Polymer

Abstract

A polymer that is capable of affording a heat storage material superior in humidity permeability and shape retention after phase transition and that is superior in molding processability is provided. The polymer includes constitutional units (A) derived from ethylene, constitutional units (B) represented by a specified formula, and optionally includes constitutional units (C) represented by another specified formula. Where the total number of the units (A), the units (B), and the units (C) is 100%, the number of the units (A) accounts for 70% to 99%, the total number of the units (B) and the units (C) accounts for 1% by weight to 30% by weight. Where the total number of the units (B) and the units (C) is 100%, the number of the units (B) accounts for 1% to 100% and the number of the units (C) accounts for 0% to 99%.

Claims

1. A polymer comprising structural units (A) derived from ethylene and constitutional units (B) represented by formula (1) below and optionally comprising at least one type of constitutional units (C) selected from the group consisting of constitutional units represented by formula (2) below and constitutional units represented by formula (3) below, wherein where the total number of the units (A), the units (B), and the units (C) is 100%, the number of the units (A) accounts for 70% to 99% and the total number of the units (B) and the units (C) accounts for 1% to 30%; and where the total number of the units (B) and the units (C) is 100%, the number of the units (B) accounts for 1% to 100% and the number of the units (C) accounts for 0% to 99%, ##STR00062## in formula (1) R represents a hydrogen atom or methyl group, L.sup.1 represents COO, OCO, or O, L.sup.2 represents a single bond, CH.sub.2, CH.sub.2CH.sub.2, CH.sub.2CH.sub.2CH.sub.2, CH.sub.2CH(OH)CH.sub.2, or CH.sub.2CH(CH.sub.2OH), L.sup.3 represents a single bond, COO, OCO, O, CONH, NHCO, CONHCO, NHCONH, NH, or N(CH.sub.3), L.sup.6 represents an alkyl group having 14 to 30 carbon atoms; ##STR00063## in formula (2), R represents a hydrogen atom or a methyl group, L.sup.1 represents COO, OCO, or O, L.sup.4 represents an alkylene group having 1 to 8 carbon atoms, L.sup.5 represents a hydrogen atom, an epoxy group, CH(OH)CH.sub.2OH, a carboxyl group, a hydroxyl group, an amino group, or an alkylamino group having 1 to carbon atoms; ##STR00064## in each of the horizontal chemical formulae represented by L.sup.1, L.sup.2, or L.sup.3 in formula (1) and formula (2) above, the left side thereof corresponds to the top side of formula (1) or formula (2) and the right side thereof corresponds to the bottom side of formula (1) or formula (2), wherein a ratio A defined by formula (I) is 0.95 or less, and wherein A=.sub.1/.sub.0 (I) in formula (I), wherein .sub.1 is a value obtained by a method comprising: measuring the absolute molecular weight and the 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 logarithms of absolute molecular weights as abscissa against logarithms of intrinsic viscosities as ordinate, approximating with formula (I-I) in the least squares sense logarithms of absolute molecular weights and logarithms of intrinsic viscosities within the range of from the logarithm of the weight-average molecular weight of the polymer to the logarithm of the z-average molecular weight of the polymer on the abscissa, and representing the slope of the straight line showing formula (I-I) by .sub.1,
log [.sub.1]=.sub.1 log M.sub.1+log K.sub.1formula (I-I) in formula (I-I), [.sub.1] represents the intrinsic viscosity (unit: dl/g) of the polymer, M.sub.1 represents the absolute molecular weight of the polymer, and K.sub.1 is a constant; and wherein in formula (I), .sub.0 is a value obtained by a method comprising: measuring the absolute molecular weight and the intrinsic viscosity of a polyethylene standard substance 1475a by gel permeation chromatography using an apparatus equipped with a light scattering detector and a viscosity detector, plotting the measured data with logarithms of absolute molecular weights as abscissa against logarithms of intrinsic viscosities as ordinate, approximating with formula (I-II) in the least squares sense logarithms of absolute molecular weights and logarithms of intrinsic viscosities within the range of from the logarithm of the weight-average molecular weight of the polyethylene standard substance 1475a to the logarithm of the z-average molecular weight of the polymer on the abscissa, and representing the slope of the straight line showing formula (I-II) by .sub.0,
log [.sub.0]=.sub.0 log M.sub.0+log K.sub.0formula (I-II) in formula (I-II), [.sub.0] represents the intrinsic viscosity (unit: dl/g) of the polyethylene standard substance 1475a, M.sub.0 represents the absolute molecular weight of the polyethylene standard substance 1475a, and K.sub.0 is a constant; and wherein in the measurement of the absolute molecular weight and the intrinsic viscosity of the polymer and the polyethylene standard substance 1475a by gel permeation chromatography, the mobile phase is orthodichlorobenzene and the measurement temperature is 155 C.

2. The polymer according to claim 1, the fusion enthalpy (H) of which observed within a temperature range of not lower than 10 C. and lower than 60 C. by differential scanning calorimetry is 50 J/g or more.

3. The polymer according to claim 1, having been crosslinked.

4. The polymer according to claim 1, having a gel fraction of 20% or more.

5. The polymer according to claim 1, wherein where the total number of all the constitutional units contained in the polymer is 100%, the total number of the units (A), the units (B), and the units (C) accounts for 90% or more.

6. A molded article comprising the polymer according to claim 1.

7. A foamed article comprising the polymer according to claim 1.

8. A resin composition comprising a polymer (1) that is the polymer according to claim 1, and a polymer (2) that is a polymer whose melting peak temperature or glass transition temperature observed by differential scanning calorimetry is 50 C. to 180 C. except for the exceptive polymers defined below, wherein where the total amount of the polymer (1) and the polymer (2) is 100% by weight, the content of the polymer (1) is 30% by weight to 99% by weight and the content of the polymer (2) is 1% by weight to 70% by weight; wherein exceptive polymer is any polymer comprising constitutional units (A) derived from ethylene and constitutional unit (B) represented by formula (1) below and optionally comprising at least one type of constitutional units (C) selected from the group consisting of constitutional units represented by formula (2) below and constitutional units represented by formula (3) below, where the total number of the units (A), the units (B), and the units (C) is 100%, the number of the units (A) accounts for 70% to 99% and the total number of the units (B) and the units (C) accounts for 1% to 30%; where the total number of the units (B) and the units (C) is 100%, the number of the units (B) accounts for 1% to 100% and the number of the units (C) accounts for 0% to 99%, ##STR00065## in formula (1), R represents a hydrogen atom or a methyl group, L.sup.1 represents COO, OCO, or O, L.sup.2 represents a single bond, CH.sub.2, CH.sub.2CH.sub.2, CH.sub.2CH.sub.2CH.sub.2, CH.sub.2CH(OH)CH.sub.2, or CH.sub.2CH(CH.sub.2OH), L.sup.3 represents a single bond, COO, OCO, O, CONH, NHCO, CONHCO, NHCONH, NH, or N(CH.sub.3), L.sup.6 represents an alkyl group having 14 to 30 carbon atoms; ##STR00066## in formula (2), R represents a hydrogen atom or a methyl group, L.sup.1 represents COO, OCO, or O, L.sup.4 represents an alkylene group having 1 to 8 carbon atoms, L.sup.5 represents a hydrogen atom, an epoxy group, CH(OH)CH.sub.2OH, a carboxyl group, a hydroxyl group, an amino group, or an alkylamino group having 1 to carbon atoms; ##STR00067## in each of the horizontal chemical formulae represented by L.sup.1, L.sup.2, or L.sup.3 in formula (1) and formula (2) above, the left side thereof corresponds to the top side of formula (1) or formula (2) and the right side thereof corresponds to the bottom side of formula (1) or formula (2).

9. The polymer according to claim 1, wherein where the total number of the units (B) and the units (C) is 100%, the number of the units (B) accounts for 60% to 100% and the number of the units (C) accounts for 0% to 40%.

10. The polymer according to claim 1, wherein where the total number of the units (A), the units (B) and the units (C) is 100%, the number of the units (A) accounts for 70% to 97.5% and the total number of the units (B) and the units (C) accounts for 2.5% to 30%.

11. The polymer according to claim 10, wherein where the total number of the units (B) and the units (C) is 100%, the number of the units (B) accounts for 60% to 100% and the number of the units (C) accounts for 0% to 40%.

Description

EXAMPLES

(1) The present invention is described in more detail below with reference to Examples and Comparative Examples. [I] Numbers (unit: c,v0) of constitutional units (A) derived from ethylene, constitutional units (B) represented by the above Formula (1), and constitutional units (C) represented by the above Formula (2) contained in a polymer

(2) A nuclear magnetic resonance spectrum (hereinafter, NMR spectrum) was measured under the measurement conditions shown below using a nuclear magnetic resonance spectrometer (NMR).

