JPH09278987A - Epoxy resin composition - Google Patents

Epoxy resin composition

Info

Publication number
JPH09278987A
JPH09278987A JP8855396A JP8855396A JPH09278987A JP H09278987 A JPH09278987 A JP H09278987A JP 8855396 A JP8855396 A JP 8855396A JP 8855396 A JP8855396 A JP 8855396A JP H09278987 A JPH09278987 A JP H09278987A
Authority
JP
Japan
Prior art keywords
epoxy resin
resin composition
polymer
thermal shock
functional group
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Pending
Application number
JP8855396A
Other languages
Japanese (ja)
Inventor
Tatsumi Kawaguchi
竜巳 河口
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Sumitomo Durez Co Ltd
Original Assignee
Sumitomo Durez Co Ltd
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Sumitomo Durez Co Ltd filed Critical Sumitomo Durez Co Ltd
Priority to JP8855396A priority Critical patent/JPH09278987A/en
Publication of JPH09278987A publication Critical patent/JPH09278987A/en
Pending legal-status Critical Current

Links

Landscapes

  • Compositions Of Macromolecular Compounds (AREA)
  • Paints Or Removers (AREA)

Abstract

PROBLEM TO BE SOLVED: To obtain an epoxy resin composition capable of giving a covering excellent in thermal shock resistance and moisture resistance, and useful for a powder coating material, etc., as an insulating covering material for an electric.electronic part material by using the composition containing a specific thermal shock resistance improver. SOLUTION: This epoxy resin composition contains (A) an epoxy resin, (B) a hardener such as an acid anhydride, a polyamine or a novolak-type phenolic resin, (C) a filler such as an inorganic filler having <=20μm average particle diameter and (D) an acrylic resin as a polymer of an acrylate monomer and having a functional group such as an epoxy, a carboxyl or OH as a thermal shock resistance improver. Preferably, the composition contains 1-20wt.% of the component D based on whole of the composition.

Description

【発明の詳細な説明】Detailed Description of the Invention

【0001】[0001]

【発明の属する技術分野】本発明は、熱衝撃性と耐湿性
に優れ、電気・電子部品の絶縁被覆に好適に用いられる
エポキシ樹脂組成物に関するものである。
BACKGROUND OF THE INVENTION 1. Field of the Invention The present invention relates to an epoxy resin composition which is excellent in thermal shock resistance and moisture resistance and is suitable for insulating coating of electric / electronic parts.

【0002】[0002]

【従来の技術】従来、エポキシ樹脂は優れた反応性、作
業性そしてその硬化物特性から電気・電子、塗料、接着
剤等の幅広い分野で使用されている。普通エポキシ樹脂
は加熱状態で硬化した後、冷却して最終用途に供され
る。電気・電子部品の絶縁被覆に使用される場合、エポ
キシ樹脂の線膨張係数と被覆される素子のそれとの差に
より内部応力が生じ、熱衝撃が加わった場合に剥離や破
壊が起じやすい。
2. Description of the Related Art Epoxy resins have hitherto been used in a wide variety of fields such as electric / electronics, paints and adhesives because of their excellent reactivity, workability and cured product characteristics. Usually, epoxy resin is cured in a heated state and then cooled to be used for an end use. When used as an insulating coating for electric / electronic components, internal stress is generated due to the difference between the linear expansion coefficient of the epoxy resin and that of the element to be coated, and peeling or breakage easily occurs when a thermal shock is applied.

【0003】内部応力を低減する方法として一般に、最
適な樹脂や硬化剤の選択による方法、CTBN等を改質
剤として添加する方法などがある。しかし、前者ではフ
レキシブルな化学構造を導入することによるガラス転移
温度(Tg)の低下、後者では流れ性や硬化性の低下、
また樹脂と改質剤の相溶性の点から密着性が不十分で、
それによる耐湿性の低下などの問題点がある。また、ス
チレン系熱可塑性エラストマーを添加することにより熱
衝撃性を改善する方法(特開平6−93171号公報)
も知られているが、近年、より高い熱衝撃性を要求され
ることが多く、このような分野においては依然として不
十分である。
As a method of reducing the internal stress, generally, there is a method of selecting an optimum resin or curing agent, a method of adding CTBN or the like as a modifier. However, the former lowers the glass transition temperature (Tg) by introducing a flexible chemical structure, and the latter lowers the flowability and curability.
In addition, the adhesion is insufficient from the viewpoint of compatibility between the resin and the modifier,
There is a problem such as a decrease in moisture resistance. Further, a method for improving thermal shock resistance by adding a styrene-based thermoplastic elastomer (Japanese Patent Laid-Open No. 6-93171).
However, in recent years, higher thermal shock resistance is often required, and it is still insufficient in such a field.

