CN1771343B - 用于制造金属基质复合材料的组合物 - Google Patents
用于制造金属基质复合材料的组合物 Download PDFInfo
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Abstract
在一个具体实施方式中,一种与熔融金属混合以制造金属基质复合材料的组合物(10),该组合物的特征在于:一种陶瓷补强填充剂(12),该陶瓷补强填充剂不能被熔融铝润湿和/或在熔融铝中不具有化学稳定性,该陶瓷补强填充剂涂有一种陶瓷材料,该陶瓷材料可以被熔融铝润湿并在熔融铝中具有化学稳定性。在一个相关具体实施方式中,一种制造多孔预成型坯的组合物(20),该预成型坯被熔融金属渗透以制造金属基质复合材料,该组合物的特征在于:一种陶瓷补强填充剂(23),该陶瓷补强填充剂不能被熔融铝润湿,该陶瓷补强填充剂涂有一种陶瓷材料(22)并任选地涂有例如镍的金属(21),该陶瓷材料可以被熔融铝润湿。该陶瓷材料可以通过例如真空溅射的真空沉积技术涂布在陶瓷补强填充剂上。
Description
技术领域
本发明涉及其中补强填充剂与金属相交互分散(interdisperse)的材料。换言之,本发明涉及金属基质复合材料(MMC)。
背景技术
金属基质复合材料(MMC)是其中补强填充剂与金属相交互分散的一类材料。参看Rohatgi,Defense Science Journal,Vol.43,No.4,October 1993,pp 323-349。在一种MMC材料的制备中,微粒陶瓷补强填充剂与熔融金属混合,然后将该混合物冷却以形成MMC制品。在另一种MMC材料的制备中,使含有陶瓷补强填充剂的多孔陶瓷预成型坯被熔融金属浸透,然后将填充了金属的预成型坯冷却以形成MMC制品。MMC比金属刚硬和坚固但是比陶瓷有延性。
一般而言,为了使通过上述第一种制备方法(将陶瓷补强填充剂与熔融金属混合然后将该混合物冷却以形成MMC制品)制得的MMC获得高性能,应该是:(a)陶瓷补强填充剂具有被熔融金属良好润湿的能力;(b)陶瓷补强填充剂具有在熔融金属中良好的化学稳定性;(c)陶瓷补强填充剂具有在熔融金属中良好的分散性;(d)形成MMC后,陶瓷补强填充剂具有与金属之间良好的粘合性。
一般而言,为了使通过上述第二种方法(使预成型坯被熔融金属浸湿然后将填充了金属的预成型坯冷却以形成MMC制品)制得的MMC获得高性能,应该是:(a)预成型坯的陶瓷补强填充剂具有被熔融金属良好润湿的能力;和(b)形成MMC后,陶瓷补强填充剂具有与金属之间良好的粘合性。
在MMC中表现良好的陶瓷补强填充剂(例如与熔融铝混合的二硼化钛或碳化钛;或被熔融铝浸透的多孔碳化硼预成型坯)相对昂贵,从而明显提高MMC制品的成本。成本相对较低的陶瓷补强填充剂在MMC中的性能很差。例如,氧化铝(Al2O3)和二氧化硅(SiO2)是成本相对较低的补强填充剂材料,但是二氧化硅和氧化铝都不能被熔融铝润湿。氧化铝补强填充剂粒子容易在熔融铝中聚结而不是较好地分散,而二氧化硅在熔融铝中起反应以形成富含硅的Al和Al2O3。如果能够使用不能被熔融铝润湿的那类相对低成本陶瓷补强填充剂来制造较低成本的高性能MMC,这将是MMC工艺的重大进展。
发明内容
本发明是一种与熔融金属混合以制造金属基质复合材料的组合物,该组合物的特征在于:一种陶瓷补强填充剂,该陶瓷补强填充剂不能被熔融铝润湿和/或在熔融铝中不具有化学稳定性,该陶瓷补强填充剂涂有一种陶瓷材料,该陶瓷材料可以被熔融铝润湿并且在熔融铝中具有化学稳定性。
在另一具体实施方式中,本发明是一种制造多孔预成型坯的组合物,该预成型坯被熔融金属浸透以制造金属基质复合材料,该组合物的特征在于:一种陶瓷补强填充剂,该陶瓷补强填充剂不能被熔融铝润湿,该陶瓷补强填充剂涂有一种陶瓷材料,该陶瓷材料可以被熔融铝润湿。
