Solid anti-friction devices – materials therefor – lubricant or se – Lubricants or separants for moving solid surfaces and... – Organic nitrogen compound
Reexamination Certificate
2001-09-18
2003-12-02
Mullis, Jeffrey (Department: 1711)
Solid anti-friction devices, materials therefor, lubricant or se
Lubricants or separants for moving solid surfaces and...
Organic nitrogen compound
C508S567000, C508S577000, C524S210000, C524S230000, C524S504000
Reexamination Certificate
active
06656889
ABSTRACT:
CROSS REFERENCE TO RELATED PATENT APPLICATION
The present patent application claims the right of priority under 35 U.S.C. 119 (a)-(d) of German Patent Application No. 100 46 774.1, filed Sep. 21, 2000.
FIELD OF THE INVENTION
The present invention relates to compositions containing matrix polymer, graft polymer and unique additive mixtures. The present invention also relates to the production of molded articles, and molded articles prepared from the compositions of the present invention. The additive mixture is also a subject of the present invention.
BACKGROUND OF THE INVENTION
Acrylonitrile-butadiene-styrene graft copolymer (ABS) molding compositions have already been used for many years in large quantities as thermoplastic resins for the production of all types of molded parts. The property spectrum of these resins typically ranges from relatively brittle to extremely tough.
A special area of use of ABS molding compositions is the production of molded parts by injection molding (e.g., housings, toys and vehicle parts), in which it is an important factor that the polymer material have good flowability. Also, the molded parts produced in this way typically must have a good notched-bar impact strength as well as a good resistance to thermal stresses.
The object therefore exists of achieving, for a given rubber content, a given rubber particle size and given matrix resin molecular weight, toughness values that are as high as possible while retaining the good thermoplastic flowability. In this connection the high toughness values should as far as possible be obtained independently of the type of matrix resin that is employed, and especially when using the styrene/acrylonitrile copolymers and &agr;-methylstyrene/acrylonitrile copolymers typical of ABS.
One possible way of improving the toughness of ABS polymers with a given rubber content, given rubber particle size and given matrix molecular weight is to add special silicone oil compounds (see EP-A 6521). However, disadvantages associated with using silicone oil compounds include poor paintability, unsatisfactory printability or impaired yield stress values (danger of stress whitening). The addition of minor amounts of ethylene/propylene
on-conjugated diene (EPDM) rubber (see EP-A 412 370) or AES polymer (see EP-A 412 371) has also been described. Both methods require the use of considerable amounts of relatively expensive additive components however.
The use of large amounts of individual low molecular weight additive components, may in special cases improve the processability, although this is typically offset by a negative effect on other properties, such as toughness, modulus of elasticity and thermal stability.
SUMMARY OF THE INVENTION
In accordance with the present invention, there is provided a thermoplastic molding composition comprising:
A) 5 to 95 wt. % of a thermoplastic polymer selected from at least one of thermoplastic homopolymers, thermoplastic copolymers and thermoplastic terpolymers, said thermoplastic polymer being prepared from at least one monomer selected from styrene, &agr;-methylstyrene, nuclear-substituted styrene, methyl methacrylate, acrylonitrile, methyacrylonitrile, maleic anhydride and N-substituted maleimide;
B) 5 to 95 wt. % of at least one graft polymer prepared from,
B.1) 5 to 90 parts by weight of at least one monomer selected from styrene, &agr;-methylstyrene, nuclear-substituted styrene, methyl methacrylate, acrylonitrile, methyacrylonitrile, maleic anhydride and N-substituted maleimide, and
B.2) 10 to 95 parts by weight of at least one rubber having a glass transition temperature of ≦10° C.; and
C) 0.05 to 10 parts by weight, based on 100 parts of A+B, of a combination of at least three components selected from components (I), (II), (III) and (IV), wherein
component (I) has at least one structural unit represented by the following formula:
M being a metal, and
n being the valency of the metal M, component (II) has at least one structural unit represented by
and at least one structural unit represented by
component (III) has at least one structural unit represented by the following formula,
and
component (IV) is a compound different from those of components (I), (II) and (III), and is selected from at least one of: paraffin oils; hydrocarbon waxes; polystyrene produced by using C
8
-C
18
alkyl mercaptans as molecular weight regulators, and having a mean weight averaged molecular weight between 2000 and 15,000; styrene/acrylonitrile copolymer produced by using C
8
-C
18
alkyl mercaptans as molecular weight regulators, and having a mean weight averaged molecular weight of between 2000 and 15,000; &agr;-methylstyrene/acrylonitrile copolymer produced by using C
8
-C
18
alkyl mercaptans as molecular weight regulators, and having a mean weight averaged molecular weight of between 2000 and 15,000; and poly(methyl methacrylate) produced by using C
8
-C
18
alkyl mercaptans as molecular weight regulators, and having a mean weight averaged molecular weight of between 2000 and 15,000; C
6
-C
32
alkanols; and C
6
-C
32
alkenols.
