TW555801B - Silane-crosslinked polyolefin resin composition and insulated cable covered with the composition - Google Patents

Abstract

A silane-crosslinked polyolefin resin composition comprising (1) a base polymer, (2) a carrier polymer A incorporated with an organic unsaturated silane represented by the formula RR'SiY2 and a free radical generating agent and (3) a carrier polymer B incorporated with a silanol condensation catalyst and an antioxidant, wherein the base polymer contains a linear, medium to low density polyethylene with a degree of dispersion (Mw/Mn) of 4 or more, has an average density of 0.915 g/cm<3> to 0.935 g/cm<3> and shows a heat deformation percentage (JIS K 6723) after melt-kneading of not more than 40%. The resin composition is excellent in extrudate surface smoothness and heat resistance and is suitably used as the covering material for insulated cables which does not need the water-crosslinking step.

Description

555801 A7-B7 V. Description of the invention (1) Field of the invention The present invention relates to a silane crosslinked resin composition, which includes a basic polymer, an organic unsaturated silane, a radical generator, a silanol condensation catalyst, and if necessary ' Other additional components are fused with each other and form an insulated cable, in which the wires are covered with this composition. Relevant techniques are widely used for cross-linking and electricity irradiation and cross-linking. Ethylene warm water is not saturated. It is made in the following. It is simple to cross-link polyethylene and its cross-linking in warm water. One of the methods described above can be easily controlled by cross-beam irradiation cross-linking. The silane grafting is reversed to the silane grafting condensation catalyst, which has the advantages. One widely known as silicon should be applied to polyolefins, and will be produced in the future. Methods include organosilicon water crosslinkers, crosslinkers, known as alkane crosslinkers, and grafting from silanes. The chemical alkylation method, the phase cost represents the actual method, which is based on the polymer. This method is significantly lower than the chemical as an example. The example is poly, which includes the presence of a biological agent in contact with water.

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Employees and Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs, India and Vice-Presidents, such as JP — B — 48-171 1 and]? -Bayi 57-4 9 1 0 9. However, compared with other cross-linking methods, the warm water cross-linking method has a lower installation cost, and its disadvantage is that it requires more time and cost for cross-linking treatment. When the wire is covered with a water-crosslinkable resin composition, the crosslinking reaction proceeds very slowly at ordinary temperatures and therefore the crosslinking needs to be promoted in warm water at about 80 ° C or in a high-temperature, high-humidity container. Even under these conditions, it takes almost a full day to promote the reaction, and therefore requires a large capital expenditure on the cross-linking processing equipment. -4- This paper is again applicable to the Chinese National Standard (CNS) A4 specification (210 X 297 mm) 555801 A7 B7 V. Description of the invention (2) Therefore, even if the installation cost is very low, the maximum cost of this cross-linking processing cost must be paid This results in a reduction of the aforementioned advantages of the method. In addition, various attempts have been made so far to shorten the cross-linking treatment time of the water-crosslinkable resin as an extruded covered electric wire. For example, the methods disclosed in J P-A — 5 7 -208006 and JP — A — 62 — 106947 involve the addition of catalysts and / or auxiliaries to improved silane compounds to promote crosslinking. JP — A — 60 — 254520 discloses a method for improving the contact between resin and water during the crosslinking of water-crosslinkable resin-coated wires, thereby shortening the crosslinking time. In addition, JP_A — 4 — 331241 discloses a method in which the cross-linking treatment of a water-crosslinkable resin-coated wire is performed in an ultrasonic environment to promote the diffusion of water into the water-crosslinkable resin, and thus shorten it. Special feature for cross-linking. However, all the aforementioned methods can only shorten the time required for crosslinking treatment with warm water or steam, and cannot eliminate the water crosslinking step itself. Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. Also, warm water cross-linking of polyethylene has a disadvantage. Its improvement in resin heat resistance is lower than chemical cross-linking and electron beam irradiation cross-linking. Therefore, the use of linear, medium to low density polyethylene as a basic resin to effectively improve heat resistance has increased. However, the use of linear, medium to low density polyethylene (lower density polyethylene or its equivalent has a higher melting point and higher melt viscosity) as the basic resin will easily cause some problems such as in the extruder The generation of heat causes premature cross-linking and the formation of a rough surface due to friction with the mold. J P — A — 7-1 3 0 2 3 8 discloses an embodiment in which linear, medium to low density polyethylene is used alone as a raw material. However, the paper size of this method applies to the Chinese National Standard (CNS) A4 specification (210 X 297 mm) -5-555801 A7 B7 V. Description of the invention (3) Provides stable processability without eliminating the water crosslinking step. The present invention requires the object of the present invention to overcome the foregoing problems, to provide a silane-crosslinked polyolefin resin composition that has excellent smoothness and excellent heat resistance on the surface of the extrudate, and further provides an insulated cable. The wire was extruded and coated with a silane-crosslinked polyolefin resin composition, and a sheath was immediately applied after the covering. The present inventors have made extensive investigations to solve the foregoing problems, and have found that this goal can be achieved by using a specific crosslinked polyolefin. This is printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. According to the present invention, (i) a silane-crosslinked polyolefin resin composition containing (1) a basic polymer and (2) a carrier polymer A combined with an organic unsaturated silane is provided. Is represented by the molecular formula RR 'SiY2, where R is a monovalent olefin unsaturated hydrocarbon group, Y is a hydrolyzable organic group and R' is a monovalent hydrocarbon group, which is different from the aliphatic unsaturated hydrocarbon group or is the same as Y, and bears Free radical generator and (3) carrier polymer (B) combined with silanol condensation catalyst with antioxidant, where the basic polymer contains linear, medium to low density polyethylene with a dispersion (Mw / Mn) of 4 or Furthermore, this polymer has an average density of 0.915 g / cm3-0.935 g / cm3 and shows the percentage of thermal deformation after melt-kneading. (Measured according to JIS K6723) not more than 40%. In the silicon fluorene crosslinked polyolefin resin composition (i), it is preferred that the base polymer contains a mixture of 4-5 to 100 parts by weight of the following, and the dispersion (Mw of linear, medium to low density polyethylene) / Mn) is 4 or -6-This paper size is applicable to Chinese National Standard (CNS) A4 (210 X 297 cm) 555801 A7 B7 V. Description of the invention (4) (Please read the precautions on the back and fill out this page) More, and high density or low density polyethylene with a weight ratio of 0 to 5 5 or a basic polymer containing 7 5 to 10 weight ratio of a linear, medium to low density polyethylene with a dispersion (Mw / Mn ) Is 4 or more, and at least one polyolefin having a weight ratio of 0 to 2 5 is selected from the group consisting of ethylene ethyl acrylate copolymer (EEA), ethylene-vinyl acetate copolymer ( EVA), ethylene-methyl methacrylate copolymer (EMMA), hydrogenated block copolymers derived from hydrogenated monoblock copolymers which include polymer blocks composed primarily of at least one vinyl aromatic compound, and mainly Polymer block composed of at least one conjugated diene compound And mixtures thereof. Printed in the Silane Crosslinked Polyolefin Resin Composition (i) by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. More preferably, the carrier polymer A is selected from a group containing ethylene-ethyl acrylate copolymers. (EEA), ethylene monomethyl methacrylate copolymer (EMMA), hydrogenated block copolymer, which is derived from hydrogenated monoblock copolymer, which includes a polymer block mainly composed of at least one vinyl aromatic compound, and A polymer block mainly composed of at least one conjugated diene compound, and a mixture thereof. The carrier polymer B is selected from the group consisting of polyethylene, polypropene, and ethylene-α-olefin. Copolymer, and the total amount of carrier polymers A and B is 3-1 5% by weight, relative to all polymers. An insulated cable is also provided here, in which the wires have been coated with the aforementioned silane-crosslinked polyolefin resin composition, which is obtained by coating the wires with a resin composition, and thereafter covering the coated wires with a sheath material cover. According to the present invention, (ii) Silane cross-linked polyolefin resin is also provided. The paper size is applicable to Chinese National Standard (CNS) A4 (210 X 297 mm) 555801 A7 — B7 V. Description of the invention (5 products including ( 1) the basic polymer and (2) the carrier polymer C which binds an organic unsaturated silane, which is represented by the molecular formula RR 'SiY2, where R is a monovalent olefin unsaturated hydrocarbon group, Y is a hydrolyzable organic group, and R' It is a monovalent hydrocarbon group, which is different from an aliphatic unsaturated hydrocarbon group or the same as Y, and has a radical generator and a silanol condensation catalyst. The basic polymer contains linear, medium to low density polyethylene and its dispersion (

