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JPS511039

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DESCRIPTION JPS511039
■ Manufacturing method of piezoelectric polymer composite ■ Japanese Patent Application No.
4.5-60640 [Phase] Application No. 45 (1970) July 13 @ inventor Kitayama Toyoki Musashino
City Midoricho 3 9 11 Nippon Telegraph and Telephone Corporation Electric Corporation The
present invention relates to a method of manufacturing a flexible polymer piezoelectric
composite film or sheet according to the present invention. is there. (It is characterized in that a
polymer material (herein, fine particles of fine particles are compounded to form a film or a
sheet, and then it is stretched and then a direct current voltage is applied to form a piezoelectric
body). It is The present inventor first manufactures a piezoelectric polymer composite
characterized in that a polymer material (this piezoelectric fine particle is complexed, and then a
direct current voltage is applied at an appropriate temperature to perform polarization operation.
Invented the method. (Japanese Patent Application No. 45-16246) According to the abovementioned method of the present invention, a piezoelectric substance of only polymers, for
example, a piezoelectric substance larger than that of a polypeptide, vinylidene fluoride and the
like can be obtained In practice, it is desirable that the piezoelectric properties be as large as
possible, provided that there is no significant difference in other physical properties.
Furthermore, it is desirable that the mechanical strength of the film or sheet of the piezoelectric
polymer composite be as strong as possible. In the above invention, in order to increase the
piezoelectricity of the piezoelectric polymer composite, the content of the piezoelectric inorganic
material must be increased, and as the content is increased, the mechanical strength tends to
decrease. is there. In the present invention, a polymer / piezoelectric fine particle core [111111]
compound is stretched for the purpose of obtaining a polymer composite having larger
piezoelectricity than the above-mentioned invention (Japanese Patent Application No. 45-16246),
and then It is characterized in that the polarization operation is performed to obtain large
piezoelectricity. By putting this stretching process in the middle. Also, a film having high
mechanical tensile strength in the stretching direction can be obtained. Following the above
invention (Japanese Patent Application No. 45-16246), the object is to increase the piezoelectric
coefficient of the piezoelectric polymer composite (As a result of various investigations, adding a
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stretching operation in film or sheet production further increases the size) It has been found that
a piezoelectric polymer composite having piezoelectricity can be produced. There are the
following methods for combining the polymer material with the piezoelectric fine particles. (2) In
the case of a thermoplastic polymer, it is formed into a film or sheet after mixing using a roll
plastograph or the like at a temperature higher than the softening point.
(1) In the case of a powdered polymer, it is mixed with piezoelectric fine particles as it is and is
formed into a film or sheet by a heating press. (2) Dissolve the polymer material in a suitable
solvent, and then mix the piezoelectric fine particles with a ball mill etc. (After thoroughly mixing,
use a solvent casting method to form a sheet or film. It is possible to mix 10 to 90% by weight of
piezoelectric fine particles with respect to the polymer material in the proportion of the polymer
material and the piezoelectric fine particles. However, it is better to use conditions including
mechanical strength, the magnitude of piezoelectric voltage, and the quality of stretching (more
preferably, 30 to 80% by weight of piezoelectric fine particles). As the piezoelectric fine particles,
a ferroelectric piezoelectric material is preferable, and in addition to the peropskite type
ferroelectric, Rochelle salt, antimony sulfur iodide, etc. may be used. The size of the piezoelectric
particles may be 100 mesh or more, and fine particles of 350 mesh or more are also effective. It
was confirmed that the stretching method was effective by any of the following methods. ■ Roll
stretching at room temperature. If it is difficult to stretch, it may be better to heat it a little and
make the rail [111111] EndPage: 1. ■ Mechanical tension (stretching by this. In this method,
stretching is often performed effectively by raising the temperature a little. {Circle over (2)} The
film formed by the solvent casting method is stretched in the same manner as in the above {circle
over (1)} or {circle over (3)} in a state where the solvent is not completely removed. In this
method, it is often very easy to stretch by selecting an appropriate solvent. After stretching in
this manner, appropriate electrodes are attached to both sides of the film, and a DC voltage is
applied to perform polarization operation. Also in this case, it is more effective to set the
temperature to about 80.degree. Further, the higher the direct current applied voltage, the better.
When the voltage is applied close to dielectric breakdown, the piezoelectric voltage becomes
larger. Moreover, in order to increase the stretchability and the mechanical strength of the
product, a plasticizer can be added as necessary, but if it does not lower the insulation resistance
so much, it does not greatly affect the piezoelectric voltage. Examples of the present invention
will be shown below. EXAMPLE 1 100 g of barium titanate powder (particle size: 325 mesh or
less) and polyvinylidene fluoride 101 are mixed by a heating roll at 200 ° C., and molded into a
sheet 1 having a thickness of 200 μ by pressing at the same temperature. 旅 こ の シ ー ト 室温
室温 115 115 115 115 115 115 115 115 115 115 115 115 115 延伸 延伸 延伸 延伸 延伸 シ ー
ト 延伸 シ ー ト 延伸 シ ー ト 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸
延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸 延伸. From this, a
sample with a width of 5 lines and a length of 40 mm is cut out and double-sided (this carbon
paste is used as a coloring electrode).
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The copper ribbon is taken out as a lead from these two sides. Then, the piezoelectric coefficients
of the samples prepared by applying a direct current voltage (100 KV / c In>) at 120 ° C. for 15
hours are as shown in the following table. Draw ratio 11.523 Piezoelectric coefficient (X109
cgsesu) 40180400500 Example 2 10 g of titanium zirconate in 100 g of a tetrahydrofuran
solution containing 10% of a vinyl chloride polymer is mixed in an agate planetary motion ball
mill for 4 hours, and glass is prepared Pour onto a plate and evaporate the solvent at 50'C. Next,
the solvent was sufficiently removed in a stretched state in a film stretcher in a state in which the
solvent is still present, and the polarization operation was performed on the thus-prepared
sample in the same manner as in Example 1 and the results are shown in the following Table. It
is. DC applied voltage 60 KV / crIL temperature 110 ° C., 15 hours stretch ratio 12
piezoelectricity (X109 cgsesu) 10100 Example 3 20 ° polypropylene 20 g and barium titanate
fine particles 3011 are mixed using a plastograph at 200 ° C., the same temperature Then, the
film is formed by a heat press (this is molded and stretched at 80 ° C. and stretched by a
stretcher. The measurement results of a sample subjected to processing under the conditions of
direct current voltage 40 KV / (m, 120 ° C., 15 hours) in the same manner as Example 1 are as
shown in the following Table. Stretching Ratio 11.73 Piezoelectric Coefficient (XIOcgsesu) 2820
As an application of the piezoelectric polymer composite of the present invention, it can be used
as a flexible film. In that case, the piezoelectric coefficient becomes high, which is more effective
as an electric / force conversion element in the voice band. The frequency characteristic is
uniform without the influence of resonance or the like because the elastic modulus is small.
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