JPH05318681A - Resin laminated matter for which modified propylene polymer is used - Google Patents

Abstract

PURPOSE:To hold even high heat welding properties to the surface of polyamide as mechanical strength, heat resistance and oil resistance are kept on, by a method wherein the title laminated matter is constituted of a modified propylene polymer, which is obtained by making a propylene polymer and vinyl monomers each containing aromatic and functional groups in a molten state perform polymerization reaction, and a layer of polyamide. CONSTITUTION:Vinyl monomers each containing aromatic and epoxy groups or carboxyl group are mixed up with a propylene polymer, melting, kneading and polymerization of which are made to perform in the presence of a radical initiator and a plopylene-polyamide resin laminated matter wherein a specific modified propylene polymer and the surface of polyamide possess excellent heat welding properties is obtained. Then as for preparation, after performance of melting, kneading and polymerization reaction of the powdery or pelletlike propylene polymer obtained by impregnating the same with the vinyl monomer containing the epoxy group or carboxyl group, the vinyl monomer containing a functional group and the vinyl monomer containing the aromatic group by heating while pressurizing the same by an extruding machine, strand discharged through a die is cooled and obtained as a pellet by a pelletizer.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a useful polypropylene-polyamide laminate, and more specifically, a resin laminate comprising a specific modified propylene-based polymer excellent in heat fusion property with polyamide and polyamide. Regarding

[0002]

2. Description of the Related Art Polypropylene itself is low in cost, excellent in mechanical strength, heat resistance and oil resistance and, in addition, excellent in appearance. Therefore, it is widely used as a film, a sheet, a molded product and the like in food packaging materials and the like. However, polypropylene has the drawback of being poor in gas barrier properties against oxygen and the like. Therefore, in order to provide polypropylene with a gas barrier property, a resin laminate in which polyamide is laminated has been devised.

However, such polypropylene is
It has no polar groups or reactive active groups (reactive polar groups) in its molecular structure, and therefore is a problematic resin for secondary processing, and has high heat fusion property with the polyamide layer. I can't have it.

Therefore, the affinity of the polypropylene surface with respect to the polyamide is determined by various methods such as various surface treatments on the surface of the polypropylene molded article or addition of other polymer substances. Attempts have been made to improve the.

For example, as a method of adding other polymer substances to polypropylene, a method of adding a resin having a reactive polar group such as a carboxylic acid modified polyolefin or a saponified ethylene-vinyl acetate copolymer, etc. However, various attempts have been made such as a method of improving the heat fusion property by adding an inorganic substance to polypropylene.

A method using a so-called carboxylic acid-modified polypropylene obtained by melt-kneading a polyolefin with various vinyl monomers such as acrylic acid or maleic anhydride in the presence of a radical initiator. Further, there is also provided a method in which a resin mixture obtained by melt-kneading a copolymer of ethylene and acrylic acid or the like with the modified polypropylene and a radical initiator is laminated with polyamide so as to have thermal adhesiveness ( Tokkyo 4-210
No. 2).

[0007]

However, the method of imparting the heat fusible property to the polyamide by adding the polar group-containing resin to the propylene-based polymer is a polar group in order to improve the heat fusible property. If the amount is increased, the compatibility with the propylene-based polymer, which is a non-polar polymer, will be reduced, and eventually the polypropylene's original properties (physical properties) will be lost. There are also cases where the layer itself delaminates. Therefore, there is a limit (upper limit) that the introduction amount of the polar group must be kept within a range that does not reduce various physical properties, and as a result, the effect of improving the heat fusion property is naturally limited. After all, the reality is that we have not reached the point where the demand is satisfied. Even if the method of adding an inorganic substance is used, there is a drawback in that the intended use is also limited.

Further, a polyamide resin obtained by using a so-called modified polypropylene, which is obtained by melt-kneading a vinyl monomer such as acrylic acid or maleic anhydride with polypropylene in the presence of a radical initiator. The effect of improving heat fusion in the laminate is not sufficient with polypropylene modified with the vinyl monomer alone, and in food packaging applications, interlayer adhesion of the laminate due to contact with water vapor. Has a drawback that it cannot be used for this purpose.

Further, polypropylene itself is
As long as the conventional method based on the melt-kneading method is applied to the radical-disintegrating polymer, there is a problem that the decomposition reaction of polypropylene inevitably occurs and the original physical properties are lost.

