CN108117395B - 一种六方氮化硼-玻璃复合材料及其制备方法 - Google Patents
一种六方氮化硼-玻璃复合材料及其制备方法 Download PDFInfo
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- 239000002131 composite material Substances 0.000 title claims abstract description 50
- 239000011521 glass Substances 0.000 title claims abstract description 48
- ZOXJGFHDIHLPTG-UHFFFAOYSA-N Boron Chemical compound [B] ZOXJGFHDIHLPTG-UHFFFAOYSA-N 0.000 title claims abstract description 26
- 229910052796 boron Inorganic materials 0.000 title claims abstract description 26
- 238000002360 preparation method Methods 0.000 title claims abstract description 14
- 239000000843 powder Substances 0.000 claims abstract description 47
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 claims abstract description 35
- 238000005245 sintering Methods 0.000 claims abstract description 30
- PZNSFCLAULLKQX-UHFFFAOYSA-N Boron nitride Chemical compound N#B PZNSFCLAULLKQX-UHFFFAOYSA-N 0.000 claims abstract description 26
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 claims abstract description 23
- CPLXHLVBOLITMK-UHFFFAOYSA-N magnesium oxide Inorganic materials [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 claims abstract description 19
- 239000005368 silicate glass Substances 0.000 claims abstract description 17
- 239000000395 magnesium oxide Substances 0.000 claims abstract description 16
- 238000000034 method Methods 0.000 claims abstract description 14
- AXZKOIWUVFPNLO-UHFFFAOYSA-N magnesium;oxygen(2-) Chemical compound [O-2].[Mg+2] AXZKOIWUVFPNLO-UHFFFAOYSA-N 0.000 claims abstract description 13
- 229910052769 Ytterbium Inorganic materials 0.000 claims abstract description 12
- 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
- NAWDYIZEMPQZHO-UHFFFAOYSA-N ytterbium Chemical compound [Yb] NAWDYIZEMPQZHO-UHFFFAOYSA-N 0.000 claims abstract description 12
- 239000004408 titanium dioxide Substances 0.000 claims abstract description 11
- 238000010438 heat treatment Methods 0.000 claims abstract description 10
- 238000007731 hot pressing Methods 0.000 claims abstract description 10
- 239000002994 raw material Substances 0.000 claims abstract description 10
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims abstract description 8
- 229910002804 graphite Inorganic materials 0.000 claims abstract description 8
- 239000010439 graphite Substances 0.000 claims abstract description 8
- TWNQGVIAIRXVLR-UHFFFAOYSA-N oxo(oxoalumanyloxy)alumane Chemical compound O=[Al]O[Al]=O TWNQGVIAIRXVLR-UHFFFAOYSA-N 0.000 claims abstract description 8
