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Hybrid bilayered vanadium oxide electrodes with large and tunable interlayer distances in lithium-ion batteries

Journal Article · · Journal of Colloid and Interface Science
The interlayer distances in layered electrode materials, influenced by the chemical composition of the confined interlayer regions, have a significant impact on their electrochemical performance. Chemical preintercalation of inorganic metal ions affects the interlayer spacing, yet expansion is limited by the hydrated ion radii. Herein, we demonstrate that using varying concentrations of decyltrimethylammonium (DTA+) and cetyltrimethylammonium (CTA+) cations in chemical preintercalation synthesis followed by hydrothermal treatment, the interlayer distance of hybrid bilayered vanadium oxides (BVOs) can be tuned between 11.1 Å and 35.6 Å. Our analyses reveal that these variations in interlayer spacing are due to different amounts of structural water and alkylammonium cations confined within the interlayer regions. Increased concentrations of alkylammonium cations not only expand the interlayer spacing but also induce local bending and disordering of the V-O bilayers. Electrochemical cycling of hybrid BVO electrodes in non-aqueous lithium-ion cells show that specific capacities decrease as interlayer regions expand, suggesting that the densely packed alkylammonium cations obstruct intercalation sites and hinder Li+ ion transport. Furthermore, we found that greater layer separation facilitates the dissolution of active material into the electrolyte, resulting in rapid capacity decay during extended cycling. In conclusion, this study emphasizes that layered electrode materials require both spacious interlayer regions as well as high structural and chemical stabilities, providing guidelines for structural engineering of organic–inorganic hybrids.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
AC05-00OR22725
OSTI ID:
2573526
Journal Information:
Journal of Colloid and Interface Science, Journal Name: Journal of Colloid and Interface Science Vol. 674; ISSN 0021-9797
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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