(3) <Proton Nuclear Magnetic Resonance (.sup.1H-NMR) Measurement Conditions>

(4) Device: AVANCEM 600HD manufactured by Bruker BioSpin K.K. Measurement probe: 10-mm cryoprobe Measurement solvent: 1,1,2,2-tetrachloroethane-d9 Sample concentration: 20 mg/mL Measurement temperature: 135 C. Measuring method: proton method Number of transients: 64 Pulse width: 30 degrees Pulse repetition time: 4 seconds Measurement standard: tetramethylsilane
<Carbon Nuclear Magnetic Resonance (.sup.13C-NMR) Measurement Conditions> Device: AVANCEIII 600HD manufactured by Bruker BioSpin K.K. Measurement probe: 10-mm cryoprobe Measurement solvent: mixed solvent of 1,2-dichlorobenzene/1,1,2,2-tetrachloroethane-d.sub.2=85/15 (volumetric ratio) Sample concentration: 100 mg/mL Measurement temperature: 135 C. Measurement method: proton decoupling method Number of transients: 256 Pulse width: 45 degrees Pulse repetition time: 4 seconds Measurement standard: tetramethylsilane
<Numbers of Constitutional Units (A.sub.1) Derived from Ethylene and Constitutional Units (C.sub.1) Derived from Methyl Acrylate Contained in an Ethylene-methyl Acrylate Copolymer>(Unit: %)

(5) For the .sup.13C-NMR. spectrum of an ethylene-methyl acrylate copolymer measured under the above-described .sup.13C-NMR. measurement conditions, integral values within the following ranges a.sub.1, b.sub.1, c.sub.1, d.sub.1, and e.sub.1, and then the numbers of constitutional units (A.sub.1) derived from ethylene and the constitutional units (C.sub.1) derived from methyl acrylate were calculated from the contents (numbers) of three types of diad (EE, EA, AA) calculated from the following formulae. Herein, EE represents ethylene-ethylene diad, EA represents ethylene-methyl acrylate diad, and AA represents methyl acrylate-methyl acrylate diad. a.sub.1: 28.1-30.5 ppm b.sub.1: 31.9-32.6 ppm c.sub.1: 41.7 ppm d.sub.1: 43.1-44.2 ppm e.sub.1: 45.0-46.5 ppm EE=a.sub.1/4+b.sub.1/2 EA=e.sub.1 AA=c.sub.1+d.sub.1

(6) The number of constitutional units (A.sub.1)=100the number of constitutional units (C.sub.1)

(7) The number of constitutional units (C.sub.1)=100(EA/2+AA)/(EE+EA+AA)

(8) <Conversion (X.sub.1) of Constitutional Units (C.sub.1) Derived from Methyl Acrylate to Constitutional Units (B.sub.2) Represented by Formula (1)>(Unit: %)

(9) In an example in which there was obtained a polymer composed of constitutional units (A.sub.2) derived from ethylene, constitutional units (B.sub.2) represented by Formula (1), and constitutional units (C.sub.2) derived from methyl acrylate by reacting an ethylene-methyl acrylate copolymer with a long chain alkyl alcohol, integral values within the ranges f.sub.1 and g.sub.1 given below were determined for a .sup.13C-NMR spectrum of the polymer measured under the .sup.13C-NMR measurement conditions shown above. Then, a conversion (X.sub.1) with which the constitutional units (C.sub.1) derived from methyl acrylate contained in the ethylene-methyl acrylate copolymer were converted to the constitutional units (B.sub.2) represented by Formula (1) of the polymer was calculated from the formula given below. f.sub.1: 50.6-51.1 ppm g.sub.1: 63.9-64.8 ppm
Conversion(X.sub.1)=100g.sub.1/(f.sub.1+g.sub.1)
<Numbers of Constitutional Units (A.sub.2) Derived from Ethylene, Constitutional Units (B.sub.2) Represented by the Formula (1), and Constitutional Units (C.sub.2) Derived from Methyl Acrylate Contained in a Polymer>(Unit: %)

(10) The number of constitutional units (A.sub.2) derived from ethylene, the number of constitutional units (B.sub.2) represented by the Formula (1), and the number of constitutional units (C.sub.2) derived from methyl acrylate contained in a polymer were calculated from the following formulae, respectively.

(11) The number of constitutional units (A.sub.2) contained in a polymer=the number of constitutional units (A.sub.1) contained in an ethylene-methyl acrylate copolymer

(12) The number of constitutional units (B.sub.2) contained in a polymer=(the number of constitutional units (C.sub.1) contained in an ethylene-methyl acrylate copolymer)conversion (X.sub.1)/100

(13) The number of constitutional units (C.sub.2) contained in a polymer=(the number of constitutional units (C.sub.1) contained in an ethylene-methyl acrylate copolymer)(the number of constitutional units (B.sub.2) contained in a polymer)

(14) As to a polymer produced using an ethylene-ethyl acrylate copolymer instead of an ethylene-methyl acrylate, the constitutional units (A.sub.2), (B.sub.2), and (C.sub.2) were calculated in the same manner except that the integration range f.sub.1 to 59.6-60.1 ppm.

(15) <Numbers of Constitutional Units (A.sub.3) Derived from Ethylene and Constitutional Units (C.sub.3) Derived from Methyl Methacrylate Contained in an Ethylene-methyl Methacrylate Copolymer>(Unit: %)

(16) For the .sup.13C-NMR spectrum of an ethylene-methyl methacrylate copolymer measured under the above-described .sup.13C-NMR measurement conditions, integral values within the following ranges a.sub.2, b.sub.2, c.sub.2, and d.sub.2, and then the numbers of constitutional units (A.sub.3) derived from ethylene and the constitutional units (C.sub.3) derived from methyl methacrylate were calculated from the contents (numbers) of three types of diad (EE, EM, MM) calculated from the following formulae.

(17) Herein, EE represents ethylene-ethylene diad, EM represents ethylene-methyl methacrylate diad, and MM represents methyl methacrylate-methyl methacrylate diad. a.sub.2: 28.1-31.5 ppm b.sub.2: 44.5-45.0 ppm c.sub.2: 45.0-46.0 ppm d.sub.2: 46.0-47.0 ppm EE=a.sub.2/4 EM=d.sub.2 MM=b.sub.2+C.sub.2

(18) The number of constitutional units (A.sub.3)=100the number of constitutional units (C.sub.3)

(19) The number of constitutional units (C.sub.3)=100(EM/2+MM)/(EE+EM+MM)

(20) <Conversion (X.sub.2) of Constitutional Units (C.sub.3) Derived from Methyl Methacrylate to Constitutional Units (B.sub.4) Represented by Formula (1)>(Unit: %)

(21) In an example in which there was obtained a polymer composed of constitutional units (A.sub.4) derived from ethylene, constitutional units (B.sub.4) represented by Formula (1), and constitutional units (C.sub.4) derived from methyl methacrylate by reacting an ethylene-methyl methacrylate copolymer with a long chain alkyl alcohol, integral values within the ranges f.sub.2 and g.sub.2 given below were determined for a .sup.13C-NMR spectrum of the polymer measured under the .sup.13C-NMR measurement conditions shown above. Then, a conversion (X.sub.2) with which the constitutional units (C.sub.3) derived from methyl methacrylate contained in the ethylene-methyl methacrylate copolymer were converted to the constitutional units (B.sub.4) represented by Formula (1) of the polymer was calculated from the formula given below. f.sub.2: 50.6-51.1 ppm g.sub.2: 63.9-64.8 ppm
Conversion(X.sub.2)=100g.sub.2/(f.sub.2+g.sub.2)
<Numbers of Constitutional Units (A4) Derived from Ethylene, Constitutional Units (B.sub.4) Represented by the Formula (1), and Constitutional Units (C.sub.4) Derived from Methyl Methacrylate Contained in a Polymer>(Unit: %)

(22) The number of constitutional units (A.sub.4) derived from ethylene, the number of constitutional units (B.sub.4) represented by the Formula (1), and the number of constitutional units (C.sub.4) derived from methyl acrylate contained in the polymer were calculated from the following formulae, respectively

(23) The number of constitutional units (A.sub.4) contained in a polymer=the number of constitutional units (A.sub.3) contained in an ethylene-methyl methacrylate copolymer

(24) The number of constitutional units (B.sub.4) contained in a polymer=(the number of constitutional units (C.sub.3) contained in an ethylene-methyl methacrylate copolymer)conversion (X.sub.2)/100

(25) The number of constitutional units (C.sub.4) contained in a polymer=(the number of constitutional units (C.sub.3) contained in an ethylene-methyl methacrylate copolymer)(the number of constitutional units (B.sub.4) contained in a polymer)

(26) <Numbers of Constitutional Units (A.sub.5) Derived from Ethylene and Constitutional Units (C.sub.5) Derived from Glycidyl Methacrylate Contained in an Ethylene-glycidyl Methacrylate Copolymer>(Unit: %)

(27) For the .sup.1H-NMR spectrum of an ethylene-glycidyl methacrylate copolymer measured under the above-described .sup.1H-NMR measurement conditions, integral values within the following ranges a.sub.3, b.sub.3, c.sub.3, d.sub.3, e.sub.3, and f.sub.3, and then the numbers of constitutional units (A.sub.5) derived from ethylene and the constitutional units (C.sub.5) derived from glycidyl methacrylate were calculated from the following formulae. a.sub.3: 0.30-2.15 ppm b.sub.3: 2.50-2.68 ppm c.sub.3: 2.68-2.86 ppm d.sub.3: 3.00-3.22 ppm e.sub.3: 3.93-4.01 ppm f.sub.3: 4.23-4.36 ppm

(28) The number of constitutional units (A.sub.5)=the number of (a.sub.3C.sub.55)/4

