WO1981001006A1 - Compositions resineuses possedant une tendance reduite a l'inflammation et une aptitude au traitement amelioree - Google Patents
Compositions resineuses possedant une tendance reduite a l'inflammation et une aptitude au traitement amelioree Download PDFInfo
- Publication number
- WO1981001006A1 WO1981001006A1 PCT/US1980/001317 US8001317W WO8101006A1 WO 1981001006 A1 WO1981001006 A1 WO 1981001006A1 US 8001317 W US8001317 W US 8001317W WO 8101006 A1 WO8101006 A1 WO 8101006A1
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- polymer
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Classifications
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- C—CHEMISTRY; METALLURGY
- C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
- C08K—Use of inorganic or non-macromolecular organic substances as compounding ingredients
- C08K13/00—Use of mixtures of ingredients not covered by one single of the preceding main groups, each of these compounds being essential
- C08K13/02—Organic and inorganic ingredients
-
- 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
Definitions
- organic halides are quite effective in providing styrene resins with a reduced tendency to ignite when an external heat source is applied, they generally do not reduce the tendency of polymers to drip while burning and, in order to cause the polymers to achieve a rating within the range of V-l to V-0, as provided under Subject 94, Underwriters Laboratories Tests For Flammability of Plastic Materials (hereinafter referred to as "UL-94"), a large amount of halide-containing compounds must be added.
- plasticizers and lubricating agents such as oils, waxes, fatty acids such a stearic acid, fatty acid derivatives such as butyl steara etc. It is also known that the addition of such additives while improving the melt flow behavior also detracts from such desirable polymer properties as tensile strength, tensile modulus, and heat distortion, thus creating a situation where a compromise of processability and physica properties must be accepted.
- O copolymers do not, however, significantly improve processability (high-shear flow). Therefore, plasticizers or lubricating agents may be added to improve processability. As stated above, the addition of these modifiers detracts from desirable polymer properties such as tensile strength and heat distortion, thereby leading to a compromise between processability and physical properties.
- butadiene an amorphous alpha-olefin polymer, a halide- -containing flame-retardant compound, and an antimony compound.
- fire-retardant polystyrene compositions which comprise a polystyrene component, a metal oxide (whi functions as a synergist in improving the efficiency of th halogen additive) and a fire-retardant halogen additive ar obtained by first mixing the metal oxide with a minor amou of the polystyrene component, subjecting the mixture to hi intensity mixing, comminuting the mixture, blending the co minuted mixture with the other ingredients of the composit compounding said blend, and comminuting said blend.
- An object of the present invention is to provide resinous compositions which have a reduced tendency to ignite when an external heat source is applied.
- a further object is to provide resinous compositions which have improved processability while maintaining desirable polyme qualities such as tensile strength and resistance to distortion at higher temperatures.
- resinous compositions having the said properties are obtained from physical mixtures of (A) from about 90.2 to about 65.3 parts by weight of rubber-reinforced styrene polymer; (B) from about 0 to about 10 parts by weight of a styrene-butadiene block copolymer having the configuration A(BA) , where n equals 1 to 3, and where A represents a styrene polymer block and B represents a butadiene polymer block, said block copolymer having a weight average molecular weight within the molecular weight range of about 50,000 -to about 500,000; (C) from about 0.2 to about 4 parts by weight of an olefin polymer wherein the copolymers such as ethylene-propylene have a specific gravity of from about 0.80 to about 0.98 and a Mooney Viscosity (ML-8 at 212° Farenheit or 100° Centigrade) of from about 25 to about 50 and the homopolymers such as polyethylene have
- Figures 1 and 2 represent, respectively, a two-dimensional display of UL-94 V-O ratings for various combinations of the block copolymer and alpha-olefin polymer components of the resinous composition and a representation of a three-dimensional figure wherein the Z-axis is added to project the values of Figure 1 onto varying test sample thicknesses.
- the Z-axis represents tes sample thickness.
