Note: Descriptions are shown in the official language in which they were submitted.
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Modified aminotriazine resin and method for the
production thereof
The invention relates to a modified aminotriazine resin
as claimed in claim 1, a process for the production
thereof as claimed in claim 10 and the use thereof as
claimed in claim 14.
Aminotriazine resins are condensates of an
aminotriazine with a carbonyl compound. The
industrially most important aminotriazine resins are
melamine-formaldehyde resins.
Aminotriazine resins in which the primary aminotriazine
condensates are modified, for example, with alcohols or
polyols contain ether groups in their structure; they
are referred to as modified aminotriazine resins. WO
03/046053 Al or WO 03/106558 Al discloses, for example,
modified aminotriazine resins which have a sufficiently
high melt viscosity so that they can be processed by
thermoplastic methods, such as, for example, extrusion
or injection molding.
Such resins are usually obtained by a method in which a
modified aminotriazine resin is prepared in liquid
form, said resin is then concentrated to give a resin
melt and the resin melt is then converted by reaction
at elevated temperature in extruders, kneaders or the
like.
The thermoplastically processable modified
aminotriazine resins thus obtained have several
disadvantages.
They exhibit relatively low reactivity in the
conversion in the extruder, in which as large an
increase as possible in the molar mass of the resins
should take place. In order to achieve an increase in
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the molar mass at a sufficient rate,
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high extrusion temperatures are necessary in the case
of the known resins. High extrusion temperatures are
disadvantageous since the extrusion process is
difficult to control and there is the danger of
spontaneous curing of the resins in the extruder.
A further disadvantage of the known aminotriazine
resins is their slow curing during the final shaping.
High curing temperatures, long residence times and
relatively large amounts of curing catalysts are
required in order to bring about final curing.
Furthermore, modified aminotriazine resin solutions
having a molar formaldehyde:aminotriazine ratio of not
less than 2:1 could be prepared to date in a stable
manner at room temperature. Higher proportions of
aminotriazine cannot be realized or can be realized
only by a very complicated reaction procedure. In
general, the product or the aminotriazine is
precipitated from the resin solutions on cooling to
room temperature, with the result that the further
processing is very complicated. The higher the
formaldehyde content, the more undesired emissions of
methanol and formaldehyde occur both during the
processing of the resins and from the end product. A
further disadvantage is the easy combustability of the
resins, which is likewise higher the higher the
formaldehyde content and the degree of modification of
the resins.
Accordingly, an object of the present invention was to
find an aminotriazine resin which does not have said
disadvantages.
This object is achieved by an aminotriazine resin as
claimed in claim 1.
The present invention relates to a modified aminotriazine
resin, in particular melamine- formaldehyde
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resin, which is obtainable by reacting a modified
aminotriazine resin melt with at least one
aminotriazine present in the form of a
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solid and/or a suspension, in particular melamine, at a
temperature of from 130 to 250 C and in a residence
time of from 30 to 600 s.
The advantage of the aminotriazine resin according to
the invention is that it exhibits increased reactivity
during the increase of molar mass in the extruder and
during the final curing. In this way, a major part of
the undesired cleavage products which are otherwise
released only during processing and in the end product
are removed in the extruder itself. Furthermore, the
aminotriazine resins according to the invention can
also be prepared in a stable and simple manner with
high aminotriazine contents.
Suitable aminotriazines for the preparation of the
modified aminotriazine resin melt are, for example,
melamine, guanamines, oxoaminotriazines, such as, for
example, ammeline or ammelide, or substituted
melamines. Melamine is preferably used. For the
preparation of the modified aminotriazine resin melt,
certain proportions of urea and/or dicyandiamide can be
used in addition to the aminotriazine.
Suitable carbonyl compounds for the preparation of the
modified aminotriazine resin melt are, for example,
formaldehyde, acetaldehyde, isobutyraldehyde, acetone,
methyl ethyl ketone, glyoxylic acid, glyoxylic acid
methyl ester hemiacetal, glyoxal, glutardialdehyde or
diethyl ketone. A preferably used carbonyl compound is
formaldehyde.
In the modified aminotriazine resin, the primary
condensates of carbonyl compound and aminotriazine are
partly or completely etherified with C1-Cq-alcohols. The
partly or completely etherified condensates can be
partly or completely transetherified in a further
reaction step, the transetherification preferably being
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effected with aliphatic C9-C18-alcohols or aromatic
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alcohols, diols or polyols or mixtures thereof.