(29) The number of constitutional units (C.sub.5)=the number of (b.sub.3+c.sub.a+d.sub.3+e.sub.3+f.sub.3)/5

(30) <Conversion (X.sub.3) of Constitutional Units (C.sub.5) Derived from Glycidyl Methacrylate to Constitutional Units (B.sub.6) Represented by Formula (1)>(Unit: %)

(31) In an example in which there was obtained a polymer composed of constitutional units (A.sub.6) derived from ethylene, constitutional units (B.sub.6) represented by Formula (1), and constitutional units (C.sub.6) derived from glycidyl methacrylate by reacting an ethylene-glycidyl methacrylate copolymer with a long chain alkyl carboxylic acid, integral values within the ranges X, Y and Z given below were determined for a .sup.1H-NMR. spectrum of the polymer measured under the .sup.1H-NMR measurement conditions shown above. Subsequently, the constitutional units (B.sub.6) derived from the long chain alkyl carboxylic acid (the total of the positional isomers B.sub.6-1 and B.sub.6-2 of the addition reaction) was calculated from the following formulas. W: 3.10-3.30 ppm X: 3.55-4.05 ppm Y: 4.05-4.80 ppm Z: 5.00-5.40 ppm

(32) Constitutional units (B.sub.6-1)=((X-2Z)+(Y-2W-2Z)/4)/2

(33) Constitutional units (B.sub.6-2)=Z

(34) Constitutional units (C.sub.6)=W
Conversion(X.sub.3)=100(B.sub.6-1+B.sub.6-2)/(B.sub.6-1+B.sub.6-2+C.sub.6)
<Numbers of Constitutional Units (A.sub.6) Derived from Ethylene, Constitutional Units (B.sub.6) Represented by the Formula (1), and Constitutional Units (C.sub.6) Derived from Glycidyl Methacrylate Contained in a Polymer>(Unit: %)

(35) The number of constitutional units (A.sub.6) derived from ethylene, the number of constitutional units (B.sub.6) represented by the Formula (1), and the number of constitutional units (C.sub.6) derived from glycidyl methacrylate contained in the polymer were calculated from the following formulae, respectively.

(36) The number of constitutional units (A.sub.6) contained in a polymer=the number of constitutional units (A.sub.5) contained in an ethylene-glycidyl methacrylate copolymer

(37) The number of constitutional units (B.sub.6) contained in a polymer=(the number of constitutional units (C.sub.5) contained in an ethylene-glycidyl methacrylate copolymer)conversion (X.sub.3)/100

(38) The number of constitutional units (C.sub.6) contained in a polymer=(the number of constitutional units (C.sub.5) contained in an ethylene-glycidyl methacrylate copolymer)(the number of constitutional units (B.sub.6) contained in a polymer) [II] Content of unreacted compound having an alkyl group having 14 to 30 carbon atoms (unit: % by Weight)

(39) In Production of polymer in each Example, the product obtained is a mixture of the polymer and the unreacted compound having an alkyl group having 14 to 30 carbon atoms. The content of the unreacted compound having an alkyl group having 14 to 30 carbon atoms contained in the product was measured by the following method using gas chromatography (GC). The content of the unreacted compound is a value determined when the total weight of the resulting polymer and the unreacted compound is 100% by weight. [GC measurement conditions] GC device: Shimadzu GC2014 Column: DB-5MS (60 m, 0.25 mmphi, 1.0 m) Column temperature: A column held at 40 C. is heated to 300 C. at a rate of 10C/min and then held at 300 C. for 40 minutes. Vaporizing chamber/detector temperature: 300 C./300 C. (FID) Carrier gas: helium Pressure: 220 kPa Full flow: 17.0 mL/min Column flow rate: 1.99 mL/min Purge flow rate: 3.0 mL/min Line speed: 31.8 mm/sec Injection system/split ratio: split injection/6:1 Injection amount: 1 L Sample preparation method: 8 mg/mL (o-dichlorobenzene solution) (1) Production of calibration curve [Solution preparation]

(40) Into a 9-mL vial tube was weighed 5 mg of a standard, then 100 mg of n-tridecane was weighed thereinto as an internal standard substance, and then 6 mL of o-dichlorobenzene was added as a solvent to dissolve the sample completely, and thus a standard solution for production of a calibration curve was obtained. Two additional standard solutions were prepared in the same manner as above except that the amount of the standard was changed to 25 mm and 50 mm.

(41) [GC Measurement]

(42) A standard solution for producing a calibration curve was measured under the GC measurement conditions described above, and a calibration curve in which the GC area ratio of the standard and the internal standard substance was plotted on the ordinate and the weight ratio of the weight of the standard and the weight of the internal standard substance was plotted on the abscissa, and then the slope a of the calibration curve was determined. (2) Measurement of content of an object to be measured (unreacted compound having an alkyl group having 14 to 30 carbon atoms) in a sample (product)
[Solution Preparation]

(43) Into a 9-mL vial tube were weighed 50 nag of a sample and 100 mg of n-tridecane, and 6 mL of o-dichlorobenzene was added to completely dissolve the sample at 80 C., and thus a sample solution was obtained.

(44) [GC Measurement]

(45) The sample solution was measured under the GC measurement conditions specified above, and then the content Ps of the object to be measured in the sample was calculated according to the following formula. P.sub.S: Content of an object to be measured contained in a sample (% by weight) W.sub.S: Weight of the sample (mg) W.sub.IS: Weight of the internal standard substance (IS) (mg) A.sub.S: Peak area count number of the object to be measured A.sub.IS: Peak area count number of the internal standard substance (IS) A: Slope of the calibration curve of the object to be measured

(46) $P_S=\frac{W_{\mathrm{IS}}{A}_S}{W_S{A}_{\mathrm{IS}}a}100$
[III] Method of Evaluating Physical Properties of Polymer (1) Melting peak temperature (T.sub.m, unit: C.), melting enthalpy (H, unit: J/g) observed within a temperature range of from 10 C. (inclusive) to 60 C. (exclusive)

(47) An aluminum pan in which about 5 mg of a sample was enclosed was (1) held at 150 C. for 5 minutes, then (2) cooled from 150 C. to 50 C. at a rate of 5 C./minute, then (3) held at 50 C. for 5 minutes, and then (4) heated from 50 C. to about 150 C. at a rate of 5 C./minute, using a differential scanning calorimeter (DSC Q100 manufactured by TA Instruments) under nitrogen atmosphere. The differential scanning calorimetry curve produced by the calorimetric measurement in the step (4) was defined as a melt curve. The melt curve was analyzed by the method in accordance with JIS K7121-1987 and a melting peak temperature was determined. The melting enthalpy H (J/g) was determined by analyzing the portion of the melt curve within the temperature range of from 10 C. (inclusive) to 60 C. (exclusive) by the method in accordance with JIS K7122-1987. (2) Ratio A defined by formula (I) (unit: none)

(48) The absolute molecular weight and the intrinsic viscosity of each of the polymer and the polyethylene standard substance 1475a (available from National Institute of Standards and Technology) were measured by gel permeation chromatography (GPC) using an apparatus equipped with a light scattering detector and a viscosity detector. GPC device: HLC-8121 GPC/HT manufactured by TOSOH Corporation Light scattering detector: Precision Detectors PD2040 Differential pressure viscosity detector: Viscotek H502 GPC column: GMHHR-H(S) HT three columns, produced by TOSOH Corporation Sample solution concentration: 2 mg/mL Injection amount: 0.3 L. Measurement temperature: 155 C. Dissolution conditions: 145 C., 2 hr Mobile phase: orthodichlorobenzene (with addition of 0.5 mg/mL of BHT) Flow rate during elution: 1 mL/minute Measurement time: about 1 hour
[GPC Device]

(49) As a GPC device equipped with a differential refractometer (RI), HLC-8121 GPC/HT manufactured by TOSOH Corporation was used. PD2040 manufactured by Precision Detectors was connected as a light scattering detector (LS) to the GPC device. The scattering angle used for light scattering detection was 90. H502 manufactured by Viscotek was connected as a viscosity detector (VISC) to the GPC device. LS and VISC were installed in the column oven of the GPC device and were connected in order of LS, RI, and VISC. For the calibration of LS and VISC and the correction of the delay volume between the detectors, a polystyrene standard substance Polycal TDS-PS-N (weight average molecular weight Mw: 104,349, polydispersity: 1.04) produced by Malvern was used at a solution concentration of 1 mg/mL. As the mobile phase and the solvent, orthodichlorobenzene to which dibutylhydroxytoluene had been added as stabilizer at a concentration of 0.5 mg/mL was used. The conditions for dissolving the sample were 145 C. and 2 hours. The flow rate was adjusted to 1 mL/minute. Three columns, GMHHR-H(S) HT manufactured by TOSOH Corporation, connected in series were used. The temperatures of the column, the sample injection part, and the detectors were adjusted to 155 C. The sample solution concentration was adjusted to 2 mg/mL. The injection amount (sample loop volume) of the sample solution was adjusted to 0.3 mL. The refractive index increment (dn/dc) of NIST1475a and the sample in orthodichlorobenzene was adjusted to 0.078 mL/g. The dn/dc of the polystyrene standard substance was adjusted to 0.079 mL/g. In determining an absolute molecular weight and an intrinsic viscosity ([]) from the data of the respective detectors, calculation was carried out using data-processing software OmniSEC (version 4.7) available from Malvern with reference to the document Size Exclusion Chromatography, Springer (1999). The refractive index increment is a rate of change of the refractive index relative to the concentration change.

