KR20170055122A - Polycarbonate resin composition and molded article comprising the same - Google Patents
Polycarbonate resin composition and molded article comprising the same Download PDFInfo
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- KR20170055122A KR20170055122A KR1020150157897A KR20150157897A KR20170055122A KR 20170055122 A KR20170055122 A KR 20170055122A KR 1020150157897 A KR1020150157897 A KR 1020150157897A KR 20150157897 A KR20150157897 A KR 20150157897A KR 20170055122 A KR20170055122 A KR 20170055122A
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L69/00—Compositions of polycarbonates; Compositions of derivatives of polycarbonates
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
- C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L25/00—Compositions of, homopolymers or copolymers of compounds having one or more unsaturated aliphatic radicals, each having only one carbon-to-carbon double bond, and at least one being terminated by an aromatic carbocyclic ring; Compositions of derivatives of such polymers
- C08L25/02—Homopolymers or copolymers of hydrocarbons
- C08L25/04—Homopolymers or copolymers of styrene
- C08L25/08—Copolymers of styrene
- C08L25/10—Copolymers of styrene with conjugated dienes
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
- C08L51/00—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers
- C08L51/04—Compositions of graft polymers in which the grafted component is obtained by reactions only involving carbon-to-carbon unsaturated bonds; Compositions of derivatives of such polymers grafted on to rubbers
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Abstract
Description
The present invention relates to a polycarbonate resin composition and a molded article comprising the polycarbonate resin composition, and more particularly to a polycarbonate resin composition excellent in hydrolysis resistance in a high temperature and high humidity environment and a molded article containing the same, .
The polycarbonate resin is well known as an amorphous high transparency thermoplastic resin having high impact resistance at room temperature, excellent mechanical properties such as impact strength, excellent thermal properties such as flame retardance and heat resistance, and high dimensional stability. Materials for OA such as mobile materials, mobile phones, notebooks and printers, materials for various containers, and the like.
In addition, not only a polycarbonate resin but an acrylonitrile-butadiene-styrene copolymer is alloyed to secure a high fluidity at a molding temperature lower than that of a polycarbonate resin, thereby improving workability and moldability, Have also been actively studied.
However, a polycarbonate resin is a condensation polymer having a carbonic acid ester repeating unit, and a carbonate group in the polycarbonate resin reacts with water to cause a molecular weight loss of the polycarbonate resin, Resulting in loss of physical properties of the polycarbonate resin. Also, various catalysts, such as acids and bases, or chemical residues of the emulsion polymerization process can increase the rate of hydrolysis of the polycarbonate resin and, when used in applications that are exposed to high temperature and high humidity environments, can lead to severe polycarbonate resin failure .
An object of the present invention is to provide a polycarbonate resin composition excellent in hydrolysis resistance in a high temperature and high humidity environment while providing the same mechanical properties and flame retardancy as those of the prior art.
Another object of the present invention is to provide a molded article comprising the polycarbonate resin composition.
These and other objects of the present invention can be achieved by the present invention described below.
In order to achieve the above object, the present invention provides a thermoplastic resin composition comprising 55 to 85% by weight of a polycarbonate resin, 5 to 25% by weight of an aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer, 7 to 18% by weight of a flame retardant, 3% by weight of an aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer, wherein the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer is polymerized by bulk polymerization.
The present invention also provides a molded article comprising the polycarbonate resin composition.
According to the present invention, there is provided an effect of providing a polycarbonate resin composition excellent in hydrolysis resistance in a high temperature and high humidity environment and a molded article containing the same, while providing mechanical properties and flame retardancy equal to or higher than those of the above.
Hereinafter, the present invention will be described in detail.
The present inventors have found that when a polycarbonate resin is alloyed with an aromatic vinyl compound-conjugated diene-based compound-vinyl cyanide copolymer, an aromatic group polymerized by bulk polymerization to minimize the residue of the polymerization process promoting hydrolysis When a certain amount of aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate is contained as a hydrolytic stabilizer using a vinyl compound-conjugated diene compound-vinyl cyan compound copolymer, And the present invention has been completed on the basis thereof.
The polycarbonate resin composition according to the present invention will be described in detail as follows.
From 5 to 25% by weight of an aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer, from 7 to 18% by weight of a flame retardant and from 1 to 3% by weight of a compatibilizing agent, wherein the aromatic vinyl The compound-conjugated diene compound-vinyl cyanide copolymer is characterized in that it is polymerized by bulk polymerization.
The polycarbonate resin is not particularly limited, and may be, for example, a resin polymerized by including a bisphenol-based monomer and a carbonate precursor.
