Resin composition of thermosetting resin and thermoplastic resin

Abstract: The resin composition which contains thermosetting resin as Component (A), a thermoplastic resin as Component (B), and at least one compound selected from the group consisting of an epoxy resin capable of dissolving the thermoplastic resin and a reactive diluent possessing at least one epoxy group as Component (C) in a ratio such that the proportions of Components (A), (B), and (C) fall respectively in the ranges of 30 to 96% by weight, 2 to 50% by weight, and 2 to 49% by weight, based on the total weight of the resin composition. The resin composition is capable of producing a molded article combining the highly satisfactory mechanical and thermal properties of a thermosetting resin and the highly satisfactory toughness of a thermoplastic resin.

Description: FIELD OF THE INVENTION This invention relates to a resin composition which uniformly contains a thermosetting resin and a thermoplastic resin and permits production of a shaped article combining highly desirable mechanical and thermal properties of the thermosetting resin and highly desirable toughness of the thermoplastic resin. BACKGROUND OF THE INVENTION In recent years, shaped articles of thermosetting resin and composite materials using matrices of thermosetting resin have been finding extensive applications in the general industrial field and the electric field because they exhibit higly desirable dimensional stability, heat resistance, mechanical properties, chemical resistance, and weather proofing properties. Such molded articles of thermosetting resins have low toughness and impact resistance due to the low elongation and brittleness of the resin. Thus, improvement in these properties have been desired. In order to improve the toughness and impact resistance of molded articles of thermosetting resins, a rubber component, plastic resin component or a filler have been incorporated into the thermosetting resins. In the case of incorporation of the rubber component into the thermosetting resin, however, since the rubber component impairs the heat resistance and mechanical properties of the molded article in spite of its ability to improve the toughness and impact resistance of the molded article, the amount of the rubber component is limited. In some applications, it is incorporated into the thermosetting resin only in a low ratio and consequently has an insufficient effect in improving the desired properties. When the thermosetting resin is mixed with a thermoplastic resin, the thermoplastic resin is added to the thermosetting resin as fine powder, or the thermoplastic resin is dissolved in a solvent and subsequently the thermosetting resin is added to the resultant solution (mixture). When the thermoplastic resin is added to a thermosetting resin in a finely divided form, the produced composition lacks homogeneity, and tends to degrade the mechanical properties of the molded article obtained therefrom. When the mixing is effected with the aid of a solvent, the method has the disadvantage that the removal of the solvent from the produced composition is required; the procedure for the production of the composition is troublesome; and the solvent remaining in the produced composition in a minute amount impairs, for example, the heat resistance of the molded article. SUMMARY OF THE INVENTION An object of the invention is to provide a resin composition which is free from the disadvantages mentioned above and which is produced homogeneously and easily by mixing a thermosetting resin and a thermoplastic resin in the absence of a solvent. A further object of the invention is a resin composition that permits production of a molded article excelling in heat resistance and in mechanical properties such as toughness and impact resistance. Additional objects and characteristics of the present invention will become apparent from the following disclosure of the invention. It has now been found that these and other objects of the invention can be attained by a resin composition comprising (A) at least one thermosetting resin (hereinafter called "Component (A)"); (B) at least one thermoplastic resin (hereinafter called "Component (B)"); and (C) at least one compound selected from an epoxy resin capable of dissolving the thermoplastic resin and a reactive diluent possessing at least one epoxy group (hereinafter called "Component (C)"); characterised in that the proportions of Components (A), (B) and (C) fall respectively in the ranges of 30 to 85% by weight, 10 to 30% by weight, and 5 to 49% by weight, based on the total weight of Components (A), (B) and (C), in that the weight ratio of Component (B) to Component (C) is not more than 2, in that Component (A) is at least one resin selected from a bisphenol A type epoxy resin, a urethane modified bisphenol A type epoxy resin, a novolak type epoxy resin, a cresol-novolak type epoxy resin, a glycidyl amine type epoxy resin and a bismaleimide resin, in that Component (B) is at least one resin selected from a polycarbonate, a polyether