JPH0657229A - Mixing of adhesive components under agitation - Google Patents

Abstract

PURPOSE:To mix at least two components with each other under agitation within a short time to such a degree of uniformity as not to cause unwetting by mechanically agitating the components under applied ultrasonic waves. CONSTITUTION:At least two components are mixed with each other by mechanical agitation under application of ultrasonic waves. The application of ultrasonic waves is performed in such a way that the above components are fed to an agitation mixer and ultrasonic waves are applied continuously in the period during which they are mechanically agitated or that ultrasonic waves are applied for a definite time in the final stage in which they have been thoroughly agitated and mixed. The mechanical agitation and mixing performs macroscopic agitation and mixing, and the fine vibrations and activation effected by the ultrasonic waves performs microscopic diffusion and mixing. This process is suited to mix lowly compatible components with each other. When it is adopted to agitate and mix an amide resin or a thermoplastic polyamide precursor with an epoxy resin, an adhesive having a uniform composition can be produced within a short time.

Description

Detailed Description of the Invention

[0001]

BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to a method for stirring and mixing an adhesive, and more particularly to a method for stirring and mixing an adhesive comprising a composition obtained by stirring and mixing two or more components.

[0002]

2. Description of the Related Art In the process of assembling semiconductor devices,
TA used in TAB (Tape Automated Bonding) method, which has a three-layer structure of a protective layer, an adhesive layer, and an insulating film.
Tapes for B have come to be widely used. TAB
To mount semiconductor integrated circuit devices such as LSIs on tapes for tape, punching such as slits and holes, removing the protective layer, adhering the copper foil to the adhesive layer, forming wiring patterns, etc. It is made through the process. In order to meet today's demands for high-density packaging, higher quality TAB tapes are required. One of the requirements for improving the quality of the TAB tape is application of an adhesive.

In manufacturing a TAB tape, in order to transfer an adhesive layer having a constant thickness to a base film, first, a transfer film is coated and dried. A polyimide film, which is excellent in properties such as heat resistance and other mechanical properties, is usually used as the base film, and an amide-based adhesive film suitable for bonding the polyimide film and the copper foil as an adhesive. An adhesive agent in which a resin and an epoxy resin are mixed is used.

[0004]

However, polyethylene terephthalate (PET), which is a film for transferring an adhesive obtained by mixing the amide resin and the epoxy resin, is used as a transfer film.
When applied to a film, the film of the adhesive was locally broken and the surface of the PET film was exposed, which may cause so-called cissing. The size of this cissing is large and small, and if a TAB tape (flexible carrier tape) is manufactured from a PET film that has cissing, the TAB
Defective products occur during tape manufacturing.

Therefore, it is possible to improve the affinity with the PET film to which the adhesive is applied, but such treatment may transfer the adhesive layer on the PET film to a base film such as a polyimide film. become unable. Therefore, the inventors of the present invention have conducted extensive studies to apply an adhesive to a PET film so as not to cause cissing. As a result, when epoxy resin is applied alone, cissing occurs, but amide resin is applied alone. However, it was found that cissing did not occur. From these results, after stirring and mixing the amide resin and the epoxy resin for a long time, the adhesive was aged (aged) for a longer time, and the adhesive was treated with PE.
When it was applied to the T film, cissing did not occur. However, stirring and mixing for a long period of time and aging for a longer period of time are not suitable for industrial production, and further increase the production cost.

[0006]

Therefore, in view of such circumstances, the inventors of the present invention have conducted research to obtain a method capable of uniformly stirring and mixing in a short time without causing cissing, and as a result,
This led to the present invention.

The gist of the method for stirring and mixing an adhesive according to the present invention is that the method for stirring and mixing an adhesive comprising a composition obtained by stirring and mixing two or more components is Ultrasonic waves are applied to the mixture while mechanically stirring the components to mix them.

Further, in the method of stirring and mixing an adhesive according to the present invention, the two or more components are an amide resin and an epoxy resin.

Further, in the method of stirring and mixing an adhesive according to the present invention, the two or more components are a thermoplastic polyimide precursor and an epoxy resin.

Further, in the method of stirring and mixing the adhesive according to the present invention, the oscillation frequency of ultrasonic waves is 30 to 60 KH.
z, and more preferably 40 to 50 KHz.

[0011]

The agitation and mixing of the adhesive according to the present invention is carried out by applying ultrasonic waves while mechanically agitating the two or more components when agitating and mixing two or more components. As for the timing, ultrasonic waves may be continuously applied during the period of mechanical stirring after adding two or more components to the stirring / mixing tank, or the final step of mechanically stirring and sufficiently stirring and mixing. Alternatively, ultrasonic waves may be applied for a certain period of time.
Two or more kinds of components are mixed by mechanical stirring and macroscopic stirring and mixing, and then microscopic diffusion and mixing are performed by micro vibration and activation by ultrasonic waves to obtain an adhesive with a uniform composition. To be Further, two or more kinds of components may be components having excellent compatibility with each other, but the present invention is particularly suitable for mixing components having poor compatibility.

