Advancing the Performance of Lithium-Rich Oxides in Cooperation with Inherent Complexities: Engineering Domain Structure

Garcia, Juan C. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000259118850); Iddir, Hakim [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000152856474); Gutierrez, Arturo [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000228993089); Mallick, Subhadip [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000251088845); Lin, Yulin [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)]; Wen, Jianguo [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000237550044); Dogan, Fulya [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:000000017997266X); Adhikari, Hari [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0009000626860756); Croy, Jason R. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000258393666)

doi:10.1021/acs.chemmater.5c00828

DOE OSTI · 3374428

Advancing the Performance of Lithium-Rich Oxides in Cooperation with Inherent Complexities: Engineering Domain Structure

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Abstract

The nanodomain structure of lithium- and manganese-rich, composite cathode materials has been systematically altered through synthesis conditions while keeping larger-scale morphological differences to a minimum. Clear changes in electrochemical performance across the samples studied are observed, especially with respect to the anomalous impedance at low states-of-charge. Atomic-scale modeling, coupled to electrochemical measurements and physical characterization, reveals the local consequences of the high-voltage activation charge process as a function of specific domain structures. Furthermore, the results explain the influence of different postactivation structures on the insertion of Li-ions and the associated impedance during discharge. This work adds to our series of studies on lithium- and manganese-rich oxides, demonstrating that the inherent performance of LMRs can be greatly enhanced through rational, highly controlled synthetic strategies based on an understanding of synthesis–structure–property relationships across length scales.

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Garcia, Juan C. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000259118850), Iddir, Hakim [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000152856474), Gutierrez, Arturo [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000228993089), Mallick, Subhadip [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000251088845), Lin, Yulin [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)], Wen, Jianguo [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0000000237550044), Dogan, Fulya [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:000000017997266X), Adhikari, Hari [Argonne National Laboratory (ANL), Argonne, IL (United States). Center for Nanoscale Materials (CNM)] (ORCID:0009000626860756), Croy, Jason R. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000258393666). 2025-08-18. Advancing the Performance of Lithium-Rich Oxides in Cooperation with Inherent Complexities: Engineering Domain Structure. https://doi.org/10.1021/acs.chemmater.5c00828

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