Yang Jun, Zhao Xinran, Peng Jinyang, Yang Jiachen, Shi Minjie, Zhang Liqiu, Yan Chao
School of Materials Science and Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, Jiangsu, PR China.
College of Biological, Chemical Sciences and Engineering, Jiaxing University, Jiaxing 314001, Zhejiang, PR China.
J Colloid Interface Sci. 2025 Dec 15;700(Pt 1):138339. doi: 10.1016/j.jcis.2025.138339. Epub 2025 Jul 2.
Redox-active organic compounds with tailored conjugated architectures have gained prominence as pivotal electrode materials in aqueous batteries, owing to their unique ion (de)intercalation mechanisms that avoid crystalline lattice distortion during redox processes. Despite their potential, organic materials are hindered by limitations including inadequate active site density and structural degradation due to electrolyte dissolution during electrochemical cycling. Addressing these limitations, we develop an innovative electron-delocalized organic molecule, designated as PTAQ, which incorporates a π-conjugated imidazole-linked framework with extensive electron delocalization and a reduced band gap, which is favorable for electron transfer. Additionally, a new redox active group (CN) was added, and the amount of CO was increased, thereby enhancing ion embedding capability, as validated by in-situ analyses and theoretical calculations. As electrode for aqueous ammonium-ion batteries (AAIBs), PTAQ exhibits a high specific capacity of 220.9 mAh g (at 1 A g) with wide operating voltage (-0.9-1.0 V) and maintains a capacity retention of 98.8 % after 10,000 cycles at 5 A g. Furthermore, an all-organic PTAQ//polyimide full cell was constructed, demonstrating a specific capacity of 65.6 mAh g at 1 A g over 200 cycles, with an impressive capacity retention rate of 94.2 %. This work advances the understanding of NH storage mechanisms in organic materials while establishing molecular engineering strategies for tailoring high-performance organic electrodes in aqueous ammonium-ion batteries (AAIBs). This enables technological innovation in sustainable energy storage systems with higher energy density.
具有定制共轭结构的氧化还原活性有机化合物，因其独特的离子（脱）嵌入机制，在氧化还原过程中可避免晶格畸变，已成为水系电池中关键的电极材料。尽管具有潜力，但有机材料仍受到一些限制，包括活性位点密度不足以及在电化学循环过程中由于电解质溶解导致的结构降解。为了解决这些限制，我们开发了一种创新的电子离域有机分子，命名为PTAQ，它包含一个具有广泛电子离域和减小的带隙的π共轭咪唑连接框架，这有利于电子转移。此外，添加了一个新的氧化还原活性基团（CN），并增加了CO的含量，从而提高了离子嵌入能力，这已通过原位分析和理论计算得到验证。作为水系铵离子电池（AAIBs）的电极，PTAQ在1 A g下表现出220.9 mAh g的高比容量，工作电压范围宽（-0.9 - 1.0 V），在5 A g下循环10000次后容量保持率为98.8%。此外，构建了全有机PTAQ//聚酰亚胺全电池，在1 A g下200次循环中比容量为65.6 mAh g，容量保持率高达94.2%，令人印象深刻。这项工作增进了对有机材料中NH存储机制的理解，同时建立了用于在水系铵离子电池（AAIBs）中定制高性能有机电极的分子工程策略。这为具有更高能量密度的可持续储能系统带来了技术创新。