ketone, a polysulfone, a polyether sulfone, a polyether imide and an aromatic polyester, and in that Component (C) is at least one epoxy compound selected from a glycidyl ester type epoxy resin, glycidyl aniline, diglycidyl aniline, glycidyl toluidine, diglycidyl toluidine, diglycidyl ether, butane diol glycidyl ether, 2-glycidyl phenyl glycidyl ether, resorcinyl-diglycidyl ether, an alkylphenol glycidyl ether, phenyl glycidyl ether, butyl-glycidyl ether, cresol-glycidyl ether, styrene oxide, hexanediol diglycidyl ether and polypropyleneglycol diglycidyl ether. DETAILED DESCRIPTION OF THE INVENTION Since during the course of the production of the resin composition, Component (C) dissolves Component (B) and it further functions as a medium between Component (A) and Component (B), the production process is easy to carry out and the thermosetting resin and the thermoplastic resin are homogenously mixed without the use of a solvent. The molded article obtained from the resin composition, therefore, retains the outstanding mechanical properties inherent in the thermosetting resin component and, at the same time, acquires a notable improvement in toughness and consequently in impact resistance. Examples of a glycidyl amine type epoxy resin in Component (A) include a tri- or tetra-glycidyl amine type epoxy resin. Examples for each type of epoxy resin are shown in Table 1 below. One resin or a mixture of two or more resins described above may be used. The commercially available bismaleimide resins include, for example, the product of Mitsubishi Gas Chemical Ltd. marketed under the trademark designation of "BT Resin" such as "BT-2160L", "BT-2160", "BT-2164" and "BT-2170" (these resins are reaction products of 2,2-bis(cyanatophenyl)propane and bis(4-maleimidophenyl)-methane) and the product of Boots Technochemie marketed under the trademark designation of "Compimide" such as "Compimide H-800". As Component (A), it is possible to use in combination two or more different resins selected from the same type or different types, such as, for example, the combination of an epoxy resin and a bismaleimide resin, to suit the particular application. In the present invention, polycarbonate, polyester, polyether sulfone, polyether imide, and aromatic polyester are preferred for Component (B) since they are easily dissolved in Component (C) to form a homogeneous mixture. Optionally, two or more of the specified thermoplastic resins may be used in combination for Component (B). The thermoplastic resin as Component (B) is preferably used in the form of particles having diameters of not more than about 400 µm, preferably not more than about 100 µm. Further, it preferably has a glass transition temperature of not less than about 100°C, from the standpoint of heat resistance. A typical example of the glycidyl-ester type epoxy resin for Component (C) is the product of Shell Chemical Co. marketed under the trademark designation of "Epikote 191". Two or more of the specified epoxy resins and/or reactive diluents may be used in combination for Component (C). The epoxy resin and/or reactive diluent to be used as Component (C) preferably has a viscosity of not more than about 150 poises at 25°C. Generally, Component (B) and Component (C) are appropriately selected such that the latter component is able to dissolve the former component at a lower temperature than the curing temperature of the resin composition. If this relationship is not satisfied, the resin composition produced will lack the homogeneity required, and the advantages of this invention will not be attained. Example of preferred combinations of Component (B) and Component (C) are as follows. Component (B) Component (C) PES GAN, GOT, PGE, GE, HGE, PPG PEI GAN, GOT, PGE, HGE, PPG PSu GAN, GOT, PGE, BGE, HGE, PPG PC GOT, PGE, BGE, HGE (Note) PES: Polyether sulfone (e.g., VICTREX: product of Imperial Chemical Industries Co.) PEI: Polyether imide (e.g., ULTEM: product of General Electric Plastics) PSu: Polysulfon (e.g., Udel: product of Union Carbide Co.) Pc: Polycarbonate (e.g., Panlite: product of Teijin Kasei Co.) GAN: Glycidyl aniline GOT: Glycidyl toluidine PGE: Phenyl glycidyl ether BGE: Butyl glycidyl ether GE: Glycidyl ester type epoxy resin (e.g., Epikote 191: product of Shell Chemical Co.) HGE: Hexanediol diglycidyl ether PPG: Polypropylene glycol diglycidyl ether It is preferred to use a bismaleimide resin comprising a bismaleimide and a biscyanic acid ester, as Component (A). The bismaleimide is preferably a compound represented by the following formula (1) or a prepolymer derived from the compound alone or derived by addition reaction of a compound such as amine to the compound: wherein R 1 represents a divalent aromatic or aliphatic group, and X 1 and x 2 , which may be the same or different, each represents a hydrogen atom, a halogen atom or an alkyl group. Examples for each aromatic and aliphatic group includes, diphenylene ether and diphenylene methane. Examples for each halogen atom and alkyl group includes chlorine atom and methyl, respectively. The prepolymer