CN109643591B - 导热电绝缘材料 - Google Patents

导热电绝缘材料 Download PDF

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Publication number
CN109643591B
CN109643591B CN201780050691.8A CN201780050691A CN109643591B CN 109643591 B CN109643591 B CN 109643591B CN 201780050691 A CN201780050691 A CN 201780050691A CN 109643591 B CN109643591 B CN 109643591B
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China
Prior art keywords
thermally conductive
paper
conductive filler
thermal conductivity
filler
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CN201780050691.8A
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CN109643591A (zh
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米切尔·T·黄
罗伯特·H·特平
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3M Innovative Properties Co
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3M Innovative Properties Co
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    • H01B3/18—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances
    • H01B3/48—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances fibrous materials
    • H01B3/52—Insulators or insulating bodies characterised by the insulating materials; Selection of materials for their insulating or dielectric properties mainly consisting of organic substances fibrous materials wood; paper; press board
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Abstract

本发明描述了一种具有大于0.4W/m‑K的热导率的导热电绝缘纸。导热电绝缘纸为非织造纸，所述非织造纸包含芳族聚酰胺纤维、芳族聚酰胺纸浆、基料材料；以及导热填料的协同共混物，其中所述协同共混物包含初级导热填料；以及第二导热填料。

Description

导热电绝缘材料
背景技术
技术领域
本发明涉及适用于电绝缘应用的材料。具体地，本发明涉及适用于变压器、马达、发生器和其它电气装置的电绝缘材料。具体地，本技术涉及一种具有导热填料的协同共混物的导热电绝缘材料。背景技术
热量为电力变压器、马达、发生器和其它电气装置的不期望的副产物。较高操作温度通常减小装置寿命和可靠性以及对实际装置设计施加设计约束。在电力变压器、马达和发生器中所用的电绝缘材料(诸如常规电绝缘纸)通常为不良热导体并且可限制装置的热耗散。
改善电气装置的热转移性能可以为常规电气装置设计提供较低的温度增加或者可实现新的较小电气装置设计。较低装置操作温度根据阿仑尼乌斯方程提供改善的可靠性，该方程推断，操作温度增加10℃使绝缘材料的寿命缩短一半。较低装置操作温度也可以通过减少电阻(焦耳加热)损耗来改善电气装置的效率。较低装置操作温度还可使电气装置在较高功率水平下运行或提供较高过载容量。较低温度升高也可使装置重新设计为更紧凑的装置尺寸，并且通过使用少量金属来更有效地使用原材料，这可降低总装置系统成本。
