CN118125831A - 一种高介电性能氮化硅复合陶瓷及其制备方法 - Google Patents

一种高介电性能氮化硅复合陶瓷及其制备方法 Download PDF

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CN118125831A
CN118125831A CN202410250050.9A CN202410250050A CN118125831A CN 118125831 A CN118125831 A CN 118125831A CN 202410250050 A CN202410250050 A CN 202410250050A CN 118125831 A CN118125831 A CN 118125831A
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silicon nitride
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high dielectric
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韩钰
张一铭
侯东
聂京凯
卢理成
祝志祥
刘辉
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State Grid Smart Grid Research Institute Co ltd
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Abstract

一种高介电性能氮化硅复合陶瓷及其制备方法，属于电工绝缘陶瓷技术领域，克服现有技术中绝缘支柱用材料介电性能差的缺陷。本发明高介电性能氮化硅复合陶瓷的制备方法包括以下步骤：步骤1、将氮化硅粉末、烧结助剂、分散剂、粘结剂和水混合制备浆料；所述烧结助剂包括Y2O3、Al2O3和Bi2O3，Y2O3：Al2O3：Bi2O3：氮化硅粉末的质量比为(0.01‑0.15)：(0.01‑0.13)：(0.01‑0.08)：1；步骤2、制备造粒粉；步骤3、压制成型；步骤4、排胶；步骤5、在负压下进行第一步烧结，随后在氮气压力下进行第二步烧结。本发明氮化硅复合陶瓷具有优异的介电性能。

