CN111065613B - 陶瓷复合材料 - Google Patents

陶瓷复合材料 Download PDF

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CN111065613B
CN111065613B CN201880055581.5A CN201880055581A CN111065613B CN 111065613 B CN111065613 B CN 111065613B CN 201880055581 A CN201880055581 A CN 201880055581A CN 111065613 B CN111065613 B CN 111065613B
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moo
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CN111065613A (zh
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贾里·汉努
贾里·朱蒂
赫利·贾图南
米科·尼洛
托莫·斯波科斯基
汉娜·卡哈里
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Abstract

一种制备陶瓷‑金属复合材料的方法，包括将陶瓷粉末溶解到水中获得陶瓷水溶液；将金属粉末与陶瓷水溶液混合以获得包含陶瓷沉积在金属颗粒表面的粉末，所述金属粉末具有多峰粒度且最大粒度是装置的最小尺寸的四分之一；将包含陶瓷沉积在金属颗粒表面的所述粉末与粒度尺寸在50μm以下的陶瓷粉末混合，以获得粉末混合物；将陶瓷的饱和水溶液添加到所述粉末混合物中以获得包括陶瓷和金属的水溶液复合物；压缩所述水溶液复合物以形成包括陶瓷和金属的陶瓷‑金属复合材料的盘状物；移除所述陶瓷‑金属复合材料的水分；所述盘状物中陶瓷的含量为10vol％‑35vol％。可替换的，还可以制备陶瓷‑陶瓷复合材料。

Description

陶瓷复合材料
技术领域
本发明涉及一种陶瓷复合材料，尤其涉及这种材料的制备方法。
背景技术
陶瓷材料被广泛用于许多行业，包括采矿，航空航天，医药，炼油，食品和化学工业，包装科学，电子，工业和电传输以及引导光波传输。在由金属和陶瓷制成的复合材料中，通过陶瓷硬化颗粒增强金属基质材料。这使得可以将金属的轻重量与陶瓷的耐用性相结合。陶瓷复合材料可用于制造电子元件。电子元件可以是有源元件，例如半导体或电源，也可以是无源元件，例如电阻或电容。
发明内容
一方面提供了独立权利要求的主题。实施例在从属权利要求中定义。
在下面的描述中更详细地阐述了实现的一个或多个示例。根据说明书和权利要求书，其他特征将显而易见。
具体实施方式
以下实施例是示例性的。尽管说明书可能在多个位置引用“一”，“一个”或“一些”实施例，但这并不一定意味着每个此类引用均指的是同一实施例，或者该特征仅适用于单个实施例。不同实施例的单个特征也可以组合以实现其他实施例。此外，词语“包括”，“包含”和“含有”应理解为不将所描述的实施例限制为仅由已经提到的那些特征组成，并且这些实施例还可以包含尚未被特别提到的特征/结构。
可以在室温下通过少量水和Li2MoO4粉末制备Li2MoO4陶瓷。通过挤压和去除多余的水来实现所述陶瓷的致密化。因此，可以通过控制模具尺寸和陶瓷材料的量来调节陶瓷产品的形状和尺寸。可以在120℃下进行后处理，以去除陶瓷上的残留水。然而，后处理步骤不是必须的，或者后处理步骤可以在低于120℃的温度下进行。低温陶瓷材料具有的介电性能可以与在540℃下烧结制成的Li2MoO4陶瓷具有的介电性能相类似(例如，相对介电常数为5.1，在9.6GHz下损耗角正切值为0.00035)。