热转移性能可以通过将热传递介质改变成具有更高热导率的介质或者通过将具有高热阻的材料替换成具有更低热阻或者更高热导率的材料来改善。
用于电绝缘的纸包括牛皮纸或纤维素基纸、有机纸、无机/有机杂合纸和无机纸。适用于本发明的可商购获得的非织造纸的示例包括以商品名CeQUIN得自美国3M公司(3MCompany,USA)的那些，包括但不限于CeQUIN I(约90％的无机元素)、CeQUIN II(CeQUIN I的两层复合物)、CeQUIN X(用于B阶段应用的增强湿强度)以及CeQUIN 3000(约74％的无机元素加有机纤维增强材料)；ThermaVolt无机绝缘纸、ThermaVolt AR无机绝缘纸、FLAMEBARRIER FRB(包括但不限于FLAME BARRIER-FRB-NT压延绝缘纸和FLAME BARRIER FRB-NC未压延绝缘纸)。可从杜邦公司(www2.dupont.com)商购获得的电绝缘材料的示例可以商品名NOMEX获得，包括但不限于NOMEX纸410型、411型(较低密度版本)、414型、418型(包含云母)、419型(418型的低密度版本)和E56型。可从SRO集团(中国)有限公司(SRO Group(China))商购获得的电绝缘材料的示例可以商品名X-FIPER获得；并且从中国烟台美士达特种纸业股份有限公司(Yantai Metastar Special Paper Co.,Ltd.,China)以商品名METASTAR获得。
许多这些常规纸通常用于高温电绝缘应用中，在这些应用中这些纸的热稳定性、电学特性和机械特性十分重要。
常规电绝缘材料通常具有0.25W/m-K或更小的热导率。当这些纸用于电磁线圈绕组时，在导体中生成的热量积聚，并且线圈的温度升高，因为热量不能有效地从线圈绕组传输出去。由于可能因常规电绝缘纸的热导率相对低而引起的热量积聚，线圈的功率密度受到限制。
因此，需要较高热导率的电绝缘纸，其可改善热耗散并在电力变压器、马达、发生器和其它电气装置中提供较低装置操作和热点温度。
发明内容
在某些电绝缘应用中，需要在电气设备应用中达到合适性能的具有较高热导率的材料。
本发明的材料适用于在变压器、马达、发生器以及需要电气部件绝缘的其它装置中为电气部件提供绝缘。
本发明的至少一些实施方案提供一种导热电绝缘纸。导热电绝缘纸为非织造纸，该导热电绝缘纸包含：芳族聚酰胺纤维、芳族聚酰胺纸浆、基料材料；以及导热填料的协同共混物，其中该协同共混物包含初级导热填料；以及第二导热填料。该纸可以另外包含以下中的至少一种：丙烯酸纤维、低导热性无机填料，诸如高岭土和阻燃剂。
在其它实施方案中，导热电绝缘纸包含20重量％-30重量％的有机组分，其中该有机组分的一部分是纤维状的；以及70重量％-80重量％的无机组分，其中该无机组分的一部分为导热填料的协同共混物，其中该协同共混物包含初级导热填料；以及第二导热填料。有机组分包括聚合物纤维、聚合物纸浆和基料材料的组合。并且在一些方面，该纸包括以下组合：对位芳族聚酰胺纤维、丙烯酸类纤维；对位芳族聚酰胺纸浆和丙烯酸胶乳基料材料。在一些实施方案中，无机组分还包括以下中的至少一种：低导热填料、无机阻燃剂和无机颜料。
在一个示例性方面，第一导热填料为具有大于或等于40W/m-K的热导率的高热导率填料，并且第二导热填料为具有小于40W/m-K的热导率的低热导率填料。在一些实施方案中，第一导热填料为氮化硼，并且第二导热填料为以下中的至少一种：二氧化硅、氧化铝和ATH。本文所述的示例性纸的热导率大于0.4W/m-K。
在一个示例性方面，示例性纸是不含纤维素的，并且同样地该纸具有适用于电绝缘系统热类155(F类)、180(H类)、200(N类)和220(R类)中的高热稳定性。
如本说明书中所用：
“不含纤维素的”是指仅含有痕量纤维素基材料，例如含有小于0.5重量％纤维素基材料，优选含有小于0.1重量％纤维素基材料，更优选不含纤维素基材料；
“直接融合”是指无居间层，例如粘合剂层；
“非织造纸”是指主要由短纤维构成的片状材料；
“短纤维”是指长度短于一英寸的纤维；
“MD”或“纵向”是指与材料的连续片材的卷绕方向平行的方向；并且
“其它无机填料”为具有小于0.6W/m-K的热导率的无机填料。
