COPOLÍMERO DE ETILENO / 1-BUTENO MODIFICADO POR ENXERTO, COMPOSIÇÃO DE RESINA DE POLIAMIDA E PRODUTO MOLDADO

Abstract

One embodiment of the present invention provides a graft-modified ethylene / 1-butene copolymer suitable as an impact resistance modifier for engineering plastics such as polyamide, and also provides a polyamide resin composition having an excellent balance between the fluidity and impact resistance of a molded body by using said graft-modified ethylene / 1-butene copolymer.　One embodiment of the present invention provides a graft-modified ethylene / 1-butene copolymer (A) in which an ethylene / 1-butene copolymer (a) that satisfies requirements (a-i) and (a-ii) is graft-modified with a polar compound. The requirements (a-i) and (a-ii) are disclosed in the specification.

Description

1 / 50 Graft-modified ethylene / 1-butene copolymer, polyamide resin composition and molded product. Technical Field

[001] One embodiment of the present invention relates to a graft-modified ethylene / 1-butene copolymer, a polyamide resin composition comprising the graft-modified ethylene / 1-butene copolymer and use thereof. Background Technique

[002] Polyamide resins have been widely used in the automotive sector and in the electrical and electronic fields, taking advantage of their excellent properties as engineering plastics. Automotive and electrical components used in these fields may need to have impact resistance due to the requirements of their function. As a method to impart impact resistance, a method for composing a polyolefin resin modified with a polyamide resin is known (Patent Literature 1 and 2).

[003] Polyamide resins are used, for example, in automotive components and, in recent years, there have been strong demands for them to be lightweight to reduce fuel consumption, resulting in requirements for them to be thinner. However, in general, when made thinner, the impact resistance of a molded product made of polyamide resin decreases drastically. List of Citations

[004] Patent Literature [Patent Literature 1] JP5-32886A [Patent Literature 2] JP-T-2021-503022A Summary of the Invention Technical Problem

[005] The modified polyolefin resins disclosed in Patent Literature 1 and 2 are ethylene-propylene-based modified polymers. The present inventors have confirmed that Petition 870250081626, dated 11 / 09 / 2025, pp. 117 / 166 2 / 50 Polyamide resins containing these polymers cannot achieve both the impact resistance of a molded product containing the polyamide resin and the flowability; that is, it is difficult to improve the impact resistance of a molded product without compromising the flowability of the polyamide resin, and therefore there is room for improvement. Thus, an objective of one embodiment of the present invention to solve this problem is to provide a graft-modified ethylene / 1-butene copolymer suitable as an impact modifier for an engineering plastic, such as polyamide, and to provide an excellent polyamide resin composition in balance between the impact resistance of a molded product and flowability, using the graft-modified ethylene / 1-butene copolymer. Solution to the Problem

[006] The present invention comprises the following aspects: {1} A graft-modified ethylene / 1-butene copolymer (A), obtained by graft-modifying an ethylene / 1-butene copolymer (a) with a polar compound, wherein the ethylene / 1-butene copolymer (a) satisfies the following requirements (ai) and (a-ii): Requirement (ai): a ratio (MFR10 / MFR2.16) of a melt flow rate (MFR10) measured under conditions of 190°C and a charge of 10 kg according to ASTM D1238 to a melt flow rate (MFR2.16) measured under conditions of 190°C and a charge of 2.16 kg according to ASTM D1238 is in the range of 6.7 to 9.0; and requirement (a-ii): the vinyl group content is in the range of 5.0 to 20.0 groups and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100,000 carbon atoms, as calculated by 1H-NMR.

[007] {2} The graft-modified ethylene / 1-butene copolymer (A) according to {1}, wherein the polar compound is at least one selected from the group consisting of an ethylenically unsaturated compound containing a hydroxyl group, a Petition 870250081626, dated 11 / 09 / 2025, pp. 118 / 166 3 / 50 an ethylenically unsaturated compound containing an amino group, an ethylenically unsaturated compound containing an epoxy group, an aromatic vinyl compound, an unsaturated carboxylic acid and a derivative thereof, a vinyl ester compound, and vinyl chloride.

[008] {3} A graft-modified ethylene / 1-butene copolymer (A), obtained by graft-modifying an ethylene / 1-butene copolymer (a) with a polar compound, wherein the graft-modified ethylene / 1-butene copolymer (A) satisfies the following requirements (Ai) to (Av): Requirement (Ai): a ratio (MFR10 / MFR2.16) of a melt flow rate (MFR10) measured under conditions of 190°C and a load of 10 kg according to ASTM D1238 to a melt flow rate (MFR2.16) measured under conditions of 190°C and a load of 2.16 kg according to ASTM D1238 is in the range of 11.5 to 18.0; requirement (A-ii): the vinyl group content is in the range of 5.0 to 20.0 groups and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100,000 carbon atoms, as calculated by 1H-NMR; Requirement (A-iii): the amount of graft modification is in the range of 0.1 to 2.0% by mass based on 100% by mass of the graft-modified ethylene / 1-butene copolymer (A); Requirement (A-iv): a melt flow rate (MFR2.16) measured in accordance with ASTM D1238 under conditions of 190°C and a charge of 2.16 kg, is in the range of 0.01 to 5.00 g / 10 min; and requirement (Av): a density measured in accordance with ASTM D1505 under conditions of 25°C, is in the range of 850 to 885 kg / m3.

[009] {4} The graft-modified ethylene / 1-butene copolymer (A) according to {3}, wherein the polar compound is at least one selected from the group consisting of an unsaturated carboxylic acid and a derivative thereof.

[010] {5} A polyamide resin composition comprising 1 to 50 parts by mass of ethylene / 1-butene copolymer Petition 870250081626, dated 11 / 09 / 2025, pp. 119 / 166 4 / 50 graft-modified (A) according to any one of {1} to {4} and 50 to 99 parts by mass of a polyamide resin (B), based on 100 parts by mass of a total of graft-modified ethylene / 1-butene copolymer (A) and polyamide resin (B).

[011] {6} The polyamide resin composition according to {5}, wherein the polyamide resin (B) is one or more aliphatic polyamide resins selected from the group consisting of polyamide 6, polyamide 66, polyamide 11, polyamide 12, polyamide 612, polyamide 610 and polyamide 1010.

[012] {7} A pellet comprising the polyamide resin composition according to {5} or {6}.

[013] {8} A molded product comprising a polyamide resin composition according to {5} or {6}.

[014] {9} An injection molded article comprising a polyamide resin composition according to {5} or {6}.

[015] {10} An automotive component comprising a polyamide resin composition according to {5} or {6}.

[016] {11} An electronic component comprising a polyamide resin composition according to {5} or {6}.

[017] {12} An automotive electrical component comprising a polyamide resin composition according to {5} or {6}. Advantageous Effects of the Invention

[018] The graft-modified ethylene / 1-butene copolymer (A) obtained in an embodiment of the present invention is suitable as an impact modifier, while inhibiting a decrease in the flowability of an engineering plastic, such as polyamide.

[019] Furthermore, a polyamide resin composition comprising graft-modified ethylene / 1-butene copolymer (A) of an embodiment of the present invention has adequate fluidity to produce a molded product, and the molded product obtained exhibits high impact resistance even when made more Petition 870250081626, dated 11 / 09 / 2025, pages 120 / 166 5 / 50 fine. In other words, the composition of the polyamide resin is excellent in balancing the impact resistance of a molded product with its fluidity. Description of the Modalities

[020] Specific embodiments of the present invention will be described in detail below. However, the present invention is in no way limited to the following embodiments, but may be implemented with appropriate modifications within the intended scope of the present invention.

[021] As used herein, the term a indicating a numerical range is used to mean that the numerical values ​​before and after a are included as a lower limit value and an upper limit value, respectively.

[022] As used herein, the term a indicating a numeric range means that even if the unit is specified before or after a, both values ​​will have the same unit, unless otherwise specified.

[023] In this description, a combination of two or more preferred aspects is a more preferred aspect. Furthermore, in the present description, each component in a composition or each constituent unit in a polymer may be included individually or in a combination of two or more of them, unless otherwise specified.

[024] In the present description, the content of each component in a composition or of each constituent unit in a polymer refers, in the case where each component or a plurality of substances or constituent units corresponding to each constituent unit in the polymer is present in the composition, to the total content of the corresponding substances present in the composition or to the plurality of each constituent unit present in the polymer, unless otherwise specified. <Copolímero de etileno / 1-buteno (a)>

[025] An ethylene / 1-butene copolymer (a) is used as Petition 870250081626, dated 11 / 09 / 2025, pp. 121 / 166 6 / 50 Graft-modified ethylene / 1-butene copolymer feedstock (A) according to one embodiment of the present invention. The ethylene / 1-butene copolymer (a) may be referred to as a component (a).

[026] The ethylene / 1-butene copolymer (a) generally meets the following requirements (ai) and (a-ii). [Requirement (ai)]

[027] A ratio (MFR10 / MFR2.16) of a melt flow rate (MFR10) measured under conditions of 190°C and a load of 10 kg according to ASTM D1238 to a melt flow rate (MFR2.16) measured under conditions of 190°C and a load of 2.16 kg according to ASTM D1238 is in the range of 6.7 to 9.0.

[028] MFR10 / MFR2. 16 is preferably in the range of 6.8 to 8.9, more preferably from 6.9 to 8.8 and even more preferably from 7.0 to 8.7. When the MFR10 / MFR2.16 of the ethylene-1-butene copolymer (a) falls within the above range, and the ethylene / 1-butene copolymer (a) is graft modified with a polar compound to produce a graft-modified ethylene / 1-butene copolymer (A), the polyamide resin composition, obtained by mixing the graft-modified copolymer (A) with a polyamide resin, exhibits excellent flowability, and a molded product containing the composition exhibits excellent impact resistance. [Requirement (a-ii)]

[029] The vinyl group content is in the range of 5.0 to 20.0 groups, and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100,000 carbon atoms, as calculated by 1H-NMR.

