CN113185289B - 一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷及其制备方法 - Google Patents

一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷及其制备方法 Download PDF

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CN113185289B
CN113185289B CN202110347455.0A CN202110347455A CN113185289B CN 113185289 B CN113185289 B CN 113185289B CN 202110347455 A CN202110347455 A CN 202110347455A CN 113185289 B CN113185289 B CN 113185289B
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zirconate titanate
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边浪
曹文武
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Jiangsu Acoustic Industry Technology Innovation Center
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Abstract

一种超低介电损耗的铌锰酸铅‑铌镍酸铅‑锆钛酸铅高压电性铁电陶瓷及其制备方法。本发明属于压铁电材料领域。本发明是为了解决现有软性陶瓷高介电损耗的技术问题。本发明的一种超低介电损耗的铌锰酸铅‑铌镍酸铅‑锆钛酸铅高压电性铁电陶瓷的化学通式为x Pb(Mn1/ 3Nb2/3)O3‑(0.55‑x)Pb(Ni1/3Nb2/3)O3‑0.135PbZrO3‑0.315PbTiO3，其中x＝0.01‑0.03。制备方法：按陶瓷成分配比配料，然后依次经过预烧、压片、排胶、烧结，再经烧银和极化后得到超低介电损耗的铌锰酸铅‑铌镍酸铅‑锆钛酸铅高压电性铁电陶瓷。本发明的方法预烧温度低，通过配方与工艺的优化烧结出铌锰酸铅‑铌镍酸铅‑锆钛酸铅弛豫铁电陶瓷，准静态d33测试仪测量压电常数达760pC/N的同时，介电损耗低于0.5％，性能优异。