Mw / Mn) is 4 or more, this polymer has an average density of 0 · 915g / cm3-〇 · 935g / cm3 and shows the percentage of thermal deformation after melting and kneading (measured according to JIS K6723) not exceeding 40% . Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs, please read the following notes: Qin I, I I, III, and III. In the silane crosslinked polyolefin resin composition (ii), it is preferable that the basic polymer contains the following mixture. 4 5 — 1 0 0 part by weight linear, medium to low density polyethylene with a dispersion (Mw / Mn) of 4 or more, and 0-5 5 part by weight high density or low density polyethylene; or The base polymer contains a mixture of 7 5-1 0 0 parts by weight of linear, medium to low density polyethylene with a dispersion (Mw / Mn) of 4 or more, and 0-2 5 parts by weight of at least A polyolefin selected from the group consisting of ethylene ethyl acrylate copolymer (E EA), ethylene monovinyl acetate copolymer (EVA), ethylene monomethyl methacrylate copolymer (EMMA), Hydrogenated block copolymer obtained from a hydrogenated monoblock copolymer comprising a polymer block mainly composed of at least one vinyl aromatic compound and a polymer block mainly composed of at least one conjugated diene compound, and Mixture that The mixture has an average density of carrier polymerization 0 · 9 1 5 g / 1 0 · 9 3 5 g / This paper size applies to China National Standard (CNS) A4 (210 X 297 mm) -8- 555801 A7 B7 Intellectual Property of the Ministry of Economic Affairs Printed by the Bureau ’s Consumer Cooperatives 5. Description of Invention (6) Object A is selected from a group that includes ethylene-ethyl acrylate copolymer (EEA), ethylene-methyl methacrylate copolymer (EMMA) A hydrogenated block copolymer derived from a hydrogenated monoblock copolymer comprising a polymer block mainly composed of at least one vinyl aromatic compound and a polymer block mainly composed of at least one conjugated diene compound, and Its mixture, and the content of the carrier polymer C is 4 to 13% by weight, relative to all polymers. Also provided herein is an insulated cable obtained by coating an electric wire with the aforementioned silane-crosslinked polyolefin resin composition, and thereafter coating the coated electric wire with a sheath material. According to the present invention, there is further provided (iii) a silane-crosslinked polyolefin resin composition comprising a basic polymer, an organic unsaturated silane which is represented by a molecular formula RR 'SiY2, wherein R is a monovalent olefin unsaturated hydrocarbon group, and Y is hydrolyzable Organic group and R 'is a monovalent hydrocarbon group which is different from aliphatic unsaturated hydrocarbon group or the same as Y, radical generator and silanol condensation catalyst, wherein the basic polymer contains linear, medium to low density polyethylene and its dispersion Degree (Mw / Mn) is 4 or more, this polymer has an average density of 0 · 915g / cm3-0 · 935g / cm3 and shows the percentage of thermal deformation after melting and kneading (measured according to JIS K6723) not exceeding 4 0%. The silane-crosslinked polyolefin resin composition (iii) should preferably contain a mixture of 45 to 100 parts by weight of a linear medium to low density polyethylene having a dispersion degree (M, / Μη) of 4 or more, and 0- 5 5 parts of high-density or low-density polyethylene by weight; or mixtures of the following, • II ^ 1 ^ 1 ϋ ϋ n ϋ ϋ ϋ n ϋ I (please read the precautions on the back 1) (This page) 0.

This paper size applies Chinese National Standard (CNS) A4 specification (210 X 297 public love) 555801 Α7 Β7 V. Description of the invention (7) 7 5 — 1 0 0 Partial weight ratio of linear, medium to low density polyethylene and its dispersion (Mw / Mn) is 4 or more, and at least one polyolefin having a weight ratio of 0 to 2 5 is selected from the group consisting of ethylene-ethyl acrylate copolymer (EEA), ethylene-acetic acid Vinyl Ester Copolymer (EVA), Ethylene Monomethyl Methacrylate Copolymer (EMMA), Hydrogenated Block Copolymers Derived from Hydrogenated Monoblock Copolymers Containing Polymers Mainly Consisting of At least One Vinyl Aromatic Compound Blocks and polymer blocks composed mainly of at least one conjugated diene compound, and mixtures thereof. More preferably, the base polymer comprises a mixture of 5 to 100 parts by weight of a granular polymer and 0 to 9 5 parts by weight of granules form a polymer. Also provided herein is an insulated cable obtained by coating an electric wire with the aforementioned silane-crosslinked polyolefin resin composition, and thereafter coating the coated electric wire with a sheath material. Description of the preferred system The linear medium to low density polyethylene used in the basic polymer of the present invention is an ethylene copolymer whose main component is an olefin which can be obtained from various polymerization methods such as gaseous polymerization, solution polymerization and suspension polymerization. Various catalysts are used under low, medium or high pressure, such as Ziegler type catalysts and chromium-based catalysts. The α-olefin may be a C3-C12 olefin, such as propylene, butene-1, pentene-1, octene-1, 4-methylpentene-1, 4-methylhexamethylene-1, 4 , 4 dimethylpentan-1, ren-1, dec-1, Jade paper size is applicable to China National Standard (CNS) A4 specifications (210 X 297 mm) .1Π. ~

