Ethylene-pentene-hexene copolymer, process for its...

Synthetic resins or natural rubbers -- part of the class 520 ser – Synthetic resins – Polymers from only ethylenic monomers or processes of...

Reexamination Certificate

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C526S124300, C526S125600, C526S348400, C526S348600, C526S905000, C526S916000, C524S128000, C524S323000, C524S330000, C524S333000, C524S342000, C524S343000, C524S348000, C524S394000, C524S399000, C524S400000, C524S579000

Reexamination Certificate

active

06191246

ABSTRACT:

FIELD OF THE INVENTION
This invention relates to polymerization. It relates in particular to a polymer, and to a process for producing such a polymer.
SUMMARY OF THE INVENTION
According to a first aspect of the invention, there is provided a polymer which comprises a polymerization product obtained by polymerizing at least ethylene, 1-pentene and 1-hexene.
In other words, in accordance with the first aspect of the invention, there is provided a polymer of at least ethylene, 1-pentene and 1-hexene.
In particular, the polymerization product or polymer may be a terpolymer of ethylene, 1-pentene and 1-hexene.
Thus, according to a second aspect of the invention, there is provided a terpolymer of ethylene, 1-pentene and 1-hexene.
The Applicant has found that, generally, such terpolymers exhibit good properties when moulded into film. These properties are controlled mainly by the relative proportions of ethylene, 1-pentene and 1-hexene in the terpolymer.
The molar ratio of ethylene to the sum of n-pentene-1 and n-hexene-1 in the terpolymer may be between 99.9:0.1 and 90.0:10.0, while the molar ratio of 1-pentene to 1-hexene therein may be between 0.1:99.9 and 99.9:0.1.
The terpolymer may have a melt flow rate, as measured according to ASTM D 1238, in the range of about 0.01 to about 100 g/10 min.
The terpolymer may have a density, as measured according to ASTM D 1505, in the range of about 0.89 to about 0.95 g/cm
3
.
In a first embodiment of the invention, the terpolymer may, when it is bottom blown into a film having a thickness of 30 microns on a 31.77 mm extruder with 220° C. melt temperature using a 2:1 blow ratio, comply with the following requisites:
(a) a melt flow index, as measured according to ASTM D 1238, of 0.01 to 100 g/10 minutes;
(b) a density, as measured according to ASTM D 1505, of 0.890 to 0.950 g/cm
3
;
(c) an impact strength, as measured according to ASTM D 1709, of greater than 60 g;
(d) a tear strength, as measured according to ASTM D 1922, of greater than 3.0 g/&mgr;m in the machine direction (MD) and greater than 12 g/&mgr;m in the transverse direction (TD); and
(e) contains units derived from 1-pentene and 1-hexene between 0.1 and 10 molar % as determined by
13
C NMR (samples dissolved in 1.2 dichlorobenzene).
Such a polymer thus has superior impact strength and good tear properties when blown into a film.
In a second embodiment of the invention, the terpolymer may, when it is bottom blown into a film having a thickness of 30 microns on a 31.77 mm extruder with 220° C. melt temperature using a 2:1 blow ratio, comply with the following requisites:
(a) a melt flow index, as measured according to ASTM D 1238, of 0.01 to 100 g/10 minutes;
(b) a density, as measured according to ASTM D 1505, of 0.890 to 0.950 g/cm
3
;
(c) an impact strength, as measured according to ASTM D 1709, of greater than 50 g;
(d) a tensile strength at break, as measured according to ASTM D 882, of greater than 25 MPa in the machine direction (MD) and greater than 25 MPa in the transverse direction (TD); and
(e) contains units derived from 1-pentene and 1-hexene between 0.1 and 10 molar % as determined by
13
C NMR (samples dissolved in 1,2dichlorobenzene).
Such a polymer thus has superior impact strength and good tensile strength at break when blown into a film.
In a third embodiment of the invention, the terpolymer may, when it is bottom blown into a film having a thickness of 30 microns on a 31.77 mm extruder with 220° C. melt temperature using a 2:1 blow ratio, comply with the following requisites:
(a) a melt flow index, as measured according to ASTM D 1238, of 0.01 to 100 g/10 minutes;
(b) a density, as measured according to ASTM D 1505, of 0.890 to 0.950 g/cm
3
;
(c) an impact strength, as measured according to ASTM D 1709, of greater than 40 g;
