Li[Lix/3Mn2x/3M1−x]O2 (M = Ni, Mn, Co) (HE-NMC) materials, which can be expressed as a combination of trigonal LiTMO2 (TM = transition metal) and monoclinic Li2MnO3 phases, are of great interest as high capacity cathodes for lithium-ion batteries. However, structural stability prevents their commercial adoption. To address this, Si doping was applied, resulting in improved stability. Raman and differential capacity analyses suggest that silicon doping improves the structural stability during electrochemical cycling. Furthermore, the doped material exhibits a 10% higher capacity relative to the control. The superior capacity likely results from the increased lattice parameters as determined by X-ray diffraction (XRD) and the lower resistance during the first cycle found by impedance and direct current resistance (DCR) measurements. Density functional theory (DFT) predictions suggest that the observed lattice expansion is an indication of increased oxygen vacancy concentration and may be due to the Si doping.
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We gratefully acknowledge support from National Science Foundation under Grant Nos. DMR-1410850 and 1410946 for the collaborative GOALI research. We also thank Tengjiao Qi, Michael Balogh, and Nicholas Pieczonka for their assistance with the experiments and Jung-Hyun Kim for helpful discussions.
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Nation, L., Wu, Y., James, C. et al. Si-doped high-energy Li1.2Mn0.54Ni0.13Co0.13O2 cathode with improved capacity for lithium-ion batteries. Journal of Materials Research 33, 4182–4191 (2018). https://doi.org/10.1557/jmr.2018.378