@article{Shi2024, 
author = {Zixiong Shi and Simil Thomas and Zhengnan Tian and Dong Guo and Zhiming Zhao and Yizhou Wang and Shuo Li and Nimer Wehbe and Abdul-Hamid Emwas and Osman M. Bakr and Omar F. Mohammed and Husam N. Alshareef},
title = {A tailored highly solvating electrolyte toward ultra lean-electrolyte Li–S batteries},
year = {2024},
journal = {Nano Research Energy},
volume = {3},
pages = {e9120126},
keywords = {Li–S batteries, donicity, Li2S dissociation, lean-electrolyte, S3•– radical},
url = {https://www.sciopen.com/article/10.26599/NRE.2024.9120126},
doi = {10.26599/NRE.2024.9120126},
abstract = {Low electrolyte usage is a key to attaining high-energy-density lithium–sulfur (Li–S) batteries. However, this is still a tremendous challenge for traditional ether-based electrolytes that follow a dissolution–precipitation mechanism. Highly solvating electrolytes, which can facilitate polysulfide dissolution and alter reaction pathway, are considered a promising strategy. Nonetheless, mechanistic understanding and kinetic evaluation remain insufficient while the principle of Li2S nucleation and dissociation has not been elucidated. Herein, we unveil the Li-ion solvation and polysulfide speciation in the solvents with different denticity and donicity. The origin of S3•– radical-directed path and three-dimensional Li2S precipitation in high-donicity electrolytes has been uncovered. It is revealed that ammonium ions enable the facile dissolution and dissociation of Li2S via Lewis acid-base interaction and H···S2– binding. Consequently, Li–S batteries with a low electrolyte and sulfur (E/S) ratio of 5 μL·mgs–1 achieve a high capacity of 1092 mAh·g–1. Even at a harsh E/S ratio of 3 μL·mgs–1 and a high sulfur loading of 4 mg·cm–2, they still sustain a stable operation over 30 cycles. Our work sheds light on the underlying reaction mechanism and rationalizes the design of highly solvating electrolytes, which in turn opens a new avenue for achieving pragmatic lean-electrolyte Li–S batteries.}
}