%0 Journal Article
%A Miao Liu
%A Anubhav Jain
%A Ziqin Rong
%A Xiaohui Qu
%A Pieremanuele Canepa
%A Rahul Malik
%A Gerbrand Ceder
%A Kristin A Persson
%B Energy & Environmental Science
%D 2016
%G eng
%N 10
%P 3201 - 3209
%R 10.1039/C6EE01731B
%T Evaluation of sulfur spinel compounds for multivalent battery cathode applications
%V 9
%8 10/2016
%! Energy Environ. Sci.
%X <p><span>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, Cr</span><small><span>2</span></small><span>S</span><small><span>4</span></small><span>, Ti</span><small><span>2</span></small><span>S</span><small><span>4</span></small><span>&nbsp;and Mn</span><small><span>2</span></small><span>S</span><small><span>4</span></small><span>&nbsp;spinel compounds exhibit improved Mg</span><small><span>2+</span></small><span>&nbsp;mobility (diffusion activation energy &lt;650 meV) relative to their oxide counterparts, however the improved mobility comes at the expense of lower voltage and thereby lower theoretical specific energy. Ca</span><small><span>2+</span></small><span>&nbsp;intercalating into Cr</span><small><span>2</span></small><span>S</span><small><span>4</span></small><span>&nbsp;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.</span></p>