The method of obtaining products, coatings and films based on fluoro

 

(57) Abstract:

The invention relates to methods of obtaining products, coatings and films based on fluoro svobodnovihrevym forming. Fluoropolymer elastomer grades SCF-32 or SCF-26 dissolved in a mixture of alkyl(meth)acrylic monomer and copolymerizes with him oligoadenylate in their mass ratio(0,85-0,97): (0,03-0,15) and copolymerized in mass at room temperature in the presence of peroxide or hydroperoxide initiator and activator - tertiary aromatic amine or a salt of a metal of variable valence. Additionally, use a solution of paraffin wax in an organic solvent, and shaping is done by the method of free casting with simultaneous copolymerization, and the mass ratio of the silicone elastomer and a mixture of alkyl(meth)acrylate and oligoadenylate (0.1 to 0.4): 1. The invention makes it possible to obtain solutions ftorkauchukov volume items in the block, the films and coatings of greater thickness with a high level of heat and wear resistance, impact resistance and resistance to corrosive environments. 3 table.

The invention relates to the production of polymerization of plastics, in particular the production of polymer compositions based on forcause odnopetlevom the molding and curing curing at room temperature in the mass, that allows you to get agressiveone coating, solid gasket-sealing materials, body parts and products, operating at elevated temperature in contact with aggressive environments, as well as desinsection polymerizable adhesives polymers which, due to their chemical nature have low self-adhesion.

Known compositions based ftorkauchukov in the form of sealants and Polakov obtained by dissolving forecasters in ketones and esters. Data composition containing the fluoropolymer elastomer, a solvent, vulcanizing and accelerating agents, characterized by a rather wide temperature range operation. (Labutin A. P. anti-Corrosion and sealing materials based on SC. - L.: Chemistry, 1982, S. 82-83).

However, they do not have their own adhesion to metals and require the use of adhesive sublayer. For the formation of thin coatings are required hot drying air blower at a temperature of 50-120oC. the Process is accompanied by shrinkage of the film due to the need for diffusion separation solvent component. The presence in the compositions of organic solvents delays the curing and worsens the condition is Holocene on the basis of their bulk products, as well as films and coatings of greater thickness. In addition, the use directionspanel solvent is not possible to modify the structure of the fluoroelastomer made to improve complex performance properties.

Know the use of low molecular weight plasticizers in the compositions based ftorkauchukov. The introduction of plasticizers can improve technological properties and frost resistance. (C. P. Novitskaya, H. N. Nudelman, A. A. Dontsov. Forecaster. - M.: Chemistry, 1988, S. 112-113).

However, due to directionspanel plasticizers and their tendency to migrate from the scope of the compositions on the surface of the product significantly reduced the level of the adhesive interaction when attaching to metal substrates. Thus deteriorate heat and thermal stability, aggression stability and strength properties of the material. In addition, most of the plasticizer evaporates in the second stage of vulcanization (with temperature control), which also leads to a significant shrinkage of the products, the formation of these cracks or pores. Modification of the supramolecular structure of the fluoroelastomer made in the presence of traditional plasticizers does not occur.

A method of obtaining modified p is of ionizing radiation. (Japan Patent 57-18530, 08 F 259/08, 1982).

The disadvantages of the method are related to the fact that in order to initiate the process of graft polymerization requires the use of special sources of ionizing radiation corresponding to the expensive equipment and special protection measures.

A method of obtaining fluorinated resins grafted polymerization of the monomer in the presence of the elastomer containing fluoride and peroxide groups. The process is carried out in aqueous medium dispersion of fluorine-containing elastomer, and the polymerization is carried out at an elevated temperature in the presence of at least one reductant. (French Patent 2619384, 08 F 259/08, 1989).

In General, the disadvantages of the method are as sophisticated technology and mnogostadiinost obtain a grafted fluorine-containing copolymers, complexity, requiring use of special equipment. First, according to the invention using fluoroelastomer of peroxide groups. Industrially produced florkowski do not contain such groups. Therefore, they must be entered in the macromolecule in the relevant chemical transformations and technological operations. Secondly, the process of grafting monomial copolymerization final product you want to select, filter and dry, and used water requires treatment and recovery.

