Rapid synthesis of dielectric tantalum-based oxynitrides

Rapid synthesis of dielectric tantalum-based oxynitrides
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电介质钽基氮氧化物的快速合成

DOI:
10.1016/j.matdes.2019.108416
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发表时间:
2020-02
期刊:
影响因子:
8.4
通讯作者:
Zhongshuai Wu
Zhongshuai Wu
中科院分区:
材料科学1区
文献类型:
--
作者:
Duan Li;Liang Zeng;Bin Li;Xuejin Yang;Qiuping Yu;Zhongshuai Wu

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通式为ata (O,N)3(a = Sr, Ba)的钙钛矿型氮氧化物具有很高的介电常数,是一类很有前途的介电材料。这些材料的传统合成路线总是需要多个加工步骤,长时间和高温。在本研究中,热力学计算预测了可行的合成反应,可能的杂质和合理的工艺参数。然后,利用改进的无压火花等离子烧结装置,以尿素为氮源,将SrCO3/ baco3和ta2o5直接煅烧,制备出SrTaO2N和BaTaO2N陶瓷粉末。10分钟内可制得高纯度氮氧化物。对其热稳定性、耐腐蚀性和介电性能进行了评价。结果表明,SrTaO2N在空气中的热稳定性为475℃,BaTaO2N在空气中的热稳定性为605℃。氮氧化物具有良好的耐热水和强酸/强碱性能。在100 Hz下,BaTaO2N的相对介电常数高达9550,介电损耗降至0.001,而SrTaO2N的相对介电常数分别为3141和0.017。在−10 ~ 200℃时,BaTaO2N介电常数的温度依赖性较弱。这种高效的合成方法使钽基氮化氧储能材料的快速制备成为可能。
Perovskite-type oxynitride with a general formula ofATa(O,N)3(A= Sr, Ba) is a class of promising dielectric material due to their very high permittivity. Conventional synthesis routes for these materials always require multiple processing steps, long durations and elevated temperatures. In this study, thermodynamic calculations were employed to predict the feasible synthesis reactions, possible impurities and reasonable processing parameters. Then, ceramic powders of SrTaO2N and BaTaO2N were fabricated through direct calcination of SrCO3/BaCO3and Ta2O5with urea as nitrogen source by using a modified pressureless spark plasma sintering set-up. High-purity oxynitrides can be obtained within 10 min. Thermal stability, corrosion resistance and dielectric property were evaluated. The results showed that SrTaO2N was thermally stable up to 475 °C in air while that temperature for BaTaO2N was 605 °C. The oxynitrides possessed a good resistance to hot water and strong acid/alkali. BaTaO2N had a very high room-temperature relative permittivity up to 9550 with a dielectric loss down to 0.001 at 100 Hz, while the values for SrTaO2N were 3141 and 0.017 respectively. The temperature dependence of permittivity for BaTaO2N was weak at −10–200 °C. The efficient synthesis method enabled the fast preparation of the tantalum-based oxynitride materials for energy storage applications.
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