Si 2 BN QuantumDots as Efficient Detectors of Carbamazepine in Aqueous Environment: First principles study

doi:10.21203/rs.3.rs-3454168/v1

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Si 2 BN QuantumDots as Efficient Detectors of Carbamazepine in Aqueous Environment: First principles study

https://doi.org/10.21203/rs.3.rs-3454168/v1

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Pharmaceuticals and personal care products (PPCPs) excreted into the environment have dangerous consequences on environmental impacts and public health. Therefore, it is crucial to find efficient methods for the treatment of these pollutants. Currently, a wide range of physical, biological, and chemical processes are being explored for the removal of such contaminants. Here we consider the capability of the ultrathin Si2BN quantum dots to adsorb and eliminate Carbamazepine. Based on first-principles calculations, we studied the electronic structure and the adsorption energy of Carbamazepine (CBZ) by a stable Si2BN nanoflakes. We estimated the adsorption energies on two different sites of Si2BN monolayer. The calculated positive values (~0.83eV) of adsorption energy implies that the considered Si2BN nanoflakes are able to adsorb Carbamazepine through all the proposed adsorption sites.

Two-dimensional Si2BN

Carbamazepine CBZ

DFT

pharmaceuticals

Pharmaceutical wastes in effluents are quickly becoming a global concern [1]. Due to the wide spread use and disposal of these items, they have accumulated quickly in nearby aquatic habitats [2, 3]. Carbamazepine represents one of these wastes which has medical applications to treat seizures(5H-dibenzo[b,f]azepine-5-carboxamide(CBZ; C₁₅H₁₂N₂O) (proprietary name Tegretol ) is an important drug for the treatment of epilepsy which is the second most common central neuron system disease after stroke[4]. The drug has replaced both phenytoin and phenobarbitone as the first line anticonvulsant for a number of paediatric seizure disorders[5]. According to previous studies, global CBZ usage is around 1.01 kt per year. CBZ has been found in a variety of water sources, including surface water, ground water, wastewater treatment plants, and even drinking water, as a result of its widespread use. As a result, the occurrence of CBZ in various water resources is being regarded a global problem [6–13]. CBZ is said to be hazardous to aquatic organisms such as bacteria, algae, invertebrates, and fish [14]. The standard concentration of CBZ in wastewater-irrigated soils has been determined to be 0.02–15 g kg^-1[15]. When the concentration of the active ingredient in CBZ is equivalent to or found to exceed 1.0 g L^-1in an aquatic environment, an environment assessment should be done, according to the US Food and Drug Administration [16]. As a result, effective treatment solutions for removing this pollutant from the aquatic environment are necessary. Traditional treatment techniques used in wastewater treatment plants (WWTPs) can only remove 32–35 percent of trace contaminants such as CBZ from wastewaters [7, 17]. CBZ's high persistence may have led to its discharge from WWTPs without biodegradation or transformation [17].

Removal of this important carbamazepine drug as a waste has been performed using different traditional techniques such as oxidation, ozonation, photocatalysis of UV radiation, and others have reportedly been used to remediate effluents including pharmaceutical wastes [18]. However, these procedures have only resulted in partial drug degradation or the generation of carcinogenic or hazardous end products such as dioxins, chlorinated phenols,trihalomethanes,chlorinated phenoxyphenols, and others [18].Recent research has identified adsorption as an efficient and cost-effective method for treating persistent contaminants [19–21]. A wide range of materials, including clays, polymers, and many carbon-based compounds have been studied for adsorption of various types of aqueous contaminants [21]. Silicon boron nitride (Si₂BN mono layer) has attracted substantial attention among all other forms of adsorbents reported in recent studies due to its mechanical and chemical stabilities, as well as its high specific surface area. Si₂BN monolayer, have been widely researched as adsorbents due to their simple synthesis, excellent pollutant removal at a low dosage, and cost effectiveness. Analogous to graphene, Andriotis et al.18 designed Si₂BN two dimensional sheets based on extensive ab initio density functional theory (DFT) simulations. A monolayer Si₂BN sheet has a hexagonal lattice with sp² hybridization and consists of Si, B, and N atoms in plane buckling. The authors have reported that the Si2BN sheet has high flexibility, high electron mobility, tunable band structure, and high thermal conductivity. Further, the stability of the structure is examined by molecular dynamics simulation, and the results confirmed the structural stability up to 1000 K [22]. In this study molecular modeling analysis has been carried out to investigate the stability of CBZ compound with the aim of providing a better understanding on the relative toxicity due to CBZ

