KR910007982A - 유기실리콘 물질 - Google Patents

유기실리콘 물질 Download PDF

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KR910007982A
KR910007982A KR1019900016340A KR900016340A KR910007982A KR 910007982 A KR910007982 A KR 910007982A KR 1019900016340 A KR1019900016340 A KR 1019900016340A KR 900016340 A KR900016340 A KR 900016340A KR 910007982 A KR910007982 A KR 910007982A
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chain extender
polysiloxane
polyene
carbon
double bonds
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KR1019900016340A
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KR960015454B1 (ko
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케네스 바드 존
쉬미트 버니어 줄리아
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스티븐 에이치, 마르코비츠
헤르큘레스 인코포레이티드
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    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08G—MACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G77/00—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
    • C08G77/48—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms
    • C08G77/50—Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms by carbon linkages
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/04—Reinforcing macromolecular compounds with loose or coherent fibrous material
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • C08J5/241—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres
    • C08J5/244—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs using inorganic fibres using glass fibres
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J5/00—Manufacture of articles or shaped materials containing macromolecular substances
    • C08J5/24—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs
    • C08J5/249—Impregnating materials with prepolymers which can be polymerised in situ, e.g. manufacture of prepregs characterised by the additives used in the prepolymer mixture
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08L—COMPOSITIONS OF MACROMOLECULAR COMPOUNDS
    • C08L83/00—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers
    • C08L83/14—Compositions of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon only; Compositions of derivatives of such polymers in which at least two but not all the silicon atoms are connected by linkages other than oxygen atoms
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/0353—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement
    • H05K1/0366—Organic insulating material consisting of two or more materials, e.g. two or more polymers, polymer + filler, + reinforcement reinforced, e.g. by fibres, fabrics
    • C—CHEMISTRY; METALLURGY
    • C08—ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08J—WORKING-UP; GENERAL PROCESSES OF COMPOUNDING; AFTER-TREATMENT NOT COVERED BY SUBCLASSES C08B, C08C, C08F, C08G or C08H
    • C08J2383/00—Characterised by the use of macromolecular compounds obtained by reactions forming in the main chain of the macromolecule a linkage containing silicon with or without sulfur, nitrogen, oxygen, or carbon only; Derivatives of such polymers
    • C08J2383/04—Polysiloxanes
    • H—ELECTRICITY
    • H05—ELECTRIC TECHNIQUES NOT OTHERWISE PROVIDED FOR
    • H05K—PRINTED CIRCUITS; CASINGS OR CONSTRUCTIONAL DETAILS OF ELECTRIC APPARATUS; MANUFACTURE OF ASSEMBLAGES OF ELECTRICAL COMPONENTS
    • H05K1/00—Printed circuits
    • H05K1/02—Details
    • H05K1/03—Use of materials for the substrate
    • H05K1/0313—Organic insulating material
    • H05K1/032—Organic insulating material consisting of one material

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Medicinal Chemistry (AREA)
  • Health & Medical Sciences (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Materials Engineering (AREA)
  • Manufacturing & Machinery (AREA)
  • Inorganic Chemistry (AREA)
  • Microelectronics & Electronic Packaging (AREA)
  • Reinforced Plastic Materials (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Silicon Polymers (AREA)

Abstract

내용 없음

Description

유기실리콘 물질
본 내용은 요부공개 건이므로 전문내용을 수록하지 않았음

Claims (16)

