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Five-Volt-Class High-Capacity All-Solid-State Lithium Batteries Strategy and performance: Achieved >5 V operability and ultrahigh areal capacity (35.3 mAh cm−2) in ASSBs using a fluoride solid electrolyte, LiCl–4LTF, with high Li+ conductivity (1.7 × 10−5 S cm−1). Mechanistic insight: Synchrotron X-ray analyses and theory reveal that the >100x Li+ conductivity enhancement over Li2TiF6 arises from increased Li+ concentration and interfacial Cl substitution, predominantly at surface/interface regions. Interfacial stability: As a 5 V–stable shielding layer, LiCl–4LTF enables excellent rate and cycling performance of spinel cathodes (e.g., 106 mAh g−1 at 2C with 75.2% retention after 200 cycles), outperforming unstable LNbO coatings.
Arrhenius plots of Li+ conductivities and crystal structures of Li2TiF6 with TiF6
Electrochemical stability windows
Versatility: Effectiveness is validated across high-voltage spinels (LNMO, LCMO, LFMO), low-voltage extended operation (258 mAh g−1), and pouch-type full cells.
Comparison of cycling performance with LNMO electrodes in ASSBs
By combining exceptional >5 V oxidative stability with fast Li+ transport, LiCl–4LTF enables record-high areal capacity and stable high-voltage operation across multiple ASSB architectures, establishing a broadly applicable interfacial design paradigm.
Source: Son et al., Nature Energy, 2025
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