Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Processes of preparing a desired or intentional composition...
Reexamination Certificate
2000-02-07
2003-05-20
Toomer, Cephia D. (Department: 1714)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Processes of preparing a desired or intentional composition...
C524S115000
Reexamination Certificate
active
06566428
ABSTRACT:
The present invention relates to polycarbonate/ABS moulding compositions which are rendered flame-resistant with phosphorus compounds and which have outstanding mechanical properties, in particular a high heat-resistance.
EP-A 0 640 655 describes moulding compositions consisting of aromatic polycarbonate, styrene-containing copolymers and graft polymers which can be rendered flame-resistant using monomeric and/or oligomeric phosphorus compounds.
EP-A 0 363 608 describes flame-resistant polymer mixtures consisting of aromatic polycarbonate, styrene-containing copolymer or graft copolymer as well as oligomeric phosphates as flame-resistant additives. For many applications, such as for example moulded articles inside housings, the heat resistance of these mixtures is often not adequate.
The object of the present invention is, therefore, to provide flame-resistant polycarbonate/ABS moulding compositions which have outstanding heat-resistance in addition to the high flame-resistance which is required.
Surprisingly, it has now been found that by using the mono- and/or oligo-phosphorus compounds according to the invention flame-resistant moulding compositions can be obtained which produce moulded items with very good mechanical properties and outstanding heat-resistance.
The present invention therefore provides flame-resistant, thermoplastic moulding compositions containing
A 5 to 95, preferably 10 to 90 parts by weight, in particular 20 to 80 parts by weight of aromatic polycarbonate or polyestercarbonate
B 1 to 60, preferably 1 to 40 parts by weight, in particular 2 to 30 parts by weight of at least 1 graft polymer of
B.1 5 to 95, preferably 20 to 60 wt. %, of one or more vinyl monomers on
B.2 5 to 95, preferably 40 to 80 wt. % of one or more graft substrates with a glass transition temperature below 10° C., preferably 0° C., in particular <−20° C. and an average particle size (d
50
value) of 0.05 to 5 &mgr;m, preferably 0.20 to 0.35 &mgr;m, in particular 0.25 to 0.30 &mgr;m.
C 0 to 50, preferably 1 to 30, in particular 2 to 25 parts by weight of a thermoplastic vinyl (co)polymer
D 0.5 to 20 parts by weight, preferably 1 to 18 parts by weight, in particular 2 to 15 parts by weight, of at least one phosphorus compound of the general formula (I)
in which
A independently of each other, represents halogen, preferably chlorine and/or bromine, a C
1
-C
8
alkyl, preferably C
1
-C
4
alkyl, in particular methyl, C
6
-C
10
aryl, preferably phenyl, or C
7
-C
12
aralkyl, preferably phenyl—C
1
-C
4
alkyl, in particular benzyl, group,
R
1
, R
2
, R
3
and R
4
, independently of each other, represent an optionally halogenated C
1
-C
8
alkyl group, or a C
5
-C
6
cycloalkyl, C
6
-C
20
aryl, or C
7
-C
12
aralkyl group, each optionally substituted by halogen and/or a C
1
-C
4
alkyl group,
y each, independently, is 0, 1, 2, 3 or 4,
n each, independently, is 0 or 1, preferably 1,
N is 0.3 to 30
and optionally further phosphorus compound(s) of the following formula (II)
in which the groups R
1
, R
2
, R
3
, R
4
, n and N are defined as above and
x represents a mononuclear or polynuclear aromatic group with 6 to 30 carbon atoms, with the exception of diphenyl,
E 0.05 to 5 parts by weight, preferably 0.1 to 1 part by weight, in particular 0.1 to 0.5 parts by weight of a fluorinated polyolefin,
wherein the sum of the parts by weight of all the components A+B+C+D+E is 100.
Component A
Aromatic polycarbonates and/or aromatic polyestercarbonates in accordance with component A which are suitable according to the invention are known from the literature or can be prepared by processes known from the literature (to prepare aromatic polycarbonates see for example Schnell “Chemistry and Physics of Polycarbonates” Interscience Publishers 1964 as well as 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; and to prepare aromatic polyestercarbonates, e.g. DE-OS 3 077 934).
Aromatic polycarbonates are prepared e.g. by reacting diphenols with carbonic acid halides, preferably phosgene, and/or with aromatic dicarboxylic acid dihalides, preferably benzene dicarboxylic acid dihalides, by the phase interface process, optionally using chain terminators, 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
1
represents a single bond, a C
1
-C
5
alkylene, C
2
-C
5
alkylidene, C
5
-C
6
cycloalkylidene, —O—, —SO—, —CO—, —S—, —SO
2
— or C
6
-C
12
arylene group, which may be fused to further aromatic rings which may optionally contain heteroatoms, or a group of the formula
or a group of the formula (V)
B independently of each other, represents a C
1
-C
8
alkyl, preferably C
1
-C
4
alkyl, in particular methyl, halogen, preferably chlorine and/or bromine, C
6
-C
10
aryl, preferably phenyl, C
7
-C
12
aralkyl, or phenyl-C
1
-C
4
alkyl, preferably benzyl, group,
x each, independently, is 0, 1 or 2,
p is 1 or 0 and
R
5
and R
6
can be individually chosen for each Z, and independently of each other, represent hydrogen or a C
1
-C
6
alkyl group, preferably hydrogen, methyl and/or ethyl,
Z is carbon, and
m is an integer, from 4 to 7, preferably 4 or 5,
with the proviso that R
5
and R
6
are both alkyl groups on at least one Z atom.
Preferred diphenols are hydroquinone, resorcinol, 4,4-dihydroxydiphenyl, 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, &agr;,&agr;-bis-(hydroxyphenyl)-diisopropyl-benzenes such as their ring-brominated and/or ring-chlorinated derivatives.
Particularly preferred diphenols are 4,4-diphenylohenol, 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 mixtures.
The diphenols are known from the literature or can be obtained using processes known from the literature.
Suitable chain terminators 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-(1,3-tetramethylbutyl)-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-di-tert-butylphenol, p-iso-octylphenyl, p-tert-octylphenol, p-dodecylphenol and 2-(3,5-dimethylheptyl)-phenol and 4-(3,5-dimethylheptyl)-phenol. The amount of chain terminators to be used is generally between 0.5 and 10 mol. %, with respect to the molar sum of the particular diphenols used.
The thermoplastic aromatic polycarbonates have average weight-averaged molecular weights (M
w
, determined e.g. by ultracentrifuge or light scattering measurements) of 10,000 to 200,000, preferably 20,000 to 80,000.
The thermoplastic aromatic polycarbonates may be branched in a known manner, in fact by the incorporation of 0.05 to 2.0 mol. %, with respect to the sum of diphenols used, of trifunctional or more than trifunctional compounds, for example those with three or more than three phenolic groups.
Homopolycarbonates or copolycarbonates are suitable. To prepare copolycarbonates according to the invention as component A, 1 to 25 wt. %, preferably 2.5 to 25 wt. % (with respect to the total amount of diphenols being used), of polydiorganosiloxanes with hydroxy-aryloxy terminal g
Alberts Heinrich
Eckel Thomas
Wittmann Dieter
Zobel Michael
Bayer Aktiengesellschaft
Gil Joseph C.
Preis Aron
Toomer Cephia D.
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