A study on ZIF-67 augmented Electrocoagulation process for Wastewater Treatment

A study on ZIF-67 augmented Electrocoagulation process for Wastewater Treatment | Research Square window.SnipcartSettings = { analytics: { enabled: false } }; (function() { var accessVector = localStorage.getItem('access_vector') || ''; window.dataLayer = window.dataLayer || []; if (accessVector) { window.dataLayer.push({ user: { profile: { profileInfo: { snid: accessVector } } } }); } })(); (function(w,d,s,l,i){w[l]=w[l]||[];w[l].push({'gtm.start':new Date().getTime(),event:'gtm.js'});var f=d.getElementsByTagName(s)[0],j=d.createElement(s),dl=l!='dataLayer'?'&l='+l:'';j.async=true;j.src='https://www.googletagmanager.com/gtm.js?id='+i+dl;f.parentNode.insertBefore(j,f);})(window,document,'script','dataLayer','GTM-K279D39R'); Browse Preprints In Review Journals COVID-19 Preprints AJE Video Bytes Research Tools Research Promotion AJE Professional Editing AJE Rubriq About Preprint Platform In Review Editorial Policies Our Team Advisory Board Help Center Sign In Submit a Preprint Cite Share Download PDF Research Article A study on ZIF-67 augmented Electrocoagulation process for Wastewater Treatment Muhammad Uzair, Muhammad Fahad Tariq, Farhan Javed, Mohammed Kadhom, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-7376258/v1 This work is licensed under a CC BY 4.0 License Status: Posted Version 1 posted You are reading this latest preprint version Abstract The persistent contamination of water bodies with toxic pollutants represents a significant challenge that requires appropriate treatment. This research investigated the potential of ZIF-67 augmented electrocoagulation l treatment for wastewater treatment. The investigation focused on key variables, including pH (5-9), current density (9.26-23.15 mA/cm 2 ), ZIF-67 dose (30-50 mg/L), dye concentration (50-100 mg/L), and reusability. The results demonstrated a notable enhancement in the elimination of textile dye, with a significant increase from 82.32% to 95.40% observed in the electrocoagulation process when 50 mg/L of ZIF-67 was introduced. The maximum dye removal (up to 99 %) was achieved at the optimum parameters of pH 7, current density 18.52 mA/cm 2 , 50 mg/L ZIF-67, and 50 mg/L dye concentration, respectively, demonstrating efficient reusability. For real wastewater treatment, at optimal conditions, the chemical oxygen demand (COD), biological oxygen demand (BOD) and colour removals achieved were 42.21%, 39.10% and 59.11%, respectively. The research suggested that an electrocoagulation combined MOF process has the potential to be an effective method for the wastewater remediation. advanced oxidation process electrocoagulation metal organic framework wastewater treatment ZIF-67 Figures Figure 1 Figure 2 Figure 3 Figure 4 Figure 5 Figure 6 Figure 7 Figure 8 Figure 9 Figure 10 Figure 11 1. Introduction The natural resources of water, air, and land are under great threat because of rapid urbanization and industrialization. Freshwater is a scarce resource, and it is of great concern to prevent environmental pollution that results in a deterioration of water quality. Furthermore, the direct realize of industrial wastewater into the water bodies has resulted in significant adverse effects on the ecosystem. This is due to toxicity of the wastewater, which has led to the contamination of freshwater channels and rivers with a range of pollutants, including industrial waste, synthetic dyes, and pharmaceuticals. A number of industries, including pharmaceutical, textiles, paper, cosmetics, leather, food, and paint are responsible for the discharge of harmful and carcinogenic compounds into the environment through wastewater [ 1 , 2 ]. The introduction of such pollutants is accountable for adverse effects on the biodiversity of the ecosystem. Textile industries represent a significant source of water pollution on a global scale. Over 700,000 dyes are produced annually for the textile industry. It is estimated that approximately 80% of all industrial wastewater discharged originates from the textile sector. This wastewater contains elevated pollutant concentrations, primarily in the form of dyes [ 3 – 6 ]. A variety of hazardous dyes, heavy metals (such as mercury, chromium, cadmium, lead, and arsenic), and aromatic compounds have been identified in textile wastewater [ 7 ]. Dyes are highly stable, carcinogenic, and recalcitrant pollutants in wastewater that have been shown to have adverse effects on humans and plants. The elimination of these hazardous dyes from wastewater is a crucial step for ensuring environmental safety [ 8 – 12 ]. A number of techniques for wastewater treatment have been the subject of resent research including chemical, physical, and biological methods. These methods include biodegradation, adsorption [ 13 ], membrane filtration, ion exchange, sedimentation, electrocoagulation treatment, ozonation [ 14 ], Fenton oxidation [ 15 ], photo catalysis [ 16 ] and electrocoagulation [ 17 ]. These techniques, when applied in standalone technology, may not be sufficient to treat textile effluent. For instance, the biological approach is unsuitable for the removal of colour from dyes, due to the fact that the majority of dyes are harmful to the microorganisms used in the procedure. Physical methods such as membrane filtration and ion exchange have notable constraints, namely that they are most effective when dealing with tiny volumes of wastewater. However, the combination of some approaches has been effectively used in the treatment of different dyes. electrocoagulation processes, such as electrocoagulation (EC) have attracted considerable attention for their many benefits. Traditional chemical coagulation is highly affected by variations in the organic load of textile wastewater. Variations in the amount of coagulant used can affect this method results in process inefficiencies. Coagulants can also contribute to the presence of additional pollutants. To address these issues, researchers have turned to the electrocoagulation process, which eliminates the need for any additional chemicals. Electrocoagulation achieves rapid decolourisation, resulting in a reduced amount of sludge. Electrocoagulation has several advantages over traditional technologies. It requires smaller units, is not-specific in nature, can be easily automated, and is associated with reduced operating costs [ 18 , 19 ]. In EC, the metal cations are produced by anodic oxidation, while the hydroxyl ions are produced by electrolysis at the cathode. The hydroxyl ions and metal cations undergo a chemical reaction to form metal hydroxide complexes, which have a high adsorption capacity and are able to bind contaminants. Several coagulant species with pH-dependent properties are formed in the solution. The coagulants formed disrupt and counteract the charge of the pollutant dye molecules, causing them to aggregate and form flocs. These flocs are then separated by sedimentation or flotation. The impurities are propelled upwards on the liquid's surface in the EC cell by tiny hydrogen gas bubbles generated at the cathode [ 20 , 21 ]. Khoram et al. [ 22 ] have investigated the Electrocoagulation method for the remidation of textile dye wastewater under the optimal conditions pH 5.5 and current density 15 mA/cm 2 the decolorization, and COD removal was obtained 98 and 40% respectively. Bener et al. [ 23 ] studied how various levels of current density from 12.5 to 100 mA/cm 2 affected the effectiveness of TOC removal (10–22.5%) from actual textile wastewater. Mousazadeh et al. [ 24 ] was reported the high removal of COD 96% by using electrocoagulation method at Current density 25 Am for 50 min of treatment time. In another research work, Bayramoglu et al. [ 25 ] has studied the maximum COD removal 98% obtained at maximum current density 150 mA/cm 2 after 25 min of treatment time. Efficient adsorbents with high porosity and large surface area can improve the economic and energy efficient treatment of dyes by adsorption. In this regard, metal-organic frameworks (MOFs) have favourable adsorption properties due to their unique properties. The MOF structure consists of porous crystalline frameworks formed by bonding metal complexes to organic linkers [ 26 , 27 ]. MOFs have superior performance in wastewater treatment compared to other porous materials such as activated carbon, zeolites, and polymers. The pore size and form of MOF materials can be easily adjusted from the microporous to the mesoporous scale by changing the connectivity of the inorganic component and the type of the organic linker. Recently, MOF materials have found applications in various fields, including drug delivery, adsorption of organic molecules, gas adsorption, separation, catalysis, electrode materials, nanomaterial carriers, magnetism, polymerisation, and membranes [ 28 ]. Zeolitic imidazolate frameworks 67 (ZIF-67) are highly favoured among metal-organic frameworks due to their exceptional capabilities, they are having some advantages over other MOFs such as good adsorption capability, Larger Surface area and good thermal property, and as well as their affordability, facile synthesis, and structural robustness. Within this particular class, the ZIF-67 has shown remarkable efficacy in removing dyes during the process of wastewater treatment process [ 18 , 29 , 30 ]. However, the limitation of stand-alone technologies has prompted research into sophisticated integrated methods that offer benefits such as accelerated treatment and cost efficiency. The present research elucidates the parametric effects of the ZIF 67 augmented electrocoagulation process for the pollutants reduction in wastewater. The effects of parameters such as pH, MOF dose, current density, and dye concentration were investigated to study the removal of color, BOD and COD. The catalyst was characterised using techniques such as the Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopic (SEM), Energy Dispersive X-ray Spectroscopy (EDX), and Bruner– Emmet–Teller (BET). The real wastewater was characterized for the BOD 5 , COD, Turbidity and pH values. 