Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Mixing of two or more solid polymers; mixing of solid...
Reexamination Certificate
2001-06-21
2004-04-20
Woodward, Ana (Department: 1711)
Synthetic resins or natural rubbers -- part of the class 520 ser
Synthetic resins
Mixing of two or more solid polymers; mixing of solid...
C525S074000, C525S186000, C525S203000, C525S205000, C525S206000
Reexamination Certificate
active
06723790
ABSTRACT:
FIELD OF THE INVENTION
Polymers containing repeat units derived from &agr;-methylenelact(ones)(ams) such as &agr;-methylenebutyrolactones and which have reactive groups are toughened by mixing with a rubbery material which has complimentary reactive groups, or polymers containing repeat units derived from &agr;-methylenelact(ones)(ams) are toughened by mixing with polymeric core-shell particles having an elastomeric core and a specified thermoplastic shell; or blends of polymers containing repeat units derived from &agr;-methylenelact(ones)(ams) with thermoplastics often yield compositions which have a higher modulus and/or heat deflection temperature than the thermoplastic alone.
TECHNICAL BACKGROUND
Thermoplastics comprise a large body of commercially important products. Among the uses of thermoplastics are those in which the optical properties of the polymer are important, particularly when the polymer is an optically clear material with little distortion of optical images. Such polymers, for example poly(methyl methacrylate) (PMMA) and certain polycarbonates are used as substitutes for glass where toughness is important. In uses such as for safety glazing and signage, other properties such as weather and/or heat resistance may also be important. For example if such a part needed to be thermally sterilized, it must withstand the temperature of the sterilization process. Polycarbonates often have poor weathering and/or hydrolysis resistance, while PMMA has a relatively low glass transition temperature (Tg), so its heat resistance is poor. Thus polymers with a combination of good optical properties, and heat and weathering resistance are desired.
The polymers of certain &agr;-methylenelact(ones)(ams) (AMLs) have the combination of good properties, but often are quite brittle, see for instance U.S. Pat. No. 5,880,235, and the discussion at columns 1-3, and D. Arnoldi, et al., Kunststoffe, vol. 87, p. 734-736 (1997). Thus if one could toughen these polymers without compromising their other superior properties, useful compositions would result.
While the toughening of AMLs using toughening agents is in the Applicant's knowledge not reported in the literature, toughening of thermoplastics in general using toughening agents is known. For example, poly(meth)acrylates have been toughened by a number of methods, see for instance U.S. Pat. Nos. 5,625,001 and 5,998,554, and World Patent Application 99/12986.
Tougheners for various types of engineering resins [including (meth)acrylics] and other polymers are sold by Rohm and Haas Co., Philadelphia, Pa, U.S.A. under the tradename Paraloid®, such as their EXL™ series which is believe to be a core-shell polymeric particle product with a rubber core and thermoplastic shell, and also see for instance U.S. Pat. Nos. 3,678,133, 3,793,402, 3,808,180, 3,985,703, 4,180,494, and 4,543,383.
Other types of thermoplastics have been toughened by the addition of elastomeric polymers which contain reactive groups such as epoxides, see for instance U.S. Pat. No. 4,753,980.
Conversely, AMLs may be used to improve the properties of thermoplastics, including thermoplastics containing functional groups which potentially may react with the AML. Such thermoplastics include polyamides, polyesters, and polyacetals, and nonfunctional group containing thermoplastics such as styrene/acrylonitrile copolymers. It is believed that to be most effective in improving properties, the AML should be dispersed within a matrix of the thermoplastic. Polymer-polymer blends of various polymers are well known in the art, but to Applicants' knowledge, no blends of AMLs with other polymers have been reported.
