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001     894489
005     20240711085650.0
024 7 _ |a 10.1002/aenm.202003399
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037 _ _ |a FZJ-2021-03252
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100 1 _ |a Voronina, Natalia
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245 _ _ |a Electronic Structure Engineering of Honeycomb Layered Cathode Material for Sodium‐Ion Batteries
260 _ _ |a Weinheim
|c 2021
|b Wiley-VCH
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520 _ _ |a In this work, the rational design of O′3-type Na[Ni2/3−xCoxSb1/3]O2, a solid solution of Na[Ni2/3Sb1/3]O2–Na[Co2/3Sb1/3]O2, is introduced. Because of the difficulty of the Co3+/2+ redox reaction, the electronic structures of Na[Ni2/3−xCoxSb1/3]O2 compounds are engineered to build electroconducting networks in the oxide matrix through electrochemical oxidation of Co2+ to Co3+, after which the formed Co3+ does not participate in the electrochemical reaction but improves the electrical conductivity in the structure. Density functional theory calculations reveal a reduced bandgap energy after the formation of Co3+ during desodiation of Na1−y[Ni2/3−xCoxSb1/3]O2. Using the oxidized Co3+ species while improving the electrical conductivity, the Na[Ni2/3−xCoxSb1/3]O2 (x = 1/6) electrode exhibits excellent cyclability for 1000 cycles with ≈72.5% capacity retention at 2C (400 mA g−1) and activity even at 50C (10 A g−1) in Na cells. Operando X-ray diffraction and ex situ X-ray absorption near-edge structure investigations reveal suppressed lattice variations upon charge and discharge compared with those of Na[Ni2/3Sb1/3]O2 achieved by the presence of the electrochemical-driven Co3+ in the structure. These findings offer a new strategy for the development of cathode materials for sodium-ion batteries, providing important insight into their structural transformations and the electronic nature of advanced cathode materials.
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700 1 _ |a Kim, Hee Jae
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700 1 _ |a Konarov, Aishuak
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700 1 _ |a Yaqoob, Najma
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700 1 _ |a Lee, Kug-Seung
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700 1 _ |a Kaghazchi, Payam
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700 1 _ |a Guillon, Olivier
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700 1 _ |a Myung, Seung-Taek
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773 _ _ |a 10.1002/aenm.202003399
|g Vol. 11, no. 14, p. 2003399 -
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856 4 _ |u https://juser.fz-juelich.de/record/894489/files/Advanced%20Energy%20Materials%20-%202021%20-%20Voronina%20-%20Electronic%20Structure%20Engineering%20of%20Honeycomb%20Layered%20Cathode%20Material%20for.pdf
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