Premium
Theoretical Studies on the Charging and Discharging of Poly(acrylonitrile)‐Based Lithium‐Sulfur Batteries
Author(s) -
Zhu Tianwei,
Mueller Jonathan E.,
Hanauer Matthias,
Sauter Ulrich,
Jacob Timo
Publication year - 2017
Publication title -
chemelectrochem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.182
H-Index - 59
ISSN - 2196-0216
DOI - 10.1002/celc.201700549
Subject(s) - polysulfide , acrylonitrile , cathode , battery (electricity) , sulfur , density functional theory , adsorption , lithium (medication) , chemistry , ion , molecule , materials science , chemical physics , chemical engineering , computational chemistry , electrode , polymer , organic chemistry , thermodynamics , electrolyte , physics , medicine , power (physics) , copolymer , engineering , endocrinology
Based on a previous study where key structural motifs of poly(acrylonitrile) (PAN) and sulfur/PAN (SPAN) were identified and their energies evaluated by using density functional theory, here plausible mechanisms for battery charging and discharging at a SPAN cathode were identified. Based on a simplified model for battery operation, we find that discharging the battery involves the formation of lithium polysulfide intermediates and the reductive adsorption of Li + ions onto S n PAN. In both discharging and charging, Li atoms preferentially coordinate with N atoms on the backbone, leading to strong Li‐S n PAN adsorption energies. Furthermore, we found that spatially separating a dissociated S n Li fragment from the backbone is difficult, providing a plausible explanation for the ability of a SPAN cathode to hinder polysulfides from diffusing to the cathode, leading to a reduction of the polysulfide shuttle mechanism.