Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries
Abstract
The internal shuttle effect caused by polysulfides dissolution and migration negatively impacts lithium–sulfur battery performance. In this paper, a mesoscale simulation strategy, which involves atomistic calculation and coarse-grained molecular modeling, is employed to evaluate silicene as a potential cathode host material to immobilize polysulfides. Adsorption energies of insoluble polysulfides (Li2Sx with x =1, 2) and soluble polysulfide Li2S4 on pristine and doped silicene sheets are calculated. Results show that the adsorption is thermodynamically favorable and N-doped silicene is helpful in trapping intermediate discharge products, Li2S2 and Li2S4. The dissociation and reduction of long-chain polysulfides to short-chain polysulfides are observed. Electronic structure analysis shows that Li2Sx molecules interact with silicene via strong chemical bonds. The atomistic structure evolution of Li2S layer formation on silicene is also investigated in this study. It is found that Li2S (110) layer forms first, and then, it is converted to Li2S (111) layer by introducing more Li2S molecules to the substrate. Li2S (111)/silicene interfacial structure is thermodynamically stable, and the interaction is dominated by Li–Si bonds. A coarse-grained model is developed to study and compare the growth of Li2S on silicene and graphene. Lastly, Li2S-induced surface coverage is faster on silicene than on graphene, which indicatesmore »
- Authors:
-
- Texas A & M Univ., College Station, TX (United States). Dept. of Mechanical Engineering
- Texas A & M Univ., College Station, TX (United States). Dept. of Chemical Engineering
- Publication Date:
- Research Org.:
- Texas A & M Univ., College Station, TX (United States). Texas A & M Engineering Experiment Station; Purdue Univ., West Lafayette, IN (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
- OSTI Identifier:
- 1430275
- Grant/Contract Number:
- EE0006832
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Coordination Chemistry
- Additional Journal Information:
- Journal Volume: 69; Journal Issue: 11-13; Journal ID: ISSN 0095-8972
- Publisher:
- Taylor & Francis
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 25 ENERGY STORAGE; 36 MATERIALS SCIENCE; Lithium-sulfur battery; internal shuttle effect; silicene; polysulfide retention; surface passivation
Citation Formats
Liu, Zhixiao, Balbuena, Perla B., and Mukherjee, Partha P. Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries. United States: N. p., 2016.
Web. doi:10.1080/00958972.2016.1184265.
Liu, Zhixiao, Balbuena, Perla B., & Mukherjee, Partha P. Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries. United States. https://doi.org/10.1080/00958972.2016.1184265
Liu, Zhixiao, Balbuena, Perla B., and Mukherjee, Partha P. Fri .
"Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries". United States. https://doi.org/10.1080/00958972.2016.1184265. https://www.osti.gov/servlets/purl/1430275.
@article{osti_1430275,
title = {Evaluating silicene as a potential cathode host to immobilize polysulfides in lithium–sulfur batteries},
author = {Liu, Zhixiao and Balbuena, Perla B. and Mukherjee, Partha P.},
abstractNote = {The internal shuttle effect caused by polysulfides dissolution and migration negatively impacts lithium–sulfur battery performance. In this paper, a mesoscale simulation strategy, which involves atomistic calculation and coarse-grained molecular modeling, is employed to evaluate silicene as a potential cathode host material to immobilize polysulfides. Adsorption energies of insoluble polysulfides (Li2Sx with x =1, 2) and soluble polysulfide Li2S4 on pristine and doped silicene sheets are calculated. Results show that the adsorption is thermodynamically favorable and N-doped silicene is helpful in trapping intermediate discharge products, Li2S2 and Li2S4. The dissociation and reduction of long-chain polysulfides to short-chain polysulfides are observed. Electronic structure analysis shows that Li2Sx molecules interact with silicene via strong chemical bonds. The atomistic structure evolution of Li2S layer formation on silicene is also investigated in this study. It is found that Li2S (110) layer forms first, and then, it is converted to Li2S (111) layer by introducing more Li2S molecules to the substrate. Li2S (111)/silicene interfacial structure is thermodynamically stable, and the interaction is dominated by Li–Si bonds. A coarse-grained model is developed to study and compare the growth of Li2S on silicene and graphene. Lastly, Li2S-induced surface coverage is faster on silicene than on graphene, which indicates that a silicene-based cathode host will experience more acute surface passivation, which will adversely affect cathode performance.},
doi = {10.1080/00958972.2016.1184265},
journal = {Journal of Coordination Chemistry},
number = 11-13,
volume = 69,
place = {United States},
year = {Fri May 27 00:00:00 EDT 2016},
month = {Fri May 27 00:00:00 EDT 2016}
}
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