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Dual-site HSAB regulation enabling ion-channel broadening and synergistic enhancement of air stability and lithium compatibility in sulfide solid electrolytes
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DOI：10.1016/j.jechem.2026.04.065.png)
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Abstract
En 中文
Sulfide-based solid electrolytes (SSEs) are promising candidates for all-solid-state lithium batteries owing to their high ionic conductivity and good mechanical compliance, yet their severe air sensitivity and interfacial instability toward lithium metal remain major challenges. Herein, a cation-anion dual-site synergistic regulation strategy guided by hard-soft acid-base (HSAB) theory is proposed. By introducing Bi3+ at cation sites and Br− into the anionic framework, a novel SSE, Li5.46P0.96Bi0.04S4.38Cl1.5Br0.12, is successfully constructed. Dual-site substitution induces anionic disorder, enlarges the lattice volume, and optimizes Li+ migration pathways while preserving the host structure, enabling a high ionic conductivity of 13.6 mS cm−1 at room temperature. Moreover, the formation of stable Bi–S units markedly enhances the air stability of the electrolyte, enabling it to maintain structural integrity for up to 10 h under humid air exposure while effectively suppressing H2S release. Meanwhile, an in-situ formed Li-Bi alloy interphase significantly improves interfacial compatibility with lithium metal, enabling a high critical current density of 1.57 mA cm−2 and long-term stable cycling exceeding 1000 h at 0.2 mA cm−2 in lithium symmetric cells. This work provides an intrinsically chemical and engineering-feasible design paradigm for developing high-performance and air-stable SSEs.
Keywords:
sulfide solid electrolytes
dual-site regulation
ionic conductivity
air stability
lithium compatibility
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