Hyunji Kweon , Jungmin Kang , Bonyoung Ku , Sunha Hwang , Jinho Ahn , Lahyeon Jang , Myungeun Choi , Sang-Yeop Lee , Jihoe Lee , Hoseok Lee , Hun-Gi Jung , Jang-Yeon Hwang , Hee-Dae Lim , Jongsoon Kim
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Using the first-principles calculations and experiments, we demonstrate that the P2-K<sub>0.48</sub>[Li<sub>0.1</sub>Mn<sub>0.9</sub>]O<sub>2</sub> (P2-KLMO) delivers improved electrochemical performance, specific capacity and average discharge voltage of ∼124.4 mA h g<sup>−1</sup> and ∼2.7 V (vs. K<sup>+</sup>/K) at 0.05C (1C = 260 mA g<sup>−1</sup>), outperforming P2-K<sub>0.5</sub>MnO<sub>2</sub>. <em>Operando</em> X-ray diffraction analysis confirms the P2-OP4 phase transition and Mn<sup>3+</sup>-induced Jahn-Teller distortion are significantly suppressed in P2-KLMO. These improvements are attributed to the lithium introduction into transition metal layers, leading to strengthened structural stability and enhanced K<sup>+</sup> diffusion kinetics. Moreover, synthetic accessibility through the conventional solid-state method provides an additional advantage for practical application of Li-incorporated Mn-based P2-type cathodes in KIBs. 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引用次数: 0
摘要
锰基层状氧化物由于其低摩尔质量而产生的高比容量而被广泛认为是钾离子电池的正极材料。然而,由于Mn3+的Jahn-Teller效应引起的结构不稳定性和K+的大离子半径导致其电化学性能较差。在此,我们提出了一种有效的结构稳定策略,通过在过渡金属层中加入锂来稳定kib的p2型mn基层状氧化物阴极。通过第一性原理计算和实验,我们证明了P2-K0.48[Li0.1Mn0.9]O2 (P2-KLMO)在0.05C (1C = 260 mA g - 1)下具有更好的电化学性能,比容量和平均放电电压为~ 124.4 mA h g - 1和~ 2.7 V (vs. K+/K),优于P2-K0.5MnO2。Operando x射线衍射分析证实,P2-KLMO明显抑制了P2-OP4相变和Mn3+诱导的Jahn-Teller畸变。这些改进归功于锂引入过渡金属层,从而增强了结构稳定性和K+扩散动力学。此外,通过传统的固态方法合成可及性为锂掺杂锰基p2型阴极在kib中的实际应用提供了额外的优势。我们相信我们的研究为设计高性能和实用的阴极材料提供了一种简单而有效的策略。
Enhancing power capability and fast discharge behavior in P2-type K layered cathodes through structural stabilization via introducing Li-ions into TM layers
Mn-based layered oxides are widely recognized as cathode materials for potassium-ion batteries (KIBs) due to their high specific capacity derived from their low molar mass. However, the structural instability caused by the Jahn-Teller effect of Mn3+ and the large ionic radius of K+ results in poor electrochemical performance. Herein, we propose an effective structural stabilization strategy for P2-type Mn-based layered oxide cathodes of KIBs through Li-incorporation into the transition metal layer. Using the first-principles calculations and experiments, we demonstrate that the P2-K0.48[Li0.1Mn0.9]O2 (P2-KLMO) delivers improved electrochemical performance, specific capacity and average discharge voltage of ∼124.4 mA h g−1 and ∼2.7 V (vs. K+/K) at 0.05C (1C = 260 mA g−1), outperforming P2-K0.5MnO2. Operando X-ray diffraction analysis confirms the P2-OP4 phase transition and Mn3+-induced Jahn-Teller distortion are significantly suppressed in P2-KLMO. These improvements are attributed to the lithium introduction into transition metal layers, leading to strengthened structural stability and enhanced K+ diffusion kinetics. Moreover, synthetic accessibility through the conventional solid-state method provides an additional advantage for practical application of Li-incorporated Mn-based P2-type cathodes in KIBs. We believe our study offers a simple yet effective strategy for designing high-performance and practical cathode materials for KIBs.
期刊介绍:
The Journal of Energy Chemistry, the official publication of Science Press and the Dalian Institute of Chemical Physics, Chinese Academy of Sciences, serves as a platform for reporting creative research and innovative applications in energy chemistry. It mainly reports on creative researches and innovative applications of chemical conversions of fossil energy, carbon dioxide, electrochemical energy and hydrogen energy, as well as the conversions of biomass and solar energy related with chemical issues to promote academic exchanges in the field of energy chemistry and to accelerate the exploration, research and development of energy science and technologies.
This journal focuses on original research papers covering various topics within energy chemistry worldwide, including:
Optimized utilization of fossil energy
Hydrogen energy
Conversion and storage of electrochemical energy
Capture, storage, and chemical conversion of carbon dioxide
Materials and nanotechnologies for energy conversion and storage
Chemistry in biomass conversion
Chemistry in the utilization of solar energy