(50) .sub.1 and a.sub.0 in Formula (I) were calculated by the method described below, and both of them were substituted into Formula (I) to calculate A.
A=.sub.1/.sub.0(I)

(51) .sub.1 is a value obtained by a method comprising plotting the measured data with logarithms of molecular weights of the polymer as abscissa versus logarithms of intrinsic viscosities of the polymer as ordinate, approximating in the least squares sense logarithms of absolute molecular weights and logarithms of intrinsic viscosities within the range of from the logarithm of the weight-average molecular weight of the polymer to the logarithm of the z-average molecular weight of the polymer on the abscissa, and representing the slope of the straight line showing Formula (I-I) by .sub.1,
log [.sub.1]=.sub.1 log M.sub.1+log K.sub.1(I-I)
in Formula (I-I), [.sub.1] represents the intrinsic viscosity (unit: dl/g) of the polymer, M.sub.1 represents the absolute molecular weight of the polymer, and K.sub.1 is a constant. A value obtained by a method comprising plotting the measured data with logarithm of logarithms of absolute molecular weights of the polyethylene standard substance 1475 as abscissa versus logarithms of intrinsic viscosities of the polyethylene standard substance 1475 as ordinate, approximating in the least squares sense logarithms of absolute molecular weights and logarithms of intrinsic viscosities within the range of from the logarithm of the weight-average molecular weight of the polyethylene standard substance 1475 to the logarithm of the z-average molecular weight of the polyethylene standard substance 1475 on the abscissa, and representing the slope of the straight line showing Formula (I-II) by .sub.0,
log [.sub.0]=.sub.0 log M.sub.0+log K.sub.0(I-II)
In Formula (I-II), [.sub.0] represents the intrinsic viscosity (unit Wg) of the polyethylene standard substance 1475a, M.sub.0 represents the absolute molecular weight of the polyethylene standard substance 1475a, and K.sub.0 is a constant. (3) Activation energy of flow (E.sub.a, unit: kJ/mol)

(52) The activation energy of flow Ea was determined by the method described below. Using a strain controlling type rotary viscometer (rheometer), a melt complex viscosity-angular frequency curve of the polymer was measured under the following conditions (a) to (d). The above-mentioned melt complex viscosity-angular frequency curve is a log-log curve in which the melt complex viscosity (unit: Pa.Math.sec) is plotted on the ordinate and the angular frequency (unit: rad/sec) is plotted on the abscissa. Measurement was carried out under nitrogen. Condition (a) Geometry: parallel plate; diameter: 25 mm, plate distance: 1.5 to 2 mm Condition (b) Strain: 5% Condition (c) Shear rate: 0.1 to 100 rad/sec Condition (d) Temperature: 170, 150, 130, 110, 90 C.

(53) Then, for each of the melt complex viscosity-angular frequency curves measured at the individual temperatures other than 170 C., the angular frequency was multiplied by aT and the melt complex viscosity was multiplied by 1/a.sub.T such that the curve superposed the melt complex viscosity-angular frequency curve at 170 C. a.sub.T was determined such that the melt complex viscosity-angular frequency curves at the individual temperatures other than 170 C. superposed the melt complex viscosity-angular frequency curve at 170 C.

(54) Then, at each temperature (T), [ln(a.sub.T)] and [1/(T+273.16)] were determined and [ln(a.sub.T)] and [1/(T+273.16)] were approximated in the least squares sense by the following Formula (II), and then the slope m of the straight line showing Formula (II) was determined. The m was substituted into the following Formula (III) and Ea was calculated.
ln(a.sub.T)=m(1/(T+273.16))+n(II)
E.sub.a=|10.008314m|(III) a.sub.T: shift factor E.sub.a: activation energy of flow (unit: kJ/mol) T: temperature (unit: OC)

(55) Using Ochestrator produced by TA Instruments as calculation software, there was adopted an E.sub.a value in the case that the correlation factor r2 in approximating [ln(a.sub.T)] and [1/T+273.16)] in the least squares sense by Formula (II) is 0.9 or more. (4) Extensional viscosity nonlinear index (k, unit: none)

(56) The extensional viscosity nonlinear index k was determined by the method described below.

(57) There were measured a viscosity .sub.1(t) of a polymer at an extension time t when the polymer was uniaxially stretched at a temperature of 110 C. at a strain rate of 1 sec.sup.1 under a nitrogen atmosphere using a viscoelasticity measuring apparatus (ARES manufactured by TA instruments), and a viscosity .sub.E0.1(t) of the polymer at an extension time t when the polymer was uniaxially stretched at a temperature of 110 C. at a strain rate of 0.1 sec.sup.1. The .sub.E1 (t) and the .sub.E0.1 (t) measured at an arbitrary same extension time t were substituted into the following formula to calculate (t).
(t)=.sub.E1 (t)/.sub.E 0.1(t)

(58) The logarithm of (t) (ln((t))) was plotted versus the extension time t, and ln((t)) an t were approximated in the least squares sense using the following formula within a range oft of from 2.0 sec to 2.5 sec. The slope of the straight line showing the following formula is k.
ln((t))=kt

(59) There was adopted k in the case where the correlation function r2 used for performing approximation in the least squares sense using the above formula was 0.9 or more. (5) Molding processability

(60) Each of the specimens (20 mm in length, 20 mm in width, 1 mm in thickness) prepared by compression molding under the conditions described in Examples and Comparative Examples was subjected to D hardness measurement using a Durometer Hardness tester (DIGITAL HARDNESS TESTER MODEL RH-305A, manufactured by EXCEL) in accordance with JIS K7215, and it was checked whether the specimen cracked during the measurement.

(61) In addition, a specimen (20 mm in length, 20 mm in width, 1 mm in thickness) was put on a glass plate (MICRO SLIDE GLASS produced by Matsunami Glass Ind., Ltd.; 91 mm in length, 26 mm in width, 0.9 to 1.2 mm in thickness) at the plane center thereof and was left standing in a gear oven at 40 C. for 30 minutes. Then, the glass plate was taken out of the gear oven and was left standing at 23 C. for 30 minutes. Then, the glass plate was made to stand with its longitudinal axis stood vertically, and at that time it was examined whether the specimen fell down without adhering to the glass plate.

(62) A specimen which did not fracture and failed to adhere to the glass plate was judged to be very good in molding processability and this was expressed by the symbol . A specimen which did not fracture but adhered to the glass plate was judged to be good in molding processability and this was expressed by the symbol . A specimen which fractured was judged to be poor in molding processability and this was expressed by the symbol . The specimens which fractured were judged to be poor in molding processability and were not subjected to the adhesion evaluation. (6) Shape retention

(63) As the shape retention after a polymer phase-transferred from crystals to amorphous, shape retention at 90 C., which is higher than the melting peak temperature of the polymer, was evaluated. Each of the specimens prepared by compression molding under the conditions described in Examples and Comparative Examples (20 mm in length, 20 mm in width, 1 mm in thickness) was put on the plane center of a glass plate (MICRO SLIDE GLASS produced by Matsunami Glass Ind., Ltd.; 91 mm in length, 26 mm in width, 0.9 to 1.2 mm in thickness) and was left standing in a gear oven at 90 C. for 30 minutes, and then change in shape of the specimen was evaluated. A specimen with which no change in shape, such as crack, shrinkage, or settling, was observed is judged as being good in shape retention and this is expressed by the symbol . A specimen with which change in shape was observed is judged as being poor in shape retention, and this is expressed by the symbol . (7) Water vapor transmission rate per a thickness of 1 mm (unit: gmm/m.sup.2/24 hours)

(64) Using the specimens produced by compression molding under the conditions described in Examples and Comparative Examples (0.5 mm in thickness for Examples 1, 2, 4 and Comparative Examples 3, 4; 1.0 mm in thickness for Examples 5, 6, 7, 9, 10, 11, 12, 13), measurement was performed at 23 C. and 90 (NRH according to JIS K7129B using a water vapor transmission analyzer (PERMATRAN-W 3/33, manufactured by MOCON). The measured water vapor transmission rate (g/m.sup.2/24 hours) was converted into a water vapor transmission rate per a thickness of 1 mm, and thus a water vapor transmission rate per a thickness of 1 mm (gmm/m.sup.2/24 hours) was calculated.

