Note: Descriptions are shown in the official language in which they were submitted.
1 30Q5~3
TITLE OF THE INVENTION
Butene-l copolymer
BACKGROUND OF THE INVENTION
(1) Field of the Invention
The present invention relates to a butene-l copolymer.
More specifically, the present invention relates to a
butene-l copolymer containing hexene~1 units and parti-
cularly excellent in workability and mechanical property.
(2) Description of the Related Art
In recent years, butene-l copolymers have been noted as
a soft or semi-rigid resinsO
Heretofore, such butene-l copolymers have often been
produced by a method of conducting solution polymerization
or slurry polymerization using titanium tric~loride as a
catalyst, but butene-l copolymers produced by this method
are poor in random property and, molded films prepared
therefrom show reduced transparency.
Furthermore, it has already been known a method of
producing a butene-1 copolymer by a solution polymerization
process using a magnesium chloride support type catalyst as
a catalyst (Japanese Patent Laid-Open No. 61-108615).
-- 1 --
1 ')( `~5~3
However, the copolymer obtained by this method has
characteristics that the distribution width of the molecular
weight is narrow. It has been known that the distribution
width of the molecular weight of the butene-1 copolymer
gives an effect on the fabricability of the copolymer such
molbability of the copolymer and the~butene-1 copolymer
obtained by the method as described above involves the
problem that the fabricability upon extrusion molding is not
sufficient due to the narrow distribution width of the
molecular weight.
While on the other hand, it has already been known such
a method of carrying out gas phase polymerization by using a
titanium trichloride catalyst used so far (Japanese Patent
Laid-Open No. 60-192716), but the thus obtained butene-1
copolymer has poor random property and, accordingly, the
films molded therefrom involves the problem that the trans-
parency i5 reduced as described above.
SUMMARY OF THE INVENTION
The object of the present invention is to provide a
butene-1 copolymer having preferable fabricability and
mechanical property together.
More specifically, it is an object of the present
invention to provide a butene-1 copolymer excellent in
-- 2
1 3 0 ~
fabricability such as moldability, and transparency and
appearance of the molding product, as well as excellent in
mechanical property such as impact shock resistance.
The present invention for attaining the foregoing
purpose provides a butene-1 copolymer containing hexene-1
units and butene-1 units within a molar ratio from 1 : 99 to
20 : 80, wherein the intrinsic viscosity of the copolymer is
within a range from 0.9 to 7.2 dl/g, the weight average
molecular weight/number average molecular weight is within a
range from 4 to 15, the temperature difference between the
highest value and the lowest value for the melting point of
the copolymer measured by the differential thermal scanning
analysis is within a range from 2 to 40C, the hexene-1
block property of the copolymer measured by NMR spectrum
analysis is not greater than 0.005, and the content of the
boiling diethylether soluble ingredient in the copolymer is
within a range from 3 to 30% by weight.
DESCRIPTION OF THE PREFERRED EMBODIMENT
The butene-l copolymer according to the present inven-
tion contains hexene-1 units and butene-1 units. The
crystallinity of the copolymer is mainly improved by the
containment of the hexene-1 unit.
The copolymer according to the present invention
-- 3
1 3 0 9 5 ) 3
contains the hexene-l unit and the butene-1 unit at a molar
ratio within a range from 1 : 99 to 20 : 80. If the molar
ratio of the ethylene unit contained in the copolymer is
lower than the above specified range, the transparency of
the molded film is lowered since the degree of crystallinity
of the copolymer is not reduced. While on the other hand,
if the molar ratio of the hexene-1 unit is higher than the
above specified range, the copolymer becomes inhomogenous
and sticky.
Particularly in the present invention, the above-
specified molar ratio is preferably set within a range from
1 : 99 to 15 : 85. By specifying the ratio within the
range, it is possible to obtain a copolymer capable of
producing a molded film of more homogenous and higher
transparency.
The intrinsic viscosity ( n) of the butene-l copolymer
according to the present invention measured in a decalin
solution at 135C is within a range from 0.g to 7.2 dl/g.
The intrinsic viscosity (~) gives an effect mainly on the
moldability and the mechanical property of the copolymer.
If the intrinsic viscosity (n) is lower than 0.9 dl/g,
the mechanical strength of the molding product, particular-
ly, the impact shock resistance produced by using the
copolymer is reduced. On the other hand, if it is higher
than 7.2 dl/g, the moldability is degraded.
