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Title: Mesoscale Elucidation of Surface Passivation in the Li–Sulfur Battery Cathode

We report the cathode surface passivation caused by Li 2S precipitation adversely affects the performance of lithium-sulfur (Li-S) batteries. Li 2S precipitation is a complicated mesoscale process involving adsorption, desorption and diffusion kinetics, which are affected profoundly by the reactant concentration and operating temperature. In this work, a mesoscale interfacial model is presented to study the growth of Li 2S film on carbon cathode surface. Li 2S film growth experiences nucleation, isolated Li 2S island growth and island coalescence. The slow adsorption rate at small S 2- concentration inhibits the formation of nucleation seeds and the lateral growth of Li 2S islands, which deters surface passivation. An appropriate operating temperature, especially in the medium-to-high temperature range, can also defer surface passivation. Fewer Li 2S nucleation seeds form in such an operating temperature range, which facilitates heterogeneous growth and thereby inhibits the lateral growth of the Li 2S film, which may also result in reduced surface passivation. Finally, the high specific surface area of the cathode microstructure is expected to mitigate the surface passivation.
Authors:
 [1] ; ORCiD logo [1]
  1. Texas A & M Univ., College Station, TX (United States). Department of Mechanical Engineering
Publication Date:
Grant/Contract Number:
EE0006832
Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 9; Journal Issue: 6; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Research Org:
Texas A&M Engineering Experiment Station, 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; 36 MATERIALS SCIENCE; Li2S precipitation; lithium−sulfur battery; mesoscale modeling; morphology evolution; surface passivation
OSTI Identifier:
1430645