2025-8-19：祝贺团队固态电池研究论文在Materials Today (IF 22)发表！
发布时间：2025-08-18
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Unravelling the stablization effect of flourination on the interface and bulk phase of electrodes in all-solid-state lithium metal batteries
Ziling Jiang1, 3, Siwu Li2, Jie Yang1,3, Miao Deng1,3, Ziyu Lu1, 3, Zhenyu Wang4, Lin Li1,3, Feixiang Wu5,*, Chuang Yu1, 2, 3, *
Chlorine-rich argyrodite Li5.5PS4.5Cl1.5 (LPSCl) solid electrolyte exhibits exceptionally high Li-ion conductivity and is considered a highly promising candidate for all-solid-state lithium metal batteries (ASSLMBs). However, the compatibility issue with both the ultra-high-nickel cathode LiNi0.9Mn0.05Co0.05O2 (NCM955) and lithium metal anode remains a significant challenge. In this work, we propose a ![]()
customized fluorination regulation strategy and systematically investigate the cross-scale mechanisms of fluorine in ASSLMBs. On the cathode side, it is discovered for the first time that, a LiF-doped electrolyte, Li5.5PS4.5Cl1.4F0.1 (LPSClF0.1), enables the penetration of F⁻ into the single-crystal NCM955 during cycling. These F⁻ partially substitute O2- in the lattice, modulating the local electronic structure and forming strong covalent Ni–F bonds. This effectively increases the migration barrier for Ni2+, suppresses lattice oxygen activation, and reduces irreversible oxygen release, thereby enhancing the structural stability of the NCM955 cathode. On the anode side, LiF doping increases the critical current density of the electrolyte from 0.6 mA cm-2 to 3.1 mA cm-2. Furthermore, when paired with a molten SnF2-treated lithium metal—a fluorine-rich composite SEI composed of LiF, LiCl, and Li-Sn alloy can be obtained. This layer facilitates fast Li⁺ transport and homogenizes the electric field distribution, thereby balancing the local current density, regulating the nucleation and growth of Li, ultimately inhibiting the dendrite growth and ensuring highly reversible Li plating/stripping. Benefitting from the multilevel regulation of “atomic doping-bulk phase stabilization-interfacial engineering”, the assembled NCM955/LPSClF0.1/Li@SnF2 battery demonstrates a capacity retention of 80.6% after 250 cycles at 0.5C (25°C), and exhibits excellent performance at both –20°C (0.1C) and 60°C (0.5C). This work not only uncovers the synergistic roles of fluorination across atomic (bonding interactions), mesoscale (interfacial architecture), and macroscopic (battery performance) dimensions, but also establishes a universal design paradigm for bulk-interface synergy in wide-temperature-range, high–energy-density ASSLMBs.