1 3a`,553
The molecular weight distribution of the copolymer
according to the present invention, that is, the ratio of
(Mw/Mn) between the weight average molecular weight (Mw) and
the number average molecular weight (Mn) of the copolymer is
within a range from 4 to 15. The molecu~ar weight distribu-
tion provides transparency to the resultant molding product,
as well as gives an effect on the moldability and the
mechanical strength of the molding product. In the butene-l
copolymer obtained by the conventional production process,
the distribution width of the molecular weight tends to be
narrow, production of molding product having sufficient
moldability is difficult and when molded into film-like
shape, the transparency of the film is often insufficient.
That is, those copolymers with the molecular weight
distribution of not more than 4 has no sufficient mold-
ability and, further, show insufficient transparency in the
case of molding into a film-like shape. Furthermore, if
the molecular we.ight distribution is broader'~ mechanical
strength such as impact shock resistance is reduced.
Particularly, in the present invention, the molecular
weight distribution is preferably within a range from 4 to
10. Those copolymers within the range have preferable
moldability and transparency, as well as the show parti-
cularly, desirable mechanical property.
When the butene-l copolymer according to the present
1 3 ~3, 5 ~ 3
invention is analyzed by using a differential thermal
scanning analysis, two kinds of endothermic curves showing
lowest melting point and highest melting point can be
obtained. Among them, the highest melting point is usually
within a range from 80 to 120C. In the present invention,
the highest melting point is a peak appearing at the highest
temperature side when the copolymer subjected to drying
treatment is heated from 0 to 200C at a temperature elevat-
ing rate of 10C/min and endothermic peak is measured,
while the lowest melting point is a peak or a shoulder on
the most lowest temperature side.
Then, in the copolymer according to the present
invention, it is desirable that the difference between the
highest melting point and the lowest melting point
(temperature difference between the highest value and the
lowest value of the melting point) measured by using a
differential thermal scanning analysis is within a range
from 2 to 40C. The temperature difference~particularly
giv~s an effect on the fabricability and the temperature
upon press-bonding film-like molding products in stack (heat
seal temperature)~
That is, if the temperature difference as described
above is less than 2C (containing 0C), the heat seal
temperature goes higher to worsen the heat sealing property
in the case of molding into a film. While on the other
1 3~"'`553
hand, if the temperature difference is greater than 40C,
the copolymer becomes sticky to reduce the molding per-
formance. Particularly, if the highest melting point is
lower than 80C, stickiness may possibly occur in the
copolymer even at the ambient temperature and it can not
usually be used as the starting material for the molding
product. Furthermore, if the highest melting point is
higher than 120C, the heat sealing temperature is too high
to preferably conduct heat sealing.
Furthermore, the melting calorie of the copolymer
according to the present invention measured by the dif-
ferential thermal scanning analysis (defined by a straight
line connecting the base lines of peaks or shoulders
appearing in the difference thermal scanning analysis) is
preferably within a range from 2 to 25 cal/g. If the
melting heat calorie is lower than 2 cal/g, the copolymer
may tend to be sticky. While on the other hand, if it is
higher than 25 cal/g, the transparency of the film-like
molding product may be lowered.
Particulary, butene-l copolymer within 4 - 15 cal/g of
melting calorie is not sticky and gives good transparent
molding product.
The block property (X) of hexene-l unit in the main
chain of the butene-l copolymer according to the present
invention can be measured along with the following equation
1 ~0',553
by measuring the 1 C-NMR of the butene-l copolymer and
identifying each of triad by utilizing the method as
described in "Macromolecules", 15, 353 (1982) for the result
of the measurement:
X = I/H
where I represents a block polymerization ratio in the
hexene-1 chain in the copolymer and it is usually re-
presented by the following equation:
I ICH2(HH)
CH2(BH)
And in the equation above, ICH2(HH) represents a
spectral band intensity of -CH2- contained in main chain by
measuring the 3C-NMR of the butene-l homopolymer as an
P . CH2(BH) represents a spectral band
intensity of -CH2- identified a sequence of butene-l-hexene-
1 cr hexene-1-butene-l.
H is a content of a hexene-l unit in the butene-l
copolymer and usually represented by the general equation:
H(mol%) = I Br(H) x lOO
Br(B) Br(H)
In the equation above, IBr(H) represents a spectral
band intensity of all sequences containing hexene-l unit in
triad. The examples of the sequences are -H-H-H-, -B-H-H-
1 3Q ~ 553
and -B-H-B- etc. in which H represents hexene-l unit and B
represents butene-l unit.