本文所述的非织造纸的至少一个实施方案的优点在于，其在导热填料的相同总体浓度下实现比具有单一高热导率填料的材料高的热导率，同时具有足够的介电强度以及良好的机械强度。所公开的非织造纸的另一种属性包括高温度热稳定性，例如，该示例性材料适用于电绝缘系统热类155(F类)、180(H类)、200(N类)和220(R类)。示例性绝缘纸表现出良好的柔韧性，使得能够在线圈内成绕组或成形，这使得它们能够用于电变压器、马达、发生器和需要电气部件绝缘的其它装置中。
本发明的上述发明内容并非旨在描述本发明的每个公开的实施方案或每种实施方式。下文的详细描述更具体地示出了本发明的实施方案。
附图说明
在下文中将引用本发明的非限制性实施例且参考附图对本发明进行部分描述，在附图中：
图1为示出在根据本发明的示例性导热电绝缘纸中由于导热填料的协同共混物而引起的热导率增强的图表。
图2为示出通过比较所计算和测量的相对热导率因子获得的在根据本发明的示例性导热电绝缘纸中的热导率的改善的图表。
虽然本发明可修正为各种修改形式和另选形式，但其具体形式已在附图中以举例的方式示出，并且将详细描述。然而，应当理解，本发明不将本发明限制于所描述的特定实施方案。正相反，本发明覆盖落入如由所附权利要求书所限定的本发明的范围内的所有修改、等同物和另选方案。
具体实施方式
在以下说明中，应当理解，其它实施方案是设想的并且可在不脱离本发明范围的情况下完成。因此，以下具体实施方式不应被视为具有限制意义。
除非另外指明，否则本说明书和权利要求书中所使用的表达特征尺寸、量和物理特性的所有数在所有情况下均应理解成由术语“约”修饰。因此，除非相反的指明，否则在本说明书和所附权利要求书中列出的数值参数均为近似值，这些近似值可根据本领域技术人员利用本文所公开的教导内容来寻求获得的期望性能而变化。使用由端值表述的数值范围包括该范围内的所有数字和任何值(例如，1至5包括1、1.5、2、2.75、3、3.80、4和5)。
改善材料热导率的常规方法为将最高导热填料的最高负载放入材料中。高热导率填料包括具有大于50W/m-K的热导率的填料并且包括碳纳米管、金刚石颗粒和氮化硼。这些高热导率填料在绝缘纸中用于常规使用可能是昂贵的。
本发明的至少一些实施方案的非织造电绝缘纸包括由短纤维制成的薄片材料，即，小于一英寸(2.54cm)长、优选小于半英寸(1.27cm)的纤维。在本发明的至少一个实施方案中，非织造纸中的大部分纤维是有机的。然而，示例性非织造纸可包含少量无机纤维(<5重量％)。
示例性非织造纸可包含约15重量％至约50重量％、优选约20重量％至约30重量％有机组分和约50重量％至约85重量％、优选约70重量％至约80重量％的无机组分，其中有机组分的一部分是纤维状的。有机组分可包括有机纤维和基料材料。有机组分的一部分包括导热填料的协同共混物，其中该协同共混物包含初级导热填料；以及第二导热填料。无机组分也可包括其它导热填料、低导热填料、其它无机填料、无机阻燃剂、无机颜料等。
该非织造电绝缘纸包括导热填料的协同共混物，其中该协同共混物包含初级导热填料；以及第二导热填料。制品可被制成用于电气设备诸如变压器、马达、发生器的绝缘纸。热量为电力变压器、马达和发生器的不期望的副产物。本发明的绝缘纸可用作层绝缘，以使电变压器中的相同绕组内的电导体的连续层绝缘。导体和绝缘纸在线圈绕组内的多个交替层为其中热耗散为电变压器内的挑战的一个区域。在电动马达或发生器中，槽衬电绝缘定位在发热导体线材和更导热金属材料之间。低导热槽衬材料将为马达或发生器内可能限制热耗散的区域。
本文所述的示例性绝缘材料的较高热导率可改善电气装置的散热，从而导致较低操作温度。此外，来自较高导热纸的改善的热耗散可允许装置/线圈尺寸减小，其中来自较高导热纸的改善的热耗散/较低操作温度可有助于补偿由于装置尺寸减小而导致的操作温度升高，而不显著改变装置的操作温度，从而形成总系统材料成本降低的尺寸较小的变压器。
如本文所述的示例性导热纸或包括示例性导热纸的导热层合体也具有在电动马达/发生器应用中用作槽衬的可能，在这些应用中槽衬被手动/手工插入。马达制造商期望马达/发生器中热耗散得以改善的较高热导率槽衬绝缘材料。为了充当槽衬，绝缘材料必须具有足够的柔韧性，以使得它能够弯曲并成形以用于插入马达定子和/或转子中的狭槽中。
