CN112110734B - 一种青色氮化硅陶瓷及其制备方法 - Google Patents

一种青色氮化硅陶瓷及其制备方法 Download PDF

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CN112110734B
CN112110734B CN201910544214.8A CN201910544214A CN112110734B CN 112110734 B CN112110734 B CN 112110734B CN 201910544214 A CN201910544214 A CN 201910544214A CN 112110734 B CN112110734 B CN 112110734B
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silicon nitride
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rare earth
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张景贤
刘宁
段于森
马瑞欣
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Shanghai Institute of Ceramics of CAS
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Abstract

本发明涉及一种青色氮化硅陶瓷及其制备方法,所述制备方法包括:以氮化硅粉体或/和硅粉体作为原料粉体,再加入烧结助剂和着色剂并混合,得到混合粉体,所述烧结助剂选自Al2O3、AlN、CaO、MgO、Y2O3、YAG、Ce2O3、Y2O3:Ce3+中至少一种,所述着色剂为稀土金属钕的氧化物;将所得混合粉体和粘结剂混合,再经压制成型,得到陶瓷坯体;将所得陶瓷坯体经真空排胶后,再进行烧结,得到所述青色氮化硅陶瓷。

Description

一种青色氮化硅陶瓷及其制备方法
技术领域
本发明涉及一种青色氮化硅陶瓷及其制备方法和应用,属于陶瓷制备方法技术领域。
背景技术
氮化硅陶瓷是一种传统的结构陶瓷材料。具有高强度、高韧性、抗冲击和抗热震、介电损耗小等优良的性能,被广泛的应用于各个领域,如刀具、模具、耐火材料、阀门等。近年来,随着人们对装饰品要求的不断提高,彩色氮化硅陶瓷可凭借它优异的机械性能,鲜艳高雅的色调,金属光泽及环境友好,无毒害无过敏等特点,普遍应用于高档手表的表壳,表链,高级纽扣,手机外壳等,特别值得关注的是氮化硅陶瓷将成为5G时代手机背板的主要候选材料。
因为价带和导带之间的间隙很大(3.5-5.5eV),氮化硅本身是无色的。但受添加剂,杂质和烧结条件的影响氮化硅陶瓷的颜色比较单调多为灰色,而且随着所形成的硅化物杂质的增加氮化硅陶瓷颜色变深。很明显单一的颜色难以满足人们对氮化硅陶瓷装饰材料日益增长的需求,因此,彩色氮化硅陶瓷的研究开发具有广阔的市场前景。青色象征着坚强,希望,古朴和庄重,传统的器物和服饰常常采用青色,同时青色作为一种中国特有的颜色,颇受人们的喜欢。
发明内容
针对上述问题,本发明的目的在于提供一种青色氮化硅陶瓷及其制备方法和应用,且所得青色氮化硅陶瓷色彩分布均匀且机械性能优良。
一方面,本发明提供了一种青色氮化硅陶瓷的制备方法,包括:
以氮化硅粉体或/和硅粉体作为原料粉体,再加入烧结助剂和着色剂并混合,得到混合粉体,所述烧结助剂选自Al2O3、AlN、CaO、MgO、Y2O3、YAG、Ce2O3、Y2O3:Ce3+中至少一种,所述着色剂为稀土金属钕的氧化物;
将所得混合粉体和粘结剂混合,再经压制成型,得到陶瓷坯体;
将所得陶瓷坯体经真空排胶后,再进行烧结,得到所述青色氮化硅陶瓷。
较佳地,所述原料粉体、烧结助剂和着色剂的质量比为(85~96.5):(5~0.5):(10~3),各质量百分比之和为100%,当原料粉体含有硅粉体时,所述硅粉的质量按照换算成氮化硅粉体后的质量计算。
