Electro-Fenton process at semi-pilot scale. A study to scale up the reactor for industrial applications.

doi:10.21203/rs.3.rs-2504059/v1

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Electro-Fenton process at semi-pilot scale. A study to scale up the reactor for industrial applications.

https://doi.org/10.21203/rs.3.rs-2504059/v1

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In this study, we report the development of the electro-Fenton (EF) process at a semi-pilot scale plant using an open undivided electrochemical reactor design. To do so, a series of three-dimensional (3D) cathodes constituted of packed and fixed bed of glassy carbon pellets and dimensionally stable anodes (DSA) are employed. To highlight the treatment efficiency of the EF process, bisphenol A (BPA), that is known to be a persistent molecule, is used as model molecule. First, the applied current intensity was studied and optimized in order to determine the limiting current of O₂reduction under hydrodynamics conditions of 0.6 m³.h^-1. Then, the effect of cathode’s number on the removal efficiency of BPA versus time of electro-Fenton treatment was investigated. Many parameters were carried out using the EF reactor i.e., the effect of the initial pollutant concentration as well as the effect of the treatment flow rate. The obtained results demonstrate that the degradation efficiency of BPA increases with the cathode’s number increases and the pollution charge the decreases. Only few seconds of treatment by EF process were needed to eliminate BPA for the dilute solutions (≤ 10 mg.L^-1). The biodegradability of the treated solution and its mineralization were also investigated by refereeing to the measurements of COD, TOC and BOD₅. Finally, the scale-up strategy of the reactor design to an industrial pilot plant is discussed.

Electro-Fenton process

Scaled-up reactor

Semi-pilot plant

Three-dimensional cathode

Water treatment

Bisphenol A.

The industrialization in developed countries has led to the emergence of persistent pollutants in the environment (Chmayssem and Hauchard 2015, 2017). These pollutants, known as emerging pollutants, are continuously released into aquatic environments, causing harm to both aquatic and terrestrial organisms, as well as to human health (Jiang et al. 2013; Rivera-Utrilla et al. 2013). To avoid the entrance of this pollution in the environmental cycle and limit its negative impacts, it is crucially important to develop new technologies for water remediation.

So far, the biological treatment is certainly a process of choice for the remediation of waters, however, the presence of toxic and persistent molecules may limit its application. For this reason, advanced oxidation processes (AOPs) have received great interest in the recent years (Bouafia and Alloune 2007; Oller et al. 2011; Qutob et al. 2022). These processes consist of producing highly reactive derivatives for the destruction of the target pollutants, mainly hydroxyl radicals (^•OH). The latter are nonselective oxidant species that typically leads to the degradation of organic matter and enhances the effluents biodegradability (Zaviska et al. 2009a; Brillas et al. 2009; Panizza and Cerisola 2009).

Indeed, electro-Fenton (EF) process is a powerful advanced oxidation process that has been shown to effectively degrade organic matter at laboratory scale (Poza-Nogueiras et al. 2018). The process involves reducing dissolved oxygen (O₂) at the cathode, which generates hydrogen peroxide (H₂O₂) also known as Fenton's reagent (Jiang and Zhang 2007; Brillas et al. 2009; Nidheesh and Gandhimathi 2012). This electrochemical reaction occurs in an acidic medium (pH ~ 3) and requires the addition of iron (Fe²⁺) in low quantities. The electro-generated H₂O₂species react with the Fe²⁺ions to produce ^•OH in homogeneous medium (Fig. 1).