Closest to the present invention is the invention according to which the fluorine-containing polymer is dissolved in the acrylic monomer or a mixture of polyfunctional co monomer, followed by polymerization in mass with getting hard polymeric materials or materials with the structure of interpenetrating polymers. The composition of the invention can be used as the basis for dental masses characterized after polymerization, low water absorption and high adhesion to dental prostheses. The polymerization process is carried out at elevated temperature (55-100oC) for 10-150 minutes or by photopolymerization under the action of visible or ultraviolet rays for 7-10 minutes at room temperature. (Patent EPO 0358195, 08 F 259/08, 1990).

The obstacles to achieve the desired technical result when using the compositions, their production and use in accordance with the invention, taken as a prototype include the following. First, the stated ratio forelectioneering compositions (see tables 1, 2, 4, and 5 describe ptItsa mainly in the swelled state. Indeed, such structures are suitable for fabrication of the basics of dental prostheses and basic materials, which use excessive contact pressure in forming the matrix, or when working with a spatula and other dental instruments. However, under normal conditions they do not have svobodnovihrevye properties and is not suitable for the production of coatings and bulk products according to the technology of liquid-phase formation without excessive pressure. Secondly, the need for the polymerization of unsaturated components of the compositions at elevated temperatures complicates their use in obtaining, for example, coatings gumirovicha destination on a metal basis, because the method involves heating the entire area of the substrate for the implementation of the curing process. It is known that in the process of heating the vapor pressure of the monomer increases, and it begins to evaporate from the solution volume. Thirdly, according to the patent prototype curing can be carried out at room temperature in a relatively short period of time by photopolymerization in the presence of photofinishing agents. This method has significant limitations on the thickness photopolymerizable layer, as is required using special emitters of ultraviolet and visible rays sufficiently large energy capacity.

The task of the invention is the expansion of the range and applications of polymer compositions based ftorkauchukov, namely the development of a method of obtaining compositions with variable viscosity, fluidity, ability to svobodnaia the molding and curing the curing of the mass that can be obtained from solutions of fluoroelastomer made solid products in the unit, as well as the films and coatings of greater thickness at room temperature.

The technical result is to simplify the technology for compositions that are characterized by high adhesion to metal substrates and low shrinkage after curing curing without heat and without the use of sources of excess energy, as well as polymeric materials of different hardness high heat and wear resistance, impact resistance and resistance to corrosive environments. Simultaneously with the implementation of the method svobodolyubivoi processing technologies ftorkauchukov is a modification of the matrix fluoroelastomer made due to the formation of grafted and crosslinked copolymers.

This technical result is achieved by implementation of the method of obtaining the with oligopyrroles, with the subsequent molding and copolymerization in bulk in the presence of a peroxide initiator and a tertiary aromatic amine as activator of polymerization by the fact that the silicone elastomer SCF-32, constituting the copolymer vinylidenefluoride with Cryptosporidium or SCF-26, which represents a copolymer of vinylidenefluoride with HEXAFLUOROPROPYLENE, dissolved in a mixture of alkyl(meth)acrylic monomer with copolymerizable with him oligopyrroles taken in a weight ratio of(0,85-0,97):(0,15-0,03) accordingly, when the total weight ratio of fluoropolymer elastomer : alkyl(meth)acrylic monomer and oligopyrroles (0,1-0,4): 1, respectively, and shaping is done by the method of free casting with simultaneous copolymerization in bulk at room temperature in the presence of a tertiary aromatic amine or a salt of a metal of variable valence as a polymerization activator, peroxide or hydroperoxide initiator and a solution of paraffin in toluene.

The invention consists in the following.

Distinctive features of forecasters are high temperature resistance, ozone resistance, chemical resistance to oils, fuels, solvents, acids and d the part with the adhesive mount in particular, to metal substrates. The macromolecules of these rubbers are characterized by a high energy density cohesion. Significant intermolecular interactions lead high rigidity of the polymers of this class. As a result, they are virtually plastiroute, bad calandrella and processed. These factors hinder their full use for solving urgent problems of quality gammirovanie and production of high-performance protective coatings and products of polyfunctional destination. The combination of ftorkauchukov with plasticizers or translate them into solutions using organic solvents can improve the processability. However, in these cases there are problems and limitations associated with the inevitable migration of the plasticizer and the need to remove directionspublic low-molecular components from the scope of the product to be cast.

