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

Publication Type

Journal Article

Date Published

10/2016

Abstract

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.

Journal

ACS Applied Materials & Interfaces

Volume

8

Year of Publication

2016

Issue

5

Pagination

3021 - 3031

ISSN

1944-8244

Short Title

ACS Appl. Mater. Interfaces

Refereed Designation

Refereed