Of course, many studies have reported the effectiveness of the electro-Fenton process in degrading various chemical pollutants, including dyes (Zhou et al. 2007; Rosales et al. 2009; Zahedi et al. 2022), pesticides (Ozcan et al. 2013), pharmaceutical residues (Mansour et al. 2015; Long et al. 2019), and other industrial pollutants such as phenols and phenolic compounds, anilines, cresols, and so on (Yuan et al. 2013; Asghar et al. 2015; Malinović et al. 2022). This highlights the versatility and potential of the electro-Fenton process as a powerful tool for the remediation of contaminated water, however, these studies have been conducted using various types of electrochemical reactors, which vary in design and the material of the cathode which must reduce oxygen in a two-electron process and the material of the anode (BDD, PbO₂, Pt…) (Yang et al. 2022; Feng et al. 2023). These variations in design and materials used can have an impact on the efficiency and effectiveness of the electro-Fenton process. Therefore, choosing an appropriate electrochemical reactor design and materials is crucial for achieving optimal results in pollutant degradation. Despite the high efficiency of electrochemical reactors at the laboratory scale, it is important to design an appropriate reactor that allows for easy scaling-up of the EF process. This should take into consideration factors such as high electrode surface areas, low-cost electrode materials, and a design that supports high flow rates. Furthermore, it is important to consider the energy consumption of the EF process, as it can have an impact on the final treatment cost. To that end, more energy-efficient processes should be prioritized in order to keep costs low (Wang et al. 2022).

In our previous works (Chmayssem et al. 2017; Bakhti et al. 2020), a new design of electrochemical reactor for the application of electro-Fenton process at the laboratory scale was reported (Fig. S1). This reactor (PRIAM’s series) is an open undivided electrochemical reactor with a three-dimensional cathode of a fixed bed of glassy carbon pellets. The approach used in the reactor design provides high geometric surface area, which is beneficial for the electro-Fenton process. Additionally, the porous structure of the cathode may also increase the real contact between the solution and the electrode, which can enhance the efficiency of the process (Rodrigo Quejigo et al. 2018).

One such pollutant is bisphenol A (BPA), which is known to not be effectively degraded by biological treatment and ultimately ends up polluting the environment, including surface water (Gözmen et al. 2003; Liu et al. 2021; Niu et al. 2022; Okon et al. 2022). Different processes have been examined to remove BPA from natural water or wastewater as already reported elsewhere (Bouafia and Alloune 2007; Zaviska et al. 2009b; Serpone et al. 2010; Chen et al. 2007; Katsumata et al. 2004; Seibert et al. 2019; Tay et al. 2012; Qiang et al. 2013; Kuramitz et al. 2004; Cui et al. 2009; Brugnera et al. 2010; Lin et al. 2013; Zhao et al. 2014; Dolatabadi et al. 2021; Sajiki and Yonekubo 2004; Yuan et al. 2013; Rivero et al. 2014). While these processes have demonstrated high efficiency in treating BPA in small volumes, none of them have been scaled up. Therefore, it is of great importance to test the electro-Fenton process on a semi-pilot scale to treat BPA.

In this study, we report the design of a new electrochemical reactor at a semi-pilot scale with a fixed bed of packed cathodes made of glassy carbon pellets. This electrochemical reactor is optimized for the application of electro-Fenton process to treat persistent pollutants. Herein, bisphenol A was served as model molecule for our investigation. We carried out various parameters to scale-up the developed process to an industrial treatment plant. Additionally, we investigated the mineralization of BPA during treatment and the biodegradability of the treated solutions at different treatment times and for different initial concentrations of the pollutant.

2.1 Chemicals and materials

Glassy carbon pellet material (SIGRADUR^®K, high purity) was obtained from HTW (Germany) and has an appropriate average diameter of 3 mm. Bisphenol A used to the preparation of polluted water (C₁₅H₁₆O₂, 2.2-Bis(4-hydroxyphenyl)propane – purity > 99%) and sodium sulfate used as supporting electrolyte (Na₂SO₄ – purity > 99%) were purchased from Sigma-Aldrich. Iron (II) sulfate heptahydrate (Fe₂SO₄.7H₂O – purity 98%) was obtained from Scharlau chemicals. For mobile phase preparation, acetonitrile (HPLC grade) was also purchased from Sigma-Aldrich for mobile phase preparation. Demineralized water was obtained in our laboratory by an appropriate production system (Millipore). Other chemicals used were of analytical grade reagents. All the measurements and experiments were carried out at laboratory temperature.