[030] The vinyl group content is preferably in the range of 5.5 to 17.0 groups, more preferably from 6.0 to 14.0 groups and even more preferably from 6.5 to 11.0 groups. The total number of unsaturated bonds is preferably in the range of 45.0 to 190.0 bonds, more preferably from Petition 870250081626, dated 11 / 09 / 2025, pp. 122 / 166 7 / 50 50.0 to 180.0 calls, and even more preferably 55.0 to 170.0 calls.

[031] When the graft-modified ethylene / 1-butene copolymer (A) produced by graft modification of the ethylene / 1-butene copolymer (a) having a total amount of unsaturated linkages in the above range with a polar compound is mixed with a polyamide resin to produce a polyamide resin composition, the polyamide resin composition exhibits excellent flowability and a molded product that exhibits excellent impact resistance can be obtained.

[032] The vinyl group content refers to the number of vinyl double bonds per 100,000 carbon atoms.

[033] The total number of unsaturated bonds refers to the total number of vinylic double bonds, vinylidene double bonds, disubstituted olefinic double bonds and trisubstituted olefinic double bonds per 100,000 carbon atoms.

[034] The vinyl group content and the total amount of unsaturated bonds can be calculated by measuring 1H-NMR under the conditions described in a section of Examples described later. <Método de produção de copolímero de etileno / 1-buteno (a)>

[035] The ethylene / 1-butene copolymer (a) satisfying requirements (ai) and (a-ii) can be produced by a publicly known method. The ethylene / 1-butene copolymer (a) can be prepared, for example, by copolymerizing ethylene and 1-butene in the presence of a publicly known catalyst capable of polymerizing an olefin (for example, a catalyst composed mainly of a solid titanium component and an organometallic compound, a vanadium-based catalyst composed of a soluble vanadium compound and an alkylaluminum halide compound, or a zirconium-based catalyst composed of a zirconium metallocene compound and a compound Petition 870250081626, dated 11 / 09 / 2025, pp. 123 / 166 8 / 50 organoaluminum-oxy). The catalyst is preferably a catalyst containing a metallocene compound as a catalyst component.

[036] Component (a) preferably satisfies one or more requirements selected from the group consisting of the following requirements (a-iii) to (a-vi), more preferably satisfies two or more requirements and, particularly preferably, satisfies all requirements. [Requirement (a-iii)]

[037] MFR2,16 is in the range of 2.0 to 20.0 g / 10 min.

[038] The MFR2.16 is preferably in the range of 2.2 to 18.0 g / 10 min, more preferably 2.5 to 16.0 g / 10 min, even more preferably 2.6 to 15.0 g / 10 min and, particularly preferably, 3.0 to 14.0 g / 10 min. When the MFR2.16 of the ethylene-1-butene copolymer (a) falls within the above range, and the ethylene / 1-butene copolymer (a) is graft modified with a polar compound to produce a graft modified ethylene / 1-butene copolymer (A), the polyamide resin composition, obtained by mixing the graft modified copolymer (A) with a polyamide resin, exhibits excellent flowability, and a molded product containing the composition exhibits excellent impact resistance. [Requirement (a-iv)]

[039] The content of an ethylene-derived constituent unit is in the range of 70 to 95 mol%, and the content of a 1-butene-derived constituent unit is in the range of 5 to 30 mol%, provided that the total content of an ethylene-derived constituent unit and a 1-butene-derived constituent unit is 100 mol%.

[040] The content of an ethylene-derived constituent unit is preferably in the range of 73 to 93 mol%, more preferably 76 to 91 mol%, even more preferably 78 to 89 mol% and particularly Petition 870250081626, dated 11 / 09 / 2025, pp. 124 / 166 9 / 50 preferably from 80 to 87 mol%, and the content of a constituent unit derived from 1-butene is preferably in the range of 7 to 27 mol%, more preferably from 9 to 24 mol%, even more preferably from 11 to 22 mol%, and particularly preferably from 13 to 20 mol%.

[041] The content (mol %) of the constituent units derived from each comonomer is calculated, for example, by 13C-NMR spectrum analysis. When the content of a 1-butene-derived constituent unit in component (a) falls within the above range, and the ethylene / 1-butene copolymer (a) is graft-modified with a polar compound to produce a graft-modified ethylene / 1-butene copolymer (A), the polyamide resin composition, obtained by mixing the graft-modified copolymer (A) with a polyamide resin, exhibits excellent flowability, and a molded product containing the composition exhibits excellent impact resistance.

[042] Ethylene and 1-butene, which are monomers that constitute an ethylene / α-olefin copolymer (a), may be, for example, monomers derived from fossil fuels and / or monomers derived from biomass, and these monomers may be used individually or in combination of two or more of them. [Requirements (av)]

[043] The density measured under the condition of 25°C, according to the ASTM D1505 standard, is in the range of 850 to 885 kg / m3.

[044] The density is preferably in the range of 855 to 882 kg / m3, more preferably from 860 to 879 kg / m3, even more preferably from 861 to 878 kg / m3 and, particularly preferably, from 865 to 876 kg / m3. When the density of the ethylene / 1-butene copolymer (a) falls within the above range, and the ethylene / 1-butene copolymer (a) is graft modified with a polar compound to produce a graft modified ethylene / 1-butene copolymer (A), the polyamide resin composition obtained by mixing the graft modified copolymer (A) with a Petition 870250081626, dated 11 / 09 / 2025, pages 125 / 166 10 / 50 polyamide resin exhibits excellent fluidity, and a molded product containing the polyamide resin composition is lightweight and exhibits excellent impact resistance. [Requirements (a-vi)]

[045] The ratio (Mw / Mn) between the weight-average molecular weight (Mw) and the number-average molecular weight (Mn) measured by gel permeation chromatography (GPC) is in the range of 1.2 to 3.5.

[046] When graft-modified ethylene / 1-butene copolymer (A) produced by graft modification of ethylene / 1-butene copolymer (a) with a polar compound is mixed with a polyamide resin to produce a polyamide resin composition, the use of ethylene / 1-butene copolymer (a) having an Mw / Mn in the above range inhibits the stickiness of a molded product containing the polyamide resin composition. <Copolímero de etileno / 1-buteno modificado por enxerto (A)>

[047] The graft-modified ethylene / 1-butene copolymer (A) according to one embodiment of the present invention is a copolymer obtained by graft modification of the ethylene / 1-butene copolymer (a) with a polar compound. <Composto Polar>

[048] In one embodiment of the present invention, the polar compound is used to graft modify the ethylene / 1-butene copolymer (a) to produce the graft-modified ethylene / 1-butene copolymer (A).

[049] The polar compound is preferably at least one selected from the group consisting of an ethylenically unsaturated compound containing a hydroxyl group, an ethylenically unsaturated compound containing an amino group, an ethylenically unsaturated compound containing an epoxy group, an aromatic vinyl compound, an unsaturated carboxylic acid and a derivative thereof, a vinyl ester compound, and vinyl chloride. From the point of view of reactivity with a polyamide resin, the Petition 870250081626, dated 11 / 09 / 2025, pages 126 / 166 11 / 50 A polar compound is most preferably at least one selected from the group consisting of an unsaturated carboxylic acid and a derivative thereof. [ 050]Examples of ethylenically unsaturated compounds containing hydroxyl groups include (meth)acrylic acid esters, such as hydroxyethyl (meth)acrylate, 2-hydroxypropyl (meth)acrylate, 3-hydroxypropyl (meth)acrylate, 2-hydroxy-3-phenoxypropyl (meth)acrylate, 3-chloro-2-hydroxypropyl (meth)acrylate, glycerin mono(meth)acrylate, pentaerythritol mono(meth)acrylate, trimethylolpropane mono(meth)acrylate, tetramethylolethane mono(meth)acrylate, butanediol mono(meth)acrylate, polyethylene glycol mono(meth)acrylate and 2-(6-hydroxyhexanoyloxy)ethyl acrylate; 10-undecen-1-ol, l-octen-3-ol, 2-methanol norbornene, hydroxystyrene, hydroxyethyl vinyl ether, hydroxybutyl vinyl ether, N-methylol acrylamide, 2-(meth)acryloyloxyethyl acid phosphate, glyceryl monoallyl ether, allyl alcohol, allyloxyethanol and 2-butene-1,4-diol. [ 051]Examples of ethylenically unsaturated compounds containing an amino group include alkyl ester-based derivatives of acrylic acid or methacrylic acid, such as aminoethyl (meth)acrylate, propylaminoethyl (meth)acrylate, dimethylaminoethyl methacrylate, aminopropyl (meth)acrylate, phenylaminoethyl methacrylate and cyclohexylaminoethyl methacrylate; vinylamine-based derivatives, such as N-vinyldiethylamine and N-acetylvinylamine; allylamine-based derivatives, such as allylamine, methacrylate, N-methylacrylamine, N,N-dimethylacrylamide and N,N-dimethylaminopropylacrylamide; acrylamide-based derivatives, such as acrylamide and N-methylacrylamide; an aminostyrene, such as p-aminostyrene; 6-aminohexylsuccinimide and 2-aminoethylsuccinimide.

