TW202402956A - 具有陶瓷微球體之有機聚矽氧烷組成物 - Google Patents
具有陶瓷微球體之有機聚矽氧烷組成物 Download PDFInfo
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- 239000000203 mixture Substances 0.000 title claims abstract description 43
- 229920001296 polysiloxane Polymers 0.000 title claims abstract description 30
- 239000000919 ceramic Substances 0.000 title claims abstract description 29
- 239000004005 microsphere Substances 0.000 title 1
- 239000002245 particle Substances 0.000 claims abstract description 39
- -1 polysiloxanes Polymers 0.000 claims abstract description 31
- 239000003063 flame retardant Substances 0.000 claims abstract description 11
- 229920000435 poly(dimethylsiloxane) Polymers 0.000 claims description 13
- 239000004205 dimethyl polysiloxane Substances 0.000 claims description 11
- 238000006116 polymerization reaction Methods 0.000 claims description 10
- LYCAIKOWRPUZTN-UHFFFAOYSA-N Ethylene glycol Chemical compound OCCO LYCAIKOWRPUZTN-UHFFFAOYSA-N 0.000 claims description 9
- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 claims description 7
- 239000003054 catalyst Substances 0.000 claims description 7
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 claims description 5
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- WGCNASOHLSPBMP-UHFFFAOYSA-N hydroxyacetaldehyde Natural products OCC=O WGCNASOHLSPBMP-UHFFFAOYSA-N 0.000 claims description 5
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- 229910018072 Al 2 O 3 Inorganic materials 0.000 claims description 2
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- 229910017089 AlO(OH) Inorganic materials 0.000 claims description 2
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- CSNNHWWHGAXBCP-UHFFFAOYSA-L Magnesium sulfate Chemical compound [Mg+2].[O-][S+2]([O-])([O-])[O-] CSNNHWWHGAXBCP-UHFFFAOYSA-L 0.000 description 2
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- FSIJKGMIQTVTNP-UHFFFAOYSA-N bis(ethenyl)-methyl-trimethylsilyloxysilane Chemical compound C[Si](C)(C)O[Si](C)(C=C)C=C FSIJKGMIQTVTNP-UHFFFAOYSA-N 0.000 description 2
