Thermoplastic resin composition with low lustre and soft surface touch and article moulded therefrom

FIELD: chemistry.

SUBSTANCE: composition contains (A) about 10-80 wt % soft rubber-like resin based on a vinyl aromatic copolymer, (B) about 4-60 wt % rubber-modified resin based on a vinyl aromatic copolymer and (C) about 5-80 wt % resin based on a vinyl aromatic-vinyl cyanide copolymer. Resin (A) contains as a dispersion phase rubber particles with content of graft polymer of about 40-90%, and average particle diameter of about 6-20 mcm. The moulded article is made by moulding from said thermoplastic resin composition and has a soft surface touch with average surface roughness of about 400-800 nm.

EFFECT: invention enables to obtain moulded articles with a pleasant low lustre and high impact viscosity.

16 cl, 5 dwg, 2 tbl, 10 ex

 

The technical FIELD

The present invention relates to compositions of thermoplastic resin with a low gloss and soft-touch surface and to a molded product out of it. More specifically, the present invention relates to compositions of thermoplastic resin having low gloss and high impact strength, and also has a soft-touch surface, which includes soft kauchukopodobnoe resin-based vinylaromatic copolymer having a high swelling index, and which, as a dispersed phase comprises particles of rubber, in which the proportion of grafted polymer is in certain ranges and in which the average particle diameter is within a specific range, and a molded product from a specified composition.

PRIOR art

In General, ABS resin (Acrylonitrile-butadiene-styrene resin) has a good combination of properties such as impact resistance, chemical resistance, heat resistance and mechanical strength, and the ability to run, and easy to use; therefore, it is widely used for manufacturing various products such as car parts, housings of electrical/electronic equipment and similar devices, as well as for the manufacture of household and personal devices/predmeta the items.

In recent years, increased demand for thermoplastic resin having low gloss and soft-touch surface with different characteristics from the traditional solid and glossy plastics. In particular, increased demand for interior parts of automobiles and buildings electrical/electronic equipment, which people are forced to touch or to see for a long period of time. Moreover, the tightening of environmental regulations has caused an increased demand for a resin with a low gloss, produced without coating and is suitable for direct molding.

There are three method of manufacturing a resin with a low gloss, in particular ABS resin with low gloss. The most widely used method consists of applying an additive that eliminates gloss/matte substances, such as inorganic filler, acrylic resin or styrene resin containing cross-linkage. Another way is to remove the gloss during subsequent processing. Using this method, the effect of the lack of gloss is achieved by etching moulded products (extrusion relief on the product during the molding or by coating. Another method includes forming on the surface microrelief due to the control of the particle size of the rubber being in the dispersed phase in the OLE ABS. Such surface microrelief may have a low gloss due to scattering of the incident light.

Although the method of obtaining the effect of low gloss by adding a matting agent in many respects convenient, its disadvantage is that even gloss may not be obtained due to non-uniform distribution of the additive. Furthermore, the method of etching of the molded product during the molding or coating may increase production costs and may be unacceptable for environmental reasons. On the other hand, although the advantage of the method of obtaining a rough surface by controlling the particle size of the rubber is no additional process step, its disadvantage is that at the same time get low gloss and soft-touch surface impossible.

To reduce the gloss of the resin in the patent US 5475053 described use as a matting agent spherical particles of the graft-copolymer, and in the patent US 4652614 described use as matting modifier spherical particles of the graft-copolymer containing rubber in the amount of approximately from 5 to 80%. In addition, to reduce gloss in patent US 4668737 described using spherical particles of rubber, having a structure of the IPA core/sheath, approximately from 0.05 to 20 μm, and in the patent US 5237004 describes the use of polymeric particles with a size of approximately from 2 to 15 microns.

However, in the case of the use of supplements containing rubber particles, can occur stratification of the material, the deterioration of physical properties and partial emergence of high gloss; moreover, it leads to increased production costs. Furthermore, since the resin have a more dense structure compared with particles of rubber obtained by polymerization in bulk or solution polymerisation, to get soft to the touch the surface of the resin is difficult.

On the contrary, to obtain a low gloss and resistance to shock loads in a single product, in patent US 5605963 and the patent EP 0668319 described resin ABS, including large rubber particles. However, despite receiving low gloss, a modified surface, soft to the touch, could not be obtained.

Although in Japanese patent No. 3673084 and Japanese published patent application No. 2000-141322 described the use of wood flour for modification of the surface texture, it complicates the processing of resins with conventional molding temperatures.

Accordingly, the authors of the present invention was able to obtain a composition of a thermoplastic resin having a soft-touch surface, and is also low gloss and high impact strength the introduction of soft koukopoulos resin-based vinylaromatic copolymer, which as the dispersed phase comprises rubber particles with a fraction of the grafted polymer comprising from about 40 to 90%, with an average particle diameter of approximately from 6 to 20 μm, and a molded product from a specified resin.

The INVENTION

Technical task

The present invention is to obtain composition a thermoplastic resin with soft touch surface and molded articles thereof.

Another objective of the present invention is to obtain composition a thermoplastic resin having low gloss, and molded articles thereof.

Another objective of the present invention is to obtain composition a thermoplastic resin having high impact strength, and molded articles thereof.

Other objectives and advantages of the present invention discussed in the following description and the attached claims.

Technical solution

The present invention provides a composition of thermoplastic resin having a soft surface, low gloss and high impact strength, and molded articles thereof.

The composition of thermoplastic resin of the present invention comprises (A) from about 10 to 80 wt%. agqoy koukopoulos resin-based vinylaromatic copolymer, which includes as a dispersed phase of rubber particles with a fraction of the grafted polymer, component approximately from 40 to 90%, and the average diameter of the particles constituting approximately from 6 to 20 μm; (C) from about 4 to 60% of the mass. modified rubber resin based vinylaromatic copolymer; and (C) from about 5 to 80 wt%. resin-based vinylaromatic-vinylcyanide copolymer.