在一实施例中，所述陶瓷复合材料包含钼酸锂Li2MoO4。
在一实施例中，替代钼酸锂Li2MoO4或除了钼酸锂Li2MoO4之外，所述陶瓷复合材料可包含例如NaCl，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，KH2PO4，Li2WO4，Mg2P2O7和/或V2O5。
钼酸锂Li2MoO4可以用作制备所述陶瓷复合材料的原料。根据一实施例，所述原材料可以是泥质的(粘土的)材料，糊剂，浆液或粘性较小的流体，所述粘性较小的流体是能够形成或模制所述陶瓷复合材料。
用于制造包含所述陶瓷复合材料的电子元件的方法，所述陶瓷复合材料含有钼酸锂，所述方法可以包括压力模制(压模)，成型(注浆成型)，浸涂或2D/3D打印(二维或三维打印)。
因此，实施例公开了一种电子元件，包括一种包含所述陶瓷复合材料的电子元件所述陶瓷复合材料含有钼酸锂Li2MoO4。所述电子元件可以包括电池，电连接路径和调节电子设备中的至少一种。
一实施例涉及陶瓷-金属复合材料。另一实施例涉及陶瓷-陶瓷复合材料。陶瓷材料本身非常耐用且稳定。可以通过向陶瓷基质材料中添加金属或另一种类型的陶瓷来改变所述陶瓷材料的特性。金属通常是可延展和耐用的材料，并且具有高的热导率。陶瓷通常是化学稳定和抗氧化的，并且它们具有高的熔化温度。示例性地，陶瓷-金属复合材料能够组合金属和陶瓷两者的最佳特性，例如陶瓷的硬度和高热强度以及金属的电导率。示例性地，陶瓷-陶瓷复合材料能够结合不同陶瓷材料的所述最佳特性，例如多种电性能和磁性能，包括铁电特性，热电特性，压电特性，铁氧体特性，高介电特性和铁磁特性。
示例性地，陶瓷-金属复合材料可以用于制造电子元件，例如电阻，电容和其他电子元件。示例性地，陶瓷-金属复合材料也可以用于在机床中以代替金属刀片。示例性地，陶瓷-陶瓷和/或陶瓷-金属复合材料也可用于传感器中以替代常规的高温压电陶瓷，以及用于铁氧体中替代磁性材料，例如线圈的芯。示例性地，陶瓷-金属复合材料和/或陶瓷-陶瓷复合材料还可以用于陶瓷-金属界面，用于生物医学中，作为制动器中的摩擦材料，光电元件中和/或作为装甲车辆中的防碎裂物。
示例性地，陶瓷-陶瓷复合材料可以用于制造电子元件，例如电容，线圈，传感器，致动器，高频无源器件，能量存储和收集器，调谐元件和变压器。
公开了一种先进的陶瓷-金属复合材料和制造所述先进的陶瓷-金属复合材料的方法。此外，公开了一种先进的陶瓷-陶瓷复合材料和制造所述先进的陶瓷-陶瓷复合材料的方法。示例性地，陶瓷-金属复合材料和陶瓷-陶瓷复合材料可用于在电子设备(例如，印刷电子设备)的低温制造中生产电阻，电容和/或导体。在低温(例如室温)下制造能够实现所述电子元件的节能制造。在低温制造中，金属相和陶瓷相之间的扩散不会发生或扩散极小，这可以在保持陶瓷和金属的原始介电，铁电和磁性能情况下，改善所述复合材料的电性能。因此可以防止或减少生成额外相，例如有耗介质的额外相。
一实施例公开了一种制造陶瓷-金属复合材料的方法。另一实施例公开了一种制造陶瓷-陶瓷复合材料的方法。例如，所述陶瓷包含在室温下结晶的钼酸锂(Li2MoO4)。替代钼酸锂的/除钼酸锂之外，所述陶瓷可以包含例如NaCl，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，KH2PO4，Li2WO4，Mg2P2O7和/或V2O5。所述陶瓷-金属复合材料包含金属颗粒作为添加剂(例如，所述金属颗粒是Al，Fe，Ni，Co，Ag，Cu，TbxDy1-xFe2，NdFeB，SmCo5和/或其他元素或合金，其中所述元素或所述合金具有所需的热，电和/或磁功能)。所述陶瓷-陶瓷复合材料包含陶瓷颗粒(例如PZT，BaxSr1-xTiO3，TiO2，Al2O3，KNBNNO和相关材料，铁氧体相关材料和/或其他电陶瓷材料)。