2. Materials and methods 2.1. Materials and Reagents The Reactive Black 5 (RB-5) dye of analytical grade was obtained from Sigma-Aldrich (USA). The following chemicals were utilized in this study: sodium hydroxide (NaOH) with a purity of 99%, hydrochloric acid (HCl) of 37% concentration cobalt (II) nitrate hexahydrate Co(NO 3 ) 2 ⋅6H 2 O with a purity of 98%, 2-methylimidazole, deionized water (DI), sodium chloride (NaCl), and ethyl alcohol which were delivered by Merck, Germany. All compounds were of analytical grade and were employed without additional purification. The standard solutions were prepared through standard methods. The actual textile effluent was obtained from a nearby textile manufacturing facility (combined fabrics Lahore Pk). The synthetic textile effluent was prepared in the laboratory by dissolving the RB-5 and electrolyte in distilled water. 2.2. Synthesis of ZIF-67 ZIF-67 was synthesized using the procedure outlined in a previous publication [ 31 ], as illustrated in Fig. 1 . Two solutions were each made by dissolving 0.717 g of (Co(NO 3 ) 2 ⋅6H 2 O) in 50 ml of deionized water. Furthermore, 1.622 grams of 2-methylimidazole was added to the second solution along with 50 millilitres of deionized water. Subsequently, the mixture was then agitated until a transparent solution was obtained. Next, the solution of Co (NO 3 ) 2 ⋅6H 2 O was introduced into the 2-methylimidazole solution and agitated for 30 minutes at ambient temperature. The ZIF-67 purple precipitates were obtained by centrifuging using a centrifuge (Model 800D, Canfort, China) the mixture for 20 minutes at a speed of 3000 rpm. The precipitates were then washed three times with ethanol and water and then dried under a vacuum at a temperature of 80 ○ C for 24 hours. 2.3. Experimental Figure 2 depicts the experimental configuration employed in the investigation. The experimental arrangement comprises a glass reactor housing aluminium electrodes with dimensions of 15 cm in length, 5 cm in width, and 0.2 cm in thickness The electrodes are connected to a direct current (DC) power source, specifically a Dazheng PS-605D model form China). The electrodes were meticulously abraded with sandpaper and then immersed in a diluted HCl solution for a duration of 10 minutes. Additionally, they were rinsed with distilled water to eliminate any surface contaminants and prevent electrode passivation before to each experimental trial. The distance between the vertical electrodes was maintained at a constant value of 1 cm. In each trial, the reactor was filled with one litre of dye solution. An electrolyte, sodium chloride (NaCl), was supplied in the quantity of 1.0 gram. The pH level was then adjusted by the addition of the require quantities of 1 M NaOH and 1 M HCl solution. The prescribed amount of ZIF-67 was loaded, and continuous stirring was conducted using a magnetic stirrer (Model 79-1A, Canfort, China) [ 32 – 34 ]. Samples were obtained at specific intervals, subjected to filtration, and examined with the UV-visible spectrophotometer (PerkinElmer Lambda 35 double beam) to determine the concentration of the dye. The absorbance of all samples was analysed at the wavelength of maximum absorption, which was measured to be 596 nm [ 35 ]. 2.4. Characterization techniques The Bruker Alpha-E FTIR spectrometer was employed to determination of the functional groups present on the surface of ZIF-67. This analysis was conducted using an Attenuated Total Reflectance-Fourier-Transform Infrared Spectroscopy (ATR-FTIR) and spectrum with a covering the wavelength range of 400 to 4000 cm − 1 at a resolution of 2 cm − 1 using diamond single-reflection attenuated total reflectance. The Nova Nano SEM 450 analyser was used to assess the elemental composition of the catalyst and examine its surface structure through Energy-Dispersive X-ray spectroscopy (EDX). Images were captured using an electron beam with an acceleration voltage of 10 kV. The Micrometrics-ASAP-2020 detector was used to analyse the surface area and pore size via usage of the Brunauer–Emmett–Teller (BET) technique. The samples were subjected to a vacuum degassing process for eight hours at a temperature of 150°C. The nitrogen adsorption-desorption isotherms, with a purity level of 99.99%, were tested at a temperature of 77 Kelvin. 3. Results and discussion 3.1. Catalyst characterization The functional groups present on the surface of ZIF-67 were identified through the utilization of the Attenuated Total Reflectance-Fourier-Transform Infrared (ATR-FTIR) spectrometer, with measurements obtained within the spectral range of 500–4,000 cm⁻¹. The primary bands were identified in the 600-1500 cm -1 wavenumber range (Figure 3), indicating the stretching and bending properties of the imidazole ring. The band observed at 1418.41 cm −1 is attributed to the C-N stretching in the imidazole, while the range of 1000-1350 cm -1 is associated with the in-plane bending vibration of the imidazole ring. It is also noteworthy to mention the band at 991.10 cm −1 refers to C-N [36].The bands at 2919.62 cm −1 indicate C-H in the imidazole ring, whereas the distinctive peak in ZIF-67 occurred at 1560.66 cm -1 , which correlates to C=N. The peak at 3220.86 cm −1 corresponds to the O-H stretching vibration [36, 37]. After treatment the peaks drift from 1418.41 cm -1 to 1418.28 cm -1 for C-N group, for C=N stretching peaks changes from 1560.66 cm -1 to 1568.98 cm -1 . This drift due to the adsorption of RB 5 dye on the surface of the catalyst. The morphological surface analysis of ZIF-67, as detected by SEM, is presented in Figure 4. As illustrated in Figure 4a, the SEM (Figure 4a) revealed the presence of rhombic dodecahedron crystals of ZIF-67, exhibiting a porous encasement surface geometry. The results depicted in Figure 4b demonstrate that after the treatment the following EC-MOF combined process, the formation of a rough surface morphology with agglomerated crystals may be attributed to the generation of aluminium flocs within the EC process. Additionally, it is evident that some of the flocs, which contain entrapped dye molecules, have also agglomerated on ZIF-67 crystals. The elemental analysis of the ZIF-67 catalyst was conducted using energy-dispersive X-ray spectroscopy (EDX). Figure 4b illustrates the EDX spectrum of ZIF-67, both before and after the treatment, which displays the presence of the elements C, N, O and Co. Table 1 presents the EDX elemental composition of ZIF-67 (untreated) and ZIF-67 (treated). The data indicate that ZIF-67 is primarily composed of carbon (27.78%), oxygen (40.56%), cobalt (20.41%), gold (3.87%), and nitrogen (7.38%). Table. 1. EDX composition of ZIF-67. Element Before treatment After treatment Weight % Atomic % Weight % Atomic % C 27.78 39.90 39.58 46.08 N 7.38 9.24 32.66 32.6 O 40.56 44.45 24.08 21.04 Co 20.41 6.07 0.13 0.03 Au 3.87 0.34 3.55 0.25 The surface area and pore size of the catalyst were determined using the Brunauer–Emmett–Teller (S BET ) technique, with values of 247.64 m²/g and 0.0441 cm³/g, respectively. 3.2. Effect of pH The impact of pH on the decolorization process was investigated by modifying the pH of the dye solution across the acidic to alkaline range. The outcomes of this investigation are presented in Figure 5. The results indicate that significant reductions in dye concentration are achieved when using both EC and EC-MOF methods at a pH level that is neither acidic nor alkaline. In the electrocoagulation (EC) procedure (Figure 5a), the degree of decolourisation was markedly high at both acidic and neutral pH levels, with values of 64.12 % and 72.33% respectively. Nevertheless, a reduction in RB-5 removal efficiency was observed at a basic pH of 9, with a value of 51.49% recorded after 30 minutes of treatment. During the electrocoagulation process, the formation of a number of different monomeric and polymeric metal hydroxide complexes occurs, which is influenced by the pH of the solution [38]. Under acidic conditions, Al 3+ ions undergo a transformation into soluble monomeric species, including Al(OH) 2+ , Al(OH) 2+ , and Al(OH) 3 . Conversely, in basic environments, monomeric species undergo a transformation into polymeric species, including Al 2 (OH) 2 4+ and Al 6 (OH) 15 3+. The soluble monomeric and polymeric cations are transformed into insoluble Al(OH) 3 , resulting in the formation of the dominant species Al(OH) 4 − [39]. This reduces the degree of attack by the coagulant on the dye molecules, given that the dye molecule is anionic in nature. At a pH of 7, the primary form of Al(OH) 3 exhibits minimal solubility and readily attracts dye molecules. It may be separated using flotation techniques. The EC-MOF method (as illustrated in Figure 5b) demonstrated a 91.66% decolourisation at pH 7 and an 84.32% reduction at pH 5. These findings suggest that incorporating ZIF-67 into the EC process enhances its efficacy. This is due to the fact that the supplementary adsorbent enhances the capacity for capturing dye molecules by providing a larger surface area and facilitating the expeditious removal of dye [31]. 