In some embodiments of the present invention soft koutsokoumnis vinylaromatic copolymer (A) may have a swelling index of approximately from 13 to 30.

Soft koutsokoumnis vinylaromatic copolymer (A) may include a matrix comprising vinylaromatic-vinylcyanide copolymer; and rubber particles, which are dispersed in the matrix and contain a fraction of the grafted polymer component approximately from 40 to 90%and have an average particle diameter of approximately from 6 to 20 microns.

The rubber particles may have a shape that encloses vinylaromatic monomers, vinylcyanide monomers, vinylaromatic-vinylcyanide copolymer or mixture of these substances.

In one example implementation, soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer may include from about 45 to 90% of the mass. vinyl is a romantic monomer, from about 5 to 35 wt%. vinylcyanide monomer and about 5 to 20% of the mass. rubber-based diene with conjugated double bonds, and can be obtained by continuous polymerization or continuous polymerization in solution.

In some embodiments, a modified rubber resin (B) based on vinylaromatic copolymer may be a graft copolymer (graft copolymer)containing from about 40 to 80% of the mass. rubber-based diene with conjugated double bonds, from about 8 to 45% of the mass. vinylaromatic monomer and from about 2 to 30 wt%. vinylcyanide monomer, and may contain rubber particles having an average particle diameter of approximately from 0.1 to 0.8 μm.

In some embodiments vinylaromatic-vinylcyanide copolymer (C) may include from about 40 to 90% of the mass. vinylaromatic monomer and from about 10 to 60 wt%. vinylcyanide monomer.

In some embodiments the present invention may relate to a molded product molded from the composition of thermoplastic resin. The average surface roughness (Ra) of the molded product can be from approximately 400 to 800 nm, and the height of the surface roughness at ten points (Rz) can PR is approximately range from 2000 to 7000 nm. In addition, the gloss of the molded products are defined using measuring Shine when light is incident at an angle of 60 degrees, may be approximately 40 or less. Molded product can be obtained by injection molding at a temperature of approximately component from 180 to 280°C., and the temperature of the cylinder of the extruder, approximately component is from 40 to 80°C.

DESCRIPTION of GRAPHIC MATERIALS

Figure 1 presents images of soft koukopoulos resin-based vinylaromatic copolymer (A1)used in the Examples 1-4, obtained using a transmission electron microscope (TEM).

Figure 2 presents TEM images of soft koukopoulos resin-based vinylaromatic copolymer (A2)used in the Examples 5 and 6.

Figure 3 presents the TEM images of soft koukopoulos resin-based vinylaromatic copolymer (A3)used in Comparative Examples 1 and 2.

4 shows the TEM image of the molded articles obtained in accordance with Example 1.

Figure 5 presents the TEM image of the molded articles obtained in accordance with Comparative Example 1.

INFORMATION CONFIRMING the POSSIBILITY of carrying out the INVENTION

(A) Soft kauchukopodobnoe resin-based vinylaromatic copolymer

When fo is mowani products made of ABS resin, which contains koutsokoumnis particles, a number kauchukopodobnoe particles is dispersed on the surface of the molded product forming on the surface a tiny ledges. These protrusions may scatter incident light, thereby reducing the gloss.

However, since the particles of the rubber phase contained in traditional ABS resin, are small and hard shell, formed by instilling a large number of densely Packed monomers on a rubber component, the proportion of grafted polymer is high, and the particles of the rubber phase have a dense structure.

In addition, this structure impedes the penetration of solvents into the resin, therefore, the traditional ABS resin has a low swelling index. In traditional ABS resin solid form of particles of the rubber phase may persist even after the formation of the product, and the protrusions may be formed only on limited areas in which rubber particles dispersed in such a way that the degree of surface roughness is low. Thus, from traditional ABS resin is difficult to produce products having low gloss and soft-touch surface.

Soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer suitable for use in accordance with aseason invention, may as dispersed phase include soft rubber particles having a larger particle diameter than the particles introduced into traditional ABS resin.

In particular, since the particles of the rubber phase soft koukopoulos resin (A) based on vinylaromatic copolymer can have a larger particle diameter than the diameter of the traditionally used rubber particles, and a small proportion of the grafted polymer, and may also be present in the form of particles, which are other monomers or polymers, such particles of the rubber phase are very flexible structure. Soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer also has a relatively high rate of swelling because of the ease of penetration into the resin other solvents.

In addition, in the manufacture of molded articles of the compositions of the present invention, including soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer, shown in figure 4, during the molding morphology of soft rubber particles can be modified with obtaining on the entire surface of the molded products of small protrusions and grooves. The microroughness of the surface is increased in the process of forming fine protrusions and grooves, and thus can be obtained a good low gloss and soft-touch surface of the ü.

Soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer used according to the present invention, includes vinylaromatic monomer, vinylcyanide monomer and rubber-based diene with conjugated double bonds. In one example implementation, soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer may include from about 45 to 90% of the mass. vinylaromatic monomer, from about 5 to 35 wt%. vinylcyanide monomer and about 5 to 20% of the mass. rubber-based diene with conjugated double bonds.

More specifically, soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer includes a matrix comprising vinylaromatic-vinylcyanide copolymer, and rubber particles dispersed in the matrix.

Rubber particles dispersed in a soft koukopoulos the resin (A) based on vinylaromatic copolymer, preferably may take the form, in which are enclosed vinylaromatic monomer, vinylcyanide monomer, vinylaromatic-vinylcyanide copolymer or mixture of these substances.

