<p>Na<sub>3</sub>SbS<sub>4</sub> has currently emerged as a promising candidate for solid-state electrolytes (SSEs) owing to its high air stability, excellent room-temperature ionic conductivity and broad electrochemical stability window. Nevertheless, due to the sodium dendrites growth, its practical application is still limited. Herein, an electrostatic shielding strategy is proposed to shield the initial dendrite growth tips from subsequent dendrite propagation via LiCl doping. Systematic investigation of a series of Na<sub>3</sub>SbS<sub>4</sub>-xLiCl (<i>x</i> = 0.5, 1, 1.5, 2) SSEs reveals that the Li⁺/Cl⁻ co-doping could enhance the dendrite suppression capability, which might originate from the localized electric field at interface between metallic Na anode and Na<sub>3</sub>SbS<sub>4</sub> SSEs. This localized electric field could facilitate uniform Na⁺ flux distribution through space-charge-mediated ion redistribution, which could effectively suppress uneven current that leads to sodium dendrite growth. The Na<sub>3</sub>SbS<sub>4</sub>-0.5LiCl retains its crystal phase after doping while its CCD was enhanced to 1.89&#xa0;mA&#xa0;cm<sup>−2</sup>. Meanwhile, the Na|Na<sub>3</sub>SbS<sub>4</sub>-0.5LiCl|FeS<sub>2</sub> full cells exhibit a capacity of 81&#xa0;mAh&#xa0;g<sup>−1</sup> and a Coulombic efficiency of 90% at 20th cycles. This electrostatic shielding strategy establishes fundamental criteria for mitigating dendrite propagation in chalcogenide SSEs through interfacial charge redistribution and ion transport kinetics optimization, thereby advancing the engineering roadmap for high-power-density ASSBs.</p>

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Enhancing sodium dendrite suppression capability of Na3SbS4 solid-state electrolyte via electrostatic shielding by LiCl doping

  • Lanlan Xing,
  • Chengwei Gao,
  • Linling Tan,
  • Shiliang Kang,
  • Qing Jiao,
  • Changgui Lin

摘要

Na3SbS4 has currently emerged as a promising candidate for solid-state electrolytes (SSEs) owing to its high air stability, excellent room-temperature ionic conductivity and broad electrochemical stability window. Nevertheless, due to the sodium dendrites growth, its practical application is still limited. Herein, an electrostatic shielding strategy is proposed to shield the initial dendrite growth tips from subsequent dendrite propagation via LiCl doping. Systematic investigation of a series of Na3SbS4-xLiCl (x = 0.5, 1, 1.5, 2) SSEs reveals that the Li⁺/Cl⁻ co-doping could enhance the dendrite suppression capability, which might originate from the localized electric field at interface between metallic Na anode and Na3SbS4 SSEs. This localized electric field could facilitate uniform Na⁺ flux distribution through space-charge-mediated ion redistribution, which could effectively suppress uneven current that leads to sodium dendrite growth. The Na3SbS4-0.5LiCl retains its crystal phase after doping while its CCD was enhanced to 1.89 mA cm−2. Meanwhile, the Na|Na3SbS4-0.5LiCl|FeS2 full cells exhibit a capacity of 81 mAh g−1 and a Coulombic efficiency of 90% at 20th cycles. This electrostatic shielding strategy establishes fundamental criteria for mitigating dendrite propagation in chalcogenide SSEs through interfacial charge redistribution and ion transport kinetics optimization, thereby advancing the engineering roadmap for high-power-density ASSBs.