In accordance with the present invention, there is further provided an additive composition which comprises at least three components selected from compounds (I), (II), (III) and (IV).
Other than in the operating examples, or where otherwise indicated, all numbers expressing quantities of ingredients, reaction conditions, etc. used in the specification and claims are to be under stood as modified in all instance by the term “about.”
DETAILED DESCRIPTION OF THE INVENTION
Preferably each of the components (I) to (IV) contains at least one terminal aliphatic C
6
-C
32
hydrocarbon radical.
According to the invention suitable examples of thermoplastic polymers A) include those prepared from monomers selected from styrene, &agr;-methylstyrene, p-methylstyrene, vinyltoluene, halogenated styrene, methyl acrylate, methyl methacrylate, acrylonitrile, maleic anhydride, N-substituted maleimide and mixtures thereof.
The polymers A) are resin-like, thermoplastic and rubber-free. Particularly preferred thermoplastic polymers A) include those prepared from the polymerization of: styrene; methyl methacrylate; styrene/acrylonitrile mixtures; styrene/acrylonitrile/methyl methacrylate mixtures; styrene/methyl methacrylate mixtures; acrylonitrile/methyl methacrylate mixtures; &agr;-methylstyrene/acrylonitrile mixtures; styrene/&agr;-methylstyrene/acrylonitrile mixtures; &agr;-methylstyrene/methyl methacrylate/acrylonitrile mixtures; styrene/&agr;-methylstyrene/methyl methacrylate mixtures; styrene/&agr;-methylstyrene/methyl methacrylate/acrylonitrile mixtures; styrene/maleic anhydride mixtures; methyl methacrylate/maleic anhydride mixtures; styrene/methyl methacrylate/maleic anhydride mixtures; and styrene/acrylonitrile/N-phenylmaleimide mixtures.
Polymers from which thermoplastic polymer A) may be selected are known and can be produced by free-radical polymerisation, in particular by emulsion, suspension, solution or bulk polymerisation. The polymers preferably have mean weight averaged molecular weights ({overscore (M)}
w
) of 20,000 to 200,000 and intrinsic viscosities (&eegr;) of 20 to 110 ml/g (measured in dimethylformamide at 25° C.).
Suitable rubbers B.2) (also referred to herein as “graft bases”) for the production of the graft polymers B) include, for example, polybutadiene, butadiene/styrene copolymers, butadiene/acrylonitrile copolymers, polyisoprene or alkyl acrylate rubbers based on C
1
-C
8
alkyl acrylates, in particular ethyl acrylate, butyl acrylate and ethylhexyl acrylate.
The acrylate rubbers, from which rubber B.2) may be selected, may optionally contain up to 30 wt. % (referred to the rubber weight) of monomers such as vinyl acetate, acrylonitrile, styrene, methyl methacrylate and/or vinyl ether incorporated by copolymerisation. The acrylate rubbers may also contain small amounts, preferably up to 5 wt. % (referred to the weight of rubber) of crosslinking, ethylenically unsaturated monomers incorporated by polymerisation. Crosslinking agents include, for
Bayer Aktiengesellschaft
Franks James R.
Gil Joseph C.
Mullis Jeffrey
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