Description

一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性 铁电陶瓷及其制备方法
技术领域
本发明属于压铁电材料领域，具体涉及一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷及其制备方法。
背景技术
信息化是21世纪重要的时代特征，电子陶瓷作为一大类新型的信息材料，发展迅速；压电陶瓷材料作为电子陶瓷的一种，在高压、医疗、导航、通讯和智能系统等高新技术领域获得广泛的应用。近年来，随着电子信息器件走向集成化、微型化以及新的技术领域也对压电陶瓷材料性能提出更高的要求，而新型压电陶瓷材料的研究是高性能压电器件及很多前沿科学技术领域研究的基础，有迫切的市场需求和重大社会价值。
锆钛酸铅[Pb(ZrxTi1-x)O3,PZT]基的压电陶瓷被广泛应用于执行器、传感器、压电变压器、微电子器件等领域。然而，在掺杂改性追求高压电常数的过程中，其介电损耗也随之升高，目前商用的PZT-5H陶瓷，其压电常数高达700pC/N的同时，介电损耗高达2％。这极大限制了其在应用中的工作稳定性。较高的介电损耗容易引起陶瓷本身温度的升高，从而损害器件的性能。基于这个原因，如果能让陶瓷在拥有较高压电常数的同时，又具有很小的其介电损耗是研究人员一直追求的目标。
发明内容
本发明是为了解决现有软性陶瓷高介电损耗的技术问题，而提供一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷及其制备方法。
本发明的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的化学通式为x Pb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3，其中x＝0.01-0.03。
本发明的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的制备方法按以下步骤进行：
步骤一、配料：以MnO2、PbO、TiO2、ZrO2、NiO、Nb2O5作为原料，按照超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的化学计量比称取原料，其中PbO的物质的量过量1.5％，球磨烘干；
步骤二、预烧：将步骤一烘干的粉体置于坩埚中，然后在马弗炉中预烧粉体；
步骤三、压片：将步骤二得到的预烧粉体二次球磨烘干，然后加入聚乙烯醇溶液研磨均匀，过筛后压制成胚体；
步骤四、排胶：将步骤三得到的胚体放入马弗炉中进行排胶，得到排胶后胚件；
步骤五、烧结：将步骤四得到的排胶后胚件放于马弗炉中，以同组分粉料覆盖胚件进行埋烧，先以3℃/min～10℃/min的升温速度升至1000～1100℃，保温1h～3h，然后以1.5℃/min～2.5℃/min的升温速度升至1200～1300℃，保温2.5h～3.5h，保温结束以3℃/min～10℃/min的降温速度降至750～850℃，然后自然冷却至室温，得到陶瓷片；
步骤六、烧银：将步骤五烧结好的陶瓷片表面打磨处理，然后在陶瓷片的上、下表面涂抹银浆，再置于马弗炉中进行烧银，自然冷却至室温，得到被银的陶瓷片；
步骤七、极化：将步骤六得到的被银的陶瓷片置于20～35℃的硅油中，施加电场进行极化，得到超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷。
进一步限定，步骤二中预烧的过程为：以3℃/min～10℃/min的升温速度升温至700～740℃，并在该温度下保温1.5h～3h，得到预烧粉体。
进一步限定，步骤三中所述聚乙烯醇溶液的加入量为步骤二得到的预烧粉体的5wt％～7wt％。
进一步限定，步骤三中所述过筛是过80～200目筛。
进一步限定，步骤三中所述压制的压力为150Mpa～300MPa。
进一步限定，步骤四中所述排胶的过程为：先以0.5℃/min～1.5℃/min的升温速度升至180～220℃，保温1.5h～2.5h，然后以0.2℃/min～0.4℃/min的升温速度升至580～620℃，保温1.5h～2.5h。
进一步限定，步骤五中先以5℃/min的升温速度升至1050℃，保温1h，然后以2℃/min的升温速度升至1260℃，保温3h，保温结束以5℃/min的降温速度降至800℃。
进一步限定，步骤六中所述烧银的过程为：以3℃/min～10℃/min的升温速度升温至630～670℃，并在该温度下保温20min～40min。
进一步限定，步骤七中所述极化的电场强度为1kV/mm～3kV/mm，极化时间为5min～15min。
本发明相比现有技术的优点如下：
1)本发明的方法预烧温度低，通过配方与工艺的优化烧结出铌锰酸铅-铌镍酸铅-锆钛酸铅弛豫铁电陶瓷，准静态d33测试仪测量压电常数达760pC/N的同时，介电损耗低于0.5％，准静态d33测试仪测量压电常数达950pC/N的同时介电损耗仅为1.1％。
2)本发明选择原子半径相近的微量锰元素替代镍元素，避开了单纯掺杂造成的性能暴降，得到了超低介电损耗的软性陶瓷，解决了软性陶瓷高介电损耗的问题，极大的拓展了软性陶瓷的应用范围，使其可以应用在功率型器件中，且其较大的压电常数有利于降低驱动电压。
附图说明
图1为实施例1制备的xPb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3陶瓷的介电温谱；
图2为实施例1制备的xPb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3陶瓷的P-E曲线。
具体实施方式
实施例1：本实施例的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的化学式为xPb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3，其中x＝0.1、0.2、0.3。
制备实施例1的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的方法按以下步骤进行：
步骤一、配料：以MnO2、PbO、TiO2、ZrO2、NiO、Nb2O5作为原料，按照xPb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3的化学计量比称取原料，其中PbO的物质的量过量1.5％，球磨烘干；其中MnO2、PbO、TiO2、ZrO2、NiO、Nb2O5均为市售的化学纯原料(纯度≥99％)；球磨烘干过程为：球磨介质为酒精，加入酒精的质量为原料总质量的80％，磨球直径8mm，磨球数目为覆盖球磨罐1/3处，球磨24h后烘干；
步骤二、预烧：将步骤一烘干的粉体置于坩埚中，然后在马弗炉中，以5℃/min的升温速度升温至720℃，并在该温度下保温2h，得到预烧粉体；
步骤三、压片：将步骤二得到的预烧粉体二次球磨24h烘干，然后加入聚乙烯醇溶液研磨均匀，过100目筛后于150MPa下压制成直径13mm，厚度1mm的圆片状胚体；所述聚乙烯醇溶液的加入量为步骤二得到的预烧粉体的5wt％；
步骤四、排胶：将步骤三得到的胚体放入马弗炉中，先以1℃/min的升温速度升至200℃，保温2h，然后以0.3℃/min的升温速度升至600℃，保温2h进行排胶，得到排胶后胚件；
步骤五、烧结：将步骤四得到的排胶后胚件放于马弗炉中，以同组分粉料覆盖胚件进行埋烧，先以5℃/min的升温速度升至1050℃，保温1h，然后以2℃/min的升温速度升至1260℃，保温3h，保温结束以5℃/min的降温速度降至800℃，然后自然冷却至室温，得到陶瓷片；
步骤六、烧银：将步骤五烧结好的陶瓷片表面打磨处理，然后在陶瓷片的上、下表面涂抹银浆，再置于马弗炉中，以5℃/min的升温速度升温至650℃，并在该温度下保温30min进行烧银，自然冷却至室温，得到被银的陶瓷片；
步骤七、极化：将步骤六得到的被银的陶瓷片置于30℃的硅油中，施加2kV/mm电场进行极化10min，得到超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷即xPb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3陶瓷。
对比例1：按照铌镍酸铅-锆钛酸铅压电陶瓷(0.55Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3)的化学计量比以及实施例1的制备方法制备得到铌镍酸铅-锆钛酸铅压电陶瓷。
对比例2：按照铌锰酸铅-锆钛酸铅压电陶瓷((0.05Pb(Mn1/3Nb2/3)O3-0.47PbZrO3-0.48PbTiO3)的化学计量比以及实施例1的制备方法制备得到铌锰酸铅-锆钛酸铅压电陶瓷，与实施例1的制备方法的区别在于：烧结的具体过程为：将排胶后胚件放于马弗炉中，以同组分粉料覆盖胚件进行埋烧，先以5℃/min的升温速度升至1000℃，然后以2℃/min的升温速度升至1200℃，保温3h，然后自然冷却至室温，得到陶瓷片；极化的温度为120℃，施加4kv/mm电场极化10min。其他步骤及参数与实施例1相同。
测试：将实施例1和对比例1-2所制备的陶瓷室温静置24h测试其电学性能，电学性能测试结果列于表1。介电温谱见图1，P-E曲线见图2。
表1电学性能测试结果
组分 d<sub>33</sub>(pC/N) tanδ k<sub>p</sub> Q<sub>m</sub> T<sub>c</sub>(℃) ε
x＝0.01 950 1.1％ 0.55 69 115 6981
x＝0.02 760 0.45％ 0.55 247 125 5415
x＝0.03 650 0.41％ 0.56 425 130 4781
对比例1 1200 3.4％ 0.63 34 105 9715
对比例2 280 0.36％ 0.53 920 300 1230

