Zhang Ruolan, Hong Chengkai, Yu Chunyang, Zhou Yongfeng
State Key Laboratory of Synergistic Chem-Bio Synthesis, School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, China.
Chemistry. 2025 May 22;31(29):e202500763. doi: 10.1002/chem.202500763. Epub 2025 Apr 24.
Aqueous Zn-iodine (Zn-I) batteries are considered to be potential energy storage systems due to their safety, environmental friendliness, and cost-effectiveness. However, the shuttle effect of polyiodide leads to cathode active mass loss and anode Zn corrosion, which greatly reduces the cycle life of Zn-I batteries. Herein, we report an N-modified alternating copolymer nanoflower composite (NH-NFs-PDA) as a new type of iodine host candidate to effectively inhibit the polyiodide shuttle effect in Zn-I battery. As a result, the NH-NFs-PDA/I-based Zn-I battery demonstrates a high specific capacity of 185.42 mAh g at 1 A g, with a coulombic efficiency of 99%. Moreover, it exhibits excellent cycling stability, achieving 10,000 cycles at 10 A g with an average capacity decay rate of only 0.0008% per cycle, ranking it among the best-performing polymeric host-based Zn-I₂ batteries in the literature. Density functional theory (DFT) and in-situ ultraviolet-visible (UV-Vis) measurements illustrate the impressive suppression of polyiodide shuttle effect comes from the strong interaction between N-modification enhanced polyhydroxy sites in NH-NFs-PDA and polyiodide. This work may shed new light on the design of advanced polymeric iodine hosts in Zn-I₂ batteries.
水系锌碘(Zn-I)电池因其安全性、环境友好性和成本效益而被认为是潜在的储能系统。然而,多碘化物的穿梭效应导致正极活性物质损失和负极锌腐蚀,这大大降低了Zn-I电池的循环寿命。在此,我们报道了一种N修饰的交替共聚物纳米花复合材料(NH-NFs-PDA)作为一种新型碘宿主候选物,可有效抑制Zn-I电池中的多碘化物穿梭效应。结果,基于NH-NFs-PDA/I的Zn-I电池在1 A g下表现出185.42 mAh g的高比容量,库仑效率为99%。此外,它还表现出优异的循环稳定性,在10 A g下实现了10000次循环,平均容量衰减率仅为每循环0.0008%,在文献中基于聚合物宿主的最佳性能Zn-I₂电池中名列前茅。密度泛函理论(DFT)和原位紫外可见(UV-Vis)测量表明,对多碘化物穿梭效应的显著抑制来自NH-NFs-PDA中N修饰增强的多羟基位点与多碘化物之间的强相互作用。这项工作可能为Zn-I₂电池中先进聚合物碘宿主的设计提供新的思路。