<p>Deep fast-charging capability has become the core pursuit for practical applications of aqueous zinc metal batteries, yet it is critically impeded by unfavorable interfacial field evolution at the electrode/electrolyte interface under high-current–density conditions. The coexistence of sluggish Zn<sup>2+</sup> desolvation, competitive H<sub>2</sub>O reduction corrosion, uneven electric field, and concentration field collectively leads to poor rate performance. To tackle these issues, a bolstered interfacial field chemistry strategy was developed via sulfosuccinic acid to precisely regulate the physicochemical and electrochemical properties within the inner Helmholtz plane. The tuned interfacial field comprises a homogeneous distribution of interfacial ions and electric fields, promoting fast desolvation and interfacial electron transfer. Consequently, the modified Zn||Cu asymmetric cells deliver an outstanding average Coulombic efficiency of 99.48% over 1600 cycles at 2&#xa0;mA&#xa0;cm<sup>−2</sup> and 1&#xa0;mAh&#xa0;cm<sup>−2</sup>. Furthermore, the modified Zn||Zn symmetric cells demonstrate exceptional stability under challenging conditions of 5&#xa0;mA&#xa0;cm<sup>−2</sup>, 2&#xa0;mAh&#xa0;cm<sup>−2</sup> (over 1600&#xa0;h), and 10&#xa0;mA&#xa0;cm<sup>−2</sup>, 10&#xa0;mAh&#xa0;cm<sup>−2</sup> (over 675&#xa0;h, depth of discharge = 17.08%). Impressively, a substantial cumulative capacity of 3500&#xa0;mAh&#xa0;cm<sup>−2</sup> is attained at 10&#xa0;mAh&#xa0;cm<sup>−2</sup> and a 56.93% Zn utilization rate. Besides, the enhanced Zn (10&#xa0;µm) ||I<sub>2</sub> (10.87&#xa0;mg&#xa0;cm<sup>−2</sup>) full cell sustains over 1490 cycles at 1&#xa0;A&#xa0;g<sup>−1</sup> with 77.13% capacity retention and a harsh N/P ratio of 2.31. Remarkably, the Zn (10&#xa0;µm) ||I<sub>2</sub> pouch cell achieves over 680 cycles with an ultralow N/P ratio of 2.04.</p>

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Bolstered Interfacial Field Chemistry for Deep Fast-Charging Aqueous Zinc Metal Batteries

  • Minxi Sun,
  • Yining Chen,
  • Congge Lu,
  • Jingkang Ma,
  • Qiuyuan Feng,
  • Shaoxing Li,
  • Tao Zhang,
  • Shuang Zhou,
  • Anqiang Pan

摘要

Deep fast-charging capability has become the core pursuit for practical applications of aqueous zinc metal batteries, yet it is critically impeded by unfavorable interfacial field evolution at the electrode/electrolyte interface under high-current–density conditions. The coexistence of sluggish Zn2+ desolvation, competitive H2O reduction corrosion, uneven electric field, and concentration field collectively leads to poor rate performance. To tackle these issues, a bolstered interfacial field chemistry strategy was developed via sulfosuccinic acid to precisely regulate the physicochemical and electrochemical properties within the inner Helmholtz plane. The tuned interfacial field comprises a homogeneous distribution of interfacial ions and electric fields, promoting fast desolvation and interfacial electron transfer. Consequently, the modified Zn||Cu asymmetric cells deliver an outstanding average Coulombic efficiency of 99.48% over 1600 cycles at 2 mA cm−2 and 1 mAh cm−2. Furthermore, the modified Zn||Zn symmetric cells demonstrate exceptional stability under challenging conditions of 5 mA cm−2, 2 mAh cm−2 (over 1600 h), and 10 mA cm−2, 10 mAh cm−2 (over 675 h, depth of discharge = 17.08%). Impressively, a substantial cumulative capacity of 3500 mAh cm−2 is attained at 10 mAh cm−2 and a 56.93% Zn utilization rate. Besides, the enhanced Zn (10 µm) ||I2 (10.87 mg cm−2) full cell sustains over 1490 cycles at 1 A g−1 with 77.13% capacity retention and a harsh N/P ratio of 2.31. Remarkably, the Zn (10 µm) ||I2 pouch cell achieves over 680 cycles with an ultralow N/P ratio of 2.04.