Modeling graphene oxide decorated with FeO, SO and NO

Area of Science:

• Computational materials science
• Quantum chemistry
• Surface science

Background:

• Graphene oxide (GrO) is a promising material for various applications.
• Modulating GrO's electronic structure is key to enhancing its performance.
• Decoration with specific species offers a pathway to tune GrO properties.

Purpose of the Study:

• To computationally investigate the effect of FeO, SO, and NO decoration on graphene oxide's electronic structure and reactivity.
• To assess the potential of decorated GrO for electrode and sensing applications.
• To understand how different decorating species influence GrO's properties.

Main Methods:

• Density Functional Theory (DFT) calculations using the B3LYP/LANL2MB level of theory.
• Optimization of pristine graphene, GrO, and decorated GrO structures (GrO/FeO, GrO/SO, GrO/NO).
• Analysis of electronic properties (dipole moment, HOMO/LUMO gap), reactivity descriptors, DOS/PDOS, MESP, QTAIM, and NCI.

Main Results:

• Decoration significantly altered total dipole moments and HOMO/LUMO energy gaps.
• GrO/SO exhibited the largest dipole moment and smallest energy gap, indicating high reactivity.
• GrO/FeO and GrO/SO displayed strong electrophilic character and high softness, while GrO/NO showed moderate reactivity.
• DOS/PDOS analysis revealed new states near the Fermi level, facilitating charge transfer.
• QTAIM and NCI analyses elucidated bonding and interaction types.

Conclusions:

• The choice of decorating species precisely tunes the electronic and reactive properties of GrO.
• GrO/FeO and particularly GrO/SO are identified as promising candidates for advanced electrode and gas sensing technologies.
• Computational insights provide a foundation for experimental development of functionalized GrO materials.