title: Origin of Electrochemical, Structural, and Transport Properties in Nonaqueous Zinc Electrolytes.
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/Zn(2+)). 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.
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
authors.forename: Sang-Don
authors.initials: SD
authors.lastname: Han
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
authors.forename: Nav Nidhi
authors.initials: NN
authors.lastname: Rajput
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
authors.forename: Xiaohui
authors.initials: X
authors.lastname: Qu
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
authors.forename: Baofei
authors.initials: B
authors.lastname: Pan
authors.affiliation: Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Department of Mechanical Engineering, Worcester Polytechnic Institute , Worcester, Massachusetts 01609, United States.
authors.forename: Meinan
authors.initials: M
authors.lastname: He
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
authors.forename: Magali S
authors.initials: MS
authors.lastname: Ferrandon
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
authors.forename: Chen
authors.initials: C
authors.lastname: Liao
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Environmental Energy Technologies Division, Lawrence Berkeley National Laboratory , Berkeley, California 94720, United States.
authors.forename: Kristin A
authors.initials: KA
authors.lastname: Persson
authors.affiliation: Joint Center for Energy Storage Research, Argonne National Laboratory , Lemont, Illinois 60439, United States.|Chemical Sciences and Engineering Division, Argonne National Laboratory , Lemont, Illinois 60439, United States.
authors.forename: Anthony K
authors.initials: AK
authors.lastname: Burrell
keywords: Coulombic efficiency; anodic stability; electrode/electrolyte interface; nonaqueous electrolyte; reversible deposition; solvation structure