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- 125000003903 2-propenyl group Chemical group [H]C([*])([H])C([H])=C([H])[H] 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-M Bicarbonate Chemical compound OC([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-M 0.000 description 1
- 229920002799 BoPET Polymers 0.000 description 1
- 125000004648 C2-C8 alkenyl group Chemical group 0.000 description 1
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical class [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 1
- BVKZGUZCCUSVTD-UHFFFAOYSA-L Carbonate Chemical compound [O-]C([O-])=O BVKZGUZCCUSVTD-UHFFFAOYSA-L 0.000 description 1
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- JYYOBHFYCIDXHH-UHFFFAOYSA-N carbonic acid;hydrate Chemical compound O.OC(O)=O JYYOBHFYCIDXHH-UHFFFAOYSA-N 0.000 description 1
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- 239000007795 chemical reaction product Substances 0.000 description 1
- 230000000052 comparative effect Effects 0.000 description 1
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- 239000000446 fuel Substances 0.000 description 1
- 238000005227 gel permeation chromatography Methods 0.000 description 1
- 230000017525 heat dissipation Effects 0.000 description 1
- 238000006459 hydrosilylation reaction Methods 0.000 description 1
- 239000011261 inert gas Substances 0.000 description 1
- 229910052809 inorganic oxide Inorganic materials 0.000 description 1
- 229910052943 magnesium sulfate Inorganic materials 0.000 description 1
- 235000019341 magnesium sulphate Nutrition 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000001247 metal acetylides Chemical class 0.000 description 1
- 229910000000 metal hydroxide Inorganic materials 0.000 description 1
- 150000004692 metal hydroxides Chemical class 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- CKFGINPQOCXMAZ-UHFFFAOYSA-N methanediol Chemical compound OCO CKFGINPQOCXMAZ-UHFFFAOYSA-N 0.000 description 1