- Figure 3 is a two-dimensional plot of Shear Rheology (Instron Drive) information at 160°C for various combinations, in accordance with the invention, of block copolymers and/or olefin polymers of crosshead speed (inches/minute) versus pounds of force.
- Shear Rheology Instron Drive
- Figure 4 is a two-dimensional plot of Shear Rheology (Instron Drive) information at 160°C for various combinations, in accordanc with the invention, of block copolymers and/or olefin polymers of shear rate (seconds- ) versus apparent viscosit (poise).
- Figure 5 is a two-dimensional plot of Shear Rheology (Ametek Drive) information at 160°C for various combinations, in accordance with the invention, of block copolymers and olefin polymers of shear rate (seconds " ) versus apparent viscosity (poise).
- Figure 6 is a two-dimensional plot of Shear Rheology (Instron Drive) information at 160°C for various combinations, in accordanc with the invention, of block copolymers and olefin polymers of shear rate (seconds " ) versus apparent viscosity (poise).
- the Component (A) preferably comprises impact- resistant interpolymers or graft copolymers of monovinyl aromatic compounds having the vinyl radical directly at ⁇ tached to a carbon atom of the aromatic nucleus, e.g., styrene, with a minor proportion of a natural or synthetic rubber, e.g., butadiene.
- the rubber is preferably dispersed in the form of a plurality of particles, a majority of which have diameters within the range of from about 0.2 to 5 microns, and, within said plurality of particles, at least a majority of the particles have monovinyl aromatic polymer occluded therein. More preferably, Component (A) comprises
- O ⁇ .IPI from about 65.3 to about 90.2 parts by weight of impact resistant interpolymers or graft copolymers of a styrene matrix with a minor proportion of butadiene rubber dispersed in the form of a plurality of particles, a majority of which have diameters within the range of from about 0.2 to about 5 microns, and within said plurality of particles, at least a majority of the particles have styrene polymer occluded therein, wherein the molecular weight of the styrene matrix is from about 100,000 to about 500,000.
- Component (A) comprises from about 65.3 to about 90.2 parts by weight of interpolymers or graft copolymers of a styrene matrix with about 7.2 weight percent polybutadiene rubber dispersed in the form of a plurality of particles, a majority of the polybutadiene rubber particles have diameters within the range of from about 0.2 to about 5 microns, and within said plurality of polybutadiene rubber particles, at least a majority have styrene polymer occluded therein, wherein the molecular weight of the styrene matrix is about 190,000. Impact resistant styrene polymers are well-known items of commerce.
- Suitable methods of making the preferred interpolymers or graft copolymers can be found in Amos et al. (US Patent No. 2,694,692), Ruffing et al. (US Patent No. 3,243,481) and McCurdy et al. (US Patent No. 3,945,976), the teachings of which are herein incorporated by reference thereto.
- Another suitable method of producing Component (A) can be found in Ostromislen ⁇ ky (US Patent No. 1,613,673), the disclosure of which is herein incorporated by reference.
- the Component (B) is comprised preferably of block copolymers of the configuration A-B-A wherein A represents polymer blocks of an alkenyl-substituted aromatic hydro ⁇ carbon, e.g., styrene, and B represents polymer blocks of conjugated dienes, e.g., butadiene, said block copolymer containing from about 10 to about 50 percent by weight of A and from about 90 to about 50 percent by weight of B.
- A represents polymer blocks of an alkenyl-substituted aromatic hydro ⁇ carbon, e.g., styrene
- B represents polymer blocks of conjugated dienes, e.g., butadiene
- the Component (B) is comprised of block copolymers of the configuration A(BA) , where n equals 1 to 3, A represents styrene, B represents butadiene, and the percent by weight ratio of styrene to butadiene of from about 10:90 to about 50:50, which have a weight average molecular weight, as determined by gel permeation chromatography, within the molecular weight range of from about 50,000 to about 500,000 and in an amount within the range of from about 0.8 to about 10 parts by weight when the object is to produce resinous compositions which have a reduced tendency to ignite when an external heat source is applied and from about 0 to about 10 parts by weight when the object is to provide physical blends which have improve processability while maintaining desirable polymer properties such as tensile strength and resistance to distortion at higher temperatures.
