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Novel Computational Approaches to Li Diffusion and Electron Transport for High Capacity Battery Materials

Published online by Cambridge University Press:  04 April 2011

Stefano Leoni ,
Gotthard Seifert ,
Luis Craco  and
Salah Eddine Boulfelfel
Stefano Leoni*
Affiliation:
Physical Chemistry Division, Dresden University of Technology, Dresden, Germany.
Gotthard Seifert
Affiliation:
Physical Chemistry Division, Dresden University of Technology, Dresden, Germany.
Luis Craco
Affiliation:
Physical Chemistry Division, Dresden University of Technology, Dresden, Germany.
Salah Eddine Boulfelfel
Affiliation:
Department of Geosciences, Stony Brook University, Stony Brook, New Yory, U.S.A.
*
*stefano.leoni@chemie.tu-dresden.de
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Abstract

The intrinsic channel structure and low volume work makes olivines phosphates (LiMPO4) versatile for Li uptake and release. The understanding of Li cation diffusion/transport mechanisms inside olivines are crucial aspects, which we address using advanced molecular dynamics simulations. Activation energies calculated from DFT concluded 1D diffusion within channels as also indicated by neutron diffraction direct imaging techniques. On explicitly including temperature we find that - besides main conduction paths along the easy channels - distinct, less frequent but relevant diffusion paths exist. We point out that capacity and diffusion/conduction issues must be understood in a much more detail-rich framework, under realistic simulation conditions within finite temperature simulations. For evaluating electrical conductivity, we use advanced DFT methods to correctly capture the insulating states of the charged and discharged olivine materials. Based on the Kubo formalism, reliable conductivity/resistivity curves can be calculated for comparison with experiments and for anticipating properties.

Keywords

diffusionionic conductorsimulation
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 1313: Symposium KK – Materials for Advanced Lithium Batteries , 2011 , mrsf10-1313-kk08-09
Copyright
Copyright © Materials Research Society 2011

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References

REFERENCES

1. Armand, M., Tarascon, J. M., Nature 451, 652 (2008).Google Scholar
2. Whittingham, M., Chem. Rev. 104, 4271 (2004).Google Scholar
3. Bruce, P. G., Solid State Ionics 179, 752 (2008).Google Scholar
4. Ellis, B. L., Lee, K. T., Nazar, L. F., Chem. Mater. 22, 691 (2010).Google Scholar
5. Goodenough, J. B., Kim, Y., Chem. Mater. 22, 587 (2010).Google Scholar
6. Islam, M.; Driscoll, D.; Fisher, C.; Slater, P. Chem Mater 17, 5085 (2005).Google Scholar
7. Morgan, D., der Ven, A. V., Ceder, G., Electrochem. Solid. St. 7, A30 (2004).Google Scholar
8. Nishimura, S.-I., Kobayashi, G., Ohoyama, K., Kanno, R., Yashima, M., Yamada, A., Nat. Mater. 7, 70 (2008).Google Scholar
9. Amin, R., Maier, J., Balaya, P., Chen, D. P., Lin, C. T., Solid State Ionics 179, 1683 (2008).Google Scholar
10. Dellago, C., Bolhuis, P., Geissler, P., Lect. Notes Phys. 703, 349 (2006).Google Scholar
11. Sørensen, M., Voter, A. J., Chem. Phys. 112, 9599 (2000).Google Scholar
12. Voter, A., Phys Rev Lett 78, 3908 (1997).Google Scholar
13. Boulfelfel, S. E., Seifert, G., Leoni, S., preprint.Google Scholar
14. Kotliar, G., Savrasov, S. Y., Haule, K., Oudovenko, V. S., Parcollet, O. and Marianetti, C. A., Rev. Mod. Phys. 78, 865 (2006).Google Scholar
15. Craco, L., Leoni, S., submitted to Phys. Rev. Lett.Google Scholar
16. Deb, A., Bergmann, U., Cairns, E. J. and Cramer, S. P., J. Synchrotron Rad. 11, 497 (2004).Google Scholar
17. Grenzebach, C., Anders, F. B., Czycholl, G., Phys. Rev. B 74, 195119 (2006).Google Scholar
18. Craco, L., Laad, M. S., Leoni, S., Europhysics Letters 91, 27001 (2010).Google Scholar