CN108002841B - 六方氮化硼-镱硅氧氮陶瓷基复合材料及其原位制备方法 - Google Patents
六方氮化硼-镱硅氧氮陶瓷基复合材料及其原位制备方法 Download PDFInfo
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- 239000011153 ceramic matrix composite Substances 0.000 title claims abstract description 26
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 title claims abstract description 22
- 229910052769 Ytterbium Inorganic materials 0.000 title claims abstract description 22
- 229910052796 boron Inorganic materials 0.000 title claims abstract description 22
- 239000000463 material Substances 0.000 title claims abstract description 22
- XUIMIQQOPSSXEZ-UHFFFAOYSA-N Silicon Chemical compound [Si] XUIMIQQOPSSXEZ-UHFFFAOYSA-N 0.000 title claims abstract description 20
- 229910052710 silicon Inorganic materials 0.000 title claims abstract description 20
- 239000010703 silicon Substances 0.000 title claims abstract description 20
- 238000011065 in-situ storage Methods 0.000 title claims abstract description 19
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000000843 powder Substances 0.000 claims abstract description 47
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims abstract description 31
- 238000005245 sintering Methods 0.000 claims abstract description 27
- 229910052581 Si3N4 Inorganic materials 0.000 claims abstract description 23
- 229910052582 BN Inorganic materials 0.000 claims abstract description 21
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims abstract description 18
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 15
- UZLYXNNZYFBAQO-UHFFFAOYSA-N oxygen(2-);ytterbium(3+) Chemical compound [O-2].[O-2].[O-2].[Yb+3].[Yb+3] UZLYXNNZYFBAQO-UHFFFAOYSA-N 0.000 claims abstract description 12
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- 229910052757 nitrogen Inorganic materials 0.000 claims description 6
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- 229910052786 argon Inorganic materials 0.000 claims description 3
- 230000001788 irregular Effects 0.000 claims description 2
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 2
- 238000000034 method Methods 0.000 abstract description 11
- BRWNQZHCDHXZSB-UHFFFAOYSA-N [Si][Yb] Chemical compound [Si][Yb] BRWNQZHCDHXZSB-UHFFFAOYSA-N 0.000 abstract description 6
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- 238000002844 melting Methods 0.000 description 1
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- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
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- FIXNOXLJNSSSLJ-UHFFFAOYSA-N ytterbium(III) oxide Inorganic materials O=[Yb]O[Yb]=O FIXNOXLJNSSSLJ-UHFFFAOYSA-N 0.000 description 1