  1. 디사이클로펜타디엔을 포함한 폴리사이클릭 폴리엔을 규소에 결합된 2개 이상의 수소원자를 갖는 사이클릭폴리실록산과 반응시켜 폴리사이클릭 폴리엔 잔기, 및 탄소-규소 결합을 통해 결합된 사이클릭 폴리실록산 잔기를 포함한 예비중합체를 제조하고, 섬유 보강물질을 예비중합체로 함침시킨 다음, 함침된 물질이 용액을 가열하여 예비중합체를 경화시킴으로 포함하여 프레프레그(prepreg)를 제조하는 방법에 있어서, 상기 사이클릭 폴리실록산이 규소에 결합된 3개 이상의 수소원자를 가지며, 상기 폴리엔 및 폴리실록산이 하이드로실화 반응에 반응성이 높은 적어도 2개 비방향족, 비공역된 탄소-탄소 이중결합을 갖는 적어도 하나의 폴리엔을 포함한 쇄연장제와 반응하고, 상기 탄소-탄소 이중결합이 선형 탄소 잔기상에서 알파, 베타 또는 감마 위치에 존재하여, 변형된 폴리사이클릭 지방족 환 구조에서 2개의 교두보(bridgehead)위치 다음에 있거나, 또는 사이클릭부텐 환에 존재하며, 상기 반응은 예비중합체가 100℃에서 300 내지 3,000cp의 점도를 갖고, 사이클릭 폴리실록산의 유용한 ≡SiH 그룹의 65% 내지 약 75%가 반응할 때까지 지속되는 것을 특징으로 하는 방법.
  2. 제1항에 있어서, 반응을 가열 단계에 의해 증발되는 탄화수소 용매 중에서 수행함을 또한 특징으로 하는 프레프레그의 제조방법.
  3. 제2항에 있어서, 탄화수소 용매가 헥산, 헵탄, 옥탄, 펜탄, 톨루엔, 메틸에틸케톤 또는 크실렌임을 특징으로 하는 프레프레그의 제조방법.
  4. 제2항에 있어서, 탄화수소 용매가 예비중합체 용액의 10 내지 30 중량%를 차지함을 또한 특징으로 하는 프레프레그의 제조방법.
  5. 제1항 내지 제4항중 어느 한 항에 있어서, 쇄 여장제의 분자량이 1,000미만임을 특징으로 하는 프레프레그의 제조방법.
  6. 제5항에 있어서, 쇄 연장제의 분자량이 500 미만임을 특징으로 하는 프레프레그의 제조방법.
  7. 제5항에 있어서, 쇄 연장제가 디알릴, 디비닐 또는 비스-노르보네닐 화합물임을 또한 특징으로 하는 프레프레그의 제조방법.
  8. 제5항에 있어서, 쇄 연장제가 5-비닐-2-노르보넨, 5-에틸리덴-2-노르보넨, 또는 트리사이클로펜타디엔의 대칭 이성체임을 또한 특징으로 하는 프레프레그의 제조방법.
  9. 제1항 내지 제8항중 어느 한 항에 있어서, 폴리앤(a) 및 폴리실록산(b)이 각각 하이드로실화 반응에 모두 반응성이 있는 2개의 탄소-탄소 이중결합을 가지며, 폴리앤(a), 폴리실록산(b)및 쇄 연장제(c)의 관계 비율이 각각 하기와 같음을 또한 특징으로 하는 프레프레그의 제조방법.
  10. 제9항에 있어서, 폴리엔(a)가 디사이클로펜타디엔이고, 쇄 연장제(c)가 5-비닐-2-노르보낸임을 또한 특징으로 하는 프레프레그의 제조방법.
  11. 제1항 내지 제10항중 어느 한항에 있어서, 폴리엔(a)및 쇄 연장제(c)중의 이중결합, 폴리실록산(b)중의 SiH 결합이 비율이 약 1.1:1 이상임을 특징으로 하는 프레프레그의 제조방법.
  12. 제11항에 있어서, 폴리엔(a) 및 쇄 연장제(c)중의 이중결합, 폴리실록산(b)중의 SiH 결합의 비율이 약 1.1:1 내지 1.2:1의 범위임을 또한 특징으로 하는 프레프레그의 제조방법.
  13. 제9항에 있어서, 폴리엔(a)가 F1사이클로텐타디엔, 및 트리사이클로 펜타디엔의 비대칭 이성체의 혼합물을 포함하고 폴리실록산(b)가 메틸하이드로사이클로실록산의 혼합물이며, 쇄 연장제(c)는 트리사이클로펜타디엔의 대칭 이성체임을 또한 특징으로 하는 프레프레그의 제조방법.
  14. 제13항에 있어서, 폴리엔(a)및 쇄 연장제(c)중의 이중결합, 폴리실록산(b) 중의 SiH 결합의 비율이 약 0.8:1 내지 1.2:1의 범위임을 또한 특징으로 하는 프레프레그의 제조방법.
  15. 제13항 또는 제14항에 있어서, 트리사이클로펜타디엔의 비율이 예비중합체의 약 15 내지 35중량%이고, 탄소-탄소 이중결합, SiH 결합의 비가 약 1:1임을 특징으로 하는 프레프레그의 제조방법.
  16. 전도성 물질로 피복되어 인쇄 회로기판을 형성시키는 적층판에서의 제1항 내지 제15항중 어느 한 항에서 청구된 방법에 의해 제조된 프레프레그의 용도.
    ※ 참고사항 : 최초출원 내용에 의하여 공개하는 것임.
KR1019900016340A 1989-10-16 1990-10-15 유기실리콘 물질 KR960015454B1 (ko)