3.3. Effect of current density The current density represents a crucial factor in the electrocoagulation process, which is employed for the production of aluminium hydroxide complexes with the objective of eliminating dye molecules. An investigation was conducted to examine the impact of the current density parameter on the elimination of dye, within the range of 9.26 to 23.15 mA/cm 2 . The results, as illustrated in Figure 6, demonstrate a notable improvement in the removal of dye as the applied current density is increased. In a single electrocoagulation (EC) procedure (Figure 4a), a high current density of 23.15 mA/cm 2 resulted in the removal of 71.2% of the dye. However, at a lower current density of 9.26 mA/cm 2 , only 51.1% of the dye was removed. In conditions of high current density, the formation of metal ions is increased, resulting in the synthesis of a greater amount of metal hydroxide flocs. This causes the rapid removal of dye molecules. Consequently, the rate of electrocoagulation processes is greatly increased. The increased formation of bubbles, mixing, and mass transfer in the aqueous solution leads to a higher efficiency in removing dye [40]. A comparison of the EC procedure with EC-MOF (Figure 6b) revealed that the EC-MOF yielded superior results. The removal efficiency of the RB-5 dye was found to be 95.40%, 92.22%, and 75.02% at current densities of 23.15, 18.52, and 9.26 mA/cm 2 , respectively. The removal efficiency of RB-5 dye molecules decreased to 92.22% and 85.65% respectively. This reduction may be attributed to the sluggishness of electrocoagulation processes at the diminished current density [41]. Moreover, a decrease in the current value results in a diminished synthesis of coagulants within the solution, consequently leading to a decreased elimination of the dye due to the reduced anodic dissolution of Al ions. 3.4. Effect of ZIF-67 dose The influence of the ZIF-67 dosage on the effectiveness of RB-5 removal was investigated within the range of 30–50 mg. The results, as illustrated in Figure 7, demonstrate that the utilisation of a greater quantity of ZIF-67 as an adsorbent result in a significantly enhanced percentage of dye removal. At a dosage of 50 mg/L of ZIF-67, the decolorization efficiency reached its maximum value, equating to 95.9%. Lower dosages such as 40 mg/l and 30 mg/l of ZIF-67 results in the reduction of decolorization efficiencies which was equal to 82.2% and 76.2%, respectively. An increase in the quantity of adsorbent results in a greater availability of sorption sites, enhanced diffusion, and a larger, more accessible surface area. These characteristics contribute to the enhanced efficiency of dye removal when a high dosage of ZIF-67 is employed [41]. 3.5. Effect of dye concentration The impact of the initial RB-5 concentration was investigated by modifying the concentration of the dye in solutions with starting concentration of 50 mg/l, 75 mg/l, and 100 mg/l. As was illustrated in Figure 8, the experimental results demonstrated a significant reduction of 95.54% in the dye concentration when the initial concentration was low. However, an inverse correlation between dye concentration and decolorization. The observed decrease in efficiency may be attributed to a modification in the proportion of dye molecules to the produced Al flocs and the active sites of ZIF-67 in the electro-coagulation coupled MOF treatment process, which in turn leads to a longer treatment time being necessary. The removal of the dye is somewhat restricted due to the existence of a certain quantity of aluminium hydroxide coagulants, generated at a given applied current density, and a defined number of accessible adsorption sites at a specific ZIF-67 dose [42]. Specially, when the concentrations were increased to 75 mg/l and 100 mg/l, the effectiveness of elimination reduced to 91.9% and 82.32%, respectively. 3.6. Single and combined process comparison A comparative study was conducted to evaluate the performance of stand-alone technologies, specifically EC and MOF-ZIF-67, in conjunction with a combined process, EC-MOF. The study was conducted under optimal conditions, specifically at a pH of 7, a dye concentration of 50 mg/l, and a ZIF-67 dose of 50 mg/l. The results (Figure 9) demonstrate that the combined process (EC-MOF) exhibits high dye elimination due to the synergistic effects. The dye elimination achieved in the ZIF-67 MOF adsorption process was only 46.2%, while the EC process showed up to 72.01% removal. However, the EC-MOF combined process boosted the removal efficiency to up to 95.40%. These findings demonstrate that the advantages of stand-alone technologies are coactively amplified in the combined process for the rapid degradation of organic pollutants. 3.7. Reusability studies The catalyst's lifespan and cost-effectiveness are largely contingent upon its reusability. The reusability of the ZIF-67 catalyst was investigated over three cycles in the MOF-EC process. Following the initial treatment cycle of the dye, the ZIF-67 was washed with ethanol and subjected to vacuum drying at 50°C for 24 hours [43]. Subsequently, the dried ZIF-67 was reused for a further treatment process up to three cycles. The removal efficiency achieved in the respective cycles was 98.9% in the first cycle, 92.3% in the second cycle, and 86.1% in the third cycle (see Figure 10). The insignificant drop in ZIF-67 activity in EC-MOF indicates stable performance and remarkable reusability. 3.9. Treatment of real textile effluent The real textile wastewater was initially characterized and subsequently treated byZIF-67 augmented electrocoagulation process at optimal parameters such as pH 7, current density 18.52 mA/cm 2 and 50 mg dosage of ZIF-67 catalyst. The effective effluent treatment was achieved within a period of 30 minutes time. The ZIF-67 enhanced electrocoagulation process results in the removal of 42.23% COD, 39.10% BOD and 59.11% colour. The combined effect of eletro-flocs in the presence of ZIF-67 crystals lead to a significant enhancement in the elimination of pollutants. The pre and post treatment characterization of textile effluent is shown in Table 2. Table 2. Characterization of the real wastewater containing RB-5 dye. Parameter Before Treatment After Treatment pH 7 7.3 COD (mg/L) 310 182 TDS (mg/L) 3800 890 BOD 5 190 131 Turbidity (NTU) 7.85 1.42 Colour Yellow Colourless COD – the chemical oxygen demand , TDS – the total dissolved solid; BOD – the biochemical oxygen demand ; NTU – the nephelometric turbidity units. 4. Conclusions The findings of this research demonstrate the efficacy of the ZIF-67-aided electrocoagulation process for the treatment of textile wastewater. The comparative analysis of the processes revealed that the combined MOF-ZIF-67 process exhibited a notable enhancement in colour elimination compared to the standalone processes such as ZIF-67 and MOF. At the optimal pH of 7, current density of 18.52 mA/cm², 50 mg/l of ZIF-67, and a dye concentration of 50 mg/l, a colour elimination rate of 99% was achieved. The reusability study demonstrated the high efficiency of ZIF-67, with 80.3% removal achieved after the third cycle. The combined process demonstrated the elimination of colour in real wastewater up to 59.11%, COD removal 42.23 % and 39.10% BOD 5 reduction. Consequently, the combined process exhibited a notable enhancement in performance in comparison to standalone technologies for the expeditious degradation of organic pollutants. Therefore, the electrocoagulation combined MOF process is an effective approach for wastewater remediation applications. Declarations CRediT authorship contribution statement Muhammad Uzair: Investigation, Methodology,Validation , Writing—original draft preparation, Writing—review and editing, Muhammad Fahad Tariq: Conceptualization, Data curation, Formal analysis, Methodology, Validation, Writing—original draft preparation, Writing—review and editing, Software, Visualization, Farhan Javed: Supervision,Conceptualization, Investigation, Resources, Writing—original draft preparation, Writing—review and editing, Visualization Data curation, Validation, Writing—review and editing, Funding acquisition. Mohammed Kadhom: Methodology, Validation, Writing—original draft preparation, Writing—review and editing, Software, Visualization. Shakirullah: Data curation, Formal analysis, Writing—review and editing, Visualization. Declaration of Competing Interest The authors declare no competing financial interests or personal relationships that could influence the work reported in this paper. Acknowledgments The authors acknowledge the financial support provided by HEC (NRPU-16521) and technical support by UET Lahore is gratefully acknowledged. Data availability statement All relevant data are available in this paper. References Masood, Z., et al., Application of nanocatalysts in advanced oxidation processes for wastewater purification: Challenges and future prospects. Catalysts, 2022. 12 (7): p. 741. Gadipelly, C., et al., Pharmaceutical industry wastewater: review of the technologies for water treatment and reuse. Industrial & Engineering Chemistry Research, 2014. 53 (29): p. 11571-11592. Rahmani, A., H. Rahmani, and K. Rahmani, Degradation Reactive Black 5 dye from aqueous solutions using ozonation with pumices and pumices modified by nanoscale zero valent iron (nZVI). GLOBAL NEST JOURNAL, 2020. 22 (3): p. 336-341. Hu, E., S. Shang, and K.-L. Chiu, Removal of reactive dyes in textile effluents by catalytic ozonation pursuing on-site effluent recycling. 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Kumbur, Treatment of fruit juice concentrate wastewater by electrocoagulation: Optimization of COD removal. International Advanced Researches and Engineering Journal, 2018. 2 (1): p. 53-57. Chokshi, N.P., et al., Heterogeneous catalytic ozonation of Reactive Black 5 with cobalt oxide. Int. J. Chemtech. Res, 2017. 