JPS6369860A - Production of composite resin material - Google Patents

Abstract

PURPOSE:To obtain a composite resin containing molecular chains of polyamide and polyolefin entangled with each other and having excellent molding fluidity and physical properties, by carrying out the melting and kneading of a polyolefin with a polyamide simultaneous to the modification of the polyolefin in the presence of a specific modifying agent and an organic peroxide. CONSTITUTION:100pts.wt. of a mixture of (A) 50-95wt.%, preferably 60-90wt.% polyamide resin (e.g. nylon 6) having a relative viscosity of 1.5-5 and (B) 5-50wt.%, preferably 10-40wt.% polyolefin having a melt index of 0.05-50g/10min is compounded with (C) 0.02-5pts.wt., preferably 0.07-1pt.wt. of an alpha,beta-unsaturated imide compound (e.g. N-cyclohexylmaleimide), (D) 0.01-3 pts.wt., preferably 0.05-0.8pt.wt. of an alpha,beta-unsaturated carboxylic acid (anhy dride) compound (e.g. acrylic acid) and (E) 0.001-0.8pt.wt., preferably 0.008-0.2pt.wt. of an organic peroxide, and the mixture is kneaded under melt ing.

Description

[Detailed Description of the Invention] <Industrial Application Field> The present invention relates to a method for producing a resin composite in which a polyamide resin and a specific modified polyolefin are entangled with each other, and the modified polyolefin is partially crosslinked. .

<Prior Art> In recent years, there has been active research into improving the impact strength of polyamide resins and expanding their applications. The method usually adopted for this purpose is to first prepare a modified polyolefin rubber by introducing a functional group into EPR or EPDM rubber, and then melt blend the modified polyolefin rubber with polyamide resin. Yes, impact-resistant nylon resins that actually have practical value are being manufactured and sold. Conventional studies have mainly focused on how to modify polyolefins to improve their compatibility and dispersibility with polyamides, and the selection of modifiers having functional groups has been an important point. So far, known modified polyolefins include copolymerization or grafting of compounds having carboxylic acid groups or acid anhydride groups, as described in Japanese Patent Publication No. 42-12546 and Japanese Patent Publication No. 55-44108. Typical examples include modified polyolefins introduced using the method described above. These prior examples disclose a method of blending and kneading a modified polyolefin prepared in advance with polyamide as described above, but in the case of such a method, fine dispersion into the polyamide matrix proceeds successfully. Therefore, one of the necessary conditions is that the modified polyolefin rubber is basically not crosslinked (for example, the modified polyolefin characteristics of Japanese Patent Publication No. 44108/1983).

In addition, when polyamide and polyolefin are mixed together, unsaturated carboxylic acid or its anhydride and peroxide are present,
A method for obtaining a polyamide composition simultaneously with the modification of a polyolefin (Japanese Unexamined Patent Publication No. 60-49018) or a method for melt-kneading polyamide and an ethylene/unsaturated carboxylic acid copolymer in the presence of peroxide (Japanese Unexamined Patent Application Publication No. 55-1988) No. 125153) are known, and are described as being effective as techniques for increasing the viscosity of low water absorption nylon resins and textile waste products.

<Problems to be solved by the invention> However, JP-A-60-49018 and JP-A-55
It has been found that the method disclosed in Japanese Patent No. 125153 increases the melt viscosity, often causing crosslinking and deteriorating the fluidity during molding. This is Japanese Patent Publication No. 55-1251
One of the reasons is that polyolefins are easily crosslinked by peroxides, as stated in the 1953 publication, but furthermore, when polyolefins are modified with unsaturated carboxylic acids or their anhydrides, It has been found that polyamides tend to react with polyolefins, and as a result, the fluidity of the entire composition is extremely reduced. Furthermore, in the above method, if crosslinking of the polyolefin progresses faster than the polyolefin is finely dispersed in the polyamide, dispersion may become insufficient, resulting in a decrease in the impact strength and appearance of the molded product, which is also an issue that needs to be resolved. It is one.