Applications Claiming Priority (3)

Application Number Priority Date Filing Date Title
US422214 1989-10-16
US07/422,214 US5008360A (en) 1989-10-16 1989-10-16 Organosilicon materials
US422,214 1989-10-16

Publications (2)

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KR910007982A true KR910007982A (ko) 1991-05-30
KR960015454B1 KR960015454B1 (ko) 1996-11-14

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US (1) US5008360A (ko)
EP (1) EP0423689A3 (ko)
JP (1) JPH07110903B2 (ko)
KR (1) KR960015454B1 (ko)
BR (1) BR9005207A (ko)
CA (1) CA2027696A1 (ko)
MX (1) MX22862A (ko)

Families Citing this family (32)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
JP2966463B2 (ja) * 1990-03-27 1999-10-25 信越化学工業株式会社 硬化性樹脂組成物
US5242979A (en) * 1990-10-05 1993-09-07 Hercules Incorporated Organosilicon compositions containing hydrocarbon elastomers
US5340644A (en) * 1990-10-05 1994-08-23 Hercules Incorporated Organosilicon compositions
US5118735A (en) * 1990-10-05 1992-06-02 Hercules Incorporated Organosilicon composition comprising stabilizers
US5147945A (en) * 1990-12-31 1992-09-15 Hercules Incorporated Organosilicon polymers and prepolymers comprising a coupling monomer
US5171817A (en) * 1991-04-15 1992-12-15 Hercules Incorporated Organosilicon compositions containing siloxane elastomers
US5196498A (en) * 1991-09-24 1993-03-23 Hercules Incorporated Organosilicon polymers
US5254655A (en) * 1992-02-05 1993-10-19 Hercules Incorporated Organosilicon polymers, and dyes, exhibiting nonlinear optical response
US5298536A (en) * 1992-02-21 1994-03-29 Hercules Incorporated Flame retardant organosilicon polymer composition, process for making same, and article produced therefrom
US5523374A (en) * 1992-12-03 1996-06-04 Hercules Incorporated Curable and cured organosilicon compositions
USH1388H (en) * 1992-12-23 1994-12-06 Hercules Incorporated Polyolefin polymer and method of making same
US5334688A (en) * 1993-04-19 1994-08-02 Hercules Incorporated Fully substituted cyclopolysiloxanes and their use for making organosilicon polymers
US5408026A (en) * 1993-08-23 1995-04-18 Cowan; Patrick J. Curable and cured organosilicon compositions, and process for making same
US5451637A (en) * 1994-05-10 1995-09-19 Hercules Incorporated Organosilicon compositions prepared from unsaturated elastomeric polymers
JPH07309950A (ja) * 1994-05-17 1995-11-28 Toray Dow Corning Silicone Co Ltd 有機ケイ素重合体およびその製造方法
US5512376A (en) * 1994-06-20 1996-04-30 Hercules Incorporated Nonpolar polymers comprising antiplasticizers
DE4423893C2 (de) * 1994-07-07 1996-09-05 Freudenberg Carl Fa Flachdichtung mit flexibler Leiterplatte
US5859105A (en) * 1997-02-11 1999-01-12 Johnson Matthey, Inc. Organosilicon-containing compositions capable of rapid curing at low temperature
US5852092A (en) * 1997-02-11 1998-12-22 Johnson Matthey, Inc. Organosilicon-containing compositions having enhanced adhesive properties
US6911518B2 (en) 1999-12-23 2005-06-28 Hybrid Plastics, Llc Polyhedral oligomeric -silsesquioxanes, -silicates and -siloxanes bearing ring-strained olefinic functionalities
US7888435B2 (en) * 1999-08-04 2011-02-15 Hybrid Plastics, Inc. Process for continuous production of olefin polyhedral oligomeric silsesquioxane cages
TWI224617B (en) * 1999-11-08 2004-12-01 Kaneka Corp Copper foil with insulating adhesive
DE10026432A1 (de) 2000-05-29 2002-02-14 3M Espe Ag Präpolymere (Meth)acrylate mit polycyclischen oder aromatischen Segmenten
JP2002327078A (ja) * 2001-04-27 2002-11-15 Kanegafuchi Chem Ind Co Ltd ポリカルボシランプリプレグ及びそれを用いた積層板
US6872792B2 (en) 2001-06-25 2005-03-29 Lord Corporation Metathesis polymerization adhesives and coatings
US7651642B2 (en) * 2001-07-23 2010-01-26 Momentive Performance Materials Inc. Stabilized polyorganosiloxane composition
DE102004039111A1 (de) * 2003-08-14 2005-04-14 Shin-Etsu Chemical Co., Ltd. Härtbare Silikonharzzusammensetzung
JP2007077252A (ja) * 2005-09-13 2007-03-29 Shin Etsu Chem Co Ltd 硬化性シリコーン組成物
JP2008069210A (ja) * 2006-09-12 2008-03-27 Shin Etsu Chem Co Ltd 多環式炭化水素基含有シリコーン系硬化性組成物
IT201700089373A1 (it) * 2017-08-03 2019-02-03 Petroceramics S P A Materiale composito fibro-rinforzato pre-impregnato e materiale composito ceramico fibro-rinforzato, ottenuto per formatura e successiva pirolisi di detto materiale pre-impregnato
IT201700089430A1 (it) * 2017-08-03 2019-02-03 Petroceramics S P A Materiale composito fibro-rinforzato pre-impregnato e manufatto ottenuto per formatura e completo indurimento di detto materiale composito fibro-rinforzato pre-impregnato
US10892256B2 (en) * 2018-01-31 2021-01-12 Nanolumens Acquisition, Inc. Light emitting display system having improved fire performance