That is, when the amount of the vinyl monomer is increased in order to improve the heat fusion property, it is necessary to increase the amount of the radical initiator in accordance with the increase in the amount of the vinyl monomer. However, there was a problem in performance. Further, if the amount of the radical polymerization initiator is reduced in order to suppress the decomposition reaction, the polymerization rate of the functional group-containing vinyl monomer will be reduced, and problems of various performances will come out.

Further, a method of laminating a resin mixture obtained by melt-kneading a copolymer of ethylene and acrylic acid and the like with a radical initiator to polypropylene modified with carboxylic acid to obtain heat fusion property is described. However, the manufacturing process is time-consuming, and the polypropylene resin mixture produced is not yet sufficiently heat-fusible.

As described above, as long as the conventional method as described above is followed, it is satisfactory in terms of heat fusion property with the surface of polyamide, various physical properties of polypropylene, and manufacturing process.
The reality is that a laminate with a polyamide resin of extremely high usefulness cannot be obtained.

Therefore, a polyamide having a very high practicability, which does not lose the mechanical properties, heat resistance, oil resistance and other properties of polypropylene, and has a high heat fusion property with the surface of the polyamide. If a laminate with a resin can be obtained, it can be expected that the application can be expanded and the production efficiency can be greatly improved.

Therefore, the inventors of the present invention eagerly started research in order to solve and solve the above-mentioned drawbacks of the conventional method. The problem to be solved by the present invention is to eliminate complicated steps, and at the same time, while maintaining various properties such as mechanical strength, heat resistance and oil resistance, in particular, high heat fusion property with a polyamide surface. And a resin laminate of polypropylene and polyamide.

[0015]

The present inventors have focused on the problems to be solved by the invention as described above,
As a result of earnest and repeated studies, it was obtained by carrying out a melt-kneading polymerization reaction between an aromatic vinyl monomer and a functional group-containing vinyl monomer in the presence of a propylene polymer in a molten state in an extruder. The specific modified propylene-based polymer is very high with the polyamide surface without deteriorating the properties of the propylene-based polymer due to the combined effect of the aromatic vinyl monomer and the functional group-containing vinyl monomer. The present invention has been completed here by finding that it is possible to provide a laminate of an excellent polypropylene and a polyamide resin having a heat fusion property.

Further, the modified propylene-based polymer obtained by the above-mentioned polymerization method itself has high transparency, and the use thereof is further widened.

[0017]

[Structure] That is, the present invention provides a layer of a modified propylene-based polymer obtained by subjecting a propylene-based polymer in a molten state to a melt-kneading polymerization reaction of an aromatic vinyl monomer and a functional group-containing vinyl monomer. And a polyamide layer, specifically, a propylene-based polymer, an aromatic vinyl monomer and an epoxy group-containing vinyl monomer or a carboxyl group-containing vinyl monomer. Of a specific modified propylene-based polymer and a polyamide surface, which are obtained by reacting a polymer with a radical initiator in the presence of a radical initiator, and a melt-kneading polymerization reaction, and have an extremely high heat fusion property, which is extremely practical. It is intended to provide a propylene-polyamide resin laminate. The present invention will be described in detail below.

First, the preparation of the modified propylene polymer used in the present invention will be described below. The propylene-based polymer used in preparing the modified propylene-based polymer refers to a propylene homopolymer and a copolymer of propylene-based other olefins or ethylenic vinyl monomers. To do. It is preferable that each of the propylene-based polymers contains 75% by weight or more of propylene. Specifically, isotactic polypropylene, propylene-ethylene copolymer, propylene-ethylene-
Butene copolymer, propylene-butene copolymer, maleic anhydride-modified polypropylene and the like are particularly representative. Of course, these propylene-based polymers may be mixed and used. Further, deviating from the object of the present invention,
Other polymers may be used within a range that does not impair the effects of the present invention and within a range that does not impair the properties of the propylene-based polymer.

Here, the functional group-containing vinyl monomer must be a vinyl monomer having a functional group capable of reacting with the terminal functional group of the polyamide, and specifically, an epoxy group-containing vinyl monomer. It is preferably a vinyl monomer or a carboxyl group-containing vinyl monomer.

As typical examples of the epoxy group-containing vinyl monomer, glycidyl methacrylate, glycidyl acrylate, allyl glycidyl ether, methacryl glycidyl ether and the like can be given, which may be used alone or in combination of two or more kinds. Of course good things.

