KR20200007211A - Thermosetting silicone_based resin composition for adhesive film and adhesive film manufactured by using the same - Google Patents

Abstract

The present invention relates to a thermosetting silicone resin composition for an adhesive film, which comprises: 1) a silicone-based resin represented by chemical formula 1, (R^1_3SiO_1/2)_a(SiO_4/2)_b(HO_1/2)_c(R^2_2HSiO_1/2)_d(R^3_2R^4SiO_1/2)_e; 2) at least one rubber component including linear silicone rubber represented by chemical formula 2, (R^5_2R^6SiO_1/2(R^7_2SiO_2/2)_f(R^8R^9SiO_2/2)_g(R^10_2R^11SiO_1/2); 3) organohydrogenpolysiloxane cross-linking agent; 4) hydrosilylation catalyst; and 5) silicone oil including a hydrophilic group, and to an adhesive film formed using the same.

Description

Thermosetting silicone-based resin composition for an adhesive film and an adhesive film formed using the same {THERMOSETTING SILICONE_BASED RESIN COMPOSITION FOR ADHESIVE FILM AND ADHESIVE FILM MANUFACTURED BY USING THE SAME}

The present invention relates to a thermosetting silicone resin composition for an adhesive film and an adhesive film formed using the same.

In recent years, flat panel type image display apparatuses, such as a liquid crystal, a plasma, and organic EL, attract attention. In a flat panel image display device, a matrix of a plurality of pixels each composed of a semiconductor layer, a phosphor layer, or a light emitting layer constituting an active element is usually arranged between a pair of substrates having at least one light transmittance such as glass. It has a display area (image display part) arrange | positioned at the type | mold. Generally, the said display area | region (image display part) and the circumference | surroundings of the protection part formed from optical plastics, such as glass and an acrylic resin, are hermetically sealed with the adhesive agent.

In such an image display apparatus, in order to prevent the fall of visibility (visibility) by reflection of outdoor light, an indoor light, etc., the thin image display apparatus which interposed the resin composition between the protection part and the image display part is manufactured, As the curable resin composition used, thermosetting or ultraviolet curing resins are used.

In addition, the touch method has become one of the important input methods in the modern society, and thus the touch screen panel (TSP) is gradually expanding its area. With the advent of the iPhone with capacitive touch in 2007, the growth of smart phones and tablet PCs has led to a rapid increase in demand, and notebooks and all-in-one PCs (all-in-one). TSP is increasingly used as an input device for various devices needed in schools, offices, and homes, as well as general appliances, white appliances such as TVs, refrigerators, washing machines, and automobiles, as well as existing electronic devices. It is expected to increase. There are many types of TSPs depending on the driving method, but nowadays, most of the most demanding personal electronic devices adopt the capacitive method. Therefore, the research and development of optical adhesive materials with the necessary properties for manufacturing the capacitive TSP are actively conducted. It is becoming.

The TSP has a structure in which a transparent electrode and a display module are positioned under the cover window, which initially used an air gap between the cover window and the electrode. Full lamination (or direct bonding) filled with adhesive materials is a general trend. Optical adhesive materials used to bond each layer in the full lamination structure can be roughly divided into optically clear adhesive (OCA) of a transparent double-sided tape type and optically clear resin (OCR, LOCA) of a transparent liquid type. have. Here, the term optically clear means that the transmittance of the material itself is 90% or more, and refers to a very transparent state.

Polymers used as adhesive materials for optics include acrylic, silicone, and urethane, but they have excellent transparency, are easy to design, and can be quickly cured through UV (ultraviolet). In terms of phosphorus, acrylic polymers that have advantages are most used. Silicone-based polymers have excellent heat resistance, and urethane-based materials have their advantages because they can control their physical properties by combining soft and hard segments.

Optical adhesive materials not only adhere each component layer to each other but also have advantages in terms of image quality improvement. In the structure with the air gap, the light from the backlight unit is reflected by the refractive index difference between the air layer and the film layer, causing some loss, which results in a blurry image as a whole, leading to deterioration of image quality.

However, when the air gap is filled with the optical adhesive material, the difference in refractive index between the film layer and the adhesive material is reduced, and the light loss from the backlight unit is also reduced, thereby enabling clear and bright image expression, thereby improving visibility. In addition, there is an advantage in vibration resistance and impact resistance due to the filling (gap filling) of the adhesive material.