(65) [IV Method for Evaluating Physical Properties of Crosslinked Polymer

(66) (1) Gel fraction (unit: % by weight)

(67) About 500 mg of each of the crosslinked polymers prepared under the conditions described in Examples and Comparative Examples as a measurement sample, and an empty net basket made of wire net (opening: 400 meshes) were weighed, respectively. A net basket containing the crosslinked polymer and 50 mL of xylene (produced by Kanto Chemical Co., Inc., Cica Special Grade; a mixture of o-, m-, and p-xylene and ethylbenzene; the total content of o-, m-, and p-xylene was 85% by weight more) were introduced into a 100-mL test tube, followed by heated extraction at 110 C. for 6 hours. After the extraction, the net basket containing extraction residue was picked out of the test tube, followed by drying under reduced pressure at 80 C. for 8 hours in a vacuum dryer, and then the net basket containing the extraction residue after drying was weighed. The gel weight was calculated from the weight difference of the net basket containing extraction residue after drying and the empty net basket. The gel fraction (% by weight) was calculated based on the following formula.
Gel fraction=(weight of gel/weight of measured sample)100
[V] Method of Evaluating Physical Properties of Foamed Article (1) Gel fraction (unit: % by weight)

(68) About 500 mg of each of the foamed articles prepared under the conditions described in Examples and Comparative Examples as a measurement sample, and an empty net basket made of wire net (opening: 400 meshes) were weighed, respectively. A net basket containing a foamed article and 50 mL of xylene (produced by Kanto Chemical Co., Inc., Cica Special Grade; a mixture of o-, m-, and p-xylene and ethylbenzene; the total content of o-, m-, and p-xylene was 85% by weight more) were introduced into a 100-mL test tube, followed by heated extraction at 110 C. for 6 hours. After the extraction, the net basket containing extraction residue was dried under reduced pressure at 80 C. for 8 hours in a vacuum dryer, and then the net basket containing the extraction residue after drying was weighed. The gel weight was calculated from the weight difference of the net basket containing extraction residue after drying and the empty net basket. The gel fraction (% by weight) was calculated based on the following formula.
Gel fraction=(weight of gel/weight of measured sample)100 (2) Foamability

(69) For the foamed articles prepared under the conditions described in Examples and Comparative Examples, one having an expansion ratio of 2 or more is expressed by , and one having an expansion ratio of less than 2 or the case that no foamed article was obtained is expressed by .

(70) [VI] Method for Evaluating Physical Properties of a Crosslinked Resin Composition

(71) (1) Melting peak temperature (T.sub.m, unit: C.), melting enthalpy (H, unit: J/g) of from 10 C. (inclusive) to 60 C. (exclusive)

(72) An aluminum pan in which about 5 mg of a sample was enclosed was (1) held at 200 C. for 5 minutes, then (2) cooled from 200 C. to 50 C. at a rate of 5 C./minute, then (3) held at 50 C. for 5 minutes, and then (4) heated from 50 C. to about 200 C. at a rate of 5 C./minute, using a differential scanning calorimeter (DSC Q100 manufactured by TA Instruments) under nitrogen atmosphere. The differential scanning calorimetry curve produced by the calorimetric measurement in the step (4) was defined as the melt curve. The melt curve was analyzed by the method in accordance with JIS K7121-1987 and a melting peak temperature was determined.

(73) The melting enthalpy H (J/g) was determined by analyzing the portion of the melt curve within the temperature range of from 10 C. (inclusive) to 60 C. (exclusive) by the method in accordance with JIS K7122-1987. (2) Permanent compression set (unit: %)

(74) Measurement was conducted in accordance with JIS K6262 under conditions including a test temperature of 70 C., a compression ratio of 25%, and a test time of 22 hours. [VII] Raw materials
<Copolymer having Constitutional Units (A) and Constitutional Units (C)> A-1: Ethylene-methyl acrylate copolymer Acryft CG4002 (produced by

(75) Sumitomo Chemical Co., Ltd.), the number of constitutional units derived from ethylene: 88.9% (72.4% by weight), the number of constitutional units derived from methyl acrylate: 11.1% (27.6% by weight), MFR (measured at 190 C. and 21 N): 6.0 g/10 minutes A-1: Ethylene-methyl acrylate copolymer

(76) The ethylene-methyl acrylate copolymer A-1 was produced as follows.

(77) In an autoclave type 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, and thus an ethylene-methyl acrylate copolymer A-1 was obtained. The composition and the MFR of the resulting copolymer A-1 were as follows. The number of constitutional units derived from ethylene: 87.1% (68.8% by weight), the number of constitutional units derived from methyl acrylate: 12.9% (31.2% by weight), MFR. (measured at 190 C. and 21 N): 40.5 g/10 minutes A-1: Ethylene-methyl methacrylate copolymer

(78) The ethylene-methyl methacrylate copolymer A-1 was produced as follows.

(79) In an autoclave type reactor, ethylene and methyl methacrylate were copolymerized using tert-butyl peroxypivalate as a radical polymerization initiator, at a reaction temperature of 202 C. and a reaction pressure of 199 MPa, and thus an ethylene-methyl methacrylate copolymer A-1 was obtained. The composition and the MFR of the resulting copolymer A-1 were as follows. The number of constitutional units derived from ethylene: 88.8% (69.0% by weight), the number of constitutional units derived from methyl methacrylate: 11.2 (31.0% by weight), MFR (measured at 190 C. and 21 N): 40.0 g/10 minutes A-2: Ethylene-ethyl acrylate copolymer NUC-6570 (produced by NUC), the number of constitutional units derived from ethylene: 92.2% (76.8% by weight), the number of constitutional units derived from ethyl acrylate: 7.8% (23.2% by weight), MFR (measured at 190 C. and 21 N): 20 g/10 minutes A-3: Ethylene-glycidyl methacrylate copolymer Bondfast 20C (produced by Sumitomo Chemical Co., Ltd.), the number of constitutional units derived from ethylene: 95.3% (80.0% by weight), the number of constitutional units derived from glycidyl methacrylate: 4.7% (20.0% by weight), MFR (measured at 190 C. and 21 N): 13 g/10 minutes
<Compound having an Alkyl Group having 14 to 30 Carbon Atoms> B-1: KALCOL 220-80 (a mixture of n-docosyl alcohol, n-eicosyl alcohol, and n-octadecyl alcohol) (produced by Kao Corporation) B-2: n-Eicosyl alcohol (produced by Tokyo Chemical Industry Co., Ltd.) B-3: KALCOL 8098 (n-octadecyl alcohol) (produced by Kao Corporation) B-3: n-Octadecyl alcohol (produced by Tokyo Chemical Industry Co., Ltd.) B-4: KALCOL 6098 (n-hexadecyl alcohol) (produced by Kao Corporation) B-5: KAT,COL 4098 (n-tetradecyl alcohol) (produced by Kao Corporation) B-6: n-Octadecanoic acid (produced by Tokyo Chemical Industry Co., Ltd.)
<Catalyst> C-1: Tetra(n-butyl) orthotitanate (produced by Tokyo Chemical Industry Co., Ltd.) C-2: Tetra(n-octadecyl) orthotitanate (produced by Tokyo Chemical Industry Co., Ltd.)
<Olefin Polymer> D-1: SUMITOMO NOBLEN D101 (propylene homopolymer, melting point: 163 C.) (produced by Sumitomo Chemical Co., Ltd.) D-2: SUMITOMO NOBLEN 5131 (propylene random copolymer, melting point: 132 C.) (produced by Sumitomo Chemical Co., Ltd.) D-3: HI-ZEX 3300F (high-density polyethylene, melting point: 132 C.) (produced by Prime Polymer Co., Ltd.)
<Organic Peroxide> E-1: PERCUMYL D (dicumyl peroxide) (one-minute half-life temperature: 175 C.) (produced by NOF Corporation) E-2: PERHEXYL I (tert-hexylperoxyisopropyl monocarbonate) (one-minute half-life temperature: 155 C.) (produced by NOF Corporation) E-3: Kayahexa AD-40C (mixture comprising 2,5-dimethyl-2,5-di(tert-butylperoxy)hexane, calcium carbonate, and amorphous silicon dioxide) (one-minute half-life temperature: 180 C.) (produced by Kayaku Akzo Corporation)
<Crosslinking Aid> F-1: Hi-Cross MS50 (mixture of trimethylolpropane trimethacrylate and amorphous silicon dioxide) (produced by Seiko Chemical Co., Ltd.)
<Foaming Agent> G-1: CELLMIC CAP (mixture comprising azodicarbonamide and dinitrosopentamethylenetetramine) (decomposition temperature: 125 to 130 C.) (produced by Sankyo Kasei Co., Ltd.)
<Additives> H-1: Zinc stearate (produced by Nitto Kasei Kogyo K. K.) H-2: Zinc oxide (produced by Honjo Chemical Corporation)
<Antioxidant> I-1: IRGANOX 1010 (pentaerythritol-tetrakis[3-(3,5-di-tert-butyl-4-hydroxyphenyl) propionate]) (produced by BASF A.G.)
<Processing Heat Stabilizer> J-1: IRGAFOS 168 (tris(2,4-di-tert-butylphenyl)phosphite) (produced by BASF A.G.)

Example 1

(80) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-eicosyl acrylate-methyl acrylate copolymer)

(81) In a 3-L separable flask, 150 g (40.5 parts by weight) of copolymer A-1, 170 g (46.0 parts by weight) of compound B-2, and 50 mL (13.5 parts by weight) of catalyst C-1 were dissolved in 880 mL of heptane and were stirred under a nitrogen atmosphere at 100 C. for 3 hours, and then the mixture was reprecipitated in 5 L of ethanol, affording a polymer (ex1, ethylene-n-eicosyl acrylate-methyl acrylate copolymer). Moreover, the polymer (ex1) was compression molded at 100 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the polymer (ex1) are shown in Table 1. (2) Preparation of resin composition comprising polymer (ex1) and organic peroxide

(82) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex1) obtained in Example 1 (1) and 2.0 parts by weight of an organic peroxide E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex1) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(83) The resin composition obtained in Example 1 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex1-1) was obtained. The gel fraction of the crosslinked polymer (ex1-1) is shown in Table 1. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(84) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex1) obtained in Example 1 (1), 2.0 parts by weight of an organic peroxide E-1, 8.2 parts by weight of a foaming agent, 2.0 parts by weight of an additive X-1, and 1.0 part by weight of an additive H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex1), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(85) The resin composition obtained in Example 1 (4) was filled into a mold having dimensions of 45 mm45 mm5 mm and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 1.