【0004】[0004]

【本発明が解決しようとする課題】本発明は、電気的特
性及び他の特性を低下させる事なく耐熱衝撃性の優れる
粉体塗料に好適な材料を研究した結果、アクリル酸エス
テルモノマーの重合体であり、重合体中に官能基を有す
るアクリル樹脂を含有することにより、被覆した電気・
電子部品の特性として熱衝撃性と耐湿性に優れる硬化物
を与えるエポキシ樹脂組成物を提供することにある。
DISCLOSURE OF INVENTION Problems to be Solved by the Invention In the present invention, as a result of research on a material suitable for a powder coating having an excellent thermal shock resistance without deteriorating the electrical characteristics and other characteristics, a polymer of an acrylic acid ester monomer is obtained. In addition, by including an acrylic resin having a functional group in the polymer,
An object of the present invention is to provide an epoxy resin composition which gives a cured product having excellent thermal shock resistance and moisture resistance as characteristics of electronic parts.

【0005】[0005]

【課題を解決するための手段】本発明は、エポキシ樹
脂、硬化剤、充填剤を必須成分するエポキシ樹脂組成物
において、アクリル酸エステルモノマーの重合体であ
り、重合体中に官能基を有するアクリル樹脂を熱衝撃性
改良材として含有することを特徴とするエポキシ樹脂組
成物である。
The present invention relates to an epoxy resin composition comprising an epoxy resin, a curing agent and a filler as essential components, which is a polymer of acrylic acid ester monomer and has a functional group in the polymer. An epoxy resin composition comprising a resin as a thermal shock improver.

【0006】本発明において熱衝撃性改良材として使用
するアクリル樹脂は、その分子中にエポキシ基、カルボ
キシル基、ヒドロキシル基等の官能基を有しており、エ
ポキシ樹脂と相溶性が高く、分散性が良いために剪断強
度および剥離強度に優れると考えられる。また、高い伸
びが得られるために、低弾性率化となり、応力を緩和す
る。その結果、熱衝撃により生ずる内部応力に対し、強
度が上回っているために剥離や破壊が起らず、更に水も
侵入しにくいために耐湿性が向上すると考えられる。
The acrylic resin used as the thermal shock improver in the present invention has a functional group such as an epoxy group, a carboxyl group and a hydroxyl group in its molecule, has a high compatibility with the epoxy resin, and has a high dispersibility. It is considered that it is excellent in shear strength and peeling strength due to its good hardness. Further, since a high elongation is obtained, the elastic modulus is lowered and the stress is relaxed. As a result, it is considered that since the strength is higher than the internal stress generated by the thermal shock, peeling or breakage does not occur, and water does not easily enter, so that the moisture resistance is improved.

【0007】アクリル酸エステルモノマーの重合体であ
り、官能基を有するアクリル樹脂としては、呉羽化学工
業社製パラロイドEXL−2314、パラロイドEXL
−3386等が挙げられる。かかるアクリル樹脂の配合
量はエポキシ樹脂100重量部に対して1〜20重量部
が好ましい。この配合量が1重量部未満の場合は熱衝撃
性に対する効果が小さくなり、20重量部をこえると高
粘度となり、流れ性が低下するようになる。
Acrylic resins having a functional group, which are polymers of acrylic acid ester monomers, include Paraloid EXL-2314 and Paraloid EXL manufactured by Kureha Chemical Industry Co., Ltd.
-3386 etc. are mentioned. The amount of the acrylic resin compounded is preferably 1 to 20 parts by weight with respect to 100 parts by weight of the epoxy resin. If the blending amount is less than 1 part by weight, the effect on the thermal shock resistance becomes small, and if it exceeds 20 parts by weight, the viscosity becomes high and the flowability deteriorates.