在另一具体实施方式中,本发明是一种用陶瓷材料涂布陶瓷补强填充剂的方法,该方法的特征在于下述步骤:(a)将陶瓷补强填充剂置于真空室内,和(b)使一种陶瓷材料在真空室中汽化以使该陶瓷材料沉积在陶瓷补强填充剂上。
在又一具体实施方式中,本发明是一种通过下述方法制得的金属基质复合材料制品,该方法的特征在于下述步骤:(a)将熔融铝或熔融铝合金与这部分第一段的组合物混合以形成其混合物;和(b)将该混合物冷却以形成金属基质复合材料制品。
在再一具体实施方式中,本发明是一种通过下述方法制得的金属基质复合材料制品,该方法的特征在于下述步骤:(a)由这部分第二段的组合物形成多孔预成型坯;(b)使该多孔预成型坯与熔融铝或熔融铝合金接触以使熔融铝或熔融铝合金渗入多孔预成型坯以制造被渗透的预成型坯;和(c)将该被渗透的预成型坯冷却以形成金属基质复合材料制品。
在又一具体实施方案中,本发明是一种由铝或铝合金和不能被熔融铝润湿和/或在熔融铝中不具有化学稳定性的陶瓷补强填充剂制备金属基质复合材料制品的方法,所述方法包括
a)使用可由熔融铝润湿和在熔融铝中具有化学稳定性的陶瓷材料涂布陶瓷填充剂,
b)将熔融铝或熔融铝合金与涂布的陶瓷补强填充剂混合以形成其熔融混合物,
c)浇铸该熔融混合物,和
d)冷却该混合物以形成金属基质复合材料制品。
附图的简要说明
图1是本发明的由涂有一层碳化硼的氧化铝粒子构成的组合物的截面图。
图2是本发明的由涂有一层二硼化钛的二氧化硅粒子构成的另一种组合物的截面图,该二硼化钛层上又涂有一层镍。
本发明的实施方式
参照图1,显示了本发明的由涂有一层碳化硼12的氧化铝补强填充剂粒子12构成的组合物10的截面图。在传统的等离子溅射室中将碳化硼等离子溅射到机械搅拌过的氧化铝粒子上,从而在氧化铝粒子12上形成该层碳化硼12。未涂布的氧化铝粒子不能被熔融铝“润湿”。此处使用的术语润湿是指接触角大于九十度。碳化硼涂层被熔融铝(例如温度高于1000℃的铝)润湿。
可以通过任何适当的技术(例如滑移浇铸),使图1所示的具体材料形成多孔陶瓷预成型坯,使多孔预成型坯与熔融铝接触以使熔融铝(或熔融铝合金)渗入多孔陶瓷预成型坯,然后冷却形成MMC制品。由于熔融铝润湿了氧化铝粒子12上的碳化硼层11,因此熔融铝会通过毛细作用进入多孔预成型坯。
图1所示的具体材料并不特别适合与熔融铝(或熔融铝合金)混合以浇铸MMC制品,因为碳化硼层11容易在能够浇铸熔融铝之前与熔融铝反应,也就是说,碳化硼层在熔融铝中不是化学上稳定的,而且所得的脱除涂层的氧化铝粒子容易在熔融铝中聚结。因此,当在本发明中使用氧化铝补强填充剂与熔融铝混合以浇铸MMC制品时,使用的是一种化学上稳定的陶瓷材料涂层,例如二硼化钛或更优选的额外涂有钨或镍的二硼化钛。类似地,当使用石墨补强填充剂时,陶瓷材料涂层可以是碳化硅或者二硼化钛,后者更优选额外涂有钨、钴或镍。
现在参照图2,显示了本发明的另一种高度优选的组合物20的截面图,该组合物由涂有一层二硼化钛22的二氧化硅补强填充剂粒子23构成,该二硼化钛层22又涂有一层镍21。二硼化钛层22被熔融铝润湿,而镍层21增强了组合物20被熔融铝润湿的能力。在传统的等离子溅射室中将二硼化钛等离子溅射到机械搅拌过的二氧化硅粒子上,然后通过退火过程将基本无定形的二硼化钛转化成更密实和结晶状的退火二硼化钛,由此在二氧化硅粒子23上形成二硼化钛层22。可以通过X射线衍射分析法进行陶瓷材料涂层结构的测定以确定其是无定形的还是退火的。
