U.S. patent application number 09/833208 was filed with the patent office on 2002-01-24 for resin composition for building material and insulating glass.
This patent application is currently assigned to Asahi Glass Company Ltd.. Invention is credited to Kotera, Seigo, Matsuyama, Yoshitaka, Nakagawa, Hideki, Shibuya, Takashi.
Application Number | 20020009557 09/833208 |
Document ID | / |
Family ID | 26520553 |
Filed Date | 2002-01-24 |
United States Patent
Application |
20020009557 |
Kind Code |
A1 |
Shibuya, Takashi ; et
al. |
January 24, 2002 |
Resin composition for building material and insulating glass
Abstract
An insulating glass comprising two or more glass sheets which
are arranged to face one another to form an air space layer
therebetween by a spacer made of a resin having a JIS A hardness of
from 10 to 90 at 25.degree. C., prepared by using a thermoplastic
resin composition comprising a butyl type rubber and a crystalline
polyolefin, wherein the proportion of the butyl type rubber is from
50 to 98 wt %, and the proportion of the crystalline polyolefin is
from 2 to 50 wt %, based on the total amount of the two.
Inventors: |
Shibuya, Takashi; (Kanagawa,
JP) ; Kotera, Seigo; (Kanagawa, JP) ;
Nakagawa, Hideki; (Kanagawa, JP) ; Matsuyama,
Yoshitaka; (Kanagawa, JP) |
Correspondence
Address: |
OBLON SPIVAK MCCLELLAND MAIER & NEUSTADT PC
FOURTH FLOOR
1755 JEFFERSON DAVIS HIGHWAY
ARLINGTON
VA
22202
US
|
Assignee: |
Asahi Glass Company Ltd.
Kanagawa
JP
|
Family ID: |
26520553 |
Appl. No.: |
09/833208 |
Filed: |
April 12, 2001 |
Related U.S. Patent Documents
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Application
Number |
Filing Date |
Patent Number |
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09833208 |
Apr 12, 2001 |
|
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|
08894564 |
Oct 16, 1997 |
|
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6235356 |
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Current U.S.
Class: |
428/34 ; 428/516;
428/517 |
Current CPC
Class: |
C08L 23/10 20130101;
E06B 3/66328 20130101; C08L 23/22 20130101; C03C 27/10 20130101;
B32B 17/1055 20130101; B32B 17/10036 20130101; Y10T 428/31917
20150401; C08L 23/04 20130101; Y10T 428/31913 20150401; C08L 23/22
20130101; C08L 2666/04 20130101 |
Class at
Publication: |
428/34 ; 428/516;
428/517 |
International
Class: |
E06B 003/24 |
Foreign Application Data
Date |
Code |
Application Number |
Dec 26, 1995 |
JP |
7-339629 |
Aug 14, 1996 |
JP |
8-214865 |
Dec 25, 1996 |
JP |
PCT/JP96/03787 |
Claims
1. A resin composition for building material, which comprises a
butyl type rubber and a crystalline polyolefin, wherein the
proportion of the butyl type rubber is from 50 to 98 wt %, and the
proportion of the crystalline polyolefin is from 2 to 50 wt %,
based on the total amount of the two.
2. A resin composition for building material, which comprises a
butyl type rubber, a crystalline polyolefin and an inorganic
filler, wherein the proportion of the butyl type rubber is from 50
to 98 wt %, and the proportion of the crystalline polyolefin is
from 2 to 50 wt %, based on the total amount of the butyl type
rubber and the crystalline polyolefin, and the proportion of the
inorganic filler is at most 200 parts by weight per 100 parts by
weight of the sum of the butyl type rubber and the crystalline
polyolefin.
3. The resin composition for building material according to claim 1
or 2, wherein the crystalline polyolefin is at least one polymer
selected from polyethylene, polypropylene and their modified
products.
4. An insulating glass comprising two or more glass sheets which
are arranged to face one another as spaced by a spacer to form an
air space layer therebetween, wherein said spacer is made of a
thermoplastic resin composition having a JIS A hardness of from 10
to 90 at 25.degree. C.
5. The insulating glass according to claim 4, wherein said spacer
is made of a thermoplastic resin composition having a creep
compliance J, as an index for creep characteristics, of from
1.times.10.sup.-10 (cm.sup.2/dyne) to 1.times.10.sup.-5
(cm.sup.2/dyne) as measured after 5 minutes from initiation of the
measurement in a shear deformation mode at 40.degree. C.
6. The insulating glass according to claim 4 or 5, wherein said
thermoplastic resin composition comprises at least two types of
thermoplastic resins, one of which is a hot-melt moldable rubber or
elastomer, and a drying agent.
7. The insulating glass according to claim 4 or 5, wherein said
thermoplastic resin composition comprises the following
components:
8 Hot-melt moldable rubber or elastomer 10 to 80 wt % Thermoplastic
resin other than said 0 to 50 wt % ruber or elastomer Tackifier 0
to 15 wt % Drying agent and additives 10 to 60 wt %
8. The insulating glass according to claim 4 or 5, wherein said
thermoplastic resin composition comprises a butyl type rubber and a
crystalline polyolefin, wherein the proportion of the butyl type
rubber is from 50 to 98 wt %, and the proportion of the crystalline
polyolefin is from 2 to 50 wt %, based on the total amount of the
two.
9. The insulating glass according to claim 4 or 5, wherein said
thermoplastic resin composition comprises a butyl type rubber, a
crystalline polyolefin and an inorganic filler, wherein the
proportion of the butyl type rubber is from 50 to 98 wt %, and the
proportion of the crystalline polyolefin is from 2 to 50 wt %,
based on the total amount of the butyl type rubber and the
crystalline polyolefin, and the proportion of the inorganic filler
is at most 200 parts by weight per 100 parts by weight of the sum
of the butyl type rubber and the crystalline polyolefin.
10. The insulating glass according to claim 8 or 9, wherein the
crystalline polyolefin is at least one polymer selected from
polyethylene, polypropylene and their modified products.
11. The insulating glass according to any one of claims 7 to 10,
wherein the moisture permeation constant of the thermoplastic resin
other than said rubber or elastomer, or the moisture permeation
constant of the crystalline polyolefin, is at most
300.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.multidot.Pa.
12. The insulating glass according to any one of claims 6 to 11,
wherein the moisture permeation constant of said hot-melt moldable
rubber or elastomer, or the moisture permeation constant of the
butyl type rubber, is at most 3000.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.s- ec.multidot.Pa.
13. The insulating glass according to any one of claims 4 to 12,
wherein the moisture permeation constant of said thermoplastic
resin composition is at most 5000.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.s- ec.multidot.Pa.
Description
TECHNICAL FIELD
[0001] The present invention relates to a resin composition for
building material, particularly a resin composition for a spacer
for an insulating glass, and an insulating glass employing a spacer
made of a resin.
BACKGROUND ART
[0002] In recent years, insulating glasses have attracted attention
from the viewpoint of energy saving, and they are commercial
products, the demand of which continues to increase. For their
production, many steps are required. Accordingly, their costs are
high as compared with usual glass sheets, and it is desired to
further lower the costs.
[0003] Most of insulating glasses presently available have a
structure as shown in FIG. 4, wherein at least two glass sheets 1a
and 1b are arranged to face one another via a spacer 2 to form an
air space layer between the glass sheets 1a and 1b. And, a primary
sealing material 3 is interposed between the spacer 2 and the glass
sheets 1a and 1b to insulate the air space layer from the external
air, and a cavity (recess) defined by the peripheral surface of the
spacer and the inside surfaces of the peripheral portions of the
glass sheets facing to one another, is sealed by a cold-setting
secondary sealing material represented by a polysulfide type or a
silicone type sealing material.
