JPH0612152B2 - 合成樹脂から共押出し法により製造される自動車配管 - Google Patents
合成樹脂から共押出し法により製造される自動車配管Info
- Publication number
- JPH0612152B2 JPH0612152B2 JP2311667A JP31166790A JPH0612152B2 JP H0612152 B2 JPH0612152 B2 JP H0612152B2 JP 2311667 A JP2311667 A JP 2311667A JP 31166790 A JP31166790 A JP 31166790A JP H0612152 B2 JPH0612152 B2 JP H0612152B2
- Authority
- JP
- Japan
- Prior art keywords
- layer
- polyamide
- thickness
- synthetic resin
- outer layer
- 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.)
- Expired - Lifetime
Links
- 229920003002 synthetic resin Polymers 0.000 title claims description 10
- 239000000057 synthetic resin Substances 0.000 title claims description 10
- 238000001125 extrusion Methods 0.000 title 1
- 229920002292 Nylon 6 Polymers 0.000 claims abstract description 10
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 claims abstract description 8
- 239000005977 Ethylene Substances 0.000 claims abstract description 8
- -1 polyethylene Polymers 0.000 claims abstract description 8
- 229920001577 copolymer Polymers 0.000 claims abstract description 7
- IMROMDMJAWUWLK-UHFFFAOYSA-N Ethenol Chemical compound OC=C IMROMDMJAWUWLK-UHFFFAOYSA-N 0.000 claims abstract description 4
- 239000004698 Polyethylene Substances 0.000 claims abstract description 4
- 239000004743 Polypropylene Substances 0.000 claims abstract description 4
- 229920000573 polyethylene Polymers 0.000 claims abstract description 4
- 229920001155 polypropylene Polymers 0.000 claims abstract description 4
- 239000010410 layer Substances 0.000 claims description 53
- 238000004090 dissolution Methods 0.000 claims description 9
- 239000012790 adhesive layer Substances 0.000 claims description 7
- 229920000299 Nylon 12 Polymers 0.000 claims description 6
- 229920000571 Nylon 11 Polymers 0.000 claims description 5
- 238000000034 method Methods 0.000 claims description 5
- FPYJFEHAWHCUMM-UHFFFAOYSA-N maleic anhydride Chemical compound O=C1OC(=O)C=C1 FPYJFEHAWHCUMM-UHFFFAOYSA-N 0.000 claims 1
- 239000004952 Polyamide Substances 0.000 abstract description 2
- 229920003023 plastic Polymers 0.000 abstract description 2
- 239000004033 plastic Substances 0.000 abstract description 2
- 229920002647 polyamide Polymers 0.000 abstract description 2
- 239000002318 adhesion promoter Substances 0.000 abstract 1
- 239000003112 inhibitor Substances 0.000 abstract 1
- 239000000446 fuel Substances 0.000 description 12
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 7
- 235000019441 ethanol Nutrition 0.000 description 7
- 239000000178 monomer Substances 0.000 description 5
- 239000000203 mixture Substances 0.000 description 4
- 239000000126 substance Substances 0.000 description 4
- OKKJLVBELUTLKV-UHFFFAOYSA-N Methanol Chemical compound OC OKKJLVBELUTLKV-UHFFFAOYSA-N 0.000 description 3
- 238000002347 injection Methods 0.000 description 3
- 239000007924 injection Substances 0.000 description 3
- 239000000463 material Substances 0.000 description 3
- JPVYNHNXODAKFH-UHFFFAOYSA-N Cu2+ Chemical compound [Cu+2] JPVYNHNXODAKFH-UHFFFAOYSA-N 0.000 description 2
- 230000001476 alcoholic effect Effects 0.000 description 2
- 229910001431 copper ion Inorganic materials 0.000 description 2
- JGEMYUOFGVHXKV-UPHRSURJSA-N malealdehyde Chemical compound O=C\C=C/C=O JGEMYUOFGVHXKV-UPHRSURJSA-N 0.000 description 2
- 150000001298 alcohols Chemical class 0.000 description 1
- 125000001931 aliphatic group Chemical group 0.000 description 1
- 150000001491 aromatic compounds Chemical class 0.000 description 1
