Theoretical study of the interaction of fullerenes with the emerging contaminant carbamazepine for detection in aqueous environments

Abstract

The global increase in drug consumption exposes the growing need to develop new systems for the detection, capture, and treatment of bioactive molecules. Carbamazepine is one instance of such contaminants at the top of the ranking commonly found in sewage treatment systems. This work, therefore, presents a theoretical study of fullerene C60 and its derivatives with substitutional doping with B, Al, Ga, Si, Ge, N and P, for the detection and capture of carbamazepine is aqueous medium. Solvation effects were included by means of the Polarizable Continuum Solvent method. The results indicate that doped fullerenes are sensitive for the detection of carbamazepine both in gaseous and aquatic environments. Investigation on the intermolecular interactions between the drug and the fullerene molecule were carried out, allowing the characterization of the interactions responsible for stabilizing the adsorption of carbamazepine to the fullerenes. The theoretical survey revealed that fullerenes doped with Al, Ga, Si and Ge chemically adsorb carbamazepine whereas for the case of fullerenes doped with other heteroatoms physisorption is responsible for the molecular recognition. Relying on DFT calculations, the fullerene derivatives C59Al, C59Si and C59Ga are the most suitable to act both as a sensor and to uptake carbamazepine in aquatic environments.

Decoding Chemical Bonds: Assessment of the Basis Set Effect on Overlap Electron Density Descriptors and Topological Properties in Comparison to QTAIM

“…The trends in the chemical bond descriptors reported here are in line with the literature and are chemically meaningful. QTAIM is widely adopted to yield information about features of chemical bonding using a simple post-SCF treatment ,,− with low computational cost. On the other hand, OP descriptors have been utilized ,− mainly for studying different systems (diatomics, solids, and lanthanide-based compounds) and were recently extended to a proper treatment of molecular systems using LMOs. ,, While QTAIM basis set dependency is a recurring subject in the literature, − ,− the dependence of OP chemical bond descriptors on the basis functions has not been reported yet.…”

“…Quantum chemical bonding descriptors provide a valuable tool for understanding the electronic structure and interatomic interactions in different molecular systems. − Chemical bond analysis can support both experimental and computational results, providing insights into the effect of the chemical environment on atomic interactions. Among the various chemical bond models available, the quantum theory of atoms in molecules (QTAIM), energy decomposition analysis (EDA), − electron localized function (ELF), and natural bond orbitals (NBOs) are widely used.…”

“…QTAIM has been the most commonly applied because the topology parameters can be calculated via a simple post-SCF treatment that does not require many computational resources. In addition, this model has been applied with a variety of quantum chemical methodologies, such as density functional theory (DFT) ,,,, and complete active space (CAS) , level of theory. Recently, Long and collaborators studied the nature of the Am–N bonding in (Cp′ 3 Am) 2 (μ-4,4′-bpy) and pointed out that Am–N bonds have an unexpected ionic character that differs from the covalent nature widely observed in Ln–Cp compounds.…”

Carbon-Based Nanoadsorbents for the Removal of Emerging Pollutants

“…Fullerene’s properties have been effectively used to increase its utility in the environmental domain. The detection and capture of carbamazepine in an aqueous media were investigated theoretically using fullerene and its derivatives doped with B, Al, Ga, Si, Ge, N, and P. The fullerene derivatives doped with Al, Si, and Ga are the strongest candidates for serving as sensors and uptaking carbamazepine in aquatic conditions, according to DFT simulations [61]. Mesoporous carbon nanospheres (MCNs) were employed to efficiently remove methyl orange (MO), rhodamine (RhB), and p-hydroxybenzoic acid (p-HBA), with a removal efficacy of more than 95% [62].…”

(Ro)vibrational Spectroscopic Constants, Lifetime and QTAIM Evaluation of Fullerene Dimers Stability

“…The unique physical and chemical properties of fullerenes attracted a lot of attention aimed at their possible applications to organic electronics. For example, as components of photovoltaic cells [ 8 , 9 ], for the development of sensors employed for the capture of pollutants [ 10 , 11 ], or for electron transport through self-assembled monolayers of functionalized fullerenes [ 12 , 13 ]. In this context, information about the intermolecular potential between fullerene molecules, the equilibrium distance, and energy minima of the van der Waals contacts are of great importance to understanding these phenomena [ 14 ].…”