[052] Examples of ethylenically unsaturated compounds containing an epoxy group include glycidyl acrylate, glycidyl methacrylate; mono- and alkyl diglycidyl esters of acid Petition 870250081626, dated 11 / 09 / 2025, pages 127 / 166 12 / 50 dicarboxylic acid (the alkyl group of monoglycidyl ester has 1 to 12 carbon atoms), such as mono- and diglycidyl esters of maleic acid, mono- and diglycidyl esters of fumaric acid, mono- and diglycidyl esters of crotonic acid, mono- and diglycidyl esters of tetrahydrophthalic acid, mono- and diglycidyl esters of itaconic acid, mono and diglycidyl esters of butene tricarboxylic acid, mono and diglycidyl esters of citraconic acid, mono and diglycidyl esters of endo-cis-bicyclo[2.2.1]hept5-ene-2,3-dicarboxylic acid (nadic(TM) acid), mono- and diglycidyl esters of endo-cis-bicyclo[2.2.1]hept-5-ene-2-methyl acid 2,3dicarboxylic acid (acid methylnadic(TM)), and mono- and diglycidyl esters of allyl succinic acid; an alkyl glycidyl ester of p-styrene carboxylic acid, allyl glycidyl ether, 2-methylallyl glycidyl ether, p-glycidyl styrene ether, 3,4-epoxy-1-butene, 3,4-epoxy-3-methyl-1-butene, 3,4-epoxy-1-pentene, 3,4-epoxy-3methyl-1-pentene, 5,6-epoxy-1-hexene and vinylcyclohexene monoxide.

[053] Examples of aromatic vinyl compounds include styrene, α-methylstyrene, o-methylstyrene, p-methylstyrene, m-methylstyrene, p-chlorostyrene, m-chlorostyrene, p-chloromethylstyrene, 4-vinylpyridine, 2-vinylpyridine, 5-ethyl-2-vinylpyridine, 2-methyl-5-vinylpyridine, 2-isopropenylpyridine, 2-vinylquinoline, 3-vinylisoquinoline, N-vinylcarbazole and N-vinylpyrrolidone.

[054] Examples of vinyl ester compounds include vinyl acetate, vinyl propionate, n-butyrate vinyl, vinyl isobutyrate, vinyl pivalate, vinyl caproate, vinyl versatate, vinyl laurate, vinyl stearate, vinyl benzoate, p-tert-butylbenzoate vinyl, vinyl salicylate and vinyl cyclohexanecarboxylate.

[055] An example of an unsaturated carboxylic acid includes an unsaturated carboxylic acid with 3 to 10 carbon atoms, preferably 3 to 8 carbon atoms. An example of a Petition 870250081626, dated 11 / 09 / 2025, pp. 128 / 166 13 / 50 unsaturated carboxylic acid derivative includes a derivative of an unsaturated carboxylic acid with 3 to 10 carbon atoms, preferably 3 to 8 carbon atoms.

[056] Examples of unsaturated carboxylic acids include acrylic acid, maleic acid, fumaric acid, tetrahydrophthalic acid, itaconic acid, citraconic acid, crotonic acid, isocrotonic acid and nadic acid(TM) (endocis-bicyclo[2,2,1]hept-5-ene-2,3-dicarboxylic acid).

[057] Examples of unsaturated carboxylic acid derivatives include acid halide, ester, imide, acid anhydride and ester compounds of unsaturated carboxylic acids, and specific examples of these include maleyl chloride, maleimide, maleic anhydride, citraconic anhydride, monomethyl maleate, dimethyl maleate and glycidyl maleate.

[058] At least one selected from the group consisting of the unsaturated carboxylic acid and its derivative is suitably at least one selected from the group consisting of an unsaturated dicarboxylic acid and its acid anhydride, and particularly at least one selected from the group consisting of maleic acid, nadic acid(TM) and their acid anhydrides.

[059] The unsaturated carboxylic acid, which is a monomer that constitutes the graft-modified ethylene / 1-butene copolymer (A), may be, for example, a monomer derived from fossil fuels and / or a monomer derived from biomass, and these monomers may be used individually or in combination of two or more of them. <Copolímero de etileno / 1-buteno modificado por enxerto (A)>

[060] The graft-modified ethylene / 1-butene copolymer (A) generally meets one or more of the selected requirements from the group consisting of the following requirements (Ai) to (Av), preferably two or more of the requirements and, more preferably, all of the requirements. Petition 870250081626, dated 11 / 09 / 2025, pp. 129 / 166 14 / 50 [Requirement (Ai)]

[061] The ratio (MFR10 / MFR2.16) of the melt flow rate (MFR10) measured under conditions of 190°C and a load of 10 kg according to ASTM D1238 to the melt flow rate (MFR2.16) measured under conditions of 190°C and a load of 2.16 kg according to ASTM D1238 is in the range of 11.5 to 18.0.

[062] The MFR10 / MFR2.16 is preferably in the range of 12.5 to 17.6, more preferably from 13.0 to 17.3 and even more preferably from 13.5 to 17.0. When the MFR10 / MFR2.16 of the graft-modified ethylene / 1-butene copolymer (A) is in the above range, the polyamide resin composition exhibits excellent flowability and a molded product exhibiting excellent impact resistance can be produced.

[063] MFR10 of the graft-modified ethylene / 1-butene copolymer (A) is preferably in the range of 0.1 to 100 g / 10 min, more preferably 0.5 to 90 g / 10 min, even more preferably 1 to 80 g / 10 min, more preferably 70 g / 10 min, even more preferably 3 to 65 g / 10 min, particularly preferably 4 to 60 g / 10 min and, even more preferably, 5 to 58 g / 10 min. The graft-modified ethylene / 1-butene copolymer (A) having MFR10 in the above range is readily dispersed in polyamide. Therefore, when graft-modified ethylene / 1-butene copolymer (A) is blended with a polyamide resin to produce a polyamide resin composition, the polyamide resin composition exhibits excellent flowability, and a molded product containing the polyamide resin composition exhibits excellent impact resistance. [Requirement (A-ii)]

[064] The vinyl group content is in the range of 5.0 to 20.0 groups, and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100,000 carbon atoms, as calculated by 1H-NMR. Petition 870250081626, dated 11 / 09 / 2025, pp. 130 / 166 15 / 50

[065] The vinyl group content is preferably in the range of 5.5 to 17.0 groups, more preferably from 6.0 to 14.0 groups and even more preferably from 6.5 to 11.0 groups. The total number of unsaturated bonds is preferably in the range of 45.0 to 190.0 bonds, more preferably from 50.0 to 180.0 bonds and even more preferably from 55.0 to 170.0 bonds.

[066] When graft-modified ethylene / 1-butene copolymer (A) having a total amount of unsaturated linkages in the above range is blended with a polyamide resin to produce a polyamide resin composition, the polyamide resin composition exhibits excellent flowability, and a molded product exhibiting excellent impact resistance can be obtained.

[067] The vinyl group content and the total amount of unsaturated bonds can be calculated by measuring 1H-NMR under the conditions described in the Examples section described later. [Requirement (A-iii)]

[068] The amount of graft modification is in the range of 0.1 to 2.0% by mass based on 100% by mass of the graft-modified ethylene / 1-butene copolymer (A).

[069] The amount of graft modification is preferably in the range of 0.3 to 1.7% by mass, more preferably 0.3 to 1.5% by mass and even more preferably 0.5 to 1.2% by mass. When the amount of graft modification in the graft-modified ethylene / 1-butene copolymer (A) falls within the above range, the polyamide resin composition exhibits excellent flowability, and a molded product containing the polyamide resin composition exhibits excellent impact resistance.

[070] The amount of graft modification can be calculated by measuring FT-IR under the conditions described in the Example section described later. Petition 870250081626, dated 11 / 09 / 2025, pages 131 / 166 16 / 50 [Requirement (A-iv)]

[071] The melt flow rate (MFR2,16) measured under conditions of 190°C and a charge of 2.16 kg according to ASTM D1238 is in the range of 0.01 to 5.00 g / 10 min.

[072] The MFR2,16 described above is preferably in the range of 0.02 to 4.75 g / 10 min, more preferably from 0.04 to 4.00 g / 10 min, even more preferably from 0.08 to 3.00 g / 10 min, and particularly preferably from 0.10 to 2.00 g / 10 min. When the MFR2,16 of the graft-modified ethylene / 1-butene copolymer (A) is within the above range, an excellent formability polyamide resin composition is obtained, and an excellent impact-resistant molded product can be produced. [Requirement (Av)]

[073] The density measured under conditions of 25°C according to ASTM D1505 is 850 to 885 kg / m3.

[074] The density is preferably in the range of 858 to 882 kg / m3, more preferably 859 to 880 kg / m3, even more preferably 866 to 879 kg / m3, and even more preferably 870 to 877 kg / m3. When the density of the graft-modified ethylene / 1-butene copolymer (A) falls within the above range, a lightweight, thinner-shaped product exhibiting excellent impact resistance can be produced from a polyamide resin composition containing the graft-modified ethylene / 1-butene copolymer (A) and a polyamide resin.

[075] In the graft-modified ethylene / 1-butene copolymer (A), the position at which the polar compound is grafted onto the ethylene / 1-butene copolymer (a) is not particularly limited, provided that the polar compound is attached to an arbitrary carbon atom in the ethylene / 1-butene copolymer (a). <Método para produção de copolímero de etileno / 1-buteno modificado por enxerto (A)> Petition 870250081626, dated 11 / 09 / 2025, pages 132 / 166 17 / 50

[076] The graft-modified ethylene / 1-butene copolymer (A) is obtained by several publicly known production methods, for example, by a graft reaction of the ethylene / 1-butene copolymer (a) with the polar compound in the presence of a radical initiator. Examples of the method for producing the graft-modified ethylene / 1-butene copolymer (A) by a graft reaction of the ethylene / 1-butene copolymer (a) with the polar compound include the following methods: (1) A method for melting the ethylene / 1-butene copolymer (a) and adding the polar or similar compound to copolymerize them by grafting. (2) A method for dissolving ethylene / 1-butene copolymer (a) in a solvent and adding the polar or graft-like compound and copolymerizing them.

