CN113416075A - 一种制备Diamond/SiC复合材料的方法 - Google Patents

一种制备Diamond/SiC复合材料的方法 Download PDF

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CN113416075A
CN113416075A CN202110791110.4A CN202110791110A CN113416075A CN 113416075 A CN113416075 A CN 113416075A CN 202110791110 A CN202110791110 A CN 202110791110A CN 113416075 A CN113416075 A CN 113416075A
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黄国钦
邢波
徐西鹏
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Abstract

本发明公开了一种制备Diamond/SiC复合材料的方法,包括如下步骤:1)制备金刚石预制体:将金刚石、石墨、硅粉、粘结剂按质量比混合均匀并压制生坯,将生坯在1000‑1200℃保护气氛下碳化得金刚石预制体;2)制备Diamond/SiC复合材料:将金刚石预制体置于氮化硅粉末上,于1500‑1700℃真空炉中充分反应1‑2h即得Diamond/SiC复合材料。本发明有效的避免了过量硅粉对样品的粘连,便于后续样品处理。

Description

一种制备Diamond/SiC复合材料的方法
技术领域
本发明涉及材料领域,具体涉及一种制备Diamond/SiC复合材料的方法。
背景技术
Diamond/SiC复合材料具有较高的热导率、较低的热膨胀系数与密度以及良好的综合力学性能,是极具发展前景的新一代电子封装材料。Diamond/SiC复合材料的制备工艺,已有大量学者进行了约20年的研究。现有技术例如:
CN201110065272.6提供了一种高性能Diamond/SiC电子封装材料的制备工艺,首先按重量百分比,将10~15%的粘接剂,5~20%的石墨,20~40%的硅粉,30~60%的金刚石颗粒湿混,混合时间16~24h。然后在10~50MPa压力和150℃的温度下温压成形获得复合材料毛坯。在氩气保护气氛中1100℃烧结24h,随炉冷却后得到具有一定强度和孔隙度的Diamond/Si/C多孔基体。然后将气相渗透的渗料置于石墨坩埚中,将所制备的Diamond/Si/C多孔基体置于该石墨坩埚上,然后整体置于高真空烧结炉中进行真空气相渗透1-2h,渗透温度1500~1650℃,真空度-0.08~-0.01MPa。随炉冷却后即可获得致密的Diamond/SiC电子封装材料。
CN201710571894.3公开了一种金刚石/碳化硅复合材料,包括如下重量份的原料:粘结剂10-15份、碳黑5-20份、碳化硅30-60份、金刚石30-60份。该发明的Diamond/SiC复合材料在原料中加入碳化硅,并采用碳黑代替石墨,在渗硅反应中使气相硅能够完全渗透,与碳黑发生反应,生成的复合材料中没有残存的碳,且复合材料不易变形。
根据复合材料制备过程中硅的形态,可将制备方式分为真空液相渗透和气相渗透。真空液相渗透指使单质硅熔融渗透到预制体空隙中并与预制体中的碳源反应。气相渗透是利用熔融硅低压蒸发原理,渗透到预制体空隙并与预制体中的碳源反应。实验显示,气相渗透法的成品率远低于液相渗透法成品率。然而,液相渗透法制备的样品会被熔融硅包围,导致样品分离和加工困难,成为业界难以克服的难题。
发明内容
本发明的主要目的,在于提供一种制备Diamond/SiC复合材料的方法。本发明要解决的是真空渗透法制备Diamond/SiC复合材料时,熔融硅包裹样品导致样品分离和加工困难的问题。
本发明解决其技术问题的所采用的技术方案之一是:
一种制备Diamond/SiC复合材料的方法,包括如下步骤:
1)制备金刚石预制体:将金刚石、石墨、硅粉、粘结剂按质量比混合均匀并压制生坯,将生坯在1000-1200℃保护气氛下碳化得金刚石预制体;
2)制备Diamond/SiC复合材料:将金刚石预制体置于与硅粉的粉末混合物上,其中,氮化硅粉末占粉末混合物的40%-80%,于1500-1700℃真空炉中充分反应1-2h即得Diamond/SiC复合材料。
优选地,生坯中,金刚石、石墨、硅粉、粘结剂的质量比范围为20-80%的金刚石,5-25%的石墨,5-35%的硅粉,10-30%的粘结剂。
优选地,金刚石预制体与氮化硅粉末的质量比范围为(1:10)-(1:100)。例如,为1:20,1:30,1:40,1:50,1:60,1:70,1:80,1:90。