is obtained by a heat-reaction of a bismaleimide under the presence of a catalyst, if desired. The reaction may be conducted under the presence of a compound having at least one amino group, such as triethylene diamine and 2-methyl imidazole. The reaction is conducted until the viscosity of the reaction product becomes from 10 to 1000 poise at 25°C. The biscyanic acid ester is preferably selected from the group consisting of a cyanic acid ester represented by the following formula (2) and a prepolymer derived from the cyanic acid ester. R 2 (O-C=N) 2 wherein R 2 represents a divalent aromatic group, n is an integer of from 2 to 10, and -O-C=N bonds directly to the aromatic ring group represented by R 2 . Examples for R 2 include diphenylene propane. Component (A) containing the bismaleimide resin further may contain an epoxy resin, preferably in an amount of from about 5 to 50 weight% based on the total weight of Component (A). In the combination of Component (A)/ Component (B)/Component (C), for the purpose of simplifying the procedure for providing the resin composition, it is desirable to dissolve Component (B) initially in Component (C) and subsequently to add Component (A) to the resulting solution. These three components may be mixed simultaneously. The weight ratio of Component (B)/Component (C) is not more than about 2. If this ratio exceeds about 2, the produced composition possesses a viscosity so high as to make its handling difficult and, when it is used as a prepreg, entails a disadvantage that its ability to impregnate fibers is lowered and its tackiness is insufficient. Moreover, the molded article obtained from the composition has inferior mechanical properties. The necessary amount of Component (C) is determined depending on the amount of Component (B), and it is preferably restricted to the smallest allowable level at which the produced resin composition has the desired homogeneity. The resin composition of the present invention, depending on the purpose, the use, and the conditions of use, may have incoporated therein a reinforcing material such as reinforcing fibers, for example, glass fibers, carbon fibers, aromatic polyamide fibers, or metal fibers in addition to the essential components thereof mentioned above. A mixture of these two or more type of fibers may be used. The reinforcing fibers preferably have a tensile strain of at least about 1.3%. Usually glass fibers and aromatic fibers have a tensile strain of at least about 2.5%. When carbon fibers having a tensile strain of less than about 1.3% are used, a cured composite having insufficient impact resistance is obtained. In order to obtain a composite having a high mechanical properties, it is preferable to use carbon fibers having a tensile strength of at least about 400 kgf/mm 2 and a tensile modulus of elasticity of at least about 30,000 kg/mm 2 . The reinforcing fibers usually are used up to about 70 volume% based on the total volume of the resin composition (including fibers). It may further optionally have incorporated therein, for example, a material which increases the toughness of the molded articles, such as butadiene-acrylonitrile rubber, a flame-retardant such as antimony trioxide, a filler such as powdered silica, a coloring agent. These additive materials are incorporated in the composition in an amount up to about 7.03% by weight based on the weight of the total weight of the composition (including the additive materials). Some of the resins used in this invention require use of a curing agent and a curing accelerator and others are of a kind not requiring these agents. Thus, these agents may be suitably selected as occasion demands. As a curing agent, and a curing accelerator, materials which are conventionally used for such purposes can be used in the present invention. A curing agent for an epoxy resin and a curing accelerator for other thermosetting resins are typically used in amounts of from about 25 to 45% by weight and 0 to about 3% by weight, respectively, based on the total weight of Components (A), (B) and (C) in the composition. Examples of a curing agent for an epoxy resin include an aromatic amine such as m-phenylene diamine, diaminodiphenyl methane, diaminodiphenyl sulfone, and m-xylene diamine; a boron trifluoride complex such as BF 3 monoethylamine and BF 3 benzylamine; an acid anhydride such as phthalic acid anhydride, trimellitic acid anhydride, pyromellitic acid anhydride, and benzophenone, tetracarboxylic acid anhydride; an imidazole such as 2-ethyl-4-methylimidazole, 2-ethylimidazole, 2,4-dimethylimidazole, and 2-phenylimidazole, dicyandiamide, and a dibasic acid dihydrazide. Two or more curing agent may be used in combination. Examples of a curing accelerator include a urea compound such as 3-(3,4-dichlorophenyl)-1,1-dimethyl urea, an organic metal salt such as Co(III) or Fe(III)acetylacetonate, a peroxide such as dicumyl peroxide, and an imidazole compound such as 2-ethyl-4-methylimidazole and 2-phenyl-4-methyl-5-hydroxymethylimidazole. A curing accelerator may be used in combination