[0004] Heretofore, various improvements in productivity by
simplification or automation and attempts for cost down have been
studied and proposed for the process for producing insulating
glasses. For example, a system for folding an aluminum spacer, or
automation of the method of injection the cold-setting sealing
material, may be mentioned. Further, as shown in FIG. 5, a method
of employing a resin having a drying agent kneaded therein, as a
spacer 4 instead of an aluminum spacer, has been proposed.
[0005] However, an insulating glass employing such a cold-setting
sealing material requires curing for a long period of time for
setting of the sealing material after preparation of the insulating
glass, irrespective of the type of the spacer used. Accordingly,
the product can not be shipped until completion of the curing.
[0006] Thus, it is necessary to provide a space for curing in the
plant and to ship the product after storing it for a predetermined
period of time, whereby the time period of delivery tends to be
long, and it has been difficult to meet the demand of customers.
Further, in order to comply with the demand which appears to
increase in future, a wider space for curing will be required, and
to secure adequate supply of insulating glasses while avoiding such
a wider space, it is considered necessary to shorten the curing
time.
[0007] From the viewpoint of lowering the costs for insulating
glasses, a method has been proposed in which a molded product made
of a resin having a drying agent kneaded therein is used as a
spacer, and an insulating glass is prepared without using a
secondary sealing material (JP-B-61-20501). However, this resin for
spacer is inadequate in hardness as a spacer, and with the spacer
made of the above resin alone, it has been practically difficult to
maintain the shape of an insulating glass.
[0008] Further, an insulating glass is known in which a material
having a drying agent kneaded into an extrusion moldable hard
resin, for example, a thermoplastic resin such as a vinyl chloride
resin or a hot-melt butyl and having a JIS A hardness (HsA) of 95,
is used as a spacer (JP-A-7-17748). However, if this material
having a hardness of HsA95 is used as a spacer or a sealing
material for an insulating glass, the stress which will be exerted
to the glass sheets or the sealing portion of the insulating glass
will be so large that there will be difficulties such that the
sealing portion undergoes peeling or the glass sheets of the
insulating glass undergo breakage. Accordingly, at present, no
insulating glass is known which fully satisfies the properties such
as useful life, dimensional stability and moldability required for
an insulating glass solely by a spacer without using a secondary
sealing material.
[0009] Meanwhile, as illustrated by a hot-melt butyl in the
above-mentioned publications, a butyl type rubber is used as a
sealing agent for building material by virtue of its adhesive
property, high weather resistance and low moisture permeability.
However, the hardness is low, and it has a cold flow property.
Accordingly, depending upon the particular purpose of use, it has a
problem from the viewpoint of durability for a long period of time,
if used alone. Further, it also has a problem that the melt
viscosity is high, and the operation efficiency is poor. To improve
the hardness, it has been proposed to mix various fillers, but if
it is attempted to improve the hardness only by adding a filler,
the melt viscosity tends to increase, whereby the operation
efficiency will be impaired, and in some cases, the tensile
strength or the tear strength tends to be low, such being
undesirable.
[0010] Namely, the butyl type rubber has a function to seal the
interface between the spacer and the glass sheets and to maintain
the air tightness, and thus it is suitable for use as an end
sealing material for an insulating glass. In such a case, as the
hardness of the butyl type rubber is low, it is common to use a
spacer made of a metal such as aluminum, and the butyl type rubber
is disposed as a sealing material between the spacer and the glass
sheets. Thus, the process for producing an insulating glass will be
complicated, since it is required to use a spacer made of a metal
as described above.
[0011] Accordingly, it is desired to develop a sealing agent which
does not require a spacer made of a metal and which is capable of
simplifying the production process. At present, no insulating glass
has been known which fully satisfies the properties such as useful
life, dimensional stability and moldability required for an
insulating glass solely by a spacer without using a secondary
seal.
[0012] An object of the present invention is to provide a resin
composition which satisfies properties required for use as building
material, particularly a resin composition for a spacer which does
not substantially require the above-mentioned secondary sealing
material in an insulating glass. Further, another object of the
present invention is to solve the problem of curing which requires
a long period of time after the preparation and to provide an
insulating glass which is capable of realizing high productivity
which has not been attained heretofore.
DISCLOSURE OF THE INVENTION
[0013] The present invention provides a resin composition for
building material, which comprises a butyl type rubber and a
crystalline polyolefin, wherein the proportion of the butyl type
rubber is from 50 to 98 wt %, and the proportion of the crystalline
polyolefin is from 2 to 50 wt %, based on the total amount of the
two.
[0014] Further, the present invention provides a resin composition
for building material, which comprises a butyl type rubber, a
crystalline polyolefin and an inorganic filler, wherein the
proportion of the butyl type rubber is from 50 to 98 wt %, and the
proportion of the crystalline polyolefin is from 2 to 50 wt %,
based on the total amount of the butyl type rubber and the
crystalline polyolefin, and the proportion of the inorganic filler
is at most 200 parts by weight per 100 parts by weight of the sum
of the butyl type rubber and the crystalline polyolefin.
[0015] Still further, the present invention provides an insulating
glass comprising two or more glass sheets which are arranged to
face one another as spaced by a spacer to form an air space layer
therebetween, wherein said spacer is made of a thermoplastic resin
composition having a JIS A hardness of from 10 to 90 at 25.degree.
C.
BRIEF DESCRIPTION OF THE DRAWINGS
[0016] FIG. 1 is a schematic partial cross-sectional view showing
an example of the structure of an insulating glass of the present
invention. FIG. 2 is a schematic partial cross-sectional view
showing the structure of an insulating glass prior to double
glazing by means of a spacer made of a thermoplastic resin
composition. FIG. 3 is a schematic view of an extruder used for
melting a thermoplastic resin composition in the present invention.
FIG. 4 is a cross-sectional view showing an example of the
structure of a conventional insulating glass. FIG. 5 is a
cross-sectional view showing an example of the structure of a
conventional insulating glass. FIG. 6 is a schematic
cross-sectional view illustrating an example of the method for
measuring creep compliance J.
BEST MODE FOR CARRYING OUT THE INVENTION
[0017] Now, the present invention will be described in further
detail with reference to the drawings.
[0018] FIG. 1 is a schematic partial cross-sectional view showing
an example of the structure of an insulating glass of the present
invention, wherein the insulating glass 10 comprises two glass
sheets 1a and 1b which are held in a predetermined distance solely
by a spacer 20 so as to form an air space layer 30 inbetween. The
spacer 20 is made of a thermoplastic resin composition having a JIS
A hardness of from 10 to 90. Here, the above "solely by a spacer
20" means that no other secondary sealing material or metal spacer
is required, and primer treatment which may be applied as the case
requires, is included.
[0019] The thermoplastic resin composition used as a spacer
material in the construction of the insulating glass of the present
invention is a thermoplastic resin composition having a JIS A
hardness of from 10 to 90 at 25.degree. C. As such a resin
composition for spacer, any thermoplastic resin composition may be
used so long as it has the above-mentioned properties.
[0020] Further, a thermoplastic elastomer which is used in various
fields in recent years, or a rubber material having the
vulcanization density adjusted to make it melt-flowable by heating,
is also included in the "thermoplastic resin composition" for the
purpose of the present invention, so long as it has the
above-mentioned properties. Further, a blend product having a
so-called plasticizer such as dibutyl phthalate or di-2-ethylhexyl
phthalate incorporated to such a thermoplastic resin composition,
is also included in the "thermoplastic resin composition" for the
purpose of the present invention, so long as it has the
above-mentioned properties.
