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<p>Li<sub>1.3</sub>Al<sub>0.3</sub>Ti<sub>1.7</sub>(PO<sub>4</sub>)<sub>3</sub> (LATP) is a promising solid-state electrolyte for all-solid-state lithium batteries due to its high ionic conductivity and cost advantage. However, its practical application is hindered by poor interfacial compatibility with lithium metal and lithium dendrite penetration. In this study, a distinct interfacial engineering strategy that differs from conventional polymer coatings was developed by constructing an in-situ gelled hydroxypropyl methylcellulose layer on LATP electrolyte membranes. Unlike previously reported polyvinylidene fluoride or inorganic modifications, the hydroxypropyl methylcellulose layer underwent gelation with liquid electrolyte to form a dual-functional gel interface. This unique architecture not only provided a physical barrier against side reactions and dendrite growth but also established low-energy-barrier pathways for lithium ion transport. Consequently, the interfacial resistance dramatically decreased from 780 Ω to 160 Ω, the electrochemical window expanded from 3.74&#xa0;V to 4.62&#xa0;V, and symmetric cells achieved over 1000&#xa0;h of stable cycling. When paired with lithium iron phosphate cathodes, full cells retained 95% capacity after 100 cycles. This work presents a new paradigm for polymer/inorganic composite electrolyte interface engineering, advancing the development of high-safety solid-state batteries.</p> Graphical Abstract <p></p>

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Interfacial engineering of Li1.3Al0.3Ti1.7(PO4)3-based solid electrolyte membranes via hydroxypropyl methylcellulose modification

  • 期刊论文

  • 发表日期：

    2026年5月3日

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  • Changyu Li,
  • Yuanhua Lin,
  • Yun Huang,
  • Qiang Zeng,
  • Xing Li,
  • Wanying Liu

摘要

Li1.3Al0.3Ti1.7(PO4)3 (LATP) is a promising solid-state electrolyte for all-solid-state lithium batteries due to its high ionic conductivity and cost advantage. However, its practical application is hindered by poor interfacial compatibility with lithium metal and lithium dendrite penetration. In this study, a distinct interfacial engineering strategy that differs from conventional polymer coatings was developed by constructing an in-situ gelled hydroxypropyl methylcellulose layer on LATP electrolyte membranes. Unlike previously reported polyvinylidene fluoride or inorganic modifications, the hydroxypropyl methylcellulose layer underwent gelation with liquid electrolyte to form a dual-functional gel interface. This unique architecture not only provided a physical barrier against side reactions and dendrite growth but also established low-energy-barrier pathways for lithium ion transport. Consequently, the interfacial resistance dramatically decreased from 780 Ω to 160 Ω, the electrochemical window expanded from 3.74 V to 4.62 V, and symmetric cells achieved over 1000 h of stable cycling. When paired with lithium iron phosphate cathodes, full cells retained 95% capacity after 100 cycles. This work presents a new paradigm for polymer/inorganic composite electrolyte interface engineering, advancing the development of high-safety solid-state batteries.

Graphical Abstract