制造陶瓷-金属复合材料或陶瓷-陶瓷复合材料的示例性方法包括制备具有多峰粒度的金属或陶瓷粉末，其中最大粒度为电子设备最小尺寸的四分之一。所述方法进一步包括将Li2MoO4粉末溶解在水中以获得Li2MoO4的水溶液。将所述金属或陶瓷粉末与所述Li2MoO4的水溶液混合。
由此获得一种粉末，所述粉末包含沉积在所述金属或陶瓷颗粒的表面上的Li2MoO4，所述粉末与粒度小于50μm的钼酸锂混合。因此所述粉末包括水溶液中的Li2MoO4，如上所述的Li2MoO4颗粒以及提供电性能的金属或陶瓷颗粒。与金属材料或陶瓷材料相比，所述陶瓷-金属复合或所述陶瓷-陶瓷复合材料中Li2MoO4的含量为10-30vol％(体积百分比)。例如，将0.1-0.5ml的Li2MoO4饱和水溶液添加到0.8-1.2g的粉末混合物中以获得复合物。然后将获得的所述复合物通过例如250MPa的模压在模具中(例如在直径为10mm的模具中)压缩，形成固体的盘状物。压缩模塑后所述复合物/盘状物的水含量为2.5-3.0wt％(质量百分比)。水分含量超过3wt％可能会使所述盘状物难以处理。最终产物的Li2MoO4含量为14-35vol％。
可将所述盘状物在烤炉中于120℃的温度下干燥16小时以去除残留的水。或者，可以在室温下或在20℃至120℃的任何温度下干燥所述盘状物，但在这种情况下，需要更长的干燥时间。干燥后，将所述盘状物的表面抛光以除去粘附的杂质，并获得用于电极的光滑表面。然后可以通过例如使用丝网印刷油墨在所述盘状物表面上制备电极。
因此，用于制造陶瓷-金属复合材料或陶瓷-陶瓷复合材料的示例性方法包括使用具有多峰粒度(例如，低于180μm)的金属或陶瓷颗粒，其中金属或陶瓷颗粒的最大粒度为电子设备最小尺寸的四分之一，以及使用具有小粒径(即，小于50μm)的钼酸锂颗粒以获得所述盘状物，其中所述具有小粒径的钼酸锂颗粒是使用Li2MoO4的饱和水溶液，并在250MPa的压力下，抗粘模具中进行压制成型。可替代地，可以使用3D打印来获得所属盘状物。所述陶瓷-金属复合材料和所述陶瓷-陶瓷复合材料可用于各种应用，包括电子应用，例如印刷电子中使用的材料。所述陶瓷-金属复合材料可以是导热的，并且具有高的热强度和很多电陶瓷的典型特性。
在一实施例中，替代钼酸锂Li2MoO4或除了钼酸锂Li2MoO4之外，所述陶瓷-金属复合材料或所述陶瓷-陶瓷复合材料可包含例如NaCl，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，KH2PO4，Li2WO4，Mg2P2O7和/或V2O5。
一种所述陶瓷-金属复合材料的制造方法，包括将Li2MoO4溶解在水中以获得Li2MoO4的水溶液或将其他陶瓷粉末溶解在水中以获得所述其他陶瓷的水溶液。将金属粉末与所述Li2MoO4的水溶液或所述其他陶瓷的水溶液混合，所述金属粉末具有多峰粒度且最大颗粒尺寸为电子设备最小尺寸的四分之一，以获得包含Li2MoO4沉积在所述金属颗粒表面的粉末，或包含所述其他陶瓷沉积在所述金属颗粒表面的粉末；将所述包含Li2MoO4沉积在所述金属颗粒表面的粉末与粒度小于50μm的Li2MoO4混合以获得粉末混合物，或将所述包含其他陶瓷沉积在所述金属颗粒表面的粉末与粒度小于50μm的所述其他陶瓷粉末混合，以获得粉末混合物；将Li2MoO4的饱和水溶液添加到所述粉末混合物中，以获得包含Li2MoO4以及金属的水溶液复合物，或将所述其他陶瓷的饱和水溶液添加到所述粉末混合物中，以获得包含所述其他陶瓷以及金属的水溶液复合物。