[0021] Specifically, the above resin composition to be used in the
present invention preferably contains at least one of a low
moisture permeable hot-melt moldable rubber or elastomer and a low
moisture permeable thermoplastic resin other than such rubber or
elastomer. More preferably it contains both of them. Further, in
order to prevent penetration of moisture into the air space layer
of an insulating glass when such an insulating glass is
constructed, the resin composition preferably has a predetermined
amount of a drying agent kneaded therein.
[0022] The above low moisture permeable hot-melt moldable rubber or
elastomer is preferably a rubber or elastomer having a moisture
permeation constant of at most 3000.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.multidot.Pa.
Particularly preferred among them is a butyl type rubber such as
halogenated butyl rubber or butyl rubber composed mainly of
polyisobutylene, or isobutylene and isoprene. Such thermoplastic
resins and low moisture permeable hot-melt moldable rubbers or
elastomers may be used alone or in combination as a blend of two or
more of them.
[0023] The low moisture permeable thermoplastic resin other than
said rubber or elastomer may, for example, be polyethylene,
polypropylene, vinylidene chloride or polyvinyl chloride, or a
copolymer of monomers constituting such polymers, or a modified
product thereof. Particularly preferred is high density
polyethylene. The moisture permeation constant of these
thermoplastic resins is preferably at most 3000.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.multidot.Pa, more
preferably at most 500.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.m- ultidot.Pa. Such a
thermoplastic resin contributes to the dimensional stability of the
spacer.
[0024] To the resin composition for spacer in the present
invention, in addition to the above-mentioned low moisture
permeable hot-melt moldable rubber or elastomer and the
thermoplastic resin other than such rubber or elastomer, a drying
agent may be incorporated, and further an inorganic filler or other
additives may be incorporated as the case requires. As the drying
agent, any drying agent which is commonly used as mixed to a
sealing material or a spacer for a conventional insulating glass,
such as zeolite, alumina or silica gel, may be used.
[0025] Such a resin composition for spacer comprises the
above-mentioned components as desired components. However,
additives such as a tackifier, a lubricant, a pigment, an
antistatic agent, an antioxidant, a heat stabilizer, a filler and a
blowing agent, may be incorporated to the above thermoplastic
resin, as the case requires.
[0026] Such a resin composition for spacer is prepared by kneading
the above-described components. In its preparation, the necessary
components will be blended so that the JIS A hardness of the
resulting resin composition will be at most 90 at 25.degree. C. The
reason for limiting the hardness to at most 90 is as follows.
[0027] If it is attempted to use a thermoplastic resin having a JIS
A hardness exceeding 90 as a spacer for an insulating glass, no
substantial creep takes place, and thus when a durability test
specified in JIS R3209 is carried out thereon, the stress due to
expansion of air at a high temperature will be exerted to the
bonding interface between the glass sheets and the spacer.
Therefore, if the bonding force is inadequate, peeling will result,
and even if an adequate bonding force is secured, the glass is
likely to break. Even with an adhesive currently available, it is
possible to obtain a bonding force high enough to be durable
against a stress due to expansion of the air space layer due to a
high temperature or a high pressure. However, breakage of the glass
is likely to occur under such a high pressure at a high
temperature, whereby the productivity decreases substantially, and
such is not suitable for the purpose of the present invention
intended to reduce the production costs.
[0028] On the other hand, if the hardness is too low, there will be
a problem in the dimensional stability of the insulating glass.
Accordingly, it is necessary to blend the necessary components so
that the JIS A hardness of the resin composition will be at least
10 at 25.degree. C. Further, even if the JIS A hardness is at least
10, if the hardness is relatively small, sheet-shifting is likely
to result when the air space layer is thick.
[0029] In an insulating glass which is commonly used, the thickness
of the air space layer is from about 4 to 18 mm (6 mm or 12 mm in
many cases). Accordingly, in a case where the hardness is
relatively low, even if no sheet-shifting takes place with one
having an air space layer thickness of 6 mm, sheet-shifting may
sometimes takes place with one having an air space layer thickness
of 12 mm. By making the hardness to a level of at least 40, it is
possible to avoid sheet-shifting even with one having an air space
layer thickness of 12 mm. Therefore, in the insulating glass of the
present invention, the JIS A hardness of the thermoplastic resin
spacer is particularly preferably at least 40.
[0030] In an insulating glass wherein a resin composition having a
JIS A hardness exceeding 90 is used as a spacer, the stress exerted
to glass sheets will be large. Therefore, even with an insulating
glass employing either one of glass sheets having thicknesses of 5
mm and 3 mm, as stipulated in JIS R3209, glass breakage will result
during an accelerated durability test.
[0031] Whereas, in the case of an insulating glass wherein a resin
composition having a JIS A hardness of 90 is used as a spacer, no
glass breakage will occur in the above test with an insulating
glass wherein glass sheets having a thickness of 5 mm are used. On
the other hand, with an insulating glass wherein glass sheets
having a thickness of 3 mm are used, there has been a possibility
that glass breakage occurs in the above test. Accordingly, the
upper limit of the JIS A hardness of the resin composition for
spacer is 90. Further, with an insulating glass wherein a resin
composition having a JIS A hardness of 75 is used as a spacer, no
glass breakage will occur in the above test in either case of
insulating glasses employing glass sheets having thicknesses of 5
mm and 3 mm. Glass sheets for insulating glasses commonly used at
present have a thickness of 3 mm, and the JIS A hardness of the
resin composition for spacer is accordingly preferably within a
range of from 40 to 75.
[0032] While the JIS A hardness dictates a stress exerted
instantaneously, the creep compliance J as an index for creep
characteristics, indicates a resin property in a case where a
continuous stress is exerted, and it is represented by a reciprocal
number of the modulus of elasticity. This creep compliance J is
measured, for example, as follows.
[0033] FIG. 6 is a schematic cross-sectional view showing a method
for measuring the creep compliance J. A resin material 60 to be
measured, is shaped to have a thickness of 12 mm and a size of the
surface area bonded to each glass sheet 61a or 61b being
10.times.50 (mm). And, the glass sheets are pulled in the
directions shown by arrows in the FIG. at an ambient temperature of
40.degree. C. so that a stress of 0.2 kg/cm.sup.2 is always exerted
to the resin material, whereby the creep compliance J is calculated
from the elongation of the material after 5 minutes. The value of J
does not depend on the thickness of the glass sheets 61a and 61b,
but here, glass sheets having a thickness of 5 mm are used.
[0034] For example, when an insulating glass is put on a pallet,
for the transportation after its preparation, a glass sheet on one
side of the insulating glass will be adsorbed by suction cups. It
is likewise adsorbed also when the insulating glass is taken out
from the pallet. Such a so-called "cantilever" state of the
insulating glass by suction cups will usually be at most 5 minutes.
Further, the outdoor temperature in the summer time is likely to
rise to about 40.degree. C. Therefore, in order to prevent
sheet-shifting during the operation, the creep compliance J is
preferably at most 1.times.10.sup.-5 (cm.sup.2/dyne) as measured
after 5 minutes from initiation of the measurement in a shear
deformation mode at 40.degree. C. Further, if the creep compliance
J is less than 1.times.10.sup.-10 (cm.sup.2/dyne) as measured after
5 minutes from initiation of the measurement in a shear deformation
mode at 40.degree. C., there will be no substantial creep, whereby
the stress exerted between the glass sheets and the spacer
increases to bring about a problem such as peeling or glass
breakage. Accordingly, J is preferably at least 1.times.10.sup.-10
(cm.sup.2/dyne) as measured after 5 minutes from initiation of the
measurement in a shear deformation mode at 40.degree. C.
