Journal
NANOSCALE
Volume 11, Issue 25, Pages 12347-12357Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9nr01228a
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Funding
- Villum Foundation [VKR023453]
- Independent Research Fund Denmark [4184-00143A]
- Carlsberg Foundation [CF17-0823]
- Danish National Research Foundation [DNRF93]
- U.S. Department of Energy [DE-SC0002626]
- DOE Office of Science [DE-AC02-06CH11357]
- Danscatt
- U.S. Department of Energy (DOE) [DE-SC0002626] Funding Source: U.S. Department of Energy (DOE)
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Nano-sized particles of rutile TiO2 is a promising material for cheap high-capacity anodes for Li-ion batteries. It is well-known that rutile undergoes an irreversible order-disorder transition upon deep discharge. However, in the disordered state, the LixTiO2 material retains a high reversible ion-storage capacity of >200 mA h g(-1). Despite the promising properties of the material, the structural transition and evolution during the repeated battery operation has so far been studied only by diffraction-based methods, which only provide insight into the part that retains some long-range order. Here, we utilize a combination of ex situ and operando total scattering with pair distribution function analysis and transmission electron microscopy to investigate the atomic-scale structures of the disordered LixTiO2 forming upon the discharge of nano-rutile TiO2 as well as to elucidate the phase behavior in the material during the repeated charge-discharge process. Our investigation reveals that nano-rutile upon Li-intercalation transforms into a composite of similar to 5 nm domains of a layered LixTiO2 alpha-NaFeO2-type structure with similar to 1 nm LixTiO2 grain boundaries with a columbite-like structural motif. During repeated charge-discharge cycling, the structure of this composite is retained and stores Li through a complete solid-solution transition with a remarkably small volume change of only 1 vol%.
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