Doping of group IVB elements for nickel-rich cobalt-free cathodes

Guo, Shengnan; Lei, Xincheng; Wang, Jiayi; Su, Jie; Wang, Yingying; Liu, Xiaozhi; Ji, Pengxiang; Zhao, Kangning; Wang, Xuefeng; Gu, Lin; Yao, Zhenpeng; Su, Dong

doi:10.1016/j.jechem.2023.07.041

Journal of Energy Chemistry

2023

DOI: 10.1016/j.jechem.2023.07.041

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Doping of group IVB elements for nickel-rich cobalt-free cathodes

Shengnan Guo,

Xincheng Lei,

Jiayi Wang

et al.

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2024

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Cited by 9 publications

References 80 publications

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Unveiling the Structural and Chemical Evolution of Layered Oxide Cathode for Na‐Ion Batteries Induced by Water Vapor

Ji,

Lei,

Wang

et al. 2024

Adv Funct Materials

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Na‐ion batteries (NIBs) have received considerable attention as promising alternatives to lithium‐ion batteries, particularly for low‐speed electric vehicles and large‐scale energy storage applications. Currently, layered oxide compounds are considered the most important cathode materials for NIBs. However, they suffer from reduced capacity and a shortened lifespan when exposed to water vapor during storage or battery assembly. This article elaborates on the structural and chemical evolution of NaNi1/3Fe1/3Mn1/3O2 (NFM) cathode at the atomic scale in a pure water vapor environment. The Na+/H+ exchange induces the formation of a spinel‐like phase via a multi‐site nucleation mechanism. This transition preferentially occurs either at the cathode surface or along planar defects such as twin boundaries and grain boundaries. Additionally, numerous microcracks perpendicular to <003> direction appear inside NFM grains, further exacerbating the structural deterioration. Upon prolonged exposure to water vapor, NFM grains decompose into a mixture of Na2O and transition metal oxide nanoparticles (FeO, NiO, and MnO), accompanied by the generation of oxygen gas. This research provides a comprehensive atomic‐scale insight into the water vapor instability mechanism of layered oxide cathodes, offering guidance for the design and manufacture of the next generation of water vapor‐tolerant layered oxide cathodes in NIBs.

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Unveiling the Structural and Chemical Evolution of Layered Oxide Cathode for Na‐Ion Batteries Induced by Water Vapor

Ji,

Lei,

Wang

et al. 2024

Adv Funct Materials

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Molybdenum‐Doped Cobalt‐Free Cathode Realizing the Electrochemical Stability by Enhanced Covalent Bonding

Wang,

Lei,

Guo

et al. 2024

Small

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The doping strategy effectively enhances the capacity and cycling stability of cobalt‐free nickel‐rich cathodes. Understanding the intrinsic contributions of dopants is of great importance to optimize the performances of cathodes. This study investigates the correlation between the structure modification and their performances of Mo‐doped LiNi0.8Mn0.2O2 (NM82) cathode. The role of doped Mo's valence state has been proved functional in both lattice structural modification and electronic state adjustment. Although the high‐valence of Mo at the cathode surface inevitably reduces Ni valence for electronic neutrality and thus causes ion mixing, the original Mo valence will influence its diffusion depth. Structural analyses reveal Mo doping leads to a mixed layer on the surface, where high‐valence Mo forms a slender cation mixing layer, enhancing structural stability and Li‐ion transport. In addition, it is found that the high‐valence dopant of Mo6+ ions partially occupies the unfilled 4d orbitals, which may strengthen the Mo─O bond through increased covalency and therefore reduce the oxygen mobility. This results in an impressive capacity retention (90.0% after 200 cycles) for Mo‐NM82 cathodes with a high Mo valence state. These findings underscore the valence effect of doping on layered oxide cathode performance, offering guidance for next‐generation cathode development.

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In Situ Transmission Electron Microscopy Methods for Lithium‐Ion Batteries

Ji,

Lei,

2024

Small Methods

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In situ Transmission Electron Microscopy (TEM) stands as an invaluable instrument for the real‐time examination of the structural changes in materials. It features ultrahigh spatial resolution and powerful analytical capability, making it significantly versatile across diverse fields. Particularly in the realm of Lithium‐Ion Batteries (LIBs), in situ TEM is extensively utilized for real‐time analysis of phase transitions, degradation mechanisms, and the lithiation process during charging and discharging. This review aims to provide an overview of the latest advancements in in situ TEM applications for LIBs. Additionally, it compares the suitability and effectiveness of two techniques: the open cell technique and the liquid cell technique. The technical aspects of both the open cell and liquid cell techniques are introduced, followed by a comparison of their applications in cathodes, anodes, solid electrolyte interphase (SEI) formation, and lithium dendrite growth in LIBs. Lastly, the review concludes by stimulating discussions on possible future research trajectories that hold potential to expedite the progression of battery technology.

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Doping of group IVB elements for nickel-rich cobalt-free cathodes

Cited by 9 publications

References 80 publications

Unveiling the Structural and Chemical Evolution of Layered Oxide Cathode for Na‐Ion Batteries Induced by Water Vapor

Unveiling the Structural and Chemical Evolution of Layered Oxide Cathode for Na‐Ion Batteries Induced by Water Vapor

Molybdenum‐Doped Cobalt‐Free Cathode Realizing the Electrochemical Stability by Enhanced Covalent Bonding

In Situ Transmission Electron Microscopy Methods for Lithium‐Ion Batteries

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