[0035] As mentioned above, the thickness of the air space layer in
an insulating glass is from about 4 to 18 mm in many cases.
Therefore, even if the creep compliance J is less than
1.times.10.sup.-5 (cm.sup.2/dyne) as measured after 5 minutes from
initiation of the measurement in a shear deformation mode at
40.degree. C., if the creep compliance J is relatively large,
sheet-shifting may sometimes occur when the air space layer is
thick. For example, when the creep compliance J is large, even if
no sheet-shifting occurs with one having an air space layer
thickness of 6 mm, sheet-shifting may sometimes occur with one
having an air space layer thickness of 12 mm. Therefore, by
adjusting the creep compliance to a level of at most
1.times.10.sup.-6 (cm.sup.2/dyne), it is possible to avoid
sheet-shifting even with one having an air space layer thickness of
12 mm.
[0036] Further, it is particularly preferred that the lower limit
of the creep compliance J is 1.times.10.sup.-9 (cm.sup.2/dyne).
Namely, at a value of 1.times.10.sup.-10 (cm.sup.2/dyne), for
example, in a durability test stipulated in JIS R3209, even if
glass sheets do not break with an insulating glass employing glass
sheets having a thickness of 5 mm, glass sheets may sometimes break
with an insulating glass employing glass sheets having a thickness
of 3 mm. Therefore, to avoid breakage of glass sheets with glass
sheets of various thicknesses, it is particularly preferred that
the lower limit of the creep compliance J is 1.times.10.sup.-9
(cm.sup.2/dyne) as measured after 5 minutes from initiation of the
measurement in a shear deformation mode at 40.degree. C.
[0037] In summary, as the resin composition to be used as a spacer
in the present invention, it is particularly preferred to employ
one having a JIS A hardness of from 40 to 75 and a creep compliance
J within a range of from 1.times.10.sup.-6 to 1.times.10.sup.-9
(cm.sup.2/dyne) as measured after 5 minutes from initiation of the
measurement in a shear deformation mode at 40.degree. C.
[0038] Further, it is preferred that as the entire resin
composition, the moisture permeation constant is at most
500.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.multidot.Pa, and
further, in order to maintain the dew point property, the moisture
permeation constant is preferably at most 500.times.10.sup.-13
cm.sup.3.multidot.cm/cm.sup.2.multidot.sec.multidot.Pa.
[0039] Specific examples of the resin composition for spacer having
the foregoing JIS A hardness, creep compliance J and moisture
permeation constant, will be described in Examples which will be
given hereinafter. However, blend components of preferred resin
compositions and their blend proportions are as follows.
1 Hot-melt moldable rubber or elastomer 10 to 80 wt % Thermoplastic
resin other than said 0 to 50 wt % ruber or elastomer Tackifier 0
to 15 wt % Drying agent and additives 10 to 60 wt % (carbon black,
talc, etc.)
[0040] Here, the additives include, for example, a lubricant, a
pigment, an antistatic agent, a plasticizer, an aging-preventive
agent, a heat stabilizer, an antioxidant, a hydrolyzable silyl
group-containing compound such as a silane coupling agent, a
blowing agent and a filler containing an inorganic filler. The term
"additives" used elsewhere means those having an inorganic filler
extruded from the above additives and having a tackifier included
thereto.
[0041] As other preferred resin compositions for spacer, the
following compositions may be mentioned wherein a butyl type rubber
is used as the hot-melt moldable rubber or elastomer, and a
crystalline polyolefin is used as the thermoplastic resin other
than said rubber and elastomer.
[0042] A resin composition comprising a butyl type rubber and a
crystalline polyolefin, wherein the proportion of the butyl type
rubber is from 50 to 98 wt %, and the proportion of the crystalline
polyolefin is from 2 to 50 wt %, based on the total amount of the
two.
[0043] A resin composition comprising a butyl type rubber, a
crystalline polyolefin and an inorganic filler, wherein the
proportion of the butyl type rubber is from 50 to 98 wt %, and the
proportion of the crystalline polyolefin is from 2 to 50 wt %,
based on the total amount of the butyl type rubber and the
crystalline polyolefin, and the proportion of the inorganic filler
is at most 200 parts by weight per 100 parts by weight of the sum
of the butyl type rubber and the crystalline polyolefin.
[0044] In the present invention, the butyl type rubber may, for
example, be a homopolymer of isobutylene, a copolymer thereof with
other monomer, or a modified product thereof. Preferred as the
copolymer, is a copolymer obtainable by copolymerization with a
relatively small amount of isoprene (one usually called butyl
rubber). The modified product may, for example, be halogenated
butyl rubber or partially cross-linked butyl rubber. Particularly
preferred butyl type rubbers are a copolymer of isobutylene with
isoprene, which is usually called butyl rubber, and partially
cross-linked butyl rubber.
[0045] In the present invention, the crystalline polyolefin may,
for example, be a homopolymer of an olefin such as ethylene or
propylene, a copolymer thereof with other monomer, or a modified
product thereof, which has crystallizability. The structure of the
polymer is preferably a syndiotactic structure or an isotactic
structure, but it may contain other structures. The olefin is
particularly preferably ethylene or propylene.
[0046] The copolymer may, for example, be a copolymer of two or
more olefins, or a copolymer of an olefin with other monomers, and
preferred is a copolymer of ethylene or propylene with other
monomer which does not hinder the crystallizability. As the
copolymer, a block copolymer is preferred to an alternating
copolymer or a random copolymer. The modified product may, for
example, be a crystalline polyolefin having functional groups such
as acid anhydride groups, carboxyl groups or epoxy groups
introduced.
[0047] A particularly preferred crystalline polyolefin in the
present invention is polyethylene or polypropylene as a substantial
homopolymer. For example, as the polyethylene, low density
polyethylene, intermediate density polyethylene or high density
polyethylene may be used. The crystallinity of the crystalline
polyolefin is preferably at least 30%, more preferably at least
50%. For example, with respect to usual crystalline polyolefins,
typical values of crystallinity are from 50 to 60% with low density
polyethylene, from 75 to 90% with high density polyethylene, and
from 55 to 65% with polypropylene. The molecular weight is not
particularly limited, but the number average molecular weight is
from about 200,000 to 800,000 with polyethylene, and from about
100,000 to 400,000 with polypropylene.
[0048] As described above, polyethylene or polypropylene has high
crystallizability and thus is less moisture permeable than the
butyl type rubber. With one having a lower melt viscosity among
them, the melt viscosity of the composition decreases and the
moldability improves as compared with a case where the butyl type
rubber is used alone. Accordingly, various inorganic fillers may be
blended, whereby a resin material for spacer having high hardness
can be realized, and such is particularly preferred also from the
viewpoint of the economical efficiency.
[0049] In the above resin composition, the proportion of the
crystalline polyolefin in the total amount of the butyl type rubber
and the crystalline polyolefin is from 2 to 50 wt %, preferably
from 5 to 40 wt %. If the proportion of the crystalline polyolefin
is less than 2 wt %, it tends to be difficult to attain the high
hardness of the butyl type rubber, and if it exceeds 50 wt %, the
nature of the crystalline polyolefin tends to be predominant,
whereby the characteristics of the butyl type rubber tend to be
hardly obtainable.
