High-voltage all-solid-state batteries (ASSBs) promise high-energy-density storage, but oxidative instability of solid-state electrolytes at cathode interfaces remains a major obstacle. Here, we report a sacrificial-additive strategy for durable, high-voltage operation of low-cost Zr-based halide ASSBs. Introducing LiPO2F2 (LPOF) into Li2ZrCl4O (LZCO) markedly enhances interfacial and oxidative stability. Paired with uncoated LiCoO2, the ASSBs deliver over 80% capacity after 700 cycles at 2 C (4.6 V cutoff) and cycle stably under ultrahigh cathode loadings of 35.7 mg cm-2. Notably, the cells sustain 5 V operation with over 80% capacity after 380 cycles at 2 C and over 70% retention after 3500 cycles at 7 C. Experimental characterizations reveal that LPOF preferentially forms a LiF- and Li3PO4-rich layer that stabilizes the high-voltage cathode/electrolyte interface, which is further supported by theoretical calculations. This work establishes sacrificial-additive engineering as an effective route toward durable high-voltage halide-based ASSBs.
Extending the cycle life of LiCoO2 (LCO) cathodes under elevated cutoff voltages remains a critical challenge for lithium-ion batteries, as accelerated degradation is often governed by reaction heterogeneity and interfacial instability. Herein, we report a composite cathode composed of micron-sized LCO and nanoscale Li...
Jin-Yang Li, He Huang, Hao Guo et al.· Small· 0 citations
The development of solid-state batteries with high safety and energy density is critical for next-generation storage. However, conventional halide electrolytes like Li2ZrCl6 suffer from low room-temperature ionic conductivity. We propose a synergistic Sm3+ and O2− co-doping strategy and synthesize a novel oxychloride L...
Si-Cheng Ou, Zhi-Peng Xia, Ke Wang et al.· RSC Advances· 0 citations
Solid-state sodium metal batteries are promising candidates for grid-scale energy storage due to their inherent safety and low cost. However, the development of solid electrolytes that support high-rate (>20 C) cycling for fast-charging applications remains a major challenge. Herein, we explore how adding SiO2 affects...
An-Qi Zhu, Peng-Tao Qiu, Yan-Qiong Luo et al.· ACS Applied Materials and In...· 0 citations
Lithium cobalt oxide (LCO) cathode materials are widely used in 3C electronic products but suffer from rapid capacity fading at high voltages (>4.2 V). We propose a synergistic LiF/ZrO2 double-coating strategy to construct a flexible-rigid intimately intermingled nano-mosaic artificial interphase on Al-doped LiCoO2 (LC...
Zhi-Rong Chen, Chen Cheng, Shu-Hao Dong et al.· ACS Applied Materials and In...· 0 citations
The propylene carbonate (PC)-based electrolyte system is characterized by a wide liquid range and favorable Li+ migration kinetics, which endows it with excellent low-temperature applicability when paired with hard carbon (HC) anodes in lithium-ion batteries (LIBs). However, the PC-induced SEI structure is loose, which...
Jing-Jiang Yang, Tian-Miao Zhao, Yi-Fan Wang et al.· Langmuir· 1 citation
Li-rich Mn-based layered oxides (LRMOs) are promising high-energy cathodes for all-solid-state batteries (ASSBs), but their application is limited by irreversible O2 evolution during lattice O2−/O22− redox and interfacial degradation at high voltages. Here we report a “coat–sinter–wash” synthetic strategy that simultan...
Jia-Chen Ying, Gao-Hong Liu, Bing-Liang Wang et al.· Science Advances· 0 citations
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