<br>BH4 取代的硫代磷酸盐固体电解质中的锂超离子传导,Advanced Science

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BH4 取代的硫代磷酸盐固体电解质中的锂超离子传导
Advanced Science ( IF 14.3 ) Pub Date : 2022-12-11 , DOI: 10.1002/advs.202204942
Yong-Jin Jang ₁ , Hyungeun Seo ₁ , Young-Su Lee ₂ , Sora Kang ₃ , Woosuk Cho ₃ , Young Whan Cho ₂ , Jae-Hun Kim ₁

Affiliation

与传统液体电解质相比，固体电解质可以更好地提高安全性能，实现高能量密度的锂离子电池。硫化物基固体电解质由于其高离子电导率（可与液体电解质相媲美）而引起了广泛关注。其中，硫代磷酸锂，包括银银矿，被广泛研究。在这项研究中，即使不进行热处理，通过简单快速的研磨方法制备了含有BH ₄ ^-阴离子的硫代磷酸锂固体电解质。合成的材料在25℃下表现出高达11 mS cm ^-1的高离子电导率，远高于报道的值。为了阐明其背后的机制，研究了硫代磷酸盐局部结构，其对离子电导率的影响迄今为止仍不清楚。通过拉曼光谱和固态核磁共振光谱来鉴定硫化物样品中的硫代磷酸盐局部结构。根据分析结果，确定所制备的电解质样品中不同硫代磷酸盐单元的比例。研究发现，通过改变LiBH ₄的量和研磨条件可以改变硫代磷酸盐的局部结构，这显着影响离子电导率。采用所制备的固体电解质的全固态电池表现出优异的循环和倍率性能。

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Lithium Superionic Conduction in BH4-Substituted Thiophosphate Solid Electrolytes

Compared with conventional liquid electrolytes, solid electrolytes can better improve the safety properties and achieve high-energy-density Li-ion batteries. Sulfide-based solid electrolytes have attracted significant attention owing to their high ionic conductivities, which are comparable to those of their liquid counterparts. Among them, Li thiophosphates, including Li-argyrodites, are widely studied. In this study, Li thiophosphate solid electrolytes containing BH₄⁻ anions are prepared via a simple and fast milling method even without heat treatment. The synthesized materials exhibit a high ionic conductivity of up to 11 mS cm⁻¹ at 25 °C, which is much higher than reported values. To elucidate the mechanism behind, the thiophosphate local structure, whose effect on the ionic conductivity remains unclear to date, is investigated. Raman and solid-state NMR spectroscopies are performed to identify the thiophosphate local structure in the sulfide samples. Based on the analysis results, the ratios of the different thiophosphate units in the prepared electrolyte samples are determined. It is found that the thiophosphate local structure can be varied by changing the amount of LiBH₄ and the milling conditions, which significantly impact the ionic conductivity. The all-solid-state cell with the prepared solid electrolyte exhibits superior cycle and rate performances.

更新日期：2022-12-11

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