Example 2

(86) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-eicosyl acrylate-methyl acrylate copolymer)

(87) In 500 mL of xylene were dissolved 60 g (26.0 parts by weight) of A-1, 151 g (65.3 parts by weight) of B-2, and 20 mL (8.7 parts by weight) of C-1, which were then stirred under a nitrogen atmosphere in a 3-L separable flask at 150 C. for 3 hours, and then the mixture was reprecipitated in 3 L of ethanol, affording a polymer (ex2, ethylene-n-eicosyl acrylate-methyl acrylate copolymer). Moreover, the polymer (ex2) was compression molded at 100 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the polymer (ex2) are shown in Table 1.

Example 3

(88) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-hexadecyl acrylate-ethyl acrylate copolymer)

(89) 45.4 g (56.8 parts by weight) of A-2, 30.7 g (38.4 parts by weight) of B-3, and 3.9 g (4.9 parts by weight) of C-1 were kneaded with a Labo Plastomill (Model 65C150, manufactured by Toyo Seiki Seisaku-sho, Ltd.) under a nitrogen atmosphere, at a rotation speed of 60 rpm, at a chamber temperature of 150 C., for 20 minutes. The resulting mixture was dissolved in 100 mL of xylene at 100 C. and then was reprecipitated in 500 mL of ethanol, affording a polymer (ex3, ethylene-n-hexadecyl acrylate-ethyl acrylate copolymer). Moreover, the polymer (ex3) was compression molded at 100 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex3) are shown in Table 1.

Example 4

(90) (1) Production of polymer composed of constitutional units (A) and constitutional units (B) (reaction product of ethylene-glycidyl methacrylate copolymer/n-octadecanoic acid)

(91) 50.7 g (72.5 parts by weight) of A-3 and 19.3 g (27.5 parts by weight) of B-6 were kneaded with a Labo Plastomill (Model 65C150, manufactured by Toyo Seiki Seisaku-sho, Ltd.) under a nitrogen atmosphere, at a rotation speed of 80 rpm, at a chamber temperature of 200 C., for 10 minutes. The resulting mixture was dissolved in 100 mL of xylene at 100 C. and then was reprecipitated in 500 mL of ethanol, affording a polymer (ex4) (reaction product of ethylene-glycidyl methacrylate copolymer/n-hexadecanoic acid). Moreover, the polymer (ex4) was compression molded at 210 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the polymer (ex4) are shown in Table 1. (2) Preparation of resin composition comprising polymer and organic peroxide

(92) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex4) obtained in Example 4 (1) and 2.0 parts by weight of an organic peroxide E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex4) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(93) The resin composition obtained in Example 4 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex4-1) was obtained.

(94) The gel fraction of the crosslinked polymer (ex4-1) is shown in Table 1. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(95) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex4) obtained in Example 4 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex4), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(96) The resin composition obtained in Example 4 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 1.

Example 5

(97) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer)

(98) Using a continuous twin screw extruder, 43.7 parts by weight of A-1, 41.4 parts by weight of B-1, and 14.9 parts by weight of C-2 were kneaded under a pressure reduction of 10 kPa, at a rotation speed of 150 rpm and a temperature of 180 C., for a kneading time of 7 minutes, affording a polymer (ex5, ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer). Moreover, the polymer (ex5) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex5) are shown in Table 1. (2) Preparation of resin composition comprising polymer and organic peroxide

(99) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex5) obtained in Example 5 (i) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex5) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(100) The resin composition obtained in Example 5 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex5-1) was obtained. The gel fraction of the crosslinked polymer (ex5-1) is shown in Table 1. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(101) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex5) obtained in Example 5 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex5), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(102) The resin composition obtained in Example 5 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 1.

Example 6

(103) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-docosyl methacrylate-n-eicosyl methacrylate-n-octadecyl methacrylate-methyl methacrylate copolymer)

(104) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer, a cooling tube, a Dean-Stark tube, and a finger baffle was replaced by nitrogen, and then 40.00 g of A-1, 32.95 g of B-1, 0.70 g of C-2, and 58 mL of heptane were added, and then heated to reflux for 33 while setting an oil bath temperature at 150 C. Then, the oil bath temperature was set at 120 C. and the solvent was distilled off under a pressure reduction of 1 kPa for 3 hours, and thus, a polymer ((ex6, ethylene-n-docosyl methacrylate-n-eicosyl methacrylate-n-octadecyl methacrylate-methyl methacrylate copolymer) was obtained. Moreover, the polymer (ex6) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex6) are shown in Table 1. (2) Preparation of resin composition comprising polymer and organic peroxide

(105) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer obtained in Example 6 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex6) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(106) The resin composition obtained in Example 6 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex6-1) was obtained.

(107) The gel fraction of the crosslinked polymer (ex6-1) is shown in Table 1. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(108) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex6) obtained in Example 6 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex6), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(109) The resin composition obtained in Example 6 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 1.

Example 7

(110) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer)

(111) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer, a cooling tube, a Dean-Stark tube, and a finger baffle was replaced by nitrogen, and then 40.00 g of A-1, 37.95 g of B-1, 0.72 g of C-2, and 58 mL of heptane were added, and then heated to reflux for 9 while setting an oil bath temperature at 170 C. Then, the oil bath temperature was set at 120 C. and the solvent was distilled off under a pressure reduction of 1 kPa for 3 hours, and thus, a polymer (ex7) (ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex7) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex7) are shown in Table 1.

Example 8

(112) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-octadecyl acrylate-methyl acrylates copolymer)

(113) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer, a cooling tube, a Dean-Stark tube, and a finger baffle was replaced by nitrogen, and then 60.00 g of A-1, 41.32 g of B-3, 1.07 g of C-2, and 263 mL of heptane were added, and then heated to reflux for 12 while setting an oil bath temperature at 170 C. Then, the oil bath temperature was set at 120 C. and the solvent was distilled off under a pressure reduction of 1 kPa for 3 hours, and thus, a polymer (ex8) (ethylene-n-octadecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex8) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex8) are shown in Table 1.

Example 9

(114) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-hexadecyl acrylate-methyl acrylate copolymer)

(115) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer, a cooling tube, a Dean-Stark tube, and a finger baffle was replaced by nitrogen, and then 40.00 g of A-1, 28.71 g of B-4, 0.72 g of C-2, and 58 mL of heptane were added, and then heated to reflux for 12 while setting an oil bath temperature at 170 C. Then, the oil bath temperature was set at 120 C. and the solvent was distilled off under a pressure reduction of 1 kPa for 3 hours, and thus, a polymer (ex9) (ethylene-n-hexaclecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex9) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex9) are shown in Table 2.

Example 10

(116) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-tetradecyl acrylate-methyl acrylates copolymer)

(117) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer, a cooling tube, a Dean-Stark tube, and a finger baffle was replaced by nitrogen, and then 40.00 g of A-1, 25.36 g of B-5, 0.72 g of C-2, and 58 mL of heptane were added, and then heated to reflux for 12 while setting an oil bath temperature at 170 C. Then, the oil bath temperature was set at 120 C. and the solvent was distilled off under a pressure reduction of 1 kPa for 3 hours, and thus, a polymer (ex10) (ethylene-n-tetradecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex10) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex10) are shown in Table 2.

Example 11

(118) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer)

(119) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer and a finger baffle was replaced by nitrogen, and then 80.00 g of A-1, 77.79 g of B-1, and 1.65 g of C-2 were added, and then heated and stirred under a pressure reduction of 1 kPa for 12 while setting an oil bath temperature at 130 C., and thus a polymer (exit) (ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (exit) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex11) are shown in Table 2. (2) Preparation of resin composition comprising polymer and organic peroxide

(120) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex11) obtained in Example 11 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 11 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex11) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(121) The resin composition obtained in Example 11 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex11-1) was obtained. The gel fraction of the crosslinked polymer (ex11-1) is shown in Table 2.

Example 12

(122) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-octadecyl acrylate-methyl acrylates copolymer)

(123) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer and a finger baffle was replaced by nitrogen, and then 80.00 g of A-1, 65.64 g of B-3, and 1.65 g of C-2 were added, and then heated and stirred under a pressure reduction of 1 kPa for 12 while setting an oil bath temperature at 130 C., and thus a polymer (ex12) (ethylene-n-octadecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex12) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex12) are shown in Table 2. (2) Preparation of resin composition comprising polymer and organic peroxide

(124) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex12) obtained in Example 12 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex12) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(125) The resin composition obtained in Example 12 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex12-1) was obtained. The gel fraction of the crosslinked polymer (ex12-1) is shown in Table 2. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(126) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex12) obtained in Example 12 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex12), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(127) The resin composition obtained in Example 12 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 2.