- 239000013518 molded foam Substances 0.000 description 1
- 150000004767 nitrides Chemical class 0.000 description 1
- 238000013021 overheating Methods 0.000 description 1
- 229920002223 polystyrene Polymers 0.000 description 1
- 239000011148 porous material Substances 0.000 description 1
- 238000000634 powder X-ray diffraction Methods 0.000 description 1
- 230000035939 shock Effects 0.000 description 1
- 125000006850 spacer group Chemical group 0.000 description 1
- 230000001960 triggered effect Effects 0.000 description 1
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Abstract
本發明係關於一種組成物,其包含反應性聚矽氧烷及含羥基前驅物、阻燃劑、及微米尺寸之中空陶瓷粒子。該組成物可用於製備可用於向諸如鋰離子電池組之應用提供熱絕緣、耐燃性、及可壓縮性之絕緣、可壓縮、及耐燃性發泡材料。
Description
本發明係關於一種含有微米尺寸的陶瓷粒子之有機聚矽氧烷組成物。
可充電鋰離子電池組(lithium-ion battery, LiB)常用於包括電動車(electric vehicle, EV)及電網能量儲存系統之多種應用中。儘管LiB具有高能量密度及穩定性之理想特性,但安全性擔憂目前限制了其有用性。首先,LiB電池(cell)之故障可由於製造缺陷、內部短路、過熱、過量充電、或機械衝擊而觸發;其次,由發生故障的電池產生之熱可傳播,藉此導致鄰近電池中之熱失控。由此等熱事件產生之快速壓力堆積增加了著火及爆炸風險。
可藉由將提供熱絕緣及耐燃性的熱障壁置放於LiB模組中之電池之間而緩解熱失控。諸如氣凝膠、陶瓷纖維、及雲母板之常用熱障壁提供此類特性;然而,氣凝膠及陶瓷纖維缺點係機械彈性較差,而雲母板缺點係可壓縮性較差。另一方面,雖然聚矽氧吹塑發泡體提供充分可壓縮性,且因此適合於低能量密度及中等能量密度之電池組,但其缺點係熱絕緣不足以阻止極高能量密度電池組包之熱失控。因此,可充電電池組熱障壁領域中期望產生提供熱絕緣、耐燃性、及令人滿意的可壓縮性之障壁。
本發明藉由提供以下解決所屬技術領域中之需求:一種組成物,其以該組成物之重量計包含,a) 2至50重量百分比之經至少兩個Si-H基團官能化且聚合度在5至1000範圍內之聚矽氧烷;b) 1至50重量百分比之水、醇、二醇、多元醇、或含有一或多個矽醇基團之化合物;c) 10至90重量百分比之經至少一個乙烯系不飽和基團官能化且聚合度在20至2000範圍內之聚矽氧烷;其中
組分a、b、及c之總濃度以該組成物之重量計在35至95重量百分比範圍內;d)催化量之矽氫化催化劑;e) 1至30重量百分比之阻燃劑;及f) 1至35重量百分比之體積平均粒度在25 µm至300 µm範圍內的中空陶瓷粒子。
本發明之組成物可用於提供作為鋰離子電池組中之可壓縮、熱絕緣、及耐燃性間隔物之發泡材料。
本發明係一種組成物,其以該組成物之重量計包含,a) 2至50重量百分比之經至少兩個Si-H基團官能化且聚合度在5至1000範圍內之聚矽氧烷;b) 1至50重量百分比之水、醇、二醇、多元醇、或含有一或多個矽醇基團之化合物;c) 10至90重量百分比之經至少一個乙烯系不飽和基團官能化且聚合度在20至2000範圍內之聚矽氧烷;其中組分a、b、及c之總濃度以該組成物之重量計在35至95重量百分比範圍內;d)催化量之矽氫化催化劑;e) 1至30重量百分比之阻燃劑;及f) 1至35重量百分比之體積平均粒度在25 µm至300 µm範圍內的中空陶瓷粒子。
經至少兩個、較佳至少三個Si-H基團官能化之聚矽氧烷(a)具有在5至1000或至500或至200範圍內之聚合度。含羥基化合物(b)較佳係苯甲醇或C
2-C
8烷基二醇。經至少一個、較佳至少兩個乙烯系不飽和基團官能化之聚矽氧烷(c)具有在20或100或200或300至2000或至1500或至1000範圍內之聚合度。以組成物之重量計,組分a、b、及c之總重量百分比在35百分比或50至95百分比範圍內。