【0008】本発明で原料として使用されるエポキシ樹
脂としては、例えばビスフェノールA型エポキシ樹脂、
ビスフェノールF型エポキシ樹脂などのジグリシジルエ
ーテル型エポキシ樹脂、フェノールノボラック型エポキ
シ樹脂、クレゾールノボラック型エポキシ樹脂などのノ
ボラック型エポキシ樹脂、グリシジルエステル型エポキ
シ樹脂、グリシジルアミン型エポキシ樹脂、線状脂肪族
型エポキシ樹脂、被素環型エポキシ樹脂、ハロゲン化エ
ポキシ樹脂などがあげられるが、これらに限定されるも
のではない。
Examples of the epoxy resin used as a raw material in the present invention include bisphenol A type epoxy resin,
Diglycidyl ether type epoxy resin such as bisphenol F type epoxy resin, novolac type epoxy resin such as phenol novolac type epoxy resin, cresol novolac type epoxy resin, glycidyl ester type epoxy resin, glycidyl amine type epoxy resin, linear aliphatic type epoxy resin Examples of the resin include, but are not limited to, a resin, an epoxy resin to be encapsulated, and a halogenated epoxy resin.

【0009】本発明に使用される硬化剤および硬化促進
剤としては、酸無水物、ポリアミン、ノボラック型フェ
ノール樹脂、第3級アミン、イミダゾール化合物等の1
種以上を選んで使用する。更に、必要に応じて充填材が
使用される。充填剤は、通常平均粒径が20μm以下の
無機充填材が使用され、例えばジルコン粉末、タルク粉
末、結晶シリカ粉末、熔融シリカ粉末、炭酸カルシウム
粉末、マグネシア粉末、ケイ酸カルシウム粉末、水和ア
ルミナ粉末、アルミナ粉末などが挙げられる。本発明に
おいては必要に応じ顔料、カップリング剤、レベリング
剤などの添加剤を配合する事が出来る。
The curing agent and curing accelerator used in the present invention include acid anhydrides, polyamines, novolac type phenolic resins, tertiary amines, imidazole compounds and the like.
Select and use more than one seed. Further, a filler is used if necessary. As the filler, an inorganic filler having an average particle size of 20 μm or less is usually used. For example, zircon powder, talc powder, crystalline silica powder, fused silica powder, calcium carbonate powder, magnesia powder, calcium silicate powder, hydrated alumina powder. , Alumina powder and the like. In the present invention, additives such as pigments, coupling agents, leveling agents and the like can be added if necessary.

【0010】本発明のエポキシ樹脂組成物は注型材料等
の液状、粉体塗料等の粉状、成形材料等の顆粒状、塊状
など何れの状態でもよいが、代表的な用途としては粉体
塗料が挙げられる。
The epoxy resin composition of the present invention may be in a liquid state such as a casting material, a powder state such as a powder coating material, a granular state such as a molding material or a lump state, but a typical use is a powder state. Examples include paints.

【0011】本発明のエポキシ樹脂組成物を製造する方
法として、例えば粉体塗料の場合をあげると、所定の割
合で秤量した原料成分をミキサーによって充分混合した
後、エクストルーダー、コニーダーあるいはロール等で
溶融混合し、次いで粉砕機にて粉砕する方法がある。上
記方法によって得られる粉体塗料により電気・電子部品
の絶縁被覆を行う方法としては、流動浸漬法、静電流動
浸漬法、ころがし法、ふりかけ法、ホットスプレー法、
静電スプレー法等、一般の粉体塗装方法が用いられる。
As a method for producing the epoxy resin composition of the present invention, for example, in the case of powder coating, the raw material components weighed in a predetermined ratio are thoroughly mixed with a mixer, and then the mixture is extruded, cokneadered or rolled. There is a method of melt-mixing and then pulverizing with a pulverizer. As a method for performing insulation coating of electric / electronic parts with the powder coating obtained by the above method, a fluidized dipping method, an electrostatic fluidized dipping method, a rolling method, a sprinkling method, a hot spray method,
A general powder coating method such as an electrostatic spray method is used.

【0012】また、注型材料、成形材料の場合について
も公知の技術で製造でき、絶縁材料として使用できる。
Also, in the case of casting materials and molding materials, they can be manufactured by known techniques and can be used as insulating materials.

