TY - JOUR
T1 - Understanding Electrochemical Sulfur-Based Phase Evolution via Complementary Insight from Operando Spatially Resolved X-ray Diffraction and X-ray Absorption Spectroscopy
AU - Quilty, Calvin D.
AU - Hill, Ryan C.
AU - Dunkin, Mikaela R.
AU - Rodriguez Campos, Armando
AU - Kingan, Arun
AU - Von Stein, Nicholas
AU - Housel, Lisa M.
AU - Takeuchi, Esther S.
AU - Okasinski, John
AU - Du, Yonghua
AU - Wierzbicki, Dominik
AU - Zhong, Hui
AU - Zhong, Zhong
AU - Vo, Nghia T.
AU - Drakopoulos, Michael
AU - Wang, Lei
AU - Marschilok, Amy C.
AU - Yan, Shan
AU - Takeuchi, Kenneth J.
N1 - Publisher Copyright:
© 2025 The Authors. Published by American Chemical Society
PY - 2025
Y1 - 2025
N2 - Lithium/sulfur batteries are emerging as promising candidates for use in large-scale energy storage, but practical challenges, including insufficient power density and polysulfide shuttling, remain. This work presents the first use of operando energy dispersive X-ray diffraction (EDXRD) to monitor Li/S electrochemistry within a liquid electrolyte. Complementary operando synchrotron-based EDXRD, X-ray absorption spectroscopy (XAS), X-ray powder diffraction (XPD), and ex situ laboratory Raman analysis provide evidence for α-S8conversion upon discharge into Li2Sxpolysulfide phases and conversion into β-S8during charge. Understanding the underlying mechanisms of sulfur reduction and oxidation within thick electrodes will enable advances in next-generation Li/S batteries and material design.
AB - Lithium/sulfur batteries are emerging as promising candidates for use in large-scale energy storage, but practical challenges, including insufficient power density and polysulfide shuttling, remain. This work presents the first use of operando energy dispersive X-ray diffraction (EDXRD) to monitor Li/S electrochemistry within a liquid electrolyte. Complementary operando synchrotron-based EDXRD, X-ray absorption spectroscopy (XAS), X-ray powder diffraction (XPD), and ex situ laboratory Raman analysis provide evidence for α-S8conversion upon discharge into Li2Sxpolysulfide phases and conversion into β-S8during charge. Understanding the underlying mechanisms of sulfur reduction and oxidation within thick electrodes will enable advances in next-generation Li/S batteries and material design.
UR - https://www.scopus.com/pages/publications/105017859132
U2 - 10.1021/acs.jpclett.5c01902
DO - 10.1021/acs.jpclett.5c01902
M3 - Article
C2 - 41042707
AN - SCOPUS:105017859132
SN - 1948-7185
VL - 16
SP - 10558
EP - 10567
JO - Journal of Physical Chemistry Letters
JF - Journal of Physical Chemistry Letters
ER -