Sulfide-based all-solid-state lithium-ion batteries (ASSLBs) hold promise in realizing improved safety and high energy density. In this study, we present the innovative use of polyvinylidene difluoride (PVDF) polymer as a sacrificial agent for heat reduction of LiCoO₂ (LCO), which facilitates the bidirectional interfacial compatibility between the composite LCO–Li₆PS₅Cl (LPSCl). An in situ formed CoO/Li₂CO₃/LiF interlayer on the LCO surface not only improves the cathode's performance 4.5 V but also allows for increased cathode loading. The initial capacity of PVDF-treated LCO (145.3 mA h g⁻¹) is substantially higher than that of bare-LCO, with the latter experiencing a sharp capacity decline after 100 cycles. ASSLBs with high cathode loading (16.63 mg cm⁻²) could deliver an areal capacity over 1.96 mA h cm⁻² (162.8 mA h g⁻¹) at 0.3C and retain 80.33% capacity retention after 80 cycles at 0.3C. The in situ phase transformation CoO interphase derived from lattice LCO reinforces the stability and structural integrity of the particles, thereby keeping intact the cathode particle. The Li₂CO₃/LiF interphase greatly enhances the interface stability and reduces side reactions between LCO and LPSCl. This cost-effective and efficient strategy offers a significant advancement in developing high-performance cathodes for ASSLBs.

中文翻译：

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Janus在LiCoO2和Li6PS5Cl固体电解质之间原位形成CoO/Li2CO3/LiF中间层，提高了硫化物基全固态电池的4.5V性能


硫化物基全固态锂离子电池（ASSLB）有望实现更高的安全性和高能量密度。在这项研究中，我们创新性地使用聚偏二氟乙烯（PVDF）聚合物作为LiCoO ₂ （LCO）热还原的牺牲剂，这促进了复合材料LCO-Li ₆ PS ₅ Cl（LPSCl）之间的双向界面相容性。 LCO表面上原位形成的CoO/Li ₂ CO ₃ /LiF中间层不仅提高了阴极的4.5 V性能，而且还允许增加阴极负载。经过PVDF处理的LCO的初始容量（145.3 mA hg ^-1 ）显着高于裸LCO，但后者在100次循环后容量急剧下降。具有高阴极负载（16.63 mg cm ^-2 ）的ASSLBs可以在0.3C下提供超过1.96 mA h cm ^-2 （162.8 mA hg ^-1 ）的面积容量，并在0.3C下80个循环后保留80.33%的容量保持率。来自晶格 LCO 的原位相变 CoO 界面增强了颗粒的稳定性和结构完整性，从而保持阴极颗粒的完整性。 Li ₂ CO ₃ /LiF界面大大增强了界面稳定性并减少了LCO和LPSCl之间的副反应。这种经济高效的策略为开发 ASSLB 高性能阴极提供了重大进步。