Study of Earth-Abundant, Mn-Rich Cathodes for Vehicle Applications and Beyond

Chen, Jiajun

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Study of Earth-Abundant, Mn-Rich Cathodes for Vehicle Applications and Beyond

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The development of sustainable materials for lithium-ion batteries (LIB) is of paramount significance with the ever-growing demand of energy storage for the transportation sector. Lithium- and manganese-rich (LMR) oxides are of great interests because of inherently high capacities/energies and the potential economic benefits associated with earth-abundant manganese-based compositions. However, despite the attractive properties discussed above, LMR commercialization has been hindered by several challenges. This research addresses challenges spanning from atomic to cell levels. First, the synthesis and morphological control of LMR cathode precursors are significant for LIB performance. A deep comprehensive fundamental understanding of synthetic mechanisms and kinetics has been conducted for further optimization and better control of the processing and morphology of the particle. Delving into foundational mechanisms, the complex local structure of these oxides results in unique electrochemical behavior including the participation of oxygen in the redox processes, voltage fade accompanied by a voltage hysteresis (energy inefficiency), surface instabilities leading to capacity loss, and rising impedance with cycling along with striking impedance behavior at low SOCs. This study presents a comprehensive study of one of the most significant issues facing LMRs, an anomalous rise in area specific impedance at low SOCs, as well as overall impedance rise and surface damage due to electrolyte interactions. Finally, considering real-world implications, the last part of this study focuses on electrode engineering and combining experimental data with techno-economic modeling to evaluate Co-free LMR cathodes in comparison to other commercial cathode materials. The work presented herein endeavors to bridge the knowledge gap across various length-scales, from atomic-level complexity to broader cell-level implications, to innovate and enhance the realm of LMR cathodes for LIB.

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