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 description 1
- 238000009833 condensation Methods 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 239000005357 flat glass Substances 0.000 description 1
- 230000008014 freezing Effects 0.000 description 1
- 238000007710 freezing Methods 0.000 description 1
- 239000007788 liquid Substances 0.000 description 1
- 238000012423 maintenance Methods 0.000 description 1
- 230000003647 oxidation Effects 0.000 description 1
- 238000007254 oxidation reaction Methods 0.000 description 1
- 229910052760 oxygen Inorganic materials 0.000 description 1
- 239000001301 oxygen Substances 0.000 description 1
- 229920000098 polyolefin Polymers 0.000 description 1
- 239000011241 protective layer Substances 0.000 description 1
- 229920005989 resin Polymers 0.000 description 1
- 239000011347 resin Substances 0.000 description 1
- 230000000284 resting effect Effects 0.000 description 1
- 239000004094 surface-active agent Substances 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Substances O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
- 239000003643 water by type Substances 0.000 description 1
Classifications
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F02—COMBUSTION ENGINES; HOT-GAS OR COMBUSTION-PRODUCT ENGINE PLANTS
- F02M—SUPPLYING COMBUSTION ENGINES IN GENERAL WITH COMBUSTIBLE MIXTURES OR CONSTITUENTS THEREOF
- F02M37/00—Apparatus or systems for feeding liquid fuel from storage containers to carburettors or fuel-injection apparatus; Arrangements for purifying liquid fuel specially adapted for, or arranged on, internal-combustion engines
- F02M37/0011—Constructional details; Manufacturing or assembly of elements of fuel systems; Materials therefor
- F02M37/0017—Constructional details; Manufacturing or assembly of elements of fuel systems; Materials therefor related to fuel pipes or their connections, e.g. joints or sealings
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B1/00—Layered products having a non-planar shape
- B32B1/08—Tubular products
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/06—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material
- B32B27/08—Layered products comprising a layer of synthetic resin as the main or only constituent of a layer, which is next to another layer of the same or of a different material of synthetic resin
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/30—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers
- B32B27/306—Layered products comprising a layer of synthetic resin comprising vinyl (co)polymers; comprising acrylic (co)polymers comprising vinyl acetate or vinyl alcohol (co)polymers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/32—Layered products comprising a layer of synthetic resin comprising polyolefins
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B27/00—Layered products comprising a layer of synthetic resin
- B32B27/34—Layered products comprising a layer of synthetic resin comprising polyamides
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
- B32B7/04—Interconnection of layers
- B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
-
- F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
- F16—ENGINEERING ELEMENTS AND UNITS; GENERAL MEASURES FOR PRODUCING AND MAINTAINING EFFECTIVE FUNCTIONING OF MACHINES OR INSTALLATIONS; THERMAL INSULATION IN GENERAL
- F16L—PIPES; JOINTS OR FITTINGS FOR PIPES; SUPPORTS FOR PIPES, CABLES OR PROTECTIVE TUBING; MEANS FOR THERMAL INSULATION IN GENERAL
- F16L9/00—Rigid pipes