Two-dimensional (2D) materials are atomically thin structures with high carrier mobility [23, 24], an adjustable band gap [25, 26], strong light-mater interactions [27–29], and a large specific surface area [30]. Because of their outstanding features, they are suitable candidates for a variety of applications such as nanoelectronics [31, 32], optoelectronics [24, 33], highcapacity battery electrodes [34, 35], sensors [36–39], and water treatment [40–43]. The 2D material family encompasses a large range of materials with a wide range of physical properties.silicene[44, 45],phosphorene [46, 47],antimonene [48, 49], hexagonal boron nitride/phosphide [50, 51] are examples of novel 2D materials. The use of 2D materials can considerably improve water treatment. it is therefore considered in this study. For a wide spectrum of oils, organic solvents, and dyes, porous boron nitride nanosheets demonstrate remarkable sorption [52]. Si₂BN monolayers with reactive surface Si atoms and ultra-high carrier mobility [53, 54] are another intriguing 2D material. Si₂BN was proposed as a possible candidate for high-capacity anode material [55] and hydrogen storage [56] because of these features. We anticipate that the reactive surface gives Si₂BN a high capacity to absorb various contaminants, resulting in effective water treatment.

Therefore, the ability of Si₂BN to adsorb Carbamazepine (CBZ) by calculating the adsorption strength and charge transfer is investigated here.

UV-Vis spectra before and after the adsorption are investigated because it can be used as a characteristic tool to confirm the adsorption of Carbamazepine.

In this work, Molecular modeling analyses have been carried out using Gaussian 16 program to investigate the adsorption behavior of Carbamazepine over the Si₂BN nanoflake on two different adsorption sites (edge and surface). To this aim DFT calculations are performed to analyze the geometry, the adsorption energy and the electronic structure of the resulting complexes to provide a better understanding of the adsorption process and stability of the formed complexes

DFT simulations [57, 58] are used to study the optimal structures of Carbamazepine and the physical properties of Si2BN flakes using Gaussian 09. The hybrid functional Becke-three Parameters-Lee-Yang-Parr(B3LYP) is employed in our calculations of the electronic properties [59, 60] and the 6–31 g basis set are used in the calculations. This level of theory has been tested and shown to accurately explain the structural and electrical properties of Si- and C-based 2D materials [61–64].

The interactions between the Si₂BN monolayer and Carbamazepine are approximately computed such that the resultant adsorption energy gives an estimation of the adsorption between Si₂BN and Carbamazepine. The optical properties are calculated using time dependent-DFT (TD-DFT) calculations and mapping of the MESP at the same level based on the optimized structures from DFT results.

3.1. Structural properties of Si2BN and Carbamazepine Model Molecules

The fully optimized structure of 2D Si2BN and Carbamazepine are shown in Fig. 1. The structural parameters, such as bond lengths (Si–Si − 2.24 Å, Si–B − 1.95 Å, Si–N − 1.75 Å and B–N − 1.46 Å) were found to be in good agreement with previously reported results. [65, 66, 67] Also for Carbamazepine (N-C -1.43 Å, N-H – 1.01 Å, C = O -1.24 Å, C-C − 1.4 Å, C-H -1.08 Å ).