In particular, when an amide resin and an epoxy resin are agitated and mixed as two or more kinds of components, or when a thermoplastic polyimide precursor and an epoxy resin are agitated and mixed, an adhesive having a uniform composition is used. Can be manufactured in time. When the adhesive obtained by stirring and mixing with ultrasonic waves in addition to this mechanical stirring is applied to, for example, a PET film, the thin film of the applied adhesive layer is broken and peeled off, and the underlying PET film is removed. There is no so-called repelling that is exposed.

[0013]

EXAMPLES Next, examples of the stirring and mixing method of the adhesive according to the present invention will be described. Here, the outline of the process of mounting the circuit element on the flexible printed wiring board manufactured using the TAB tape will be described.

First, an adhesive is applied to a PET film and dried, then the adhesive layer formed on the PET film is transferred to a polyimide film, and then the polyimide film and copper foil are transferred via the transferred adhesive layer. And heat bond. Next, a flexible printed wiring board is manufactured by performing mechanical processing or etching, and the circuit element is soldered to the obtained flexible printed wiring board.
For this reason, such an adhesive is a material that can firmly bond the polyimide film and the copper foil, and needs to be thermoplastic so as to be heat-bonded, while it needs heat resistance to withstand soldering. Since such properties are required, the adhesive for producing the TAB tape is an adhesive composed of a composition in which an amide resin and an epoxy resin are mixed, or a thermoplastic polyimide precursor and an epoxy. An adhesive that is composed of a composition in which a resin is mixed is used.

For example, in stirring and mixing the amide-based resin and the epoxy-based resin, first, the amide-based resin and the epoxy-based resin are placed in a known stirring tank and mechanically stirred and mixed. This mechanical stirring and mixing may be carried out, for example, in an amide resin production reaction tank or may be carried out in another stirring and mixing tank. Also, the stirring mechanism, such as rotating the stirring bar, rotating the screw or ribbon,
There is no limitation. Furthermore, conditions such as stirring speed, stirring time, stirring temperature and the like are selected according to the characteristics of the resin to be stirred and mixed, that is, the viscosity and compatibility.

An ultrasonic wave oscillator is attached to the mechanical stirring and mixing tank, and the frequency of the ultrasonic wave oscillator is 30 to 60 KHz, more preferably 40 to 50 KHz.
Ultrasonic waves are applied to the mixture that is mechanically stirred and mixed in the stirring and mixing tank. The ultrasonic wave may be applied continuously or intermittently during the mechanical stirring, but the ultrasonic wave is applied for 1 minute to several tens of minutes, and even about several minutes is sufficient. Is obtained.

As the amide-based resin used in the present invention, a known polyamide resin can be used, but a polyamide resin having an epoxy group at the terminal can be preferably used. Known thermoplastic polyimides can also be used, and the precursor before conversion into polyimide is used in the stirring and mixing method of the present invention, and the precursor is converted into polyimide after mixing with the epoxy resin.

Here, as a specific example of the adhesive composed of an amide-based resin and an epoxy-based resin to which the method of stirring and mixing the adhesive of the present invention is applied, the following general formula 1

[Chemical 1] (In the formula, R ₁ , R ₂ and R ₃ are divalent organic groups, and m and n are 1
Examples of the adhesive agent include an epoxy-terminated polyamide resin having a structure represented by an integer of 30), an epoxy resin, and an epoxy resin curing agent.

Such an epoxy-terminated polyamide resin is obtained by reacting a carboxylic acid-terminated polyamide with an epoxy resin in an amount approximately equivalent to that of the carboxylic acid, and the polyamide uses dicarboxylic acid as a monomer. Adipic acid, sebacic acid, dodecanoic acid, etc. may be used alone or in combination of two or more.

On the other hand, as the epoxy resin, an epoxy resin having the same or different structure as that used for reacting the epoxy-terminated polyamide resin is used. As the epoxy resin, bisphenol A type epoxy resin, cresol novolac type epoxy resin, phenol novolac type epoxy resin, glycidyl ether type epoxy resin, naphthalene type epoxy resin and the like are used. However, a bifunctional epoxy resin having two epoxy groups in the molecule is preferable as the epoxy resin to be reacted with the polyamide. Further, these epoxy resins are used alone or as a mixture of two or more kinds.

Further, the adhesive composed of an epoxy-terminated polyamide resin, an epoxy resin, and an epoxy resin curing agent is, in addition to these three components, for example, a resin component such as an acrylic resin, a phenol resin, an imide resin, a rubber resin, or an epoxy resin. A curing accelerator for the resin, a curing catalyst, various inorganic / organic fillers, etc. may be mixed. Further, the solvent used is required to dissolve both the epoxy resin and the polyamide resin, for example, methyl ethyl ketone, toluene, chlorobenzene, trichloroethylene, methylene chloride, methyl cellosolve, ethyl cellosolve, dimethylformamide, dimethylacetamide, methanol, ethanol, isopropyl. Alcohol or the like is used.