【0013】[0013]

【実施例】次に本発明を実施例により更に詳しく説明す
る。
Next, the present invention will be described in more detail with reference to examples.

【0014】実施例1 ビスフェノールA型エポキシ樹脂(エポキシ当量950) 50重量部 アクリル酸エステルモノマーの重合体であり、 重合体中に官能基を有するアクリル樹脂(EXL−2314) 5 熔融シリカ粉末(平均粒径15μm) 50 トリメリット酸無水物 4 トリフェニルフォスフィン 0.1 上記組成物を配合し、ヘンシェルミキサーで混合し、コ
ニーダーにて溶融混練した後、粉砕機で粉砕する事によ
り平均粒径40〜60μmのエポキシ樹脂組成物からな
る粉体塗料を得た。
Example 1 Bisphenol A type epoxy resin (epoxy equivalent 950) 50 parts by weight Polymer of acrylic acid ester monomer, acrylic resin having functional group in polymer (EXL-2314) 5 fused silica powder (average) Particle size 15 μm) 50 Trimellitic anhydride 4 Triphenylphosphine 0.1 The above composition is blended, mixed with a Henschel mixer, melt-kneaded with a cokneader, and then ground with a grinder to give an average particle size of 40. A powder coating consisting of an epoxy resin composition of -60 μm was obtained.

【0015】実施例2 ビスフェノールA型エポキシ樹脂(エポキシ当量950) 50重量部 アクリル酸エステルモノマーの重合体であり、重合体中に官能基を有するアク リル樹脂(EXL−2314) 20 熔融シリカ粉末(平均粒径15μm) 50 トリメリット酸無水物 4 トリフェニルフォスフィン 0.1 上記組成物を配合し、ヘンシェルミキサーで混合し、コ
ニーダーにて溶融混練した後、粉砕機で粉砕する事によ
り平均粒径40〜60μmのエポキシ樹脂組成物からな
る粉体塗料を得た。
Example 2 Bisphenol A type epoxy resin (epoxy equivalent 950) 50 parts by weight Acrylic resin (EXL-2314), which is a polymer of acrylic acid ester monomer and has a functional group in the polymer, 20 fused silica powder ( Average particle size 15 μm) 50 trimellitic anhydride 4 triphenylphosphine 0.1 The above composition is blended, mixed with a Henschel mixer, melt-kneaded with a cokneader, and then crushed with a crusher to obtain an average particle size. A powder coating material having an epoxy resin composition of 40 to 60 μm was obtained.

【0016】比較例1 実施例1において、アクリル酸エステルモノマーと官能
基を有するアクリル樹脂を配合せず、他は同様の方法に
て平均粒径40〜60μmのエポキシ樹脂組成物からな
る粉体塗料を得た。
Comparative Example 1 A powder coating composition made of an epoxy resin composition having an average particle size of 40 to 60 μm in the same manner as in Example 1 except that the acrylic ester monomer and the acrylic resin having a functional group were not blended. Got

【0017】比較例2 実施例1において、アクリル酸エステルモノマーと官能
基を有するアクリル樹脂の代わりにスチレン系熱可塑性
エラストマー(旭化成社製 タフテックH−1031)
を配合し、他は同様の方法にて平均粒径40〜60μm
のエポキシ樹脂組成物からなる粉体塗料を得た。
Comparative Example 2 In Example 1, a styrene thermoplastic elastomer (Tuftec H-1031 manufactured by Asahi Kasei Co., Ltd.) was used instead of the acrylic ester monomer and the acrylic resin having a functional group.
In the same manner as above, but with an average particle size of 40 to 60 μm.
A powder coating material comprising the above epoxy resin composition was obtained.

【0018】比較例2 実施例2において、アクリル酸エステルモノマーと官能
基を有するアクリル樹脂を40重量部配合し、他は同様
の方法にて平均粒径40〜60μmのエポキシ樹脂組成
物からなる粉体塗料を得た。
Comparative Example 2 A powder made of an epoxy resin composition having an average particle size of 40 to 60 μm was prepared in the same manner as in Example 2, except that 40 parts by weight of an acrylic acid ester monomer and an acrylic resin having a functional group were mixed. Got body paint.

