A Sodium Polysulfide Battery with Liquid Solid Electrolyte Improving Sulfur Utilization Using P2S5 as Additive and Tetramethylurea as Catholyte Solvent

Abstract

Herein, the proof of concept of a sodium polysulfide battery consisting of two electrode chambers being separated by a solid electrolyte is described. The concept is suited for dissolved polysulfide cathodes and has the advantage that both half reactions can be optimized separately. The formation of solid sulfide discharge products is identified as the major limiting factor for cell cycling. This issue can be alleviated by adding solid P2S5. Further improvement can be achieved by replacing diglyme 2G as the cathode compartment solvent with tetramethylurea TMU . Using TMU, the cell cycles with Coulombic efficiencies gt;99 and capacities of 800 amp; 8201;mAh amp; 8201;g amp; 8722;1 are maintained for at least 30 cycles. Viscosity, density, conductivity, and the electrochemical stability window values of the 2G amp; 8208; and TMU amp; 8208;based electrolytes are compared. The latter shows higher viscosity 2.806 vs 1.603 amp; 8201;mPa amp; 8201;s , higher density 1.016 vs 0.996 amp; 8201;g amp; 8201;cc amp; 8722;1 , and higher conductivity 4.27 vs 1.45 amp; 8201;mS amp; 8201;cm amp; 8722;1 . The oxidative stability limit of the TMU electrolyte is 3.2 amp; 8201;V versus Na Na, which is sufficient for polysulfide redox reactions. Vis spectroscopy is used to follow the electrode reaction. In case of TMU, the reaction is based on the redox activity of S3 amp; 8722; radicals blue coloration of the catholyte solutio