2.2 Solution preparation

Synthetic solutions of bisphenol A were prepared in demineralized water without any organic solvents addition in order to limit the introduction of organic matter only to BPA. The pH of the solution was adjusted to 2.9 ± 0.1 using H₂SO_4.The Na₂SO₄was added as supporting electrolyte at the concentration of 0.05 M. The Fe (II) was added to the solution at the concentration of 0.5 mM.

2.3 Design of electro-Fenton process

The electrochemical reactor at semi-pilot scale is designed as an open reactor (one-compartment) made of polyvinyl chloride (PVC) and has a rectangular geometric dimensions of 41.5 cm (L) x 19 cm (l) x 32 cm (H). The volumic capacity of the reactor is of 15 L. The electrochemical reactor at semi-pilot scale contains up to five three-dimensional (3D) cathodes made up of a compact and fixed bed of glassy carbon pellets. These later were surrounded by 6 dimensionally stable anodes (DSA) made up of titanium mesh and covered by a thin layer of ruthenium oxide (Ti/RuO₂). However, the electrodes are removable so the reactor could contain more or less electrodes (Fig. 2 & 3).

The three-dimensional cathodes have an internal geometric dimension of 24 cm × 12 cm × 2.8 ± 0.2 cm (L, W, and H) and were filled with glassy carbon pellets (» 680 g per cathode) (Fig. 2). A metal mesh is placed at the vicinity of the fixed bed (in the center) as a current collector by the high side. The electrodes are geometrically set in continuous but electrically were connected in parallel. The reactor was designed to treat the contaminated solution in batch mode. A centrifugal pump is used for the experimental setup to feed the electrochemical reactor with a constant flow rate that was fixed using a flow meter (typically 10 L.min^-1(0.6 m³.h^-1) at semi-pilot scale reactor).

Concerning the flow direction, the solution goes through the width of the fixed bed of the electrodes (perpendicularly to the electrodes section) during the treatment. Also, assuming a plug flow at the level of the cathode, the liquid flow velocity through the fixed bed is estimated at 0.0058 m.s^-1. So far, air pumps and air diffusers were used in the experimental setup to continually supply the solution by air (oxygen) (Fig. 3). The sampling at different times was carried out at the outlet side of the cathode. The main physicochemical proprieties of the glassy carbon pellets used for packing the fixed bed three-dimensional cathodes are presented in the supplementary information (Table 1).

2.4 Analytical procedures and equipment

2.4.1 High Performance Liquid Chromatography

High performance liquid chromatography (HPLC, Waters^TM 600 MILLIPORE system, Waters^TM 600 Pump, Waters^TM 717 plus autosampler, Photodiode Array DetectionWaters^TM 996) were used. HPLC analyzes were performed on reversed-phase column Waters C₁₈(Symmetry 4.6 mm × 25 cm, 5µm). The composition of the mobile phase was 40/60 (V/v) Acetonitrile / Ultra-Pure Water. The PAD detector was set at 278 nm and the flow rate of the mobile phase was fixed at 1 mL/min. The injection volume in the HPLC system was 50 µL. Empower 2 Software was used respectively for HPLC control and results processing. The retention time of bisphenol A was 4.6 minutes under the above-cited conditions.

2.4.2 Total Organic Carbon

Total organic carbon (TOC) measurements were carried out using Shimadzu Total Organic carbon analyzer (TOC-V_CPH). Organic carbon compounds were mineralized and converted into CO₂, which was detected and measured by a non-dispersive infrared detector (NDIR). Reproducible TOC values were always obtained using the standard non-purgeable organic carbon (NPOC) method. TOC-CONTROL V software (Version 2.10) was used for TOC analyzer control and results processing.