IBr(B) represents a spectral band intensity of all
sequences containing butene-1 unit in triad. The examples
of the sequences are -B-B-B-, -B-B-H- and -H-B-H- etc.
It is necessary that the block property (X) of hexene-l
unit in the butene-l copolymer according to the present
invention is not greater than 0.005 and the lower value is
better. Accordingly, most preferred value is 0. If the
block property (X) of hexene-l unit is greater than 0.005,
the transparency of the film-like molding product is
reduced, for instance.
The boiling diethyl ether soluble content in the
butene-l copolymer according to the present invention has to
be within a range from 2 to 25~ by weight. Generally,
solubility to the boiling diethyl ether tends to be lowered
as the polymerization degree of the copolymer becomes higher
and it tends to be reduced as the crystalli~1ty is in-
creased. The copolymer according to the present invention
has a meaning of restricting the ingredient of low poly-
merization degree in the copolymer and the crystallinity by
controlling the boiling diethyl ether soluble content within
the range described above.
Accordingly, if the boiling diethyl ether soluble
content is less than 2~ by weight, the transparency of the
3~
film-like molding product is reduced. While on the other
halld, if it exceeds 25% by weight, stickiness may occur
since the content oE the low polymerization ingredient is
increased .
The butene-1 copolymer according to the present
invention can be produced easily by reacting ethylene and
butene-1 at a gas phase by using a specific solid catalyst
ingredient containing magnesium represen\ted by the general
fonnula:
MgRlr~2
Mg(OR1) X
where Rl and R2 represent alk~l group, and m and n can
satisfy the relationship: 0 < m < 2 and n satisfies
0 < n < 2; an organic aluminum compound and a specific
electron donating compound.
Specifically, the copolymer according ~o the presen-t
invention can be produced by the production process as
described in the speci:Eications of Japanese Publication NQS.
~3-302 dated January 5, 1988; 63-165408 dated July 8, 1988; 63-51409
dated March 4, 1988 and 63-54406 dated March 8, 1988.while
referring to the characterislics of the copolymer as described abo~7e
and by experimentally setting production conditions.
The process for producing the butene-1 copolymer
- 10 - '
~ ", `, ~ 5 3
according to the present invention is to be explained along
wi~h the method as described in the s~ecification of
Japanese Publication No. 63-51409, but the butene-l
copolymer according to the present invention i5 not
restricted to the production process described above.
The copolymer according to the present invention can
easily be produced by reacting butene-l and ethylene under
gas phase polymerization conditions at the presence of a
catalyst comprising a solid catalyst ingredient (A)
described later, an organic aluminum compound (B) and an
electron ~onating colllpound (c).
'rhe solid catalyst ingredient (~) is prepared by
chlorinating at least one organic magnesium compound
represented by the formula:
formula: MgR1R2
where Rl and R2 which may be identical or different with
each other represent alkyl group with 1 to 20 carbon atoms,
with at least one chlorinating agent to obtain a support and
bringing the support in contact with a titanium (IV) halide
at a temperature within a range from -25 to ~180C under the
presence of an electron donor.
The organic magnesium compound can include those alkyl
magnesium compounds such as diethyl magnesium, ethylbutyl
I J (..` J J ~ 3
magnesium, ethylhexyl magnesium, ethyloctyl magnesium,
dibutyl magnesium, butylhexyl magnesium, butyloctyl
magnesium and dicyclohexyl magnesium.
The chlorinating agent can include chlorine gas and
alkyl chloride. The combined use of chlorine gas and butyl
chloride is preferred in the present invention.
Chlorination is usually carried out at 0 - 100C, pre-
ferably, from 20 to 60C, particularly preferably, from 20
to 40C.
In the chlorination, a portion of alkyl groups bonded
to magnesium atom is replaced with chlorine atoms. In
addition, since at least a portion of alkyl groups is left,
formation of normal cyrstal lattice is inhibited by the
effect of the residual alkyl group to form not-layerous
product with extremely small crystal grain size having an
appropriate surface area and pore volume.
Not-layerous product thus obtained is subjected to
treatment with titanium (IV) halide under the presence of an
electron donor, if required, after the alcohol treatment.
Processing of titanium (IV) halide is usually conducted at a
temperature within a from -25C to +180C.
Titanium (IV) halide can include titanium tetrahalide,
trihalogenated alkoxy titanium, dihalogenated alkoxy
titanium and monohalogenated alkoxy titanium, titanium
tetrachloride being particularly preferred for use.
