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Title: Hole Polaron Diffusion in the Final Discharge Product of Lithium–Sulfur Batteries

Poor electronic conductivity of bulk lithium sulfide (Li 2S) is a critical challenge for the debilitating performance of the lithium–sulfur battery. In this study we focus on investigating the thermodynamic and kinetic properties of native defects in Li 2S based on a first-principles approach. It is found that the hole polaron p + can form in Li 2S by removing a 3p electron from an S 2– anion. The p + diffusion barrier is only 90 meV, which is much lower than the Li vacancy (V Li ) diffusion barrier. Hence p + has the potential to serve as a charge carrier in the discharge product. Once the vacancy–polaron complex (V Li -––2p +) forms, the charge transport will be hindered due to the relatively higher diffusion barrier of the complex. Heteroatom dopants, which can decrease the p + formation energy and increase V Li formation energy, are expected to be introduced to the discharge product to improve the electronic conductivity.
Authors:
 [1] ; ORCiD logo [2] ; ORCiD logo [1]
  1. Texas A & M Univ., College Station, TX (United States). Dept. of Mechanical Engineering
  2. Texas A & M Univ., College Station, TX (United States). Dept. of Chemical Engineering
Publication Date:
Grant/Contract Number:
EE0006832
Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 32; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Texas A & M Univ., College Station, TX (United States)
Sponsoring Org:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1430631
Alternate Identifier(s):
OSTI ID: 1430595

Liu, Zhixiao, Balbuena, Perla B., and Mukherjee, Partha P.. Hole Polaron Diffusion in the Final Discharge Product of Lithium–Sulfur Batteries. United States: N. p., Web. doi:10.1021/acs.jpcc.7b06869.
Liu, Zhixiao, Balbuena, Perla B., & Mukherjee, Partha P.. Hole Polaron Diffusion in the Final Discharge Product of Lithium–Sulfur Batteries. United States. doi:10.1021/acs.jpcc.7b06869.
Liu, Zhixiao, Balbuena, Perla B., and Mukherjee, Partha P.. 2017. "Hole Polaron Diffusion in the Final Discharge Product of Lithium–Sulfur Batteries". United States. doi:10.1021/acs.jpcc.7b06869. https://www.osti.gov/servlets/purl/1430631.
@article{osti_1430631,
title = {Hole Polaron Diffusion in the Final Discharge Product of Lithium–Sulfur Batteries},
author = {Liu, Zhixiao and Balbuena, Perla B. and Mukherjee, Partha P.},
abstractNote = {Poor electronic conductivity of bulk lithium sulfide (Li2S) is a critical challenge for the debilitating performance of the lithium–sulfur battery. In this study we focus on investigating the thermodynamic and kinetic properties of native defects in Li2S based on a first-principles approach. It is found that the hole polaron p+ can form in Li2S by removing a 3p electron from an S2– anion. The p+ diffusion barrier is only 90 meV, which is much lower than the Li vacancy (VLi–) diffusion barrier. Hence p+ has the potential to serve as a charge carrier in the discharge product. Once the vacancy–polaron complex (VLi-––2p+) forms, the charge transport will be hindered due to the relatively higher diffusion barrier of the complex. Heteroatom dopants, which can decrease the p+ formation energy and increase VLi– formation energy, are expected to be introduced to the discharge product to improve the electronic conductivity.},
doi = {10.1021/acs.jpcc.7b06869},
journal = {Journal of Physical Chemistry. C},
number = 32,
volume = 121,
place = {United States},
year = {2017},
month = {7}
}