<p>Artificial solid electrolyte interphase offers a promising route to improve the lifespan and safety of quasi-solid-state sodium-metal batteries (QSMBs), yet its limited ion conductivity and the low liquidity of the polymer electrolyte often result in unstable Na plating/stripping kinetics and poor interfacial durability. Herein, we propose a surface-induced “top” Na deposition mechanism facilitated by an ultra-sodiophilic ionic/electronic mixed conductor interphase exhibiting strong Na<sup>+</sup> adsorption affinity, which ensures fast and dendrite-free Na anode operation. The embedded Na<sub>3</sub>Sb alloy phase, featuring high electronic conductivity and strong Na<sup>+</sup> adsorption energy, significantly accelerates interfacial ion diffusion and nucleation kinetics, forming a smooth and compact Na deposition layer that facilitates stable solid electrolyte interphase formation and preserves interfacial integrity. Consequently, Na||Na symmetric cells employing a 1, 3-dioxolane-based gel polymer electrolyte deliver an ultra-long-cycling lifespan of 1000&#xa0;h at 0.5&#xa0;mA&#xa0;cm<sup>−2</sup> with a low overpotential of 40&#xa0;mV. Moreover, QSMBs incorporating the modified Na anode and Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> cathode demonstrate outstanding cycling stability (74.1% capacity retention after 9000 cycles at 2C) and superior rate capability (91.7&#xa0;mAh&#xa0;g<sup>−1</sup> at 5C). The work provides mechanistic insights and practical strategies for regulating Na deposition, paving the way toward high-performance QSMBs.</p><p></p>

错误:搜索内容不能为空,请输入英文关键词
错误:关键词超出字数限制,请精简
高级检索

Ultra-Sodiophilic Mixed Conductor Interphase Enabling Uniform Top Deposition for Quasi-Solid-State Sodium-Metal Batteries

  • Chunching Lu,
  • Guangxiang Zhang,
  • Yuxiang Niu,
  • Yupeng Zhu,
  • Siyuan Li,
  • Hua Huo,
  • Yulin Ma,
  • Pengjian Zuo,
  • Geping Yin,
  • Yunzhi Gao,
  • Liguang Wang,
  • Chuankai Fu,
  • Wei Chen

摘要

Artificial solid electrolyte interphase offers a promising route to improve the lifespan and safety of quasi-solid-state sodium-metal batteries (QSMBs), yet its limited ion conductivity and the low liquidity of the polymer electrolyte often result in unstable Na plating/stripping kinetics and poor interfacial durability. Herein, we propose a surface-induced “top” Na deposition mechanism facilitated by an ultra-sodiophilic ionic/electronic mixed conductor interphase exhibiting strong Na+ adsorption affinity, which ensures fast and dendrite-free Na anode operation. The embedded Na3Sb alloy phase, featuring high electronic conductivity and strong Na+ adsorption energy, significantly accelerates interfacial ion diffusion and nucleation kinetics, forming a smooth and compact Na deposition layer that facilitates stable solid electrolyte interphase formation and preserves interfacial integrity. Consequently, Na||Na symmetric cells employing a 1, 3-dioxolane-based gel polymer electrolyte deliver an ultra-long-cycling lifespan of 1000 h at 0.5 mA cm−2 with a low overpotential of 40 mV. Moreover, QSMBs incorporating the modified Na anode and Na3V2(PO4)3 cathode demonstrate outstanding cycling stability (74.1% capacity retention after 9000 cycles at 2C) and superior rate capability (91.7 mAh g−1 at 5C). The work provides mechanistic insights and practical strategies for regulating Na deposition, paving the way toward high-performance QSMBs.