可以如下进行退火过程:在涂布步骤后将氩气加入等离子溅射室,然后将组合物加热至足以使陶瓷材料退火的温度以使陶瓷材料基本不会与熔融铝进行反应。基本无定形的二硼化钛涂层可以在1000℃下退火大约1小时。基本无定形的氮化钛涂层可以在700℃下退火大约1或2小时并在1000℃下退火大约半小时。然后通过传统的无电镀镍法形成镍层21。镍层21增强了组合物被熔融铝或熔融铝合金润湿的能力。或者,如果在等离子溅射过程中加热填充材料(例如加热至500-700℃)的话,就可以在填充材料上涂布已经是退火涂料的二硼化钛(或氮化钛或其它陶瓷材料)。
图2所示的具体材料特别适合与熔融铝混合以浇铸MMC制品,因为退火的二硼化钛层22在可以浇铸熔融铝之前不会与熔融铝反应(即使没有镍层21),也就是说,退火的二硼化钛层22在熔融铝中是化学上稳定的。另一方面,如果陶瓷补强填充剂上涂布的二硼化钛(或者氮化钛)没有退火,那么令人吃惊的是,二硼化钛(或者氮化钛或者几乎任何其它以其它方式为非反应性的陶瓷材料)会与熔融铝或熔融铝合金反应。当二硼化钛或氮化钛没有退火并且与熔融铝或熔融铝合金反应时,钛就容易有利地与铝形成合金。
上述与图1和图2有关的论述涉及具体实施方式。但是,应该理解的是,在大范围内,本发明是一种与熔融金属混合以制造金属基质复合材料的组合物或者一种制造多孔预成型坯(其被熔融金属浸透以制造金属基质复合材料)的组合物,该组合物包括:陶瓷补强填充剂,该陶瓷补强填充剂不能被熔融铝润湿和/或在熔融铝中不具有化学稳定性,该陶瓷补强填充剂涂有一种陶瓷材料,该陶瓷材料可以被熔融铝、熔融镁、熔融铜、熔融钛或其合金润湿和/或在其中具有化学稳定性。
该陶瓷补强填充剂优选选自氧化物、碳化物、硼化物或氮化物,例如砂子、粘土、富铝红柱石、氧化铝、二氧化钛、氧化镁、二氧化硅、碳、氧化铁、氧化钇、氧化锆、氧化钼、氧化钽、碳化铌、碳化钨和碳化硅。陶瓷补强填充剂最优选选自氧化铝、碳化硅、二氧化硅或针状富铝红柱石。陶瓷材料涂层优选选自二硼化钛、氮化铝、氮化钛、碳化钛、碳化硅或碳化硼。任选的额外金属涂层优选选自W、Mo、Ti、Ni、Cu、Hf、Fe、Co、Al或Si。可以通过任何合适的方法但是优选通过传统的等离子溅射法在陶瓷补强填充剂上涂布陶瓷材料。最优选地,任选涂布在陶瓷材料涂层上的金属是镍或钨。可以通过任何适当的方法,例如无电沉积、电镀和等离子溅射法在陶瓷材料层上涂布金属层。
涂有二硼化钛的针状富铝红柱石是本发明的一种优选具体实施方式。涂有二硼化钛,然后涂有镍的针状富铝红柱石也是本发明的一种优选具体实施方式。涂有碳化硅的碳(无定形碳或石墨碳)是本发明的一种优选具体实施方式。涂有碳化硅然后涂有钨、铜或镍的碳(无定形碳或石墨碳)也是本发明的一种优选具体实施方式。陶瓷补强填充剂可以是任何形状的,例如片晶状、须晶状或纤维状以及纵横比接近或等于1的粒子状。
陶瓷补强填充剂上的陶瓷材料涂层的厚度优选小于1微米,更优选小于半微米,再优选小于1/10微米。优选较薄的涂层以降低组合物的成本。然而,太薄的陶瓷材料涂层仍会留下相当部分的填充剂与熔融金属接触,从而导致填充剂的化学不稳定性和/或填充剂聚结。最优选地,涂层既薄又能完全覆盖填充剂。补强填充剂的粒度典型为10至100微米。
本发明的金属基质复合材料制品可以如下由本发明的组合物制成:(a)将例如熔融铝或熔融铝合金的熔融金属与这种组合物混合以形成金属-组合物混合物;和(b)然后将该金属-组合物混合物冷却以形成金属基质复合材料制品。在多数情况下,可以在步骤(b)之前将金属-组合物混合物加入模具中。
本发明的金属基质复合材料制品也可以如下由本发明的组合物制成:(a)形成多孔预成型坯,该多孔预成型坯含有这种组合物;(b)使多孔预成型坯被例如熔融铝或熔融铝合金的熔融金属浸透以形成被浸透的预成型坯;和(b)将被浸透的预成型坯冷却以形成金属基质复合材料制品。例如,该预成型坯可以包括具有针形态的互连富铝红柱石细粒(针状富铝红柱石)作为陶瓷补强填充剂。