The Si2BN planar structure exhibits so-called planar sp²hybridization and two different bonding types. One s-orbital, two p-orbitals, and three chemical species (Si, B, and N atoms) with various valence electrons in the final orbitals make up the majority of the sp² hybridization. The s, p_x, and p_y orbitals combine to generate s bonding (in-plane) in the valence band (occupied states) in these orbitals, while the s* orbitals stand in for anti bonding in the conduction band (unoccupied states). The strongest covalent bonds, or s bonds, are what give the Si₂BN structure its high formation energy and elastic characteristics, as seen in Fig. 1, The Si atom has Si, B, and N as nearest neighbors, while each B (N) has two Si atoms and one N (B) atom as nearest neighbors. The Si atoms find themselves in electron-deficient position and the variation in bonds works as an electron reservoir for an ad-atom or a molecule on the sheet (or NT) surface. The p_z orbitals pointing out of plane of the Si₂BN monolayer are odd with respect to the planar symmetry, which is not coupled with s bonding states. The side interactions with neighboring p_z orbitals form delocalized π bonding and π* anti-bonding orbitals.

The lattice consists of different layers, each layer having hexagonal arrangements of silicon, boron and nitrogen atoms different layers are arranged in such a manner that boron in one layer is immediately above or below nitrogen and vice versa it implies that there is continous migration of dative bond across layers which provide stability of the molecule. In particular layer boron-nitrogen bond is formed by overlap sp² hybride orbital also silicon atom changed its hybridization from SP³ to SP² to maintain planer structure as shown in Fig. 1.

3.2. Si2BN-Carbamazepine physiochemical properties calculation

The capability of Si₂BN nanoflake to adsorb pharmaceutical compounds, such Carbamazepine, is investigated. We start by considering different adsorption positions as shown in Fig. 2

Figure 2 shows that the adsorption process is mainly by the Si atoms in the flakes due to their interactive π-bond electrons. The adsorption energy (Ea) is calculated to insure the stability of the adsorption and to compare the adsorption strength among different adsorption sites using the equation: Ea = (E_Si2BN + E_carb − E_c). Where E_Si2BN, E_carb, and E_c is the ground state energies of the flake before adsorption, Carbamazepine and the flake after adsorption, respectively. The calculated positive values of the adsorption energy in Table 1 insure a successful adsorption process. The adsorption strength is comparable in the two adsorption sites, however, adsorption energy in case of edge adsorption is slightly higher. Atoms on edge sites could be more active than atoms on the surface. There are a variety of causes for this, including differing chemical environments compared to atoms on inner surfaces, which may also cause charge redistribution at the interface, and low CN (coordination number),since the exposed atoms at the edge of Si₂BN may have unsaturated bonds, such as dangling bonds, that can act as active sites for adsorption. These unsaturated bonds are highly reactive and can form strong interactions with Carbamazepine's functional groups. As shown in Fig. 3 also The Si₂BN edge might offer more freedom for Carbamazepine to adsorb in favorable positions due to reduced steric hindrance. This increased freedom can result in better alignment of bonding groups, leading to stronger adsorption on the edge. according to research on Si₂BN and its functionalized ones, the edges can also promote the hydrogen evolution reaction (HER), [68].

The stronger adsorption at the edge might involve less charge transfer between Carbamazepine and Si₂BN compared to surface adsorption. The edge sites could interact through weaker vander Waals forces or other non-covalent interactions, allowing Carbamazepine to retain more of its original charge and result in a lower positive charge on the adsorbed molecule. The adsorption of Carbamazepine on the surface may induce charge redistribution within the Si2BN material as previously mentioned. The presence of the adsorbed molecule could lead to changes in the local electronic structure, resulting in a higher positive charge. The charge transfer (ΔQ = Q_f − Q_i, with Q_f and Q_i are the initial and final charge on Si₂BN and Carbamazepine is calculated using Mullikan charge analysis [69] to provide additional information on the adsorption process and it provides a clear picture of donation and back donation between the two structures [70]. The values of ΔQ in Table 1, as shown Carbamazepine has positive charge while Si₂BN has negative charge. This means that when Carbamazepine approaches and interacts with the Si₂BN surface, there is a possibility of charge transfer between the molecule and the surface. The Si₂BN material may have a different electron affinity or electronegativity compared to Carbamazepine. As a result, electrons from the adsorbate (carbamazepine) can be transferred to the Si₂BN surface, making it relatively more negatively charged. And also the Electron Redistribution which previously mentioned, CBZ may experience charge redistribution. The electric field generated by the charged or polarized surface affects the distribution of electrons within the molecule. This redistribution leads to a separation of charge within the Carbamazepine, resulting in a partial positive charge on certain regions of the molecule.

