer (COC), polystyrene (PS), polyvinyl chloride (PVC), acrylonitrile-styrene copolymer (AS), acrylonitrile-butadiene-styrene copolymer (ABS), polymethyl methacrylate (PMMA), polyvinyl alcohol (PVA), polyethylene terephthalate (PET), polyacrylonitrile (PAN), polyamide 6 (PA6), polyamide 66 (PA66), polycarbonate (PC), polyphenylene sulfide (PPS), and polyether ether ketone (PEEK).

[0210] The ethylene-α-olefin copolymer as polymer 2 is a copolymer having structural units derived from ethylene and structural units derived from an α-olefin. Examples of the α-olefin include propylene, 1-butene, 1-pentene, 1-hexene, 1-heptene, 1-octene, 4-methyl-1-pentene, and 4-methyl-1-hexene, and these may be used alone or in combination of two or more. The α-olefin is preferably C 4~8 and more preferably 1-butene, 1-hexene, or 1-octene.

[0211] The density of high-pressure low-density polyethylene (LDPE) and ethylene-α-olefin copolymer as polymer 2 is 860 to 960 kg / m 3 is.

[0212] In one embodiment, polymer 2 has structural unit A and structural unit C, where structural unit A and structural unit C are as described for polymer 1. Polymer 2 is preferably a polymer in which the number of structural units A is 0 to 99% and the total number of structural units C is 1 to 100%, relative to 100% in total of structural units A and structural units C, and more preferably a polymer in which the number of structural units A is 70 to 99% and the total number of structural units C is 1 to 30%.

[0213] Examples of polymer 2 include the following: Acrylic acid polymers, methacrylic acid polymers, vinyl alcohol polymers, methyl acrylate polymers, ethyl acrylate polymers, n-propyl acrylate polymers, n-butyl acrylate polymers, methyl methacrylate polymers, ethyl methacrylate polymers, n-propyl methacrylate polymers, n-butyl methacrylate polymers, vinyl formate polymers, vinyl acetate polymers, vinyl propionate polymers, vinyl (n-butylate) polymers, methyl vinyl ether polymers, ethyl vinyl ether polymers, n-propyl vinyl ether polymers, n-butyl vinyl ether polymers, maleic anhydride polymers, glycidyl acrylate polymers, glycidyl methacrylate polymers, 3-(dimethylamino)propyl acrylate polymers, 3-(dimethylamino)propyl methacrylate polymers, ethylene-acrylic acid copolymers, ethylene-methacrylic acid copolymers, ethylene-vinyl alcohol copolymers, ethylene-methyl acrylate copolymers, ethylene- Ethyl acrylate copolymer, ethylene-n-propyl acrylate copolymer, ethylene-n-butyl acrylate copolymer, ethylene-methyl methacrylate copolymer, ethylene-ethyl methacrylate copolymer, ethylene-n-propyl methacrylate copolymer, ethylene-n-butyl methacrylate copolymer, ethylene-vinyl formate copolymer, ethylene-vinyl acetate copolymer, ethylene-vinyl propionate copolymer, ethylene-vinyl (n-butylate) copolymer, ethylene-methyl vinyl ether copolymer, ethylene-ethyl vinyl ether copolymer, ethylene-n-propyl vinyl ether copolymer, ethylene-n-butyl vinyl ether copolymer, ethylene-maleic anhydride copolymer, ethylene-glycidyl acrylate copolymer, ethylene-glycidyl methacrylate copolymer, ethylene-3-(dimethylamino)propyl acrylate copolymer, and ethylene-3-(dimethylamino)propyl methacrylate copolymer. Preferably, polymer 2 is an ethylene-based copolymer. Examples of the ethylene-based copolymer include an ethylene-unsaturated carboxylic acid copolymer, an ethylene-vinyl alcohol copolymer, an ethylene-unsaturated carboxylic acid ester copolymer, an ethylene-vinyl carboxylate copolymer, and an ethylene-alkyl vinyl ether copolymer. Examples of the ethylene-unsaturated carboxylic acid copolymer include ethylene-acrylic acid copolymer, ethylene-methacrylic acid copolymer, and ethylene-maleic anhydride copolymer. Examples of ethylene-unsaturated carboxylic acid ester copolymers include ethylene-methyl acrylate copolymer, ethylene-ethyl acrylate copolymer, ethylene-n-propyl acrylate copolymer, ethylene-n-butyl acrylate copolymer, ethylene-methyl methacrylate copolymer, ethylene-ethyl methacrylate copolymer, ethylene-n-propyl methacrylate copolymer, ethylene-n-butyl methacrylate copolymer, ethylene-glycidyl acrylate copolymer, ethylene-glycidyl methacrylate copolymer, ethylene-3-(dimethylamino)propyl acrylate copolymer, and ethylene-3-(dimethylamino)propyl methacrylate copolymer. Examples of ethylene-vinyl carboxylate copolymers include ethylene-vinyl formate copolymer, ethylene-vinyl acetate copolymer, ethylene-vinyl propionate copolymer, and ethylene-vinyl (n-butylate) copolymer.

[0214] Polymer 2 is more preferably an ethylene-unsaturated carboxylic acid copolymer or an ethylene-unsaturated carboxylic acid ester copolymer, and even more preferably an ethylene-acrylic acid copolymer, ethylene-methacrylic acid copolymer, ethylene-vinyl alcohol copolymer, ethylene-methyl acrylate copolymer, ethylene-ethyl acrylate copolymer, ethylene-n-propyl acrylate copolymer, ethylene-n-butyl acrylate copolymer, ethylene-methyl methacrylate copolymer, ethylene-ethyl methacrylate copolymer, ethylene-n-propyl methacrylate copolymer, or ethylene-n-butyl methacrylate copolymer.

[0215] From the viewpoint of moldability, the polymer 2 preferably has a melt flow rate (MFR) of 0.1 to 100 g / 10 min, more preferably 0.1 to 30 g / 10 min, as measured in accordance with JIS K7210 at a temperature of 190° C. and a load of 21 N.

[0216] The amount of ethylene structural units in the ethylene copolymer resin is preferably 50 to 99% by weight.

[0217] The heat storage composition E may be molded into any shape. When the heat storage composition E is extrusion molded, injection molded, vacuum molded, blow molded, or roll molded, from the viewpoint of moldability, the melt flow rate (MFR) of the heat storage composition E measured in accordance with JIS K7210 at 230°C under a load of 2.16 kgf is preferably 0.1 to 30 g / 10 min.

[0218] When the heat storage composition E is spun into fibers as described below, the melt flow rate (MFR) of the heat storage composition E measured in accordance with JIS K7210 at 230°C under a load of 2.16 kgf is preferably 0.1 to 1000 g / 10 min, more preferably 10 to 500 g / 10 min, and even more preferably 20 to 100 g / 10 min.

[0219] When the heat storage composition E is spun into fibers as described below, the shear rate is measured at 270°C and 1.216 x 10 3 sec -1 The shear viscosity η at 100 Pa·s is preferably 3 to 100 Pa·s, more preferably 4 to 80 Pa·s, and even more preferably 5 to 60 Pa·s.

[0220] When the heat storage composition E contains an additive, the additive may be pre-blended with one or more raw materials used in the manufacturing process of the heat storage composition E, or may be blended after the heat storage composition E is manufactured. When the production process includes a step of crosslinking a polymer, the additive may be blended into the polymer before or after crosslinking. When an additive is to be blended into the heat storage composition E after the heat storage composition E has been produced, the additive can be blended into the heat storage composition E while the composition is being melt-kneaded.

[0221] The amount of these additives to be added is preferably 0.001 to 10 parts by weight, more preferably 0.005 to 5 parts by weight, and even more preferably 0.01 to 1 part by weight, relative to 100 parts by weight of the heat storage composition E.

[0222] Inorganic fillers include, for example, talc, calcium carbonate, and calcined kaolin.

[0223] Organic fillers include, for example, fibers, wood flour, and cellulose powder.

[0224] Examples of antioxidants include phenol-based antioxidants, sulfur-based antioxidants, phosphorus-based antioxidants, lactone-based antioxidants, and vitamin-based antioxidants.

[0225] Examples of the ultraviolet absorber include benzotriazole-based ultraviolet absorbers, tridiamine-based ultraviolet absorbers, anilide-based ultraviolet absorbers, and benzophenone-based ultraviolet absorbers.

[0226] Examples of the light stabilizer include hindered amine light stabilizers and benzoate light stabilizers.

[0227] Examples of pigments include titanium dioxide and carbon black.

[0228] Adsorbents include, for example, metal oxides such as zinc oxide and magnesium oxide.

[0229] Metal chlorides include, for example, iron chloride and calcium chloride.

[0230] Lubricants include, for example, fatty acids, higher alcohols, fatty amides, and fatty esters.

[0231] The heat storage composition E may be produced by melt-kneading the phase-change substance A and the polymer 2, and, if necessary, other additives, etc., in advance to prepare a high-concentration masterbatch, and then adding the phase-change substance A and / or the polymer 2 and melt-kneading the mixture to produce the composition.

[0232] The heat storage composition E may be produced by simply mixing the phase change material A and the polymer 2, and if necessary, other additives, etc.; by dissolving the phase change material A in a solvent and then mixing the polymer 2 and if necessary, other additives, etc.; by dissolving the polymer 2 in a solvent and then mixing the phase change material A and if necessary, other additives, etc.; by mixing the phase change material A and the polymer 2 with a solvent or a solution in which if necessary, other additives, etc. are dissolved in the solvent; or by mixing a solution in which the phase change material A is dissolved in a solvent with a solution in which the polymer 2 and if necessary, other additives, etc. are dissolved in the solvent.

[0233] The heat storage composition E may be produced by first simply mixing the phase change material A and the polymer 2, and, if necessary, other additives, or mixing them after dissolving them in a solvent, to prepare a high-concentration master batch, and then adding the phase change material A or the polymer 2, either as is or after dissolving it in a solvent if necessary, and mixing them.

[0234] The heat storage composition E may be produced by mixing a monomer or prepolymer of polymer 1, a monomer or prepolymer of polymer 2, and, if necessary, other additives, and may be produced by further polymerizing the mixture. Examples of polymerization methods include bulk polymerization, cast polymerization, solution polymerization, suspension polymerization, and emulsion polymerization.

[0235] The heat storage composition E obtained by the above method can be used as a raw material to produce a polymer and a molded article.

[0236] Molded body By molding the heat storage composition E, a molded article containing the composition can be produced.

