Lithium Sulfonate Functionalization of Carbon Cathodes as a Substitute for Lithium Nitrate in the Electrolyte of Lithium–Sulfur Batteries
Journal article, 2020

A method for grafting lithium sulfonate (LiSO3) groups to carbon surfaces is developed and the resulting carbons are evaluated for their potential to reduce the lithium polysulfide (LiPS) shuttle in lithium–sulfur (Li–S) batteries, replacing the common electrolyte additive lithium nitrate (LiNO3). The LiSO3 groups are attached to the ordered mesoporous carbon (CMK3) surface via a three-step procedure to synthesize LiSO3-CMK3 by bromomethylation, sodium sulfite (Na2SO3) substitution, and cation exchange. As a comparison, ethylenediamine (EN)-substituted CMK3, EN-CMK3, is also synthesized and tested. When used as a cathode in Li–S batteries, the unfunctionalized CMK3 suffers from strong LiPS shuttling as evidenced by its low initial Coulombic efficiencies (ICEs, <10%) compared to its functionalized derivatives EN-CMK3 and LiSO3-CMK3 (ICEs >75%). Postcycling analysis reveals the benefits of cathode surface functionalization on the lithium anode via an attenuated LiPS shuttle. When monitored at open circuit, the functionalized cathodes maintain their cell voltages much better than the CMK3 control and concurrent electrochemical impedance spectroscopy reveals their higher total cell resistance, which provides evidence for a reduced LiPS shuttle in the vicinity of both electrodes. Overall, such surface groups show promise as cathode-immobilized “lithium nitrate mimics.”.


lithium nitrate

lithium polysulfide shuttle

surface functionalization

Li–S batteries


Samuel Joseph Fretz

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Urbi Pal

Deakin University

Gaetan M.A. Girard

Deakin University

P. C. Howlett

Deakin University

Anders Palmqvist

Chalmers, Chemistry and Chemical Engineering, Applied Chemistry

Advanced Functional Materials

1616-301X (ISSN) 16163028 (eISSN)

Vol. 30 35 2002485

Subject Categories

Materials Chemistry

Other Chemical Engineering

Other Chemistry Topics



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