In addition, in the case of the optical adhesive material to be applied to the next-generation flexible TSP based on the plastic substrate, in addition to the condition that the modulus of the adhesive should be kept low and uniform in order to withstand the stress caused by the deformation of the substrate, Excellent operation reactivity of the pressure-sensitive adhesive film is essential.

For this reason, the optical adhesive material market is gradually increasing, and further research and development on the optical adhesive material is needed.

US Patent No. 6,949,294 Japanese Patent Publication No. 2008-282000

The present invention is to provide a thermosetting silicone-based resin composition for an adhesive film excellent in durability and light transparency, and an adhesive film formed using the same.

One embodiment of the present invention,

1) a silicone-based resin represented by Formula 1;

2) at least one rubber component including a linear silicone rubber represented by Formula 2 below;

3) organohydrogenpolysiloxane crosslinkers;

4) hydrosilylation catalysts; And

5) Silicone fluids including hydrophilic groups

It provides a thermosetting silicone resin composition for an adhesive film comprising a.

[Formula 1]

(R ¹ ₃ SiO _1/2 ) _a (SiO _4/2 ) _b (HO _1/2 ) _c (R ² ₂ HSiO _1/2 ) _d (R ³ ₂ R ⁴ SiO _1/2 ) _e

[Formula 2]

(R ⁵ ₂ R ⁶ SiO _1/2 ) (R ⁷ ₂ SiO _2/2 ) _f (R ⁸ R ⁹ SiO _2/2 ) _g (R ¹⁰ ₂ R ¹¹ SiO _1/2 )

In Chemical Formulas 1 and 2,

R ¹ , R ² , R ³ , R ⁵ , R ⁷ , R ⁸ and R ¹⁰ are the same as or different from each other, and each independently, a substituted or unsubstituted hydrocarbon group,

R ⁴ , R ⁶ , R ⁹ and R ¹¹ are each independently an alkenyl group,

a, b, c, d, e, f and g are weight ratios,

a / b is 0.5 to 1.5, (a + b) is 1, c is 0.01 to 0.05, d / (c + d) and e / (c + e) are each 0 to 0.99,

g / (f + g) is 0-0.1.

Moreover, another embodiment of this invention provides the adhesive film formed using the said thermosetting silicone type resin composition for adhesive films.

Thermosetting silicone resin composition for pressure-sensitive adhesive film according to an embodiment of the present invention, by including the silicone resin represented by the formula (1) is not only excellent in durability but also excellent in light transparency. In addition, the thermosetting silicone-based resin composition for pressure-sensitive adhesive film according to an embodiment of the present invention, by maintaining a low modulus and glass transition temperature to improve the flexibility (flexibility) of the electronic device at low temperatures, minimize the stress during deformation and the touch sensor High sensitivity can be achieved. Accordingly, the pressure-sensitive adhesive film formed by using the thermosetting silicone resin composition for pressure-sensitive adhesive film according to the present invention may be more preferably applied to electronic devices such as a flexible display.

In addition, the thermosetting silicone-based resin composition for an adhesive film according to an exemplary embodiment of the present invention includes the silicone oil containing the hydrophilic group, thereby minimizing outgassing during film formation, and thus high temperature and high humidity conditions of the adhesive film. Can improve the reliability. In addition, it is possible to prevent the lowering of visibility of the optical display and the lowering of sensitivity of the TSP.

1 is a photograph showing an outgas evaluation result of Example 1 as an exemplary embodiment of the present invention.
2 is a photograph showing an outgas evaluation result of Example 2 as an exemplary embodiment of the present invention.
3 is a photograph showing an outgas evaluation result of Example 3 as an exemplary embodiment of the present invention.
Figure 4 is a prior art, a photograph showing the outgas evaluation results of Comparative Example 2.
Figure 5 is a prior art, a photograph showing the outgas evaluation results of Comparative Example 3.
Figure 6 is a prior art, a photograph showing the outgas evaluation results of Comparative Example 4.
Figure 7 is a prior art, a photograph showing the outgas evaluation results of Comparative Example 5.
8 is a prior art, a photograph showing the outgas evaluation results of Comparative Example 1.

Hereinafter, the present application will be described in detail.

