CN113233901B - 致密高纯锶钽氧氮化物陶瓷及其制备方法 - Google Patents

致密高纯锶钽氧氮化物陶瓷及其制备方法 Download PDF

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CN113233901B
CN113233901B CN202110745116.8A CN202110745116A CN113233901B CN 113233901 B CN113233901 B CN 113233901B CN 202110745116 A CN202110745116 A CN 202110745116A CN 113233901 B CN113233901 B CN 113233901B
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strontium tantalum
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李端
李俊生
曾良
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National University of Defense Technology
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Abstract

本发明公开了一种致密高纯锶钽氧氮化物陶瓷的制备方法，包括将锶钽氧氮化物陶瓷粉体与乙醇混合均匀，球磨后干燥并过筛，得到预烧结粉体，将预烧结粉体在加压、保护气氛或者在加压、真空条件下进行放电等离子烧结，烧结温度为1300℃～1400℃，经冷却，得到陶瓷初烧结体，将陶瓷初烧结体在氨气气氛、无压力条件下进行二次烧结，降温冷却后，得到致密高纯锶钽氧氮化物陶瓷。本发明的制备方法时间短，制得的致密高纯锶钽氧氮化物陶瓷具有高纯度、高密度、高介电常数、低介电损耗的优点，有广泛的应用前景。

