Epoxy resin encapsulating composition with enhanced moisture resistance and method for producing the same

Abstract: An epoxy resin encapsulating composition for semiconductor packages consisting essentially of an epoxy resin adduct of epichlorohydrin and an aromatic hydroxyl-containing compound, and an inorganic ion-exchange solid material admixed with the epoxy resin adduct. The ion-exchange solid material is selected to have the capability of exchanging its mobile anions with the undesired chlorine ions which occur inherently in the package made from the encapsulating composition and are very likely to corrode the metallic conductor on the semiconductor to be encapsulated. The ion-exchange solid material is characterized to include antimony and bismuth as basic materials forming an ion-exchange network which carries the mobile anions to be substituted with the chlorine ions. This ion-exchange material also is found to be also effective for trapping undesired alkali metal ions, for example, Na⁺ which may be present in the composition itself or permeate in the packages made therefrom and also act to corrode the conductor. Preferred ion-exchange material for the epoxy resin encapsulating composition is found to be represented by the formula: SbBixOy(OH)z(NO₃)w·n(H₂O) in which x represents 0.2 to 2.0, y represent 1.0 to 5.0, z represents 0.1 to 3.0, w represents 0.1 to 3.0 and n represents 0.5 to 3.0.

Description: The present invention is directed to an epoxy resin encapsulating composition with enhanced moisture resistance for semiconductor packages and a method for producing the same. In recent years, there has been a growing demand for miniaturizing semiconductor packages in the form of, for example, a small outline package (SOP) and a flat package (FP) which are capable of being directly mounted on a circuit board by means of solder dip leads. In this direct mounting process, it is a standard industry practice to dip the entire package in a soldering bath and then place it on the circuit board for simultaneous soldering of the external leads to the corresponding lands on the circuit board. Due to this recent industry demand for dipping the entire package in the soldering bath prior to the mounting thereof, increasing emphasis is being placed on adding enhanced moisture resistance to an epoxy resin encapsulating composition for the semiconductor packages, or on utilizing the epoxy resin encapsulating composition which has an enhanced moisture resistance which remains intact even when it is dipped in the soldering bath, thereby subjecting it to the intense heat and vapor of the solder. Such enhanced moisture resistance is also required for the packages which are exposed in the actual operating condition to an elevated termperature environment. It is known that epoxy resins made from epichlorohydrin and an aromatic hydroxyl-containing compound inevitably contain a certain amount of undesirable by-products, in which the chlorines of the epichlorohydrin are coupled with certain epoxy groups of the resulting epoxy resin. This undesirable by-product is very likely to be hydrolyzed when exposed to heat in the presence of moisture and chlorine ions, which show strong corrosive action in the presence of moisture and eventually corrode the metallic conductor of the semiconductor, such as an aluminum conductor, so as to damage the semiconductor or to reduce the moisture resistance of the package. In order to avoid such unacceptable reduction in moisture resistance, attempts have been made to reduce the amount of by-product contained in the epoxy resin adduct. However, this approach involves complicated and difficult treatments which are not practically acceptable and do not assure complete removal of the undesired by-product. In this respect, the remaining by-product will act to lower the moisture resistance as it is hydrolyzed into the corrosion inducing ions when the package or epoxy resin encapsulating composition is subjected to heat and moisture at the soldering process or in a high temperature operating environment. Further, there is another problem, in that the package, when subjected to the soldering process, suffers from the permeation of the chlorine ions (Cl-) possibly contained in a flux employed in the soldering process, through a minute gap developed between the external leads and the molded composition, due to the heat stress applied thereto at the time of the soldering process. To this end, it is desirable to utilize a suitable ion exchanger which is capable of trapping the corrosion-inducing ions occurring in the package after the encapsulation from the standpoint of successfully preventing the lowering of the moisture resistance due to such undesirable ions. A composition using fillers such as antimony trioxide or antimony tetraoxide is disclosed in United States patent no. 4,042,550. It is an object of the present invention to provide an epoxy resin encapsulating composition with enhanced moisture resistance for semiconductor packages, which is capable of trapping the undesired chlorine ions (Cl-) and similar halogen ions occurring after the encapsulation, succesfully protecting the metallic conductor of the semiconductor encapsulated in the package from being corroded by the action of the undesired ions. According to a first aspect of the present invention, there is provided an epoxy resin encapsulating composition with enhanced moisture resistance for semiconductor