The present invention is to provide a thermosetting silicone resin composition for pressure-sensitive adhesive film and a pressure-sensitive adhesive film formed using the same, which has the advantage that shrinkage during curing is suppressed, does not discolor under long-term aging conditions, and the elastic modulus fluctuation range is small due to temperature change.

Thermosetting silicone resin composition for pressure-sensitive adhesive film according to an embodiment of the present invention, 1) the silicone resin represented by the formula (1); 2) at least one rubber component including a linear silicone rubber represented by Formula 2; 3) organohydrogenpolysiloxane crosslinkers; 4) hydrosilylation catalysts; And 5) silicone oils comprising hydrophilic groups.

In general, a resin having two oxygen atoms bonded to one silicon atom in a silicone resin is called a D-type silicone resin, and a resin having three oxygen atoms bonded to one silicon atom in a silicone resin is T. The resin having one oxygen atom bonded to one silicon atom in the silicone resin is called a -type silicone resin, and the resin having an oxygen atom bonded to one silicon atom in the silicone resin is 4 Personal resin is called Q-type silicone resin.

However, the thermosetting silicone resin composition for pressure-sensitive adhesive film according to the present invention is applied by applying a silicone resin represented by the formula (1), and at least one rubber component including a linear silicone rubber represented by the formula (2), durability Not only is it excellent, it is excellent in light transparency, and it can maintain a low modulus and a touch sensor sensitivity, and can apply it to electronic elements, such as a flexible display, more preferably.

In one embodiment of the present invention, based on the total weight of the rubber component and the organohydrogenpolysiloxane crosslinking agent, the total weight of the silicone resin may be greater than 0 to 0.9 times or less. When the total weight of the silicone resin exceeds 0.9 times, the modulus and glass transition temperature of the pressure-sensitive adhesive film are formed too high, which may significantly reduce the flexibility of the flexible TSP at low temperatures.

In one embodiment of the present invention, R ¹ , R ² , R ³ , R ⁵ , R ⁷ , R ⁸ and R ¹⁰ of Formulas 1 and 2 are each independently an alkyl group; Or an aryl group.

The alkyl group may be linear, branched, or cyclic, and the number of carbon atoms is not particularly limited, but is preferably 1 to 30. Specific examples include methyl group, ethyl group, propyl group, n-propyl group, isopropyl group, butyl group, n-butyl group, isobutyl group, tert-butyl group, sec-butyl group, 1-methyl-butyl group, 1- Ethyl-butyl group, pentyl group, n-pentyl group, cyclopentyl group, isopentyl group, neopentyl group, tert-pentyl group, hexyl group, n-hexyl group, cyclohexyl group, 1-methylpentyl group, 2- Methylpentyl group, 4-methyl-2-pentyl group, 3,3-dimethylbutyl group, 2-ethylbutyl group, heptyl group, n-heptyl group, 1-methylhexyl group, cyclopentylmethyl group, cyclohexylmethyl group, jade Methyl, n-octyl, tert-octyl, 1-methylheptyl, 2-ethylhexyl, 2-propylpentyl, n-nonyl, 2,2-dimethylheptyl, 1-ethyl-propyl, 1,1-dimethyl-propyl group, isohexyl group, 2-methylpentyl group, 4-methylhexyl group, 5-methylhexyl group, etc. are mentioned, but it is not limited to these.

The aryl group may be monocyclic or polycyclic, and the carbon number is not particularly limited, but is preferably 6 to 30 carbon atoms. Specific examples may include a phenyl group, biphenyl group, terphenyl group, naphthyl group, triphenylenyl group, anthracenyl group, phenanthryl group, pyrenyl group, perylenyl group, chrysenyl group, fluorenyl group, and the like. It doesn't happen.

In an exemplary embodiment of the present invention, specific examples of the linear silicone rubber may include a compound having the following structural formula, but are not limited thereto.

M ^Vi D ₄₂₀ M ^Vi

M ^Vi D ₈₀₀ M ^Vi

M ^Vi D ₁₁₀₀ M ^Vi

M ^Vi D ₁₄₀₀ M ^Vi

M ^Vi D ^Vi ₄ D ₅₀₀₀ M ^Vi

M ^Vi D ^Vi ₁₀ D ₅₀₀₀ M ^Vi

M ^Vi D ^Vi ₇ D ₃₂₀₀ M ^Vi

M ^Vi D ^Vi ₂ D ₄₂₀₀ D ^Ph2 ₂₅₀ M ^Vi

In the above formula, M ^Vi is R ₃ and SiO _1/2 unit, D is R _'2 and SiO _2/2 unit, D ^Vi is R ₂ and SiO _2/2 unit, D ^Ph2 is R _"2 SiO _2/2 Unit,

Each R is independently a vinyl group,

Each R ′ is independently a substituted or unsubstituted hydrocarbon group,

R "is a phenyl group.

