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DOE OSTI · 3001466

Understanding Electrochemical Sulfur-Based Phase Evolution via Complementary Insight from Operando Spatially Resolved X-ray Diffraction and X-ray Absorption Spectroscopy

Quilty, Calvin D. [Stony Brook Univ., NY (United States)]·Hill, Ryan C. [Stony Brook Univ., NY (United States)] (ORCID:0000000273303091)·Dunkin, Mikaela R. [Stony Brook Univ., NY (United States)] (ORCID:0000000303280020)·Rodriguez Campos, Armando [Stony Brook Univ., NY (United States)]·Kingan, Arun [Stony Brook Univ., NY (United States)]·Von Stein, Nicholas [Stony Brook Univ., NY (United States)]·Housel, Lisa M. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Takeuchi, Esther S. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000185181047)·Okasinski, John [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)]·Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X)·Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Zhong, Hui [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Zhong, Zhong [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Vo, Nghia T. [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000236837377)·Drakopoulos, Michael [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)]·Wang, Lei [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Marschilok, Amy C. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000191740474)·Yan, Shan [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000297159100)·Takeuchi, Kenneth J. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:000000018129444X)
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Abstract

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. Here, 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-S 8 conversion upon discharge into Li 2 S x polysulfide phases and conversion into β-S 8 during 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.

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36 MATERIALS SCIENCEX-ray diffractionX-ray spectroscopyelectrochemical conversionlithium batterylithium sulfur batteryoperando

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Quilty, Calvin D. [Stony Brook Univ., NY (United States)], Hill, Ryan C. [Stony Brook Univ., NY (United States)] (ORCID:0000000273303091), Dunkin, Mikaela R. [Stony Brook Univ., NY (United States)] (ORCID:0000000303280020), Rodriguez Campos, Armando [Stony Brook Univ., NY (United States)], Kingan, Arun [Stony Brook Univ., NY (United States)], Von Stein, Nicholas [Stony Brook Univ., NY (United States)], Housel, Lisa M. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)], Takeuchi, Esther S. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000185181047), Okasinski, John [Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)], Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X), Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Zhong, Hui [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Zhong, Zhong [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Vo, Nghia T. [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000236837377), Drakopoulos, Michael [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)], Wang, Lei [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)], Marschilok, Amy C. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000191740474), Yan, Shan [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000297159100), Takeuchi, Kenneth J. [Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:000000018129444X). 2025-10-03. Understanding Electrochemical Sulfur-Based Phase Evolution via Complementary Insight from Operando Spatially Resolved X-ray Diffraction and X-ray Absorption Spectroscopy. https://doi.org/10.1021/acs.jpclett.5c01902

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36 MATERIALS SCIENCE↗