[0050] When an inorganic filler is incorporated, the proportion of
the crystalline polyolefin in the total amount of the butyl type
rubber and the crystalline polyolefin may be small. For example,
when an inorganic filler is incorporated in an amount of at least
about 50 parts by weight per 100 parts by weight of the sum of the
butyl type rubber and the crystalline polyolefin, the proportion of
the crystalline polyolefin in the total amount of the butyl type
rubber and the crystalline polyolefin may be from 2 to 20 wt %,
whereby adequate intended effects can be obtained.
[0051] Thus, a substantially effective amount of an inorganic
filler can be incorporated to the resin composition of the present
invention comprising the butyl type rubber and the crystalline
polyolefin. The substantially effective amount means at least 1
part by weight per 100 parts by weight of the sum of the butyl type
rubber and the crystalline polyolefin. If the inorganic filler is
incorporated too much, the melt viscosity of the composition will
increase, or the tensile strength or the tear strength will
decrease. Therefore, the upper limit of the amount of its
incorporation is 200 parts by weight, preferably 150 parts by
weight. In the case where an inorganic filler is incorporated, a
preferred lower limit of the amount of its incorporation is 10
parts by weight.
[0052] As the inorganic filler, those commonly used as inorganic
fillers, such as calcium carbonate, talc, mica, and carbon black,
may be used alone or in combination as a mixture of two or more of
them.
[0053] It is particularly effective that the butyl type rubber and
the crystalline polyolefin contained in the resin composition of
the present invention are mixed at a high temperature, at least
before the resin composition of the present invention is used for
the final application. The high temperature in this mixing is a
temperature which is at least the crystal fusion point of the
crystalline polyolefin. This mixing temperature is required to be
less than the decomposition point of the butyl type rubber and is
preferably at most about 300.degree. C. which is the decomposition
point of the butyl type rubber. The temperature is particularly
preferably at most 200.degree. C. from the viewpoint of the
productivity, etc. Accordingly, the crystal fusion point of the
crystalline polyolefin is also preferably at most 200.degree.
C.
[0054] The resin composition for building material should
preferably undergo hardness change as little as possible within its
practically useful temperature range. To satisfy such a
requirement, the crystalline polyolefin is preferably one having a
crystal fusion point higher than a usual practical upper limit
temperature. The usual practical upper limit temperature for the
resin composition for building material is about 80.degree. C.
[0055] In the present invention, the crystalline polyolefin is
restrained by cohesive force of the crystalline phase, whereby even
in a temperature range exceeding the glass transition temperature,
no abrupt decrease in hardness or no fluidized state will be
observed at a temperature lower than the crystal fusion point,
which is observable with a non-crystalline resin. On the contrary,
a remarkable decrease in the melt viscosity will be observed at the
crystal fusion point as the boundary, whereby an effect for
improving the kneading efficiency with the butyl type rubber can be
expected.
[0056] To such a resin composition, a drying agent and the
above-mentioned additives which can commonly be incorporated to
resin materials for building material, can be incorporated.
Especially when this resin composition is used for a spacer, it is
preferred to incorporate a drying agent such as zeolite, silica gel
or alumina, a tackifier, a plasticizer, a silane coupling agent and
various stabilizers.
[0057] It is particularly preferred to incorporate a drying agent
such as zeolite in an amount of from 5 to 30 wt % to the resin
composition. Further, to impart the tackifying effects and
plasticizing effects, it is preferred to add polyisobutylene in an
amount of at least 200 parts by weight, particularly from 5 to 150
parts by weight, per 100 parts by weight of the butyl type rubber
other than polyisobutylene.
[0058] In summary, in the present invention, particularly preferred
blending proportions of components of the resin composition for
spacer are from 30 to 55 wt % of the butyl type rubber, from 1 to 8
wt % of the crystalline polyolefin, from 15 to 30 wt % of the
inorganic filler, and from 20 to 40 wt % of the drying agent and
additives (of course, here, the proportion of the butyl type rubber
is from 50 to 98 wt %, and the proportion of the crystalline
polyolefin is from 2 to 50 wt %, based on the total amount of the
butyl type rubber and the crystalline polyolefin).
[0059] As mentioned above, the resin composition of the present
invention is preferably prepared by mixing at least the butyl type
rubber and the crystalline polyolefin at a temperature higher than
the crystal fusion point of the crystalline polyolefin and lower
than the decomposition point of the butyl type rubber. This mixing
temperature is preferably from 100 to 280.degree. C., particularly
from 120 to 250.degree. C. Other blend components or additives may
be mixed simultaneously or may be mixed before or after the
mixing.
[0060] The composition of the present invention is substantially a
thermoplastic composition and can be mixed by a usual mixer such as
a melt mixing extruder or a kneader. Further, molding can be
carried out continuously after the above mixing operation.
Otherwise, the composition is prepared and then formed into a
molding material of a pellet form or the like, which is then
subjected to molding. As the molding method, a melt molding method
such an extrusion molding method or an injection molding method can
be used.
[0061] When this resin composition is used for a spacer, the
molding operation may be followed continuously by preparation of an
insulating glass by placing the molded product along the edge of an
insulating glass material comprising two or more glass sheets
arranged to face one another. Here, by using a high temperature
composition discharged from the molding machine, a high level of
adhesion to glass sheets can be attained. Further, by means of an
apparatus such as an applicator, the molded product can be applied
to the insulating glass material while controlling the temperature
drop of the composition. As such an apparatus, one capable of
heating is preferred.
[0062] The above-described resin composition for building material
is not limited to a composition for forming a spacer for an
insulating glass having the structure shown in FIG. 1. For example,
the resin composition for building material of the present
invention can be used as a material for a sealing material, in an
insulating glass of a structure wherein the edge is sealed by a
combination of a sealing material and a spacer made of a material
harder than this resin for building material (such as a spacer made
of a metal or a hard synthetic resin). Further, the resin
composition for building material of the present invention can be
used also as a resin material for use as a building material other
than an insulating glass.
[0063] On the other hand, as mentioned above, the resin composition
for building material of the present invention is particularly
superior as a resin composition for a resin spacer which is useful
for an insulating glass of a structure in which glass sheets are
held as spaced by the hardness of the resin material. And, by
adjusting the blending amount of the crystalline polyolefin or the
inorganic filler to obtain a resin material having a suitable
hardness, it is possible to realize a resin spacer for an
insulating glass which has a JIS A hardness (HsA) of from 10 to 90
at 25.degree. C.
[0064] The spacer material in the present invention is not
particularly limited to the above-mentioned blending components and
proportions. However, within the above blending proportions, it is
possible to obtain a resin composition having a JIS A hardness and
moisture permeation constant preferred in the present
invention.
[0065] The glass sheets to be used for the construction of the
insulating glass of the present invention may, for example, be
glass sheets for windows or doors, reinforced glass, laminated
glass, metal wire glass and heat absorbing glass, which are usually
widely used for vehicles or as building materials, as well as glass
sheets having a thin coating of a metal or other inorganic
substance applied on their surface, such as heat reflecting glass
or low reflectance glass, acrylic resin sheets so-called organic
glass, or polycarbonate sheets, and they are not particularly
limited.
[0066] Further, the insulating glass may be composed of two glass
sheets or may be composed of three or more glass sheets.
[0067] For the insulating glass of the present invention, an
adhesive dissolved in a solvent may be coated to the glass surface
against which the spacer abuts, as the case requires. And after
drying the adhesive in air, two glass sheets 1a and 1b are held in
a predetermined distance (for example 6 mm or 12 mm) as shown in
FIG. 2. Then, using a common extruder having a cylinder of a
suitable diameter as shown in FIG. 3, the above resin composition
is melted, for example, at a temperature of from 150 to 200.degree.
