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Unraveling the Complex Delithiation Mechanisms of Olivine-Type Cathode Materials, LiFexCo1-xPO4

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dc.contributor.authorStrobridge, Fiona C
dc.contributor.authorLiu, Hao
dc.contributor.authorLeskes, Michal
dc.contributor.authorBorkiewicz, Olaf J
dc.contributor.authorWiaderek, Kamila M
dc.contributor.authorChupas, Peter J
dc.contributor.authorChapman, Karena W
dc.contributor.authorGrey, Clare
dc.contributor.otherPlasma, Laser Ablation and Surface Modelling - Antwerp (PLASMANT)
dc.date.accessioned2019-04-26T08:57:03Z
dc.date.available2019-04-26T08:57:03Z
dc.date.issued25/04/16
dc.descriptionThe delithiation mechanisms occurring within the olivine-type class of cathode materials for Li-ion batteries have received considerable attention owing to the good capacity retention at high rates for LiFePO4. A comprehensive mechanistic study of the (de)lithiation reactions that occur when the substituted olivine-type cathode materials LiFexCo1-xPO4 (x = 0, 0.05, 0.125, 0.25, 0.5, 0.75, 0.875, 0.95 and 1) are electrochemically cycled is reported here, using in situ X-ray diffraction (XRD) data, and supporting ex situ 31P NMR spectra. On the first charge, two intermediate phases are observed and identified: Li1-x(Fe3+)x(Co2+)1-xPO4 for 0 < x < 1 (i.e. after oxidation of Fe2+ => Fe3+) and Li2/3FexCo1-xPO4 for 0 ≤ x ≤ 0.5 (i.e. the Co-majority materials). For the Fe-rich materials, we study how nonequilibrium, single-phase mechanisms that occur discretely in single particles, as observed for LiFePO4 at high rates, are affected by Co substitution. In the Co-majority materials, a two-phase mechanism with a coherent interface is observed, as was seen in LiCoPO4, and we discuss how it is manifested in the XRD patterns. We then compare the nonequilibrium, single-phase mechanism with the bulk single-phase and the coherent interface two-phase mechanisms. Despite the apparent differences between these mechanisms, we discuss how they are related and interconverted as a function of Fe/Co substitution and the potential implications for the electrochemistry of this system.
dc.identifier.urihttps://demo7.dspace.org/handle/123456789/445
dc.languageen
dc.publisherAmerican Chemical Society
dc.titleUnraveling the Complex Delithiation Mechanisms of Olivine-Type Cathode Materials, LiFexCo1-xPO4
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