Examples of the non-sprinol-based monomer include bis (4-hydroxyphenyl) methane, bis (4-hydroxyphenyl) ether, bis (4-hydroxyphenyl) sulfone, bis (4-hydroxyphenyl) sulfone, bis (4-hydroxyphenyl) ketone, 1,1-bis (4-hydroxyphenyl) ethane, 2,2-bis (4-hydroxyphenyl) propane (bisphenol A; BPA), 2,2-bis (4-hydroxyphenyl) butane, 1,1-bis (4-hydroxyphenyl) cyclohexane (bisphenol Z; BPZ) Propane, 2,2-bis (4-hydroxy-3-bromophenyl) propane, 2 (4-hydroxy-3-methylphenyl) propane, 2,2-bis (4-hydroxy-3-chlorophenyl) ) Propane, 1,1-bis (4-hydroxyphenyl) -1-phenylethane, bis (4-hydroxyphenyl) diphenylmethane and?,? Polydimethylsiloxane And an acid.
The carbonate precursor may be at least one selected from the group consisting of dimethyl carbonate, diethyl carbonate, dibutyl carbonate, dicyclohexyl carbonate, diphenyl carbonate, ditolyl carbonate, bis (chlorophenyl) carbonate, m-cresyl carbonate, dinaphthyl carbonate, bis Diphenyl carbonate), carbonyl chloride (phosgene), triphosgene, diphosgene, carbonyl bromide, and bishaloformate.
The polycarbonate resin may have a melt index (300 DEG C, 1.2 kg) of 5 to 25 g / 10 min, 8 to 23 g / 10 min, or 10 to 22 g / 10 min, Two or more kinds of carbonate resins can be used in combination. Within this range, excellent workability and moldability are obtained, and an excellent balance of physical properties is obtained. The melt index refers to the melt index measured under the standard measurement ASTM D1238 (300 DEG C, 1.2 kg).
The polycarbonate resin may have a weight average molecular weight of 30,000 to 100,000 g / mol, 30,000 to 70,000 g / mol, or 40,000 to 45,000 g / mol, for example, and has excellent tensile strength and elongation within this range.
The polycarbonate resin may include, for example, 55 to 85% by weight, 60 to 80% by weight, or 65 to 75% by weight of the polycarbonate resin composition, and has an excellent flowability and impact strength within this range .
As described above, the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer of the present invention is characterized by being polymerized by bulk polymerization. In this case, the residue of the polymerization process for promoting the hydrolysis is minimized and the hydrolysis resistance is excellent. In the case of emulsion polymerization, the chemical residues remaining in the emulsion polymerization process such as the emulsifier added during emulsion polymerization and the coagulant added during coagulation promote the hydrolysis of the polycarbonate resin, and therefore, the use thereof is excluded in the present invention.
The aromatic vinyl compound-conjugated diene compound-vinyl cyan compound copolymer may be, for example, a graft copolymer in which an aromatic vinyl compound and a vinyl cyan compound are graft-polymerized to a rubbery polymer polymerized including a conjugated diene compound In this case, a high melt index can be secured even at a low temperature.
The aromatic vinyl compound-conjugated dienic compound-vinyl cyan compound copolymer can be alloyed with the polycarbonate resin, for example, and in this case, it has an excellent balance of mechanical properties and physical properties.
The aromatic vinyl compound may be at least one selected from the group consisting of styrene,? -Methylstyrene, p-methylstyrene, o-ethylstyrene, p-ethylstyrene and vinyltoluene, and the aromatic vinyl compound- And may be contained in an amount of 50 to 80% by weight, 60 to 75% by weight, or 65 to 70% by weight based on the compound-vinyl cyanide copolymer. Within this range, a high melt index can be obtained even at a low temperature .
Examples of the conjugated diene compound include compounds derived from the group consisting of 1,3-butadiene, 2,3-dimethyl-1,3-butadiene, 2-ethyl-1,3-butadiene, 1,3-pentadiene, isoprene and chloroprene , And the rubber polymer polymerized by polymerizing the conjugated diene compound may be added in an amount of 5 to 30% by weight, 5 to 20% by weight, based on the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer, or 10 to 13% by weight, and an excellent balance of mechanical properties and physical properties within this range can be obtained.
The vinyl cyan compound may be at least one member selected from the group consisting of nitrile, methacrylonitrile, and ethacrylonitrile, and the aromatic vinyl compound-conjugated diene compound-vinyl cyan compound copolymer may be used in an amount of 10 to 30 wt% %, 10 to 25 wt.%, Or 15 to 20 wt.% Of the total weight of the composition. Within this range, there is an excellent balance of mechanical properties and physical properties.
The aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer may have a melt index (220 ° C, 10 kg) of 1 to 20 g / 10 min, 5 to 15 g / 10 min, or 7 to 10 g / 10 min. Within this range, excellent workability and moldability can be obtained within this range, and an excellent balance of physical properties can be obtained. The melt index refers to the melt index measured under the standard measurement ASTM D1238 (220 DEG C, 10 kg).
The aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer may have an average particle diameter of 0.1 to 10 μm, 0.5 to 5 μm, or 1 to 3 μm, for example. Within this range, a balance of mechanical properties and physical properties It has excellent effect.
The aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer may be contained in an amount of 5 to 25% by weight, 10 to 20% by weight, or 15 to 20% by weight based on the polycarbonate resin composition, In this case, a high melt index is secured even at a low temperature, and the residue of the polymerization process for promoting the hydrolysis is minimized, and the hydrolysis resistance is excellent.
The flame retardant is not particularly limited as long as it can be used in the polycarbonate resin composition, and may be, for example, a phosphorus-based flame retardant.
The phosphorus flame retardant may be, for example, 5 to 20 wt%, 7 to 15 wt%, or 8 to 9 wt% of phosphorus (P) relative to the phosphorus flame retardant.
The phosphorus flame retardant may be, for example, an aromatic phosphoric acid ester compound, and the aromatic phosphoric acid ester compound may be, for example, bisphenol A bis (dialkyl phosphate), bisphenol A bis (diaryl phosphate) or a mixture thereof. The alkyl group may be, for example, an alkyl group having 1 to 20 carbon atoms or a carbon number of 1 to 15, and the aryl group may be an aryl group having 6 to 30 carbon atoms or 6 to 20 carbon atoms.
The flame retardant may include, for example, from 7 to 18% by weight, from 8 to 15% by weight, or from 10 to 15% by weight of a flame retardant based on the polycarbonate resin composition and has excellent heat resistance, flame retardancy and fluidity within this range .
The compatibilizing agent acts as a hydrolytic stabilizer that prevents hydrolysis by preventing the polycarbonate resin composition from reacting with chain ends of the polycarbonate resin that is broken due to hydrolysis in the polycarbonate resin composition so as to prevent further decomposition, To minimize the contact between the resin in the resin composition and the moisture outside the resin composition to lower the hydrolysis rate. The hydrolysis stabilizer is not particularly limited as long as it can function as the hydrolysis stabilizer. Examples of the hydrolysis stabilizer include glycidyl Containing acrylic copolymer, and specific examples thereof may be an aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate copolymer.
The aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate copolymer may be, for example, a random copolymer, and the glycidyl (meth) acrylate may be an aromatic vinyl compound-vinyl cyan compound- 0.5 to 2.5% by weight, or 0.8 to 2.2% by weight, based on the total amount of the silyl (meth) acrylate copolymer, and has excellent hydrolysis resistance within this range.
The content of the aromatic vinyl compound and the vinyl cyan compound in the aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate copolymer may be within 100% by weight with the glycidyl (meth) acrylate Is not particularly limited, but it may be, for example, 10 to 90% by weight or 20 to 80% by weight, respectively.
The glycidyl (meth) acrylate may be, for example, glycidyl acrylate or glycidyl methacrylate.
For example, the compatibilizing agent may have a melt index (200 ° C, 5 kg) of 1 to 10, 2 to 9, 2 to 6, or 6 to 9, and within this range, an effect of excellent mechanical properties and hydrolysis resistance have.
The compatibilizing agent may be contained in an amount of 1 to 5% by weight, 1 to 4% by weight, or 1 to 3% by weight based on the polycarbonate resin composition. Within this range, an effect of excellent mechanical properties and hydrolysis resistance have.
For example, the polycarbonate resin composition may have a tensile strength retention (%) of 60% or more, 85% or more, or 100 to 110% after 500 hours of heat resistance humidity test (80 ° C and 85% , The tensile strength retention ratio (%) after elongation may be 10% or more, 20% or more, or 25 to 35%.
For example, the polycarbonate resin composition may have a elongation percentage (%) of 5% or more, 15% or more, or 20% to 30% after 500 hours of heat resistance humidity test (80 ° C, 85% The retention rate (%) may be 0.5% or more, 1% or more, or 1 to 5%.