[0237] The method for molding the heat storage composition E is not particularly limited, and examples thereof include injection molding, extrusion molding, vacuum molding, pressure molding, press molding, transfer molding, cast molding, compression molding, laminate molding, inflation molding, calendar molding, blow molding, hollow molding, two-color molding, foam molding, insert molding, in-mold coating molding, rotational molding, hand layup molding, spray-up molding, matched die molding, vacuum injection molding, filament winding molding, centrifugal molding, and pultrusion molding.

[0238] Examples of the molded article of the present invention include injection molded articles, extrusion molded articles, vacuum molded articles, pressure molded articles, press molded articles, transfer molded articles, cast molded articles, compression molded articles, laminate molded articles, inflation molded articles, calendar molded articles, blow molded articles, hollow molded articles, two-color molded articles, foam molded articles, insert molded articles, in-mold coating molded articles, rotational molded articles, hand lay-up molded articles, spray-up molded articles, matched die molded articles, vacuum injection molded articles, filament winding molded articles, centrifugal molded articles, pultrusion molded articles, sheets, films, etc. The molded article may have a single layer structure or a multilayer structure.

[0239] The molded article of the present invention may be a multilayer structure comprising a layer of the composition of the present invention and a layer other than the layer. Examples of materials constituting the layer other than the layer of the composition of the present invention include resins, metals, paper, leather, etc. other than the composition of the present invention. The multilayer structure can be produced by laminating a layer of the composition of the present invention and a layer other than the layer.

[0240] Since the heat storage composition E has excellent moldability and shape retention, it can be in any shape, such as a spherical, angular (cubic), bead-like, cylindrical (pellet-like), powder, rod-like (stick-like), needle-like, fibrous (fiber-like), strand-like, thread-like, string-like, rope-like, cord-like, plate-like, sheet-like, membrane-like (film-like), woven fabric-like, nonwoven fabric-like, box-like (capsule-like), foam-like, and any three-dimensional shape, and the shape can be selected depending on the purpose of use.

[0241] Furthermore, when the thermal storage composition E is in the form of a sphere, a cube, a bead, a cylinder (pellet), or a powder, the thermal storage composition E may form a core-shell structure in which the thermal storage composition E is covered with a material different from the thermal storage composition E (hereinafter, sometimes referred to as "material D"), or a core-shell structure in which material D is covered with the thermal storage composition E. Note that material D is, for example, an organic compound, a polymer, a metal, or an inorganic compound other than a metal. Material D may also be a thermal functional material, which will be described later.

[0242] Furthermore, when the heat storage composition E is rod-shaped (stick-shaped), needle-shaped, fibrous (fiber-shaped), strand-shaped, thread-shaped, string-shaped, rope-shaped, or cord-shaped, it may form a core-sheath structure in which the heat storage composition E is covered with material D, or a core-sheath structure in which material D is covered with the heat storage composition E.

[0243] Furthermore, when the heat storage composition E is in the form of a plate, sheet, membrane (film), woven fabric, nonwoven fabric, box, or capsule, it may form a laminated structure in which the heat storage composition E is covered on both sides or one side with material D, or a laminated structure in which material D is covered on both sides or one side with heat storage composition E.

[0244] a foam-like molded body; A molded body having a shape different from a foam shape, or material D, is It may form a core-shell structure, a core-sheath structure or a laminated structure.

[0245] The thermal storage composition E may be spun. The thermal storage composition E may be formed into, for example, fiber parts, fibers, filaments, yarns, fabrics, nonwoven fabrics, wadding, and building materials.

[0246] In one embodiment, the heat storage composition E is a heat storage material (fiber, building material, etc.). The cross-sectional shape of the heat storage material (fiber, building material, etc.) may be a circular cross-section, a modified cross-section such as a polygonal or multi-lobed cross-section, or a hollow cross-section.

[0247] In one embodiment, the heat storage composition E is fibrous, and the single fiber fineness of the fiber is not particularly limited, but is preferably 1 dtex or more from the viewpoint of ease of fiberization, and is preferably 20 dtex or less from the viewpoint of fiber flexibility.

[0248] Examples of methods for producing such fibers include dry spinning, wet spinning, and melt spinning, with melt spinning being preferred. General spinning methods use chips containing a thermal storage composition as the raw material and mainly involve two steps: spinning and drawing. Examples of spinning methods suitable for producing fibers containing thermal storage composition E include a continuous polymerization spinning method in which thermal storage composition E is spun continuously from the thermal storage composition production process without being chipped, a direct spinning and drawing method (spin-draw method) in which the spinning and drawing steps are performed in one step, a high-speed spinning method that does not require a drawing step, a POY-DTY method in which a drawn yarn (DTY) is obtained through a false twisting step after a semi-drawn yarn (POY), and a spunbond method. These methods are more streamlined than the general spinning methods.

[0249] In one embodiment, the fiber containing the heat storage composition E may be a composite fiber. A composite fiber is a fiber formed by bonding two or more types of fibers made of different components together in a single yarn. Examples of composite fibers include core-sheath composite fibers, bonded composite fibers, splittable composite fibers, and islands-in-the-sea composite fibers.

[0250] The single fiber fineness of the composite fiber containing the heat storage composition E is not particularly limited, but is preferably 1 dtex or more from the viewpoint of ease of fiberization, and is preferably 20 dtex or less from the viewpoint of fiber flexibility.

[0251] Examples of the structure of the core-sheath type composite fiber include a core-sheath structure in which the heat storage composition E is covered with the material D, or a core-sheath structure in which the material D is covered with the heat storage composition E, and preferably a core-sheath structure in which the heat storage composition E is covered with the material D. The material D is preferably the polymer 2, and more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66).

[0252] As a composite fiber having a core-sheath structure in which the thermal storage composition E is covered with the material D, a composite fiber having an area ratio of the core in the cross section in the fiber diameter direction of 10 to 90% is preferred. From the viewpoint of temperature regulating function, the area ratio of the core is preferably 10% or more, and from the viewpoint of fiber strength, the area ratio of the core is preferably 90% or less. When the core contains polypropylene, from the viewpoint of dyeability of the entire fiber, the area ratio of the core is preferably 20 to 60%.

[0253] In order to control the core-sheath composite morphology, it is preferable that the ratio of the melt viscosity of the sheath component to that of the core component is in the range of 0.3 to 4.0.

[0254] Bonded composite fibers generally crimp due to differences in shrinkage rates, etc., but when the composite fiber is crimped spirally, the heat storage composition E may be on the inside of the spiral, or the material D may be on the inside of the spiral, and preferably the bonded composite fiber has the heat storage composition E on the inside of the spiral. Material D is preferably the polymer 2, and more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66).

[0255] As for the structure of the splittable conjugate fiber, when the splittable conjugate fiber is composed of a central radial fiber and multiple surrounding wedge-shaped fibers, the heat storage composition E may be the central radial fiber, or the material D may be the central radial fiber, and preferably the splittable conjugate fiber is the central radial fiber of the heat storage composition E. Material D is preferably polymer 2, more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66). The splittable conjugate fiber may be split and opened by chemical treatment to obtain ultrafine fibers.

[0256] As for the structure of the islands-in-sea type composite fiber, the heat storage composition E may be the sea fiber, or the material D may be the sea fiber, and preferably the islands-in-sea type composite fiber is one in which the material D is the sea fiber. Material D is preferably polymer 2, and more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66). In the islands-in-sea type composite fiber, the sea fiber may be removed by chemical treatment to obtain ultrafine fibers composed of a plurality of island fibers.

[0257] Examples of the form of the fiber containing the heat storage composition E include long fibers (multifilament, monofilament) and short fibers (staple). The long fibers (multifilament, monofilament) may be used as they are, or may be false-twisted to form a false-twisted yarn, or may be air-blended to form a blended yarn. The short fibers (staple) may be used as they are, or may be spun to form a spun yarn, or may be blended to form a blended yarn. They may be core-spun yarns in which long fibers are combined with short fibers, or may be twisted to form a doubled-twisted yarn, a twisted yarn, or a covered yarn.

[0258] The fiber containing the heat storage composition E may contain additives such as antioxidants, pigments, dyes, antibacterial agents, deodorizers, antistatic agents, flame retardants, inert fine particles, light-absorbing heat generating agents, moisture-absorbing heat generating agents, far-infrared heat generating agents, ultraviolet absorbers, ultraviolet scattering agents, infrared shielding agents, lubricants, oils, sizing agents, and other additives. The additives can be added during or after spinning.

[0259] The antioxidant to be added is not particularly limited and can be appropriately selected depending on the purpose, and examples thereof include phenolic compounds, phosphorus compounds, hindered amine compounds, etc. Only one type of antioxidant may be used, or two or more types may be used in combination.

[0260] The phenolic compound antioxidant is a radical chain reaction inhibitor having a phenol structure, and may be used alone or in combination of two or more. Among them, pentaerythritol-tetrakis(3-(3,5-di-t-butyl-4-hydroxyphenol)propionate) (e.g., Irganox 1010 manufactured by BASF), 2,4,6-tris(3',5'-di-t-butyl-4'-hydroxybenzyl)mesitylene (e.g., Adeka Stab AO-330 manufactured by ADEKA), 3,9-bis[1,1-dimethyl-2-[β-(3-t-butyl-4-hydroxy-5-methylphenyl)propionyloxy]ethyl]-2,4, 8,10-Tetraoxaspiro[5,5]-undecane (e.g., Sumilizer GA-80 manufactured by Sumitomo Chemical, Adeka Stab AO-80 manufactured by ADEKA), 1,3,5-tris[[4-(1,1-dimethylethyl)-3-hydroxy-2,6-dimethylphenyl]methyl]-1,3,5-triazine-2,4,6(1H,3H,5H)-trione (e.g., THANOX1790 manufactured by Tokyo Chemical Industry Co., Ltd., CYANOX1790 manufactured by CYTEC) are preferably used due to their high oxidative decomposition inhibitory effect. Among these, 3,9-bis[1,1-dimethyl-2-[β-(3-t-butyl-4-hydroxy-5-methylphenyl)propionyloxy]ethyl]-2,4,8,10-tetraoxaspiro[5,5]-undecane (e.g., Sumilizer GA-80 manufactured by Sumitomo Chemical Co., Ltd., Adeka Stab AO-80 manufactured by ADEKA) and 1,3,5-tris[[4-(1,1-dimethylethyl)-3-hydroxy-2,6-dimethylphenyl]methyl]-1,3,5-triazine-2,4,6(1H,3H,5H)-trione (e.g., THANOX1790 manufactured by Tokyo Chemical Industry Co., Ltd., CYANOX1790 manufactured by CYTEC) are particularly suitable for use because, when exposed to nitrogen oxide gases, the phenolic compound itself is unlikely to convert to a quinone compound, which is a cause of yellowing, and therefore can suppress yellowing of the composition due to nitrogen oxide gases during long-term storage.