- 238000010297 mechanical methods and process Methods 0.000 claims abstract description 5
- 238000000465 moulding Methods 0.000 claims abstract description 5
- 230000001681 protective effect Effects 0.000 claims abstract description 5
- 239000000203 mixture Substances 0.000 claims abstract description 4
- 238000003825 pressing Methods 0.000 claims abstract 4
- 229910052582 BN Inorganic materials 0.000 claims description 19
- 239000000377 silicon dioxide Substances 0.000 claims description 15
- 239000000919 ceramic Substances 0.000 claims description 14
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical group [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 8
- 235000012239 silicon dioxide Nutrition 0.000 claims description 8
- 238000000498 ball milling Methods 0.000 claims description 7
- 239000011159 matrix material Substances 0.000 claims description 7
- 239000013078 crystal Substances 0.000 claims description 6
- 239000002245 particle Substances 0.000 claims description 6
- 229910052581 Si3N4 Inorganic materials 0.000 claims description 5
- HQVNEWCFYHHQES-UHFFFAOYSA-N silicon nitride Chemical compound N12[Si]34N5[Si]62N3[Si]51N64 HQVNEWCFYHHQES-UHFFFAOYSA-N 0.000 claims description 5
- PNEYBMLMFCGWSK-UHFFFAOYSA-N Alumina Chemical compound [O-2].[O-2].[O-2].[Al+3].[Al+3] PNEYBMLMFCGWSK-UHFFFAOYSA-N 0.000 claims description 4
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 4
- 229910052786 argon Inorganic materials 0.000 claims description 4
- 238000002156 mixing Methods 0.000 claims description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 2
- 229910052757 nitrogen Inorganic materials 0.000 claims description 2
- 239000000463 material Substances 0.000 abstract description 4
- 239000011153 ceramic matrix composite Substances 0.000 abstract description 2
- 239000012071 phase Substances 0.000 description 41
- 238000005452 bending Methods 0.000 description 10
- 229910052681 coesite Inorganic materials 0.000 description 7
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- 229910052682 stishovite Inorganic materials 0.000 description 7
- 229910052905 tridymite Inorganic materials 0.000 description 7
- BPQQTUXANYXVAA-UHFFFAOYSA-N Orthosilicate Chemical compound [O-][Si]([O-])([O-])[O-] BPQQTUXANYXVAA-UHFFFAOYSA-N 0.000 description 6
- 239000011777 magnesium Substances 0.000 description 6
- 239000010936 titanium Substances 0.000 description 6
- 229910052782 aluminium Inorganic materials 0.000 description 5