通过成型压力在模具中压缩所述水溶液复合物，以形成包含Li2MoO4和金属的陶瓷-金属复合材料的盘状物，或包含所述其他陶瓷和金属的陶瓷-金属复合材料的盘状物；干燥所述盘状物以除去所述陶瓷-金属复合材料中的水；其中所述盘状物中Li2MoO4或所述其他陶瓷的含量为10vol％至35vol％。
所述金属包括Al，Fe，Ni，Co，Ag，Cu，TbxDy1-xFe2，NdFeB，SmCo5和/或其他金属元素或金属合金。
所述其他陶瓷包含NaCl，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，KH2PO4，Li2WO4，Mg2P2O7和/或V2O5中的至少一种。
一种陶瓷-陶瓷复合材料的制造方法，包括将含有Li2MoO4或其他陶瓷的第一陶瓷粉末溶解于水中，得到第一陶瓷的水溶液。将第二陶瓷粉末与所述第一陶瓷的水溶液混合，所述第二陶瓷粉末具有多峰粒度且最大颗粒尺寸为电子设备最小尺寸的四分之一，以获得包含第一陶瓷沉积在所述第二陶瓷颗粒表面上的粉末；将上述已获得的所述粉末与粒径小于50μm的第一陶瓷粉末混合，得到粉末混合物；将所述第一陶瓷的饱和水溶液添加到所述粉末混合物中以获得包含所述第一陶瓷和所述第二陶瓷的水溶液复合物；通过成型压力在模具中压缩所述水溶液复合物，以形成包含第一陶瓷和第二陶瓷的陶瓷-陶瓷复合材料的盘状物；干燥所述盘状物以除去所述陶瓷-陶瓷复合材料中的水；其中所述盘状物中第一陶瓷含量为10vol％-35vol％。
所述第一陶瓷包含Li2MoO4，NaCl，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，KH2PO4，Li2WO4，Mg2P2O7和/或V2O5中的至少一种。所述第二陶瓷包含PZT，BaxSr1-xTiO3，TiO2，Al2O3，KNBNNO及相关材料，铁氧体相关材料以及其他电陶瓷材料中的至少一种。所述第一陶瓷和所述第二陶瓷彼此不同。
所述水溶液复合物的压缩在100至500MPa的成型压力下进行，优选地为250MPa。
所述盘状物可以在20℃至120℃的温度下干燥至少16小时，优选地在120℃的温度下干燥16小时。
干燥后，可以对所述盘状物的表面进行抛光以获得光滑的盘状物表面，其中在光滑的盘状物表面上制备电极(例如通过印刷)。
所述陶瓷-金属复合材料的陶瓷含量可以为10vol％-35vol％，并且包括具有多峰粒度的金属粉末，其中最大粒度为电子装置(电子元件)的最小尺寸的四分之一。所述陶瓷-金属复合材料可以通过上述方法获得。
所述陶瓷-陶瓷复合材料的第一陶瓷含量可以为10vol％-35vol％，并且包括具有多峰粒度的第二陶瓷粉末，其中最大粒度为电子装置(电子元件)的最小尺寸的四分之一。所述陶瓷-陶瓷复合材料可以通过上述方法获得。
公开了一种电子元件，包括所述陶瓷-金属复合材料或所述陶瓷-陶瓷复合材料。所述电子元件可以包括电阻，导体和电容器的至少一种。
所述陶瓷-金属复合材料或所述陶瓷-陶瓷复合材料可用于电子元件，例如电阻，电容，线圈，传感器，致动器，高频无源设备，能量存储和收集器，调谐元件和/或变压器。
公开了一种电子产品，所述电子产品包括所述电子元件。
所述第二陶瓷粉末的粒径可以大于50μm。这能够最大化所述复合材料中第二陶瓷粉末的量。所述复合材料中第二陶瓷粉末的量可以高于65vol％。因此，所述第二陶瓷粉末可以是所述复合材料中的主要成分。
