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<p>High-voltage quasi-solid-state lithium metal batteries are considered a promising system for realizing high-energy–density energy storage. However, their development is significantly constrained by the interfacial incompatibility between quasi-solid electrolytes and electrode materials, specifically high-voltage cathodes and lithium metal anodes. Herein, a gradient quasi-solid polymer electrolyte (GQSPE) based on poly(1,3-dioxolane) (PDOL) was constructed by confining the high-voltage-stable additive succinonitrile (SN) to the cathode-facing side, enriching the lithium-metal-compatible additive 1,2-dimethoxyethane (DME) in the anode-facing side and forming a transition zone with an additive gradient distribution that facilitates continuous Li<sup>+</sup> conduction. The resulting GQSPE shows an ionic conductivity of 1.70 × 10<sup>−4</sup> S cm<sup>−1</sup> and a high Li<sup>+</sup> transference number of 0.63. Notably, atypical hydrogen bonding (N≡C–C–H···O–C) between SN and PDOL significantly expands the electrochemical window to 5.2&#xa0;V (vs. Li⁺/Li), enabling effective compatibility with the high-voltage LiNi<sub>0.33</sub>Mn<sub>0.33</sub>Co<sub>0.33</sub>O<sub>2</sub> (NCM111) cathodes. On the lithium anode side, the enriched DME in GQSPE facilitates a stable, inorganic-rich solid electrolyte interphase (SEI). Through this design, GQSPE achieves its interfacial compatibility with both high-voltage cathodes and lithium metal anodes. Consequently, Li|GQSPE@CE|NCM111 cells retain 63.4% of their capacity after 340 cycles in a high-voltage range of 3.0–4.3&#xa0;V. The gradient electrolyte design strategy provides a choice for advancing high-energy-density quasi-solid-state lithium metal batteries.</p>

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Gradient quasi-solid polymer electrolyte improves interfacial compatibility in high-voltage lithium metal batteries

  • 期刊论文

  • 发表日期：

    2026年5月9日

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  • Hongbing Lu,
  • Yanan Zhang,
  • Yating Zhang,
  • Weiteng Lin,
  • Xuan Li,
  • Kemeng Ji,
  • Mingming Chen

摘要

High-voltage quasi-solid-state lithium metal batteries are considered a promising system for realizing high-energy–density energy storage. However, their development is significantly constrained by the interfacial incompatibility between quasi-solid electrolytes and electrode materials, specifically high-voltage cathodes and lithium metal anodes. Herein, a gradient quasi-solid polymer electrolyte (GQSPE) based on poly(1,3-dioxolane) (PDOL) was constructed by confining the high-voltage-stable additive succinonitrile (SN) to the cathode-facing side, enriching the lithium-metal-compatible additive 1,2-dimethoxyethane (DME) in the anode-facing side and forming a transition zone with an additive gradient distribution that facilitates continuous Li+ conduction. The resulting GQSPE shows an ionic conductivity of 1.70 × 10−4 S cm−1 and a high Li+ transference number of 0.63. Notably, atypical hydrogen bonding (N≡C–C–H···O–C) between SN and PDOL significantly expands the electrochemical window to 5.2 V (vs. Li⁺/Li), enabling effective compatibility with the high-voltage LiNi0.33Mn0.33Co0.33O2 (NCM111) cathodes. On the lithium anode side, the enriched DME in GQSPE facilitates a stable, inorganic-rich solid electrolyte interphase (SEI). Through this design, GQSPE achieves its interfacial compatibility with both high-voltage cathodes and lithium metal anodes. Consequently, Li|GQSPE@CE|NCM111 cells retain 63.4% of their capacity after 340 cycles in a high-voltage range of 3.0–4.3 V. The gradient electrolyte design strategy provides a choice for advancing high-energy-density quasi-solid-state lithium metal batteries.