Also the obtained dipole moment results of the formed complexes (3.96, 3.66 Debye) showed an increase in the reactivity of these complexes towards the surrounded environment as shown in Table 1.

Table 1

The adsorption energy (E_a), charge transfer (ΔQ), and energy gap (E_g) of Si₂BN nanoflake before and after adsorption.
Structure	E_a (eV)	ΔQ(e)	E_g (eV)	Dipole moment Debye
Si₂BN	-	-	0.5083	0.000141
Carbamazepine	-	-	4.4392	4.105898
Si₂BN edge	0.832750474	0.041501	0.7347	3.958081
Si₂BN surface	0.82450542	0.060142	0.71702	3.661987

The increased dipole moment is due to Surface Induced Dipole Moment in which The interaction with the Si₂BN surface can induce a dipole moment in Carbamazepine. The negatively charged surface can attract the positively charged regions of the molecule and repel the negatively charged regions, further enhancing the positive charge separation. As also noticed that the dipole moment of the Edge adsorbed molecules is little higher this can be attributed to stronger interactions, the presence of unsaturated bonds or defects, higher surface reactivity, and a preferred adsorption orientation at the edge of Si₂BN.

3.3. Electronic properties

The effect of adsorption on electronic characteristics is explored by computing the energy gaps shown in Table 1 and displaying them. The highest occupied molecular orbital (HOMO) and lowest unoccupied molecular orbital (LUMO) are also proven to present the origin of the lowest energy molecular states. HOMO/LUMO of Si2BN nanoflakes are shown in Fig. 4. The interactive π-electrons from Si-atoms interact to produce moderate π-bonds with lower energies than the B-N sigma bonds, which subsequently appear as the HOMO and LUMO that distribute on Si atoms Fig. 4 (a) and (b). The development of strong interactions between Carbamazepine and the nanoflake Si atoms (Fig. 4 (c-d)) indicates that the interacting π -electrons of the low energy states are the key reason for boosting the adsorption of the Si2BN nanoflake. As observed in the HOMO and LUMO distributions in Fig. 4 (c-d), the distribution of HOMO and LUMO cubes on flake atoms rather than the adsorbed Carbamazepine incase of adsorption on both positions implies that Carbamazepine forms stronger bonds with the flake than Si–Si bonds.

As seen in figure (4), the energy gap in case of edge adsorption location (0.7347 eV) is greater than that in case of surface position (0.71702 eV). This is due to the Electronic Interaction Strength since The interaction strength between Carbamazepine and Si₂BN can vary between the edge and surface. The stronger interaction at the edge might result in more significant charge redistribution, leading to alterations in the energy levels and the energy gap and also due to Quantum confinement effects may be more pronounced at the edge of Si₂BN compared to the surface. These effects can lead to changes in the energy levels of Carbamazepine adsorbed at the edge.

3.4.Molecular Electrostatic Potential (MESP):

Based on the electronic density, the molecular electrostatic potential (MEP) is a highly useful descriptor for identifying areas of electrophilic attack, nucleophilic reactions, and hydrogen-bonding interactions [70, 71]. Since it is related to the electronegativity and the partial charge changes on the different atoms of Si₂BN and Carbamazepine. Molecular electrostatic potential (MESP) maps are created for the studied chemical structures at DFT level of theory using B3LYP/6- 31G. The maps show negative and positive potentials using colors from red to dark blue. Red represents severe negative potentials, while dark blue represents positive potentials. Yellow zones have less negative potentials than red, and green regions are neutral. The electronegativity of connected atoms affects both potential distribution and color. Coupling strong electronegative atoms with less electronegative atoms shows red colors since The presence of atoms with approximately identical electronegativity narrows the color spectrum significantly. As a result, we may rely on the MESP maps as a physical characteristic to determine if the active locations of interest can conduct nucleophilic or electrophilic chemical interactions. In Fig. 5,The MESP map of pure Si₂BN sheet consists of light and dark blue, green, and light yellow colors. The light and dark green and yellow colors are observed mainly at boron atoms and in the centers of Si₂BN sheet, indicating slightly negative to neutral potentials at the core of the sheet. This may be due to some delocalized electrons from silicon atoms. The terminals have light and dark blue colors, likely due to the presence of less electronegative H atoms attached to nitrogen atoms, resulting in electrophilic reactions. therefore, it is the acidic hydrogen atom. Green color confirms the neutral part and zero potential of Si₂BN. the positive (blue) regions of MEP demonstrated nucleophilic reactivity, while the negative (red) areas represented electrophilic reactivity. While in case of Carbamazepine the The red area in the diagram was centered around the oxygen and neighboring atoms. The nucleophilic reactivity of the molecule, however, was focused on the hydrogen atoms at the edges, even though the blue area was not clearly visible. This molecule can be useful for intermolecular interactions and metallic bonds. The findings from the charge analysis phase also support this conclusion.