优选地,粘结剂为热固性树脂,所述的热固性树脂种类包括如下中的至少一种:酚醛树脂、环氧树脂、聚酰亚胺树脂、密胺树脂等。
本发明的又一技术方案为:
一种制备Diamond/SiC复合材料的方法,包括如下步骤:
(1)对渗硅材料预处理:将硅粉置于氮气保护氛围中加热至化学反应温度1100℃-1300℃,保温1h-2h,得到氮化预处理硅粉,其中部分硅粉已与氮气反应生成氮化硅;
(2)将氮化预处理硅粉用于制备Diamond/SiC复合材料:
a.制备金刚石预制体:将金刚石、石墨、硅粉、粘结剂按质量比混合均匀并压制生坯,将生坯在1000℃-1200℃保护气氛下碳化得金刚石预制体;
b.制备Diamond/SiC复合材料:将金刚石预制体置于氮化预处理硅粉上,于1500℃-1700℃真空炉中充分反应1-2h即得Diamond/SiC复合材料。
优选地,所述的“部分”是40%-80%的硅粉生成氮化硅。例如,50%、60%、70%。如果氮化硅比例超过80%会使埋粉中的样品周围单质硅源过少,导致渗硅失败;如果低于40%,埋粉中的硅单质过多,熔融硅会将细小的氮化硅及样品粘在一起,后处理更加困难。
优选地,生坯中,金刚石、石墨、硅粉、粘结剂的质量比范围为20-80%的金刚石,5-25%的石墨,5-35%的硅粉,10-30%的粘结剂。
优选地,金刚石预制体与氮化预处理硅粉的质量比范围为(1:10)-(1:100)。例如,为1:20,1:30,1:40,1:50,1:60,1:70,1:80,1:90。
优选地,粘结剂为热固性树脂,种类包括如下中的至少一种:酚醛树脂、环氧树脂、聚酰亚胺树脂、密胺树脂等热固型树脂。
与单纯使用硅粉做渗硅材料相比,本发明具有以下优势:
样品完整性:单质硅的熔点为1410℃,真空渗透法制备Diamond/SiC复合材料需加热到1500℃-1700℃,过量的硅粉熔融,将样品紧紧包裹,冷却后难以分离,给后续加工带来巨大的劳力和成本,成为业界难以克服的难题。本发明采用氮化处理后的硅粉或氮化硅粉与硅粉的混合材料作为渗硅材料,高温下,渗透的硅源首先来源于渗料中的游离硅,其次为氮化硅分解的硅,有效的避免了过量硅粉对样品的粘连,制品后续处理极其容易。
附图说明
下面结合附图和实施例对本发明作进一步说明。
图1硅单质作为渗硅材料制得的Diamond/SiC复合材料;
图2采用氮化预处理硅粉作为渗硅材料制得的Diamond/SiC复合材料。
具体实施方式
以下对比例和实施例中,粘结剂的具体种类是酚醛树脂。
对比例1
1.制备金刚石预制体:将金刚石40%、石墨20%、硅粉20%、粘结剂20%混合均匀并压制生坯,将生坯在1200℃保护气氛下碳化即得金刚石预制体;
2.制备Diamond/SiC复合材料:将金刚石预制体置于分析纯的硅粉上,在真空炉中于1600℃反应2h即得Diamond/SiC复合材料。金刚石预制体与分析纯的硅粉的质量比为1:50。
结果见图1,图1显示硅熔融后与样品紧密粘连在一起,难以分离。
实施例1
1.硅粉预处理:将分析纯的硅粉置于坩埚中,于氮气气氛下加热至1200℃反应1.5h,得到氮化预处理硅粉;
2.制备金刚石预制体:将金刚石40%、石墨20%、硅粉20%、粘结剂20%混合均匀并压制生坯,将生坯在1200℃保护气氛下碳化即得金刚石预制体;
3.制备Diamond/SiC复合材料:将金刚石预制体置于氮化预处理硅粉上,于1600℃真空炉中反应2h即得Diamond/SiC复合材料。金刚石预制体与氮化预处理硅粉的质量比为1:50。
结果见图2,图2显示样品表面无粘连。
实施例2
1.硅粉预处理:将分析纯的硅粉置于坩埚中,于氮气气氛下加热至1100℃反应2h,得到氮化预处理硅粉;
2.制备金刚石预制体:将金刚石70%、石墨5%、硅粉5%、粘结剂20%混合均匀并压制生坯,将生坯在1100℃保护气氛下碳化即得金刚石预制体;
3.制备Diamond/SiC复合材料:将金刚石预制体置于氮化预处理硅粉上,于1700℃真空炉中反应1h即得Diamond/SiC复合材料。金刚石预制体与氮化预处理硅粉的质量比为1:10。
实施例3
1.硅粉预处理:将分析纯的硅粉置于坩埚中,于氮气气氛下加热至1300℃反应1h,得到氮化预处理硅粉;
2.制备金刚石预制体:将金刚石25%、石墨25%、硅粉25%、粘结剂25%混合均匀并压制生坯,将生坯在(1000-1200)℃保护气氛下碳化即得金刚石预制体;
3.制备Diamond/SiC复合材料:将金刚石预制体置于氮化预处理硅粉上,于1500℃真空炉中反应2h即得Diamond/SiC复合材料。金刚石预制体与氮化预处理硅粉的质量比为1:100。
以上所述,仅为本发明较佳实施例而已,故不能依此限定本发明实施的范围,即依本发明专利范围及说明书内容所作的等效变化与修饰,皆应仍属本发明涵盖的范围内。