Description

致密高纯锶钽氧氮化物陶瓷及其制备方法
技术领域
本发明涉及高性能介电陶瓷材料制备技术领域，尤其涉及一种致密高纯锶钽氧氮化物陶瓷及其制备方法。
背景技术
作为一种新型钙钛矿类材料，锶钽氧氮化物SrTaO2N在室温下有着较高的介电常数，耐酸碱腐蚀，热稳定性好，在高性能电容器等领域有着广泛的应用前景。致密化主要是烧结过程，即颗粒重排靠近，使陶瓷致密化以及晶粒生长的过程，主要影响因素有烧结温度、升温速率和保温时间，在加压烧结过程中压力也会对陶瓷的致密化产生影响。对于烧结温度，烧结温度过高时会导致陶瓷晶粒生长过大或组织机构不均匀，还会促进二次结晶，而过低的烧结温度则会导致晶粒发育不完全材料无法充分致密化，对于介电材料，密度和孔隙率是影响陶瓷介电性能的重要参数，需要选择最佳的烧结温度以获得密度高、孔隙率低的样品们才能得到良好的介电性能。对于升温速率，过快的升温速率将会提高晶粒的长大速度，或出现异常长大，陶瓷表面快速致密化，使其内部气孔难以消除，孔隙率过高。保温过程中，材料的各部分温度均匀化并完全结晶成瓷，当保温时间较短时，陶瓷各部分温度不均匀，晶粒不能充分发育长大，晶界过多；而保温时间延长时，陶瓷中的晶粒重新排列并进一步长大，所得陶瓷材料也会更加致密。针对目前主流的氨化加无压烧结的制备方法有工艺时间长、产物纯度和致密度偏低等不足，因此，对于致密化材料新烧结工艺及参数的研究是至关重要的，现亟待发展一种耗时短的方法烧结得到高密度、高纯度、高介电常数的锶钽氧氮化物陶瓷。
发明内容
本发明要解决的技术问题是克服现有技术的不足，提供一种制备周期较短、具有高纯度、高密度、高介电常数的致密高纯锶钽氧氮化物陶瓷及其制备方法。
为解决上述技术问题，本发明采用以下技术方案：
一种致密高纯锶钽氧氮化物陶瓷的制备方法，包括以下步骤：
S1、将锶钽氧氮化物陶瓷粉体与乙醇混合均匀，经球磨后，干燥、过筛，得到预烧结粉体；
S2、将步骤S1所得的预烧结粉体，在加压、保护气氛条件下或者在加压、真空条件下进行放电等离子烧结，所述加压的压力为140MPa～150MPa，所述放电等离子烧结的烧结温度为1300℃～1400℃，升温速率为300℃/min～500℃/min，烧结保温0～10min，然后自然冷却，得到陶瓷初始烧结体；
S3、将步骤S2所得的陶瓷初始烧结体在氨气气氛、无压力条件下进行二次烧结，烧结温度为1310℃～1500℃，该烧结温度需大于步骤S2中的烧结温度，升温速率为10℃/min～20℃/min，烧结保温1min～80min，然后降温冷却，得到致密高纯锶钽氧氮化物陶瓷。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S2中，烧结保温0～5min。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S3中，烧结保温20min～60min。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S1中，所述球磨采用的球磨罐材质为聚氨酯、氧化铝或氧化锆，所述球磨采用的球磨珠材质为聚氨酯、氧化铝或氧化锆，所述球磨的时间为1h～8h，所述干燥的温度为50℃～200℃，所述干燥的时间为1h～18h，所述过筛的目数为3000目～10000目。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S1中，所述球磨的时间为2h～4h，所述干燥的温度为100℃～150℃，所述干燥的时间为6h～12h，所述过筛的目数为3000目～6000目。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S2中，所述保护气氛为氮气、氦气和氩气中的一种或多种。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S3中，所述降温冷却的冷却速率为1℃/min～200℃/min。
上述的致密高纯锶钽氧氮化物陶瓷的制备方法，优选的，步骤S3中，所述降温冷却的冷却速率为10℃/min～100℃/min。
作为一个总的发明构思，本发明还提供一种上述的制备方法制得的致密高纯锶钽氧氮化物陶瓷。
本发明中，步骤S1采用的原料锶钽氧氮化物陶瓷粉体的制备方法可参考申请人在先申请并公开的专利文献，包括以下步骤：
(1)将4.43g碳酸锶粉末、6.63g五氧化二钽粉末与9g尿素溶于50mL无水乙醇并球磨，得到混合浆料；
(2)将混合浆料充分干燥，得到混合前驱体粉末；
(3)将混合前驱体粉末放置在坩埚中，在保护气氛下1000℃煅烧，得到锶钽氧氮化物陶瓷粉体，即SrTaO2N陶瓷粉体。
与现有技术相比，本发明的优点在于：
本发明采用放电等离子烧结通过焦耳热效应及场效应实现对材料的高效高速加热，可加速原子扩散，从而加速致密化，本发明采用的烧结温度较传统烧结方式低，可在热力学上抑制氧氮化物分解，烧结过程中可施加高的压力，且保温时间短，能有效控制晶粒生长速度，利于获得细晶结构。本发明通过两步法烧结氧氮化物，可尽可能提高产物的致密度，同时通过特定温度、压力和保温时间使材料的开气孔率占总气孔率的比例最高，便于二次烧结时氨气的进入，在氨气气氛中进行二次烧结既使得放电等离子烧结中分解的氧氮化物恢复了化学计量比，又消除了剩余的大部分气孔率，进一步提高产物的致密度和纯度。
附图说明
图1为本发明实施例1制得的致密高纯锶钽氧氮化物陶瓷的光学图片。
图2为本发明实施例1制得的致密高纯锶钽氧氮化物陶瓷的XRD谱图。
图3为本发明实施例1制得的致密高纯锶钽氧氮化物陶瓷的SEM图。
图4为本发明实施例1制得的致密高纯锶钽氧氮化物陶瓷的介电常数和损耗角正切值频谱曲线图。
具体实施方式
以下结合说明书附图和具体优选的实施例对本发明作进一步描述，但并不因此而限制本发明的保护范围。以下实施例中所采用的原料和仪器均为市售。
实施例1：
一种本发明的致密高纯锶钽氧氮化物陶瓷的制备方法，包括以下步骤：
S1、将5g锶钽氧氮化物陶瓷粉体与20mL无水乙醇混合均匀，在聚氨酯球磨罐中用聚氨酯球磨珠球磨4h，在100℃下干燥8h，然后在6000目过筛，得到预烧结粉体。
S2、将步骤S1所得4g预烧结粉体放入Φ12mm的石墨模具中，在放电等离子烧结设备中进行初始烧结，工艺条件为：压力140MPa，气氛为氮气，升温速率300℃/min，烧结温度为1300℃，保温时间为1min，自然冷却后得到陶瓷初烧结体。
S3、将步骤S2所得的陶瓷初始烧结体放入管式炉，在无机械压力、氨气气氛条件下进行二次烧结，烧结工艺条件为：升温速率为20℃/min，烧结温度为1350℃，保温时间为60min，冷却速率为30℃/min。降温冷却后得到致密高纯锶钽氧氮化物陶瓷。
本实施例中，锶钽氧氮化物陶瓷粉体的制备过程如下：
(1)将4.43g碳酸锶粉末、6.63g五氧化二钽粉末与9g尿素溶于50mL无水乙醇并球磨，得到混合浆料；
(2)将混合浆料充分干燥，得到混合前驱体粉末；
(3)将混合前驱体粉末放置在坩埚中，在保护气氛下1000℃煅烧，得到锶钽氧氮化物陶瓷粉体，即SrTaO2N陶瓷粉体。
将本实施例制得的致密高纯锶钽氧氮化物陶瓷片上下表面打磨，其光学图片如图1所示，其颜色为深棕褐色，与氧氮化物陶瓷粉体相近，其物相组成及微观形貌分别如图2和图3所示。由图2和图3可知，本实施例制备得到的SrTaO2N氧氮化物陶瓷几乎为纯相，其微观结构致密，晶粒尺寸约300nm。经测试，所得陶瓷片致密度为94.36％(致密度为体积密度/理论密度，SrTaO2N的理论密度为8.021g/cm3)，闭气孔率为5.23％。图4为本实施例制得的致密高纯锶钽氧氮化物陶瓷在室温下介电常数和损耗角正切值随频率变化曲线，由图可知，其在300Hz下有着极高的介电常数(9550)和较低的损耗(0.001)。
对比例1：
一种锶钽氧氮化物陶瓷的制备方法，与实施例1基本相同，不同之处在于：
步骤S2中，并未采用放电等离子烧结设备进行初烧结，而是采用传统无压烧结炉，升温速率为10℃/min，烧结温度为1300℃，保温时间为1min。
本对比例制备得到的SrTaO2N氧氮化物陶瓷片致密度为55.84％，闭气孔率为36.38％，物相组成为SrTa(O,N)3和Sr5Ta4O15。可见，此对比例产物相对密度和纯度都较实施例1明显降低，而闭气孔率高。这是由于采用传统无压方式初烧结，陶瓷初烧结体的致密度较低，其气孔率较高且气孔大，使得在二次烧结时很难致密化，而传统初烧结较慢的升温速率又从动力学上加快了氧氮化物的分解。
对比例2：
一种锶钽氧氮化物陶瓷的制备方法，与实施例1不同之处在于：没有步骤S3，即直接对氧氮化物进行放电等离子烧结，其机械压力140MPa，气氛为氮气，升温速率300℃/min，烧结温度为1300℃，保温时间为1min，自然冷却后得到陶瓷烧结体。
本对比例制备得到的EuTa(O,N)3氧氮化物陶瓷片相对密度为91.88％，闭气孔率为7.4％，物相组成为SrTa(O,N)3、Sr5Ta4OTa3N5和Ta3N5。可见，此对比例产物纯度较实施例1低。这是由于采用高压、快速升温和提高烧结温度的放电等离子烧结方法虽然从一定程度上能快速致密化氧氮化物，但因其分解温度低于烧结温度，产物分解严重且无法恢复化学计量比。
实施例2：
一种本发明的致密高纯锶钽氧氮化物陶瓷的制备方法，与实施例1的制备过程基本相同，区别仅在于：步骤S2中，放电等离子烧结温度为1400℃，保温时间为3min。
经检测，本实施例制备得到的SrTaO2N氧氮化物陶瓷片致密度为95.62％，闭气孔率为3.76％，在室温、300Hz下介电常数为5935，介电损耗为0.0016。
虽然本发明已以较佳实施例揭露如上，然而并非用以限定本发明。任何熟悉本领域的技术人员，在不脱离本发明技术方案范围的情况下，都可利用上述揭示的技术内容对本发明技术方案做出许多可能的变动和修饰，或修改为等同变化的等效实施例。因此，凡是未脱离本发明技术方案的内容，依据本发明技术实质对以上实施例所做的任何简单修改、等同变化及修饰，均应落在本发明技术方案保护的范围内。