C. and extruded from a die having a suitable forward end shape to
interpose the composition between the two glass sheets, followed by
cooling to form a spacer.
[0068] This double glazing method is merely an example, and the
method for producing the insulating glass of the present invention
is not limited to such a method. For example, a spacer having a
desired shape may preliminarily be molded from the above-mentioned
resin composition, and the spacer may, for example, be heat bonded
to two glass sheets to form an insulating glass.
[0069] Suitable as the above adhesive may, for example, be an
adhesive (a) containing a combination of polyester polyol and
polyisocyanate, or a reaction product thereof, or an adhesive (b)
containing as an effective component a polymer or prepolymer
obtainable by reacting a chain extender and a terminal reactive
oligomer having butylene groups as repeating units.
[0070] Preferred as the adhesive (a) is an adhesive wherein a high
molecular weight polyester polyol having a molecular weight of at
least 10,000 prepared from at least one aliphatic dicarboxylic acid
as a starting material, is the main agent, and a polyisocyanate
containing at least two isocyanate groups per molecule, is a curing
agent.
[0071] The polyisocyanate may, for example, be a polyisocyanate
such as 2,4-tolylene diisocyanate, 2,6-tolylene diisocyanate,
phenylene diisocyanate, xylene diisocyanate, 4,4-diphenylmethane
diisocyanate, naphthylene-1,5-diisocyanate or a hydrogenated
compound thereof, ethylene diisocyanate, propylene diisocyanate,
tetramethylene diisocyanate, hexamethylene diisocyanate, isophorone
diisocyanate, 1-methyl-2,4-diisocyanate cyclohexane,
1-methyl-2,6-diisocyanate cyclohexane, dicyclohexylmethane
diisocyanate or triphenylmethane triisocyanate, as well as an
adduct compound, burette compound or isocyanate nurate compound of
the above polyisocyanate and trimethylol propane.
[0072] To facilitate the initial bond strength, the aromatic
polyisocyanate is preferred, and to improve the compatibility with
the spacer and to improve the bond strength in the present
invention, an aliphatic polyisocyanate is preferred. These
polyisocyanate compounds may be used alone or in combination as a
mixture of two or more of them. The content of the polyisocyanate
is not particularly limited, but from the viewpoint of imparting a
curing property to the composition, it is preferably contained in a
blend ratio of from 1 to 10 time in equivalent to hydroxyl groups
of the polyester polyol.
[0073] This adhesive (a) preferably contains a silane coupling
agent. In such a case, the silane coupling agent is a hydrolyzable
silyl group-containing compound having at least one member of an
epoxy group, an amino group and a mercapto group in its molecule,
such as .gamma.-glycidoxypropyltrimethoxysilane,
di(.gamma.-glycidoxypropyl)dimet- hoxysilane,
.beta.-(3,4-epoxycyclohexyl)ethyltrimethoxysilane,
.gamma.-aminopropyltriethoxysilane,
N-.beta.-aminoethyl-.gamma.-aminoprop- yldimethoxymethylsilane,
.gamma.-(N-phenylamino)propyltrimethoxysilane,
mercaptopropyltrimethoxysilane or
mercaptopropyltriethoxysilane.
[0074] The amount of such an agent is not particularly limited, but
usually, from the viewpoint of economical efficiency, the amount
may suitably be from 0.05 to 10 parts by weight, to the polyester
polyol and polyisocyanate.
[0075] In the adhesive (b), the terminal reactive oligomer
containing butylene groups as repeating units, is a compound
containing a C.sub.4 bivalent hydrocarbon as repeating units and
having a reactive functional group such as a hydroxyl group, a
carboxyl group, an amino group, a mercapto group, an epoxy group or
an isocyanate group at the oligomer terminal. It is a compound
which is capable of forming a high molecular weight polymer
functioning as an adhesive, when reacted with a chain extender
having a functional group capable of reacting with such a
functional group, for cross-linking or extension of the chain.
[0076] The butylene groups as repeating units may, for example, be
ethylethylene groups [--CH.sub.2CH(CH.sub.2CH.sub.3)--],
1,2-dimethylethylene groups [--CH(CH.sub.3)--CH(CH.sub.3)--],
1,1-dimethylethylene groups [--C(CH.sub.3).sub.2--CH.sub.2--] or
tetramethylene groups [--(CH.sub.2).sub.4--].
[0077] The above chain extender may, for example, be a
polyisocyanate containing a compound having at least three
functional isocyanate groups, as at least one component, a blend
product containing a silane coupling agent such as a compound
having at least three-functional hydrolyzable alkoxysilyl groups,
as at least one component, or a blend product containing a compound
having at least three functional double bonds and a radical
initiator reactive therewith. From the viewpoint of e.g. the
storage stability such as pot life, the above exemplified
polyisocyanate is preferred.
[0078] To such an adhesive (a) or (b), a solvent, a catalyst, a
pigment, a filler, an antioxidant, a thermal stabilizer or an
aging-preventive agent, may be further added as the case
requires.
[0079] Now, the present invention will be described in further
detail with reference to Examples and Comparative Examples.
However, the present invention is by no means restricted to such
Examples.
Examples of the Resin Composition for Building Material (1)
[0080] Firstly, Examples will be given which relates to a resin
composition for building material comprising a butyl type rubber
and a crystalline polyolefin, wherein the proportion of the butyl
type rubber is from 50 to 98 wt % and the proportion of the
crystalline polyolefin is from 2 to 50 wt %, based on the total
amount of the two, and a resin composition for building material
comprising a butyl type rubber, a crystalline polyolefin and an
inorganic filler, wherein the proportion of the butyl type rubber
is from 50 to 98 wt % and the proportion of the crystalline
polyolefin is from 2 to 50 wt %, based on the total amount of the
butyl type rubber and the crystalline polyolefin, and the
proportion of the inorganic filler is at most 200 parts by weight,
per 100 parts by weight of the sum of the butyl type rubber and the
crystalline polyolefin.
[0081] The following Composition Examples 1 to 7 represent Examples
of the present invention, and Composition Examples 8 to 12 are
Comparative Examples.
Composition Example 1
[0082] As the butyl type rubber, butyl rubber having a Mooney
viscosity of 47 ML(1+8) 100.degree. C. was used, and as the
crystalline polyolefin, a high density polyethylene (HDPE) having a
melt index of 20, a crystal fusion point of 130.degree. C. and a
crystallinity of about 80%, was used.
[0083] The butyl rubber and HDPE were melt-mixed at 160.degree. C.
at 20 rpm for 30 minutes by a laboplastomill. The hardness (HsA)
was measured in accordance with JIS K6301. The melt viscosity was
measured by a capilograph at 160.degree. C and represented by a
value at a shear rate of 91 sec.sup.1. With respect to the moisture
permeation constant, a moisture pressure of about 20 mmHg was
exerted to one side of a thin film at 60.degree. C., and the other
side was evacuated, whereby the moisture permeation constant was
obtained from the rate of moisture permeated through the thin film.
With respect to the tackiness at 160.degree. C. (high temperature
tack), a case where adequate tack was obtained, was identified by
.largecircle., a case where the tack was inadequate, was identified
by x, and a case where the tack was inbetween, was identified by
.DELTA..
[0084] Using the above materials and methods, a composition
comprising 70 wt % of the butyl rubber and 30 wt % of HDPE was
evaluated. The results are shown in Table 1. In Tables 1, 2 and 3,
the numerical values for the composition of the material are
represented by wt %, the melt viscosity is represented by a unit of
10.sup.4 poise, and the moisture permeation constant is represented
by a unit of 10.sup.--13 cm.sup.3.multidot.cm/(cm- .sup.2
sec.multidot.Pa).