In this regard, in the present invention is used methodological principle informed selection and use as modifying agents effect of liquid polyfunctional reactive compounds, which in the first stage perform the role rastvorjajus the C solutions. In the future, their presence allows you to minimize the proportion of volatile reactants and get directly in the process of forming solid products in the unit, as well as the films and coatings of different thickness due to the fact that the monomers themselves into a polymeric material. In the curing process of curing the monomer component in the presence of fluoroelastomer made may be a modification of the structure of the material due to the formation of grafted and crosslinked copolymers, mixed polymer-polymer composites for various microheterogenous organization.

Macromolecule ftorkauchukov are saturated and do not contain reactive groups and double bonds. However, in the presence of polymerizable monomers may obtain graft copolymers, the education of a certain number of gel-fraction, as well as homopolymers.

The possibility of formation of graft copolymers and cross-linked structures due to the fact that the hydrogen atom in vinylidenefluoride the links on one side only shielded fluorocarbon group, and the bond energy of C-H in them lowered inductive influence of the neighboring groups. Therefore, the hydrogen atom comes off free radicals with destinasi to them and linking of polymer chains.

Raising the level of the adhesive interaction according to the invention is associated with a relatively low viscosity verkaufsmanager compositions. On the one hand, this allows to achieve a higher occupancy of the surface of the substrate and contributes to a larger area of interfacial contact. On the other - when combining the processes of conversion of monomer in the high-polymer and bonding between the surfaces formed an Association of different types, including the most durable and chemical. This contributes to the expansion of the range of adhesives for the technically valuable polymers which, due to their chemical nature have low self-adhesion.

The implementation of the method of obtaining products, coatings and films from a solution of a silicone elastomer in a mixture of alkyl(meth)acrylic monomer and oligoadenylate with the subsequent molding and copolymerization components in the mass at room temperature ensures the achievement of the technical result consists in the reduction of total physical and chemical shrinkage. It is essential when obtaining from a liquid polymerizable compositions precision castings, products with predetermined dimensional relationships, as well as coatings and films, characterized is not removed from the volume of the composition, and they turn into polymeric material in the curing process of curing. In the presence of pre-dissolved fluoro process proceeds according to the mechanism of heterogeneous copolymerization, when at a certain conversion of the monomer forming the copolymer or homopolymer is allocated in the form of globular formations in the matrix of the fluoroelastomer made. Upon further curing of the total volumetric shrinkage of the reaction mass is reduced, apparently due to local shrinkage in muggleborns space, which can concentrate phase fluoro. In addition, certain can contribute to the formation of microposts in the interfacial regions, for example due to the loose packing of the particles of the new phase. Coatings and films prepared at room temperature, have less internal stresses in comparison with similar products, otverzhdennye at elevated temperature.

To translate ftorkauchukov in the solution according to the invention using an alkyl(meth)acrylic monomers, which are the "best" solvents that are compatible with fluorine-containing polymers and capable of dissolving the latter at certain temperatures and time conditions with education the mi ratios, represent a relatively low viscosity of the system and easily processed into products, coatings and films by the method of svobodnislovo molding with simultaneous copolymerization of the components of the composition at room temperatures.

The possibility of transition from formautonomie solution to solid verkaufsstellen it is the composite at room temperature is due to the fact that the composition further comprises a polymerization activators of the type of tertiary aromatic amines (for peroxide initiators) or salts of metals of variable valency (in cases where hydroperoxide initiators) as activators. In combination with activators peroxides and hydroperoxides are able to initiate reaction of Homo - and graft polymerization at room and moderately elevated temperatures due to the low activation energy of formation of initiating radicals. Changing the ratio and nature of the components, it is possible to adjust the speed of the curing process, as well as the properties of the final copolymers.

In the proposed method as alkyl(meth)acrylic monomers are used esters of acrylic and methacrylic acid, namely methyl acrylate (MA), acrylate (Omarov are dissolving ability in relation to perkowska, volatility, activity in the reactions of Homo - and graft polymerization, and the generation of heat during polymerization.

By solving ability (the dissolution rate of a fixed amount of fluoroelastomer made at a certain temperature) is used, the monomers are not significantly different. On the basis of butyl ester of (meth)acrylic acid having a high molecular weight and their own original viscosity, produces solutions with a high prevalence of dynamic viscosity and with the worst turnover compared to methyl and ethyl homologues.

Esters of acrylic acid (MA, EA, BA) are characterized, on the one hand, a lower boiling points and thus have a higher volatility and a sharp odor. With other more active in the polymerization compared with esters of methacrylic acid, and also have a higher teploobrazovaniem. These factors are important when carrying out the process in the mass, as the increased speed and excess heat can lead to local overheating, the formation of pores and other negative phenomena.