[077] In these methods, the amount of polar compound used is generally from 0.010 to 15 parts by mass and preferably from 0.010 to 5.0 parts by mass, based on 100 parts by mass of the ethylene / 1-butene copolymer (a). The amount of radical initiator used is generally from 0.001 to 1.0 parts by mass and preferably from 0.005 to 0.30 parts by mass, based on 100 parts by mass of ethylene / 1-butene copolymer (a).

[078] As a radical initiator, for example, an organic peroxide, an azo compound or a metal hydride can be used. The radical initiator can be used by mixing it directly with the polar compound (e.g., maleic acid or its anhydride), the ethylene / 1-butene copolymer (a) before modification and other components, but it can also be used after it has been dissolved in a small amount of organic solvent. The organic solvent is not particularly limited, as long as it is an organic solvent capable of dissolving the radical initiator.

[079] The reaction temperature in the grafting reaction is generally in the range of 70 to 280 °C and preferably 80 to 260 °C. The reaction time in the grafting reaction is generally Petition 870250081626, dated 11 / 09 / 2025, pages 133 / 166 18 / 50 0.5 to 15 hours, and preferably 1 to 10 hours.

[080] Using an extruder or similar, graft-modified ethylene / 1-butene copolymer (A) can also be produced by reacting the polar compound with the ethylene / 1-butene copolymer (a) in the presence of the radical initiator in the absence of a solvent. The reaction in the absence of a solvent is generally carried out preferably at or above the melting point temperature of the ethylene / 1-butene copolymer (a) for 0.5 to 10 minutes. <Resina de poliamida (B)>

[081] The polyamide resin (B), which is the main component of the polyamide resin composition according to an embodiment of the present invention, is not particularly limited, and various conventionally known polyamide resins, such as an aliphatic polyamide, a semi-aromatic polyamide or an aromatic polyamide, may be used without limitation within the range that does not impair the effects of the present invention. For example, an amino acid lactam or a melt-moldable polyamide resin obtained by a polycondensation reaction between an organic diamine and an organic dicarboxylic acid may be used as polyamide resin (B).

[082] Examples of organic dicarboxylic acids include organic dicarboxylic acids with 4 to 12 carbon atoms, such as adipic acid, pimelic acid, suberic acid, phthalic acid, terephthalic acid, isophthalic acid, naphthalenedicarboxylic acid, phenylenedioxydiacetic acid, sebacic acid, and dodecanedioic acid; and organic dicarboxylic acids with 13 or more carbon atoms, such as oxydibenzoic acid, diphenylmethanedicarboxylic acid, diphenylsulfondicarboxylic acid, and biphenyldicarboxylic acid. Examples of organic diamines include organic diamines with 2 to 13 carbon atoms, such as hexamethylenediamine, octamethylenediamine, nonanediamine, octanediamine, decanediamine, undecanediamine, and dodecanediamine. Petition 870250081626, dated 11 / 09 / 2025, pp. 134 / 166 19 / 50

[083] An example of polyamide resin (B) includes a polycondensate of an organic dicarboxylic acid with 4 to 12 carbon atoms and an organic diamine with 2 to 13 carbon atoms.Examples of polycondensates include polyhexamethylene adipamide [polyamide 66], which is a polycondensate of hexamethylene diamine and adipic acid; polyhexamethylene azelamide [polyamide 69], which is a polycondensate of hexamethylene diamine and azelaic acid; polyhexamethylene sebacamide [polyamide 610], which is a polycondensate of hexamethylene diamine and sebacic acid; and polyhexamethylene dodecanamide [polyamide 612], which is a polycondensate of hexamethylene diamine and dodecanedioic acid; polydecamethylene sebacamide [polyamide 1010], which is a polycondensate of decamethylene diamine and sebacic acid; semi-aromatic polyamides (polyamide 6T, polyamide 9T, polyamide 10T, and polyamide 11T), which are polycondensates of aromatic dicarboxylic acids and aliphatic diamines; and polybis(4-aminocyclohexyl)methanedodecane, which is a polycondensate of bisp-aminocyclohexylmethane and dodecanedioic acid.

[084] An example of polyamide resin (B) also includes a polycondensate of an ω-amino acid. An example of a ω-amino acid polycondensate includes polyundecanamide [Polyamide 11], which is a polycondensate of ω-aminoundecanoic acid.

[085] An example of polyamide resin (B) also includes a one-lactam ring-opening polymer. Examples of one-lactam ring-opening polymers include polycapramide [polyamide 6], which is an ε-aminocaprolactam ring-opening polymer, and polylauric lactam [polyamide 12], which is an ε-aminolaurolactam ring-opening polymer.

[086] The polyamide (B) resin can be modified with a small amount of trivalent or higher polyhydroxylated compound and polycarboxylic acid, such as a triol or a tricarboxylic acid, provided it exhibits thermoplasticity.

[087] From the point of view of the balance between the fluidity of Petition 870250081626, dated 11 / 09 / 2025, pp. 135 / 166 20 / 50 polyamide resin composition and the impact resistance of a molded product, the polyamide resin (B) is preferably one or more aliphatic polyamide resins selected from the group consisting of polyamide 6, polyamide 66, polyamide 11, polyamide 12, polyamide 612, polyamide 610 and polyamide 1010.

[088] Among them, the polyamide resin (B) is preferably an aliphatic polyamide and more preferably polyhexamethylene adipamide [polyamide 66], polyhexamethylene azelamide [polyamide 69] and polycapramide [polyamide 6].

[089] In addition, for example, a polyamide resin produced from adipic acid, isophthalic acid and hexamethylenediamine can be used, and a mixture of two or more compound polyamide resins, such as a mixture of polyamide 6 and polyamide 66, can be used as polyamide resin (B).

[090] A feedstock for polyamide (B) resin can be a feedstock derived from fossil fuels or a feedstock derived from biomass. A feedstock derived from fossil fuels and a feedstock derived from biomass can be combined for use.

[091] The number average molecular weight (Mn) of the polyamide resin (B) measured by GPC is preferably in the range of 15,000 to 27,000, more preferably from 17,000 to 25,000 and particularly preferably from 19,000 to 23,000.

[092] The spiral flow length of polyamide resin (B) measured with an injection molding machine is preferably in the range of more than 600 mm, more preferably more than 625 mm and particularly preferably more than 650 mm.

[093] The spiral flow length of polyamide 66 measured under conditions of a melting temperature of 290°C and an injection pressure of 900 Bar preferably falls within the above range, Petition 870250081626, dated 11 / 09 / 2025, pages 136 / 166 21 / 50 and the spiral flow length of polyamide 6 measured under conditions of a melting temperature of 260°C and an injection pressure of 900 Bar preferably falls within the above range.

[094] When a polyamide resin (B) with a number average molecular weight (Mn) and a spiral flow length within the above range is used, the inherent fluidity of the polyamide resin (B) can be sufficiently displayed in the polyamide resin composition, and this fluidity is not significantly impaired even when mixed with graft-modified ethylene / 1-butene copolymer (A). As a result, the fluidity of the polyamide resin composition and the impact resistance of a molded product containing the polyamide resin composition are excellent in a well-balanced manner. <Composição de resina de poliamida>

[095] The polyamide resin composition according to one embodiment of the present invention preferably contains 50 to 99 parts by mass of polyamide resin (B) and 1 to 50 parts by mass of graft-modified ethylene / 1-butene copolymer (A), based on 100 parts by mass of the total content of polyamide resin (B) and graft-modified ethylene / 1-butene copolymer (A). The polyamide resin composition more preferably contains 65 to 97 parts by mass of polyamide resin (B) and 3 to 35 parts by mass of graft-modified ethylene / 1-butene copolymer (A), and particularly and preferably contains 80 to 95 parts by mass of polyamide resin (B) and 5 to 20 parts by mass of graft-modified ethylene / 1-butene copolymer (A).

[096] When the content of polyamide resin (B) and the content of graft-modified ethylene / 1-butene copolymer (A) in the polyamide resin composition are within the above range, a molded product of the polyamide resin composition exhibits high impact resistance, even when thinner.

[097] It is assumed that the reason for the fluidity of the composition Petition 870250081626, dated 11 / 09 / 2025, pp. 137 / 166 22 / 50 polyamide resin and the impact resistance of the molded product are excellent in a well-balanced manner, as follows.

[098] That is, the ethylene / 1-butene copolymer (a) generally has an MFR10 / MFR2.16 ratio within a specific range and therefore has long chain branches. In addition, the ethylene / 1-butene copolymer (a) generally has a vinyl group content and a total amount of unsaturated linkages within specific ranges. Therefore, the graft-modified ethylene / 1-butene copolymer (A) using the ethylene / 1-butene copolymer (a) has a viscosity ratio close to that of the polyamide resin (B), and the graft-modified ethylene / 1-butene copolymer (A) is easily dispersed in the polyamide resin composition. Furthermore, the graft-modified ethylene / 1-butene copolymer (A) is grafted with the polar compound and therefore has high compatibility with the polyamide resin (B).Therefore, it is conjectured that the graft-modified ethylene / 1-butene copolymer (A) is more likely to be additionally dispersed in the polyamide resin composition, so that the fluidity of the polyamide resin composition and the impact resistance of the molded product are excellent in a well-balanced manner. <Outros componentes>

[099] The polyamide resin composition according to one embodiment of the present invention may additionally contain a component other than polyamide resin (B) and graft-modified ethylene / 1-butene copolymer (A), provided that the purpose of the present invention is not impaired. That is, the polyamide resin composition according to one embodiment of the present invention may contain additives such as a weathering stabilizer, a heat stabilizer, an ultraviolet ray absorber, an infrared ray absorber, an antistatic agent, an anti-slip agent, an agent Petition 870250081626, dated 11 / 09 / 2025, pp. 138 / 166 23 / 50 antiblocking agent, an antifogging agent, a lubricant, a pigment, a dye, a plasticizer, an anti-aging agent, a hydrochloric acid absorber, an antioxidant, a crystal nucleating agent, an antifungal agent, an antibacterial agent, a flame retardant, an organic filler, a release agent, a surfactant, and a softener, if necessary, provided that the purpose of the present invention is not impaired. These additives may be contained individually or in multiple additives. The polyamide resin composition according to one embodiment of the present invention may also contain another polymer, provided that this does not impair the purpose of the present invention. <Método para produção de composição de resina de poliamida>

