Flame-resistant polycarbonate blends

Details Flame-resistant polycarbonate blends Flame-resistant polycarbonate blends

2002-02-27

2004-08-31

Szekely, Peter (Department: 1714)

Synthetic resins or natural rubbers -- part of the class 520 ser

Synthetic resins

Processes of preparing a desired or intentional composition...

C524S108000, C524S139000

Reexamination Certificate

active

06784232

ABSTRACT:

The present invention provides blends which contain phosphonate amines and are based on polycarbonate and graft polymers selected from the group consisting of silicone, EP(D)M and acrylate rubbers as graft substrate, which have exceptional flame resistance and very good mechanical properties such as stress cracking resistance or ease of flow while exhibiting high heat resistance.
U.S. Pat. Nos. 4,073,767 and 5,844,028 describe cyclic phosphorus compounds including phosphorinane rings as suitable flame retardants for polyurethanes, polycarbonates, polyesters and polyamides. In U.S. Pat. No. 4,397,750, specific cyclic phosphonate esters are described as efficient flame retardants for polypropylene and other polyolefins. U.S. Pat. No. 5,276,066 and U.S. Pat. No. 5,844,028 describe specific (1,3,2-dioxaphosphorinanemethane) amines which are suitable flame retardants for polyurethanes, polyesters, styrene polymers, PVC, PVAc or polycarbonate.
U.S. Pat. No. 3,505,431, FR-P 1 371 139, U.S. Pat. No. 3,711,577, U.S. Pat. No. 4,054,544 describe acyclic triphosphonate amines, some of which are halogenated.
EP-A 0 640 655 describes moulding compositions made from aromatic polycarbonate, styrene-containing copolymers and graft polymers which can be made flame resistant with monomeric and/or oligomeric phosphorus compounds.
EP-A 0 363 608 describes flame resistant polymer mixtures made from aromatic polycarbonate, styrene-containing copolymers or graft copolymers and also oligomeric phosphates as a flame resistant additive. For many applications such as, for example, in the internal sections of housings, the heat resistance of these mixtures is often inadequate.
U.S. Pat. No. 5,061,745 describes polymer mixtures made from aromatic polycarbonate. ABS graft polymers and/or styrene-containing copolymers and with monophosphates as flame retardant additives. For the production of thin-walled housing parts, the level of stress cracking resistance of these mixtures is often inadequate.
The object of the present invention is the provision of polycarbonate blends with exceptional flame resistance and exceptional mechanical properties such as stress cracking resistance, processability and ease of flow. This range of properties is demanded in particular for applications in the data processing sector such as, for example, for housings of monitors, printers, copiers, etc.
It has now been found that blends based on polycarbonate and graft polymers selected from the group consisting of silicone, EP(D)M and acrylate rubbers which contain phosphonate amines have the required properties.
The invention therefore provides blends which contain polycarbonate and/or polyestercarbonate, at least one rubber-elastic graft polymer selected from the group consisting of silicone, EP(D)M and acrylate rubbers as graft substrate and 0.1 to 30 parts by weight (with respect to the entire mixture) of phosphonate amine of the formula (I)
A
3-y
—N—B
y
  (I),
in which
A represents a group of the formula (IIa)
R
1
and R
2
, independently, represent an unsubstituted or substituted C
1
-C
10
alkyl group or an unsubstituted or substituted C
6
-C
10
aryl group,
R
3
and R
4
, independently, represent an unsubstituted or substituted C
1
-C
10
alkyl group or an unsubstituted or substituted C
6
-C
10
aryl group or
R
3
and R
4
together represent an unsubstituted or substituted C
3
-C
10
alkylene group,
y has the numerical value 0,1 or 2 and
B independently, represents hydrogen, an optionally halogenated C
2
-C
8
alkyl group, or an unsubstituted or substituted C
6
-C
10
aryl group.
The invention preferably provides thermoplastic moulding compositions (blends) containing
A) 40 to 99, preferably 60 to 98.5 parts by wt. of an aromatic polycarbonate and/or polyestercarbonate.