with a curing agent. The resin composition of the present invention can be prepared, for example, by a method described below. All of the components are supplied to a kneading device and kneaded therein usually under application of heat, desirably in an atmosphere of inert gas. The heating temperature used in this case is lower than the temperature at which the thermosetting resin begins to cure. Alternatively, for example, Component (B) can be dissolved in Component (C) and subsequently the resultant solution is kneaded with Component (A), when necessary, in combination with a curing agent. These steps are carried out generally at a temperature in the range of from about 20° to 200°C, preferably at a temperature in the range of from about 50° to 150°C, for 0.5 to 5 hours. When a prepreg is formed by impregnating reinforcing fibers with the resin composition of the present invention, the impregnation can be carried out by the conventional hot melt method which is disclosed in, for example, U.S. Patent Application Serial No. 761,290. In the hot melt method a fiber strand or fabric is impregnated with a resin composition, the viscosity of which is decreased by heating to a proper temperature (not higher than the curing temperature of the resin composition) so that impregnation can be conducted. The impregnation is conducted by dipping a fiber strand or fabric into the resin composition, or by placing fiber strands or a fabric in contact with a film of the resin composition and heat-pressing them. Thus a prepreg having reinforcing fibers therein is produced, and it is used for preparation of a molded article (composite) by curing the resin composition. For forming the resin composition of the present invention to a molded article, any conventional method can be used including thermal curing, ultraviolet curing, electron beam curing, and curing by the use of water. The appropriate combination of production method and curing method can be easily selected, depending on the particular kind of the thermosetting resin being used in the resin composition. Since Component (C) dissolves Component (B) and the mixture of Component (C) and Component (B) missible with the thermosetting resin Component (A), a homogeneous mixture of the three components is obtained. Moreover, the resin composition does not require a solvent and, therefore, does not have the disadvantageous of a residual solvent. It is a highly satisfactory resin composition combining highly desirable heat resistance due to the thermosetting resin and highly desirable toughness and impact resistance due to the thermoplastic resin. In some cases Component (B) precipitates in the form of fine particles when the homogeneous mixture of Component (B) and Component (C) is mixed with Component (A). Of course, even in this case, the three components are mixed with much higher homogeneity than when Component (A) and Component (B) are merely mixed with each other. The resin composition, in the form of either simply molded articles or molded articles made of composite material consisting of the resin composition and reinforcing fibers, will find extensive applications, for example, in the electric field, the medical field, the space and aeronautic field, the civil engineering and construction fields, and the general industrial field. Now, the present invention will be described more specifically below with reference to working examples and comparative experiments, but the present invention is not to be construed as being limited thereto. In Examples and Comparative Examples, all parts percents and ratios, including the mixing ratio of materials used in a resin composition, are by weight unless otherwise specified. In the Examples and Comparative Examples, the glass transition temperature was measured using a differential scattering calorimeter, and fracture toughness was measured by the double cantilever tear test (ASTM D3433-75). Examples 1-5 Various epoxy resins were used as Component (A). Components (A), (B), and (C), varying in kind and mixing ratio from one combination to another as indicated in Table 2, were weighed out and placed in a beaker. In the beaker, they were stirred and heated at 110°C for one hour to produce a homogeneous mixture of Components (A), (B), and (C). Then, this mixture and an epoxy resin curing agent such as diaminodiphenyl sulfon added thereto were heated and mixed at 100°C for one hour to produce a thermosetting resin composition. This composition was placed in a silicone rubber mold and cured therein at 180°C for two hours under application of pressure (5 kg/cm 2 ), to obtain a cured article made of the resin composition. A test piece was cut from the cured article and tested for glass transition temperature, fracture toughness, and Izod impact energy. The results are shown in Table 3 below. Comparative Examples 1-7 Resin compositions were produced by following the procedure of Examples 1 to 5, except that only Component (A) was used (Comparative Examples 1-5); Component (B) was omitted (Comparative Example 6); and a butadiene-acrylonitrile