TW201229055A - Liquid addition curable metallosiloxane - Google Patents

Liquid addition curable metallosiloxane Download PDF

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TW201229055A
TW201229055A TW100139506A TW100139506A TW201229055A TW 201229055 A TW201229055 A TW 201229055A TW 100139506 A TW100139506 A TW 100139506A TW 100139506 A TW100139506 A TW 100139506A TW 201229055 A TW201229055 A TW 201229055A
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Taiwan
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decane
compound
group
propyl
vinyl
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TW100139506A
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Chinese (zh)
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Tomoya Egawa
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Daicel Corp
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    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G77/00Macromolecular compounds obtained by reactions forming a linkage containing silicon with or without sulfur, nitrogen, oxygen or carbon in the main chain of the macromolecule
    • C08G77/48Macromolecular 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
    • C08G77/58Metal-containing linkages

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  • Chemical & Material Sciences (AREA)
  • Health & Medical Sciences (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Medicinal Chemistry (AREA)
  • Polymers & Plastics (AREA)
  • Organic Chemistry (AREA)
  • Compositions Of Macromolecular Compounds (AREA)
  • Polymers With Sulfur, Phosphorus Or Metals In The Main Chain (AREA)
  • Structures Or Materials For Encapsulating Or Coating Semiconductor Devices Or Solid State Devices (AREA)
  • Silicon Polymers (AREA)

Abstract

Metallosiloxane compound of the present invention is obtained by passing first process and second process. The first process is that bifunctional silane compound(S1) and metal compound(M) as zirconium compound or titanium compound react with H2O according to need. The second process is that reaction product of the first process and monofunctional silane compound(S2) react with H2O according to need. The metallosiloxane compound is produced by the sliane compound(S1): the metal compound(M): the silane compound(S2): H2O in first process: H2O in second process react at a specific molar ratio. The metallosiloxane compound has at least one Si-H bond or C2-10 alkenyl group in a molecule. The metallosiloxane compound is an addition curable compound without outgas and has excellent heat-resistant non-xanthochroism property when contained in curable resin composition and than cured.

Description

201229055 六、發明說明: 【發明所屬之技術領域】 本發明係關於具有加成硬化性的金屬矽氧烷、及具 有该金屬石夕氧烧的硬化性樹脂組成物以及其硬化物。 【先前技術】 近年來半導體裝置、光電子裝置等固態元件裝置的 大電流化進展,隨之發熱量有增大的傾向。因此,對於 此等之裝置的封裝用等封裝材料逐漸開始要求高耐熱性 和耐久性。又,對於光電子裝置用的封裝材料除了上述 以外,還要求透明性。 為了要回應上述要求,逐漸開始有使用含有無機系 化合物的樹脂組成物作為耐熱性、耐熱安定性(耐熱著色 性)、透明性等優良之樹脂材料。在專利文獻i中記載有 將聚茂金屬(P〇iymetalloxane)化合物或金屬四烷氧化物 與含烯基的單矽烷醇進行反應製得之反應生成物予以水 解及縮合而製造之矽烷化聚茂金屬化合物。又,在專利 文獻2令記載有在烷氧矽烷化合物或包含其之混合物中 添加烧氧錯化合物或包含其之混合物以及水或水與水溶 性有機溶劑的混合物,藉由進行烧氧我化合物與烧氧 鍅化,物的部分共水解縮合而製造之有機溶劑可溶性的 錯m ^而’此等之錢化聚茂金屬化合物及錐石夕 氧烧為固n ’並無針對其耐熱無黃變性進行探討。 [先前技術文獻] [專利文獻] [專利文獻1]曰本特開2009“ 739 1〇號公報 201229055 [專利文獻2]日本特開2009-286986號公報 【發明内容】 [發明欲解決的課題] 本發明之目的在於提供一種加成硬化性的金屬矽氧 烧化合物’當其含於硬化性樹脂組成物中並硬化時,耐 熱無黃變性優良,且未出現逸出氣體。 又,本發明之其他目的在於提供一種硬化性樹脂組 成物’其含有上述金屬矽氧烷化合物,且未產生逸出氣 體’藉由使其硬化而可製得耐熱無黃變的無機系硬化樹 脂。 又’本發明之其他目的在於提供一種耐熱無黃變的 硬化物’其係將上述硬化性樹脂組成物硬化而製得。 [用以解決課題之手段] 本發明者為了解決上述課題而進行潛心探討之結果 ’發現使2官能之矽烷化合物與單官能之矽烷化合物與金 屬化合物與視需要的Η"以特定的莫耳比進行反應而製 得之新穎金屬矽氧烷化合物,包含該金屬矽氧烷化合物 的硬化性樹脂組成物在硬化時沒有逸出氣體的產生,此 外將該硬化性樹脂組成物硬化而成之硬化物具有優良的 耐熱無黃變性,本發明臻於完成。 即’本發明係提供一種金屬矽氧烷化合物,其特徵 為:藉由歷經使以下列式(i) 201229055 (式中,I^,R2係相同或不同,表示氮原子、Cl_10烷基、 C2-10烯基、C6_14芳基或(37_15芳烷基;Χ、χ2係相同或不同 ,表示Cl. -10烧氧基、鹵素原子或經基) 表示之矽烷化合物(S 1)與以下列式(2) Y3201229055. EMBODIMENT OF THE INVENTION [Technical Field] The present invention relates to a metal siloxane having addition curability and a curable resin composition having the metal oxysulphur and a cured product thereof. [Prior Art] In recent years, a large current of a solid-state device such as a semiconductor device or an optoelectronic device has progressed, and the amount of heat generation tends to increase. Therefore, packaging materials such as packages for such devices are beginning to require high heat resistance and durability. Further, in addition to the above, the encapsulating material for an optoelectronic device requires transparency. In response to the above-mentioned requirements, a resin composition containing an inorganic compound is used as a resin material excellent in heat resistance, heat stability (heat resistance colorability), transparency, and the like. Patent Document i describes a decane-forming polysiloxane produced by reacting a reaction product obtained by reacting a polymetallocene (P〇iymetalloxane) compound or a metal tetraalkoxide with an alkenyl group-containing monostanol. Metal compound. Further, Patent Document 2 describes a method of adding a burned oxygen-containing compound or a mixture thereof and a mixture of water or water and a water-soluble organic solvent to an alkoxysilane compound or a mixture thereof, by performing an oxygen-burning compound and Oxygen oximation, partial co-hydrolysis condensation of the substance to produce an organic solvent soluble error m ^ and 'such as the money-forming polymetallocene compound and cone-shaped oxygen burning solid n ' is not resistant to its heat-resistant yellow-free Discuss it. [PRIOR ART DOCUMENT] [Patent Document 1] Japanese Patent Application Laid-Open No. Hei. No. Hei. No. 2009-286986 [Patent Document 2] JP-A-2009-286986 An object of the present invention is to provide an addition-hardening metal oxy-oxygen compound which is excellent in heat-resistant and non-yellowing properties when it is contained in a curable resin composition and hardens, and does not exhibit an escape gas. Another object of the present invention is to provide a curable resin composition which contains the above metal oxoxane compound and which does not generate an escape gas, which can be cured to obtain a heat-resistant, non-yellowing inorganic hardening resin. Another object of the present invention is to provide a cured product which is resistant to heat and yellowing, which is obtained by curing the above-mentioned curable resin composition. [Means for Solving the Problems] The present inventors have conducted intensive discussions to solve the above problems. A novel method for reacting a bifunctional decane compound with a monofunctional decane compound and a metal compound with a desired oxime ratio in a specific molar ratio was found. The metal siloxane compound, the curable resin composition containing the metal siloxane compound does not generate gas at the time of curing, and the cured product obtained by hardening the curable resin composition has excellent heat-resistant and yellow-free resistance. The present invention is completed. That is, the present invention provides a metal oxoxane compound characterized by: by the following formula (i) 201229055 (wherein, I^, R2 are the same or different, represent nitrogen a decane compound represented by an atom, a Cl_10 alkyl group, a C2-10 alkenyl group, a C6_14 aryl group or a (37-15 aralkyl group; the fluorene or fluorene 2 is the same or different and represents a Cl.-10 alkoxy group, a halogen atom or a trans group) S 1) and Y3 with the following formula (2)

I γ1-Μ — Y4 ⑵I γ1-Μ — Y4 (2)

I Y2 (式中,Μ表示錯或鈦;Y1〜Y4係相同或不同’表示ci-i2 烷氧基或鹵素原子) 表示之金屬化合物(M)進行反應或使該石夕烧化合物(S 1) 與該金屬化合物(M)與H20進行反應之第1步驟、和使該 第1步驟的反應生成物與以下列式(3) R3I Y2 (wherein, Μ represents a wrong or titanium; Y1 to Y4 are the same or different 'is a ci-i2 alkoxy group or a halogen atom), and the metal compound (M) is reacted or the compound is sintered (S 1 a first step of reacting the metal compound (M) with H20, and a reaction product of the first step and R3 of the following formula (3)

I X3 — Si — R5 (3) (式中,R3〜R5係相同或不同,表示氫原子、C^o烷基、 C2-1Q烯基、C:6-]4芳基或C?-丨5芳烧基;X3表示Cuio燒氧基 、鹵素原子或經基) 表示之矽烷化合物(S2)進行反應或使該第丨步驟的反鹿 生成物與該矽烷化合物(S2)與Ηβ進行反應之第2步驟而 得,以該石夕烧化合物(S 1):該金屬化合物(μ):該妙境化 合物(S2):第1步驟的H2〇:第2步驟的H2〇 = m: η: V· • κ ·珏 :b之莫耳比,且在m,n,k,a,b滿足以下的關係⑴〜(v)的 全部條件下反應而製造,且在1分子中至少具有1個 鍵或C2_1Q烯基。 201229055 (i) m> 0,n> 0,k> 〇,ag 〇,b$ 〇 (ii) n/m ^ 3 (iii) (iv) (a + am)/(m + n) = 〇.〇3〜〇 8 (ah-(2a + am)} 當X3為烷氧基或 時 ’ b=0 〇 素原子時,b^k;當X3為羥基 (上述式中,當Xl,X2同時為羥基時 ;當僅Χ、Χ2的任一者為羥基時,ar 同時非經基時,ani = 〇,ah==2m+4n) ,am,ah 為 am = 2m,ah = 4n = m,ah = m + 4n ;當 X1,X2 上述金屬碎氧烧化合物 度下為液態。 又’本發明係提供—種 具有Si ·Η鍵的化合物與具有 樹脂組成物,其特徵為至少 (Α)與氫化矽烷化觸媒(c)。 較佳為在0〜9 〇 °C的任何溫 硬化性樹脂組成物,其包含 C2-1 〇烯基的化合物之硬化性 含有上述金屬矽氧烷化合物 上述硬化性樹脂組成物較佳為 劑(D) 〇 進一步含有無機填充 又,上述硬化性樹脂組成物較佳 偶合劑(Ε)。 為進一步含有矽烷 此外,本發明提供— 化而成之硬化物。 種將上述硬化性樹脂組成物硬 [發明的效果] 氧烷 產生 與本發明相關之金屬矽氧烷化合物 化合物的硬化性樹脂組成物在硬化 ,將該硬化性樹脂組成物硬化而成 ’包含該金屬矽 時無逸出氣體之 之硬化物具有優 it 201229055 良的耐熱無黃變性。因此,對led等電子裝置之封裝劑 或密封劑、耐熱硬被覆等而言乃為有用。 【實施方式】 [用以實施發明的形態ί [金屬矽氧烷化合物(a)] 本發明之金屬矽氧烷化合物(A)係具有下列特徵之 化合物:藉由歷經使以下列式(j) R1I X3 — Si — R5 (3) (wherein R3 to R5 are the same or different and represent a hydrogen atom, a C^o alkyl group, a C2-1Q alkenyl group, a C:6-]4 aryl group or a C?-丨 group. 5 aryl group; X3 represents a Cuio alkoxy group, a halogen atom or a decane compound represented by a group) (S2) is reacted or the anti-deer product of the second step is reacted with the decane compound (S2) and Ηβ. In the second step, the compound (S 1): the metal compound (μ): the miracle compound (S2): H2 in the first step: H2 in the second step = m: η: V· • κ · 珏: the molar ratio of b, and m, n, k, a, b are produced by reacting under the following conditions (1) to (v), and have at least one molecule in one molecule. Key or C2_1Q alkenyl. 201229055 (i) m>0,n>0,k> 〇,ag 〇,b$ 〇(ii) n/m ^ 3 (iii) (iv) (a + am)/(m + n) = 〇. 〇3~〇8 (ah-(2a + am)} When X3 is an alkoxy group or when 'b=0 a halogen atom, b^k; when X3 is a hydroxyl group (in the above formula, when Xl, X2 are simultaneously When hydroxy; when only Χ, Χ2 is hydroxy, ar is non-base, ani = 〇, ah == 2m + 4n), am, ah is am = 2m, ah = 4n = m, ah = m + 4n ; when X1, X2 is a liquid in the above-mentioned metal oxidizing compound degree. Further, the present invention provides a compound having a Si Η bond and a resin composition characterized by at least (Α) and hydrogenation. The decane-forming catalyst (c) is preferably any thermosetting resin composition of 0 to 9 〇 ° C, and the curability of the compound containing C2-1 decenyl group contains the above-mentioned metal oxirane compound. The resin composition preferably has the agent (D), further contains an inorganic filler, and the curable resin composition is preferably a coupling agent. In order to further contain a decane, the present invention provides a cured product. Curable resin composition Hard [Effects of the Invention] Oxygen gas is produced by curing a curable resin composition of a metal oxoxane compound compound according to the present invention, and hardening the curable resin composition to have no escape gas when the metal ruthenium is contained. The hardened material has excellent heat-resistant and non-yellowing properties of 20120055. Therefore, it is useful for an encapsulant or a sealant for an electronic device such as led, a heat-resistant hard coating, etc. [Embodiment] [A form for implementing the invention] [Metal oxoxane compound (a)] The metal oxoxane compound (A) of the present invention is a compound having the following characteristics: by the following formula (j) R1

I X1 — Si — X2 ( I) R2 (式中’ r\r2係相同或不同,表示氫原子、Cl-1()烷基、I X1 — Si — X2 ( I) R2 (wherein 'r\r2 is the same or different, meaning hydrogen atom, Cl-1() alkyl group,

Cm稀基、C6.M芳基或(37_15芳烷基;χΐ,χ2係相同或不同 ,表不C丨-丨〇烷氧基、鹵素原子或羥基) 表示之♦烧化合物(S1)與以下列式(2) Υ3 γ1 —一 (2) v2 (式中,Μ表示鍅或鈦;γι〜γ4係相同或不同,表示Ci i2 烧氧基或齒素原子) 表示之金屬化合物(M)與視需要之H2〇進行反應之第ί步 驟、與該第1步驟的反應生成物與以下列式(3) (式中’ R3〜R5係相同或不同,表示氫原子、Cm 〇烧基、 C2-1Q:^基' C6'M芳基或C7.15芳烷基;X3表示C丨-丨〇烷氧基 201229055 、鹵素原子或羥基) 表示之矽烷化合物(s 2)、盥 , ^ )興視需要之H20進行反應之第2 步驟而製得’該矽烧彳卜人 s物(s 1):該金屬化合物(M):該 矽烷化合物(S2):第聰 第V驟的H2〇 :第2步驟的H20 = m : n •k:a:b之莫耳比,日 丑在1n,n,k,a,b滿足以下的關係⑴ 〜(v)的全部條件進行反 订汉應而製造,且在1分子中至少且 有1個Si-H鍵或C2-lQ烯基。 、 ⑴ m>〇,n>0,k>〇a^〇b“ (ii) η/mg 3 (iii) (iv) U+am)/(m + n) = 〇 〇3〜〇 8 ^ = {ah (2a+am)} 當X3為烷氧基或鹵素原 時,b = 〇 〇 子時,bgk;當X3為羥基 (上述式中,當X丨,χ2同時 马 I 基時 ’ &111,3}1為3111 = 2111,311::=:411 ,當僅X 1,X 2的任一者為跑笼。古 為红基時,am = m,ah = m + 4n ;當 Χ、χ2 同時非經基時,am = 〇,ah = 2rn + 4n) 就〇2.10稀基而言,可列舉乙稀基、稀丙基、2_ 丁婦 基2戊烯基2-己炔基等。就Cn〇稀基而言,較佳為 乙稀基晞丙基。另外,當如後述般使用S種以上石夕燒 化口物(S1)、金屬化合物(M)、矽烷化合物(s2)時,爪,订 ’ k係各該等的合計量之莫耳比。 在本發明中,於上述第丨步驟,係使為烷氧基或鹵素 原子的水解性基及羥基之任一官能基(χ1,χ2)與在1分子 内具有兩個所謂2官能之石夕烧化合物(S1)[以下稱為2官 能之矽烷化合物(S1)]及金屬化合物^)進行反應。兹認 201229055 為於第1步驟中,形成2官能之矽烷化合物(S1)的矽原子 與金屬原子(Zr,Ti)透過氧原子鍵結而成之主鏈。 使第1步驟中的金屬化合物(M)的使用量相對於2官 能之矽烷化合物(S1)為3倍莫耳以下,使相對於[上述式 (η)]、「上述2官能之矽烷化合物(S1)與金屬化合物 的合計使用量」之「HA與矽烷化合物(S1)中的羥基之合 計使用量」的比為〇.〇3〜〇_8(莫耳比)[上述式(iii)]。玆認 為藉由在如上述般的條件下使2官能之矽烷化合物U 與金屬化合物(Μ)及視需要之ίο進行反應而合成主鏈 ,最後製得之金屬矽氧烷化合物(A)在較佳為〇〜9〇它的 任何/孤度下會谷易成為液態。可將相對於「2官能之矽烷 化合物(S1)與金屬化合物(M)之合計使用量」的「Η"與 Μ化合物(S i)中的經基合計使用量」之莫耳比設定為 較佳0.05〜0.6,特佳〇」〜〇 45之範圍。 接著於上述第2步驟中,使在第丨步驟製得之反應液 與3為烷氧基或鹵素原子的水解性基及羥基之任一官能基 (X )與在1分子内具有1個所謂單官能之矽烷化合物(S2)[ 以下稱為單官能之矽烷化合物(S2)]及視需要之H2〇進行 ,應玆^為於第2步驟中製得在側鏈上導入源自於單官 切烧化合物(S2)之⑦烧基而成之金屬*氧烧化合物。 在本發月中,係使上述單官能之矽烷化合物(^2)的 使用里為與第1步驟中製得之反應液中殘存的水解性基 之莫耳數為等量或超過其之莫耳數[上述式(iv)]。單官能 夕烷化D物(S2)的莫耳數較佳為在第丨步驟中製得之 反應液中殘存之水解性基莫耳數的1.5倍以上,進一步更 -10- 201229055 佳為2乜以上。於第2步 。 ,,^ Ψ 错由使早吕能之矽烷化合 物(S2)的使用量成為如 ^ , λ 上述鈸,則可使最後製得之金屬 石夕氧炫化合物(Α)中的欢銥ω . . 解性基之殘留為最低限度,且硬 化時不產生逸出ϋ體,i Αι ” 可I得能獲得耐熱無黃變之硬化 物的金屬矽氧烷化合物。 在本發明中,备7 ^ 田g月匕之矽烷化合物(S1)的官能基 χ,χ之任一者或雙方太全-«· 士 飞又万為羥基時,於第1步驟令的h2◦之使 用量係依其數目減少或可不使用H2〇。又,於第2步驟中 ’當早官能之石夕烧化合物(S2)的官能基奶為經基時,可 不使用H2O。 上述第1步驟與第?牛锁k 。 一罘2步驟中的反應可在例如50〜 150t較佳為60〜13GX:,更佳為6G〜刚。c下進行。惟, 的滴下較佳為在例如_3(rc以下的溫度下進行。又, 上述第丨步驟與第2步驟中的反應時間亦因反應溫度、使 用之矽烷化合物及金屬化合物的種類而不同,可設為例 如1 〇分鐘〜1 0小時較佳為1〜5小時。 上述的製造方法中製造之金屬矽氧烷化合物(A)較 佳為在0〜9CTC之任何溫度下為液態,更佳為在〇〜7〇<t 之任何溫度下,特佳為〇〜30。(:之任何溫度下為液態。 [2官能之矽烷化合物(si)] 使用於製造本發明之金屬矽氧烷化合物的反應 之2官能之矽烧化合物(S 1)可使用以下列式(1) R1Cm dilute group, C6.M aryl group or (37_15 aralkyl group; χΐ, χ 2 is the same or different, and represents C 丨-decyloxy group, halogen atom or hydroxyl group) represents ▲ burning compound (S1) and the following The formula (2) Υ3 γ1 —1(2) v2 (wherein Μ represents 鍅 or titanium; γι γ γ4 is the same or different, meaning Ci i2 alkoxy or dentate atom) represents a metal compound (M) and The reaction step of the reaction of H2 视 as needed and the reaction product of the first step are the same as or different from the following formula (3) (wherein R3 to R5 are the same or different, and represent a hydrogen atom, a Cm sulphur group, C2 -1Q: ^'s 'C6'M aryl or C7.15 aralkyl; X3 represents C丨-decyloxy 201229055, halogen atom or hydroxy) decane compound (s 2), 盥, ^) The second step of the reaction of H20 is carried out as needed to prepare 'the 矽 彳 彳 s s (s 1): the metal compound (M): the decane compound (S2): H2 第 of the first V: The second step of H20 = m : n • k: a: b molar ratio, the ugly of 1n, n, k, a, b satisfies the following relationship (1) ~ (v) all conditions are reversed Manufactured, and at least one molecule A Si-H bond alkenyl group or C2-lQ. , (1) m > 〇, n > 0, k > 〇 a ^ 〇 b " (ii) η / mg 3 (iii) (iv) U + am) / (m + n) = 〇〇 3 ~ 〇 8 ^ = {ah (2a+am)} When X3 is alkoxy or halogen, b = scorpion, bgk; when X3 is hydroxy (in the above formula, when X 丨, χ 2 is simultaneously a horse I ' & 111, 3} 1 is 3111 = 2111, 311::=:411, when only X 1, X 2 is running cage. When the ancient is red, am = m, ah = m + 4n; , χ 2 at the same time non-basic, am = 〇, ah = 2rn + 4n) For the 〇2.10 dilute group, examples thereof include an ethyl group, a dilute propyl group, a 2-butyl group, a 2-pentenyl group, a 2-hexynyl group, and the like. In the case of a Cn 〇 基 group, a propyl propyl group is preferred. Further, as described later, S species, a metal compound (M), and a decane compound (s2) are used. In the present invention, in the above-mentioned second step, a hydrolyzable group which is an alkoxy group or a halogen atom and a functional group of a hydroxyl group are used. (χ1, χ2) and two so-called bifunctional sinter compounds (S1) in one molecule [hereinafter referred to as bifunctional decane compound (S1)] The metal compound is reacted. It is recognized that 201229055 is a main chain in which a ruthenium atom of a bifunctional decane compound (S1) and a metal atom (Zr, Ti) are bonded through an oxygen atom in the first step. The amount of the metal compound (M) used in the first step is 3 times or less relative to the bifunctional decane compound (S1), and is relative to [the above formula (η)] and the above-mentioned bifunctional decane compound (S1). The ratio of "the total amount of use of the hydroxyl group in HA and the decane compound (S1)" to the total amount of the metal compound used is 〇.〇3 to 〇8 (mol ratio) [the above formula (iii)]. It is considered that the main chain is synthesized by reacting a bifunctional decane compound U with a metal compound (Μ) and, if necessary, under the conditions as described above, and finally the metal oxirane compound (A) is obtained. Good for 〇~9〇 Any of its / orphans will be easy to become liquid. It is possible to set the molar ratio of "the total amount of the base in the "Η" and "the total amount of the base in the bismuth compound (S i)" to the "the total amount of the difunctional decane compound (S1) and the metal compound (M)". Good range of 0.05~0.6, especially good 〇"~〇45. Then, in the second step, the reaction liquid obtained in the second step and the functional group (X) of the hydrolyzable group and the hydroxyl group which are 3 alkoxy groups or halogen atoms and one molecule are contained in one molecule. The monofunctional decane compound (S2) [hereinafter referred to as monofunctional decane compound (S2)] and, if desired, H2 ,, should be prepared in the second step from the side chain. A metal*oxygen compound obtained by burning a 7-base of the compound (S2). In the present month, the monofunctional decane compound (^2) is used in the same amount as or more than the number of moles of the hydrolyzable group remaining in the reaction liquid prepared in the first step. Ear number [the above formula (iv)]. The number of moles of the monofunctional alkylene group D (S2) is preferably 1.5 times or more of the number of hydrolyzable base moles remaining in the reaction liquid prepared in the second step, and further more -10-201229055 is preferably 2乜 Above. In step 2. , , ^ Ψ 由 由 使 使 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 早 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱 铱The residue of the decomposable group is minimal, and no liberated steroid is produced during hardening, and i Αι ” can obtain a metal oxoxane compound which can obtain a hardened material which is resistant to heat and yellowing. In the present invention, preparation 7 ^ 田g月The functional group of the decane compound (S1), which is either or both, is too complete - «··················································· H2 is used. Further, in the second step, when the functional group milk of the early-functional stone compound (S2) is a warp group, H2O may not be used. The first step and the first cow lock k. The reaction in the step can be carried out, for example, at 50 to 150 t, preferably 60 to 13 GX:, more preferably 6 G to just c. However, the dropping is preferably carried out at a temperature of, for example, _3 (rc or less. The reaction time in the above first step and the second step is also due to the reaction temperature, the type of decane compound and the metal compound used. The difference may be, for example, 1 minute to 10 hours, preferably 1 to 5 hours. The metal oxirane compound (A) produced in the above production method is preferably liquid at any temperature of 0 to 9 CTC. More preferably, it is preferably 〇30 at any temperature of 〇~7〇<t. (: liquid at any temperature. [2-functional decane compound (si)] used in the manufacture of the metal ruthenium of the present invention The bifunctional calcined compound (S 1 ) for the reaction of the oxyalkyl compound can be used in the following formula (1) R1

