Stereoisomeric engineering mediated zinc metal electrodeposition: Critical balance of solvation and adsorption capability

Wen Liu , Qiwen Zhao , Ruheng Jiang , Xuyan Ni , Tiancheng You , Canglong Li , Yanzi Deng , Bingang Xu , Yuejiao Chen , Libao Chen
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Abstract

The exceptional electrochemical performance of zinc anodes is frequently impeded by inadequate deposition kinetics and interfacial chemistry. Herein, we introduce the stereoisomerism to inform the balanced selection of electrolyte additives, taking into account their solvation and adsorption properties, to achieve the optimal deposition behaviors and electrochemical performance. The three-point coplanar adsorption configuration, in comparison to two-point adsorption, effectively mitigates the interference of water molecules and establishes a coplanar templating effect. This approach fosters a uniform distribution of charges, encourages the preferential orientation growth of (002) planes for uniform zinc deposition. Moreover, an appropriate level of solvation ability can modulate the solvation structure without substantially increasing the de-solvation energy barrier, thereby facilitating faster deposition kinetics than what is observed in cases of strong solvation. As a result, Zn//Zn cell can achieve an excellent performance of more than 3470 ​h at 2 ​mA ​cm−2 and 1 mAh cm−2, and Zn//AC full cell can work for 50000 cycles at 3 ​A ​g−1. Additionally, under practical conditions (N/P=4.37), the assembled Zn//I2 full cell demonstrates stable lifespan for 710 cycles at 1 ​A ​g−1. This work showcases the interplay between adsorption configuration of stereoisomeric additives on the cycling.

Abstract Image

立体异构体工程介导的锌金属电沉积:溶剂化和吸附能力的临界平衡
锌阳极优异的电化学性能经常受到不充分的沉积动力学和界面化学的阻碍。在此,我们引入立体异构来指导电解质添加剂的平衡选择,考虑其溶剂化和吸附性能,以实现最佳的沉积行为和电化学性能。与两点吸附相比,三点共面吸附构型有效地减轻了水分子的干扰,建立了共面模板效应。这种方法促进了电荷的均匀分布,促进了(002)平面的优先取向生长,以实现均匀的锌沉积。此外,适当水平的溶剂化能力可以调节溶剂化结构,而不会大幅增加脱溶剂能垒,从而促进比强溶剂化情况下观察到的更快的沉积动力学。结果表明,Zn//Zn电池在2 mA cm - 2和1 mAh cm - 2下可实现3470 h以上的优异性能,Zn//AC电池在3 a g - 1下可工作50000次。此外,在实际条件下(N/P=4.37),组装的Zn/ I2完整电池在1 A g−1下可以稳定使用710次。这项工作展示了立体异构体添加剂在循环中的吸附构型之间的相互作用。
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CiteScore
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