Family Cites Families (18)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US2665287A (en) * 1948-08-09 1954-01-05 Allied Chem & Dye Corp Production of cyclic organosilicon compounds
BE553159A (ko) * 1955-12-05
DE1125619B (ko) * 1960-07-08
US3197432A (en) * 1962-07-02 1965-07-27 Gen Electric Transparent resinous organopolysiloxanes
US3197433A (en) * 1962-07-02 1965-07-27 Gen Electric Optically clear organopolysiloxane resins
US3220972A (en) * 1962-07-02 1965-11-30 Gen Electric Organosilicon process using a chloroplatinic acid reaction product as the catalyst
US3271362A (en) * 1966-02-07 1966-09-06 Gen Electric Process for reaction of silanic hydrogen with unsaturated organic compounds
US3929850A (en) * 1971-11-19 1975-12-30 Huels Chemische Werke Ag Process for the production of polymeric hydrocarbons having reactive silyl end groups
JPS5133540B2 (ko) * 1973-10-08 1976-09-20
US3992427A (en) * 1975-02-25 1976-11-16 Dow Corning Limited Preparation of organosilicon compounds
JPS5917669B2 (ja) * 1976-08-24 1984-04-23 信越化学工業株式会社 積層板
SU767112A1 (ru) * 1978-05-24 1980-09-30 Волгоградский Политехнический Институт Способ получени бис (хлорсилил) трицикло-/5.2.1.02.6/ деканов
JPS6178794A (ja) * 1984-09-26 1986-04-22 Toshiba Silicone Co Ltd オルガノシクロシロキサン
CA1273144A (en) * 1985-05-07 1990-08-21 Takafumi Uemiya Cross-linked optical siloxane polymer
JPS62207333A (ja) * 1986-03-08 1987-09-11 Nippon Petrochem Co Ltd シリコ−ン共重合体
US4900779A (en) * 1986-08-27 1990-02-13 Hercules Incorporated Organosilicon polymers
US4902731A (en) * 1986-08-27 1990-02-20 Hercules Incorporated Organosilicon prepolymers
US4877820A (en) * 1987-03-20 1989-10-31 Hercules Incorporated Cross-linked organosiloxane polymers

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EP0423689A3 (en) 1991-10-09
BR9005207A (pt) 1991-09-17
CA2027696A1 (en) 1991-04-17
US5008360A (en) 1991-04-16
KR960015454B1 (ko) 1996-11-14
AU6463390A (en) 1991-04-18
JPH03221539A (ja) 1991-09-30
JPH07110903B2 (ja) 1995-11-29
MX22862A (es) 1993-11-01
AU626003B2 (en) 1992-07-23
EP0423689A2 (en) 1991-04-24

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