Abstract
Aqueous zinc-ion batteries (AZIBs) have been regarded as prospective rechargeable energy storage devices because of the high theoretical capacity and low redox potential of Zn metal. However, the uncontrollable formation of dendrites and the water-induced side reactions at the Zn/electrolyte interface, and the poor reversibility under a high current density (> 2 mA·cm−2) and large area capacity (> 2 mAh·cm−2) still limit the practical applications of AZIBs. Therefore, a strategy that can overcome these difficulties is urgently needed. Here, we introduce an environmentally friendly and low-cost additive, namely urea, to the electrolyte of AZIBs to induce uniform Zn deposition and suppress the side reactions. Measurements of the adsorption behavior, electrochemical characterization, and observations of the morphology revealed the interfacial modification induced by urea on the Zn/electrolyte interface, demonstrating its huge potential in AZIBs. Consequently, the long-term cycling stability (over 2100 h) of a Zn/Zn symmetric cell under a high current density of 5 mA·cm−2 and a capacity of 5 mAh·cm−2 was achieved with a 1 mol·L−1 ZnSO4 electrolyte with the urea additive. Additionally, the assembled Zn/NH4V4O10 full cell with urea exhibited excellent cycling performance and an outstanding average Coulombic efficiency of 99.98%. These results indicate that this is a low-cost and effective additive strategy for realizing highly reversible AZIBs.
Graphical abstract
摘要
由于锌金属具有较高的理论容量和较低的氧化还原电势, 水系锌离子电池成为一种极具前景的可充电储能装置。然而, 锌负极/电解液界面上不可控的枝晶生长和副反应, 以及锌负极在大电流密度(> 2 mA·cm−2)和大面沉积量(> 2 mAh·cm−2)下较差的可逆性严重限制了它的实际应用。因此, 迫切需要开发一种能够克服以上缺陷的策略。本文将一种环保、低成本的添加剂——尿素加入1 mol·L−1 ZnSO4电解液中, 用以诱导锌的均匀沉积并抑制副反应发生。添加剂吸附行为的测定、电池电化学性能的表征和锌负极形貌的观察共同揭示了尿素添加剂在Zn/ZnSO4界面上引起的界面修饰效果, 展现了其巨大的应用潜力。在5 mA·cm−2的电流密度和5 mAh·cm−2的面沉积量下, 使用尿素添加剂的Zn/Zn对称电池可稳定循环超2100 h。所组装的Zn/NH4V4O10全电池也具有良好的循环性能和99.98%的平均库仑效率。以上结果表明, 使用尿素作为电解液添加剂是一种成本低廉且行之有效的界面修饰策略。
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This study was financially supported by the Key Science and Technology Program of Henan Province (Nos. 212102210219 and 232102241020), the Ph.D. Research Startup Foundation of Henan University of Science and Technology (No. 400613480015), and the Postdoctoral Research Startup Foundation of Henan University of Science and Technology (No. 400613554001).
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Xu, BR., Li, QA., Liu, Y. et al. Urea-induced interfacial engineering enabling highly reversible aqueous zinc-ion battery. Rare Met. 43, 1599–1609 (2024). https://doi.org/10.1007/s12598-023-02541-4
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DOI: https://doi.org/10.1007/s12598-023-02541-4