10 : p. 402-409. Liang, C., et al., ZIF-67 derived hollow cobalt sulfide as superior adsorbent for effective adsorption removal of ciprofloxacin antibiotics. Chemical engineering journal, 2018. 344 : p. 95-104. Afarinandeh, A., et al., Controlled removal of fluoride by ZIF-8, ZIF-67, and Ni-MOF of different morphologies. Arabian Journal of Chemistry, 2023. 16 (7): p. 104837. Akhtar, A., et al., Electrocoagulation of Congo Red dye-containing wastewater: Optimization of operational parameters and process mechanism. Journal of Environmental Chemical Engineering, 2020. 8 (5): p. 104055. Javed, F., et al., Treatment of Reactive Red 241 dye by electro coagulation/biosorption coupled process in a new hybrid reactor. Desalin. Water Treat, 2019. 166 : p. 83-91. Javed, F., et al., Elimination of basic blue 9 by electrocoagulation coupled with pelletized natural dead leaves (Sapindus mukorossi) biosorption. International Journal of Phytoremediation, 2021. 23 (5): p. 462-473. Noreen, N., et al., Treatment of methylene blue in aqueous solution by electrocoagulation/micro-crystalline cellulosic adsorption combined process. Desalination and Water Treatment, 2020. Bayazıt, G., Ü.D.G. , and D. Ünal, Biosorption of Acid Red P-2BX by lichens as low cost biosorbents. International Journal of Environmental Studies. Cite Share Download PDF Status: Posted Version 1 posted You are reading this latest preprint version Research Square lets you share your work early, gain feedback from the community, and start making changes to your manuscript prior to peer review in a journal. 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Also discoverable on Platform About Our Team In Review Editorial Policies Advisory Board Help Center Resources Author Services Accessibility API Access RSS feed Manage Cookie Preferences © Research Square 2026 | ISSN 2693-5015 (online) Privacy Policy Terms of Service Do Not Sell My Personal Information {"props":{"pageProps":{"initialData":{"identity":"rs-7376258","acceptedTermsAndConditions":true,"allowDirectSubmit":true,"archivedVersions":[],"articleType":"Research Article","associatedPublications":[],"authors":[{"id":505406009,"identity":"77955d26-d5ba-451c-9999-9b0d54c406b4","order_by":0,"name":"Muhammad Uzair","email":"","orcid":"","institution":"University of Engineering \u0026 Technology","correspondingAuthor":false,"prefix":"","firstName":"Muhammad","middleName":"","lastName":"Uzair","suffix":""},{"id":505406010,"identity":"5197c35c-3c6f-4785-ae7e-71171e853e5e","order_by":1,"name":"Muhammad Fahad Tariq","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAA5ElEQVRIiWNgGAWjYBAC+wM8DAw8DAd47NubDwD5EjIEtRgwQLTIGfAcSwBp4SFai7GBRI4BSIAILexnD354U3MncTtDzudXN2oseBjYDx/dgNcvPHnJknOOPUvc2XB2m3XOMaDDeNLSbuB3WI6BNG/D4cSGg73bjHPYgFokeMzwa+F/Y/wbrOUwzzPjnH/EaJHIMQPZYmxwjIf5cW4bUVremFnOOXZYTrKHzYw5t0+Ch42gX/hzjG+8qTnMwy//+PHnnG91cvzsh4/h1YIM2CTAJLHKQYD5AymqR8EoGAWjYOQAAGErSgWx07kKAAAAAElFTkSuQmCC","orcid":"https://orcid.org/0009-0003-1110-9036","institution":"University of Engineering and Technology","correspondingAuthor":true,"prefix":"","firstName":"Muhammad","middleName":"Fahad","lastName":"Tariq","suffix":""},{"id":505406011,"identity":"d9d1520e-44bb-4777-8b68-f1a142b92be7","order_by":2,"name":"Farhan Javed","email":"","orcid":"","institution":"University of Engineering and Technology","correspondingAuthor":false,"prefix":"","firstName":"Farhan","middleName":"","lastName":"Javed","suffix":""},{"id":505406012,"identity":"4e58f800-bad2-4c8f-bb9f-ee551fc6b8ec","order_by":3,"name":"Mohammed Kadhom","email":"","orcid":"","institution":"KUS: Al-Karkh University of Science","correspondingAuthor":false,"prefix":"","firstName":"Mohammed","middleName":"","lastName":"Kadhom","suffix":""},{"id":505406013,"identity":"d807d0e6-a048-4fc0-a848-0b36908acb0b","order_by":4,"name":"Shakir Ullah","email":"","orcid":"","institution":"University of Engineering and Technology","correspondingAuthor":false,"prefix":"","firstName":"Shakir","middleName":"","lastName":"Ullah","suffix":""}],"badges":[],"createdAt":"2025-08-14 18:19:39","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-7376258/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-7376258/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":90406067,"identity":"2ffad7d8-1e16-40d4-8a25-1b27859ab2ea","added_by":"auto","created_at":"2025-09-02 11:09:01","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":176920,"visible":true,"origin":"","legend":"\u003cp\u003eZIF-67 synthesis steps\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/9f2f2e0cb070be5b4b1b66a4.png"},{"id":90406198,"identity":"dbaa573d-a671-4fe5-94b3-195a47138994","added_by":"auto","created_at":"2025-09-02 11:09:05","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":174730,"visible":true,"origin":"","legend":"\u003cp\u003eSchematic view of the experimental setup.\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/7a70f24a2ef009af99db31b1.png"},{"id":90406218,"identity":"70755fac-c9e4-4035-83e2-ee31b2c39da3","added_by":"auto","created_at":"2025-09-02 11:09:05","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":42874,"visible":true,"origin":"","legend":"\u003cp\u003eATR-FTIR spectra of ZIF-67 a) before treatment, b) after treatment\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/ac525c775cabf7e0be18f362.png"},{"id":90406653,"identity":"38004b72-47b3-4337-9ead-cee04f7e3fd1","added_by":"auto","created_at":"2025-09-02 11:17:05","extension":"png","order_by":4,"title":"Figure 4","display":"","copyAsset":false,"role":"figure","size":559113,"visible":true,"origin":"","legend":"\u003cp\u003e(a) SEM and EDX of ZIF-67 (a) before and (b) after treatment.\u003c/p\u003e","description":"","filename":"4.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/c78aa737b57f8c098f91e420.png"},{"id":90406072,"identity":"e54c6ae6-7ff9-4690-9d54-69d50983e963","added_by":"auto","created_at":"2025-09-02 11:09:02","extension":"png","order_by":5,"title":"Figure 5","display":"","copyAsset":false,"role":"figure","size":209410,"visible":true,"origin":"","legend":"\u003cp\u003eEffect of pH on RB-5 removal using the (a) EC process (C\u003csub\u003eRB-5\u003c/sub\u003e=75 mg/l, j=18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e) and (b) EC-MOF process (C\u003csub\u003eRB-5\u003c/sub\u003e=75 mg/l, j=18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e, C\u003csub\u003eZIF-67\u003c/sub\u003e=50 mg/l).\u003c/p\u003e","description":"","filename":"5.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/47617fbcb75f9ec2dfdaf8d8.png"},{"id":90406219,"identity":"8ff2a6ce-d227-43c8-a408-58662dbe7b67","added_by":"auto","created_at":"2025-09-02 11:09:05","extension":"png","order_by":6,"title":"Figure 6","display":"","copyAsset":false,"role":"figure","size":226940,"visible":true,"origin":"","legend":"\u003cp\u003eEffect of current density on RB-5 removal using the (a) EC process (C\u003csub\u003eRB-5\u003c/sub\u003e=75 mg/l, pH 7) and (b) EC-MOF process (C\u003csub\u003eRB-5\u003c/sub\u003e=75 mg/l, pH 7, C\u003csub\u003eZIF-67\u003c/sub\u003e=50 mg/l).\u003c/p\u003e","description":"","filename":"6.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/77556e005a61c54832fb5327.png"},{"id":90406232,"identity":"7f5074ae-8f68-4120-a622-38e886bd9470","added_by":"auto","created_at":"2025-09-02 11:09:06","extension":"png","order_by":7,"title":"Figure 7","display":"","copyAsset":false,"role":"figure","size":122861,"visible":true,"origin":"","legend":"\u003cp\u003eEffect of MOF dose (EC-MOF process, C\u003csub\u003eRB-5\u003c/sub\u003e=50 mg/l, pH 7, j=18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e).\u003c/p\u003e","description":"","filename":"7.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/ed3b302d20daa9b3341fd1ba.png"},{"id":90406194,"identity":"e71ad076-80db-4371-85d1-1671f9d707de","added_by":"auto","created_at":"2025-09-02 11:09:04","extension":"png","order_by":8,"title":"Figure 8","display":"","copyAsset":false,"role":"figure","size":104896,"visible":true,"origin":"","legend":"\u003cp\u003eEffect of dye concentration (EC-MOF process, pH 7, C\u003csub\u003eZIF-67\u003c/sub\u003e=50 mg/L, j=18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e).\u003c/p\u003e","description":"","filename":"8.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/0fd1a3a89c1e832226dde3b4.png"},{"id":90406659,"identity":"5dc8bc1e-d332-4495-8727-4a0ffc3022a9","added_by":"auto","created_at":"2025-09-02 11:17:07","extension":"png","order_by":9,"title":"Figure 9","display":"","copyAsset":false,"role":"figure","size":136634,"visible":true,"origin":"","legend":"\u003cp\u003eA comparative analysis of the removal efficiency of RB-5 utilizing the individual and integrated processes for its elimination.\u003c/p\u003e","description":"","filename":"9.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/460e7a4e57f1aee4f23e7908.png"},{"id":90406132,"identity":"47be36ea-efa1-4d8b-a921-11030c773d77","added_by":"auto","created_at":"2025-09-02 11:09:02","extension":"png","order_by":10,"title":"Figure 10","display":"","copyAsset":false,"role":"figure","size":67585,"visible":true,"origin":"","legend":"\u003cp\u003eZIF-67 catalyst reusability.\u003c/p\u003e","description":"","filename":"10.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/af65da608f4c9cb749c8cf52.png"},{"id":90406209,"identity":"0eec924e-ca98-4924-a3f2-7879ebd39f67","added_by":"auto","created_at":"2025-09-02 11:09:05","extension":"png","order_by":11,"title":"Figure 11","display":"","copyAsset":false,"role":"figure","size":90764,"visible":true,"origin":"","legend":"\u003cp\u003eDegradation of the real textile wastewater by hybrid EC and MOF process, pH 7, j =18.52 mA/cm\u003csup\u003e2 \u003c/sup\u003e, ZIF 67=50\u0026nbsp; mg/l.