[0261] The phosphorus-based antioxidant is a phosphorus-based antioxidant that reduces peroxides without generating radicals and is itself oxidized, and may be used alone or in combination of two or more. Among them, tris(2,4-di-t-butylphenyl)phosphite (e.g., Irgafos 168 manufactured by BASF) and 3,9-bis(2,6-di-t-butyl-4-methylphenoxy)-2,4,8,10-tetraoxa-3,9-diphosphaspiro[5,5]undecane (e.g., Adeka STAB PEP-36 manufactured by ADEKA) are preferably used because of their high oxidative decomposition inhibitory effect.

[0262] Furthermore, an antioxidant with a phenolic and phosphorus skeleton is 2,4,8,10-tetra-t-butyl-6-[3-(3-methyl-4-hydroxy-5-t-butylphenyl)propoxy]dibenzo[d,f][1,3,2]dioxaphosphepine (Sumitomo Chemical's Sumilizer GP), which exhibits excellent oxidative decomposition inhibitory effects, particularly in high-temperature processing at 230°C or higher, and is therefore suitable for use.

[0263] The hindered amine-based antioxidant is a hindered amine-based antioxidant that has the effect of capturing radicals generated by ultraviolet light or heat and regenerating phenol-based antioxidants that have been deactivated by their antioxidant function. A single type may be used, or two or more types may be used in combination. Among these, aminoether-based hindered amine-based compounds or high-molecular-weight hindered amine-based compounds having a molecular weight of 1,000 or more are preferably used. Among hindered amine-based compounds, aminoether-based hindered amine-based compounds have low basicity. The present inventors conducted extensive research into the yellowing of polyolefin compositions caused by nitrogen oxide gases and phenolic compounds, and found that a lower basicity of the hindered amine-based compound can inhibit the conversion of phenolic compounds, which serve as antioxidants, and phenolic compounds contained in packaging materials, into quinone-based compounds, which cause yellowing. In other words, aminoether-based hindered amine-based compounds are preferred because they can inhibit the yellowing of polyolefin compositions caused by nitrogen oxide gases and phenolic compounds during long-term storage. Specific examples of aminoether-type hindered amine compounds include, but are not limited to, bis(1-undecanoxy-2,2,6,6-tetramethylpiperidin-4-yl)carbonate (e.g., Adekastab LA-81 manufactured by ADEKA) and bis[2,2,6,6-tetramethyl-1-(octyloxy)piperidin-4-yl] decanedioate (e.g., Tinuvin PA123 manufactured by BASF). In addition to aminoether-type hindered amine compounds, specific examples of low-basic hindered amine compounds include, but are not limited to, esters of 4-hydroxy-2,2,6,6-tetramethyl-1-piperidineethanol and 3,5,5-trimethylhexanoic acid (e.g., Tinuvin 249 manufactured by BASF). High-molecular-weight hindered amine compounds with a molecular weight of 1,000 or more are preferred because they can inhibit leaching from the interior of polyolefin compositions due to washing or cleaning using organic solvents and have excellent durability in inhibiting oxidative decomposition.A specific example of a high molecular weight hindered amine compound having a molecular weight of 1000 or more is N-N'-N''-N'''-tetrakis(4,6-bis(butyl-(N-methyl-2,2,6,6-tetramethylpiperidin-4-yl)amino)triazin-2-yl)-4,7-diazadecane-1,10-diamine) (for example, SABOSTAB manufactured by SABO) UV119), poly((6-((1,1,3,3-tetramethylbutyl)amino)-1,3,5-triazine-2,4-diyl)(2,2,6,6-tetramethyl-4-piperidinyl)imino)-1,6-hexanediyl(2,2,6,6-tetramethyl-4-piperidinyl)imino)) (e.g., CHIMASSORB944 manufactured by BASF), polycondensate of dibutylamine-1,3,5-triazine-N,N'-bis(2,2,6,6-tetramethyl-4-piperidyl)-1,6-hexamethylenediamine and N-(2,2,6,6-tetramethyl-4-piperidyl)butylamine (e.g., CHIMASSORB2020 manufactured by BASF), and the like.

[0264] The fabric or cloth containing the fibers containing the heat storage composition E may be any of woven fabrics, knitted fabrics, and nonwoven fabrics. Examples of weaves include plain weave, twill weave, satin weave, and variations thereof, dobby, jacquard, etc. Examples of knitting structures include weft knitting, warp knitting, and variations thereof.

[0265] The fabric or nonwoven fabric containing the fibers containing the heat storage composition E is not particularly limited in terms of basis weight, gauge, etc.

[0266] The woven or nonwoven fabric containing the fiber containing the heat storage composition E may consist solely of the fiber containing the heat storage composition E, or may be woven or knitted with other fibers. Examples of other fibers include inorganic fibers such as carbon fiber, inorganic fiber, and metal fiber; refined fibers such as lyocell; regenerated fibers such as rayon, cupra, and polynosic; semi-synthetic fibers such as acetate, triacetate, and promix; synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane; natural fibers such as plant fibers like cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute); and animal fibers like wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), silk, and feathers like down and feathers. The proportion of the fibers containing the heat storage composition E used is not particularly limited, but is preferably 20 to 100% by weight.

[0267] The nonwoven fabric containing fibers containing the heat storage composition E may contain heat-fusible binder fibers. The heat-fusible binder fiber is preferably a composite fiber of a core-sheath type, a bonded type, or the like, containing the present heat storage composition E and a material with a melting point different from that of the heat storage composition E. The material with a melting point different from that of the heat storage composition E is preferably the above-mentioned polymer 2, and more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66).

[0268] When the heat-fusible binder fiber is used, its content is preferably 5 to 20% by weight of the total fibers of the nonwoven fabric.

[0269] The method for producing a nonwoven fabric containing fibers containing the heat storage composition E usually includes a web-forming step and a web-bonding step. Examples of the web-forming step include a dry method, a wet method, a spunbonding method, a meltblown method, and an airlaid method, and examples of the web-bonding step include a chemical bonding method, a thermal bonding method, a needle punching method, and a hydroentanglement method.

[0270] Fabrics and materials containing fibers containing the heat storage composition E have a temperature regulating function, and therefore the fabrics and materials can have a smaller basis weight and be thinner, making them light and soft to the touch without compromising the fashionability of the clothing. In one embodiment, fabrics and materials containing the fibers of the present invention containing polymer 1 (high molecular weight phase change material) have superior texture and washing durability compared to fabrics and materials containing fibers containing compound L (low molecular weight phase change material) encapsulated in microcapsules.

[0271] Thermal Functional Materials Examples of thermofunctional materials include cool-to-the-touch materials, moisture-absorbing and heat-generating materials, light-absorbing and heat-generating materials, far-infrared radiation materials, heat-retaining materials, heat-shielding materials, and water-absorbing and quick-drying materials. Thermofunctional materials can be, for example, a part of a fiber, a fiber, a filament, a thread, a fabric (cloth or fabric), a nonwoven fabric, a filling, or a building material.

[0272] Examples of the cool-to-the-touch material include materials containing inorganic fillers, fibers with high thermal conductivity, and materials that quickly absorb and diffuse moisture to remove heat of vaporization. The types of fibers that exhibit a cool-to-the-touch feel are not particularly limited, and examples include refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane, natural fibers such as plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute), wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk, and feathers such as down and feathers. Preferably, when made into a fabric, the cool touch evaluation value Qmax = 0.2 W / cm 2 The above is a cooling material. The above Qmax is measured using a ThermoLab testing machine KES-F7-11 manufactured by Kato Tech Co., Ltd. The hot plate of the testing machine, which has been heated to ambient temperature +10°C (or 20°C), is placed on the fabric, and the maximum amount of heat transferred from the hot plate to the fabric is measured.

[0273] The inorganic filler is not particularly limited, and examples thereof include calcium carbonate such as light calcium carbonate and heavy calcium carbonate, barium carbonate, magnesium carbonate such as basic magnesium carbonate, calcium sulfate, barium sulfate, titanium dioxide, iron oxide, tin oxide, titanium oxide, zinc oxide, magnesium oxide, ferrite powder, zinc sulfide, zinc carbonate, aluminum nitride, silicon nitride, boron nitride, satin white, diatomaceous earth such as calcined diatomaceous earth, calcium silicate, aluminum silicate, magnesium silicate, amorphous silica, amorphous synthetic silica, silica such as colloidal silica, colloidal alumina, pseudoboehmite, aluminum hydroxide, magnesium hydroxide, alumina, alumina hydrate, lithopone, zeolite, hydrated halloysite, clay, hydrotalcite, aluminosilicate, talc, pyrophyllite, and saponite. smectites such as hectorite, sauconite, stevensite, montmorillonite, beidellite, and nontronite; micas such as vermiculite, phlogopite, biotite, zinnwaldite, muscovite, paragonite, celadonite, and glauconite; kaolins such as clinochlore, chamosite, nimite, pennantite, sudoite, donbassite, clintite, margarite, sulite, antigorite, lizardite, chrysotile, mesite, cronsteadite, berthierite, greenalite, garnierite, kaolinite, dickite, nacrite, and halloysite; mineral pigments such as delaminated kaolin, calcined kaolin, sepiolite, palygorskite, imogolite, allophane, hisingerite, penwithite, activated clay, bentonite, sericite, graphite, and carbon fiber. These may be used alone or in combination of two or more.

[0274] The shape of the inorganic filler is not particularly limited, but examples thereof include regular shapes such as spheres, needles, and plates, or irregular shapes.

[0275] Examples of the high thermal conductivity fibers include highly oriented polyethylene fibers and highly oriented polybenzoxazole fibers whose thermal conductivity has been increased by stretching and orientation.

[0276] The moisture-absorbing heat-generating material utilizes the exothermic reaction (heat of condensation) in which kinetic energy is converted into thermal energy. The moisture-absorbing heat-generating material generates heat when it absorbs moisture and releases moisture in low-humidity environments, thereby controlling temperature and humidity. The types of fibers that exhibit moisture absorption and heat generation are not particularly limited, but include, for example, refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane, plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute), natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk, and feathers such as down and feathers.