所述第二陶瓷粉末可以由不溶性金属/陶瓷形成，并且所述复合材料中大于65vol％由所述第二陶瓷粉末形成。
所述不溶性颗粒的粒径分布是多峰的，其中最大颗粒的粒径大于50μm。这增强了模具的填充和所述盘状物的制备。
所述复合材料的制造过程中的温度不超过150℃，也不需要超过溶液的沸腾温度。在压缩过程中不需要额外加热，而是可以在室温下进行压缩。可以在压缩并制成所述盘状物后执行可选的热处理。准备所述盘状物的处理时间只需要2至5分钟。
对于本领域技术人员而言显而易见的是，随着技术的进步，可以以各种方式来实现本发明的构思。本发明及其实施例不限于上述示例，而是可以在权利要求的范围内变化。

Claims (27)

1.一种合成陶瓷-金属复合材料的方法，其特征在于，所述方法包括：
将陶瓷粉末溶解在水中以获得所述陶瓷的水溶液；
将金属粉末与所述陶瓷的水溶液混合，以获得包含所述陶瓷沉积在金属颗粒表面的粉末，所述金属粉末具有多峰粒度且最大粒度大于50μm小于180μm；
将包含所述陶瓷沉积在金属颗粒表面的所述粉末与所述陶瓷粉末混合，以获得粉末混合物，混合的所述陶瓷粉末的粒度小于50μm；
将所述陶瓷的饱和水溶液添加到所述粉末混合物中，以获得包含所述陶瓷以及金属的水溶液复合物；
在模具中将所述水溶液复合物压缩，以形成所述陶瓷-金属复合材料的盘状物，所述陶瓷-金属复合材料包含所述陶瓷粉末以及所述金属；
干燥所述盘状物以除去所述陶瓷-金属复合材料中的水；
所述盘状物中所述陶瓷粉末的含量为10vol％-35vol％；以及
所述盘状物中所述金属的含量大于65vol％。
2.根据权利要求1所述的方法，其特征在于，所述陶瓷为Li2MoO4或其他陶瓷。
3.根据权利要求2所述的方法，其特征在于，所述金属包括Al，Fe，Ni，Co，Ag，Cu，TbxDy1- xFe2，NdFeB合金，SmCo5。
4.根据权利要求2或3所述的方法，其特征在于，所述其他陶瓷包括Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，Li2WO4，Mg2P2O7和/或V2O5中的至少一种。
5.根据权利要求1-4任一项所述的方法，其特征在于，所述水溶液复合物的压缩在成型压力100到500MPa下进行。
6.根据权利要求5所述的方法，其特征在于，所述水溶液的压缩在成型压力250MPa下进行。
7.根据权利要求1-4任一项所述的方法，其特征在于，所述盘状物在20℃至120℃的温度下干燥至少16小时。
8.根据权利要求7所述的方法，其特征在于，所述盘状物在120℃下干燥16小时。
9.根据权利要求1-4任一项所述的方法，其特征在于，干燥后，将所述盘状物的表面抛光以获得光滑的盘状物表面，然后在所述光滑的盘状物表面上制备电极。
10.根据权利要求1-4任一项所述的方法，其特征在于，干燥后，将所述盘状物的表面抛光以获得光滑的盘状物表面，然后通过印刷在所述光滑的盘状物表面上制备电极。
11.一种合成陶瓷-陶瓷复合材料的方法，其特征在于，所述方法包括：
将Li2MoO4或其他陶瓷粉末溶解在水中以获得第一陶瓷的水溶液；
将第二陶瓷粉末与所述第一陶瓷的水溶液混合，以获得包含所述Li2MoO4沉积在所述第二陶瓷颗粒表面的粉末或所述其他陶瓷沉积在所述第二陶瓷颗粒表面的粉末，所述第二陶瓷粉末具有多峰粒度且最大粒度大于50μm且小于180μm；
将包含所述Li2MoO4沉积在所述第二陶瓷颗粒表面的所述粉末与所述Li2MoO4混合，以获得粉末混合物，或将包含所述其他陶瓷沉积在所述第二陶瓷颗粒表面的所述粉末与所述其他陶瓷粉末混合，以获得粉末混合物，所述Li2MoO4或所述其他陶瓷粉末的粒度小于50μm；
