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some challenges are obstructing the practical application of the Li-S batteries, including the low utility and reversibility of insulating S and Li 2 S 2 /Li 2 S (Li 2 S 1-2 ) solids; the dissolution and poor cycling efficiency due to the shuttling behavior of soluble lithium polysulfides (LiPSs, e.g. Li 2 S 8 , Li 2 S 6 , and Li 2 S 4 ); the degradation of the electrode integrity resulting from large volume changes; and the low Columbic efficiency and safety issues caused by overactive lithium metal anodes. [1d,2] Success has been achieved with various strategies, for example, material confinement, [3] LiPS adsorption, [4] electrolyte modification, [5] and artificial solid-electrolyte interphase construction, [6] enabling new insights into nanoscale structures that can have a significant impact on improving battery performance.One key issue still impeding commercialization of Li-S batteries, however, is the existing compromise on the practical energy density, arising from the low amount of S (sulfur loading of <2.0 mg cm −2 ) and the excess electrolyte (electrolyte/sulfur ratios of >11 µL mg −1 ) that are currently used, which compensates for the sluggish electron and Li ion transfer in the insulating solid S and the Li 2 S 1-2 discharge products. [2b,c,7] It has been proved that pre-distribution of S among porous and conductive carbon materials is significant for improving S utilization since sufficient electronic/ionic channels are constructed. [3a,8] When the soluble LiPS intermediates are dissolved in electrolyte, however, the redistribution of Li 2 S 1-2 precipitates can block the porous structure of the cathode surface. The limited charge transfer due to the thick and non-conductive features of the Li 2 S 1-2 layer (as shown in Figure 1a) causes low specific capacity and electrode degradation, especially under the practical harsh kinetic conditions (e.g., high rate, high loading mass, and lean electrolyte). [1d,9] Possible ways to solve the problem are inhibiting the dissolution of LiPS intermediates or achieving a uniform deposition of Li 2 S 1-2 , not only on the surface but also throughout the whole cathode. Previous studies have indicated the pivotal role of LiPS dissolution in improving the reaction kinetics, because of the dominant interfacial reactions for S based cathodes. [9b,e,10] Therefore, uniform deposition of Li 2 S 1-2 throughout the whole cathode is essential for obtaining superior performance, as shown in Figure 1b.Currently, the formation mechanism of the Li 2 S 1-2 layer on the cathode surface is still unclear, although it has been Challenges from the insulating S and Li 2 S 2 /Li 2 S (Li 2 S 1-2 ) discharge products are restricting the development of the high-energy-density Li-S battery system. The deposition of insulating Li 2 S 1-2 on the surfaces of S based cathodes (e.g., S and Li 2 S) limits the reaction kinetics, leading to inferior electrochemical performance. In this work, the impact of binders on the deposition of Li 2 S 1-2 on S based cathodes is revealed, along with...
some challenges are obstructing the practical application of the Li-S batteries, including the low utility and reversibility of insulating S and Li 2 S 2 /Li 2 S (Li 2 S 1-2 ) solids; the dissolution and poor cycling efficiency due to the shuttling behavior of soluble lithium polysulfides (LiPSs, e.g. Li 2 S 8 , Li 2 S 6 , and Li 2 S 4 ); the degradation of the electrode integrity resulting from large volume changes; and the low Columbic efficiency and safety issues caused by overactive lithium metal anodes. [1d,2] Success has been achieved with various strategies, for example, material confinement, [3] LiPS adsorption, [4] electrolyte modification, [5] and artificial solid-electrolyte interphase construction, [6] enabling new insights into nanoscale structures that can have a significant impact on improving battery performance.One key issue still impeding commercialization of Li-S batteries, however, is the existing compromise on the practical energy density, arising from the low amount of S (sulfur loading of <2.0 mg cm −2 ) and the excess electrolyte (electrolyte/sulfur ratios of >11 µL mg −1 ) that are currently used, which compensates for the sluggish electron and Li ion transfer in the insulating solid S and the Li 2 S 1-2 discharge products. [2b,c,7] It has been proved that pre-distribution of S among porous and conductive carbon materials is significant for improving S utilization since sufficient electronic/ionic channels are constructed. [3a,8] When the soluble LiPS intermediates are dissolved in electrolyte, however, the redistribution of Li 2 S 1-2 precipitates can block the porous structure of the cathode surface. The limited charge transfer due to the thick and non-conductive features of the Li 2 S 1-2 layer (as shown in Figure 1a) causes low specific capacity and electrode degradation, especially under the practical harsh kinetic conditions (e.g., high rate, high loading mass, and lean electrolyte). [1d,9] Possible ways to solve the problem are inhibiting the dissolution of LiPS intermediates or achieving a uniform deposition of Li 2 S 1-2 , not only on the surface but also throughout the whole cathode. Previous studies have indicated the pivotal role of LiPS dissolution in improving the reaction kinetics, because of the dominant interfacial reactions for S based cathodes. [9b,e,10] Therefore, uniform deposition of Li 2 S 1-2 throughout the whole cathode is essential for obtaining superior performance, as shown in Figure 1b.Currently, the formation mechanism of the Li 2 S 1-2 layer on the cathode surface is still unclear, although it has been Challenges from the insulating S and Li 2 S 2 /Li 2 S (Li 2 S 1-2 ) discharge products are restricting the development of the high-energy-density Li-S battery system. The deposition of insulating Li 2 S 1-2 on the surfaces of S based cathodes (e.g., S and Li 2 S) limits the reaction kinetics, leading to inferior electrochemical performance. In this work, the impact of binders on the deposition of Li 2 S 1-2 on S based cathodes is revealed, along with...
Batteries & Supercaps www.batteries-supercaps.org Review doi.org/10.1002/batt.202200097 Lithium-sulfur (LiÀ S) batteries are recognized as one of the most promising technologies with the potential to become the next-generation batteries. However, to ensure LiÀ S batteries reach commercialization, complex challenges remain, among which the tailoring of an appropriate electrolyte is the most important. This review discusses the role of electrolytes in LiÀ S batteries, focusing on the main issues and solutions for the shuttle mechanism of polysulfides and the instability of the interface with lithium metal. Herein, we present a background on LiÀ S chemistry followed by the state-of-the-art electrolytes highlighting the different strategies undertaken with liquid and solid electrolytes.
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