CN1162983A - 人造玻璃纤维 - Google Patents
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Abstract
人造玻璃纤维具有在pH4-5下至少为20纳米/天的溶解速度以及在1400℃下10-70泊的熔体粘度并且由含有18-30%重量Al2O3的组合物形成。
Description
本发明涉及人造玻璃纤维(MMVF),该纤维在使用中保持稳定,但它可以显示出生理优点。
MMV纤维是由玻璃熔体,如岩石、矿渣、玻璃和其它矿物熔体产生的。该熔体是通过将具有所需的分析结果的矿物组合物在熔窑中熔化而形成的。该组合物通常是通过将岩石或矿物混合从而产生所需的分析结果而形成的。该矿物组合物通常具有氧化物分析结果,它包括至少32%SiO2,低于30%Al2O3和至少10%CaO。在本说明书中的成分分析是以重量计算的并且以氧化物计算。氧化铁可以是氧化亚铁和三氧化二铁的混合物,但在本文中以FeO描述。
在熔炉中高效低成本地形成熔体以及由该熔体高效低成本地形成纤维要求该组合物具有合适的液线温度并且在成纤工艺中具有合适的粘度。这些要求对用来熔化的组合物的选择产生了一些限制。
尽管没有科学证据证明与制造及使用MMV纤维有关的健康危害,但是商业利润已经促使制造商提供这样一些MMV纤维,这些纤维保持了所需的玻璃性能(例如在高温和潮湿条件下的稳定性),但是它们还保证具有改进的生理安全性。
改进的安全性的保证通常是根据体外试验作出的,这些试验测定了纤维在用来模拟肺液的液体,如pH值为7.4-7.8的Gamble溶液中的溶解速度或降解性。在pH7.5下溶解速度升高的结果是该纤维通常具有较低的耐潮湿性。
已经公开了许多专利申请,它们描述了在这种体外试验中具有较高的溶解速度的纤维,例如WO87/05007,WO89/12032,EP412878,EP459897,WO92/09536,WO93/22251和WO94/14717。
这些专利申请许多申请以及声称在体外试验中具有较高的溶解速度的纤维的一个特点是该纤维具有较低的铝含量。例如,在WO87/05007中指出Al2O3必需低于10%。岩棉和矿渣棉的铝含量通常在5-15%(以Al2O3重量计)并且许多声称在生理上合适的纤维中的许多纤维其铝含量低于4%,并且经常低于2%。已经知道在这些低Al2O3组合物中还包括磷,以增加在这种pH7.5溶解速度试验中的溶解速度。
这些低Al2O3纤维中许多纤维存在的一个问题(除了它们是否具有提高的生理适应性的不确定性以外)是熔化性能不能完全满足在常规的或容易适应的熔化和成纤装置中制造。举例来说,其在方便的成纤温度下的粘度相当低。另一个问题是在pH7.5下的高溶解速度会导致在安装后可能会遇到的潮湿条件下的稳定性下降。
除了体外试验以外,还进行了体内研究试验。例如,Oberdorster在VDI通讯853,1991,第17-37页中指出在肺对纤维的清除过程中存在两种基本机理,即在中心附近肺液中的溶解和在由肺中巨噬细胞包围的纤维附近产生的酸性环境(保持在pH4.5-5)中的溶解。可以认为巨噬细胞促进了纤维从肺中除去,它通过促使被包围的纤维区域发生局部溶解,导致纤维变细和断裂以降低平均纤维长度从而可以让巨噬细胞吞食并将较短的纤维从肺中送出。这种机理描述在Morimoto等人的职业环境病(Occup.Environ.Med)1994,51,62-67,特别是图3和7的文章和Luoto等人的环境研究(Environmental Research)66(1994)198-207和空气除尘(Staub-Reinhaltung der Luft)52(1992)419-423的文章中。
传统的玻璃纤维以及声称在肺液(在pH7.5下)中具有高溶解度的MMV纤维在pH4.5下的溶解度比在pH7.5下的溶解度要差,并且所推测的由巨噬细胞产生的攻击不会明显的有助于缩短纤维并且将纤维从肺中最终除去。
