Huang Cong, Zhao Xin, Liu Shuang, Hao Yisu, Tang Qunli, Hu Aiping, Liu Zhixiao, Chen Xiaohua
College of Materials Science and Engineering, Hunan Province Key Laboratory for Advanced Carbon Materials and Applied Technology, Hunan University, Changsha, 410082, P. R. China.
Adv Mater. 2021 Sep;33(38):e2100445. doi: 10.1002/adma.202100445. Epub 2021 Aug 2.
Zn anodes suffer from poor Coulombic efficiency (CE) and serious dendrite formation due to the unstable anode/electrolyte interface (AEI). The electrical double layer (EDL) structure formed before cycling is of great significance for building stable solid electrolyte interphase (SEI) on Zn surface but barely discussed in previous research about the stabilization of Zn anode. Herein, saccharin (Sac) is introduced as electrolyte additive for regulating the EDL structure on the AEI. It is found that Sac derived anions are preferentially adsorbed on the Zn metal surface instead of water dipole, creating a new H O-poor EDL structure. Moreover, the unique SEI is also detected on the Zn surface due to the decomposition of Sac anions. Both are proved to be capable of modulating Zn deposition behavior and preventing side reactions. Encouragingly, Zn|Zn symmetric cells using Sac additive deliver a high cumulative plated capacity of 2.75 Ah cm and a high average CE of 99.6% under harsh test condition (10 mA cm , 10 mAh cm ). The excellent stability is also achieved at a high rate of 40 mA cm . The effectiveness of this Sac additive is further demonstrated in the Zn-MnO full cells.
锌阳极由于阳极/电解质界面(AEI)不稳定,库仑效率(CE)较低且会严重形成枝晶。循环前形成的双电层(EDL)结构对于在锌表面构建稳定的固体电解质界面(SEI)具有重要意义,但在先前关于锌阳极稳定化的研究中几乎未被讨论。在此,引入糖精(Sac)作为电解质添加剂来调节AEI上的EDL结构。研究发现,Sac衍生的阴离子优先吸附在锌金属表面而非水偶极上,从而形成了一种新的贫水EDL结构。此外,由于Sac阴离子的分解,在锌表面还检测到了独特的SEI。两者均被证明能够调节锌的沉积行为并防止副反应。令人鼓舞的是,使用Sac添加剂的锌|锌对称电池在苛刻的测试条件(10 mA cm²,10 mAh cm²)下具有2.75 Ah cm²的高累积镀覆容量和99.6%的高平均CE。在40 mA cm²的高电流密度下也实现了优异的稳定性。这种Sac添加剂的有效性在锌-二氧化锰全电池中得到了进一步证明。