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

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.

doi:10.1149/2.0481605jes

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

Journal Article · Tue Feb 09 04:00:00 UTC 2016 · Journal of the Electrochemical Society

DOI: https://doi.org/10.1149/2.0481605jes · OSTI ID:1430231

Dysart, Arthur D. ^[1]; Burgos, Juan C. ^[2]; Mistry, Aashutosh ^[3]; Chen, Chien-Fan ^[3]; Liu, Zhixiao ^[3]; Hong, Chulgi Nathan ^[4]; Balbuena, Perla B. ^[2]; Mukherjee, Partha P. ^[3]; Pol, Vilas G. ^[4]

Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering; TexasA&M University
Texas A & M Univ., College Station, TX (United States). Department of Chemical Engineering
Texas A & M Univ., College Station, TX (United States). Department of Mechanical Engineering
Purdue Univ., West Lafayette, IN (United States). School of Chemical Engineering

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.

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Research Organization:: Texas A & M Univ., College Station, TX (United States). Perla B. Balbuena

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Contributing Organization:: Texas A&M High Performance Computing Facilities, and Texas Advanced Computer Center

Grant/Contract Number:: EE0006832

OSTI ID:: 1430231

Journal Information:: Journal of the Electrochemical Society, Journal Name: Journal of the Electrochemical Society Journal Issue: 5 Vol. 163; ISSN 0013-4651

Publisher:: The Electrochemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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