[0277] The light-absorbing and heat-generating material is a material that absorbs sunlight and converts it into thermal energy. Examples of light-absorbing and heat-generating fibers containing a light-absorbing and heat-generating material include fibers in which a light-absorbing and heat-generating material such as zirconium carbide or organic dyes, which are highly efficient at absorbing specific wavelengths of sunlight and converting them into thermal energy, is fixed to the interior or surface of the fiber. Specific examples include, but are not limited to, refined fibers such as lyocell; regenerated fibers such as rayon, cupra, and polynosic; semi-synthetic fibers such as acetate, triacetate, and promix; synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane; plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute); natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk; and feathers such as down and feathers.

[0278] The far-infrared emitting material is a material that emits far-infrared rays when heated. Examples of far-infrared processed fibers containing a far-infrared emitting material include fibers having ceramics or the like with high far-infrared emitting properties fixed to the interior or surface of the fiber, and more specifically, although not limited to, refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane, plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute), natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk, and feathers such as down and feathers.

[0279] The heat-retaining material is a material that traps a large amount of air with low thermal conductivity within the fabric and prevents the warm air from escaping. Examples of fibers that exhibit heat-retaining properties include, but are not limited to, hollow fibers and feathers. More specifically, examples include refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane, natural fibers such as plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute), wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk, as well as down and feathers. Preferably, feathers such as down and feathers are used.

[0280] The heat-shielding material is a material that blocks sunlight. Examples of fibers that exhibit heat-shielding properties include, but are not limited to, fibers with inorganic particles kneaded into them, and fibers and fabrics that reflect or scatter sunlight by making the fibers and fabrics layered or hollow. More specific examples include refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane, cotton, cellulosic fibers, and plant fibers such as hemp (flax, ramie, hemp, and jute), natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk, as well as feathers and down.

[0281] The moisture-absorbing and quick-drying material is a material that quickly absorbs and dries sweat, keeping the inside of clothing dry and comfortable. The types of fibers that exhibit moisture-absorbing and quick-drying properties are not particularly limited, but include ultra-fine fibers that utilize capillary action, fibers with a specially designed shape to increase the surface area, fibers that combine hydrophilic and hydrophobic properties, and fabrics that utilize changes in the crimp state of fibers due to humidity. More specifically, refined fibers such as lyocell, regenerated fibers such as rayon, cupra, and polynosic, semi-synthetic fibers such as acetate, triacetate, and promix, acrylic, acrylic fibers, vinylon ... Examples of suitable fibers include synthetic fibers such as ethylenediamine, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane; plant fibers such as cotton, cellulose fibers, and hemp (flax, ramie, hemp, and jute); natural animal fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, etc.), and silk; and feathers such as down and feathers.

[0282] The cross-sectional shape of the fibers containing the thermal functional material may be circular, irregular such as polygonal or multi-lobed, or hollow.

[0283] The single yarn fineness of the fiber containing the thermal functional material is not particularly limited, but is preferably 1 dtex or more from the viewpoint of ease of fiberization, and is preferably 20 dtex or less from the viewpoint of fiber flexibility.

[0284] The fiber containing the thermal functional material may be a composite fiber. A composite fiber is a fiber formed by bonding two or more types of fibers made of different components within a single yarn. Examples of composite fibers include core-sheath composite fibers, bonded composite fibers, splittable composite fibers, and islands-in-the-sea composite fibers.

[0285] The single yarn fineness of the fiber containing the thermal functional material is not particularly limited, but is preferably 1 dtex or more from the viewpoint of ease of fiberization, and is preferably 20 dtex or less from the viewpoint of fiber flexibility.

[0286] Examples of the form of the fiber containing the thermal functional material include long fibers (multifilament, monofilament) and short fibers (staple). The long fibers (multifilament, monofilament) may be used as they are, or may be false-twisted to form a false-twisted yarn, or may be air-blended to form a blended yarn. The short fibers (staple) may be used as they are, or may be spun to form a spun yarn, or may be blended to form a blended yarn. They may be core-spun yarns in which long fibers are combined with short fibers, or may be twisted to form a doubled yarn, twisted yarn, or covered yarn.

[0287] The fiber containing the thermofunctional material may contain additives such as antioxidants, pigments, dyes, antibacterial agents, deodorizers, antistatic agents, flame retardants, inert fine particles, light-absorbing heat-generating materials, moisture-absorbing heat-generating materials, far-infrared heat-generating materials, ultraviolet absorbers, lubricants, ultraviolet scattering agents, infrared shielding agents, oils, sizing agents, and other additives. The additives can be added during or after spinning.

[0288] Complex The composite of the present invention contains the heat storage composition E. It may further contain the thermal functional material. The composite may be formed into any shape, for example, a composite fiber, a filament, a thread, a fabric, a nonwoven fabric, or a filling.

[0289] The composite of the present invention may be a composite fiber. The composite fiber refers to a fiber formed by bonding two or more types of fibers made of different components within a single yarn. Examples of the composite fiber include core-sheath composite fibers, bonded composite fibers, splittable composite fibers, and islands-in-sea composite fibers.

[0290] The single filament fineness of the composite fiber is not particularly limited, but is preferably 1 dtex or more from the viewpoint of ease of fiberization, and is preferably 20 dtex or less from the viewpoint of fiber flexibility.

[0291] Examples of the structure of the core-sheath type composite fiber include a core-sheath structure in which the heat storage composition E is covered with a thermal functional material, or a core-sheath structure in which the thermal functional material is covered with the heat storage composition E, and preferably a core-sheath structure in which the heat storage composition E is covered with the thermal functional material.

[0292] As the composite fiber having a core-sheath structure in which the heat storage composition E is covered with a thermal functional material, the composite fiber is preferably one in which the area ratio of the core in the cross section in the fiber diameter direction is 10% to 90%. From the viewpoint of the durability of the thermal function, the area ratio of the core is preferably 10% or more, and from the viewpoint of fiber strength, the area ratio of the core is preferably 90% or less.

[0293] Bonded composite fibers generally crimp due to differences in shrinkage rates, etc., but when the composite fibers crimp in a spiral shape, the heat storage composition E may be on the inside of the spiral, or the thermal functional material may be on the inside of the spiral, and preferably, the bonded composite fibers have the heat storage composition E on the inside of the spiral.

[0294] As for the structure of the splittable conjugate fiber, when the splittable conjugate fiber is composed of a central radial fiber and a plurality of surrounding wedge-shaped fibers, the central radial fiber may be the heat storage composition E, or the thermal functional material may be the thermal functional material, and preferably the splittable conjugate fiber is the central radial fiber of the heat storage composition E. The splittable conjugate fiber may be split and opened by chemical treatment to form ultrafine fibers.

[0295] As for the structure of the islands-in-sea type composite fiber, the heat storage composition E may be the sea fiber, or the thermal functional material may be the sea fiber.

[0296] Examples of the form of the composite fiber containing (is) the composite of the present invention include long fibers (multifilament, monofilament) and short fibers (staple). The long fibers (multifilament, monofilament) may be used as they are, or may be false-twisted to form a false-twisted yarn, or may be air-blended to form a blended yarn. The short fibers (staple) may be used as they are, or may be spun to form a spun yarn, or may be blended to form a blended yarn. They may be core-spun yarns in which long fibers are combined with short fibers, or may be twisted to form a doubled-twisted yarn, a twisted yarn, or a covered yarn.

[0297] The composite of the present invention may contain additives such as antioxidants, pigments, dyes, antibacterial agents, deodorants, antistatic agents, flame retardants, inert fine particles, light-absorbing heat-generating materials, moisture-absorbing heat-generating materials, far-infrared heat-generating materials, ultraviolet absorbers, ultraviolet scattering agents, infrared shielding agents, lubricants, oils, sizing agents, and other additives. The additives can be added during or after spinning.

[0298] The fabrics and nonwoven fabrics spun from the composite fibers containing (are) the composite of the present invention may be woven, knitted, or nonwoven. Examples of weaves include plain weave, twill weave, satin weave, and variations thereof, dobby, jacquard, etc. Examples of knitted structures include weft knitting, warp knitting, and variations thereof.

[0299] The fabric or nonwoven fabric containing (or being) the composite of the present invention may be made by blending, interweaving, interknitting, or intertwisting the fibers of the thermal storage composition E with the fibers of the thermal functional material.Furthermore, it may be made by interweaving or interknitting with other fibers. Other fibers include inorganic fibers such as carbon fiber, inorganic fiber, and metal fiber; refined fibers such as lyocell; regenerated fibers such as rayon, cupra, and polynosic; semi-synthetic fibers such as acetate, triacetate, and promix; synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane; plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute); natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk; and feathers such as down and feathers. Examples of weaves include plain weave, twill weave, satin weave, and variations thereof, dobby weave, jacquard weave, etc. Examples of knitting structures include weft knitting, warp knitting, and variations thereof. The weave and knitting structures may be biased so that the heat storage material is more effective in terms of heat storage effect.

[0300] The fabric or material, which is a woven fabric or nonwoven fabric containing (or is) the composite of the present invention, is not particularly limited in terms of basis weight, gauge, etc.

[0301] Fabrics or nonwoven fabrics containing (are) the composite of the present invention may be laminated. One type of fabric or nonwoven fabric containing the heat storage composition E may be laminated, or two or more types of such fabrics or nonwoven fabrics may be laminated, or such fabrics or nonwoven fabrics may be laminated together with fabrics or nonwoven fabrics containing a thermal functional material. The lamination method and number of layers are not particularly limited. When laminated with a cooling-touch material, it is preferable that the cooling-touch material be on the skin side. When laminated with a heat-retaining material, it is preferable that the heat storage composition E be the intermediate layer or on the skin side.

[0302] The nonwoven fabric containing (or being) the composite of the present invention may contain heat-fusible binder fibers. The heat-fusible binder fiber is preferably a core-sheath or laminated composite fiber composed of the heat storage composition E and a material with a melting point different from that of the heat storage composition E. The material with a melting point different from that of the heat storage composition E is preferably the polymer 2, more preferably polypropylene (PP), polyethylene terephthalate (PET), polytrimethylene terephthalate (PTT), polybutylene terephthalate (PBT), polyamide 6 (PA6), or polyamide 66 (PA66).

[0303] When the heat-fusible binder fiber is used, its content is preferably 5 to 20% by weight of the total fibers of the nonwoven fabric.

