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• W2047113715 startingPage "1760" @default.
• W2047113715 abstract "Much of current research in electrochemical energy storage is devoted to new electrode chemistries and reaction mechanisms that promise substantial increases in energy density. Unfortunately, most high capacity electrodes exhibit an unacceptably large hysteresis in their voltage profile. Using a first-principles multi-scale approach to examine particle level dynamics, we identify intrinsic thermodynamic and kinetic properties that are responsible for the large hysteresis exhibited by many high capacity electrodes. Our analysis shows that the hysteresis in the voltage profile of high capacity electrodes that rely on displacement reactions arises from a difference in reaction paths between charge and discharge. We demonstrate that different reaction paths are followed (i) when there is a large mismatch in ionic mobilities between the electrochemically active species (e.g. Li) and displaced ionic species and (ii) when there is a lack of a thermodynamic driving force to redistribute displaced ions upon charging of the electrode. These insights motivate the formulation of design metrics for displacement reactions in terms of fundamental properties determined by the chemistry and crystallography of the electrode material, properties that are now readily accessible with first-principles computation." @default.
• W2047113715 created "2016-06-24" @default.
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• W2047113715 date "2014-01-01" @default.
• W2047113715 modified "2023-10-07" @default.
• W2047113715 title "Designing the next generation high capacity battery electrodes" @default.
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• W2047113715 doi "https://doi.org/10.1039/c3ee43154a" @default.
• W2047113715 hasPublicationYear "2014" @default.
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