Please read and read first. Note on the back w Win page I Order Printed by the Intellectual Property Bureau of the Ministry of Economic Affairs, printed by the Consumer Cooperatives of the Ministry of Economic Affairs Printed by the Employees ’Cooperative of the Intellectual Property Bureau of the Ministry of Economics, printed by 555801 A7 _— _ B7 V. Description of the invention (8), Undene-1 and dodecene-1. The polyethylene used in the base polymer of the present invention is high density polyethylene or low density polyethylene. High-density polyethylene is an ethylene polymer that is obtained from various polymerization methods, such as gaseous polymerization, solution polymerization, and suspension polymerization. Various catalysts are used at low, medium, or high pressures, such as Ziegler-type catalysts and chromium-based catalysts. catalyst. Low density polyethylene refers to ethylene polymers which are prepared by high-pressure polymerization using a tubular method or an autoclave method. The basic polymer of the present invention preferably contains a mixture of linear, medium to low-density polyethylene having a weight ratio of 4 5 to 100 parts with a dispersion (Mw / Mn) of 4 or more, and a weight ratio of 0 to 55 parts High density or low density polyethylene, this mixture has an average density of 0 · 9 1 5 g / cm3-0 · 935 g / cm3. When the average density is lower than 0 · 9 1 5 g / cm3 or when the amount of mixed low density polyethylene exceeds 5 5 parts by weight, the heat resistance tends to decrease; when the average density is higher than 0 · 9 3 5 g / cm3, the resin The composition tends to be rigid and unsuitable for preparing large-sized wires and cables. The polyolefin used in the basic polymer of the present invention may be, for example, ethylene-ethyl acrylate copolymer (EEA), ethylene-vinyl acetate copolymer (EVA), ethylene-methyl methacrylate copolymer (EMMA), and hydrogenated copolymer. Segmented copolymer obtained from a hydrogenated monoblock copolymer comprising a polymer block mainly composed of at least one vinyl aromatic compound and a polymer block mainly composed of at least one conjugated diene compound, such as hydrogenated styrene One isoprene block copolymer (SEPS) and hydrogenated styrene. One paper size applies Chinese National Standard (CNS) A4 specification (210 X 297 public love). • 11 · ----------- I equipment — 丨! !! Order 丨!丨 — 丨-(Please read ‘Seven notes on the back side and then fill out this page] 555801 Α7 Β7 V. Description of the invention (9) Butadiene block copolymer (SEBS). The basic polymer of the present invention preferably comprises a mixture of the following linear, medium to low-density polyethylenes with a weight ratio of 7 5 to 1 00, a dispersion (Mw / Mn) of 4 or more, and 0 to 2 5 parts by weight Compared to the aforementioned polyolefins, this mixture has an average density of 0.915 g / cm3 to 0.935 g / cm3. When the average density is lower than 0.915 g / cm3 or when the amount of the blended polyolefin exceeds 25 parts by weight, heat resistance tends to decrease; when the average density is higher than 0.935 g / cm3, the resin composition tends to be rigid and unsuitable Prepare large size wires and cables. In the method for producing the silane-crosslinked polyolefin resin composition (iii), the base polymer preferably includes a mixture of 5 to 100 parts by weight of granular polymers and 0 to 9 5 parts by weight of granules. polymer. When the amount of the particulate polymer is less than 5 parts by weight, the unsaturated organic silane tends to have poor dispersion, resulting in a local crosslinking reaction and fish eyes. Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. The organic unsaturated silanes used in the present invention are grafted on the basic resin as the cross-linking point between the basic resin molecules. The organic unsaturated silane-based compound used in the present invention is represented by the molecular formula RR 'SiY2, where R is a monovalent olefin unsaturated hydrocarbon group, Y is a hydrolyzable organic group, and R' is a monovalent hydrocarbon group which is different from a fat The group of unsaturated hydrocarbon groups may be the same as Y. The organic unsaturated silanes used are preferably those in which R ′ is the same as Y and which is represented by the molecular formula RS i Y3, such as vinyltrimethoxysilane, vinyltriethyloxysilane, vinyltributoxysilane, allyl Trimethyloxysilane and allyltriethoxysilane. Silane is added in an amount of 0 · 1--12- This paper size is applicable to Chinese National Standard (CNS) A4 (210 X 297 public love) 555801 A7 ___ B7 Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 5. ) 5% by weight, preferably 0.7-7% by weight of the total weight. When this amount is less than 0. 1% by weight, it will branch; when this amount exceeds 5% by weight, there will be disadvantages. The free radical generator used in the present invention is used as a silicon initiator. The free radical generator used may be various organic esters, which can exert a strong polymerization initiation effect, such as dianthrene α, 0: '-di (tertiary butylperoxydiisopropyl) butyl peroxide, tri Grade butyl anisyl peroxide, extruded and peracid oxide, monobenzene, two-three grade, Dibenzylfluorenyl peroxide, 2,5-dimethyl-2,5-bis (tertiary butylperoxy) hexane, tertiary butylperoxy tert-valerate, and tertiary butylethylhexyl ester . The amount of the free-radical generator to be added is a weight ratio of 0. 0, preferably a total weight of 0. 05 to 0. 2% by weight. When the amount is less than 0.01% by weight, it is insufficiently performed; when the amount exceeds 0.5% by weight, it tends to be bad and the surface of the extruded object also tends to be bad. In the production of silane-crosslinked polyolefin resin composition (free radical generator and organic unsaturated silane can be added to this, the carrier polymer A can be swelled in the liquid mixture of the organic unbased generator. At this time, it is added Polymer A needs to be preheated, but the temperature must not be higher than the junction. It must be non-meltable. The carrier polymer A must be compatible with the basic polymer to be crosslinked and organically unsaturated. The substance A must not be easily peroxy- 2-1-0. In contrast, the silane ratio is 5% heavier than the polymer grafting reaction process i). In the method of the present invention, the carrier polymerizes saturated silane and free radicals. Concentrated silane, the melting point of the carrier crystal, so the polymer must be solid and silane. The term "ground reacts with silane and please read the note on the back first. This paper size applies to Chinese National Standard (CNS) A4 specifications (210 X 297)蜚) -13-555801 A7 B7 5. Description of the invention (11) Must be dispersible or soluble in the basic polymer. A suitable carrier polymer A should be non-hygroscopic. That is, it is preferable that the carrier polymer A absorbs water relatively slowly in order to minimize the possibility of premature hydrolysis and condensation of an organic unsaturated silane. In any case, substantially no water should be present in the carrier polymer A. The carrier polymer A is generally used in the form of particles, i.e., fine particles or granules, preferably in the form of granules. The carrier polymer A used in the present invention may be, for example, ethylene-ethyl acrylate copolymer (EEA), ethylene-methyl methacrylate copolymer (EMMA), and hydrogenated block copolymer which is obtained from hydrogenated monoblock copolymer. It includes a polymer block mainly composed of at least one vinyl aromatic compound and a polymer block mainly composed of at least one conjugated diene compound, such as hydrogenated styrene isoprene block copolymer (SEPS) and Hydrogenated styrene butadiene block copolymer (SEBS), and mixtures thereof. The silanol condensation catalyst used in the present invention printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economics may be, for example, an organometallic compound such as dibutyltin dilaurate, tin acetate, dibutyltin diacetate, dibutyltin dicaprylate , Lead naphthalate, zinc caprate, cobalt naphthalate, tetrabutyl titanate, lead stearate, zinc stearate, cadmium stearate, barium stearate and calcium stearate. These compounds are added in an amount of from 0.01 to 0.2% by weight, preferably from 0.02 to 0.1% by weight, relative to the total weight of the polymer. When the amount is less than 0.01% by weight, the cross-linking reaction does not proceed sufficiently. When the amount exceeds 0.2% by weight, the cross-linking is partially performed in the extruder at the time of extrusion, which deteriorates the appearance of the extruded part. In the method for producing a silane-crosslinked polyolefin resin composition (i), a silanol condensation catalyst and an antioxidant can be added to the carrier polymer B of the present invention. 14- This paper is in accordance with China National Standard (CNS) A4. (210 X 297 public love) 555801 A7 B7 5. Description of the invention (12), it is kneaded and granulated with the carrier polymer B. The support polymer B should be in the form of particles and should be solid and compatible with the base polymer to be crosslinked. The carrier polymer B of the present invention is usually used in the form of particles, i.e., fine particles or granules, preferably in the form of granules. The carrier polymer B used in the present invention may be, for example, a copolymer of polyethylene, polypropene, and an olefin with an α-olefin. The α-olefin is a Cs-C12 olefin, such as propylene, butene-1, pentene. Ene-1, octene-1, 4-methylpentene-1, 4-methylhexene-1, 4, 4,4-dimethylpentene-1, nonene-1, decene-1, ten Monoene-1 and dodecene-1, and mixtures of these polymers. In the method for producing a silane-crosslinked polyolefin resin composition (ii), printed by a consumer cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs, a radical generator, a silanol condensation catalyst, and an organic unsaturated silane can be added to the carrier polymer of the present invention. In C, the carrier polymer C is swollen in a liquid mixture obtained from a dissolved radical generator and a silanol condensation catalyst in an organic unsaturated silane. At this time, in order to add unsaturated silane to a high concentration, the carrier polymer C needs to be preheated, but the temperature must not be higher than the melting point of the crystal, so the polymer may not be melted. The carrier polymer C must be in the form of particles and must be solid and compatible with the base polymer to be crosslinked and the organic unsaturated silane. The term "compatible" here means that the carrier polymer C must not easily react with the organic unsaturated silane and must be dispersible or soluble in the base polymer. A suitable carrier polymer C should be non-hygroscopic. That is, it is preferable that the carrier polymer C absorbs water relatively slowly in order to minimize the possibility of premature hydrolysis and shrinkage of the organic unsaturated silane. In any case, substantially no water should be present in the carrier polymer C. Carrier polymer C Tong-15 · This paper size applies to China National Standard (CNS) A4 (210 X 297 public love) 555801 A7 B7 Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 5. Description of the invention (13) Use in form, that is, fine particles or granules, preferably in the form of granules. The carrier polymer C used in the present invention may be, for example, ethylene-ethyl acrylate copolymer (EEA), ethylene-methyl methacrylate copolymer (EMMA), a hydrogenated block copolymer derived from a hydrogenated monoblock copolymer comprising a polymer block composed primarily of at least one vinyl aromatic compound and a polymer composed primarily of at least one conjugated diene compound Blocks, such as hydrogenated styrene isoprene block copolymer (SEPS) and hydrogenated styrene butadiene block copolymer (SEBS), and mixtures thereof. In the method for producing the silane-crosslinked polyolefin resin composition (i), a carrier polymer is added so that the total amount of the carrier polymers A and B is in a range of 3 to 15% by weight, relative to all polymers. When the amount is less than 3% by weight, sufficient grafting does not occur; when the amount exceeds 15% by weight, defective extrusion tends to occur and it is economically disadvantageous. In the method for producing a silane-crosslinked polyolefin resin composition (i i), the amount of the carrier polymer C is in the range of 4 to 13% by weight, relative to all polymers. When the amount is less than 4% by weight, sufficient grafting does not occur: when the amount exceeds 13% by weight, defective extrusion tends to occur, and it is economically disadvantageous. If necessary and desired in all methods for producing the silane-crosslinked polyolefin resin composition (i), (ii), and (iii), other conventionally used additives may be added to the resin composition of the present invention, including For example, antioxidants, neutralizers, ultraviolet absorbers, antistatic agents, pigments, dispersants, thickeners, corrosion inhibitors, antifungal agents, flow regulators and their (please read and read the notes on the back. 5 · Write this page) Loading · This paper size is applicable to China National Standard (CNS) A4 (210 X 297 public love) • 16- 555801 A7 ____ B7 V. Description of the invention (14) It is made of inorganic materials and other synthetic resins. · The silane-crosslinked polyolefin resin composition of the present invention is excellent in thermal deformation characteristics and can be used in various applications. Although the heat resistance can be improved by subjecting the composition to a post-crosslinking treatment, such as steam treatment or warm water treatment after extrusion, this step can be omitted. In addition, the resin composition of the present invention is particularly suitable for producing insulated cables having good heat resistance and flexibility. After the electric wire has been covered with the resin composition of the present invention, the covered electric wire can be immediately covered with a sheath material without going through a water crosslinking step. For this purpose, the percentage of thermal deformation immediately after extrusion should not exceed 40%. The sheath material used herein may be, for example, a vinyl chloride resin composition. The present invention will be described in detail by the following examples, which are only used for illustration and not for limiting the present invention. Preparation of carrier polymers A, B, and C: Preparation of carrier polymers A: Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economy To 80 ° C. Thereafter, a liquid mixture obtained by dissolving 2 parts by weight of D C P in 45 parts by weight of VTMO S was poured into this supermixer, and the E E A was impregnated for 10 minutes with stirring.