SUMMARY OF THE INVENTION
This invention concerns a first composition, comprising:
(a) a first polymer comprising the repeat units:
(i) at least about 10 mole percent of the total repeat units of
(ii) at least about 0.1 mole percent of a repeat unit containing a first reactive functional group;
(iii) up to about 89.9 mole percent of repeat units derived from one or more monomers which are free radically copolymerizable with (a)(i) and (a)(ii); and
(b) about 1 weight percent to about 50 weight percent based on the total weight of (a) and (b), of a second polymer which is elastomeric and contains a second reactive functional group which may react with said first reactive functional group;
or
(c) a third polymer comprising the repeat units
(i) at least about 10 mole percent of the total repeat units of
(ii) up to about 90 mole percent of repeat units derived from one or more monomers which are free radically copolymerizable with (b)(i); and
(d) about 1 percent by weight to about 60 percent by weight based on the total weight of (c) and (d), of a fourth polymer which is core-shell particles made up of an elastomeric polymer core and a polymeric thermoplastic shell, said thermoplastic shell comprising repeat units derived from methyl methacrylate
wherein:
n is 0, 1 or 2;
X is —O— or —NR
9
—; and
R
1
, R
2
, R
5
, R
6
, each of R
3
, and each R
4
, are independently hydrogen, a functional group, hydrocarbyl or substituted hydrocarbyl; and
R
9
is hydrogen, hydrocarbyl or substituted hydrocarbyl.
This invention also concerns a second composition, comprising:
(e) a fifth polymer comprising the repeat units:
(i) at least about 10 mole percent of the total repeat units of
(ii) optionally a repeat unit containing a third reactive functional group;
(iii) up to about 90 mole percent of repeat units derived from one or more monomers which are free radically copolymerizable with (e)(i), and (e)(ii), if present; and
(f) a sixth polymer which is a thermoplastic and which may optionally contain one or more fourth reactive functional groups which may react with said third functional group;
provided that in said composition (b) is present as a continuous or cocontinuous phase and (a) is present as a dispersed or cocontinuous phase;
and wherein:
n is 0, 1 or 2;
X is —O— or —NR
9
—; and
R
1
, R
2
, R
5
, R
6
, each of R
3
, and each R
4
, are independently hydrogen, a functional group, hydrocarbyl or substituted hydrocarbyl; and
R
9
is hydrogen, hydrocarbyl or substituted hydrocarbyl.
DETAILS OF THE INVENTION
Certain terms are used herein as defined below.
By “hydrocarbyl group” is meant a univalent group containing only carbon and hydrogen. If not otherwise stated, it is preferred that hydrocarbyl groups (and alkyl groups) herein contain 1 to about 30 carbon atoms.
By “substituted hydrocarbyl” is meant a hydrocarbyl group which contains one or more substituent groups which are inert under the process conditions to which the compound containing these groups is subjected. The substituent groups also do not substantially interfere with the process. If not otherwise stated, it is preferred that substituted hydrocarbyl groups herein contain 1 to about 30 carbon atoms. Included in the meaning of “substituted” are heteroaromatic rings. In substituted hydrocarbyl all of the hydrogens may be substituted, as in trifluoromethyl.
By “functional group” is meant a group other than hydrocarbyl or substituted hydrocarbyl which is inert under the process conditions to which the compound or polymer containing the group is subjected. The functional groups also do not substantially interfere with any process described herein that the compound or polymer in which they are present may take part in. Examples of functional groups include halo (fluoro, chloro, bromo and iodo), ether such as —OR
22
wherein R
22
is hydrocarbyl or substituted hydrocarbyl.
By “reactive functional group” is meant a functional group that may react with another functional group present in the process or composition. By “may react” is meant that the functional group may react with its counterpart reactive group, but it is not necessary that such reaction happen or that all of the reactive functional groups react with one another. Usually in the formation of the compositions described herein some fraction of these reactive functional groups will react.
By “copolymerizable under free radical conditions” is meant that the (
Brandenburg Charles J.
Dean David M.
Flexman Edmund A.
Hofmann George Henry
Puts Rutger D.
Belopolsky Inna Y.
E. I. du Pont de Nemours and Company
Woodward Ana
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