In one embodiment of the present invention, the crosslinking agent is an organohydrogenpolysiloxane containing a hydrogen atom bonded to at least two silicon atoms in one molecule, the content of the crosslinking agent is an alkenyl group bonded to a silicon atom of the linear silicone rubber The number of hydrogen atoms bonded to the silicon atoms of the organohydrogenpolysiloxane crosslinking agent per one may be from 0.01 to 10.

Examples of the crosslinking agent include MD _a D ^H _b M, MD ^H _c M, M ^H _d Q _f , and the like. In this case, M is' and ₃ SiO _1/2 unit, D is R 'R ₂ SiO _2/2 units, and, D is ^H R'HSiO _2/2 units and, M ^H is HR' ₂ SiO _1/2 units and, Q is SiO _4/2 units and, (a + b) is from 10 to 100, and, c, d, and f are each independently from 1 to 100. In addition, said R 'is a substituted or unsubstituted hydrocarbon group each independently.

Specific examples of the crosslinking agent include compounds having the following structural formulas, but are not limited thereto.

MD ₁₇ D ^H ₄ M

MD ₂₀ D ^H ₁₀ M

MD ₂₃ D ^H ₃₃ M

MD ₁₅ D ^H ₃₀ M

MD ^H ₄₅ M

M ^H ₂ Q

M ^H ₄ Q

M ^H ₉ Q

In one embodiment of the present invention, the hydrosilylation catalyst is a catalyst for promoting a hydrosilylation reaction. More specifically, the hydrosilylation catalyst may use ruthenium, rhodium, palladium, osmium, iridium, and platinum, and complexes of these metals. However, the present invention is not limited thereto. Preferably, the hydrosilylation catalyst used in the present invention is a platinum-containing catalyst. Suitable platinum-containing hydrosilylation catalysts include finely divided metal platinum, platinum on finely ground carriers such as alumina, platinum compounds such as chloropltinic acid, Karstedt platinum catalysts and complexes of platinum compounds, and the like. to be.

The content of the hydrosilylation catalyst may be 1 ppm to 50 ppm based on the total weight of the thermosetting silicone resin composition.

It is often found that a large amount of bubbles due to outgases are formed when silicone or acrylic OCA is bonded between substrates of plastic material and exposed to conditions of high temperature and high humidity. This is known to occur when the moisture contained in the OCA is vaporized with the temperature rises and separated from the OCA, so that it is trapped between low-permeability plastic substrates and does not escape quickly. Therefore, as in the exemplary embodiment of the present application, when a small amount of silicone oil having compatibility with silicone OCA and a hydrophilic group is added to the OCA, excess water is absorbed to significantly reduce or prevent bubble formation by outgas. can do. One example is a nonionic silicone surfactant.

In one embodiment of the present invention, the content of the silicone oil including the hydrophilic group may be 0.01 to 10% by weight, based on the total weight of the thermosetting silicone-based resin composition, may be 0.1 to 1% by weight. . When the content of the silicone oil containing the hydrophilic group is less than 0.01% by weight based on the total weight of the thermosetting silicone-based resin composition, it is difficult to expect the effect of preventing outgas, and when it exceeds 10% by weight, the mechanical properties of the OCA itself This can lead to a number of negative issues such as degradation and flexibility at low temperatures and poor optical reliability at high temperature and high humidity conditions.

In an exemplary embodiment of the present invention, the silicone oil including the hydrophilic group may include a nonionic silicone-based surfactant, and more specifically, homo or co-polymerized polyalkylene oxide modified polyorganosiloxane ( It may include polyalkyleneoxide (homo- or copolymer) modified polyorganosiloxane.

In one embodiment of the present invention, the rubber component may further include an α-olefin. The α-olefin may include ethene, propene, 1-butene, isobutene, 1-octene, 1-decene, 1-tetradecene, 1-octadecene, and the like, but is not limited thereto.