例如，导热绝缘层合材料可包括本公开的层合到聚合物膜表面的导热电绝缘纸。在示例性实施方案中，聚合物膜可为导热聚合物膜，诸如美国临时专利申请62/541,920和62/541,929所述的，该专利全文以引用方式并入本文中。在另一方面，导热聚合物膜可为取向膜，其包括由聚对苯二甲酸乙二醇酯或聚萘二甲酸乙二醇酯形成的取向层以及分散在取向层内的基本上球形的氧化铝颗粒。氧化铝颗粒可以20重量％至40重量％的含量存在于取向膜中。氧化铝颗粒具有20微米或更小、或15微米或更小、或10微米或更小的D99值以及在1至7微米、或1至5微米、或1至3微米范围内的中值尺寸值。
在另选的实施方案中，导热绝缘材料可具有层合到导热聚合物膜的两个表面的导热电绝缘纸。任选地，层合粘合剂层可设置在导热电绝缘纸和导热聚合物膜之间以将各层粘结在一起。
在一些实施方案中，设想了高水平层合构造，其包括多个交替的导热电绝缘纸和导热聚合物膜层。
合适的非织造纸可包含有机纤维，诸如但不限于芳族聚酰胺纤维，包括间位芳族聚酰胺和对位芳族聚酰胺纤维；聚苯硫醚(PPS)纤维；聚酯纤维；聚酰胺纤维、丙烯酸类纤维、三聚氰胺纤维、聚醚醚酮(PEEK)纤维、聚酰亚胺纤维或它们的组合。有机纤维可占非织造纸的有机组分的约40％至80％。在示例性方面，可使用纤维的组合。纤维可在化学组成以及尺寸上发生改变，并且可被选择以改善示例性非织造纸的可制造性以及最终特性。在一些实施方案中，芳族聚酰胺纤维(例如对位芳族聚酰胺纤维)可与非芳族聚酰胺纤维组合以形成本公开的非织造纸。芳族聚酰胺纤维与非芳族聚酰胺纤维的比率可为约15:1至约8:1。
纤维状组分的至少一部分可每份质量具有高表面积，其中表面积大于10m2/g。例如，高表面积纸浆可有利于在纸形成过程中保持纸浆液。为了增加非织造纸中所用的纤维的表面积，可能期望将纤维的至少一部分形成原纤维或将其制成纸浆，以形成纸浆。例如，芳族聚酰胺纤维纸浆可取代示例性非织造纸中的一部分芳族聚酰胺纤维。例如，芳族聚酰胺纤维纸浆可取代示例性纸中的60％至80％芳族聚酰胺纤维。
在一些方面，电绝缘非织造纸的无机组分可任选地包括高表面积无机纤维，诸如具有约0.6μm或更小的平均直径的玻璃微纤维。
在本发明的至少一个实施方案中，非织造纸的有机组分还包括聚合物基料。聚合物基料可占有机组分的约25％至60％。合适的聚合物基料可包括胶乳基材料。在另一方面，合适的聚合物基料可包括但不限于丙烯酸、丙烯酸共聚物、腈、苯乙烯胶乳、瓜尔胶、淀粉和天然橡胶胶乳。在一个示例中，电绝缘纸包含按重量计约7％至约25％的聚合物基料。
如上所述，电绝缘纸包括导热填料的协同共混物，其中该协同共混物包含初级或第一导热填料；以及第二导热填料。第一导热填料为具有大于或等于40W/m-K的热导率的高热导率填料。
例如，氮化硼广泛分类为高导热填料，然而，氮化硼颗粒的各向异性根据正在引用的尺寸而产生完全不同的热导率。六边形氮化硼薄片颗粒具有各向异性的热导率，其中报告的值在(xy)底面方向上为400W/m-K并且在(z)薄片厚度方向上为2W/m-K。在氮化硼颗粒填充的复合材料中，片状取向和颗粒至颗粒的填充特性可影响复合材料的所测量热导率。在文献中已报告各向同性的热导率为50W/m-K(P.Bujard等人，制造中的热信息和电气部件的操作：I-THERM'88(Thermal Phenomena in the Fabrication and Operation ofElectronic Components:I-THERM'88)，国际间会议(InterSociety Conference)，第41-49页，1988)。
其它高热导率填料包括氮化铝(170W/m-K)和碳化硅(360W/m-K)。虽然金属颗粒诸如铜颗粒、铁颗粒、铅颗粒和银颗粒等，举例来说，全部具有超过100W/m-K的热导率，其由于其电导率而不能用于本文所述的示例性绝缘纸中。同样，石墨和碳纳米管不能用于本发明的绝缘纸中。
具有小于40W/m-K的较低热导率的第二导电填料可以选自熔融的无定形二氧化硅(1.5W/m-K)、氧化锆(～2W/m-K)、氧化锌(21W/m-K)和氧化铝(26W/m-K)。
此外，电绝缘非织造纸的无机组分可以包括另一种无机填料。在一个方面，合适的其它无机填料包括但不限于高岭土、滑石、云母、碳酸钙、蒙脱石、绿土、膨润土、伊利石、绿泥石、海泡石、绿坡缕石、埃洛石、蛭石、合成锂皂石、累托石、珍珠岩、以及它们的组合。这些其它无机填料可被表面处理以促进其掺入示例性纸中。合适类型的高岭土包括但不限于水洗高岭土、分层高岭土、煅烧高岭土和经表面处理的高岭土。在一个示例中，电绝缘纸包含按重量计约5％至约20％的高岭土。
