# Photocatalytic Luminous Textiles for the Treatment of Wastewater Issued from Petroleum Activity: Photocatalytic Process Extrapolation

Achraf Amir Assadi, H. Zeghioud, Nacer Belkessa, Amina Rabahi, Atef El Jery, Moutaz Aldrdery, Aymen Amine Assadi

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## To cite this version:

Achraf Amir Assadi, H. Zeghioud, Nacer Belkessa, Amina Rabahi, Atef El Jery, et al., Photocatalytic Luminous Textiles for the Treatment of Wastewater Issued from Petroleum Activity: Photocatalytic Process Extrapolation. Catalysts, 2024, 14 (10), pp.663. 10.3390/catal14100663. hal-04718648

HAL Id: hal-04718648

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Submitted on 2 Oct 2024

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leading to the destruction of harmful organic contaminants present in a test matrix [6,7]. Photocatalysis is one of the popular AOPs for converting organic pollutants into harmless products, like CO₂, H₂O, and mineral acids [8,9]. Furthermore, it is cost-effective, safe, non-selective, and compatible with treating a broad range of organic contaminants. Semiconductor photocatalysis leads to the mineralization of organic pollutants when irradiated with ultraviolet (UV) or visible light [10].

Photocatalytic luminous textiles consist of a core, a guiding light, and a cladding. Both parts have a different refractive index in order to allow for the homogeneous propagation of light on photocatalytic surfaces.

Some previous works showed the possibility of using them to remove pollution by removing optical and mechanical cladding and coating them with TiO₂ [11]. Indeed, this TiO₂ on luminous textiles has several advantages, allowing for the development of a compact reactor with mass transfer enhancement compared to configurations with TiO₂ illuminated with an external UV lamp [12].

Different works have reported the use of TiO₂-coated optical fiber for the photocatalytic degradation of organic pollutants such as 4-chlorophenol [13,14]. Tong et al. report that a fiber honeycomb reactor coupled with a PTC (parabolic trough concentrator) leads to a volume-averaged concentration of production 19.25-times higher than optical fiber monolith reactors (OFMRs) [15]. On the other hand, the coupling of photocatalyst-coated optical fiber with a 318 nm ultraviolet-A light-emitting diode may activate the photocatalysts through interfacial photon-electron excitation, all while minimizing photonic energy losses [16–19].

The originality of the present photocatalytic system is due to the use of more than one luminous textile for simulated oil wastewater using different methods of irradiation to enhance the removal of pollutants. Here, naphthalene and benzene were chosen as target pollutants in wastewater with a high value of turbidity from petroleum activity. Moreover, process extrapolation was investigated to confirm the laboratory performance.

## 2. Materials and Methods

### 2.1. *Photocatalysts*

#### 2.1.1. TiO₂ Deposed on Cellulosic Paper

This photocatalyst is a non-woven porous support based on TiO₂ deposited on cellulosic paper. The catalytic support is prepared by the Ahlstrom Paper Group Research Center. Silica acts as an inorganic binder and protector between textile fibers and titanium dioxide; it also contributes to the adsorption of the pollutant and intermediate products. The mass load is 16 g of TiO₂ PC500 per m² with an equivalent amount of SiO₂. The size of the elemental particles of titanium dioxide is 5 to 10 nm, and that of silica particles is 20 to 30 nm. A dry mixture of 50 wt.% colloidal silica and 50 wt.% titanium dioxide nanoparticles (TiO₂-PC500 Anatase, Purity > 99%, Millennium inorganic chemicals, Chaignes, France) is suspended in pure water. The deposition of 16 g/m² of dry TiO₂-PC500 on cellulosic paper was ensured by preparing a solution with 40% dry powder and 60% pure water. An industrial-sized press was used to impregnate the paper with the suspension. The obtained paper was dried in an oven at 105 °C and then stored in rolls for subsequent use. The surface morphology of TiO₂-PC500-CelulPap was analyzed with a field emission scanning electron microscopy (FE-SEM, Sirion 200, FEI Company, Hillsboro, OR, USA) (Figure 1A).

More information and catalytic characterizations are presented in our previous investigations [11].