Composition Example 2
[0085] Using the same materials and methods as in Composition
Example 1, evaluation was carried out in the same manner as in
Composition Example 1 with respect to a composition comprising 80
wt % of the butyl rubber and 20 wt % of the HDPE. The results are
shown in Table 1.
Composition Example 3
[0086] Using the same butyl rubber and HDPE as used in Composition
Example 1 and further using talc and HAF type carbon black as
inorganic fillers, a test was carried out in the same method as in
Composition Example 1.
[0087] Evaluation was carried out with respect to a composition
comprising 47.5 wt % of the butyl rubber, 2.5 wt % of the HDPE, 30
wt % of talc and 20 wt % of carbon black, and the results are shown
in Table 2.
Composition Example 4
[0088] Using the same materials as in Composition Example 3, a
composition comprising 45 wt % of the butyl rubber, 5 wt % of HDPE,
30 wt % of talc and 20 wt % of carbon black, was prepared and
evaluated in the same manner as in Composition Example 3, and the
results are shown in Table 2.
Composition Example 5
[0089] Using a partially cross-linked butyl rubber having a Mooney
viscosity of 45 ML(1+3) 121.degree. C. as the butyl type rubber and
using the same HDPE as in Composition Example 1, as the crystalline
polyolefin, a composition comprising 80 wt % of the partially
cross-linked butyl rubber and 20 wt % of HDPE was prepared and
evaluated in the same manner as in Composition Example 1, and the
results are shown in Table 3.
Composition Example 6
[0090] Using the same partially cross-linked butyl rubber and HDPE
as used in Composition Example 5 and a polyisobutylene having a
molecular weight of 12,000, a composition comprising 67.5 wt % of
the partially cross- linked butyl rubber, 22.5 wt % of HDPE and 10
wt % of the polyisobutylene having a viscosity average molecular
weight of 12,000 (hereinafter referred to as PIB-A), was prepared
and evaluated in the same manner as in Composition Example 1, and
the results are shown in Table 3.
Composition Example 7
[0091] A composition comprising 67.5 wt % of a polyisobutylene
having a viscosity average molecular weight of 72,000 (hereinafter
referred to as PIB-B) as the butyl type rubber, 10 wt % of PIB-A
and 22.5 wt % of the same HDPE as used in Composition Example 1,
was prepared and evaluated in the same manner as in Composition
Example 1, and the results are shown in Table 4.
Composition Example 8
[0092] The same HDPE as used in Composition Example 1 was by itself
evaluated in the same manner as in Composition Example 1, and the
results are shown in Table 1. Further, the hardness was measured by
HsD only in this Example.
Composition Example 9
[0093] Using the same materials and methods as used in Composition
Example 1, a composition comprising 40 wt % of the butyl rubber and
60 wt % of HDPE, was prepared and evaluated, and the results are
shown in Table 1.
Composition Example 10
[0094] The same butyl rubber as used in Composition Example 1 was
by itself evaluated in the same manner as in Composition Example 1,
and the results are shown in Table 1.
Composition Example 11
[0095] Using the same materials as in Composition Example 3, a
composition comprising 50 wt % of the butyl rubber, 30 wt % of talc
and 20 wt % of carbon black, was prepared and evaluated in the same
manner as in Composition Example 3, and the results are shown in
Table 2.
[0096] Using the same materials as in Composition Example 3, a
composition comprising 45 wt % of the butyl rubber, 35 wt % of talc
and 20 wt % of carbon black, was prepared and evaluated in the same
manner as in Composition Example 3, and the results are shown in
Table 2.
2 TABLE 1 Melt Moisture High Butyl Hard- visc- permeation
temperature rubber HDPE ness osity constant tack Compo- 70 30 40
1.61 35.3 .smallcircle. sition Example 1 Compo- 80 20 10 1.62 47.3
.smallcircle. sition Example 2 Compo- 0 100 (68) 0.541 7.5 x sition
Example 8 Compo- 40 60 90 0.985 16.5 x sition Example 9 Compo- 100
0 0 2.52 158 .smallcircle. sition Example 10
[0097]
3 TABLE 2 Moisture High Butyl Carbon Melt permeation temperature
rubber HDPE Talc black Hardness viscosity constant tack Composition
47.5 2.5 30 20 25 3.58 9.2 .largecircle. Example 3 Composition 45 5
30 20 45 3.16 3.8 .largecircle. Example 4 Composition 50 0 30 20 0
3.85 23.3 .largecircle. Example 11 Composition 45 0 35 20 0 4.02
21.8 .largecircle. Example 12
[0098]
4 TABLE 3 Partially Moisture High crosslinked Polyiso- Melt
permeation temperature butyl rubber HDPE butylene Hardness
viscosity constant tack Composition 80 20 -- 28 4.08 54.0
.largecircle. Example 5 Composition 67.5 22.5 10 42 2.87 43.5
.largecircle. Example 6
[0099]
5 TABLE 4 Moisture High Melt permeation temperature PIB-A PIB-B
HDPE Hardness viscosity constant tack Composition 10 67.5 22.5 55
2.65 43.5 .largecircle. Example 7
[0100] As shown in Table 1, by adding polyethylene, it was possible
to increase the hardness without impairing the moisture
permeability and tackiness which are the characteristics of the
butyl rubber. Further, as shown in Table 2, by adding an inorganic
filler, high hardness was realized simply by adding a small amount
of polyethylene. Further, as shown in Tables 3 and 4, a partially
cross-linked butyl rubber can be used instead of the butyl rubber,
and polyisobutylene may be incorporated.
Examples of the Resin Composition for Building Material (2)
Composition Example 13
[0101] With the composition shown in Table 5, components other than
the drying agent, were kneaded to obtain a resin composition having
a JIS A hardness of 65, and then the drying agent composed of 4A
type dry zeolite powder was added thereto, and the mixture was
further kneaded to uniformly disperse the drying agent to obtain a
resin composition for spacer having a JIS A hardness of 85.
Composition Examples 14 to 30
[0102] In the same manner as in Composition Example 13, with the
formulation as shown in Table 5, a resin composition for spacer
having a JIS A hardness as shown in Table 6 after mixing the
zeolite, was obtained.
Examples of the Insulating Glass
[0103] Now, Examples in which insulating glasses were prepared by
using the resin compositions for spacers of the above Composition
Examples 13 to 30 will be given. The following Examples 1 to 13 are
Examples of the present invention, and Examples 14 to 18 are
Comparative Examples.
EXAMPLE 1
[0104] Two float glass sheets having a size of 320x500 mm and a
thickness of 3 mm or 5 mm with spacer abutting portions
preliminarily treated with a primer, were held with a space of 6 mm
or 12 mm therebetween, and by means of a rubber extruder having a
cylinder with a diameter of 40 mm, the resin composition for spacer
of Composition Example 13 was extrusion molded to form a spacer
along the periphery of the glass sheets, to obtain an insulating
glass of the present invention.
EXAMPLES 2 TO 18
[0105] In the same procedure as in Example 1, using the resin
compositions for spacers of Composition Examples 14 to 30,
insulating glasses were prepared in the same manner as in Example
1.
[0106] Evaluation Methods
[0107] Sheet-shifting resistance test: A glass sheet on one side of
each insulating glass thus obtained was fixed, and a load of 13 kg
was exerted to the other glass sheet, whereby the lowering amount
of the glass sheet on the loaded side was measured at a temperature
of 25.degree. C. The one with a shifting amount being not more than
0.5 mm in 20 minutes was rated as "pass".