- 239000007791 liquid phase Substances 0.000 description 5
- 229910052719 titanium Inorganic materials 0.000 description 5
- 238000002441 X-ray diffraction Methods 0.000 description 4
- 229910052749 magnesium Inorganic materials 0.000 description 4
- OGIDPMRJRNCKJF-UHFFFAOYSA-N titanium oxide Inorganic materials [Ti]=O OGIDPMRJRNCKJF-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 3
- 230000009286 beneficial effect Effects 0.000 description 2
- 230000015572 biosynthetic process Effects 0.000 description 2
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- 238000004458 analytical method Methods 0.000 description 1
- 229910052593 corundum Inorganic materials 0.000 description 1
- 238000002425 crystallisation Methods 0.000 description 1
- 230000008025 crystallization Effects 0.000 description 1
- 238000001035 drying Methods 0.000 description 1
- 238000010292 electrical insulation Methods 0.000 description 1
- 239000005350 fused silica glass Substances 0.000 description 1
- 238000011065 in-situ storage Methods 0.000 description 1
- 230000008595 infiltration Effects 0.000 description 1
- 238000001764 infiltration Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 150000002739 metals Chemical class 0.000 description 1
- 231100000956 nontoxicity Toxicity 0.000 description 1
- 238000004321 preservation Methods 0.000 description 1
- 238000010298 pulverizing process Methods 0.000 description 1
- 239000010453 quartz Substances 0.000 description 1
- 238000001878 scanning electron micrograph Methods 0.000 description 1
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- 229910001845 yogo sapphire Inorganic materials 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‑玻璃复合材料及其制备方法。采用六方氮化硼粉、三氧化二镱粉和二氧化硅粉为主要原料，氧化镁、三氧化二铝和二氧化钛中的一种或两上以上氧化物为烧结助剂。原料粉经物理机械方法混合6～24小时，烘干、过筛后装入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5～15℃/分钟，烧结温度为1700～2000℃、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在短时间内制备得到致密度高、可加工性好、室温及高温强度优异的六方氮化硼‑玻璃复合材料，玻璃包含两相：二氧化硅玻璃和富镱硅酸盐玻璃。
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-玻璃复合材料及其制备方法。
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，它具有较高的热导率、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。
但由于特殊的层状结构，导致六方氮化硼陶瓷烧结较为困难，致使强度和硬度偏低，限制其作为结构材料更广泛的应用，而制备复合材料是改善其性能的一条有效途径。文献1：Journal of the American Ceramic Society.1999，82(9)：2563–2565中，RodneyW.Trice等人通过在h-BN中引入氧化物烧结助剂形成Y2Si2O7第二相明显提高了h-BN陶瓷的弯曲强度；文献2：Journal of the European Ceramic Society 2000，20：1923-1928中，Wen等人通过热压烧结途径成功制备了h-BN/熔融石英复合材料，充分发挥了h-BN和石英各自的性能优势最终得到综合性能良好的复合材料制品。文献3：Materials Science&Engineering A.2015，633：194–199中，Cai等人制备的h-BN/MAS复合材料具有较高的弯曲强度和断裂韧性。