Several XRD analysis were performed on the photocatalytic material. The recorded X-ray diffractogram presented in Figure 1B reveals two distinctive peaks of the TiO₂ anatase phase, one around 25° and the other, less intense, at 38°. Additionally, other peaks at 48°, 54°, and 62° show the presence of crystal faces (200), (211), and (204), which are attributed to the structure of TiO₂ anatase. Instead, a large peak at 25 degrees was seen in the XRD pattern, indicating that the silica is amorphous.
<figure><img src="image_3.png" /><figcaption>**Figure 1.** (A) SEM pictures of TiO₂-PC500 on cellulosic paper. (B) XRD spectra of TiO₂-PC500. (C) SEM pictures of the textile: (a) planar view, (b) sliced view and (c) a lighted textile sample.</figcaption></figure>

### 2.1.2. Photocatalytic Luminous Textile

The luminous textile, produced by Brochier Technologies Company, Villeurbanne, France (UVtex®), is obtained by weaving optical fibers with textile fibers in the following manner: warp yarns are composed of textile fibers in the same way as traditional textiles. On the other hand, the weft threads will be a mixture of optical fibers and alternating textile threads. A cold LED lamp is used to radiate the entire surface of the fabric tissue. The optical fiber and textile fiber consisted of polymethyl methacrylate, made by Mitsubishi, Minato City, Tokyo (PMMA CK-20 Eska™ fiber), and polyester, Hattersheim Germany (Trévira CS™ fiber), respectively. Figure 1C illustrates a scanning electron microscopy image characterizing the photocatalyst, showing an example of microscopic modifications on the surface of TiO₂-coated optical fibers.
## 2.2. Batch Reactor

The batch reactor constituted a beaker made of glass, where 750 mL of the naphthalene solution was placed (Figure 2). The inner wall of the beaker pressed the canvas of TiO₂ deposed on cellulosic paper with a surface area of 0.2 m². It was illuminated by an external UV lamp (Philips PL-24W/10/4P, Amsterdam, The Netherlands), and the whole system was covered with aluminum film in order to protect the operator from UV rays and, thus, increase the light intensity within the tank by reflection during experiments.

<figure><img src="image_4.png" /><figcaption>**Figure 2.** Operating diagram of the batch reactor with external UV lamp.</figcaption></figure>

The reactor was used for pollutant treatment with photocatalytic luminous textiles. In fact, the photocatalytic luminous textile is immersed in the bottom of batch reactor containing solution. UV irradiation was supported by an in-situ LED source directly connected to fabric, emitting at 365 nm with an irradiation of 240 mW/cm².

## 2.3. Configurations of Photocatalytic Luminous Textiles in Batch Reactor

To investigate the performance of photocatalytic luminous textiles toward the degradation of organic pollutants, the batch reactors were tested at different configurations using photocatalyst TiO₂ on luminous textiles with cold LED irradiation. Different reactor configurations are presented in Figure 3.

The system setup consists of a pump that is fed by the solution from the tray and sent to the column. A septum is placed just after the pump for sampling. A valve, to fix the flow rate, is located downstream of this pump. Then, there is the possibility of passing the water either in the column or in the tray (bypass) through a three-way valve. More details are provided in our previous investigations [19].

The solution passing through the reactor circulates in the annular space. Indeed, TiO₂ on a sheet of luminous textiles (30 × 80 cm²) coiled like a spiral all along the column (d = 7 cm, L = 100 cm), which should be in contact with the feed solution. The system works in a closed loop for water but, once out of the reactor, is returned to the tray.
<figure><img src="image_5.png" /><figcaption>**Figure 3.** Different tested configurations of photocatalytic luminous textiles (PLTs) in batch reactor, optical fiber irradiated by different levels of radiation (LED UV and/or external lamp UV): (A) PLT irradiated LED UV; (B) PLT irradiated by external UV; (C): PLT double-sided fiber irradiated by 2 UV LEDs (D) PLT irradiated by LED UV and external UV (E): 2 PLT double-sided fiber irradiated by one UV LED; (F) irradiation spectrum of the UV/LED lights.</figcaption></figure>
## 2.4. Analytical Methods and Tools

### 2.4.1. Reverse-Phase Ultra-Performance Liquid Chromatography (RP-UPLC)

The pollutants were analyzed using reverse-phase ultra-performance liquid chromatography (RP-UPLC) (Agilent 1260 Infinity Standard; Santa Clara, CA, USA). After the photocatalytic treatment, the solution was filtered in order to remove any suspended TiO₂ particles. Afterwards, the water sample was analyzed. The mobile phase (eluent A) was ultra-pure water and used as a buffer solution, while eluent B was acetonitrile. Organic solvents used to prepare the mobile phases were UPLC-grade, and the eluent flow rate was maintained at 0.4 mL/min.

