Greatly Suppressed Shuttle Effect for Improved Lithium Sulfur Battery Performance through Short Chain Intermediates

Abstract

The high solubility of long-chain lithium polysulfides and their infamous shuttle effect in lithium sulfur battery lead to rapid capacity fading along with low Coulombic efficiency. To address above issues, we propose a new strategy to suppress the shuttle effect for greatly enhanced lithium sulfur battery performance mainly through the formation of short-chain intermediates during discharging, which allows significant improvements including high capacity retention of 1022 mAh/g with 87% retention for 450 cycles. Without LiNO-containing electrolytes, the excellent Coulombic efficiency of ∼99.5% for more than 500 cycles is obtained, suggesting the greatly suppressed shuttle effect. In situ UV/vis analysis of electrolyte during cycling reveals that the short-chain LiS and LiS polysulfides are detected as main intermediates, which are theoretically verified by density functional theory (DFT) calculations. Our strategy may open up a new avenue for practical application of lithium sulfur battery.

Recent Advances in Applying Vulcanization/Inverse Vulcanization Methods to Achieve High‐Performance Sulfur‐Containing Polymer Cathode Materials for Li–S Batteries

“…j) The corresponding UV/vis spectra first‐order derivative curves of S‐GSH electrodes at a current rate of C/3. Reproduced with permission . Copyright 2016, American Chemical Society.…”

“…Yan and co‐workers presented a copolymer of elemental sulfur with sulfhydryl‐functionalized graphene nanosheets (as shown in Figure g, and the copolymer is denoted as S‐GSH), which can suppress the shuttle effect based on the formation of short chain polysulfide discharge products. They used in situ UV/vis spectra to identify the discharge products according to the UV/vis reflection wavelength “standards” (Figure i) obtained from the spectra of different polysulfide concentrations.…”

Simultaneous Suppression of the Dendrite Formation and Shuttle Effect in a Lithium–Sulfur Battery by Bilateral Solid Electrolyte Interface

“…The high energy density, low cost, and the environmentally friendly nature of Li‐S batteries make them attractive for use in automotive or stationary electrical energy storage applications 1, 2, 3, 4, 5, 6, 7. However, the severe shuttle effect and dendrite growth, and the inferior Coulombic efficiency that characterize these Li‐S batteries have greatly limited their lifespan 4, 8, 9, 10.…”

Revisiting Scientific Issues for Industrial Applications of Lithium–Sulfur Batteries

“…[16,17] Therefore, it is difficult for the active materials to obtain or lose electrons quickly from the current collector, leading to increased electronic resistivity and poor rate performance. [21][22][23] The involved reactions can be illustrated as follows: Consequently, the utilization of active material is low with undermined discharge capacity.…”