A modified aminotriazine resin in the context of the
present invention is also one which, in addition to or
instead of the etherification and/or
transetherification with alcohols, diols and polyols,
is obtained, for example, by incorporating by
condensation or subsequently adding other customary
modifiers, such as, for example, caprolactam, sulfites,
sulfonamides, carbamates, salts of maleic or fumaric
acid monoamides, epoxides, bisepoxides or isocyanates.
Furthermore, fillers and/or reinforcing fibers, further
polymers and stabilizers, UV absorbers and/or
auxiliaries may be present in the modified
aminotriazine resin.
Particularly preferably, the modified aminotriazine
resin melt is formed from a condensate of the
components melamine and formaldehyde.
It usually has a molar carbonyl compound:aminotriazine
ratio of from 2:1 to 3.5:1, higher carbonyl contents up
to 6:1 also being possible.
Advantageously, the reaction of the modified
aminotriazine resin melt with at least one
aminotriazine takes place at a temperature of from 190
to 250 C. This ensures that the aminotriazine metered
in reacts particularly rapidly with the aminotriazine
resin melt.
The required amount of aminotriazine is dependent on a
plurality of parameters:
1) which carbonyl:aminotriazine ratio is to be present
in the end product and
2) the carbonyl:aminotriazine ratio possessed by the
starting aminotriazine resin melt.
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This gives (at a predetermined throughput) the amount
of aminotriazine which has to be metered in. (The
addition of the aminotriazine shifts the
carbonyl:aminotriazine ratio, i.e. reduces it.)
The amount of aminotriazine metered in is preferably
chosen so that, in the resulting aminotriazine resin,
the molar ratio of the sum of the carbonyl compounds to
the sum of the aminotriazines is from 0.1 to 1.5 units
smaller than the molar ratio of the sum of the carbonyl
compounds to the sum of the aminotriazines in the
modified aminotriazine resin melt.
In the resulting aminotriazine resin, the molar ratio
of the sum of the carbonyl compounds to the sum of the
aminotriazines is particularly preferably from 0.3 to
1.0 unit smaller than the molar ratio of the sum of the
carbonyl compounds to the sum of the aminotriazines in
the modified aminotriazine resin melt. Aminotriazine
resins which have this molar ratio are readily
processable and the reaction is technically readily
controllable. This formulation defines the amount of
aminotriazine metered in.
In the modified aminotriazine resin, the molar
carbonyl:aminotriazine ratio is preferably less than
2:1, particularly preferably less than 1.6:1.
It has not been possible to date to prepare modified
aminotriazine resins having such high aminotriazine
contents in stable form in a conventional manner. They
exhibit particularly low emissions, advantageous flame-
retardant properties and a very fast curing rate.
The invention furthermore relates to a process for the
preparation of a modified aminotriazine resin,
characterized in that
- a modified aminotriazine resin melt is
prepared,
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- the modified aminotriazine resin melt is then
converted by reaction in at least one extruder
or kneader,
at least one aminotriazine, in particular
melamine, being metered in as a solid and/or as
a suspension before and/or during the reactive
conversion into the modified aminotriazine
resin melt,
whereupon the modified aminotriazine resin is
discharged.
The modified aminoplast resin melt is prepared, for
example, as described in WO 03/046053 or in WO
03/106558 or by concentration of modified aminoplast
resin solutions in thin-film evaporators according to
WO 04/056900 Al.
The aminotriazine metered into the aminotriazine resin
melt surprisingly reacts with the aminotriazine resin
melt, and a clear resin strand which can be further
processed in a conventional manner is obtained.
The aminotriazine metered in acts as a crosslinking
center, as a flame-retardant component and also as a
scavenger for the carbonyl compounds used. Furthermore,
readily volatile cleavage products are liberated in the
reactive incorporation of the aminotriazine, so that
the modified aminotriazine resins according to the
invention have lower emissions than the modified
aminotriazine resins which can be prepared using
conventional methods.
Advantageously, the solid aminotriazine is in the form
of small lumps or in the form of powder.
At least one aminotriazine is preferably metered into
at least one extruder or kneader.
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The aminotriazine metered in is thus well distributed
and incorporated into the aminotriazine resin melt.
The extruder used is, for example, a twin-screw
extruder. It is also possible to operate two extruders
or kneaders in series.
The aminotriazine metered in can be metered in
gravimetrically in the form of a solid. The
aminotriazine is preferably added as a suspension.