电绝缘非织造纸的无机组分可以任选地包括无机阻燃剂。无机阻燃剂可为任何合适的材料。合适的无机阻燃材料的示例包括金属氢氧化物，例如氢氧化镁(MgOH)和三水合氧化铝(ATH)。无机阻燃剂可占非织造纸的至多约20重量％，优选至多约15重量％。在本发明的一些方面，无机阻燃剂可具有足够高的热导率，使得其可用作第二导热填料或用作第三导热填料。例如，ATH具有10至30W/m-K之间的热导率。
本发明的含有无机纤维和无机颗粒中的一种或两种的非织造纸可被称为无机基纸。在电晕/部分放电存在下，无机基纸与例如完全有机基间位芳族聚酰胺纸相比，提供改善的长期电压耐力，因为已知无机材料比有机材料更耐电晕处理。(参见例如2001年10月15日至10月18日在俄亥俄州辛辛那提(Cincinnati,Ohio 10/15-10/18/2001)的电绝缘会议(EIC)/电气制造和线圈绕组(EMCW)展览会2001(The Electrical Insulation Conference(EIC)/Electrical Manufacturing and Coil Winding(EMCW)Expo 2001)，高温电绝缘短期课程(High Temperature Electrical Insulation Short Course)，第21页)。与例如完全有机基间位芳族聚酰胺纸相比，这些无机基纸还可提供用于改善热耗散的更大尺寸稳定性以及更高热导率。
在许多实施方案中，电绝缘纸被成形为可经由标准纸工艺形成的非织造导电纸。例如，制剂的元素可在水中混合为浆液，在造纸筛网上脱水，并干燥。非织造电绝缘纸可被压延以产生高密度纸并且/或者电绝缘纸的若干片材可被堆叠和压延以直接熔合相邻片材并形成较厚的高密度纸。结果是非织造的导热电绝缘纸可以适用于电气设备，例如用于在变压器、马达、发生器或其它电气装置内的电绝缘体。
在一些实施方案中，示例性绝缘材料还可包括膜或网片增强材料。在一个方面，与本文所述的示例性电绝缘导热纸的厚度相比，相对薄的非导热膜可层合到用于机械或电介质增强的示例性纸，并且当与常规的绝缘纸层合体相比时仍可导致改善层合体热导率。例如，薄聚酯薄膜可以层合到本文所述的示例性纸的一侧或两侧。层合可以是膜到纸的直接层合或还可包括将该膜结合至示例性纸的薄粘合剂层。
在另选的方面，可将热导率膜层合到本文所述的示例性导热纸中以便使层合体的热导率最大化。可商购获得的导热膜包括可得自紧固胶粘带制品公司(Fastel AdhesiveProducts)(加利福尼亚州圣克莱门特(San Clemente,CA))的Devinall THB 500聚酰亚胺和Devinall THB 300聚酰亚胺以及可得自杜邦公司(DuPont)(特拉华州威明顿市(Wilmington,DE))的Kapton200MT聚酰亚胺膜、Kapton 300MT聚酰亚胺膜。
实施例
以下提供的实施例和比较例有助于理解本发明，且这些实施例和比较例不应被理解为对本发明范围的限制。除非另外指明，否则所有的份数和百分比均按重量计。使用下述测试方法和方案来评估以下示例性实施例和比较例。
材料
Figure BDA0001972164980000091
样品制备：
使用本领域已知的方法制造示例性电绝缘非织造纸，如下：
将表1至5中提供的10重量％的对位芳族聚酰胺纸浆(比表面积12-15m2/g)、1.5重量％丙烯酸纤维(0.1纤度×3mm)、3.5重量％的对位芳族聚酰胺纤维(1.7旦尼尔×6mm)和10重量％的丙烯酸胶乳的混合物以及75重量％的填料用水分散，以形成固体含量为按重量计约0.06％-0.9％的含水浆液。通过造纸筛网和压机(Williams标准纸浆测试设备)完成脱水。然后将纸干燥。
通过在1000PLI(179kg/cm)的压力和约370℉(188℃)-380℉(193℃)的温度下在钢辊之间以3ft/分钟(0.9m/分钟)的速度压延来形成压延纸。示例性纸的组成信息和测量特性提供在表1至6中。
非织造/聚合物膜层合体制备
使用迈耶棒(#20线号)将层合粘合剂涂覆到聚合物膜的表面上，然后在实验室烘箱中在250℉(121℃)下干燥1次。然后在实验室热辊层合机(ChemsultantsInternational)中，使用购自(密歇根州米德兰陶氏化工(Dow Chemical Company,MidlandMI))的ROBONDTML-330/CR 9-101层合粘合剂在250℉(121℃)和5ft/分钟下，将压延纸层层合到膜上。重复该过程以将第二压延纸层施加到聚合物膜的另一侧上以产生纸/聚合物膜/纸层合体。
