Hydrogen‐Bond Network‐Mediated Solvation Engineering Enables Synchronous Optimization of Zinc Anodes Kinetics and Iodine Cathodes Redox

Advanced Functional Materials, vol. 35

Abstract

Abstract The stability and durability of Zn anodes are compromised by the synergistic effects of H 2 O‐mediated side reactions, unstable interfacial charge transfer, electrolyte decomposition, and dendrite formation induced by the space‐charge layer. To overcome these challenges, a polypeptide additive, fish scale protein (FSP), with diverse surface morphology, is introduced to strengthen the stability of Zn anodes through multilevel regulation. Comprehensive studies integrating structural characterizations, first‐principles calculations, and molecular dynamics simulations reveal that this strategy reconstructs the hydrogen‐bond (HB) network within the electrolyte, thereby reducing the activity of free H 2 O, enhancing thermodynamic stability, and accelerating charge‐transfer kinetics in Zn anodes. Moreover, the modified electrolyte suppresses the Grotthuss proton conduction mechanism, significantly impeding proton transport to the Zn surface and attenuating the kinetics of the HER. Therefore, the Zn anodes exhibit excellent cycling stability (4200 h). Furthermore, the Zn||CPC ZHSCs with FSP demonstrate stable cycling over 35 000 cycles. Additionally, the interaction between FSP and polyiodide eliminates the shuttle effect of polyiodides, enabling Zn─I 2 batteries with exceptional cycling stability under high‐load conditions (8.4 mg I 2 loading, 4000 stable cycles). This coordinates a multi‐level control strategy, which provides a promising strategy for developing highly stable Zn anodes, ZHSCs, and Zn─I 2 batteries.

Authors 10

1. Tianlong Wu

   Xinjiang University

   Affiliation as printed

   State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

   College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China

2. Murong Xi

   Xinjiang University

   Affiliation as printed

   State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

   College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China

3. Yudai Huang corresponding

   Xinjiang University

   Affiliation as printed

   State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

   College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China

4. Xiaoxuan Chen corresponding

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH Institute of Energy Technologies IET‐1‐Fundamental Electrochemistry 52425 Jülich Germany

5. Yasin Emre Durmus

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH Institute of Energy Technologies IET‐1‐Fundamental Electrochemistry 52425 Jülich Germany

6. Han Zhang

   Xinjiang University

   Affiliation as printed

   State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

   College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China

7. Juan Ding

   Xinjiang University

   Affiliation as printed

   State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

   College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China

8. Hermann Tempel

   Forschungszentrum Jülich

   Affiliation as printed

   Forschungszentrum Jülich GmbH Institute of Energy Technologies IET‐1‐Fundamental Electrochemistry 52425 Jülich Germany

9. Rüdiger‐A. Eichel Aachen

   Forschungszentrum Jülich · Jülich Aachen Research Alliance · RWTH Aachen University

   Affiliation as printed

   Forschungszentrum Jülich GmbH Institute of Energy Technologies IET‐1‐Fundamental Electrochemistry 52425 Jülich Germany

   Jülich‐Aachen Research Alliance Section JARA‐Energy 52425 Jülich Germany

   RWTH Aachen University Institute of Physical Chemistry Landoltweg 2 52074 Aachen Germany

   Forschungszentrum Jülich GmbH Institute of Energy Technologies IET‐1‐Fundamental Electrochemistry 52425 Jülich Germany

10. Zhouliang Tan corresponding

    Xinjiang University

    Affiliation as printed

    State Key Laboratory of Chemistry and Utilization of Carbon Based Energy Resources; College of Chemistry Xinjiang University Urumqi Xinjiang 830017 P. R. China

    College of Chemistry, Xinjiang University, Urumqi, Xinjiang, 830017 P. R. China