Description

一种高介电性能氮化硅复合陶瓷及其制备方法
技术领域
本发明属于电工绝缘陶瓷技术领域，具体涉及一种高介电性能氮化硅复合陶瓷及其制备方法。
背景技术
氮化硅陶瓷具有高强度、高韧性、高热导率，以及优异的抗氧化、抗蠕变、高电阻率等性能，是应用最广泛的结构陶瓷之一。随着粉末冶金技术的不断发展，作为综合性能最为优良的结构-功能一体化的陶瓷材料，氮化硅受到越来越多的关注。氮化硅陶瓷兼具高强度、高电阻率、高介电常数和低介电损耗的特性，使其在特高输电领域具有潜在的应用价值。
直流穿墙套管是特高压直流输电系统的重要设备。支柱绝缘子、盆式绝缘子是穿墙套管气体内绝缘核心部件，起到支撑导杆的关键作用。现役的特高压气体内绝缘支柱常用氧化铝与环氧树脂的复合材料，在高电压等级下易发生闪络事故，对线路安全造成极大隐患，因此对材料的介电性能提出更高的要求。
发明内容
因此，本发明要解决的技术问题在于克服现有技术中绝缘支柱用材料介电性能差的缺陷，从而提供一种高介电性能氮化硅复合陶瓷及其制备方法。
为此，本发明提供了以下技术方案。
第一方面，本发明提供了一种高介电性能氮化硅复合陶瓷的制备方法，包括以下步骤：
步骤1、将氮化硅粉末、烧结助剂、分散剂、粘结剂和水混合制备浆料；
所述烧结助剂包括Y2O3、Al2O3和Bi2O3，Y2O3：Al2O3：Bi2O3：氮化硅粉末的质量比为(0.01-0.15)：(0.01-0.13)：(0.01-0.08)：1；
步骤2、将所述浆料采用喷雾造粒制备造粒粉；
步骤3、将所述造粒粉压制成型，制得陶瓷生坯；
步骤4、将所述陶瓷生坯进行排胶；
步骤5、将排胶后的陶瓷生坯在负压下进行第一步烧结，随后在氮气压力下进行第二步烧结。
进一步的，步骤5包括：
先在70-95KPa压力下升温至1100～1500℃，保温1～5小时；随后充入氮气，加压到0.1～5MPa，升温至1750～1900℃，保温1～5小时。
进一步的，所述步骤1满足以下条件中的至少一项：
(1)所述氮化硅粉末为氮化硅微米粉；优选的，所述氮化硅微米粉的平均粒径为0.4-1.0微米；
(2)所述氮化硅粉末为α-Si3N4；
(3)所述分散剂包括聚丙烯酰胺、羟甲基纤维素钠或Darvan C-N的一种或多种；
(4)所述粘结剂包括聚乙烯醇、聚丙烯酸或聚乙二醇中的一种或多种；
(5)所述分散剂与氮化硅粉末的质量比为(0.01-0.25)：1；
(6)所述粘结剂与氮化硅粉末的质量比为(0.03-0.26)：1；
(7)所述浆料固含量为43～55wt.％。
进一步的，所述步骤1包括：
将氮化硅粉末、烧结助剂、分散剂和水在砂磨机中进行预混合；
然后将预混合后的物质转移到搅拌桶中，加入粘结剂，并继续混合；
优选的，在砂磨机中预混1～10小时；
优选的，在搅拌桶中搅拌0.5～6小时。
进一步的，喷雾造粒后还包括干燥、过筛的步骤。
进一步的，所述干燥条件为在110～150℃下干燥1～20小时；
和/或
所述过筛为过60～120目筛网，取筛下物作为造粒粉。
进一步的，所述步骤3中，压制成型的工艺包括干压成型和冷等静压成型中的至少一种。
进一步的，干压成型的压力为70～120MPa，保压5～10分钟；
和/或
冷等静压的压力为100～300MPa，保压5～10分钟。
进一步的，步骤4满足以下条件中的至少一项：
(1)将所述陶瓷生坯在流动的空气中进行排胶；优选的，空气流量为0.5-4L/min；
(2)所述排胶包括：1～5小时从室温升温到300～450℃，保温1～6小时，再1～5小时升温致550～650℃，保温0.5～5小时，随后再1～3小时升温至750～850℃。
第二方面，本发明提供了一种根据所述制备方法制得的高介电性能氮化硅复合陶瓷。
氮气压力下指的是氮气环境的正压力下。
本发明技术方案，具有如下优点：
1.本发明高介电性能氮化硅复合陶瓷的制备方法包括以下步骤：步骤1、将氮化硅粉末、烧结助剂、分散剂、粘结剂和水混合制备浆料；所述烧结助剂包括Y2O3、Al2O3和Bi2O3，Y2O3：Al2O3：Bi2O3：氮化硅粉末的质量比为(0.01-0.15)：(0.01-0.13)：(0.01-0.08)：1；步骤2、将所述浆料采用喷雾造粒制备造粒粉；步骤3、将所述造粒粉压制成型，制得陶瓷生坯；步骤4、将所述陶瓷生坯进行排胶；步骤5、将排胶后的陶瓷生坯在负压下进行第一步烧结，随后在氮气压力下进行第二步烧结。
本发明采用Y-Al-Bi三元复合烧结助剂，通过Y2O3烧结助剂降低电导势垒，提升温度稳定性；Bi2O3烧结助剂引入界面能级，增加入陷电荷，此外低熔点氧化物Bi2O3和Al2O3还可降低烧结温度。
采用微负压与气压相结合的烧结工艺，先在低温下通过微负压烧结减少内部缺陷，随后在氮气压力下升温提高至密度，从而提高介性能。
该方法制备工艺简单，可控性强，制备的氮化硅复合材料致密度高，具有优异的介电性能。
本发明制得的氮化硅复合陶瓷致密度大于98％，在50Hz下介电常数在7.6-8.5之间(20℃)，介电损耗小于0.01(20℃)，具有优异的介电性能。
附图说明
为了更清楚地说明本发明具体实施方式或现有技术中的技术方案，下面将对具体实施方式或现有技术描述中所需要使用的附图作简单地介绍，显而易见地，下面描述中的附图是本发明的一些实施方式，对于本领域普通技术人员来讲，在不付出创造性劳动的前提下，还可以根据这些附图获得其他的附图。
