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    • 2. 发明授权
    • Process for producing highly adherent silicon-containing polyamic acid
and corsslinked silicon-containing polyimide
    • 用于生产高粘附性含硅聚酰胺酸和连接的含硅聚酰亚胺的方法
    • US4818806A
    • 1989-04-04
    • US93143
    • 1987-09-02
    • Kouichi KunimuneYoshiya KutsuzawaHiromi EgawaShiro Konotsune
    • Kouichi KunimuneYoshiya KutsuzawaHiromi EgawaShiro Konotsune
    • C08G73/00C08G73/10C08G77/455C08G77/04
    • C08G73/1085C08G73/106C08G77/455
    • A process for producing a silicon-containing polyamic acid of a specified inherent viscosity as a precursor affording polyimide resins having a considerable extent of heat resistance as adhesives or resins for multilayer laminated composite materials, and a good adhesion onto inorganic materials, metals or resins, and a crosslinked silicon-containing polyimide resin prepared from the polyamic acid are provided, which process comprises reacting a tetracarboxylic acid dianhydride of formula (1) (A mols), a diamine of formula (2) (B mols) and an aminosilicon compound of formula (3) (C mols), satisfying the expressions of (4) and (5): ##STR1## wherein R.sup.1 is a tetravalent carboxylic aromatic group; R.sup.2 is an aliphatic, alicyclic, aromatic aliphatic or carboyclic aromatic group each of a specified number of carbon atoms, a specified polysiloxane group, or a formula of ##STR2## wherein R.sup.8 is a specified hydrocarbon group or hydrogen atom; ##STR3## (s: 1 to 4); R.sup.4 is alkyl, phenyl or alkyl-substituted phenyl each of a specified number of carbon atoms; X is alkoxy, acetoxy or halogen; and 1.ltoreq.k.ltoreq.3, and which polyimide resin is produced by baking a solution containing the above polyamic acid at 50.degree. to 450.degree. C.
    • 制备具有特定的特性粘度的含硅聚酰胺酸作为前体的方法,其提供具有相当程度耐热性的聚酰亚胺树脂作为多层层压复合材料的粘合剂或树脂,以及对无机材料,金属或树脂的良好粘附性, 和由聚酰胺酸制备的交联的含硅聚酰亚胺树脂,该方法包括使式(1)的四羧酸二酐(A摩尔),式(2)的二胺(B摩尔)和氨基硅化合物 (3)(3)(3)(3)(3)(3)(3)(3)(IMA) )其中R1是四价羧酸芳族基团; R2是指定数量的碳原子的脂肪族,脂环族,芳香族脂肪族或碳环芳香族基团,特定的聚硅氧烷基团,或者其中R8是特定的烃基或氢原子的式 + TR (s:1至4); R4是烷基,苯基或烷基取代的苯基,各自具有特定数目的碳原子; X是烷氧基,乙酰氧基或卤素; 和1
    • 5. 发明授权
    • Method for producing polymers of alpha-olefin
    • α-烯烃聚合物的制备方法
    • US4103078A
    • 1978-07-25
    • US340854
    • 1973-03-13
    • Akihiro SatoShiro KonotsuneAtsuyuki KachiHiroshi Shimizu
    • Akihiro SatoShiro KonotsuneAtsuyuki KachiHiroshi Shimizu
    • C08F4/02C08F10/00
    • C08F10/00C08F4/025C08F2410/04
    • Polymers of .alpha.-olefin such as polyethylene, polypropylene, copolymers of ethylene with propylene, butene-1 or styrene, are produced by the (co-) polymerization using a catalyst obtained by mill-mixing an oxide of a metal belonging to I, II, III, VII or VIII Group of the Periodic Table of Elements such as MgO or SiO.sub.2 or B.sub.2 O.sub.3, with a trivalent metal halide such as AlCl.sub.3, then reacting the resultant mixture with a transition metal compound such as TiCl.sub.4 in the presence of an aromatic compound such as xylene, and activating the resultant solid reaction product with an organoaluminum compound such as triethyl aluminum.In the preparation of the present catalyst, no dehydrochlorination occurs. The present catalyst has an excellent utilization efficiency of transition metal compound in the polymerization. Further, no polymer film forms on the wall surface of the polymerization vessel.