Example 13

(128) (1) Production of polymer composed of constitutional units (A), constitutional units (B), and constitutional units (C) (ethylene-n-hexadecyl acrylate-methyl acrylate copolymer)

(129) The atmosphere in a separable flask having a capacity of 0.3 L and equipped with a stirrer and a finger baffle was replaced by nitrogen, and then 80.00 g of A-1, 58.83 g of B-4, and 1.65 g of C-2 were added, and then heated and stirred under a pressure reduction of 1 kPa for 12 while setting an oil bath temperature at 130 C., and thus a polymer (ex13) (ethylene-n-hexadecyl acrylate-methyl acrylate copolymer) was obtained. Moreover, the polymer (ex13) was compression molded at 150 C. for 10 minutes to prepare a specimen being 1 mm in thickness, which was then evaluated. The physical property values and the evaluation results of the polymer (ex13) are shown in Table 2. (2) Preparation of resin composition comprising polymer and organic peroxide

(130) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex13) obtained in Example 13 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex13) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(131) The resin composition obtained in Example 13 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (ex13-1) was obtained. The gel fraction of the crosslinked polymer (ex13-1) is shown in Table 2. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(132) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (ex13) obtained in Example 13 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (ex13), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(133) The resin composition obtained in Example 13 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 2.

Comparative Example 1

(134) (1) Production of polymer composed of constitutional units (B) (octadecyl methacrylate homopolymer)

(135) 18.8 mL of octadecyl methacrylate (produced by Tokyo Chemical Industry Co., Ltd.) and 39.4 mg of 2,2c-azobisisobutyronitrile (10-hour half-life temperature: 65 C.) (produced by Tokyo Chemical Industry Co., Ltd.) were dissolved in 18.5 mL of toluene, and stirring was performed under a nitrogen atmosphere, at 80 C. for 3 hours in a 100 mL eggplant flask, and then the mixture was reprecipitated in 100 mL of ethanol, and thus a polymer composed of the units (B) (cf1, octadecyl methacrylate homopolymer) was obtained. Moreover, the polymer (cf1) was compression molded at 120 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the polymer (cf1) are shown in Table 2. The activation energy of flow E and the extensional viscosity nonlinear index k were disclosed as being not measurable because the specimens were poor in shape retention at the measurement temperatures and the specimens sagged downward to deform during the measurement. (2) Preparation of resin composition comprising polymer and organic peroxide

(136) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (cf1) obtained in Comparative Example 1 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf1) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(137) The resin composition obtained in Comparative Example 1 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (cf1-1) was obtained. The gel fraction of the crosslinked polymer (cf1-1) is shown in Table 2. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(138) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (cf1) obtained in Comparative Example 1 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf1), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(139) The resin composition obtained in Comparative Example 1 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was at a temperature of 140 C., but no foamed article was obtained. The foamability of the foamed article are shown in Table 2.

Comparative Example 2

(140) (1) Production of polymer composed of constitutional units (B) (reaction product of glycidyl methacrylate homopolymer/n-octadecanoic acid)

(141) 85.5 mL of glycidyl methacrylate (produced by Tokyo Chemical Industry Co., Ltd.) and 5.5 g of di-tert-butyl peroxide (10-hour half-life temperature: 124 C.) (produced by Tokyo Chemical Industry Co., Ltd.) were dissolved in 37.6 g of n-pentyl propionate, and stirring was performed under a nitrogen atmosphere, at 152 C. for 5.5 hours in a 200 mL eggplant flask, and then the mixture was reprecipitated in 1 L of ethanol, and thus an intermediate (cf2-0, glycidyl methacrylate homopolymer) was obtained.

(142) To 20 g of the resulting intermediate (cf2-0) was added 40 g of B-3, and stirring was performed in the presence of nitrogen at 130 C. for 3 hours in a 100-mL eggplant flask. The product was dissolved in 100 mL of tetrahydrofuran and then was reprecipitated in 500 mL of ethanol, and a polymer (cf2) composed of the units (B) (reaction product of glycidyl methacrylate homopolymer/n-octadecanoic acid) was thereby obtained. Moreover, the polymer (cf2) was compression molded at 120 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the polymer (cf2) are shown in Table 2. The activation energy of flow E and the extensional viscosity nonlinear index k were not measurable because the specimens were poor in shape retention at the measurement temperatures and the specimens sagged downward to deform during the measurement. (2) Preparation of resin composition comprising polymer and organic peroxide

(143) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer (cf2) obtained in Comparative Example 2 (1) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf2) and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(144) The resin composition obtained in Comparative Example 2 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (cf2-1) was obtained. The gel fraction of the crosslinked polymer (cf2-1) is shown in Table 2. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(145) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the polymer obtained in Comparative Example 2 (1), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf2), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(146) The resin composition obtained in Comparative Example 2 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was at a temperature of 140 C., but no foamed article was obtained. The foamability of the foamed article are shown in Table 2.

Comparative Example 3

(147) (1) Ethylene-octene copolymer

(148) An ethylene-octene copolymer ENGAGE 8003 (produced by The Dow Chemical Company) was compression molded at 120 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated. The physical property values and the evaluation results of the ethylene-octene copolymer (cf3) are shown in Table 2. (2) Preparation of resin composition comprising polymer and organic peroxide

(149) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the ethylene-octene copolymer ENGAGE 8003 (produced by The Dow Chemical Company) and 2.0 parts by weight of E-1 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf3)2 and the organic peroxide was prepared. (3) Preparation of crosslinked polymer

(150) The resin composition obtained in Comparative Example 3 (2) was filled into a mold having a cavity size of 50 mm in length, 50 mm in width, and 0.3 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 165 C., a time of 30 minutes, and a pressure of 10 MPa, and thus a crosslinked polymer (cf3-1) was obtained. The gel fraction of the crosslinked polymer (cf3-1) is shown in Table 2. (4) Preparation of resin composition comprising polymer, organic peroxide, and foaming agent

(151) Using a micro compounder (Xplore, manufactured by DSM), 100 parts by weight of the ethylene-octene copolymer ENGAGE 8003 (produced by The Dow Chemical Company), 2.0 parts by weight of E-2, 8.2 parts by weight of G-1, 2.0 parts by weight of H-1, and 1.0 part by weight of H-2 were kneaded under conditions including a kneading temperature of 80 C., a kneading time of 5 minutes, and a screw rotation speed of 100 rpm, and thus a resin composition comprising the polymer (cf3), the organic peroxide and the foaming agent was prepared. (5) Preparation of foamed article

(152) The resin composition obtained in Comparative Example 3 (4) was filled into a mold having a cavity size of 45 mm in length, 45 mm in width, and 5 mm in thickness and then was subjected to heating and compression under conditions including a temperature of 140 C., a time of 30 minutes, and a pressure of 20 MPa. Then, the mold was released at a temperature of 140 C., affording a foamed article. The gel fraction and the foamability of the foamed article are shown in Table 2.

Comparative Example 4

(153) (1) Production of ethylene--olefin copolymer

(154) To a 5-liter autoclave equipped with a stirrer, dried under reduced pressure and then purged with nitrogen was added 1.4 L of a toluene solution containing 706 g of -olefin C2024 (a mixture of olefins having 18 carbon atoms, 20 carbon atoms, 22 carbon atoms, 24 carbon atoms, and 26 carbon atoms, respectively, produced by INEOS), and subsequently, toluene was added so that the liquid amount might become 3 L. The temperature of the autoclave was raised to 60 C., and then ethylene was added so that its partial pressure might become 0.1 MPa, thereby stabilizing the system. A hexane solution of triisobutylaluminum (0.34 mol/L, 14.7 ml) was added thereto. Subsequently, a toluene solution of dimethylanilinium tetrakis(pentafluorophenyl)borate (1.0 mmol/13.4 mL) and a toluene solution of diphenylmethylene(cyclopentadienyl)(fluorenyl)zirconium dichloride (0.2 mmol/L, 7.5 mL) were charged to initiate polymerization, and then ethylene gas was fed such that the total pressure is kept constant. After a lapse of 3 hours, 2 ml of ethanol was added, thereby stopping the polymerization. After the stop of the polymerization, an ethylene--olefin copolymer (cf4) was deposited by adding a toluene solution containing the polymer into acetone, and the polymer (cf4) collected by filtration was further washed with acetone twice. The resulting polymer (cf4) was vacuum dried at 80 C., affording 369 g of the polymer (cf4). The polymer (cf4) was compression molded at 100 C. for 10 minutes to prepare specimens being 1 mm and 0.5 mm in thickness, respectively, which were then evaluated.

(155) The physical property values and the evaluation results of the polymer (cf4) are shown in Table 2.

Example 14

(156) (1) Production of crosslinked polymer (crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer)

(157) Using a twin screw extruder, 100 parts by weight of the polymer (exit) obtained in Example 11 (1), 1.5 parts by weight of E-3, 1.5 parts by weight of F-1, 0.1 parts by weight of I-1, and 0.1 parts by weight of J-1 were kneaded under conditions including a kneading temperature of 220 C., a residence time of 2 minutes, and a screw rotation speed of 500 rpm, and thus a crosslinked polymer (ex14-1, crosslinked ethylene n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer) was prepared. (2) Evaluation of crosslinked polymer

(158) The gel fraction and the permanent compression set were evaluated for the crosslinked polymer (ex14-1) obtained in Example 14 (1). The evaluated results are shown in Table 3. The permanent compression set was not measurable because the specimen was drawn to deform when being detached from a compression plate.