【0019】実施例1、2及び比較例1〜3の樹脂組成
物について粉体特性及び150℃で1時間硬化させ、得
られた硬化物の特性、部品特性について表1に示す。
Table 1 shows the powder properties of the resin compositions of Examples 1 and 2 and Comparative Examples 1 to 3 and the properties and parts properties of the cured products obtained by curing at 150 ° C. for 1 hour.

【表1】 [Table 1]

【0020】(測定方法) 1.流れ率:所定温度の乾燥機中に10φ×7mmの試
験片(粉体塗料のタブレット)を30分間放置した時の
直径増加率である。流れ率は次式により計算される。 流れ率(%)=[{処理後の直径の平均(mm)−10(mm)}/
10(mm)]×100 2.ゲル化時間:一定量の粉体塗料を所定温度の熱板上
にのせ、所定のヘラで練り合わせゲル化(糸が引かなく
なる状態)に要する時間である。 3.煮沸吸水率:粉体塗料硬化物の試験片(50×50
×2mm)を沸騰水中に2時間浸漬した後の増加した質
量と浸漬前の試験片の質量の百分率である。 煮沸吸水率(%)={(W2−W1)/W1}× 100 W1:煮沸前の試験片質量 W2:煮沸後の試験片質量 4.耐湿性:電子部品(バリスタ)に粉体塗料を塗装
し、150℃、1時間の硬化条件で硬化させた後、プレ
ッシャークッカー試験機に放置し一定時間毎に定電流を
流した時の電圧を測定し、その変化率によって評価す
る。表中における数値は電圧変化率が5%以上となる処
理時間である。 5.熱衝撃性:電子部品(バリスタ)に粉体塗料を塗装
し、150℃、1時間の硬化条件で硬化させた後、所定
の条件に設定したヒートサイクル試験機に放置し、塗装
物のクラックの入り具合を見るものである。表中におけ
る数値は塗装物にクラックが生じたサイクル数である。
(Measurement method) 1. Flow rate: The rate of increase in diameter when a test piece of 10φ × 7 mm (tablet of powder coating) was left for 30 minutes in a dryer at a predetermined temperature. The flow rate is calculated by the following formula. Flow rate (%) = [{average diameter after treatment (mm) -10 (mm)} /
10 (mm)] × 100 2. Gelation time: This is the time required for putting a certain amount of powder coating material on a hot plate having a predetermined temperature and kneading with a predetermined spatula for gelation (state in which the yarn is not pulled). 3. Boiled water absorption: Test piece of cured powder coating (50 x 50
X 2 mm) is the percentage of the increased mass after immersion in boiling water for 2 hours and the mass of the test piece before immersion. Boiled water absorption rate (%) = {(W2-W1) / W1} × 100 W1: mass of test piece before boiling W2: mass of test piece after boiling 4. Moisture resistance: Powder coating is applied to electronic parts (varistor), cured at 150 ° C for 1 hour, then left in a pressure cooker tester and the voltage when a constant current is applied at regular intervals is set. It measures and evaluates by the change rate. The numerical value in the table is the processing time at which the voltage change rate is 5% or more. 5. Thermal shock resistance: Powder coating is applied to electronic parts (varistor), cured at 150 ° C for 1 hour, and then left in a heat cycle tester set to predetermined conditions to prevent cracking of the coated object. It is to see how well it enters. The numerical value in the table is the number of cycles in which the coated article cracked.

【0021】[0021]

【発明の効果】本発明のアクリル酸エステルモノマーの
重合体であり、官能基を有するアクリル樹脂を配合した
エポキシ樹脂組成物を絶縁被覆材として用いた場合、電
気的特性及び他の特性を低下させる事なく、熱衝撃性と
耐湿性に優れる被覆を与える事が出来る。
EFFECT OF THE INVENTION When an epoxy resin composition which is a polymer of an acrylic acid ester monomer of the present invention and contains an acrylic resin having a functional group is used as an insulating coating material, electrical properties and other properties are deteriorated. It is possible to give a coating with excellent thermal shock resistance and moisture resistance without any problem.