- A represents styrene
- B represents butadiene
- the percent by weight ratio of styrene to butadiene of from about 10:90 to about 50:50,
- the Component (B) is comprised of styrene-butadiene block copolymers of the configuration A(BA) , where A and B respectively are polymer blocks of styrene and butadiene and n equals 1 to 3 and the percent by weight ratio of styrene to butadiene is from about 10:90 to about 50:50, which have a weight average molecular weight, as determined by gel permeation chromatography, within the molecular weight range of from about 60,000 to about 300,000, in an amount within the range of from about 1.8 to about 4.3 parts by weight when the object is to produce resinous compositions which have a reduced tendency to ignite when an external heat source is applied and from about 0 to about 4.3 parts by weight when the object is to provide physical blends which have improved processability while maintaining desirable polymer properties as tensile strength and resistance to distortion at higher temperatures.
- the block copolymer contains from about 10 to about 50 percent by weight styrene and from about 90 to about 50 percent by weight butadiene.
- Suitable methods of making block copolymers can be found in Holden et al. (US Patent No. 3,231,635) and Zellin ⁇ ki (US Patent Nos. 3,251,905 and 3,287,333), the teachings of which are herein incorporated by reference.
- the Component (C) preferably comprises from about
- an olefin polymer/copolymer wherein the copolymers such as ethylene-propylene have a specific gravity of from about 0.80 to about 0.98 and a Mooney Viscosity (ML-8 at 212° Farenheit or 100° Centigrade) of about 25 to 50 and the homopolymers such as polyethylene have a density of from about 0.80 to about 0.98 and a Melt Index determined in accordance with American Society for Testing Materials (hereinafter referred to as ASTM) D-1238 of from about 5 to about 50.
- ASTM Melt Index determined in accordance with American Society for Testing Materials
- the Component (C) comprises from about 0.2 to about 4 parts by weight of an alpha-olefin polymer/copolymer having polymerized therein from about 0 to about 100 percent by weight of ethylene and from about 10& to about 0 percent by weight of a copolymerizable ethylenically unsaturated monomer, wherein the copolymers such as ethylene-propylene have a specific gravity of from about 0.80 to about 0.98 and a Mooney Viscosity (ML-8 at 212° Farenheit or 100° Centigrade) of from about 25 to about 50 and the homopolymers such as polyethylene have a density of from about 0.80 to about 0.98 and a Melt Index determined in accordance with American Society for Testing Materials (hereinafter referred to as ASTM) D-1238 of from about 5 to about 50. Still more
- the Component (C) comprises from about 0.2 to about 4 parts by weight of an amorphous alpha-olefin polyme copolymer having polymerized therein from about 0 to about 100 percent by weight of ethylene and from about 100 to about 0 percent by weight of a copolymerizable ethylenicall unsaturated monomer such as propylene or acrylic acid, wherein the copolymers such as ethylene-propylene have a specific gravity of from about 0.80 to about 0.98 and a Moo Viscosity (ML-8 at 212° Farenheit or 100° Centigrade) of from about 25 to about 50 and the homopolymers such as poly ethylene have a density of from about 0.80 to about 0.98 an a Melt Index determined in accordance with ASTM-D-1238 of from about 5 to about 50.
- an amorphous alpha-olefin polyme copolymer having polymerized therein from about 0 to about 100 percent by weight of ethylene and from about 100 to about 0 percent
- the Component (C) comprises from about 0.3 to about 1.3 parts by weight of an amorphous alpha-olefin polymer/copolymer having poly ⁇ merized therein from about 0 to about 100 percent by weight of ethylene and from about 100 to about 0 percent by weight of propylene wherein the copolymers of ethylene-propylene have a specific gravity of from about 0.84 to about 0.95 and a Mooney Viscosity (ML-8 at 212° Farenheit or 100° Centigrade) of from about 29 to about 44 and the homo ⁇ polymers of polypropylene and polyethylene have a density of from about 0.84 to about 0.95 and a Melt Index determine in accordance with ASTM-D-1238 of from about 7 to about 42.
