Publications by authors named "Alison H McCarthy"

Aqueous electrochemical systems suffer from a low energy density due to a small voltage window of water (1.23 V). Using thicker electrodes to increase the energy density and highly concentrated "water-in-salt" (WIS) electrolytes to extend the voltage range can be a promising solution.

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Ni-rich NMC is an attractive Li-ion battery cathode due to its combination of energy density, thermal stability, and reversibility. While higher delivered energy density can be achieved with a more positive charge voltage limit, this approach compromises sustained reversibility. Improved understanding of the local and bulk structural transformations as a function of charge voltage, and their associated impacts on capacity fade are critically needed.

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Iron based materials hold promise as next generation battery electrode materials for Li ion batteries due to their earth abundance, low cost, and low environmental impact. The iron oxide, magnetite Fe3O4, adopts the spinel (AB2O4) structure. Other 2+ cation transition metal centers can also occupy both tetrahedral and/or octahedral sites in the spinel structure including MgFe2O4, a partially inverse spinel, and ZnFe2O4, a normal spinel.

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Article Synopsis
  • The study used synchrotron-based operando energy dispersive X-ray diffraction (EDXRD) to analyze lithiated lithium vanadium oxide (LVO) within thick porous electrodes (TPEs) during cycling.
  • Homogeneous phase transitions were observed across the thickness of the electrodes at multiple cycling stages, confirming uniform lithiation and correlating loss in capacity over cycles to decreasing active material availability.
  • The findings were further supported by continuum modeling and SEM observations of particle fracture, enhancing the understanding of lithium transport properties in high-rate cycling conditions.
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Water-in-salt (WIS) electrolytes provide a promising path toward aqueous battery systems with enlarged operating voltage windows for better safety and environmental sustainability. In this work, a new electrode couple, LiVO-LiMnO, for aqueous Li-ion batteries is investigated to understand the mechanism by which the WIS electrolyte improves the cycling stability at an extended voltage window. Operando synchrotron transmission x-ray microscopy on the LiMnO cathode reveals that the WIS electrolyte suppresses the mechanical damage to the electrode network and dissolution of the electrode particles, in addition to delaying the water decomposition process.

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One of the inherent challenges with Li-S batteries is polysulfide dissolution, in which soluble polysulfide species can contribute to the active material loss from the cathode and undergo shuttling reactions inhibiting the ability to effectively charge the battery. Prior theoretical studies have proposed the possible benefit of defective 2 D MoS materials as polysulfide trapping agents. Herein the synthesis and thorough characterization of hydrothermally prepared MoS nanosheets that vary in layer number, morphology, lateral size, and defect content are reported.

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FeO nanoparticles (NPs) with an average size of 8-10 nm have been successfully functionalized with various surface-treatment agents to serve as model systems for probing surface chemistry-dependent electrochemistry of the resulting electrodes. The surface-treatment agents used for the functionalization of FeO anode materials were systematically varied to include aromatic or aliphatic structures: 4-mercaptobenzoic acid, benzoic acid (BA), 3-mercaptopropionic acid, and propionic acid (PA). Both structural and electrochemical characterizations have been used to systematically correlate the electrode functionality with the corresponding surface chemistry.

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