TWI401226B - 能增強有機及/或無機材料之玻璃股線 - Google Patents
能增強有機及/或無機材料之玻璃股線 Download PDFInfo
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Description
本發明係關於玻璃“強化”股線(或“纖維”),亦即可增強有機及/或無機材料且可用為紡織股線者;此等股線可經由包括下述之方法製得:將從位於通常以電阻加熱予以加熱的襯套之底部中的小孔流出之熔融玻璃流予以機械地衰減。
本發明更特定地有關具有高比楊氏模數且具有特別有利的SiO2-Al2O3-CaO-MgO型四元組成物之玻璃股線。
玻璃強化股線領域為玻璃工業中的非常特殊領域。此等股線係用特殊的玻璃組成物所製成,所用的玻璃必須能夠經由使用上述方法抽拉成直徑數微米的絲形式,該等方法必須容許能夠滿足強化功能的連續股線之形成。
於某些應用中,尤其是在航空學中,目標係得到能夠在動態條件下操作且因而能夠耐住高機械應力之大型組件。此等組件通常是以有機及/或無機材料及強化料為基底,例如呈玻璃股線形式者,其通常佔有超過50%的體積。
此等組件的機械性質及效用性可經由改善強化料的機械性能,尤其是比楊氏模數而改進。
強化料的性質,於玻璃強化股線的情況中,主要是由成分玻璃的組成物所主宰。最廣用來強化有機及/或無機材料的玻璃股線係由E-玻璃或R-玻璃所製成。
E-玻璃股線常用來形成強化料,以其本身形式者或呈經組織化的組合體例如織物者。可在E-玻璃纖維化的條件係極為有利者-對應於使玻璃具有接近1000泊(poise)的黏度之溫度的操作溫度相當地低,為約1200℃,其液相溫度低於操作溫度約120℃,且其脫硫化率係低者。
在ASTM D 578-98標準中所定義的用於電子和航空領域中之E-玻璃組成如下(以重量%為單位):52至56% SiO2;12至16% Al2O3;16至25% CaO;5至10% B2O3;0至5% MgO;0至2% Na2O+K2O;0至0.8% TiO2;0.05至0.4% Fe2O3;及0至1% F2。
不過,散裝的E-玻璃具有約33Mpa/kg/m3的相當低比楊氏模數。
ASTM D 578-98標準述及其他的E-玻璃強化股線,隨意地,不含硼的玻璃。此等股線具有下面的組成物(以重量百分比為單位):52至62% SiO2;12至16% Al2O3;16至25% CaO;0至10% B2O3;0至5% MgO;0至2% Na2O+K2O;0至1.5% TiO2;0.05至0.8% Fe2O3;及0至1% F2。
無硼E-玻璃的纖維化條件比含硼E-玻璃所用者較不利,不過,彼等仍然保持經濟上可接受者。其比楊氏模數保留在相當於E-玻璃之效能水平。
此外,從US 4 199 364也已知有一種不貴的玻璃,既不含硼也不含氟者,具有與E-玻璃相稱的機械性質,尤其是張力強度。
於散裝中,R-玻璃係已知有好的機械性質,尤其是關於比楊氏模數,為約33.5Mpa/kg/m3。不過,其熔化和纖維化條件比上述E-玻璃類似更具緊縮性,因而使R-玻璃的最後成本更為高。
R-玻璃的組成物給於FR-A-1 435 073之中,其為如下者(以重量百分比為單位):50至65% SiO2;20至30% Al2O3;2至10% CaO;5至20% MgO;15至25% CaO+MgO;SiO2/Al2O3=2至2.8;MgO/SiO2<0.3。
為增加玻璃股線的機械強度之其他嘗試也已有進行過,不過通常都會損及彼等的可纖維化性,加工因而變得更困難或施加修改既有纖維化設施之需要。
綜上所述,有需要使玻璃強化股線具有儘可能接近E-玻璃的成本,以及顯示出比得上R-玻璃的效能水準之機械性質。
本發明的目的是提供結合R-玻璃的機械性質,特別是其比楊氏模數,與趨近E-玻璃的改良熔化及纖維化性質的該玻璃強化股線。
此目的因下述玻璃股線而達到,該玻璃股線的組成物包含在下面所界定的限值內之成分(以重量百分比表出):SiO2 50-65%
Al2O3 12-20%
CaO 12-17%
MgO 6-12%
CaO/MgO ≦2,較佳者≧1.3
Li2O 0.1-0.8%,較佳者≦0.6%
BaO+SrO 0-3%
B2O3 0-3%
TiO2 0-3%