packages, consisting essentially of the admixture of an epoxy resin adduct of epichlorohydrin and an aromatic hydroxyl-containing compound, with an inorganic ion-exchange solid material, said ion-exchange solid material being in the form of particles dispersed in the epoxy resin adduct and capable of exchanging its mobile anions with the chlorine ions which originate from the epichlorohydrin and occur in the epoxy resin adduct as a result of possible hydrolysis of the corresponding chlorides, said ion-exchange solid material being represented by the general formula: SbBixOy(OH)z(NO₃)w.n(H₂O) in which x represents 0.2 to 2.0, y represents 1.0 to 5.0, z represents 0.1 to 3.0, w represents 0.1 to 3.0 and n represents 0.5 to 3.0. Although the mechanism for the reaction is not fully understood by chemists, this particular inorganic ion-exchange solid material shows remarkable capacity for trapping and stably holding the undesired chlorine ions (Cl-) on its network, thus preventing them from reacting with the moisture present in the encapsulating composition and acting to corrode the aluminum conductor in the semiconductor package. Such undesirable chlorine ions (Cl-) in addition to resulting from the corresponding chloride with the certain epoxy groups in the epoxy resin itself, may enter from outside the package as they permeate from a flux employed in the soldering process, through minute gaps between the external leads of the package and the molded composition of the package, such gaps being developed while soldering, due to the difference in expansion coefficients between the leads and the molding material. The above inorganic ion-exchange material could, alternatively, trap the chlorine ions (Cl-) entering the package from outside. Other halogen ions such as bromine ions (Br-) which may be present in the epoxy resin composition as a result of brominating the epoxy resin for a flame retardation purpose, can also be effectively trapped by the inorganic ion-exchange material, so as to be prevented from acting to corrode the aluminum conductor, as in the case of the chlorine ions (CL-). According to a second aspect of the invention, there is provided a method of preparing an epoxy resin encapsulating composition, comprising the steps of mixing the particles of said ion-exchange material into the molten epoxy resin to provide a first mixture; kneading the resulting first mixture so as to disperse the particles of the ion-exchange material uniformly into the epoxy resin; cooling the first mixture to solidify said first mixture; milling the solidified first mixture to the corresponding powder; blending a curing agent for the epoxy resin with the powder of the first mixture to provide a second mixture; heating the second mixture to melt, thereby partially curing the epoxy resin; cooling the second mixture to solidify it; and grinding the solidified second mixture to produce the encapsulation composition in powder form. Preferably, 10 to 100 parts by weight of water is mixed into the molten epoxy resin adduct together with the particles of said ion-exchange material at the step of providing the first mixture in order to positively hydrolize the chloride attached to the molecules of the epoxy resin into chlorine ions and at the same time to trap the chlorine ions on the network of the ion-exchange material by exchanging the mobile anions on the network with the chlorine ions in the water solution, said ion exchange material being mixed in excess amount relative to the chlorine ions to be removed for leaving a sufficient amount of the mobile anion on the network for another ion-exchange reaction, the resulting first mixture being dewatered prior to milling the solidified first mixture. A novel epoxy resin encapsulating composition with enhanced moisture resistance for semiconductor packages in accordance with the present invention consists, essentially, of the admixture of an epoxy resin adduct of epichlorohydrin and an aromatic hydroxyl-containing compound, and an inorganic ion-exchange solid material in the form of particles dispersed in the epoxy resin adduct. The ion-exchange solid material is characterized to include antimony and bismuth as basic materials and is represented by the following formula: SbBixOy(OH)z(NO₃) w.n(H₂O) in which x represents 0.2 to 2.0, y represents 1.0 to 5.0, z represents 0.1 to 3.0, w represents 0.1 to 3.0 and n represents 0.5 to 3.0. Also incorporated in the admixture are a curing agent and optionally a cure accelerator, flame retardant, filler and mold release agent. Prepartion of the above composition can be made with any known procedures, for example, by blending suitable amounts of the ingredients of the composition in a suitable rotary mixture followed by kneading the resulting admixture, cooling it and therafter grinding it to powder. The epoxy resin applicable to the present invention can be selected from any normally used epoxy resins which are widely utilized to formulate the conventional molding compositions including cresol novolac and phenol novolac. Preferably, ortho-cresol novolac is utilized to obtain satisfactory moisture resistance which have epoxy equivalent weights of 180 to 220. The curing agent for the epoxy resin is also well known in the art and can be selected solely or in combination from the group consisting of amines; acid anhydrides such as maleic anhydride, succinic anhydride, phthalic anhydride, tetrahydrophtalic anhydride; and