The system consisted of a pump (Waters) (Quaternary solvent manager), an apolar column Waters BEH C18 (2.1 × 100 mm), a UV detector diode array (Waters L10UPL 694A) for analysis of 195–400 nm. The volume of injection was 50 µL.

### 2.4.2. Total Organic Carbon Calculation

To determine the extent of mineralization of pollutant treated, and of the by-products formed during photocatalysis treatment, Total Organic Carbon (TOC) samples were measured using a Shimadzu TOC-5000A analyzer—Kyoto; Japan). TOC analysis was carried out at 680 °C using a platinum catalyst. Having this value, the percentage of mineralization can be calculated based on Equation (2).

## 2.5. Chemical Reagents

All the solvents like naphthalene (99% purity) and benzene (98% purity) were purchased from Sigma-Aldrich (St. Louis, MO, USA), and hydrochloric acid (HCl, 37% v/v), sodium hydroxide (NaOH, 98% purity), isopropanol (IPA, C₃H₈O), 1,4-benzoquinone (BQ, C₆H₄O₂) were also acquired from Sigma-Aldrich. The solution was prepared with high-purity water obtained from a Millipore Milli-Q system. Bentonite was used to modify the turbidity of solution. The measurements of turbidity were performed using a turbidimeter (turbidity 1100 NTU).

The scavenging experiments were performed using 100 mM of IPA and BQ each, according to the optimization of IPA, to determine the contributions of •OH and HO₂•/O₂• involved in the photocatalytic elimination of target pollutants.

## 2.6. Experimental Procedure

Photolysis, adsorption, and degradation of naphthalene and benzene solution were investigated under various conditions to highlight the real degradation of pollutants. Indeed, the experiments were carried out in a beaker under magnetic stirring for two types of photocatalysis. The solution was continuously exposed to UV lamp or UV-LED light maintained at ambient temperature for 6 h. At a regular interval of time, samples were collected to monitor their degradation. The pollutant degradation was assessed by HPLC. The photocatalytic removal efficiency (RE) for naphthalene was calculated using the following equation:

$$ RE(\%) = \frac{C^{\text{in}} - C^{\text{fin}}}{C^{\text{in}}} \times 100 \quad (1) $$

where C^in and C^fin are the initial and final concentrations of pollutants (mg/L).

The mineralization of pollutant by photocatalytic treatment was evaluated according to Equation (2):

$$ \text{Mineralization}(\%) = \frac{\text{TOC}^{\text{initial}} - \text{TOC}^{\text{final}}}{\text{TOC}^{\text{initial}}} \times 100 \quad (2) $$

TOC^initial and TOC^final are the initial and final TOC of samples before and after treatment, respectively.
**3. Results and Discussion**

In order to determine the interesting photocatalytic configuration, several experiments based on (i) varying the sheet of photocatalytic luminous textile, (ii) using the bundled multiple fiber optics or individually coupled fiber optics to vary the effective surface area under identical illumination conditions and (iii) using an external UV lamp were tested and analyzed.

**3.1. *Effect of Catalyst***

The effect of the catalyst on the degradation rate of naphthalene was evaluated using two types of configurations: TiO₂ on cellulosic paper under UV irradiation and TiO₂ optical fiber under LED irradiation with a solution at pH 6.1.

As shown in Figure 4, no significative photolysis of naphthalene is noted (less than 9% after 3 h of treatment). The photocatalytic treatment of 16 mg/L of naphthalene during 350 min leads to a degradation efficiency of 51% with the TiO₂ cellulosic paper photocatalyst; however, more than 60% was recorded in the presence of TiO₂ optical fiber. This could be due to the fact that in situ radiation with direct contact between light and the photocatalyst particles will enhance the performance [11].

<figure><img src="image_6.png" /><figcaption>**Figure 4.** (a) Photocatalytic degradation of naphthalene with photolysis, TiO₂ on optical fiber and cellulosic paper (pH 6.1, C₀: 16 mg/L) and (b) mineralization of naphthalene from optical fiber and cellulosic paper.</figcaption></figure>
The pseudo-first-order kinetic model is usually used to fit all datasets. The Langmuir–Hinshelwood (L-H) model, generally used to describe the mechanism of heterogeneous photocatalytic reactions, can be simplified to highlight the apparent first-order reaction for diluted solutions (Equation (3)) [19]:

$$ \ln\left(\frac{C_0}{C}\right) = k_{app} \times t \qquad (3) $$

$C_0$ and $C$ (mg/L) are the concentration of the target compound at time $t = 0$ and $t$, respectively. The apparent reaction rate constant $k_{app}$ (min$^{-1}$) is given by the slope of the graph $\ln(C_0/C) = f(t)$.