Na2O+K2O <2%
F2 0-1%
Fe2O3 <1%
氧化矽(SiO2)為形成本發明玻璃的網眼織物的諸氧化物中之一者且在彼等的穩定性上扮演著必要的角色。於本發明範疇中,於氧化矽含量低於50%時,玻璃的黏度會變得太低且在纖維化之中有增加的脫硫化之風險。於高出65%時,玻璃會變得非常黏稠且難以熔化。較佳者,氧化矽含量係在58%與63%之間。
氧化鋁(Al2O3)也構成本發明玻璃的網眼織物形成劑且在有關模數上,扮演著一必要的角色,其係與氧化矽結合。於本發明所界定的限制之範疇內,將此氧化物的濃度百分比減低到低於12%會導致比楊氏模數之減低且助成最大脫琉化率之增加,而在此氧化物的濃度百分比太大幅增加之下,大於20%會有脫琉化風險且會增高黏度。較佳者,所選組成物的氧化鋁含量係在從13至18%的範圍之內。有利者,氧化矽和氧化鋁的含量和係大於70%且更佳
者大於75%,此可能達到有利的比楊氏模數值。
石灰(CaO)係用來調整黏度及控制玻璃的脫琉化。CaO含量較佳者係在從13至15%的範圍之內。
氧化鎂(MgO),像CaO一般,係作為黏度減低劑且也對比楊氏模數具有有益之效應。MgO含量係在從6至12%,較佳者從7至9%的範圍內。
CaO/MgO重量比經證明為控制脫琉化的必要因素。本案發明人已鑑定出不超過2,但較佳者大於1.3的CaO/MgO比可促進玻璃在數種相中的結晶化(鈣長石:CaO.Al2O3.2 SiO2和透輝石CaO.MgO.2 SiO2,或甚至鎂橄欖石:2MgO.SiO2或頑石輝石:MgO.SiO2),彼等會在消耗液相之下進行成長競爭。此種競爭具有限制結晶相的最大成長率之效應且因而減低玻璃脫琉化之風險,並促使其正確地纖維化。
於該玻璃組成物中可含其他鹼土金屬氧化物,例如BaO和SrO。此等氧化物的總含量要保持在低於3%,較佳者低於1%,以便不增加玻璃的密度,以免具有降低比楊氏模數的效應。一般原則上,該組成物的實質地不含BaO和SrO。
氧化鋰(Li2O)也像MgO一般作為黏度減低劑且也會增加比楊氏模數。於高於0.8%時,Li2O導致操作溫度的實質減低,且因而使成形溫度範圍縮小(操作溫度與液相溫度之間的差值),此不再使玻璃得以令人滿意地纖維化。
再者,Li2O係昂貴者,其基本上只由兩種原料所提供,一種為合成且昂貴者,亦即碳酸鋰,且另一種為天然者,亦即只含7至8% Li2O的鋰輝石(其因而需要在批料中大量導入)。氧化鋰也具有高度揮發性,導致在熔化中約50%的流失率。基於全部此等理由,本發明玻璃組成物中的Li2O含量係在從0.1至0.8%之間變異且較佳者為限制到0.6%且更佳者0.5%。
較佳者,Al2O3、與MgO和Li2O的含量和係等於23%或更高者,藉此可以獲得非常合用的比楊氏模數值(大於36Mpa/kg/m3),同時具有良好的可纖維化性。
氧化硼(B2O3)係作為黏度減低劑。其在本發明玻璃組成物中的含量係經限制在3%,較佳者2%以避免污染物揮發排放問題。
氧化鈦係作為黏度減低劑且有助於增加比楊氏模數。其可用雜質形式存在(其在組成物中的含量為0至0.5%)或也可以有意地添加。不過,其有意添加需要使用非標準原料(導入最少可能的雜質於批料中者),由是增加成本。TiO2的有意添加有利地只用於低於3%,較佳者低於2%的含量,高於此含量時,玻璃會招致非所欲的黃色。
Na2O和K2O可加到本發明組成物中以助成有限的脫琉化且可能減低玻璃的黏度。不過,Na2O和K2O的含量必須保持在低於2%以避免危及玻璃的抗水解性。較佳者,該組成物含有低於0.8%的此兩種氧化物。
組成物中可包含氟(F2)以幫助玻璃熔化及纖維化。
不過,其含量要限制到1%,因為在高於此含量時,會有污染性排放物及爐子耐火料的腐蝕之風險。
氧化鐵(以Fe2O3形式表示)通常呈為雜質形式存在於本發明組成物中。Fe2O3含量必須低於1%,較佳者等於0.5%或更低者,以期不會不可接受地損及股線的顏色及纖維化設施的操作,特別是爐子的熱傳性。
較佳者,該玻璃股線具有包含在下面界定的限值內之成分之組成物(以重量百分比表示):SiO2 58-63%
Al2O3 13-18%
CaO 12.5-15%
MgO 7-9%
CaO/MgO 1.5-1.9
Li2O 0.1-0.5%
BaO+SrO 0-1%
B2O3 0-2%
TiO2 0-0.5%
