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Enhancing Bidirectional Sulfur Conversion Through p-d Orbital Hybridization via Vacancy Engineering.

Yan Chen¹, Dan Li¹, Yufang Chen²

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Exploration (Beijing, China)

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Summary

Researchers developed a new catalyst, CWO-M, by regulating oxygen vacancies in CoWO4 to improve lithium-sulfur batteries (LSBs). This catalyst enhances kinetics, boosting performance and stability for advanced energy storage solutions.

Keywords:

bidirectional catalysis lithium–sulfur batteries oxygen vacancy

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Published on: October 12, 2019

Area of Science:

Materials Science
Electrochemistry
Catalysis

Background:

Lithium-sulfur batteries (LSBs) offer high energy density but suffer from the shuttle effect and slow redox kinetics.
These limitations hinder their practical application in energy storage.

Purpose of the Study:

To develop a strategy for accelerating polysulfide kinetics in LSBs.
To investigate the role of oxygen vacancy concentration in CoWO4 as a catalyst.

Main Methods:

Experimental synthesis and characterization of CoWO4 with modulated oxygen vacancies (CWO-M).
Density functional theory (DFT) calculations to understand catalytic mechanisms.
Electrochemical testing of CWO-M/S cathodes in LSBs.

Main Results:

CWO-M exhibits optimal adsorption energy and catalytic capacity for polysulfides due to p-d orbital hybridization.
Demonstrated a bidirectional catalytic effect, accelerating both sulfur reduction and Li2S oxidation.
Achieved excellent rate performance (768 mAh g⁻¹ at 2 C) and high capacity retention (91.1% after 100 cycles at 0.2 C).
Stable cycling with high capacity (4 mAh cm⁻²) at high sulfur loading (8.02 mg cm⁻²) and low E/S ratio (8 µL mg S⁻¹).

Conclusions:

Modulating oxygen vacancy concentration in CoWO4 provides effective bidirectional catalysis for LSBs.
CWO-M significantly enhances the electrochemical performance and stability of LSBs.
This approach offers valuable insights for designing advanced catalysts for high-performance LSBs.