Synergistic Co-Optimization Strategy for Electron-Ion Transport Kinetics in all-Solid-State Sulfurized...

Area of Science:

• Materials Science
• Electrochemistry
• Energy Storage

Background:

• Sulfurized polyacrylonitrile (SPAN) cathodes offer high conductivity for lithium-sulfur batteries.
• Current micron-sized granular SPAN (GSPAN) cathodes face limitations in all-solid-state lithium-sulfur batteries (ASSLSBs) due to poor electron/ion transport.
• These limitations hinder electrochemical performance in ASSLSBs.

Purpose of the Study:

• To address the electrochemical performance limitations of SPAN cathodes in ASSLSBs.
• To design and fabricate a nanofibrous SPAN cathode (FSPAN) with enhanced charge transport pathways.
• To validate a materials design strategy for improving ASSLSB performance.

Main Methods:

• Fabrication of a nanofibrous SPAN cathode (FSPAN) using electrospinning and programmed pyrolysis.
• Characterization of the 3D-interwoven nanofiber architecture for continuous conductive networks.
• Evaluation of electrochemical performance, including specific capacity and rate capability.

Main Results:

• The FSPAN cathode exhibits a 3D-interwoven nanofiber architecture facilitating efficient charge-carrier migration.
• Optimized ion/electron transport dynamics significantly reduce interfacial resistance and enhance redox kinetics.
• Achieved a high reversible specific capacity of 1467.2 mAh g^-1 at 0.2 C.
• Demonstrated a stable discharge capacity of ≈500 mAh g^-1 at 2 C, a fivefold improvement over GSPAN.

Conclusions:

• The nanofibrous architecture of FSPAN effectively overcomes the kinetic limitations of conventional SPAN cathodes in ASSLSBs.
• Spatially synergistic optimization of charge transport pathways is a viable strategy for enhancing ASSLSB performance.
• The developed FSPAN cathode represents a significant advancement for high-performance all-solid-state lithium-sulfur batteries.