2.4.3 Chemical Oxygen Demand

Chemical oxygen demand (COD) measurements were carried out using HACH^® DR/2500 method (8000). COD vials were obtained from Hach Lange (Ref. HI93754B-25). Only 2mL of the solution were added into the COD via land oxidized for 2 hours at 150°C with dichromate (K₂Cr₂O₇) at acidic pH using Hach DRB 200 oven. After COD values were measured using a spectrophotometer (DR/2500) at 620 nm after calibration.

2.4.4 Biochemical Oxygen Demand

Biochemical oxygen demand (BOD) measurements were carried out using OxiTop system (from WTW) for 5 days (BOD₅) in order to check the biodegradability of BPA and its by-products after treatment by electro-Fenton process. Activated sludge taken from wastewater treatment of the municipality of Rennes was used as source of micro-organisms. The method was described in details in previous works (Mansour et al. 2011).

2.5 Performance determination

The removal efficiency of BPA is defined as following: [(C₀– C_t) ×100] / C_t, where C_tis the concentration of bisphenol A after time of treatment (t) and C₀is the initial concentration of bisphenol A before treatment.

In our previous work, we studied and optimized an electrochemical reactor for the treatment of bisphenol A (BPA) using the electro-Fenton process at a laboratory scale (Chmayssem et al. 2017). We investigated the effect of the applied current intensity on the removal efficiency of BPA during the treatment process. Our findings revealed that the limiting current intensity under the hydrodynamic conditions of 6 L.min^-1 was found to be approximately 0.8 A (0.51 A / 100 g of glassy carbon pellets). Furthermore, the limiting current density was determined to be 0.012 A/cm², taking into account the section of the fixed bed that is exposed to the flow.

In this work, the focus was on optimizing the current intensity for the treatment of bisphenol A (BPA) using the electro-Fenton process at a semi-pilot scale. To achieve this, the variation of the removal efficiency according to time for different applied current intensities ranging from 10 A to 30 A was studied. The results, illustrated in Figure 4, show that the removal efficiency improves with an increase in the applied current intensity, until the range of 15 to 17.5 A is reached. However, for higher intensities, the treatment appears to be less efficient. This suggests that the applied current intensity is higher than the limiting current for the O₂ reduction and that a portion of the produced H₂O₂ is being reduced to H₂O (Babić et al. 1993; Noe et al. 2012). Therefore, the limiting current intensity under the hydrodynamic conditions corresponding to 10 L.min^-1 (600 L/h) was determined to be near 17.5 A (0.51 A / 100 g of glassy carbon pellets). Theoretically, this current should be divided equally among 5 cathodes and therefore, each cathode should be supplied by 3.5 A as the cathodes were connected electrically in parallel.

To verify the hypothesis that the number of electrodes affects the removal efficiency of BPA during the treatment by electro-Fenton process, we investigated the effect of the electrodes number using the semi-pilot scale reactor. To do this, two experiments were carried out using an initial concentration of 10 mg/L of BPA. The first experiment used the typical reactor configuration of 5 cathodes and 6 anodes, and the second experiment used a configuration of only one 3D-cathode and 2 DSA-anodes (configuration 2). Figure 5 shows the variation of the removal efficiency of BPA over time for both cases. As expected, the typical reactor configuration (5 cathodes and 6 anodes) was found to be more efficient in degrading BPA compared to the configuration of only one cathode (configuration 2). This is likely due to the increased efficiency of reducing oxygen into H₂O₂ and producing ^•OH as the number of cathodes in the electrochemical reactor increases.