现有的由岩石、矿渣和其它相当高的碱土金属混合物形成的MMV纤维在pH4.5下比在pH7.5下具有更高的溶解速度,但是它们具有较低的溶体粘度。现有的纤维不能将pH4.5下的溶解速度与熔体性能良好地结合在一起。近来根据体外试验声称较好的纤维在具有所需的低铝含量时具有较低的熔体粘度。低熔体粘度与正常的生产相比不可避免地降低了生产效率。
人们需要提供这样一种MMV纤维,这种纤维由于在pH4.5下的溶解速度而显示出在肺中的生物可降解性,其熔体性能可以使其具有正常的、高生产效率,并且可以由廉价原料生产。优选地,它们在使用中向环境潮湿条件暴露时具有良好的耐候性。
根据本发明,由在1400℃下熔体粘度为10-70泊的组合物形成人造玻璃纤维。该组合物具有下列分析结果,以氧化物的重量计算,它包括
SiO2 32-48%
Al2O3 18-30%
CaO 10-30%
MgO 2-20%
FeO 2-15%
Na2O+K2O 0-10%
TiO2 0-6%
其它组分 0-15%并且该纤维在pH4.5下的溶解速度至少为20纳米/天。
根据本发明,出乎人们意料是可以提供在pH4.5下具有良好的溶解速度的纤维从而使通过巨噬细胞的肺清除容易进行(如此促进了生物可降解性),即使该纤维在pH7.5下具有较低的或中等溶解速度。这就可以在潮湿条件下保持良好的稳定性(不会失去生物可降解性)。该纤维具有合适的常规熔体性能,如液线温度,结晶速度和熔体粘度。该纤维可以用廉价的原料制得。
该纤维的另一个优点在于当它们向潮湿和冷凝水暴露时,所形成的含有溶解产物的溶液具有升高的pH值,但是,该纤维在升高的pH值下具有较低的溶解性;因此它们溶解很少并且具有较高的稳定性。
可以在上述一般的范围中选择成分分析结果,从而获得所限定的熔体粘度和pH4.5下的溶解速度的结合。此外,还很容易选择该组合物,从而使该组合物和纤维可以具有其它的所需性能,例如液线温度和烧结温度。
举例来说,如果发现任何特定熔体在1400℃下的粘度太高,就可以通过降低SiO2+Al2O3总量而使该粘度降低。类似地,如果熔体粘度太低,可以通过将SiO2+Al2O3总量提高,通常在55-75%范围内,经常在60-75%范围内,或者通过降低碱金属氧化物的含量而使粘度增加。类似地,也可以通过增加碱土金属氧化物成分和FeO的总量而使粘度降低。
如果pH4.5下的溶解速度太低,可以通过减少SiO2量而使之增加,但随后必需增加Al2O3含量以保持熔体性能。
SiO2量一般为至少32%,经常为至少34%,优选地为至少35%。通常它低于47%,优选地低于45%,优选地常为38-42%。
Al2O3量通常为至少18%,常常为至少19%,但优选地至少20%,经常为至少24%。通常它低于28%,优选地低于26%。经常优选地是20-23%。
SiO2+Al2O3的总量通常为55-75%,一般至少为56%,优选地至少为57%。在优选的产物中,它通常超过60%,最优选地至少为61%或62%。通常它低于70%或68%,优选地低于65%。SiO2+Al2O3总量通常为57-70%。
CaO量通常至少为14%,优选地为至少18%。通常它低于28%,优选地低于25%。经常优选地含量为14-20%。
MgO量通常为至少5%,优选地为至少6%,并且常常至少为8%,通常它低于15%,优选地低于11%。常常优选地为7-12%。
FeO通常为至少3%,优选地为至少5%。通常它低于12%,优选地低于10%,最优选地为低于8%,经常优选地是5-7%。
优选的CaO+MgO+FeO为25-40%。
碱(Na2O+K2O)通常至少为1%,优选地为至少2%。通常它低于5%,优选地低于3%。
该组合物中经常还含有不超过3%或4%,通常为不超过2%的TiO2。TiO2的量通常至少为0.2%,经常为至少0.5%或1%。
在该组合物中还可以任何数量存在多种其它的成分,它们不会脱离所需的性能。可以包括的这些成分的例子为P2O5,B2O3,BaO,ZrO2,MnO,ZnO和V2O5。
