High-Voltage Recyclable Organic Cathode Enabled by Heteroatomic Substitution for Aqueous Zinc-Ion Batteries,Advanced Energy Materials

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High-Voltage Recyclable Organic Cathode Enabled by Heteroatomic Substitution for Aqueous Zinc-Ion Batteries
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2024-03-11 , DOI: 10.1002/aenm.202400580
Dawei Du ₁ , Jiyao Zhou ₁ , Zilong Yin ₁ , Guanzheng Feng ₁ , Weixiao Ji ₁ , He Huang ₁ , Siping Pang ₁

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N-type organic compounds present themselves as promising high-capacity cathodes for aqueous Zn-ion batteries. However, a common challenge is their working voltages often falling below 1 V versus Zn²⁺/Zn. To bridge this gap, a high-voltage organic material is first developed, 5,6,11,12-tetraazanaphthacene (TANC), using a heteroatomic substitution strategy. TANC feature a large π-conjugated plane enriched with π−π interactions, which not only enhancing structural stability but also boosting charge transfer kinetics. The TANC cathode is achieved from its dihydro precursor, denoted as 2H-TANC, via a facile in situ activation process within the battery itself. This electrochemical synthesis method is cost-effective and environmentally friendly compared to traditional chemical method. The cathode shows a record-high discharge voltage of 1.15 V (vs Zn²⁺/Zn) among n-type organic materials and maintains cycling stability over 47,500 cycles. Furthermore, spent TANC electrodes can be efficiently recycled via a simple extraction process. The work marks a significant step toward the development of high-voltage, affordable, and recyclable organic electrode materials, steering them to the forefront of future sustainable battery technologies.

中文翻译：

通过杂原子取代水系锌离子电池实现高压可回收有机阴极

N型有机化合物有望成为水性锌离子电池的高容量正极。然而，一个常见的挑战是它们的工作电压通常低于 1 V（相对于 Zn ²⁺ /Zn）。为了弥补这一差距，首先使用杂原子取代策略开发了一种高压有机材料，即 5,6,11,12-四氮杂萘 (TANC)。 TANC 具有富含 π−π 相互作用的大 π 共轭平面，这不仅增强了结构稳定性，还增强了电荷转移动力学。 TANC 阴极是由其二氢前体（表示为 2H-TANC）通过电池本身内的简单原位激活过程实现的。与传统的化学方法相比，这种电化学合成方法具有成本效益且环保。该阴极在n型有机材料中表现出创纪录的1.15 V放电电压（相对于Zn ²⁺ /Zn），并在47,500次循环中保持循环稳定性。此外，用过的 TANC 电极可以通过简单的提取过程进行有效回收。这项工作标志着向开发高电压、经济实惠且可回收的有机电极材料迈出了重要一步，引导它们走向未来可持续电池技术的最前沿。

更新日期：2024-03-11

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