Preparation of carrier polymer B. One hundred parts by weight of LDPE, 15 parts by weight of -17- This paper size applies to China National Standard (CNS) A4 specifications (210 X 297 male cage) 555801 A7 B7 Employees of Intellectual Property Bureau, Ministry of Economic Affairs Printed by Consumer Cooperatives. 5. Description of the invention (15) DBTDL, 16 parts by weight antioxidant and 5 parts by weight lubricant, kneaded and granulated with a pressure kneader (3 liter capacity, made by MORIYAMA SEISAKUSHO). Preparation of carrier polymer C: First, 100 parts by weight of E EA was injected into a super mixer, stirred and mixed, and preheated to 80 ° C. After that, a liquid mixture obtained by dissolving 2 parts by weight of DCP and 15 parts by weight of DBTDL in 45 parts by weight of V TMO S was poured into this super mixer, and the EEA was impregnated for 10 minutes with stirring. Example 1-15 and Comparative Example 1-18 In the method for producing a silane-crosslinked polyolefin resin composition (i), a base polymer, a carrier polymer A, and a carrier polymer B are shown in the table. The ratio of 1 to a and 2 to a is melted and mixed, and extruded into a tape. The percentage of thermal deformation of this extruded tape immediately after being extruded was evaluated. In addition, the covered wire extruding was performed by using the same composition as the tape extruding, and the surface smoothness of the extruded piece was evaluated. The results of this evaluation are shown in Tables 1-b and 2-b. Examples 6 to 10 and Comparative Examples 9 to 16 In the method for producing a silane-crosslinked polyolefin resin composition (ii), the basic polymer and the carrier polymer C are shown in Tables 3-a and 4 -The proportion of a is melted and blended, and extruded into a tape. Evaluate the tape (please read the note on the back-installation-matters and write this page) This paper size is applicable to China National Standard (CNS) A4 (210 X 297 mm) -18 · 555801 A7 B7 V. Description of the invention (16) Percent thermal deformation immediately after extrusion. In addition, the covered wire extrusion was performed by using the same composition as the tape extrusion, and the surface smoothness of the extrusion was evaluated. The results of this evaluation are shown in Tables 3-b and 4-b. Example 1 1 to 15 and Comparative Examples 1 7 to 2 5 In a method for producing a silane-crosslinked polyolefin resin composition (iii), a basic polymer was mixed with a solution (which is a radical generator It is obtained by dissolving unsaturated organic silane compound with silanol condensation catalyst), melted and mixed according to the ratios shown in Tables 5-a and 6-a, and extruded into a tape. At this time, the amount of the mixed solution was adjusted by a fixed transfer pump so as to reach a portion of the weight ratio shown in the table. The extruded tape is used to evaluate the percentage of thermal deformation. In addition, the covered wire extrusion was performed by using the same composition as the tape extrusion, and the surface smoothness of the extrusion was evaluated. The results of this evaluation are shown in Tables 5-b and 6-b 〇 The raw materials used are as follows. (1) EEA: Ethylene · Ethyl Acrylate Copolymer (EA content: 23% by weight, density ... 935g / cm3, granular shaped product) (2) EVA: Ethylene · Vinyl Acetate Copolymer (VA content : 25% by weight, density: 950g / cm3, granular shaped product) (3) VTMOS: vinyltrimethoxysilane (4) DCP: dianisyl peroxide This paper applies Chinese national standards ( CNS) A4 specification (21〇x 297 mm) (Please read the notes on the back before filling in this page) · ϋ ϋ ϋ ϋ ί i_i ϋ 1 · «ϋ tmme ϋ ϋ 1 · —I · Intellectual Property Bureau, Ministry of Economic Affairs Printed by Employee Consumption Cooperatives-19- 555801 Printed by Employee Consumption Cooperatives of the Intellectual Property Bureau of the Ministry of Economy A7 B7 V. Description of Invention (17) (5) DBTDL: Dibutyltin dilaurate (6) Antioxidants: Phenol antioxidants Irganox 1010 (by

Ciba-Geigy Corp. (7) Lubricant: Low molecular weight polyethylene / Sanwax 171P (manufactured by