将所述Li2MoO4的饱和水溶液添加到所述粉末混合物中，以获得包含所述Li2MoO4以及所述第二陶瓷的水溶液复合物，或将所述其他陶瓷的饱和水溶液添加到所述粉末混合物中，以获得包含所述其他陶瓷以及所述第二陶瓷的水溶液复合物；
在模具中将所述水溶液复合物压缩，以形成所述陶瓷-陶瓷复合材料的盘状物，所述陶瓷-陶瓷复合材料包含所述Li2MoO4以及所述第二陶瓷，或包含所述其他陶瓷以及所述第二陶瓷；
干燥所述盘状物以除去所述陶瓷-陶瓷复合材料中的水；
所述盘状物中所述Li2MoO4或所述其他陶瓷的含量为10vol％-35vol％，以及所述盘状物中所述第二陶瓷的含量大于65vol％。
12.根据权利要求11所述的方法，其特征在于，
所述第一陶瓷包括Li2MoO4，Na2Mo2O7，K2Mo2O7，(LiBi)0.5MoO4，Li2WO4，Mg2P2O7和/或V2O5中的至少一种；
所述第二陶瓷包括PZT，BaxSr1-xTiO3，TiO2，Al2O3，KNBNNO，铁氧体陶瓷材料以及其他电陶瓷材料中的至少一种；
所述第一陶瓷和所述第二陶瓷彼此不相同。
13.根据权利要求11或12所述的方法，其特征在于，所述水溶液复合物的压缩在成型压力100到500MPa下进行。
14.根据权利要求13所述的方法，其特征在于，所述水溶液的压缩在成型压力250MPa下进行。
15.根据权利要求11或12所述的方法，其特征在于，所述盘状物在20℃至120℃的温度下干燥至少16小时。
16.根据权利要求15所述的方法，其特征在于，所述盘状物在120℃下干燥16小时。
17.根据权利要求11或12所述的方法，其特征在于，干燥后，将所述盘状物的表面抛光以获得光滑的盘状物表面，然后在所述光滑的盘状物表面上制备电极。
18.根据权利要求11或12所述的方法，其特征在于，干燥后，将所述盘状物的表面抛光以获得光滑的盘状物表面，然后通过印刷在所述光滑的盘状物表面上制备电极。
19.一种通过如权利要求1-10中任一项所述的方法制备的陶瓷-金属复合材料，其特征在于，所述陶瓷-金属复合材料中陶瓷的含量为10vol％-35vol％，而且包括金属粉末，所述金属粉末具有多峰粒度且最大粒度大于50μm小于180μm。
20.一种通过如权利要求11-18中任一项所述的方法制备的陶瓷-陶瓷复合材料，其特征在于，所述陶瓷-陶瓷复合材料中的第一陶瓷含量为10vol％-35vol％，而且包括第二陶瓷粉末，所述第二陶瓷粉末具有多峰粒度且最大粒度大于50μm小于180μm。
21.一种电子元件，其特征在于，所述电子元件包括如权利要求19中所述的陶瓷-金属复合材料。
22.根据权利要求21所述的电子元件，其特征在于，所述电子元件包括电阻，导体和电容中的至少一种。
23.一种电子元件，其特征在于，所述电子元件包括如权利要求20中所述的陶瓷-陶瓷复合材料。
24.根据权利要求23所述的电子元件，其特征在于，所述电子元件包括电阻，导体和电容中的至少一种。
25.一种将权利要求19中所述的陶瓷-金属复合材料应用在电子元件中的方法，所述电子元件包括电阻，电容，线圈，传感器，致动器，高频无源器件，能量存储和收集器，调谐元件和变压器中的一种或多种。
26.一种将权利要求20中所述的陶瓷-陶瓷复合材料应用在电子元件中的方法，所述电子元件包括电阻，电容，线圈，传感器，致动器，高频无源器件，能量存储和收集器，调谐元件和变压器中的一种或多种。
27.一种电子产品，其特征在于，所述电子产品包括如权利要求25或26所述的电子元件。
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