通常合适的是含有P2O5和/或B2O3,以调整熔体性能或调整溶解性。P2O5和B2O3和总量通常不超过10%。P2O5的量通常不超过B2O3的量,并且通常为至少1%或2%。B2O3经常不存在。优选地具有1-8%,通常1-5%的P2O5和0-5%B2O3(经常为1-4%B2O3)。
这些多种其它成分的总量通常低于15%,经常低于10%或8%。所存在的这些成分每一种通常以不超过2%的量存在,除了P2O5和/或B2O3可以以上述较大的量存在以外。
该熔体可以具有常规结晶性能,但是当需要使结晶降至最小时,可以通过含有相当低数量的镁,例如2-6%MgO而实现这一点。
当需要产生具有改进的耐火性的纤维时,通常需要增加FeO量,该量优选地至少为6%,举例来说,不超过8%或更高,例如10%,MgO应该至少为8%。
该组合物的分析结果优选地应使该纤维在pH4.5下的溶解速度为至少25,优选地至少40纳米/天。溶解速度尽可能地高是合适的(它与适度的耐潮湿性和耐热性能的保持一致),但是,超过150或100纳米/天通常是不必要的,通常它低于80纳米/天。
尽管已经指出在pH7.5下的高溶解速度是一种合适的性能(作为所说的生物可降解性的一种指标),但是事实上它经常是一种不合适的性能其原因在于它表示在向潮湿暴露时具有较差的耐候性。在pH7.5下在肺中的溶解不是使纤维可生物降解所绝对要求的。优选地该纤维在pH7.5下在Gambles溶液中的溶解速度为低于25,最优选地为低于15纳米/天。
该组合物在1400℃下的粘度通常为至少12或15泊,优选地为至少18泊。虽然它可以高达60泊,但是通常低于40泊,并且优选地不超过30泊。
当需要该纤维具有良好的耐火性能时,优选地应该是烧结温度至少为800℃,优选地至少为1000℃。
液线温度通常至少为1200℃,经常为至少1240℃。它可以高达1400℃,但优选地不超过1340℃。
在本发明中采用上述中等铝熔体的优点在于它可以在该组合物中包含容易获得的具有中等铝含量的原料,如岩石,砂和废料。因此它可以使采用昂贵的高氧化铝原料,如矾土或高岭土的要求降至最小,并且同时使采用昂贵的非常低的氧化铝原料,如硅砂或橄榄石,铁矿等原料的要求降至最小。这些较昂贵的原料如果需要也是实用的。典型地,可以用来作为该组合物中的一部分或全部的中等氧化铝材料包括斜长岩和响岩和辉长岩。
该组合物典型地通过将适当数量的天然岩石和砂原料,如斜长岩、辉长岩、石灰石、白云石、辉绿岩、磷灰石、含硼原料和废料,如矿棉废料、硅酸铝、矿渣,特别是高铝(20-30%)矿渣,如钢渣、铸造砂、滤尘、粉煤灰、底灰和来自耐火材料生产的高铝废料。
该组合物可以以常规方式转化成熔体,例如在气体加热窑炉中或在电熔炉中或在冲天炉中。本发明的一个优点在于该组合物可以很容易地具有合理的低液线温度(同时在1400℃下保持适当的粘度)并且它使形成熔体所需的能量达到最少。
该熔体可以常规方式转化成纤维,例如通过喷吹工艺或通过串联转子法,例如在WO92/06047中所说的方法。
本发明的纤维可以具有任何方便的纤维直径和长度。
在本发明中溶解速度采用下列试验过程测定。
将300毫克纤维放在含有500毫升经过改进的Gamble溶液(即带有络合剂)的聚乙烯瓶中,其pH值分别调整为7.5或4.5,一天对pH检查一次,如有必要可以采用HCl来进行调整。
在一周时间内进行这些试验。将这些瓶子放在温度为37℃的水浴中,并且一天剧烈摇晃两次。在一天和四天以后从该溶液中取出数等份并且在Perkin-Elmer原子吸收分光光度计上对硅进行分析测定。
经过改进的Gamble溶液具有下列组成:
克/升
MgCl2·6H2O 0.212
NaCl 7.120
CaCl2·2H2O 0.029
Na2SO4 0.079
Na2HPO4 0.148
NaHCO3 1.950
(酒石酸二钠)·2H2O 0.180
(柠檬酸三钠)·2H2O 0.152
90%乳酸 0.156
甘氨酸 0.118
丙酮酸钠 0.172
甲醛水溶液 1毫升
通过测定至少200根单个纤维的直径对每种样品的纤维直径的分布进行测定,它采用***法和扫描电子显微镜或光学显微镜(1000倍)。采用读数来计算该纤维样品的比表面,并且考虑该纤维的比重。
