Advanced Electron Energy Loss Spectroscopy for Battery Studies

Yin, Zhoulan; Zhao, Wenguang; Li, Jianyuan; Peng, Xiaoyuan; Lin, Cong; Zhang, Dongke; Zeng, Zhiyuan; Liao, Hong‐Gang; Chen, Haibiao; Lin, Hai; Pan, Feng

doi:10.1002/adfm.202107190

Cited by 43 publications

(21 citation statements)

References 141 publications

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“…Because the XAS spectra were collected under TEY mode, they can be used to reflect the surface information variation upon charging/discharging. The XAS spectra of LCO and LCOMF are very similar in their pristine states (Figure a,c), while multiple signals appeared at lower photon energies after charging to 4.2 V in both samples (Region 1), corresponding to Co 2+ with the O h symmetry. , However, the Co 2+ signals disappeared in the 4.6 V-charged samples, accompanied by the presence of low-valence oxygen (O 2 n – ) (Figure b,d) . When discharged to 2.8 V, the Co 2+ signal appears again with the reduction of O 2 n – into O 2– .…”

Section: Resultsmentioning

confidence: 88%

Reversible Li Intercalation in Layered Cathodes Enabled by Dopant-Induced Medium-Range Orders

Ou,

Luo,

Zhang

et al. 2023

Chem. Mater.

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Doping could effectively tune the electrochemical performance of layered oxide cathodes in Li-ion batteries, whereas the working mechanism is usually oversimplified (i.e., a “pillar” effect). Although the Jahn–Teller effect is generally regarded as the fundamental origin of structural instability in some oxides, more polyhedral distortions are associated with pseudo-JTE (PJTE), which involves vibronic couplings. In this work, the atomic structures of doped LiCoO2 by Mg cations, F anions, and both were investigated thoroughly to reveal the atomic environments of these dopants and their influence on electrochemical performance. The function of these dopants as pillars is well discussed from the view of PJTE manipulation. Briefly, the MgO4 tetrahedra in Mg-doped LiCoO2 could suppress the charge transfer from the ligand to Co in neighboring octahedra, thus depressing PJTE. Although F doping does increase the ligand-field strength, the induced octahedral distortion reduces the structural stability dramatically. Comparatively, Mg/F co-doping generates the CoO5F–MgO4F2–CoO5F medium-range orders (MROs), which could depress both structural distortion and charge transfer in Co-centered octahedra for reduced PJTE. The reduced PJTE accounts for the improved electrochemical performance, making the co-doped LiCoO2 offer the best performance: a 70% capacity retention after 200 cycles within the potential range of 2.8–4.6 V, followed by Mg-doped LiCoO2. In contrast, although F-doping could induce an extra rock salt-like surface layer for higher capacity, its cycling improvement is rather limited. These results highlight the importance of structural modulation in enhancing the material performance and propose that the manipulation of PJTE would be an effective strategy in developing novel high-performance oxide cathodes.

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Section: Resultsmentioning

confidence: 88%

Reversible Li Intercalation in Layered Cathodes Enabled by Dopant-Induced Medium-Range Orders

Ou,

Luo,

Zhang

et al. 2023

Chem. Mater.

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“…To analyze the TiO x structure more accurately, the valence state of the Ti elements in TiO x has been calibrated by the ratio of L 3 peak area to L 2 peak area in the Ti L edge spectrum (also known as the white line ratio). , In the present study, the commercial Ti 2 O 3 and TiO 2 nanorods were selected as the standard samples for Ti 3+ and Ti 4+ titanium oxides to calibrate the average valence state of the Ti atom in TiO x and determine the stoichiometric number x of O element. Low-magnification TEM images show that commercial Ti 2 O 3 nanorods consist of large particles with a diameter greater than 100 nm (Figure S4b), whereas TiO 2 nanorods exhibit the regular rod-like morphology (Figure S4c).…”

Section: Resultsmentioning

confidence: 99%

Quantitative Analysis of the Interface between Titanium Dioxide Support and Noble Metal by Electron Energy Loss Spectroscopy

Chen,

Qi,

et al. 2023

ACS Appl. Mater. Interfaces

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The interface structure of supported catalysts plays a significant role in the strong metal−support interactions (SMSI). However, it remains limited on interpreting interface structures, thus affecting the understanding of SMSI origin and impact on catalytic performance. Herein, electronic energy loss spectroscopy was adopted to characterize the interface microstructures of Pt/ TiO 2 materials. After high-temperature reduction processing, it was observed that the coating on the surface of the Pt metal particles was TiO x . Then, based on Gaussian function fitting, an effective and valid method was established for quantitative analysis on Ti L edge loss spectrum. This method allowed us to accurately determine the stoichiometric number of TiO x phases. In order to probe the classical phenomenon of strong metal−support interactions in more detail, we also discussed and analyzed the origin of TiO x and its effect on the electronic structure of the material using density functional theory calculations. The structure of surfaces and interfaces as well as the chemical evolution of supported catalysts on a microscale have been revealed, thereby providing a new analysis method and research perspectives for the future study of metal−support interactions.

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“…[127a,153] Electron energy loss spectroscopy analysis the atomic-scale electron state in energy materials, including the elemental valence and concentration distribution, e.g., the chemical composition distribution of the cathode from surface to bulk. [154] Nuclear magnetic resonance (NMR) captures the localized atomic structure and environment, e.g., recognizing the lithium diffusion path by analyzing 7 Li spectra. [155] Neutron-related characterization including neutron depth profiling (NDP), neutron diffraction, and neutron reflectometry, are sensitive to light elements such as H and Li.…”

Section: Morphologic/mechanical Properties and Characterizationmentioning

confidence: 99%

Bridging Multiscale Characterization Technologies and Digital Modeling to Evaluate Lithium Battery Full Lifecycle

Liu

Zhang

et al. 2022

Advanced Energy Materials

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The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/aenm.202200889. realize carbon-neutral growth have been put forward by countries all over the world, e.g., China aims to cut CO 2 emissions net-zero by 2060. [1] A promising means to reduce the dependence of our societies on fossil fuels is the development of advanced energy materials. [2] Lithium-ion batteries (LIBs) show great potential as high performance energy storage devices for consumer electronics, electrified transportation, and grid-level energy storage systems because of their inherent advantages, such as high energy density, high working voltage, low self-discharge rate, and long cycle stability, over other traditional battery systems (e.g., lead-acid battery, nickel-metal hydride battery). [3] Despite impressive progress in LIB technologies since the first invention of commercial LIBs in 1992, [4] further expansion and large-scale application of LIBs are currently hindered by limited fast charging ability, relatively low energy density, safety concerns under thermal/mechanical/electrical abuse conditions, capacity decay, and cycle stability. [4,5] Government around the world has set ambitious targets to promote more practical and higher performance batteries technology, such as the American "Battery 500 project" (500 Wh kg −1 in 2021), Chinese "Made in China 2025" (400 Wh kg −1 in 2025), Japanese "RISING II" (500 Wh kg −1 in 2030). [6] Achieving higher energy density has been a priority in recent LIB research to realize longer

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Advanced Electron Energy Loss Spectroscopy for Battery Studies

Cited by 43 publications

References 141 publications

Reversible Li Intercalation in Layered Cathodes Enabled by Dopant-Induced Medium-Range Orders

Reversible Li Intercalation in Layered Cathodes Enabled by Dopant-Induced Medium-Range Orders

Quantitative Analysis of the Interface between Titanium Dioxide Support and Noble Metal by Electron Energy Loss Spectroscopy

Bridging Multiscale Characterization Technologies and Digital Modeling to Evaluate Lithium Battery Full Lifecycle

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