I X1 一 Si — X2 (1 \ I ) R2 -11- 201229055 (式中’ R丨,R2係相同或 本-片 。烯基、C6 14芳A : / 『虱原子、Ci,烷基、 ,表以芳烧基;χ1,χ2係㈣或不同 烷氧基、豳素原子或羥基) 表示’且從先相始—直使㈣製造^ 石夕氧烧等之周知的二炫氧…合物 物或二羥基矽烷化合物。 -南化矽烷化合 ?尤:甲之R ,R中的Cl,烷基而言 基、丙基、異丙基、丁基、異 ^甲基乙 美、P其、立甘 、及丁基、三級丁 Μ 1 癸基等;就^烯基而言, 烯基、烯丙基、2_丁稀基、2-戊烯基、:= 其而‘一 厥暴等,就 6-丨4方基而§ ,可列舉 言,可列舉节基等。 π基4 ’ ’洗。15芳烷基而 就上述式(1)中之xl,xy 甲氧基、乙氧12烷氧基而$,可列舉 G乳&、丙氧基、丁氧基犛. ,可列舉氟;f子Μ « ,就鹵素原子而言 書中,:=/、原子、漠原子等。另外,於本說明 、匕3個以上h_H鍵的矽烷化合物稱^tw扪 的矽烷化合物;將勺入“匆稱為「_ J 口初,將包含丨個以上乙烯基、 稀基的石夕烷化合物稱為「 丙基專C。。 不含住缸Q· 邓丞!」的矽烷化合物丨將 建及(:2」〇烯基的矽烷化合 矽烷化合物。 初稱為「其他」 就Η型二烷氧矽烷化合物 矽烷、二r I A J幻舉例如二甲氧基 一乙氧基矽烷、二丙氧基矽烷、二 々 含兩個氫原+__ 氧基石夕院等 。子之一 Cu烷氧矽烷化合物; 碎烧、甲基二乙氧…、甲 二-::基 夕说、乙基二甲氧基石夕烧、乙基二乙氧基石夕貌、 -12- 201229055I X1 -Si - X2 (1 \ I ) R2 -11- 201229055 (wherein R R, R 2 is the same or the present - alkene. Alkenyl, C6 14 aryl A: / "虱 atom, Ci, alkyl, , The formula is an aryl group; χ1, χ2 series (four) or different alkoxy groups, halogen atoms or hydroxyl groups) and 'from the first phase-to-four (4) to make ^ 夕 氧 oxygen burning, etc. Or dihydroxy decane compound. - Nanhua decane compound? Especially: R of R, R in R, alkyl, propyl, isopropyl, butyl, isomethylamine, P, gan, and butyl, Third-order butyl hydrazine 1 fluorenyl group; in the case of alkenyl group, alkenyl group, allyl group, 2-butylenyl group, 2-pentenyl group, := which is a violent storm, etc., 6-丨4 Square base and §, can be listed, can be listed as a basis. Π-base 4'' wash. The arylalkyl group and the x1, xy methoxy group and the ethoxy 12 alkoxy group in the above formula (1) may be exemplified by G emulsion & propoxy group; butoxybutane. f子Μ « , in the book of halogen atoms, :=/, atom, desert atom, etc. In addition, in the present description, 矽 化合物 化合物 匕 匕 h 化合物 化合物 化合物 化合物 化合物 化合物 化合物 ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; ; The compound is called "propyl-specific C. The decane compound which does not contain the cylinder Q·Deng Yu!" will be a decane-based decane compound of (2) nonenyl group. Alkoxy decane compound decane, di r IAJ magical action such as dimethoxy-ethoxy decane, dipropoxy decane, diterpenoid containing two hydrogenogens +__oxyxite, etc. Compound; calcined, methyldiethoxy..., formazan-:: icaine, ethyldimethoxy zebra, ethyldiethoxylate, -12- 201229055

乙基二丙氧基石夕烧、乙其__丁〆* A 基一丁乳基矽烷、丙基二曱氧基 矽烷、丙基二乙氧基矽俨 ^ w 乳丞 孔土夕烷、丙基二丙氧基矽烷、丙基二 丁氧基石夕烧、丁基二甲惫萁 T氧基矽烷、丁基二乙氧基矽烷、 丁基二丙氧基石夕烧、丁基- 丞一丁氧基矽烷、苯基二甲氧基 石夕烧、本基一乙氧基石夕炫、^且_工匕 沉本基一丙氧基矽烷、苯基二 丁氧基矽烷、萘基二甲氧其石贫诗 r轧基矽烷、萘基二乙氧基矽烷、 萘基二丙氧基石夕烧、萃美__ τθ 一丁乳基矽烷、苄基二曱氧基 碎烧、¥基一乙氧基硬炫_、宅耸-系甚β ^ ^ 卞基一丙氧基矽烷、节基二 丁氧基矽烷等含1個氫原子夕^ ^ 乳你于之一C〗-〗2烷氧矽烷化合物等。 就乙烯基型二烷氧矽烷化合物而言,可列舉例如二 (2 乙烯基二曱氧基矽烷、二烯丙基二曱氧基矽烷、 烯基)丙基二甲氧基矽烷、二(2_戊烯基)二甲氧基矽烷、 二乙稀基二乙氧基Μ、二稀丙基二乙氧基我、二(2_ 丁烯基)丙基二乙氧基矽烷、二(2_戊烯基)二乙氧基矽烷 、二乙烯基二丙氧基矽烷、二烯丙基二丙氧基矽烷、二 (2-丁烯基)丙基二丙氧基矽烷、二(2_戊烯基)二丙氧基矽 烷、一乙烯基二丁氧基矽烷、二烯丙基二丁氧基矽烷、 二(2-丁烯基)丙基二丁氧基矽烷、二(2_戊烯基)二丁氧基 石夕烧等二(:2.10烯基二Cm烷氧矽烷化合物;曱基乙稀基 二甲氧基矽烷、乙基乙烯基二甲氧基矽烷、丙基乙烯基 二甲氧基矽烷、丁基乙烯基二甲氧基矽烷、甲基乙烯基 二乙氧基矽烷、乙基乙烯基二乙氧基矽烷、丙基乙烯基 二乙氧基矽烷、丁基乙烯基二乙氧基矽烷、甲基烯丙基 二甲氧基矽烷、乙基烯丙基二甲氧基矽烷、丙基烯丙基 二甲氧基矽烧、丁基烯丙基二甲氧基矽烷、甲基烯丙基 -13- 201229055 二乙氧基矽烷、乙基烯丙基二乙氧基矽烷、丙基烯丙基 二乙氧基石夕烷、丁基烯丙基二乙氧基石夕烷等〇11〇烷^ C2-10烯基二Cu烷氧矽烷化合物;苯基乙烯基二曱氧基 矽烷'萘基乙烯基二甲氧基矽烷、苯基乙烯基二乙氧二 石夕烷、萘基乙稀基二乙氧基石夕烧、苯基乙稀基二丙氧^ 矽烷、萘基乙烯基二丙氧基矽烷、苯基乙烯基二丁氧美 矽烷、萘基乙稀基二丁氧基矽烷、笨基烯丙基二曱氧ς 矽烷、萘基烯丙基二甲氧基矽烷、苯基烯丙基二乙氧基 矽烷、萘基烯丙基二乙氧基矽烷、苯基烯丙基二丙氧基 矽烷、萘基烯丙基二丙氧基矽烷、笨基烯丙基二丁氧ς 矽烷、萘基烯丙基二丁氡基矽烷等C014芳基c2 烯基二 c!-!2烷氧矽烷化合物;苄基乙烯基二甲氧基矽烷、苄基 乙烯基二乙氧基矽烷、苄基乙烯基二丙氧基矽烷、苄基 乙烯基二丁氧基矽烷、节基烯丙基二甲氧基矽烷、苄基 烯丙基二乙氧基矽烷、苄基烯丙基二丙氧基矽烷、苄基 烯丙基二丁氧基矽烷等(:7七芳烷基q 1G烯基二CH2烷氧 矽烷化合物。 就其他二烷氧矽烷化合物而言,可列舉例如二甲基 二甲氧基錢、二乙基二甲氧基我、二丙基二曱氧基 石夕烧、二丁基二甲氧基钱、二甲基二乙氧基#、二 乙基二乙氧基矽烷、二丙基二乙氧基矽烷、二丁基二乙 氧基石夕洗、二甲基:丙氧基石夕院、二乙基二丙氧基 一 -丙基-丙氧基矽烷、二丁基二丙氧基矽烷、二甲基Ethyl dipropoxylate, Ethyl bromide, acetonyl decyl propyl decyl decane, propyl dimethoxy decane, propyl diethoxy hydrazine Dipropoxydecane, propyl dibutoxylate, butyl dimethyl hydrazine Toxy decane, butyl diethoxy decane, butyl dipropoxy sulphur, butyl - butyl Oxydecane, phenyl dimethoxy sulphur, base-ethoxy ethoxy sulphate, _ _ 匕 本 一 一 丙 丙 丙 丙 丙 丙, phenyl dibutoxy decane, naphthyl dimethoxy Shishishishi rolling decane, naphthyl diethoxy decane, naphthyl dipropoxy sulphur, smelting __ τθ butyl decyl decane, benzyl di decyl oxyhydrolysis, ¥ ethoxy Base hard _, house shrub - system very β ^ ^ thiol-propoxy decane, benzyl dibutoxy decane, etc. containing one hydrogen atom 夕 ^ ^ milk you in one C 〗 - 2 alkoxy decane Compounds, etc. The vinyl type dialkoxy oxane compound may, for example, be bis(2-vinyldimethoxy decane, diallyl decyloxydecane, alkenyl)propyldimethoxydecane, or two (2). _pentenyl) dimethoxy decane, diethylene diethoxy hydrazine, dipropyl propyl diethoxy I, bis (2-butenyl) propyl diethoxy decane, two (2 _ Pentenyl)diethoxydecane, divinyldipropoxydecane, diallyldipropoxydecane, bis(2-butenyl)propyldipropoxydecane, bis(2-penta) Alkenyl)dipropoxydecane, monovinyldibutoxydecane, diallyldibutoxydecane, bis(2-butenyl)propyldibutoxydecane, bis(2-pentene) Di(n-butoxylate) and other two (: 2.10 alkenyl di-Cm alkoxy oxane compounds; mercaptoethylene dimethoxy decane, ethyl vinyl dimethoxy decane, propyl vinyl dimethoxy Base decane, butyl vinyl dimethoxy decane, methyl vinyl diethoxy decane, ethyl vinyl diethoxy decane, propyl vinyl diethoxy decane, butyl vinyl diethoxy Base decane, methallyl dimethoxy decane, ethyl allyl dimethoxy decane, propylallyl dimethoxy oxime, butyl allyl dimethoxy decane, methyl Allyl-13- 201229055 diethoxy decane, ethyl allyl diethoxy decane, propyl allyl diethoxy oxane, butyl allyl diethoxy oxalate, etc. Decane^C2-10 alkenyl di-alkoxy oxane compound; phenylvinyl dimethoxy decane 'naphthylvinyl dimethoxy decane, phenyl vinyl diethoxy oxalate, naphthyl Dilute diethoxy sinter, phenylethylene dipropoxy decane, naphthyl vinyl dipropoxy decane, phenyl vinyl dibutoxymethane, naphthyl ethylene dibutoxy decane , stupidyl propylene dioxime decane, naphthyl allyl dimethoxy decane, phenyl allyl diethoxy decane, naphthyl allyl diethoxy decane, phenyl allyl C014 aryl c2 alkenyl c!-!2 alkane such as dipropoxydecane, naphthylallyldipropoxydecane, stupylallyl dibutoxynonane, naphthylallyldibutylidene decane Oxygen a compound; benzyl vinyl dimethoxy decane, benzyl vinyl diethoxy decane, benzyl vinyl dipropoxy decane, benzyl vinyl dibutoxy decane, benzyl propyl dimethoxy Basear, benzylallyldiethoxydecane, benzylallyldipropoxydecane, benzylallylbisbutoxydecane, etc. (7 7 heptaalkyl q 1G alkenyl di CH 2 alkane Oxidane compound. As the other dialkoxy oxane compound, for example, dimethyl dimethoxy money, diethyl dimethoxy, dipropyl dimethoxy oxy, dibutyl dimethyl Oxyl money, dimethyl diethoxy #, diethyl diethoxy decane, dipropyl diethoxy decane, dibutyl diethoxy scoline, dimethyl: propoxy XI Xiyuan , diethyldipropoxy-propyl-propoxydecane, dibutyldipropoxydecane, dimethyl