Further, only typical examples of the carboxyl group-containing vinyl monomer are acrylic acid,
Methacrylic acid, itaconic acid, maleic anhydride, maleic acid and the like are commonly used vinyl monomers, and it goes without saying that these may be used alone or in combination of two or more kinds.

As typical examples of the aromatic vinyl monomer, styrene, methylstyrene, vinyltoluene, vinylxylene, ethylvinylbenzene,
Of course, isopropyl styrene, chlorostyrene, dichlorostyrene, bromostyrene, etc. may be used alone or in combination of two or more kinds.

Further, only typical vinyl monomers copolymerizable with the above-mentioned epoxy group-containing vinyl monomer or carboxyl group-containing vinyl monomer will be given below. Vinyl esters of
Various alkyl esters such as acrylic acid, methacrylic acid or maleic acid; or acrylonitrile,
Various vinyl cyanides, etc., and these copolymerizable vinyl monomers may be used in combination.

The amount of the functional group-containing vinyl monomer added is preferably 20% by weight or less of the propylene polymer,
More preferably, the range of 0.1 to 10% by weight is suitable. When it exceeds 20% by weight, the polymerization rate is lowered and the amount of unreacted monomer is increased, which is not preferable, and further, there is a problem that mechanical properties are lowered. .

The amount of the aromatic vinyl monomer added is preferably 35% by weight or less of the propylene polymer,
More preferably, the range of 2 to 10% by weight is suitable. If it exceeds 35% by weight, the various properties of polypropylene are apt to be impaired, which is also undesirable. Further, the aromatic vinyl monomer is at least the same amount or more of the addition amount of the functional group-containing vinyl monomer, in order to prevent the modified propylene polymer from having a low molecular weight and to improve the heat fusion property with the polyamide layer, preferably. Is preferably added in an amount of 1 to 5 times.

As the radical polymerization initiator (radical initiator), the characteristic feature of the present invention is that the main melt-kneading polymerization reaction is carried out at a temperature of the melt-kneading temperature of the propylene-based polymer, so that it is reduced by half for one minute. The decomposition temperature is 1
It is desirable to be in the range of 30 to 250 ° C.

Specific examples of the radical initiator having such characteristics include tert-butyl peroctate, bis (tert-butyl peroxy) trimethylcyclohexane, cyclohexanone peroxide, benzoyl peroxide, dicumyl peroxide and tert-butyl peroxide.
Butyl perbenzoate, dimethyl di (tert-butyl peroxy) hexane or dimethyl di (ter)
Organic peroxides such as t-butylperoxy) hexyne are particularly representative.

The amount of the organic peroxide used is usually 0.1 to 10 relative to 100 parts by weight of the total amount of vinyl monomers.
It is preferably within the range of parts by weight, more preferably 1 to
A range of 5 parts by weight is suitable.

As other additives, it is necessary to use a stabilizer because polypropylene itself is a radical-disintegrating polymer unlike polyethylene. However, it is necessary to consider the type and amount of addition so as not to hinder the polymerization of various vinyl monomers as described above.

As such stabilizers, only typical ones are exemplified by pentaerythrityl-tetrakis (di-tert-butyl-hydroxyphenyl) propionate) and ocdecyl (di-tert-butyl-).
Hydroxyphenyl) propionate, thiobis (methyl-tert-butylphenol) or trimethyl-
Various hindered phenolic stabilizers such as tris (di-tert-butylhydroxybenzyl) benzene; tetrakis (di-t-butylphenyl) biphenylene phosphite or tris (di-t-butylphenyl) phosphite, Various phosphorus stabilizers; various metal soaps such as zinc stearate or calcium stearate; and various antacid adsorbents such as magnesium oxide or hydrotalcite.

The amount of the stabilizer used is usually 0.01 to 1 with respect to 100 parts by weight of the propylene polymer.
Parts by weight, preferably 0.05 to 0.5 parts by weight.
The method for producing the polypropylene polymer of the present invention will be described.

The melt-kneading polymerization reaction of the propylene-based polymer with the functional group-containing vinyl monomer and the aromatic vinyl monomer is carried out by various kneading vessels such as a Banbury mixer or various continuous kneading such as an extruder. It can be performed using a machine. Above all, an extruder is preferable in view of industrial production such as granulation (chemical). In addition, the twin-screw extruder is more suitable for supplying reactants and kneading,
Alternatively, it can be said that management of the polymerization time and the like is easier.

