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A benzo[a]phenazine-based redox species with highly reversible two-electron reaction for aqueous organic redox flow batteries
Electrochimica Acta ( IF 5.5 ) Pub Date : 2022-11-29 , DOI: 10.1016/j.electacta.2022.141644
Junyoung Park , Youngho Lee , Deokhee Yun , Doeun Kim , Gyungmin Hwang , Byeongjik Han , Yongbeom Kim , Jaehyun Jung , Joonhyeon Jeon

In aqueous organic redox flow batteries (AORFBs), the inherent problems, such as low energy and poor chemical stability, remain obstacles to the growth of AORFBs for the large-scale energy storage system (ESS). To address these challenges, this paper describes a novel benzo[a]phenazin-5-ol methanesulfonate (BHPS, C16H10N2O4S) containing sulfonic acid and hydroxyl functional groups, which undergoes a highly stable and reversible two-electron redox reaction in aqueous media, and allows high chemical stability, superb conductivity, high redox potential (−0.943 V) and excellent solubility. The superior chemical and electrochemical properties of the proposed BHPS are demonstrated through various experiments, including full cell-cycling tests, along with theoretical molecular analysis. Experimental results show that the BHPS with highly conductive sulfonic acid group (along with hydroxyl group) leads to 1.83 times higher kinetic constant (1.32 × 10−3 cm s  1) and 98.07 times higher solubility (1.47 M) than the benzo[a]phenazine-5-ol (HBP, C16H10N2O). Further, the BHPS/Fe(CN)6 flow-cell cycling for 100 cycles at 60 mA cm−2 results in great coulombic and energy efficiencies of average 99.5 and 81.9%, along with dramatic charge-and-discharge capacity retention ratios of average 99.79 and 99.25% with initial charge and discharge capacities of 49.11 and 48.76 mAh, respectively. The BHPS successfully synthesized by the attachment of the sulfonic acid and hydroxyl groups to benzo[a]phenazine provides a promising anodic organic species for highly efficient AORFBs, and its performance can be further optimized by molecular engineering.



中文翻译:

用于水性有机氧化还原液流电池的具有高度可逆双电子反应的苯并[a]吩嗪基氧化还原物质

在水系有机氧化还原液流电池(AORFBs)中,低能量和化学稳定性差等固有问题仍然是大规模储能系统(ESS)中AORFBs发展的障碍。为了应对这些挑战,本文介绍了一种新型苯并[a]吩嗪-5-醇甲磺酸盐 (BHPS, C 16 H 10 N 2 O 4S)含有磺酸和羟基官能团,在水性介质中发生高度稳定和可逆的双电子氧化还原反应,具有高化学稳定性、优异的导电性、高氧化还原电位(-0.943 V)和优异的溶解性。拟议的 BHPS 卓越的化学和电化学性能通过各种实验得到证明,包括全电池循环测试以及理论分子分析。实验结果表明苯并 [ a  ]phenazine-5-ol (HBP, C 16 H 10 N 2 O)。此外,BHPS/Fe(CN) 6流动电池在 60 mA cm -2下循环 100 次导致库仑效率和能量效率达到平均 99.5% 和 81.9%,以及显着的平均充电和放电容量保持率99.79 和 99.25%,初始充电和放电容量分别为 49.11 和 48.76 mAh。通过将磺酸和羟基连接到苯并[ a ]吩嗪成功合成的BHPS为高效AORFBs提供了一种有前途的阳极有机物种,其性能可以通过分子工程进一步优化。

更新日期:2022-11-29
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