1 3~j,5~3
As the electron donor, an organic compound containing
oxygen, nitrogen, phosphorus or sulfur can be used.
Specific examples of the electron donor can include
amines, amides, ketones, nitriles, phosphines, phos-
phoamides, esters, ethers, thioethers, thioesters, acid
anhydrides, acid halides,~acid amides, aldehydes and organic
acids.
Among them, preferred are organic acids, esters,
ethers, ketones and acid anhydrides. Examples of specific
compounds can include benzoic acid, p-methoxy bonzoic acid,
p-ethoxy benzoic acid, toluic acid, diisobutyl phthalate,
benzoquinone, benzoic anhydride and ethylene glycol butyl
ether.
The solid catalyst ingredient (A) thus prepared
desirably has halogen/titanium ratio (molar ratio) from 3 to
200, preferably, from 4 to 100 and magnesium/titanium ratio
(molar ratio) from 1 to 90, preferably, 5 to 70.
There is no particular restrictions for the organic
aluminum compound (B) but trialkyl aluminum is particularly
preferred.
As the electron donating compound (C) the heterocyclic
compound represented by the following formula can be-
used:
5 ' 3
~ R6
R \ / R3
R5 \ R7
where R3 and R6 represent hydrocarbon group, preferably,
substituted or~not substituted saturated or not-saturated
hydrocarbon with 2 to 5 carbon atoms, R4, R5 and R7
represent hydrogen or hydrocarbon group, preferably,
hydrogen.or substituted or not-substituted saturated or not-
saturated hydrocarbon group with 1 to 5 carbon atoms respec-
tively.
The heterocyclic compound can include, for example,
1,4-cineole, 1,8 cineole, n-cineole, pinol, benzofuran, 2,3-
dihydrobenzofuran (coumaran), 2H-chromene, 4H-chromeme,
chroman, isochroman, dibenzofuran and xanthene. Each of
these heterocyclic compounds may be used alone or two or
more of them may be used together.
Among the various heterocyclic compounds described
above, 1,8-cineole is particularly preferre~
The composition of the catalyst upon producing the
butene-1 copolymer according to the present invention is
such that the organic aluminum compound (B) is within a
range usually from 0,1 to 1000 molar times, preferably, from
1 to 500 molar times to the titanium atom of the tetravalent
titanium compound in the solid catalyst ingredient (A).
Further, the electron donating compound (C) is used within
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5 3
such a range usually from 0.1 to 500 molar times, prefer-
ably, from 0.5 to 200 molar times based on the titanium
atoms of the tetravalent titanium compound in the solid
catalyst ingredient (A).
The gas phase polymerization temperature is usually
from 45 to 80C and, preferably, from 50 to 70C.
The polymerization pressure can properly be set within
such a range as the liquefication of the starting material
ingredient does not substantially occur and it is usually
from l to 15 kg/cm2.
Further, the molar ratio of introducing hexene-1 and
butene-1 can properly be set within a range of the molar
ratio between both of them in the copolymer to be obtained,
that is, within a range from 1 : 99 to 15 : 85.
Furthermore, molecular weight controller such as
hydrogen may be present together with an aim of adjusting
the molecular weight. In addition, an inert gas having a
. .
boiling poLnt lower than butene-1, for exa~ple, nitrogen,
methane, ethane, propane may be present together with an aim
of preventing the coagulation of the copolymer.
The butene-l copolymer according to the present inven-
tion thus obtained can preferably be used as a material
suitable to the film-like molding product or various kind of
pipes.
Since the butene-1 copolymer according to the present
- 15 -
1 3~J ;~J J3
invention has broader width of the molecular weight
distribution as compared with the conventional buten-1
copolymer, it has satisfactory processability, that is, the
molding pressure upon molding is within a preferable range,
the appearance of the resultant molding product is extremely
satisfactory and, particularly, the transparency of the film
is excellent when it is molded into a film-like product.
Further, the temperature for carrying out heat sealing
by using the film-like molding product is within a satis-
factory range and, in addition, the heat sealing property is
also preferred.
Furthermore, the butene-1 copolymer according to the
present invention has satisfactory mechanical property and
it is particulary excellent in the impact shock resistance.
The present invention is to be explained referring to
examples and comparative examples.