-'丁氧基吩检、-7 A ^ 一乙基二丁氧基矽烷、二丙基二丁氧基 石夕烧、二丁其-丁备甘 氧基矽烷等二CM0烷基二C丨.丨2烷氧矽 -14- 201229055 烷化合物;二苯基二甲氧基矽烷、二萘基二甲氧基矽烷 、二苯基二乙氧基矽烷、二萘基二乙氧基矽烷、二苯基 二丙氧基矽烷、二萘基二丙氧基矽烷、二苯基二丁氧基 矽烷、二萘基二丁氧基矽烷等二C6-M芳基二Cl.12烷氧矽 烷化合物;二苄基二曱氧基矽烷、二苄基二乙氧基矽烷 、二苄基二丙氧基矽烷、二苄基二丁氧基矽烷等二c7_15 芳烷基二Cl-12烷氧矽烷化合物;曱基苯基二甲氧基矽烷 、乙基苯基二甲氧基矽烷、丙基苯基二〒氧基矽烷、丁 基苯基二曱氧基矽烷、甲基苯基二乙氧基矽烷、乙基苯 基二乙氧基矽烷、丙基苯基二乙氧基矽烷、丁基苯基二 乙氧基矽烷、甲基萘基二甲氧基矽烷、乙基萘基二曱氧 基矽烷、丙基萘基二甲氧基矽烷、丁基萘基二甲氧基矽 烷、甲基萘基二乙氧基矽烷、乙基萘基二乙氧基矽烷、 丙基萘基二乙氧基矽烷、丁基萘基二乙氧基矽烷等 烷基C6_ Η芳基二cu!2烷氧矽烷化合物;曱基苄基二甲氧 基矽烷、乙基苄基二曱氧基矽烷'丙基苄基二曱氡基矽 烷、丁基节基二甲氧基矽烷、甲基节基二乙氧基矽=、 乙基苄基二乙氧基矽烷、丙基苄基二乙氧基矽烷、丁基 苄基二乙氧基矽烷等烷基芳烷基二(^心烷 烷化合物等。 就Η型二鹵化矽烷化合物而言,可列舉例如二氟矽烷 、二氣矽烷、二溴矽烷等含兩個氫原子之二_化矽烷化 合物;二氟甲基矽烷、二氣曱基矽烷、二溴曱基矽烷、 二氟乙基矽烷、二氣乙基矽烷、二溴乙基矽烷、二氟丙 基矽烷、二氣丙基矽烷、二溴丙基矽烷、二氟丁基矽烷 -15- 201229055 、一乳丁基石夕、p A 况、二溴丁基矽烷、二氟苯基矽烷、二氣 本基矽烷、二溴〜 τ 兴本基矽烷、二氟萘基矽烷、二氣萘基矽 烷、二溴苯其& & ’ 土夕烷、氟苄基矽烷、二氣苄基石夕烷、二漠 卞基矽烷等含= 、 個虱原子之二_化矽烷化合物等。 就乙烯基裀_ 1一 _化矽烷化合物而言,可列舉例如二 氟二乙烯基矽焓、_ 一 ^ 於 一氣一乙稀基石夕烧、二漠二乙稀基石夕 2 氟一烯丙基矽烷、二氣二烯丙基矽烷、二溴二烯 丙基矽烷、二·_μ 俨 _ 氟一(2_ 丁烯基)矽烷、二氣二(2-丁烯基)矽 、: /臭—(2· 丁烯基)矽烷、二氟二(2-戊烯基)矽烷、二 二二(2-戊稀基)石夕烧、二漠二(2_戊烯基)石夕院等二齒化二 no烯基♦烧化合物;二氣甲基乙烯基⑦烧、二氣乙基 俨烯土夕烷、—氟丙基乙烯基矽烷、二氟丁基乙烯基矽 元—氣曱基乙烯基矽烷、二氯乙基乙烯基矽烷、二氣 土乙烯基矽烷、二氣丁基乙烯基矽烷、二溴甲基乙烯 基石夕檢、一、、白1 4+ _ 一 /臭乙基乙烯基矽烷、二溴丙基乙烯基矽烷、 一溴丁基乙烯基矽烷、二氟甲基烯丙基矽烷、二氟乙基 烯丙基矽烷、二氟丙基烯丙基矽烷、二氟丁基烯丙基矽 烷一氣甲基烯丙基矽烷、二氯乙基烯丙基矽烷、二氯 基烯丙基矽烷、二氣丁基烯丙基矽烷二溴甲基烯丙 土矽烷、二溴乙基烯丙基矽烷、二溴丙基烯丙基矽烷、 2溴丁基烯丙基矽烷等二鹵化Cl_1Q烷基Cm烯基矽烷化 σ物,二氟苯基乙烯基矽烷、二氟萘基乙烯基矽烷、二 氯苯基乙烯基矽烷、二氯萘基乙烯基矽烷、二溴苯基乙 烯基矽烷、二溴萘基乙烯基矽烷、二氟苯基烯丙基矽烷 、一氟萘基烯丙基矽烷、二氣苯基烯丙基矽烷、二氯萘 -16 - 201229055 =!:c 丙基秒燒、二漠萘基烯丙基 乙“埽基μ化合物;…基 广基夕烧、…基乙稀基石夕燒、二㈣基乙婦基石夕 =二氟卡基稀丙基石夕烧、二氣节基稀丙基石夕院、二演 =稀丙基錢等二_C7.15芳貌基C21G稀基Μ化合 物專。 就其他二齒化石夕烷化合物而言,可列舉例如二氟二 甲基石夕院、二氯二甲基找、二漠二甲基#、二氣二 乙基矽烷、二氯二乙基矽烷、二溴二乙基矽烷、二敗二 两基妙丙基Μ、:漠:丙基耗、二氣二 丁基石夕烧、二氯二丁基我、二演二丁基耗等二函化 二匚,.1()烷基矽烷化合物;二氟二笨基矽烷、二氯二苯基 石夕烧、二漠二苯基我、三氟二萘基錢、:氣二蔡基 矽烷、二溴二萘基矽烷等二鹵化二c0 i4芳基矽烷化合物 :—氟二苄基矽烷、二氯二苄基矽烷、二溴二苄基矽烷 等二齒化二C^5芳烷基矽烷化合物;二氟曱基苯基矽烷 、二氟乙基苯基矽烷、二氟丙基笨基矽烷、二氟丁基苯 基矽烷、二氣曱基苯基矽烷、二氯乙基苯基矽烷、二氯 内基苯基石夕烧、二氣丁基苯基矽烷、二溴曱基萘基矽烷 、二溴乙基萘基矽烷、二溴丙基萘基矽烷、二溴丁基萘 基石夕院4二齒化Cuo院基c:6—,4芳基石夕烧化合物;二氟甲 基节基矽烷、二氟乙基苄基矽烷、二氟丙基苄基矽烷、 一氟丁基节基矽烷、二氣曱基节基矽烷、二氯乙基苄基 砂烷、二氯丙基苄基矽烷、二氯丁基苄基矽烷、二溴曱 基苄基矽烷、二溴乙基节基矽烷 '二溴丙基苄基矽烷、 -17- 201229055 二漠丁基苄基矽烷等二商化c 合物等。 1-10院基C"7_丨5芳烧基石夕烧化 就Η型二羥基矽烷化合物而言,可列舉例如二羥基矽 烷(含兩個氫原子);甲基二羥基矽烷、乙基二羥基矽烷 、丙基二羥基矽烷、丁基二羥基矽烷、苯基二羥基矽烷 、萘基二羥基矽烷、苄基二羥基矽烷等含1個氫原子之二 羥基矽烷化合物。 就乙烯基型二羥基矽烷化合物而言,可列舉例如二 乙烯基二羥基矽烷、二烯丙基二羥基矽烷、二(2 丁烯基 )二羥基矽烷、二(2_戊烯基)二羥基矽烷等二C21Q烯基二 經基梦院化合物;甲基乙職4基錢、乙基乙稀基 二羥基矽烷、丙基乙烯基二羥基矽烷、丁基乙烯基二羥 基矽烷、甲基烯丙基二羥基矽烷、乙基蝉丙基二羥基矽 烷、丙基烯丙基二羥基矽烷、丁基烯丙基二羥基矽烷等 烷基C:2⑴烯基二羥基矽烷化合物;苯基乙烯基二羥 基矽烷、萘基乙烯基二羥基矽烷、苯基烯丙基二羥基矽 院、萘基稀丙基二經基石夕烧fc614芳紅210稀基二經基 矽烷化合物;节基乙烯基二羥基矽烷、苄基烯丙基二羥 基矽烷等c^5芳烷基C2_1()烯基二羥基矽烷化合物等。 就其他二録钱化合物而言,可列舉例如二甲基 二經基我、二乙基二經基#、二丙基二經基石夕烧、 二丁基二羥基矽烷等二Cm。烷基二羥基矽烷化合物丨二 苯基二經基錢、二蔡基二經基石夕燒等二c⑷芳基二經 基矽烷化合物;二节基二羥基矽烷等二C7i5芳烷基二羥 基石夕烧化合物]基苯基二經基錢、乙基苯基二經基 -18- 201229055 矽烷、丙基苯基二羥基矽烷、丁基笨基二羥基矽烷、曱 基萘基二録錢、乙基萘基二隸錢、丙基蔡基二 羥基矽烷、丁基萘基二羥基矽烷等Ci,烷基Gw芳基二 經基石夕烧化合物;甲基$基二録錢、乙基f基二經 土夕烷丙基苄基一羥基矽烷、丁基苄基二羥基矽烷等 c,-10烷基c^5芳烷基二羥基矽烷等。就矽烷化合物(S1) 而言,上述例示之化合物可單獨使用或混合兩種以上使 用。 就矽烷化合物(S1)中之作為上述式(1)中的Rl,R22- 'Butoxy phenanthrene, -7 A ^ ethyl dibutoxy decane, dipropyl dibutoxy sulphide, dibutyl butyl butyl ethoxy decane, etc.丨2 alkoxy 矽-14- 201229055 alkyl compound; diphenyl dimethoxy decane, dinaphthyl dimethoxy decane, diphenyl diethoxy decane, dinaphthyl diethoxy decane, diphenyl a di-C6-M aryldiCl.12 alkoxy oxane compound such as bispropoxydecane, dinaphthyldipropoxydecane, diphenyldibutoxydecane or dinaphthyldibutoxydecane; a di-c7-15 aralkyl di-Cl-12 alkoxy oxane compound such as benzyl dimethoxy decane, dibenzyl diethoxy decane, dibenzyl dipropoxy decane or dibenzyl dibutoxy decane; Phenyl dimethoxy decane, ethyl phenyl dimethoxy decane, propyl phenyl dimethoxy decane, butyl phenyl dimethoxy decane, methyl phenyl diethoxy decane, B Phenyl phenyl diethoxy decane, propyl phenyl diethoxy decane, butyl phenyl diethoxy decane, methyl naphthyl dimethoxy decane, ethyl naphthyl dimethoxy decane, C Naphthyl Methoxydecane, butylnaphthyldimethoxydecane, methylnaphthyldiethoxydecane, ethylnaphthyldiethoxydecane, propylnaphthyldiethoxydecane,butylnaphthyl An alkyl C6_ arylaryl di cu! 2 alkoxy oxane compound such as ethoxy decane; decyl benzyl dimethoxy decane, ethyl benzyl dimethoxy decane 'propyl benzyl dinonyl decane, Butyl benzyl dimethoxy decane, methyl benzyl diethoxy oxime =, ethyl benzyl diethoxy decane, propyl benzyl diethoxy decane, butyl benzyl diethoxy decane An alkyl aralkyl bis(cyclohexane) compound or the like. Examples of the quinone dihalogenated decane compound include dihydrogenated decane having two hydrogen atoms such as difluorodecane, dioxane or dibromodecane. a compound; difluoromethyl decane, dioxadecane decane, dibromodecyl decane, difluoroethyl decane, dioxoethyl decane, dibromoethyl decane, difluoropropyl decane, di-propyl propyl decane, Dibromopropyl decane, difluorobutyl decane-15- 201229055, monobutyl butyl oxalate, p A condition, dibromobutyl decane, difluorophenyl decane, two Benyl decane, dibromo~τ Xingbenyl decane, difluoronaphthyl decane, dinaphthyl decane, dibromobenzene, && 'oxalin, fluorobenzyl decane, dibenzyl benzyl oxacyclohexane,卞 矽 矽 矽 等 含 含 、 、 、 、 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 。 Ethyl sulphate, sulphate, sulphate, sulphate, difluoro diallyl decane, dibromo diallyl decane, di- _μ 俨 _ fluoro-(2-butenyl) ) decane, di-di(2-butenyl) fluorene, : / odor - (2 · butenyl) decane, difluoro bis (2-pentenyl) decane, di-di(2-pentyl) Two-toothed two-alkenyl-burning compounds such as Shi Xizhuo, Er Mo Er (2_pentenyl), Shi Xiyuan, etc.; two-gas methyl vinyl 7-burning, di-n-ethyl decene, and fluorene Propyl vinyl decane, difluorobutyl vinyl fluorene - gas fluorenyl vinyl decane, dichloroethyl vinyl decane, di-glycol vinyl decane, di-butyl butyl vinyl decane, dibromomethyl Alkenyl stone test, one, white 1 4+ _ a / stinking ethyl vinyl decane, dibromopropyl vinyl decane, monobromobutyl vinyl decane, difluoromethyl allyl decane, difluoroethyl Allyl decane, difluoropropyl allyl decane, difluorobutyl allyl decane mono methallyl decane, dichloroethylallyl decane, dichloroallyl decane, two gas Dihalogenated Cl_1Q alkyl Cm alkenyl such as butyl allyl decane dibromomethyl allybendane, dibromoethyl allyl decane, dibromopropylallyl decane, 2 bromobutyl allyl decane矽 alkylated σ, difluorophenyl vinyl decane, difluoronaphthyl vinyl decane, dichlorophenyl vinyl decane, dichloronaphthyl vinyl decane, dibromophenyl vinyl decane, dibromo naphthyl ethylene Base decane, difluorophenyl allyl decane, monofluoronaphthyl allyl decane, di-phenyl phenyl allyl decane, dichloronaphthalene-16 - 201229055 =!: c propyl second burn, dioxin naphthyl Allyl B "mercapto-μ compound; ... base broad-based kiln, ... vinylidene base shovel, bis (tetra)-based ethylglycosyl sulphate = difluoro-kappa propyl sulphate Burning, di integrity propoxy group dilute cornerstone Xi hospital, the play money = thin n-propyl group and other two _C7.15 appearance aryl group Μ C21G diluted compound specifically. Examples of other bidentate compound compounds include, for example, difluorodimethyl shi xiyuan, dichloro dimethyl hydride, dimethyl dimethyl ketone, dioxetane hexane, and dichlorodiethyl decane. , dibromodiethyl decane, di-n-bis-di-m-propyl propyl hydrazine,: desert: propyl consumption, di-n-butyl dibutyl sulphate, dichlorodibutyl I, di-dibutyl consumption, etc. Diterpenoid, .1 () alkyl decane compound; difluorodiphenyl decane, dichlorodiphenyl sulphur, dimo-diphenyl, trifluorodinaphthyl, dioxin, dibromo Dihalogenated di c0 i4 aryl decane compound such as dinaphthyl decane: a bidentate di-C 2 aralkyl decane compound such as fluorodibenzyl decane, dichlorodibenzyl decane or dibromodibenzyl decane; Fluorinyl phenyl decane, difluoroethyl phenyl decane, difluoro propyl decyl decane, difluoro butyl phenyl decane, di-p-phenylphenyl decane, dichloroethyl phenyl decane, dichloro Phenyl sulfonate, di-butyl butyl decane, dibromodecylnaphthyl decane, dibromoethylnaphthyl decane, dibromopropylnaphthyl decane, dibromobutylnaphthyl sylvestre 4 Toothed Cuo Institute c: 6-, 4 aryl sulphur compound; difluoromethyl benzyl decane, difluoroethyl benzyl decane, difluoropropyl benzyl decane, monofluorobutyl decyl decane, two Gas fluorenyl decyl decane, dichloroethyl benzyl sane, dichloropropyl benzyl decane, dichlorobutyl benzyl decane, dibromodecyl benzyl decane, dibromoethyl decyl decane 'dibromo Divalent benzyl decane, -17- 201229055 di-dibutylbenzyl decane, etc. 1-10 院基基 C"7_丨5 芳烧石石化化 Although the oxime-type dihydroxy decane compound, for example, dihydroxy decane (containing two hydrogen atoms); methyl dihydroxy decane, ethyl dihydroxy A dihydroxydecane compound containing one hydrogen atom such as decane, propyl dihydroxy decane, butyl dihydroxy decane, phenyl dihydroxy decane, naphthyl dihydroxy decane or benzyl dihydroxy decane. The vinyl type dihydroxy decane compound may, for example, be divinyl dihydroxy decane, diallyl dihydroxy decane, bis (2 butyl) dihydroxy decane or bis (2-pentenyl) dihydroxy group. Di-C21Q alkenyl dimethyst compound such as decane; methyl group 4 eq., ethyl ethylene dihydroxy decane, propyl vinyl dihydroxy decane, butyl vinyl dihydroxy decane, methyl ally Alkyl C: 2 (1) alkenyl dihydroxy decane compounds such as dihydroxy decane, ethyl propyl propyl dihydroxy decane, propyl allyl dihydroxy decane, butyl allyl dihydroxy decane; phenyl vinyl dihydroxy Decane, naphthylvinyl dihydroxy decane, phenylallyl dihydroxy fluorene, naphthyl propyl dimethacrylate, fc614 aromatic red 210 dibasic decane compound; benzyl vinyl dihydroxy decane, A c^5 aralkyl C2_1() alkenyl dihydroxydecane compound such as benzylallyldihydroxydecane. The other two-money compound may, for example, be a dimethyl group such as dimethyldithiol, diethyldiyl#, dipropyldiyl sulphate or dibutyldihydroxydecane. Alkyl dihydroxy decane compound 丨diphenyl dipyridyl, dica aryl dipyridyl sulphate and the like c (4) aryl dipyridyl decane compound; di-block dihydroxy decane and other two C7i5 aralkyl dihydroxy sulphur Burning compound] phenyl phenyl dipyridyl, ethyl phenyl diionyl-18- 201229055 decane, propyl phenyl dihydroxy decane, butyl phenyl dihydroxy decane, decyl naphthyl diphthyl, ethyl Na, such as naphthyl dihydrogen, propyl decyl dihydroxy decane, butyl naphthyl dihydroxy decane, alkyl Gw aryl dichrox sulphate compound; methyl group 二 two recorded money, ethyl f group di C, 10-alkyl c^5 aralkyl dihydroxy decane, etc., such as oxacyclopropylbenzyl monohydroxy decane, butyl benzyl dihydroxy decane, and the like. In the case of the decane compound (S1), the above-exemplified compounds may be used singly or in combination of two or more. As the decane compound (S1), R1, R22 in the above formula (1)

