Green synthesis of functionalized graphene-based material with dimethyl but-2-ynedioate for electrochemical energy storage devices

Functionalization of graphene with dimethyl acetylenedicarboxylate is achieved through a microwave-assisted Diels-Alder reaction. The physical, chemical, and electrochemical properties of the modified sheets are thoroughly investigated by complementary characterization techniques. Density Functional Theory calculations are employed to examine the functionalization mechanism and to highlight the role of defects such as epoxide bridges introduced in graphene during exfoliation. Our findings provide valuable insights into the development of efficient and cost-effective methods for large-scale production of high-quality graphene-based materials. Specifically, the electrochemical properties of anode materials containing functionalized graphene are evaluated for Li-ion electrochemical energy storage devices, demonstrating excellent electrochemical reversibility and rate capability. The cyclic voltammetry analysis reveals material stabilization after a few cycles, resulting in a coulombic efficiency of up to 95 % and a discharge capacity of 162.3 mA·h·g−1. The galvanostatic cycling test indicates that the material electrode retains 57 % of its initial capacity at a C-rate of 10C, indicating high-power capability. These promising results position organic modified graphene as a potential material for Li-ion capacitors, with a specific capacity that aligns with the last intercalation stage capacity at a lower potential. Overall, the study's findings offer significant contributions to the advancement of graphene-based materials in energy storage applications.