In other words, the method of kneading polyamide and polyolefin (in which a modifier and peroxide are present to obtain a composition at the same time as modifying the polyolefin) is effective as a comparatively low-cost manufacturing process; A composition with excellent physical properties such as stability, molding fluidity, and impact strength has not yet been obtained, and there is currently a need for technological development of a method to obtain a resin composition that has all of these properties. be.

<Means for Solving the Problems> The present inventors have discovered that when kneading polyamide and polyolefin, e.g.
We investigated the possibility of stably producing a composition with excellent molding fluidity and physical properties using a method for simultaneously modifying polyolefin and obtaining a thick composition in the presence of a modifier and a peroxide. By using extremely limited amounts of both a saturated imide compound and an unsaturated carboxylic acid or its anhydride, a previously unknown resin composite in which molecular chains of polyamide and modified polyolefin are entangled with each other can be obtained. The present invention was achieved by discovering that

That is, the present invention uses polyamide resin 50 to 95 ifj
C) 0.02 to 5 parts by weight of α,β-unsaturated imide compound, tjJα, β-unsaturated carboxylic acid compound, based on 100 M bearing part of a mixture of t% and [F]) polyolefin 5 to 50% by weight The present invention provides a method for producing a resin composite, which comprises melting and kneading a mixture of 0.01 to 3 parts by weight of the anhydride thereof and 0.001 to 0.8 parts by weight of the organic peroxide.

The features of the present invention are summarized as follows.

(1) The presence of a specific amount of a specific unsaturated imide compound, unsaturated carboxylic acid compound or its anhydride, and organic peroxide during melt-kneading of polyamide and polyolefin improves mechanical properties such as molding fluidity and impact strength. Resin composites with excellent physical properties can be stably produced.

(2) The key point of the present technology is that both an imide compound and a carboxylic acid derivative are used as modifiers for polyolefins in limited quantities, and the purpose cannot be achieved using only one modifier.

(3) There is no conventional method known of using at least two types of modifiers and simultaneously blending them into polyamide at the same time as modifying the polyolefin.

(A) In this method, polyolefin is partially crosslinked, but crosslinking progresses simultaneously with modification during the crosslinking process with polyamide. A phase-separated structure can be obtained.

Partially crosslinked modified polyolefins fall into a category that has been excluded as ineffective in the prior art, and from this point of view they are unique, and the novelty and effectiveness of the present method lies in this point.

(5) Partial crosslinking of the above polyolefin proceeds in the polyamide matrix, so the polyamide molecular chains and polyolefin molecular chains are entangled, but in this method, the polyolefin is modified mainly with an imide compound, so reaction with the polyamide is suppressed. This has the advantage that overall liquidity does not deteriorate.

(6) In other words, the resin composite as used in the present invention is not just a mixture, but a structure in which the molecular chains of polyamide and polyolefin are entwined with each other with almost no reaction, so-called interpenetrating polymers). Structure (Inter-penetrating Poly
er Networks).

This is thought to improve mechanical properties such as impact strength while maintaining good fluidity. This resin composite provides a novel concept in the field of polyamides and modified polyolefins.