图1为实施例1制备得到的高介电性能氮化硅复合陶瓷的SEM电镜图。
具体实施方式
提供下述实施例是为了更好地进一步理解本发明，并不局限于所述最佳实施方式，不对本发明的内容和保护范围构成限制，任何人在本发明的启示下或是将本发明与其他现有技术的特征进行组合而得出的任何与本发明相同或相近似的产品，均落在本发明的保护范围之内。
实施例中未注明具体实验步骤或条件者，按照本领域内的文献所描述的常规实验步骤的操作或条件即可进行。所用试剂或仪器未注明生产厂商者，均为可以通过市购获得的常规试剂产品。
实施例1
本实施例提供一种高介电性能氮化硅复合陶瓷的制备方法，包括以下步骤：
(1)取10kg平均粒径为0.9um的α-Si3N4粉末，烧结助剂氧化钇0.5kg、氧化铝0.3kg、氧化铋0.15kg，以及分散剂聚丙烯酰胺(平均Mn150000)0.15kg放入砂磨机中，以去离子水为球磨介质，预混2小时。随后把混合后的浆料转移到搅拌桶中，加入粘结剂聚乙二醇(平均Mn 8000)0.5kg，固含量调整为53wt.％，继续搅拌1小时。
(2)采用喷雾干燥工艺对浆料进行造粒处理，随后在130℃下干燥8小时，干燥后过60目筛网，取筛下物作为造粒粉。
(3)将造粒粉在100MPa压力下干压成型10min，并在250MPa的压力下进一步冷等静压处理10min，制得陶瓷生坯。
(4)将陶瓷生坯在流动的空气下进行排胶：气流量为3L/min，3小时从室温升温到400℃，保温5小时，再3小时升温致600℃，保温3小时，再1小时升温至800℃不保温。
(5)排胶后的陶瓷生坯在气压烧结炉中进行烧结：先在90KPa压力下，升温至1300℃，保温4小时。随后充入氮气，加压到1MPa，升温至1850℃，保温5小时。
图1为实施例1制得的氮化硅复合陶的SEM电镜图，由图1可知本发明制得的氮化硅复合陶瓷的微观形貌均匀，致密度高。
实施例2
本实施例提供一种高介电性能氮化硅复合陶瓷的制备方法，包括以下步骤：
(1)取10kg平均粒径为0.7um的α-Si3N4粉末，烧结助剂氧化钇0.53kg、氧化铝0.25kg、氧化铋0.12kg，以及分散剂聚丙烯酰胺(平均Mn150000)0.15kg放入砂磨机中，以去离子水为球磨介质，预混2小时。随后把混合后的浆料转移到搅拌桶中，加入粘结剂聚乙二醇(平均Mn 8000)0.55kg，固含量调整为55wt.％，继续搅拌1小时。
(2)采用喷雾干燥工艺对浆料进行造粒处理，随后在130℃下干燥8小时，干燥后过60目筛网，取筛下物作为造粒粉。
(3)将造粒粉在100MPa压力下干压成型8min，并在250MPa的压力下进一步冷等静压处理8min，制得陶瓷生坯。
(4)将陶瓷生坯在流动的空气下进行排胶：气流量为2L/min，3小时从室温升温到400℃，保温5小时，再3小时升温致600℃，保温4小时，再1小时升温至800℃不保温。
(5)排胶后的生坯在气压烧结炉中进行烧结：先在85KPa压力下，升温至1400℃，保温4小时。随后充入氮气，加压到1MPa，升温至1850℃，保温3小时。
实施例3
本实施例提供一种高介电性能氮化硅复合陶瓷的制备方法，包括以下步骤：
(1)取10kg平均粒径为0.4um的α-Si3N4粉末，烧结助剂氧化钇0.5kg、氧化铝0.35kg、氧化铋0.15kg，以及分散剂聚丙烯酰胺(平均Mn150000)0.15kg放入砂磨机中，以去离子水为球磨介质，预混2小时。随后把混合后的浆料转移到搅拌桶中，加入粘结剂聚乙二醇(平均Mn 8000)0.5kg，固含量调整为50wt.％，继续搅拌1小时。
(2)采用喷雾干燥工艺对浆料进行造粒处理，随后在130℃下干燥8小时，干燥后过60目筛网，取筛下物作为造粒粉。
(3)将造粒粉在100MPa压力下干压成型10min，并在250MPa的压力下进一步冷等静压处理10min。
(4)将陶瓷生坯在流动的空气下进行排胶：气流量为2.5L/min，3小时从室温升温到400℃，保温5小时，再3小时升温致600℃，保温2小时，再1小时升温至800℃不保温。
(5)排胶后的生坯在气压烧结炉中进行烧结：先在90KPa压力下，升温至1400℃，保温4小时。随后充入氮气，加压到1MPa，升温至1850℃，保温5小时。
对比例1
本对比例与实施例1基本相同，不同之处在于未采用氧化铋烧结助剂，所选的烧结助剂为氧化钇0.5kg、氧化铝0.3kg。
对比例2
本对比例与实施例1基本相同，不同之处在于烧结助剂氧化铋用量为0.9kg。
对比例3
本对比例与实施例1基本相同，不同之处在于未采用微负压与气压相结合的两步烧结工艺，仅采用气压烧结：充入氮气，加压到1MPa，升温至1300℃，保温4小时，随后升温至1850℃，保温5小时。
试验例
将实施例1-3和对比例1-3制得的氮化硅复合陶瓷分别双面减薄致5mm，经双面抛光后进行介电性能测试，测试依据GB/T 5594.4-2015，测试结果见表1。
表1氮化硅复合陶瓷性能
由表1可知，本发明氮化硅复合陶瓷相较于对比例的致密度和介电常数均有提高，介电损耗也显著降低。
显然，上述实施例仅仅是为清楚地说明所作的举例，而并非对实施方式的限定。对于所属领域的普通技术人员来说，在上述说明的基础上还可以做出其它不同形式的变化或变动。这里无需也无法对所有的实施方式予以穷举。而由此所引申出的显而易见的变化或变动仍处于本发明创造的保护范围之中。

