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  Mo-Incorporated Magnetite Fe3O4 Featuring Cationic Vacancies Enabling Fast Lithium Intercalation for Batteries

Guo, S., Koketsu, T., Hu, Z., Zhou, J., Kuo, C.-Y., Lin, H.-J., et al. (2022). Mo-Incorporated Magnetite Fe3O4 Featuring Cationic Vacancies Enabling Fast Lithium Intercalation for Batteries. Small, 2203835, pp. 1-12. doi:10.1002/smll.202203835.

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 Creators:
Guo, Shasha1, Author
Koketsu, Toshinari1, Author
Hu, Zhiwei2, Author           
Zhou, Jing1, Author
Kuo, Chang-Yang1, Author
Lin, Hong-Ji1, Author
Chen, Chien-Te1, Author
Strasser, Peter1, Author
Sui, Lijun1, Author
Xie, Yu1, Author
Ma, Jiwei1, Author
Affiliations:
1External Organizations, ou_persistent22              
2Zhiwei Hu, Physics of Correlated Matter, Max Planck Institute for Chemical Physics of Solids, Max Planck Society, ou_1863461              

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 Abstract: Transition metal oxides (TMOs) as high-capacity electrodes have several drawbacks owing to their inherent poor electronic conductivity and structural instability during the multi-electron conversion reaction process. In this study, the authors use an intrinsic high-valent cation substitution approach to stabilize cation-deficient magnetite (Fe3O4) and overcome the abovementioned issues. Herein, 5 at% of Mo4+-ions are incorporated into the spinel structure to substitute octahedral Fe3+-ions, featuring approximate to 1.7 at% cationic vacancies in the octahedral sites. This defective Fe-2.93 ▫0.017Mo0.053O4 electrode shows significant improvements in the mitigation of capacity fade and the promotion of rate performance as compared to the pristine Fe3O4. Furthermore, physical-electrochemical analyses and theoretical calculations are performed to investigate the underlying mechanisms. In Fe-2.93 ▫0.017Mo0.053O4, the cationic vacancies provide active sites for storing Li+ and vacancy-mediated Li+ migration paths with lower energy barriers. The enlarged lattice and improved electronic conductivity induced by larger doped-Mo4+ yield this defective oxide capable of fast lithium intercalation. This is confirmed by a combined characterization including electrochemical impedance spectroscopy (EIS), cyclic voltammetry (CV), galvanostatic intermittent titration technique (GITT) and density functional theory (DFT) calculation. This study provides a valuable strategy of vacancy-mediated reaction to intrinsically modulate the defective structure in TMOs for high-performance lithium-ion batteries.

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Language(s): eng - English
 Dates: 2022-09-042022-09-04
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: -
 Identifiers: ISI: 000849568900001
DOI: 10.1002/smll.202203835
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Title: Small
  Other : Small
Source Genre: Journal
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Publ. Info: Weinheim, Germany : Wiley-VCH
Pages: - Volume / Issue: - Sequence Number: 2203835 Start / End Page: 1 - 12 Identifier: ISSN: 1613-6810
CoNE: https://pure.mpg.de/cone/journals/resource/1000000000017440_1