Fast Polysulfide Conversion Catalysis and Reversible Anode Operation by A Single Cathode Modifier in Li-Metal Anode-Free Lithium-Sulfur Batteries

Abstract

The two major issues confronting the commercialization of rechargeable lithium-sulfur (Li−S) batteries are the sluggish kinetics of the sulfur electrochemical reactions on the cathode and inadequate lithium deposition/stripping reversibility on the anode. They are commonly mitigated with additives designed specifically for the anode and the cathode individually. Here, we report the use of a single cathode modifier, In2Se3, which can effectively catalyse the polysulfide reactions on the cathode, and also improve the reversibility of Li deposition and removal on the anode through a LiInS2/LiInSe2 containing solid electrolyte interface formed in situ by the Se and In ions dissolved in the electrolyte. The amounts of dissolved Se and In are small relative to the amount of In2Se3 administered. The benefits of using this single modification approach were verified in Li-metal anode-free Li−S batteries with a Li2S loading of 4 mg cm−2 and a low electrolyte/Li2S ratio of 7.5 μL mg−1. The resulting battery showed 60 % capacity retention after 160 cycles at the 0.2 C rate and an average Coulombic efficiency of 98.27 %, comparing very well with recent studies using separate electrode modifiers.