[0108] Accelerated durability test: In accordance with JIS R3209,
the test was carried out on the insulating glass having a spacer
with a thickness of 6 mm.
[0109] Dew point measurement: The measurement was carried out in
accordance with the method and the apparatus described in JIS
R3209. The results of the measurements are shown in Table 6.
[0110] In the Table,
[0111] Evaluation Item
[0112] A: Initial dew point (highest dew point among six
samples)
[0113] B: Dew point (.degree. C.) upon completion of class 1 of JIS
R3209 accelerated durability test
[0114] C: Dew point (.degree. C.) upon completion of class 2 of JIS
R3209 accelerated durability test
[0115] D: Dew point (.degree. C.) upon completion of class 3 of JIS
R3209 accelerated durability test
[0116] E: JIS class 3 judgement
[0117] F: Glass breakage of the insulating glass with a thickness
(5 mm/6 mm/5 mm: glass sheet/air space layer/glass sheet) during
the durability test (out of 100 samples)
[0118] G: Glass breakage of the insulating glass with a thickness
(3 mm/6 mm/3 mm: glass sheet/air space layer/glass sheet) during
the durability test (out of 100 samples)
[0119] H: Sheet shifting
[0120] Evaluation results a:
[0121] Dew point was lower than -60.degree. C.
[0122] b: Glass breakage occurred, since the spacer was hard
[0123] c: Sheet-shifting was observed with an air space layer
thickness of 12 mm, and no sheet-shifting was observed with 6
mm.
6 TABLE 5 Butyl type rubber Inorganic Partially filler Butyl
crosslinked PIB- PIB- Carbon Additives rubber butyl rubber A B HDPE
Talc black Tackifier Zeolite Composition 28.7 28.7 10.6 10.6 21.4
Example 13 Composition 35.2 5.3 11.7 10.6 10.6 5.3 21.3 Example 14
Composition 25.6 17.0 4.2 10.6 10.6 10.6 21.4 Example 15
Composition 29.8 4.3 12.8 10.6 10.6 10.6 21.4 Example 16
Composition 19.1 25.6 2.1 10.6 10.6 10.6 21.4 Example 17
Composition 17.0 25.6 4.2 10.6 10.6 10.6 21.4 Example 18
Composition 21.3 21.3 4.2 10.6 10.6 10.6 21.4 Example 19
Composition 42.6 4.2 10.6 10.6 10.6 21.4 Example 20 Composition
14.8 25.6 6.4 10.6 10.6 10.6 21.4 Example 21 Composition 15.6 15.6
15.8 10.6 10.6 10.6 21.4 Example 22 Composition 21.3 4.2 21.3 10.6
10.6 10.6 21.4 Example 23 Composition 45.9 0.9 10.6 10.6 10.6 21.4
Example 24 Composition 46.8 10.6 10.6 10.6 21.4 Example 25
Composition 11.5 46.0 10.6 10.6 21.3 Example 26 Composition 5.6
51.9 10.6 10.6 21.3 Example 27 Composition 21.3 25.6 10.6 10.6 10.6
21.4 Example 28 Composition 8.5 4.2 34.0 10.6 10.6 10.6 21.3
Example 29 Composition 12.5 15.6 18.7 10.6 10.6 10.6 21.4 Example
30
[0124]
7 TABLE 6 Spacer physical properties Evaluation items for
insulating glasses Hardness J A B C D E F G H Example 1 85 -- a a a
a Pass 0 0 Nil Example 2 80 -- a a a a Pass 0 0 Nil Example 3 65 --
a a a a Pass 0 0 Nil Example 4 75 -- a a a a Pass 0 0 Nil Example 5
40 1 .times. 10.sup.-6 a a a a Pass 0 0 Nil Example 6 60 5 .times.
10.sup.-7 a a a a Pass 0 0 Nil Example 7 65 1 .times. 10.sup.-7 a a
a a Pass 0 0 Nil Example 8 65 1 .times. 10.sup.-7 a a a a Pass 0 0
Nil Example 9 70 2 .times. 10.sup.-8 a a a a Pass 0 0 Nil Example
10 90 -- a a a a Pass 0 0 Nil Example 11 90 1 .times. 10.sup.-9 a
-55 -54 -40 Pass 0 4 Nil Example 12 20 -- a a a a Pass 0 0 c
Example 13 10 1 .times. 10.sup.-5 a a a a Pass 0 0 c Example 14 95
-- a a a Stopped b 0 4 Nil Example 15 95 -- a a a Stopped b 11 19
Nil Example 16 0 5 .times. 10.sup.-4 a a a a Pass 0 0 Observed
Example 17 95 1 .times. 10.sup.-10 -60 10 Stopped Stopped b 9 14
Nil Example 18 92 1 .times. 10.sup.-10 -60 5 Stopped Stopped b 9 11
Nil
[0125] From the results of Table 6, it is evident that by adjusting
the hardness of the spacer to a level of from 10 to 90, it is
possible to reduce glass breakage of the insulating glass and at
the same time it is possible to prevent the sheet-shifting or the
like. In such a case, it is possible to obtain an insulating glass
having the shape of the insulating glass maintained without
increase of the dew point with a spacer made solely of the above
resin composition.
[0126] On the other hand, with insulating glasses of Examples 10
and 11, certain glass breakage is observed in a case where glass
sheets having a thickness of 3 mm was used, although no glass
breakage is observed in a case where glass sheets having a
thickness of 6 mm were used. Further, with the insulating glasses
of Examples 12 and 13, sheet-shifting is sometimes observed in a
case where the thickness of the air space layer was 12 mm, although
no sheet-shifting is observed in the case where the thickness of
the air space layer was 6 mm.
[0127] From this, it is evident that as the hardness of the resin
composition for spacer, HsA of from 40 to 75 is particularly
preferred. Further, it is evident that as the value for the creep
compliance J of the resin composition for spacer, from
1.times.10.sup.-10 to 1.times.10.sup.-5 is preferred, and from
1.times.10.sup.-9 to 1.times.10.sup.-6 is particularly
preferred.
[0128] In the resin composition for spacer used for the insulating
glass of Example 10, the proportion of the butyl type rubber was
98.08 wt % and the proportion of the crystalline polyolefin was
1.92 wt %, based on the total amount of the butyl type rubber and
the crystalline polyolefin. On the other hand, with the insulating
glass of Example 10, certain sheet-shifting may sometimes result
depending upon the thickness of the air space layer. This indicates
that the proportion of the butyl type rubber being from 50 to 98 wt
% and the proportion of the crystalline polyolefin being from 2 to
50 wt %, based on the total amount of the butyl type rubber and the
crystalline polyolefin, substantially includes the blend
proportions of the above Composition Example 22, but the blend
proportions as in Composition Examples 13 to 21 and 23 are
preferred.
[0129] The resin composition for spacer used for the insulating
glass of Example 18 is included in the compositional range of the
resin composition for building material of the present invention.
From this, it is evident that the resin composition in Example 18
(Composition Example 30) is the one which is not suitable for use
as a spacer, among resin composition for building material of the
present invention.
[0130] The resin composition for building material in the present
invention is useful not only for the above-mentioned spacer but
also for a sealing material for building material. Thus, the resin
composition of
[0131] Composition Example 30 is suitable as a low moisture
permeable sealing material to seal the exterior wall material which
is not as brittle as a glass sheet.
Industrial Applicability
[0132] According to the present invention, an operation for filling
a secondary sealing material can be reduced, no curing time is
required, the number of process steps for preparing an insulating
glass can be substantially reduced, and the insulating glass can be
presented at high productivity and low costs.
* * * * *