Suspension media which may be used are, for example,
water, alcohols, such as, for example, butanol or
methanol, diols or polyols, such as, for example,
simulsols, caprolactone derivatives, polyester polyols,
oligoester polyols, trimethylolpropane or mixtures of
these components. Concentrated resin solutions having a
higher viscosity are possible as further suspension
media. In order to obtain a pumpable and meterable
suspension, the suspension can be stirred and heated.
The solids content of the suspension is from about 30
to about 90% by weight, preferably from about 40 to 80%
by weight.
It is particularly advantageous to use the modified
aminotriazine resin melt and/or at least a part of the
transetherification agents and/or modifiers used for
the modification as suspension media.
An advantage of the addition of the aminotriazine as a
suspension is the better meterability in comparison
with the addition in the form of a solid.
Suitable aminotriazines for metering into the modified
aminotriazine resin melt are, for example, melamine,
oxoaminotriazines, such as, for example ammeline or
ammelide, guanamines or substituted melamines. At least
one aminotriazine metered in is preferably melamine.
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In a preferred embodiment, a mixture of different
aminotriazines is metered in. It is thus possible to
prepare different resin types having advantageous
properties. The higher the chosen proportion of
oxoaminotriazines, the greater is the curing rate of
the resulting resin.
It is furthermore preferred if, in addition to or
instead of a mixture of different aminotriazines, a
mixture of at least one aminotriazine and a compound
present in encapsulated form is metered in. The
compound present in encapsulated form contains
phosphorus and/or nitrogen and/or boron in chemically
bonded form. The compound is, for example, an inorganic
or organic phosphorus, nitrogen and/or boron compound
and preferably has both flame-retardant and proton-
liberating activity. For example, ammonium
polyphosphate, melamine polyphosphate, phosphoric acid
esters and phosphonic acid esters based on the reaction
of phosphorus pentoxide or phosphorus trioxide with
pentaerythritol or dipentaerythritol, and the ammonium
and melamine salts thereof serve as the encapsulated
compound, it being possible to use a modified
aminoplast resin as capsule wall material. Modified
aminotriazine resins having even better flameproof
properties and even higher reactivity and curing rate
are obtainable thereby since, in addition to its flame-
retardant activity, the encapsulated compound also acts
as a curing catalyst.
After the reactive conversion of the modified
aminotriazine resin melt to which at least one
aminotriazine has been added in the extruder or
kneader, the modified aminotriazine resin obtained is
compounded, for example granulated and discharged.
Granulators usually used are pelletizers, granulating
mills, hot die face cutting granulators or tableting
apparatuses.
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The modified aminotriazine resins obtainable by the
process according to the invention have a variety of
uses.
They can be used, for example, as injection molding
resins. It is also possible to process the
aminotriazine resins according to the invention with a
substrate material to give a composite material. For
example, fibers, tiles, woven fabrics, wood and/or
polymers can be used as substrate materials.
Furthermore, the aminotriazine resins according to the
invention can be used for the production of shaped
articles, such as pipes, sheets, profiles or fibers.
The modified aminotriazine resins according to the
invention have increased reactivity with respect to an
increase in molar mass compared with the conventional
modified aminotriazine resins having the same molar
carbonyl:aminotriazine ratio. The aminotriazine metered
in acts as a crosslinking center and accelerates the
crosslinking both in the extruder and during t.he final
curing. Accordingly, the addition of a separate curing
catalyst can be dispensed with in certain applications.
Below, the invention is explained with reference to
examples.
1 Preparation of the modified aminotriazine resin
having high reactivity
Modified aminotriazine resin melts as described in WO
04/056900 Al were prepared. The starting composition of
the modified aminotriazine resin melts, the amount of
aminotriazine added in the extruder, the amount of
added capsules
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and of polyol as modifier or suspension medium and the
composition of the modified aminotriazine resins
according to the invention as end product in granular
form after the reactive conversion are stated in table
1. Melamine or oxoaminotriazines were used as
aminotriazine added in the extruder.
Table 1 states the amount in % by weight of melamine
powder having the customary particle size distribution
which was added and the amount in % by weight of
melamine which was added in the amount of polyol in
which it was suspended.
The experimental parameters for the reactive conversion
of the aminotriazine resin melts and the properties of
the resulting modified aminotriazine resins having high
reactivity are shown in table 2.
