14-Electron Redox Chemistry Enabled by Salen-Based π-Conjugated Framework Polymer Boosting High-Performance...

Area of Science:

• Materials Science
• Electrochemistry
• Polymer Chemistry

Background:

• Organic materials for energy storage suffer from limited redox centers, poor charge transport, and instability.
• These limitations hinder their practical application in devices like lithium-ion batteries (LIBs).

Purpose of the Study:

• To develop a stable, redox-active organic material with enhanced charge transport for LIBs.
• To address the limitations of existing organic electrode materials.

Main Methods:

• Synthesis of a redox-active salen-based framework polymer (RSFP) with π-conjugated configuration.
• Ex situ X-ray photoelectron spectroscopy (XPS) to analyze structural evolution.
• Density functional theory (DFT) calculations to understand lithium-ion binding interactions.

Main Results:

• RSFP achieved a superior reversible capacity of 671.8 mAh g⁻¹ at 0.05 A g⁻¹ after 168 cycles.
• Exceptional performance with 946.2 mAh g⁻¹ reversible capacity after 3500 cycles at 2 A g⁻¹.
• XPS revealed active C═N, C─O, and C═O sites, with electrochemical triggering of C═O enhancing performance.

Conclusions:

• The developed RSFP overcomes key limitations of organic materials for energy storage.
• The material shows remarkable capacity retention and stability for LIB applications.
• This research offers a new pathway for designing high-performance redox-active organic electrode materials.