經至少一個乙烯系不飽和基團官能化之聚矽氧烷較佳經兩個C
2-C
8烯基,更佳兩個乙烯基或兩個烯丙基官能化。經至少一個乙烯系不飽和基團官能化之聚矽氧烷最佳地係經兩個乙烯基官能化之聚二甲基矽氧烷。經兩個乙烯基官能化之聚二甲基矽氧烷有利地經設計以具有10,000至50,000 mPa·s範圍內之黏度。此黏度宜藉由組合不同聚合度之二乙烯基官能化之聚二甲基矽氧烷,亦即雙峰分布之二乙烯基官能化之聚二甲基矽氧烷來達成。
矽氫化催化劑較佳係基於鉑之催化劑,諸如氯鉑酸,且以以組成物之重量計,一般在0.5 ppm至200 ppm Pt範圍內之催化量使用。
組成物亦包含1或2或3重量百分比至30或至20或至15重量百分比之阻燃劑,其係在加熱時釋放CO
2或水或兩者之金屬氫氧化物、碳酸鹽、碳酸氫氧化物(hydroxide-carbonate)、或水合物。阻燃劑之實例包括Al(OH)
3、Mg(OH)
2、Ca(OH)
2 、MgCO
3·3H
2O(水碳鎂石)、Mg
5(CO
3)
4(OH)
2·4H
2O(水菱鎂礦)、MgCa(CO
3)
2(碳鈣鎂礦)、AlO(OH)(勃姆石(boemite))、NaHCO
3、及水合MgSO
4(瀉利鹽)。
組成物進一步包含1或5或10重量百分比至35或至30至25重量百分比之填充空氣或填充惰性氣體之中空陶瓷粒子。如本文所用,「陶瓷(ceramic)」係指諸如鋁(例如,結晶或半結晶Al
2O
3)、矽(例如,結晶或半結晶SiO
2)、或鈣(例如,結晶或半結晶CaO)之金屬的結晶或半結晶無機氧化物、氮化物、碳化物、氮氧化物、或碳氧化物,或其組合。結晶度可藉由X射線粉末繞射量測。如本文所用,用語「半結晶(semi-crystalline)」係指具有非晶及結晶區域之陶瓷材料。中空陶瓷粒子之平均體積粒度如使用諸如Beckman Coulter LS 130粒度分析儀之動態光散射分析儀所量測,係25 µm或50 µm或70 µm至300 µm或至200 µm或至150 µm。所得物品之密度在0.10或0.15 g/cm
3至0.90或至0.50 g/cm
3範圍內。
組成物可用於製備如實質上描述於例如US 5,358,975中之聚有機矽氧烷發泡體物品。經至少三個Si-H基團官能化之聚矽氧烷有利地在基於鉑之催化劑存在下與以下接觸:a)醇、二醇、多元醇、或矽醇,及b)二乙烯基官能化之聚二甲基矽氧烷,以形成具有-Si-CH
2-CH
2-Si-基團及-Si-O-R基團的有機聚矽氧烷之交聯網狀結構,其中R係醇、二醇、多元醇、或矽醇之結構單元(亦即反應產物)。
可能有利的係使用2部分方法製備發泡材料,其中在第一容器中,將下列摻合,以形成部分A組成物:二乙烯基官能化之聚二甲基矽氧烷之第一部分;阻燃劑之第一部分;基於鉑之催化劑;一或多種含羥基化合物;及中空陶瓷粒子之第一部分。在第二容器中,將下列摻合,以形成部分B組成物:二乙烯基官能化之聚二甲基矽氧烷之剩餘部分;聚合物樹脂摻合物,其係二乙烯基官能化之聚二甲基矽氧烷與交聯有機聚矽氧烷樹脂之混合物;阻燃劑之剩餘部分;經至少三個Si-H基團官能化之聚矽氧烷;及中空陶瓷粒子之剩餘部分。隨後將部分A及B合併且混合,隨後傾倒於兩個離型膜片之間以形成本發明之發泡材料。
因此,在另一態樣中,本發明係一種絕緣、可壓縮性、及耐燃性發泡材料,其以發泡材料之重量計包含35至95重量百分比之聚有機矽氧烷發泡體;1至30重量百分比之阻燃劑;及1至35重量百分比之體積平均粒度在25 µm至300 µm範圍內之中空陶瓷粒子;其中該發泡材料之密度在0.10至0.90 g/cm
3範圍內。
在又一態樣中,本發明係一種電池組模組,其包含含有空間分離之電池組電池陣列及接觸相鄰電池組電池之聚有機矽氧烷發泡體材料的殼體。聚有機矽氧烷發泡體可藉由用發泡體填充相鄰電池組電池之間的空間及/或藉由用發泡體覆蓋電池組電池來接觸電池組電池。電池組模組可進一步包含殼體的內部邊緣處的端板,該等端板與最接近邊緣的電池組電池直接或間接接觸。發泡體材料可插入至相鄰電池組電池之間及在電池與端板之間的空腔中;可替代地,可將發泡體前驅物施加於電池上且至空腔中,隨後固化以形成發泡材料。
已發現,本發明之發泡材料在LiB熱障壁應用中提供熱絕緣、耐燃性、及可壓縮性之所要特性。
在以下實例中,ViMe
2SiO
1/2/(CH
3)
3Si-O
1/2/SiO
4/2樹脂之M
w及M
n藉由凝膠滲透層析,使用封裝有5 mm直徑
尺寸之二乙烯苯交聯聚苯乙烯珠粒孔隙類型混合-C (Mixed-C) (Polymer Laboratory)之gpc管柱測定。THF用作移動相且偵測藉由折射率偵測器進行。
實例1-製備具有陶瓷粒子之發泡有機聚矽氧烷物品
