Enhancement of quantum capacitance in graphene electrodes by chemical modifications using aliphatic/aromatic molecules and their radicals

TL;DR

This study demonstrates that chemical functionalization of graphene with aliphatic and aromatic radicals significantly enhances its quantum capacitance, potentially improving supercapacitor electrode performance.

Contribution

The paper introduces a theoretical approach showing radical functionalization of graphene markedly increases quantum capacitance, a novel insight for supercapacitor material design.

Findings

Radical functionalization yields quantum capacitance above 200 μF/cm^2

Localized density of states near Fermi level enhances capacitance

Atomic dislocation and vacancies influence functionalization effects

Abstract

We have carried out the systematic study of quantum capacitance (C$_Q$) in functionalized graphene. The functionlization of graphene has been done by doping with different aliphatic and aromatic molecules and their radicals. Using density functional theory calculations, we first analyze the electronic band structure of the functionalized graphene and subsequently obtained the quantum capacitance in each system. We observed that the quantum capacitance can be enhanced by doping aliphatic and aromatic molecules and their radicals on graphene sheet, especially radical functionalized graphene shows significant enhancement in C$_Q$. Our theoretical investigation reveals that aromatic and aliphatic radicals generates localized density of states near the Fermi level, due to a charge localization. As a result, a very high quantum capacitance (above 200 $\mu F/cm^2$) compared to pristine graphene has been estimated. Effects of atomic dislocation and the vacancy defect on graphene during functionalization has also been incorporated in our investigation. Obtain results predict that the formation of molecular radicals while functionalization of graphene could be an efficient way to synthesize highly efficient graphene based supercapacitor electrode materials which in turn may significantly improve the performance of supercapacitors.