(Manufactured by Sanyo Kasei K · K ·) (8) LDPE: Low-density polyethylene (density: 0.923 g / cm3, granular shaped article) (9) L-LDPE (1): Linear, medium to low-density polyethylene (Density: 0.917 g / cm3 'Dispersion: 7 · 8' granular shaped article) (1〇) L-LDPE (2): Linear, medium to low density polyethylene (Density: 0.919 g / cm3, Dispersion: 3 · 9, granular shaped article) (11) L-LDPE (3): Linear, medium to low density polyethylene (density: 0 · 902g / cm3, dispersion: 5, granular shaped article) ( 12) L-LDPE (4): linear, medium to low density polyethylene (density: 0 · 925g / cm3, dispersion: 5, granular shaped product) (13) L-LDPE (5): linear, medium to Low density polyethylene (density: 0 · 918g / cm3, dispersion: 4 · 5, fine particles) (14) L-LDPE (6) •• linear, medium to low density polyethylene (density ·· 0 · 920g / cm3, dispersion ·· 3 · 6, fine ϋ ϋ 1 ϋ ϋ n ϋ Βϋ «I · ϋ ϋ I i · — ϋ ϋ 1.— 1« ϋ · 1 Order --------- · ( Please read &quot; read the precautions on the back side and fill in this page to write this page) This paper size is applicable to China National Standard (CNS) A4 regulations Grid (210 X 297 public love) -20 · 555801 A7 ___ B7 V. Description of the invention (18 pieces) (Please read the precautions on the back to write this page) (15) HDPE: High density polyethylene (density 0 · 950 g / cm3, granular shaped product) The evaluation method is as follows. (16) Extrude the appearance of the tape (check for fisheye presence):

50 mm 0, single screw extruder (manufactured by TANABE Plastic Machine Κ · Κ ·) 130 — * 160 — 180 — 190 -1 8 0 ° CL / D: 20, compression ratio: 3 · 5, with belt die: Width 100mm, edge gap: 1mm, number of screw rotations: 40rpm Appearance of belt (fisheye) Evaluation: Evaluation order 0 &gt; Δ &gt; X, level 0 rated as acceptable (17) Thermal deformation percentage (%): basis JIS Κ 6 7 2 3 (1 8) Extruded coated wire appearance (evaluation of the smoothness of the extruded surface): 50 mm single screw extruder printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economy (manufactured by TANABE Plastic Machine Κ • Κ · ) 130-160 -180 -190-180 ° C, L / D: 24, compression ratio: 4 · 0, conductor diameter: 0 · 8mm0, coating thickness 1 · O〇mm0, number of screw rotation: 4 0 rpm, Appearance evaluation of covered electric wires: Evaluation order 0> ASX, level 0 comment-21-This paper size is applicable to China National Standard (CNS) A4 specification (210 X 297 mm) 555801 A7 B7 V. Invention description (19) is acceptable (1 9) Ease of winding after the wire is covered (cable flexibility evaluation): Coiled wire winding evaluation: Evaluation sequence 0> Δ &gt; X, level 0 is acceptable (2 0) Overall evaluation: 0: All of (16), (18), and (19) are 0, and No more than 40% in (17) X ·· Any X in (1 6), (1 8) and (1 9), or more than 40% in (17) (please read tif Matters written on this page) Binding. Printed by the Consumers ’Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs 1-a Composition Examples Comparative Examples 1 2 3 4 5 1 2 L-LDPE (l) 50 50 50 80 80 40 L-LDPE ( 2) 50 50 60 LDPE 50 50 HDPE 50 EEA 20 EVA 20 Carrier polymer A 5 5 5 5 5 5 5 Carrier polymer B 2 2 2 2 2 2 2

This paper size applies to China National Standard (CNS) A4 (210 X 297 mm) -22- 555801 A7 B7 V. Description of the invention (20)

Table 1 — b Evaluation results Examples Comparative Examples 1 2 3 4 5 1 2 Average density of basic polymer (g / cm3) 0.918 0.920 0.934 0.921 0.924 0.922 0.919 Tape appearance 0000 Thermal deformation percentage (% ) 29 20 23 37 33 21 24 Extruded wire smoothness 〇〇〇〇〇〇 Wire winding evaluation 〇 〇〇〇〇〇 Overall evaluation 〇 〇〇〇〇XX (Please read, read the precautions on the back before filling out this Page) S · Printed by Employees ’Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 2—a Component comparison example 3 4 5 6 7 8 L-LDPE (l) 40 40 70 70 L-LDPE (3) 50 L-LDPE (4 ) 50 LDPE 60 50 HDPE 60 50 EEA 30 EVA 30 Carrier polymer A 5 5 5 5 5 5 Carrier polymer B 2 2 2 2 2 2 I · ^ 1 ϋ 1 · 1 ϋ ϋ · ϋ l_i one one 0, · n 1_ ϋ ϋ-1 ϋ ϋ · This paper size applies to China National Standard (CNS) A4 (210 χ 297 mm) • 23- 555801 A7 B7 V. Description of the invention (21) Printed by the Consumers ’Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs system

Table 2 — b Evaluation results Comparative Example 3 Average density of basic polymers 4 5 6 7 8 (g / cm3) 0.921 0.937 0.922 0.927 0.913 0.938 Tape appearance 〇〇〇〇 × 〇 Thermal deformation percentage (%) 42 12 60 55 60 19 Extruded wire appearance XXXXXX Wire winding evaluation 0 × 〇〇〇X Overall evaluation XXXXXX Table 3 — a Component Example Comparative Example 6 7 8 9 10 9 10 L-LDPE (l) 50 50 50 80 80 40 L- LDPE (2) 50 50 60 LDPE 50 50 HDPE 50 EEA 20 EVA 20 Carrier polymer c 5 5 5 5 5 5 5 (Please read the notes on the back first and write this page) This paper size applies to Chinese National Standard (CNS) A4 specification (210 X 297 mm) • 24 · 555801 A7 B7 V. Description of the invention (22) Printed by the Consumer Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs

