Origin of Electrochemical, Structural, and Transport Properties in Nonaqueous Zinc Electrolytes

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• 作者：Sang-Don Han ; Nav Nidhi Rajput ; Xiaohui Qu ; Baofei Pan ; Meinan He ; Magali S. Ferrandon ; Chen Liao ; Kristin A. Persson ; Anthony K. Burrell
• 刊名：ACS Applied Materials & Interfaces
• 出版年：2016
• 出版时间：February 10, 2016
• 年：2016
• 卷：8
• 期：5
• 页码：3021-3031
• 全文大小：633K
• ISSN：1944-8252

文摘

Through coupled experimental analysis and computational techniques, we uncover the origin of anodic stability for a range of nonaqueous zinc electrolytes. By examination of electrochemical, structural, and transport properties of nonaqueous zinc electrolytes with varying concentrations, it is demonstrated that the acetonitrile–Zn(TFSI)₂, acetonitrile–Zn(CF₃SO₃)₂, and propylene carbonate–Zn(TFSI)₂ electrolytes can not only support highly reversible Zn deposition behavior on a Zn metal anode (≥99% of Coulombic efficiency) but also provide high anodic stability (up to ～3.8 V vs Zn/Zn²⁺). The predicted anodic stability from DFT calculations is well in accordance with experimental results, and elucidates that the solvents play an important role in anodic stability of most electrolytes. Molecular dynamics (MD) simulations were used to understand the solvation structure (e.g., ion solvation and ionic association) and its effect on dynamics and transport properties (e.g., diffusion coefficient and ionic conductivity) of the electrolytes. The combination of these techniques provides unprecedented insight into the origin of the electrochemical, structural, and transport properties in nonaqueous zinc electrolytes.