[100] The polyamide resin composition according to one embodiment of the present invention can be produced by a publicly known method for producing a resin composition accompanied by melt kneading or the like, whereby polyamide resin (B), graft-modified ethylene / 1-butene copolymer (A) and the other arbitrary component are used as raw materials and mixed sequentially or simultaneously. <Aplicação>

[101] The polyamide resin composition according to one embodiment of the present invention exhibits excellent fluidity, and the molded product obtained exhibits high impact resistance, even when made thinner. Therefore, the polyamide resin composition can be used to produce various pellets and molded products. <Pélete>

[102] One embodiment of the present invention is a pellet containing the polyamide resin composition. The pellet has, for example, a spherical, cylindrical, lenticular or cubic shape. The pellet can be produced by a known pelletizing method. A Petition 870250081626, dated 11 / 09 / 2025, pp. 139 / 166 Example 24 / 50 of the method for producing the pellet includes a method for homogeneous melt mixing, for example, of polyamide resin (B), graft-modified ethylene / 1-butene copolymer (A) and another arbitrary component, extruding the mixture with an extruder and then hot or wire cutting the extrudate to produce a spherical, cylindrical or lenticular pellet. In this case, the pellet can be cut in either water or a gas stream, such as air. Furthermore, a cubic pellet can be obtained, for example, by homogeneously mixing the mixture, forming a sheet with a roller or similar and using a sheet pelletizer. The pellet size is preferably 3 cm or less at the longest part of the pellet.

[103] The pellet can be used, for example, to produce a molded product, preferably a melt-formed molded product. The melt-forming can be performed by an arbitrary melt-forming method, such as compression forming, injection molding or extrusion forming. <Artigo moldado por injeção>

[104] One embodiment of the present invention is an injection-molded article comprising the polyamide resin composition. The injection-molded article can be obtained by injection molding the polyamide resin composition by a commonly used method.

[105] The injection-molded article of one embodiment of the present invention is used in a wide range of applications, from household items such as daily necessities and recreational applications, to general industrial applications and industrial products. Examples of applications of the injection-molded article include components or members of various products such as household appliances, telecommunications equipment, electrical and electronic equipment, automobiles, and others. Petition 870250081626, dated 11 / 09 / 2025, pages 140 / 166 25 / 50 vehicles, ships, aircraft, construction materials, civil engineering materials, agricultural materials, power tools, food containers, films, sheets and fibers. Among these, injection-molded articles can be suitablely used as automotive components or members.

[106] The injection molded article can also be used appropriately as components for, for example, a gasoline vehicle, a hybrid vehicle (HV), a plug-in hybrid vehicle (PHV), an electric vehicle (EV), a fuel cell vehicle (FCV). The injection molded article can also be used appropriately as a component for an electric motorcycle.

[107] Automotive components or members include a wide range of components or members, and examples of these include interior components or members, such as a door trim, a door module, an instrument panel, a center panel, a roof panel, a rear door panel, accelerator and brake pedals; vertical exterior panels, such as a door, a fender and a tailgate; horizontal exterior panels, such as a hood and a roof; engine room members, such as an air intake, a front module and a fan shroud; and automotive electrical components.

[108] Examples of automotive electrical components include a wiring harness connector, a cable connector, a lamp socket, a sensor-mounted switch, a combination switch, a battery, an engine mount, a power module, a converter, a capacitor, an insulator, an engine terminal block, and an electric compressor. Examples

[109] Next, an embodiment of the present invention will be described in more detail based on Examples, but the present invention is in no way limited to these Examples.

[110] Each component used in the Examples and Examples Petition 870250081626, dated 11 / 09 / 2025, pages 141 / 166 26 / 50 The following comparisons are made. <Copolímero de etileno / 1-buteno (a)>

[111] To produce the graft-modified ethylene / 1-butene copolymer (A), ethylene / 1-butene copolymers (a-1) to (a-11) and (a'-1) polymerized using a metallocene-based catalyst were used. <Exemplo de produção 1; Produção de copolímero de etileno / 1buteno (a-1)>

[112] In one of the supply ports of a continuous polymerization vessel with an internal volume of 130 L and equipped with stirring blades, a hexane solution of tri-isobutylaluminum was fed as cocatalyst at a rate of 12 mmol / h, a hexane solution of bis(4-methylphenyl)methylene(cyclopentadienyl)(1,2,3,4,7,8,9,10-octahydro-1,1,4,4,7,7,10,10-octamethyldibenzo(b,h)fluoren-12yl)zirconium dichloride as the main catalyst at a rate of 0.0082 mmol / h, and a modified methylaluminoxane hexane suspension solution at a rate of 0.034 mmol / h, and was continuously fed with dehydrated and purified normal hexane used as the polymerization solvent, so that the total rate of catalyst solution and normal hexane was 37.3 L / h.

[113] At the same time, at another supply port of the polymerization vessel, ethylene was continuously fed at a rate of 6.6 kg / h, 1-butene at 8.1 kg / h and hydrogen at 110 NL / h, to carry out continuous solution polymerization under the conditions of a polymerization temperature of 155 °C, a total pressure of 2.5 MPaG and a residence time of 0.5 hours. The standard hexane / toluene mixed solution of ethylene / 1-butene copolymer, produced in the polymerization vessel, was continuously discharged through an outlet provided on one side of the polymerization vessel and was introduced into a connecting tube with a coating portion having been Petition 870250081626, dated 11 / 09 / 2025, pp. 142 / 166 27 / 50 heated with 3 kg / cm2 of steam so that the temperature of the normal ethylene / 1-butene copolymer hexane solution was 130°C.

[114] The standard hexane solution of ethylene / 1-butene copolymer, which had been maintained at approximately 200°C in the connecting tube with a vapor jacket, was continuously fed into a flash tank by adjusting the opening of a pressure control valve installed at the end of the connecting tube to maintain a pressure of approximately 2.5 MPaG. A supply port for methanol injection as a catalyst deactivator was provided just downstream of the pressure control valve, and methanol was injected at about 11 L / h to join the standard hexane solution of ethylene / 1-butene copolymer. Furthermore, during the transfer of the solution to the flash tank, the solution temperature and the opening of the pressure control valve were adjusted so that the pressure in the flash tank was maintained at approximately 0.05 MPaG and the temperature of the vapor portion in the flash tank was maintained at approximately 200°C.Next, the ethylene / 1-butene copolymer was passed through a single-screw extruder with the die temperature set to 170 °C, and the resulting filament was cooled in a water bath and then cut with a pelletizer to obtain the ethylene / 1-butene copolymer (a-1) in pellet form. The yield was 8.2 kg / 2 h. <Exemplo de Produção 2; Produção de copolímero de etileno / 1buteno (a-2)>

[115] The ethylene / 1-butene copolymer (a-2) was produced in the same manner as in Production Example 1, except that the 1-butene feed rate was adjusted to 7.5 kg / h. <Exemplo de Produção 3; Produção de copolímero de etileno / 1buteno (a-3)>

[116] The ethylene / 1-butene copolymer (a-3) was produced from Petition 870250081626, dated 11 / 09 / 2025, pp. 143 / 166 28 / 50 same way as in Production Example 1, except that the 1-butene feed rate was adjusted to 7.4 kg / h. <Exemplo de Produção 4: Produção de copolímero de etileno / 1buteno (a-4)>

[117] The ethylene / 1-butene copolymer (a-4) was produced in the same manner as in Production Example 1, except that bis(4-methylphenyl)methylene(cyclopentadienyl)(1,2,3,4,7,8,9,10-octahydro-1,1,4,4,7,7,10,10-octamethyldibenzo(b,h)fluoren-12yl)zirconium dimethyl and tetrakis(pentafluorophenyl)borate triphenylcarbenium were used as the main catalysts, and the 1-butene feed rate was set to 9.8 kg / h, the ethylene feed rate to 6.9 kg / h and the polymerization temperature to 130°C. <Exemplo de Produção 5; Produção de copolímero de etileno / 1buteno (a-5)>

[118] The ethylene / 1-butene copolymer (a-5) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 6.4 kg / h, the ethylene feed rate was adjusted to 5.0 kg / h and the polymerization temperature was adjusted to 160°C. <Exemplo de Produção 6; Produção de copolímero de etileno / 1buteno (a-6)>

[119] The ethylene / 1-butene copolymer (a-6) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 9.4 kg / h, the ethylene feed rate was adjusted to 6.6 kg / h and the polymerization temperature was adjusted to 150°C. <Exemplo de Produção 7; Produção de copolímero de etileno / 1buteno (a-7)>

[120] The ethylene / 1-butene copolymer (a-7) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 9.1 kg / h, the ethylene feed rate was adjusted to 6.4 kg / h and the temperature was Petition 870250081626, dated 11 / 09 / 2025, pages 144 / 166 29 / 50 polymerization was adjusted to 150°C. <Exemplo de Produção 8; Produção de copolímero de etileno / 1buteno (a-8)>

[121] The ethylene / 1-butene copolymer (a-8) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 8.7 kg / h, the ethylene feed rate was adjusted to 6.2 kg / h and the polymerization temperature was adjusted to 150°C. <Exemplo de Produção 9; Produção de copolímero de etileno / 1buteno (a-9)>

[122] The ethylene / 1-butene copolymer (a-9) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 8.8 kg / h, the ethylene feed rate was adjusted to 6.4 kg / h and the polymerization temperature was adjusted to 140°C. <Exemplo de Produção 10; Produção de copolímero de etileno / 1buteno (a-10)>

[123] The ethylene / 1-butene copolymer (a-10) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was adjusted to 9.8 kg / h, the ethylene feed rate was adjusted to 5.9 kg / h and the polymerization temperature was adjusted to 140°C. <Exemplo de Produção 11; Produção de copolímero de etileno / 1buteno (a-11)>

[124] The ethylene / 1-butene copolymer (a-11) was produced in the same manner as in Production Example 4, except that the 1-butene feed rate was set to 9.4 kg / h, the ethylene feed rate was set to 5.8 kg / h and the polymerization temperature was set to 140°C. <Copolímero de etileno / 1-buteno (a'-1)> ENGAGE 7447 (manufactured by The Dow Chemical Company) was used as an ethylene / 1-butene copolymer (a'-1).

