Elucidating the Discharge Behavior of Aqueous Zinc Sulfur Batteries in the Presence of Molybdenum(IV) Chalcogenide Catalyst: The Criticality of Interfacial Electrochemistry

作者：Zhongling Wang, Jason Kuang, Armando Rodriguez-Campos, Chuntian Cao, A. Kingan, Patrick J. Barry, Ryan C. Hill, David J. Arnot, Adora Christianne, David C. Bock, Yonghua Du, Seong‐Min Bak, Lu Ma, Dali Yang, Akhil Tayal, Michael Drakopoulos, Zhong Zhong, Nghia T. Vo, Kim Kisslinger, Xiao Tong, Esther S. Takeuchi, Matthew R. Carbone, Deyu Lu, Lei Wang, Shan Yan, Kenneth J. Takeuchi, Amy C. Marschilok · 发表于：ACS Applied Materials & Interfaces · 年份：2024 · DOI：10.1021/acsami.4c14388 · 被引用次数：6 · 研究领域：Advanced battery technologies research、Electrocatalysts for Energy Conversion、Perovskite Materials and Applications

The aqueous zinc–sulfur battery holds promise for significant capacity and energy density with low cost and safe operation based on environmentally benign materials. However, it suffers from the sluggish kinetics of the conversion reaction. Here, we highlight the efficacy of molybdenum(IV) sulfide (MoS 2 ) to reduce the overpotential of S-ZnS conversion in aqueous electrolytes and study the discharge products formed at the solid–solid and solid–liquid interfaces using experimental and theoretical approaches. Specifically, the MoS 2 -catalyzed electrochemical conversion reaction is characterized via ex situ X-ray diffraction (XRD), transmission electron microscopy (TEM) with energy dispersive spectroscopy (EDS), Raman spectroscopy, synchrotron-based Mo K -edge X-ray absorption spectroscopy (XAS), and in situ synchrotron-based X-ray computed tomography (XCT). Additionally, operando synchrotron-based S K -edge XAS and X-ray fluorescence (XRF) maps are collected to determine the spatial evolution of sulfur-based species at the electrode–electrolyte interface. Coupling the operando S K -edge XAS data with the simulated spectra and fitting the data suggested a possible ZnS 2 intermediate phase.