Claims (8)

1.一种致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，包括以下步骤：
S1、将锶钽氧氮化物陶瓷粉体与乙醇混合均匀，经球磨后，干燥、过筛，得到预烧结粉体；
S2、将步骤S1所得的预烧结粉体，在加压、保护气氛条件下或者在加压、真空条件下进行放电等离子烧结，所述加压的压力为140MPa～150MPa，所述放电等离子烧结的烧结温度为1300℃～1400℃，升温速率为300℃/min～500℃/min，烧结保温0～10min，然后自然冷却，得到陶瓷初始烧结体；
S3、将步骤S2所得的陶瓷初始烧结体在氨气气氛、无压力条件下进行二次烧结，烧结温度为1310℃～1500℃，该烧结温度需大于步骤S2中的烧结温度，升温速率为10℃/min～20℃/min，烧结保温1min～80min，然后降温冷却，得到致密高纯锶钽氧氮化物陶瓷。
2.根据权利要求1所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S2中，烧结保温0～5min。
3.根据权利要求1所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S3中，烧结保温20min～60min。
4.根据权利要求1～3中任一项所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S1中，所述球磨采用的球磨罐材质为聚氨酯、氧化铝或氧化锆，所述球磨采用的球磨珠材质为聚氨酯、氧化铝或氧化锆，所述球磨的时间为1h～8h，所述干燥的温度为50℃～200℃，所述干燥的时间为1h～18h，所述过筛的目数为3000目～10000目。
5.根据权利要求4所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S1中，所述球磨的时间为2h～4h，所述干燥的温度为100℃～150℃，所述干燥的时间为6h～12h，所述过筛的目数为3000目～6000目。
6.根据权利要求1～3中任一项所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S2中，所述保护气氛为氮气、氦气和氩气中的一种或多种。
7.根据权利要求1～3中任一项所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S3中，所述降温冷却的冷却速率为1℃/min～200℃/min。
8.根据权利要求7所述的致密高纯锶钽氧氮化物陶瓷的制备方法，其特征在于，步骤S3中，所述降温冷却的冷却速率为10℃/min～100℃/min。
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