- an amorphous alpha-olefin polymer/copolymer having poly ⁇ merized therein from about 0 to about 100 percent by weight of ethylene and from about 100 to about 0 percent by weight of propylene
- alpha-olefin polymers/copolymers can be found in Reding et al. (US Patent No. 3,197,449),- Schmid et al. (US Patent No. 3,300,457), Anspon et al. (US Patent No. 3,485,812), Thomson et al. (US Patent No. 3,520,861), and Shurts (US Patent No. 3,912,698), the disclosures of which are herein incorporated by reference.
- the Component (D) preferably comprises a halide- containing organic ignition retardant. More preferably, th
- O PI Component (D) comprises a halide-containing ignition retardant which is generally well-known in the art selected from the group represented by Formulae (I) to (VI).
- the Component (D) comprises from about 7 to about 20 parts by weight of a bromine- containing ignition retardant selected from the group consisting of hexabromodiphenyl ether, octabromodiphenyl ether, decabromodiphenyl ether, l,2-bis(tribromophenoxy)- ethane, 1,2-bis(pentabromophenoxy)ethane, tetrabromo bi ⁇ phenol-A, ethylene(N,N' )-bis-tetrabromophthalimide, tetrabromophthalic anhydride, and hexabromobenzene.
- the Component (D) comprises from about 9 to about 15 parts by weight of decabromodiphenyl ether(decabromodiphen oxide).
- Barkhuff, Jr. et al. U.S. Patent No. 4,069,288
- Barkhuff, Jr. et al. U.S. Patent No. 4,069,288
- the Component (E) preferably comprises a metal oxide synergist, such as antimony trioxide, bismuth tri-
- the Component (E) comprises from about 2 to about 6 parts by weight of antimony trioxide. Most preferably, the Component (E) comprises from about 2.5 to about 5 parts by weight of antimony trioxide. Methods of incorporating the antimony compound can be found in Bethea et al. (US Patent No. 3,988,296), the disclosure of which is herein incorporated by reference.
- the ingredients may be blended by any of the conventional melting and mixing apparatuses which will result in a generally uniform dispersion of all ingredients throughout the resulting product.
- Illustrative apparatuses include Banbury mixers, compounding rolls, single screw extruders, twin screw extruders, etc.
- the preferred apparatus is the twin screw extruder.
- the ingredients may either be combined in an apparatus such as a dry blender before being fed into the mixing and melting extruding apparatus or two or more of the ingredients may be pre-mixed and fed as a stream into the hot melt of the remaining ingredients.
- the preferred technique involves premixing a small amount of the impact resistant styrene polymer with the metal oxide (which has a synergistic effect in improving ' the efficiency of the halogen additive) and the halogen- containing additive, and feeding this as a separate stream from the remaining ingredients into a twin screw extruder.
- Viscosity (ML-8 at 212°F (100°C)) of 36 whi is comme ⁇ cally available under the trade
- OMPI D A styrene-butadiene linear block copoly ⁇ mer with a weight ratio of butadiene to styrene of 72 to 28 copolymerized therein and a weight average molecular weight of about 66,000 which is commerically available under the trade designation KRATON 2103 sold by Shell Chemical Company.
- a low density polyethylene with a melt index determined in accordance with ASTM- -D-1238, Condition E, of 35, and a density of about .92, which is commercially available as
- G A polymer of ethylene and acrylic acid with a weight ratio of ethylene to acrylic acid of 92 to 8 copolymerized therein, a density of about .93, and a Melt Index determined in accordance with ASTM-D-1238, Condition E, of 9, which is commercially available as Dow EAA Resin 459 sold by The Dow Chemical Company.
