Wang Dan, Bai Yuxuan, Zhou Zixiang, Yao Qi, Cao Wei, Ma Yangmin, Wang Chao
College of Chemistry and Chemical Engineering, Shaanxi Collaborative Innovation Center of Industrial Auxiliary Chemistry & Technology, Key Laboratory of Auxiliary Chemistry and Technology for Chemical Industry, Ministry of Education, The Youth Innovation Team of Shaanxi Universities, Shaanxi University of Science and Technology, Xi'an, Shaanxi 710021, China.
Scientific Instrument Center, Shanxi University, Taiyuan 030006, People's Republic of China.
ACS Appl Mater Interfaces. 2024 May 22;16(20):26121-26129. doi: 10.1021/acsami.4c02285. Epub 2024 May 10.
The design of aqueous zinc-ion batteries (ZIBs) that have high specific capacity and long-term stability is essential for future large-scale energy storage systems. Cathode materials with extended π-conjugation and abundant active sites are desirable to enhance the charge storage performance and the cycling stability of the aqueous ZIB. Based on this concept, 6,9-dihydropyrazino[2,3-]quinoxaline-2,3,7,8(1,4)-tetrone was chosen as the monomer to be electropolymerized onto carbon cloth (PDHPQ-Tetrone/CC). When used as the cathode material for aqueous ZIBs, an exceptional cycling life (>20,000 cycles) at a current density of 10 A g was achieved, with the specific capacity maintained at 82.8% and with the Coulombic efficiency at around 100% throughout cycling. At the charge-discharge current density of 0.1 A g, the ZIB with PDHPQ-Tetrone/CC achieved a high specific capacity of 248 mAh g. Kinetic analyses showed that both surface-capacitive-controlled processes and semi-infinite diffusion-controlled processes contribute to the stored charge. The charge storage mechanism was investigated with ex situ characterizations and involves the redox processes of carbonyl/hydroxyl and amino/imino groups coupled with insertion and extraction of both Zn and H.
设计具有高比容量和长期稳定性的水系锌离子电池（ZIBs）对于未来大规模储能系统至关重要。具有扩展π共轭和丰富活性位点的阴极材料有利于提高水系ZIB的电荷存储性能和循环稳定性。基于这一概念，选择6,9-二氢吡嗪并[2,3 - ]喹喔啉-2,3,7,8(1,4)-四酮作为单体在碳布上进行电聚合（PDHPQ - 四酮/CC）。当用作水系ZIB的阴极材料时，在10 A g的电流密度下实现了优异的循环寿命（>20,000次循环），比容量保持在82.8%，并且在整个循环过程中库仑效率约为100%。在0.1 A g的充放电电流密度下，具有PDHPQ - 四酮/CC的ZIB实现了248 mAh g的高比容量。动力学分析表明，表面电容控制过程和半无限扩散控制过程都对存储电荷有贡献。通过非原位表征研究了电荷存储机制，该机制涉及羰基/羟基和氨基/亚氨基基团的氧化还原过程以及Zn和H的嵌入和脱出。