In examples Cl, 2 and 3, modified aminotriazine resins
having a formaldehyde:aminotriazine ratio of 2:1 were
prepared. In comparative example Cl, no aminotriazine
was added during the extrusion. In examples 2 and 3,
the formaldehyde:aminotriazine ratio of 2:1 in the end
product was achieved by reactive conversion of a
modified aminotriazine resin melt having a
formaldehyde:melamine ratio of 2.5:1 with melamine or
oxoaminotriazines.
In examples C4 and 5, modified aminotriazine resins
having a formaldehyde:melamine ratio of 2.5:1 were
prepared. In comparative example C4, no aminotriazine
was added during the extrusion. In example 5, the
formaldehyde:melamine ratio of 2.5:1 in the end product
was achieved by reactive conversion of a modified
aminotriazine resin melt having a formaldehyde:melamine
ratio of 3:1 with melamine.
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In the examples C8 and 9, modified aminotriazine resins
having a formaldehyde:melamine ratio of 3:1, which
contain the transetherification agent Simulsol BPPE,
were prepared. In comparative example C8 no
aminotriazine was added during the extrusion. In
example 9, the formaldehyde:melamine ratio of 3:1 in
the end product was achieved by reactive conversion of
a modified aminotriazine resin melt having a
formaldehyde:melamine ratio of 3.5:1 with melamine,
suspended in Simulsol BPPE.
In example 6, a modified aminotriazine resin having a
very low formaldehyde:melamine ratio of 1.5:1 was
prepared. It was obtained by reactive conversion of a
modified aminotriazine resin melt having a
formaldehyde:melamine ratio of 2:1 with melamine.
In example 7, a modified aminotriazine resin having a
formaldehyde:melamine ratio of 1.71:1, which contains
the encapsulated compound Exolit AP462, was prepared.
It was obtained by reactive conversion of a modified
aminotriazine resin melt having a formaldehyde:melamine
ratio of 2:1 with melamine and Exolit AP462.
The extrusion was effected under a devolatilizing
vacuum PEXtr and at an average temperature of barrels 2-
8 of the extruder of T02_$, a melt temperature of TMelt
and a screw speed nEXtr. The feed into the extruder is
stated as m' Extr_in and the output from the extruder is
stated as m' EXtr_oõt.
The extruded stand of the modified aminotriazine resin
according to the invention was cooled after extrusion
and granulated. Tg designates the glass transition
temperature of the granules and rl the melt viscosity
measured isothermally at 130 C.
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Table 2 also mentions the content of methanol in % by
weight, based on the total weight of the extrudates.
This is determined by means of gas chromatography after
acidic total hydrolysis of the methoxy groups of the
resin. The methanol content corresponds to the methanol
which can potentially be released, and it is for this
reason that as low a methanol content as possible is
desired in the resin.
The curing time in s, stated in table 2, designates the
duration which is required to reach 10 Pa=s at 180 C
(dynamic mechanical analysis DMA).
From tables 1 and 2, it is evident that those modified
aminotriazine resins which were prepared by reactive
conversion with addition of aminotriazines are more
reactive, potentially have lower emissions and have a
higher viscosity in comparison with the resins having
the same formaldehyde:aminotriazine ratio which were
prepared in a conventional manner under similar and in
some cases more stringent extrusion conditions but
without addition of aminotriazines. It can also be seen
that an additional improvement in said properties can
be achieved on addition of oxoaminotriazines and
encapsulated compounds, such as Exolit AP462.
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Starting composition of the Addition in the extruder (o by Composition of
modified aminotriazine resin after
modified aminotriazine resin weight, based on amount of the reactive
conversion in the extruder
melts aminotriazine resin melt)
Addition [% by weight] Content of [% by weight]
Ex. Molar Modifier Content Aminotriazine Capsules3 Suspension Aminotriazine
Modifier Capsules3 Molar ratiol
No. ratio1 polyol2 of medium polyol2 F:aminotriazine
F:M [o by melamine polyolz
0
wt.] by
0
wt. ] cNn
C1 2.0:1 - 58.9 - - - 64.2 - - 2.0:1 2 2.5:1 - 53.4 13.3 (M) - - 66.0 - -
2.0:1 o
0
3 2.5:1 53.4 13 (OAT) - - 66.0 - - 2.0:1
0
C4 2.5:1 - 53.4 - - - 58.2 - - 2.5:1
3.0:1 - 48.9 8.9 (M) - - 59.4 - - 2.5:1
6 2.0:1 - 58.9 19.6 (M) - - 73.5 - - 1.5:1
7 2.0:1 - 58.9 10.0 (M) 12.2 - 61.5 - 10 1.71:1
C8 3.0:1 13.12 42.5 - - - 46.3 14.3 - 3.0:1
WO 2006/024544 13a - PCT/EP2005/009513
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9 3.5:1 - 45.0 7.5 (M)9 - 16.239 47.5 14.3 - 3.0:1
Table 1
1 M...melamine F...formaldeh de OAT...oxoaminotriazines
y (mixture of 73% of ammeline, 25% of ammelide, 2% of cyanuric acid)
2 Simulsol BPPE
3 Exolit AP462
9 Melamine added in suspension in polyol
0 N
Ln
tD
iP
iP
N
0
0
O
N
I
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Conditions in the reactive conversion of the modified Properties of the
modified aminotriazine resins
aminotriazine resin melts in the extruder after the reactive conversion in the
extruder
Ex. T02-1 TMelt TMax PExtr nExtr m' extr-iõ m' Extr-out Tg rl [ Pa = s] Curing
Content Appearance
No. [ C] [ C] [ C] [mbar] [rpm] [kg/h] [kg/h] [ C] isothermally time of
at 130 C DMA5 at methanol
180 C by M1
~
[s] wt.]
