Jamil, Sidra Mudasar, Farhan Yuan, Tiange Fasehullah, Muhammad Ali, Ghulam Chae, Keun Hwa Voznyy, Oleksandr Zhan, Yiqiang Xu, Maowen 2024-03-28T08:00:05Z 2024-03-28T08:00:05Z 2024-03-28 2024-03 1944-8244 https://pubs.kist.re.kr/handle/201004/149539 Mn-rich P2-type layered oxide cathode materials suffer from severe capacity loss caused by detrimental phase transition and transition metal dissolution, making their implementation difficult in large-scale sodium-ion battery applications. Herein, we introduced a high-valent Sb5+ substitution, leading to a biphasic P2/O3 cathode that suppresses the P2-O2 phase transformation in the high-voltage condition attributed to the stronger Sb-O covalency that introduces extra electrons to the O atom, reducing oxygen loss from the lattices and improving structural stability, as confirmed by first-principle calculations. Besides, the enhanced Na+ diffusion kinetics and thermodynamics in the modified sample are associated with the enlarged lattice parameters. As a result, the proposed cathode delivers a discharge capacity of 142.6 mAh g(-1) at 0.1C between 1.5 and 4.3 V and excellent performance at a high mass loading of 8 mg cm(3 )with a specific capacity of 131 mAh g(-1) at 0.2C. Furthermore, it also possesses remarkable rate capability (90.3 mAh g(-1) at 5C), specifying its practicality in high-energy-density sodium-ion batteries. Hence, this work provides insights into incorporating high-valent dopants for high-performance Mn-rich cathodes. English American Chemical Society Sb-Doped Biphasic P2/O3-Type Mn-Rich Layered Oxide Cathode Material for High-Performance Sodium-Ion Batteries Article 10.1021/acsami.3c15667 1 ACS Applied Materials & Interfaces, v.16, no.12, pp.14669 - 14679 ACS Applied Materials & Interfaces 16 12 14669 14679 N scie scopus 001187287300001 2-s2.0-85188124630 Nanoscience & Nanotechnology Materials Science, Multidisciplinary Science & Technology - Other Topics Materials Science Article OXYGEN REDOX CHEMISTRY HIGH-ENERGY PHASE-TRANSITION HIGH-CAPACITY LONG-LIFE NI CO NA2/3NI1/3MN2/3O2 SUBSTITUTION STABILITY high-valent dopants Mn-rich layered oxides P2/O3 biphasic structure robust oxygen framework sodium-ion batteries