Example 1 ~
(1) Preparation of Solid Catalyst Ingredient (A)
300 ml of butyloctyl magnesium (in 20~ heptane solu-
tion) was charged in a four-necked flask equipped with a
mechanical stirrer, reflux condenser, dropping funnel, gas
supply valve and thermometer, nitrogen was introduced into
the flask and, while maintaining the inside of the flask to
- 16 -
r~ r- r- 7
~ J ~ ,i "~
a inert atmosphere, 5 liter of butyl chloride was added at
room temperature by using the dropping funnel. Then,
chlorine gas was added for chlorination at a rate of 5
ml/min.
Then, 2.5 l of silicone oil was added at a temperature
25 to 35C, and 113 ml of ethanol was further dropped to the
mixture. The resultant chlorides were precipitated by the
addition of ethanol. The liquid mixture containing the
precipitates were agitated at 40C for one hour and then the
temperature was elevated to 75 - 80C and the solution was
left over one night at that temperature.
The solution at high temperature was quietly added by
using a siphon into a solution containing diisobutyl
phthalate (electron donor) and an excess amount of TiC14 and
cooled to -25C, to precipitate a reaction intermediate in
low temperature TiCl4. Then, the temperature of the mixed
solution, containing the precipitate was elevated to the room
temperature.
Then, diisobutyl phthalate as the electron donor was
further added to the mixed solution containing the pre-
cipitate, temperature was elevated to 100 - 110C and the
mixed solution was maintained at that temperature for one
hour. The reaction product was settled, washed with heptane
at 85C for 5 - 6 times and the solution was transferred to
another vessel by way of a siphon.
- 17 -
1 3 ") '` ~, 5 3
Further, an excess amount of TiC14 was added to the
solution and the mixture was stirred at 110C for one hour.
The resultant settling product and the solution were
separated by siphon and, thereafter, the resultant catalyst
ingredient (precipitate) was washed with heptane for several
times (5 - 6 times at 80C).
The resultant precipitate was collected and dried under
a slightly reduced pressure. In this way, a solid catalyst
ingredient (A) with the Ti content of 3.0% by weight was
obtained.
(2) Preparation of Catalyst
The solid catalyst ingredient (A) obtained in (1) above
was charged into a catalyst preparation vessel such that the
titanium concentration in one liter was 2 mmol. 30 mmol/-
liter of triisobutyl aluminum and 12 mmol/liter of 1,8-
cineole were charged to the catalyst preparation vessel.
Then, propylene was charged in such an amount as 50 g per 1
m~ol of titanium atoms and the temperature inside the
catalyst preparation vessel was elevated to 40C to conduct
the reaction for the preparation of the catalyst.
(3) Preparation of Butene-1 Copolymer
Using a fluidized bed polymerization vessel of 300 mm
diameter and 100 liter volume, there were supplied a Ti
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1 30q553
catalyst slurry obtained by re-preparing the catalyst
obtained in (2) above into 3.6 mmol/l converted as Ti atom
from the catalyst preparation vessel to the polymerization
reactor at a flow rate of 0.15 l/hr, triisobutyl aluminum at
a flow rate of 30 mmol/hr and 1,8-cineole at a flow rate of
24 mmol/hr respectively to the polymerization reactor.
Polymerization was conducted at a reaction temperature
of 60C while controlling the partial pressure of butene-1
to 3 kg/cm2, the partial pressure of nitrogen to 4 kg/cm2
and the partial pressure of hydrogen such that the intrinsic
viscosity (n ) of the resultant polymer had the value shown
in Table 1 respectively and supplying butene-1, hexene-1,
hydrogen gas and nitrogen gas such that gas space velocity
is at 35 cm/sec.
Examples 2 - 4 and Comparative Examples 1 and 6
Butene-l copolymer was produced in the same manner as
in Example 1 except for changing the introduction rate of
butene-l and hexene-1.
Comparative Examples 2 - 3
(1) Preparation of the Solid Catalyst Ingredient
To a 500 ml volume three-necked flask made of glass
(e~uipped with thermometer and stirrer) heated and dried, 75
ml of anhydrous heptane, 75 ml of titanium tetrabutoxide and
-- 19 --
1 3~','553
10 g of anhydrous magnesium chloride were completely dis-
solved. Then, the solution was cooled to 40C, to which 15
ml of methyl hydrogen polysiloxane was added to precipitate
magnesium chloride-titanium tetrabutoxide complex. After
washing the precipitate with purified heptane, 8.7 ml of
silicon tetrachloride and 1~8 ml of diheptyl phthalate were
added and maintained at 50C for 2 hours. Then, they were
further washed with purified heptane to obtain a solid
catalyst ingredient.