0
C1 225 220 245 400 330 10.7 9.6 81 1500 300 19.2 Clear
2 223 221 240 950 330 8.4 9.1 82 1800 250 18.4 Clear tD
3 220 215 230 950 330 8.4 9.1 82 2300 220 18.1 Opaque
0 0
C4 230 222 250 400 330 11.4 10.4 72 450 420 22.7 Clear
N
225 220 245 950 330 8.5 9.2 74 600 350 21.8 Opaque N
6 216 205 230 950 330 8.6 10.6 85 4900 210 16.2 Opaque
7 144 142 150 950 330 5.7 7.0 85 12 000 180 15.5 White
C8 235 222 250 400 330 9.3 8.3 50 50 580 20.2 Clear
9 230 220 245 950 330 8.5 9.3 55 150 450 19.1 Opaque
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Table 2
Determination of the curing time, time to reach 10 Pa=s at 180 C
~
0
N
Ln
tD
iP
iP
N
0
0
0
N
j
N I
N
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2 Production of a pure resin sheet from the modified
aminotriazine resin
A pressed sheet having the dimensions 100 x 100 x 3 mm
was produced from the modified aminotriazine resins,
prepared in 1, of experiments Cl, 2, 6, 7, C8, 9. A
laminate press served as a mold therefor. The granules
were milled and the powder was then introduced into the
stainless steel mold heated to 100 C and was melted for
about 8 min at this temperature.
Thereafter, the compression mold was heated to 180 C,
placed for 30 min in the press at 180 C and pressed at
80 bar. Thereafter, the test specimen was cooled in the
press to 70 C for a duration of about 15 min.
The pure resin sheet was removed from the mold at 70 C.
Test bars were produced from this pure resin sheet and
were used for carrying out mechanical tests and fire
tests in experiments A to F.
The fire test UL-94 is a test for determining the
flammability of materials. Classification is effected
according to fire classes V-0, V-1, V-2, n.p. V-0 is
the highest and therefore best fire class, i.e. the
fire behavior fulfills all test criteria. n.p. means
not passed, i.e. the fire behavior is poor. The UL-94
test is carried out according to ASTM 2863, vertically.
Furthermore, the time required for curing, the
emissions during processing and the volume contraction
as a measure of the shrinkage of the resin on curing
were determined.
The properties of the pure resin sheet are shown in
table 3.
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With respect to the fire tests, table 3 shows that the
modified aminotriazine resins according to the
invention have improved fire behavior in comparison
with the conventional resins. In experiments A and E,
which were carried out with conventional comparative
resins to which no aminotriazine was added, the fire
test was not passed. In experiments B, C and F, which
were carried out using the aminotriazine resins
according to the invention, fire classes V-1 and V-2
were reached. In experiment D, carried out using a
resin according to the invention additionally
containing the encapsulated compound AP462, it was
possible to achieve the best fire class V-0.
It is furthermore evident from table 3 that no
deterioration in the mechanical properties, such as
tensile strength and elongation at break, occurs in
comparison with the conventional modified aminotriazine
resins as a result of the reactive conversion of the
resin melts with aminotriazines.
The reactivity of the modified aminotriazine resins
according to the invention is substantially increased
in comparison with the conventional resins having the
same formaldehyde:melamine ratio. This is evident from
a substantially shorter curing time of the resins
according to the invention.
