Chemical preintercalation of magnesium ions into ⍺-MoO3 structure for improved electrochemical stability in Li-ion cells

Omo-Lamai, Darrell; Zhang, Xinle; Andris, Ryan; Zachman, Michael J.; Pomerantseva, Ekaterina

doi:10.1016/j.jallcom.2024.175954

Chemical preintercalation of magnesium ions into ⍺-MoO₃ structure for improved electrochemical stability in Li-ion cells

Journal Article · Sun Aug 11 00:00:00 EDT 2024 · Journal of Alloys and Compounds

DOI:https://doi.org/10.1016/j.jallcom.2024.175954· OSTI ID:2573527

Omo-Lamai, Darrell ^[1]; Zhang, Xinle ^[1]; Andris, Ryan ^[1]; ^[2]; Pomerantseva, Ekaterina ^[1]

Drexel Univ., Philadelphia, PA (United States)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Chemical preintercalation of layered materials, used as electrodes in intercalation-based energy storage devices, represents a promising strategy to enhance electrochemical stability and extend cycle life. However, standardized synthesis approaches for the chemical preintercalation of diverse ions into various layered materials are lacking, necessitating the development of specific synthesis routes for each ion and layered phase combination. In this study, we present the first successful demonstration of Mg²⁺ ion chemical preintercalation into the interlayer region of α-MoO₃, revealing its stabilizing effect during cycling in non-aqueous Li-ion cells. Using ethanol during hydrothermal treatment facilitated molybdenum reduction, which was critical for Mg²⁺ ion preintercalation. Interestingly, we found that Mg preintercalation was accompanied by the incorporation of water. Mg-preintercalated α-MoO₃ exhibited enhanced charge storage capacity, electrochemical stability, and power capability compared to pristine α-MoO₃ electrodes. This improved performance is attributed to the structural stabilization provided by Mg²⁺ pillars, which prevent undesirable phase transformations during repeated Li intercalation/deintercalation, and increased Li⁺ ion diffusion due to the shielding of electrostatic interactions between electrochemically cycled ions and the α-MoO₃ lattice, enabled by structural water. In conclusion, our study offers new insights into developing chemical preintercalation synthesis approaches that can be broadly applied to a wide range of pillaring ions and layered material hosts.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2573527

Alternate ID(s):: OSTI ID: 2429638

Journal Information:: Journal of Alloys and Compounds, Journal Name: Journal of Alloys and Compounds Vol. 1005; ISSN 0925-8388

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Chemical preintercalation of magnesium ions into ⍺-MoO3 structure for improved electrochemical stability in Li-ion cells

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Chemical preintercalation of magnesium ions into ⍺-MoO₃ structure for improved electrochemical stability in Li-ion cells