根据SiO2的溶解(骨架溶解),计算所溶解的比厚度,获得溶解速度(纳米/天)。该计算是基于该纤维中的二氧化硅含量、比表面积和溶解的硅数量。
在本说明书中,烧结温度采用下列试验方法测定。
将要测试的由纤维组合物制成的矿棉样品(5×5×7.5厘米)放在预热到700℃的窑炉中。在暴露1.5小时以后,测定样品的收缩和烧结情况。每次采用新的样品重复该方法并且窑炉温度超过前一次窑炉温度50℃直到达到最高的窑炉温度,在该最高温度下看不到该样品在烧结或没有过份的收缩。
在本说明书中,在1400℃下的粘度(泊)根据Bottinga和Weill,美国科学文摘,272卷,1972年5月,455-475页中所说的方法进行计算。
下面是本发明的实施例。
通过将合适比例的原料混合而形成组合物,并且在坩埚窑炉中将每一种组合物熔化并且通过串联喷吹工艺而成纤。该组合物的分析结果及其性能描述在下表中。产品A-Q根据本发明而制造。
产物V具有与工业渣棉相似的分析结果,可以看到,它具有低铝含量,高钙含量和相当低的熔体粘度以及中等的在pH7.5下的溶解速度。产物X与渣棉V有些类似,但它仍具有相当低的熔体粘度,喷丝不容易。此外,由于FeO和MgO含量较低,其纤维热稳定性较低。
产物Y是高铝产物,但是其所有成分的比例使得其熔体粘度太高,喷丝不容易。
产物Z与常规的岩棉产物相似,它具有正常的良好产物性能,但是其在pH4.5下的溶解性较低。它具有相对高的氧化硅含量和相对低的氧化铝含量。
该新纤维可以以任何对MMV纤维来说是常规的方式提供。因此它们可以作为由松散的、未粘结的纤维组成的产物来提供。更为常见的是,它们与粘结剂一起提供,例如由于以常规方式形成纤维并将它们连结在一起。一般说来,可以将该产物作为毡、片或其它成型制品而成型。
本发明的产物可以用于任何MMV纤维的常规目的,例如作为用作保温材料、隔火材料和防护或噪音降低及调节的毡状、板状、管状或其它形状的产物,或者以适用于培育生长介质,或作为纤维、塑料或其它产物增强的游离纤维或作为填料的形状。
纤维种类 | SiO2 Al2O3 TiO2 FeO CaO MgO Na2O K2O% % % % % % % % | 1400℃下的粘度泊 | pH值7.5时的溶解速度(纳米/天) | pH值4.5时的溶解速度(纳米/天) | 烧结温度℃ |
ABCDEFGHIJKLMNOPQVXYZ | 34.5 28.0 1.8 3.3 25.4 5.6 0.6 0.836.2 26.3 1.9 4.9 17.7 10.8 1.0 1.138.3 25.0 1.7 3.0 24.9 5.6 0.7 0.838.1 24.7 1.8 4.6 17.4 11.3 1.2 0.843.2 20.0 1.6 5.0 16.6 11.5 1.2 0.843.2 19.8 1.5 3.4 24.7 5.6 1.0 0.847.7 19.4 0.8 3.7 16.6 10.8 0.4 0.443.7 18.8 3.6 5.4 16.4 9.7 1.8 0.745.6 18.1 1.5 5.3 16.5 9.7 2.5 0.746.9 18.9 0.5 3.3 17.0 9.5 3.4 0.544.1 18.7 1.6 5.2 16.5 9.8 3.3 0.739.6 24.3 1.8 3.2 21.7 6.7 1.8 0.843.8 20.4 1.2 10.3 15.6 8.3 0.2 0.342.9 23.2 0.7 8.8 17.5 5.1 0.6 1.443.1 19.9 1.6 10.1 15.0 9.3 0.6 0.437.8 18.3 0.9 12.0 15.8 10.1 4.7 0.340.0 22.2 2.0 7.5 15.2 10.7 1.5 0.842.7 8.8 0.3 0.4 36.9 9.4 0.7 0.343.1 14.0 0.7 0.5 34.3 5.2 0.7 1.539.7 32.8 1.7 7.0 15.7 2.1 0.3 