近日，郑州大学郭玮团队报道了分子内N···I卤素键抑制溶解实现高负载有机锌电池。2025年8月18日出版的《美国化学会志》发表了这项成果。

水基锌离子电池的发展面临着长期的挑战，即如何协调高质量负载能力和极端耐受性，特别是对于容易在水基电解质中溶解的有机阴极。

研究组提出了一种卤素键偶氮基阴极材料，4,4 '' -偶氮吡啶碘化（AZPY-I），通过碘介导的吡啶氮位点的分子稳定进行工程设计。分析表明，AZPY-I采用由定向N··I卤素键稳定的robthemt π -π共轭框架，在水中具有超低溶解度（<0.5 mg mL^-1），同时引入具有六电子转移能力的双氧化还原活性位点（N = N和I₂基团）。

AZPY-I电池在0.5 A g^-1时的高质量负载为22.8 mg cm^-2，提供接近理论的202 mAh g^-1容量，在150次循环中保持92%的容量。在超高电流密度（8 A g^-1, ~34.5 C）下，电池表现出优异的可循环性，可进行15万次循环，每次循环容量衰减0.00032%。这项工作建立了卤素键合分子工程作为设计耐溶解有机电极的通用范例，将分子晶体学与实际电池指标联系起来。

附：英文原文

Title: Dissolution Inhibition via Intramolecular N···I Halogen Bond Enables High-Loading Zn-Organic Battery

Author: Peng Yang, Jiahao Guo, Silong Lin, Yongzhu Fu, Wei Guo

Issue&Volume: August 18, 2025

Abstract: The development of aqueous zinc-ion batteries faces persistent challenges in reconciling high mass-loading capabilities with extreme tolerance, particularly for organic cathodes prone to dissolution in aqueous electrolyte. Here, we present a halogen-bonded azo-based cathode material, 4,4′-azopyridine-iodide (AZPY-I), engineered through iodine-mediated molecular stabilization of pyridinic nitrogen sites. Analyses reveal that AZPY-I adopts a robust π–π conjugated framework stabilized by directional N···I halogen bonds, achieving ultralow solubility (<0.5 mg mL–1 in H2O) while introducing dual redox-active sites with six-electron transfer capability (N═N and I2 moieties). The Zn||AZPY-I cell delivers a near-theoretical capacity of 202 mAh g–1 with a high mass loading of 22.8 mg cm–2 at 0.5 A g–1, sustaining a 92% capacity retention over 150 cycles. At an ultrahigh current density (8 A g–1, ～34.5 C), the cell demonstrates exceptional cyclability for 150,000 cycles with 0.00032% capacity decay per cycle. This work establishes halogen-bonded molecular engineering as a universal paradigm for designing dissolution-resistant organic electrodes, bridging molecular crystallography with practical battery metrics.

DOI: 10.1021/jacs.5c07277

Source: https://pubs.acs.org/doi/abs/10.1021/jacs.5c07277