rubber (product of Ube Industries, Ltd. marketed under trademark designation of "CTBN, Hycar 1300×13") was used in the place of Component (B) (Comparative Example 7). The resin compositions were similarly processed to produce cured articles, which were tested for the same physical properties. The results are shown in Table 3. From the results, it is clear that the products of Examples 1-5 were superior to those of Comparative Examples 1-7 in terms of fracture toughness, and Izod impact energy. The product of Comparative Example 7 was satisfactory in toughness but was notably deficient in heat resistance. Examples 6-10 and Comparative Examples 8-12 Cured articles were obtained by following the procedures of Examples 1-5, except that a phenolic resin or bismaleimide resin shown in Table 4 below was used as Component (A). The resin compositions using the phenol resin were further post-cured by eight hours standing at 220°C. The cured articles were tested for the same properties as mentioned above. The results are shown in Table 4. From the results, it is evident that the products of Example 6-10 were superior to those of Comparative Examples 8-12 in terms of fracture toughness and Izod impact energy. Examples 11-15 and Comparative Examples 13-17 Resin compositions for prepregs were obtained by using the materials shown in Table 5 below as Components (A), (B), and (C) in mixing ratios shown in Table 5, to obtain homogeneous mixtures, and by incorporating curing promoters shown in Table 5 in amounts shown in Table 5. Resin films 60 µm thick were obtained from the thus-obtained compositions using a film coater. Carbon fibers ("Besfight IM-500", product of Toho Rayon Co., Ltd.) having a tensile strength of 500 kgf/mm 2 and a modulus of elasticity of 30,000 kg/mm 2 were placed on each film and the resin composition was impregnated therein by heating to a temperature of 100°C and pressing at 4 kg/cm 2 to obtain a unidirectional (direction of fibers) prepreg having a weight of 150 g/m 2 and containing 34% by weight of the resin. From each prepreg, necessary number of sheets were obtained by cutting, and they were laminated. The laminated product was heat-cured to obtain a molded plate by autoclave moIding at 180°C, 4 kg/cm 2 . Test pieces were obtained by cutting the plate, and the glass transition temperature, the interlaminar shear strength (ILSS; measured according to ASTM D2344 with respect to the fiber direction), the compressive strength (measured with respect to the fiber direction according to ASTM D3410), the damaged area resulting from an impact of 340 kgcm/cm and the compressive strength after the impact were measured. The test piece for subjecting the impact test was prepared by laminate 16 prepreg sheets in such a manner that directions of carbon fibers in the prepregs become 45°/0°/-45°/90°/90°/-45°/0°/45°/45°/0°/-45°/90°/90°/-45°/0°/45°. The results obtained are shown in Table 5. Comparative Examples 13-17 Comparative test pieces were produced in the same manner as in Examples 11-15 except that Component (B) or Components (B) and (C) were not used. The properties of the comparative test pieces were measured in the same manner as in Examples 11-15, and the results are shown in Table 5. As can be seen in Table 5, there were no remarkable differences between the thermal characteristics of the test pieces of Examples 11-15 and those of the Comparative Examples. However, the damaged areas caused by the impact were much smaller in the test pieces of Examples 11-15 than those of Comparative Examples 13-17, and the compressive strengths after impact were much higher in the samples of Examples 11-15 than those of Comparative Examples 13-17. These results demonstrate that the composites obtained from the composition of the present invention were superior to those of Comparative Examples 13-17 in impact resistance. Example 16 Using the materials and mixing ratios shown in Table 5 below, Component (B) was mixed with Component (C) at 110°C for one hour while stirring. To the above-described mixture, Component (A) and curing accelerator shown in Table 5 were added in the mixing ratio shown in Table 5, and the resultant mixture was mixed by using a roll mill to obtain a resin composition for a prepreg. Using this composition, a prepreg was produced in the same manner as in Examples 11-15, and a molded plate was obtained from the prepreg in the same manner as in Examples 11-15. The composite properties were measured in the same manner as in Examples 11-15, and the results are shown in Table 5. From the results it can be seen that the composite obtained from the composition of the present invention had excellent impact resistance. Examples 17-23 and Comparative Examples 18-22 The same experiments as in Examples 11-17 and Comparative Examples 13-17 were conducted except that materials and mixing ratios shown in Table 6 below were used. The results are shown in Table 6. From the results it can be seen that the composites obtained from the composition of the present invenion had excellent impact resistance.