In connection with the above in General, the most preferred is the use according to the specific conditions of obtaining products, coatings or films (ambient temperature, the efficiency of the heat sink and others) it is advisable to use alkylacrylate and/or additives.

Using oligopyrroles different functionality type TGM-3, MGF-9, MDF-2, etc. is determined by the possibility of additional modification of the material by obtaining crosslinked, branched structures with a large number of gel-fraction, which accordingly affects the properties of the obtained materials.

To ensure the possibility of obtaining coatings and films from verkaufsmanager compositions at room temperature in the invention is provided the use of a solution of paraffin in toluene as component, reducing the inhibiting effect of oxygen and prevent the surface stickiness of the coating or film products. The introduction of such additives is due to the fact that the polymerization of the monomers by radical-chain mechanism can also be inhibited by oxygen. This is especially true when carrying out the process at low temperatures in relatively thin layers, i.e., at large values of the surface reaction system to its volume. Sleds the block or at an elevated temperature, when this effect largely disappears. Paraffin does not combine with the components of the composition and therefore migrates to the surface of the cast film products, forming a protective layer, which limits the contact with oxygen. Due to this hardening is not significantly inhibited in the surface layers of the coating. The quantity and concentration of the solution of paraffin in toluene is traditional compositions, cured by polymerization mechanism for the formation of a continuous thin protective layer. If necessary it can be removed from the surface after curing curing by dissolving or mechanically.

In accordance with the invention as silicone elastomer used is a copolymer of vinylidenefluoride with HEXAFLUOROPROPYLENE (fluoropolymer elastomer SCF-26) or a copolymer of vinylidenefluoride with Cryptosporidium (fluoropolymer elastomer SCF-32). The claimed ratios allow to achieve on the basis of these ftorkauchukov in combination with the alkyl(meth)acrylic monomers and oligopyrroles homogeneous solutions of different viscosity, capable of svobodnaia formation. When the content of ftorkauchukov relative to the monomers is less than zapatergenoa the resulting material is characterized by low level of heat and wear resistance, and resistance to corrosive environments and high volumetric shrinkage due to the small fraction of the matrix fluoroelastomer made. When using ftorkauchukov more than the declared value, the solutions differ loss svobodnovihrevym properties and fluidity. Further increase in the content of SCF-26 and SCF-32 (50 wt.% or more) leads to the formation of swollen, high-viscosity systems are not suitable for use on svobodolyubivoi technology. Therefore, such systems are not illustrated examples.

As the polymerization initiators used hydroperoxides and peroxides. For example, of cumene hydroperoxide (gitaris), tert-butylhydroperoxide, benzoyl peroxides (PB) and lauroyl (PL), methyl ethyl ketone peroxide (PMAC) and others.

These initiators are used in combination with activators of polymerization, which allows to carry out the process at room temperature. As such can be used tertiary aromatic amines, in particular dimethylaniline (DMA) and dimethylacetamide (DMPT) in combination with the initiators of the peroxide number. To activate the decomposition of hydroperoxides in the redox reaction, preferably the use of salts of metals of variable valence is ritel, representing a 0.6% solution of vanadium pentoxide in acidic phosphate.

The number of initiators and activators is also traditional and due to the following factors. When initiating polymerization process at temperatures of about room through the use of systems initiator - activator, the amount of generated radicals is much less than the same amount of initiator undergoing homolytic decomposition at elevated temperatures. This reduces the overall efficiency of initiation. In this regard, to ensure an acceptable time curing conditions verkaufsmanager compositions require higher initiator concentration compared to termokataliticheskikh. When the content of the initiators of up to 1 wt. hours per monomer compositions inherent low curing rate (especially in the presence of inhibitors). The speed of the process begins to significantly increase only with the introduction of, for example, the IB is more than 1 wt.h. in combination with equimolar amount of activator (DMA).

When curing curing in the presence of initiators in amounts of more than 3 wt.h. (100 wt.h. monomer) of the reaction mixture quickly which reaches boiling point of the alkyl(meth)acrylic monomer. The vapour pressure of the monomer in the volume caused by overheating, creates internal stresses in the composite, which lead to cracks, pores and receiving substandard products.