- F16L9/12—Rigid pipes of plastics with or without reinforcement
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2250/00—Layers arrangement
- B32B2250/05—5 or more layers
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2250/00—Layers arrangement
- B32B2250/24—All layers being polymeric
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/50—Properties of the layers or laminate having particular mechanical properties
- B32B2307/54—Yield strength; Tensile strength
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2307/00—Properties of the layers or laminate
- B32B2307/50—Properties of the layers or laminate having particular mechanical properties
- B32B2307/558—Impact strength, toughness
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2597/00—Tubular articles, e.g. hoses, pipes
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B32—LAYERED PRODUCTS
- B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
- B32B2605/00—Vehicles
- B32B2605/08—Cars
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
- Y10S—TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y10S138/00—Pipes and tubular conduits
- Y10S138/07—Resins
Landscapes
- Engineering & Computer Science (AREA)
- General Engineering & Computer Science (AREA)
- Mechanical Engineering (AREA)
- Chemical & Material Sciences (AREA)
- Combustion & Propulsion (AREA)
- Laminated Bodies (AREA)
- Rigid Pipes And Flexible Pipes (AREA)
- Extrusion Moulding Of Plastics Or The Like (AREA)
Description
車重層配管に関するものである。ここで自動車配管なる
語は、可撓性質をも含めて意味するものであって、自動
車組立ての際に組込まれるものであるが、その後の修
理、保守の際に組込まれるものも含む。この配管は主と
して燃料の給送に使用され、この燃料はアルコール性組
成分を含有することがある。自動車配管が問題となる限
り、これはことにアルコール性媒体給送用配管である。
従って、このアルコール媒体なる語は、単にアルコール
添加燃料もしくは主としてアルコールから成る燃料のみ
でなく、窓ガラスワイパー用液、ブレーキ系の圧力媒体
も含む。周知の通り圧縮空気ブレーキ系には、凝縮水の
氷結を防止するためにアルコールが導入される。本発明
においてアルコールは、ことにメチルアルコール、エチ
ルアルコール、これらの水の混合物を意味するが、高級
アルコールも含まれる。
る筒状外層を有する。これは自動車配管の強度を決定す
る。さらにポリアミド6もしくは6.6或はポリアミド11
もしくは12から成る保護層が設けられるが、これはポリ
アミド12から成る外層との間の介在層により接着されて
いる。この介在層はポリオレフィンから構成される。こ
の公知の自動車配管は、特別の稼働条件下にあっても、
信頼性があり長期間にわたる耐用寿命を有する。この特
別の稼働条件は、自動車配管中を給送される媒体が、例
えば表面活性剤を含有し或は酸素を遊離させる場合に生
起する。上述した公知の自動車配管(DE3821723号)以
外のものは、しばしば応力ひずみ及び厄介な酸化をもた
らす。しかしながら他方において、この公知の自動車配
管の合成樹脂は、燃料に可溶性の物質、例えば未反応の
材料モノマー或はオリゴマーを含有する。そこで燃料が
自動車配管の多層壁から可溶性分を溶出させる事態が生
じ得る。これは上記と公知自動車配管の耐用寿命にほと
んど影響を及ぼすことはないが、他の観点から好ましく
ない。すなわち自動車に燃料を補給してから長時間経過
した場合、例えば船積みされ或は引渡しまでに数週間、
数ケ月を要する場合に、燃料配管中において燃料組成が
変化する。すなわち燃料に含有されるアルコール及び芳
香族化合物が脂肪族組成分よりもはるかに早く自動車配
管の重層壁中に拡散し、この燃料組成の変化により、上
記物質の溶解性限界が変化し、これがまず多層配管壁か
ら溶出する。ことにポリアミド11もしくは12のモノマー
及びオリゴマーは、このいわば休息中の燃料中に析出し
結晶化して沈澱する。銅イオンの存在はこの結晶化挙動
を促進し、多くの場合加速化される。燃料中の銅イオン
は、例えば、燃料ポンプコレクターの摩耗から生ずる。
この沈澱物質はフィルタの目詰りをもたらし、気化器の
フロート室中に集積され、噴射エンジンの場合には噴射
ノズルの目詰りをもたらす。或はまた噴射ポンプの壁縁
辺に堆積することもある。さらに公知の自動車配管はそ
の引張り強さ及び靭性において改善の余地がある。
題は、使用される合成樹脂中の可溶性含有分が障害をも
たらす量まで溶出することがなく、さらに極めて高い引
張り強さ及び靭性を有する、合成樹脂の共押出し法によ
り製造される自動車配管を提供することである。
る筒状外層、ポリアミド6から成る中間層、エチレン及
びビニルアルコールから形成される共重合体から成る耐
溶解層及びポリアミド6から成る内層を有し、外層と中
間層の間にポリエチレンもしくはポリプロピレンから成
る接着層が設けられている、合成樹脂から共押出し法に
より製造される自動車配管により解決されることが本発
明者らにより見出された。なお上記外層の厚さは0.2か
ら0.7mmであるのが好ましい。これは中間層についても
同様である。本発明の好ましい実施態様によれば、耐溶
解層を構成する共重合体のエチレン分は30から45%であ
り、厚さは0.1から0.2mmである。接着層は種々の要件に
適応し、ことに該層を形成する合成樹脂がマレイン酸ヒ
ドリドから成る活性側鎖を有し、層厚さが0.05から0.2m
mの場合に引張り強さ及び靭性を高めることに寄与す
る。内層は著しく薄く、例えば0.1から0.3mmもしくはそ
れ以下の厚さとするのが好ましい。
明自動車配管においてまず耐溶解層及びこれより外方に
在る層からモノマー、オリゴマー或はその他の物質が溶
出しないことである。内層は極めて薄いので、これから
溶出する物質の量は極めて微量で障害を与えない。さら
に内層は特にポリアミド6から構成されているので、溶
解性のモノマー及びオリゴマーを実質的にほとんど含有
していない。さらに上述した層構成により強力に結合
し、高い引張り強さ及び靭性をもたらされる。
本発明実施例についてさらに詳細に説明する。
動車配管を示すものである。これはポリアミド11或は12