The polyamide used in the present invention is not particularly limited, and refers to any melt-moldable polymer composed of an amino acid, a lactam, or a diamine, and a dicarboxylic acid. Examples of constituent components include amino acids such as 6-aminocaproic acid, lI-aminoundecanoic acid, I2-aminododecanoic acid, and nokura-aminomethylbenzoic acid, lactams such as ε-caprolactam and ω-laurolactam, tetramethylenediamine, Hexamethylene diamine, undecamethylene diamine, dodecamethylene diamine, 2.2.4-72
．． 4.4-) Limethylhexamethylenediamine, 5-
Methylnonamethylenediamine, metaxylylenediamine, paraquinlylenediamine, ■,3-bis(aminomethyl)cyclohexane, I,4-bis(aminomethyl)cyclohexane, ■-amino-3-aminomethyl-3,5
, 5-)limethylcyclohexane, bis(A-aminocyclohexyl)methane, bis(3-methyl-4-aminocyclohexyl)methane, 2,2-bis(A-aminocyclohexyl)propane, bis(aminopropyl)piperazine , diamines such as aminoethylpiperazine and adipic acid, speric acid, azelaic acid, sepadic acid, dodecadionic acid, terephthalic acid, isophthalic acid, 2-chloroterephthalic acid, 2-methylterephthalic acid, 5-methylisophthalic acid, 5-sodium It can be selected from dicarboxylic acids such as sulfoisophthalic acid, hexahydroterephthalic acid, hexahydroisophthalic acid, diglycolic acid and the like. Polyamides particularly useful in the present invention include polycaproamide (nylon 6), polyhexamethylene adipamide (
Nylon 66), polyhexamethylene diamine (nylon 610), polyhexamethylene dodecamide (nylon 6I2), polyundecaneamide (nylon 11), polydodecanamide (nylon +2), copolymerized polyamides thereof, mixed polyamides, etc. It is. The degree of polymerization of the polyamide used here is limited to 7L, and any polyamide with a relative viscosity within the range of 1.5 to 5.0 can be arbitrarily selected. There are no particular restrictions on the method for producing polyamide, and it can be prepared by conventionally known methods such as melting and solid phase polymerization.

The polyolefin (B) used in the present invention is basically a non-polar polymer without functional groups, and includes α-olefins and dienes having 2 to 20 carbon atoms, evaporated ethylene, propylene, butene-1, pentene-1,4 -Methylpentene-
11-isobutylene, 1,4-hexadiene, dinoclopentadiene, 2,5-norbornadiene, 5-ethyl-
It is a polymer whose main components include 2,5-norbornadiene, 5-ethyrythenenorbornene, 5-(1'-flobenyl)-2-norbornene, butanene, isoprene, and chloroprene. As copolymerization components, functional group-containing components other than unsaturated imide compounds, unsaturated carboxylic acids, and unsaturated acid anhydrides can be used, examples of which include acrylic esters, methacrylic esters, acrylamide, and metal acrylates. Common examples include salts, methacrylic acid metal salts, and the like.

Specific examples of polyolefins particularly useful in the present invention include polyethylene, polypropylene, polybutene, poly(A
-Methylpentene-1), poly(ethylene/propylene), poly(ethylene/butene-1), poly(ethylene/
Examples include poly(ethylene/propylene/dicyclopentadiene), poly(ethylene/propylene/2.5-norbornadiene), poly(ethylene/propylene 15-ethylidenenorbornene), etc. . ■ Dust content of polyolefin: There are no particular restrictions, and the melt index is usually 0.
05 to 50 f/10 minutes can be arbitrarily selected. Furthermore, even if the polyolefin manufacturing method is difficult, there are no limitations, and known methods such as high-pressure radical polymerization, low-pressure catalyst method, and solution polymerization method can be employed.

In the present invention, (A) polyamide resin 50 to 95% by weight, preferably 55 to 93% by weight, more preferably 60 to 9% by weight.
0ntft% and fB) polyolefin 5-50% by weight, preferably 7-45% by weight, more preferably 10
It is used in a proportion of ~40% by weight. If the blending ratio is outside this limited range, it is not preferable because the desired balance of physical properties such as impact strength and rigidity cannot be achieved.

Examples of the ((D) a,β-unsaturated imide compounds used in the present invention are maleimide, N-methylmaleimide,
N-ethylmaleimide, N-propylmaleimide, N-
Butylmaleimide, N-octylmaleimide, N-phenylmaleimide, N-(O-methylphenyl)maleimide, N-(m-methylphenyl)maleimide, N-(p
-methylphenyl)maleimide, N-(methoxyphenyl)maleimide, N-(chlorphenyl)maleimide,
These include N-(carboxyphenyl)maleimide, N-benzylmaleimide, N-naphthylmaleimide, N-cyclohexylmaleimide, itaconimide, N-methylitaconimide, N-phenylitaconimide, and the like.