[125] The physical properties of ethylene copolymer / 1 Petition 870250081626, dated 11 / 09 / 2025, pages 145 / 166 30 / 50 butene (a) were evaluated using the following methods of measuring physical properties. Each evaluation result is shown in Table 1. [MFR2.16, MFR10, and MFR10 / MFR2.16]

[126] Each melt flow rate (MFR2.16 and MFR10) were measured under conditions of 190°C and a load of 2.16 kg and under conditions of 190°C and a load of 10 kg according to ASTM D1238, respectively, and the ratio of MFR10 / MFR2.16 was then calculated. [Density]

[127] Density was measured at 25°C according to ASTM D1505. [Content (composition) of the constituent unit derived from the comonomer]

[128] The content of a constituent unit derived from a comonomer was measured using a nuclear magnetic resonance (NMR) measuring instrument (model JNM GX-400, manufactured by JEOL Ltd.). A 0.35 g sample was dissolved in 2.0 mL of hexachlorobutadiene by heating. After filtering this solution through a glass filter (G2), 0.5 mL of deuterated benzene was added and the resulting solution was loaded into an NMR tube with an internal diameter of 10 mm and subjected to 13C-NMR measurement at 120 °C. The number of accumulations was set to 8,000 or more. The content of a constituent unit derived from ethylene and the content (mol%) of a constituent unit derived from 1-butene in the ethylene / 1-butene copolymer were quantitatively determined from the obtained 13C-NMR spectrum. [Vinyl group content, vinylidene group content, total amount of unsaturated bonds]

[129] A 0.35 g sample was dissolved in 2.0 mL of hexachlorobutadiene by heating. After filtering this solution through a glass filter (G2), 0.5 mL of deuterated benzene was added and the resulting solution was loaded into an NMR tube with an internal diameter of 10 mm and subjected to measurement 1H. [Reference to document 870250081626, dated 11 / 09 / 2025, page 146 / 166] 31 / 50 NMR at 120 °C. The number of accumulations was adjusted to 100 or more. The vinyl group content, vinylidene group content, and total amount of unsaturated bonds (bonds / 100,000 carbon atoms) in the ethylene / 1-butene copolymer were quantitatively determined from the obtained 1H-NMR spectrum. The 1H-NMR measurement was performed using a nuclear magnetic resonance (NMR) measuring instrument (model JNM GX-400, manufactured by JEOL Ltd.).

[130] In the 1H-NMR spectrum, signals derived from a vinyl double bond, a vinylidene double bond, a disubstituted olefinic double bond, and a trisubstituted olefinic double bond were observed as signals derived from the double bonds. From the integrated intensity of each signal, the vinyl group content, the vinylidene group content, and the total amount of unsaturated bonds, which is the total amount of vinyl double bonds, vinylidene double bonds, disubstituted olefinic double bonds, and trisubstituted olefinic double bonds, were quantitatively determined. The amount of double bond was quantitatively determined using the peak positions of the signal and the quantification formula described in JP2022-142958A. [Molecular weight distribution (Mw / Mn)]

[131] Gel permeation chromatography (GPC) measurement was performed to obtain a molecular weight in terms of polystyrene Mi-PSt of each fraction. Then, Mi-PSt was converted to a molecular weight in terms of EPR, Mi-EPR using the following formulas: [n]i-PSt X Mi-Pst = [n]i-EPR X Mi-EPR, [n]i-pst= 1.37 X 10-4X Mi-pst0, 686, and [n]i-EPR = 7.2 x 10-4x Mi-EPR0, 667.

[132] A molecular weight distribution (Mw / Mn) was calculated using the molecular weights in terms of EPR.

[133] Gel permeation chromatography (GPC) measurement Petition 870250081626, dated 11 / 09 / 2025, pages 147 / 166 The 32 / 50 assay was performed using an Alliance GPC-2000 gel permeation chromatograph under the following conditions, manufactured by Waters Corporation.

[134] Separation columns: 2 TSKgel GNH6-HT columns and 2 TSKgel GNH6-HTL columns Column size: Diameter 7.5 mm and length 300 mm Column temperature: 140 °C Mobile phase: o-Dichlorobenzene (manufactured by FUJIFILM Wako Pure Chemical Corporation) Antioxidant: BHT (manufactured by Takeda Pharmaceutical Co., Ltd.) 0.025% by mass Movement rate: 1.0 mL / min Sample concentration: 15 mg / 10 mL Sample injection volume: 500 pL Detector: Differential refractometer Standard polystyrene: Polystyrene manufactured by Tosoh. Polystyrene manufactured by the Corporation for a molecular weight range of Mw < 1000 and Mw > 4 x 106 was used, and polystyrene manufactured by Pressure Chemical Co. for a molecular weight range of 1,000 < Mw < 4 x 106 was used. Petition 870250081626, dated 11 / 09 / 2025, pages 148 / 166 33 / 50 [Table 1] Table 1 Copolymer Unit (a-1) Copolymer (a-2) Copolymer (a-3) Copolymer (a-4) Copolymer (a-5) Copolymer (a-6) MFR 2.16 g / 10 min 6.2 5.7 5.3 4.5 5.2 3.3 MFR 10 g / 10 min 47 42 40 34 45 28 MFR 10 / MFR 2.16 - 7.6 7.4 7.5 7.6 8.7 8.5 Density kg / m3 870 873 874 869 871 866 Content of a constituent unit derived from ethylene % by mol 85 87 87 84 85 83 Content of a constituent unit derived from 1-butene % by mol 15 13 13 16 15 17 Vinyl group content Groups / 100,000 carbon atoms 8.7 8.3 9.1 9.0 7.4 9.3 Vinylidene group content Groups / 100,000 carbon atoms 22.1 21.1 23.7 6.9 15.6 13.6 Total number of unsaturated bonds Bonds / 100,000 carbon atoms 109.6 102.6 111.8 55.9 101.8 121.1 Mw / Mn - 2.7 2.5 2.6 2.3 2.3 2.3 Petition 870250081626, dated 11 / 09 / 2025, pages 149 / 166 34 / 50 Table 1 (continued) Copolymer Unit (a-7) Copolymer (a-8) Copolymer (a-9) Copolymer (a-10) Copolymer (a-11) Copolymer (a'-1) MFR 2.16 g / 10 min 5.5 13.4 9.4 3.0 5.0 5.0 MFR 10 g / 10 min 45 99 70 24 38 32 MFR 10 / MFR 2.16 - 8.2 7.4 7.4 8.0 7.6 6.4 Density kg / m3 867 868 869 863 864 868 Content of a constituent unit derived from ethylene % by mol 84 84 85 82 82 84 Content of a constituent unit derived from 1-butene % by mol 16 16 15 18 18 16 Vinyl group content Groups / 100,000 carbon atoms 9.2 8.8 9.0 8.9 8.9 4.6 Vinylidene group content Groups / 100,000 carbon atoms 19.7 19.7 20.1 18.4 14.9 7.9 Total number of unsaturated bonds Bonds / 100,000 carbon atoms 119.4 106.0 112.3 102.5 106.3 36.6 Mw / Mn - 2.4 2.4 2.5 2.3 2.3 2.3 Petition 870250081626, dated 11 / 09 / 2025, pages 150 / 166 35 / 50<Copolímero de etileno / 1-buteno modificado por enxerto (A)>

[135] The graft-modified ethylene / 1-butene copolymers (A-1) to (A-11) and (A'-1) obtained by the following production methods were used as graft-modified ethylene / 1-butene copolymers (A).

