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Title: Towards Next Generation Lithium-Sulfur Batteries: Non-Conventional Carbon Compartments/Sulfur Electrodes and Multi-Scale Analysis

Abstract

In this work, a novel heterofunctional, bimodal-porous carbon morphology, termed the carbon compartment (CC), is utilized as a sulfur host as a lithium-sulfur battery cathode. A multi-scale model explores the physics and chemistry of the lithium-sulfur battery cathode. The CCs are synthesized by a rapid, low cost process to improve electrode-electrolyte interfacial contact and accommodate volumetric expansion associated with sulfide formation. The CCs demonstrate high sulfur loading (47 %-wt. S) and ca. 700 mAh g -1 reversible capacity with high coulombic efficiency due to their unique structures. Density functional theory and ab initio Molecular Dynamics characterize the interface between the C/S composite and electrolyte during the sulfur reduction mechanism. Stochastic realizations of 3D electrode microstructures are reconstructed based on representative SEM images to study the influence of solid sulfur loading and lithium sulfide precipitation on microstructural and electrochemical properties. A macroscale electrochemical performance model is developed to analyze the performance of lithium-sulfur batteries. The combined multi-scale simulation studies explain key fundamentals of sulfur reduction and its relation to the polysulfide shuttle mechanism: how the process is affected due to the presence of carbon substrate, thermodynamics of lithium sulfide formation and deposition on carbon, and microstructural effects on the overall cellmore » performance.« less

Authors:
 [1];  [2];  [3];  [3];  [3];  [1];  [2];  [3];  [1]
  1. Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering
  2. Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
  3. Texas A & M Univ., College Station, TX (United States). Department of Mechanical Engineering
Publication Date:
Research Org.:
Texas A & M Univ., College Station, TX (United States). Perla B. Balbuena
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Contributing Org.:
Texas A&M High Performance Computing Facilities, and Texas Advanced Computer Center
OSTI Identifier:
1430231
Grant/Contract Number:  
EE0006832
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 5; Journal ID: ISSN 0013-4651
Publisher:
The Electrochemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; 33 ADVANCED PROPULSION SYSTEMS; density functional theory; ab initio; molecular dynamics; mesoscale modeling; sonochemical synthesis

Citation Formats

Dysart, Arthur D., Burgos, Juan C., Mistry, Aashutosh, Chen, Chien-Fan, Liu, Zhixiao, Hong, Chulgi Nathan, Balbuena, Perla B., Mukherjee, Partha P., and Pol, Vilas G. Towards Next Generation Lithium-Sulfur Batteries: Non-Conventional Carbon Compartments/Sulfur Electrodes and Multi-Scale Analysis. United States: N. p., 2016. Web. doi:10.1149/2.0481605jes.
Dysart, Arthur D., Burgos, Juan C., Mistry, Aashutosh, Chen, Chien-Fan, Liu, Zhixiao, Hong, Chulgi Nathan, Balbuena, Perla B., Mukherjee, Partha P., & Pol, Vilas G. Towards Next Generation Lithium-Sulfur Batteries: Non-Conventional Carbon Compartments/Sulfur Electrodes and Multi-Scale Analysis. United States. doi:10.1149/2.0481605jes.
Dysart, Arthur D., Burgos, Juan C., Mistry, Aashutosh, Chen, Chien-Fan, Liu, Zhixiao, Hong, Chulgi Nathan, Balbuena, Perla B., Mukherjee, Partha P., and Pol, Vilas G. Tue . "Towards Next Generation Lithium-Sulfur Batteries: Non-Conventional Carbon Compartments/Sulfur Electrodes and Multi-Scale Analysis". United States. doi:10.1149/2.0481605jes. https://www.osti.gov/servlets/purl/1430231.
@article{osti_1430231,
title = {Towards Next Generation Lithium-Sulfur Batteries: Non-Conventional Carbon Compartments/Sulfur Electrodes and Multi-Scale Analysis},
author = {Dysart, Arthur D. and Burgos, Juan C. and Mistry, Aashutosh and Chen, Chien-Fan and Liu, Zhixiao and Hong, Chulgi Nathan and Balbuena, Perla B. and Mukherjee, Partha P. and Pol, Vilas G.},
abstractNote = {In this work, a novel heterofunctional, bimodal-porous carbon morphology, termed the carbon compartment (CC), is utilized as a sulfur host as a lithium-sulfur battery cathode. A multi-scale model explores the physics and chemistry of the lithium-sulfur battery cathode. The CCs are synthesized by a rapid, low cost process to improve electrode-electrolyte interfacial contact and accommodate volumetric expansion associated with sulfide formation. The CCs demonstrate high sulfur loading (47 %-wt. S) and ca. 700 mAh g-1 reversible capacity with high coulombic efficiency due to their unique structures. Density functional theory and ab initio Molecular Dynamics characterize the interface between the C/S composite and electrolyte during the sulfur reduction mechanism. Stochastic realizations of 3D electrode microstructures are reconstructed based on representative SEM images to study the influence of solid sulfur loading and lithium sulfide precipitation on microstructural and electrochemical properties. A macroscale electrochemical performance model is developed to analyze the performance of lithium-sulfur batteries. The combined multi-scale simulation studies explain key fundamentals of sulfur reduction and its relation to the polysulfide shuttle mechanism: how the process is affected due to the presence of carbon substrate, thermodynamics of lithium sulfide formation and deposition on carbon, and microstructural effects on the overall cell performance.},
doi = {10.1149/2.0481605jes},
journal = {Journal of the Electrochemical Society},
number = 5,
volume = 163,
place = {United States},
year = {2016},
month = {2}
}

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    Works referencing / citing this record:

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