TY - JOUR
T1 - Operando characterization of intermediates produced in a lithium-sulfur battery
AU - Gorlin, Yelena
AU - Siebel, Armin
AU - Piana, Michele
AU - Huthwelker, Thomas
AU - Jha, Himendra
AU - Monsch, Georg
AU - Kraus, Florian
AU - Gasteiger, Hubert A.
AU - Tromp, Moniek
N1 - Publisher Copyright:
© The Author(s) 2015.
PY - 2015
Y1 - 2015
N2 - One of the technological barriers to electrification of transport is the insufficient storage capacity of the Li-ion batteries on which the current electric cars are based. The lithium-sulfur (Li-S) battery is an advanced technology whose successful commercialization can lead to significant gains in the storage capacity of batteries and promote wide-spread adoption of electric vehicles. Recently, important Li-S intermediates, including polysulfides, S3•-, and Li2S, have been shown to present unique X-ray absorption near edge structure (XANES) features at the sulfur K-edge. As a result, a combination of XANES characterization with electrochemistry has the potential to contribute to the understanding of Li-S chemistry. In this study, we present an operando XANES cell design, benchmark its electrochemical and spectroscopic performance, and use it to track reaction intermediates during the discharge of the battery. In particular, by employing electrolyte solvents with either a high or a low dielectric constant, we investigate the influence of the solvent on the conversion of polysulfide species to Li2S. Our results reveal that Li2S is already formed after ∼25-30% discharge in both types of electrolyte solvents, but that further conversion of polysulfides to Li2S proceeds more rapidly in a solvent with a low dielectric constant.
AB - One of the technological barriers to electrification of transport is the insufficient storage capacity of the Li-ion batteries on which the current electric cars are based. The lithium-sulfur (Li-S) battery is an advanced technology whose successful commercialization can lead to significant gains in the storage capacity of batteries and promote wide-spread adoption of electric vehicles. Recently, important Li-S intermediates, including polysulfides, S3•-, and Li2S, have been shown to present unique X-ray absorption near edge structure (XANES) features at the sulfur K-edge. As a result, a combination of XANES characterization with electrochemistry has the potential to contribute to the understanding of Li-S chemistry. In this study, we present an operando XANES cell design, benchmark its electrochemical and spectroscopic performance, and use it to track reaction intermediates during the discharge of the battery. In particular, by employing electrolyte solvents with either a high or a low dielectric constant, we investigate the influence of the solvent on the conversion of polysulfide species to Li2S. Our results reveal that Li2S is already formed after ∼25-30% discharge in both types of electrolyte solvents, but that further conversion of polysulfides to Li2S proceeds more rapidly in a solvent with a low dielectric constant.
UR - http://www.scopus.com/inward/record.url?scp=84929455684&partnerID=8YFLogxK
U2 - 10.1149/2.0081507jes
DO - 10.1149/2.0081507jes
M3 - Article
AN - SCOPUS:84929455684
SN - 0013-4651
VL - 162
SP - A1146-A1155
JO - Journal of the Electrochemical Society
JF - Journal of the Electrochemical Society
IS - 7
ER -