The polycarbonate resin composition may be prepared, for example, from the group consisting of stabilizers, pigments, dyes, ultraviolet absorbers, antioxidants, colorants, release agents, lubricants, antistatic agents, fillers and plasticizers depending on the purpose, And may include at least one selected additive.
The molded article according to the present invention is characterized by including the polycarbonate resin composition.
The molded article may be an injection molded article, and may be a material for various containers such as a TV, a computer, a monitor, a copier, a scanner, a telephone, and the like.
It is to be understood that both the foregoing general description and the following detailed description of the present invention are exemplary and explanatory only and are not to be taken by way of illustration in the practice of the practice of this invention. And it is natural that such variations and modifications are included in the appended claims.
[Example]
Examples 1 to 4 and Comparative Examples 1 to 6
Acrylonitrile-butadiene-styrene copolymer (ABS 1) polymerized by bulk polymerization, acrylonitrile-butadiene-styrene copolymer (ABS 2) polymerized by emulsion polymerization, flame retardant, The compatibilizing agent 1 and the compatibilizing agent 2 were mixed using the super mixer at the contents (% by weight) shown in the following Table 1, and they were melted and melted at a temperature of 250 to 280 캜 using a twin-screw extruder. Kneaded and extruded to prepare a resin composition in the form of a pellet. The prepared pelletized resin composition was dried at 80 DEG C for 4 hours or more and injection molded to prepare a specimen. The specimen was left at room temperature (20 to 26 DEG C) for 48 hours or more, and the physical properties thereof were measured.
The respective components in Table 1 are as follows.
PC 1: A polycarbonate resin having a melt index of 22 g / 10 min (300 캜, 1.2 kg) and a weight average molecular weight of 41,000 g / mol
PC 2: A polycarbonate resin having a melt index of 10 g / 10 min (300 캜, 1.2 kg) and a weight average molecular weight of 50,000 g / mol
ABS 1: An acrylonitrile-butadiene-styrene copolymer (product name MA201, manufactured by LG Chemical Co., Ltd.) polymerized by a bulk polymerization having a melt index of 8 g / 10 min (220 캜, 10 kg)
ABS 2: acrylonitrile-butadiene-styrene copolymer (DP270E, product of LG Chemical Co., Ltd.) polymerized by emulsion polymerization, having a weight average molecular weight of 78,000 g /
* Flame retardant: bisphenol A bis (diphenylphosphate) (product name FP-700, manufactured by Asahi Denka Co., Ltd.)
* Commercialization 1: Styrene-acrylonitrile-glycidyl methacrylate three-way random copolymer (product name: SAG-001 manufactured by Nantong Sunny Polymer New Material Technology Co., Ltd.) having glycidyl methacrylate content of 1 ± 0.2 wt%
* Commercialization 2: Styrene-acrylonitrile-glycidyl methacrylate three-way random copolymer (product name: SAG-002, manufactured by Nantong Sunny Polymer New Material Technology Co., Ltd.) having glycidyl methacrylate content of 2 ± 0.2 wt%
[Test Example]
The physical properties of the polycarbonate resin composition specimens obtained in Examples 1 to 4 and Comparative Examples 1 to 6 were measured by the following methods, and the results are shown in Table 1 below.
How to measure
* Melt Index (g / 10 min): Standard Measurement The melt index of the polycarbonate resin was measured according to ASTM D1238 (300 ° C, 1.2 kg condition) and standard measurement ASTM D1238 (220 ° C, , The melt index of the acrylonitrile-butadiene-styrene copolymer was measured, and the melt index of the polycarbonate resin composition was measured according to the standard measurement ASTM D1238 (250 ° C, 2.16 kg).
* Weight average molecular weight (Mw, g / mol): Measured by PS standard using Agilent 1200 series GPC.
* Impact strength (Notched Izod, kgfcm / cm): Measured according to standard measurement ASTM D256 using 1/8 "specimen.
* Flame Retardancy (UL-94): The flame retardancy of specimens was measured by the UL-94 vertical combustion test method using UL Flame retardancy tester (FTT-0082) manufactured by FTT.
Tensile Strength (TS, kgf / cm 2 ): Measured according to standard measurement ASTM D638 using specimens.
* Elongation (TE,%): Standard measurement using sample. Measurement was made according to ASTM D638.
* Tensile Strength and Elongation after Heat Resistance Humidity Test: Heat resistance humidity test was conducted for 100, 500, 750 and 1,000 hours under the conditions of constant temperature and humidity 80 ° C. and humidity 85%. Tensile strength and tensile strength And elongation were measured.
* Tensile strength and elongation retention (%): Tensile strength and elongation after 500 hours and 1,000 hours of elongation before tensile strength and humidity resistance test are shown as percentage.
