Wei Mingfeng, Duan Fengxue, Li Bao, Wang Yizhan, Wu Lixin
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun 130012, People's Republic of China.
Key Laboratory of Physics and Technology for Advanced Batteries (Ministry of Education), College of Physics, Jilin University, Changchun 130012, People's Republic of China.
Nano Lett. 2024 Apr 10;24(14):4124-4131. doi: 10.1021/acs.nanolett.3c05034. Epub 2024 Mar 14.
Dynamic reversible noncovalent interactions make supramolecular framework (SF) structures flexible and designable. A three-dimensional (3D) growth of such frameworks is beneficial to improve the structure stability while maintaining unique properties. Here, through the ionic interaction of the polyoxometalate cluster, coordination of zinc ions with cationic terpyridine, and hydrogen bonding of grafted carboxyl groups, the construction of a 3D SF at a well-crystallized state is realized. The framework can grow in situ on the Zn surface, further extending laterally into a full covering without defects. Relying on the dissolution and the postcoordination effects, the 3D SF layer is used as an artificial solid electrolyte interphase to improve the Zn-anode performance. The uniformly distributed clusters within nanosized pores create a negatively charged nanochannel, accelerating zinc ion transfer and homogenizing zinc deposition. The 3D SF/Zn symmetric cells demonstrate high stability for over 3000 h at a current density of 5 mA cm.
动态可逆的非共价相互作用使超分子框架（SF）结构具有灵活性和可设计性。这种框架的三维（3D）生长有利于在保持独特性能的同时提高结构稳定性。在此，通过多金属氧酸盐簇的离子相互作用、锌离子与阳离子三联吡啶的配位以及接枝羧基的氢键作用，实现了处于良好结晶状态的三维SF的构建。该框架可在锌表面原位生长，进一步横向扩展形成无缺陷的全覆盖层。依靠溶解和后配位效应，三维SF层被用作人工固体电解质界面以改善锌阳极性能。纳米孔内均匀分布的簇形成带负电荷的纳米通道，加速锌离子转移并使锌沉积均匀化。三维SF/锌对称电池在5 mA cm的电流密度下表现出超过3000小时的高稳定性。