0.746.9 13.2 3.0 6.4 17.1 9.4 2.6 1.3 | 21.219.424.720.022.827.134.725.130.844.030.330.821.936.819.815.019.48.215.2100.023.7 | 9.56.87.47.95.04.83.05.83.10.92.65.73.94.610.27.113.91.57.82.0 | 34.845.153.864.257.947.021.038.644.435.241.14939.745.951.961.561.141.159.859.33.0 | >800>800>800>800>800>800>800>800>800>800>800>800>1000>900>1000>1000>1000>700>700>1000>1000 |
Claims (15)
1.一种由人造玻璃纤维组成的产物,该纤维由含有下列成分的组合物形成,以氧化物重量计,
SiO2 32-48%
Al2O3 18-30%
CaO 10-30%
MgO 2-20%
FeO 2-15%
Na2O+K2O 0-10%
TiO2 0-6%
其它组分 0-15%
并且该组合物的粘度在1400℃下为10-70泊,
并且该纤维在pH4.5下溶解速度至少为20纳米/天。
2.根据权利要求1的产物,其中该组合物分析结果包括
SiO2 32-48%
Al2O3 18-30%
SiO2+Al2O3 60-75%
CaO 10-30%
MgO 2-20%
FeO 2-12%
Na2O+K2O 0-7%
TiO2 0-4%
其它组分 0-10%。
3.根据权利要求1的产物,其中SiO2+Al2O3的量为55-75%。
4.根据前面权利要求中任意一个的产物,其中
SiO2 34-45%
Al2O3 19-28%
CaO 14-25%
MgO 6-15%
FeO 3-8%
Na2O+K2O 低于5%。
5.根据前面权利要求中任意一个的产物,其中氧化硅与氧化铝的含量之和为61-68%。
6.根据前面权利要求中任意一个的产物,其中氧化铝的量为20-26%。
7.根据前面权利要求中任意一个的产物,其中氧化镁的量为至少8%,氧化铁的量为至少6%。
8.根据前面权利要求中任意一个的产物,其中TiO2的量0-3%,该组合物还含有总量为0-10%的P2O5和/或B2O3,和0-4%其它成分。
9.根据前面权利要求中任意一个的产物,其中它在pH4.5下的溶解速度为25-100纳米/天,优选地为40-80纳米/天。
10.根据前面任一权利要求的产物,其中该组合物在1400℃下的粘度为15-40泊。
11.根据权利要求8的产物,其中所说的粘度为18-30泊。
12.根据前面任一权利要求的产物,其中该纤维在pH7.5下的溶解速度低于15纳米/天。
13.根据前面任一权利要求的产物,其中该纤维的烧结温度至少为800℃,优选地为至少1000℃。
14.根据前面任一权利要求的产物,其中该组合物的液线温度为1240-1340℃。
15.根据前面任一权利要求的产物,它选自保温产物,和隔火防护产物,和噪音降低或调节或保护产物,和培育生长介质,和用纤维增强或填充的产物。
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GB9424126A GB9424126D0 (en) | 1994-11-23 | 1994-11-23 | Man-made vitreous fibres |
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GB9424126.2 | 1994-11-23 | ||
GBGB9500667.2A GB9500667D0 (en) | 1995-01-13 | 1995-01-13 | Man-made vitreous fibres |
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