Preferably, the average particle diameter of the rubber may range from 6 to 20 μm, more preferably, from about 6.5 to 15 μm, and most preferably, from about 7 to 15 μm. If the particle diameter is approximately less than 6 μm, this makes it difficult to obtain a sufficiently low gloss, and if the particle diameter is approximately more than 20 μm, it is difficult to obtain a high toughness. The average particle diameter of the rubber can be measured using a measuring device, which uses the scattering of laser light on the basis of the volume average diameter of the particles. In addition, the average particle diameter can be measured with the scale marks on the image transmission electron microscope or on the basis of the mass-average particle diameter.

In accordance with the present invention, the proportion of grafted polymer in the rubber particles dispersed in the soft koukopoulos the resin (A) based on vinylaromatic copolymer can be measured by the following method. A certain amount of soft koukopoulos resin (A) based on vinylaromatic copolymer is placed in acetone and stirred to dissolve, and then leave at room temperature for 2 days, after which the gel and the solution is separated by centrifugation. At this point, the particles of the rubber phase in the gel, separated. Then the gel is dried in a vacuum oven at a temperature of approximately 50°C during the day and calculate the proportion of grafted polymer in accordance with the following Equation 1.

Equation 1

In the above Equation 1 dried gel (% mass.) mean % mass. the dried gel obtained from soft koukopoulos resin-based vinylaromatic copolymer, and rubber (% mass.) mean % mass. rubber-based diene with conjugated double bonds, is added in the manufacture of soft kauchukopodobnoe resin-based vinylaromatic copolymer.

The proportion of grafted polymer in the rubber particles may preferably be approximately from 40 to 90%, more preferably from about 60 to 90%, most preferably from about 70 to 90%. If the proportion of grafted polymer is approximately less than 40%, the rubber particles may be unstable, making it difficult to obtain a sufficiently high toughness, and, if the proportion of grafted polymer is approximately more than 90%, then it is difficult to obtain the desired soft to the touch.

Swelling index soft koukopoulos resin (A) based on vinylaromatic copolymer can be measured in accordance with the following method. One gram soft koukopoulos resin (A) based on vinylaromatic copolymer is placed in a 35 ml of a solvent composed of a mixture of toluene and methyl ethyl ketone in a volume ratio of 5:5, preparing the mixed solution. Peremeshany the solution weakly shake, dissolving soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer and then left to swell at room temperature for 21 hours.

Then the swollen gel is centrifuged at about 25,000 rpm and measure the weight of the wet gel. Then, the wet gel is dehydrated by vacuum drying for 4 hours at 105°C and measure the mass of the dried gel. Swelling index soft koukopoulos resin (A) based on vinylaromatic copolymer can be calculated in accordance with the following Equation 2.

Equation 2

Preferably the rate of swelling of soft koukopoulos resin (A) based on vinylaromatic copolymer may range from 13 to 30, more preferably from about 15 to 25. If the swelling index is in the range from about 13 to 30, can be obtained soft-touch surface, nice low gloss and high impact strength.

Non-limiting examples vinylaromatic monomer used for the manufacture of soft koukopoulos resin (A) based on vinylaromatic copolymer may include styrene, α-methylsterols, 2-methylsterol, 3-methylsterol, 4-methylsterol, 2-atillery, 3-atillery, 4-atillery, 4-n-propellera, 4-tert-butalbiral, 1-vinylnaphthalene, 2-vinilla is Talin, vinylcolor etc. Such vinylaromatic monomers can be used as such or in combination with each other. Among these monomers, preferred is styrene.

Vinylcyanide monomer used for the manufacture of soft koukopoulos resin (A) based on vinylaromatic copolymer can include copolymerizing unsaturated hydrocarbon group and a cyanide group. In one example implementation of the hydrogen atoms of the unsaturated hydrocarbon may be partially substituted C1-C6is an alkyl group.

Non-limiting examples vinylcyanide monomers may include Acrylonitrile, Methacrylonitrile, ethacrynate etc. Such monomers can be used as such or in combination with each other. Among these monomers, preferred is Acrylonitrile.

Non-limiting examples of rubbers on the basis of the diene with conjugated double bonds, used for the manufacture of soft koukopoulos resin (A) based on vinylaromatic copolymer may include diene rubbers such as polybutadiene, politicalbetting, polyacrylonitrile and similar rubbers; saturated rubbers obtained by the addition of hydrogen to the diene rubbers; isoprene rubbers; chloroprene rubbers; polymethylacrylate; ethylene-p is cut-diene ternary polymer (EPDM) and similar substances. Such rubbers can be used as such or in combination with each other.

Rubber-based diene with conjugated double bonds preferably may be a butadiene rubber or strollerderby rubber, more preferably butadiene rubber. In one example implementation, the viscosity of a solution of butadiene rubber may be from approximately 30 to 200 SP in 5% styrene solution, preferably from about 100 to 200 SP, more preferably from about 150 to 200 SP.

Soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer can be obtained by a well-known polymerization methods. Preferably use the method of continuous polymerization or continuous polymerization in solution.

When using traditional methods of polymerization, such as polymerization in emulsion or polymerization in suspension, stable obtaining particles of the rubber phase having an average particle diameter of approximately from 6 to 20 μm, is difficult. In addition, there are difficulties in the manufacture of such traditional ways of particles of the rubber phase comprising a large number of seized substances and a high proportion of grafted polymer, component approximately from 40 to 90%, and even more difficult is to teach swelling index in the range from approximately 13 to 30.

In one example implementation, soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer can be obtained in accordance with the following method.

The method of the present invention involves mixing approximately 100 mass. parts of a mixed solution comprising from about 40 to 60 mass. parts vinylaromatic monomer, from about 10 to 25 mass. parts vinylcyanide monomer, from about 7 to 20 mass. parts of the rubber-based diene with conjugated double bonds, and from about 5 to 30 mass. parts of solvent, from about 0.005 to 0.03 mass. parts of a polymerization initiator, to obtain a mixture; and slowly adding the mixture to the reactor and the subsequent conduct of the continuous polymerization under mild conditions with the formation of soft particles of the rubber phase. In one example implementation, to 100 mass. parts of the mixed solution may be added approximately 0.005 to 0.5 mass. parts of the agent controlling the molecular weight.