第一組分(部分A)藉由使用Flacktek快速混合器,混合下列而製備:黏度係約40,000 mPas之二甲基乙烯基矽烷氧基封端之聚二甲基矽氧烷(聚合物1,11.3 pbw),及1)具有約1,900 mPa·s之黏度及約0.22 wt.% Vi的二甲基乙烯基矽烷氧基封端之聚二甲基矽氧烷與2)具有5:40:55的ViMe
2SiO
1/2:(CH
3)
3Si-O
1/2:SiO
4/2結構單元比率、5000的M
n及21,400的M
w的ViMe
2SiO
1/2/(CH
3)
3Si-O
1/2/SiO
4/2樹脂之64:36 w/w摻合物(聚合物-樹脂摻合物,64.9 pbw);及Micral 855氫氧化鋁(15.2 pbw)。在2000 rpm下攪拌內容物30 s,此後將Pt(0)與二乙烯基四甲基二矽氧烷之錯合物(0.93 pbw,0.62 wt% Pt)、1,4-丁二醇(2.6 pbw)、及苯甲醇(3.3 pbw)添加至混合物中,且以2000 rpm攪拌內容物30 s。最後,向混合物中添加Elminas Spheres HCMS-W150中空陶瓷粒子(平均體積粒度係100 µm;20 pbw)且以2000 rpm攪拌內容物30 s。
在2000 rpm下攪拌內容物30 s,此後將氯鉑酸與二乙烯基四甲基二矽氧烷之錯合物(0.93 pbw,0.62 wt% Pt)、1,4-丁二醇(2.6 pbw)、及苯甲醇(3.3 pbw)添加至混合物中,且以2000 rpm攪拌內容物30 s。最後,向混合物中添加Elminas Spheres HCMS-W150中空陶瓷粒子(平均體積粒度係100 µm;20 pbw)且以2000 rpm攪拌內容物30 s。
第二組成物(部分B)類似地藉由將聚合物1 (8.9 pbw)、聚合物樹脂摻合物(51 pbw)、以及Hymod M855氫氧化鋁(26.4 pbw)混合在一起來製備。在2000 rpm下攪拌內容物30 s,此後向混合物中添加具有30 mPa·s黏度及1.6 wt% SiH含量之直鏈有機氫聚矽氧烷(6.7 pbw)及具有5 mPa·s黏度及0.7 wt% SiH含量之聚二甲基有機氫矽氧烷(5.1 pbw),且以2000 rpm攪拌內容物30 s。隨後,向混合物中添加Elminas Spheres HCMS-W150中空陶瓷粒子(20 pbw)且以2000 rpm攪拌內容物30 s。
隨後混合等量的部分A及B,且將混合物傾倒於兩個離型膜片(無光澤麥拉膜(mylar film))之間。使用夾持輥控制初始(在發泡之前)厚度在0.045吋。樣本在70℃下固化5分鐘,隨後在100℃下固化15分鐘,產生用於進一步測試之發泡體薄片。(密度=0.31 g/cm
3)
實例2-製備具有陶瓷粒子之發泡有機聚矽氧烷物品
除了將Elminas Spheres HCMS THERMO-W75中空陶瓷粒子(平均體積粒度係80 µm,20 pbw)用於部分A及B中之外,以實質上相同之方式進行製備實例1之發泡物品的程序。(密度=0.31 g/cm
3)\
實例3-製備具有陶瓷粒子之發泡有機聚矽氧烷物品
除了將Elminas Spheres HCMS-W300中空陶瓷粒子(平均體積粒度係180 µm,20 pbw)用於部分A及B中之外,以實質上相同之方式進行製備實例1之發泡物品的程序。(密度=0.34 g/cm
3)
熱絕緣及可燃性
使用設置於液壓機上之加熱板來測試如實例中所描述而製備之發泡體的熱絕緣及可燃性。將加熱板設定為600℃,其中絕緣體位於表面之頂部上。使用Kapton膠帶將四個熱電偶(K型)固定於鋁散熱片(4" × 4" × 0.47")上。隨後樣本(4" × 4")置放於且使用Kapton膠帶固定於散熱片上。使用Kapton膠帶將額外熱電偶(K型)附接至樣本表面。自熱表面移除絕緣體且將附接至散熱片之樣本快速置放於熱表面上,其中樣本表面面向加熱板表面且Al散熱片面向相對側。壓力快速增加至355 kPa。使用資料記錄器記錄加熱板表面與樣本表面之間的介面溫度及樣本表面與散熱片之間的介面溫度。一旦達至300 s之時間,釋放壓力,且結束測試。在樣本表面<300℃之溫度視為可接受的。在整個測試中無可觀測的火焰視為可接受之耐燃性。
硬度
硬度使用蕭氏00硬度計量測。將測試樣品置於硬平坦表面上。隨後將蕭氏00硬度計之壓頭按壓至樣品上,確保其平行於表面。在與樣品牢固接觸期間讀取硬度。<80之硬度視為可接受的。
壓縮力
壓縮力使用配備有100 kg測力計、直徑係40 mm之鋁探針的TA.HDplus質構分析儀、及平坦重型鋁基材來量測。使用直徑係1"之模切將聚矽氧發泡體樣本切成圓形,且置放於基材與探針之間。探針最初設定為與樣本厚度相同之高度,且以1 mm/sec之速率降低直至壓力達到最大。樣本厚度及壓力記錄為壓縮力曲線。記錄在原始樣本厚度之30%下的壓力。<500 kPa之壓縮力視為可接受的。