The titanium content in the resultant solid catalyst
ingredient was 3.0% by weight and the diheptyl phthalate
content was 25.0~ by weight.
(2) Preparation of Butene-l Copolymer
Into a 20 liter polymerization reactor, were con-
tinuously introduced 5 kg of butene-l per one hour and
hexene-1 in such an amount as giving hexene-l unit amount
shown in Table l, 10 mmol of triethyl aluminum, 1 mmol of
vinyltriethoxysilane and the solid catalyst obtained in (1)
above in an amount of 0.05 mmol converted as titanium atom,
and the partial pressures of the butene-1 and hexene-1 in
the gas phase were adjusted such that the intrinsic
viscosity of the resultant copolymer showed the value as
described in Table 1. The reaction temperature was kept at
70C.
- 20 -
~ J
The polymerization solution was withdrawn continuously
such that the liquid amount in the reactor was 10 liter and
a small amount of ethanol was added to the withdrawn reac-
tion product to stop the polymerizing reaction and, at the
same time, not-reacted ingredients were removed to obtain
butene-l copolymer.
Comparative Examples 4 - 5
Into a 10 liter polymerization reactor, 5 kg of butene-
1 per one hour and hexene-1 in such an amount as giving the
hexene-l unit amount shown in Table 1, 20 mmol of dietyhyl
aluminum and 10 mmol of titanium trichloride (manufactured
by Toho Titanium Co., Ltd.~ were continuously charged at
this ratio. The partial pressure of hydrogen in the gas
phase was kept at 2.7 kg/cm2 and the partial pressure of
butene-l and hexene-1 in the gas phase were adjusted such
that the intrinsic viscosity of the resultant copolymer
showed the values as described in Table l. The reaction
temperature was ]cept at 70C.
The polymerization solution was continuously withdrawn
such that the liquid in the reaction vessel was 10 liter and
methanol was added by 1 liter per hour to the withdrawn
reaction product to stop the polymerizing reaction and then
the unreacted ingredients were removed by water washing to
obtain butene-1 copolymer.
- 21 -
1 3(~C)5~3
Measuring Method
Physical properties and characteristics of the
resultant butene-l copolymer were measured as described
below.
IntrinsiC viscosity ( n )
Intrinsic viscosity was measured in decalin at 135C.
Molecular wei~ht distribution (Mw/Mn)
Showdex AD807 and AD80M/S were attached each by two to
a gel permeation chromatography (GPC) device 150C manufac-
tured by ~aters Co. and molecular weight distribution was
measured. The measuring temperature was at 135C.
Differential thermal scanning analysis
The resultant butene-1 copolymer was dried and used as
the specimen.
The temperature of the specimen was elevated from 0 to
200C at a temperature rising rate of 10C/min and the endo-
thermic peak was measured.
Block property of hexene-1
13C NMR spectrum of the resultant butene-1 copolymer
1 30~5L)3
was measured and each of triad was identified by utilizing
the method as described in the "Macromoleculars" previously
cited for the result of the measurement and the property
was determined by the following equation described pre-
viously:
X = I/H
Boiling diethyl ether soluble component
A specimen prepared by drying the resultant butene-l
copolymer, molding into a press sheet of 1 mm thickness and
cut into 1 mm square was subjected to Soxhlet extraction
with diethyl ether for 6 hours to determine the soluble
content.`
Resin pressure
Using a T die cast molding machine having a screw of 20
mm diameter, the resin pressure was measure~ at a drawing
rate of 7 m/min to obtain a film of 20 ~m thickness.
Haze
Measured according to ASTM D-1003.
Heat seal temperature
A film of 20 ,um thickness was prepared from the
- 23 -
1 3G~553
resultant copolymer by using a T die cast molding ~achine
with a screw diameter of 20 mm and at a drawing rate of 7
m/min.
A specimen of 15 mm width obtained by press-bonding the
film with each other for one second by applying a load of 2
kg/cm at a predetermined temperature in a heat sealer was
subjected to peeling at a peeling rate of 20 mm/min and at a
peeling angle of 180 and the heat seal temperature was
defined as the temperature when the peeling resistance was
310.
Izod impact strength
The strength was measured according to JIS-~-7110. The
measuring temperature was 0C.
The obtained measuring results are shown in Table 1.
- 24 -
~ 1 3 0 `, 5 5 3
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