Because during the traditional methods of making particles of rubber, using at least about 0.04 wt. parts of polymerization initiator for rapid inversion of phases, rubber particles quickly instilled a great amount of monomers forming hard Obolo the ku, and this impedes the penetration of other monomers or polymers in the inner part of the particles of rubber.

Accordingly, the particles of the rubber phase obtained above in the traditional way, can have a small size and dense structure, which complicates the implementation of other particles in the particles of the rubber phase.

On the contrary, in accordance with the method of the present invention can be used approximately 0.005 to 0.03 mass. parts of a polymerization initiator; this causes a slow inversion of the phases, and the polymerization mixture can be produced under mild conditions, in which the mixing rate and degree of conversion can be controlled gradually (step by step). Consequently, may decrease the amount of grafted monomer to increase the capture rate of other monomers or polymers of the rubber particles, and, thus, can be increased particle size. In such cases, since the rubber particles are very plastic, resin can be easily modified when performing molding and may be enhanced by the microroughness on the surface.

In one of the embodiments of the present invention, the mixture can be loaded in the first reactor with a speed factor of approximately 10 to 50 kg/h, stirred at a speed of approximately component from 70 to Ob/min, and subjected to polymerization to obtain the degree of conversion, component approximately 30 to 40%. The polymerization product may be loaded into the second reactor, stirred at a speed of approximately component is from 40 to 80 rpm, and subjected to further polymerization to obtain a degree of conversion of approximately component from 55 to 80%. Optionally, the method may also include the step of discharging unreacted monomer from the reactor after the polymerization.

The number of soft koukopoulos resin (A) based on vinylaromatic copolymer of the present invention may comprise from about 10 to 80 wt. -%, preferably from about 20 to 70 wt. -%, more preferably from about 35 to 65% of the mass. in terms of the total weight of the resin composition. If the number of soft koukopoulos resin (A) based on vinylaromatic copolymer is approximately less than 10 wt. -%, it is difficult to obtain a certain level of low gloss and good soft to the touch surface, and if this amount is more than 80 wt. -%, there cannot be obtained a sufficient resistance to shock loads.

(C) a Modified rubber resin based vinylaromatic copolymer

Modified rubber resin (B) based on vinylaromatic copolymer N. the present invention may contain from about 40 to 80% of the mass. rubber-based diene with conjugated double bonds, calculated on the total weight of the modified rubber resin (B) based on vinylaromatic copolymer. When using these ranges can be obtained the desired resistance to shock loads.

In addition, to improve the resistance to shock loads molded articles molded from the composition of thermoplastic resin of the present invention, the modified rubber resin (B) based on vinylaromatic copolymer may preferably contain rubber particles with an average diameter of approximately comprising from 0.1 to 0.8 μm. The average particle diameter of the rubber can be measured using a measuring device, which uses the scattering of laser light on the basis of the volume average diameter of the particles. In addition, the average particle diameter can be measured with the scale marks on the image transmission electron microscope or on the basis of the mass-average particle diameter.

Modified rubber resin (B) based on vinylaromatic copolymer can be obtained by a well-known polymerization methods such as emulsion polymerization, polymerization in suspension polymerization in volume, etc. In one example implementation, the modified rubber chemicals the resin (B) based on vinylaromatic copolymer can be obtained by graft-copolymerization of from about 8 to 45% of the mass. vinylaromatic monomer, from about 2 to 30 wt%. vinylcyanide monomer and from about 40 to 80% of the mass. rubber-based diene with conjugated double bonds.

To make the resin's ability to process and heat resistance, at the time of manufacture of the modified rubber resin (B) based on vinylaromatic copolymer, the resin can be added to the monomers, for example acrylic acid, methacrylic acid, maleic anhydride and N-substituted maleimide. The amount used of the monomer may be from about 0 to 15 wt%. in terms of the total weight of the modified rubber resin (B) based on vinylaromatic copolymer.

Non-limiting examples of rubbers based on dienes with conjugated double bonds, used for the manufacture of modified rubber resin (B) based on vinylaromatic copolymer may include diene rubbers such as polybutadiene, politicalbetting, polyacrylonitrile and similar rubbers; saturated rubbers obtained by the addition of hydrogen to the diene rubbers; isoprene rubbers; chloroprene rubbers; polymethylacrylate; ethylene-propylene-diene ternary polymer (EPDM) and similar substances. Such rubbers can be used as such or in combination with each other. Preferred is shown rubbers are diene rubbers, and more preferred is polybutadiene rubber.

Non-limiting examples vinylaromatic monomer used for producing the modified rubber resin (B) based on vinylaromatic copolymer may include styrene, α-methylsterols, 2-methylsterol, 3-methylsterol, 4-methylsterol, 2-atillery, 3-atillery, 4-atillery, 4-n-propellera, 4-tert-butalbiral, 1-vinylnaphthalene, 2-vinylnaphthalene, vinyltoluene and so on, and these monomers can be used as such or in combination with each other. Among these monomers, preferred is styrene.

Non-limiting examples vinylcyanide monomer suitable for the manufacture of modified rubber resin (B) based on vinylaromatic copolymer may include Acrylonitrile, Methacrylonitrile, ethacrynate etc. Such monomers can be used as such or in combination with each other.

The composition of thermoplastic resin may include from about 4 to 60% of the mass. modified rubber resin (B) based on vinylaromatic copolymer, preferably from about 8 to 40% of the mass. If the number of modified rubber resin (B) based on vinylaromatic copolymer is approximately less than 4 wt. -%, this makes it difficult to obtain a certain level of resistance to shock n is gruska, if the amount is more than 60 wt. -%, it deteriorates the fluidity of the resin and its ability to be processed.

