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Title: Origin of electrochemical, structural and transport properties in non-aqueous 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(CF 3SO 3) 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). 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. Lastly, the combination of these techniques provides unprecedented insight into the origin of the electrochemical, structural, and transport properties in nonaqueous zinc electrolytes

Authors:
 [1];  [2];  [2];  [1];  [3];  [1];  [1];  [2];  [1]
  1. Argonne National Lab. (ANL), Lemont, IL (United States)
  2. Argonne National Lab. (ANL), Lemont, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States); Worcester Polytechnic Institute, Worcester, MA (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1248374
Alternate Identifier(s):
OSTI ID: 1454452
Grant/Contract Number:  
AC02-06CH11357; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 8; Journal Issue: 5; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; nonaqueous electrolyte; electrode/electrolyte interface; reversible deposition; Coulombic efficiency; anodic stability; solvation structure

Citation Formats

Han, Sang -Don, Rajput, Nav Nidhi, Qu, Xiaohui, Pan, Baofei, He, Meinan, Ferrandon, Magali S., Liao, Chen, Persson, Kristin A., and Burrell, Anthony K. Origin of electrochemical, structural and transport properties in non-aqueous zinc electrolytes. United States: N. p., 2016. Web. doi:10.1021/acsami.5b10024.
Han, Sang -Don, Rajput, Nav Nidhi, Qu, Xiaohui, Pan, Baofei, He, Meinan, Ferrandon, Magali S., Liao, Chen, Persson, Kristin A., & Burrell, Anthony K. Origin of electrochemical, structural and transport properties in non-aqueous zinc electrolytes. United States. doi:10.1021/acsami.5b10024.
Han, Sang -Don, Rajput, Nav Nidhi, Qu, Xiaohui, Pan, Baofei, He, Meinan, Ferrandon, Magali S., Liao, Chen, Persson, Kristin A., and Burrell, Anthony K. Thu . "Origin of electrochemical, structural and transport properties in non-aqueous zinc electrolytes". United States. doi:10.1021/acsami.5b10024. https://www.osti.gov/servlets/purl/1248374.
@article{osti_1248374,
title = {Origin of electrochemical, structural and transport properties in non-aqueous zinc electrolytes},
author = {Han, Sang -Don and Rajput, Nav Nidhi and Qu, Xiaohui and Pan, Baofei and He, Meinan and Ferrandon, Magali S. and Liao, Chen and Persson, Kristin A. and Burrell, Anthony K.},
abstractNote = {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). 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. Lastly, the combination of these techniques provides unprecedented insight into the origin of the electrochemical, structural, and transport properties in nonaqueous zinc electrolytes},
doi = {10.1021/acsami.5b10024},
journal = {ACS Applied Materials and Interfaces},
number = 5,
volume = 8,
place = {United States},
year = {2016},
month = {1}
}

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