Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries,Chemistry of Materials

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Engineering Solution-Processed Non-Crystalline Solid Electrolytes for Li Metal Batteries
Chemistry of Materials ( IF 7.2 ) Pub Date : 2023-01-18 , DOI: 10.1021/acs.chemmater.2c03071
Pooja Vadhva ₁ , Thomas E Gill ₁ , Joshua H Cruddos _{1,

2} , Samia Said ₁ , Marco Siniscalchi ₃ , Sudarshan Narayanan _{2,

3} , Mauro Pasta _{2,

3} , Thomas S Miller _{1,

2} , Alexander J E Rettie _{1,

2}

Affiliation

Non-crystalline Li-ion solid electrolytes (SEs), such as lithium phosphorus oxynitride, can uniquely enable high-rate solid-state battery operation over thousands of cycles in thin film form. However, they are typically produced by expensive and low throughput vacuum deposition, limiting their wide application and study. Here, we report non-crystalline SEs of composition Li–Al–P–O (LAPO) with ionic conductivities > 10^–7 S cm^–1 at room temperature made by spin coating from aqueous solutions and subsequent annealing in air. Homogenous, dense, flat layers can be synthesized with submicrometer thickness at temperatures as low as 230 °C. Control of the composition is shown to significantly affect the ionic conductivity, with increased Li and decreased P content being optimal, while higher annealing temperatures result in decreased ionic conductivity. Activation energy analysis reveals a Li-ion hopping barrier of ≈0.4 eV. Additionally, these SEs exhibit low room temperature electronic conductivity (< 10^–11 S cm^–1) and a moderate Young’s modulus of ≈54 GPa, which may be beneficial in preventing Li dendrite formation. In contact with Li metal, LAPO is found to form a stable but high impedance passivation layer comprised of Al metal, Li–P, and Li–O species. These findings should be of value when engineering non-crystalline SEs for Li-metal batteries with high energy and power densities.

中文翻译：

用于锂金属电池的工程溶液处理非晶固体电解质

非结晶锂离子固体电解质 (SE)，例如锂磷氮氧化物，可以独特地以薄膜形式实现数千次循环的高速固态电池操作。然而，它们通常是通过昂贵且低通量的真空沉积生产的，限制了它们的广泛应用和研究。在这里，我们报告了组成为 Li–Al–P–O (LAPO) 的非晶态 SE，其离子电导率 > 10 ^–7 S cm ^–1在室温下通过从水溶液中旋涂然后在空气中退火制成。可以在低至 230 °C 的温度下合成亚微米厚度的均匀、致密、平坦的层。组成的控制显示显着影响离子电导率，增加 Li 和减少 P 含量是最佳的，而较高的退火温度导致离子电导率降低。活化能分析显示 ≈0.4 eV 的锂离子跃迁势垒。此外，这些 SE 表现出较低的室温电子电导率（< 10 ^–11 S cm ^–1) 和 ≈54 GPa 的中等杨氏模量，这可能有利于防止锂枝晶的形成。在与锂金属接触时，发现 LAPO 形成了一个稳定但高阻抗的钝化层，该钝化层由铝金属、Li-P 和 Li-O 物质组成。这些发现在为具有高能量和功率密度的锂金属电池设计非晶态 SE 时应该很有价值。

更新日期：2023-01-18

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