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Abstract
本发明涉及陶瓷基复合材料领域，具体为一种六方氮化硼‑镱硅氧氮陶瓷基复合材料及其原位制备方法。采用六方氮化硼粉、氧化镱粉、氧化硅粉和氮化硅粉为原料，经物理机械方法混合8～24小时，烘干、过筛后装入内壁涂有BN的石墨模具中冷压成型，以10～20MPa的压强冷压1～10分钟，在通有保护气氛的热压炉内烧结，升温速率为5～20℃/分钟，烧结温度为1800～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。采用本发明方法能够获得致密的高氮化硼含量的六方氮化硼‑镱硅氧氮陶瓷基复合材料，六方氮化硼基体相的体积分数为50～90％，镱硅氧氮增强相的体积分数为10～50％，该复合材料同时具有良好的力学性能和可加工性能。
Description
技术领域
本发明涉及陶瓷基复合材料领域，具体为一种六方氮化硼-镱硅氧氮陶瓷基复合材料及其原位制备方法。
背景技术
在氮化硼的诸多晶型中，以六方氮化硼(h-BN)最为稳定，六方氮化硼具有较高的热导率、较低的热膨胀系数、良好的抗热震性能、低的介电常数和介电损耗、可靠的电绝缘性、优异的可加工性、对大多数金属不浸润、无毒等性能，在诸多领域得到了广泛应用。但由于其特殊的层状结构，烧结致密性较差，导致六方氮化硼陶瓷自身的强度和硬度偏低，限制了其作为结构材料更广泛的应用。
镱硅氧氮(Yb4Si2O7N2)具有1870℃的高熔点且在烧结过程中易于晶化，作为氮化硅陶瓷的晶间相，可以提高高温弹性模量、弯曲强度和断裂韧性等力学性质。文献1：Journal of the American Ceramic Society.1997，80(3)：750-756中Park等人研究了不同Yb2O3添加量对于Si3N4陶瓷的显微结构、化学成分以及力学性质的影响，发现当Si3N4的晶界相为Yb4Si2O7N2时，Si3N4陶瓷可以在1400℃高温仍然保持较高的弯曲强度(870MPa)。另外，文献2：Materials Science and Technology.2003，19：544-548中Guo等人通过研究不同服役温度和载荷下的弯曲蠕变行为，认为Yb4Si2O7N2的加入有利于Si3N4陶瓷获得良好的抗蠕变性能。而镱硅氧氮在六方氮化硼中的应用尚未见相关报道。
与之类似的Y4Si2O7N2-BN复合材料，专利1：公开号CN 102351541 A和专利2：公开号CN 102432298 A的结果表明，氮化硼的优选含量为10～30vol.％，此时所获得的复合材料具有较高的致密度(～95％)和良好的力学性能，但随着氮化硼含量的继续增加，复合材料的致密度明显降低，力学性能不佳。由于Y4Si2O7N2本身的硬度较高(10.3±0.3GPa)，少量氮化硼的引入对复合材料可加工性能的改善效果有限。
发明内容
本发明的目的在于提供一种力学性能优良且可加工性好的六方氮化硼-镱硅氧氮陶瓷基复合材料及其原位制备方法，此复合材料中六方氮化硼为主相(≥50vol.％)，镱硅氧氮为增强相。
为了实现本发明的上述目的，本发明采用如下的技术方案：
一种六方氮化硼-镱硅氧氮陶瓷基复合材料，该复合材料由六方氮化硼基体相和镱硅氧氮增强相组成，其中六方氮化硼基体相的体积分数为50～90％，镱硅氧氮增强相的体积分数为10～50％。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料，六方氮化硼基体相的体积分数优选为50～70％，镱硅氧氮增强相的体积分数优选为30～50％。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，原料粉为六方氮化硼粉、氧化镱粉、氧化硅粉及氮化硅粉；原料六方氮化硼粉、氧化镱粉、氧化硅粉、氮化硅粉的摩尔比为(22.36～51.49)：4：1：1；原料粉经物理机械方法混合8～24小时，烘干、过筛后装入内壁涂有BN的石墨模具中冷压成型，以10～20MPa的压强冷压1～10分钟，在通有保护气氛的热压炉内烧结，升温速率为5～20℃/分钟，烧结温度为1800～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，六方氮化硼粉粒度范围为0.5～10微米，氧化镱粉、氧化硅粉及氮化硅粉的粒度范围为200～400目。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，物理机械方法混合采用在氮化硅球磨罐中以无水乙醇为介质湿法球磨。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，保护气氛为氮气或氩气。
所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，烧结方式为热压烧结。
本发明具有以下优点及有益效果：
1.本发明使用的原料简单，以六方氮化硼(h-BN)粉、氧化镱(Yb2O3)粉、氧化硅(SiO2)粉和氮化硅(Si3N4)粉机械混合后的混合粉末作为原料。
2.工艺简单，成本低。本发明通过简单的一步原位热压合成的方法，在设定的工艺参数条件下获得了高氮化硼含量、无杂质且致密的BN-Yb4Si2O7N2陶瓷基复合材料。
3.优异的力学性能。本发明获得的BN-Yb4Si2O7N2陶瓷基复合材料致密度高(94.21～98.75％)，弯曲强度达到258～338MPa，压缩强度达到386～803MPa，断裂韧性为1.61～2.06MPa·m1/2。同时，该复合材料具有较低的硬度(0.76～2.69GPa)，保持了良好的可加工性，可用普通刀具进行高精度加工。
附图说明
图1为BN-(30～50)vol％.Yb4Si2O7N2复合材料的X射线衍射图谱。
图2为BN-40vol％.Yb4Si2O7N2复合材料的相分布形貌。
具体实施方式