Claims (4)

【特許請求の範囲】[Claims] 【請求項1】 エポキシ樹脂、硬化剤、充填剤を必須成
分とするエポキシ樹脂組成物において、アクリル酸エス
テルモノマーの重合体であり、重合体中に官能基を有す
るアクリル樹脂を熱衝撃性改良材として含有することを
特徴とするエポキシ樹脂組成物。
1. An epoxy resin composition comprising an epoxy resin, a curing agent and a filler as essential components, wherein an acrylic resin which is a polymer of an acrylic acid ester monomer and has a functional group in the polymer is used as a heat shock improver. An epoxy resin composition comprising:
【請求項2】 アクリル酸エステルモノマーの重合体で
あり、重合体中に官能基を有するアクリル樹脂における
官能基としては、エポキシ基、カルボキシル基またはヒ
ドロキシル基である請求項1記載のエポキシ樹脂組成
物。
2. The epoxy resin composition according to claim 1, which is a polymer of an acrylic acid ester monomer, and the functional group in the acrylic resin having a functional group in the polymer is an epoxy group, a carboxyl group or a hydroxyl group. .
【請求項3】 アクリル酸エステルモノマーの重合体で
あり、重合体中に官能基を有するアクリル樹脂を組成物
全体に対して1〜20重量部含有する事を特徴とする請
求項1又は2記載のエポキシ樹脂組成物。
3. A polymer of an acrylic acid ester monomer, wherein 1 to 20 parts by weight of an acrylic resin having a functional group in the polymer is contained in the entire composition. Epoxy resin composition.
【請求項4】 請求項1、2又は3記載のエポキシ樹脂
組成物からなる粉体塗料。
4. A powder coating comprising the epoxy resin composition according to claim 1.
JP8855396A 1996-04-10 1996-04-10 Epoxy resin composition Pending JPH09278987A (en)

Priority Applications (1)

Application Number Priority Date Filing Date Title
JP8855396A JPH09278987A (en) 1996-04-10 1996-04-10 Epoxy resin composition

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
JP8855396A JPH09278987A (en) 1996-04-10 1996-04-10 Epoxy resin composition

Publications (1)

Publication Number Publication Date
JPH09278987A true JPH09278987A (en) 1997-10-28

Family

ID=13946064

Family Applications (1)

Application Number Title Priority Date Filing Date
JP8855396A Pending JPH09278987A (en) 1996-04-10 1996-04-10 Epoxy resin composition

Country Status (1)

Country Link
JP (1) JPH09278987A (en)

Similar Documents

Publication Publication Date Title
JPS61268750A (en) Epoxy resin composition for semiconductor sealing use
JP3484546B2 (en) Powder coating composition
KR20100130966A (en) Epoxy resin composition for semiconductor encapsulation and semiconductor device using the same
JPH0511125B2 (en)
CA1141058A (en) Epoxy resin moulding composition
JPH09278986A (en) Epoxy resin composition
JPH09278987A (en) Epoxy resin composition
JPH09278988A (en) Epoxy resin composition
JP2008056838A (en) Epoxy resin powder coating
JPH0711105A (en) Epoxy resin composition with excellent thermal impact property
JP2000072986A (en) Epoxy resin powder coating material
JPH0693171A (en) Epoxy resin composition of excellent thermal shock resistance
JP4517182B2 (en) Epoxy resin composition for casting
JP2000072985A (en) Epoxy resin powder coating
JP2000007889A (en) Epoxy resin composition
JP2785553B2 (en) Tab-type semiconductor device sealing material and tab-type semiconductor device
JPS6225118A (en) Sealing resin composition
JPS62112622A (en) Sealing resin composition
KR100554031B1 (en) Thermosetting Epoxy Powder Coating Composition_
JPH09272787A (en) Liquid epoxy resin composition
JPH05156126A (en) Epoxy resin composition and its cured article
JPH02311520A (en) Epoxy resin composition
JPH01144441A (en) Sealing resin composition
JPS63225618A (en) Sealing resin composition and its production
JPS6245615A (en) Epoxy resin composition for sealing semiconductor device

Legal Events

Date Code Title Description
A977 Report on retrieval

Free format text: JAPANESE INTERMEDIATE CODE: A971007

Effective date: 20040820

A131 Notification of reasons for refusal

Free format text: JAPANESE INTERMEDIATE CODE: A131

Effective date: 20040827

A02 Decision of refusal

Free format text: JAPANESE INTERMEDIATE CODE: A02

Effective date: 20041228