Although the amide-based resin and the epoxy-based resin to which the stirring and mixing method of the adhesive of the present invention is applied have been described above, various kinds of thermoplastic polyimides and their precursors may also be used. That is, the present invention is naturally not limited to these adhesives, and can be applied to stirring and mixing of two or more kinds of components.

Next, the present invention will be described more specifically by way of examples, but the present invention is not limited to these examples, and the present invention is within the scope of the present invention. The present invention can be implemented with various modifications, improvements and changes based on the knowledge of those skilled in the art.

Example 1 An epoxy-terminated polyamide was prepared by using a carboxylic acid-terminated polyamide synthesized from isophorone diisocyanate and dimer acid as an amide resin and an epoxy resin "Epicoat 1001" (trade name, manufactured by Yuka Shell Epoxy Co., Ltd.). Synthesized. 40 parts by weight of this epoxy-terminated polyamide, 60 parts by weight of epoxy resin "Epicoat 1001", 5 parts by weight of dicyandiamide, 80 parts by weight of toluene, and 80 parts by weight of isopropyl alcohol were mixed. First, a screw was used to mechanically stir at a stirring temperature of 0 ° C. for 20 minutes, and then ultrasonic waves having an oscillation frequency of 50 KHz were applied for 5 minutes to perform mechanical stirring and ultrasonic stirring.

The obtained adhesive was applied onto a PET film evenly so as to have a thickness of 20 μm after drying. With respect to the PET film coated with the adhesive, the number of craters generated per 100 cm ² was investigated. As a result, the number of cissing was 0.

Example 2 As in Example 1, the stirring temperature was raised to 20 ° C. for 20 minutes,
After mechanically stirring and mixing, ultrasonic stirring was performed. As a result, when the number of repellents was examined in the same manner as in Example 1, the number of repellents was 0.

Example 3 As in Example 1, the stirring temperature was set to 20 ° C., the mixture was mechanically stirred and mixed for 2 hours, and then ultrasonically stirred. As a result, when the number of repellents was examined in the same manner as in Example 1, the number of repellents was 0.

Comparative Example 1 Mechanical stirring and mixing were carried out under the same conditions as in Example 1, but ultrasonic stirring was not performed. As a result, when the number of repellents was examined in the same manner as in Example 1, the number of repellents was eight.

When the adhesive obtained was aged for 3 days and then applied in the same manner and the number of cissing was examined in the same manner as in Example 1, the number of cissing was two. Next, the same adhesive was aged for 7 days and then applied in the same manner, and the number of cissing was examined in the same manner as in Example 1. As a result, the number of cissing was 0.

Comparative Example 2 Mechanical stirring and mixing were carried out under the same conditions as in Example 2, but ultrasonic stirring was not performed. As a result, when the number of cissings was examined in the same manner as in Example 1, the number of cissings was 5. The adhesive obtained was aged for 3 days and then applied in the same manner, and the number of cissing was examined in the same manner as in Example 1. As a result, the number of cissing was 0.

Comparative Example 3 Mechanical stirring and mixing were carried out under the same conditions as in Example 3, but ultrasonic stirring was not performed. As a result, when the number of repellents was examined in the same manner as in Example 1, the number of repellents was three. The adhesive obtained was aged for 3 days and then applied in the same manner, and the number of cissing was examined in the same manner as in Example 1. As a result, the number of cissing was 0.

[0032]

The method of stirring and mixing the adhesive according to the present invention is 2
More than one component, especially amide-based resin and epoxy-based resin, or in the stirring and mixing of the precursor of the thermoplastic polyimide and the epoxy-based resin, in addition to mechanical stirring, ultrasonic waves are applied to the mixture, Since the components are agitated and mixed by slight vibration of ultrasonic waves, even components having poor compatibility with each other can be uniformly mixed. As a result, so-called cissing does not occur even when the obtained adhesive is applied thinly on a PET film or the like, and an excellent TAB tape with stable quality can be manufactured.

Claims (4)

[Claims] 1. A method for stirring and mixing an adhesive, which comprises a composition obtained by stirring and mixing two or more components, wherein
A method of stirring and mixing an adhesive, characterized in that ultrasonic waves are applied to the mixture while mechanically stirring the one or more components, and the mixture is mixed. 2. The method of stirring and mixing an adhesive according to claim 1, wherein the two or more components are an amide resin and an epoxy resin. 3. The method of stirring and mixing an adhesive according to claim 1, wherein the two or more components are a thermoplastic polyimide precursor and an epoxy resin. 4. The oscillation frequency of the ultrasonic wave is 30 to 60K.
The stirring and mixing method for an adhesive according to any one of claims 1 to 3, wherein the method is Hz.