Understanding Electrochemical Sulfur-Based Phase Evolution via Complementary Insight from <i>Operando</i> Spatially Resolved X-ray Diffraction and X-ray Absorption Spectroscopy
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 <i>operando</i> energy dispersive X-ray diffraction (EDXRD) to monitor Li/S electrochemistry within a liquid electrolyte. Complementary <i>operando</i> synchrotron-based EDXRD, X-ray absorption spectroscopy (XAS), X-ray powder diffraction (XPD), and <i>ex situ</i> laboratory Raman analysis provide evidence for α-S<sub>8</sub> conversion upon discharge into Li<sub>2</sub>S<sub><i>x</i></sub> polysulfide phases and conversion into β-S<sub>8</sub> 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.
Authors
- Ryan C. Hill (ORCID: https://orcid.org/0000-0002-7330-3091)
- Amy C. Marschilok (ORCID: https://orcid.org/0000-0001-9174-0474)
- Nghia T. Vo (ORCID: https://orcid.org/0000-0002-3683-7377)
- Lisa M. Housel (ORCID: https://orcid.org/0000-0001-8429-5480)
- Nicolas Stein (ORCID: https://orcid.org/0000-0003-3247-0085)
- Dominik Wierzbicki (ORCID: https://orcid.org/0000-0003-0558-7405)
- Michael Drakopoulos (ORCID: https://orcid.org/0000-0001-8219-5136)
- Kenneth J. Takeuchi (ORCID: https://orcid.org/0000-0001-8129-444X)
- Esther S. Takeuchi (ORCID: https://orcid.org/0000-0001-8518-1047)
- John Okasinski (ORCID: https://orcid.org/0000-0001-9056-0623)
- Calvin D. Quilty (ORCID: https://orcid.org/0000-0002-0294-6815)
- Armando Rodriguez Campos (ORCID: https://orcid.org/0000-0003-3050-5926)
- Shan Yan (ORCID: https://orcid.org/0000-0002-9715-9100)
- Mikaela R. Dunkin (ORCID: https://orcid.org/0000-0003-0328-0020)
- Yonghua Du (ORCID: https://orcid.org/0000-0003-2655-045X)
- Zhong Zhong (ORCID: https://orcid.org/0000-0002-6145-2698)
- Lei Wang (ORCID: https://orcid.org/0000-0002-6348-8344)
- A. Kingan (ORCID: https://orcid.org/0000-0001-8344-5221)
- Hui Zhong
Institutions
- Argonne National Laboratory (US)
- Brookhaven National Laboratory (US)
- Sustainability Institute (ZA)
- Stanford Synchrotron Radiation Lightsource (US)
- National Synchrotron Light Source II
- Stony Brook University (US)
Publication Details
- Journal
- The Journal of Physical Chemistry Letters
- Published
- 2025-10-03
- DOI
- https://doi.org/10.1021/acs.jpclett.5c01902
- Primary Topic
- Chalcogenide Semiconductor Thin Films
- Type
- article
- Field-Weighted Citation Impact
- 0.00