Unraveling the Complex Delithiation Mechanisms of Olivine-Type Cathode Materials, LiFe x Co 1– x PO 4. Strobridge, F., C., Liu, H., Leskes, M., Borkiewicz, O., J., Wiaderek, K., M., Chupas, P., J., Chapman, K., W., & Grey, C., P. Chemistry of Materials, 28(11):3676-3690, 6, 2016.
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Paper Website doi abstract bibtex The delithiation mechanisms occurring within the olivine-type class of cathode materials for Li-ion batteries have received considerable attention because of the good capacity retention at high rates for LiFePO 4 . A comprehensive mechanistic study of the (de)lithiation reactions that occur when the substituted olivine-type cathode materials LiFe x Co 1−x PO 4 (x = 0, 0.05, 0.125, 0.25, 0.5, 0.75, 0.875, 0.95, 1) are electro-chemically cycled is reported here using in situ X-ray diffraction (XRD) data and supporting ex situ 31 P NMR spectra. On the first charge, two intermediate phases are observed and identified: Li 1−x (Fe 3+) x (Co 2+) 1−x PO 4 for 0 < x < 1 (i.e., after oxidation of Fe 2+ to Fe 3+) and Li 2/3 Fe x Co 1−x PO 4 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 LiFePO 4 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 LiCoPO 4 , 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 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.
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title = {Unraveling the Complex Delithiation Mechanisms of Olivine-Type Cathode Materials, LiFe x Co 1– x PO 4},
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abstract = {The delithiation mechanisms occurring within the olivine-type class of cathode materials for Li-ion batteries have received considerable attention because of the good capacity retention at high rates for LiFePO 4 . A comprehensive mechanistic study of the (de)lithiation reactions that occur when the substituted olivine-type cathode materials LiFe x Co 1−x PO 4 (x = 0, 0.05, 0.125, 0.25, 0.5, 0.75, 0.875, 0.95, 1) are electro-chemically cycled is reported here using in situ X-ray diffraction (XRD) data and supporting ex situ 31 P NMR spectra. On the first charge, two intermediate phases are observed and identified: Li 1−x (Fe 3+) x (Co 2+) 1−x PO 4 for 0 < x < 1 (i.e., after oxidation of Fe 2+ to Fe 3+) and Li 2/3 Fe x Co 1−x PO 4 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 LiFePO 4 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 LiCoPO 4 , 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 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.},
bibtype = {article},
author = {Strobridge, Fiona C and Liu, Hao and Leskes, Michal and Borkiewicz, Olaf J and Wiaderek, Kamila M and Chupas, Peter J and Chapman, Karena W and Grey, Clare P},
doi = {10.1021/acs.chemmater.6b00319},
journal = {Chemistry of Materials},
number = {11}
}Downloads: 0
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