Table 3-b Evaluation results Example Comparative Example 6 7 8 9 10 9 10 Average density of basic polymer (g / cm3) 0.918 0.920 0.934 0.921 0.924 0.922 0.919 Tape appearance 0.000% Thermal deformation percentage (% ) 26 19 27 37 32 29 14 Extruded wire appearance 00000000XX Wire winding evaluation 100,0000000 Overall evaluation 0000 × XX Table 4 — a Component Comparative Example 11 12 13 14 15 16 L-LDPE (l) 40 40 70 70 L-LDPE (3) 50 L-LDPE (4) 50 LDPE 60 50 HDPE 60 50 EEA 30 EVA 30 carrier polymer c 5 5 5 5 5 5 (Please read the back (Notes ^ write this page) · This paper size is applicable to China National Standard (CNS) A4 (210 X 297 cm). 25- 555801 A7 B7 V. Description of the invention (23)

Table 4 -b Evaluation results than S bite implementation> Example 11 12 13 14 15 16 Average density of basic polymer (g / cm3) 0.921 0.937 0.922 0.927 0.913 0.938 Tape appearance 〇〇〇 × 〇 Thermal deformation percentage (%) 42 10 50 50 65 8 Extruded wire appearance XXXXXX Wire winding evaluation 〇X 〇〇〇X Overall evaluation XXXXXX (Please read the precautions on the back to write this page)

· N I ϋ I ϋ ϋ ϋ II ^ 1 ϋ ϋ 1 ϋ ϋ 1 ϋ I Printed on the paper by the Intellectual Property Bureau of the Ministry of Economy ’s Consumer Cooperatives. The paper size applies to Chinese National Standard (CNS) A4 (210 X 297 public love) -26- 555801 A7 B7 V. Description of the invention (24) Table 5 — a Component Example Comparative Example 11 12 13 14 15 17 18 L-LDPE (5) 10 10 10 10 10 L-LDPE (6) 10 10 L-LDPE (l ) 40 40 40 70 70 40 L-LDPE (2) 50 40 50 LDPE 50 50 HDPE 50 EEA 20 EVA 20 VTMOS 2 2 2. 2 2 2 2 DCP 0.1 0.1 0.1 0.1 0.1 0.1 0.1 DBTDL 0.05 0.05 0.05 0.05 0.05 0.05 0.05 (Please read the notes on the back first to write this page) ^ r · Binding-

Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs This paper size is applicable to the Chinese National Standard (CNS) A4 specification (210 X 297 public love) -27- 555801 A7 B7 V. Description of the invention (25)

Table 5 — b Evaluation results Example Comparative Example 11 12 13 14 15 17 18 Average density of base polymer (g / cm3) 0.918 0.920 0.934 0.921 0.924 0.923 0.920 Band appearance 0.000% Thermal deformation (% ) 27 19 26 33 31 22 27 Extruded wire appearance 〇〇〇〇〇〇 Wire winding evaluation 〇 〇 〇 〇 〇 〇 Overall evaluation 〇 〇 〇 〇 〇 XX (Please read the tjf · Notes on the back to write this page) S · I · I n ϋ n · ϋ · ϋ e ^ eJ ϋ ^ 1 1 ϋ -1 ϋ ϋ-Printed on the paper by the Consumers' Cooperative of the Intellectual Property Bureau of the Ministry of Economic Affairs. The paper size applies to the Chinese National Standard (CNS) A4 (210 X 297 public love) -28- 555801 A7 B7 V. Description of the invention (26) Table 6 — a Composition Comparative Example 19 20 21 22 23 24 25 L-LDPE (5) 10 10 10 10 10 10 4 L-LDPE (l ) 30 30 60 60 96 L-LDPE (3) 60 L-LDPE (4) 40 LDPE 60 30 HDPE 60 50 EEA 30 EVA 30 VTMOS 2 2 2 2 2 2 2 DCP 0.1 0.1 0.1 0.1 0.1 0.1 0.1 DBTDL 0.05 0.05 0.05 0.05 0.05 0.05 0.05 (Please read the notes on the back first Write this page) stapling · Ministry of Economic Affairs Intellectual Property Office employees consumer cooperatives printed in this paper scale applicable Chinese National Standard (CNS) A4 size (210 X 297 mm) -29- 555801 A7 B7

V. Description of the invention (27) Table 6 — b__ Evaluation results Example Comparative Example 19 20 21 22 23 24 25 Average density of basic polymer (g / cm3) 0.921 0.937 0.922 0.927 0.910 0.937 0.917 Tape appearance 〇〇〇〇〇 〇X Thermal Deformation Percentage (%) 44 16 57 59 55 17 42 Extruded wire appearance XXXXXXX Wire winding evaluation 〇X 〇〇〇X 〇 Overall evaluation XXXXXXX (Please read • Read the notes on the back 3 Write this page) Ministry of Economic Affairs Printed by the Consumer Property Cooperative of the Intellectual Property Bureau From Tables 1 to b to 6 — b, it can be clearly seen that the resin composition of Examples 1 to 15 has excellent extrusion processability and smooth surface (extrusion line appearance). And show very high heat resistance. That is, the percentage of thermal deformation immediately after extrusion does not exceed 40%, and therefore the crosslinking treatment step can be eliminated. In addition, it can be seen that these resin compositions have good processability and heat resistance for using any crosslinking method. In contrast, the resin compositions of the comparative examples were all unsatisfactory in terms of surface smoothness, and there was no good balance between extrusion processability and heat resistance. According to the present invention, a silane-crosslinked polyolefin resin composition can be provided which has excellent extruded surface smoothness and heat resistance. When the resin composition is used to cover an electric wire, a water crosslinking step can be omitted and a sheath can be immediately applied to the covered electric wire to form a cable. As a result, the yield of the cable can be greatly improved, while the production cost can be significantly reduced. As such, the present invention greatly contributes to the production of insulated cables. Appropriate rule paper quasi-standard bidder 10 (2 rule 30

Claims (1)