- OMPI H A low density polypropylene having a densit of about .90, with a flow rate determined i accordance with ASTM-D-1238, Condition L, o 12, which is commerically available under t ttrraaddee ddeessiiggnnaaltion PROFAX 6331 sold by Hercules, Inc.
- Examples 1 to 26 were prepared for testing by me compounding the additives specified in Table 1 below into Component J on a two-roll mill with a roll temperature of about 340° Farenheit and then compression molding the resultant composition, of the additives and Component J, in accordance with ASTM-D-638-77, at a temperature of about 390° Farenheit under a pressure of about 25,000 pounds per square inch, into samples of the size specified by Underwriter's Laboratory Tests for Flammability of Plastic Materials (UL-94) of 1/2 inch by 6 inches.
- the sample thicknesses are set forth in Table 1.
- Table 1 The data presented in Table 1 is graphically portrayed in Figure 1, a two-dimensional display which reflects the variations in amounts of A and B, and Figure a three-dimensional display which projects the UL-94, V-O ratings achieved by variations in amounts of A and B onto the Z-axis which represents sample thickness.
- Examples 27-32 were prepared for testing by twic extruding the additives and Component J on a 0.8 inch twin screw extruder, manufactured by Welding Engineers, Inc., a a speed of about 200 revolutions per minute and a barrel temperature of about 400° Farenheit and then compression molding the resultant composition, of the additives and Component J, in accordance with ASTM-D-638-77, at a temperature of about 390° Farenheit under a pressure of ab 25,000 pounds per square inch, into samples of the size specified by Underwriter's Laboratory Tests for Flammabili of Plastic Materials (UL-94) of 1/2 inch by 6 inches.
- the sample thicknesses are set forth in Table 2.
- Examples 33 to 41 were prepared for testing by melt compounding the additives (ignition retardants plus 3 percent B and 1 percent A) into the Component I, either by the two-roll mill process used for Examples 1 to 26 above (hereinafter referred to as Process R) or by the twin scre process used for Examples 27 to 32 above (hereinafter referred to as Process S). These processes are referred t by their letter designation in Table 3.
- Examples 33 to 41 contain varying levels of the preferred ignition-retardant additives, decabromodiphenyl oxide and antimony trioxide, as reflected in Table 3 below with a weight ratio of decabromodiphenyl oxide to antimony trioxide of about 3.5 to 1 in each example.
- Examples 42 to 48 were prepared for testing by Process S (see Example 27). The tests used to evaluate certain physical properties are set forth in the following key:
- Tensile Yield Tensile Yield - measured in accordance with ASTM-D-638-77 in units of pounds per square inch.
- Tensile Rupture Tensile Rupture - measured in accordance with ASTM-D-638-77 in units of pounds per square inch.
- the Rheology (Instron Drive) data for Examples 42 to 48 was determined using an Instron Rheometer with a melt temperature of 160° Centigrade, a die diameter of 0.05 inch, and a die length of 1.005 inches and an Instron Model TTC drive unit produced by Instron Engineering Corporation. The data obtained is set forth in Table 5.
- Examples 49 to 52 were prepared for testing by Process S (see Example 1).
- the Rheology (Ametek drive) data for Examples 49 to 52 was determined using an Instron Rheometer, a melt temperature of 160° Centigrade, a die diameter of 0.05 inch, and a die length of 1.005 inches, and an Ametek Model LRS-20 drive unit produced by Ametek Testing Equipment Systems. The data obtained is set forth in Table 6.
- Examples 53 to 55 were prepared for testing by Process S (see Example 27). The tests used to evaluate
- the Rheology (Instron Drive) data for Examples 53 to 55 was determined using an Instron Rheometer with a melt temperature of 160° Centigrade, a die diameter of 0.05 inch and a die length of 1.005 inches and an Instron Model TTC drive unit produced by Instron Engineering Corporation. The data obtained is set forth in Table 8.
- Table 8 The data presented in Table 8 is graphically portrayed in Figure 6 which is a plot of curves based on contrasting the parameters of apparent viscosity (poise) and shear rate (seconds ).