Cmo烧基而言,特佳為^5烷基,就C2,稀基而言’,特 佳為C2_5烯基。就Ri,R、f ’基於耐熱無黃變之點,較 佳為甲基、乙基、苯基、乙烯基、烯丙基。又基於耐水 解性之點,更佳為苯基。 就上述式(1)中之χ1,χ2中的Ci i2烷氡基而言特佳為 C』氧基。京尤上述χι,χ2而言,基於取得性之點,較佳 二认二基乙氧基、氣原子、溴原+、羥基,基於反應 則的安定性之點,更佳為甲氧基、乙氧基。 就矽烷化合物(S1)而言,在上述之中,具體上較佳為 :1-U烷基二〇1.12烷氧矽烷(進一步為二Ci 5烷基二 烷氧矽烷)、二C6_M芳基二C1烷氧矽烷(進一步為二笨基 :烷氧矽烷),尤其可適合使用二甲基二甲氧基矽烷 其:乙基二曱氧基矽烷、二苯基二甲氧基矽烷、二乙烯 土一曱氧基矽烷、二烯丙基二曱氧基矽烷、二甲基二乙 氧:矽烷、二乙基二乙氧基矽烷、二笨基二乙氧基矽烷 、二乙歸基二乙氧基矽烷或二烯丙基二乙氧基矽烷。 -19- 201229055 [單官能之矽烷化合物(S2)] 。。使用於製造本發明之金屬矽氧烷化合物(a)的反應 之單S忐之^夕烷化合物(S2),可使用以下列式 Γζ X3 — Si — R5 I (3) R4 ^式中,R3〜R5係相同或不同,表示氫原子、Cm。烷基、 2-^稀基、C6_M芳基或q 1S芳烷基;X3表示烷氧基 、齒素原子或羥基) 表:且從先前開始—直使用於製造聚矽氧烷、聚金屬 :氧烷等之周知的單烷氧矽烷化合物、單齒化矽烷化合 物或單羥基矽烷化合物。 其。上弋中之R〜R中的C!-丨〇炫基、C2-丨0烯基、c6M芳 :或C7·15芳烷基而言,可使用於上述2官能之矽烷化合物 而一 1下马R 、R者。就X3中的Ci-10烷氧基、鹵素原子 3,可使用於上述矽烷化合物(S1)中例示作為χ1,χ2者 产就Η型單烷氧矽烷化合物而言,可列舉例如曱氧基矽 儿乙氧基矽烷、丙氧基矽烷、丁氧基矽烷等含3個氫原 之烷氧矽烷化合物;曱基曱氧基矽烷、曱基乙 、田甘 τ基丙氧基矽烷、甲基丁氧基矽烷、乙基甲氧 \ τ ^ 己基乙氧基矽烷、乙基丙氧基矽烷、乙基丁羞 基石夕、检、;t « ^ 丙基甲氧基矽烷、丙基乙氧基矽烷、丙基丙氧 土矽烷、丙基丁氧基矽烷、丁基甲氧基矽烷、丁基乙 基石夕、拉、 ^ 丁基丙氧基矽烷、丁基丁氧基矽烷、苯基甲氧 -20- 201229055 基石夕烧、苯基乙惫|石^ 虱丞矽烷、本基丙氧基矽烷、苯基丁氧 基石夕烧、萘基甲氣I石々、P ^ ^ 丞矽烷、萘基乙氧基矽烷、萘基丙氧 基矽烷、萘基丁氧基矽烷、苄基甲氧基矽烷、苄基乙氧 基矽烷、卞基丙氧基矽烷'苄基丁氧基矽烷等含兩個氫 原子之。丨-12烷氧矽烷化合物;二甲基甲氧基矽烷、二乙 基曱氧基矽 基碎 基丙 、 —一- 基梦 C 丨-1 2 、二 基碎 基丁 烷; 氧基 芳烷 乙烯 氧基 、 — 基丁 二乙 二乙 ‘、一丙基甲氧基矽烷、二丁基甲氧基矽烷 甲基乙氧基矽烷、二乙基乙氧基矽烷、二丙基乙氧 烷、- 丁基乙氧基矽烷、=甲基丙氧基矽烷、二乙 氧基石夕烧、二丙基丙氧基⑦炫、二τ基丙氧基石夕烧 甲基丁氧基矽烷、1乙基丁氧基矽烷、〕丙基丁氧 烷L二丁基丁氧基矽烷等含丨個氫原子之二Ci iQ烷基 :烷氧矽烷,二苯基〒氧基矽烷、二萘基甲氧基矽烷 笨基乙氧基矽烷、二萘基乙氧基矽烷、二苯基丙氧 烷 '一奈基丙氧基矽烷、二苯基丁氧基矽烷、二萘 氧基矽烷等含1個氫原子之二C6_M芳基cN12烷氧矽 二节基甲氧基石夕烧、二节基乙氧基妙烧、二节基丙 夕烧一苄基丁氧基石夕烧等含1個氫原子之二c7_15 基c丨-丨2烷氧矽烷等。 就乙稀基型單烧氧♦烧化合物而言,可列舉例如三 基甲氧基矽烷、三乙烯基乙氧基矽烷、三乙烯基丙 矽烷、二乙烯基丁氧基矽烷、三烯丙基甲氧基矽烷 烯丙基乙氧基矽烷、三烯丙基丙氧基矽烷、三烯丙 氧基矽烷等二Cno烯基C!-!2烷氧矽烷化合物;曱基 烯基甲氧基矽烷、甲基二乙烯基乙氧基矽烷、甲基 烯基丙氧基矽烷、甲基二乙烯基丁氧基矽烷、乙基 -21 - 201229055 二乙烯基甲氧基矽烷、乙基二乙烯基乙氧基矽烷、乙基 二乙烯基丙氡基矽烷、乙基二乙烯基丁氧基矽烷、丙基 二乙稀基曱氧基矽烷、丙基二乙烯基乙氧基矽烷、丙基 二乙稀基内氧基矽烷、丙基二乙烯基丁氧基矽烷、丁基 二乙烯基曱氧基矽烷、丁基 二乙烯基丙氧基矽烷、丁基 二烯丙基甲氧基矽烷、曱基 二烯丙基丙氧基矽烷、甲基 二烯丙基甲氧基矽烷、乙基 二烯丙基两氧基矽烧、乙基 二烯丙基甲氧基矽烷、丙基 二烯丙基两氧基矽烷、丙基 二烯丙基甲氧基石夕烷、丁基 二烯丙基丙氧基矽烷、丁基 炫基二c2.1Q烯基Cl_12烷氧矽 氧基矽烷、苯基二乙烯基乙 氧基矽炫、苯基二乙烯基丁 氧基矽烧、萘基二乙烯基乙 氧基矽烷、萘基二乙烯基丁 氧基矽烷、苯基二烯丙基乙 氧基矽烷、苯基二烯丙基丁 氧基矽烷、萘基二烯丙基乙 氧基矽烧、萘基二烯丙基丁 稀基Ci-i2燒氧石夕院;苄基二 乙婦基乙氧基石夕烧、节基二 一乙缔基乙氧基石夕炫、丁基 二乙烯基丁氧基矽烷、曱基 二烯丙基乙氧基矽烷、曱基 一烯丙基丁氧基石夕烧、乙基 二烯丙基乙氧基矽烷、乙基 二烯丙基丁氧基石夕烧、丙基 二稀丙基乙氧基矽烷、丙基 二烯丙基丁氧基矽烷、丁基 二稀丙基乙氧基矽烷、丁基 二稀丙基丁氧基矽烷等(:卜10 院化合物;苯基二乙烯基甲 氧基石夕烷、苯基二乙烯基丙 氧基石夕烷、萘基二乙烯基甲 氧基石夕烷、萘基二乙烯基丙 氧基石夕貌、苯基二烯丙基甲 氧基矽烷、苯基二烯丙基丙 氧基矽烷、萘基二烯丙基甲 氧基矽烷、萘基二烯丙基丙 氧基矽烷等Q-U芳基二c2-丨〇 乙烯基甲氧基矽烷、苄基二 乙烯基丙氧基矽烷、苄基二 -22- 201229055 乙烯基丁氧基矽烷、节基二烯丙基甲氧基矽烷、苄基 烯丙基乙氧基矽烷、苄基二烯丙基丙氧基矽烷、苄基 烯丙基丁氧基矽烷等c^5芳烷基二C2-i〇烯基Cii2烷氧矽 烷化合物等。 就 乙 稀 基 型 單 例如 二 甲 基 乙 稀 基 烷、 丙 基 乙 烯 基 烷、 二 Ψ 基 乙 稀 基 烷、 二 丙 基 乙 烯 基 烷、 二 曱 基 乙 稀 基 烷、 •—" 丙 基 乙 稀 基 烷、 '* 曱 基 乙 烯 基 烧' 二 丙 基 乙 烯 基 烷、 二 甲 基 烯 丙 基 烧、 丙 基 '烯 丙 基 院、 二 甲 基 稀 丙 基 烷、 — 丙 基 烯 丙 基 烷、 — 甲 基 稀 丙 基 烷、 '- 丙 基 稀 丙 基 烷、 二 甲 基 稀 丙 基 烧、 二 丙 基 烯 丙 基 烷等 二 C, -10 烷 基 c2 乙烯 基 甲 氧 基 矽 烧 乙烯基乙氧基石夕烧 乙稀基丙氧基石夕烧 貌氧石夕烧化合物而 甲氧基矽烷、二乙 甲氧基石夕烧、二丁 乙氧基石夕烧、二乙 乙氧基石夕烧、二丁 丙氧基石夕烧、二乙 丙氧基矽烷、二丁 丁氧基石夕烧、二乙 丁氧基石夕院、二丁 曱氧基矽烷、二乙 甲氧基矽烷、二丁 乙氧基石夕院、二乙 乙氧基碎院、二丁 丙氧基矽烷、二乙 丙氧基矽烷、二丁 丁氧基矽烷、二乙 丁氧基矽烷、二丁 -ίο稀基C!」2烧氡石夕 、二萘基乙稀基甲 言’進一步可列舉 基乙烯基甲氧基矽 基乙烯基甲氧基矽 基乙細基乙氧基梦 基乙烯基乙氧基矽 基乙烯基丙氧基矽 基乙烯基丙氧基石夕 基乙烯基丁氧基矽 基乙烯基丁氧基矽 基烯丙基甲氧基矽 基烯丙基甲氧基矽 基烯丙基乙氧基石夕 基稀丙基乙氧基碎 基烯丙基丙氧基矽 基稀丙基丙氧基碎 基細丙基丁乳基碎 基稀丙基丁,基碎 烷化合物;二苯基 氧基矽烷、二苯基 二萘基乙烯基乙氧基矽烷、二苯基 二萘基乙烯基丙氧基矽烷、二苯基 -23- 201229055 乙烯基丁氧基矽烷 萘基乙烯基丁氧基矽烷、二苯基The Cmo alkyl group is particularly preferably a C5 alkyl group, and is preferably a C2_5 alkenyl group for C2 and a dilute group. In the case where Ri, R, and f' are based on heat-resistant and non-yellowing, a methyl group, an ethyl group, a phenyl group, a vinyl group, and an allyl group are preferable. Further, based on the point of resistance to hydrolysis, it is more preferably a phenyl group. With respect to the oxime 1 in the above formula (1), the Ci i2 alkyl fluorenyl group in oxime 2 is particularly preferably a C oxime group. In the above-mentioned χι, χ2, based on the acquisition point, it is preferable to recognize the di-ethoxy group, the gas atom, the bromine source, and the hydroxyl group, and it is more preferably a methoxy group based on the stability of the reaction. Ethoxy. With respect to the decane compound (S1), among the above, specifically, it is preferably: 1-U alkyldioxane 1.12 alkoxy decane (further diCi 5 alkyl dialkoxy oxane), di C6_M aryl group II C1 alkoxy oxane (further a di-phenyl: alkoxy decane), especially suitable for the use of dimethyl dimethoxy decane: ethyl dimethoxy decane, diphenyl dimethoxy decane, divinyl hydride Monodecyloxydecane, diallyl decyloxydecane, dimethyldiethoxy:decane, diethyldiethoxydecane, diphenyldiethoxydecane, diethylaminodiethoxy Alkane or diallyldiethoxydecane. -19- 201229055 [Monofunctional decane compound (S2)]. . The monosulfonium compound (S2) used in the production of the metal oxoxane compound (a) of the present invention can be used in the following formula: X3 - Si - R5 I (3) R4 where R3 ~R5 is the same or different and represents a hydrogen atom and Cm. Alkyl, 2-(diethyl), C6_M aryl or q 1S aralkyl; X3 represents alkoxy, dentate or hydroxy) Table: and from the beginning - used directly in the manufacture of polyoxanes, polymetals: A well-known monoalkoxydecane compound, monodentate decane compound or monohydroxydecane compound such as oxane. its. In the above-mentioned R~R, C!-oxime group, C2-丨0 alkenyl group, c6M aryl group or C7.15 aralkyl group can be used for the above-mentioned bifunctional decane compound. R, R. The Ci-10 alkoxy group and the halogen atom 3 in the above-mentioned decane compound (S1) can be exemplified as the oxime type 1 and the oxime type 2 is produced by the oxime type monoalkoxydecane compound. a three-hydrogen alkoxydecane compound such as ethoxylated decane, propoxy decane or butoxy decane; fluorenyl decyl decane, decyl ethane, tiangan tau propoxy decane, methyl butyl Oxy decane, ethyl methoxy τ hexyl ethoxy decane, ethyl propoxy decane, ethyl butyl sulfoxide, t; t « ^ propyl methoxy decane, propyl ethoxy decane , propyl propoxy decane, propyl butoxy decane, butyl methoxy decane, butyl ethyl oxalate, lat., butyl methoxy decane, butyl butoxy decane, phenyl methoxy-20- 201229055 基石夕烧, phenylacetamone|stone^ decane, benzyl propoxy decane, phenylbutoxyxanthene, naphthylmethyl sulphate, P ^ ^ decane, naphthyl ethoxy Decane, naphthylpropoxydecane, naphthylbutoxydecane, benzylmethoxydecane, benzyl ethoxy decane, mercaptopropoxy decane 'benzyl Butoxy oxane or the like contains two hydrogen atoms.丨-12 alkoxy oxane compound; dimethyl methoxy decane, diethyl decyl decyl propyl propyl, — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — — Vinyloxy, —butyl diethylene di', monopropyl methoxy decane, dibutyl methoxy decane methyl ethoxy decane, diethyl ethoxy decane, dipropyl ethoxy hydride, - butyl Ethyl ethoxy decane, = methyl propoxy decane, diethoxy sulphur, dipropyl propoxy 7 s, di τ propyl propoxy sulphate methyl butoxy decane, 1 ethyl butoxy a di-Ci iQ alkyl group containing a hydrogen atom such as a decane, a propyl butyl oxane, a dihydrogen decyl oxane or the like: an alkoxy decane, a diphenyl decyloxy decane, a dinaphthyl methoxy decane a ethoxylated decane, a dinaphthyl ethoxy decane, a diphenylpropoxy oxane-n-n-propoxy decane, a diphenylbutoxy decane, a dinaphthyloxydecane, etc. C6_M aryl cN12 alkoxy fluorenyl bis- methoxy oxysulfan, bis- ethoxy ethoxylate, bis- cyanosine, benzylbutoxybutane, etc., containing two hydrogen atoms, two c7-15 bases C丨-丨2 alkoxy oxane and the like. Examples of the ethylene-based mono-smoke-oxygen compound include, for example, trimethoxymethoxydecane, trivinylethoxysilane, trivinylpropane, divinylbutoxydecane, and triallyl. a di-Cno-alkenyl C!-!2 alkoxy oxane compound such as methoxy decyl allyl ethoxy decane, triallyl propoxy decane or triallyloxy decane; decyl alkenyl methoxy decane , methyl divinyl ethoxy decane, methyl alkenyl propoxy decane, methyl divinyl butoxy decane, ethyl-21 - 201229055 divinyl methoxy decane, ethyl divinyl ethene Oxy decane, ethyl divinyl propyl decane, ethyl divinyl butoxy decane, propyl diethylene decyl decane, propyl divinyl ethoxy decane, propyl diethylene Vinoxy decane, propyl divinyl butoxy decane, butyl divinyl decyl decane, butyl divinyl propoxy decane, butyl diallyl methoxy decane, fluorenyl Allyl propoxy decane, methyl diallyl methoxy decane, ethyl diallyl dioxy oxime, ethyl two Propyl methoxy decane, propyl diallyl methoxy decane, propyl diallyl methoxy oxa alkane, butyl diallyl propoxy decane, butyl hexyl c2.1Q ene Base Cl_12 alkoxy methoxy decane, phenyl divinyl ethoxy oxime, phenyl divinyl butoxy oxime, naphthyl divinyl ethoxy decane, naphthyl divinyl butoxy decane , phenyl diallyl ethoxy decane, phenyl diallyl butoxy decane, naphthyl diallyl ethoxy oxime, naphthyl diallyl butyl Ci-i 2 oxyn夕院; benzyl diethoxylate ethoxylate, stilbene di-ethyl ethoxy oxime, butyl divinyl butoxy decane, decyl diallyl ethoxy decane, hydrazine 1,1-Allyl butoxybutane, ethyl diallyl ethoxy decane, ethyl diallyl butoxylate, propyl dipropyl ethoxy decane, propyl dially Butyoxy decane, butyl dipropyl ethoxy decane, butyl dipropyl butyl decane, etc. (: Bu 10 compound; phenyl divinyl methoxy oxa alkane, benzene Divinylpropoxy aspartame, naphthyldivinylmethoxy azene, naphthyldivinylpropoxylate, phenyldiallylmethoxydecane, phenyl diallylpropoxy Q aryl di c2-fluorenyl vinyl methoxy decane, benzyl divinyl propoxy decane, etc., such as decane, naphthyl diallyl methoxy decane, naphthyl diallyl methoxy decane, Benzyl di-22- 201229055 vinyl butoxy decane, benzyl diallyl methoxy decane, benzyl allyl ethoxy decane, benzyl diallyl propoxy decane, benzyl ally a c^5 aralkyldiC2-idecenyl Cii2 alkoxy oxane compound, etc., such as butyloxydecane, etc., in the case of a vinyl group such as dimethylethene, propylvinylalkane or diamyl Ethylene alkyl, dipropyl vinyl alkane, dimercapto ethylene oxide, •—" propyl vinyl alkane, '* mercapto vinyl burned' dipropyl vinyl alkane, dimethylene Propyl burn, propyl 'allyl hospital, dimethyl diallyl, propyl Di-propyl, -methyl-propyl propyl, '-propyl-propyl propyl, dimethyl propyl, dipropyl allyl, etc., two C, -10 alkyl c2 vinyl methoxy Sintering of vinyl ethoxylates, Ethylene, Ethyloxypropene, Oxygen, and Oxygen, and methoxy decane, dimethoxy methoxy sulphide, dibutyl ethoxy sulphur, diethoxy ethoxylate Xishou, dibutoxylate, bis-propoxy decane, dibutoxy oxybutan, dibutoxy sulphate, dibutoxy decane, dimethoxy decane, dibutyl Oxygen stone court, ethylene glycol diacetate, dibutyl propoxy decane, diethylene propoxy decane, dibutyl butoxy decane, diethoxybutane, dibutyl- ίο dibasic C!" 2 Calcined bismuth, dinaphthylethylene, 'further exemplified, vinyl vinyl methoxy fluorenyl vinyl methoxy fluorenyl ethoxy ethoxymethyl vinyl fluorenyl vinyl propyl Oxyfluorenyl vinyl propoxy fluorenyl vinyl butoxymethyl vinyl butoxy decyl allyl Oxyalkyl allyl methoxy methoxy allyl ethoxy ethoxylate propyl ethoxy ethoxy allyl propoxy hydrazino propyl propyl aryl propyl propyl butyl acrylate Crude propyl butyl, hydroxyalkylene compound; diphenyloxydecane, diphenyldinaphthylvinylethoxy decane, diphenyldinaphthylvinylpropoxydecane, diphenyl-23 - 201229055 Vinyl butoxydecylnaphthyl vinylbutoxydecane, diphenyl