555801, published Thai A8 B8 C8 D8 patent application scope printed by the Intellectual Property Bureau of the Ministry of Economic Affairs employee consumer cooperatives 1. A silane crosslinked polyolefin resin composition, which contains (1) a basic polymer, (2) a carrier polymer A of which Combined with organic unsaturated silanes, it is represented by the molecular formula RR 'SiY2, where R is a monovalent olefin unsaturated hydrocarbon group, Υ is a hydrolyzable organic group and R' is a monovalent hydrocarbon group which is different from an aliphatic unsaturated hydrocarbon group or the Υ, with a free radical generator and (3) a carrier polymer B combined with a silanol condensation catalyst and an antioxidant 'wherein the basic polymer contains linear, medium to low density polyethylene with a dispersion (Mw / Mn) of 4 Or more, this polymer has an average density of 0 · 915g / cm3-0.935g / cm3, and shows that the percentage of thermal deformation (measured according to JI s K6723) after melt-kneading does not exceed 40%. 2 · A silane-crosslinked polyolefin resin composition comprising a basic polymer and a carrier polymer C in which an organic unsaturated silane is combined, which is represented by the molecular formula RR 'SiY2, where R is a monovalent olefin unsaturated hydrocarbon group, Y Is a hydrolyzable organic group and R ′ is a monovalent hydrocarbon group, which is different from an aliphatic unsaturated hydrocarbon group or the same as Y, and has a radical generator and a silanol condensation catalyst, wherein the basic polymer includes a linear, intermediate To low density polyethylene with a dispersion (Mw / Mn) of 4 or more, this polymer has an average density of 0.915g / c-0 · 9 3 5 gc and shows the percentage of thermal deformation after melt-kneading (according to JISK 6 7 2 3 measurement) not more than 40%. 3. A silane crosslinked polyolefin resin composition comprising a basic polymer and an organic unsaturated silane which is represented by the molecular formula RR 'SiY2 (where R is a monovalent olefin unsaturated hydrocarbon group, Y is a hydrolyzable organic group and This paper size applies to China National Standard (CNS) A4 specification (210 × 297 mm) Please read the note of Λ first, then note the matter -31-A8B8C8D8 Printed by the Intellectual Property Bureau Staff Consumer Cooperatives of the Ministry of Economic Affairs 555801 6. Scope of patent application R ' It is a monovalent hydrocarbon group which is different from the aliphatic unsaturated hydrocarbon group or the same as Y), the radical generator and the silanol condensation contact, and are mixed with each other through melting; wherein the basic polymer contains linear, medium to low density polyethylene Its dispersion (Mw / Mn) is 4 or more. This polymer has an average density of 0 · 915g / cm3 — 〇 · 935g / cm3 and shows the percentage of thermal deformation after melt-kneading (measured according to JIS K6723) Not more than 40%. 4. The silane-crosslinked polyolefin resin composition according to any one of claims 1 to 3 in the scope of the patent application, wherein the basic polymer contains the following mixture, a linear, medium to 4 to 10 part by weight ratio Low density polyethylene is a high density or low density polyethylene with a dispersion (Mw / Mn) of 4 or more and a weight ratio of 0 to 5 5 parts. 5. The silane-crosslinked polyolefin resin composition according to any one of claims 1 to 3 in the scope of the patent application, wherein the basic polymer comprises the following mixture, and the linear proportion of the weight ratio of 7 5 to 100 is linear to low Density polyethylene has at least one polyolefin having a dispersion degree (Mw / Mn) of 4 or more, and a weight ratio of 0 to 25 in a group consisting of an ethylene-ethyl acrylate copolymer ( EEA), ethylene-vinyl acetate copolymer (EVA), ethylene-methyl methacrylate copolymer (EMMA), hydrogenated block copolymers which are derived from hydrogenated monoblock copolymers and contain at least one vinyl aromatic Polymer blocks composed of family compounds and polymer blocks composed primarily of at least one conjugated diene compound, and mixtures thereof. 6 · If you apply for the silane-crosslinked polyolefin resin group in item 3 of the patent scope, the paper size applies to the Chinese National Standard (CNS) A4 specification (210 X 297 mm) (please read the V precautions on the back first to write this page) • 32- A8B8C8D8 555801 Six, patent application scope of the product 'wherein the basic polymer contains the following mixture, 5 to 100 parts by weight of granular polymers and 5-100 parts by weight of particles to form polymerization Thing. 7. The silane-crosslinked polyolefin resin composition according to item 1 of the patent application, wherein the carrier polymer A is selected from the group consisting of polyethylene, poly (propylene) and ethylene copolymers. An alpha-olefin. 8. The silane-crosslinked polyolefin resin composition according to item 1 of the application, wherein the carrier polymer B is selected from the group consisting of ethylene-ethyl acrylate copolymer (ΕΕΑ), ethylene monomethyl Methyl acrylate copolymer (EMMA), hydrogenated block copolymer derived from a hydrogenated monoblock copolymer, which includes a polymer block mainly composed of at least one vinyl aromatic compound and mainly composed of at least one conjugated diene Polymeric blocks of compounds, and mixtures thereof. 9 · The silane-crosslinked polyolefin resin composition according to item 1 of the patent application range, wherein the total amount of the carrier polymers A and B is 3 to 1 5% by weight, relative to all polymers. 10. The silane-crosslinked polyolefin resin composition according to item 2 of the patent application, wherein the carrier polymer C is selected from the group consisting of polyethylene, poly (propylene) and ethylene copolymers. There is an α-olefin, such as the silane-crosslinked polyolefin resin composition in the second item of the patent application, wherein the amount of the carrier polymer C is 4 to 13% by weight, relative to all polymers ^ 1 2 · —A kind of insulated cable, in which the wires are covered with patent paper. The paper size is applicable to China National Standard (CNS) A4 (210 X 297 mm). 33- (Please read the precautions on the back first to write this page) —i I III «ϋ 1_ I ϋ 1 immm I ϋ ϋ I ^ Printed by the Consumer Cooperatives of the Intellectual Property Bureau of the Ministry of Economic Affairs 555801 A8 B8 C8 D8 VI. Scope of Patent Application The silane crosslinked polyolefin resin composition of any one of the items 1 to 11 in the scope. 1 3 · An insulated cable obtained by covering an electric wire with a silane-crosslinked polyolefin resin composition as described in any one of claims 1 to 11 of the scope of patent application, and thereafter covering the covered electric wire Cover with jacket material. -------------- Installation --- (please sst »first. Note on the back side to write this page) Employees of the Intellectual Property Bureau of the Ministry of Economic Affairs, Co-operative Society printed this paper. The paper standards are applicable to Chinese national standards. (CNS) A4 size (210 X 297 mm) -34-