The unsaturated imide compounds preferably used in the present invention have a melting point of 180°C or lower and a boiling point of 200°C or higher at normal pressure, particularly N-cyclohexylmaleimide, N-benzylmaleimide, N-phenylmaleimide, N- (Carboxyphenyl)maleimide and the like are suitable compounds.

Examples of the (D) a,β-unsaturated carboxylic acid compound or its anhydride used in the present invention include acrylic acid, methacrylic acid, maleic acid, fumaric acid, itaconic acid, crotonic acid, methylmaleic acid, Methyl fumaric acid, mesaconic acid, citraconic acid, glutaconic acid, methyl hydrogen maleate, ethyl hydrogen maleate, butyl hydrogen maleate, methyl hydrogen itaconate, ethyl itaconate hydrate, maleic anhydride, itaconic anhydride, citraconic anhydride, etc. It is. Even if an unsaturated carboxylic acid derivative has 12, the melting point is 180℃ or less and the boiling point is 20℃ at normal pressure.
Those above 0°C can be preferably used, especially acrylic acid,
Suitable compounds include methacrylic acid, maleic acid, fumaric acid, methyl hydrogen maleate, maleic anhydride, itaconic anhydride, and the like.

Examples of (t)organic peroxides used in the present invention include cumene hydroperoxide, t-butylcumyl peroxide, di-t-butyl peroxide, 2,5-dimethyl-2,5-di(t -butylperoxy)hexane, 2
,5-dimethyl-2,5-di(t-butylperoxy)
Hexane-(3), 2,5-dimethylhexane-2,5
-cybidroba-oxide, t-butyl hydroperoxide, di-isopropylbenzene hydroperoxide, p-methane hydroperoxide, 1, l-bis-t-butylperoxy-3,3,5-trimethylcyclohexane, n -butyl-4°4-bis-t-butylperoxyvalerate, t-butylperoxybenzoate, and the like.

In the present invention, it is necessary to rapidly decompose at the melting temperature, and an organic peroxide having a half-life of 1 minute within the range of 150 to 250°C is preferably used. If the decomposition temperature is outside the above range, it is not preferable because the danger during handling is too high or the polyolefin is not effectively modified.

In the present invention, (C) a is added to a total of 100 parts by weight of the resins (A) polyamide resin and (2) polyolefin.

0.02 to 5 parts by weight, preferably 0.05 to 3 parts by weight, more preferably 0.07 to 3 parts by weight of the β-unsaturated imide compound.
1 part by weight, ■ 0.01 to 3 parts by weight, preferably 0.02 to 3 parts by weight of α, β-unsaturated carboxylic acid compound or its anhydride.
1 part by weight, preferably 0.05 to 0.8 parts by weight, and (g) 0.001 to 0.0% of the organic peroxide, preferably 0.004 to 0.5 parts by weight, and Preferably, a method of adding 0.008 to 0.2 parts by weight and melt-kneading the mixture is adopted. α.

If the amount of the β-unsaturated imide compound and the modifier for the α,β-unsaturated carboxylic acid reading conductor added is less than the above lower limit, the compatibility between the polyamide and polyolefin will be poor and physical properties such as impact strength will decrease. So I don't like it. On the other hand, if the amount of modifier added exceeds the above upper limit, not all of the modifier will be consumed for modifying the polyolefin, and the residual material will bleed out onto the surface of the molded product, impairing the appearance or reducing the stability of the polyolefin. An undesirable phenomenon occurs.