The interaction between Si₂BN nanoflake and Carbamazepine redistributes electric charge due to their different electronegativity. This results in localized increases in electrostatic potentials where they interact, as observed by potential value changes for edge and surface adsorption (-7.33 to 7.33 a.u and − 7.611 to 7.611 a.u, respectively). The differences in electrostatic potentials depend on the atom configurations and charge distributions within nanoflake and Carbamazepine.

3.5 The UV-visible absorption spectrum of Si2BN and Formed Complexes

In addition to how adsorption affects electrical characteristics, its impact on optical properties has also been studied and is depicted in Fig. 5. The optical absorption spectra of Si₂BN before and after Carbamazepine adsorption are examined using time-dependent DFT simulations. The first 8 excited states are taken into account for the optical transitions. As depicted in Fig. 3 (e, f), the conspicuous absorption peak of pristine Si₂BN, which initially resided around ~ 1889 nm, underwent a notable blue shift to approximately ~ 1725 nm and ~ 1747 nm upon edge and surface adsorption of Carbamazepine, respectively.

primary absorption peaks arise due to excitations that are relatively distant from the highest occupied molecular orbital to lowest unoccupied molecular orbital (HOMO → LUMO or H → L) transitions, a phenomenon elucidated in Table 2. Among the excited states, the eighth one (S8) in Si₂BN emerges with the highest oscillator strength. This state exhibits diverse transitions, with the most substantial contributions originating from H → L + 2 (29.6%) and H-2 → L (25.28%). Post adsorption, the principal excitations deviate from H-L transitions. In line with the UV–Vis spectra, Table 2 demonstrates a shift towards higher energies in the dominant excitation subsequent to adsorption. For instance, the S8 transition, which was at 0.6563 eV in Si₂BN, shifted, to 0.7184 eV and 0.7096 eV to in Si₂BN-Carbamazepine for edge and surface adsorption, respectively.

The H → L transition, prominent in the lower excited states, offers a means to determine the optical gap and juxtapose it with the electronic counterpart. The data in Table 2 reveals that the lowest excited state in Si₂BN is S2, where S1 displays zero oscillator strength, indicating forbidden transitions. In contrast, for S2, the H → L transition dominates (96.5%), signifying an optical band gap of 0.2834 eV, nearly half the magnitude of the electronic gap. The reduced optical band gap points to a pronounced interaction between electrons and holes, leading to the formation of excitonic states within the electronic energy gap.Analogous to the prevalent excitation, the lowest excitation also encounters a blue shift towards higher energies after adsorption, as outlined in Table 2. Consequently, the UV–Vis spectra, both before and after adsorption, can serve as a distinctive tool to authenticate the adsorption of distinct pollutants.

The observed blue shift subsequent to carbamazepine adsorption on Si₂BN originates from alterations within the electronic structure and energy levels due to the interaction with the nanoflake. This shift can be elucidated by the rise in energy level of the highest occupied molecular orbital (HOMO) from 352 in the Si₂BN substrate to 414 in the complex formed with carbamazepine. This increase provides a plausible explanation for the observed blue shift in the UV absorption spectrum.

