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<p>The design of solid electrolyte interphases (SEIs) for poly(vinylidene fluoride)-based solid-state batteries has largely focused on solvent-affinity of Li<sup>+</sup> to generate robust but ionically sluggish LiF-rich layers, inherently compromising transport kinetics. Here, we establish a paradigm based on quantifiable physicochemical descriptors (ionic potential and donor number) to guide the design of amphitropic ion pairs (AIPs). These AIPs are engineered to simultaneously tailor both the solvent-affinity and anion-affinity of Li<sup>+</sup>: a solventphilic cation with high ionic potential (Al<sup>3+</sup>) first sequesters reactive solvents, clearing the path for a high-donor-number, lithium-philic anion (NO<sub>3</sub><sup>−</sup>) to remodel solvation. This rationally guided, sequential mechanism enables the <i>in situ</i> synthesis of a LiF/Li<sub>3</sub>N heterostructured SEI, where dendrite-suppressing LiF domains are seamlessly integrated with ultra-fast Li<sub>3</sub>N ion channels. This design heterogeneity effectively enhances stability and kinetics, yielding a robust and highly conductive interface. Consequently, Li∣Li cells achieve &gt;2000 h of stable cycling, and Li∣LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> full cells surpass 600 cycles.</p>

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Amphitropic ion pairs induce a heterostructured solid electrolyte interphase in solid-state lithium batteries

  • 期刊论文

  • 发表日期：

    2026年5月12日

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  • Wangkaichen Du,
  • Ziyu Lou,
  • Shuoyi Chen,
  • Xunjie Yin,
  • Sijia Chi,
  • Xuerui Yi,
  • Li Wang,
  • Shichao Wu,
  • Quan-Hong Yang

摘要

The design of solid electrolyte interphases (SEIs) for poly(vinylidene fluoride)-based solid-state batteries has largely focused on solvent-affinity of Li+ to generate robust but ionically sluggish LiF-rich layers, inherently compromising transport kinetics. Here, we establish a paradigm based on quantifiable physicochemical descriptors (ionic potential and donor number) to guide the design of amphitropic ion pairs (AIPs). These AIPs are engineered to simultaneously tailor both the solvent-affinity and anion-affinity of Li+: a solventphilic cation with high ionic potential (Al3+) first sequesters reactive solvents, clearing the path for a high-donor-number, lithium-philic anion (NO3−) to remodel solvation. This rationally guided, sequential mechanism enables the in situ synthesis of a LiF/Li3N heterostructured SEI, where dendrite-suppressing LiF domains are seamlessly integrated with ultra-fast Li3N ion channels. This design heterogeneity effectively enhances stability and kinetics, yielding a robust and highly conductive interface. Consequently, Li∣Li cells achieve >2000 h of stable cycling, and Li∣LiNi0.8Co0.1Mn0.1O2 full cells surpass 600 cycles.