TY - JOUR
T1 - Enhancing structural flexibility in P2-type Ni-Mn-based Na-layered cathodes for high power-capability and fast charging/discharging performance
AU - Ku, Bonyoung
AU - Ahn, Jinho
AU - Lee, Hoseok
AU - Ahn, Hobin
AU - Lee, Jihoe
AU - Kweon, Hyunji
AU - Choi, Myungeun
AU - Jung, Hun Gi
AU - Ihm, Kyuwook
AU - Sim, Eunji
AU - Yoo, Jung Keun
AU - Kim, Jongsoon
N1 - Publisher Copyright:
© 2024
PY - 2025/1
Y1 - 2025/1
N2 - P2-type Ni-Mn-based Na-layered cathodes suffer from severely large structural changes, such as the direct P2-O2 phase transition, occurring during charging to the high voltage region, resulting in the poor power-capability with large overpotential, as well as the diminished cycle-performance. In this study, through a combination of first-principles calculations and various experiments, we demonstrate that enhanced structural flexibility through Co-Al co-substitution provides smooth and continuous structural changes in the P2-type Ni-Mn-based Na-layered cathode without the direct phase transition, enabling the highly improved electrochemical performances. P2-type Na0.67[Ni0.35Co0.1Mn0.5Al0.05]O2 delivers a high discharge capacity of approximately ∼156.31 mAh g−1 and an energy density of ∼551.71 Wh kg−1 at 10 mA g−1, outperforming P2-type Na0.67[Ni0.35Mn0.65]O2. These performance differences are especially pronounced during fast charging/discharging process, highlighting the enhanced power-capability and Na+ diffusion kinetics due to improved structural flexibility. Moreover, smooth and continuous structural changes enable improved cycle performance, including reduced voltage decay during prolonged cycling, for P2-type Na0.67[Ni0.35Co0.1Mn0.5Al0.05]O2. These results highlight that introducing structural flexibility is one of the most efficient ways to enhance power-capability and fast-charging/discharging performance in P2-type Ni-Mn-based Na-layered cathodes, while also improving cyclability.
AB - P2-type Ni-Mn-based Na-layered cathodes suffer from severely large structural changes, such as the direct P2-O2 phase transition, occurring during charging to the high voltage region, resulting in the poor power-capability with large overpotential, as well as the diminished cycle-performance. In this study, through a combination of first-principles calculations and various experiments, we demonstrate that enhanced structural flexibility through Co-Al co-substitution provides smooth and continuous structural changes in the P2-type Ni-Mn-based Na-layered cathode without the direct phase transition, enabling the highly improved electrochemical performances. P2-type Na0.67[Ni0.35Co0.1Mn0.5Al0.05]O2 delivers a high discharge capacity of approximately ∼156.31 mAh g−1 and an energy density of ∼551.71 Wh kg−1 at 10 mA g−1, outperforming P2-type Na0.67[Ni0.35Mn0.65]O2. These performance differences are especially pronounced during fast charging/discharging process, highlighting the enhanced power-capability and Na+ diffusion kinetics due to improved structural flexibility. Moreover, smooth and continuous structural changes enable improved cycle performance, including reduced voltage decay during prolonged cycling, for P2-type Na0.67[Ni0.35Co0.1Mn0.5Al0.05]O2. These results highlight that introducing structural flexibility is one of the most efficient ways to enhance power-capability and fast-charging/discharging performance in P2-type Ni-Mn-based Na-layered cathodes, while also improving cyclability.
KW - First-principle calculation
KW - High voltage
KW - Na-ion batteries
KW - Oxygen redox
KW - Stabilization
UR - https://www.scopus.com/pages/publications/85210536285
U2 - 10.1016/j.ensm.2024.103930
DO - 10.1016/j.ensm.2024.103930
M3 - Article
AN - SCOPUS:85210536285
SN - 2405-8297
VL - 74
JO - Energy Storage Materials
JF - Energy Storage Materials
M1 - 103930
ER -
