Affiliation:
1. State Key Laboratory of Control and Simulation of Power System and Generation Equipments Tsinghua University Beijing 100084 P. R. China
2. Centre for Clean Environment and Energy School of Environment and Science Griffith University Gold Coast Campus Gold Coast Queensland 4222 Australia
3. College of Chemical and Biological Engineering Zhejiang University Hangzhou 310027 P. R. China
Abstract
AbstractThe practical viability of high‐energy‐density lithium–sulfur (Li–S) batteries stipulates the use of a high‐loading cathode and lean electrolyte. However, under such harsh conditions, the liquid–solid sulfur redox reaction is much retarded due to the poor sulfur and polysulfides utilization, leading to low capacity and fast fading. Herein, a self‐assembled macrocyclic Cu(II) complex (CuL) is designed as an effective catalyst to homogenize and maximize the liquid‐involving reaction. The Cu(II) ion coordinated with four N atoms features a planar hybridization, showing a strong bonding affinity toward lithium polysulfides (LiPSs) along the orbital via steric effects. Such a structure not only lowers the energy barrier of the liquid–solid conversion (Li2S4 to Li2S2) but also guides a 3D deposition of Li2S2/Li2S. As such, with a 1 wt% electrolyte additive of CuL, a high initial capacity of 925 mAh g−1 and areal capacity of 9.62 mAh cm−2 with a low decay of 0.3%/cycle can be achieved under a high sulfur loading of 10.4 mg cm−2 and low electrolyte/sulfur ratio of 6 µL mgs−1. This work is expected to inspire the design of homogenous catalysts and accelerate the uptake of high‐energy‐density Li–S batteries.
Funder
State Grid Corporation of China
Subject
Mechanical Engineering,Mechanics of Materials,General Materials Science
Cited by
15 articles.
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