(C) Resin-based vinylaromatic-vinylcyanide copolymer

Resin (C) on the basis of vinylaromatic-vinylcyanide copolymer can be obtained by copolymerization of from about 40 to 90% of the mass. vinylaromatic monomer and from about 10 to 60 wt%. vinylcyanide monomer, calculated on the total weight of the resin (C) on the basis of vinylaromatic-vinylcyanide copolymer.

To give the resin (C) on the basis of vinylaromatic-vinylcyanide copolymer ability to process and heat resistance, the resin (C) on the basis of vinylaromatic-vinylcyanide copolymer may also include acrylic acid, methacrylic acid, maleic anhydride or N-substituted maleimide, and the monomers can be introduced in the amount of approximately from 0 to 30% of the mass. in terms of the total weight of the resin (C) on the basis of vinylaromatic-vinylcyanide copolymer.

Non-limiting examples vinylaromatic monomer used for producing the resin (C) on the basis of vinylaromatic-vinylcyanide copolymer may include styrene, α-methylsterols, 2-methylsterol, 3-methylsterol, 4-methylsterol, 2-atillery, 3-atillery, 4-atillery, 4-n-propellera, 4-tert-butylthio is, 1-vinylnaphthalene, 2-vinylnaphthalene, vinyltoluene and so on, and these monomers can be used as such or in combination with each other. Among these monomers, preferred is styrene.

Resin (C) on the basis of vinylaromatic-vinylcyanide copolymer may include from about 40 to 90% of the mass. vinylaromatic monomer, preferably from about 50 to 85% of the mass. If the number vinylaromatic monomer is less than 40 wt. -%, it can significantly increase the viscosity of the rubber, and thus, the ability of the composition of thermoplastic resin with a low gloss processing may deteriorate. If this amount is more than 90 wt. -%, it may deteriorate the toughness of the composition.

Non-limiting examples vinylcyanide monomer may include Acrylonitrile, Methacrylonitrile, ethacrynate etc. These monomers can be used as such or in combination with each other. Among these monomers, preferred is Acrylonitrile. The amount used vinylcyanide monomer may preferably be approximately from 10 to 60% of the mass.

In one example implementation, the composition of thermoplastic resin may include about 5 to 80 wt. -%, preferably from about 10 to 50 wt. -%, resin (C) on the basis of ventilationskomponenter copolymer. If the amount of resin (C) on the basis of vinylaromatic-vinylcyanide copolymer is less than 5 wt. -%, the ability of a composition of thermoplastic resin with a low gloss processing may deteriorate, and if this amount is more than 80 wt. -%, it is difficult to obtain a sufficiently high toughness.

The composition of thermoplastic resin may also include an additive selected from flame retardants, stabilizers, modifiers, increasing shock strength, antioxidants, light stabilizers, pigments, dyes, inorganic fillers, and additives such can be used as such or in combination with each other. Inorganic fillers may include asbestos, glass fiber, talc, sulfates, and similar substances. Additives can be incorporated in the amount of approximately 30 mass. parts or less in terms of approximately 100 mass. parts (A)+(B)+(C), for example, from about 0.001 to 30 mass. parts.

The composition of thermoplastic resin can be obtained by traditional methods. For example, granular form of the resin composition can be obtained by simultaneously mixing the above components and selected additives in the mixer and subsequent ekstrudirovannym the molten mixture through a conventional extruder.

Fo movano product molded from the composition of thermoplastic resin of the present invention may have a high impact strength. As shown in figure 4, on the surface of the molded product can be shaped many frequent small protrusions that increase the surface microroughness and creates a soft touch and nice low gloss.

In one example implementation, the average surface roughness (Ra) of the molded articles molded from the compositions of thermoplastic resin, may be approximately from 400 to 800 nm, and the height of the roughness at ten points (Rz) may be from about 2000 to 7000 nm. The average surface roughness (Ra) and the height of the roughness at ten points (Rz) can be measured using a device for measuring a surface profile VEECO Optical Profiler NT-1100; method of measurement of this value is described in detail below. In addition, the gloss of the molded products are defined using measuring Shine when light is incident at an angle of 60°, may be approximately 40 or less. As lowering of the measured values of the gloss may decrease the gloss of the product. Thus, the degree of gloss obtained according to the present invention, has no lower boundary of the minimum value. The gloss measured when light is incident at an angle of 60°, can be defined when p is power meter gloss BYK-Gardner Gloss Meter.

Also the impact strength Izod molded product, measured respectively on the sample 1/8 inch (3,2·10-3m) and ¼ inch (6,4·10-3m) in accordance with ASTM D256, may be approximately 20 to 30 kgf·cm/cm (from 196 to 294 N·m/m) and from about 7 to 25 kgf·cm/cm (from 167 to 245 N·m/m).

Thus, since the composition of thermoplastic resin and molded product can have a pleasant soft-touch surface, low gloss and impact strength, the composition of thermoplastic resin may be used for the manufacture of various products, such as internal/external parts or enclosures of electrical/electronic equipment, car parts, small household and personal/household goods and similar items.

In one example implementation, the composition of thermoplastic resin can be molded details electrical/electronic equipment or buildings TVs sets of microphone and headphones, mobile phones, digital cameras, GPS navigators, washing machines, computers, MP3 players, DVD players, video players, CD players, washing machines and automation equipment office. Also the composition of thermoplastic resin can be used for the manufacture of internal/external on the hoist hire.

Non-limiting examples of the forming methods include extrusion molding, injection molding or injection molding, which can be easily carried out by experts in the field of technology.

In one example implementation of the molded product can be obtained from the composition of thermoplastic resin using a molding machine under pressure at approximately 180 to 280°C and the temperature of the cylinder of the extruder, approximately component is from 40 to 80°C.

