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Manipulating the local electronic structure is employed to address the capacity/voltage decay and poor rate capability of Li-rich layered cathodes (LLOs) via the dual-doping of Na+ and F− ions, as well as the regulation of Li+/Ni2+ intermixing and the content of 'Li-O-Li' configuration. The designed cathode exhibits a high initial Coulombic efficiency of about 90%, large specific capacity of 296 mAh g−1 and energy density of 1047 Wh kg−1 at 0.2 C, and a superior rate capability of 222 mAh g−1 at 5 C with a good capacity retention of 85.7% even after 500 cycles. And the operating voltage is increased without compromising the high-capacity advantage. Such improved electrochemical performances primarily result from the band shift of the TM 3d-O 2p and non-bonding O-2p to lower energy, which would decrease Li+ diffusion activation energy and increase oxygen vacancy forming energy, finally improving the Li+ diffusion kinetics and stabilizing lattice oxygen. Moreover, the increased 'Li-O-Li' configuration in the Li2MnO3 phase via increasing the Mn concentration can increase the reversible capacity to offset the negative effect of inactive doping and Li+/Ni2+ intermixing. This strategy of modulating the local electronic structure of LLOs provides great potential to design high-energy-density Li-ion batteries. © 2021 Wiley-VCH GmbH
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Advanced Functional Materials
ISSN: 1616-301X
Year: 2021
Issue: 30
Volume: 31
1 9 . 9 2 4
JCR@2021
1 8 . 5 0 0
JCR@2023
ESI HC Threshold:142
JCR Journal Grade:1
CAS Journal Grade:1
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ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 2
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