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Abstract
Compositions resineuses possedant une tendance reduite a l'inflammation lorsqu'une source exterieure de chaleur est appliquee, et une aptitude au traitement amelioree en termes d'ecoulement en cisaillement, de telles compositions comprenant un polymere de styrene renforce par du caoutchouc, copolymere en bloc de styrene-butadiene (facultatif pour ameliorer le flux), un polymere d'olefine, un retardateur d'inflammation contenant des halogenures et un compose d'antimoine.
Priority Applications (1)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
AU63996/80A AU6399680A (en) | 1979-10-09 | 1980-10-07 | Resinous compositions having reduced tendency to ignite and improved processability |
Applications Claiming Priority (2)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
US8303279A | 1979-10-09 | 1979-10-09 | |
US83032 | 1979-10-09 |
Publications (1)
Publication Number | Publication Date |
---|---|
WO1981001006A1 true WO1981001006A1 (fr) | 1981-04-16 |
Family
ID=22175738
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
PCT/US1980/001317 WO1981001006A1 (fr) | 1979-10-09 | 1980-10-07 | Compositions resineuses possedant une tendance reduite a l'inflammation et une aptitude au traitement amelioree |
Country Status (3)
Country | Link |
---|---|
EP (1) | EP0039357A4 (fr) |
JP (1) | JPS56501369A (fr) |
WO (1) | WO1981001006A1 (fr) |
Cited By (3)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB2232677A (en) * | 1989-06-08 | 1990-12-19 | Labofina Sa | Impact resistant polymeric composition |
WO1997018262A1 (fr) * | 1995-11-14 | 1997-05-22 | The Dow Chemical Company | Compositions ignifuges a base de polymeres modifies au caoutchouc |
JP2015081340A (ja) * | 2013-10-24 | 2015-04-27 | 東洋スチレン株式会社 | 樹脂組成物およびそれからなる成形体 |
Families Citing this family (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JP6328404B2 (ja) * | 2013-10-23 | 2018-05-23 | 東洋スチレン株式会社 | スチレン系難燃性樹脂組成物およびそれからなる成形体 |
Citations (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4219466A (en) * | 1978-11-09 | 1980-08-26 | Asahi-Dow Limited | Impact resistant resin containing compositions having reduced flammability |
Family Cites Families (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
JPS53149244A (en) * | 1977-06-01 | 1978-12-26 | Asahi Chem Ind Co Ltd | Resin composition |
-
1980
- 1980-10-07 EP EP19800902101 patent/EP0039357A4/fr not_active Withdrawn
- 1980-10-07 JP JP50254780A patent/JPS56501369A/ja active Pending
- 1980-10-07 WO PCT/US1980/001317 patent/WO1981001006A1/fr not_active Application Discontinuation
Patent Citations (1)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US4219466A (en) * | 1978-11-09 | 1980-08-26 | Asahi-Dow Limited | Impact resistant resin containing compositions having reduced flammability |
Non-Patent Citations (1)
Title |
---|
See also references of EP0039357A4 * |
Cited By (5)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
GB2232677A (en) * | 1989-06-08 | 1990-12-19 | Labofina Sa | Impact resistant polymeric composition |
GB2232677B (en) * | 1989-06-08 | 1993-06-30 | Labofina Sa | Polymeric material composition |
WO1997018262A1 (fr) * | 1995-11-14 | 1997-05-22 | The Dow Chemical Company | Compositions ignifuges a base de polymeres modifies au caoutchouc |
US6372831B1 (en) | 1995-11-14 | 2002-04-16 | The Dow Chemical Company | Flame resistant rubber modified polymer compositions |
JP2015081340A (ja) * | 2013-10-24 | 2015-04-27 | 東洋スチレン株式会社 | 樹脂組成物およびそれからなる成形体 |
Also Published As
Publication number | Publication date |
---|---|
EP0039357A1 (fr) | 1981-11-11 |
JPS56501369A (fr) | 1981-09-24 |
EP0039357A4 (fr) | 1982-03-29 |
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