<p>The coupling of fast redox kinetics, high-energy density, and prolonged lifespan is a permanent aspiration for aqueous rechargeable zinc batteries, but which has been severely hampered by a narrow voltage range and suboptimal compatibility between the electrolytes and electrodes. Here, we unprecedentedly introduced an electric ambipolar effect for synergistic manipulation on Zn<sup>2+</sup> ternary-hydrated eutectic electrolyte (ZTE) enabling high-performance Zn-Br<sub>2</sub> batteries. The electric ambipolar effect motivates strong dipole interactions among hydrated perchlorates and bipolar ligands of L-carnitine (L-CN) and sulfamide, which reorganized primary cations solvation sheath in a manner of forming Zn[(L-CN)(SA)(H<sub>2</sub>O)<sub>4</sub>]<sup>2+</sup> configuration and dynamically restricting desolvated H<sub>2</sub>O molecules, thus ensuring a broadened electrochemical window of 2.9&#xa0;V coupled with high ionic conductivity. Noticeably, L-CN affords an electrostatic shielding effect and an <i>in situ</i> construction of organic–inorganic interphase, endowing oriented Zn anode plating/stripping reversibly for over 2400&#xa0;h. Therefore, with the synergy of electro/nucleophilicity and exceptional compatibility, the ZTE electrolyte dynamically boosts the conversion redox of Zn-Br<sub>2</sub> batteries in terms of high specific capacity and stable cycling performance. These findings open a window for designing electrolytes with synergetic chemical stability and compatibility toward advanced zinc-ion batteries.</p>

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Integrating Electric Ambipolar Effect for High-Performance Zinc Bromide Batteries

  • Wenda Li,
  • Hengyue Xu,
  • Shanzhe Ke,
  • Hongyi Zhang,
  • Hao Chen,
  • Gaijuan Guo,
  • Xuanyi Xiong,
  • Shiyao Zhang,
  • Jianwei Fu,
  • Chengbin Jing,
  • Jiangong Cheng,
  • Shaohua Liu

摘要

The coupling of fast redox kinetics, high-energy density, and prolonged lifespan is a permanent aspiration for aqueous rechargeable zinc batteries, but which has been severely hampered by a narrow voltage range and suboptimal compatibility between the electrolytes and electrodes. Here, we unprecedentedly introduced an electric ambipolar effect for synergistic manipulation on Zn2+ ternary-hydrated eutectic electrolyte (ZTE) enabling high-performance Zn-Br2 batteries. The electric ambipolar effect motivates strong dipole interactions among hydrated perchlorates and bipolar ligands of L-carnitine (L-CN) and sulfamide, which reorganized primary cations solvation sheath in a manner of forming Zn[(L-CN)(SA)(H2O)4]2+ configuration and dynamically restricting desolvated H2O molecules, thus ensuring a broadened electrochemical window of 2.9 V coupled with high ionic conductivity. Noticeably, L-CN affords an electrostatic shielding effect and an in situ construction of organic–inorganic interphase, endowing oriented Zn anode plating/stripping reversibly for over 2400 h. Therefore, with the synergy of electro/nucleophilicity and exceptional compatibility, the ZTE electrolyte dynamically boosts the conversion redox of Zn-Br2 batteries in terms of high specific capacity and stable cycling performance. These findings open a window for designing electrolytes with synergetic chemical stability and compatibility toward advanced zinc-ion batteries.