    • 通过(共)聚合,使用通过将属于I,II的金属的氧化物混合而获得的催化剂制备α-烯烃如聚乙烯,聚丙烯,乙烯与丙烯的共聚物,丁烯-1或苯乙烯的聚合物 ,III,VII或VIII族元素如MgO或SiO 2或B 2 O 3与三价金属卤化物如AlCl 3组合,然后使所得混合物与诸如TiCl 4的过渡金属化合物在芳族化合物的存在下反应 例如二甲苯,并用有机铝化合物如三乙基铝活化所得的固体反应产物。
    • 7. 发明授权
    • Soluble polyimide-siloxane precursor, process for producing same and
cross-linked polyimide-siloxane
    • 可溶性聚酰亚胺硅氧烷前体,其生产方法和交联聚酰亚胺硅氧烷
    • US4672099A
    • 1987-06-09
    • US833712
    • 1986-02-27
    • Kouichi KunimuneYoshiya KutsuzawaShiro Konotsune
    • Kouichi KunimuneYoshiya KutsuzawaShiro Konotsune
    • C08G73/00C08G73/10C08G77/455H01L21/312C08G77/04
    • C08G73/106C08G77/455
    • A novel soluble polyimide-siloxane precursor having a good storage stability in solution and forming a superior coating on silicon wafer, glass, etc. under heating conditions of low temperature and short time; a process for producing the same; and a cross-linked polyimidesiloxane obtained by heating the above precursor are provided, which precursor hasan imide-amic acid chain part expressed by the formula (1) ##STR1## bonded by a bonding structure expressed by the formula (5)--SiR.sup.7.sub.3-k Y.sup.1.sub.k-1 --O--SiR.sup.7.sub.3-k Y.sup.1.sub.k-1 -- (5) wherein each I, in a total number of m+n+1, represents independently any one of constituting units expressed by the following formulas (2), (3) and (4): ##STR2## wherein R.sup.1 represents a tetravalent carbocyclic aromatic group; R.sup.2, R.sup.4, R.sup.5, R.sup.6, R.sup.7 and Y.sup.1 each are a specified group; l is 1 to 100; m is 0 or an integer; n is an integer; and 1.ltoreq.k.ltoreq.3, andwhich process comprises a first step of reacting a tetracarboxylic acid dianhydride, a diaminosiloxane, a diamine and an aminosilicon compound, each specified, in a solvent under specified conditions, and a second step of heating the resulting reaction solution in the presence of a silylating agent under specified reaction conditions.
    • 一种新颖的可溶性聚酰亚胺硅氧烷前体,在低温和短时间的加热条件下,在溶液中具有良好的储存稳定性,并在硅晶片,玻璃等上形成优异的涂层; 其制造方法; 提供通过加热上述前体得到的交联聚酰亚胺硅氧烷,该前体具有通过式(5)表示的键合结构键合的式(1)表示的酰亚胺 - 酰胺链部分, -SiR73-kY1k-1-O-SiR73-kY1k-1-(5)其中,总数m + n + 1中的每个I独立地表示由下式(2),( (4):(1)其中R1表示四价碳环芳族基团;(4) R2,R4,R5,R6,R7和Y1各自为指定基团; l为1〜100; m为0或整数; n是整数; 和1
    • 8. 发明授权
    • Silicone-polyimide precursor and process for producing same
    • 硅酮 - 聚酰亚胺前体及其制备方法
    • US4591653A
    • 1986-05-27
    • US770223
    • 1985-08-28
    • Kouichi KunimuneYoshiya KutsuzawaShiro Konotsune
    • Kouichi KunimuneYoshiya KutsuzawaShiro Konotsune
    • C08G73/00C08G73/10C08G77/54C07F7/08C07F7/10
    • C08G77/54C08G73/106
    • A silicone-polyimide precursor which affords a coating having a conspicuous adhesion onto silicon wafer, glass, etc. and also an improved strength, hardness, etc. after baking, and a process for producing the same are provided,which precursor is expressed by the formula (1) ##STR1## wherein R.sup.1 represents a tetravalent, carbocyclic aromatic group; R.sup.2, R.sup.3 and R.sup.6 are the same or different groups being 1.about.6 C alkyl, phenyl or alkyl-substituted phenyl of 7.about.12 C; R.sup.4 and R.sup.5 are the same or different groups being ##STR2## wherein s represents an integer of 1 to 4; said group ##STR3## has an average formula weight of 368 to 7,968; X represents alkoxy, acetoxy, halogen atom or hydroxy; ms at both the ends of the formula (1) independently represent an integer of 1 to 3; and l represents an integer of 1 to 30; andwhich process comprises reacting the following compounds (2), (3) and (4): ##STR4## wherein the symbols R.sup.1, etc. are as defined above, and the mixing ratio of (2), (3) and (4) are specified.