The content of the α-olefin may be 0 to 20% by weight based on the total weight of the thermosetting silicone resin composition for the adhesive film.

In addition, the thermosetting silicone resin composition for an adhesive film according to an exemplary embodiment of the present invention may include one or more additives such as a reaction inhibitor, a stress regulator, a viscosity regulator, a curing agent, a dispersant, a stabilizer, and a radical stabilizer, depending on the use thereof. have. These additives can be used individually or in mixture of 2 or more types.

Moreover, the adhesive film which concerns on one Embodiment of this invention is formed using the said thermosetting silicone type resin composition, It is characterized by the above-mentioned. Since the thermosetting silicone resin composition according to the present invention has excellent adhesiveness and flexibility, high initial transmittance and high heat / light transparency, the thermosetting silicone resin composition may be particularly suitably used for optical-related components and display-related components. By using the low modulus and glass transition temperature of the adhesive film, it is possible to reduce the stress during deformation of the electronic device at low temperatures, and to implement the appropriate sensitivity of the flexible touch panel sensor.

More specifically, it can be used for bonding to various small, medium and large flat panel displays such as liquid crystal panels, and is particularly suitable as a bonding material in the manufacture of large displays.

The adhesive film may be manufactured using a method known in the art, except for using the thermosetting silicone resin composition for an adhesive film according to the present invention.

Hereinafter, the present specification will be described in more detail with reference to Examples. However, the following examples are merely to illustrate the present specification, but not to limit the present specification.

< Example >

< Production Example  1> Preparation of Silicone Resin A

9,016 g of MQ resin (2.7% OH, M / Q = 0.7, toluene solution of 60% solids) was added to a reactor equipped with a Dean-Stark separator, heated at 110 ° C. for 2 hours, and refluxed to remove 12 ml of water. After cooling the reactor containing the resin to 45 ° C., 121.6 g of 1,1,3,3-tetramethyldisilazane (1,1,3,3-tetramethyldisilazane) was added to 4.5 g of dimethyldi (isopropylamino) silane. (dimethyldi (isopropylamino) silane) was added together with reflux and heated at 111 ° C. for 2 hours to remove 0.7 ml of water. The final product was a clear pale yellow solution.

Coating samples were prepared based on 60% solids as described in Table 1 below.

< Example  1>

A silicone resin (60% toluene solution) 36.68g, 1- tetradecene 2.64g, first linear silicone rubber AM ^Vi D ₃₂₀₀ D ^Vi M ^Vi ₇ 31.65g of using a SpeedMixer Flacktek ^TM 40 seconds at 800rpm, at 1,850rpm 40 seconds, 40 seconds at 2,350 rpm. Thereafter, 0.51 g of a crosslinking agent MD ₁₅ D ^H ₃₀ M, 0.84 g of a silicone surfactant, and 27.57 g of toluene were added and mixed in the same manner to prepare 100 g of a 60% solids solution. The resin / rubber ratio was 0.90 and the H (crosslinking agent) / Vi ratio was 5.0. Transfer 40 g of this to a 2 oz container, add 0.05 g of 1-ethynyl-1-cyclohexane (ECH), stir for 1 minute with a wooden stick, add 0.24 g of 5,000 ppm platinum Karstedt catalyst, and stir for 1 minute to give a homogeneous solution. made. A small amount of silicone solution was applied onto the Housewell FL132 fluorine release film and the coating was formed using a film applicator and then dried for 30 minutes in a well ventilated hood. Thereafter, the resultant was transferred to an oven and cured at 135 ° C. for 5 minutes to finally produce a film having a thickness of 100 μm. The remaining examples were prepared in the same manner except for the surfactant. Thereafter, the film was cut to a size of 52 mm x 76 mm to remove the fluorine release film, and then bonded using a rubber roller between PET films of the same size. The sample was left to stand in a constant temperature and humidity chamber at 85 ° C./85% for 24 hours to investigate whether or not bubbles were generated by outgassing by visual inspection.

TABLE 1

< Experimental Example >

The properties of the prepared film were evaluated and shown in Table 2 below.