Na2O+K2O <0.8%
F2 0-1%
Fe2O3 <0.5%
特別有利者為使該組成物具有在從0.40至0.44,且較佳者等於0.42或更低的Al2O3/(Al2O3+CaO+MgO)重量比例,藉此可以得到具有1250℃或更低者,較佳者1210℃或更低的液相溫度。
一般而言,本發明玻璃股線不含氧化硼B2O3或氟F2。
本發明玻璃股線係從具有上述組成物的玻璃使用下述製程得到者:將從位在一或多個襯套的底部中之許多個小孔流出的許多熔融玻璃流縮小成一或多片連續絲形式,然後將此等絲合併成一或多條股線,再將彼等股線收集在移動的承載體之上。此可為轉動性承載體,使股線收集或捲繞包裝體形式,或為在使用也作為抽拉股線所用的裝置斬切、股線時的橫移承載體之形式,或在使用抽拉股線的裝置噴佈股線時橫向移動以形成一蓆之承載體。
隨意地在進一步轉化操作之後,所得到的股線可隨即呈各種形式:連續股線、切短股線、編織布、針織布、辮條、帶或蓆,此等股線係由直徑可在從約5至30微米內的絲所構成。
給到襯套的熔融玻璃係從純原料,或更常者,天然原料(即可能含微量雜質者)而得到,此等原料係以恰當比例混合後再熔化。熔融玻璃的溫度係以習用方式調節以使其纖維化且避免脫琉化問題。在將絲合併成股線形式之前,通常用膠料(size)組成物將彼等塗覆,目的在於防止彼等磨耗及使彼等隨後摻和到要強化的材料之內。
從本發明股線所得複合物包含至少一種有機材料及/或至少一種無機材料與玻璃股線,其中至少某些股線為本發明股線。
下面的實施例係用以闡明本發明而絕不是限制本發明。
由直徑17微米的玻璃絲所製成的玻璃股線係經由具有表1所給以重量百分比表示的組成物之熔融玻璃縮減而得。
玻璃黏度等於103泊(poise desipascal.second)時的溫度表為T(log η-3)。
玻璃的液相溫度以T液相(Tliquidus)表之,此溫度係對應於可琉化成為玻璃的大部份耐火相具有零成長速率之溫度且因而對應於此琉化相之熔點。
其中也報導出散裝玻璃的比楊氏模數,此係從根據ASTM C 1259-01標準測量到的楊氏模數與以阿基米得法(the Archimedes method)測量到的密度計算出者(即,測得之比楊氏模數),以及從以既有數據建立的模型使用統計軟體套組計算之值(即計算所得比楊氏模數值)。於對散裝玻璃測得之比楊氏模數與對使用此相同玻璃所製絲組成物之粗紡線(roving)所得比楊氏模數之間存在著良好的相關性。因此,在表1中的值可提供以纖維化後玻璃所具模數而論的機械性質之估計。此表也給出,作為比較例者,對不含Li2O的玻璃(實施例6),根據US 4,199,364實施例5的玻璃(實施例7),E-玻璃以及R-玻璃所得測量值。
顯然地,本發明實施例展示出在熔化和纖維化性質與
機械性質之間的優異協調。此等纖維化性質係特別有利者,尤其是具有約1210℃的液相溫度,此係遠低於R-玻璃者。纖維化範圍為正值,特別是在T(log η=3)與T液相之間的差值為大於50℃,且可能高達68℃。
從本發明組成物所得玻璃(實施例1至5)之比楊氏模數顯著地高於E-玻璃且也較R-玻璃和不含Li2O的玻璃(實施例6)更改進。
顯著地,使用本發明玻璃之下,可因而達到比R-玻璃實質較佳的機械性質,同時明顯地降低纖維化溫度,使其接近用E-玻璃所得值。
本發明玻璃可結晶化成為三相。於液相時,其為透輝石(diopside),此因為比鈣長石(anorthite)(實施例6)更不耐火而更為有利。透輝石在本發明玻璃中的最大成長速率低於在具有2.14的CaO/MgO比例的實施例7玻璃中者(減低至少50%)。
本發明玻璃股線比R-玻璃股線較不貴,此可有利地在某些應用中置換,尤其是航空應用,用於強化直昇機槳葉,或用於光學電纜。
Claims (10)
- 一種玻璃強化股線,其組成物包含在下面所界定的限值中之成分(以重量百分比表示):SiO2 58-63% Al2O3 12-20% CaO 12-17% MgO 6-12% CaO/MgO 1.3-2 Li2O 0.1-0.8% BaO+SrO 0-3% B2O3 0-3% TiO2 0-3% Na2O+K2O <2% F2 0-1% Fe2O3 <1%,其中該玻璃強化股線的比楊氏模數係至少36 MPa/Kg/m3。