[136] The physical properties of the graft-modified ethylene / 1-butene copolymer (A) were evaluated by the physical property measurement method described above and by a graft modification amount measurement method described later. The evaluation results are presented in Table 2. [Graft-modified ethylene / 1-butene copolymer (A1)]

[137] A solution of 100 g maleic anhydride (MAH) and 5 g of 2,5-dimethyl-2,5-di-(t-butylperoxy)-3-hexyne (product name: Perhexyne 25B, manufactured by NOF CORPORATION) in acetone was mixed with 10 kg of ethylene / 1-butene copolymer (a-1). The resulting mixture was then fed into a twin-screw extruder with a screw diameter of 25 mm and L / D=42 through a hopper, and extruded into a strand at a resin temperature of 250 °C, a screw rotation speed of 150 rpm and a discharge rate of 7 kg / h. The resulting strand was completely cooled and then granulated to obtain a graft-modified ethylene / 1-butene copolymer (A-1). [Graft-modified ethylene / 1-butene copolymer (A2)]

[138] The graft-modified ethylene / 1-butene copolymer (A-2) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-2) was used. [Graft-modified ethylene / 1-butene copolymer (A3)] Petition 870250081626, dated 11 / 09 / 2025, pages 151 / 166 36 / 50

[139] The graft-modified ethylene / 1-butene copolymer (A-3) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-3) was used. [Graft-modified ethylene / 1-butene copolymer (A4)]

[140] The graft-modified ethylene / 1-butene copolymer (A-4) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-4) was used. [Graft-modified ethylene / 1-butene copolymer (A5)]

[141] The graft-modified ethylene / 1-butene copolymer (A-5) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-5) was used. [Graft-modified ethylene / 1-butene copolymer (A6)]

[142] The graft-modified ethylene / 1-butene copolymer (A-6) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-6) was used. [Graft-modified ethylene / 1-butene copolymer (A7)]

[143] The graft-modified ethylene / 1-butene copolymer (A-7) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-7) was used. Petition 870250081626, dated 11 / 09 / 2025, pages 152 / 166 37 / 50 [Graft-modified ethylene / 1-butene copolymer (A8)]

[144] The graft-modified ethylene / 1-butene copolymer (A-8) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-8) was used. [Graft-modified ethylene / 1-butene copolymer (A9)]

[145] The graft-modified ethylene / 1-butene copolymer (A-9) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-9) was used. [Graft-modified ethylene / 1-butene copolymer (A10)]

[146] The graft-modified ethylene / 1-butene copolymer (A-10) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-10) was used. [Graft-modified ethylene / 1-butene copolymer (A11)]

[147] The graft-modified ethylene / 1-butene copolymer (A-11) was obtained in the same manner as in the graft-modified ethylene / 1-butene copolymer (A-1) preparation method above, except that the ethylene / 1-butene copolymer (a-11) was used. [Graft-modified ethylene / 1-butene copolymer (A'1)]

[148] The graft-modified ethylene / 1-butene copolymer (A'-1) was obtained in the same manner as in the method for preparing the graft-modified ethylene / 1-butene copolymer (A-1) Petition 870250081626, dated 11 / 09 / 2025, pages 153 / 166 38 / 50 above, except that the ethylene / 1-butene copolymer (a'-1) was used. [Amount of graft modification]

[149] The amount of graft modification (maleic anhydride modification amount (wt%)) in each of the graft-modified ethylene / 1-butene copolymers (A-1) to (A-11) and (A'-1) was determined from a separately prepared calibration curve based on the peak intensity at a wavenumber of 1780 cm-1 assigned to a carbonyl group in FT-IR. Petition 870250081626, dated 11 / 09 / 2025, pages 154 / 166 39 / 50 [Table 2] Table 2 Copolymer Unit (A-1) Copolymer (A-2) Copolymer (A-3) Copolymer (A-4) Copolymer (A-5) Copolymer (A-6) Copolymer (a-1) Parts by mass 100 Copolymer (a-2) Parts by mass 100 Copolymer (a-3) Parts by mass 100 Copolymer (a-4) Parts by mass 100 Copolymer (a-5) Parts by mass 100 Copolymer (a-6) Parts by mass 100 Copolymer (a-7) Parts by mass Copolymer (a-8) Parts by mass Copolymer (a-9) Parts by mass Copolymer (a-10) Parts by mass Copolymer (a-11) Parts by mass Copolymer (a'-1) Parts by mass Maleic anhydride Parts by mass 1 1 1 1 1 1 Perhexine 25B Parts by mass 0.05 0.05 0.05 0.05 0.05 0.05 Graft modification amount % by mass 0.7 0.7 0.6 0.7 0.5 0.5 MFR 2.16 g / 10 min 0.78 0.69 0.70 0.77 0.65 0.38 Petition 870250081626, dated 11 / 09 / 2025, pages 155 / 166 40 / 50 MFR 10 g / 10 min 11.5 11.2 10.2 10.9 9.4 6.3 MFR 10 / MFR 2.16 - 14.7 16.2 14.6 14.2 14.5 16.6 Density kg / m3 873 875 876 ​​871 873 870 Vinyl group content Groups / 100,000 carbon atoms 7.7 7.2 8.2 7.0 6.9 8.2 Vinylidene group content Groups / 100,000 carbon atoms 20.9 19.9 21.9 5.9 14.1 12.7 Total number of unsaturated bonds Bonds / 100,000 carbon atoms 124.8 118.4 121.5 58.0 114.8 135.1 Mw / Mn - 4.1 3.8 3.7 4.1 4.1 3.7 Table 2 (continued) Copolymer Unit (A-7) Copolymer (A-8) Copolymer (A-9) Copolymer (A-10) Copolymer (A-11) Copolymer (A'-l) Copolymer (a-1) Parts by mass Copolymer (a-2) Parts by mass Copolymer (a-3) Parts by mass Copolymer (a-4) Parts by mass Copolymer (a-5) Parts by mass Copolymer (a-6) Parts by mass Copolymer (a-7) Parts by mass 100 Copolymer (a-8) Parts by mass 100 Copolymer (a-9) Parts by mass 100 Petition 870250081626, dated 11 / 09 / 2025, pages 156 / 166 41 / 50 Copolymer (α-10) Parts by mass 100 Copolymer (α-11) Parts by mass 100 Copolymer (α'-1) Parts by mass 100 Maleic anhydride Parts by mass 1 1 1 1 1 1 Perhexine 25B Parts by mass 0.05 0.05 0.05 0.05 0.05 0.05 Graft modification amount % by mass 0.7 0.7 0.6 0.7 0.5 0.7 MFR 2.16 g / 10 min 4.63 3.61 1.35 1.77 1.34 1.28 MFR 10 g / 10 min 53 42 16.4 22.1 16.2 14 MFR 10 / MFR 2.16 - 11.5 11.7 12.1 12.5 12.1 10.9 Density kg / m3 872 867 870 864 865 871 Vinyl group content Groups / 100,000 carbon atoms 7.4 7.3 8.1 7.8 7.1 3.9 Vinylidene group content Groups / 100,000 carbon atoms 8.9 12.3 15.3 13.1 10.3 7.4 Total number of unsaturated bonds Bonds / 100,000 carbon atoms 89.4 109.6 103.5 96.4 98.1 37.1 Mw / Mn - 3.7 4.1 4.2 3.9 3.9 4.1 Petition 870250081626, dated 11 / 09 / 2025, pages 157 / 166 42 / 50<Resina de poliamida (B)>

[150] The following polyamide resins (B-1) and (B-2) were used as polyamide resins (B). [Polyamide resin (B-1)]

[151] Polyamide 66 (product name: Amilan CM3007, manufactured by Toray Industries, Inc.), with a spiral flow length greater than 700 mm at a melting temperature of 290°C and an injection pressure of 900 bar. [Polyamide resin (B-2)]

[152] Polyamide 6 (product name: Amilan CM1007, manufactured by Toray Industries, Inc.), with a spiral flow length greater than 700 mm at a melting temperature of 260°C and an injection pressure of 900 bar. [Example 1]

[153] A dry mix was prepared by mixing 10 parts by mass of graft-modified ethylene / 1-butene copolymer (A-1) and 90 parts by mass of polyamide resin (B-1), which was polyamide 66, using a Henschel mixer.

[154] The dry mixture was then fed into the main inlet of a twin-screw extruder (L / D=40, 30 ®πΦ) set to 285°C and extruded at a screw rotation speed of 180 rpm and a discharge rate of 15 kg / h to prepare a pellet from the polyamide resin composition.

[155] The resulting pellet from the polyamide resin composition was dried at 100°C for 24 hours, and then injection molded to prepare a sample for a physical property test, and the physical properties of the polyamide resin composition were evaluated by the following test methods. The evaluation results are presented in Table 3. [Physical property test] (1) Charpy impact test

[156] Under the following test conditions, a hammer was rotated on the back of the notch of a fixed test specimen, Petition 870250081626, dated 11 / 09 / 2025, pp. 158 / 166 43 / 50 and the impact resistance was calculated based on the hammer rebound angle after specimen fracture and the initial release angle before testing. (Test conditions)

[157] Test temperature: 23°C / -40°C, hammer capacity: 4J, elevation angle: 149.9, test specimen: notched, with a remaining width of 8 mm and a width of 4 mm. (2) Fluidity

[158] Injection molding was performed in a mold with a 3.8 ®πΦ semicircular spiral groove, using an injection molding machine at a cylinder temperature of 290°C, injection pressure of 100 MPa, mold temperature of 80°C under a clamping force of 50 t, and a flow distance (spiral flow length) was then measured. [Examples 2 to 17 and Comparative Examples 1 to 4]

[159] A pellet of the polyamide resin composition was produced and dried, a test specimen was prepared, and its physical properties were evaluated in the same manner as in Example 1, except that the compositions of the graft-modified ethylene / 1-butene copolymer (A) and the polyamide resin (B) used in Example 1 were altered as shown in Tables 3 to 5. The evaluation results are shown in Tables 3 to 5. [Examples 18 to 28 and Comparative Examples 5 to 7]