基矽烷、二节基烯丙基乙氧基矽烷、二 ’ 一节基乙稀基甲氧 、一节基乙稀基丙氧 '二苄基烯丙基甲氧 、二苄基烯丙基丙氧 基矽烷.、二节基烯丙基丁氧基矽烷等二c7 i5芳烷基c2 H 歸基C I ·丨2烧氧碎燒化合物等。 就其他單烧氧矽烷化合物而言,可列舉例如三甲基 曱氧基矽烷、三曱基乙氧基矽烷、三笨基曱氡基矽烷、 二苯基乙氧基矽烷、苯基二曱基甲氧基矽烷、苯基二甲 基乙氧基矽烷、苯基二乙基甲氧基矽烷、苯基二乙基乙 氧基石夕烧、二苯基甲基甲氧基矽烷、二笨基曱基乙氧基 矽烷、二苯基乙基甲氧基矽烷、二苯基乙基乙氧基矽烷 等。 就Η型單齒化矽烷化合物而言,可列舉例如單I石夕烷 、單氣矽烷、單溴矽烷等含3個氫原子之單_化石夕烧化合 物;氟甲基矽烷、氣曱基矽烷、溴曱基矽燒、氟乙基石夕 貌、氯乙基矽烷、溴乙基矽烷、氟丙基矽烷、氯丙基矽 燒、溴丙基矽烷、氟丁基矽烷、氯丁基矽烧、漠丁基石夕 貌、氟苯基矽烷、氣苯基矽烷、溴苯基矽院、氟蔡基石夕 燒、氣萘基矽烷、溴萘基矽烷、氟节基矽貌、氯节基石夕 -24- 201229055 烷、溴苄基矽烷等含兩個氫原子之單齒化矽烷化合物; 說一甲基石夕烧、氯二甲基石夕炫、溴二甲基石夕燒、敗二乙 基矽烷、氣二乙基矽烷、溴二乙基矽烷、氟二丙基矽烷 、氯二丙基矽烧、溴二丙基矽烷、氟二丁基矽烷、氯二 丁基矽烷、溴二丁基矽烷等含1個氫原子之單鹵化二C11C 烧基碎烧化合物;氟二苯基矽烷、氣二苯基矽烷、溴二 笨基矽烧、氟二萘基碎烧、氯二萘基矽烧、溴二萘基石夕 烷等含1個氳原子之單鹵化二C6-!4芳基矽烷化合物;氟二 苄基矽烷、氣二苄基矽烷、溴二苄基矽烷等含丨個氫原子 之單函化二C:7」5芳烷基矽烷化合物;氟曱基苯基矽烷、 氟乙基苯基矽烷、氟丙基苯基矽烷、氟丁基苯基矽烷、 氣甲基苯基矽烷、氣乙基苯基矽烷、氣丙基苯基矽烷、 氯丁基苯基矽烷、溴甲基萘基矽烷、溴乙基萘基矽烷、 溴丙基萘基矽烷、溴丁基萘基矽烷等含i個氫原子之單鹵 化Ci-M烷基芳基矽烷化合物;氟甲基苄基矽烷、氟 乙基卞基矽烷、氟丙基苄基矽烷、氟丁基苄基矽烷、氯 土苄基石夕烧氣乙基 > 基石夕烧、氣丙基节基石夕烧、氣 丁基苄基矽烷、溴甲基苄基矽烷、溴乙基苄基矽烷、溴 丙基苄基矽烷、〉臭丁基苄基矽烷等含1個氫原子之單鹵化 Cl-1G燒基C7-15芳烷基矽烷化合物等。 就乙烯基型單鹵化矽院化合物而言,可列舉例如氟 一乙烯基矽烷、氣三乙烯基矽烷、溴三乙烯基矽烷、氟 一烯丙基矽烷、氯三烯丙基矽烷、溴三烯丙基矽烷等單 鹵化二Cm烯基矽烷化合物;氟甲基二乙烯基矽烷、氣 甲基二乙烯基矽烷、溴曱基二乙烯基矽烷、氟乙基二乙 -25- 201229055 烯基矽烷' 氯乙基-7 ,嗓苴& p " 土一乙烯基矽烷、溴乙基二乙烯基矽浐 、氟丙基二乙稀基石70 岬丞矽烷、氣丙基二乙烯基矽烷、溴丙 二乙烯基矽烷、氟丁其__ 7祕I a, ^ 土 载丁基一乙烯基矽烷、氣丁基二乙烯基 矽烷、溴丁基二乙烯基矽烷、a甲基二烯丙基矽烷、氯 曱基一烯丙基矽烷、溴曱基二烯丙基矽烷、氟乙基二烯 丙基矽烷、氯乙基二烯丙基矽烷、溴乙基二烯丙基矽烷 、氟丙基二烯丙基矽烷、氣丙基二烯丙基矽烷、溴丙基 稀丙基石夕烧氧丁基二浠丙基石夕烧、氯丁基二浠丙基 矽烷、溴丁基二烯丙基矽烷等單_化。^烷基二c2 ^烯 基矽烷化合物;氟苯基二乙烯基矽烷、氯苯基二乙烯基 矽烷、溴苯基二乙烯基矽烷、氟萘基二乙烯基矽烷、氯 蔡基二乙稀基石夕烷、溴萘基二乙烯基矽烷、氟苯基二烯 丙基矽烷、氣苯基二烯丙基矽烷、溴苯基二烯丙基矽烷 、氟萘基二烯丙基矽烧、氯萘基二稀丙基矽烧、溴萘基 二稀丙基石夕烧等單函化c^4芳基二C210烯基矽烷化合物 ,氟V基二乙烯基石夕烧、氯苄基二乙稀基石夕烧、溴苄基 二乙烯基矽烷、氟苄基二烯丙基矽烷、氣苄基二烯丙基 石夕烧、溴苄基二烯丙基矽烷等單鹵化C7_15芳烷基二c2 烯基矽烷化合物。 就乙烯基型單鹵化石夕炫化合物而言,進一步可列舉 例如氟一甲基乙稀基碎焼《、風1 一甲基乙稀基碎烧、漠二 曱基乙稀基石夕烧、氟二乙基乙稀基石夕燒、氣二乙基乙稀 基矽烷、溴二乙基乙烯基矽烷、氟二丙基乙烯基矽烷、 氣二丙基乙婦基石夕炫《、溴二丙基乙烯基石夕烧、氟二丁基 乙烯基石夕燒、氣二丁基乙稀基石夕烧、溴二丁基乙稀基石夕 -26- 201229055 基矽烷、氯二甲基 II二乙基稀丙基石夕 烯丙基石夕燒、氟二 烷、溴二丙基烯丙 丁基稀丙基石夕院、 烷基c2_1G烯基矽烷 苯基乙婦基石夕烧、 基矽烷、氯二萘基 氣二苯基稀丙基石夕 稀丙基梦烧、氣二 烷、溴二萘基烯丙 石夕烧化合物;氟二 烧、漠、二苄基乙稀 苄基烯丙基石夕烧、 芳烷基c2.1()烯基矽 氟乙基苯基乙晞基 基笨基乙烯基矽烷 基乙烯基石夕烧、氣 烯基矽烷、溴甲基 石夕烷、溴丙基萘基 、既曱基苯基稀丙 丙基苯基烯丙基石夕 苯基烯丙基石夕烧、 烯丙基矽烷、氯丁 基矽烷、溴乙基萘 烷、氟二甲基烯丙 曱基稀丙基碎燒、 基石夕院、溴二乙基 氯二丙基烯丙基矽 浠丙基石夕烧、氯二 烧等單鹵化二c, _ i 〇 乙烯基矽烷、氯二 烷、氟二萘基乙烯 萘基乙稀基石夕貌、 基矽烷'溴二苯基 氯一奈基烤丙基妙 C 6 -丨4芳基C 2 - Π)婦基 氯二苄基乙烯基矽 烯丙基矽烷、氯二 烷等單鹵化二C7_15 苯基乙烯基矽烷、 乙烯基矽烷、氟丁 基矽烷、氣乙基苯 烧、氯丁基苯基乙 >臭乙基萘基乙稀基 基萘基乙烯基矽烷 基稀丙基石夕炫、氣 丙基矽烷、氯曱基 矽烷、氯丙基苯基 、溴甲基萘基烯丙 烯丙基矽烷、溴二 烷、氣二乙基烯丙 丙基烯丙基矽烷、 基矽烷、氟二丁基 溴二丁基烯丙基矽 化合物;氟二苯基 溴二笨基乙烯基矽 乙烯基矽烷、溴二 烷、氣二苯基烯丙 萘基烯丙基石夕烧、 基矽烷等單函化二 苄基乙烯基矽烷、 基矽烷、氟二苄基 溴二苄基烯丙基矽 烷化合物;氟甲基 矽烷、氟丙基苯基 、氣曱基苯基乙稀 丙基苯基乙烯基石夕 萘基乙烯基石夕院.、 乙烯基矽烷、溴丁 基矽烷、氟乙基苯 烷、氟丁基苯基烯 氣乙基苯基烯丙基 基苯基烯丙基石夕烧 基烯丙基矽烷、溴 -27- 201229055 丙基奈基烯丙基石夕烷、漠丁基萘基烯丙基石夕烷等單齒化 C丨,貌基C6…芳基c2·】。婦基石夕炫化合物;氟尹基节基乙 稀基石夕貌、氟乙基节基乙稀基Μ、氟丙基f基乙❹ 矽烷、氟丁基苄基乙烯基矽烷氯甲基苄基乙烯基矽烷 =基节基乙烯基石夕炫、氯丙基节基乙烯基石夕炫、氯 丁基卞基乙烯基矽烧、溴甲其苹 — ,吴y基苄基乙烯基矽烷、溴乙基 稀基石夕炫、漠丙基节基乙稀基石夕炫、漠丁基节基 :,、說…基埽丙基石夕燒、氟乙基节基稀丙 =、氣丙基节基稀丙基石夕烧、氣丁基节基稀丙基石夕 ::甲基’基烯丙基矽烷、氯乙基节基烯丙基矽烷、 ::基节基稀丙基石夕烧、氣丁基节基稀丙基石夕貌 ί =丙基妙燒、演乙基节基W漠丙基节 丙㈣烧、漠丁基节基稀丙基錢等單“ CU 丞匕7-丨5方烷基(:2·1()烯基矽烷化合物等。 就其他單齒化石夕烧化合物而言,可列 基矽烷、氣二甲美石々栌、、、自一田^ - r 、氣…:一甲基夕说/臭二甲基錢、貌三笨基石夕烧 軋二本基矽烷、漠三苯基矽烷、氟笨基二 氯苯基二甲基…漠苯基二甲基…氣 石夕院、氯苯基二乙基石夕烧、漠苯基二乙 二: 某_甲真ru? a- 元 氣* 一本 m二氣二苯基甲基石夕烧、演二苯基甲基妙烧、 乱-本基乙基矽烷、氯二苯基乙基矽 矽烷等。 、〜本基乙基 單羥基矽 矽烷、丁 苄基羥基 ^就Η型單經基矽烷化合物而言,可列舉例如 烷;甲基羥基矽烷、乙基羥基矽烷、丙基羥基 基羥基矽烷、苯基羥基矽烷、萘基羥基矽烷、 -28- 201229055 矽烷等含兩個氫原子之羥基矽烷化合物;二甲基羥基矽 烷、二乙基羥基矽烷、二丙基羥基矽烷、二丁基羥基矽 烧等含1個氫原子之二Cl,烷基羥基矽烷化合物;二苯基 羥基矽烷、二萘基羥基矽烷等含1個氫原子之二CV14芳基 經基%院化合物;二苄基羥基矽烷等含1個氫原子之二 C7-ls芳烷基羥基矽烷化合物;甲基苯基羥基矽烷 '乙基 苯基羥基矽烷、丙基笨基羥基矽烷'丁基苯基羥基矽烷 、甲基萘基羥基矽烷、乙基萘基羥基矽烷、丙基萘基羥 基矽烷、丁基萘基羥基矽烷等含i個氫原子之C11Q烷基 芳基羥基矽烷化合物;甲基苄基羥基矽烷、乙基苄 基羥基矽烷、丙基苄基羥基矽烷、丁基苄基羥基矽烷等 έ 1個氫原子之Ci-io烧基C?-〗5芳烧基經基石夕烧化合物等。 就乙烯基型單羥基矽烷化合物而言,可列舉例如三 乙烯基羥基矽烷、三烯丙基羥基矽烷等三I丨〇烯基羥基 矽烷化合物;甲基二乙烯基羥基矽烷、乙基二乙烯基羥 基矽烷、丙基二乙烯基羥基矽烷、丁基二乙烯基羥基矽 烷、甲基二烯丙基羥基矽烷、乙基二烯丙基羥基矽烷、 丙基二烯丙基羥基矽烷、丁基二烯丙基羥基矽烷等 烷基二C2_1Q烯基羥基矽烷化合物;苯基二乙烯基羥基矽 烷、萘基二乙烯基羥基矽烷、苯基二烯丙基羥基矽烷、 萘基二烯丙基羥基矽烷等Gw芳基二Gw埗基羥基矽烷 化合物,节基二乙烯基羥基矽烷、节基二烯丙基羥基矽 烧等C7-,5芳院基Cuo烧基二Cno烯基羥基矽烧化合物等 〇 就乙烯基型單羥基矽烷化合物而言,進一步可列舉 -29- 201229055 例如二甲基乙烯基羥基矽烷、二乙基乙烯基羥基矽烷、 二丙基乙烯基羥基矽烷、二丁基乙烯基羥基矽烷、二甲 基烯丙基羥基矽烷、二乙基烯丙基羥基矽烷、二丙基烯 丙基羥基矽烷、二丁基烯丙基羥基矽烷等二Ci i〇烷基 烯基羥基矽烷化合物;二苯基乙烯基羥基矽烷、二 萘基乙烯基羥基矽烷、二苯基烯丙基羥基矽烷、二萘基 烯丙基羥基矽烷等二C6 M芳基C2_1G烯基羥基矽烷化合物 ,一苄基乙稀基經基石夕烧、 C7-15芳烷基c2_1()烯基羥基矽 羥基矽烷、乙基苯基乙烯基 經基矽烷、丁基苯基乙烯基 經基矽烷、乙基萘基乙烯基 羥基矽烷、丁基萘基乙烯基 羥基矽烷、乙基苯基烯丙基 經基矽烷、丁基苯基烯丙基 羥基矽烷、乙基萘基烯丙基 羥基矽烷、丁基萘基烯丙基 基C2_ , 〇烯基羥基矽烷化合物 、乙基节基乙烯基羥基矽烷 、丁基节基乙烯基羥基矽烷 、乙基节基烯丙基羥基矽烷 、丁基节基烯丙基羥基矽烷 烯基羥基矽烧化合物等。 二 苄 基 烯 丙 基 羥 基 矽 烷 等 二 烷 化 合 物 > 甲 基 苯 基 乙 烯 基 羥 基 矽 烷 N 丙 基 苯 基 乙 烯 基 羥 基 矽 烷 甲 基 萘 基 乙 稀 基 羥 基 矽 燒 丙 基 萘 基 乙 烯 基 羥 基矽 烷 \ 甲 基 苯 基 烯 丙 基 羥 基 矽 烧 丙 基 苯基烤 丙 基 羥 基 矽 燒 •V 甲 基 萘 基 稀 丙 基 經 基 矽 烷 、 丙 基 萘 基 烯 丙 基 羥 基 矽 烷 等 C, -10 烷 基 C 6 - 1 4 芳 » 甲 基 苄 基 乙 稀 基 羥 基石夕 烧 丙 基 苄 基 乙 烯 基 羥 基ί夕 烧 、 甲 基 苄 基 婦 丙 基 羥 基碎 烧 、 丙 基 苄 基 晞 丙 基 羥 基 矽 烧 等 C, •10 烷 基 C7 -15 芳 烷 基 C2- 1 0 可列舉例如三甲基 醇、苯基二甲基矽 就其他單羥基矽烷化合物而言, 矽烷醇、三乙基矽烷醇、三苯基矽烷 -30- 201229055 炫醇、苯基二乙基石夕p 丞矽烷醇、二苯基甲基矽烷醇、二 乙基矽烷醇等。就矽烧 一 7况化合物(S2)而言’上述 合物可單獨使用或混合兩種以上使用。 就作為上述式^ 、之R〜R的Cm。烷基而言, 為C丨-5烧基,就C 2 Μ嫌直1 士 ..,,, 2_10烯基而吕,特佳為c2_5烯基。就 R而言,基於耐熱無黃變之點,較佳為甲基、乙基 基、乙缔基、烯丙基。又基於耐水解性之點,更: 基0 就上述式(2)中之X3中的Ci」2烷氧基而言,特Base decane, bis- allyl ethoxy decane, bis-ethylidene methoxy, benzylidene propyloxy-dibenzylallyl methoxy, dibenzyl allylic propyl Di-c7 i5 aralkyl c2 H such as oxydecane, bis- allylic butoxybutane, sulfhydryl compound, etc. Examples of the other mono-oxygen decane compound include trimethyl decyl decane, tridecyl ethoxy decane, triphenyl decyl decane, diphenyl ethoxy decane, and phenyl fluorenyl. Methoxy decane, phenyl dimethyl ethoxy decane, phenyl diethyl methoxy decane, phenyl diethyl ethoxy oxime, diphenyl methyl methoxy decane, diphenyl hydrazine Ethyl ethoxy decane, diphenylethyl methoxy decane, diphenyl ethyl ethoxy decane, and the like. Examples of the fluorene-type monodentate decane compound include a single-fossil-burning compound containing three hydrogen atoms such as mono-I-taxane, mono-halogenane or monobromodecane; fluoromethyl decane and gas decyl decane; , bromomethyl oxime, fluoroethyl oxime, chloroethyl decane, bromoethyl decane, fluoropropyl decane, chloropropyl oxime, bromopropyl decane, fluorobutyl decane, chlorobutyl oxime, Desert butyl stone, fluorophenyl decane, phenyl phenyl decane, bromophenyl fluorene, fluorocaffeyl sulphate, phthalnaphthyl decane, bromonaphthyl decane, fluorinated fluorene, chlorohexyl sulphate - 201229055 A monodentate decane compound containing two hydrogen atoms, such as an alkane or a bromobenzyl decane; said monomethyl sulphur, chloro dimethyl sulphur, bromo dimethyl sulphur, sulphur diethyl decane , gas diethyl decane, bromodiethyl decane, fluorodipropyl decane, chlorodipropyl oxime, bromodipropyl decane, fluorodibutyl decane, chlorodibutyl decane, bromodibutyl decane, etc. Monohalogenated di-C11C calcined compound containing one hydrogen atom; fluorodiphenyl decane, diphenyl decane, bromine diphenyl oxime, a monohalogenated di-C6-!4 aryl decane compound containing one fluorene atom, such as dinaphthyl calcination, chlorodinaphthyl oxime, bromodinaphthyl linane or the like; fluorodibenzyl decane, gas dibenzyl decane, a monofunctional di-C:7"5 aralkyl decane compound containing a hydrogen atom such as bromodibenzylnonane; fluorononylphenyl decane, fluoroethylphenyl decane, fluoropropyl phenyl decane, fluorobutyl Phenyl decane, gas methylphenyl decane, gas ethyl phenyl decane, gas propyl phenyl decane, chlorobutyl phenyl decane, bromomethyl naphthyl decane, bromoethyl naphthyl decane, bromopropyl a monohalogenated Ci-M alkylaryldecane compound containing one hydrogen atom such as naphthyldecane or bromobutylnaphthyldecane; fluoromethylbenzyl decane, fluoroethyl decyl decane, fluoropropylbenzyl decane, Fluoryl butyl benzyl decane, chlorobenzyl benzyl sulfonate ethyl > ketone, gas propyl gangyl, butyl benzyl decane, bromomethylbenzyl decane, bromoethyl benzyl decane A monohalogenated Cl-1G alkyl C7-15 aralkyl decane compound containing one hydrogen atom such as bromopropylbenzyl decane or > odor butyl benzyl decane. Examples of the vinyl type monohalogenated broth compound include, for example, fluoro-vinyl decane, gas trivinyl decane, bromotrivinyl decane, fluoromonoallyl decane, chlorotriallyl decane, and bromotriene. Monohalogenated di-Cm alkenyl decane compound such as propyl decane; fluoromethyl divinyl decane, gas methyl divinyl decane, bromodecyl divinyl decane, fluoroethyl diethyl-25- 201229055 alkenyl decane Chloroethyl-7 , 嗓苴 & p " soil-vinyl decane, bromoethyl divinyl fluorene, fluoropropyl diethylene sulphate 70 decane, gas propyl divinyl decane, bromopropyl Divinyl decane, fluorobutane __ 7 secret I a, ^ butyl 1,4-vinyl decane, butyl butyl divinyl decane, bromobutyl divinyl decane, a methyl diallyl decane, Chloroyl-allyl decane, bromodecyl diallyl decane, fluoroethyl diallyl decane, chloroethyl diallyl decane, bromoethyl diallyl decane, fluoropropyldiene Propyl decane, propylene propylene diallyl decane, bromopropyl propyl sulfoxide, butyl butyl fluorenyl sulfonate, chlorine Silane two Hay propyl group, diallyl silane-bromobutyl and the like of a single _. ^alkyl di c2 ^ alkenyl decane compound; fluorophenyl divinyl decane, chlorophenyl divinyl decane, bromophenyl divinyl decane, fluoronaphthyl divinyl decane, chlorocaline diethylene sulphate Cyclohexane, bromonaphthyldivinylnonane, fluorophenyl diallyl decane, gas phenyl diallyl decane, bromophenyl diallyl decane, fluoronaphthyl diallyl oxime, chloronaphthalene A mono-c^4 aryl-di-C210 alkenyl decane compound such as dipropyl sulfonium bromide, bromo-naphthyl di-propyl sulfonium, etc., fluorine V-based divinyl sulphate, chlorobenzyl diethylene sulphate Monohalogenated C7_15 aralkyl di-c2 alkenyl decane compound such as calcined, bromobenzyldivinyl decane, fluorobenzyl diallyl decane, gas benzyl diallyl, bromobenzyl diallyl decane . In the case of the vinyl-type monohalogenated fossil compound, for example, fluoromethylidene ruthenium ruthenium, wind 1 methyl methacrylate-based sinter, sulphur-based sulphur base sulphur, and fluorine Diethylethylene base stone, gas, diethyl diethyl decane, bromodiethyl vinyl decane, fluorodipropyl vinyl decane, gas dipropyl ethoxylate, shuangxuan, bromodipropylethylene Base stone simmering, fluorodibutylvinyl sulphate, gas dibutyl ethane sulphate, bromodibutyl sulphate -26 - 201229055 decane, chlorodimethyl II diethyl propyl sulphate Allyl group, fluorodialkyl, bromodipropylallyl propyl propyl sulfanyl, alkyl c2_1G alkenyl decyl phenyl ethoxylate, decyl, chloronaphthyl diphenyl hydride Basestone dimethyl propyl dream, gas dioxane, bromodinaphthyl allylate compound; fluorodicarb, desert, dibenzylethylene benzyl allylate, aralkyl c2.1 () Alkenyl fluoroethyl phenyl ethionyl phenyl vinyl fluorenyl vinyl cerium, oxyalkylene decane, bromomethyl oxalate, bromopropyl Naphthyl, decylphenyl propyl propyl propyl allylate, phenyl phenyl allylate, allyl decane, chlorobutyl decane, bromoethyl decalin, fluorodimethyl methacryl Dilute propyl sinter, base stone shed, bromo diethyl chlorodipropylallyl propyl sulfonium, chlorinated dihalogenated monohalogenated c, _ i 〇 vinyl decane, chlorodialkyl, fluorodi Naphthylvinylnaphthylethylene sulphate, decyl-bromodiphenylchloro-n-propyl-bromopropyl C 6 -丨4 aryl C 2 - fluorene) benzyl dibenzyl vinyl lyl allyl Monohalogenated di-C7_15 phenyl vinyl decane, vinyl decane, fluorobutyl decane, gas ethyl benzene, chlorobutyl phenyl b> odor ethyl naphthyl vinyl naphthyl Vinyl decyl propyl sulfanthine, propyl propyl decane, chlorodecyl decane, chloropropyl phenyl, bromomethylnaphthyl propylene propyl decane, brominated dioxane, gas diethyl allylic propylene Propyl decane, decane, fluorodibutyl bromodibutylallyl fluorene compound; fluorodiphenyl bromide, styryl vinyl quinone vinyl decane, brominated dioxane, gas two Mono-, dibenzylvinyl decane, decane, fluorodibenzyl bromodibenzylallyl decane compound; fluoromethyl decane, fluoropropyl benzene Base, gas phenyl propyl propyl phenyl vinyl vinyl naphthyl vinyl sylvestre, vinyl decane, bromobutyl decane, fluoroethyl benzene, fluorobutyl phenyl olefin ethyl phenyl Allyl phenylallyl fluorenyl allyl decane, bromine -27- 201229055 propyl nalyl ally lysine, butyl butyl naphthyl propyl sulfoxide, etc. Base C6...arylc2·]. Women's base stone Xixuan compound; fluorinyl benzyl ether base stone, fluoroethyl benzyl hydrazine, fluoropropyl f-ethyl hydrazine, fluorobutyl benzyl vinyl decyl chloromethyl benzyl ethylene矽 矽 基 基 基 基 基 基 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 、 Basestone Xixuan, Mo-propyl propyl group, ethylene base stone Xixuan, desert butyl node:,, say, 埽 埽 石 夕 、, fluoroethyl jieji propylene =, propyl propyl propyl propyl Burned, gas butyl benzyl propyl sulfoxide:: methyl 'allyl decane, chloroethyl benzyl propyl decane, :: benzyl propyl sulfonium, gas butyl sulfhydryl基石夕貌 ί = propyl smoldering, playing ethyl ketone group W propyl propyl propylene (four) burning, desert butyl ketone propyl propyl money and other single "CU 丞匕 7-丨 5 octadecyl (: 2 · 1() alkenyl decane compound, etc. For other single-toothed fossil sinter compounds, cyclable decane, dimethyl meteocarbazine, and from a field ^ - r , gas... /Smelly dimethyl money, looks three stupid Base stone Xishan rolling two base decane, desert triphenyl decane, fluorophenyl dichlorophenyl dimethyl ... desert phenyl dimethyl ... gas stone Xi courtyard, chlorophenyl diethyl sulphur, sulphur二二二: A _甲真 ru? a- 元气* A m-gas diphenylmethyl sulphur, a diphenylmethyl smoldering, a chaotic-propenyl decane, a chlorodiphenyl矽矽 矽矽 等 〜 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本 本a hydroxy decane compound containing two hydrogen atoms, such as decane, phenyl hydroxy decane, naphthyl hydroxy decane, -28-201229055 decane; dimethyl hydroxy decane, diethyl hydroxy decane, dipropyl hydroxy decane, dibutyl hydroxy group a di-CV14 aryl group containing one hydrogen atom, such as a di-hydrogen atom-containing di-Cl, an alkyl hydroxy decane compound; a diphenyl hydroxy decane, a dinaphthyl hydroxy decane, or the like; a C7-ls aralkyl hydroxy decane compound containing one hydrogen atom such as decane; methyl phenyl group矽 ' 'ethyl phenyl hydroxy decane, propyl hydroxy hydroxy decane 'butyl phenyl hydroxy decane, methyl naphthyl hydroxy decane, ethyl naphthyl hydroxy decane, propyl naphthyl hydroxy decane, butyl naphthyl hydroxy a C11Q alkylarylhydroxydecane compound containing one hydrogen atom such as decane; methylbenzyl hydroxydecane, ethylbenzylhydroxydecane, propylbenzylhydroxydecane, butylbenzylhydroxydecane, etc. 1 hydrogen atom For the vinyl type monohydroxydecane compound, for example, trivinyl hydroxy decane, triallyl hydroxy decane, and the like are exemplified. Tertyl hydroxy decane compound; methyl divinyl hydroxy decane, ethyl divinyl hydroxy decane, propyl divinyl hydroxy decane, butyl divinyl hydroxy decane, methyl diallyl hydroxy decane, Alkyl di-C 2_1Q alkenyl hydroxy decane compounds such as diallyl hydroxy decane, propyl diallyl hydroxy decane, butyl diallyl hydroxy decane; phenyl divinyl hydroxy decane, naphthyl divinyl hydroxy group Decane, phenyldiene Gw aryl di Gw decyl hydroxy decane compound such as propyl hydroxy decane or naphthyl diallyl hydroxy decane, C7-, 5 aryl-based group such as benzyl divinyl hydroxy decane and decyl diallyl hydroxy fluorene Cuo-based di-Cno alkenyl hydroxy fluorinated compound, etc., in terms of a vinyl type monohydroxy decane compound, further exemplified by -29 to 201229055, for example, dimethylvinyl hydroxy decane, diethyl vinyl hydroxy decane, dipropylene Vinyl hydroxy decane, dibutyl vinyl hydroxy decane, dimethyl allyl hydroxy decane, diethyl allyl hydroxy decane, dipropyl allyl hydroxy decane, dibutyl allyl hydroxy decane, etc. Di-Ci i 〇 alkyl alkenyl hydroxy decane compound; diphenyl vinyl hydroxy decane, dinaphthyl vinyl hydroxy decane, diphenyl ally hydroxy decane, dinaphthyl propyl hydroxy decane, etc. a C2_1G alkenyl hydroxydecane compound, a benzylidene group via a ketone, a C7-15 aralkyl c2_1() alkenyl hydroxy hydroxy hydroxy decane, an ethyl phenyl vinyl hydrazin, a butyl phenyl ethene Base decane, ethylnaphthylvinyl Base decane, butyl naphthyl vinyl hydroxy decane, ethyl phenyl allyl decyl decane, butyl phenyl allyl hydroxy decane, ethyl naphthyl allyl hydroxy decane, butyl naphthyl allyl Base C2_ , decyl hydroxy decane compound, ethyl benzyl hydroxy decane, butyl benzyl vinyl hydroxy decane, ethyl benzyl hydroxy decane, butyl benzyl hydroxy hydroxy decyl hydroxy Simmering compounds, etc. Dioxane compound such as dibenzylallyl hydroxydecane> Methylphenyl vinyl hydroxy decane N propyl phenyl vinyl hydroxy decyl methyl naphthyl ethylene hydroxy hydrazine propyl naphthyl vinyl hydroxy decane \ Methyl phenyl allyl hydroxy oxime propyl phenyl propyl hydroxy oxime • V methyl naphthyl propyl propyl decyl, propyl naphthyl propyl hydroxy decane, etc. C, -10 alkyl C 6 - 1 4 aryl » methyl benzyl ethylene hydroxy sulphur propyl benzyl hydroxy hydroxy oxime, methyl benzyl propyl hydroxy calcination, propyl benzyl propyl hydroxy oxime, etc. C, • 10 alkyl C7 -15 aralkyl C2- 1 0 may, for example, be trimethyl alcohol or phenyl dimethyl hydrazine. For other monohydroxy decane compounds, stanol, triethyl stanol, triphenyl Base decane-30- 201229055 Alkyl alcohol, phenyldiethyl phosphatene, diphenylmethyl decyl alcohol, diethyl stanol, and the like. In the case of the smoldering compound (S2), the above compounds may be used singly or in combination of two or more. It is Cm which is R to R of the above formula. In the case of an alkyl group, it is a C丨-5 alkyl group, and the C 2 Μ is a straight one. .,,, 2-10 alkenyl group, and particularly preferably a c2_5 alkenyl group. In the case of R, a point which is based on heat resistance and no yellowing is preferably a methyl group, an ethyl group, an ethyl group or an allyl group. Further, based on the point of hydrolysis resistance, more: base 0 is the Ci"2 alkoxy group in X3 in the above formula (2),