镱硅酸盐以玻璃态的形式与六方氮化硼(h-BN)陶瓷复合，目前尚没有相关报道。
发明内容
本发明的目的在于提供一种制备六方氮化硼-玻璃复合材料的方法，通过添加氧化物烧结助剂在六方氮化硼陶瓷基体中形成SiO2玻璃相和富Yb硅酸盐玻璃相，制备得到一种致密度高，室温及高温性能良好的六方氮化硼陶瓷基复合材料，解决纯h-BN陶瓷烧结困难，力学性能低等问题。
本发明的技术方案是：
一种六方氮化硼-玻璃复合材料，由六方氮化硼相、二氧化硅玻璃相和富镱硅酸盐玻璃相组成，六方氮化硼相的体积百分数为50～95％，SiO2玻璃相和富镱硅酸盐玻璃相的总体积为5～50％，两玻璃相的体积百分数分别为2.5～47.5％和2.5～47.5％。
所述的六方氮化硼-玻璃复合材料，富镱硅酸盐玻璃相中含Mg、Al、Ti元素中的一种或两种以上；SiO2玻璃相中含有Mg、Al、Ti元素中的一种或两种以上。
所述的六方氮化硼-玻璃复合材料的制备方法，原料粉通过添加氧化物烧结助剂在六方氮化硼陶瓷基体中形成SiO2玻璃相和富镱硅酸盐玻璃相。
所述的六方氮化硼-玻璃复合材料的制备方法，原料粉为六方氮化硼粉、三氧化二镱粉和二氧化硅粉，氧化物烧结助剂为氧化镁、三氧化二铝和二氧化钛；所述的BN粉为六方晶型，粒度范围为0.5～10微米；Yb2O3和SiO2粉粒度范围为200～400目；MgO、Al2O3和TiO2粉的粒度分别为120～200目。
所述的六方氮化硼-玻璃复合材料的制备方法，原料粉经物理机械方法混合6～24小时，烘干、过筛后装入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5～15℃/分钟，烧结温度为1700～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。
所述的六方氮化硼-玻璃复合材料的制备方法，物理机械方法混合采用在氮化硅球磨罐中用无水乙醇作介质湿混球磨。
所述的六方氮化硼-玻璃复合材料的制备方法，保护气氛为氩气或氮气。
所述的六方氮化硼-玻璃复合材料的制备方法，烧结方式为热压烧结。
本发明的优点及有益效果是：
1.本发明使用的原料成分简单，主要为六方氮化硼(h-BN)粉、三氧化二镱(Yb2O3)粉和二氧化硅(SiO2)粉；氧化物烧结助剂为氧化镁(MgO)、三氧化二铝(Al2O3)和二氧化钛(TiO2)。
2.工艺简单，成本低。本发明通过简单的一步热压方法，能够实现原位合成制备六方氮化硼-玻璃复合材料。在升温过程中，达到某一温度后，三氧化二镱粉与二氧化硅粉发生化学反应生成镱硅酸盐。在氧化物烧结助剂的作用下，反应生成的镱硅酸盐和过量的二氧化硅在较低的温度下就能转变为液相，随着温度的升高液相量逐渐增加直至全部转变为液相，在随炉冷却的过程中由于冷却速度较快液相来不及结晶而被保留下来，最终以玻璃态的形式存在于复合材料中。另外，该复合材料具有较低的硬度，保持了良好的可加工性，可用普通刀具进行高精度加工。
3.优异的力学性能。本发明通过将玻璃态的物质引入到六方氮化硼陶瓷中，不仅得到了室温强度优异的复合材料，同时高温强度也得到了大幅度的提高。
附图说明
图1为六方氮化硼-玻璃复合材料的X射线衍射图谱。
图2为六方氮化硼-玻璃复合材料的扫描电镜照片。
具体实施方式
在具体实施过程中，本发明六方氮化硼-玻璃复合材料中的相组成为h-BN基体相、SiO2玻璃相及富Yb硅酸盐玻璃相，其中h-BN基体相的体积百分数为50～95％(优选为70％)，SiO2玻璃相和富Yb硅酸盐玻璃相的总体积为5～50％(优选为30％)，两玻璃相的体积百分数分别为2.5～47.5％(优选为25％)和2.5～47.5％(优选为5％)。在富Yb硅酸盐玻璃相中，Yb占55～80wt％，硅酸盐占20～45wt％。
另外，富镱硅酸盐玻璃相中含Mg、Al、Ti元素中的一种或两种以上，Mg、Al、Ti元素的含量均为0.2～2wt％；SiO2玻璃相中含有Mg、Al、Ti元素中的一种或两种以上，Mg、Al、Ti元素的含量均为0.1～1wt％。
本发明六方氮化硼-玻璃复合材料的技术指标如下：复合材料的密度为2.23～3.68/cm3，杨氏模量为76～105GPa，剪切模量为35～45GPa，维氏硬度为1.6～3.1GPa，压缩强度为425～625MPa，室温弯曲强度为191～285MPa，800℃高温弯曲强度最优为496MPa。
下面通过实施例详述本发明。
实施例1
将10微米六方氮化硼(h-BN)粉11.94克、300目的三氧化二镱(Yb2O3)粉19.74克、300目的二氧化硅(SiO2)粉8.32克、120目的氧化镁(MgO)粉0.12克、120目的三氧化二铝(Al2O3)粉0.12克和120目的二氧化钛(TiO2)粉0.12克装入氮化硅球磨罐中球磨24小时，60℃烘干12小时，经过80目筛过筛，随后装入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15℃/分钟，升温至600℃开始加压，以2kN/min的速率加压至20MPa，加热到1700℃保温1小时，整个烧结过程在氩气保护下进行。所获得的复合材料经X射线衍射分析包括BN结晶相和玻璃相，其中BN结晶相的体积百分数为50％，SiO2玻璃相体积百分数为10％，富Yb硅酸盐玻璃相体积百分数为40％。测得复合材料的密度为3.68g/cm3，杨氏模量为105GPa，剪切模量为45GPa，维氏硬度为3.1GPa，压缩强度为625MPa，室温弯曲强度为273MPa。
实施例2