Thus, the result of the above, it is possible to expand the range and applications of compositions based on ftorkauchukov by developing a method of obtaining compositions with variable viscosity, fluidity, ability to svobodnaia the molding and curing the curing of the mass that can be obtained from solutions of fluoro monomers in bulk products in the unit, as well as the films and coatings of greater thickness at room temperature.

The method is as follows.

1. Preparation of the solution of fluoro monomers in.

Fluoropolymer elastomer SCF-32 or SCF-26 mixed with the alkyl(meth)acrylic monomer with copolymerizes with him oligopyrroles taken in a weight ratio of(0,85-0,97): (0,15-0,03), in General the weight ratio of fluoropolymer elastomer : monomers (0.1 to 0.4): 1. At room temperature and periodic stirring, dissolve fluoroelastomer with homogeneous solutions of different viscosities.

2. Receiving from solutions of bulk products.

3. Coatings of verkaufsmanager compositions.

For the formation of coatings, for example, on metal substrates prepared as shown above composition is applied svobodnovihrevym method on the surface of the substrate and carry out a polymerization curing directly on the substrate without heating and without the use of an intermediate adhesive sublayers and adhesives.

4. The manufacture of films from solutions of verkaufsmanager.

The prepared composition was poured into a polyethylene, Teflon, glass, or other forms and carry out the formation of a film with simultaneous copolymerization in bulk at room temperature. The film thickness calibrated Kolichestvennaya is illustrated by the following examples.

Example 1. Take 97 g of methyl methacrylate and combined with 3 g of oligoadenylate brand TGM-3. On 100 wt.h. monomers add 10 g of silicone elastomer SCF-32. With periodic stirring to obtain a homogeneous solution. Determine the time for complete dissolution of the rubber and the dynamic viscosity of the solution using a rotational viscometer "Polymer RPE-1M" at different shear rates.

Example 2. Unlike example 1 take 20 g of the silicone elastomer SCF-32 (average content) and dissolved in a mixture of monomers consisting of 91 g of MMA and 9 g TGM-3 (medium dosage of the mixture of monomers). The method of solution preparation and test methods analogous to example 1.

Example 3. Prepare and analyze a solution analogously to example 1. However, the content of fluorine is increased to 40 g, and combines it with a mixture of MMA and oligoadenylate TGM-3, taken in an amount of 85 g and 15 g, respectively.

Example 4. In contrast to examples 1-3 linkage fluoro SCF-32 is 7 g (overseas ratio minimum dosage fluoro). Conditions for obtaining of the solution and its tests similar to example 1.

Example 5. Use the amount of fluorinated rubber and monomers as in example 2. Instead of rubber SCF-32 use rubber SCF-26. Prepare the However, the content of oligoadenylate TGM-3 is 1 g (overseas dosage minimum value).

Example 7. Take 40 g of rubber SCF-32, and dissolve it in a mixture of MMA and TGM-3, taken in an amount of 80 g and 20 g, respectively (overseas ratio on the maximum content of oligoadenylate TGM-3).

Example 8. Take 50 g of silicone elastomer SCF-26 and combine it with 50 g of methyl methacrylate (prototype). Explore verkaufsmanager mixture according to example 1.

Properties of solutions are given in table 1.

The examples illustrate the influence of the type and quantity of silicone elastomer on the dissolution rate and the viscosity of the obtained solutions. These indicators copolymers vinylidenefluoride with Cryptosporidium significantly differ from the copolymers with HEXAFLUOROPROPYLENE (SCF-26). Under other equal conditions the rubber SCF-26 is characterized by a slower rate of dissolution and forms monomers more viscous solutions. Using the mixture of monomers in a ratio of 0.8: 0.2 in the presence of ftorkauchukov formed inhomogeneous solutions with visible phase boundary (example 7).

Due to the fact that the description of the application under the patent prototype not the data on the viscosity of the claimed systems in the specified proportions, was reproduced in the same conditions tested, the composition is owned, which is closest to the ratios according to the invention. Tests showed that the test composition is a swollen mass of highly viscous, do not have svobodnovihrevye properties.

Example 9. Receive bulk products.

