Dimerizing Lawsone into Bis-lawsone to Counter Solubility and Attain Facile Zn2+ Ion Diffusion for Stable Capacity in Aqueous Zinc-Ion Batteries,ACS Applied Energy Materials

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Dimerizing Lawsone into Bis-lawsone to Counter Solubility and Attain Facile Zn2+ Ion Diffusion for Stable Capacity in Aqueous Zinc-Ion Batteries
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-06-22 , DOI: 10.1021/acsaem.3c00799
Richa Gupta ₁ , Chinmaya Mirle ₁ , Kothandaraman Ramanujam ₁

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Given the higher volumetric capacity of Zn (5853 mAh cm⁻³), aqueous zinc-ion batteries can be considered as alternatives to lithium-ion batteries for energy storage applications. Here we focus on redox-active, non-toxic, and eco-friendly organic materials with quinone moiety, i.e., Lawsone (LS) and its dimer Bis-lawsone (BL), as a cathode material for Zn-ion batteries. The reversibility of LS and BL is confirmed by cyclic voltammetry between 0.3 and 1.6 V in zinc sulfate and zinc triflate electrolytes. The electrochemical performance of BL in the zinc triflate electrolyte is improved by the reduction in the solubility of BL in the electrolyte and improvement in Zn²⁺ diffusion in the BL matrix. Besides, it is known that Zn electrodes passivate better in zinc triflates, which contributes to improved plating/stripping of Zn. The dimerization strategy counteracts solubility and facilitates the diffusion of Zn²⁺, resulting in a stable charge–discharge with a specific capacity of 200 mAh g^–1. The cell attained 77% of the theoretical capacity at a current density of 100 mA g^–1. Zn-BL cells show fast kinetics and reversibility for up to 760 cycles retaining 85% of initial capacity despite the partial solubility of BL in electrolytes. In addition, the Nafion-212 membrane is introduced as a separator instead of a traditional glass fiber separator. The negatively charged backbone of Nafion helps eliminate the crossover problem by coulostatic repulsion with negatively charged BL and LS.

中文翻译：

将劳松二聚成双劳松，以平衡溶解度并实现易于 Zn2+ 离子扩散，从而实现水系锌离子电池的稳定容量

鉴于锌具有较高的体积容量（5853 mAh cm ^-3），水性锌离子电池可被视为储能应用中锂离子电池的替代品。在这里，我们重点研究具有氧化还原活性、无毒、环保的醌基有机材料，即Lawsone (LS) 及其二聚体Bis-lawsone (BL)，作为锌离子电池的正极材料。LS 和 BL 的可逆性通过硫酸锌和三氟甲磺酸锌电解质中 0.3 至 1.6 V 之间的循环伏安法得到证实。通过降低BL在电解液中的溶解度和提高Zn ^{2+ ，提高了BL在三氟甲磺酸锌电解液中的电化学性能}BL 矩阵中的扩散。此外，众所周知，锌电极在三氟甲磺酸锌中钝化效果更好，这有助于改善锌的电镀/剥离。^{二聚策略抵消了溶解度并促进了 Zn 2+}的扩散，从而实现稳定的充放电，比容量为 200 mAh g ^–1。电池在电流密度为 100 mA g ^{–1时达到理论容量的 77%}。尽管 BL 在电解质中部分溶解，但 Zn-BL 电池表现出快速动力学和可逆性，最多 760 个循环仍保留 85% 的初始容量。此外，引入Nafion-212膜作为隔膜代替传统的玻璃纤维隔膜。Nafion 的带负电主链有助于通过与带负电的 BL 和 LS 的恒电量排斥来消除交叉问题。

更新日期：2023-06-22

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