在具体实施过程中，本发明采用原位热压反应烧结的方式制备六方氮化硼-镱硅氧氮陶瓷基复合材料，以六方氮化硼(h-BN)粉、氧化镱(Yb2O3)粉、氧化硅(SiO2)粉及氮化硅(Si3N4)粉为初始原料，利用原位热压反应烧结的方式获得六方氮化硼-镱硅氧氮陶瓷基复合材料，其中原位热压过程中发生的化学反应为：
4Yb2O3+SiO2+Si3N4→2Yb4Si2O7N2
原料粉经物理机械方法混合8～24小时，烘干、过筛后装入内壁涂有BN的石墨模具中冷压成型，以10～20MPa的压强冷压1～10分钟，在通有氮气或氩气的热压炉内烧结，升温速率为5～20℃/分钟，烧结温度为1800～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。所述的BN粉为六方晶型，粒度范围为0.5～10微米，Yb2O3、SiO2及Si3N4粉的粒度范围为200～400目。
下面，通过实施例和附图进一步详述本发明。
实施例1
将5微米六方氮化硼粉(h-BN)16.74克，400目氧化镱(Yb2O3)粉20.66克、400目氧化硅(SiO2)粉0.76克、400目氮化硅(Si3N4)粉1.84克装入氮化硅球磨罐中，以无水乙醇为介质球磨12小时，60℃烘干12小时，经过80目筛过筛，随后装入内壁涂有BN的石墨模具中冷压成型，施加的压强为10MPa，保压10分钟后再放入热压炉中热压烧结，升温速率为5℃/分钟，升温的同时逐渐将压力增加至20MPa，加热到2000℃保温3小时。整个烧结过程在氮气保护下进行，获得的块体样品经X射线衍射分析为h-BN和Yb4Si2O7N2，无杂质相生成，参见图1中的(a)曲线。本实施例中，h-BN和Yb4Si2O7N2两相的体积比为70：30。
本实施例中，测定材料的致密度为94.21％，三点弯曲强度为258±13MPa，压缩强度为386±36MPa，维氏硬度为0.76±0.01GPa，断裂韧性为1.61±0.09MPa·m1/2。
实施例2
将10微米六方氮化硼粉(h-BN)14.33克，300目氧化镱(Yb2O3)粉27.25克、300目氧化硅(SiO2)粉1.00克、300目氮化硅(Si3N4)粉2.43克装入氮化硅罐中，以无水乙醇为介质球磨8小时，60℃烘干12小时，经过80目筛过筛，随后装入内壁涂有BN的石墨模具中冷压成型，施加的压强为15MPa，保压5分钟后再放入热压炉中热压烧结，升温速率为10℃/分钟，升温的同时逐渐将压力增加至30MPa，加热到1900℃保温2小时。整个烧结过程在氮气保护下进行，获得的块体样品经X射线衍射分析为h-BN和Yb4Si2O7N2，无杂质相生成，参见图1中的(b)曲线。本实施例中，h-BN和Yb4Si2O7N2两相的体积比为60：40。
本实施例中，测定材料的致密度为96.28％，三点弯曲强度为335±2MPa，压缩强度为533±50MPa，维氏硬度为1.56±0.08GPa，断裂韧性为1.90±0.02MPa·m1/2。
相应的两相分布形貌见图2，从图2可以看出，白色的Yb4Si2O7N2增强相呈不规则岛状分布在h-BN基体中。
实施例3
将0.5微米六方氮化硼粉(h-BN)11.93克，200目氧化镱(Yb2O3)粉33.81克、200目氧化硅(SiO2)粉1.26克、200目氮化硅(Si3N4)粉3.01克装入氮化硅罐中，以无水乙醇为介质球磨24小时，60℃烘干12小时，经过80目筛过筛，随后装入内壁涂有BN的石墨模具中冷压成型，施加的压强为20MPa，保压1分钟后再放入热压炉中热压烧结，升温速率为20℃/分钟，升温的同时逐渐将压力增加至40MPa，加热到1800℃保温1小时。整个烧结过程在氮气保护下进行，获得的块体样品经X射线衍射分析为h-BN和Yb4Si2O7N2，无杂质相生成，参见图1中的(c)曲线。本实施例中，h-BN和Yb4Si2O7N2两相的体积比为50：50。
本实施例中，测定材料的致密度为98.75％，三点弯曲强度为338±10MPa，压缩强度为803±45MPa，维氏硬度为2.69±0.1GPa，断裂韧性为2.06±0.06MPa·m1/2。
实施例结果表明，本发明通过简单的一步原位反应热压法可以获得致密的不含杂质相的高氮化硼含量的六方氮化硼-镱硅氧氮陶瓷基复合材料，所获得的复合材料致密度高、力学性能优异，并且保持了良好的可加工性。
Claims (6)
1.一种六方氮化硼-镱硅氧氮陶瓷基复合材料，其特征在于：该复合材料由六方氮化硼基体相和镱硅氧氮增强相组成，其中六方氮化硼基体相的体积分数为60～90％，镱硅氧氮增强相的体积分数为10～40％，镱硅氧氮增强相呈不规则岛状分布在h-BN基体中。
2.按照权利要求1所述的六方氮化硼-镱硅氧氮陶瓷基复合材料，其特征在于：六方氮化硼基体相的体积分数优选为50～70％，镱硅氧氮增强相的体积分数优选为30～50％。
3.一种权利要求1或2所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，其特征在于：原料粉为六方氮化硼粉、氧化镱粉、氧化硅粉及氮化硅粉；原料六方氮化硼粉、氧化镱粉、氧化硅粉、氮化硅粉的摩尔比为(22.36～51.49)：4：1：1；原料粉经物理机械方法混合8～24小时，烘干、过筛后装入内壁涂有BN的石墨模具中冷压成型，以10～20MPa的压强冷压1～10分钟，在通有保护气氛的热压炉内烧结，升温速率为5～20℃/分钟，烧结温度为1800～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。
4.按照权利要求3所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，其特征在于：六方氮化硼粉粒度范围为0.5～10微米，氧化镱粉、氧化硅粉及氮化硅粉的粒度范围为200～400目。
5.按照权利要求3所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，其特征在于：物理机械方法混合采用在氮化硅球磨罐中以无水乙醇为介质湿法球磨。
6.按照权利要求3所述的六方氮化硼-镱硅氧氮陶瓷基复合材料的原位制备方法，其特征在于：保护气氛为氮气或氩气。
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