The values of the reaction rate constant for naphthalene elimination with $TiO_2$ deposed on optical fiber, $TiO_2$ on cellulosic paper and photolysis (without $TiO_2$) were determined during the first hour of degradation, as shown in Table 1. It was observed that the degradation of pollutants with $TiO_2$ deposed on optical fiber more than with cellulosic paper. The values of reaction rate constants are summarized in Table 1.

<table><caption>**Table 1.** Pseudo-first-order kinetic constant of reaction.</caption><thead><tr><th>Processes</th><th>k<sub>app</sub> × 10<sup>3</sup> (min<sup>-1</sup>)</th></tr></thead><tbody><tr><td>TiO<sub>2</sub> on optical fiber</td><td>1.84</td></tr><tr><td>TiO<sub>2</sub> on cellulosic paper</td><td>1.26</td></tr><tr><td>Photolysis</td><td>0.18</td></tr></tbody></table>

The TOC of naphthalene samples before and after treatment was measured, and then the mineralization was calculated according to Equation (2). The mineralization of the pollutant gives an idea of the transformation of the generated by-products from naphthalene degradation to $CO_2$ and $H_2O$ and other small carboxylic acids during treatment [19]. A high mineralization of pollutants can be explained by the low toxicity of the treated solution. As shown in Figure 4b, the mineralization of naphthalene from the $TiO_2$ optical fiber irradiated by the LED system was evaluated at 59%; however, only 42% was obtained using $TiO_2$ on cellulosic paper. From Figure 4a,b, it seems that the mineralization of naphthalene starts with the degradation steps simultaneously, where a part of the generated reactive oxygen species (ROS) was consumed for destroying and mineralizing intermediate by-products, which explains the gradual decrease in the degradation rate with treatment time [20].

## 3.2. Effect of Initial Concentration with Photocatalytic Luminous Textile

In order to study the effect of naphthalene's initial concentration ($C_0$) on the degradation efficiency, the initial concentration was varied from 8 to 32 mg/L.

Figure 5a,b display the results of naphthalene degradation and mineralization, respectively. It was observed that the photocatalytic degradation of naphthalene decreases when increasing the initial concentration. In fact, at an initial concentration of 16 mg/L, there was about a 69% naphthalene photodegradation efficiency, while the photodegradation was reduced to about 51% at an initial concentration of 32 mg/L. This may be due to the high availability of the photogenerated reactive oxygen species (ROS: $O_2^{\ominus}$, $HO^{\bullet}$, $h^{+}$, etc.) at a low pollutant concentration [21]. In addition, when the concentration of naphthalene increases, the rate of photodecomposition decreases. This can be explained by the following: (i) the unavailability of a sufficient quantity of active sites and (ii) the competitive effect between naphthalene molecules and an intermediate by-product toward the active sites of the photocatalyst [22].
<figure><img src="image_7.png" /></figure>

<figure><img src="image_8.png" /><figcaption>**Figure 5.** (a) Photocatalytic degradation of naphthalene with optical fiber and (b) photocatalytic mineralization of naphthalene with optical fiber (pH = 6).</figcaption></figure>
In other words, for high concentrations, naphthalene molecules and their intermediates occupy the active sites, which causes a reduction in the number of electron holes, which consequently reduces the photocatalytic efficiency. The results indicate that the degradation efficiency and reaction rate become slower at a high initial concentration of naphthalene. At low concentrations, the degradation is observed as quickly. As the concentration increases, degradation is reduced due to the blocked active sites of the photocatalyst, decreasing the surface area. Similar results were reported by Eskandarian et al. [23].

From Figure 5b, it seems that the mineralization of naphthalene is significantly affected by an increasing initial concentration. Indeed, the mineralization decreases from 79% to 59% with increasing the naphthalene concentration from 8 to 32 mg/L. This can be explained by the fact that the increase in the initial concentration leads to a lower availability of the active sites for adsorbing pollutant molecules and the generated intermediate by-products [24]. Assuming that the photocatalytic process is a series of successive reactions, the competition toward the active sites of the catalyst becomes more important. Therefore, the by-products formed cannot be degraded [25].