[0304] The method for producing a nonwoven fabric containing (is) the composite of the present invention typically includes a web-forming step and a web-bonding step. The web-forming step includes a dry method, a wet method, a spunbonding method, a meltblown method, an airlaid method, etc., and the web-bonding step includes a chemical bonding method, a thermal bonding method, a needle punching method, a hydroentanglement method, etc.

[0305] In the production of filling containing (or being) the composite of the present invention, fibers containing the heat storage composition E may be mixed with fibers containing a thermal functional material. Other fibers may also be mixed. Examples of other fibers include inorganic fibers such as carbon fiber, inorganic fibers, and metal fibers; refined fibers such as lyocell; regenerated fibers such as rayon, cupra, and polynosic; semi-synthetic fibers such as acetate, triacetate, and promix; synthetic fibers such as acrylic, acrylic fibers, vinylon, vinylidene, polyvinyl chloride, polyethylene, polychlor, aramid, polybutylene terephthalate (PBT), polytrimethylene terephthalate (PTT), polyamide 66 (PA66), and urethane; plant fibers such as cotton, cellulosic fibers, and hemp (flax, ramie, hemp, and jute); natural fibers such as wool, sheep's wool, animal hair (angora, cashmere, mohair, alpaca, camel, and the like), and silk; and feathers such as down and feathers. Furthermore, a filling containing a thermal functional material may be laminated with a woven or nonwoven fabric containing the heat storage composition E. The filling containing the composite of the present invention is a product in which the composite is filled inside a bag-shaped exterior body.

[0306] Since fabrics or materials containing the composite of the present invention have a temperature regulating function, the fabric or material can have a smaller basis weight and be thinner, which makes the fabric or material light and soft to the touch without compromising the fashionability of the clothing. Furthermore, fabrics or materials containing the composite of the present invention containing polymer 1 (a high-molecular-weight phase-change material) have superior washing durability compared to fabrics or materials containing a composite material containing compound L (a low-molecular-weight phase-change material) encapsulated in microcapsules.

[0307] In one embodiment, the heat storage composition E has excellent heat storage capacity, moldability, shape retention, and moisture permeability, and can therefore be suitably used, for example, as a product or component thereof that directly or indirectly requires heat or cold insulation capacity. Note that the composition of the present invention, which has excellent heat storage capacity, may also be used for articles that do not require heat storage capacity.

[0308] Examples of products or components that directly or indirectly require heat or cold insulation performance include building materials, furniture, interior goods, bedding, bathroom materials, vehicles, air conditioning equipment, electrical appliances, thermal containers, clothing, daily necessities, agricultural materials, fermentation systems, thermoelectric conversion systems, and heat transfer media.

[0309] Examples of building materials include flooring, wall materials, wallpaper, ceiling materials, roofing materials, underfloor heating systems, tatami mats, doors, sliding doors, shutters, shoji screens, windows, and window frames.

[0310] When used as a flooring, wall, ceiling, or roofing material, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and an insulating material containing material D and / or a heat shielding material containing material D can be suitably used in order to maintain a more constant indoor space temperature against fluctuations in the external environmental temperature.

[0311] Examples of the heat insulating material include polystyrene foam, polyurethane foam, acrylic resin foam, phenolic resin foam, polyethylene resin foam, foamed rubber, glass wool, rock wool, foamed ceramic, vacuum heat insulating material, and composites thereof.

[0312] Examples of the heat shielding material include aluminum plates, aluminum foils, aluminum powder-containing paints, ceramic powder paints, and composites thereof.

[0313] When used as a wall material, ceiling material, or roof material, in order to impart fire resistance, it is preferable to use, for example, a plate-shaped, sheet-shaped, or foam-shaped laminate of the heat storage composition E and a flame-retardant, semi-non-flammable, or non-flammable fire-resistant material containing the material D.

[0314] Examples of the fireproofing material include concrete, gypsum, wood-based cement, calcium silicate, glass, metal, intumescent fireproofing material, material containing a flame retardant, and composites thereof.

[0315] When used as a component of a floor heating system, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E, an insulating material containing material D, and a sensible heat storage material containing material D can be suitably used in order to efficiently utilize the heat generated from heating elements such as heating cables, surface heaters, and hot water pipes to maintain room temperature.

[0316] Examples of the sensible heat storage material include concrete, mortar, concrete slab, and composites thereof.

[0317] When used as a tatami component, in order to maintain a more constant indoor temperature despite fluctuations in the external environmental temperature, it is preferable to use, for example, a laminate having the heat storage composition E in the form of a plate, sheet, or foam, an insulating material containing material D, a tatami board containing material D, and a tatami facing containing material D. Furthermore, when used as a tatami board material, it is preferable to use a heat storage tatami board containing a mixture of heat storage composition E and wood fiber, and when used as a tatami facing material, it is preferable to use a heat storage tatami facing containing heat storage fiber that forms a core-sheath structure with fibrous (fiber-like) or strand-like heat storage composition E and a tatami facing material containing material D.

[0318] When used as a door component, a sliding door component, or a storm shutter component, a laminate having, for example, a plate-, sheet-, or foam-shaped heat storage composition E, an insulating material containing material D, and a surface material containing material D can be suitably used in order to maintain a more constant room temperature in a room separated by the door, sliding door, or storm shutter.

[0319] When used as a component of a shoji screen, in order to maintain a more constant room temperature in the room separated by the shoji screen and to provide a certain degree of light transmittance, it is preferable to use, for example, a foamed or nonwoven heat storage composition E, or a laminate having shoji paper containing foamed or nonwoven heat storage composition E and material D.

[0320] When used as a window component, in order to maintain a more constant indoor space temperature against fluctuations in the external environmental temperature and to provide a certain degree of light transmittance, it is preferable to use, for example, a laminate containing the foamed or nonwoven heat storage composition E and glass, polycarbonate, or polymethyl methacrylate.

[0321] When used as a window frame component, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and a metal window frame or a window frame made of a polymer other than polymer 1 can be suitably used in order to maintain a more constant indoor space temperature against fluctuations in the external environmental temperature, and to reduce the temperature difference between the room temperature and the window frame to prevent condensation.

[0322] Examples of furniture, interior items, and bedding include partition boards, blinds, curtains, carpets, futons, and mattresses.

[0323] When used as a component of a partition board, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E, an insulating material containing material D, and a surface material containing material D can be suitably used in order to maintain a more constant room temperature in the room separated by the partition board.

[0324] When used as a blind component, in order to maintain a more constant indoor temperature despite fluctuations in the external environmental temperature and to impart light-shielding performance, it is preferable to use, for example, a laminate having a plate- or sheet-shaped heat-shielding material containing the heat storage composition E and the material D. For example, when the blind blades are composed of a heat-shielding surface and a heat-storing surface as described above, the blinds can be used with the heat-shielding surface facing outward in the summer and with the heat-storing surface facing outward during the day in the winter and then turned inward at night, thereby controlling the amount of solar heat entering the building depending on the season and time of day, thereby reducing the power consumption of air-conditioning equipment.

[0325] When used as curtains, carpets, or futons, in order to impart any desired texture or feel, it is preferable to use a heat-storing woven fabric or heat-storing nonwoven fabric containing, for example, a heat-storing fiber that forms a core-sheath structure with a fibrous (fiber-like) or strand-like heat-storing composition E and a fiber material containing material D.

[0326] When used as a carpet, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and a woven or nonwoven fabric containing fibers containing material D can be suitably used to impart any texture or feel.

[0327] When used as a mattress, for example, a foamed heat storage composition E can be suitably used to impart flexibility.

[0328] Examples of bathroom materials include bathtub materials, bathtub lid materials, bathroom floor materials, bathroom wall materials, and bathroom ceiling materials.

[0329] When used as a bathtub material or bath cover material, in order to maintain a more constant temperature of the water in the bathtub despite fluctuations in the temperature in the bathroom, it is preferable to use, for example, a laminate having a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E, an insulating material containing material D, and a surface material containing material D.

[0330] When used as a bathroom flooring material, bathroom wall material, or bathroom ceiling material, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E, an insulating material containing material D, and a heat-shielding material containing material D can be suitably used in order to maintain a more constant bathroom temperature despite fluctuations in the external environmental temperature.

[0331] Examples of vehicle components include engine warm-up systems, gasoline evaporation loss prevention devices (canisters), vehicle air conditioning, interior materials, components for containers of refrigerated vehicles, and components for containers of heated vehicles.

[0332] Examples of components for air conditioning equipment include heat storage materials for building thermal storage air conditioning systems, components for heat storage tanks for water thermal storage air conditioning systems, components for heat storage tanks for ice thermal storage air conditioning systems, heat transfer medium piping materials or their insulation materials, refrigerant piping materials or their insulation materials, and duct materials for heat exchange ventilation systems.

[0333] Electrical appliances include, for example: Electronic devices such as televisions, Blu-ray recorders, DVD recorders, monitors, displays, projectors, rear projection televisions, stereo systems, radio cassette players, digital cameras, digital video cameras, mobile phones, smartphones, laptops, desktops, tablet PCs, PDAs, printers, 3D printers, scanners, home game consoles, portable game consoles, electronic storage batteries and electronic transformers; Electric heaters, fan heaters, dehumidifiers, humidifiers, heated carpets, kotatsu, electric blankets, electric lap blankets, electric foot warmers, heated toilet seats, heated toilet seats, irons, trouser presses, futon dryers, clothes dryers, hair dryers, hair irons, thermal massagers, thermal therapy devices, dishwashers, dish dryers, dry-type food waste disposal machines and other heated household appliances; Heating appliances such as induction cooking heaters, hot plates, microwave ovens, oven ranges, rice cookers, rice cake makers, bread makers, toasters, electronic proofers, electric pots, electric kettles, and coffee makers; Cooking appliances that generate frictional heat, such as mixers, food processors, and rice polishers; and Refrigerators and freezers, constant temperature and humidity coolers, milk coolers, brown rice coolers, vegetable coolers, cool rice storage bins, refrigerated and frozen showcases, prefabricated coolers, prefabricated refrigerated showcases, hot and cold food delivery carts, wine cellars, food vending machines, bento warming cabinets, etc.

[0334] When used as a member of an electronic device, for example, a plate- or sheet-like heat storage composition E can be suitably used to protect the electronic components constituting the electronic device from heat generated by the electronic components. In particular, in the case of highly integrated electronic components and the like that generate a large amount of local heat, for example, a laminate comprising a plate- or sheet-like heat storage composition E and a highly thermally conductive material containing material D can be suitably used to efficiently absorb the heat generated from the heat generating element into the plate- or sheet-like heat storage composition E.

