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• W4313454315 endingPage "794" @default.
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• W4313454315 abstract "Ni-containing layered/cation-ordered LiTMO2s (TM = transition metal) suffer from Ni-migration to the Li-layer at the unit cell level, concomitant transformation to a spinel/rock salt structure, hindrance toward Li-transport, and, thus, fading in Li-storage capacity during electrochemical cycling (i.e., repeated delithiation/lithiation), especially upon deep delithiation (i.e., going to high states-of-charge). Against this backdrop, our previously reported work [ACS Appl. Mater. Interfaces 2021, 13, 25836-25849] revealed a new concept toward blocking the Ni-migration pathway by placing Zn2+ (which lacks octahedral site preference) in the tetrahedral site of the Li-layer, which, otherwise, serves as an intermediate site for the Ni-migration to the Li-layer. This, nearly completely, suppressed the Ni-migration, despite being deep delithiated up to a potential of 4.7 V (vs Li/Li+) and, thus, resulted in significant improvement in the high-voltage cyclic stability. In this regard, by way of conducting operando synchrotron X-ray diffraction, operando stress measurements, and 3D atom probe tomography, the present work throws deeper insights into the effects of such Zn-doping toward enhancing the structural-mechanical-compositional integrity of Li-NMCs upon being subjected to deep delithiation. These studies, as reported here, have provided direct lines of evidence toward notable suppression of the variations of lattice parameters of Li-NMCs, including complete prevention of the detrimental c-axis collapse at high states-of-charges and concomitant slower-cum-lower electrode stress development, in the presence of the Zn-dopant. Furthermore, the Zn-dopant has been found to also prevent the formation of Ni-enriched regions at the nanoscaled levels in Li-NMCs (i.e., Li/Ni-segregation or structural densification) even upon being subjected to 100 charge/discharge cycles involving deep delithiation (i.e., up to 4.7 V). Such detailed insights based on direct/real-time lines of evidence, which reveal important correlations between the suppression of Ni-migration and high-voltage compositional-structural-mechanical stability, hold immense significance toward the development of high capacity and stable layered Li-TM-oxide based cathode materials for the next-generation Li-ion batteries." @default.
• W4313454315 created "2023-01-06" @default.
• W4313454315 creator A5010215375 @default.
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• W4313454315 date "2023-01-03" @default.
• W4313454315 modified "2023-09-25" @default.
• W4313454315 title "Understanding the Effects of Tetrahedral Site Occupancy by the Zn Dopant in Li-NMCs toward High-Voltage Compositional–Structural–Mechanical Stability via Operando and 3D Atom Probe Tomography Studies" @default.
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• W4313454315 doi "https://doi.org/10.1021/acsami.2c15054" @default.
• W4313454315 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/36594652" @default.
• W4313454315 hasPublicationYear "2023" @default.
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