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Issue 36, 2013
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Magnetic measurements as a viable tool to assess the relative degrees of cation ordering and Mn3+ content in doped LiMn1.5Ni0.5O4 spinel cathodes

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Abstract

The magnetic properties of the doped high-voltage spinels LiMn1.5Ni0.42M0.08O4 (M = Cr, Fe, Co, Cu, Al, and Ga) as well as the Mn-rich spinels LiMn1.5+xNi0.5−xO4 (x = 0, 0.05, 0.1) synthesized by a tank-reactor coprecipitation method have been investigated. It is found that the Curie temperatures correlate well with the degree of cation ordering determined by measuring the capacity value at ∼2.7 V, which corresponds to the insertion of additional lithium into the empty 16c octahedral sites of the spinel lattice. Additionally, it is found that the saturation magnetization near 0 K provides a reliable means of calculating the Mn3+ content in each sample based on the predicted magnetic exchange interactions of the spinel structure. The magnetic results match well with the capacity values obtained in the 4 V region of the samples when assembled as cathodes in lithium-ion cells. The Mn-rich spinels offer insight into the relationship between Mn3+ content and degree of cation ordering and how they affect the magnitude of the capacity in the ∼2.7 V region. The effects of Mn3+ content and cation ordering were isolated by examining the relationship among lattice parameter, Mn3+ content, capacity contribution at ∼2.7 V, and Curie temperature. Thus, it is posited that the Curie temperature is a reliable qualitative means of measuring the degree of cation order in a variety of doped or Mn-rich spinel oxides.

Graphical abstract: Magnetic measurements as a viable tool to assess the relative degrees of cation ordering and Mn3+ content in doped LiMn1.5Ni0.5O4 spinel cathodes

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Publication details

The article was received on 23 May 2013, accepted on 12 Jul 2013 and first published on 12 Jul 2013


Article type: Paper
DOI: 10.1039/C3TA12021J
J. Mater. Chem. A, 2013,1, 10745-10752

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    Magnetic measurements as a viable tool to assess the relative degrees of cation ordering and Mn3+ content in doped LiMn1.5Ni0.5O4 spinel cathodes

    Z. Moorhead-Rosenberg, K. R. Chemelewski, J. B. Goodenough and A. Manthiram, J. Mater. Chem. A, 2013, 1, 10745
    DOI: 10.1039/C3TA12021J

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