Example 15

(159) (1) Production of resin composition containing a polymer and a polymer different from that polymer (resin composition comprising an ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer)

(160) Using a twin screw extruder, 80 parts by weight of the polymer (ex11) obtained in Example 11 (i), 20 parts by weight of D-1, 0.1 parts by weight of I-1, and 0.1 parts by weight of J-1 were kneaded under conditions including a kneading temperature of 220 C., a residence time of 2 minutes, and a screw rotation speed of 500 rpm, and thus a resin composition (ex15) (resin composition comprising an ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer) was prepared. (2) Evaluation of resin composition

(161) The permanent compression set was evaluated for the resin composition (ex15) obtained in Example 15 (1). The evaluated results are shown in Table 3. The permanent compression set was not measurable because the specimen was drawn to deform when being detached from a compression plate.

Example 16

(162) (1) Production of resin composition containing a polymer and a polymer different from that polymer (resin composition comprising an ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer)

(163) A resin composition (ex16) (resin composition comprising an ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer) was prepared in the same manner as Example 15 except that the amount of the polymer (ex11) obtained in Example 11 (1) from 80 parts by weight to 90 parts by weight and the amount of D-1 from 20 parts by weight to 10 parts by weight. (2) Evaluation of resin composition

(164) The permanent compression set was evaluated for the resin composition (ex16) obtained in Example 16 (1). The evaluated results are shown in Table 3. The permanent compression set was not measurable because the specimen was drawn to deform when being detached from a compression plate.

Example 17

(165) (1) Production of crosslinked resin composition (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer)

(166) Using a twin screw extruder, 80 parts by weight of the polymer (ex11) obtained in Example 11 (1), 20 parts by weight of D-1, 1.0 part by weight of E-3, 1.0 part by weight of F-1, 0.1 parts by weight of I-1, and 0.1 parts by weight of J-1 were kneaded under conditions including a kneading temperature of 220 C., a residence time of 2 minutes, and a screw rotation speed of 500 rpm, and thus a crosslinked resin composition (ex16, resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer) was prepared. (2) Evaluation of crosslinked resin composition

(167) The gel fraction and the permanent compression set were evaluated for the crosslinked resin composition obtained in Example 17 (1). The evaluated results are shown in Table 3.

Example 18

(168) (1) Production of crosslinked resin composition (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer)

(169) A resin composition (ex18) (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer) was prepared in the same manner as Example 17 except that the amount of E-3 from 1.0 part by weight to 1.5 parts by weight and the amount of F-1 from 1.0 part by weight to 1.5 part by weight. (2) Evaluation of crosslinked resin composition

(170) The gel fraction and the permanent compression set were evaluated for the crosslinked resin composition (ex18) obtained in Example 18 (1). The evaluated results are shown in Table 3.

Example 19

(171) (1) Production of crosslinked resin composition (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer)

(172) A crosslinked resin composition (ex19, resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene homopolymer) was prepared in the same manner as Example 17 except that the amount of the polymer (ex11) obtained in Example 11 (1) from 80 parts by weight to 90 parts by weight and the amount of D-1 from 20 parts by weight to 10 parts by weight. (2) Evaluation of crosslinked resin composition

(173) The gel fraction and the permanent compression set were evaluated for the crosslinked resin composition (ex19) obtained in Example 19 (1). The evaluated results are shown in Table 3.

Example 20

(174) (1) Production of crosslinked resin composition (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene random copolymer)

(175) A crosslinked resin composition (ex20, resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and a polypropylene random copolymer) was prepared in the same manner as Example 17 except that 20 parts by weight of E-3 was exchanged for 20 parts by weight of D-2. (2) Evaluation of crosslinked resin composition

(176) The gel fraction and the permanent compression set were evaluated for the crosslinked resin composition (ex20) obtained in Example 20 (1). The evaluated results are shown in Table 3.

Example 21

(177) (1) Production of crosslinked resin composition (resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl a crylate-n-octadecyl acrylate-methyl acrylate copolymer and high-density polyethylene)

(178) A crosslinked resin composition (ex21, resin composition comprising a crosslinked ethylene-n-docosyl acrylate-n-eicosyl acrylate-n-octadecyl acrylate-methyl acrylate copolymer and high-density polyethylene) was prepared in the same manner as Example 17 except that 20 parts by weight of D-1 was exchanged for 20 parts by weight of D-3. (2) Evaluation of crosslinked resin composition

(179) The gel fraction and the permanent compression set were evaluated for the crosslinked resin composition (ex21) obtained in Example 21 (1). The evaluated results are shown in Table 3.

(180) TABLE-US-00001 TABLE 1 Example 1 2 3 4 5 6 7 8 Noncrosslinked polymer Content of constitutional unit (A) (%) 88.9 88.9 92.2 95.3 88.9 88.8 88.9 88.9 Content of constitutional unit (B) (%) 4.4 6.0 5.6 4.5 8.3 9.5 9.7 9.3 Content of constitutional unit (C) (%) 6.6 5.0 2.2 0.2 2.8 1.7 1.3 1.8 Content of unreacted compounds having a 1.6 12.9 ND ND 6 2.2 2.6 0.4 C14-C30 alkyl group-containing compound (wt %) Melting peak temperature Tm ( C.) 41 43 32 48 46 53 53 36 Melting enthalpy H (J/g) 65 69 54 54 79 92 104 82 Ratio A defined by Formula (I) 0.55 0.71 0.73 0.69 0.65 0.71 0.85 0.44 Activation energy of flow E.sub.a (kJ/mol) ND ND ND 79.78 ND ND 61.95 ND Extensional viscosity nonlinear index k ND ND ND 1.18 ND ND 1.06 ND Molding processability Shape retention Water vapor transmission rate 0.51 0.49 ND 0.45 0.26 0.10 0.11 ND (gmm/m.sup.2 .Math. 24 hours) Gel fraction of crosslinked polymer (wt %) 92 ND ND 88 86 89 ND ND Gel fraction of foam (wt %) 93 ND ND 96 86 84 ND ND Foamability ND ND ND ND
In the table, ND means unevaluated (for foamability) or unmeasured (for properties other than foamability).

(181) TABLE-US-00002 TABLE 2 Example Comparative Example 9 10 11 12 13 1 2 3 4 Noncrosslinked polymer Content of constitutional unit (A) (%) 88.9 88.9 87.1 87.1 87.1 Content of constitutional unit (B) (%) 9.8 9.9 10.8 10.8 10.8 Content of constitutional unit (C) (%) 1.2 1.1 2.0 2.1 2.1 Content of unreacted compounds 1.9 1.2 0.9 1.4 1.5 ND ND ND ND having a C14-C30 alkyl group-containing compound (wt %) Melting peak temperature Tm ( C.) 25 28 50 36 25 35 48 79 34 Melting enthalpy H (J/g) 73 52 92 76 65 64 49 33 83 Ratio A defined by Formula (I) 0.49 0.47 0.68 0.48 0.53 10.4 Unmeasurable 1.09 0.94 Activation energy of flow E.sub.a (kJ/mol) ND 64.85 65.57 60.56 63.96 Unmeasurable Unmeasurable 36.80 ND Extensional viscosity nonlinear index k ND 1.10 ND ND ND Unmeasurable Unmeasurable 0.13 ND Molding processability x x Shape retention x x x Water vapor transmission rate 0.90 1.43 0.09 0.36 0.99 Unmeasurable Unmeasurable 0.27 0.05 (gmm/m.sup.2 .Math. 24 hours) Gel fraction of crosslinked polymer (wt %) ND ND 90 89 89 11 10 98 ND Gel fraction of foam (wt %) ND ND ND 88 87 ND ND 90 ND Foamability ND ND ND x x ND
In the table, ND means unevaluated (for foamability) or unmeasured (for properties other than foamability).

(182) TABLE-US-00003 TABLE 3 Example 14 15 16 17 18 19 20 21 Polymer obtained in Example 11(1) 100 80 90 80 80 90 80 80 (ex11) (part(s) by weight) Propylene homopolymer (D-1) (part by 0 20 10 20 20 10 0 0 weight) Propylene random copolymer (D-2) 0 0 0 0 0 0 20 0 (part by weight) High-density polyethylene (D-3) (part 0 0 0 0 0 0 0 20 by weight) Organic peroxide (E-3) (part by 1.5 0 0 1 1.5 1 1 1 weight) Crosslinking aid (F-1) (part by weight) 1.5 0 0 1 1.5 1 1 1 Antioxidant (I-1) (part by weight) 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 Heat stabilizer (J-1) (part by weight) 0.1 0.1 0.1 0.1 0.1 0.1 0.1 0.1 Melting enthalpy H (J/g) 84 76 82 75 73 79 69 65 Gel fraction (wt %) 57 ND ND 70 76 60 22 43 Permanent compression set (%) Unmeasurable Unmeasurable Unmeasurable 56 51 25 50 28
In the table, ND means unmeasured.