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Surface Overpotential as a Key Metric for the Discharge–Charge Reversibility of Aqueous Zinc-Ion Batteries
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-07-12 , DOI: 10.1021/jacs.3c01614
Minkwan Kim 1 , Jimin Lee 1 , Yangmoon Kim 1 , Youngbin Park 1 , Heejin Kim 2 , Jang Wook Choi 1
Affiliation  

Aqueous zinc-ion batteries (AZIBs) are receiving increasing attention for power-grid energy storage systems. Nevertheless, warranting long-term reversible operation is not trivial owing to uncontrolled interfacial phenomena related to zinc dendritic growth and parasitic reactions. Herein, the addition of hexamethylphosphoramide (HMPA) to the electrolyte revealed the surface overpotential (|ηs|) to be a key metric of the reversibility. HMPA adsorbs onto active sites on the zinc metal surface, raising the surface overpotential toward lowering the nucleation energy barrier and decreasing the critical size (rcrit) of nuclei. We also correlated the observed interface-to-bulk properties by the Wagner (Wa) dimensionless number. The controlled interface enables a Zn|V6O13 full cell to retain 75.97% capacity for 2000 cycles, with a capacity loss of only 1.5% after 72 h resting. Our study not only delivers AZIBs with unparalleled cycling and storage performance but also proposes surface overpotential as a key descriptor regarding the sustainability of AZIB cycling and storage.

中文翻译:

表面过电势作为水系锌离子电池充放电可逆性的关键指标

水系锌离子电池(AZIB)在电网储能系统中越来越受到关注。然而,由于与锌枝晶生长和寄生反应相关的不受控制的界面现象,保证长期可逆操作并非微不足道。在此,向电解质中添加六甲基磷酰胺(HMPA)表明表面过电势(|η s |)是可逆性的关键指标。HMPA 吸附在锌金属表面的活性位点上,提高表面过电势,从而降低成核能垒并减小核的临界尺寸 ( r crit )。我们还通过瓦格纳 (Wa) 无量纲数将观察到的界面与本体特性相关联。受控的界面使Zn|V 6 O 13全电池在2000次循环中保持75.97%的容量,并且在静置72小时后容量损失仅为1.5%。我们的研究不仅使 AZIB 具有无与伦比的循环和存储性能,而且还提出将表面过电势作为 AZIB 循环和存储可持续性的关键描述符。
更新日期:2023-07-12
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