Use solutions according to examples 1-6, which add initiator, for example, of cumene hydroperoxide (gitaris), in the amount of 2 wt.h. in the calculation of the monomers and the mixture is stirred for 1-3 minutes. Then impose additional activator - 4 wt.h. of cobalt naphthenate or 0.5.h. vanadium accelerator also based on the monomers. Add a 10% solution of paraffin in toluene in an amount of 0.4 wt.h. from the total weight of the composition and produce stirring. By free fill fill composition dishes for based and hydrostatic determine shrinkage, volumetric shape in the form of bars for evaluating the impact strength according to GOST 19109-84, samples to determine the deformation resistance according to GOST 15088-83 and hardness according to GOST 24621-81, and resistance to aggressive media in accordance with GOST 12020-90. Carry out the polymerization of the components in the mass at room temperature for 24 hours. For hardened is) and measure its mass in the dry state. The percentage of gel fraction is determined by the formula:

Gf=[(a-b)100]/q,

where q, a and b is a mass of polymer tubes with gel-fraction and an empty tube, respectively.

In addition, determine the melt flow index (MFR) at 200oWith and a load of 5 kgf/cm2. Material properties are shown in table 2.

The data in table 2 indicate that when the content of fluorine is less than 10 wt.h. on 100 wt.h. monomers (composition-based solution with overseas ratio example 4) sharp reduction of complex material properties. Therefore, the use of such a large number of fluoroelastomer made is impractical. In General, the preferred compositions with a high content of the matrix polymer and oligoadenylate, which decisively affect the properties of the final products. With the increase in the number tetrafunctional of oligoadenylate solubility of solidified samples is reduced, due to more intensive branching and crosslinking of macromolecules. Modifying influence is manifested in the increase of the content of the gel fraction, which increases heat resistance and hardness, but leads to a decrease of the show is Holocene coatings on the metal base svobodnovihrevym applying and curing curing directly on the substrate to prepare a solution, for example, in accordance with example 2. Add gitaris in the amount of 3 wt.h. based on the monomers. After stirring enter 6 wt.h. activator of cobalt naphthenate and again mix. Pour the liquid composition on the precleaned (sandblasting or otherwise) of the metal substrate, made of steel-3. After spreading of the composition on the surface of the formed coating is applied evenly 10% solution of paraffin in toluene in the amount of 2 wt. hours from the total weight of the composition. Will polimerizuet composition and simultaneously form a coating thickness of 2-3 mm at 20oC for 20-24 hours. Experiencing the coating material adhesion to metal according to GOST 209-75, water absorption according to GOST 4650-80, deformation resistance, and the hardness and wear resistance according to GOST 11012-69. Properties of the coating material are shown in table 3.

Example 11. Fabrication of films.

For the manufacture of film materials from verkaufsmanager compositions are used, for example, the solution of example 5, into which enter the benzoyl peroxide in the amount of 2 wt.h. the number of monomers. By mixing dissolve it and evenly distribute the volume of the composition. Add to 0.7 wt.h. the activator.h. of the total composition and produce mixing. A liquid composition is poured, for example, on a plastic surface, bounded by a shoulder 2-4 mm. Form a film of the required thickness in the process of copolymerization components of the solution at the temperature and time conditions similar to example 10. Determine water absorption, heat resistance, thermal stability, aggression stability, tensile strength according to GOST 11262-80, hardness and wear resistance. Material properties are given in table 3.

See the description of the invention examples and General comparative analysis tables 1-3 indicate the effectiveness of the implementation of the method based on verkaufsmanager compositions of the claimed ratios for the manufacture of bulk products, coatings and films by the method of free casting with simultaneous copolymerization in bulk at room temperature. Technological advantages of the method and the level achieved properties of hardened materials determine the solution of tasks and achievement of the technical result according to the invention.

The method of obtaining products, coatings and films from the composition based on silicone elastomer by dissolving in a mixture of alkyl(meth)acrylic monomer and the copolymer is accordance initiator and activator of polymerization and the formation, characterized in that the silicone elastomer used is a copolymer of vinylidenefluoride with Cryptosporidium brand SCF-32, or a copolymer of vinylidenefluoride with HEXAFLUOROPROPYLENE brand SKF-26 as an initiator is a peroxide or hydroperoxide initiator, an activator - tertiary aromatic amine or a salt of a metal of variable valence and additionally use a solution of paraffin wax in an organic solvent, and shaping is done by the method of free casting simultaneously with the copolymerization at a mass ratio of the alkyl(meth)acrylic monomer and oligoadenylate(0,85-0,97): (0,03-0,15) and the mass ratio of the silicone elastomer and a mixture of alkyl(meth)acrylate and oligoadenylate (0.1 to 0.4): 1.

 

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