A “seat-squatting” strategy via lithium substitution to suppress Fe-migration in Na layered oxide cathodes

Yaoshen Niu; Zilin Hu; Huican Mao; Lin Zhou; Liguang Wang; Xiaobing Lou; Bo Zhang; Dongdong Xiao; Yang Yang; Feixiang Ding; Xiaohui Rong; Juping Xu; Wen Yin; Nian Zhang; Zhiwei Li; Yaxiang Lu; Bingwen Hu; Jun Lu; Ju Li; Yong-Sheng Hu

doi:10.1039/D4EE01867B

A “seat-squatting” strategy via lithium substitution to suppress Fe-migration in Na layered oxide cathodes†

Yaoshen Niu,

^ab Zilin Hu,^a Huican Mao,*^c Lin Zhou,^a Liguang Wang,

^d Xiaobing Lou,^e Bo Zhang,^f Dongdong Xiao,^a Yang Yang,

^a Feixiang Ding,^a Xiaohui Rong,*^g Juping Xu,^h Wen Yin,

^h Nian Zhang,ⁱ Zhiwei Li,^f Yaxiang Lu,

^a Bingwen Hu,

^e Jun Lu,^d Ju Li

*^j and Yong-Sheng Hu

*^a

Author affiliations

* Corresponding authors

^a Key Laboratory for Renewable Energy, Beijing Key Laboratory for New Energy Materials and Devices, Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, The College of Materials Sciences and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100190, China
E-mail: yshu@iphy.ac.cn

^b Frontier Institute of Science and Technology, Xi’an Jiaotong University, Xi’an 710049, China

^c Department of Energy Storage Science and Engineering, School of Metallurgical and Ecological Engineering, University of Science and Technology Beijing, Beijing 100083, China
E-mail: hcmao@ustb.edu.cn

^d Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, IL, USA

^e Shanghai Key Laboratory of Magnetic Resonance, State Key Laboratory of Precision Spectroscopy, School of Physics and Electronic Science, East China Normal University, Shanghai 200241, P. R. China

^f Key Lab for Magnetism and Magnetic Materials of the Ministry of Education, Lanzhou University, Lanzhou 730000, China

^g Yangtze River Delta Physics Research Center Co. Ltd, Liyang, China
E-mail: rongxiaohui@ioply.cn

^h Spallation Neutron Source Science Center, Dongguan 523803, China

ⁱ State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, People's Republic of China

^j Department of Nuclear Science and Engineering and Department of Materials Science and Engineering, MIT, Cambridge, MA 02139, USA
E-mail: liju@mit.edu

Abstract

Na-ion batteries (NIBs) are emerging as a promising alternative to Li-ion batteries (LIBs). To align with sustainability principles, the design of electrode materials must incorporate considerations for abundant and environmentally friendly elements, such as redox-active Fe. Despite its appeal, the enduring challenge of Fe migration in layered cathodes remains inadequately addressed over decades. Here, we propose a “seat-squatting” strategy via Li-substitution to fundamentally suppress Fe migration. Li is strategically introduced to migrate first, occupying available migration sites without inducing structural damage and effectively raising the activation energy for Fe migration. Experimental and theoretical validation using O3-Na_0.83Li_0.17Fe_0.33Mn_0.5O₂ (NaLFM) demonstrates a robust suppression of irreversible Fe migration. As a result, the NaLFM cathode delivers enhanced structural and electrochemical cycling stability. This work illustrates a compelling strategy to curb irreversible Fe migration in NIBs, offering a pathway for the development of stable and cost-effective layered oxides based on Fe redox centers.

This article is part of the themed collection: Recent Open Access Articles

Energy & Environmental Science

A “seat-squatting” strategy via lithium substitution to suppress Fe-migration in Na layered oxide cathodes†

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A “seat-squatting” strategy via lithium substitution to suppress Fe-migration in Na layered oxide cathodes

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