[0335] Examples of the highly thermally conductive material include carbon nanotubes, boron nitride nanotubes, graphite, copper, aluminum, boron nitride, aluminum nitride, aluminum oxide, magnesium oxide, and composites thereof.

[0336] When used as a component of an electronic device that is used in contact with the human body, a laminate having, for example, a plate- or sheet-shaped heat storage composition E and the housing material can be suitably used to prevent heat generated from the electronic components that make up the electronic device from being conducted to the human body through the housing that makes up the electronic device.

[0337] When used as a component of a heating-type household appliance, the heat storage composition E can be suitably used, for example, in the form of a plate or sheet, to protect other components of the heating-type household appliance from the heat generated by the heating device that constitutes the heating-type household appliance. Furthermore, in order to improve heat retention performance and reduce power consumption, for example, a laminate having the heat storage composition E in the form of a plate, sheet, or foam and an insulating material containing the material D can be suitably used.

[0338] When used as a component of a heating-type cooking appliance, the heat storage composition E in the form of, for example, a plate or sheet can be suitably used to protect other components of the heating-type cooking appliance from the heat generated by the heating device that constitutes the heating-type cooking appliance. Furthermore, in order to improve heat retention performance and reduce power consumption, for example, a laminate having the heat storage composition E in the form of a plate, sheet, or foam and an insulating material containing the material D can be suitably used.

[0339] When used as a component of a cooking appliance that generates frictional heat, a laminate having, for example, a plate- or sheet-shaped heat storage composition E and a high thermal conductor containing material D can be suitably used to protect food from frictional heat.

[0340] When used as a component of a powered thermal insulation refrigerator, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped thermal storage composition E and an insulating material containing material D and / or a heat-shielding material containing material D can be suitably used in order to maintain a more constant internal temperature against fluctuations in the external environmental temperature.

[0341] Examples of heat-insulating and cold-insulating containers include those used for transporting and storing specimens and organs, those used for transporting and storing medicines and chemical substances, and those used for transporting and storing food. Furthermore, when used as a component of a thermal insulation / cold insulation container, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and an insulating material containing material D and / or a heat-shielding material containing material D can be suitably used in order to maintain a more constant internal temperature in the face of fluctuations in the external environmental temperature.

[0342] Examples of clothing include sleepwear, winter clothing, gloves, socks, sportswear, wetsuits, drysuits, heat-resistant protective clothing, and fire-resistant protective clothing. When used in clothing, in order to maintain a constant body temperature and impart a desired tactile feel, it is preferable to use a heat-storing woven fabric or heat-storing nonwoven fabric containing heat-storing fibers that form a core-sheath structure with a fibrous (fiber-like) or strand-like fibrous material containing the heat-storing composition E and material D.

[0343] When used in wetsuits or drysuits, a laminate having, for example, the heat storage composition E in plate or sheet form, the heat storage woven fabric or the heat storage nonwoven fabric, and an insulating material containing material D can be suitably used in order to keep body temperature more constant in cold water.

[0344] When used in heat-resistant protective clothing or fire-resistant protective clothing, in order to keep body temperature more constant against heat-generating elements and flames, it is preferable to use, for example, a laminate having the heat storage composition E in a plate or sheet form, the heat storage woven fabric or the heat storage nonwoven fabric, a heat insulating material containing material D, and a heat shielding material containing material D.

[0345] Examples of everyday items include tableware, lunch boxes, water bottles, thermoses, pocket warmers, hot water bottles, ice packs, and microwave-heatable heat packs.

[0346] When used as a component of tableware or lunch boxes, the heat storage composition E may be used as a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and an insulating material containing material D in order to maintain the food temperature more constant relative to the external environmental temperature.

[0347] Fermentation systems that ferment organic waste such as commercial or household food waste, sludge, livestock manure, or livestock and fishery residues, as well as plants and trees, to produce compost or biogas include, for example, bio-type food waste processors, fermentation tanks for producing compost, and fermentation tanks for producing biogas. When used as the fermentation system, a laminate having, for example, a plate-shaped, sheet-shaped, or foam-shaped heat storage composition E and an insulating material containing material D can be suitably used in order to maintain the temperature inside the tank at a constant temperature suitable for fermentation despite fluctuations in the external environmental temperature.

[0348] Examples of agricultural materials include films for greenhouses, agricultural heat-retaining sheets, hoses and pipes for irrigation, and agricultural electric mats for raising seedlings. When used as agricultural materials, a laminate having, for example, a plate-like, sheet-like, or foam-like heat storage composition E and an insulating material containing material D can be suitably used to maintain the temperature around agricultural crops at a constant temperature suitable for crop growth despite fluctuations in the external environmental temperature. [Example]

[0349] The present invention will be described in more detail below with reference to examples and comparative examples, but the present invention is not limited to these examples.

[0350] I. The number of structural units A derived from ethylene and structural units C derived from methyl acrylate contained in the precursor polymer (ethylene-methyl acrylate copolymer) (unit: %) Nuclear magnetic resonance spectra (hereinafter referred to as NMR spectra) were measured using a nuclear magnetic resonance spectrometer (NMR) under the measurement conditions shown below. Next, the amounts (number [mol %] and weight [wt %]) of structural units A, B, and C were determined according to the method described above.

[0351] <Carbon Nuclear Magnetic Resonance ( 13 C-NMR) Measurement conditions> Equipment: AVANCE III 600HD manufactured by Bruker BioSpin Co., Ltd. Measurement probe: 10mm cryoprobe Measurement solvent: 1,2-dichlorobenzene / 1,1,2,2-tetrachloroethane-d2 = 85 / 15 (volume ratio) mixture Sample concentration: 100 mg / mL Measurement temperature: 135℃ Measurement method: Proton decoupling method Accumulation count: 256 times Pulse width: 45 degrees Pulse repetition time: 4 seconds Measurement standard: tetramethylsilane

[0352] II. Unreacted C 14~30 Content of compounds having alkyl groups (wt%) In the "Production of Substance A" of each Example, the obtained product is a mixture of Substance A and unreacted C. 14~30 The unreacted C contained in the product is a mixture of compounds with alkyl groups. 14~30 The content of the compound having an alkyl group was measured by gas chromatography (GC) using the following method. The content of the unreacted compound is a value when the total weight of substance A and the unreacted compound is taken as 100% by weight. [GC measurement conditions] GC equipment: Shimadzu GC2014 Column: DB-5MS (60 m, 0.25 mm φ, 1.0 μm) Column temperature: The column is maintained at 40°C, and the temperature is increased to 300°C at a rate of 10°C / min, and then maintained at 300°C for 40 minutes. Vaporizer / detector temperature: 300℃ / 300℃(FID) Carrier gas: Helium Pressure: 220kPa Total flow rate: 17.0mL / min Column flow rate: 1.99 mL / min Purge flow rate: 3.0 mL / min Linear speed: 31.8cm / sec Injection method / split ratio: Split injection / 6:1 Injection volume: 1μL Sample preparation method: 8 mg / mL (o-dichlorobenzene solution) (1) Creating a calibration curve [Solution preparation] 5 mg of the sample was weighed into a 9 mL vial, 100 mg of n-tridecane was weighed as an internal standard, and 6 mL of o-dichlorobenzene was added as a solvent to completely dissolve the sample, obtaining a standard solution for creating a calibration curve. Two more standard solutions were prepared in the same manner as above, except that the amount of sample was changed to 25 mg and 50 mg. [GC measurement] The standard solution for preparing the calibration curve was measured under the GC measurement conditions described above, and a calibration curve was prepared with the GC area ratio of the standard and the internal standard on the vertical axis and the weight ratio of the standard and the internal standard on the horizontal axis, and the slope a of the calibration curve was determined. (2) The substance to be measured in the sample (product) (unreacted C 14~30 Measurement of the content of compounds containing alkyl groups [Solution preparation] 50 mg of sample and 100 mg of n-tridecane were weighed into a 9 mL vial, and 6 mL of o-dichlorobenzene was added thereto and the sample was completely dissolved at 80°C to obtain a sample solution. [GC measurement] The sample solution is measured under the GC measurement conditions described above, and the content of the substance to be measured in the sample, P S was calculated according to the following formula: PS : Content of the substance to be measured in the sample (% by weight) W S : weight of sample (mg) W IS : Weight (mg) of internal standard (IS) A S : Peak area count of the object to be measured A IS : Peak area count of internal standard (IS) a: Slope of the calibration curve of the object to be measured

number

[0353] III. Raw materials Reference example 1 <Production of precursor polymer> cf1: ethylene-methyl acrylate copolymer Ethylene-methyl acrylate copolymer (cf1) was prepared as follows. In an autoclave reactor, ethylene and methyl acrylate were copolymerized using tert-butyl peroxypivalate as a radical polymerization initiator at a reaction temperature of 195°C and a reaction pressure of 160 MPa to obtain an ethylene-methyl acrylate copolymer cf1. The composition and MFR of the obtained copolymer cf1 were as follows: Number of structural units derived from ethylene: 64.5% by weight Number of structural units derived from methyl acrylate: 35.5% by weight MFR (measured in accordance with JIS K7210 at a temperature of 190°C and a load of 21N): 30g / 10min

[0354] cf2: ethylene-methyl acrylate copolymer Ethylene-methyl acrylate copolymer (cf2) was prepared as follows. In an autoclave reactor, ethylene and methyl acrylate were copolymerized using tert-butyl peroxypivalate as a radical polymerization initiator at a reaction temperature of 195°C and a reaction pressure of 160 MPa to obtain an ethylene-methyl acrylate copolymer cf2. The composition and MFR of the obtained copolymer cf2 were as follows: Number of structural units derived from ethylene: 68.8% by weight Number of structural units derived from methyl acrylate: 31.2% by weight MFR (measured in accordance with JIS K7210 at a temperature of 190°C and a load of 21N): 40.5g / 10min

[0355] <C 14~30 Compounds having alkyl groups of the formula B-1: GINOL-16 (1-hexadecanol) [manufactured by GODREJ] B-2: GINOL-18 (1-octadecanol) [manufactured by GODREJ] B-3: Kalcol 220-80 (1-docosanol) [Kao Corporation]

[0356] <Catalyst> C-1: Tetraisopropyl orthotitanate [Nippon Soda Co., Ltd.]