發泡體密度
發泡體密度係基於直徑係1吋之兩個發泡體樣本的平均厚度及重量計算。
將填充陶瓷之有機聚矽氧烷物品之特性與除不含中空陶瓷粒子外在構造上類似於實例發泡體的市售有機聚矽氧烷物品(COHRlastic聚矽氧發泡體,可購自Stockwell Elastomerics)相比較。
表1係實例1至3之發泡體及市售比較發泡體之效能特性的概述。密度以g/cm
3為單位量測;硬度以蕭氏00單位量測;壓縮力(力)以kPa@30%壓縮為單位量測;600℃下溫度(300 s後T)係指300 s後樣本表面溫度;且可燃性係指在熱絕緣測試期間火焰之可觀測性。
表1-有機聚矽氧烷物品之特性
特性 | 標準 | 比較 | 實例1 | 實例2 | 實例3 |
密度 | < 0.9 | 0.23 | 0.31 | 0.31 | 0.34 |
硬度 | < 80 | 35 | 65 | 69 | 71 |
力 | < 500 | 17 | 246 | 306 | 300 |
300 s後T | < 300 °C | 334 °C | 246 °C | 255 °C | 294 °C |
可燃性 | 無火焰 | 無火焰 | 無火焰 | 無火焰 | 無火焰 |
表1說明本發明之發泡體通過所有測試,而市售實例未通過熱絕緣測試。已意外地發現,中空陶瓷粒子降低300 s之表面溫度而不會不利地影響發泡體之其他關鍵特性。進一步發現,在50 µm至150 µm範圍內之中空陶瓷粒度在降低表面溫度方面尤其有效。
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Claims (8)
- 一種組成物,其以該組成物之重量計包含, a) 2至50重量百分比之經至少兩個Si-H基團官能化且聚合度在5至1000範圍內之聚矽氧烷; b) 1至50重量百分比之水、醇、二醇、多元醇、或含有一或多個矽醇基團之化合物; c) 10至90重量百分比之經至少一個乙烯系不飽和基團官能化且聚合度在20至2000範圍內之聚矽氧烷;其中組分a、b、及c之總濃度以該組成物之重量計在35至95重量百分比範圍內; d) 催化量之矽氫化催化劑; e) 1至30重量百分比之阻燃劑;及 f) 1至35重量百分比之體積平均粒度在25 µm至300 µm範圍內的中空陶瓷粒子。
- 如請求項1之組成物,其中經至少兩個Si-H基團官能化之該聚矽氧烷係經至少三個Si-H基團官能化;以該組成物之重量計,組分a、b、及c之總濃度在50至80百分比範圍內;且以該組成物之重量計,該阻燃劑之濃度在2至20重量百分比範圍內。
- 如請求項2之組成物,其中經至少一個乙烯系不飽和基團官能化之該聚矽氧烷係聚合度在100至1000範圍內之二乙烯基官能化之聚二甲基矽氧烷。
- 如請求項3之組成物,其中該阻燃劑係一或多種選自由下列組成之群組的阻燃劑:Al(OH) 3、Mg(OH) 2、MgCO 3·3H 2O、Mg 5(CO 3) 4(OH) 2·4H 2O、MgCa(CO 3) 2、AlO(OH)、NaHCO 3、及水合MgSO 4。
- 如請求項1至4中任一項之組成物,其中該等中空陶瓷粒子根據動態光散射具有在25 µm至200 µm範圍內之平均體積粒度。
- 如請求項1至4中任一項之組成物,其中該等中空陶瓷粒子根據動態光散射具有在50 µm至150 µm範圍內之平均體積粒度。
- 如請求項5或6之組成物,其中該等中空陶瓷粒子係結晶或半結晶Al 2O 3粒子、結晶或半結晶SiO 2粒子、或結晶或半結晶CaO粒子。
- 如請求項3之組成物,其中該二乙烯基官能化之聚二甲基矽氧烷係具有在10,000至50,000 mPa·s範圍內的組合黏度的雙峰分布之二乙烯基官能化之聚二甲基矽氧烷。
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2022
- 2022-05-09 WO PCT/CN2022/091782 patent/WO2023216073A1/en unknown
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2023
- 2023-04-19 TW TW112114650A patent/TW202402956A/zh unknown
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WO2023216073A1 (en) | 2023-11-16 |
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