Amorphous/crystalline interface synergistic catalysis: CoSₓ/MnS heterostructure for high-performance Li-CO₂ batteries

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Lithium-carbon dioxide (Li-CO₂) batteries offer high energy density and CO₂ conversion.
• Sluggish kinetics in CO₂ reduction/evolution reactions (CO₂RR/CO₂ER) limit practical applications.

Purpose of the Study:

• To design a novel catalyst for enhanced Li-CO₂ battery performance.
• To address the kinetic limitations of CO₂RR and CO₂ER.

Main Methods:

• Fabrication of a self-supporting heterostructure catalyst: amorphous CoSₓ/crystalline MnS (a-CoSₓ/c-MnS).
• Utilizing an amorphous/crystalline interface synergistic strategy.
• Characterization of the catalyst's structure, electronic properties, and electrochemical performance.

Main Results:

• The a-CoSₓ/c-MnS catalyst exhibits strong electronic coupling and optimized intermediate adsorption.
• A 3D urchin-like architecture facilitates efficient electron, ion, and gas transport.
• The catalyst effectively regulates discharge products, mitigating passivation and enabling easier decomposition.
• Achieved ultra-low overpotential (0.22 V), high Coulombic efficiency (98.62%), and energy efficiency (91.38%).
• Demonstrated stable cycling over 2000 hours at a limited capacity.

Conclusions:

• The amorphous/crystalline interface strategy significantly enhances bifunctional CO₂RR and CO₂ER activity.
• The designed catalyst improves Li-CO₂ battery efficiency and cycle life.
• This work presents a promising pathway for advanced energy storage systems.