Composite "Layered-Layered-Spinel" Electrodes for High Energy Lithium-Ion Batteries

Tuesday, October 13, 2015: 11:00
105-A (Phoenix Convention Center)
J. S. Park, J. R. Croy, B. R. Long, E. Lee (Argonne National Laboratory), and M. M. Thackeray (Argonne National Laboratory)
The lithium- and manganese-rich class of composite materials, xLi2MnO3•(1-x)LiMO2(M=Ni ,Mn, Co), have attracted  great interest as  next generation cathode materials for advanced lithium ion batteries [1]. Significant capacities of over 250mAh/g can be achieved with x values between 0.3 and 0.5; however these electrodes suffer from severe structural and electrochemical decay related to voltage fade and hysteresis [2].

Recently, structurally compatible spinel components have been incorporated into the ‘layered-layered’ structures, and it has been demonstrated that these new ‘layered-layered-spinel’ composites, with formula y[xLi2MnO3•(1-x)LiMO2]•(1-y)LiM2O4), show enhanced electrochemical properties including high first cycle efficiency and good structural stability through careful control operating voltage and composition [3,4]. In a recent study it was found that the cobalt concentration plays an important role in controlling the cycling stability of ‘layered-layered-spinel’ composites [4].

This presentation will discuss results on electrochemical properties of ‘layered-layered-spinel’ composites obtained by further exploring and optimizing electrode compositions and structures. In particular, the effect of nickel and manganese concentrations on tailoring of structures and electrochemical performance will be reviewed.


[1] M. M. Thackeray, C. S. Johnson, J. T. Vaughey, N. Li, and S. A. Hackney, J. Mat. Chem., 15, 2257 (2005).

[2] J. R. Croy, K. G. Gallagher, M. Balasubramanian, B. R. Long, and M. M. Thackeray, J. Electrochem. Soc, 161, A318 (2014).

[3] D. Kim, G. Sandi, J. R. Croy, K. G. Gallagher, S.-H. Kang, E. Lee, M. D. Slater, C. S. Johnson, M. M. Thackeray, J. Electrochem. Soc., 160, A31 (2013).

[4] B. R. Long, J. R. Croy, J. S. Park, J. Wen, D. J. Miller, M. M. Thackeray, J. Electrochem. Soc, 161, A2160 (2014)



Support from the Vehicle Technologies Program, Hybrid and Electric Systems, in particular, David Howell, Peter Faguy, and Tien Duong at the U.S. Department of Energy, Office of Energy Efficiency and Renewable Energy, is gratefully acknowledged.  

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