较佳地,所述着色剂还包含稀土金属钪的氧化物、稀土金属钇的氧化物、稀土金属镧的氧化物、稀土金属铈的氧化物、稀土金属镨的氧化物、稀土金属钷的氧化物、稀土金属钐的氧化物、稀土金属铕的氧化物、稀土金属钆的氧化物、稀土金属铽的氧化物、稀土金属镝的氧化物、稀土金属钬的氧化物、稀土金属铒的氧化物、稀土金属铥的氧化物、稀土金属镱的氧化物、稀土金属镥的氧化物中的至少一种。其中氮化硅的显色原理主要是稀土金属离子进入氮化硅陶瓷的结晶相中与其他烧结助剂形成一种显色化合物结构而呈色。
较佳地,所述氮化硅粉体的粒径范围为0.5~20μm,优选为0.5~5μm;所述硅粉体的粒径范围为0.2~30μm,优选为0.5~10μm。
较佳地,所述烧结助剂为MgO和YAG。其中MgO占混合粉体总质量的1~2wt%,YAG占混合粉体总质量的2~8wt%。选用MgO-YAG的混合粉体作为烧结助剂,可以形成充足的液相显著降低氮化硅陶瓷的烧结温度,最大程度地抑制着色剂的分解;同时使着色剂充分溶解于液相中,并伴随液相流动,使氮化硅着色更加均匀。
较佳地,当原料粉体含有硅粉体时,将所得陶瓷坯体经真空排胶、氮化处理后,再进行烧结,得到所述青色氮化硅陶瓷,所述氮化处理的气氛为氮气、或氮气和氢气的混合气,温度为1300~1500℃,时间为6~10小时;优选地,所述氮气和氢气的体积比为(90~95):(10~5)。
较佳地,所述粘结剂为聚乙烯醇缩丁醛或/和聚甲基丙烯酸甲酯,加入量为混合粉体的总质量的0.8~1wt%。
较佳地,所述真空排胶的温度为600-900℃,时间为1-3小时;优选地,所述真空排胶的升温速率为3-10℃/分钟。
较佳地,所述烧结的方式为无压烧结、气压烧结、热压烧结或等静压烧结;优选地,所述烧结的气氛为氮气气氛、惰性气氛和还原气氛中的至少一种,温度为1600~1950℃,气压为不超过10MPa(例如,0.1~10MPa),时间1~24小时;更优选地,所述烧结的升温速率为3~10℃/分钟。
另一方面,本发明提供了一种如上述的制备方法制备的青色氮化硅陶瓷。
再一方面,本发明提供了一种如上述的青色氮化硅陶瓷制备在工艺装饰品、钟表、电子、刀具和手机外壳中的应用。
与现有技术相比,本发明具有至少如下有益效果:
(1)原料来源广,基体原料采用市面上销售的商业氮化硅粉和硅粉,无需担心原料的来源问题;
(2)成本较低,采用无压烧结工艺制备青色氮化硅陶瓷制品,较之热压烧结的方式大大的减少了成本;
(3)性能无损,着色剂在高温下仍能稳定存在,使得氮化硅的烧结能达到所需温度,保证了氮化硅原有的力学性能;
(4)制造简单,适合大批量的商业化生产。
附图说明
图1为实施例1中烧结加工后氮化硅断面的SEM图,从图1中可知样品烧结致密没有孔隙。长柱状β-Si3N4晶粒相互交错,紧密堆积而成,具有明显的晶粒拔出现象,同时存在大量β-Si3N4晶界玻璃相;
图2为实施例1中烧结加工后氮化硅表面的光谱反射率曲线,从图2中可知图中共有三个反射峰,分别处在490nm,550nm,620-700nm之间,三峰混合最终样品显示青色;
图3为实施例3中烧结加工后氮化硅断面的SEM图,从图3中可知试样具有与图1和图4相近的显微组织,主要为柱状晶和晶界玻璃相组成,长柱状晶粒相互间形成很好的机械接触和连接,增加了晶粒间的断裂应力,对提高烧结体强度有利;
图4为实施例4中烧结加工后氮化硅断面的SEM图,从图4中可知该试样具有与图1和图3相近的显微组织,主要为柱状晶和晶界玻璃相组成,长柱状晶粒相互间形成很好的机械接触和连接,同时具有明显的晶粒拔出现象。
具体实施方式
以下通过下述实施方式进一步说明本发明,应理解,下述实施方式仅用于说明本发明,而非限制本发明。
在本公开中,所得青色氮化硅陶瓷具有能够在1800℃高温下稳定存在的着色剂,且该着色剂在保证氮化硅烧结完全致密的前提下,起到对氮化硅着色成青色的作用。以下示例性地说明本发明提供的青色氮化硅陶瓷的制备方法。