Claims (10)

1.一种高介电性能氮化硅复合陶瓷的制备方法，其特征在于，包括以下步骤：
步骤1、将氮化硅粉末、烧结助剂、分散剂、粘结剂和水混合制备浆料；
所述烧结助剂包括Y2O3、Al2O3和Bi2O3，Y2O3：Al2O3：Bi2O3：氮化硅粉末的质量比为(0.01-0.15)：(0.01-0.13)：(0.01-0.08)：1；
步骤2、将所述浆料采用喷雾造粒制备造粒粉；
步骤3、将所述造粒粉压制成型，制得陶瓷生坯；
步骤4、将所述陶瓷生坯进行排胶；
步骤5、将排胶后的陶瓷生坯在负压下进行第一步烧结，随后在氮气压力下进行第二步烧结。
2.根据权利要求1所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，步骤5包括：
先在70-95KPa压力下升温至1100～1500℃，保温1～5小时；随后充入氮气，加压到0.1～5MPa，升温至1750～1900℃，保温1～5小时。
3.根据权利要求1或2所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，所述步骤1满足以下条件中的至少一项：
(1)所述氮化硅粉末为氮化硅微米粉；优选的，所述氮化硅微米粉的平均粒径为0.4-1.0微米；
(2)所述氮化硅粉末为α-Si3N4；
(3)所述分散剂包括聚丙烯酰胺、羟甲基纤维素钠或Darvan C-N的一种或多种；
(4)所述粘结剂包括聚乙烯醇、聚丙烯酸或聚乙二醇中的一种或多种；
(5)所述分散剂与氮化硅粉末的质量比为(0.01-0.25)：1；
(6)所述粘结剂与氮化硅粉末的质量比为(0.03-0.26)：1；
(7)所述浆料固含量为43～55wt.％。
4.根据权利要求1或2所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，所述步骤1包括：
将氮化硅粉末、烧结助剂、分散剂和水在砂磨机中进行预混合；
然后将预混合后的物质转移到搅拌桶中，加入粘结剂，并继续混合；
优选的，在砂磨机中预混1～10小时；
优选的，在搅拌桶中搅拌0.5～6小时。
5.根据权利要求1或2所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，喷雾造粒后还包括干燥、过筛的步骤。
6.根据权利要求5所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，所述干燥条件为在110～150℃下干燥1～20小时；
和/或
所述过筛为过60～120目筛网，取筛下物作为造粒粉。
7.根据权利要求1或2所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，所述步骤3中，压制成型的工艺包括干压成型和冷等静压成型中的至少一种。
8.根据权利要求7所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，干压成型的压力为70～120MPa，保压5～10分钟；
和/或
冷等静压的压力为100～300MPa，保压5～10分钟。
9.根据权利要求1或2所述的高介电性能氮化硅复合陶瓷的制备方法，其特征在于，步骤4满足以下条件中的至少一项：
(1)将所述陶瓷生坯在流动的空气中进行排胶；优选的，空气流量为0.5-4L/min；
(2)所述排胶包括：1～5小时从室温升温到300～450℃，保温1～6小时，再1～5小时升温致550～650℃，保温0.5～5小时，随后再1～3小时升温至750～850℃。
10.一种根据权利要去1-9任一项所述制备方法制得的高介电性能氮化硅复合陶瓷。
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