本发明的金属基质复合材料制品可用于几乎无限多的应用中。例如,本发明的金属基质复合材料制品可以是选自散热器、受热器(heatsinks)、复合散热器/受热器或热底板的热处理制品。本发明的用于机动车应用领域的金属基质复合材料制品的例子包括选自盘式制动器转子、制动衬块、制动器汽缸活塞、制动钳、制动衬块背板、制动鼓、转向节、发动机气缸套、气缸盖镶圈、活塞、活塞环、主轴承嵌片、凸轮凸角、凸轮随动件、阀、阀杆导承或阀座的零件。
实施例1
将100克氧化铝粉末(来自Alcoa的A10级)置于真空溅射室的搅拌杯中。溅射靶(碳化硼)直径为15厘米并将其固定于水冷支架中。该靶离搅拌杯4厘米并以180瓦特运作。氧化铝粉末在溅射室中被涂上碳化硼,然后称重。称得涂布后的氧化铝粉末为102克。X射线光电子能谱分析表明,氧化铝上碳化硼的表面覆盖率约为80%。将涂有碳化硼的氧化铝压成盘形预成型坯并在1200℃的真空烘箱中与铝接触。铝熔化并通过毛细作用进入预成型坯,然后将其从烘箱中取出并冷却至室温以形成盘形MMC制品。
实施例2
将100克氧化铝粉末(来自Alcoa的A10级)置于真空溅射室的搅拌杯中。将溅射靶(二硼化钛)固定于水冷支架中。氧化铝粉末在溅射室中被涂上二硼化钛,然后称重。称得涂布后的氧化铝粉末为103克。X射线光电子能谱分析表明,氧化铝上二硼化钛的表面覆盖率约为85%。X射线衍射分析表明二硼化钛涂层在晶体结构上基本是无定形的。将涂有二硼化钛的氧化铝压成盘形预成型坯并在1200℃的真空烘箱中与铝接触。铝熔化并通过毛细作用进入预成型坯,然后将其从烘箱中取出并冷却至室温以形成盘形MMC制品。
实施例3
将100克氧化铝粉末(来自Alcoa的A10级)置于真空溅射室的搅拌杯中。将溅射靶(钛金属)固定于水冷支架中。真空室含有降低压力的氮气体。氧化铝粉末在溅射室中被涂上氮化钛,然后称重。称得涂布后的氧化铝粉末为102克。X射线光电子能谱分析表明,氧化铝上氮化钛的表面覆盖率约为85%。X射线衍射分析表明氮化钛涂层在晶体结构上基本是无定形的。将涂有氮化钛的氧化铝用无电镀镍溶液处理以便在氮化钛涂层上沉积100微米厚的镍层。将涂有氮化钛(该氮化钛涂有镍)的氧化铝压成盘形预成型坯并在750℃的真空烘箱中与铝接触。铝熔化并迅速通过毛细作用进入预成型坯,然后将其从烘箱中取出并冷却至室温以形成盘形MMC制品。
实施例4
将100克氧化铝粉末(来自Alcoa的A10级)置于真空溅射室的搅拌杯中。将溅射靶(二硼化钛)固定于水冷支架中。氧化铝粉末在溅射室中被涂上二硼化钛,然后称重。称得涂布后的氧化铝粉末为103克。X射线光电子能谱分析表明,氧化铝上二硼化钛的表面覆盖率约为85%。X射线衍射分析表明二硼化钛涂层在晶体结构上基本是无定形的。然后将涂有二硼化钛的氧化铝粉末在氩气中加热至1000℃达到大约1小时以便将二硼化钛涂层退火。X射线衍射分析表明,现在二硼化钛涂层在结构上基本是晶体。将涂有退火二硼化钛的氧化铝与熔融铝混合并浇铸到模具中。将模具冷却至室温以形成MMC制品。截取MMC制品的横截面并通过电子显微术观察,表明涂有二硼化钛的氧化铝粉末分散在铝中。
实施例5
将100克二氧化硅粉末(平均粒度为大约50微米)置于真空溅射室的搅拌杯中。将溅射靶(钛)固定于水冷支架中。真空室含有降低压力的氮气体。二氧化硅粉末在溅射室中被涂上氮化钛,然后称重。称得涂布后的二氧化硅粉末为104克。X射线光电子能谱分析表明,二氧化硅上氮化钛的表面覆盖率超过90%。X射线衍射分析表明氮化钛涂层在晶体结构上基本是无定形的。然后将涂有氮化钛的二氧化硅粉末在氩气中加热至1000℃达到大约半小时以便将氮化钛涂层退火。X射线衍射分析表明,现在氮化钛涂层在结构上基本是晶体。将涂有退火氮化钛的二氧化硅与熔融铝混合并浇铸到模具中。将模具冷却至室温以形成MMC制品。截取MMC制品的横截面并通过电子显微术观察,表明涂有氮化钛的二氧化硅粉末分散在铝中。