使用氮化硅粉体和/或硅粉为基体原料,加入适当比例的烧结助剂,着色剂,混合后得到混合粉体。其中,着色剂可为稀土金属钕(Nd)的氧化物或稀土金属钕(Nd)的氧化物和其他稀土金属氧化物的组合,其中所述其他稀土金属选自由钪(Sc)、钇(Y)、镧(La)、铈(Ce)、镨(Pr)、钷(Pm)、钐(Sm)、铕(Eu)、钆(Gd)、铽(Tb)、镝(Dy)、钬(Ho)、铒(Er)、铥(Tm)、镱(Yb)、镥(Lu)组成的组,其中各种稀土金属的氧化物还可以以在烧结过程中能够形成氧化物的碳酸盐,硝酸盐,乙酸盐等形式加入。其中,烧结助剂包括:Al2O3、AlN、CaO、MgO、Y2O3、YAG、Ce2O3、、Y2O3:Ce3+中至少一种。所述基体原料、着色剂、烧结助剂体系的质量比为(85-96.5):(5~0.5):(10~3),其中所述硅源的质量换算成氮化硅的质量来计算。组成在上述范围内可以保证材料的力学性能和颜色。例如,混合方式可为球磨混合,所述行星球磨机的转速为250~400r/min,优选为380r/min。作为一个优选方案,其中所述着色剂为氧化钕,其作为着色剂的加入量占原料总量的1~5wt%。作为一个优选方案,烧结助剂选用MgO和YAG粉,其中氧化镁占原料总质量的1~2wt%,YAG粉占原料总质量的2~8wt%。
在可选的实施方式中,氮化硅粉体的粒径可为0.5~20μm,优选范围0.5~5μm,在这个范围内可以确保能够烧结致密。所述硅粉的粒径可为0.2~30μm,优选范围0.5~10μm,在这个范围内可以确保硅粉完全氮化,并经过烧结后得到致密的氮化硅陶瓷材料。作为本发明所述一种青色氮化硅陶瓷的制备方法的优选方案,其中所述氮化硅粉体的粒径可为1μm,纯度为99.9%;和/或所述硅粉的粒径为5μm。
将混合粉体中,加入粘结剂和溶剂混合均匀,再经烘干除去溶剂,获得陶瓷粉末。其中,粘结剂可为聚乙烯醇缩丁醛或/和聚甲基丙烯酸甲酯(优选聚乙烯醇缩丁醛PVB),针对加入量为混合粉体(氮化硅粉体和低温烧结助剂体系及着色剂)的总质量的0.8~1wt%,其中所述硅源的质量都换算成氮化硅的质量来计算。例如,混合方式可为球磨混合,所述行星球磨机的转速为250~400r/min,优选为380r/min。
在可选的实施方式中,将使用氮化硅粉体和/或硅粉为基体原料,加入适当比例的烧结助剂,着色剂,粘结剂和溶剂进行一步球磨至混合均匀,再经烘干除去溶剂,获得陶瓷粉末。
将陶瓷粉末压制成所需尺寸的陶瓷坯体。其中,可通过干压或和等静压成型工艺进行压制成型,干压成型的压力为10~30MPa,冷等静压成型的压力为150~200MPa。
将陶瓷坯体经过真空排胶工艺后,再经高温烧结成青色氮化硅陶瓷制品。其中,真空排胶的温度可为300~900℃(优选600-900℃),保温时间1~3小时。优选,真空排胶的升温速率为3~10℃/min。作为一个优选方案,其中所述真空排胶温度为900℃,真空排胶的升温速率为3℃/min,保温时间为1h。
本发明中,上述高温烧结可以无压烧结、气压烧结、热压烧结和高温等静压烧结等多种烧结方案。其中,青色氮化硅陶瓷的烧结温度在1600~1950℃,气压为0.1~10MPa,烧结时间为1h~12h。优选,烧结的升温速率可为3~10℃/min。烧结气氛可以为氮气或氩气等惰性气氛、或/和氢气等还原性气氛。作为一个优选方案,其中所述烧结条件为无压和气压烧结。所述氮化硅陶瓷的烧结温度在1750~1850℃,烧结的升温速率为5℃/min,气压为0.2~0.6MPa,烧结时间为2~3h。
当本发明的氮化硅陶瓷材料也可以使用硅粉作为原料经过氮化处理再进行烧结来制备。氮化处理包括:氮化温度为1300℃~1500℃,氮化时间为6h~10h。所述氮化使用的氮源为氮气、或者由体积比为(90~95):(10~5)的氮气和氢气组成的混合气体。作为一个优选方案,其中氮化处理的方法包括将硅粉氮化的步骤,氮化的氮化温度为1400℃,氮化时间为8h,氮化所使用的氮源为氮气。
下面进一步例举实施例以详细说明本发明。同样应理解,以下实施例只用于对本发明进行进一步说明,不能理解为对本发明保护范围的限制,本领域的技术人员根据本发明的上述内容作出的一些非本质的改进和调整均属于本发明的保护范围。下述示例具体的工艺参数等也仅是合适范围中的一个示例,即本领域技术人员可以通过本文的说明做合适的范围内选择,而并非要限定于下文示例的具体数值。
实施例1
将61.52g氮化硅粉体和3.23g氧化钕着色剂、0.7gPVB粘结剂以及5.26g烧结助剂氧化镁-YAG粉添加在140g无水乙醇中,氧化镁和YAG荧光粉的重量比例为1:6。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中,以5℃/min的升温速率达到1800℃,在氮气气氛中保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;
烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为97.71%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为50W/m·K。采用三点弯曲试验机检测材料的弯曲强度为860MPa,单边切口梁法检测材料的断裂韧性为11.52MPa·m1 /2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出青色(L=65.04±0.5,a=-2.91±0.06,b=0.21±0.3,孟塞尔5.8BG 6.3/0.4),经过抛光后的氮化硅显示出非常好的光泽。
实施例2
将60.99g氮化硅粉体和3.11g氧化钕着色剂、0.7gPVB粘结剂以及5.89g烧结助剂氧化镁-YAG粉添加在140g无水乙醇中,氧化镁和YAG粉的重量比例为1:8。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中,以5℃/min的升温速率达到1800℃,在氮气气氛中,保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;
烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为97.15%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为44W/m·K。采用三点弯曲试验机检测材料的弯曲强度为820MPa,单边切口梁法检测材料的断裂韧性为11.13MPa·m1 /2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出青色(L=64.54±0.8,a=-2.85±0.03,b=0.51±0.15,孟塞尔3.2BG 6.3/0.4),经过抛光后的氮化硅显示出非常好的光泽。
实施例3
将65.60g氮化硅粉体和3.38g氧化钕着色剂、0.7gPVB粘结剂以及1.01g烧结助剂氧化镁添加在140g无水乙醇中。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中,以5℃/min的升温速率达到1800℃,在氮气气氛中保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;
烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为98.12%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为60W/m·K。采用三点弯曲试验机检测材料的弯曲强度为900MPa,单边切口梁法检测材料的断裂韧性为10.51MPa·m1 /2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出黄绿色(L=84.41±0.5,a=-2.06±0.1,b=1.86±0.6,孟塞尔8.0GY 8.4/0.2),经过抛光后的氮化硅显示出非常好的光泽。
实施例4
将64.00g氮化硅粉体和3.41g氧化钕着色剂、0.7gPVB粘结剂以及6.02g烧结助剂氧化铝-氧化钇添加在140g无水乙醇中,氧化铝和氧化钇的重量比例为4:5。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中,以5℃/min的升温速率达到1800℃,在氮气气氛中保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;
烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为99.56%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为53W/m·K。采用三点弯曲试验机检测材料的弯曲强度为933MPa,单边切口梁法检测材料的断裂韧性为12.85MPa·m1 /2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出绿色(L=58.92±0.6,a=-1.46±0.05,b=0.72±0.06,孟塞尔3.9G 5.7/0.2),经过抛光后的氮化硅显示出非常好的光泽。
实施例5
将61.52g氮化硅粉体和3.23g氧化钕着色剂、0.7gPVB粘结剂以及5.26g烧结助剂氧化镁-YAG粉添加在140g无水乙醇中,氧化镁和YAG粉的重量比例为1:6。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中氮气气氛下,压力为0.6MPa,以5℃/min的升温速率达到1850℃,保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为98.34%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为55W/m·K。采用三点弯曲试验机检测材料的弯曲强度为950MPa,单边切口梁法检测材料的断裂韧性为12.12MPa·m1/2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出青色(L=65.42±0.8,a=-2.89±0.04,b=0.37±0.15,孟塞尔4.5BG 6.4/0.4),经过抛光后的氮化硅显示出非常好的光泽。
实施例6
将60.99g氮化硅粉体和3.11g氧化钕着色剂、0.7gPVB粘结剂以及5.89g烧结助剂氧化镁-YAG粉添加在140g无水乙醇中,氧化镁和YAG粉的重量比例为1:8。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中氮气气氛下,压力为0.6MPa,以5℃/min的升温速率达到1850℃,保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为97.53%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为52W/m·K。采用三点弯曲试验机检测材料的弯曲强度为886MPa,单边切口梁法检测材料的断裂韧性为11.84MPa·m1/2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出青色(L=63.24±0.9,a=-2.73±0.15,b=0.64±0.28,孟塞尔3.5BG 6.3/0.4),经过抛光后的氮化硅显示出非常好的光泽。
实施例7
将64.57g氮化硅粉体和0.7gPVB粘结剂以及5.43g烧结助剂氧化镁-YAG粉添加在140g无水乙醇中,氧化镁和YAG粉的重量比例为1:6。在行星球磨机上以380r/min的转速球磨3h后将悬浊液倒出,烘干除去酒精后,将陶瓷粉末研磨碎并且过100目筛网后,等静压制备成50×50×5mm的陶瓷坯体。真空下以3℃/min的速度升温到900℃保温1h完成脱粘,经过缓慢脱粘后在碳管炉中氮气气氛下,压力为0.6MPa,以5℃/min的升温速率达到1850℃,保温2h实现烧结。可以得到致密、色彩均匀的青色氮化硅陶瓷片;
烧结的青色氮化硅陶瓷片采用阿基米德排水方法测得氮化硅陶瓷的致密度为94.32%。采用激光热导仪方法或仪器测得氮化硅陶瓷的热导率为48W/m·K。采用三点弯曲试验机检测材料的弯曲强度为992MPa,单边切口梁法检测材料的断裂韧性为13.85MPa·m1 /2。采用爱色丽X-Rite Ci64分光测色仪(配备D65光源,积分球漫反射附件,测量孔径6mm)检测氮化硅的颜色,采用CIE-1976-LAB色度系统。色度检测结果显示,氮化硅呈现出黄绿色(L=68.22±0.05,a=-1.49±0.02,b=4.49±0.22,孟塞尔2.5GY 6.7/0.6),经过抛光后的氮化硅显示出非常好的光泽。
表1为本发明中各实施例所采用的原料及其用量:
Figure BDA0002103470180000081