\u003c/p\u003e","description":"","filename":"11.png","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/98ea26f3351e0b8e7a6f976d.png"},{"id":93643282,"identity":"b0c9a354-0a70-47ad-b95b-de137110c506","added_by":"auto","created_at":"2025-10-16 03:23:41","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":2574084,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-7376258/v1/d47ef826-d7aa-43cc-8469-b8c490efe2ba.pdf"}],"financialInterests":"","formattedTitle":"A study on ZIF-67 augmented Electrocoagulation process for Wastewater Treatment","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eThe natural resources of water, air, and land are under great threat because of rapid urbanization and industrialization. Freshwater is a scarce resource, and it is of great concern to prevent environmental pollution that results in a deterioration of water quality. Furthermore, the direct realize of industrial wastewater into the water bodies has resulted in significant adverse effects on the ecosystem. This is due to toxicity of the wastewater, which has led to the contamination of freshwater channels and rivers with a range of pollutants, including industrial waste, synthetic dyes, and pharmaceuticals. A number of industries, including pharmaceutical, textiles, paper, cosmetics, leather, food, and paint are responsible for the discharge of harmful and carcinogenic compounds into the environment through wastewater [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e, \u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e]. The introduction of such pollutants is accountable for adverse effects on the biodiversity of the ecosystem. Textile industries represent a significant source of water pollution on a global scale. Over 700,000 dyes are produced annually for the textile industry. It is estimated that approximately 80% of all industrial wastewater discharged originates from the textile sector. This wastewater contains elevated pollutant concentrations, primarily in the form of dyes [\u003cspan additionalcitationids=\"CR4 CR5\" citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e]. A variety of hazardous dyes, heavy metals (such as mercury, chromium, cadmium, lead, and arsenic), and aromatic compounds have been identified in textile wastewater [\u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]. Dyes are highly stable, carcinogenic, and recalcitrant pollutants in wastewater that have been shown to have adverse effects on humans and plants. The elimination of these hazardous dyes from wastewater is a crucial step for ensuring environmental safety [\u003cspan additionalcitationids=\"CR9 CR10 CR11\" citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e]. A number of techniques for wastewater treatment have been the subject of resent research including chemical, physical, and biological methods. These methods include biodegradation, adsorption [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e], membrane filtration, ion exchange, sedimentation, electrocoagulation treatment, ozonation [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e], Fenton oxidation [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e], photo catalysis [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e] and electrocoagulation [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e]. These techniques, when applied in standalone technology, may not be sufficient to treat textile effluent. For instance, the biological approach is unsuitable for the removal of colour from dyes, due to the fact that the majority of dyes are harmful to the microorganisms used in the procedure. Physical methods such as membrane filtration and ion exchange have notable constraints, namely that they are most effective when dealing with tiny volumes of wastewater. However, the combination of some approaches has been effectively used in the treatment of different dyes. electrocoagulation processes, such as electrocoagulation (EC) have attracted considerable attention for their many benefits. Traditional chemical coagulation is highly affected by variations in the organic load of textile wastewater. Variations in the amount of coagulant used can affect this method results in process inefficiencies. Coagulants can also contribute to the presence of additional pollutants. To address these issues, researchers have turned to the electrocoagulation process, which eliminates the need for any additional chemicals. Electrocoagulation achieves rapid decolourisation, resulting in a reduced amount of sludge. Electrocoagulation has several advantages over traditional technologies. It requires smaller units, is not-specific in nature, can be easily automated, and is associated with reduced operating costs [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e, \u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eIn EC, the metal cations are produced by anodic oxidation, while the hydroxyl ions are produced by electrolysis at the cathode. The hydroxyl ions and metal cations undergo a chemical reaction to form metal hydroxide complexes, which have a high adsorption capacity and are able to bind contaminants. Several coagulant species with pH-dependent properties are formed in the solution. The coagulants formed disrupt and counteract the charge of the pollutant dye molecules, causing them to aggregate and form flocs. These flocs are then separated by sedimentation or flotation. The impurities are propelled upwards on the liquid's surface in the EC cell by tiny hydrogen gas bubbles generated at the cathode [\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e, \u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eKhoram et al. [\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e] have investigated the Electrocoagulation method for the remidation of textile dye wastewater under the optimal conditions pH 5.5 and current density 15 mA/cm\u003csup\u003e2\u003c/sup\u003e the decolorization, and COD removal was obtained 98 and 40% respectively. Bener et al. [\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e] studied how various levels of current density from 12.5 to 100 mA/cm\u003csup\u003e2\u003c/sup\u003e affected the effectiveness of TOC removal (10\u0026ndash;22.5%) from actual textile wastewater. Mousazadeh et al. [\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e] was reported the high removal of COD 96% by using electrocoagulation method at Current density 25 Am for 50 min of treatment time. In another research work, Bayramoglu et al. [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e] has studied the maximum COD removal 98% obtained at maximum current density 150 mA/cm\u003csup\u003e2\u003c/sup\u003e after 25 min of treatment time.\u003c/p\u003e\u003cp\u003eEfficient adsorbents with high porosity and large surface area can improve the economic and energy efficient treatment of dyes by adsorption. In this regard, metal-organic frameworks (MOFs) have favourable adsorption properties due to their unique properties. The MOF structure consists of porous crystalline frameworks formed by bonding metal complexes to organic linkers [\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e, \u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]. MOFs have superior performance in wastewater treatment compared to other porous materials such as activated carbon, zeolites, and polymers. The pore size and form of MOF materials can be easily adjusted from the microporous to the mesoporous scale by changing the connectivity of the inorganic component and the type of the organic linker. Recently, MOF materials have found applications in various fields, including drug delivery, adsorption of organic molecules, gas adsorption, separation, catalysis, electrode materials, nanomaterial carriers, magnetism, polymerisation, and membranes [\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e].\u003c/p\u003e\u003cp\u003eZeolitic imidazolate frameworks 67 (ZIF-67) are highly favoured among metal-organic frameworks due to their exceptional capabilities, they are having some advantages over other MOFs such as good adsorption capability, Larger Surface area and good thermal property, and as well as their affordability, facile synthesis, and structural robustness. Within this particular class, the ZIF-67 has shown remarkable efficacy in removing dyes during the process of wastewater treatment process [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e, \u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e, \u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. However, the limitation of stand-alone technologies has prompted research into sophisticated integrated methods that offer benefits such as accelerated treatment and cost efficiency.\u003c/p\u003e\u003cp\u003eThe present research elucidates the parametric effects of the ZIF 67 augmented electrocoagulation process for the pollutants reduction in wastewater. The effects of parameters such as pH, MOF dose, current density, and dye concentration were investigated to study the removal of color, BOD and COD. The catalyst was characterised using techniques such as the Fourier Transform Infrared Spectroscopy (FTIR), Scanning Electron Microscopic (SEM), Energy Dispersive X-ray Spectroscopy (EDX), and Bruner\u0026ndash; Emmet\u0026ndash;Teller (BET). The real wastewater was characterized for the BOD\u003csub\u003e5\u003c/sub\u003e, COD, Turbidity and pH values.