novolac type phenol resins such as phenol novolacs, cresol novolacs, tert-butyl phenol novolacs, and nonyl phenol novolacs. In view of improving the moisture-proof and molding characteristics, a preferred curing agent for the epoxy resins is found to be phenol novolacs or the combination of phenol novolacs and acid anhydrides. The cure accelerator which may be optionally employed comprise one or more of the conventional accelerator such as imidazoles, 1.8-diaza-bicyclo(5,4,0) undecene, salts thereof, and organic phosphines. Included in the imidazoles are, for example, 2-undecyl imidazole, 2-methyl imidazole, 1-cyanoethyl-2-ethyl-4-methyl imidazole, 2-phenyl imidazole, and 2-heptadecyl imidazole. Included in the salts of 1.8-diaza-bicyclo(5,4,0) undecene are those with phenoles, 2-ethylhexanoic acid, oleic acid, and acid carbonates. The flame retardants includes, for example, brominated epoxy resin, chlorinated paraffin, bromotoluene, hexabromobenzene, and antimony trioxide. Suitable fillers for the epoxy resin encapsulating composition are well known to be inorganic fillers such as fused silica powder, quartz glass powder, glass fiber, talc, alumina powder, calcium silicate powder, calcium carbonate powder, and barium sulfate powder. One or more kinds of the above fillers can be utilized in the present invention, and preferably fused silica powder is selected as exhibiting inherent low coefficient of heat expansion. The amount of such fillers to be incorporated will vary depending upon the kinds of the epoxy resins, curing agents, and the fillers employed. The size of the silica powder may be optionally chosen in such a manner as to improve the molding characteristics. Preferably, the silica powder is selected to have an average particle size of 10 to 30 µm. Similarly, suitable mold release agents applicable to the present encapsulating composition include carnauba wax, and similar natural or synthetic wax, metallic salts of straight-chain fatty acids, acid amides, and esters. The epoxy resin encapsulating composition may additionally include colorants such as carbon black and silane coupling agents. The above inorganic ion-exchange material employed in the present invention has a stable ion-exchange capacity at a temperature up to 400°C or more, which is much higher than the melting point of the epoxy resin as well as the temperature at which the package is soldered to a circuit board in an automated manner as to firstly dipping it in a soldering bath and placing it on the board. With this excellent stability against elevated temperature environments the ion-exchange material can successfully trap undesired ions which occur in the package or the encapsulating composition when exposed to the elevated temperature environments. By the undesired ions, herein are meant ions which, in the presence of moisture, are very liable to corrode a metallic conductor, for example, aluminum conductor of the semiconductor to be encapsulated by the composition. The undesired ions includes halogen ions such as chlorine ions Cl⁻ and bromine ions Br⁻, and alkali metal ions such as sodium ion Na⁺ and potassium ion K⁺. The chlorine ions Cl⁻ originate from the epichlorohydrin forming the epoxy resin and from a flux used for soldering the package. In fact, there are inevitably seen in the epoxy resin forming reaction that some chlorines of the epichlorohydrin are coupled with certain epoxy groups of the resulting epoxy resin which are readily hydrolized to liberate the chlorine ions Cl⁻ in situ when exposed to an elevated temperature environment or subjected to heat shock as applied, for example, at the time of dipping the package in the soldering bath prior to the soldering and in a high temperature operating condition. The bromine ions Br⁻ originate from the brominated cmpound, for example, brominated epoxy resin incorporated in the encapsulating composition for a flame retardation purpose. The sodium ions Na⁺ and potassium ions K⁺ may be present in the composition as originating from a corresponding alkali metal containing catalyst in the presence of which the epoxy resin is formed and/or may enter the composition as unavoidable impurities attendant with the silica particles to be incorporated in the composition. These undesired ions are trapped by the ion-exchange material of which hydroxly goups (OH)⁻ bonded to the positive site of the network thereof function as anion as well as cation exchanger as described hereinbefore. Although the exact reason is not clear, the nitrate ion NO₃ contained in the ion-exchange material is thought to act in association with hydroxyl group (OH)⁻ to enhance the ion-exchange capability and ion-exchanging rate thereof. In addition to this advantageous function, the ion-exchange material as defined above exhibits a superior characteristic that it firmly captures on the network thereof the undesired ions once trapped so as to prevent them from converting back into the liberated ions. The above superior characteristic is not expected from a conventional inorganic absorbent such as a metal oxides including as its basic constituents magnesium and aluminum, although it is known to capture the undesired ions to some extent. The ion-exchange material is admixed to the other ingredients in the form of particles to be uniformly dispersed in the composition. In this respect, the ion-exchange material is selected to preferably have an average particle size of not greater