[0357] Reference example 2 <Production of Substance A> A-1: Ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer After replacing the inside of a reactor equipped with a stirrer with nitrogen, 30 parts by weight of B-1, 62 parts by weight of B-2, and 0.60 parts by weight of C-1 were added to 100 parts by weight of CF1. The jacket temperature was set to 140°C, and the mixture was heated and stirred under a reduced pressure of 0.4 kPa for 5 hours to obtain polymer A-1 (ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer). The melting peak temperature Tm (°C), melting enthalpy ΔH between 10 and 60°C, and unreacted C were measured. 14~30 The content (wt %) of the compound having an alkyl group was as follows: Structural unit (A): 84.5 mol% Structural unit (B): 12.9 mol% Structural unit (C): 2.6 mol% Melting peak temperature Tm: 32°C (measurement condition 3) Melting enthalpy ΔH between 10 and 60°C: 76 J / g (measurement condition 3) Unreacted C 14~30 Content of compounds having alkyl groups: 0.9% by weight

[0358] A-2: Ethylene-n-hexadecyl acrylate-methyl acrylate copolymer After replacing the inside of a reactor equipped with a stirrer with nitrogen, 86 parts by weight of B-1 and 0.60 parts by weight of C-1 were added to 100 parts by weight of CF1, and the jacket temperature was set to 140°C, followed by heating and stirring under a reduced pressure of 0.4 kPa for 3 hours to obtain polymer A-2 (ethylene-n-hexadecyl acrylate-methyl acrylate copolymer). The melting peak temperature Tm (°C), melting enthalpy ΔH between 10 and 60°C, and unreacted C were measured. 14~30 The content (wt %) of the compound having an alkyl group was as follows: Structural unit (A): 84.1 mol% Structural unit (B): 13.3 mol% Structural unit (C): 2.6 mol% Melting peak temperature Tm: 23°C (measurement condition 3) Melting enthalpy ΔH between 10 and 60°C: 65 J / g (measurement condition 3) Unreacted C 14~30 Content of compounds having alkyl groups: 0.9% by weight

[0359] A-3: Ethylene-α-olefin copolymer After drying under reduced pressure, 1.4 L of a toluene solution containing 706 g of α-olefin C2024 (a mixture of olefins containing 18, 20, 22, 24, and 26 carbon atoms, manufactured by INEOS) was added to a 5 L autoclave equipped with a stirrer, the interior of which had been purged with nitrogen. Toluene was then added to bring the total volume to 3 L. The autoclave was heated to 60 °C, and ethylene was added to stabilize the system at a partial pressure of 0.1 MPa. A hexane solution of triisobutylaluminum (0.34 mol / L, 14.7 mL) was then added. Polymerization was initiated by adding a toluene solution of dimethylanilinium tetrakis(pentafluorophenyl)borate (1.0 mmol / L, 13.4 mL) and a toluene solution of diphenylmethylene(cyclopentadienyl)(fluorenyl)zirconium dichloride (0.2 mmol / L, 7.5 mL). Ethylene gas was then added to maintain a constant total pressure. After 3 hours, 2 ml of ethanol was added to terminate the polymerization. After termination of the polymerization, the toluene solution containing the polymer was added to acetone to precipitate an ethylene-α-olefin copolymer, and the polymer was separated by filtration and further washed twice with acetone. The obtained polymer was dried in vacuum at 80°C to obtain 369 g of the polymer. The melting peak temperature Tm (°C) of the obtained polymer A-3 and the amount of unreacted C were 14~30 The content (wt %) of the compound having an alkyl group was as follows: Structural unit (A): 84.6 mol% Structural unit (B): 15.4 mol% Melting peak temperature Tm: 34°C (measurement condition 5) Melting enthalpy ΔH between 10 and 60°C: 83 J / g (measurement condition 5)

[0360] A-4: Ethylene-n-docosyl acrylate-methyl acrylate copolymer After replacing the inside of a reactor equipped with a stirrer with nitrogen, 120 parts by weight of B-3 and 0.60 parts by weight of C-1 were added to 100 parts by weight of cf2, and the jacket temperature was set to 140°C, followed by heating and stirring under a reduced pressure of 0.4 kPa for 5 hours to obtain polymer A-4 (ethylene-n-docosyl acrylate-methyl acrylate copolymer). The melting peak temperature Tm (°C), melting enthalpy ΔH between 10 and 60°C, and unreacted C were measured. 14~30 The content (wt %) of the compound having an alkyl group was as follows: Structural unit (A): 87.1 mol% Structural unit (B): 10.9 mol% Structural unit (C): 2.0 mol% Melting peak temperature Tm: 51°C (measurement condition 3) Melting enthalpy ΔH between 10 and 60°C: 92 J / g (measurement condition 3) Unreacted C 14~30 Content of compounds having alkyl groups: 1.2% by weight

[0361] <Polymer 2> D-1: Acryft WH206-F (ethylene-methyl methacrylate copolymer, melting peak temperature 86°C) [Sumitomo Chemical Co., Ltd.] D-2: Sumitomo Noblen (propylene homopolymer, melting peak temperature 163°C) [Sumitomo Chemical Co., Ltd.] D-3: ENGAGE 8100 (ethylene-octene copolymer, melting peak temperature 57°C) [The Dow Chemical Company] D-4: Sumitomo Noblen (propylene random copolymer, melting peak temperature 132°C) [Sumitomo Chemical Co., Ltd.] D-5: Hi-Zex 3300F (high-density polyethylene, peak melting temperature 132°C) [manufactured by Brim Polymer Co., Ltd.] D-6: Acrylate WD106 (ethylene-methyl methacrylate copolymer, melting peak temperature 101°C) [Sumitomo Chemical Co., Ltd.]

[0362] <Organic peroxide> E-1: CH-12 (a mixture containing 8% by weight of 2,5-dimethyl-2,5-di(tert-butylperoxy)hexane and 92% by weight of polypropylene) (1-minute half-life temperature: 180°C) [manufactured by NOF Corporation] E-2: A mixture containing 50% by weight of 2,5-dimethyl-2,5-di(tert-butylperoxy)hexane, calcium carbonate, and amorphous silicon dioxide (1-minute half-life temperature: 180°C) [manufactured by Kayaku Akzo Co., Ltd.]

[0363] <Crosslinking aid> F-1: Hicross MS50 (a mixture of 50% by weight of trimethylolpropane trimethacrylate and 50% by weight of amorphous silicon dioxide) [manufactured by Seiko Chemical Co., Ltd.] F-2: Hicross M (trimethylolpropane trimethacrylate) [Seiko Chemical Co., Ltd.]

[0364] <Antioxidants> G-1: IRGANOX 1010 (pentaerythritol tetrakis[3-(3',5'-di-tert-butyl-4'-hydroxyphenyl)propionate]) [manufactured by BASF]

[0365] <Heat processing stabilizer> H-1: IRGAFOS168 (tris(2,4-di-tert-butylphenyl)phosphite) [manufactured by BASF]

[0366] <Lubricant> I-1: Alflow AD-281F (ethylene bis(oleic acid amide)) [NOF Corporation]

[0367] <Packaging materials> J-1: Excellen VL VL700 (linear low-density polyethylene, peak melting temperature 90°C) [Sumitomo Chemical Co., Ltd.] J-2: Sumitomo Noblen (propylene homopolymer, melting peak temperature 163°C) [manufactured by Sumitomo Chemical Co., Ltd.]

[0368] <Extruder> Twin-screw extruder (1) Screw diameter D=75mm Screw effective length L / screw diameter D=40 Single screw extruder (2) Screw diameter D=20mm Spinning equipment (3) Screw diameter D=20mm Composite spinning equipment (4) Screw diameter D=25mm Twin-screw extruder (5) Screw diameter D=15mm Screw effective length L / screw diameter D=45

[0369] IV. Preparation and evaluation of heat storage compositions

[0370] Example A1: Preparation of resin compositions containing ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and ethylene-methyl methacrylate copolymer 73.4 parts by weight of the polymer A-1 obtained in Reference Example 2, 23.8 parts by weight of D-1, 2.5 parts by weight of E-1, 0.1 parts by weight of G-1, 0.1 parts by weight of H-1, and 0.1 parts by weight of I-1 were fed to a twin-screw extruder (1) and melt-kneaded at a screw rotation speed of 350 rpm, a discharge rate of 150 kg / hr, and a maximum barrel temperature of 220°C to produce resin composition A1'. Furthermore, J-1 was fed to a single-screw extruder (2) and melt-kneaded at a discharge rate of 9 kg / hr and a maximum barrel temperature of 240°C to produce sheet-shaped J-1. Next, using a multilayer sheet molding machine equipped with a multilayer die, resin composition A1' and J-1 were multilayer extruded at a die temperature of 230°C so that the outer layer / inner layer / outer layer was J-1 / resin composition A1' / J-1 and the weight ratio of outer layer / inner layer / outer layer was 4.5 / 150 / 4.5, to produce packaged pellets of heat storage composition A1. The prepared heat storage composition A1 was spun in a spinning apparatus (3) at a maximum barrel temperature of 190°C, a die diameter of 0.8 mm, and a take-up speed of 48.5 m / min to produce an undrawn yarn, which was then subjected to a tensile test. DSC measurement was performed under measurement condition 1.

[0371] Example A2: Preparation of resin compositions containing ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and ethylene-methyl methacrylate copolymer Pellets and undrawn yarn of resin composition A2 were prepared in the same manner as in Example A1, except that 62.9 parts by weight of Polymer A-1 obtained in Reference Example 2, 34.3 parts by weight of D-1, 2.5 parts by weight of E-1, 0.1 part by weight of G-1, 0.1 part by weight of H-1, and 0.1 part by weight of I-1 were used, and a tensile test of the undrawn yarn was performed. DSC measurement was performed under measurement condition 1.

[0372] Example A3: Preparation of resin compositions containing ethylene-n-hexadecyl acrylate-n-methyl acrylate copolymer and ethylene-methyl methacrylate copolymer Pellets and undrawn yarn of resin composition A3 were prepared in the same manner as in Example A1, except that 73.4 parts by weight of Polymer A-2 obtained in Reference Example 2, 23.8 parts by weight of D-1, 2.5 parts by weight of E-1, 0.1 part by weight of G-1, 0.1 part by weight of H-1, and 0.1 part by weight of I-1 were used, and a tensile test of the undrawn yarn was performed. DSC measurement was performed under measurement condition 1.