测试方法
热导率
根据ASTM E-1530，用Unitherm型号2021保护的热流量计测量热导率值。在180℃下进行测量。在不使用任何界面流体/材料的情况下测量样品，以避免使用渗入电绝缘纸的多孔区域的界面流体/材料的任何潜在复杂性。在不使用界面流体的情况下，在热导率测量中将包括在测试板表面和样品材料表面之间的界面处的热损失，这可使得在此报告的所测量的热导率值低于实际固有材料的热导率。将较薄样品堆叠在一起，直到热阻处于仪器的校准范围内。发现购自杜邦高级纤维系统(DuPont Advanced Fibers Systems)(弗吉尼亚州里士满(Richmond,VA))的常规
Figure BDA0001972164980000102
Paper Type 410的热导率为0.10W/m-K，并且发现购自3M公司(明尼苏达州圣保罗(St.Paul,MN))的常规3MTMThermaVolt压延无机绝缘纸层合体的热导率为0.2W/m-K。
包裹物柔韧性
通过将电绝缘材料包裹在2.54mm(0.1")直径棒周围以查看是否有足够的柔韧性来包裹在棒周围而不会有任何破损，来视觉评价包裹物柔韧性。
水分吸收
将样品放置在环境室中并暴露于指定的老化条件24小时，如表9所提供。通过重力分析并比较干燥样品与指定暴露之后的样品来确定水含量百分比。
另外的测试方法
根据以下标准化测试程序测量另外的机械、电和物理特性。
Figure BDA0001972164980000101
Figure BDA0001972164980000111
表1提供具有改变量的单一高导热填料(即氮化硼)和另一种无机填料(即高岭土)的一系列绝缘纸的组成和测量特性。已发现高岭土在脱水期间帮助纸浆液保持，因此在示例性和比较例制剂两者中包含少量高岭土。
表1：具有氮化硼和粘土的导热纸(组成以重量％/体积％提供)
Figure BDA0001972164980000112
表2提供在恒定量的另一种无机填料(即高岭土)存在下具有两种热填料的协同共混物的一系列绝缘纸的组成和测量特性。高导热填料(即氮化硼)和低导热填料(即二氧化硅)的量在保持纸常数中的总无机含量时发生改变。
表2：具有氮化硼、熔融二氧化硅和粘土的导热纸(组成以重量％/体积％提供)
Figure BDA0001972164980000121
表3提供在恒定量的另一种无机填料(即高岭土)和ATH存在下具有两种热填料的协同共混物的一系列绝缘纸的组成和测量特性。高导热填料(即氮化硼)和低导热填料(即二氧化硅)的量在保持纸常数中的总无机含量时发生改变。
表3：具有氮化硼、熔融二氧化硅、ATH和粘土的导热纸(组成以重量％/体积％提 供)
Figure BDA0001972164980000122
Figure BDA0001972164980000131
表4提供在恒定量的另一种无机填料(即高岭土)存在下具有两种热填料的协同共混物的一系列绝缘纸的组成和测量特性。高导热填料(即氮化硼)和低热导率填料/阻燃剂(即ATH)的量在保持纸常数中的总无机含量时发生改变。
表4：具有氮化硼、ATH和粘土的导热纸(组成以重量％/体积％提供)
Figure BDA0001972164980000132
表5提供在恒定量的另一种无机填料(即高岭土)和ATH存在下具有两种热填料的协同共混物的一系列绝缘纸的组成和测量特性。高导热填料(即氮化硼)和低导热填料(即氧化铝)的量在保持纸常数中的总无机含量时发生改变。已发现粘土帮助纸浆液保持，因此在制剂中包含少量粘土。
表5：具有氮化硼、氧化铝、ATH和粘土的导热纸(组成以重量％/体积％提供)
Figure BDA0001972164980000141
表6提供在另一种无机填料(即高岭土)存在下具有两种热填料的协同共混物的一系列绝缘纸的组成和测量特性。高导热填料(即氮化硼)和低导热填料(即碳酸钙或碳酸钙和氧化铝)的量在保持纸常数中的总无机含量时发生改变。
表6：具有氮化硼、碳酸钙、ATH和粘土；氮化硼、碳酸钙和粘土的导热纸(组成以重 量％/体积％提供)
Figure BDA0001972164980000142
Figure BDA0001972164980000151
