<br>硼氢化物和卤化物双取代锂银矿,Materials Horizons

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硼氢化物和卤化物双取代锂银矿
Materials Horizons ( IF 12.2 ) Pub Date : 2023-11-06 , DOI: 10.1039/d3mh01450a
Ji-Hoon Han _{1,

2} , Do Kyung Kim ₃ , Young Joo Lee _{3,

4} , Young-Su Lee ₁ , Kyung-Woo Yi ₂ , Young Whan Cho ₁

Affiliation

固体电解质是全固态电池的关键组成部分，其中硫银矿锂等硫化物固体电解质由于其高离子电导率和成型性而最接近商业化。在本研究中，硼氢化物/卤化物双取代银汞矿型电解质Li _{7− α − β} PS _{6− α − β} (BH ₄ ) _α X _β (X = Cl, Br, I; α + β ≤ 1.8)，采用两步球磨法合成，无需后退火。在各种组合物中，Li _5.35 PS _4.35 (BH ₄ ) _1.15 Cl _0.5在冷压时在25℃下表现出最高的离子电导率，为16.4 mS cm ^-1 ，在低温烧结后进一步提高至26.1 mS cm ^-1 。电导率增强可归因于BH ₄增加以及卤化物占据和位点无序导致Li空位数量增加。 Li 对称电池，Li _5.35 PS _4.35 (BH ₄ ) _1.15 Cl _0。图5展示了在1 mA cm ^-2下稳定的锂沉积和剥离循环超过2,000小时，以及2.1 mA cm ^-2的高临界电流密度。以Li _5.35 PS _4.35 (BH ₄ ) _1.15 Cl _0.5作为电解质、纯Li作为负极制备的全固态电池的初始库伦效率为86.4%。尽管这些电解质的热稳定性有限，但它在保持高离子电导率的同时表现出较宽的组成范围。

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Borohydride and halide dual-substituted lithium argyrodites

Solid electrolyte is a crucial component of all-solid-state batteries, with sulphide solid electrolytes such as lithium argyrodite being closest to commercialization due to their high ionic conductivity and formability. In this study, borohydride/halide dual-substituted argyrodite-type electrolytes, Li_7−α−βPS_6−α−β(BH₄)_αX_β (X = Cl, Br, I; α + β ≤ 1.8), have been synthesized using a two-step ball-milling method without post-annealing. Among the various compositions, Li_5.35PS_4.35(BH₄)_1.15Cl_0.5 exhibits the highest ionic conductivity of 16.4 mS cm⁻¹ at 25 °C when cold-pressed, which further improves to 26.1 mS cm⁻¹ after low temperature sintering. The enhanced conductivity can be attributed to the increased number of Li vacancies resulting from increased BH₄ and halide occupancy and site disorder. Li symmetric cells with Li_5.35PS_4.35(BH₄)_1.15Cl_0.5 demonstrate stable Li plating and stripping cycling for over 2,000 hours at 1 mA cm⁻², along with a high critical current density of 2.1 mA cm⁻². An all-solid-state battery prepared using Li_5.35PS_4.35(BH₄)_1.15Cl_0.5 as the electrolyte and pure Li as the anode exhibits an initial coulombic efficiency of 86.4%. Although these electrolytes have limited thermal stability, it shows a wide compositional range while maintaining high ionic conductivity.

更新日期：2023-11-06

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