- 根據申請專利範圍第1項之玻璃股線,其中該組成物所具有的Al2O3+MgO+Li2O含量係等於23%或高於23%。
- 根據申請專利範圍第1或2項之玻璃股線,其中該組成物具有大於70%的SiO2+Al2O3含量。
- 根據申請專利範圍第1或2項之玻璃股線,其中該組成物具有從0.40至0.44的Al2O3/(Al2O3+CaO+MgO)重量比例。
- 根據申請專利範圍第1或2項之玻璃股線,其中該組成物包含在下面所界定的限值中之成分(以重量百分比表示):SiO2 58-63% Al2O3 13-18% CaO 12.5-15% MgO 7-9% CaO/MgO 1.5-1.9 Li2O 0.1-0.5% BaO+SrO 0-1% B2O3 0-2% TiO2 0-0.5% Na2O+K2O <0.8% F2 0-1% Fe2O3 <0.5%。
- 根據申請專利範圍第1或2項之玻璃股線,其中該組成物不含B2O3或F2。
- 一種如申請專利範圍第1項之玻璃強化股線所形成的組合體,其特徵在於該組合體呈梭織物形式。
- 一種複合物,其包含有機及/或無機材料和如申請專利範圍第1項之玻璃股線。
- 一種適合用於製造玻璃強化股線之玻璃組成物,該組合物包含在下面所界定的限值中之成分(以重量百分比表示): SiO2 58-63% Al2O3 12-20% CaO 12-17% MgO 6-12% CaO/MgO 1.3-2 Li2O 0.1-0.8% BaO+SrO 0-3% B2O3 0-3% TiO2 0-3% Na2O+K2O <2% F2 0-1% Fe2O3 <1%,其中該組成物所具有的Al2O3+MgO+Li2O含量係等於23%或高於23%。
- 根據申請專利範圍第9項之組成物,其中該組成物具有超過50℃之成形範圍(T(log η=3)-T液相)。
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2004
- 2004-12-16 FR FR0413443A patent/FR2879591B1/fr active Active
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2005
- 2005-12-15 ES ES05825565T patent/ES2405941T3/es active Active
- 2005-12-15 MX MX2007006989A patent/MX2007006989A/es active IP Right Grant
- 2005-12-15 US US11/722,039 patent/US20090286440A1/en not_active Abandoned
- 2005-12-15 JP JP2007546144A patent/JP5006207B2/ja active Active
- 2005-12-15 BR BRPI0518946-2A patent/BRPI0518946B1/pt active IP Right Grant
- 2005-12-15 TW TW94144552A patent/TWI401226B/zh active
- 2005-12-15 PL PL05825565T patent/PL1831118T3/pl unknown
- 2005-12-15 KR KR1020137007933A patent/KR20130041370A/ko not_active Application Discontinuation
- 2005-12-15 RU RU2007126843A patent/RU2404932C2/ru active
- 2005-12-15 CA CA2591026A patent/CA2591026C/en active Active
- 2005-12-15 CN CN200580043075.7A patent/CN101119939B/zh active Active
- 2005-12-15 KR KR1020077016026A patent/KR101291865B1/ko active IP Right Grant
