Synergetic Lattice and Surface Engineering: Stable High-Voltage Cycle Performance in P3-Type Layered Manganese Oxide
Voronina N. Köster K. Yu J.H. Kim S. Kim A.-Y. Jung H.-G. Ihm K. Yazawa K. Yashiro H. Konarov A. Huijben M. Guillon O. Kaghazchi P. Myung S.-T.
2025John Wiley and Sons Inc
Advanced Energy Materials
2025
A synergetic strategy on lattice and surface is implemented using a NaTi2(PO4)3 (NTP) ionic conductor for the P3-type Na0.67[Zn0.3Mn0.7]O2 (NZMO) cathode material; specifically, the stabilization of the oxide lattice through Ti incorporation and the reinforcement of the surface stability with P-containing moieties. This dual functionality enhances electrode performances in terms of long-term capacity retention and charge transfer. More importantly, the presence of the NTP layer contributes to the interfacial stability under high voltage conditions, which is associated with lattice oxygen redox occurring in the highly oxidized Nax[Zn0.3Mn0.7]O2 O/P phase, triggered by Zn migration from the transition metal layer to the Na layer. The enhanced electrode performance is likely attributed to enhanced surface stability, increased ionic conductivity, and the stabilization of the anionic O2−/(O2)n− redox progress at high voltage. The NTP layer suppresses surface reactions with the electrolyte by scavenging HF and H2O, while the introduced Ti contributes to the stabilization of the c-axis variations. Additionally, ab initio molecular dynamics simulations suggest that the NTP layer acts as a protective barrier against electrolyte degradation, preventing HF-induced metal ion dissolution and ensuring long-term stability. These results demonstrate the effectiveness of NTP coatings in enhancing the performance of cathode materials for sodium-ion batteries.
battery , cathode , redox , sodium , surface
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Hybrid Materials Research Center, Department of Nanotechnology and Advanced Materials Engineering & Sejong Battery Institute, Sejong University, 98 Gunja-dong, Gwangjin-gu, Seoul, 05006, South Korea
Institute of Energy Materials and Devices, Materials Synthesis and Processing (IMD-2), Forschungszentrum Jülich GmbH, Jülich, 52425, Germany
MESA+ Institute for Nanotechnology, University of Twente, Enschede, 7500 AE, Netherlands
Energy Storage Research Center, Korea Institute of Science and Technology, Seoul, 02792, South Korea
Department of Energy Science and KIST-SKKU Carbon-Neutral Research Center, Sungkyunkwan University, Suwon, 16419, South Korea
Pohang Accelerator Laboratory, Gyeongbuk, Pohang, 37673, South Korea
Jeol Resonance Inc., 3-1-2 Musashino, Tokyo, Akishima, 196–8558, Japan
Department of Chemistry and Bioengineering, Iwate University, Ueda 4-3-5, Iwate, Morioka, 020–8551, Japan
Department of Chemical and Materials Engineering, School of Engineering and Digital Sciences, Nazarbayev University, 53 Kabanbay Batyr Ave., Astana, 010000, Kazakhstan
Hybrid Materials Research Center
Institute of Energy Materials and Devices
MESA+ Institute for Nanotechnology
Energy Storage Research Center
Department of Energy Science and KIST-SKKU Carbon-Neutral Research Center
Pohang Accelerator Laboratory
Jeol Resonance Inc.
Department of Chemistry and Bioengineering
Department of Chemical and Materials Engineering
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