表7示出通过将实施例14的导热纸层合到指定的聚合物膜来制成的三种纸/聚合物膜/纸层合体构造(实施例16至实施例18)的数据。所用的膜为标准聚酯(PET)膜，诸如可购自三菱聚酯膜公司(Mitsibushi Polyester Film)(南卡罗来纳州格里尔(Greer,SouthCarolina))的Hostaphan 2262、可购自JBF RAK LLC(阿拉伯联合酋长国(United ArabEmerites))的ARYAPET A460和购自3M公司(明尼苏达州圣保罗(St.Paul,MN))的系列777和860聚酯；高热导率聚酯薄膜(HTCD PET)膜，诸如描述在美国临时专利申请62/541,920所述的，该专利以引用的方式并入本文中；以及聚酰亚胺膜，诸如购自紧固件胶粘剂和基材产品(Fastel Adhesive&Substrate Products)(加利福尼亚州圣克莱门特(San Clemente,CA))的DevinallTM500THB聚酰亚胺膜。
表7：导热纸/聚合物膜/纸层合体材料
Figure BDA0001972164980000152
Figure BDA0001972164980000161
表8示出可商购获得的无机基纸层合体的特性。表8中包括的商业纸层合体为购自3M公司(明尼苏达州圣保罗(St.Paul,MN))的3MTM ThermaVolt TvFTv柔性层合体。为了参考，测量另外的电绝缘层合体，诸如Nomex-Mylar-Nomex(3-3-3)，诸如购自杜邦公司(Dupont)(特拉华州威明顿市(Wilmington,DE))的NMN 333
Figure BDA0001972164980000165
层合体类型NMN，以具有0.12W/mK的热导率值。
表8：选择商用无机基纸层合体的特性
物理特性 TvFTv 3-1-3 TvFTv 4-2-4 TvFTv 3-3-3
标称厚度(密耳) 7 10 9
基重(lbs/yd<sup>2</sup>) 254 388 327
纵向拉伸(lbs/英寸) 52 87 101
横向拉伸(lbs/英寸) 33 63 77
纵向伸长率(％) 2 3 3
横向伸长率(％) 3 3 3
纵向撕裂(g) 170 400 480
横向撕裂(g) 200 498 588
吸湿性(％) <1 <1 <1
介电击穿电压(kV) 7.6 11 11
热导率(W/m.K) 0.19 0.21
测定示例性纸(实施例14)和示例性层合体构造(实施例17)以及二者均购自杜邦公司(Dupont)(特拉华州威明顿市(Wilmington,DE))的常规纸(
Figure BDA0001972164980000162
Type 410-3密耳)和常规层合体材料(NMN 333
Figure BDA0001972164980000163
层合体类型NMN)的水分(水)吸收含量。
表9：示例性导热绝缘纸和层合体材料与常规绝缘纸和层合体材料的水分吸收的 比较
Figure BDA0001972164980000164
Figure BDA0001972164980000171
图1为示出所选择数据的图，该数据显示与具有单一高导热填料(即来自表1的氮化硼)的类似纸相比，根据存在于纸中的氮化硼的体积百分比，第一导热填料和第二导热填料的共混物对来自表2至5的非织造纸的热导率的协同作用。氮化硼和氧化铝、氮化硼和二氧化硅以及氮化硼和ATH的组合在较低氮化硼载量下获得比可由具有单独氮化硼的纸制剂获得的更高的热导率。由于氮化硼是昂贵的，在较低载量下获得较高热导率的能力是有用的。
包含至少两种导热填料的组合的示例性电绝缘纸的所计算的总热导率系数等于每种单独组分的体积分数乘以每种单独组分的热导率之和或者为kp＝Σ(Vf,i×ki)，其中kp为示例性纸的总热导率系数，Vf,i为存在于示例性纸中的给定组分i的体积分数，并且ki为组分i的热导率系数。对于由比较例表示的每种纸(即包含单一导热填料的导热纸)重复类似的过程。
根据示例性纸材料的计算的总热导率系数，计算出所计算的相对热导率系数，并且通过含有单一导热填料(即氮化硼，如比较例中所提供)的纸的所计算总热导率系数进行归一化。相对热导率系数等于具有至少两种导热填料的示例性纸的所计算的总热导率系数减去仅具有氮化硼的纸的所计算的总热导率系数的量除以具有氮化硼的纸的所计算的总热导率系数。
