Air-Stable High-Entropy Layered Oxide Cathode with Enhanced Cycling Stability for Sodium-Ion Batteries.

IF 9.6 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Nano Letters Pub Date : 2024-08-14 Epub Date: 2024-08-01 DOI:10.1021/acs.nanolett.4c00968

Jiajia Zhan, Jiawen Huang, Zhen Li, Jujun Yuan, Shi-Xue Dou, Hua-Kun Liu, Chao Wu

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Abstract

O3-type layered oxides have been extensively studied as cathode materials for sodium-ion batteries due to their high reversible capacity and high initial sodium content, but they suffer from complex phase transitions and an unstable structure during sodium intercalation/deintercalation. Herein, we synthesize a high-entropy O3-type layered transition metal oxide, NaNi_0.3Cu_0.05Fe_0.1Mn_0.3Mg_0.05Ti_0.2O₂ (NCFMMT), by simultaneously doping Cu, Mg, and Ti into its transition metal layers, which greatly increase structural entropy, thereby reducing formation energy and enhancing structural stability. The high-entropy NCFMMT cathode exhibits significantly improved cycling stability (capacity retention of 81.4% at 1C after 250 cycles and 86.8% at 5C after 500 cycles) compared to pristine NaNi_0.3Fe_0.4Mn_0.3O₂ (71% after 100 cycles at 1C), as well as remarkable air stability. Finally, the NCFMMT//hard carbon full-cell batteries deliver a high initial capacity of 103 mAh g^-1 at 1C, with 83.8 mAh g^-1 maintained after 300 cycles (capacity retention of 81.4%).

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空气稳定的高熵层状氧化物阴极，增强了钠离子电池的循环稳定性。

O3 型层状氧化物因其高可逆容量和高初始钠含量而被广泛研究用作钠离子电池的阴极材料，但它们在钠插层/脱插层过程中存在复杂的相变和不稳定的结构。在此，我们合成了一种高熵 O3 型层状过渡金属氧化物 NaNi0.3Cu0.05Fe0.1Mn0.3Mg0.05Ti0.2O2（NCFMMT），通过在其过渡金属层中同时掺入 Cu、Mg 和 Ti，大大增加了结构熵，从而降低了形成能并提高了结构稳定性。与原始 NaNi0.3Fe0.4Mn0.3O2（100 次 1C 循环后容量保持率为 71%）相比，高熵 NCFMMT 阴极的循环稳定性显著提高（250 次 1C 循环后容量保持率为 81.4%，500 次 5C 循环后容量保持率为 86.8%），在空气中的稳定性也非常出色。最后，NCFMMT//硬碳全电池在 1C 时的初始容量高达 103 mAh g-1，循环 300 次后仍能保持 83.8 mAh g-1（容量保持率为 81.4%）。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.