Vanadium redox flow batteries (VRFBs) have shown to be a promising technology for integrating intermittent renewable energy sources into the existing electrical grid. Incorporation of carbon cloth electrodes into VRFB is an area of interest for their enhanced electrochemical performance, however, issues with performance degradation throughout the duration of the experiment persist. This study investigates the performance evolution of carbon cloth electrodes during VRFB cycling to build a hypothesis on possible reasons for the declining performance. Electrochemical impedance spectroscopy and polarization curve measurements are used in conjunction to monitor the electrode degradation and shed light on the effectiveness of carbon cloth electrodes during extended cycling experiments. A detailed investigation into the structure of the carbon cloth electrodes before and after cycling, via several material characterization tests, provides insight needed to determine an explanation for the increasing resistance. The structural integrity and surface morphology of the carbon cloth electrodes are evaluated to compare the electrode before and after cycling, displaying any changes to the electrode due to cycling. Durability of hydrophilicity during RFB cycling is found to be a key feature for future carbon cloth electrode design efforts.
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Jadhav, Ankur L. ; Juran, Taylor R. ; Kim, Matthew A. ; Bruck, Andrea M. ; Hawkins, Brendan E. ; Gallaway, Joshua W. ; Smeu, Manuel ; Messinger, Robert J. ( , Journal of the American Chemical Society)
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Stavola, Alyssa M. ; Sun, Xiao ; Guida, Dominick P. ; Bruck, Andrea M. ; Cao, Daxian ; Okasinski, John S. ; Chuang, Andrew C. ; Zhu, Hongli ; Gallaway, Joshua W. ( , ACS Energy Letters)
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Sun, Xiao ; Stavola, Alyssa M. ; Cao, Daxian ; Bruck, Andrea M. ; Wang, Ying ; Zhang, Yunlu ; Luan, Pengcheng ; Gallaway, Joshua W. ; Zhu, Hongli ( , Advanced Energy Materials)
Abstract Sulfide solid‐state electrolytes have remarkable ionic conductivity and low mechanical stiffness but suffer from relatively narrow electrochemical and chemical stability with electrodes. Therefore, pairing sulfide electrolytes with the proper cathode is crucial in developing stable all‐solid‐state Li batteries (ASLBs). Herein, one type of thioantimonate ion conductor, Li6+
x Gex Sb1−x S5I, with different compositions is systematically synthesized and studied, among these compositions, an outstanding ionic conductivity of 1.6 mS cm−1is achieved with Li6.6Ge0.6Sb0.4S5I. To improve the energy density and advance the interface compatibility, a metal sulfide FeS2cathode with a high theoretical capacity (894 mAh g−1) and excellent compatibility with sulfide electrolytes is coupled with Li6.6Ge0.6Sb0.4S5I in ASLBs without additional interface engineering. The structural stabilities of Li6.6Ge0.6Sb0.4S5I and FeS2during cycling are characterized by operando energy dispersive X‐ray diffraction, which allows rapid collection of structural data without redesigning or disassembling the sealed cells and risking contamination by air. The electrochemical stability is assessed, and a safe operating voltage window ranging from 0.7≈2.4 V (vs. In–Li) is confirmed. Due to the solid confinement in the ASLBs, the Fe0aggregation and polysulfides shuttle effects are well addressed. The ASLBs exhibit an outstanding initial capacity of 715 mAh g−1at C/10 and are stable for 220 cycles with a high capacity retention of 84.5% at room temperature.