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a Surface pathway (+Li+) Solution pathway (+S2-/S2- ) 36 Li2S (s) +e- +Li+ Li2S4 (s) E=1.85 ±0.3 V Li2S4(l)-retaining +e- Li2S4 (s) Li2S (s) Coulombic efficiency Energy EPR Intensity (a.u.) Carbon matrix Carbon matrix 1254 mAh g-1 s b CS2-/ CS2- 36 L i 2 S 4 ( s ) +e - 6 E=2.05 ±0.3 V c T=298 K E_G2 E_DOL/DME_saturated Li2S4 T=125 K 2800 3000 3200 3400 3600 Magnetic field (Gauss) in the lower discharge plateau DOL/DME Medium dielectric constant solvent and high ionic association strength anions High dielectric constant solvent E_G2_0.50 M Li S 2 4 Sulfur utlization efficiency Surface pathway Solution pathway Li2S (s) E =2 . 1 V S2- (l) Figure 3 ǀ Electrolyte dependence of sulfur discharge pathway. (a) Schematics of the effect of Li2S4-retaining solution pathway on the free-energy plot for Li2S4/Li2S (left), and different pathways in the lower discharge plateau (right). S62− is electrochemically reduced to S32− at the carbon matrix surface, and then S32− chemically reacts with solid Li2S4, producing solid Li2S and itself being regenerated to S62−. Initial S32− comes from the reduction of S42−-retaining in bulk electrolyte. As for the surface pathway, solid Li2S4 is electrochemically reduced with Li+ to solid Li2S with a higher overpotential at the carbon matrix surface; (b) Solvent and anion dependence of sulfur discharge pathway; (c) EPR spectra of E_G2, E_G2_0.5 M Li2S4 and E_DOL/DME_ saturated Li2S4 at 298 K (upper) and 125 K (lower). Page 17 of 24 S2- (l) 3PDF Image | A lithium-sulfur battery with a solution-mediated pathway
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