然后计算包含至少两种导热填料的组合的示例性纸材料的实际测量热导率的测量的相对热导率系数并且将其归一化至包含单一导热填料氮化硼的导热纸的测量的热导率。通过获得包含至少两种导热填料的示例性纸之一的测量的热导率并且减去具有氮化硼作为唯一导热填料的纸的测量的热导率并且在相同近似氮化硼载量下通过减去具有氮化硼作为唯一导热填料的纸的测量的热导率去除来发现包含至少两种导热填料的组合的示例性纸材料的所测量的相对热导率系数。
图2比较在相当体积分数的氮化硼载量下所测量的相对热导率系数和所计算的相对热导率系数。该图显示具有至少两种导热填料的纸的所测量的相对热导率系数(三角形符号)高于在考虑不同颗粒组分的体积载量差异时所计算的相对热导率系数(圆形符号)。实心符号表示具有导热填料(氮化硼、熔融二氧化硅和氧化铝三水合物)第三共混物的示例性纸的数据并且空心符号表示具有导热填料(氮化硼和氧化铝三水合物)二级共混物的示例性纸的数据。
虽然本文出于说明优选实施方案的目的对具体实施方案进行了举例说明和描述，但是本领域的普通技术人员应当理解，在不脱离本发明范围的前提下，各种替代和/或等同实施方式可以取代举例说明和描述的具体实施方案。本申请旨在涵盖本文所讨论优选实施方案的任何修改和更改。因此，显而易见，本发明旨在仅受权利要求书及其等同形式的限制。

Claims (21)

1.一种导热电绝缘纸，所述导热电绝缘纸包含：
芳族聚酰胺纤维；
芳族聚酰胺纸浆；
基料材料；以及
导热填料的协同共混物，其中所述协同共混物包含第一导热填料；以及第二导热填料；
其中所述第一导热填料为具有大于或等于40W/m-K的热导率的高热导率填料，并且所述第二导热填料为具有小于40W/m-K的热导率的低热导率填料，
其中所述第一导热填料为氮化硼并且所述第二导热填料为二氧化硅和碳酸钙中的至少一种。
2.根据权利要求1所述的纸，所述纸还包含丙烯酸纤维。
3.根据权利要求1所述的纸，所述纸还包含其它无机填料。
4.根据权利要求3所述的纸，其中所述其它无机填料包括高岭土。
5.根据权利要求1所述的纸，所述纸还包含第三导热填料。
6.根据权利要求1至5中任一项所述的纸，其中所述基料材料为丙烯酸胶乳。
7.根据权利要求1至5中任一项所述的纸，其中所述纸的所述热导率大于0.4W/m-K。
8.根据权利要求1至5中任一项所述的纸，其中所述芳族聚酰胺纤维为具有小于0.5英寸的长度的对位芳族聚酰胺纤维。
9.根据权利要求1至5中任一项所述的纸，其中所述芳族聚酰胺纸浆为对位芳族聚酰胺纸浆。
10.一种导热电绝缘纸，所述导热电绝缘纸包含：
20重量％至30重量％的有机组分，其中所述有机组分的一部分是纤维状的；以及
70重量％至80重量％的无机组分，其中所述无机组分的一部分为导热填料的协同共混物，其中所述协同共混物包含第一导热填料；以及第二导热填料；
其中所述第一导热填料为具有大于或等于40W/m-K的热导率的高热导率填料，并且所述第二导热填料为具有小于40W/m-K的热导率的低热导率填料，
其中所述第一导热填料为氮化硼并且所述第二导热填料为二氧化硅和碳酸钙中的至少一种。
11.根据权利要求10所述的纸，其中所述有机组分包括聚合物纤维、聚合物纸浆和基料材料的组合。
12.根据权利要求11所述的纸，其中所述有机组分包括以下组合：对位芳族聚酰胺纤维、丙烯酸纤维；对位芳族聚酰胺纸浆和丙烯酸胶乳基料材料。
13.根据权利要求10至12中任一项所述的纸，所述纸还包含其它无机填料。
14.根据权利要求13所述的纸，其中所述无机填料为高岭土。
15.一种用于电气设备的电绝缘材料，其中所述电绝缘材料包括根据权利要求1或10中任一项所述的纸。
16.根据权利要求15所述的用于电气设备的电绝缘材料，其中所述电气设备包括变压器、马达和发电机中的一种。
17.一种导热绝缘材料，所述导热绝缘材料包括：
根据权利要求1至14中任一项所述的导热电绝缘纸，所述导热电绝缘纸层合到聚合物膜的表面。
18.根据权利要求17所述的导热绝缘材料，其中所述聚合物膜为导热聚合物膜。
19.根据权利要求18所述的导热绝缘材料，其中所述导热电绝缘纸层合到所述导热聚合物膜的两个表面。
20.根据权利要求18所述的导热绝缘材料，所述导热绝缘材料还包括设置在所述导热电绝缘纸和所述导热聚合物膜之间的层合粘合剂层。
21.一种用于电气设备的电绝缘材料，其中所述电绝缘材料包括根据权利要求17所述的导热绝缘材料。
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