The modified aminotriazine resins according to the
invention exhibit lower emissions than the comparable
conventional resins.
Even in the case of the volume contraction as a measure
of the shrinkage of the resin during curing, there are
substantially lower values for the aminotriazine resins
according to the invention than in the case of the
conventional aminotriazine resins. Particularly low
values are to be observed in experiment D, carried out
using an aminotriazine resin containing the
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encapsulated compound Exolit AP462.
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3 Production of natural fiber composites
The modified aminotriazine resin according to the
invention, of experiments Cl, 2, 6, 7, C8, 9 from 1,
was sprinkled onto a flax fiber web having a weight per
unit area of 300-350 g/mz using a powder scattering
unit, a resin coat of about 30% of the total weight
being achieved. The powder-coated nonwoven was then
subjected to precondensation in an IR field at 190 C
for 2 min after which shapes measuring 300 x 200 mm
were punched out. 6 layers of powder-coated nonwovens
were then placed one on top of the other with the
powder-coated side facing upward, and this precondensed
fiber composite was placed in an evacuable down-stroke
press heated to 180 C. After a preheating time of 30
sec, pressing was effected to 400 kN for 20 sec in the
first pressing stage, the vacuum simultaneously being
set at 200 mbar absolute pressure. Thereafter venting
was effected for 20 sec in vacuo. In the second
pressing stage, the fiber composite was pressed until a
degree of curing of 95%, measured by means of
ultrasound, was reached. The cured composite material
was removed while hot at 180 C.
With the composite materials thus obtained, the same
tests as with the pure resin sheet from 2 were carried
out in experiments Al to Fl. The properties of the
composite materials produced are shown in table 4.
All advantages of the modified aminotriazine resins
according to the invention in comparison with the
conventional resins having the same
formaldehyde:aminotriazine ratio are also to be
observed in the case of the fiber composites produced
from the resins.
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Properties of the pure resin sheets - resin test specimens without reinforcing
fibers
Experiment Ex. No. Molar ratio6 UL-94 Tensile Elongation Curing time Mass loss
Volume
F:M 3mm sheet strength at break at 180 C during contraction
processing
(emissions)
[--] [MPa] [,--] [s] [o by wt.] ]
~
A Cl 2.0:1 n.p 35 1.5 300 4.0 10.1
0
B 2 2.0:1 V-2 35 1.7 250 3.1 9.5 cn
(from 2.5:1 tD
.P~
+ M)
0
0
0
C 6 1.5:1 (from V-1 30 1.5 210 2.2 8.2
2.0:1 + M)
D 7 1.71:1 V-0 35 1.4 180 1.8 6.5
(from 2.0:1
+ M + C)
E V8 3.0:1 + P n.p 25 2.5 580 11.0 12.2
F 9 3.0:1 + P V-2 30 2.0 450 9.0 11.0
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(from 3.5:1
+ P + M)
Table 3
6 M...Melamine F...Formaldehyde C...Capsules (Exolit AP462) P...Polyol
(Simulsol BPPE)
~
0
N
Ln
J
tD
iP
iP
N
0
0
I
O
N
I
N
N
tp
WO 2006/024544 - 19 PCT/EP2005/009513
-
Properties of the fiber composites - resin test specimens with natural fiber
reinforcement
Experiment Ex. No. Molar Fiber UL-94 Tensile Elongation Curing Mass loss
Volume
ratio' content 3mm sheet strength at break time at during contraction
F:M 180 C processing
(emissions)
[o] [--] [MPa] [o] [sec] [o by wt.] [o]
~
Al Cl 2.0:1 70 n.p 7900 3.1 350 2.1 2.5
0
N
Ln
Bl 2 2.0:1(from 70 V-2 8100 3.3 280 1.7 2.2 1O
.P~
2.5:1 + M)
0
0
C1 6 1.5:1 70 V-2 8000 3.5 230 1.4 1.6
( f r om
2.0:1 + M)
Dl 7 1.71:1 70 V-0 8200 3.7 200 0.9 0.8
(from
2.0:1 + M
+ C)
WO 2006/024544 PCT/EP2005/009513
- 19a -
El C8 3.0:1 + P 70 n.p. 6000 4.5 650 3.0 3.5
F1 9 3.0:1 + P 70 V-2 6500 4.8 480 2.8 2.9
(from
3.5:1 + P
+ M)
Table 4
~
0
M...Melamine F...Formaldehyde C...Capsules (Exolit AP462) P...Polyol (Simulsol
BPPE) ~
.P~
O
O
O