than 5 µm and a maximum particle size of not greater than 100 µm. When the average particle size is greater than 5µm, the ion-exchange capacity is not expected to increase in proportion to the increasing amount to be added. And when the maximum particle size is greater than 100 µm, the ion-exchange capacity is lowered with the decreasing specific surface area of the particle, in addition to that such greater particles are the cause of failing to uniformly disperse the particles in the composition, thus reducing the molding characteristic. In this connection, the maximum particle size of the ion-exchange material is preferably selected to be less than the average particle size of the silica incorporated in the composition as a filler in order to facilitate the uniform dispersion in the composition containing the silica particles. The present invention is further illustrated by way of the following Examples without being limited thereto and is evaluated through several test in comparison with the comparative examples. Firstly, tests were made for confirming the ion-exchange capability for several ion-exchange materials per se. The tested materials, as listed in Table 1, include those [A to I] characterized to contain antimony and bismuth as basic materials forming an ion-exchange network, a conventional ion-exchange resin [J] made of polystyrene having amino groups as ion-exchangeable anions, and inorganic absorbent material [K] of metal oxides containing as its basic constituents magnesium and aluminum. The tests were made with respect to: #1) ion-exchange capacity at 121°C; and #2) ion-exchange capacity at 121°C after being subjected to an elevated temperature of 350°C for 2 hours, which was intended to simulate the heat shock which will be applied to the materials when incorporated in the encapsulating composition. The ion-exchange capacity #1) of each material in Table 1 represents the amount of chlorine ions Cl⁻ remaining in water solution as being untrapped by the material. For this measurement, each ion-exchange or absorbent material was mixed in a 100 ml of water solution containing chlorine ion Cl⁻ in an amount of 100 ppm per unit gram of the material. The resulting water solution was heated to a temperature of 121°C for 20 hours and was thereafter measured by the ion-chromatograph analysis the amount [ppm] of the remaining ions present in the solution as being untrapped by the ion-exchange or absorbent material. The ion-exchange capacity #2) of each material was measured in the same manner except that it was exposed to an elevated temperature of 350°C for 2 hours prior to be mixed in the water solution containing the prescribed amount of the chlorine ion Cl⁻. In the following Table 2, Examples 1 to 15 and comparative examples 1 to 3 show the comparative results with and without the use of the individual ion-exchange or absorbent material listed in Table 1 for formulating corresponding epoxy resin encapsulation compositions. Each of the ion-exchange or absorbent materials (A to K) of Table 1 was admixed in the listed amount in Table 2 with the following ingredients to formulate the individual epoxy resin encapsulating composition (Examples 1 to 15, and comparative examples 1 to 3), all parts by weight: 160 parts of epoxy resin adduct of epichlorohydrin and ortho-cresole novolac [epoxy equivalent weight 195, softening point 75°C]; 90 parts of phenol novolac as curing agent [molecular weight 700, hydroxyl equivalent weight 700]; 3 parts of 2-undecyl imidazole as cure accelerating agent; 20 parts of brominated epoxy resin as flame retardant [epoxy equivalent weight 250, softening point 90°C]; 30 parts of antimony trioxide as flame retardant; 4 parts of carnauba wax as mold release agent; 4 parts of carbon black as coloring agent; and 640 parts of fused silica as filler [average particle size 20 µm] The resultant formulation of each composition was admixed to be thoroughly blended and kneaded while being heated to form a sheet product. The sheet product was then cooled to a room temperature and was ground to powder having a maximum particle size of 0.1 to 0.4 mm for preparing sample composition in powder form. For evaluation of the individual sample compositions, tests were made for each sample with respect to: #3) extract water analysis for evaluation of ion-exchange capacity; and #4) moisture resistance. With the extract water analysis #3), the ion-exchange capacity of each sample is evaluated in terms of the amount of the remaining ions Cl⁻ and Na⁺ left in the sample as a result of not being trapped by the ion-exchange material or absorbent contained in the sample composition. This test was made according to the following procedure. Each sample powder was heated at a temperature of 175°C for 5 hours to be completely cured. Then, the cured composition was ground to a particle size which passes through a 200 mesh (0.074 mm) screen powder. Subsequently, 5 g of the resulting minute sample particle or powder was placed in a flask together with 46 g of deionized water and with 4 g of methanol, which mixture was heated to a temperature 151°C for 100 hours. Thereafter, the aqueous mixture was extracted and was measured of the amount of Cl⁻ and Na⁺ ions left untrapped by ion-chromatograpy analysis. The measured amounts are listed in Table 2 in ppm. For evaluation of the moisture resistance #4), each sample powder was processed by transfer molding at 175°C at an injection pressure