Furthermore, it is widely accepted that the reaction of ^•OH with phenolic compounds is primarily considered as a pseudo-first-order reaction, suggesting a direct attack of hydroxyl radicals on BPA (Brillas et al. 2009). In light of this hypothesis, the apparent constant rate (K_app) of BPA could be calculated using the theoretical equation of a pseudo-first-order reaction. Figure 5 (inset) shows the variation of Ln (C₀/C_t) over time during the first 10 minutes of treatment of BPA (10 mg/L) by electro-Fenton process at the semi-pilot scale reactor. As expected, a linear relation is observed with a slope of 0.076 min^-1 corresponding to the value of K_app in the typical reactor configuration (5 cathodes) and 0.376 min^-1 corresponding to the value of K_app in the configuration containing only one cathode. These results indicate that the typical reactor configuration (5 cathodes) is more efficient in degrading BPA compared to the configuration of only one cathode.

The ratio of the obtained slope values is approximately 5, which confirms that the configuration of the EF reactor with 5 cathodes is 5 times more efficient than the reactor configuration that contains only one cathode. As expected, this confirms that the applied current intensity in the electrochemical reactor was equally distributed among the 5 cathodes, as the cathodes were electrically connected in parallel, resulting in a current density of 0.012 A/cm² (Fig. S2). This value is comparable to the current density found in the laboratory scale reactor of the electro-Fenton process (Chmayssem et al. 2017). In summary, these results confirm that our reactor design could be a good candidate for the scale-up of the electro-Fenton process for industrial treatment applications.

On the other hand, the electro-Fenton experiments at the semi-pilot scale reactor were initially conducted using high concentrations of BPA solutions in order to monitor the concentration of BPA during treatment and study the degradation kinetics as a function of treatment time. Herein, we investigated the impact of initial BPA concentration on the removal efficiency of BPA during treatment using the electro-Fenton process (from 10 to 150 mg.L^-1). We carried out experiments for 90 minutes at 15 A and found that as the initial concentration of BPA increased, the time required to achieve a certain level of removal efficiency also increased (Fig. 6). For instance, at a BPA concentration of 150 mg.L^-1, it took 50 minutes to achieve 90 % removal efficiency. However, as the initial concentration decreased (i.e. for 10 mg.L^-1), the time required to achieve the same removal efficiency decreased as well (less than 5 min). This suggest that this semi-pilot reactor configuration is more efficient in treating low concentration of persistent pollutant by a single pass of the solution through the fixed bed cathode.

The effect of flow rate on the removal efficiency of BPA by the EF process at semi-pilot scale was also investigated. Figure 7 illustrates the variation of the removal efficiency over time at 15 A for three different flow rates: 200 L/h, 600 L/h and 1000 L/h (the maximum flow rate at semi-pilot scale reactor). As shown, an improvement in removal efficiency was observed as the flow rate increases. For example, after 15 minutes of treatment, a removal efficiency of 45% was observed at 200 L/h, while the removal efficiency increased to 65% at a flow rate of 1000 L/h. This observation can be attributed to the increase in liquid flow velocity (v) through the fixed bed, which can be calculated as 0.0019 m.s^-1at 200 L/h and as 0.0097 m.s^-1 at 1000 L/h, ensuring more favorable hydrodynamic conditions. This results in an increase in the Reynolds number (Re= v*dp/n) and subsequently the mass transfer coefficient (km= A*v^b), which leads to an improvement in the degradation efficiency of BPA, where: dp is the particle diameter, n the kinematic viscosity, A and b constants (M. Benzina. S. Gabsi 1991; Sedahmed 1996). For this reason, it is of high importance to provide a reactor design that support high liquid flow rates that allows to apply high current intensities in optimized mode and as a result to reach high removal efficiency of BPA in short treatment time (a few m³.h^-1).