[160] A pellet of the polyamide resin composition was produced and dried, a test specimen was prepared, and its physical properties were evaluated in the same manner as in Example 1, except that the preset temperature of the twin-screw extruder was changed to 245 °C, the compositions of the graft-modified ethylene / 1-butene copolymer (A) and the polyamide resin (B) were changed as shown in Tables 4 and 5, and the cylinder temperature at the evaluation of Petition 870250081626, dated 11 / 09 / 2025, pages 159 / 166 44 / 50 fluidity was changed to 245 °C. The results of each evaluation are shown in Tables 4 and 5. Petition 870250081626, dated 11 / 09 / 2025, pages 160 / 166 45 / 50 [Table 3] Table 3 Unit Example 1 Example 2 Example 3 Example 4 Example 5 Example 6 Example 7 Copolymer (A-1) Parts by mass 10 Copolymer (A-2) Parts by mass 10 Copolymer (A-3) Parts by mass 10 Copolymer (A-4) Parts by mass 10 Copolymer (A-5) Parts by mass 10 Copolymer (A-6) Parts by mass 10 Copolymer (A-7) Parts by mass 8 Copolymer (A-8) Parts by mass Copolymer (A-9) Parts by mass Copolymer (A-10) Parts by mass Copolymer (A-11) Parts by mass Copolymer (A'-1) Parts by mass Polyamide resin (B-1) Parts by mass 90 90 90 90 90 90 92 Polyamide resin (B-2) Parts by mass Charpy impact resistance 23°C (with a notch) kJ / m2 9.6 8.9 8.9 9.1 8.6 8.7 9.0 -40°C (with a notch) kJ / m2 7.0 6.7 6.6 7.4 7.0 7.4 5.3 Petition 870250081626, dated 11 / 09 / 2025, pages 161 / 166 46 / 50 Flow rate Spiral flow length cm 72.0 73.0 74.0 74.0 74.0 72.0 76.0 Table 3 (continued) Unit Example 8 Example 9 Example 10 Example 11 Example 12 Example 13 Example 14 Copolymer (A-1) Parts by mass Copolymer (A-2) Parts by mass Copolymer (A-3) Parts by mass Copolymer (A-4) Parts by mass Copolymer (A-5) Parts by mass Copolymer (A-6) Parts by mass Copolymer (A-7) Parts by mass 10 12 Copolymer (A-8) Parts by mass 8 10 12 Copolymer (A-9) Parts by mass 8 10 Copolymer (A-10) Parts by mass Copolymer (A-11) Parts by mass Copolymer (A'-1) Parts by mass Polyamide resin (B-1) Parts by mass 90 88 92 90 88 92 90 Polyamide resin (B-2) Parts by mass Charpy impact resistance 23°C (with a notch) kJ / m2 11.3 12.8 9.0 12.0 12.7 9.2 12.1 -40°C (with a kJ / m2 7.5 8.6 6.4 6.9 8.7 5.8 7.1 Petition 870250081626, dated 11 / 09 / 2025, pages 162 / 166 47 / 50 (Notch) Flow Spiral flow length cm 75.0 73.0 76.0 74.0 72.0 74.0 73.0 [Table 4] Table 4 Example Unit 15 Example 16 Example 17 Example 18 Example 19 Example 20 Example 21 Copolymer (A-1) Parts by mass Copolymer (A-2) Parts by mass Copolymer (A-3) Parts by mass Copolymer (A-4) Parts by mass Copolymer (A-5) Parts by mass Copolymer (A-6) Parts by mass Copolymer (A-7) Parts by mass 8 10 12 Copolymer (A-8) Parts by mass 8 Copolymer (A-9) Parts by mass 12 Copolymer (A-10) Parts by mass 10 Copolymer (A-11) Parts by mass 10 Copolymer (A'-1) Parts by mass Polyamide resin (B-1) Parts by mass 88 90 90 Polyamide resin (B-2) Parts by mass 92 90 88 92 Petition 870250081626, dated 11 / 09 / 2025, pages 163 / 166 48 / 50 Charpy impact resistance 23°C (with a notch) kJ / m2 13.4 12.7 9.7 11.2 13.4 14.9 11.7 -40°C (with a notch) kJ / m2 8.6 7.9 6.8 6.1 8.5 9.9 6.4 Flow Spiral flow length cm 71.0 72.0 72.0 72.0 70.0 68.0 72.0 Table 4 (continued) Unit Example 22 Example 23 Example 24 Example 25 Example 26 Example 27 Example 28 Copolymer (A-1) Parts by mass Copolymer (A-2) Parts by mass Copolymer (A-3) Parts by mass Copolymer (A-4) Parts by mass Copolymer (A-5) Parts by mass Copolymer (A-6) Parts by mass Copolymer (A-7) Parts by mass Copolymer (A-8) Parts by mass 10 12 Copolymer (A-9) Parts by mass 8 10 12 Copolymer (A-10) Parts by mass 10 Copolymer (A-11) Parts by mass 10 Copolymer (A'-1) Parts by mass Petition 870250081626, dated 11 / 09 / 2025, pages 164 / 166 49 / 50 Polyamide resin (B-1) Parts by mass Polyamide resin (B-2) Parts by mass 90 88 92 90 88 90 90 Charpy impact resistance 23°C (with a notch) kJ / m2 13.1 15.3 11.6 13.0 15.1 14.1 11.4 -40°C (with a notch) kJ / m2 6.9 8.7 5.8 7.1 8.6 7.9 6.8 Flow Spiral flow length cm 71.0 69.0 71.0 70.0 68.0 69.0 68.0 [Table 5] Table 5 Unit Example Comparative 1 Example Comparative 2 Example Comparative 3 Example Comparative 4 Example Comparative 5 Example Comparative 6 Example Comparative 7 Copolymer (A-1) Parts by mass Copolymer (A-2) Parts by mass Copolymer (A-3) Parts by mass Copolymer (A-4) Parts by mass Copolymer (A-5) Parts by mass Copolymer (A-6) Parts by mass Copolymer (A-7) Parts by mass Copolymer (A-8) Parts by mass Petition 870250081626, dated 11 / 09 / 2025, pages 165 / 166 50 / 50 Copolymer (A-9) Parts by mass Copolymer (A-10) Parts by mass Copolymer (A-11) Parts by mass Copolymer (A'-1) Parts by mass 10 8 12 8 10 12 Polyamide resin (B-1) Parts by mass 100 90 92 88 Polyamide resin (B-2) Parts by mass 92 90 88 Charpy impact resistance 23°C (with a notch) kJ / m2 4.9 8.0 6.0 8.6 7.8 10.1 11.9 -40°C (with a notch) kJ / m2 2.7 6.3 4.7 6.8 5.4 6.3 7.3 Flowability Spiral flow length cm 76.0 71.0 72.0 69.0 67.0 65.0 62.0 Petition 870250081626, dated 11 / 09 / 2025, p. 166 / 166

Claims

1 / 3 CLAIMS 1. Graft-modified ethylene / 1-butene copolymer (A), obtained by graft modification of an ethylene / 1-butene copolymer (a) with a polar compound, characterized in that the ethylene / 1-butene copolymer (a) satisfies the following requirements (ai) and (a-ii): requirement (ai): a ratio (MFR10 / MFR2.16) of a melt flow rate (MFR10) measured under conditions of 190°C and a 10 kg load according to ASTM D1238 to a melt flow rate (MFR2.16) measured under conditions of 190°C and a 2.16 kg load according to ASTM D1238 is in the range of 6.7 to 9.0; and requirement (a-ii): the vinyl group content is in the range of 5.0 to 20.0 groups and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100,000 carbon atoms, as calculated by 1H-NMR.

2. Graft-modified ethylene / 1-butene copolymer (A), according to claim 1, characterized in that the polar compound is at least one selected from the group consisting of an ethylenically unsaturated compound containing a hydroxyl group, an ethylenically unsaturated compound containing an amino group, an ethylenically unsaturated compound containing an epoxy group, an aromatic vinyl compound, an unsaturated carboxylic acid and a derivative thereof, a vinyl ester compound and vinyl chloride.

3. Graft-modified ethylene / 1-butene copolymer (A), obtained by graft modification of an ethylene / 1-butene copolymer (a) with a polar compound, characterized in that the graft-modified ethylene / 1-butene copolymer (A) satisfies the following requirements (Ai) to (Av): requirement (Ai): a ratio (MFR10 / MFR2.16) of a melt flow rate (MFR10) measured under conditions of 190°C and a 10 kg charge according to ASTM D1238 for a melt flow rate. Petition 870250081626, dated 11 / 09 / 2025, page. 63 / 166 2 / 3 (MFR2,16) measured under conditions of 190°C and a load of 2.16 kg according to ASTM D1238 is in the range of 11.5 to 18.0; requirement (A-ii): the vinyl group content is in the range of 5.0 to 20.0 groups and the total amount of unsaturated bonds is in the range of 40.0 to 200.0 bonds, per 100.000 carbon atoms, as calculated by 1H-NMR; requirement (A-iii): a graft modification amount is in the range of 0.1 to 2.0% by mass based on 100% by mass of the graft-modified ethylene / 1-butene copolymer (A); requirement (A-iv): a melt flow rate (MFR2,16) measured in accordance with ASTM D1238 under conditions of 190°C and a charge of 2.16 kg, is in the range of 0.01 to 5.00 g / 10 min; and requirement (Av): a density measured in accordance with ASTM D1505 under conditions of 25°C, is in the range of 850 to 885 kg / m3.

4. Graft-modified ethylene / 1-butene copolymer (A), according to claim 3, characterized in that the polar compound is at least one selected from the group consisting of an unsaturated carboxylic acid and a derivative thereof.

5. Polyamide resin composition, characterized in that it comprises 1 to 50 parts by mass of graft-modified ethylene / 1-butene copolymer (A) as defined in any one of claims 1 to 4, and 50 to 99 parts by mass of a polyamide resin (B), based on 100 parts by mass of a total of graft-modified ethylene / 1-butene copolymer (A) and polyamide resin (B).

6. Polyamide resin composition according to claim 5, characterized in that the polyamide resin (B) is one or more aliphatic polyamide resins selected from the group consisting of polyamide 6, polyamide 66, polyamide 11, polyamide 12, polyamide 612, polyamide 610 and polyamide 1010.

7. Pellet, characterized in that it comprises the composition of polyamide resin as defined in claim 5.

8. Molded product, characterized in that it comprises a polyamide resin composition as defined in claim 5.

9. Injection-molded article, characterized in that it comprises a polyamide resin composition as defined in claim 5.

10. Automotive component, characterized in that it comprises a polyamide resin composition as defined in claim 5.

11. Electronic component, characterized in that it comprises a polyamide resin composition as defined in claim 5.

12. Automotive electrical component, characterized in that it comprises a polyamide resin composition as defined in claim 5. Petition 870250081626, dated 11 / 09 / 2025, pp. 65 / 166