\u003c/p\u003e"},{"header":"2. Materials and methods","content":"\u003cdiv id=\"Sec3\" class=\"Section2\"\u003e\u003ch2\u003e2.1. Materials and Reagents\u003c/h2\u003e\u003cp\u003eThe Reactive Black 5 (RB-5) dye of analytical grade was obtained from Sigma-Aldrich (USA). The following chemicals were utilized in this study: sodium hydroxide (NaOH) with a purity of 99%, hydrochloric acid (HCl) of 37% concentration cobalt (II) nitrate hexahydrate Co(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026sdot;6H\u003csub\u003e2\u003c/sub\u003eO with a purity of 98%, 2-methylimidazole, deionized water (DI), sodium chloride (NaCl), and ethyl alcohol which were delivered by Merck, Germany. All compounds were of analytical grade and were employed without additional purification. The standard solutions were prepared through standard methods. The actual textile effluent was obtained from a nearby textile manufacturing facility (combined fabrics Lahore Pk). The synthetic textile effluent was prepared in the laboratory by dissolving the RB-5 and electrolyte in distilled water.\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec4\" class=\"Section2\"\u003e\u003ch2\u003e2.2. Synthesis of ZIF-67\u003c/h2\u003e\u003cp\u003eZIF-67 was synthesized using the procedure outlined in a previous publication [\u003cspan citationid=\"CR31\" class=\"CitationRef\"\u003e31\u003c/span\u003e], as illustrated in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e. Two solutions were each made by dissolving 0.717 g of (Co(NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026sdot;6H\u003csub\u003e2\u003c/sub\u003eO) in 50 ml of deionized water. Furthermore, 1.622 grams of 2-methylimidazole was added to the second solution along with 50 millilitres of deionized water. Subsequently, the mixture was then agitated until a transparent solution was obtained. Next, the solution of Co (NO\u003csub\u003e3\u003c/sub\u003e)\u003csub\u003e2\u003c/sub\u003e\u0026sdot;6H\u003csub\u003e2\u003c/sub\u003eO was introduced into the 2-methylimidazole solution and agitated for 30 minutes at ambient temperature. The ZIF-67 purple precipitates were obtained by centrifuging using a centrifuge (Model 800D, Canfort, China) the mixture for 20 minutes at a speed of 3000 rpm. The precipitates were then washed three times with ethanol and water and then dried under a vacuum at a temperature of 80\u003csup\u003e○\u003c/sup\u003eC for 24 hours.\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec5\" class=\"Section2\"\u003e\u003ch2\u003e2.3. Experimental\u003c/h2\u003e\u003cp\u003eFigure \u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e depicts the experimental configuration employed in the investigation. The experimental arrangement comprises a glass reactor housing aluminium electrodes with dimensions of 15 cm in length, 5 cm in width, and 0.2 cm in thickness The electrodes are connected to a direct current (DC) power source, specifically a Dazheng PS-605D model form China). The electrodes were meticulously abraded with sandpaper and then immersed in a diluted HCl solution for a duration of 10 minutes. Additionally, they were rinsed with distilled water to eliminate any surface contaminants and prevent electrode passivation before to each experimental trial. The distance between the vertical electrodes was maintained at a constant value of 1 cm. In each trial, the reactor was filled with one litre of dye solution. An electrolyte, sodium chloride (NaCl), was supplied in the quantity of 1.0 gram. The pH level was then adjusted by the addition of the require quantities of 1 M NaOH and 1 M HCl solution. The prescribed amount of ZIF-67 was loaded, and continuous stirring was conducted using a magnetic stirrer (Model 79-1A, Canfort, China) [\u003cspan additionalcitationids=\"CR33\" citationid=\"CR32\" class=\"CitationRef\"\u003e32\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR34\" class=\"CitationRef\"\u003e34\u003c/span\u003e]. Samples were obtained at specific intervals, subjected to filtration, and examined with the UV-visible spectrophotometer (PerkinElmer Lambda 35 double beam) to determine the concentration of the dye. The absorbance of all samples was analysed at the wavelength of maximum absorption, which was measured to be 596 nm [\u003cspan citationid=\"CR35\" class=\"CitationRef\"\u003e35\u003c/span\u003e].\u003c/p\u003e\u003cp\u003e\u003c/p\u003e\u003c/div\u003e\u003cdiv id=\"Sec6\" class=\"Section2\"\u003e\u003ch2\u003e2.4. Characterization techniques\u003c/h2\u003e\u003cp\u003eThe Bruker Alpha-E FTIR spectrometer was employed to determination of the functional groups present on the surface of ZIF-67. This analysis was conducted using an Attenuated Total Reflectance-Fourier-Transform Infrared Spectroscopy (ATR-FTIR) and spectrum with a covering the wavelength range of 400 to 4000 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e at a resolution of 2 cm\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e using diamond single-reflection attenuated total reflectance. The Nova Nano SEM 450 analyser was used to assess the elemental composition of the catalyst and examine its surface structure through Energy-Dispersive X-ray spectroscopy (EDX). Images were captured using an electron beam with an acceleration voltage of 10 kV. The Micrometrics-ASAP-2020 detector was used to analyse the surface area and pore size via usage of the Brunauer\u0026ndash;Emmett\u0026ndash;Teller (BET) technique. The samples were subjected to a vacuum degassing process for eight hours at a temperature of 150\u0026deg;C. The nitrogen adsorption-desorption isotherms, with a purity level of 99.99%, were tested at a temperature of 77 Kelvin.\u003c/p\u003e\u003c/div\u003e"},{"header":"3. Results and discussion","content":"\u003cp\u003e\u003cstrong\u003e3.1. Catalyst characterization\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe functional groups present on the surface of ZIF-67 were identified through the utilization of the Attenuated Total Reflectance-Fourier-Transform Infrared (ATR-FTIR) spectrometer, with measurements obtained within the spectral range of 500\u0026ndash;4,000 cm⁻\u0026sup1;.\u003c/p\u003e\n\u003cp\u003eThe primary bands were identified in the 600-1500 cm\u003csup\u003e-1\u003c/sup\u003e wavenumber range (Figure 3), indicating the stretching and bending properties of the imidazole ring. The band observed at 1418.41 cm\u003csup\u003e\u0026minus;1\u003c/sup\u003e is attributed to the C-N stretching in the imidazole, while the range of 1000-1350 cm\u003csup\u003e-1\u003c/sup\u003e is associated with the in-plane bending vibration of the imidazole ring. It is also noteworthy to mention the band \u0026nbsp;at 991.10 cm\u003csup\u003e\u0026minus;1\u003c/sup\u003e refers to C-N [36].The bands at 2919.62 cm\u003csup\u003e\u0026minus;1\u003c/sup\u003e indicate C-H in the imidazole ring, whereas the distinctive peak in ZIF-67 occurred at 1560.66 cm\u003csup\u003e-1\u003c/sup\u003e, which correlates to C=N. The peak at 3220.86 cm\u003csup\u003e\u0026minus;1\u003c/sup\u003e corresponds to the O-H stretching vibration [36, 37]. After treatment the peaks drift from 1418.41 cm\u003csup\u003e-1\u003c/sup\u003e to 1418.28 cm\u003csup\u003e-1\u003c/sup\u003e for C-N group, for C=N stretching peaks changes from 1560.66 cm\u003csup\u003e-1\u003c/sup\u003e to 1568.98 cm\u003csup\u003e-1\u003c/sup\u003e. This drift due to the adsorption of RB 5 dye on the surface of the catalyst.\u003c/p\u003e\n\u003cp\u003eThe morphological surface analysis of ZIF-67, as detected by SEM, is presented in Figure 4. As illustrated in Figure 4a, the SEM (Figure 4a) revealed the presence of rhombic dodecahedron crystals of ZIF-67, exhibiting a porous encasement surface geometry. The results depicted in Figure 4b demonstrate that after the treatment the following EC-MOF combined process, the formation of a rough surface morphology with agglomerated crystals may be attributed to the generation of aluminium flocs within the EC process. Additionally, it is evident that some of the flocs, which contain entrapped dye molecules, have also agglomerated on ZIF-67 crystals.\u003c/p\u003e\n\u003cp\u003eThe elemental analysis of the ZIF-67 catalyst was conducted using energy-dispersive X-ray spectroscopy (EDX). \u003cstrong\u003eFigure 4b\u003c/strong\u003e illustrates the EDX spectrum of ZIF-67, both before and after the treatment, which displays the presence of the elements C, N, O and Co. \u003cstrong\u003eTable 1\u003c/strong\u003e presents the EDX elemental composition of ZIF-67 (untreated) and ZIF-67 (treated). The data indicate that ZIF-67 is primarily composed of carbon (27.78%), oxygen (40.56%), cobalt (20.41%), gold (3.87%), and nitrogen (7.38%).\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable. 1.\u0026nbsp;\u003c/strong\u003eEDX composition of ZIF-67.