Moreover, electro-Fenton process typically involves biodegradability change (Hou et al. 2015). Today, many studies shows that combining EF process prior to the biological treatment could be a particularly interesting solution for water remediation (Mansour et al. 2014; Olvera-Vargas et al. 2016; Aboudalle et al. 2018; Baiju et al. 2018; Arellano et al. 2020). For this reason, we evaluated the biodegradability change during treatment of BPA by EF process at semi-pilot scale reactor. To proceed, we used the BOD₅ (Biochemical Oxygen Demand) to COD (Chemical Oxygen Demand) ratio, which is a standardized measure of the biodegradability of a solution, and considered a ratio higher than 0.4 to indicate that the solution is biodegradable (Oller et al. 2011; Rivero et al. 2014). We investigated the biodegradability of BPA for different treatment times (30, 60, and 90 minutes) and for two initial BPA concentrations of 10 and 50 mg.L^-1. Additionally, we studied the mineralization of BPA by monitoring the TOC (Total Organic Carbon) versus the time of EF treatment (30, 60, and 90 minutes).

As seen in Figure 8, a significant improvement in biodegradability (BOD₅/COD > 0.6) is observed after 90 minutes of treatment, with a 33% reduction in TOC at an initial BPA concentration of 50 mg.L^-1. Additionally, good results were obtained for low concentrations of BPA (≤ 10 mg.L^-1), where only a few minutes of treatment were needed to improve biodegradability. This enhancement is also reflected in a high TOC abatement (> 70 %) at the end of the treatment (90 min). It can be observed that COD and TOC abatement increases with treatment time and as the initial BPA concentration decreases. Here, the residual TOC is mainly composed of small organic acids which are difficult to oxidize as reported elsewhere (Chmayssem et al. 2017) and typically require many hours of treatment to achieve total mineralization (Ayoub et al. 2011; Ozcan et al. 2013; Mansour et al. 2015).

For the scale-up of EF reactor to an industrial pilot plant, two cases should be considered based on the source and the concentration level of the effluent (Fig. 9). For the treatment of an industrial discharge with high contamination levels (> mg.L^-1), a batch reactor should be designed with multiple fixed bed cathodes in series as a pre-treatment process. The treatment duration will depend on the pollution charge and biodegradability level. For low concentration levels of contamination (< mg.L^-1), treatment can be directly applied through a single pass of the solution in the electrochemical reactor. Few seconds of treatment should be sufficient and biodegradability can be achieved through the electro-Fenton reactor. The current intensity should be set at 0.51 A per 100 g of glassy carbon pellets (0.012 A.cm^-2 for the section of the fixed bed exposed to the flow). Scale-up is limited by the flow rate of the solution, which should be kept within acceptable values (a few m³.h^-1). To make scaling up easier, it is recommended to keep the thickness of the 3D cathode bed constant as used in the laboratory and semi-pilot scale reactor (2 cm).

In conclusion, the design of an open undivided electrochemical reactor with the three-dimensional cathodes made up of a fixed bed of glassy carbon pellets is as an ideal configuration for the scaling-up the EF process. The semi-pilot scale plant study demonstrated high removal efficiency during the treatment of micropollutions. The short treatment time needed by the electro-Fenton process makes this design of reactor an appropriate option for enhancing the biodegradability of effluents and reducing the pollution charge as a pre-treatment process before biological treatment.

Authors Declaration

This work is original and has not been published elsewhere, nor is it currently under consideration for publication elsewhere. Also, the manuscript has not been submitted to a preprint server prior to submission on Environmental Science and Pollution Research.

Funding

The authors declare that no funds, grants, or other support were received during the preparation of this manuscript.

Availability of data and materials

The data and materials that support the findings of this study are available from the corresponding author upon reasonable request.

Competing Interests

The authors have no relevant financial or non-financial interests to disclose.

Author Contributions

All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by Ghaya AlChoubassi and Ayman Chmayssem. The work presented in the herein study was supervised by Didier Hauchard. The first draft of the manuscript was written by Ayman Chmayssem. Writing - review and editing of the manuscript was done by Samir Taha and Didier Hauchard. All authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.

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Electro-Fenton process at semi-pilot scale. A study to scale up the reactor for industrial applications.

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