Claims (8)

1.一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，该超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的化学通式为x Pb(Mn1/3Nb2/3)O3-(0.55-x)Pb(Ni1/3Nb2/3)O3-0.135PbZrO3-0.315PbTiO3，其中x = 0.02-0.03，所述超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的制备方法按以下步骤进行：
步骤一、配料：以MnO2、PbO、TiO2、ZrO2、NiO、Nb2O5作为原料，按照超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷的化学计量比称取原料，其中PbO的物质的量过量1.5%，球磨烘干；
步骤二、预烧：将步骤一烘干的粉体置于坩埚中，然后在马弗炉中预烧粉体；所述预烧的过程为：以3℃/min~10℃/min的升温速度升温至700~740℃，并在该温度下保温1.5h~3h，得到预烧粉体；
步骤三、压片：将步骤二得到的预烧粉体二次球磨烘干，然后加入聚乙烯醇溶液研磨均匀，过筛后压制成胚体；
步骤四、排胶：将步骤三得到的胚体放入马弗炉中进行排胶，得到排胶后胚件；
步骤五、烧结：将步骤四得到的排胶后胚件放于马弗炉中，以同组分粉料覆盖胚件进行埋烧，先以3℃/min~10℃/min的升温速度升至1000~1100℃，保温1h~3h，然后以1.5℃/min~2.5℃/min的升温速度升至1200~1300℃，保温2.5h~3.5h，保温结束以3℃/min~10℃/min的降温速度降至750~850℃，然后自然冷却至室温，得到陶瓷片；
步骤六、烧银：将步骤五烧结好的陶瓷片表面打磨处理，然后在陶瓷片的上、下表面涂抹银浆，再置于马弗炉中进行烧银，自然冷却至室温，得到被银的陶瓷片；
步骤七、极化：将步骤六得到的被银的陶瓷片置于20-35℃的硅油中，施加电场进行极化，得到超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷。
2.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤三中所述聚乙烯醇溶液的加入量为步骤二得到的预烧粉体的5wt%~7wt%。
3.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤三中所述过筛是过80~200目筛。
4.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤三中所述压制的压力为150MPa~300MPa。
5.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤四中所述排胶的过程为：先以0.5℃/min~1.5℃/min的升温速度升至180~220℃，保温1.5h~2.5h，然后以0.2℃/min~0.4℃/min的升温速度升至580~620℃，保温1.5h~2.5h。
6.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤五中先以5℃/min的升温速度升至1050℃，保温1h，然后以2℃/min的升温速度升至1260℃，保温3h，保温结束以5℃/min的降温速度降至800℃。
7.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤六中所述烧银的过程为：以3℃/min~10℃/min的升温速度升温至630~670℃，并在该温度下保温20min~40min。
8.根据权利要求1所述的一种超低介电损耗的铌锰酸铅-铌镍酸铅-锆钛酸铅高压电性铁电陶瓷，其特征在于，步骤七中所述极化的电场强度为1 kV/mm~3kV/mm，极化时间为5min~15min。
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