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Catalytic Polysulfide Conversion and Physiochemical Confinement for Lithium–Sulfur Batteries
Author(s) -
Sun Zixu,
Vijay Sudarshan,
Heenen Hendrik H.,
Eng Alex Yong Sheng,
Tu Wenguang,
Zhao Yunxing,
Koh See Wee,
Gao Pingqi,
Seh Zhi Wei,
Chan Karen,
Li Hong
Publication year - 2020
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.201904010
Subject(s) - polysulfide , nanocages , materials science , catalysis , chemical engineering , sulfur , cobalt , electrode , energy storage , nitride , battery (electricity) , carbon fibers , nanoparticle , lithium–sulfur battery , inorganic chemistry , nanotechnology , composite number , chemistry , composite material , electrochemistry , organic chemistry , electrolyte , power (physics) , physics , quantum mechanics , layer (electronics) , engineering , metallurgy
The lithium–sulfur (Li–S) battery is widely regarded as a promising energy storage device due to its low price and the high earth‐abundance of the materials employed. However, the shuttle effect of lithium polysulfides (LiPSs) and sluggish redox conversion result in inefficient sulfur utilization, low power density, and rapid electrode deterioration. Herein, these challenges are addressed with two strategies 1) increasing LiPS conversion kinetics through catalysis, and 2) alleviating the shuttle effect by enhanced trapping and adsorption of LiPSs. These improvements are achieved by constructing double‐shelled hollow nanocages decorated with a cobalt nitride catalyst. The N‐doped hollow inner carbon shell not only serves as a physiochemical absorber for LiPSs, but also improves the electrical conductivity of the electrode; significantly suppressing shuttle effect. Cobalt nitride (Co 4 N) nanoparticles, embedded in nitrogen‐doped carbon in the outer shell, catalyze the conversion of LiPSs, leading to decreased polarization and fast kinetics during cycling. Theoretical study of the Li intercalation energetics confirms the improved catalytic activity of the Co 4 N compared to metallic Co catalyst. Altogether, the electrode shows large reversible capacity (1242 mAh g −1 at 0.1 C), robust stability (capacity retention of 658 mAh g −1 at 5 C after 400 cycles), and superior cycling stability at high sulfur loading (4.5 mg cm −2 ).