B) 0.5 to 60, preferably 1 to 40, in particular 2 to 25 parts by wt. of at least one rubber-elastic graft polymer, selected from the group consisting of silicone, EP(D)M and acrylate rubbers as graft substrate,
C) 0 to 45, preferably 0 to 30, in particular 2 to 25 parts by wt. of at least one thermoplastic polymer, selected from the group consisting of vinyl (co)polymers and polyalkylene terephthalates,
D) 0.1 to 30 parts by wt., preferably 1 to 25 parts by wt., in particular 2 to 20 parts by wt. of phosphonate amine of the formula (I)
A
3-y
—N—B
y
  (I),
 in which
 A, B and y are defined in the same way as above, and
E) 0 to 5, preferably 0.1 to 3, in particular 0.1 to 1 parts by wt., quite specifically 0.1 to 0.5 parts by wt. of a fluorinated polyolefin,
wherein the sum of the parts by weight of all the components is 100.
Component A
Aromatic polycarbonates and/or aromatic polyestercarbonates suitable for use according to the invention in accordance with component A are known from the literature or can be prepared by methods known from the literature (to prepare aromatic polycarbonates see, for example, Schnell, “Chemistry and Physics of Polycarbonates”, Interscience Publishers, 1964 and DE-AS 1 495 626, DE-OS 2 232 877, DE-OS 2 703 376, DE-OS 2 714 544, DE-OS 3 000 610, DE-OS 3 832 396; to prepare aromatic polyestercarbonates see, for example, DE-OS 3 077 934).
Polycarbonates are prepared, for example, by reacting diphenols with carbonic acid halides, preferably phosgene and/or with aromatic dicarboxylic acid dihalides, preferably benzenedicarboxylic acid dihalides, by the phase interface method, optionally using chain stoppers; for example monophenols, and optionally using trifunctional or more than trifunctional branching agents, for example triphenols or tetraphenols.
Diphenols for preparing aromatic polycarbonates and/or aromatic polyestercarbonates are preferably those of the formula (III)
wherein
A represents a single bond, a C
1
-C
5
alkylene, C
2
-C
5
alkylidene, C
5
-C
6
cycloalkylidene, —O—, —SO—, -CO—, —S—, —SO2, or C
6
-C
12
arylene group, to which further aromatic rings, optionally containing heteroatoms, may be condensed,
 or a group of the formula (IV) or (V)
B each represent a C
1
-C12 alkyl group, preferably methyl or a halogen, preferably chlorine and/or bromine,
x each represent, independently, 0,1 or 2,
p is 1 or 0 and
R
7
and R
8
can be chosen independently for each X
1
and represent, independently, hydrogen or a C
1
-C
6
alkyl group, preferably hydrogen, methyl or ethyl,
X
1
represents carbon and
m is an integer from 4 to 7, preferably 4 or 5, with the proviso that R
7
and R
8
are simultaneously alkyl groups on at least one X
1
atom.
Preferred diphenols are hydroquinone, resorcinol, dihydroxydiphenols, bis-(hydroxyphenyl)-C
1
-C
5
-alkanes, bis-(hydroxyphenyl)-C
5
-C
6
-cycloalkanes, bis-(hydroxyphenyl)-ethers, bis-(hydroxyphenyl)-sulfoxides, bis-(hydroxyphenyl)-ketones, bis-(hydroxyphenyl)-sulfones and &agr;,&agr;-bis-(hydroxyphenyl)-diisopropyl-benzenes and their ring-brominated and/or ring-chlorinated derivatives.
Particularly preferred diphenols are 4,4′-dihydroxydiphenyl, bisphenol-A, 2,4-bis-(4-hydroxyphenyl)-2-methylbutane, 1,1-bis-(4-hydroxyphenyl)-cyclohexane, 1,1-bis-(4-hydroxyphenyl)-3,3,5-trimethylcyclohexane, 4,4′-dihydroxydiphenyl sulfide, 4,4′-dihydroxydiphenyl sulfone and their di- and tetrabrominated or chlorinated derivatives such as, for example, 2,2-bis-(3-chloro-4-hydroxyphenyl)-propane, 2,2-bis-(3,5-dichloro-4-hydroxyphenyl)-propane or 2,2-bis-(3,5-dibromo-4-hydroxyphenyl)-propane.
2,2-bis-(4-hydroxyphenyl)-propane (bisphenol-A) is particularly preferred.
The diphenols may be used individually or as any mixture thereof.
The diphenols are known from the literature or are obtainable by methods known from the literature.
Chain stoppers which are suitable for preparing thermoplastic, aromatic polycarbonates are, for example, phenol, p-chlorophenol, p-tert.-butylphenol or 2,4,6-tribromophenol, but also long-chain alkylphenols such as 4-(1,1,3,3-tetamethylbutyl)-phenol in accordance with DE-OS 2 842 005 or monoalkylphenols or dialkylphenols with a total of 8 to 20 carbon atoms in the alkyl substituents, such as 3,5-tert.-butylphenol, p-iso-octylphenol,

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