A better understanding of the invention can be achieved by consideration of the following examples, which are given to illustrate the invention and do not limit the scope of the present invention defined by the attached claims.

DESCRIPTION of embodiments of the INVENTION

Specifications of components used in Examples and Comparative Examples, described in more detail below.

(A) Soft kauchukopodobnoe resin-based vinylaromatic copolymer

(A1) To a mixture comprising 53,4 masses. parts of styrene, 17.8 masses. parts of Acrylonitrile and 20 mass. parts of ethylbenzene was added 8.8 masses. parts of butadiene rubber having a viscosity of a 5%styrene solution component 170 SP. Then to prepare a mixed solution was added 0.015 g of the masses. parts of 1,1-bis(tert-BUTYLPEROXY)cyclohexane, used in the quality of the initiator, and 0.07 wt. parts of tert-dodecylmercaptan used as an agent for controlling the molecular weight. The mixed solution was loaded into the reactor at a flow rate of 25 kg/h In the first reactor was set stirring speed of 100 rpm, and the conversion rate, which is 35%. In the second reactor was set stirring speed equal to 70 rpm, and the degree of conversion, which is 75%. The reagent discharged from the reactor, continuously transported in a device for removing volatile components, which were removed unreacted monomer and solvent. Then, the polymerization product was subjected to granulation, getting ABS resin (A1). ABS resin (A1)obtained in this way had the following characteristics: swelling index of 16.2, the average particle diameter of the rubber 8,58 μm and the proportion of grafted polymer 77,8%. TEM image of the particles of rubber, ABS resin (A1) is shown in Figure 1.

(A2) the Synthesis was carried out in the same way that getting ABS resin (A1), with the only exception that the mixing rate in the first reactor was 80 rpm thus Obtained ABS resin (A2) has the following characteristics: swelling index 19,3, average particle diameter of the rubber 14,11 μm and the proportion of grafted polymer was 82.3%. TEM image of the particles of rubber, ABS resin (A2) is shown in Fig 2.

(A3) the Synthesis was carried out in the same way that p is torching ABS resin (A1), with the only exception that applied to 0.04 mass. parts of 1,1-bis(tert-BUTYLPEROXY)cyclohexane, and the mixing rate in the first reactor was 130 rpm thus Obtained ABS resin (A3) had the following characteristics: swelling index of 11.6, the average particle diameter of the rubber 6.42 per μm and the proportion of grafted polymer of 116.8%. TEM image of the particles of rubber, ABS resin (A3) is shown in Fig 3.

(C) a Modified rubber resin based vinylaromatic copolymer

(b1) 31 mass. parts of styrene, 11 mass. parts of Acrylonitrile and 58 of the masses. parts of butadiene rubber were mixed and subjected to emulsion polymerization. Used graft-ABS (hereinafter "g-ABS) in the form of particles comprising a core and a shell containing rubber particles, the average diameter of which was of 0.32 μm, and 58% of the mass. rubber-based diene with conjugated double bonds.

(b2) g-ABS was obtained by the method described in Example (b1), except that the average particle diameter of the rubber was to 0.21 μm.

(C) Resin-based vinylaromatic-vinylcyanide copolymer

Used the SAN resin, the mass-average molecular weight of which amounted to 120,000, and 32% of the mass. Acrylonitrile.

(D) the Antioxidant

As a phenolic antioxidant with spatially complicated structure used octadecyl-3(4-hydroxy-3,5-di-tert-butylphenyl)propionate.

(E) a Modifier based on silicon, which increases the impact strength

As a modifier based on silicon, which increases the impact strength, used dimethylpolysiloxane.

Examples 1-6

The components listed in Table 1 were mixed, and the mixture was kneaded in melt and subjected to extrusion through traditional dvuhseriynyy extruder (L/D=29, f=45 mm) at a temperature of 220°C, obtaining pellets of thermoplastic resin. The resin pellets were dried at 80°C for 3 hours and molded in the form of prototypes using machines for casting under pressure loading 6 oz (0.17 kg) at 180-280°C. and the temperature of the cylinder of the extruder, part of 40-80°C. the TEM image of the test samples obtained in Example 1 is shown in Figure 4.

Comparative Examples 1-4

The components listed in Table 1 were mixed, and the mixture was kneaded in melt and subjected to extrusion through traditional dvuhseriynyy extruder (L/D=29, f=45 mm) at a temperature of 220°C, obtaining pellets of thermoplastic resin. The resin pellets were dried at 80°C for 3 hours and molded in the form of prototypes using machines for casting under pressure loading 6 oz (0.17 kg) at 180-280°C. and the temperature of the cylinder of the extruder, part of 40-80°C. the TEM image of the test samples obtained in Example 1 is shown in Figure 5.

Table 1
(A)(In)(C)(D)(E)
(A1)(A2)(A3)(b1)(b2)
Example 150--15-350,10,02
Example 250---15350,10,02
Example 360--15-250,10,02
Example 460 ---15250,10,02
Example 5-50-15-350,10,02
Example 6-60-15-250,10,02
Comparative Example 1--5015-350,10,02
Comparative Example 2--6015-250,10,02
Compare the capacity Example 3 ---20-800,10,02
Comparative Example 4---25-750,10,02

The physical properties of the test samples obtained in Examples 1-6 and Comparative Examples 1-4, was determined in accordance with the following methods, and the results are shown in Table 2.

(1) Impact strength Izod: Impact strength notched Izod was measured on samples of 1/8 inch (3,2·10-3m) and ¼ inch (6,4·10-3m) (inch kgf·cm/cm), after aging at 23°C and 50% relative humidity for 48 hours in accordance with ASTM D256

(2) gloss: gloss was measured when light is incident at an angle of 60° using a gloss meter BYK-Gardner Gloss Meter.

(3) surface Roughness: the surface Roughness was measured using a device for measuring surface roughness, VEECO Optical Profiler NT-1100. The terms used to describe the present invention, have the following meanings.