Figure BDA0002103470180000091
表2为本发明中各实施例所采用的工艺条件:
实施例 升温速率(℃/min) 烧结温度(℃) 烧结时间(h) 烧结气氛 压力(MPa)
1 5 1800 2 常压 0.1
2 5 1800 2 常压 0.1
3 5 1800 2 常压 0.1
4 5 1800 2 常压 0.1
5 5 1850 2 氮气 0.6
6 5 1850 2 氮气 0.6
7 5 1850 2 氮气 0.6
表3为本发明中各实施例所制得材料的性能:
Figure BDA0002103470180000092
Figure BDA0002103470180000101
从上表可以看出,本发明制得的氮化硅陶瓷材料具有如下特性:密度为3.2~3.4g/cm3;韧性为12MPa·m1/2左右(单边切口梁法);强度为800MPa~1100MPa(三点弯曲抗弯强度测试);热导率为40W/m·K~60W/m·K(激光热导仪,购自耐驰公司);致密度为95.0%~99.5%(阿基米德排水法);青色氮化硅陶瓷lab值为L=64±0.5,a=-2.9±0.1,b=-0.5±0.3(X-Rite Ci64分光测色仪,购自爱色丽公司)。

Claims (13)

1.一种青色氮化硅陶瓷的制备方法,其特征在于,包括:
以氮化硅粉体或/和硅粉体作为原料粉体,再加入烧结助剂和着色剂并混合,得到混合粉体,所述烧结助剂为MgO和YAG,其中MgO占混合粉体总质量的1~2wt%,YAG占混合粉体总质量的2~8wt%;所述着色剂为稀土金属钕的氧化物;所述原料粉体、烧结助剂和着色剂的质量比为(85~96.5):(5~0.5):(10~3),各质量百分比之和为100%,当原料粉体含有硅粉体时,所述硅粉的质量按照换算成氮化硅粉体后的质量计算;
将所得混合粉体和粘结剂混合,再经压制成型,得到陶瓷坯体;
将所得陶瓷坯体经真空排胶后,再进行烧结,得到所述青色氮化硅陶瓷。
2.根据权利要求1所述的制备方法,其特征在于,所述着色剂还包含稀土金属钪的氧化物、稀土金属钇的氧化物、稀土金属镧的氧化物、稀土金属铈的氧化物、稀土金属镨的氧化物、稀土金属钷的氧化物、稀土金属钐的氧化物、稀土金属铕的氧化物、稀土金属钆的氧化物、稀土金属铽的氧化物、稀土金属镝的氧化物、稀土金属钬的氧化物、稀土金属铒的氧化物、稀土金属铥的氧化物、稀土金属镱的氧化物、稀土金属镥的氧化物中的至少一种。
3.根据权利要求1所述的制备方法,其特征在于,所述氮化硅粉体的粒径范围为0.5~20μm;所述硅粉体的粒径范围为0.2~30μm。
4.根据权利要求3所述的制备方法,其特征在于,所述氮化硅粉体的粒径范围为0.5~5μm;所述硅粉体的粒径范围为0.5~10μm。
5.根据权利要求1-4中任一项所述的制备方法,其特征在于,当原料粉体含有硅粉体时,将所得陶瓷坯体经真空排胶、氮化处理后,再进行烧结,得到所述青色氮化硅陶瓷,所述氮化处理的气氛为氮气、或氮气和氢气的混合气,温度为1300~1500℃,时间为6~10小时。
6.根据权利要求5所述的制备方法,其特征在于,所述氮气和氢气的体积比为(90~95):(10~5)。
7.根据权利要求1所述的制备方法,其特征在于,所述粘结剂为聚乙烯醇缩丁醛或/和聚甲基丙烯酸甲酯,加入量为混合粉体的总质量的0.8~1wt%。
8.根据权利要求1所述的制备方法,其特征在于,所述真空排胶的温度为300~900℃,时间为1~3小时。
9.根据权利要求8所述的制备方法,其特征在于,所述真空排胶的升温速率为3~10℃/分钟。
10.根据权利要求1所述的制备方法,其特征在于,所述烧结的方式为无压烧结、气压烧结、热压烧结或等静压烧结。
11.根据权利要求10所述的制备方法,其特征在于,所述烧结的气氛为氮气气氛、惰性气氛和还原气氛中的至少一种,温度为1600~1950℃,气压为不超过10MPa,时间1~24小时。
12.根据权利要求11所述的制备方法,其特征在于,所述烧结的升温速率为3~10℃/分钟。
13.一种根据权利要求1-12中任一项中所述的制备方法制备的青色氮化硅陶瓷。
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