### 3.3. *Effect of Fiber Distribution*

In order to intensify the efficiency of TiO₂ on the optical fiber-based system, the photocatalytic degradation of naphthalene under different distributions/configurations of optical fiber was investigated, and the results are shown in Figure 6. Five configurations, as presented and named in Figure 3, were tested during 360 min of irradiation.

<figure><img src="image_9.png" /><figcaption>**Figure 6.** Photocatalytic degradation of naphthalene using TiO₂ optical fibers under different configurations (initial concentration 16 mg/L, pH = 6).</figcaption></figure>
It seems that configuration C with double-sided independent fiber irradiated by two UV-LEDs is the most efficient, where complete degradation was achieved after 330 min of treatment. This can be explained by the high number of active sites available on two luminous textiles and irradiated by sufficient light intensity from two UV-LED systems. In the second position, configuration D with photocatalytic luminous textiles (PLTs) irradiated by both UV-LEDs and an external UV lamp exhibited around an 82% naphthalene degradation efficiency. This may be due to the lighter intensity irradiating the photocatalyst surface, which leads to the generation of more reactive oxygen species, avoiding the light penetration problem throughout the naphthalene solution [25–27]. Configurations A and E present similar results during the 360 min of treatment, where around a 75% degradation efficiency is recorded after 360 min of treatment. Configuration B (luminous textile without LED UV irradiated by external UV lamp) presented the lowest photocatalytic degradation efficiency with 59% naphthalene elimination after the same duration.

### 3.4. *Effect of Turbidity*

In order to examine the effect of turbidity on the photocatalytic degradation process of naphthalene, photocatalytic tests in the presence of bentonite at a 5.8 mg/L concentration and without bentonite (pure water) were carried out using TiO₂ optical fiber as a photocatalyst, with the cellulosic paper photocatalyst irradiated by UV-LED (Figure 7). The photodegradation of naphthalene was assessed by evaluating the effect of bentonite in a batch reactor.

<figure><img src="image_10.png" /><figcaption>**Figure 7.** Effect on turbidity on photocatalytic degradation of naphthalene using TiO₂ optical fibers and cellulosic papers after 180 min (initial concentration 16 mg/L, pH = 6).</figcaption></figure>
Test results revealed that the photocatalytic degradation of naphthalene with bentonite present as an additive presents a negative effect on the photocatalytic process translated by a decrease in the degradation efficiency over time. The results show that the inhibition of bentonite was enhanced with TiO₂ deposed on cellulosic paper compared to that with optical fibers. In fact, we note an inhibition of more than 30% in terms of removal efficiency. This is due to the fact that bentonite inhibits the absorption of UV light emitted by a lamp in the case of the configuration with TiO₂ deposed on cellulosic paper. Similar behavior was reported by Khaksar et al. for phenol removal from petrochemical wastewater [28].

### 3.5. Effect of Scavenger

IPA is used to efficiently quench the generated •OH groups, and the reaction considered as second order and the rate constant are kIPA, •OH = 1.9 × 10⁹ M⁻¹s⁻¹. Moreover, it is well known that 1,4-benzoquinone (BQ, C₆H₄O₂) (kBQ, HO₂•/O₂• = 9.6 × 10⁸ M⁻¹s⁻¹) is an electron acceptor, which is able to interrupt the dissolved oxygen-accepting electrons and so acts as a very effective trap to avoid the formation of radicals (hydroperoxyl radical/superoxide radical anion, HO₂•/O₂•⁻) [29–31]. It is then possible that O₂•⁻ can be formed in our experimental conditions (pH = 6.5 > pKa (HO₂•/O₂•⁻)).

The presence of reactive oxygen species is observed during photocatalysis, as hydroxyl radicals (•OH) and superoxide radical anions (O₂•⁻) are involved in initiating the degradation mechanism. The main by-products of degradation are hydroxylated species due to the opening of the aromatic cycle [29]. Thus, to have a better understanding of the reaction mechanisms responsible for the photocatalytic degradation process, naphthalene degradation experiments were conducted under optimal conditions with the addition of chemicals that are known for their electron/hole scavenging properties [6,30]. To gain further insights into the reaction mechanism, quenching studies using scavengers were performed to identify the main radical species involved in naphthalene removal. Firstly, the degradation of naphthalene in water was performed via photocatalysis in UV-irradiated TiO₂ cellulosic paper. Parameters such as the concentration pH and mass of the catalyst were investigated.