of 68.6 bars (70 kg/cm²) in 90 sec. to provide a sample package which was a small outline 18-lead semiconductor package [SOP] encapsulating a 2.3 x 3.2 mm semiconductor chip with a comb pattern aluminum conductor of 5 µm width formed thereon. The resulting package was after-cured at 175°C for 5 hours followed by being dipped for 10 seconds in a soldering bath maintained at 260°C after machining the solder dip leads into suitable shape for a subsequent automated soldering process on a circuit board. In the next step, a suitable number of the same sample packages thus treated were subjected to a pressure cooker test [PCT] at 151°C, 5 bars (5 atmospheric pressures), and a relative humidity [RH] of 100 % for different time intervals in order to determine the moisture resistance in terms of the elapsed time required to induce the corrosion of the aluminum conductor in 50% of the sample packages subjected to the pressure cooker test. Such corrosion is determined by the occurrence of open-circuit in the comb pattern aluminum conductor which was inspected by the use of a multi-pin electric metering device. CONCLUSIONS 1) It is apparent from the results of Table 1, that the conventional ion-exchange and absorbent materials (J,K) will completely or substantially lose its ion-exchange capacity after being heat treated only at an elevated temperature of 121°C and are therefore not expected to trap the undesired ions such as Cl⁻ and Na⁺ inherent to the epoxy encapsulating composition which will occur at an elevated temperature of 121°C or more, as confirmed from the results of Table 2 in which the moisture resistances of the packages (comparative examples 2 and 3) are lowered even as compared to the package without the ion-exchange material (comparative example 1). 2) In contrast to the above, the ion-exchange materials (A to I) exhibit an excellent ion-exchange capacity at the elevated temperature of 121°C and retain this capacity even after being exposed to a further elevated temperature, say 350°C, as apparent from the results of Table 1. In fact, each of the packages (Examples 1 to 15) obtained from the encapsulating composition including such materials exhibits an improved ion-exchange capacity as well as moisture resistance, as apparent from the results of Table 2. 3) Most remarkable results with respect to the moisture resistance are obtained with the packages (Examples 1 to 10, and 14), accordingly the encapsulating compositions thereof are most preferable for semiconductor packages requiring improved moisture resistance. Although the package (Example 14) shows the best result with respect to the moisture resistance with incorporation of a larger amount, say 12 parts, of the ion-exchange material (A), the addition of too much material may lead to lowering of the molding characteristics. In this connection, the addition of small amount, say 0.05 parts, of the ion-exchange material (Example 12) is not expected to drastically improve the moisture resistance, although it is within an acceptable level. Accordingly, the ion-exchange material is preferably added in the range of 0.05 to 12 parts to the epoxy resin composition formulated in the prescribed amount as listed hereinabove. Further, as seen from the results of Table 2, the moisture resistances of the packages (Examples 14 and 15 is rather lowered although within the acceptable level when the average particle size of the ion-exchange material is increased or when the proportion of particular component constituting the ion-exchange material is outside of the preferred range. All of the above demonstrate the superiority of the present invention which satisfies enhanced moisture resistance for semiconductor packages. In addition, there is another method of producing the epoxy resin encapsulating composition which is advantageous for further improving the moisture resistance. This method comprises the steps of mixing the particles of the ion-exchange material into the molten epoxy resin to provide a first mixture, kneading the resulting first mixture so as to disperse the particles of the ion-exchange material uniformly into the epoxy resin, cooling the first mixture to solidify, milling the solidified first mixture to the corresponding powder, blending a curing agent for the epoxy resin with the powder of the first mixture to provide a second mixture, heating the second mixture to melt for partially curing of the epoxy resin, cooling the second mixture to solidify, and grinding the solidified second mixture to produce the encapsulation composition in powder. At the step of providing the first mixture, a large volume of deionized water is mixed together with the particles of the ion-exchange material into the molten epoxy resin in order to positively hydrolyze the chloride attached to the molecules of the epoxy resin into the chlorine ion and at the same time to trap the same ions on the network of the ion-exchange material by exchanging the mobile anions on the network with the chlorine ions in the water solution. The ion-exchange material is mixed in excess amount relative to the chlorine ions to be removed so as to enable sufficient amount of the mobile anion remaining on the network for another ion-exchange reaction in a later stage. The resulting first mixture is dewatered prior to milling the solidified first mixture. With this method, it is possible to reduce the amount of the undesired chlorine ion to a considerable extent.