The actual preparation was carried out by impregnating a vinyl monomer containing a functional group such as a vinyl monomer containing an epoxy group or a vinyl monomer containing a carboxyl group with an aromatic vinyl monomer.
A powdery or pelletized propylene-based polymer is supplied to an extruder and heated under pressure to 130 to 250 ° C. to carry out a melt-kneading polymerization reaction, and then the strand discharged from the die is cooled and a pelletizer is used. Used as a pellet.

These vinyl monomers may be polymerized by adding them to the propylene polymer in a molten state using a liquid feeder, but it is sufficient to mix them with the propylene polymer beforehand. After impregnating, it is preferable to supply to the extruder.

The radical initiator may be added by dissolving it in the vinyl monomers in advance, or may be added to the mixture of the propylene polymer and the vinyl monomer by using the liquid feeder. Although it is good, it is preferable to add it by dissolving it in vinyl monomers and impregnating it with a propylene-based polymer in advance.

The stabilizer is a propylene polymer,
It is necessary to use a Henschel mixer or the like in advance for mixing and placing. As described above, the propylene-based polymer, unlike the ethylene-based polymer, is a radical-disintegrating polymer, and therefore, when it is melt-heated in the presence of a radical initiator, the main chain is cleaved, so that the molecular weight is likely to decrease. However, the functional group-containing vinyl monomer, in the presence of an aromatic vinyl monomer, with a radical initiator, or, preferably, in the coexistence of a radical initiator and a stabilizer, a propylene polymer in a molten state If the graft reaction is performed on the vinyl monomer, the vinyl monomer can be efficiently subjected to the graft reaction without causing a decrease in the molecular weight.

During the graft reaction, 100% of the polymers and monomers are not graft-reacted to form a modified propylene polymer, and a propylene-based polymer and polystyrene are by-produced. Therefore, the modified propylene-based polymer referred to in the present invention includes such non-graft polymer.

The modified propylene-based polymer according to the present invention is a thermoplastic resin which is excellent in heat fusion property, printability, paintability, transparency, heat resistance, impact resistance, moisture resistance and the like. Furthermore, since the modified polymer is composed of a polar part and a non-polar part, it can be used as a compatibility improver for various polymers, and further, as a compatibility with an inorganic filler (inorganic filler). It is also an excellent solubility improver.

The polypropylene-polyamide resin laminate of the present invention is produced by an extrusion molding method using the modified propylene-based polymer obtained as described above or a mixture thereof.
It is formed into a film or sheet by a usual processing method such as an injection molding method or a calendar processing method, laminated with a polyamide film or the like, and used as a laminated film or the like.

This polypropylene-polyamide resin laminate is produced by a commonly used method such as a method of heat-sealing a sheet of a modified propylene polymer or a method of extrusion coating.

The polypropylene-polyamide resin laminate of the present invention has a two-layer structure with a modified propylene-based polymer, a structure in which a modified propylene-based resin is sandwiched between polyamide and a modified propylene-based structure. There are various forms such as a structure in which polyamide is sandwiched between resins, or a structure in which other resins such as polyethylene are laminated, and the like.

As the polyamides used here, only typical ones are shown as polymer compounds having acid amide as a repeating unit, which are obtained by ring-opening polymerization of lactam depending on the polymerization mode, and diamine and dibasic acid. The thing by polycondensation etc. are mentioned. These have a general name of nylon, and examples thereof include nylon 6, nylon 12, nylon 9, nylon 11, nylon 66, nylon 610, and the like, with nylon 6 and nylon 66 being preferred.

As described above, the polypropylene-polyamide resin laminate of the present invention has a high heat-sealing property, and is widely used particularly for applications having a high heat-sealing property such as generation of heated steam. You can

[0044]

EXAMPLES Next, the present invention will be described with reference to Examples and Comparative Examples.
This will be described more specifically. However, the present invention is not limited to these examples. In the following,
Parts and% are based on weight unless otherwise specified.

Example 1 A 20 mm single-screw extruder manufactured by Brabender of Germany was used, with a barrel temperature of 200 ° C. (however, a feeder section of 180 ° C.) and a die temperature of 2.
The temperature was set to 10 ° C.

950 parts of "Hipol B200P" (powdered polypropylene manufactured by Mitsui Petrochemical Co., Ltd.), 0.48 parts of "Irganox 1010" (product of Ciba-Gaiki), "Phosphite 168" (product of Ciba-Gaiki) And 0.45 parts of calcium stearate (stabilizer).