Ci·:烷氧基。就上述χ3而言,基於取得性之點,較 曱氧基、乙氧基、氯原子、溴原子、羥基,基於反 容易度’更佳為羥基。 就單官能之矽烷化合物(S2)而言,較佳為單_ 烧化合物’纟體上可適合使用例如三甲基♦貌醇Γ 基石夕烷醇、三苯基石夕烷醇、苯基二甲基矽烷醇、苯 乙基矽烷醇、二苯基甲基矽烷醇、二苯基乙基矽烷 本發明之金屬矽氧烷化合物,由於以在1分子中 至少1個可進行氫化矽烷化反應之Si_H鍵或c^i〇烯 特徵,故使用於製造金屬矽氧烷化合物的矽烷化合 至少1個係在1分子中具有至少"固si_H鍵的H型矽烷 物或在1分子中具有至少1個C2.1()烯基的乙烯基型 合物。 [金屬化合物(M)] 本發明中使用之金屬化合物(Μ)係以下列式(2) 苯基 之化 特佳 R3〜 、苯 為笨 佳為 佳為 應的 基石夕 三乙 基二 醇等 具有 基為 物之 化合 烧化 -31- 201229055Ci·: alkoxy group. The above-mentioned oxime 3 is more preferably a hydroxyl group based on the degree of availability than the decyloxy group, the ethoxy group, the chlorine atom, the bromine atom or the hydroxyl group. In the case of the monofunctional decane compound (S2), it is preferred to use a mono- sinter compound, for example, trimethyl phthalocyanine, triphenyl linalool, phenyl dimethyl Base stanol, phenethyl stanol, diphenylmethyl decyl alcohol, diphenylethyl decane The metal oxoxane compound of the present invention, Si_H which can be subjected to hydrogenation sulfonation reaction in at least one molecule in one molecule a bond or a c-i-decene characteristic, so that at least one of the decane compounds used in the production of the metal oxoxane compound has at least one H-type decane having at least a "fixed Si_H bond in one molecule; or at least one molecule in one molecule A vinyl compound of a C2.1()alkenyl group. [Metal compound (M)] The metal compound (Μ) used in the present invention is a quinone-based triethyl diol or the like which is preferably a phenyl group of the following formula (2); Compound with a base-burning-31- 201229055

/ 1% Μ表示鍅或鈦;γ丨〜Y4係相同或不同,砉 院氧基或齒素原子) 表不C1-1 表:就Υ〜Υ4中的C!」2烷氧基而言’可列舉甲氧基、 =軋基二丙氧基、丁氧基等,較佳為Cw烷氧基。就鹵素 '、子而s ’可列舉氟原子、氣原子、溴原子等。 就金屬化合物(M)而言,可使用以上述式(2)表示, t一直使用於製造先前聚金屬矽氧烷之鍅化合物或鈦化 α物,可列舉例如錯烷氧化物(四乙氧基化鍅、 基化鍅、四正禺〶货 ,, u,、丙ΐ _ 四正丙氧基化锆、四(三級丁氧基)化鍅 '三異 丙氧基化氣鍅、二異丙氧基化二氣锆、異丙 錯等)、鹵化扯,Α ^ * . 固化鍅(四氣化锆、四溴化鍅等)等錯系路易街 奴,對應於前述錯系路易斯酸之鈦系路易斯酸(四異丙孽 匕欽四正丙氧基化鈦等鈦烧氧化物、四氣化鈦、Ε 溴化鈦等鈦齒化等。就金屬化合物(Μ)而言,上述例示之 化〇物可單獨使用或混合兩種以上使用。 就上述γ〜γ中的Cl lz院氧基或鹵素原子而言,這 於取2性之點,較佳為丙氧基、丁氧基、氯、溴,基友 反應前的安定性之點,t佳為丙氧基、丁氧基。就較召 的金屬化合物(M)而言,可列舉四異丙氧基化锆、四正兵 氧基化锆、四(三級丁氧基)化锆、四正丁氧基化鍅、^ 八丙氧基化鈦、四正丙氧基化鈦、四(三級丁氧基)化淑 、四正丁氧基化鈦等,尤可列舉四異丙氧基化锆、四JE 丙氧基化锆等。 -32- 201229055 [觸媒] 上述反應亦有在無觸媒下進行的情ί:兄,亦可視需要 而添加酸觸媒、鹼觸媒。藉由使酸觸媒或鹼觸媒存在於 反應系統中,通常反應速度會顯著增大《鹼中包含有無 機鹼及有機鹼。就無機鹼而言,可列舉例如氫氧化鋰、 氫氧化鈉、氫氧化鉀 '氩氧化鉋等鹼金屬氫氧化物;氫 氧化鎂、氫氧化鈣、氫氧化鋇等鹼土類金屬氫氧化物; 碳酸锂、碳酸鈉、碳酸鉀、碳酸铯等鹼金屬碳酸鹽;碳 酸鎂等鹼土類金屬碳酸鹽;碳酸氫鋰、碳酸氫鈉、碳酸 氫鉀、碳酸氫鉋等鹼金屬碳酸氫鹽等。 就有機驗而言’可列舉例如乙酸鋰、乙酸鈉、乙酸 斜、乙酸絶等驗金屬有機酸鹽(尤其是鹼金屬乙酸鹽); 乙酸鎂等鹼土類金屬有機酸鹽;甲基鋰、丁基鋰(正丁基 鋰,一級丁基鋰,三級丁基鋰等)等烷基鋰;甲氧基化鋰 曱氧基化鈉、乙氧基化鈉、異丙氧基化鈉、乙氧基化 舒等驗金屬燒氧化物;苯氧基化鈉等驗金屬苯氧基化物 ,一乙基胺、N_曱基哌啶、4_二甲基胺基吡啶(DMAP)、 1,8 丫又%[5.4.0]-7·十一烯(DBU)、三乙二胺(ι,4-二吖 雙承[2.2.2]辛烷;DABC0)、15-二吖雙環[4·3.0]-5-壬烯 (D:N:、六亞甲四胺、四甲基乙二胺、三辛基胺、二甲 基本fe、N-甲基吡咯咬、N_曱基哌啶、曱基咮啉等胺 — )比啶、二曱吡啶、甲基吡啶、咪唑、2,2,- 聯Z 1,1 〇·啡琳等含氮芳香族雜環化合物等。此等之 驗可早獨使用或組合兩種以上使用。其中,較佳為三乙 基胺4·一甲基胺基吡啶等3級胺;吡啶、二甲吡啶、甲 -33- 201229055 基比啶等含氮的芳香族性雜環化合物等。 々1觸媒而5 ,可列舉例如硫酸、鹽酸、磷酸、硝 酸等無機酸、羧酸(乙酴、 丙S文專Cl-ίο飽和或不飽和一元 或多π I等)、碩酸(曱磺酸、乙磺酸等6烷磺酸、苯磺 酸1甲苯續酸等芳香族續酸等)、㈣有機酸(三氣乙 I等函化m酸、三氟甲續酸等齒化烧績酸等)等有機酸、 硫酸鹽(硫㈣等)、金屬氧化物(Si02、ai2q3#)、沸石( 具有酸性OH之Y切、X刑 .Λ〜1/ 1% Μ denotes yttrium or titanium; γ丨~Y4 is the same or different, 砉 氧基 oxy or acne atom) Table C1-1 Table: For C~”2 alkoxy in Υ~Υ4 The methoxy group, the =rolled dipropoxy group, the butoxy group and the like are mentioned, and a Cw alkoxy group is preferable. Examples of the halogen ', sub and s ' include a fluorine atom, a gas atom, a bromine atom and the like. As the metal compound (M), an anthracene compound or a titanated α compound which is always used in the production of a prior polymetalloxane can be used, and t is, for example, a stearoxy oxide (tetraethoxy).基 鍅, 鍅 鍅, 四正禺〒,, u,, ΐ _ _ tetra-n-propoxy zirconium, tetra (tri-butyloxy) ruthenium triisopropoxy oxime, two Isopropoxylated zirconium dichloride, isopropranium, etc.), halogenated, Α ^ * . Cured 鍅 (four zirconium hydride, cesium tetrabromide, etc.) and other wrong system Louis Street slaves, corresponding to the aforementioned mis- Lewis acid Titanium-based Lewis acid (titanium-sintered oxide such as tetraisopropyl sulfonium tetra-n-propoxylated titanium, titanium hydride such as titanium tetrachloride or strontium bromide, etc., in terms of metal compound (Μ), The exemplified hydrazines may be used singly or in combination of two or more. In the case of the above-mentioned γ γ γ ethoxyl or halogen atom, this is preferably a propoxy group and a butoxy group. Base, chlorine, bromine, the point of stability before the reaction of the group, t is preferably propoxy, butoxy. In view of the metal compound (M), tetraisopropoxy Zirconium hydride, zirconium oxyzide, tetrakis(tris-butoxy)zirconium, tetra-n-butoxylated ruthenium, octa-propoxylated titanium, tetra-n-propoxylated titanium, four (three Examples of butoxy-based sulfonate, tetra-n-butoxytitanium, and the like include zirconium tetraisopropoxide, zirconium tetra-JE propoxide, and the like. -32- 201229055 [Catalyst] The above reaction is also present. In the absence of catalyst, the acid catalyst can be added as needed. By allowing the acid or base catalyst to be present in the reaction system, the reaction rate is usually increased significantly. The inorganic base and the organic base are contained. Examples of the inorganic base include alkali metal hydroxides such as lithium hydroxide, sodium hydroxide, and potassium hydroxide 'argon oxide planer; magnesium hydroxide, calcium hydroxide, and barium hydroxide. Alkaline earth metal hydroxide; alkali metal carbonate such as lithium carbonate, sodium carbonate, potassium carbonate or barium carbonate; alkaline earth metal carbonate such as magnesium carbonate; lithium hydrogencarbonate, sodium hydrogencarbonate, potassium hydrogencarbonate, hydrogencarbonate planing, etc. An alkali metal hydrogencarbonate or the like. For the organic test, 'for example, lithium acetate, sodium acetate, acetic acid oblique, B Acid-exclusive metal organic acid salt (especially alkali metal acetate); alkaline earth metal organic acid salt such as magnesium acetate; methyl lithium, butyl lithium (n-butyl lithium, primary butyl lithium, tertiary butyl lithium) Etc.), such as alkyl lithium; sodium methoxy ethoxylate, sodium ethoxylate, sodium isopropoxide, ethoxylated sulphur, etc.; sodium phenoxide Metal phenoxylate, monoethylamine, N_mercaptopiperidine, 4-dimethylaminopyridine (DMAP), 1,8 丫 and % [5.4.0]-7·undecene (DBU) , triethylenediamine (ι,4-dioxane double-contained [2.2.2]octane; DABC0), 15-diindole bicyclo[4.3.0]-5-decene (D:N:,hexamethylenetetrazide Amine, tetramethylethylenediamine, trioctylamine, dimethyl basic fe, N-methylpyrrole biting, N-mercaptopiperidine, mercaptoporphyrin and the like -) pyridine, dipyridyl, methyl A nitrogen-containing aromatic heterocyclic compound such as pyridine, imidazole, 2,2,-linked Z 1,1 〇 啡 琳 琳. These tests may be used alone or in combination of two or more. Among them, a tertiary amine such as triethylamine 4·monomethylaminopyridine; a nitrogen-containing aromatic heterocyclic compound such as pyridine, dimethylpyridine or methyl-33-201229055 pyridinium is preferable. 々1 catalyst and 5, for example, sulfuric acid, hydrochloric acid, phosphoric acid, nitric acid and other inorganic acids, carboxylic acids (acetamidine, C-specific Cl-ίο saturated or unsaturated mono- or multi-π I, etc.), sour (曱Sulfonic acid, ethanesulfonic acid and other 6-alkanesulfonic acid, benzenesulfonic acid 1 toluene acid and other aromatic acid, etc.), (4) organic acid (three gas, ethylene I and other functionalized m acid, trifluoromethyl acid, etc. Acid, etc.), such as organic acids, sulfates (sulfur (tetra), etc.), metal oxides (Si02, ai2q3#), zeolites (Y-cut with acidic OH, X punishment. Λ~1