(-1) the Average surface roughness (Ra): the Average surface roughness (Ra) can be calculated as the arithmetic average deviation of the absolute values of the height deviation of surface profile from the mean line, measured on the sample length. The higher Ra, the higher the surface roughness. Unit of measure average surface roughness nm.

(3-2) the Average height of roughness at ten points (Rz): the Average height of roughness at ten points (Rz) can be calculated as the average difference in height between the five highest points and five deepest grooves, measured along the length of the sample along a line parallel to the line average roughness. The unit is nm.

The average height of roughness at ten points (Rz) is used to measure the sliding surfaces. The greater the height of the roughness at ten points (Rz), the higher the roughness of the surface.

Table 2
Impact strength IzodThe surface roughnessGloss
1/8 inch¼ InchRaRz20°60°85°
Example 121of 17.5598,642806,223,971,3
Example 220,117,1602,643805,621,673,5
Example 323,316,8633,051408,324,570,7
Example 421,418,2568,542107,428,475,4
Example 522,217,9590,140405,019,069,4
Example 624,120,1 584,544106,418,268,3
Comparative Example 118,915,3313,1117018,453,690,4
Comparative Example 220,116,8318,7122020,859,292,3
Comparative Example 314,611,190,3163081,094,496,8
Comparative Example 416,112,384,7151082,195,497,0

As can be seen from Table 2, obtained in Examples 1-6 soft kauchukopodobnoe resin-based vinylaromatic copolymer (A1 and A2), and eUSA swelling index, approximately 13 to 30, and the proportion of grafted polymer, component approximately from 40 to 90%, has a good surface roughness and low gloss and high impact strength.

It is also clear that, despite the change in the average particle diameter of the rubber, put in a modified rubber resin based vinylaromatic copolymer (B)can be obtained good surface roughness.

Thus, it is seen that with the increasing mikroheranhvatho surface, the surface of the test samples obtained in accordance with the present invention becomes low gloss and soft to the touch, like a paper or pulp mass.

On the other hand, soft kauchukopodobnoe resin-based vinylaromatic copolymer (A3)obtained in accordance with Comparative Examples 1 and 2, has a low gloss, but relatively low swelling index, and a large proportion of the grafted polymer, and thus, it is seen that the roughness of the surface of the resin is insufficient.

As shown in figure 4, the microroughness on the surface of the samples obtained in Example 1, was significantly increased, i.e. over the entire surface of the test samples there are small ledges and frequent grooves. However, as shown in Figure 5, it is seen that in the test image is f, obtained in Comparative Example 1, the tabs are only on the site where the dispersed rubber particles, and the density of the surface roughness of the specified sample is low.

In Comparative Examples 3 and 4 were used traditional compositions ABS resin, processed by extrusion in the melt. As can be seen from Table 2, the resin composition of the present invention has a low gloss, high impact strength and good surface roughness in comparison with conventional ABS resin compositions.

In the proposed above description, the present invention is described with specific preferred embodiments; however, specialists in the art should understand that the present invention can be produced changes or modifications not beyond the scope of this invention defined by the attached claims.

1. The composition is a thermoplastic resin with a low gloss with soft touch surface, including:
(A) from about 10 to 80 wt.% soft koukopoulos resin-based vinylaromatic copolymer, which as the dispersed phase comprises rubber particles with a fraction of the grafted polymer, component approximately from 40 to 90%, and the average diameter of the particles constituting approximately from 6 to 20 microns;
(B) bring the flax from 4 to 60 wt.% modified rubber resin based vinylaromatic copolymer; and
(C) from about 5 to 80 wt.% resin-based vinylaromatic-vinylcyanide copolymer.

2. The composition of thermoplastic resin according to claim 1, in which soft koutsokoumnis vinylaromatic copolymer (A) has a swelling index of approximately from 13 to 30.

3. The composition of thermoplastic resin according to claim 1, in which soft koutsokoumnis vinylaromatic copolymer (a) consists of the matrix, including vinylaromatic-vinylcyanide copolymer; and rubber particles, which are dispersed in the matrix and contain a fraction of the grafted polymer component approximately from 40 to 90%, and have an average particle diameter of approximately from 6 to 20 microns.

4. The composition of thermoplastic resin according to claim 1, in which the inside of the rubber particles contained vinylaromatic monomers, vinylcyanide monomers, vinylaromatic-vinylcyanide copolymer or mixture of these compounds.

5. The composition of thermoplastic resin according to claim 1, in which soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer includes from about 45 to 90 wt.% vinylaromatic monomer, from about 5 to 35 wt.% vinylcyanide monomer, and from about 5 to 20 wt.% rubber-based diene with conjugated double bonds.

6. The composition of thermoplastic resin according to claim 1, in which soft cow is capadonna resin (A) based on vinylaromatic copolymer obtained by continuous polymerization or continuous polymerization in solution.

7. The composition of thermoplastic resin according to claim 1, in which soft kauchukopodobnoe resin (A) based on vinylaromatic copolymer which is obtained by mixing 100 wt. including mixed solution comprising from about 40 to 60 wt. including vinylaromatic monomer, from about 10 to 25 wt. including vinylcyanide monomer, from about 7 to 20 wt. including rubber-based diene with conjugated double bonds and from about 5 to 30 wt. including solvent from approximately 0.005 to 0.03 wt. hours of polymerization initiator, and about 0.005 to 0.5 wt. including agent controlling the molecular weight, the polymerization mixture to achieve the degree of conversion, component approximately 30 to 40%, and further the polymerization product of polymerization to achieve the degree of conversion, approximately component from 55 to 80%.

