Edge functionalization of graphyne nanoribbons for lithium-ion battery electrodes: a computational study

Area of Science:

• Materials Science
• Electrochemistry
• Computational Chemistry

Background:

• Lithium-ion batteries (LIBs) are crucial for energy storage, with graphene widely used.
• Graphyne, a novel nanomaterial, shows potential for advanced electrode designs in LIBs.

Purpose of the Study:

• To investigate the suitability of 56 unique graphyne compounds as cathode materials for LIBs.
• To systematically analyze the structure and electronic properties of substituted graphyne using DFT.

Main Methods:

• Density Functional Theory (DFT) calculations were employed.
• 56 unique graphyne compounds with eight different substituents were synthesized and analyzed.
• Redox potentials of graphyne compounds were evaluated.

Main Results:

• Nitro and carbonyl functional groups significantly enhanced redox potential, reaching up to 5.0 V and 2.9 V, respectively.
• Most substituents did not alter redox potential compared to pristine graphyne.
• Tetrasubstituted trifluoromethyl graphyne reached a potential of 2.9 V.
• Highest redox potentials were linked to locally distributed configurations in multi-substituted graphyne.

Conclusions:

• Graphyne derivatives, particularly those with nitro and carbonyl groups, show significant potential as high-performance cathode materials for LIBs.
• Controlled substitution within the graphyne framework is key to optimizing redox potentials for energy storage applications.