Then, 30 parts of styrene and 20 parts of glycidyl methacrylate were added to "Perhexin 25
B ”[initiator manufactured by NOF CORPORATION] was mixed with 1.5 parts of the above powder polypropylene compound sufficiently,
Impregnated.

Thereafter, the impregnated blend thus obtained was fed to an extruder and melt-kneaded at 30 rpm to carry out a graft reaction. The ratio of the styrene content of the extruded product (content), using an infrared spectroscopic analysis of the reaction products serving此of extruded product, 700 cm ^-1 and (attributable to styrene) 1380 cm ^-1 and (attributable to polypropylene) It was 2.8% when calculated from the calibration curve based on. In addition, in order to judge the presence or absence of grafting of this product, a sample from the product was extracted by Soxhlet extraction for 4 hours in tetrahydrofuran in which polypropylene is not dissolved but only non-grafted product is dissolved. At least, the graft ratio was calculated by measuring the residual ratio.
%Met.

The extrudate thus obtained was treated using a hydraulic press.
300μ under conditions of 190 ° C and 150 atmospheres
A m-thick sheet, and a nylon 6 sheet which had been formed into a sheet shape in advance were heat-laminated for 4 minutes at 240 ° C. and 150 atm to obtain a test piece.

The peel strength of the resin laminate thus obtained was evaluated by the test method described below. The results are collectively shown in Table 1, Table 2 and Table 3. (Example 2) As an aromatic vinyl monomer, 3 of styrene was used.
Instead of using 0 part, 50 parts of this styrene were used, with which 930 parts of powdered polypropylene, 0.47 parts of "Irganox 1010", "phosphite 1"
68 ", 0.47 parts of calcium stearate (stabilizer), 0.93 parts of" Perhexin 25B "2.1 parts were changed to the same manner as in Example 1 except that an extruded product was obtained. .

Thereafter, the styrene content of the extruded product was determined in the same manner as in Example 1 and it was 4.8%. At the same time, the thermal fusion bondability of the resin laminate thus obtained was evaluated.

(Example 3) 50 parts of styrene and 40 parts of glycidyl methacrylate were added, and 910 parts of powder polypropylene and "Irganox 101" were added accordingly.
0 "0.46 part," phosphite 168 "0.46 part
Parts and calcium stearate (stabilizer) 0.91
Parts, "Perhexin 25B" 2.7 parts was changed to obtain an extruded product in the same manner as in Example 1. Thereafter, when the styrene content of the extruded product was determined in the same manner as in Example 1, it was 4.7%. At the same time, the thermal fusion bondability of the resin laminate thus obtained was evaluated.

Example 4 An extruded product was obtained in the same manner as in Example 2 except that 20 parts of methacrylic acid was used instead of 20 parts of glycidyl methacrylate.

After that, when the styrene content of the extruded product was determined, it was 4.8%. At the same time, the thermal fusion bondability of the resin laminate thus obtained was evaluated. (Comparative Example 1) Using a polypropylene blended with an antioxidant in a proportion as in Example 1, melt-blended under the same extrusion conditions as in Example 1 to obtain an extruded product, and thereafter similarly formed into a sheet. , The heat fusion property was evaluated,
There was no heat fusion property with nylon, and a resin laminate could not be obtained.

(Comparative Example 2) 930 parts of polypropylene blended with an antioxidant and 70 parts of "Admer QF540" (carboxylic acid-modified polypropylene manufactured by Mitsui Petrochemical Co., Ltd.) in the proportions of Example 1 Was melt-blended under the extrusion conditions in the same manner as in Example 1 to obtain an extruded product.

Thereafter, in the same manner as in Example 1, a resin laminate was prepared and the heat fusion property was evaluated. (Comparative Example 3) 50 parts of "Dick Styrene CR3500" [polystyrene manufactured by Dainippon Ink and Chemicals, Inc.] with respect to 930 parts of the polypropylene compound containing the antioxidant in the ratio of Example 1 was used. Department, "Admar Q
20 parts of "F540" (carboxylic acid-modified polypropylene manufactured by Mitsui Petrochemical Co., Ltd.) was melt-blended under the extrusion conditions in the same manner as in Example 1 to obtain an extruded product. The residual rate of the styrene portion was 7% as determined in the same manner as in Example 1.

Thereafter, a resin laminate was prepared in the same manner as in Example 1, but the resin portion was clouded, was layered, and was inhomogeneous, and was heat-fusible to the nylon sheet. No resin laminate was obtained.