In particular, the present invention is characterized in that (C) an α,β-unsaturated imide compound and (2) an α,β-unsaturated carboxylic acid compound or anhydride thereof are used in combination. The unsaturated imide compound is effective in improving the compatibility of polyolefin with polyamide, and also has the effect of suppressing crosslinking of the entire composite so as not to deteriorate molding fluidity. Unsaturated carboxylic acid derivatives are involved in the reaction between polyolefin and polyamide, and if the polyolefin is not sufficiently fixed in the polyamide matrix, the spinnability of the melt-kneading string will be poor and production operability will deteriorate. If the amount of the acid derivative added is too large, crosslinking of the polyolefin will occur while the polyolefin and polyamide react, resulting in extremely poor overall fluidity. Therefore α
, β-unsaturated imide compounds, α-unsaturated carboxylic acid compounds, or their anhydrides each have different expected roles, and valuable products can only be produced when both exist.

As mentioned above, the resin composite referred to in the present invention is a structure with a different concept from simply a mixture of polyamide and polyolefin or a composition in which modified polyolefin and polyamide are partially reacted, and the molecular chains of polyamide and polyolefin are It is called a recursive body because it means a structure that is intertwined with each other. However, although the details of its structure are not necessarily clear, the method of the present invention involves modifying the polyolefin with a peroxide using at least two specific modifiers (and simultaneously blending it with the polyamide). It is created for the first time by this method.

The existence of a complex structure can be proven by its solubility in solvents. For example, if you perform an operation to dissolve and remove the polyamide part of the extruder kneaded product obtained by the method of the present invention with a solvent such as metafresol, and examine the infrared absorption spectrum of the remaining material, the remaining material may be a mixture of polyolefin and polyamide. It was found that there was a polyamide that showed both characteristic spectra and could not be dissolved and removed by this operation. In other words,
This residue is thought to have a structure in which polyamide molecular chains and polyolefin molecular chains are entangled.

In addition, in the method of the present invention, the polyolefin is partially crosslinked during the kneading process. The degree of crosslinking can also be expressed in terms of solubility in a solvent. Poly(ethylene/propylene) copolymers, which are completely soluble in solvents such as toluene (before melt mixing with polyamide), can also be used in the method of the present invention (thanks to this, when dispersed in a polyamide matrix).
The following experiment showed that this was a crosslinked product with a portion insoluble in the solvent. In other words, the poly(ethylene/propylene/) copolymer remaining after hydrolyzing and removing polyamide with hydrochloric acid is not completely dissolved in toluene, and a crosslinked insoluble portion exists. It has become possible to finely disperse a partially cross-linked modified polyolefin into a polyamide matrix, which was previously unimaginable.By cross-linking the rubber component, further improvements in impact strength and rigidity have been achieved, making it of extremely practical value. A material with high quality can be obtained.

The resin composite of the present invention is made of polyamide and polyolefin pellets, powders, strips, etc.

A β-unsaturated imide compound, an α,β-unsaturated carboxylic acid compound or its anhydride, and an organic peroxide are premixed and melted by supplying the mixture in a uniaxial or multi-screw extrusion manner with sufficient crosstalk force. The most common method is kneading. The resin composite of the present invention may contain other components such as pigments, dyes, reinforcing materials, fillers, etc., as long as they do not impair its physical properties and moldability.
Heat resistant agents, antioxidants, weathering agents, lubricants, crystal nucleating agents, anti-blocking agents, mold release agents, plasticizers, antistatic agents,
Other polymers and the like can be added and introduced.

The resin composite of the present invention can be produced by injection molding, extrusion molding, intrusion molding,
Molded products with well-balanced mechanical properties can be obtained by subjecting them to compression molding and other molding methods used for normal thermoplastic resins, and these molded products can be used for various automotive parts, mechanical parts, electrical/ It is useful as electronic parts, general miscellaneous goods, etc.

<Example> The present invention will be explained in more detail with reference to Examples below.

The characteristics of the polymers and molded articles described in Examples and Comparative Examples were evaluated by the following method.

(1) Relative viscosity of polyamide: JIS K6
810(2) Melt index: JIS
K7210 (3) Tensile resistance:
ASTiVI D638(A) bending
Properties: ASTM D790 (5) Isotho impact strength: ASTM D256 (6) Injection molding fluidity: Evaluated by spiral flow length.

