Radical Anion Functionalization of Two-Dimensional Materials as a Means ofEngineering Simultaneously High Electronic...

Area of Science:

• Materials Science
• Electrochemistry
• Nanotechnology

Background:

• Two-dimensional (2D) materials like hexagonal boron nitride (h-BN) offer unique properties but often require functionalization for specific applications.
• Developing multifunctional materials for energy storage is crucial for improving device efficiency and reducing complexity.

Purpose of the Study:

• To propose a novel radical anion-based functionalization strategy for the basal plane of h-BN and other 2D materials.
• To demonstrate the potential of these functionalized materials as simultaneous cathode electroactive species and solid ion conductors.
• To explore their application in energy storage devices, particularly all-solid-state batteries and supercapacitors.

Main Methods:

• A two-step synthesis involving the formation of a Lewis adduct followed by thermal splitting to generate radical anions.
• Functionalization of h-BN with [·OBX3]- radical anions (X=F, Cl) in the presence of Li, Na, or Mg cations.
• Characterization of the resulting material's electronic conductivity and electrochemical properties.

Main Results:

• Successful synthesis of A_n[(BN)2OBX3] materials with tunable electronic conductivity (up to 1 S/cm) based on cation concentration.
• Demonstrated reversible oxidation without functional group detachment, enabling dual functionality as cathode and ion conductor.
• Predicted high performance for Li[(BN)2OBF3], including 5.6 V open circuit voltage and 1067 Wh/kg specific energy.

Conclusions:

• The proposed radical anion functionalization offers a versatile route to multifunctional 2D materials for energy storage.
• These materials can significantly enhance energy storage device efficiency by reducing component count and interfacial impedance.
• The developed materials hold promise for next-generation solid-state batteries and supercapacitors with improved performance and cost-effectiveness.