^ 、八型沸石等)、離子交換樹脂(H 型等陽離子交換樹脂等)等固態酸等。 酸觸媒、鹼觸媒的使用量並無特別限制,相對於反 應系統_的羥基1莫耳,例如為〇 〇1〜5莫耳,較佳為〇 i 〜2莫耳、更佳為0.8〜12莫耳左右。另外,當未使用酸 觸媒、鹼觸媒時,可藉由加熱等促進反應進行。 反應可在聚合抑制劑的存在下進行。反應溫度可視 反應成分或觸媒的種類等而適當選擇,例如當使用乙稀 基矽烷時為20〜200。〇,較佳為20〜l〇(TC,更佳為4〇〜 6〇°C左右。又,當使用氫化矽烷時,反應溫度可視反應 成分或觸媒的種類等而適當選擇,例如為_78〜i i〇(>c, 較佳為-30〜40°c,更佳為_10〜1(rc左右。反應可在常 壓下進行,亦可在減壓或加壓下進行。只要反應的氣體 環境不阻礙反應則無特別限定,例如空氣氣體環境、氮 氣氣體環境、氬氣氣體環境等均可。又,反應亦可以批 次式、半批次式、連續式等任何方法進行。 反應結束後,反應生成物可藉由例如過渡、濃縮、 蒸餾、萃取、晶析、再結晶、管柱色層分析法等分離手 -34- 201229055 段或、將此等組合而成的分離手段進行分離純化。可在 反應後的/昆合液中添加水、】〜7 %的稀鹽酸、丨〜7 %的小 蘇打水等水系溶劑進行洗淨。 [硬化性樹脂組成物j 本發明之硬化性樹脂組成物係包含具有Si-H鍵的化 合物與具有C2-1G烯基的化合物之硬化性樹脂組成物,其 特徵在於至少含有上述金屬矽氧烷化合物(A)與氫化矽 烷化觸媒(C)。金屬矽氧烷化合物(A)之在硬化性樹脂組 成物中的3畺為例如3 〇〜9 9重量。/〇,較佳為5 〇〜8 〇重量% 〇 本發明之硬化性樹脂組成物中,亦可含有除了金屬 矽氧烷化合物(A)以外之在!分子中具有至少1個si H鍵 或C2_10烯基的化合物(Β^當金屬矽氧烷化合物為η型 的化合物時,硬化性樹脂組成物含有在1分子中具有至少 1個C2.1Q烯基的化合物(Β)[乙烯基型的化合物又, 當金屬矽氧烷化合物(Α)為乙烯基型的化合物時硬化性 樹脂組成物含有在1分子中具有至少1個Si-H鍵的化合物 (b)[h型的化合物(B)]。 [金屬矽氧烷化合物(A)以外之在丨分子中具有至少i個 Si-H鍵或Cno烯基的化合物(B)] 就上述Η型或乙烯基型的化合物(B)而言,可使用在工 分子中具有至少!個Si_H鍵或Gw烯基,且具有以矽氧烷 鍵(Si-0-Si)構成之主鏈的η型或乙烯基型的聚石夕氧烧。就 C2_10烯基而言,可列舉可包含於上述矽烷化合物中之例 示作為C2_1G烯基者。就聚矽氧烷而言,可具體列舉直鏈 -35- 201229055 狀、分支鏈狀或環狀的矽氧烷、具有經交聯的三維結構 之聚矽氧樹脂等。 就上述化合物(B)的具體例子而言,可列舉四曱基石夕 氧院、四曱基二乙稀基矽氧院、六甲基三矽氧燒、六曱 基二乙烯基三矽氧烷、七甲基三矽氧烷、七曱基乙烯基 三石夕氧烷、八甲基四矽氧烷、八曱基二乙烯基四矽氧烧 、九甲基四矽氧烷、九甲基乙烯基四矽氧烷、九甲基二 乙烯基四矽氧烷、十甲基五矽氧烷、十甲基二乙烯基五 矽氧烷、十一甲基五矽氧烷、十一甲基乙烯基五矽氧烷 、十甲基二乙烯基五矽氧烷等、具有1〜10個(較佳為2〜 5個)(Si-O)單位之直鏈狀聚二曱基矽氧烷、含氫化矽烷 基的聚石夕氧、含乙烯基的聚矽氧等在1分子中具有至少丄 個Si-H鍵或C2_1G烯基的直鏈狀聚二烷基矽氧烷(較佳為 直鏈狀聚二C^o烷基矽氧烷);二甲基環三矽氧烷、二甲 基二乙烯基環三矽氧烷、四曱基環四矽氧烷、四曱基四 乙烯基環四矽氧烷、三甲基環五矽氧烷、三甲基三乙烯 基環五矽氧烷等、具有2〜10個(較佳為2〜5個)(si_⑺單 位之在丨分子中具有至少丨個以^鍵或烯基的環狀聚 二曱基矽氧烷等環狀聚二烷基矽氧烷(較佳為環狀聚二 ci- ίο烷基矽氧烷)等。 /〜小上通例示之化 合物的曱基等烷基的全部或一部分被苯基等芳基(較佳 為匕⑴芳基)取代而成的化合物,例如在1分子中具有至 少1個Si-H鍵或C2_1Q烯基之直鏈狀或環狀的聚二苯基 氧烷等聚二芳基矽氧烷(較佳為聚二c"。芳基矽氧二; -36- 201229055 ^…具有至少WSl-H鍵或〜。稀基 狀的聚苯基甲基彻等聚烧基芳基彻(較佳= “!成基C6.2Q方基碎氧烧);以前述聚有㈣氧烧單 成之共聚物[二甲基石夕氧烧-甲基乙烯基石夕氧烧共聚物、 -甲基⑦氧^甲基苯基⑦氧烧共聚物、=甲基妙氧燒_ 基共聚物'二甲基石夕氧烧·甲美 乙烯基矽氧烷-甲基苯基矽氧烷共聚物等]等。上述例: 之聚石夕氧烧亦可具有支鏈。x,亦可使用對.雙(二甲芙 矽烷基)苯、對-雙(二曱基乙烯基矽烷基)笨等。 土 8 0萬者,較 範圍,貝》J易 上述聚矽氧烷的分子量可使用例如1〇〇〜 佳為100〜10萬。倘若聚矽氧烷的分子量為此 於相溶故較佳。 就上述化合物(B)而言,上述聚矽氧烷可單獨使用或 組合兩種以上使用。其Μ型的化合物⑻而言,較 佳為四甲基二石夕氧烷、六甲基三石夕氧烷、四甲基環四石夕 氧烷、含氫化矽烷基的聚矽氧、對_雙(二甲基矽烷基)苯 ,就乙烯基型的化合物(Β)而言,較佳為四曱基二乙烯基 矽氧烷、六甲基三矽氧烷、四甲基四乙烯基環四矽氧烷 、含乙烯基的聚矽氧、對_雙(二曱基乙烯基矽烷基)苯。 就本發明之硬化性樹脂組成物中包含之具有“汨鍵 的化δ物與具有C2.1Q烯基的化合物而言,亦可使用η型 的金屬矽氧烷化合物(Α)與對應之乙烯基型的金屬矽氧 烷化合物(Α)。 相對於金屬矽氧烷化合物(Α)丨00重量份,可使上述 化合物(B)的含量為例如〇〜1〇〇重量份,較佳為5〜6〇重 -37- 201229055 里伤倘右上述化合物(B)的含量為此範圍,則易於硬化 故較佳。當上述硬化性樹脂組成物中包含H型的金屬矽氧 烷化合物(A)與乙烯基型的金屬矽氧烷化合物(a)的雙方 時’可不使用上述化合物(B)。 本發明之硬化性樹脂組成物中亦可包含對應於上述 例不之Η型及乙烯基型的化合物之不含3丨_只鍵與烯基 的雙方之其他矽烷化合物。 本發明之硬化性樹脂組成物中之矽原子的含量例如 為1 〇 30重量%,較佳為1 〇〜20重量。/。。又,可使硬化性 杓知▲成物中之锆或鈦原子的含量為例如i〜丨0重量% 曰較佳為1〜5重量%。藉由使矽原子及鍅或鈦原子的含 $為如此fe圍’可提升將硬化性樹脂組成物硬化製得之 硬化物的耐熱無黃變性。 [氫化矽烷化觸媒(C)] 就本發明之硬化性樹脂組成物中包含的氫化矽烷化 觸媒(C)而言’有例示i系觸媒、料觸媒、纪系觸媒等 °的氫化矽烷化反應用觸媒,可具體列舉鉑微粉末、 鉑黑、載持鉑的二氧化矽微粉末 '載持鉑的活性碳、氣 化鈾酸、氣化翻酸與醇、酸、酮等的錯合物、始的稀烴 1。物鉑-羰基乙烯基甲基錯合物等鉑的羰基錯合物、 ――乙烯基四甲基二矽氧烷錯合物或鉑_環乙烯基曱基 夕氧烷錯合物等鉑乙烯基甲基矽氧烷錯合物、鉑-膦錯合 鉑亞磷馱鹽錯合物等鉑系觸媒、以及於上述鉑系觸 、中3有鈀原子或铑原子以取代鉑原子的鈀系觸媒或铑 觸媒。Μ可使用1種,亦可併用兩種以上。其中,始 -38- 201229055 稀土甲基石夕氧燒錯合物由於反應速度良好故較佳。 本&月之硬化性樹脂組成物中的氫化石夕烧化觸媒 (c)的含s係觸媒中的鉑、鈀或铑以重量單位計較佳為 〇.〇1〜U〇〇〇PPm的範圍内之量,更佳為0.1〜500ppm的範 圍内。當併用兩種以上時,氫化矽烷化觸媒(C)的含量係 j等合計的含量^倘若氫化矽烷化觸媒(C)的含量為如此 範圍,交聯速度不會顯著變慢,且在交聯物上產生著色 等問題之疑慮較少故較佳。 [氫化矽烷化反應抑制劑] 為了要調整氫化矽烷化反應的速度,本發明之硬化 性樹脂組成物中亦可含有氫化矽烷化反應抑制劑。就此 氫化矽烷化反應抑制劑而言,有例示3 _甲基_ 1 _ 丁炔3 醇、3,5·.二甲基己炔_3-醇、苯基丁炔醇等炔醇;3甲 基小戊稀I块、3,5-二曱基_3_己稀小块等烯块類化合 物,1’3,5,7-四甲基四乙烯基環四矽氧烷、 1,3,5,7-四曱基-1,3,5,7-四己烯基環四矽氧烷、苯并*** 。就此氫化矽烧化反應抑制劑的含量而言, 、 难规上述組 成物的交聯條件而異’但在實用上,相對 、 ^ %硬化性樹脂 組成物100重量份’較佳為0 00001〜5重詈 里置伤的範圍内。 [溶劑] 在氫化矽烷化反應時可使用曱苯、己 u况、異丙醇、 曱基異丁基酮、環戊酮、丙二醇單曱基醚乙酸酯等 周知的溶劑。 & [無機填充劑(D)] 本發明之硬化性樹脂組成物亦可進— v岜含無機填 -39- 201229055 無特別限定,但可 -氧化鈦、奈米氧化 雲母、合成雲母、 化鈦、鈦酸鋇、高 銘、碳化矽、氧化 珠、玻璃纖維、石 、纖維素等。此等 開第96/3 15 72號中 、電漿法等周知的 充劑。就無機填充劑(D)而言,雖 使用1種以上之奈米二氧化矽、奈米二 錯、奈米碳管、二氧化矽、氧化鋁、 滑石、氧化鈣、碳酸鈣、氧化鍅 '氧 嶺土、私土、矽藻土、氮化硼、氮化 鋅、氧化鈽、氧化铯、氧化鎂、玻璃 墨、氫氧化鈣、氳氧化鎂、氫氧化鋁 無機填充劑(D)可利用例如於國際公 s己載之火焰水解法或、火焰熱分解法 方法來製造。 就較佳的無機填充劑(D)而言,可使用奈米二氧化石夕 、奈米一氧化鈦、奈米氧化鍅、奈米碳管等經安定化之 膠體狀無機粒子的奈米分散溶膠類等,就市售品而言, 可取得BAYER公司製的二氧化矽溶膠、Goldschmidt公司 製的Sn〇2溶膠類、MERCK公司製的Ti〇2溶膠類、Nissan Chemicals公司製的Si〇2、Zr〇2、幻2〇3及Sb2〇3溶膠或 DEGUSSA公司製的Aer〇sil分散物類等市售品。無機填充 劑(D)必須不遮斷可見光。 無機填充劑(D)可藉由表面改質而使此等之黏度舉 動產生變化。可使用周知的表面改質劑進行粒子的表面 改質。就如此的表面改質劑而言,可使用例如存在於無 機填充劑(D)的表面上之可與官能基產生共價鍵或錯合 等相互作用的化合物或、可與聚合物基質相互作用的化 合物。就如此的表面改質劑而言,可使用例如在分子内 具有羧基、(1級、2級、3級)胺基、4級銨基、羰基、環 -40- 201229055 氧丙基、乙稀基、田 甲基丙烯醯氧基、靆基等官能基的化 ° n此的表面改質劑而言,通常由在標準溫产 及㈣件下為液態,且分子内的碳數為例如15:;度 較佳為ίο以下,特佳為8以下的低分子有機化合物所構成 :刚述低分子有機化合物的分子量例如為5〇〇以下,較佳 為3 50以下,特佳為2〇〇以下。 就較佳的表面改質劑而言,可列舉例如甲酸、乙酸 丙駄丁酉夂、戊酸、己酸、丙稀酸、甲基丙稀酸、丁 烯酸、檸檬酸、已二酸、丁二酸、戊二酸、草酸、順丁 稀二酸及& 丁稀二酸等碳數1〜12的飽和或不飽和一元 及多元酸類(較佳為一元酸類);及此等之醋類(較佳為甲 基丙稀酸甲基等Cl〜Ca基醋類);酿胺類;乙酸基丙酮 、2’己二酮、3,5_庚二酮、乙酿乙酸及Ci〜c4烧基乙醯 乙酸類等β-二羰基化合物等。又’雖無特別限定,但亦 可使用周知慣用的矽烷偶合劑作為表面改質劑。 無機填充劑(D)的粒徑通常為〇.〇lnm〜 2〇〇μιη左右 ,較佳為0.111111〜10(^„1、特佳為〇111111〜5(^111左右。 若將化合物(Α)及化合物(Β)的合計含量當作1〇〇重 量份’則無機填充劑(D)的含量較佳為i〜2〇〇〇重量份, 更佳為10〜1000重量份。又,相對於電子裝置用低透濕 性樹脂組成物的總量之無機填充劑(D)的含量例如為5〜 9 5重量%,較佳為丨〇〜9 〇重量。/〇。 [矽烷偶合劑(E)] 為『要提升與基板等被接著體之接著性等,本發明 之硬化性樹脂組成物亦可進一步包含;g夕院偶合劑(E)。石夕 -41- 201229055 烷偶合劑(E)並無特別限定,可使用周知慣用的矽烷偶合 劑。就矽烷偶合劑(E)而言,係由例如四曱氧基矽烷、2 乙氧基矽烷、曱基三乙氧基矽烷、二曱基二乙氧基矽烷 、曱基二乙氧基矽烷、乙烯基三乙氧基矽烷、乙烯基三 曱氧基矽烷、乙烯基參(曱氧基乙氧基矽烷)、苯基三^ 氧基矽烷、二苯基二甲氧基矽烷、乙烯基三乙醯氧基矽 烷、γ-甲基丙烯醯氧基丙基三乙氧基矽烷、γ·甲基丙烯醯 氧基丙基三曱氧基矽烷、γ·曱基丙烯醯氧基丙基曱基二 曱氧基矽烷、γ-曱基丙烯醯氧基丙基曱基二乙氧基矽烷 、3-環氧丙氧基丙基三曱氧基矽烷、3環氧丙氧基丙2 甲基二甲氧基矽烷、3_環氧丙氧基丙基三乙氧基矽烷、 3-環氧丙氧基丙基曱基二乙氧基矽烷、2(3,4_環氧基環 己基)乙基三甲氧基矽烷、對苯乙烯基三甲氧基矽烷、% 丙烯醯氧基丙基三甲氧基矽烷、1^(0_胺基乙基胺基 丙基曱基二甲氧基矽烷、Ν_(卜胺基乙基)_γ·胺基丙基甲 基二乙氧基矽烷、Ν-(β-胺基乙基)_γ_胺基丙基三甲氧基 矽烷、Ν-(β-胺基乙基)_γ_胺基丙基三乙氧基矽烷、ν苯 基-γ-胺基丙基三甲氧基矽烷、γ-胺基丙基三甲氧基矽烷 、γ-胺基丙基三乙氧基矽烷、3_毓基丙基三甲氧基矽烷 、3-毓基丙基三乙氧基矽烷、3_巯基丙基甲基二甲氧基 矽烷、雙(二乙氧基矽烷基丙基)四硫醚、3_異氰酸酯丙基 三乙氧基矽烷等在水溶液中相對上安定者之中選出。 在硬化性樹脂組成物中,矽烷偶合劑(Ε)的使用量較 佳為0.1 20重里%左右,更佳為〇 3〜8重量%,尤佳為〇 $ 〜5重量%的範圍。就未達〇1重量%而言,會缺乏石夕烧偶 -42- 201229055 合劑(E)所造成的樹脂之交聯效果,因此無法製得緻密的 膜,又缺乏對金屬基材的偶合效果,密著性差’會難以 獲得理想的耐鹼性與防銹力。當多於20重量%時,水解 所造成的耐水、耐鹼性等諸性能會顯著降低,在造膜性 上會產生問題,又易於在經濟性之點上變為不利。 [其他添加齊J ] 此外,本發明之硬化性樹脂組成物中亦可包含聚石夕 氧樹脂、環氧樹脂、氟樹脂等有機樹脂微粉末;銀、鋼 等導電性金屬粉末等填充劑、溶劑、安定化劑(抗氧化劑 、紫外線吸收劑、耐光安定劑、熱安定化劑等)、阻燃劑 (磷系阻燃劑、ii素系阻燃劑、無機系阻燃劑等)、阻燃 助劑、交聯劑、補強材料(其他填充劑等)、核劑、偶人 劑、蠟、塑化劑、脫模劑、耐衝擊改良劑、色細 π (又良劑 、流動性改良劑、著色劑(染料、顏料等)、分散劑 , 泡劑、脫泡劑、抗菌劑、防腐劑、黏度調整劑、 '肖 ^ & ^|| 、調平劑、離子吸著體、螢光體等慣用的添加劑 他任意的成分。此等之添加劑可單獨使用或為其 V祛® 。 D兩種以 ,更佳為0〜4(TC,特佳為室溫附近⑺〜3〇。〇左90 C 何溫度下為液態,故電子裝置的封裝、密:)的任 作業性優良。因此,可作為有機電致發光裝置二布時的 需要高折射率、低透濕性的電子構件用之J、LED等 劑等使用。又,亦可作為顯 '"劑、密封 或接著劑使用。 、用之塗布劑 -43- 201229055 [硬化性樹脂組成物的製法] 本發明之硬化性樹脂組成物可藉由將上述各成分均 勻地混合而製得。為了要製得本發明之硬化性樹脂組成 物,宜使用自公轉式攪拌脫泡裝置、均質機、行星式攪 拌機、3輥磨、珠磨等一般已知的混合用機器將各進行攪 掉、溶解、混合、分散等以使各成分盡量均勻。 [硬化物] 本發明之硬化性樹脂組成物可藉由光或熱而硬化。 當藉由光而硬化時,可用汞燈等進行1〇〇〇mJ/cm2以上的 光照射。又,當藉由熱而硬化時,可在溫度5〇〜2〇(rc、 較佳為50〜190t、更佳為50〜18(rc下,以硬化時間1〇 〜600分鐘,較佳為1〇〜48〇分鐘,更佳為15〜36〇分鐘進 行硬化。當硬化溫度與硬化時間低於上述範圍下限値時 ,硬化會不充分,反之高於上述範圍上限値時,因有時 會引起樹脂成分的分解,故會有均不佳的情形。硬化條 件雖依存於各種條件,但當硬化溫度高時,則可將硬化 時間適當調短,當硬化溫度低時,則可將硬化時間適當 調長。藉由使本發明之硬化性樹脂組成物硬化,可製得 氣泡 >、且透明性優良以及財熱無黃變性優良的硬化物。 本發明之硬化性樹脂組成物可作為有機電致發光裝置、 L E D或顯示器等封裝劑、密封劑或塗布劑使用。 [實施例] 以下基於實施例更詳細地說明本發明,但本發明並 不因此等之實施例而受限。 實施例1 -44 - 201229055 在具備授拌機、溫度計、戴氏冷凝管、滴下漏斗之 玻璃製的燒瓶中遇合3.30g(25mmol)的二甲氧基甲基乙 烯基矽烷(東京化成公司製D3386)與23.40g(50mmol 70 wt%正丙醇溶液)的正丙氧基化鍅(東京化成公司製 Z0 017)、300g的正丙醇,並在-3〇。〇以下以乾燥曱醇浴進 行冷卻。接著將0.54g(30mmol)的離子交換水與40g的正 丙醇混合而成的液態以使内溫不超過_ 3 〇 〇c的方式徐徐 地滴下。滴下結束後’使内溫回到室溫’然後升溫至8〇。〇 搜拌3小時。反應結束後’自然冷卻至室溫,並藉由蒸發 器將未反應成分、揮發成分餾除。在其濃縮後之液態中 添加100g的甲苯、51.8g(380mmol)的三乙基矽烷醇(東京 化成公司製T2017),並在8(TC下攪拌2小時。反應結束 後’自然冷卻至室溫並藉由蒸發器將未反應成分、揮發 成分館除而製得液狀含乙烯基的锆矽氧烷。 實施例2 在〇 · 2 g的實施例1中製得之液狀含乙稀基的锆矽氧 烧中’添加〇 . 4 μ 1的鉑觸媒,然後添加〇 . 〇 8 4 g的氫化;ε夕烧 基末端聚矽氧(Gelest公司製DMS-H03,分子量400-500) 並混δ 。將該混合液塗布於玻璃板上’並在供箱中以 60 C 1小時、1 20°c 3小時使其硬化。在硬化物中沒有看到 氣泡’又即使靜置於1 8〇t的烘箱中500小時以上仍然無 色透明。 [產業利用性] 若利用本發明之金屬矽氧烷化合物,當將包含該金 屬石夕氧境化合物的硬化性樹脂組成物硬化時,未產生逸 -45- 201229055 出氣體,又,由於將該硬化性樹脂組成物硬化而製得之 硬化物具有優良的耐熱無黃變性,故對LED等電子裝置 的封裝劑或密封劑、耐熱硬被覆等而言乃為有用。 【圖式簡單說明】 無。 【主要元件符號說明】 無0 -46-^, octagonal zeolite, etc.), solid acid such as ion exchange resin (such as cation exchange resin such as H type). The amount of the acid catalyst and the alkali catalyst to be used is not particularly limited, and is, for example, 1 to 5 moles per hydroxy group of the reaction system, preferably 〇i 2 to 2 moles, more preferably 0.8. ~12 m or so. Further, when an acid catalyst or an alkali catalyst is not used, the reaction can be promoted by heating or the like. The reaction can be carried out in the presence of a polymerization inhibitor. The reaction temperature can be appropriately selected depending on the kind of the reaction component or the catalyst, and the like, for example, 20 to 200 when ethylene decane is used. 〇, preferably 20 to 1 〇 (TC, more preferably about 4 〇 to 6 〇 ° C. Further, when hydrogenated decane is used, the reaction temperature can be appropriately selected depending on the kind of the reaction component or the catalyst, etc., for example, _ 78~ii〇(>c, preferably -30~40°c, more preferably _10~1 (about rc. The reaction can be carried out under normal pressure, or under reduced pressure or under pressure. The reaction gas atmosphere is not particularly limited, and may be, for example, an air gas atmosphere, a nitrogen gas atmosphere, an argon gas atmosphere, etc. Further, the reaction may be carried out by any method such as batch type, semi-batch type, or continuous type. After the completion of the reaction, the reaction product can be separated by, for example, transition, concentration, distillation, extraction, crystallization, recrystallization, column chromatography, etc., by hand-34-201229055, or a combination thereof. Separation and purification can be carried out by adding water, 7% to 7 % of dilute hydrochloric acid, and 7% to 7 % of baking soda water to the water after the reaction. [Cure resin composition j. The curable resin composition contains a compound having a Si-H bond and has a C2-1G The curable resin composition of the compound of the base is characterized in that it contains at least the above metal siloxane compound (A) and a hydrogenated decylation catalyst (C). The metal siloxane compound (A) is in a curable resin composition. 3畺 is, for example, 3 〇 to 9 9 wt. /〇, preferably 5 〇 to 8 〇% by weight 〇 The curable resin composition of the present invention may contain a compound other than the metal siloxane compound (A). a compound having at least one si H bond or a C 2-10 alkenyl group in the molecule (when the metal oxoxane compound is an n-type compound, the curable resin composition contains at least one C2.1Q in one molecule) Alkenyl compound (Β) [vinyl type compound, when the metal siloxane compound (Α) is a vinyl type compound, the curable resin composition contains at least one Si-H bond in one molecule. Compound (b) [ Compound (B) of type h] [Compound (B) having at least i Si-H bond or Cno alkenyl group in an anthracene molecule other than the metal oxoxane compound (A)] For the compound of the type or the vinyl type (B), it can be used in the industrial molecule to have Having a Si_H bond or a Gw alkenyl group and having an n-type or a vinyl type polyoxo-oxygenate having a main chain composed of a decane bond (Si-0-Si). In the case of a C2_10 alkenyl group, The exemplified by the above-mentioned decane compound is exemplified as the C2_1G alkenyl group. Specific examples of the polyoxyalkylene oxide are linear-35-201229055-like, branched or cyclic fluorene oxides having cross-linking. The three-dimensional structure of the polyoxyxene resin, etc. Specific examples of the above compound (B) include tetradecyl oxalate, tetradecyldiethyl oxime, hexamethyltrioxane, Hexamethyldivinyltrioxane, heptamethyltrioxane, heptaylvinyltrioxetane, octamethyltetraoxane, octadecyldivinyltetrahydroxanthine, nine Tetraoxane, hexamethylvinyltetraoxane, hexamethyldivinyltetraoxane, decamethylpentaoxane, decamethyldivinylpentaoxane, undecylmethyl Pentaoxanes, undecylvinylpentaoxane, decamethyldivinylpentaoxane, etc., having 1 to 10 (preferably 2 to 5) (Si-O) units a chain polyglyoxiyl oxane, a hydrazine group containing a hydrazinyl group, a polyfluorene containing a vinyl group, or the like, and a linear poly 2 having at least one Si—H bond or C 2 —1 G alkenyl group in one molecule An alkyl oxane (preferably a linear polydioxane alkyl oxane); dimethylcyclotrioxane, dimethyldivinylcyclotrioxane, tetradecyl ring four a decane, a tetradecyltetravinylcyclotetraoxane, a trimethylcyclopentaoxane, a trimethyltrivinylcyclopentaoxane, or the like, having 2 to 10 (preferably 2 to 5) (i) (i) (7) unit of a cyclic polydialkyl decane having at least one cyclic polydidecyl fluorene oxide having a bond or an alkenyl group in the fluorene molecule (preferably a cyclic poly ci- Ίο alkyl oxane) and the like. And a compound obtained by substituting all or a part of an alkyl group such as a fluorenyl group of the compound exemplified by an aryl group such as a phenyl group (preferably a fluorenyl (1) aryl group), for example, at least one Si in one molecule. a polydiaryl fluorene oxide such as a linear or cyclic polydiphenyl oxyalkyl group having a H bond or a C2_1Q alkenyl group (preferably a poly-c" aryl fluorene oxide; -36- 201229055 ^... At least WSl-H bond or ~. Dense base polyphenylmethyl ruthenium aryl thiolate (preferably = "! base C6.2Q square base oxy-combustion"; with the above-mentioned poly(tetra) oxy-fired Mono-form copolymer [dimethyl oxazepine-methyl vinyl oxalate copolymer, -methyl 7 oxy-methylphenyl 7 oxy-copolymer, = methyloxo-based copolymer 'Dimethyl oxime-oxygen-methyl-vinyl oxirane-methylphenyl decane copolymer, etc.'. The above example: poly-stone oxy-sinter can also have a branch. x can also be used . bis (dimethyl fluorenyl) benzene, p- bis (didecyl vinyl decyl) stupid, etc. The soil of 80,000, the range, the molecular weight of the polypyroxane can be used, for example 1〇〇~ Good for 100~100,000. In the case of the above compound (B), the above polysiloxanes may be used singly or in combination of two or more. In the case of the quinoid compound (8), Preferably, it is tetramethyl diazepine, hexamethyl tripotax, tetramethylcyclotetrazepine, polyfluorene oxide containing hydrazine hydride, p-bis(dimethyl decyl) benzene, In the case of a vinyl type compound (Β), tetrakisyldivinyl fluorene oxide, hexamethyltrioxane, tetramethyltetravinylcyclotetraoxane, vinyl-containing poly are preferable. Oxide, p-bis(dimercaptovinyl fluorenyl) benzene. The δ bond having a hydrazone bond and a compound having a C2.1Q alkenyl group are also contained in the curable resin composition of the present invention. The n-type metal oxoxane compound (Α) and the corresponding vinyl type metal oxane compound (Α) can be used. The above compound (B) can be obtained with respect to the metal siloxane compound (Α) 丨 00 parts by weight. The content of the compound is, for example, 〇~1〇〇 by weight, preferably 5~6〇, -37-201229055, and the above compound (B) When the content is in this range, it is easy to be hardened. When the curable resin composition contains both the H-type metal siloxane compound (A) and the vinyl-type metal siloxane compound (a) The above-mentioned compound (B) may not be used. The curable resin composition of the present invention may further contain other compounds which do not contain 3丨_bond and alkenyl group corresponding to the above-mentioned examples of the oxime type and the vinyl type. The content of the ruthenium atom in the curable resin composition of the present invention is, for example, 1 〇 30% by weight, preferably 1 〇 to 20% by weight. Further, the sclerosing property can be known as ▲ The content of zirconium or titanium atoms is, for example, i to 丨0% by weight 曰, preferably 1 to 5% by weight. The heat-resistant and non-yellowing of the cured product obtained by hardening the curable resin composition can be improved by making the content of the ruthenium atom and the ruthenium or titanium atom such that it is so. [Hydrogenated decylation catalyst (C)] The hydrogenated decylation catalyst (C) contained in the curable resin composition of the present invention is exemplified as an i-type catalyst, a catalyst, a catalyst, and the like. The catalyst for hydrogenation oximation reaction, specifically, platinum fine powder, platinum black, platinum-loaded ceria micropowder, platinum-carrying activated carbon, vaporized uranium acid, gasification acid and alcohol, acid, A complex of a ketone or the like, and a starting hydrocarbon 1 . a platinum carbonyl complex such as a platinum-carbonylvinylmethyl complex, a vinyl tetramethyldioxane complex or a platinum-cyclovinyl fluorenyl alkane complex a platinum-based catalyst such as a methyl oxoxane complex, a platinum-phosphine-substituted platinum phosphite complex, and a palladium having a palladium atom or a ruthenium atom in place of the platinum atom in the above-mentioned platinum-based touch Catalyst or catalyst. Μ One type may be used, or two or more types may be used in combination. Among them, the -38-201229055 rare earth methyl oxo-oxygenated complex is preferred because of its good reaction rate. The platinum, palladium or rhodium in the s-containing catalyst of the hydrogenated calcined catalyst (c) in the hardening resin composition of the present & month is preferably 〇.〇1 to U〇〇〇PPm. The amount within the range is more preferably in the range of 0.1 to 500 ppm. When two or more kinds are used in combination, the content of the hydrogenated decylation catalyst (C) is a total amount of j, etc., and if the content of the hydrogenated decylation catalyst (C) is in such a range, the crosslinking rate does not significantly slow down, and It is preferable that there are fewer doubts about the occurrence of coloring and the like on the crosslinked product. [Hydrogenation reaction of the alkylation reaction] In order to adjust the rate of the hydrogenation reaction, the hardenable resin composition of the present invention may further contain a hydrogenation reaction inhibitor. In the case of the hydrogenation sulfonation reaction inhibitor, there are exemplified acetylene alcohols such as 3 _methyl _ 1 -butyne 3 alcohol, 3,5·. dimethylhexyne-3-ol, phenylbutynol; An alkene block compound such as a small pentane block, a 3,5-diindenyl _3_hexamide block, 1'3,5,7-tetramethyltetravinylcyclotetraoxane, 1,3 , 5,7-tetradecyl-1,3,5,7-tetrahexenylcyclotetraoxane, benzotriazole. The content of the hydrogenated cesium-sintering reaction inhibitor differs depending on the crosslinking conditions of the above composition. However, in practice, the relative % of the curable resin composition is preferably 100 parts by weight. Within the range of injury. [Solvent] A known solvent such as toluene, hexyl alcohol, isopropyl alcohol, decyl isobutyl ketone, cyclopentanone or propylene glycol monodecyl ether acetate can be used in the hydrogenation reaction. & [Inorganic Filler (D)] The curable resin composition of the present invention may also be incorporated into the v-containing inorganic filler-39-201229055 without particular limitation, but may be - titanium oxide, nano-oxidized mica, synthetic mica, Titanium, barium titanate, Gaoming, tantalum carbide, oxidized beads, glass fiber, stone, cellulose, and the like. These are known as the filling agents in the 96/3 15 72, the plasma method. In the case of the inorganic filler (D), one or more kinds of nano cerium oxide, nano erbium, carbon nanotubes, cerium oxide, aluminum oxide, talc, calcium oxide, calcium carbonate, cerium oxide are used. Oxygen, soil, diatomaceous earth, boron nitride, zinc nitride, cerium oxide, cerium oxide, magnesium oxide, glass ink, calcium hydroxide, barium magnesium oxide, aluminum hydroxide inorganic filler (D) can be utilized For example, it is manufactured by a flame hydrolysis method or a flame thermal decomposition method which is carried out by the international public. For the preferred inorganic filler (D), nano-dispersion of colloidal inorganic particles such as nano-sized cerium oxide, nano-titanium oxide, nano-cerium oxide, and carbon nanotubes can be used. As a commercial product, a cerium oxide sol manufactured by BAYER, a Sn 〇 2 sol manufactured by Goldschmidt, a Ti 〇 2 sol manufactured by MERCK, and a Si 〇 2 manufactured by Nissan Chemicals Co., Ltd. are available as a commercial product. Commercial products such as Zr〇2, Magic 2〇3, and Sb2〇3 sol or Aer〇sil dispersions manufactured by DEGUSSA. The inorganic filler (D) must not block visible light. The inorganic filler (D) can be modified by surface modification to effect such viscosity behavior. The surface modification of the particles can be carried out using a well-known surface modifier. In the case of such a surface modifier, for example, a compound which may exist on the surface of the inorganic filler (D) to cause a covalent bond or a mismatch with a functional group or the like may interact with the polymer matrix. compound of. In the case of such a surface modifier, for example, a carboxyl group, a (grade 1, 2, 3) amine group, a 4-stage ammonium group, a carbonyl group, a ring-40-201229055 oxypropyl group, ethylene group can be used in the molecule. The surface modifier of the methacrylic acid methoxy group or the fluorenyl group is usually liquid in the standard temperature production and (4), and the carbon number in the molecule is, for example, 15: The degree of the low molecular organic compound is preferably 5% or less, and the molecular weight of the low molecular organic compound is, for example, 5 Å or less, preferably 3 50 or less, and particularly preferably 2 Å or less. As preferred surface modifiers, for example, formic acid, acetobutyl acetate, valeric acid, caproic acid, acrylic acid, methyl acrylate, crotonic acid, citric acid, adipic acid, and butyl are exemplified. a saturated or unsaturated mono- and polybasic acid (preferably a monobasic acid) having a carbon number of 1 to 12, such as diacid, glutaric acid, oxalic acid, cis-succinic acid, and & succinic acid; and vinegars thereof (preferably, Cl~Ca-based vinegar such as methyl propyl acid methyl group); brewing amine; acetic acid acetone, 2' hexanedione, 3,5-heptanedione, ethyl acetate, and Ci~c4 A β-dicarbonyl compound such as an acetic acid or the like. Further, although it is not particularly limited, a well-known decane coupling agent can be used as the surface modifier. The particle size of the inorganic filler (D) is usually about 〇1 nm to 2 〇〇μιη, preferably 0.111111 to 10 (^1, particularly preferably 〇111111~5 (^111 or so. If the compound (Α) And the total content of the compound (Β) is regarded as 1 part by weight', and the content of the inorganic filler (D) is preferably i 2 parts by weight or more, more preferably 10 to 1000 parts by weight. The content of the inorganic filler (D) in the total amount of the low moisture-permeable resin composition for an electronic device is, for example, 5 to 9.5 wt%, preferably 丨〇 9 9 〇. / 〇 [矽 偶 coupling agent ( E)] The curable resin composition of the present invention may further contain a grafting agent (E), which is to be improved in adhesion to a substrate such as a substrate, etc. (E). Shi Xi-41-201229055 Alkane coupling agent ( E) is not particularly limited, and a conventionally used decane coupling agent can be used. For the decane coupling agent (E), for example, tetradecyloxydecane, 2 ethoxy decane, decyltriethoxydecane, and Mercapto diethoxy decane, decyl diethoxy decane, vinyl triethoxy decane, vinyl trimethoxy decane, vinyl ginseng (methoxy ethoxy decane), phenyl trimethoxy decane, diphenyl dimethoxy decane, vinyl triethoxy decane, γ-methyl propylene methoxy propyl triethoxy矽, γ·methacryloxypropyltrimethoxy decane, γ·mercapto propylene methoxypropyl decyl decyloxy decane, γ-mercapto propylene methoxy propyl fluorenyl diethyl Oxydecane, 3-glycidoxypropyltrimethoxydecane, 3epoxypropoxypropane 2 methyldimethoxydecane, 3_glycidoxypropyltriethoxydecane, 3-glycidoxypropylmercaptodiethoxydecane, 2(3,4-epoxycyclohexyl)ethyltrimethoxydecane, p-styryltrimethoxydecane, % propylene decyloxy Propyltrimethoxydecane, 1^(0-aminoethylaminopropylmercaptodimethoxydecane, Ν-(iaminoethyl)_γ-aminopropylmethyldiethoxydecane, Ν-(β-Aminoethyl)_γ-aminopropyltrimethoxydecane, Ν-(β-aminoethyl)_γ-aminopropyltriethoxydecane, νphenyl-γ-amine Propyltrimethoxydecane, γ-aminopropyltrimethoxydecane, γ-amine Propyltriethoxydecane, 3-mercaptopropyltrimethoxydecane, 3-mercaptopropyltriethoxydecane, 3-mercaptopropylmethyldimethoxydecane, bis(diethoxy The alkyl propyl) tetrasulfide, 3-isocyanate propyl triethoxy decane, and the like are selected among those relatively stable in an aqueous solution. In the curable resin composition, the amount of the decane coupling agent (Ε) is used. Preferably, it is 0.120% by weight, more preferably 〜3~8wt%, especially preferably 〇$~5wt%. If it is less than 1% by weight, it will lack Shixi Shaotong-42- 201229055 The cross-linking effect of the resin caused by the mixture (E) makes it impossible to obtain a dense film, and lacks the coupling effect on the metal substrate, and the poor adhesion is difficult to obtain the desired alkali resistance and rust resistance. When it is more than 20% by weight, the properties such as water resistance and alkali resistance caused by the hydrolysis are remarkably lowered, problems occur in the film forming property, and it is easy to become unfavorable at the point of economy. [Other additions] The curable resin composition of the present invention may further contain a fine powder of an organic resin such as a polysulfide resin, an epoxy resin or a fluororesin, or a filler such as a conductive metal powder such as silver or steel. Solvent, stabilizer (antioxidant, UV absorber, light stabilizer, heat stabilizer), flame retardant (phosphorus flame retardant, ii flame retardant, inorganic flame retardant, etc.), resistance Fuel additives, cross-linking agents, reinforcing materials (other fillers, etc.), nucleating agents, dolls, waxes, plasticizers, mold release agents, impact modifiers, color π (also good, fluidity improvement) Agent, colorant (dye, pigment, etc.), dispersant, foaming agent, defoaming agent, antibacterial agent, preservative, viscosity modifier, 'Shaw ^ & ^|| , leveling agent, ion sorbent, firefly A customary additive such as a light body, any of its constituents. These additives can be used alone or as V祛®. D is more preferably 0 to 4 (TC, particularly preferably around room temperature (7) to 3 〇. 〇Left 90 C is liquid at any temperature, so the packaging and density of the electronic device are excellent. Therefore, it can be used as an electronic component for high refractive index and low moisture permeability, such as J, LED, etc., in the case of an organic electroluminescence device, and can also be used as an agent, seal or adhesive. Use and coating agent-43-201229055 [Preparation method of curable resin composition] The curable resin composition of the present invention can be obtained by uniformly mixing the above components. In order to obtain the hardening of the present invention. The resin composition should be stirred, dissolved, mixed, dispersed, etc., using a generally known mixing machine such as a revolving stirring defoaming device, a homogenizer, a planetary mixer, a 3-roll mill, or a bead mill. The hardened resin composition of the present invention can be cured by light or heat. When it is cured by light, it can be irradiated with light of 1 〇〇〇mJ/cm 2 or more with a mercury lamp or the like. Further, when hardened by heat, it can be at a temperature of 5 〇 2 〇 (rc, preferably 50 to 190 ts, more preferably 50 〜 18 (rc, with a hardening time of 1 〇 to 600 minutes, preferably Harden for 1〇~48〇 minutes, preferably 15~36〇 minutes. When the hardening temperature and the hardening time are lower than the lower limit of the above range, the hardening may be insufficient, and if it is higher than the upper limit of the above range, the decomposition of the resin component may occur, which may cause poorness. Under various conditions, when the curing temperature is high, the curing time can be appropriately shortened, and when the curing temperature is low, the curing time can be appropriately lengthened. By curing the curable resin composition of the present invention, it can be produced. A cured product having excellent transparency and excellent heat and no yellowing property is obtained. The curable resin composition of the present invention can be used as an encapsulant, an encapsulant or a coating agent for an organic electroluminescence device, an LED or a display. [Examples] Hereinafter, the present invention will be described in more detail based on the examples, but the present invention is not limited by the examples. Example 1 -44 - 201229055 A 3.30 g (25 mmol) of dimethoxymethylvinyl decane (D3386, manufactured by Tokyo Chemical Industry Co., Ltd.) was placed in a glass flask equipped with a mixer, a thermometer, a Dairy condenser, and a dropping funnel. And n-propoxylated hydrazine (Z0 017, manufactured by Tokyo Chemical Industry Co., Ltd.), 23.40 g (50 mmol, 70 wt% n-propanol solution), 300 g of n-propanol, and at -3 Torr. The following is cooled in a dry decyl bath. Next, a liquid state in which 0.54 g (30 mmol) of ion-exchanged water and 40 g of n-propanol were mixed was dripped so that the internal temperature did not exceed _ 3 〇 〇c. After the end of the dropping, the internal temperature was returned to room temperature and then the temperature was raised to 8 Torr.搜 Search for 3 hours. After the completion of the reaction, the mixture was naturally cooled to room temperature, and the unreacted components and volatile components were distilled off by an evaporator. 100 g of toluene and 51.8 g (380 mmol) of triethyl stanol (T2017, manufactured by Tokyo Chemical Industry Co., Ltd.) were added to the liquid liquid after concentration, and the mixture was stirred at 8 (TC for 2 hours). After the reaction, it was naturally cooled to room temperature. The liquid-containing vinyl group-containing zirconium hydride was obtained by removing the unreacted component and the volatile component by an evaporator. Example 2 Liquid biphenyl group obtained in Example 1 of 〇·2 g Zirconium-oxygenation in the 'addition of 〇. 4 μ 1 of platinum catalyst, then add 〇. 〇 8 4 g of hydrogenation; ε 烧 末端 end poly 矽 oxygen (DMS-H03 manufactured by Gelest, molecular weight 400-500) And δ was mixed. The mixture was applied to a glass plate 'and hardened in a box at 60 C for 1 hour and 1200 ° C for 3 hours. No bubbles were observed in the hardened material' and even placed in the chamber 1 In the oven of 8 〇t, it is still colorless and transparent for more than 500 hours. [Industrial Applicability] When the metal siloxane compound of the present invention is used, when the curable resin composition containing the metal cerium compound is hardened, it is not produced.逸-45- 201229055 A gas is produced, which is obtained by hardening the curable resin composition. The cured product has excellent heat resistance and no yellowing property, so it is useful for encapsulants or sealants for electronic devices such as LEDs, heat-resistant hard coatings, etc. [Simple description of the drawing] None. [Main component symbol description] None 0 - 46-