As shown in Table 1, in the case of Examples 1 and 4 prepared according to the present invention, even though the acrylonitrile-butadiene-styrene copolymer polymerized by the bulk polymerization was included, as compared with Comparative Example 3 containing no compatibilizing agent , The mechanical properties and the flame retardancy were maintained at the same level, and the hydrolysis resistance was very excellent.
On the other hand, in the case of Comparative Example 1 in which the polycarbonate resin itself was used, the flame retardancy was extremely poor. In Comparative Example 2 including the flame retardant together with the polycarbonate resin to improve the flame retardancy of such polycarbonate resin, It was confirmed that the decomposability was remarkably decreased.
Further, in Comparative Example 4 containing a small amount of a compatibilizing agent, the effect of improving the hydrolysis resistance was insignificant, and in Comparative Example 5 containing an excessive amount of the flame retardant, the hydrolysis resistance was also poor there was.
In addition, in Comparative Example 6 including an acrylonitrile-butadiene-styrene copolymer polymerized by emulsion polymerization, it was confirmed that even if a compatibilizing agent was included, the hydrolysis resistance was extremely poor.
From this, the present inventors have found that it is possible to minimize the residue of the polymerization process for promoting the hydrolysis from the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer polymerized by the bulk polymerization and to prevent the chain ends of the polycarbonate resin It is possible to realize a polycarbonate resin composition in which the hydrolysis resistance is remarkably improved without deteriorating the physical properties through the synergistic effect of the compatibilizing agent which prevents further decomposition.
Claims (18)
Wherein the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer is polymerized by bulk polymerization.
Wherein the polycarbonate resin has a melt index (300 DEG C, 1.2 kg) of 5 to 25 g / 10 min.
Wherein the polycarbonate resin has a weight average molecular weight of 30,000 to 100,000 g / mol.
Wherein the aromatic vinyl compound-conjugated diene compound-vinyl cyanide copolymer is a graft copolymer obtained by graft-polymerizing an aromatic vinyl compound and a vinyl cyan compound on a rubbery polymer polymerized with a conjugated diene compound, Carbonate resin composition.
Wherein the aromatic vinyl compound is at least one selected from the group consisting of styrene,? -Methylstyrene, p-methylstyrene, o-ethylstyrene, p-ethylstyrene and vinyltoluene.
Wherein the conjugated diene compound is selected from the group consisting of 1,3-butadiene, 2,3-dimethyl-1,3-butadiene, 2-ethyl-1,3-butadiene, 1,3-pentadiene, isoprene and chloroprene Polycarbonate resin composition.
Wherein the vinyl cyan compound is at least one selected from the group consisting of acrylonitrile, methacrylonitrile, and ethacrylonitrile.
Wherein the flame retardant is a phosphorus-based flame retardant.
Wherein the phosphorus flame retardant is an aromatic phosphoric acid ester compound.
Wherein the phosphorus flame retardant is bisphenol A bis (dialkyl phosphate), bisphenol A bis (diaryl phosphate) or a mixture thereof.
Wherein the compatibilizer is a glycidyl group-containing acrylic copolymer.
Wherein the glycidyl group-containing acrylic copolymer is an aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate copolymer.
Wherein the glycidyl (meth) acrylate is contained in an amount of 0.1 to 5% by weight based on the aromatic vinyl compound-vinyl cyan compound-glycidyl (meth) acrylate copolymer.
Wherein the polycarbonate resin composition has a tensile strength retention (%) of 60% or more after 500 hours of heat resistance humidity test (80 DEG C, 85% humidity).
Wherein the polycarbonate resin composition has a tensile strength retention (%) of at least 10% after 1,000 hours of heat resistance humidity test (80 DEG C, 85% humidity).
Wherein the polycarbonate resin composition has an elongation retention ratio (%) of 5% or more after 500 hours of heat resistance humidity test (80 DEG C, 85% humidity).
Wherein the polycarbonate resin composition has an elongation retention ratio (%) of at least 0.5% after 1,000 hours of heat resistance humidity test (80 DEG C, 85% humidity).
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Cited By (1)
Publication number | Priority date | Publication date | Assignee | Title |
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KR20200131024A (en) * | 2019-05-13 | 2020-11-23 | 더야오 탕 | halogen-free flame-retardant polycarbonate/ABS composite material |
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KR20200131024A (en) * | 2019-05-13 | 2020-11-23 | 더야오 탕 | halogen-free flame-retardant polycarbonate/ABS composite material |
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