\u003c/p\u003e\n\u003ctable border=\"1\" cellspacing=\"0\" cellpadding=\"0\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd rowspan=\"2\" valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eElement\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" style=\"width: 246px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eBefore treatment\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd colspan=\"2\" valign=\"top\" style=\"width: 246px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eAfter treatment\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eWeight %\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eAtomic %\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eWeight %\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eAtomic %\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eC\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e27.78\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e39.90\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e39.58\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e46.08\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eN\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e7.38\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e9.24\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e32.66\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e32.6\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eO\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e40.56\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e44.45\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e24.08\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e21.04\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eCo\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e20.41\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e6.07\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e0.13\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e0.03\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eAu\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e3.87\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e0.34\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e3.55\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 123px;\"\u003e\n \u003cp\u003e0.25\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\n\u003cp\u003eThe surface area and pore size of the catalyst were determined using the Brunauer\u0026ndash;Emmett\u0026ndash;Teller (S\u003csub\u003eBET\u003c/sub\u003e) technique, with values of 247.64 m\u0026sup2;/g and 0.0441 cm\u0026sup3;/g, respectively.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.2. Effect of pH\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe impact of pH on the decolorization process was investigated by modifying the pH of the dye solution across the acidic to alkaline range. The outcomes of this investigation are presented in Figure 5.\u003c/p\u003e\n\u003cp\u003eThe results indicate that significant reductions in dye concentration are achieved when using both EC and EC-MOF methods at a pH level that is neither acidic nor alkaline. In the electrocoagulation (EC) procedure (Figure 5a), the degree of decolourisation was markedly high at both acidic and neutral pH levels, with values of 64.12 % and 72.33% respectively. Nevertheless, a reduction in RB-5 removal efficiency was observed at a basic pH of 9, with a value of 51.49% recorded after 30 minutes of treatment. During the electrocoagulation process, the formation of a number of different monomeric and polymeric metal hydroxide complexes occurs, which is influenced by the pH of the solution [38]. Under acidic conditions, Al\u003csup\u003e3+\u003c/sup\u003e ions undergo a transformation into soluble monomeric species, including Al(OH)\u003csup\u003e2+\u003c/sup\u003e, Al(OH)\u003csup\u003e2+\u003c/sup\u003e, and Al(OH)\u003csub\u003e3\u003c/sub\u003e. Conversely, in basic environments, monomeric species undergo a transformation into polymeric species, including Al\u003csub\u003e2\u003c/sub\u003e(OH)\u003csub\u003e2\u003c/sub\u003e\u003csup\u003e4+\u003c/sup\u003e and Al\u003csub\u003e6\u003c/sub\u003e(OH)\u003csub\u003e15\u003c/sub\u003e\u003csup\u003e3+.\u003c/sup\u003e The soluble monomeric and polymeric cations are transformed into insoluble Al(OH)\u003csub\u003e3\u003c/sub\u003e, resulting in the formation of the dominant species Al(OH)\u003csub\u003e4\u003c/sub\u003e\u003csup\u003e\u0026minus;\u0026nbsp;\u003c/sup\u003e[39]. This reduces the degree of attack by the coagulant on the dye molecules, given that the dye molecule is anionic in nature. At a pH of 7, the primary form of Al(OH)\u003csub\u003e3\u003c/sub\u003e exhibits minimal solubility and readily attracts dye molecules. It may be separated using flotation techniques. The EC-MOF method (as illustrated in Figure 5b) demonstrated a 91.66% decolourisation at pH 7 and an 84.32% reduction at pH 5. These findings suggest that incorporating ZIF-67 into the EC process enhances its efficacy. This is due to the fact that the supplementary adsorbent enhances the capacity for capturing dye molecules by providing a larger surface area and facilitating the expeditious removal of dye [31].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.3. Effect of current density\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe current density represents a crucial factor in the electrocoagulation process, which is employed for the production of aluminium hydroxide complexes with the objective of eliminating dye molecules. An investigation was conducted to examine the impact of the current density parameter on the elimination of dye, within the range of 9.26 to 23.15 mA/cm\u003csup\u003e2\u003c/sup\u003e. The results, as illustrated in Figure 6, demonstrate a notable improvement in the removal of dye as the applied current density is increased. In a single electrocoagulation (EC) procedure (Figure 4a), a high current density of 23.15 mA/cm\u003csup\u003e2\u003c/sup\u003e resulted in the removal of 71.2% of the dye. However, at a lower current density of 9.26 mA/cm\u003csup\u003e2\u003c/sup\u003e, only 51.1% of the dye was removed. In conditions of high current density, the formation of metal ions is increased, resulting in the synthesis of a greater amount of metal hydroxide flocs. This causes the rapid removal of dye molecules. Consequently, the rate of electrocoagulation processes is greatly increased. The increased formation of bubbles, mixing, and mass transfer in the aqueous solution leads to a higher efficiency in removing dye [40]. A comparison of the EC procedure with EC-MOF (Figure 6b) revealed that the EC-MOF yielded superior results. The removal efficiency of the RB-5 dye was found to be 95.40%, 92.22%, and 75.02% at current densities of 23.15, 18.52, and 9.26 mA/cm\u003csup\u003e2\u003c/sup\u003e, respectively. The removal efficiency of RB-5 dye molecules decreased to 92.22% and 85.65% respectively. This reduction may be attributed to the sluggishness of electrocoagulation processes at the diminished current density [41]. Moreover, a decrease in the current value results in a diminished synthesis of coagulants within the solution, consequently leading to a decreased elimination of the dye due to the reduced anodic dissolution of Al ions.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.4. Effect of ZIF-67 dose\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe influence of the ZIF-67 dosage on the effectiveness of RB-5 removal was investigated within the range of 30\u0026ndash;50 mg. The results, as illustrated in Figure 7, demonstrate that the utilisation of a greater quantity of ZIF-67 as an adsorbent result in a significantly enhanced percentage of dye removal. At a dosage of 50 mg/L of ZIF-67, the decolorization efficiency reached its maximum value, equating to 95.9%. Lower dosages such as 40 mg/l and 30 mg/l of ZIF-67 results in the reduction of decolorization efficiencies which was equal to 82.2% and 76.2%, respectively. An increase in the quantity of adsorbent results in a greater availability of sorption sites, enhanced diffusion, and a larger, more accessible surface area. These characteristics contribute to the enhanced efficiency of dye removal when a high dosage of ZIF-67 is employed [41].\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.5. Effect of dye concentration\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe impact of the initial RB-5 concentration was investigated by modifying the concentration of the dye in solutions with starting concentration of 50 mg/l, 75 mg/l, and 100 mg/l. As was illustrated in Figure 8, the experimental results demonstrated a significant reduction of 95.54% in the dye concentration when the initial concentration was low. However, an inverse correlation between dye concentration and decolorization. The observed decrease in efficiency may be attributed to a modification in the proportion of dye molecules to the produced Al flocs and the active sites of ZIF-67 in the electro-coagulation coupled MOF treatment process, which in turn leads to a longer treatment time being necessary. The removal of the dye is somewhat restricted due to the existence of a certain quantity of aluminium hydroxide coagulants, generated at a given applied current density, and a defined number of accessible adsorption sites at a specific ZIF-67 dose [42]. Specially, when the concentrations were increased to 75 mg/l and 100 mg/l, the effectiveness of elimination reduced to 91.9% and 82.32%, respectively.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.6. Single and combined process comparison\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eA comparative study was conducted to evaluate the performance of stand-alone technologies, specifically EC and MOF-ZIF-67, in conjunction with a combined process, EC-MOF. The study was conducted under optimal conditions, specifically at a pH of 7, a dye concentration of 50 mg/l, and a ZIF-67 dose of 50 mg/l. The results (Figure 9) demonstrate that the combined process (EC-MOF) exhibits high dye elimination due to the synergistic effects. The dye elimination achieved in the ZIF-67 MOF adsorption process was only 46.2%, while the EC process showed up to 72.01% removal. However, the EC-MOF combined process boosted the removal efficiency to up to 95.40%. These findings demonstrate that the advantages of stand-alone technologies are coactively amplified in the combined process for the rapid degradation of organic pollutants.