8. The composition of thermoplastic resin according to claim 1, in which a modified rubber resin (B) based on vinylaromatic copolymer is a graft copolymer containing from about 40 to 80 wt.% rubber-based diene with conjugated double bonds, from about 8 to 45 wt.% vinylaromatic monomer and from about 2 to 30 wt.% vinylcyanide monomer, and contains rubber particles having an average particle diameter of approximately from 0.1 to 0.8 μm.

9. To notice thermoplastic resin according to claim 1, in which vinylaromatic-vinylcyanide copolymer (C) comprises from about 40 to 90 wt.% vinylaromatic monomer and from about 10 to 60 wt.% vinylcyanide monomer.

10. The composition of thermoplastic resin according to claim 1, in which the resin composition further includes an additive selected from the group consisting of flame retardants, stabilizers, modifiers, increasing shock strength, antioxidants, light stabilizers, pigments, dyes, inorganic fillers and mixtures of these substances.

11. The composition of thermoplastic resin according to any one of pp.5, 8 and 9, in which vinylaromatic monomer is at least one monomer selected from the group consisting of styrene, α-methylstyrene, 2-methylstyrene, 3-methylstyrene, 4-methylstyrene, 2-ethylstyrene, 3-ethylstyrene, 4-ethylstyrene, 4-n-propertywala, 4-tert-butylstyrene, 1-vinylnaphthalene, 2-vinylnaphthalene and vinyltoluene.

12. The composition of thermoplastic resin according to any one of pp.5, 8 and 9, in which vinylcyanide monomer is at least one monomer selected from the group consisting of Acrylonitrile, Methacrylonitrile and estacionario.

13. The composition of thermoplastic resin according to claim 5 or 8, in which the rubber-based diene with conjugated double bonds is in me is greater least one rubber selected from the group consisting of polybutadiene, politicalbetting, polyacrylonitrile, isoprene rubbers, chloroprene rubbers, polymethylacrylate and ethylene-propylene-diene ternary copolymer (EPDM).

14. A molded product molded from the composition of thermoplastic resin according to any one of claims 1 to 10.

15. The moldings according to 14, characterized in that the average surface roughness (Ra) of the molded product is from about 400 to 800 nm, and the height of the surface roughness at ten points (Rz) is approximately 2000 to 7000 nm.

16. The moldings according to 14, characterized in that the gloss of the molded products are defined using measuring Shine when light is incident at an angle of 60°, approximately 40 or less.



 

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17 cl, 2 tbl

FIELD: chemistry.

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8 cl, 1 tbl

FIELD: chemistry.

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3 cl, 1 tbl, 4 ex

The invention relates to the chemistry of polymers, namely to stable compositions based resin plant (ABS) copolymers, which are structural materials

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Polymer composition // 2058987
The invention relates to polymeric compositions based resin plant (ABS) copolymers, which are widely used as structural materials, for example, for the manufacture of shells audio - and video equipment, computers, telephones, etc

Polymer composition // 2057772
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FIELD: chemistry.

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6 cl, 2 tbl

FIELD: chemistry.

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12 cl, 1 tbl, 7 ex

FIELD: chemistry

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6 cl, 1 tbl, 6 ex

FIELD: chemistry.

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11 cl, 1 tbl, 20 ex

FIELD: chemistry.

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14 cl, 4 tbl, 8 ex

FIELD: chemistry.

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15 cl, 4 dwg, 1 tbl, 4 ex

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19 cl, 1 tbl, 24 ex

FIELD: chemistry of polymers, chemical technology.

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EFFECT: improved preparing method, improved and valuable properties of polymers.

14 cl, 14 tbl, 24 ex

FIELD: chemistry of polymers, chemical technology.

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EFFECT: improved preparing method, valuable technical properties of materials.

18 cl, 5 tbl, 27 ex

Rubber composition // 2254348

FIELD: rubber industry.

SUBSTANCE: invention concerns a method for grafting polymers based on conjugated diene monomers to brominated butyl rubbers and using thus obtained grafted copolymers in rubber compositions, which, after vulcanization, acquire improved physical characteristics. Grafting procedure comprises mixing solid brominated butyl rubber with solid polymers based on conjugated diene monomer including some quantity of bonds C-S-(S)n-C with n being an integer equal from 1 to 7. Mixing is conducted at temperature above 50 over a period of time long enough to complete the grafting. Rubber composition containing above grafted polymer optionally includes one or more curing agents. Cured rubber composition is intended for manufacturing tracks.

EFFECT: increased shock-absorbing capacity of products.

14 cl, 5 dwg, 5 tbl, 3 ex

FIELD: chemistry.

SUBSTANCE: invention relates to a method of producing an asphalt modifier composition, involving: obtaining a triblock copolymer via block copolymerisation of a vinyl aromatic hydrocarbon and a diene compound with conjugated double bonds as a result of anionic polymerisation using an organic anionic initiator in a reactor, having a hydrocarbon solvent, where the step of producing the block copolymer involves: formation of a vinyl aromatic block by feeding a vinyl aromatic hydrocarbon into a reactor, having a hydrocarbon solvent, and then feeding an organic anionic initiator; forming a diene block with conjugated double bonds, bonded to the end of the vinyl aromatic block, by feeding a diene compound with conjugated double bonds into the reactor; feeding a functional additive, selected from a group consisting of compounds of formula 1, into the reactor; and obtaining an asphalt modifier composition, including a block copolymer and a functional additive, by removing a hydrocarbon solvent, Formula 1 ; in formula 1, the sum n+m-m' is equal to 35, n is an integer from 1 to 5, each of m and m' is an integer equal to at least 1, and X is an ester group [-C(=O)O-]. The invention also relates to a method of producing the asphalt modifier composition and asphalt composition.

EFFECT: asphalt modifier composition dissolves fast in asphalt without significantly reducing softening temperature of asphalt, which enables to obtain a homogeneous asphalt composition and increase effectiveness of the asphalt composition.

17 cl, 1 tbl, 4 ex

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