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<p>Compared with Zn<sup>2+</sup>, the current mainly reported charge carrier for zinc hybrid capacitors, small-hydrated-sized and light-weight NH<sub>4</sub><sup>+</sup> is expected as a better one to mediate cathodic interfacial electrochemical behaviors, yet has not been unraveled. Here we propose an NH<sub>4</sub><sup>+</sup>-modulated cationic solvation strategy to optimize cathodic spatial charge distribution and achieve dynamic Zn<sup>2+</sup>/NH<sub>4</sub><sup>+</sup> co-storage for boosting Zinc hybrid capacitors. Owing to the hierarchical cationic solvated structure in hybrid Zn(CF<sub>3</sub>SO<sub>3</sub>)<sub>2</sub>–NH<sub>4</sub>CF<sub>3</sub>SO<sub>3</sub> electrolyte, high-reactive Zn<sup>2+</sup> and small-hydrate-sized NH<sub>4</sub>(H<sub>2</sub>O)<sub>4</sub><sup>+</sup> induce cathodic interfacial Helmholtz plane reconfiguration, thus effectively enhancing the spatial charge density to activate 20% capacity enhancement. Furthermore, cathodic interfacial adsorbed hydrated NH<sub>4</sub><sup>+</sup> ions afford high-kinetics and ultrastable C‧‧‧H (NH<sub>4</sub><sup>+</sup>) charge storage process due to a much lower desolvation energy barrier compared with heavy and rigid Zn(H<sub>2</sub>O)<sub>6</sub><sup>2+</sup> (5.81 vs. 14.90&#xa0;eV). Consequently, physical uptake and multielectron redox of Zn<sup>2+</sup>/NH<sub>4</sub><sup>+</sup> in carbon cathode enable the zinc capacitor to deliver high capacity (240&#xa0;mAh&#xa0;g<sup>−1</sup> at 0.5&#xa0;A&#xa0;g<sup>−1</sup>), large-current tolerance (130&#xa0;mAh&#xa0;g<sup>−1</sup> at 50&#xa0;A&#xa0;g<sup>−1</sup>) and ultralong lifespan (400,000 cycles). This study gives new insights into the design of cathode–electrolyte interfaces toward advanced zinc-based energy storage.</p>

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NH4+-Modulated Cathodic Interfacial Spatial Charge Redistribution for High-Performance Dual-Ion Capacitors

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年1月27日

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  • Yumin Chen,
  • Ziyang Song,
  • Yaokang Lv,
  • Lihua Gan,
  • Mingxian Liu

摘要

Compared with Zn2+, the current mainly reported charge carrier for zinc hybrid capacitors, small-hydrated-sized and light-weight NH4+ is expected as a better one to mediate cathodic interfacial electrochemical behaviors, yet has not been unraveled. Here we propose an NH4+-modulated cationic solvation strategy to optimize cathodic spatial charge distribution and achieve dynamic Zn2+/NH4+ co-storage for boosting Zinc hybrid capacitors. Owing to the hierarchical cationic solvated structure in hybrid Zn(CF3SO3)2–NH4CF3SO3 electrolyte, high-reactive Zn2+ and small-hydrate-sized NH4(H2O)4+ induce cathodic interfacial Helmholtz plane reconfiguration, thus effectively enhancing the spatial charge density to activate 20% capacity enhancement. Furthermore, cathodic interfacial adsorbed hydrated NH4+ ions afford high-kinetics and ultrastable C‧‧‧H (NH4+) charge storage process due to a much lower desolvation energy barrier compared with heavy and rigid Zn(H2O)62+ (5.81 vs. 14.90 eV). Consequently, physical uptake and multielectron redox of Zn2+/NH4+ in carbon cathode enable the zinc capacitor to deliver high capacity (240 mAh g−1 at 0.5 A g−1), large-current tolerance (130 mAh g−1 at 50 A g−1) and ultralong lifespan (400,000 cycles). This study gives new insights into the design of cathode–electrolyte interfaces toward advanced zinc-based energy storage.