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The activation entropy for ionic conduction and critical current density for Li charge transfer in novel garnet-type Li6.5La2.9A0.1Zr1.4Ta0.6O12 (A = Ca, Sr, Ba) solid electrolytes
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020/01/14 , DOI: 10.1039/c9ta12193e Sanoop Palakkathodi Kammampata 1, 2, 3, 4 , Hirotoshi Yamada 5, 6, 7, 8 , Tomoko Ito 5, 6, 7, 8 , Reginald Paul 1, 2, 3, 4 , Venkataraman Thangadurai 1, 2, 3, 4
Journal of Materials Chemistry A ( IF 11.9 ) Pub Date : 2020/01/14 , DOI: 10.1039/c9ta12193e Sanoop Palakkathodi Kammampata 1, 2, 3, 4 , Hirotoshi Yamada 5, 6, 7, 8 , Tomoko Ito 5, 6, 7, 8 , Reginald Paul 1, 2, 3, 4 , Venkataraman Thangadurai 1, 2, 3, 4
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In this paper, we report the activation entropy (ΔS) values for Li-stuffed Li6.5La2.9A0.1Zr1.4Ta0.6O12 (A = Ca, Sr, Ba) garnets using a statistical mechanical approach and the role of ceramic processing in Li ion charge transfer between elemental Li and Li-stuffed Li6.5La2.9A0.1Zr1.4Ta0.6O12 garnets. The investigated solid electrolytes were prepared by a solid-state reaction and a spark plasma sintering method. The formation of the garnet-type structure was confirmed by powder X-ray diffraction. The homogeneous distribution of the elements in the prepared compositions was investigated using electron probe micro analyzer coupled with a wavelength-dispersive X-ray spectrometer. Li ion conductivity was determined using electrochemical ac impedance spectroscopy. The calculated ΔS value for garnet-type Li6.5La2.9A0.1Zr1.4Ta0.6O12 is found to be one order of magnitude higher than that of other solid electrolytes such as Li4SiO4 (Li+), Na3ZrMgP3O12 (Na+), AgI (Ag+) and Ag-β-alumina (Ag+) and comparable to that of the polymer Li ion electrolyte (PEO)10-LiClO4. SPS-processed Li6.5La2.9A0.1Zr1.4Ta0.6O12 samples showed a bulk Li ion conductivity of 5.5 × 10−4 S cm−1 at 22 °C. Among all the samples investigated in this work, Li6.5La2.9Sr0.1Zr1.4Ta0.6O12 showed an impressive Li ion charge transfer resistance (RCT) of 3.5 Ω cm2 at 25 °C without any surface coating of metal oxides, such as Al2O3 and ZnO, and exhibited a critical current density of 0.6 mA cm−2.
中文翻译：
新型石榴石型Li6.5La2.9A0.1Zr1.4Ta0.6O12（A = Ca，Sr，Ba）固体电解质中离子传导的激活熵和Li电荷转移的临界电流密度
在本文中，我们使用统计机械方法和填充陶瓷的作用报告了填充锂的6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12（A = Ca，Sr，Ba）石榴石的活化熵（ΔS）值锂与填充锂之间的锂离子电荷转移过程6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12石榴石。通过固态反应和火花等离子体烧结方法制备了所研究的固体电解质。通过粉末X射线衍射确认了石榴石型结构的形成。使用电子探针显微分析仪结合波长色散X射线光谱仪研究了元素在制备的组合物中的均匀分布。使用电化学交流阻抗谱测定锂离子电导率。发现石榴石型Li 6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12的ΔS值比其他固体电解质（如Li 4）高一个数量级。SiO 4（Li +），Na 3 ZrMgP 3 O 12（Na +），AgI（Ag +）和Ag-β-氧化铝（Ag +），与聚合物锂离子电解质（PEO）10 -LiClO 4相当。经SPS处理的Li 6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12样品在22°C下的整体锂离子电导率为5.5×10 -4 S cm -1。在这项工作中调查的所有样本中，Li 6.5 La 2.9 Sr0.1的Zr 1.4的Ta 0.6 ø 12显示令人印象深刻的锂离子的电荷转移阻力（ [R CT 3.5Ω厘米） 2在25℃下不具有金属氧化物，如Al的任何表面涂层2 ö 3和ZnO，并显示出的临界电流密度为0.6 mA cm -2。
更新日期：2020-02-10
中文翻译：
新型石榴石型Li6.5La2.9A0.1Zr1.4Ta0.6O12（A = Ca，Sr，Ba）固体电解质中离子传导的激活熵和Li电荷转移的临界电流密度
在本文中，我们使用统计机械方法和填充陶瓷的作用报告了填充锂的6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12（A = Ca，Sr，Ba）石榴石的活化熵（ΔS）值锂与填充锂之间的锂离子电荷转移过程6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12石榴石。通过固态反应和火花等离子体烧结方法制备了所研究的固体电解质。通过粉末X射线衍射确认了石榴石型结构的形成。使用电子探针显微分析仪结合波长色散X射线光谱仪研究了元素在制备的组合物中的均匀分布。使用电化学交流阻抗谱测定锂离子电导率。发现石榴石型Li 6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12的ΔS值比其他固体电解质（如Li 4）高一个数量级。SiO 4（Li +），Na 3 ZrMgP 3 O 12（Na +），AgI（Ag +）和Ag-β-氧化铝（Ag +），与聚合物锂离子电解质（PEO）10 -LiClO 4相当。经SPS处理的Li 6.5 La 2.9 A 0.1 Zr 1.4 Ta 0.6 O 12样品在22°C下的整体锂离子电导率为5.5×10 -4 S cm -1。在这项工作中调查的所有样本中，Li 6.5 La 2.9 Sr0.1的Zr 1.4的Ta 0.6 ø 12显示令人印象深刻的锂离子的电荷转移阻力（ [R CT 3.5Ω厘米） 2在25℃下不具有金属氧化物，如Al的任何表面涂层2 ö 3和ZnO，并显示出的临界电流密度为0.6 mA cm -2。
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