Claims (10)
1.一种由铝或铝合金和不能被熔融铝润湿和/或在熔融铝中不具有化学稳定性的陶瓷补强填充剂制备金属基质复合材料制品的方法,所述方法包括
a)使用可由熔融铝润湿和在熔融铝中具有化学稳定性的陶瓷材料涂布陶瓷补强填充剂,其中涂布在陶瓷补强填充剂上的陶瓷材料选自退火的二硼化钛或退火的氮化钛,
b)将熔融铝或熔融铝合金与涂布的陶瓷补强填充剂混合以形成其熔融混合物,
c)浇铸该熔融混合物,和
d)冷却该混合物以形成金属基质复合材料制品。
2.根据权利要求1所述的方法,在步骤d)之前进一步包括提供一层涂在涂布的陶瓷补强填充剂上的金属层。
3.根据权利要求1或2所述的方法,其中颗粒陶瓷补强填充剂选自砂子、富铝红柱石、氧化铝或二氧化硅。
4.根据权利要求1所述的方法,其中提供所述的金属涂层,且金属涂层的金属是镍。
5.根据上述权利要求任一项所述的方法,其中可由熔融铝润湿和在熔融铝中具有化学稳定性的陶瓷材料的涂布厚度小于1微米。
6.根据权利要求5所述的方法,其中涂布厚度小于0.5微米。
7.根据权利要求6所述的方法,其中涂布厚度小于0.1微米。
8.根据权利要求1所述的方法,其中陶瓷补强填充剂是氧化物。
9.根据权利要求2所述的方法,其中金属选自W、Mo、Ti、Ni、Cu、Hf、Fe、Co、Al或Si。
10.根据权利要求9所述的方法,其中金属是Ni或W。
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CN103302268A (zh) * | 2013-06-27 | 2013-09-18 | 重庆罗曼耐磨材料有限公司 | 一种陶瓷金属复合耐磨材料的制备方法 |
US10113502B2 (en) * | 2015-09-08 | 2018-10-30 | Ford Global Technologies, Llc | Cylinder head for an internal combustion engine |
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Also Published As
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DE602004014753D1 (de) | 2008-08-14 |
CA2521499A1 (en) | 2004-10-28 |
CN101818322A (zh) | 2010-09-01 |
JP4809216B2 (ja) | 2011-11-09 |
US20110135948A1 (en) | 2011-06-09 |
US8399107B2 (en) | 2013-03-19 |
KR20050110039A (ko) | 2005-11-22 |
ATE399886T1 (de) | 2008-07-15 |
CN1771343A (zh) | 2006-05-10 |
WO2004092430A3 (en) | 2005-01-27 |
EP1618222A2 (en) | 2006-01-25 |
WO2004092430A2 (en) | 2004-10-28 |
EP1618222B1 (en) | 2008-07-02 |
JP2006522875A (ja) | 2006-10-05 |
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