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A high-performance aqueous rechargeable zinc battery based on organic cathode integrating quinone and pyrazine
Energy Storage Materials ( IF 18.9 ) Pub Date : 2021-05-07 , DOI: 10.1016/j.ensm.2021.05.002
Yingjie Gao , Gaofeng Li , Feng Wang , Jun Chu , Pu Yu , Baoshan Wang , Hui Zhan , Zhiping Song

In spite of the recent rapid progress of organic cathode materials for aqueous rechargeable zinc batteries (ARZBs), there are still many challenges such as unaffordable synthesis, unsatisfactory electrochemical performance, and unclear mechanisms in this field. Herein, we report 5,7,12,14-tetraaza-6,13-pentacenequinone (TAPQ) as an easily-synthesized organic cathode material with a novel quinone/pyrazine hybrid structure. Benefitting from the multiple electroactive C=O and C=N bonds, TAPQ possessed a theoretical capacity of 515 mAh g–1 (based on a six-electron reaction) and a practically reversible capacity of 443 mAh g–1 within 0.1–1.6 V vs. Zn2+/Zn, both of which set new records for organic cathodes in ARZBs. The H+/Zn2+ co-insertion mechanism involving H+ as the predominant participant was confirmed by detailed investigations including various ex-situ characterizations, electrochemical tests, and DFT calculations. Based on the clear mechanism understanding, a modified voltage range of 0.5–1.6 V was adopted to simultaneously achieve high energy density (270 mAh g–1 × 0.84 V = 227 Wh kg–1) and excellent cycling stability (capacity retention of 92% after 250 cycles under 50 mA g–1, with an average Coulombic efficiency of 99.96%). Furthermore, the evolution mechanism of TAPQ electrode structure during cycling was also carefully studied to reveal the origin of capacity decline. The novel molecular structure, easy synthesis, superior electrochemical performance, and deeper mechanism understanding provide researchers important insights into the further development of organic cathode materials for ARZBs toward practical applications.



中文翻译:

基于有机阴极结合醌和吡嗪的高性能水性可充电锌电池

尽管最近用于含水可再充电锌电池(ARZB)的有机阴极材料取得了飞速发展,但仍然存在许多挑战,例如无法负担得起的合成,令人满意的电化学性能以及该领域中不清楚的机理。在这里,我们报告5,7,12,14-四氮杂-6,13-​​并五苯醌(TAPQ)作为具有新型醌/吡嗪杂化结构的易于合成的有机阴极材料。得益于多个电活性C = O和C = N键,TAPQ的理论容量为515 mAh g –1(基于六电子反应),在0.1–1.6 V范围内具有可逆的实际容量443 mAh g –1与Zn 2+ / Zn相比,两者均创下了ARZB中有机阴极的新记录。H + /锌通过详细的研究,包括各种异位表征,电化学测试和DFT计算,证实了以H +为主要参与者的2+共插入机制。基于对机制的清晰了解,采用了0.5–1.6 V的修改电压范围,以同时实现高能量密度(270 mAh g –1  ×0.84 V = 227 Wh kg –1)和出色的循环稳定性(容量保持率为92%)在50 mA g –1下250次循环后,平均库仑效率为99.96%)。此外,还仔细研究了TAPQ电极在循环过程中的演变机理,以揭示容量下降的原因。新颖的分子结构,易于合成,优异的电化学性能以及更深入的机理理解为研究人员提供了重要的见识,为ARZB有机阴极材料的进一步开发向实际应用迈进。

更新日期:2021-05-15
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