As shown in Figure 8, the addition of isopropanol significantly decreased naphthalene degradation. Interestingly, the removal rate decreased as low as 70% when IPA was added to the solution, as compared to naphthalene alone. Therefore, it can be suggested that naphthalene degradation is essentially due to •OH [10]. On one hand, it can be concluded that free radical •OH played an important role in the hydroxylation of aromatic compounds such as naphthalene [32]. On the other hand, the addition of benzoquinone showed no significant effect on the naphthalene degradation rate. This can be explained by the limited role of these radicals in the photocatalytic process [27].

<figure><img src="image_11.png" /><figcaption>**Figure 8.** Effect of scavengers on photocatalytic degradation of naphthalene as a function of irradiation time.</figcaption></figure>
### 3.6. Effect of Extrapolation on the Mineralization

To examine the effects of increasing the concentration and reactor capacity on the mineralization of naphthalene, three different tests were carried out with TiO₂ optical fibers as follows: (i) increasing naphthalene's initial concentration at 2.5 L of solution volume, with two different inlet concentrations; (ii) increasing the solution volume from 2.5 to 5 L.

As shown in Figure 9, increasing the reactor capacity by two-times for the same concentration of 16 mg/L leads to a decrease in the mineralization yield with a factor of 1.37. This can be explained by the fact that at high solution volumes, there are two-times more molecules of the pollutant needed to be adsorbed on the insufficient quantity of active sites available on the photocatalyst surface at the first steps. In the second steps, and as degradation advances, many by-products are generated that need to be mineralized while competing with naphthalene molecules to be adsorbed onto the active sites and reacting with reactive oxygen species [22].

<figure><img src="image_12.png" /><figcaption>**Figure 9.** Extrapolation of photocatalytic degradation of naphthalene using TiO₂ optical fibers with different reactor capacity and initial concentration (pH = 6).</figcaption></figure>

It appears that increasing the initial concentration of naphthalene by two-times with the same solution volume of 2.5 L inhibits the percentage of mineralization. This may be due to the increasing quantity of naphthalene molecules and the generated intermediate by-products with the same number of active sites available on the photocatalyst.

## 4. Conclusions

In this work, the performance of two types of TiO₂ cellulosic paper and TiO₂ optical fiber catalysts under LED was evaluated toward the degradation of naphthalene in aqueous solution. The TiO₂ optical fiber showed a high degradation efficiency and percentage of mineralization compared to the other photocatalysts. The increase in naphthalene's initial concentration with the TiO₂ optical fiber system has a negative effect on both photocatalytic degradation efficiency and mineralization. Different photocatalytic luminous fibers coated with the TiO₂ system were successfully prepared and tested for the investigation of the optical
fiber distribution effect on naphthalene degradation. The configuration with luminous textile double-sided fiber irradiated by two UV-LEDs presented the highest performance; however, the configuration of luminous textile irradiated by an external UV lamp (configuration B) exhibited the poorest photocatalytic performance. An inversely proportional relationship between photodegradation and turbidity was observed. We also noticed that increasing the pollutant molecules by doubling the solution volume or doubling the initial pollutant concentration has the same negative effect on the mineralization percentage of naphthalene.

**Author Contributions:** Conceptualization A.A.A. (Aymen Amine Assadi) and A.E.J.; methodology, A.A.A. (Aymen Amine Assadi); analysis, N.B., H.Z. and M.A.; investigation, A.A.A. (Achraf Amir Assadi); resources, A.A.A. (Aymen Amine Assadi) and A.E.J.; writing—original draft preparation, A.A.A. (Achraf Amir Assadi) and A.R.; writing—review and editing, H.Z. and A.A.A. (Aymen Amine Assadi); supervision, A.A.A. (Aymen Amine Assadi). All authors have read and agreed to the published version of the manuscript.

**Funding:** This research received no external funding.

**Data Availability Statement:** No new data were created or analyzed in this study. Data sharing is not applicable to this article.

**Acknowledgments:** The authors extend their appreciation to the Deanship of Research and Graduate Studies at King Khalid University for funding this work through the Large Research Project under grant number RGP2/248/45. The authors are also grateful to the IMAM University and National School of Chemistry of Rennes (ENSCR) for scientific collaboration.

**Conflicts of Interest:** Hicham Zeghioud was employed by the company Sonatrach. The remaining authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest.

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