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

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
 [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:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Journal of the Electrochemical Society
Additional Journal Information:
Journal Volume: 163; Journal Issue: 5; Journal ID: ISSN 0013-4651
The Electrochemical Society
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 Orgs:
Texas A&M High Performance Computing Facilities, and Texas Advanced Computer Center
Country of Publication:
United States
25 ENERGY STORAGE; 33 ADVANCED PROPULSION SYSTEMS; density functional theory; ab initio; molecular dynamics; mesoscale modeling; sonochemical synthesis
OSTI Identifier: