Abstract

Lithium–sulfur (Li–S) batteries are expected to be very useful for next-generation transportation and grid storage because of their high energy density and low cost. However, their low active material utilization and poor cycle life limit their practical application. The use of a carbon-coated separator in these batteries serves to inhibit the migration of the lithium polysulfide intermediate and increases the recyclability. We report the extent to which the electrochemical performance of Li–S battery systems depends on the characteristics of the carbon coating of the separator. Carbon-coated separators containing different ratios of carbon black (Super-P) and vapor-grown carbon fibers (VGCFs) were prepared and evaluated in Li–S batteries. The results showed that larger amounts of Super-P on the carbon-coated separator enhanced the electrochemical performance of Li–S batteries; for instance, the pure Super-P coating exhibited the highest discharge capacity (602.1 mAh g−1 at 150 cycles) with a Coulombic efficiency exceeding 95%. Furthermore, the separators with the pure Super-P coating had a smaller pore structure, and hence, limited polysulfide migration, compared to separators containing Super-P/VGCF mixtures. These results indicate that it is necessary to control the porosity of the porous membrane to control the movement of the lithium polysulfide.

Highlights

  • The continuously increasing worldwide demand for energy has resulted in energy storage systems becoming essential for the successful implementation of various electric devices such as electric vehicles, portable electronic devices, and energy storage systems [1,2,3,4,5,6]

  • Despite the many advantages of sulfur cathodes, Li–S batteries have poor cycle performance due to following chronic drawbacks, which lead failure at successful commercialization [7,8,9,10,11]: (1) Sulfur has insulating properties that interfere with uniform electrons throughout the active materials during operation

  • Lithium polysulfide dissolves in the electrolyte from the sulfur cathode and consumes electrons directly from the both electrodes, cathodes, and anodes inside the battery system, unlike conventional battery systems, where electrons are consumed along the conductors

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Summary

Introduction

The continuously increasing worldwide demand for energy has resulted in energy storage systems becoming essential for the successful implementation of various electric devices such as electric vehicles, portable electronic devices, and energy storage systems [1,2,3,4,5,6]. Lithium polysulfide dissolves in the electrolyte from the sulfur cathode and consumes electrons directly from the both electrodes, cathodes, and anodes inside the battery system, unlike conventional battery systems, where electrons are consumed along the conductors. This series of internal cyclic electron consumption is called the “shutting effect” [12,13,14]. The carbon-coated separators improve the cycle performance of the Li–S batteries by helping the sulfur cathodes to reuse lithium polysulfides during the repeated charging/discharging processes. Changing the VGCF to Super-P ratio in the carbon-coated separator enabled us to optimize the porosity of the separator as an effective approach to obtain a stable high-performance Li–S battery with exceptional rate capability

Materials
Preparation of the VGCF and Super-P Carbon Composite
Preparation of the Modified Separators
Preparation of the Sulfur Cathode and Cell Assembly
Electrochemical Testing
Characterization and Electrochemical Measurements
Electrochemical Performance
Conclusions
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