Zhang Bingkai, He Zhiwei, Liu Tiefeng, Li Zeheng, Zhang Shaojian, Zhao Wenguang, Yin Zu-Wei, Zhuo Zengqing, Zhang Mingjian, Pan Feng, Zhang Shanqing, Lin Zhan, Lu Jun
Guangdong Provincial Key Laboratory of Plant Resources Biorefinery, School of Chemical Engineering and Light Industry, Guangdong University of Technology, Guangzhou, 510006, China.
Jieyang Branch of Chemistry and Chemical Engineering Guangdong Laboratory, Jieyang, 515200, P. R. China.
Adv Mater. 2024 Feb;36(6):e2305748. doi: 10.1002/adma.202305748. Epub 2023 Dec 7.
The interfacial compatibility between cathodes and sulfide solid-electrolytes (SEs) is a critical limiting factor of electrochemical performance in all-solid-state lithium-ion batteries (ASSLBs). This work presents a gas-solid interface reduction reaction (GSIRR), aiming to mitigate the reactivity of surface oxygen by inducing a surface reconstruction layer (SRL) . The application of a SRL, CoO/Li CO , onto LiCoO (LCO) cathode results in impressive outcomes, including high capacity (149.7 mAh g ), remarkable cyclability (retention of 84.63% over 400 cycles at 0.2 C), outstanding rate capability (86.1 mAh g at 2 C), and exceptional stability in high-loading cathode (28.97 and 23.45 mg cm ) within ASSLBs. Furthermore, the SRL CoO/Li CO enhances the interfacial stability between LCO and Li GeP S as well as Li PS SEs. Significantly, the experiments suggest that the GSIRR mechanism can be broadly applied, not only to LCO cathodes but also to LiNi Co Mn O cathodes and other reducing gases such as H S and CO, indicating its practical universality. This study highlights the significant influence of the surface chemistry of the oxide cathode on interfacial compatibility, and introduces a surface reconstruction strategy based on the GSIRR process as a promising avenue for designing enhanced ASSLBs.
阴极与硫化物固体电解质（SEs）之间的界面兼容性是全固态锂离子电池（ASSLBs）电化学性能的关键限制因素。这项工作提出了一种气固界面还原反应（GSIRR），旨在通过诱导表面重构层（SRL）来降低表面氧的反应活性。在LiCoO₂（LCO）阴极上应用SRL CoO/Li₂CO₃产生了令人印象深刻的结果，包括高容量（149.7 mAh g⁻¹）、出色的循环稳定性（在0.2 C下400次循环后保持率为84.63%）、优异的倍率性能（在2 C下为86.1 mAh g⁻¹）以及在ASSLBs高负载阴极（28.97和23.45 mg cm⁻²）中的卓越稳定性。此外，SRL CoO/Li₂CO₃增强了LCO与Li₃GeP₂S₆以及Li₃PS₄ SEs之间的界面稳定性。值得注意的是，实验表明GSIRR机制不仅可以广泛应用于LCO阴极，还可以应用于LiNi₀.₈Co₀.₁Mn₀.₁O₂阴极以及其他还原气体如H₂S和CO，表明其实际通用性。这项研究突出了氧化物阴极表面化学对界面兼容性的重大影响，并引入了基于GSIRR过程的表面重构策略，作为设计增强型ASSLBs的一条有前景的途径。