Claims: A resin composition comprising (A) at least one thermosetting resin; (B) at least one thermoplastic resin; and (C) at least one compound selected from an epoxy resin capable of dissolving the thermoplastic resin and a reactive diluent possessing at least one epoxy group; characterised in that the proportions of (A), (B) and (C) fall respectively in the ranges of 30 to 85% by weight, 10 to 30% by weight, and 5 to 49% by weight, based on the total weight of (A), (B) and (C), in that the weight ratio of (B) to (C) is not more than 2, in that (A) is at least one resin selected from a bisphenol A type epoxy resin, a urethane modified bisphenol A type epoxy resin, a novolak type epoxy resin, a cresol-novolak type epoxy resin, a glycidyl amine type epoxy resin and a bismaleimide resin, in that (B) is at least one resin selected from a polycarbonate, a polyether ketone, a polysulfone, a polyether sulfone, a polyether imide and an aromatic polyester, and in that (C) is at least one epoxy compound selected from a glycidyl ester type epoxy resin, glycidyl aniline, diglycidyl aniline, glycidyl toluidine, diglycidyl toluidine, diglycidyl ether, butane diol glycidyl ether, 2-glycidyl phenyl glycidyl ether, resorcinyldiglycidyl ether, an alkylphenol glycidyl ether, phenyl glycidyl ether, butyl-glycidyl ether, cresol-glycidyl ether, styrene oxide, hexanediol diglycidyl-ether and polypropylene glycol diglycidyl ether. A resin composition as claimed in claim 1, wherein said glycidyl amine type epoxy resin is a triglycidyl amine type epoxy resin or a tetraglycidyl amine type epoxy resin. A resin composition as claimed in claim 1 or 2, wherein (B) is a polyether sulfone, and (C) comprises at least one compound selected from glycidyl aniline, glycidyl toluidine, phenyl glycidyl ether, a glycidyl ester epoxy resin, hexanediol diglycidyl ether and polypropylene glycol diglycidyl ether. A resin composition as claimed in claim 1 or 2, wherein (B) is a polyether imide, and (C) comprises at least one of glycidyl aniline, glycidyl toluidine, phenyl glycidyl ether, hexanediol diglycidyl ether and a polypropylene glycol diglycidyl ether. A resin composition as claimed in claim 1 or 2, wherein (B) is a polysulfone, and (C) comprises at least one of glycidyl aniline, glycidyl toluidine, phenyl glycidyl ether, butyl glycidyl ether, hexanediol diglycidyl ether and a polypropylene glycol diglycidyl ether. A resin composition as claimed in claim 1 or 2, wherein (B) is a polycarbonate, and (C) comprises at least one of glycidyl toluidine, phenyl glycidyl ether, butyl glycidyl ether, and hexanediol diglycidyl ether. A resin composition as claimed in any preceding claim, wherein (C) is present in an amount of from 5 to 30% by weight of the total weight of (A), (B) and (C). A resin composition as claimed in any preceding claim, further comprising a reinforcing fiber. A resin composition as claimed in claim 8, wherein said fiber is selected from a carbon fiber, a glass fiber and an aromatic polyimide fiber. A resin composition as claimed in claim 8 or 9, wherein the amount of said reinforcing fiber is up to about 70% by volume based on the total volume of said composition. A resin composition as claimed in any preceding claim, further comprising at least one additive selected from butadiene-acrylonitrile rubber, a flame-retardant, a filler, and a coloring agent. A resin composition as claimed in claim 11, wherein the amount of said additive is up to about 7.03 wt% based on the total weight of said composition. A resin composition as claimed in any preceding claim, further comprising at least one of a curing agent and a curing accelerator. A resin composition as claimed in claim 13, wherein the amount of the curing agent and the curing accelerator is 25 to 45% by weight and 0 to 3% by weight, respectively, based on the total weight of (A), (B) and (C). A resin composition as claimed in any preceding claim, wherein (A) comprises a thermosetting resin comprising a bismaleimide and a biscyanic acid ester. A method for producing a homogeneous resin composition comprising mixing (A), (B) and (C), characterised in that said (A), (B) and (C) are as defined in any preceding claim. A method as claimed in claim 16, wherein (B) is first dissolved in (C), and then the resultant solution is mixed with (A). A method as claimed in claim 16 or 17, wherein the mixing is conducted at a temperature in the range of from about 20 to 200°C.

Inventors: ANDOH MASATO, KOSUDA HIROYUKI, NAGATA YASUHISA, ANDOH, MASATO, KOSUDA, HIROYUKI, NAGATA, YASUHISA, ANDOH, MASATO TOHO RAYON CO. LTD., KOSUDA, HIROYUKI TOHO RAYON CO. LTD., NAGATA, YASUHISA TOHO RAYON CO. LTD.
Applicants: TOHO RAYON KK, TOHO RAYON CO., LTD.
Application year: 1987
Main classification: C08L63
IPC codes: C08L101, C08L63