N-Heteroaromatic fused-ring cyanides extended as redox polymers for high rate capability aqueous zinc-ion battery,Journal of Materials Chemistry A

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N-Heteroaromatic fused-ring cyanides extended as redox polymers for high rate capability aqueous zinc-ion battery
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2023-01-05 , DOI: 10.1039/d2ta08466j
Xinlei Wang _{1,

2} , Jie Zhou ₂ , Zhipeng Li ₁ , Weihua Tang _{1,

2}

Affiliation

Reversible zinc-ion storage in aqueous electrolytes is emerging as a promising grid-scale energy storage technology with desirable operational safety and environmental friendliness. Polymer electrodes with robust structure and good redox-activities are in high demand for the development of devices with superior rate capability. We report herein two redox polymers (PHATN-t and PHAT-t) with extended π-conjugated structure via multi-site trimerization of diquinoxalino[2,3-a:2′,3′-c]phenazine and dipyrazino[2,3-f:2′,3′-h]quinoxaline cyanides. The facile synthesis and structural features of the two polymers and their potential as high rate capability electrodes in zinc-ion supercapatteries (ZIS) have been systematically studied with both experimental tests and theoretical calculation. PHATN-t and PHAT-t exhibit maximum specific capacities of 190 and 171 mA h g⁻¹ at 0.3 A g⁻¹, which remain at 132 and 121 mA h g⁻¹ at 10 A g⁻¹, respectively. Outstanding capacity retentions of 58% and 56% are even observed at 20 A g⁻¹. Importantly, PHATN-t and PHAT-t display 86.8% and 77.6% capacity retention after 1000 cycles. Mechanistic studies show that PHATN-t possesses higher pore volume and pore size for cation hosting due to it having more extensive conjugation planes. Theoretical simulation reveals stronger electron delocalization and more undisturbed redox sites to afford higher internal charge transfer, faster reaction kinetics and thus higher capacitance output for PHATN-t.

中文翻译：

N-杂芳族稠环氰化物作为氧化还原聚合物扩展用于高倍率水性锌离子电池

水性电解质中的可逆锌离子存储正在成为一种有前途的电网规模储能技术，具有理想的操作安全性和环境友好性。具有坚固结构和良好氧化还原活性的聚合物电极对于开发具有优异倍率性能的器件有很高的需求。我们在此报告了两种氧化还原聚合物（PHATN-t 和 PHAT-t），它们通过二喹喔啉[2,3- a :2',3'- c]吩嗪和二吡嗪[2,3 的多位点三聚化具有扩展的π共轭结构- f :2',3'- h]喹喔啉氰化物。通过实验测试和理论计算，系统地研究了这两种聚合物的简便合成和结构特征及其作为锌离子超级电池（ZIS）中高倍率电极的潜力。PHATN-t 和 PHAT-t在 0.3 A g ^{-1时表现出 190 和 171 mA hg}^-1的最大比容量，在 10 A g ^-1时分别保持在 132 和 121 mA hg ^-1。^{甚至在 20 A g -1}下也观察到 58% 和 56% 的出色容量保留. 重要的是，PHATN-t 和 PHAT-t 在 1000 次循环后显示出 86.8% 和 77.6% 的容量保留率。机理研究表明，由于 PHATN-t 具有更广泛的共轭平面，PHATN-t 具有更高的阳离子承载孔体积和孔径。理论模拟揭示了更强的电子离域和更多未受干扰的氧化还原位点，以提供更高的内部电荷转移、更快的反应动力学，从而为 PHATN-t 提供更高的电容输出。

更新日期：2023-01-05

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