[0373] Example A4: Preparation of resin compositions containing ethylene-α-olefin copolymer and ethylene-octene copolymer 69.9 parts by weight of the polymer A-3 obtained in Reference Example 2, 29.9 parts by weight of D-3, 0.1 parts by weight of G-1, and 0.1 parts by weight of H-1 were fed to a twin-screw extruder (5) and melt-kneaded at a maximum barrel temperature of 220°C to produce pellets and unstretched yarn of resin composition A4, and a tensile test of the unstretched yarn was performed. DSC measurement was performed under measurement condition 1.

[0374] Comparative Example C1: Preparation of resin compositions containing ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and propylene homopolymer Resin composition C1' was prepared in the same manner as in Example A1, except that 73.4 parts by weight of polymer A-1 obtained in Reference Example 2, 23.8 parts by weight of D-2, 2.5 parts by weight of E-1, 0.1 parts by weight of G-1, 0.1 parts by weight of H-1, and 0.1 parts by weight of I-1 were used. Next, pellets and undrawn yarn of composition C1 were prepared in the same manner as in Example A1, except that the extrusion rate of J-2 was 8 kg / hr, the outer layer / inner layer / outer layer ratio was J-2 / resin composition C1' / J-2, and the weight ratio of outer layer / inner layer / outer layer was 4 / 150 / 4. Tensile tests of the undrawn yarn were performed. DSC measurements were performed under measurement condition 1.

[0375] Comparative Example C2: Preparation of resin compositions containing ethylene-n-hexadecyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and ethylene-methyl methacrylate copolymer Pellets and undrawn yarn of resin composition C2 were prepared in the same manner as in Example A1, except that 73.4 parts by weight of Polymer A-1, 23.8 parts by weight of Polymer D-6, 2.5 parts by weight of Polymer E-1, 0.1 parts by weight of Polymer G-1, 0.1 parts by weight of Polymer H-1, and 0.1 parts by weight of Polymer I-1 obtained in Reference Example 2 were used. A tensile test of the undrawn yarn was performed. DSC measurement was performed under measurement condition 1.

[0376] Comparative Example C3: Preparation of resin compositions containing ethylene-n-docosyl acrylate-methyl acrylate copolymer and propylene random copolymer The polymers A-4 (78.2 parts by weight), D-4 (19.6 parts by weight), E-2 (1.0 parts by weight), F-1 (1.0 parts by weight), G-1 (0.1 parts by weight), and H-1 (0.1 parts by weight) obtained in Reference Example 2 were fed to a twin-screw extruder (5) and melt-kneaded at a maximum barrel temperature of 220°C to produce pellets of resin composition C3. An attempt was then made to produce undrawn yarn, but yarn breakage occurred, making it difficult to obtain a sample. DSC measurement was performed under measurement condition 1.

[0377] Comparative example C4: Preparation of resin compositions containing ethylene-n-docosyl acrylate-methyl acrylate copolymer and high-density polyethylene The polymers A-4 (78.2 parts by weight), D-5 (19.6 parts by weight), E-2 (1.0 parts by weight), F-1 (1.0 parts by weight), G-1 (0.1 parts by weight), and H-1 (0.1 parts by weight) obtained in Reference Example 2 were fed to a twin-screw extruder (5) and melt-kneaded at a maximum barrel temperature of 220°C to produce pellets of resin composition C4. An attempt was then made to produce undrawn yarn, but yarn breakage occurred, making it difficult to obtain a sample. DSC measurement was performed under measurement condition 1.

[0378] V. Preparation and evaluation of fibers containing heat storage compositions

[0379] Example B1 Using a conjugate spinning apparatus (4), 40 parts by weight of the heat storage composition A1 obtained in Example A1 and 60 parts by weight of polyester were used to obtain an undrawn yarn of a sheath-core type conjugate fiber with a sheath: polyester and a core: heat storage composition A1. The obtained undrawn yarn of the sheath-core type conjugate fiber was drawn at a draw ratio of 3 to 4 times in an 80°C bath to obtain a drawn yarn. When attempts were made to reduce the fineness, it was possible to obtain a drawn yarn with a fineness of up to 3.1 dtex. The melting peak temperature Tm (°C) of the obtained drawn yarn was as follows. DSC measurement was carried out under measurement condition 2. Melting peak temperature Tm: 32℃ The enthalpy of fusion ΔH observed by differential scanning calorimetry in the temperature range of 10 to 60°C: 24 J / g

[0380] Example B2 Using a conjugate spinning apparatus (4), 40 parts by weight of the heat storage composition A1 obtained in Example A1 and 60 parts by weight of polyester was used to obtain an undrawn yarn of a sheath-core type conjugate fiber with a sheath: polyester and a core: heat storage composition A1. The obtained undrawn yarn of the sheath-core type conjugate fiber was drawn at a draw ratio of 3 to 4 times in an 80°C bath to obtain a drawn yarn, and a drawn yarn with a fineness of 4.3 dtex was obtained. The melting peak temperature Tm (°C) of the obtained drawn yarn was as follows. DSC measurement was performed under measurement condition 2. Melting peak temperature Tm: 32℃ Melting enthalpy ΔH observed by differential scanning calorimetry within the temperature range of 10 to 60°C: 25 J / g

[0381] Example B3 Using a conjugate spinning apparatus (4), 50 parts by weight of the heat storage composition A2 obtained in Example A2 and 50 parts by weight of polyester was used to obtain an undrawn yarn of a sheath-core type conjugate fiber with a sheath: polyester and a core: heat storage composition A2. The obtained undrawn yarn of the sheath-core type conjugate fiber was drawn at a draw ratio of 3 to 4 times in an 80°C bath to obtain a drawn yarn, and a drawn yarn with a fineness of 3.2 dtex was obtained. The melting peak temperature Tm (°C) of the obtained drawn yarn was as follows. DSC measurement was performed under measurement condition 2. Melting peak temperature Tm: 32℃ The enthalpy of fusion ΔH observed by differential scanning calorimetry in the temperature range of 10 to 60°C: 31 J / g

[0382] Example B4 Using a conjugate spinning apparatus (4), 50 parts by weight of the heat storage composition A3 obtained in Example A3 and 50 parts by weight of polyester was used to obtain an undrawn yarn of a sheath-core type conjugate fiber with a sheath: polyester and a core: heat storage composition A3. The obtained undrawn yarn of the sheath-core type conjugate fiber was drawn at a draw ratio of 3 to 4 times in an 80°C bath to obtain a drawn yarn, and a drawn yarn with a fineness of 3.0 dtex was obtained. The melting peak temperature Tm (°C) of the obtained drawn yarn was as follows. DSC measurement was performed under measurement condition 2. Melting peak temperature Tm: 23℃ The enthalpy of fusion ΔH observed by differential scanning calorimetry in the temperature range of 10 to 60°C: 23 J / g

[0383] Comparative Example D1 Using a conjugate spinning apparatus (4), 40 parts by weight of the heat storage composition C1 obtained in Comparative Example C1 and 60 parts by weight of polyester was used to obtain an undrawn yarn of a sheath-core type conjugate fiber with a sheath: polyester and a core: heat storage composition C1. The obtained undrawn yarn of the sheath-core type conjugate fiber was drawn at a draw ratio of 3 to 4 times in an 80°C bath to obtain a drawn yarn. When attempts were made to reduce the fineness, it was possible to obtain a drawn yarn with a fineness of up to 4.8 dtex. The melting peak temperature Tm (°C) of the obtained drawn yarn was as follows: Melting peak temperature Tm: 30℃ The enthalpy of fusion ΔH observed by differential scanning calorimetry in the temperature range of 10 to 60°C: 22 J / g

[0384] [Table 1]

[0385] [Table 2]

Claims

1. A heat storage composition comprising a substance A and a polymer 2, The heat storage composition has a peak melting temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 30 J / g or more; The substance A has a melting peak temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 30 J / g or more; The substance A includes polymer 1, The polymer 1 has a melting peak temperature in the range of 10 to 60°C and a molecular weight of more than 2000; The polymer 1 has a structural unit B represented by the following formula (1): The polymer 2 has a melting peak temperature or a glass transition temperature between 60 and 120°C, The heat storage composition has a sea-island structure, and the volume-average circle-equivalent particle diameter of the islands (dispersed phase) is 1.5 μm or less, or the area ratio of the islands (dispersed phase) is 15% or less. Heat storage composition: 【Chemical 1】 In formula (1), R １ represents a hydrogen atom or a methyl group, L １１ represents —CO—O—, —O—CO—, or —O—; L １２ is a single bond, -CH ２ -, -CH ２ -CH ２ -, -CH ２ -CH ２ -CH ２ -, -CH ２ -CH(OH)-CH ２ - or -CH ２ -CH(CH ２ OH)—, L １３ is a single bond, -CO-O-, -O-CO-, -O-, -CO-NH-, -NH-CO-, -CO-NH-CO-, -NH-CO-NH-, -NH-, or -N(CH ３ )-, L １６ is C １４～３０ represents an alkyl group represented by the formula: L １１ , L １２ , and L １３ In each of the horizontally written chemical formulas, the left side corresponds to the upper side of formula (1) (the main chain side of the polymer), and the right side corresponds to the lower side of formula (1) (the terminal side of the side chain of the polymer).

2. 2. The thermal storage composition according to claim 1, which has a plurality of melting peak temperatures, at least one of which is within the range of 60 to 120°C.

3. The heat storage composition according to claim 1 or 2, wherein the gel fraction is 15% by weight or less.

4. A thermal storage composition according to any one of claims 1 to 3, wherein substance A has a molecular weight of more than 2000.

5. A fiber comprising the heat storage composition according to any one of claims 1 to 4.

6. A heat storage fiber comprising a heat storage composition comprising substance A and polymer 2, The fiber has a peak melting temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 5 J / g or more; The substance A has a melting peak temperature between 10 and 60°C and a melting enthalpy between 10 and 60°C of 30 J / g or more; The polymer 2 has a melting peak temperature or a glass transition temperature between 60 and 120°C, The thermal storage composition of the fiber has a sea-island structure, and the circle-equivalent particle diameter of the islands (dispersed phase) is less than 0.1 μm, or the area ratio of the islands (dispersed phase) is 15% or less. Heat storage fiber.

7. The heat storage fiber according to claim 6, having a plurality of melting peak temperatures, at least one of which is within the range of 60 to 120°C.

8. The heat storage fiber according to claim 6 or 7, wherein the gel fraction of the heat storage composition within the fiber is 15% by weight or less.

9. The heat storage fiber according to any one of claims 6 to 8, wherein substance A has a molecular weight of more than 2000.

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