Claims: An epoxy resin encapsulating composition with enhanced moisture resistance for semiconductor packages, consisting essentially of the admixture of an epoxy resin adduct of epichlorohydrin and an aromatic hydroxyl-containing compound, with an inorganic ion-exchange solid material, said ion-exchange solid material being in the form of particles dispersed in the epoxy resin adduct and capable of exchanging its mobile anions with the chlorine ions which originate from the epichlorohydrin and occur in the epoxy resin adduct as a result of possible hydrolysis of the corresponding chlorides, said ion-exchange solid material being represented by the general formula: SbBixOy(OH)z(NO₃)w.n(H₂O) in which x represents 0.2 to 2.0, y represents 1.0 to 5.0, z represents 0.1 to 3.0, w represents 0.1 to 3.0 and n represents 0.5 to 3.0. An epoxy resin encapsulating composition as set forth in claim 1, wherein said mobile anion is hydroxyl group of which hydrogen acts as cation to be substituted with possible alkali metal ions present in the epoxy resin adduct. An epoxy resin encapsulating composition as set forth in claim 1 or 2, wherein 0.1 to 10 parts by weight of said ion-exchange material is mixed with 100 parts by weight of the epoxy resin adduct. An epoxy resin encapsulating composition as set forth in claim 1, 2 or 3, wherein said ion-exchange solid material has an average particle size of not more than 5 micro metre and has a maximum particle size of not more than 100 micro metre. A method of preparing an epoxy resin encapsulating composition according to any of claims 1 to 4, said method, comprising the steps of mixing the particles of said ion-exchange material into the molten epoxy resin to provide a first mixture; kneading the resulting first mixture so as to disperse the particles of the ion-exchange material uniformly into the epoxy resin; cooling the first mixture to solidify said first mixture; milling the solidified first mixture to the corresponding powder; blending a curing agent for the epoxy resin with the powder of the first mixture to provide a second mixture; heating the second mixture to melt, thereby partially curing the epoxy resin; cooling the second mixture to solidify it; and grinding the solidified second mixture to produce the encapsulation composition in powder form. A method of preparing an epoxy resin encapsulating composition as set forth in claim 5, wherein silica filler particles are blended with the first mixture at the step of providing the second mixture, said ion-exchange material being selected to have a maximum particle size not greater than that of the silica filler particles. A method of preparing an epoxy resin encapsulating composition as set forth in claim 5 or 6, wherein 0.01 to 10 parts by weight of ion-exchange material and 10 to 100 parts of water are mixed with 100 parts by weight of molten epoxy resin adduct at the step of providing the first mixture in order to positively hydrolyse the chloride attached to the molecules of the epoxy resin into chlorine ions and at the same time to trap the chlorine ions on the network of the ion-exchange material by exchanging the mobile anions on the network with the chlorine ions in the water solution, said ion-exchange material being mixed in excess amount relative to the chlorine ions to be removed for leaving a sufficient amount of the mobile anion on the network for another ion-exhcange reaction, the resulting first mixture being dewatered prior to milling the solidified first mixture.

Inventors: KAGAWA HIROHIKO, KYOTANI YASUHIRO, TORII MUNETOMO, KAGAWA, HIROHIKO, KYOTANI, YASUHIRO, TORII, MUNETOMO
Applicants: MATSUSHITA ELECTRIC WORKS LTD, MATSUSHITA ELECTRIC WORKS, LTD.
Application year: 1986
Main classification: C08L63
IPC codes: C08K3, C08G59, C08G63, C08L63