    • 提供在硅晶片,玻璃等上具有显着粘合性的涂层并且烘烤后还具有改善的强度,硬度等的涂料及其制备方法的硅 - 聚酰亚胺前体,其前体由 式(1)(1) + TR 其中R1表示四价碳环芳基; R 2,R 3和R 6是相同或不同的基团,其中R 1,R 2,R 3和R 6是相同或不同的基团, R4和R5是相同或不同的基团,其中s表示1至4的整数; 所述组的平均配方重量为368至7,968; X表示烷氧基,乙酰氧基,卤原子或羟基; 式(1)的两端的ms独立地表示1〜3的整数, l表示1〜30的整数, 并且该方法包括使下列化合物(2),(3)和(4)反应:其中符号R1等如上所定义的NH 2 R 5 SiR 63-m X m(4) 并且规定了(2),(3)和(4)的混合比。
    • 9. 发明授权
    • Metal-clad laminates and method for producing same
    • 金属覆层压板及其制造方法
    • US5300364A
    • 1994-04-05
    • US849416
    • 1992-04-29
    • Hiroaki HaseKazutsune KikutaAtsushi TakahashiShiro Konotsune
    • Hiroaki HaseKazutsune KikutaAtsushi TakahashiShiro Konotsune
    • B32B15/08H05K1/00H05K1/03H05K3/00H05K3/30H05K3/38
    • H05K1/0346B32B15/08H05K1/036H05K1/0393H05K2201/0154H05K2201/0358H05K2201/068Y10T428/24917Y10T428/31678Y10T428/31681
    • The present invention provides a flexible metal-clad laminate obtained by directly applying a polyimide precursor to a metallic conductive foil, and then drying, heating and curing the precursor to form a polyimide film, this flexible metal-clad laminate being characterized in that the polyimide film is composed of two or more polyimide layers, the linear thermal expansion coefficient of at least one of the second and later polyimide layers is larger than that of the first layer brought into contact with the metallic conductive foil, and the requirements of the following formulae are met:3.0 t.sub.n and ##EQU1## wherein t.sub.n is the thickness (.mu.m) of the outermost layer (the nth layer) of the polyimide layers, t.sub.n-1 is the thickness (.mu.m) of the film comprising the first layer to the (n-1)th layer of the polyimide layers, and Q.sub.n-1 is a double value (cm) of the curvature radius of the curl of the film comprising the first layer to the (n-1)th layer of the polyimide layers and Rz is the average surface roughness (.mu.m) of the metallic conductive foil. This board does not curl immediately after curing, and the curl does not occur even after the formation of a circuit by etching.
    • PCT No.PCT / JP91 / 01176 Sec。 一九九二年四月二十九日 102(e)日期1992年4月29日PCT 1991年9月3日PCT PCT。 出版物WO92 / 0481100 本发明提供了一种柔性金属包覆层压板,其通过将聚酰亚胺前体直接施加到金属导电箔上,然后干燥,加热和固化前体以形成聚酰亚胺膜,该柔性金属包层 其特征在于,所述聚酰亚胺膜由两层以上的聚酰亚胺层构成,所述第二层和后述的聚酰亚胺层中的至少一层的线性热膨胀系数大于与所述金属导电箔接触的所述第一层的线性热膨胀系数, 满足以下公式的要求:3.0 tn和tn-1> tn和(*化学结构*)其中tn是((my)m) 聚酰亚胺层的最外层(第n层)tn-1是包含第一层至第(n-1)层聚酰亚胺层的膜的厚度((my)m),Qn-1 是包括第一个1a的膜的卷曲的曲率半径的双重值(cm) 对于第(n-1)层的聚酰亚胺层,Rz是金属导电箔的平均表面粗糙度((my)m)。 该板在固化后不会立即卷曲,即使在通过蚀刻形成电路之后也不会发生卷曲。