The change in HOMO energy level indicates a significant influence of the interaction between carbamazepine and the Si₂BN substrate on the electronic structure of the system. Notably, distinct edge states, intensified interaction, and pronounced quantum confinement effects—resulting from the unique characteristics of nanoscale dimensions and adsorption—contribute to discrete energy levels, modifications in the band gap, and shifts in optical behaviors. These factors are primarily responsible for the more pronounced blue shift observed in edge adsorption, where these effects amplify alterations in electronic transitions compared to surface adsorption.

The distinctive attributes of nanomaterials and the accompanying shifts in electronic transitions, as exemplified by the blue shift resulting from Carbamazepine adsorption on Si2BN nanoflakes, are most effectively interpreted within the framework of this phenomenon. Post-carbamazepine adsorption at the edge position, as depicted in Fig. 2, the Si2BN structure experiences more pronounced deformation (buckling). These structural changes encompass bond stretching and bending, culminating in a more substantial blue shift, as visually depicted in Fig. 6.

In summary, our comprehensive study utilized Density Functional Theory (DFT) calculations to investigate the adsorption and detection of carbamazepine onpristine Si₂BN monolayer. The geometry optimization was carried out by using the DFT:B3LYP/6–31G which shows that Carbamazepine interact physically with Si2BN and provided important new understandings of their electrical structure. The favorable nature of the adsorption process is shown by the predicted adsorption energies of 0.833 eV for one configuration and 0.825 eV for another configuration. These results support the potential applicability of this composite system in applications involving selective chemical sensing and show that carbamazepine adsorption on Si₂BN surfaces is stable and practicable. Our research has also shown important alterations in the adsorbed system's electronic band gap. We detect a clear broadening of the band gap, with computed values of 0.735eV and 0.717 eV before and after adsorption, respectively. The significant influence of carbamazepine adsorption on the optical and electronic characteristics of Si2BN nanoflakes is indicated by this change in the electronic structure. These modifications not only confirm the viability of sensitive carbamazepine detection but also provide opportunities for fine-tuning the material's electrical properties for specialized applications. Finally, our DFT simulations offered a thorough knowledge of the adsorption mechanism, which was supported by both electronic and spectroscopic data. This research lays the groundwork for utilizing the unique features of Si₂BN nanoflakes for effective Carbamazepine detection, as well as demonstrating the potential of computational techniques in developing molecular sensing technologies.

Ethical Approval

This work is not applicablefor both human and/or animal studies.

Competing interests

I declare that the authors have no competing interests as defined by Springer, or other interests that might be perceived to influence the results and/or discussion reported in this paper.

Conflicts of Interest

The authors declare no conflict of interest.

Authors' contributions

Not right!!

M. S.;Build up the model molecules, conduct the calculations, write the manuscript and analyse the data.R. M. K., contribute in writing and analyzing data and supervise the work.A.A. S.; Contribute to the problem assignment, revise the manuscript and supervise the work.M. A. I.; Assign the problem, supervise the conducted work, contribute to analyzing data; receive the fund and supervise the work. All authors have read and agreed to the published version of the manuscript.

Funding

This research received no external funding.

Acknowledgments

The authors would like to express their gratitude to the Molecular Spectroscopy and Modeling Unit at Spectroscopy Department, National Research Centre, Egypt, for the computational facilities provided in this work.

Availability of data and materials

The data will be available upon request, contact Medhat A. Ibrahim [email protected]

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Table 2 is available in the Supplementary Files section.

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Si 2 BN QuantumDots as Efficient Detectors of Carbamazepine in Aqueous Environment: First principles study

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Abstract

Figures

1. Introduction

2. Calculation Details

3. Results and Discussion

3.1. Structural properties of Si2BN and Carbamazepine Model Molecules

3.2. Si2BN-Carbamazepine physiochemical properties calculation

3.3. Electronic properties

3.4.Molecular Electrostatic Potential (MESP):

3.5 The UV-visible absorption spectrum of Si2BN and Formed Complexes

4. Conclusions

Declarations

References

Table

Additional Declarations

Supplementary Files

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