将5微米六方氮化硼(h-BN)粉18.70克，400目的三氧化二镱(Yb2O3)粉2.87克、400目的二氧化硅(SiO2)粉8.43克、120目的氧化镁(MgO)粉0.09克、120目的三氧化二铝(Al2O3)粉0.09克和120目的二氧化钛(TiO2)粉0.09克装入氮化硅罐中球磨6小时，60℃烘干12小时，经过80目筛过筛，随后装入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，升温至600℃开始加压，以2kN/min的速率加压至30MPa，加热到1860℃保温1.5小时。整个烧结过程在氩气保护下进行，获得的复合材料经X射线衍射和能谱综合分析为h-BN结晶相、SiO2玻璃相和富Yb的硅酸盐玻璃相，其中h-BN结晶相的体积百分数为70％，SiO2玻璃相体积百分数为25％，富Yb硅酸盐玻璃相体积百分数为5％，如图1所示。制备所得到的复合材料中浅灰色的SiO2玻璃相和白色的富Yb硅酸盐玻璃相弥散均匀的分布在深色的h-BN基体中，如图2所示。在本实施例中该复合材料的密度为2.40g/cm3，杨氏模量为81GPa，剪切模量为37GPa，维氏硬度为2.4GPa，压缩强度为561MPa。特别地，该复合材料的室温弯曲强度为285MPa，而在800℃的高温弯曲强度达到了496MPa，提高幅度为74％。
实施例3
将0.5微米六方氮化硼(h-BN)粉22.80克，200目的三氧化二镱(Yb2O3)粉1.24克、200目的二氧化硅(SiO2)粉0.96克、200目的氧化镁(MgO)粉0.10克、200目的三氧化二铝(Al2O3)粉0.10克和200目的二氧化钛(TiO2)粉0.10克装入氮化硅罐中球磨12小时，60℃烘干12小时，经过80目筛过筛，随后装入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5℃/分钟，升温至600℃开始加压，以0.5kN/min的速率加压至40MPa，加热到2000℃保温3小时，整个烧结过程在氩气保护下进行。获得的复合材料经X射线衍射和能谱综合分析由h-BN结晶相、SiO2玻璃相和富Yb的硅酸盐玻璃相组成，其中h-BN结晶相的体积百分数为95％，SiO2玻璃相体积百分数为2.5％，富Yb硅酸盐玻璃相体积百分数为2.5％。测得复合材料的密度为2.23g/cm3，杨氏模量为76GPa，剪切模量为35GPa，维氏硬度为1.6GPa，压缩强度为495MPa，室温弯曲强度为191MPa。
比较例1
文献1：Journal of the American Ceramic Society.1999，82(9)：2563–2565中Rodney W.Trice等人的研究结果表明，引入22wt.％的氧化物烧结助剂得到的h-BN/Y2Si2O7复合材料的室温弯曲强度最高达到117MPa。而实施例3所获得的复合材料的室温弯曲强度为191MPa，较文献1中的强度有明显提高。
比较例2
文献4：Ceramics International.2015，9(41)：10891-10896中Zhang等人获得的h-BN/30vol％Y2SiO5复合材料室温和800℃时的弯曲强度分别为119MPa和150MPa，而实施例2中得到的h-BN/玻璃复合材料的室温和800℃高温弯曲强度分别达到285MPa和496MPa。这一结果表明：h-BN/玻璃复合材料具有更加优异的高温力学性能。
由实施例1、2、3及比较例1和2，氧化物烧结助剂的引入有利于玻璃相的形成，而玻璃与基体的复合明显提高了六方氮化硼基复合材料的力学性能。采用本发明方法能够在短时间内制备得到致密度高、可加工性好、室温及高温强度优异的六方氮化硼-玻璃复合材料。
Claims (5)
1.一种六方氮化硼-玻璃复合材料的制备方法，其特征在于：六方氮化硼-玻璃复合材料由六方氮化硼相、二氧化硅玻璃相和富镱硅酸盐玻璃相组成，六方氮化硼相的体积百分数为50～95%，SiO2玻璃相和富镱硅酸盐玻璃相的总体积为5～50%，两玻璃相的体积百分数分别为2.5～47.5%和2.5～47.5%；
原料粉通过添加氧化物烧结助剂在六方氮化硼陶瓷基体中形成二氧化硅玻璃相和富镱硅酸盐玻璃相；
原料粉为六方氮化硼粉、三氧化二镱粉和二氧化硅粉，氧化物烧结助剂为氧化镁、三氧化二铝和二氧化钛；六方氮化硼粉为六方晶型，粒度范围为0.5～10微米；三氧化二镱粉和二氧化硅粉的粒度范围分别为200～400目；氧化镁、三氧化二铝和二氧化钛的粒度范围分别为120～200目；
原料粉和氧化物烧结助剂的含量为以下三组之一：
（1）六方氮化硼粉11.94克、三氧化二镱粉19.74克、二氧化硅粉8.32克、氧化镁粉0.12克、三氧化二铝粉0.12克和二氧化钛粉0.12克；
（2）六方氮化硼粉18.70克，三氧化二镱粉2.87克、二氧化硅粉8.43克、氧化镁粉0.09克、三氧化二铝粉0.09克和二氧化钛粉0.09克；
（3）六方氮化硼粉22.80克，三氧化二镱粉1.24克、二氧化硅粉0.96克、氧化镁粉0.10克、三氧化二铝粉0.10克和二氧化钛粉0.10克。
2.按照权利要求1所述的六方氮化硼-玻璃复合材料的制备方法，其特征在于：原料粉经物理机械方法混合6～24小时，烘干、过筛后装入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5～15℃/分钟，烧结温度为1700～2000℃、烧结时间为1～3小时、烧结压强为20～40MPa。
3.按照权利要求2所述的六方氮化硼-玻璃复合材料的制备方法，其特征在于：物理机械方法混合采用在氮化硅球磨罐中用无水乙醇作介质湿混球磨。
4.按照权利要求2所述的六方氮化硼-玻璃复合材料的制备方法，其特征在于：保护气氛为氩气或氮气。
5.按照权利要求2所述的六方氮化硼-玻璃复合材料的制备方法，其特征在于：烧结方式为热压烧结。
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