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arXiv 2403.14136cond-mat.mtrl-scicond-mat.str-el
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Ni取代Na$_{3+2x}$Zr$_{2-x}$Ni$_{x}$Si$_2$PO$_{\rm 12}$的温度依赖电导率、介电弛豫、电模量和阻抗谱研究

Temperature dependent conductivity, dielectric relaxation, electrical modulus and impedance spectroscopy of Ni substituted Na$_{3+2x}$Zr$_{2-x}$Ni$_{x}$Si$_2$PO$_{\rm 12}$

Ramcharan Meena, Rajendra S. Dhaka

AI总结:

本研究采用固相反应法制备了Ni掺杂NASICON陶瓷,基于Maxwell-Wagner双层模型和KWW函数等分析了其非Debye型介电弛豫、电模量及阻抗行为,揭示了晶粒与晶界对总电导率的双重贡献。

摘要:

我们研究了采用固相反应法制备的Ni掺杂NASICON陶瓷Na$_{3+2x}$Zr$_{2-x}$Ni$_{x}$Si$_2$PO$_{\rm 12}$($x=$ 0.05--0.2)的结构、介电弛豫、电模量和阻抗行为。介电常数随温度升高而增加、随频率降低而减小的现象,可基于Maxwell-Wagner弛豫双层模型通过空间电荷极化来解释。低温下的介电损耗峰随频率变化遵循Arrhenius型行为,其偶极弛豫激活能为0.27$\pm$0.01~eV,表明所有掺杂样品中存在类似类型的缺陷。实部($ε$ $^{'}$)和虚部($ε$ $^{''}$)介电常数随频率的变化表现出宽弛豫行为,表明在测量温度范围内为非Debye型弛豫。由于在Zr位进行Ni掺杂增加了电荷载流子数量,介电常数值随掺杂量增加而降低。晶粒贡献在高频下观察到,而晶界贡献则出现在低频侧。电模量的虚部在所有样品中也表现出两种类型的弛豫峰,表明在低温下具有相似的激活能,而在高温下激活能可变。使用KWW函数对虚部模量进行拟合,结果显示为非Debye型弛豫。我们发现所有模量曲线在低温下相互重合,表现出相似的弛豫类型,而高温下的曲线在峰值频率以上表现出色散行为。交流电导率数据使用双幂律进行拟合,证实了总电导率中的晶粒和晶界贡献。

英文摘要:

We investigate the structural, dielectric relaxation, electric modulus and impedance behavior of Ni-doped NASICON ceramic Na$_{3+2x}$Zr$_{2-x}$Ni$_{x}$Si$_2$PO$_{\rm 12}$ ($x=$ 0.05--0.2) prepared using the solid-state reaction method. The increase in dielectric constant with temperature and decrease with frequency is explained on the basis of space charge polarization using the two-layer model of Maxwell-Wagner relaxation. The dielectric loss peak at lower temperatures follows the Arrhenius-type behavior with frequency having activation energy of 0.27$\pm$0.01~eV of dipolar relaxation, suggests similar type of defects are responsible for all the doped samples. The real ($ε$ $^{'}$) and imaginary ($ε$ $^{''}$) permittivity variation with frequency shows the broad relaxation behavior indicates the non-Debye type of relaxation in the measured temperature range. The permittivity values decrease with the amount of doping due to the increased number of charge carriers upon Ni doping at the Zr site. The grain contributions are observed at higher frequencies, while grain-boundary contributions occur at the lower side of frequencies. The imaginary part of the electric modulus also shows two types of relaxation peaks for all the samples indicating similar activation energy at low temperatures and variable activation energy at higher temperatures. The fitting of the imaginary modulus using KWW function shows the non-Debye type of relaxation. We find that all modulus curves merge with each other at low temperatures showing a similar type of relaxation, while curves at high temperatures show the dispersed behavior above the peak frequency. The {\it a.c.} conductivity data are fitted using the double power law confirming the grain and grain boundary contributions in total conductivity.

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