から成る環状外層1、ポリアミド6から成る中間層2、
エチレン及びビニルアルコールから形成される共重合体
から成る耐溶解層3及びポリアミド6から成る内層4を
有し、外層と中間層の間にはポリエチレン或はポリプロ
ピレンから成る接着層5が設けられる。なおポリアミド
6から成る内層4は比較的薄く形成される。上述の各層
は共押出しにより一体的に接着結合されている。
れに対して内層4はさらに薄く形成され、一般的に0.1
から0.3mmの厚さに形成される。耐溶解層3はエチレン
/ビニルアルコール共合体(エチレン部分30から40%)
から形成され、その厚さは0.1から0.2mmになされる。接
着層5を構成する合成樹脂はマレイン酸ヒドリドから成
る活性側鎖を有することができ、厚さは0.05から0.2mm
とすることが好ましい。内層4を構成する材料として
は、モノマー含有分の少ない後縮合ポリアミドを使用す
るのがことに好ましい。
製造された配管の横断面図であって、1は外層、2は中
間層、3は耐溶解層、4は内層、5は外層と中間層の間
に設けられた接着剤層を示す。
Claims (7)
- 【請求項1】ポリアミド11もしくは12から成る筒状
外層、ポリアミド6から成る中間層、エチレン及びビニ
ルアルコールから形成される共重合体から成る耐溶解層
及びポリアミド6から成る内層を有し、外層と中間層の
間にポリエチレンもしくはポリプロピレンから成る接着
層が設けられている、合成樹脂から共押出し法により製
造される自動車配管。 - 【請求項2】請求項(1)による自動車配管であって、外
層が0.2から0.7mmの厚さを有する配管。 - 【請求項3】請求項(1)或いは(2)による自動車配管であ
って、中間層が0.05から0.5mmの厚さを有する配管。 - 【請求項4】請求項(1)から(3)のいずれか1つによる自
動車配管であって、耐溶解層を構成する共重合体のエチ
レン分が30から45質量%である配管。 - 【請求項5】請求項(4)による自動車配管であって、耐
溶解層が0.1から0.2mmの厚さを有する配管。 - 【請求項6】請求項(1)から(4)のいずれか1つによる自
動車配管であって、内層が0.1から0.5mm或はそれ以下の
厚さを有する配管。 - 【請求項7】請求項(1)から(6)のいずれか1つによる自
動車配管であって、接着層を構成する合成樹脂がマレイ
ン酸アンヒドリドの活性側鎖を有し、該層の厚さが0.05
から0.2mmの厚さを有する配管。
Applications Claiming Priority (4)
Application Number | Priority Date | Filing Date | Title |
---|---|---|---|
DE3938497 | 1989-11-20 | ||
DE3938497.7 | 1990-01-17 | ||
DE4001125A DE4001125C1 (ja) | 1989-11-20 | 1990-01-17 | |
DE4001125.9 | 1990-01-17 |
Publications (2)
Publication Number | Publication Date |
---|---|
JPH03177683A JPH03177683A (ja) | 1991-08-01 |
JPH0612152B2 true JPH0612152B2 (ja) | 1994-02-16 |
Family
ID=25887251
Family Applications (1)
Application Number | Title | Priority Date | Filing Date |
---|---|---|---|
JP2311667A Expired - Lifetime JPH0612152B2 (ja) | 1989-11-20 | 1990-11-19 | 合成樹脂から共押出し法により製造される自動車配管 |
Country Status (6)
Country | Link |
---|---|
US (1) | US5076329A (ja) |
EP (1) | EP0428833B1 (ja) |
JP (1) | JPH0612152B2 (ja) |
AT (1) | ATE114028T1 (ja) |
DE (1) | DE4001125C1 (ja) |
ES (1) | ES2063875T3 (ja) |
Families Citing this family (120)
Publication number | Priority date | Publication date | Assignee | Title |
---|---|---|---|---|
US20040040607A1 (en) * | 2002-08-28 | 2004-03-04 | Wilson Reji Paul | Refrigerant hose |
US5129428A (en) * | 1989-09-11 | 1992-07-14 | Dayco Products, Inc. | Flexible hose constuction |
DE4006870C2 (de) * | 1990-03-05 | 1998-04-23 | Inventa Ag | Kraftstoffleitung |
DE4202397C2 (de) * | 1992-01-29 | 1999-01-14 | Technoflow Fuel Systems Gmbh | Kraftfahrzeug-Rohrleitung aus einem einschichtigen oder einem mehrschichtigen extrudierten Kunststoffrohr |
DE4202399C1 (ja) * | 1992-01-29 | 1993-02-04 | Technoform Caprano + Brunnhofer Kg, 3501 Fuldabrueck, De | |
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-
1990
- 1990-01-17 DE DE4001125A patent/DE4001125C1/de not_active Expired - Lifetime
- 1990-08-17 AT AT90115735T patent/ATE114028T1/de not_active IP Right Cessation
- 1990-08-17 ES ES90115735T patent/ES2063875T3/es not_active Expired - Lifetime
- 1990-08-17 EP EP90115735A patent/EP0428833B1/de not_active Expired - Lifetime
- 1990-10-31 US US07/607,152 patent/US5076329A/en not_active Expired - Lifetime
- 1990-11-19 JP JP2311667A patent/JPH0612152B2/ja not_active Expired - Lifetime
Also Published As
Publication number | Publication date |
---|---|
EP0428833B1 (de) | 1994-11-09 |
DE4001125C1 (ja) | 1990-12-13 |
ES2063875T3 (es) | 1995-01-16 |
EP0428833A2 (de) | 1991-05-29 |
ATE114028T1 (de) | 1994-11-15 |
US5076329A (en) | 1991-12-31 |
JPH03177683A (ja) | 1991-08-01 |
EP0428833A3 (en) | 1992-11-19 |
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