Example 1 Melt polymerization of ε-caprolactam to obtain a relative viscosity of 3, I
Nylon 6 of O was prepared. Poly(ethylene/propylene) having a melt index of 7 f/10 min by polymerizing a mixture of 75 mol% ethylene and 25 mol% propylene
A copolymer was prepared. N-cyclohexylmaleimi) for a total of 100 parts by weight of 675% by weight of nylon and 25% by weight of poly(ethylene/propylene) copolymer)
0.4 parts by weight, 0.3 parts by weight of maleic anhydride and 2 parts by weight.
,5-dimethyl-2,5-di(t-butylperoxy)
After adding 0.1 part by weight of hexyne-(3) and premixing the whole, 25 mm
The mixture was melt-kneaded at 0°C and pelletized. The stringability of the string discharged from the extruder was extremely stable, and almost no string breakage occurred even after continuous long-term operation.

The pellets obtained here were treated by the following two methods and subjected to infrared absorption spectroscopy and dissolution tests.

(1) The pellets were treated with hydrochloric acid to hydrolyze the nylon portion, and the infrared absorption spectrum of the residue is shown in FIG. This residue is 1460n-1°1380 as
Absorption was observed at 710 tx-' and 710 tx-'.
It can be seen that it is a (ethylene/propylene) copolymer. In addition, this residual modified poly(ethylene/propylene) copolymer badruene (because it did not completely dissolve, it was found that it was partially crosslinked during the land process. .

Robylene) copolymer is completely soluble in toluene,
It was also separately confirmed that no partial crosslinking was caused by the hydrochloric acid treatment.

(2) An attempt was made to treat the pellet with metacresol to dissolve and remove the nylon portion. This operation was repeated many times, and the infrared absorption spectrum of the residue is shown in Figure 2. This residue is the characteristic absorption of nylon 633
00 ff1-111640ax-', 1550
m-1 and polyolefin properties absorption tear 1460
ax-', 1380 tyx-', 710a-
Absorption of 1 is observed. In other words, there was a nylon 6 portion that could not be completely removed by this meta-cresol dissolution, and it was assumed that this was a composite structure in which nylon 6 molecular chains and polyolefin molecular chains were entangled with each other.

Next, after vacuum drying the pellets obtained here, a test piece was molded using an injection molding machine, and the fluidity during molding and the physical properties of the obtained test piece were measured, as shown in Table 1. ,
It turned out to be a material with high practical value.

Comparative Example 1 Poly(ethylene/propylene) used in Example 1
For flG body + oo nail i part, 1.6 parts of N-cyclohexylmaleimide, 1.2 parts by weight of maleic anhydride, and 2,5-dimethyl-2,5-di(butylperoxy)hexyne-(3 ) 0.4 m i part attached
After mixing, using an extruder with a diameter of 40JIJIφ, 25
The mixture was kneaded at 0°C. The modified poly(ethylene/
It was found that the conjugate (propylene) was not completely dissolved in toluene and was crosslinked.

After adding and mixing 25% by weight of this cross-linked modified poly(ethylene/propylene) copolymer to the nylon 6 used in Example 1, compounding was performed under the same conditions as in Example 1, and then injection molded test pieces were prepared. Physical properties were evaluated. The results are shown in Table 1, and it was found that in the method of mixing and kneading crosslinked polyolefin with nylon, the dispersibility of the polyolefin was poor, the impact strength was unsatisfactory, and the surface appearance of the molded product was not good. It has been found that crosslinking must proceed simultaneously with modification during compounding with nylon as shown in Example I.

Comparative Examples 2 to 5 Extrusion-like kneading and injection molding test pieces were evaluated for physical properties in the same manner as in Example 1 except that the amounts of N-cyclohexylmaleimide and maleic anhydride used were changed as shown in Table 1. carried out. It has been found that when the amount of the modifier added is out of the range specified in the present invention, the stability of extrusion from the extruder is poor, and the flowability and mechanical flexibility of injection molding are reduced, which is not preferable.