Claims (1)

201229055 七、申請專利範圍: 1_ 一種金屬矽氧烷化合物 下列式(1) R1 I X1 — Si — X2 I R2 特徵為:係藉由歷經使以 C1-1G烷基、 係相同或不 (式中,R,R2係相同或不同,表示氫原子、 C2.丨〇烯基、C6.丨4芳基或C7丨5芳烷基;χ丨,X2 同,表不q·丨〇烷氧基、鹵素原子或羥基) 表示之石夕3烷化合物(s 1)與以下列式(2) (2) Y1 — Μ — Y4 I Υ2 (式中,Μ表示鍅或鈦;γ1〜γ4係相同或不同,表示Cl。 烷氧基或鹵素原子) 表示之金屬化合物(M)進行反應或使該矽烷化合物 與該金屬化合物(M)與HA進行反應的第i步驟; 使該第13步驟的反應生成物與以下列式(3) I X3 — Si — R5 I (3) R4 (式中’ R3〜R5係相同或不同,表示氫原子、Ci 1〇烷基 、C2·10婦基、C6-14芳基或C7_15芳烷基;X3表示(^-10烷 氧基、幽素原子或羥基) 表示之石夕貌化合物(S2)進行反應或使該第i步驟的反應 生成物與該矽烷化合物(S2)與H2〇進行反應的第2步驟 而製得’以該矽烷化合物(S 1):該金屬化合物(M):該 -47- 201229055 矽烷化合物(S2):第1步驟的h2〇:第2步驟的H20 = m: n . k _ a . b之莫耳比,且在m . n ^ , a , b滿足以下關係 (i)〜(V)的全部條件下進行反應而製造,且在1分子中具 有至少1個Si-H鍵或C2_1〇烯基, (i) m> 0,n> 05k> 〇,a^ 〇,b^ 〇 (ii) n/m^ 3 (iii) (a + am)/(m + n) = 〇.〇3〜〇 8 (iv) (ah-(2a + am)} (v) 當X3為烷氧基或鹵素原子時,bg k ;當X3為羥 基時,b=0 (上述式中,當χ!,χ2同時為羥基時,“七係am=2m,ah = 4n :當僅X、X2的任一者為羥基時,am = m,ah = ni + 4n ;當 X,X 同時非羥基時,am = 〇,ah = 2m + 4n)。 2.如申請專利範圍第丨項之金屬矽氧烷化合物,其在〇〜 90°C的任何溫度下為液態。 3 · —種硬化性樹脂組成物,其係包含具有s丨_ H鍵的化合 物與具有C2_1G烯基的化合物之硬化性樹脂組成物,其 特徵為:至少含有如申請專利範圍第丨或2項之金屬矽 氧烧化合物(A)與氫化矽烧化觸媒(c)。 4.如申請專利範圍第3項之硬化性樹脂組成物,其進一步 含有無機填充劑(D)。 5·如申請專利範圍第3或4項之硬化性樹脂組成物其進 一步含有矽烷偶合劑(E)。 6.一種硬化物,其係將如申請專利範圍第3至5項甲任一 項之硬化性樹脂組成物硬化而成。 -48- 201229055 四、指定代表圖: (一) 本案指定代表圖為:無。 (二) 本代表圖之元件符號簡單說明: 無0 五、本案若有化學式時,請揭示最能顯示發明特徵的化學式:201229055 VII. Patent application scope: 1_ A metal oxane compound The following formula (1) R1 I X1 — Si — X2 I R2 is characterized by: by C1-G alkyl group, the same or not (in the formula , R, R2 are the same or different and represent a hydrogen atom, C2. nonenyl, C6. 丨4 aryl or C7 丨5 aralkyl; χ丨, X2 is the same, represents q·decyloxy, The halogen atom or the hydroxyl group) is represented by the following formula (2) (2) Y1 - Μ - Y4 I Υ 2 (wherein Μ represents yttrium or titanium; γ1 γ γ4 is the same or different And the i-th step of reacting the metal compound (M) with the metal compound (M) or reacting the decane compound with the metal compound (M) and HA; and the reaction product of the thirteenth step It is the same as or different from the formula (3) I X3 — Si — R5 I (3) R4 (wherein R 3 to R 5 are the same or different, and represent a hydrogen atom, a Ci 1 alkyl group, a C 2 · 10 base group, and a C 6-14 aromatic group. Or a C7_15 aralkyl group; X3 represents a (^-10 alkoxy group, a crypto atom or a hydroxy group), and the compound (S2) is reacted or made The second step of the reaction product of the i step and the reaction of the decane compound (S2) with H2 hydrazine to produce 'the decane compound (S 1): the metal compound (M): the -47-201229055 decane compound ( S2): h2〇 of the first step: H20 of the second step = m: n. k _ a. The molar ratio of b, and in m. n ^ , a , b satisfy the following relationship (i) ~ (V) It is produced by carrying out a reaction under all conditions, and has at least one Si-H bond or C2_1 nonenyl group in one molecule, (i) m > 0, n > 05k > 〇, a^ 〇, b^ 〇 (ii n/m^ 3 (iii) (a + am) / (m + n) = 〇.〇3~〇8 (iv) (ah-(2a + am)} (v) when X3 is alkoxy or In the case of a halogen atom, bg k ; when X3 is a hydroxyl group, b=0 (in the above formula, when χ!, χ2 is also a hydroxyl group, "seven systems am=2m, ah = 4n: when only X, X2 When it is a hydroxyl group, am = m, ah = ni + 4n; when X, X are non-hydroxy at the same time, am = 〇, ah = 2m + 4n). 2. The metal oxirane compound according to the scope of claim It is liquid at any temperature of 〇 ° 90 ° C. 3 · A kind of hardening resin composition containing a combination of s丨_ H bonds A curable resin composition of a compound having a C2_1G alkenyl group, characterized by comprising at least a metal oxy-oxygen compound (A) and a hydrogenated cesium-burning catalyst (c) as claimed in claim 2 or 2. 4. The curable resin composition of claim 3, which further comprises an inorganic filler (D). 5. The curable resin composition as claimed in claim 3 or 4 further contains a decane coupling agent (E). A cured product obtained by hardening a curable resin composition according to any one of claims 3 to 5 of the patent application. -48- 201229055 IV. Designated representative map: (1) The representative representative of the case is: None. (2) A brief description of the symbol of the representative figure: None 0. If there is a chemical formula in this case, please disclose the chemical formula that best shows the characteristics of the invention:
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