Claims (10)

1.一种制备Diamond/SiC复合材料的方法,包括如下步骤:
1)制备金刚石预制体:将金刚石、石墨、硅粉、粘结剂按质量比混合均匀并压制生坯,将生坯在1000-1200℃保护气氛下碳化得金刚石预制体;
2)制备Diamond/SiC复合材料:将金刚石预制体置于氮化硅粉末与硅粉的粉末混合物上,其中,氮化硅粉末占粉末混合物的40%-80%,于1500-1700℃真空炉中反应1-2h即得Diamond/SiC复合材料。
2.根据权利要求1所述的一种制备Diamond/SiC复合材料的方法,其特征在于:金刚石预制体与粉末的质量比范围为(1:10)-(1:100)。
3.根据权利要求1所述的一种制备Diamond/SiC复合材料的方法,其特征在于:金刚石、石墨、硅粉、粘结剂的质量比为20-80%的金刚石,5-25%的石墨,5-35%的硅粉,10-30%的粘结剂。
4.根据权利要求3所述的一种制备Diamond/SiC复合材料的方法,其特征在于:粘结剂为热固性树脂。
5.根据权利要求4所述的一种制备Diamond/SiC复合材料的方法,其特征在于:所述的热固性树脂种类包括如下中的至少一种:酚醛树脂、环氧树脂、聚酰亚胺树脂、密胺树脂。
6.一种制备Diamond/SiC复合材料的方法,包括如下步骤:
(1)材料预处理:将硅粉置于氮气保护氛围中加热至化学反应温度1100℃-1300℃,保温1h-2h,使部分硅粉生成氮化硅,得到氮化预处理硅粉;
(2)将氮化预处理硅粉用于制备金刚石-碳化硅复合材料:
a.制备金刚石预制体:将金刚石、石墨、硅粉、粘结剂按质量比混合均匀并压制生坯,将生坯在1000-1200℃保护气氛下碳化得金刚石预制体;
b.制备Diamond/SiC复合材料:将金刚石预制体置于步骤1)所得的氮化预处理硅粉,于1500-1700℃真空炉中充分反应1-2h即得Diamond/SiC复合材料。
7.根据权利要求6所述的一种制备Diamond/SiC复合材料的方法,其特征在于:步骤(1)所述的部分是40%-80%的硅粉生成氮化硅。
8.根据权利要求6所述的一种制备Diamond/SiC复合材料的方法,其特征在于:金刚石预制体与氮化预处理硅粉的质量比范围为(1:10)-(1:100)。
9.根据权利要求6所述的一种制备Diamond/SiC复合材料的方法,其特征在于:步骤a中金刚石、石墨、硅粉、粘结剂的质量比范围为20-80%的金刚石,5-25%的石墨,5-35%的硅粉,10-30%的粘结剂。
10.根据权利要求6或9所述的一种制备Diamond/SiC复合材料的方法,其特征在于:粘结剂为热固型树脂。
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