(A) N-6=nylon 6, ■) EPR: Poly(ethylene/propylene) copolymer, (C) NCHM: N-chlorohexylmaleimide, (f) IVILA: Maleic anhydride, (g) DBPH: 2 ,5-dimethyl-2
,5-di(t-butylperoquine)hexyne-(3) Injection molding Fluidity: Temperature 250°C, injection pressure + (100 kI
j/c4, test piece thickness 1. ON Physical properties: 23°C, bone dry Examples 2 to 15 The same operations as in Example 1 were performed with different types of polyamide, polyolefin, modifier, and peroxide, and the blending ratio to determine the stability of extrusion from the extruder. The injection molding fluidity and physical properties of the molded test pieces were evaluated and the results shown in Table 2 were obtained. It was found that in all the cases listed in Table 2, composite bodies exhibiting excellent extrusion workability 1±, injection molding fluidity, and physical properties were obtained.

261a) Polyamide N-6 = Polycaproamide, N-6f): Polyhexamethylene adipamide, N-610: Polyhexamethylene dodecamide, N-612: Polyhexamethylene dodecamide, N-12 : Polydodecanamide, N-6/66 (8
5/+5): Poly(caproamide/hexamethyleneadipamide) copolymer (wt%), N-6/66 (10
/90): Same as above, N-6/12 (80/20): Poly(caproamide/dodecaneamide) copolymer (wt%
), N-5I: polyhexamethylene isophthalamide,
N-MXD6: Polymethaxylylene adipamide, N-
PACIVI 12: Polybis(A-aminocyclohexyl)methandodecamide, N-TMDT: Polytrimethylhexamethylene terephthalamide, N-12
T: Polydodecamethylene terentalamide, N-6I/
PACM T (50150): Poly (hexamethylene isophthalamide/bis(A-aminocyclohexyl)methane terephthalamide) copolymer (wt%).

b) Polyolefin E/PP: Poly(ethylene/propylene) copolymer (
80/20 mol%), PP: polypropylene, PIVi
P: poly(A-methylpentene-1), PE: polyethylene, E/BT: poly(ethylene/butene-■) copolymer (85'/15 mol%), E/PI)/DCPD
: Poly (ethylene/propylene/dicyclopentadiene) copolymer (70/20/10 mol%), E/PP
/ND: Poly(ethylene/propylene/norbornadiene) copolymer (65/25/l 0 mol%), E
/PP/EN: Poly (ethylene/propylene 15-
Ethelidennorporene) copolymer (70/25/
5 Mo#%).

<Effects of the Invention> According to the present invention, injection molding fluidity and mechanical properties are improved by simultaneously modifying polyolefin and melt-kneading it with polyamide in the presence of at least two specific modifiers and an organic peroxide. It has become possible to produce superior materials. Moreover, in the material obtained by the method of the present invention, the crosslinked polyolefin is uniformly and finely dispersed in the polyamide matrix, and the modification and crosslinking of the polyolefin proceeds in the presence of the polyamide, so the molecular chains of the polyamide and the polyolefin are separated. Two points were previously unknown: the formation of a composite structure in which molecular chains are entangled with each other. In this regard, the present invention can provide a method for producing materials with a new concept.

[Brief explanation of the drawing]

FIG. 1 is an infrared absorption spectrum diagram of the hydrochloric acid treatment residue of the pellet obtained in Example 1, and FIG. 2 is an infrared absorption spectrum diagram of the metacresol treatment residue of the same pellet. Patent application Daitoshi Co., Ltd.

Claims (1)

[Claims] (C) 0.02 to 5 parts by weight of an α,β-unsaturated imide compound, (D) per 100 parts by weight of a mixture of (A) 50 to 95% by weight of polyamide resin and (B) 5 to 50% by weight of polyolefin; a, β-unsaturated carboxylic acid compound or its anhydride 0.01 to 3 parts by weight and (E) 0.01 to 3 parts by weight of an organic peroxide.
1. A method for producing a resin composite body, which comprises melting and kneading a mixture of 0.001 to 0.8 parts by weight.