(d) a tensile strength at yield, as measured according to ASTM D 882, of greater than 15 MPa in the machine direction (MD) and greater than 14 MPa in the transverse direction (TD); and
(e) contains units derived from 1-pentene and 1-hexene between 0.1 and 10 molar % as determined by
13
C NMR (samples dissolved in 1,2dichlorobenzene).
Such a polymer thus has good impact strength and good tensile strength at yield when blown into a film.
In a fourth embodiment of the invention, the terpolymer may, when it is injection moulded according to ASTM D 647, comply with the following requisites:
(a) a melt flow index, as measured according to ASTM D 1238, of 0.01 to 100 g/10 minutes;
(b) a density, as measured according to ASTM D 1505, of 0.890 to 0.950 g/cm
3
;
(c) an Izod notched impact strength, as measured according to ASTM D 256, of between 5 and 60 kJ/m
2
;
(d) a tensile strength at yield, as measured according to ASTM 638 M, of between 10 MPa and 25 MPa;and
(e) contains units derived from 1-pentene and 1-hexene between 0.1 and 10 molar % as determined by
13
C NMR (samples dissolved in 1,2dichlorobenzene).
Such a polymer thus has a good balance of impact strength and tensile strength at yield, when injection moulded.
More particularly, the terpolymer may be that obtained by reacting ethylene, 1-pentene and 1-hexene in at least one reaction zone, while maintaining the reaction zone at a pressure in the range between atmospheric pressure and 60 kg/cm
2
, and at a temperature between 30° C. and 120° C. in the presence of a catalyst or catalyst system.
Thus, according to a third aspect of the invention, there is provided a process for producing a polymer, which process comprises reacting at least ethylene, 1-pentene and 1-hexene in at least one reaction zone, while maintaining the reaction zone at a pressure between atmospheric pressure and 60 kg/cm
2
, and at a temperature between 30° C. and 120° C., in the presence of a catalyst system, thereby to produce a polymerized product.
The polymerized product or polymer may, as mentioned hereinbefore, be a terpolymer of said ethylene, 1-pentene and 1-hexene.
The polymerization reaction may be effected in a slurry phase. The polymerization reaction may be performed in a substantially oxygen and water free state or atmosphere, and may be effected in the presence or absence of an inert saturated hydrocarbon.
A slurrying agent or solvent is thus required, and may be an inert saturated hydrocarbon. Preferred saturated hydrocarbons suitable for use as slurrying agents or solvents are aliphatic or cyclo-aliphatic liquid hydrocarbons, such as hexane and heptane.
While the reaction temperature can be in the range of 30° C. to 120° C. as stated hereinbefore, it is preferably in the range of 50° C. to 100° C. and most preferably in the range of 60° C. to 90° C.
While the pressure can be in the range of atmospheric pressure to 60 kg/cm
2
as stated hereinbefore, it is preferably in the range 3 kg/cm
2
to 30 kg/cm
2
, still more preferably in the range 4 kg/cm
2
to 18 kg/cm
2
.
The catalyst or catalyst system may be a Ziegler-Natta based catalyst or catalyst system. Any suitable Ziegler-Natta catalyst or catalyst system for ethylene polymerization can, at least in principle, be used. A catalyst system comprising a titanium based Ziegler-Natta catalyst, and, as co-catalyst, an aluminium compound is preferred. The most preferred is a titanium-magnesium chloride supported Ziegler-Natta catalyst having a productivity of at least 25 kg polymer/gram of catalyst, where the said catalyst has the ability to incorporate at the same time about the same level of 1-pentene and 1-hexene in the polyethylene chain.
In particular, the Ziegler-Natta catalyst may be that obtained by
(i) adding dibutyl ether under inert conditions to a suspension of anhydrous magnesium chloride-in an inert saturated hydrocarbon liquid, with the molar ratio of anhydrous magnesium chloride to dibutyl ether being between 0.3:1 and 3:1, preferably between 1:1 and 2:1, and stirring the resultant mixture for a period of 30 minutes to 10 hours, preferably from 4 to 6 hours, at room temperature;
(ii) adding triethylaluminium dropwise to the suspension, with the molar ratio of triethylaluminium to anhydrous magnesium chloride being between 1:1 and 6:1, prefe

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