Low-Tortuous and Dense Electrode for High-Energy Lithium-Sulfur Batteries

Abstract

Lithium-sulfur (Li-S) batteries feature a high theoretical capacity of 1675 mAh/g and hence is considered as a promising alternative to lithium-ion batteries. However, deployment of Li-S batteries has been hindered by the low practical energy and limited cycle life. 1, 2 Reducing cathode porosity is essential to balancing the electrolyte distribution in Li-S cell, conserving more pore-filling electrolyte to extend cell cycle life. 3-5 However, low-porosity electrodes built with nanosized sulfur/carbon (S/C) materials suffer from high tortuosity that significantly deteriorates electrode wetting and hence sulfur utilization. Enabling operation of high-loading sulfur electrodes under both low-porosity and lean-electrolyte conditions is still a challenge and is seldom discussed. In this study, 6 we demonstrated a novel and facile strategy for constructing low-tortuosity through-pores across both vertical and planar directions of electrodes by casting large particles into single-particle-layer electrodes. Through multi-scale characterizations and simulations, correlations between material/electrode structures, electrolyte permeability, polysulfide migration, and sulfur reactions were elucidated. The high-loading and dense sulfur cathode fabricated by this method delivers a high specific capacity (>1000 mAh g -1 ) at a very low electrolyte/sulfur (E/S) ratio of 4 μL mg -1 . This study provides a novel approach to reducing the tortuosity of dense sulfur electrodes by manipulating the porosity distribution, which would be also applicable to improving the rate capability of other high-energy electrodes. More details of the progress will be discussed at the meeting. Reference. Dörfler, S.; Althues, H.; Härtel, P.; Abendroth, T.; Schumm, B.; Kaskel, S., Challenges and Key Parameters of Lithium-Sulfur Batteries on Pouch Cell Level. Joule 2020, 4 (3), 539-554. Xue, W.; Miao, L.; Qie, L.; Wang, C.; Li, S.; Wang, J.; Li, J., Gravimetric and volumetric energy densities of lithium-sulfur batteries. Current Opinion in Electrochemistry 2017, 6 (1), 92-99. Lu, D.; Li, Q.; Liu, J.; Zheng, J.; Wang, Y.; Ferrara, S.; Xiao, J.; Zhang, J. G.; Liu, J., Enabling High-Energy-Density Cathode for Lithium-Sulfur Batteries. ACS Appl Mater Interfaces 2018, 10 (27), 23094-23102. Kang, N.; Lin, Y.; Yang, L.; Lu, D.; Xiao, J.; Qi, Y.; Cai, M., Cathode porosity is a missing key parameter to optimize lithium-sulfur battery energy density. Nat Commun 2019, 10 (1), 4597. Feng, S.; Liu, J.; Zhang, X.; Shi, L.; Anderson, C.; Lin, Y.; Song, M.-K.; Liu, J.; Xiao, J.; Lu, D., Rationalizing nitrogen-doped secondary carbon particles for practical lithium-sulfur batteries. Nano Energy 2022, 103 . Feng, S.; Singh, R. K.; Fu, Y.; Li, Z.; Wang, Y.; Bao, J.; Xu, Z.; Li, G.; Anderson, C.; Shi, L.; Lin, Y.; Khalifah, P. G.; Wang, W.; Liu, J.; Xiao, J.; Lu, D., Low-tortuous and dense single-particle-layer electrode for high-energy lithium-sulfur batteries. Energy & Environ. Sci. 2022 .