- 2005-12-15 EP EP05825565A patent/EP1831118B1/fr active Active
- 2005-12-15 PT PT58255654T patent/PT1831118E/pt unknown
- 2005-12-15 CN CN201410192431.2A patent/CN103964687B/zh active Active
- 2005-12-15 WO PCT/FR2005/051090 patent/WO2006064164A1/fr active Application Filing
-
2007
- 2007-07-11 NO NO20073589A patent/NO340572B1/no unknown
-
2010
- 2010-08-11 RU RU2010133664/03A patent/RU2010133664A/ru not_active Application Discontinuation
-
2016
- 2016-02-29 US US15/055,898 patent/US20160176754A1/en not_active Abandoned
- 2016-02-29 US US15/055,893 patent/US20160176753A1/en not_active Abandoned
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Also Published As
Publication number | Publication date |
---|---|
MX2007006989A (es) | 2007-08-23 |
ES2405941T9 (es) | 2015-02-02 |
WO2006064164A1 (fr) | 2006-06-22 |
EP1831118B1 (fr) | 2013-02-13 |
US20090286440A1 (en) | 2009-11-19 |
CA2591026A1 (en) | 2006-06-22 |
CN103964687B (zh) | 2020-07-03 |
JP5006207B2 (ja) | 2012-08-22 |
NO340572B1 (no) | 2017-05-15 |
US20160176753A1 (en) | 2016-06-23 |
PL1831118T3 (pl) | 2013-07-31 |
ES2405941T3 (es) | 2013-06-04 |
KR101291865B1 (ko) | 2013-07-31 |
BRPI0518946A2 (pt) | 2008-12-16 |
NO20073589L (no) | 2007-07-11 |
PT1831118E (pt) | 2013-05-17 |
KR20070089228A (ko) | 2007-08-30 |
JP2008524100A (ja) | 2008-07-10 |
KR20130041370A (ko) | 2013-04-24 |
RU2010133664A (ru) | 2012-02-20 |
RU2007126843A (ru) | 2009-01-27 |
CN101119939B (zh) | 2021-04-30 |
FR2879591A1 (fr) | 2006-06-23 |
US20160176754A1 (en) | 2016-06-23 |
TW200640816A (en) | 2006-12-01 |
CN101119939A (zh) | 2008-02-06 |
CN103964687A (zh) | 2014-08-06 |
CA2591026C (en) | 2015-01-13 |
RU2404932C2 (ru) | 2010-11-27 |
EP1831118A1 (fr) | 2007-09-12 |
BRPI0518946B1 (pt) | 2018-01-09 |
FR2879591B1 (fr) | 2007-02-09 |
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