TABLE 2

As described above, the thermosetting silicone resin composition for pressure-sensitive adhesive film according to an exemplary embodiment of the present invention is not only excellent in durability but also excellent in light transparency by including the silicone resin represented by the formula (1). In addition, the thermosetting silicone-based resin composition for pressure-sensitive adhesive film according to an embodiment of the present invention, by maintaining a low modulus and glass transition temperature to improve the flexibility (flexibility) of the electronic device at low temperatures, minimize the stress during deformation and the touch sensor High sensitivity can be achieved. Accordingly, the pressure-sensitive adhesive film formed by using the thermosetting silicone resin composition for pressure-sensitive adhesive film according to the present invention may be more preferably applied to electronic devices such as a flexible display.

In addition, the thermosetting silicone-based resin composition for an adhesive film according to an exemplary embodiment of the present invention includes the silicone oil containing the hydrophilic group, thereby minimizing outgassing during film formation, and thus high temperature and high humidity conditions of the adhesive film. Can increase the reliability.

Claims (7)

1) a silicone-based resin represented by Formula 1;
2) at least one rubber component including a linear silicone rubber represented by Formula 2 below;
3) organohydrogenpolysiloxane crosslinkers;
4) hydrosilylation catalysts; And
5) Silicone fluids including hydrophilic groups
A thermosetting silicone resin composition for an adhesive film comprising:
[Formula 1]
(R ¹ ₃ SiO _1/2 ) _a (SiO _4/2 ) _b (HO _1/2 ) _c (R ² ₂ HSiO _1/2 ) _d (R ³ ₂ R ⁴ SiO _1/2 ) _e
[Formula 2]
(R ⁵ ₂ R ⁶ SiO _1/2 ) (R ⁷ ₂ SiO _2/2 ) _f (R ⁸ R ⁹ SiO _2/2 ) _g (R ¹⁰ ₂ R ¹¹ SiO _1/2 )
In Chemical Formulas 1 and 2,
R ¹ , R ² , R ³ , R ⁵ , R ⁷ , R ⁸ and R ¹⁰ are the same as or different from each other, and are each independently a substituted or unsubstituted hydrocarbon group,
R ⁴ , R ⁶ , R ⁹ and R ¹¹ are each independently an alkenyl group,
a, b, c, d, e, f and g are weight ratios,
a / b is 0.5 to 1.5, (a + b) is 1, c is 0.01 to 0.05, d / (c + d) and e / (c + e) are each 0 to 0.99,
g / (f + g) is 0-0.1. The method according to claim 1, wherein R ¹ , R ² , R ³ , R ⁵ , R ⁷ , R ⁸ and R ¹⁰ are each independently an alkyl group; Or an aryl group thermosetting silicone resin composition for pressure-sensitive adhesive film. The method of claim 1, wherein the linear silicone rubber is thermosetting silicone resin composition for pressure-sensitive adhesive film is selected from compounds of the following structural formula:
M ^Vi D ₄₂₀ M ^Vi
M ^Vi D ₈₀₀ M ^Vi
M ^Vi D ₁₁₀₀ M ^Vi
M ^Vi D ₁₄₀₀ M ^Vi
M ^Vi D ^Vi ₄ D ₅₀₀₀ M ^Vi
M ^Vi D ^Vi ₁₀ D ₅₀₀₀ M ^Vi
M ^Vi D ^Vi ₇ D ₃₂₀₀ M ^Vi
M ^Vi D ^Vi ₂ D ₄₂₀₀ D ^Ph2 ₂₅₀ M ^Vi
In the above formula, M ^Vi is R ₃ and SiO _1/2 unit, D is R _'2 and SiO _2/2 unit, D ^Vi is R ₂ and SiO _2/2 unit, D ^Ph2 is R _"2 SiO _2/2 Unit,
Each R is independently a vinyl group,
R 'is each independently a substituted or unsubstituted hydrocarbon group,
R "is a phenyl group. The thermosetting silicone resin composition for an adhesive film according to claim 1, wherein the content of the hydrosilylation catalyst is 1 ppm to 50 ppm based on the total weight of the thermosetting silicone resin composition for the adhesive film. The thermosetting silicone resin composition according to claim 1, wherein the rubber component further comprises an α-olefin. The thermosetting silicone resin composition for an adhesive film according to claim 1, wherein the silicone oil containing a hydrophilic group comprises a polyalkylene oxide modified polyorganosiloxane. The adhesive film formed using the thermosetting silicone type resin composition for adhesive films of any one of Claims 1-6.

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