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Rietveld refinement results suggest the as-produced LNMO and LNRO samples fit the structural model of monoclinic solid solution, though the nanocomposite concept concerning the mixture of layered Li Ni O (LNRO).

a Synchrotron XRD patterns, showing a similar crystal structure between these two compounds; XRD Rietveld refinement of b LNMO based on monoclinic C2/m and c LNRO based on monoclinic C2/c; d scanning electron microscopy (SEM) image of LNMO, the scale bar is 1 μm; e, f high-resolution transmission electron microscopy (HRTEM) images of LNMO with fast Fourier transform (FTT) of the selected area, the scale bar in (e) and (f) is 50 and 5 nm, respectively; g electron diffraction (ED) pattern for LNMO; h SEM image of LNRO, the scale bar is 1 μm; i, j HRTEM images of LNRO with FTT of the selected area, the scale bar in (i) and (j) is 100 and 2 nm, respectively; k ED pattern for LNROScanning electron microscopy (SEM) and high-resolution transmission electron microscopy (HRTEM) were used to further verify the morphology and crystal structure.

The above mentioned models consider different transition metals (i.e., 3d, 4d, and 5d) that have different preference for TM-O hybridization might make the complex anionic oxygen redox even more elusive.

Fundamental understanding of anionic oxygen redox is of critical importance to propose effective material design strategy to develop novel materials that harness active oxygen redox.

The first cycle voltage profiles and gas evolution rates of a LNMO and b LNRO.

The total active cathode material used for the measurement was 32.9 mg LNMO (387 μmol) and 28.6 mg LNRO (253 μmol).

The structural and electrochemical characterization of LNMO and LNRO compounds reveal three interesting observations: (1) the compounds possess a similar crystal structure, (2) they allow a similar amount of Li removal on the initial charge, but (3) they have remarkably different charge profiles (voltage plateau at 4.55 V for LNMO vs. Given these unique features, LNMO and LNRO might be suitable model compounds to investigate the underlying oxygen activation mechanisms in the high-voltage region.

The first cycle voltage profile of a LNMO and b LNRO; differential capacity (d Q/d V) plot of c LNMO and d LNRO.

Cells were cycled between 4.8 and 2.0 V at a current density of 5 m A g Despite this similarity, these two compounds exhibited noticeably different charge characteristics.

This difference was even more pronounced in the differential capacity (d Q/d V) plots (Fig. The charge profile of LNMO was characterized by a strong anodic peak at 4.55 V, corresponding to the extended voltage plateau, as well as two weak anodic peaks around 3.8 and 4.1 V.

In comparison, the strong anodic peak in the high-voltage region was absent in the charge profile of LNRO (Fig.

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Both electron diffraction (ED) patterns and fast Fourier transformation results along the [001] and [30] zone axis of C2/m and C2/c from LNMO and LNRO particle showed high structural consistency.