Electronic Structure Engineering of Honeycomb Layered Cathode Material for Sodium-Ion Batteries
Voronina N. Kim H.J. Konarov A. Yaqoob N. Lee K.-S. Kaghazchi P. Guillon O. Myung S.-T.
April 15, 2021John Wiley and Sons Inc
Advanced Energy Materials
2021#11Issue 14
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.
batteries , cathodes , electronic structure , layered , sodium
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Hybrid Materials Research Center, Department of Nano Technology and Advanced Materials Engineering, Sejong Battery Institute, Sejong University, Seoul, 05006, South Korea
Department of Chemical and Materials Engineering, School of Engineering and Digital Sciences, Nazarbayev University, 53 Kabanbay Batyr Avenue, Nur-Sultan, 010000, Kazakhstan
Forschungszentrum Jülich GmbH, Institute of Energy and Climate Research, Materials Synthesis and Processing (IEK-1), Jülich, 52428, Germany
Pohang Accelerator Laboratory, 80 Jigokro-127-beongil, Nam-gu, Pohang, 37673, Gyeongbuk, South Korea
Hybrid Materials Research Center
Department of Chemical and Materials Engineering
Forschungszentrum Jülich GmbH
Pohang Accelerator Laboratory
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