(Comparative Example 4) The same procedure as in Example 1 was repeated except that 950 parts of polypropylene containing an antioxidant and 50 parts of maleic anhydride were used in the same proportions as in Example 1. Thus, an extruded product was obtained. Then, the melt index of the extruded product thus obtained was very high as compared with polypropylene. Also,
Stickiness was recognized on the surface of the obtained sheet. After that, a resin laminate was prepared in the same manner as in Example 1 and the heat fusion property was evaluated.

Comparative Example 5 Example 1 was repeated except that 950 parts of polypropylene mixed with an antioxidant and 50 parts of styrene were used in the same proportions as in Example 1.
An extruded product was obtained in the same manner as in. After that, a resin laminate was prepared in the same manner as in Example 1 and the heat fusion property was evaluated.

(Comparative Example 6) The same procedure as in Example 1 was repeated except that 950 parts of polypropylene blended with an antioxidant and 50 parts of glycidyl methacrylate were used in the same proportions as in Example 1. An extruded product was obtained. The extrudate thus obtained had a much higher melt index than polypropylene. Also,
Stickiness was observed on the surface of the obtained sheet. After that, a resin laminate was prepared in the same manner as in Example 1 and the heat fusion property was evaluated.

[0061]

[Table 1]

<< Footnotes in Table 1 >> PP ......... abbreviation of polypropylene powder SM ......... abbreviation of styrene monomer GMA ... abbreviation of glycidyl methacrylate MAA ......... abbreviation of methacrylic acid The numerical values in parentheses in the table are , Both mean “%”. The unit of “peel strength” is “g / cm”. The unit of "melt index" is "g / 10 minutes".
The unit of "total light transmittance" is "%". The unit of "cloudiness value" is "%".

[0063]

[Table 2]

<< Footnote of Table 2 >> P-acid: Abbreviation of carboxylic acid modified polypropylene PS: Abbreviation of polystyrene MAh: Abbreviation of maleic anhydride

[0065]

[Table 3]

Here, the thermal fusion bond evaluation, the appearance and the melt index performed on the products obtained in the examples and the comparative examples are in accordance with the following methods. (1) Evaluation method of "heat fusion property" The test piece of the obtained polypropylene-polyamide resin laminate was peeled at a peeling speed of 50 m using a Tensilon tensile tester.
A 90-degree peel test was performed under the condition of m / min. (2) Method for measuring "melt index" Using the extruded pellets obtained, ASTM D-1 under the conditions of a temperature of 230 ° C and a load of 2.16 Kg.
According to 238, measurement was performed and evaluated. (3) Evaluation Method of "Transparency" The light transmittance and haze value of the obtained modified polypropylene sheet having a thickness of 300 μm (μm) were measured by a haze meter (product of Toyo Seiki Co., Ltd.).

The appearance of the sheet was visually evaluated.

[0068]

The modified propylene-based polymer according to the present invention has a high heat-melting property because the molten propylene-based polymer is melt-kneaded and polymerized with an aromatic vinyl monomer and a functional group-containing vinyl monomer. Has wearability. Therefore, the polypropylene-polyamide resin laminate of the present invention can be used especially in applications where strong adhesive force is required, such as food packaging applications where water vapor is generated, and also in gas barrier properties and the like. It is excellent.

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[Procedure amendment]

[Submission date] October 6, 1992

[Procedure Amendment 1]

[Document name to be amended] Statement

[Name of item to be corrected] Claim 3

[Correction method] Change

[Correction content]

[Procedure Amendment 2]

[Document name to be amended] Statement

[Name of item to be corrected] Claim 4

[Correction method] Change

[Correction content]

Claims (4)

[Claims] 1. A layer of a modified propylene-based polymer obtained by melt-kneading and polymerizing a molten propylene-based polymer with an aromatic vinyl monomer and a functional group-containing vinyl monomer, and a polyamide layer. Resin laminate. 2. The resin laminate according to claim 1, wherein the functional group-containing vinyl monomer is an epoxy group-containing vinyl monomer or a carboxyl group-containing vinyl monomer. 3. The resin composition according to claim 1, wherein the aromatic vinyl monomer is used in an amount of 35% by weight or less based on the propylene polymer. 4. The resin laminate according to claim 1, wherein the functional group-containing vinyl monomer is used in an amount of 20% by weight or less based on the propylene polymer.