Evaluation of sulfur spinel compounds for multivalent battery cathode applications.

Liu, M.; Jain, A.; Rong, Z.; Qu, X.; Canepa, P.; Malik, R.; Ceder, G.; Persson, K.

doi:10.1039/C6EE01731B

Evaluation of sulfur spinel compounds for multivalent battery cathode applications.

M. Liu, A. Jain, Z. Rong, X. Qu, P. Canepa, R. Malik, G. Ceder, and K. Persson; Energy Environ. Sci. 9, 3201–3209 (2016).

BibTeX

@article{Liu2016evaluation,
  author  = {Liu, M. and Jain, A. and Rong, Z. and Qu, X. and Canepa, P. and Malik, R. and Ceder, G. and Persson, K.},
  title   = {{Evaluation of sulfur spinel compounds for multivalent battery cathode applications}},
  journal = {Energy & Environmental Science},
  volume  = {9},
  pages   = {3201--3209},
  year    = {2016},
  doi     = {10.1039/C6EE01731B}
}

Abstract

The rapid growth of portable consumer electronics and electric vehicles demands new battery technologies with greater energy stored at a reduced cost. Energy storage solutions based on multivalent metals, such as Mg, could significantly increase the energy density as compared to lithium-ion based technology. In this paper, we employ density functional theory calculations to systematically evaluate the performance, such as thermodynamic stability, ion diffusivity and voltage, of a group of 3d transition-metal sulfur-spinel compounds (21 in total) for multivalent cathode applications. Based on our calculations, Cr₂S₄, Ti₂S₄ and Mn₂S_{4</sub spinel compounds exhibit improved Mg²⁺ mobility (diffusion activation energy <650 meV) relative to their oxide counterparts, however the improved mobility comes at the expense of lower voltage and thereby lower theoretical specific energy. Ca²⁺ intercalating into Cr₂S₄ spinel exhibits a low diffusion activation barrier of 500 meV and a voltage of ∼2 V, revealing a potential cathode for use in Ca rechargeable batteries.}