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.7. Reusability studies\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe catalyst\u0026apos;s lifespan and cost-effectiveness are largely contingent upon its reusability. The reusability of the ZIF-67 catalyst was investigated over three cycles in the MOF-EC process. Following the initial treatment cycle of the dye, the ZIF-67 was washed with ethanol and subjected to vacuum drying at 50\u0026deg;C for 24 hours [43]. Subsequently, the dried ZIF-67 was reused for a further treatment process up to three cycles. The removal efficiency achieved in the respective cycles was 98.9% in the first cycle, 92.3% in the second cycle, and 86.1% in the third cycle (see Figure 10). The insignificant drop in ZIF-67 activity in EC-MOF indicates stable performance and remarkable reusability.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003e3.9. Treatment of real textile effluent\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe real textile wastewater was initially characterized and subsequently treated byZIF-67 augmented electrocoagulation process at optimal parameters such as pH 7, current density 18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e and 50 mg dosage of ZIF-67 catalyst. The effective effluent treatment was achieved within a period of 30 minutes time. The ZIF-67 enhanced electrocoagulation process results in the removal of 42.23% COD, 39.10% BOD and 59.11% colour. The combined effect of eletro-flocs in the presence of ZIF-67 crystals lead to a significant enhancement in the elimination of pollutants. The pre and post treatment characterization of textile effluent is shown in Table 2.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eTable 2.\u003c/strong\u003e Characterization of the real wastewater containing RB-5 dye.\u003c/p\u003e\n\u003ctable border=\"1\" cellspacing=\"0\" cellpadding=\"0\" width=\"638\"\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eParameter\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u0026nbsp;Before Treatment\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e\u003cstrong\u003e\u0026nbsp;After Treatment\u0026nbsp;\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003epH\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e7.3\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eCOD (mg/L)\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e310\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e182\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eTDS (mg/L)\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e3800\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e890\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eBOD\u003csub\u003e5\u003c/sub\u003e\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e190\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e\u0026nbsp;131\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eTurbidity (NTU)\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003e7.85\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003e1.42\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd valign=\"top\" style=\"width: 241px;\"\u003e\n \u003cp\u003e\u003cstrong\u003eColour\u003c/strong\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 193px;\"\u003e\n \u003cp\u003eYellow\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd valign=\"top\" style=\"width: 205px;\"\u003e\n \u003cp\u003eColourless\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n\u003c/table\u003e\n\u003cp\u003e\u003cem\u003eCOD \u0026ndash; the\u0026nbsp;\u003c/em\u003e\u003cem\u003echemical oxygen demand\u003c/em\u003e\u003cem\u003e, TDS \u0026ndash; the total dissolved solid; BOD \u0026ndash; the\u0026nbsp;\u003c/em\u003e\u003cem\u003ebiochemical oxygen demand\u003c/em\u003e\u003cem\u003e; NTU \u0026ndash; the nephelometric turbidity units.\u0026nbsp;\u003c/em\u003e\u003c/p\u003e"},{"header":"4. Conclusions","content":"\u003cp\u003eThe findings of this research demonstrate the efficacy of the ZIF-67-aided\u0026nbsp;electrocoagulation\u0026nbsp;process for the treatment of textile wastewater. The comparative analysis of the processes revealed that the combined MOF-ZIF-67 process exhibited a notable enhancement in colour elimination compared to the standalone processes such as ZIF-67 and MOF. At the optimal pH of 7, current density of 18.52 mA/cm\u0026sup2;, 50 mg/l of ZIF-67, and a dye concentration of 50 mg/l, a colour elimination rate of 99% was achieved. The reusability study demonstrated the high efficiency of ZIF-67, with 80.3% removal achieved after the third cycle. The combined process demonstrated the elimination of colour in real wastewater up to 59.11%, COD removal 42.23 % and 39.10% BOD\u003csub\u003e5\u0026nbsp;\u003c/sub\u003ereduction. Consequently, the combined process exhibited a notable enhancement in performance in comparison to standalone technologies for the expeditious degradation of organic pollutants. Therefore, the electrocoagulation combined MOF process is an effective approach for wastewater remediation applications.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eCRediT authorship contribution statement\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eMuhammad Uzair:\u0026nbsp;\u003c/strong\u003eInvestigation, Methodology,Validation\u003cstrong\u003e,\u0026nbsp;\u003c/strong\u003eWriting—original draft preparation, Writing—review and editing,\u0026nbsp;\u003cstrong\u003eMuhammad Fahad Tariq:\u0026nbsp;\u003c/strong\u003eConceptualization, Data curation, Formal analysis, Methodology, Validation, Writing—original draft preparation, Writing—review and editing, Software, Visualization,\u003cstrong\u003e\u0026nbsp;Farhan Javed:\u0026nbsp;\u003c/strong\u003eSupervision,Conceptualization, Investigation, Resources, \u0026nbsp;Writing—original draft preparation, Writing—review and editing, Visualization Data curation, Validation, Writing—review and editing, Funding acquisition.\u0026nbsp;\u003cstrong\u003eMohammed Kadhom:\u0026nbsp;\u003c/strong\u003eMethodology, Validation, Writing—original draft preparation, Writing—review and editing, Software, Visualization.\u0026nbsp;\u003cstrong\u003eShakirullah:\u003c/strong\u003e Data curation, Formal analysis, Writing—review and editing, Visualization.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eDeclaration of Competing Interest\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors declare no competing financial interests or personal relationships that could influence the work reported in this paper.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAcknowledgments\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe authors acknowledge the financial support provided by HEC (NRPU-16521) and technical support by UET Lahore is gratefully acknowledged.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability statement\u0026nbsp;\u003c/strong\u003eAll relevant data are available in this paper.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eMasood, Z., et al., \u003cem\u003eApplication of nanocatalysts in advanced oxidation processes for wastewater purification: Challenges and future prospects.\u003c/em\u003e Catalysts, 2022. \u003cstrong\u003e12\u003c/strong\u003e(7): p. 741.\u003c/li\u003e\n\u003cli\u003eGadipelly, C., et al., \u003cem\u003ePharmaceutical industry wastewater: review of the technologies for water treatment and reuse.\u003c/em\u003e Industrial \u0026amp; Engineering Chemistry Research, 2014. \u003cstrong\u003e53\u003c/strong\u003e(29): p. 11571-11592.\u003c/li\u003e\n\u003cli\u003eRahmani, A., H. 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Water Treat, 2019. \u003cstrong\u003e166\u003c/strong\u003e: p. 83-91.\u003c/li\u003e\n\u003cli\u003eJaved, F., et al., \u003cem\u003eElimination of basic blue 9 by electrocoagulation coupled with pelletized natural dead leaves (Sapindus mukorossi) biosorption.\u003c/em\u003e International Journal of Phytoremediation, 2021. \u003cstrong\u003e23\u003c/strong\u003e(5): p. 462-473.\u003c/li\u003e\n\u003cli\u003eNoreen, N., et al., \u003cem\u003eTreatment of methylene blue in aqueous solution by electrocoagulation/micro-crystalline cellulosic adsorption combined process.\u003c/em\u003e Desalination and Water Treatment, 2020.\u003c/li\u003e\n\u003cli\u003eBayazıt, G., \u0026Uuml;.D.G. , and D. \u0026Uuml;nal, \u003cem\u003eBiosorption of Acid Red P-2BX by lichens as low cost biosorbents.\u003c/em\u003e International Journal of Environmental Studies.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":true,"highlight":"","institution":"","isAcceptedByJournal":false,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true},"keywords":"advanced oxidation process, electrocoagulation, metal organic framework, wastewater treatment, ZIF-67","lastPublishedDoi":"10.21203/rs.3.rs-7376258/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-7376258/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe persistent contamination of water bodies with toxic pollutants represents a significant challenge that requires appropriate treatment. This research investigated the potential of ZIF-67 augmented electrocoagulation l treatment for wastewater treatment. The investigation focused on key variables, including pH (5-9), current density (9.26-23.15 mA/cm\u003csup\u003e2\u003c/sup\u003e), ZIF-67 dose (30-50 mg/L), dye concentration (50-100 mg/L), and reusability. The results demonstrated a notable enhancement in the elimination of textile dye, with a significant increase from 82.32% to 95.40% observed in the electrocoagulation process when 50 mg/L of ZIF-67 was introduced. The maximum dye removal (up to 99 %) was achieved at the optimum parameters of pH 7, current density 18.52 mA/cm\u003csup\u003e2\u003c/sup\u003e, 50 mg/L ZIF-67, and 50 mg/L dye concentration, respectively, demonstrating efficient reusability. For real wastewater treatment, at optimal conditions, the chemical oxygen demand (COD), biological oxygen demand (BOD) and colour removals achieved were 42.21%, 39.10% and 59.11%, respectively. The research suggested that an electrocoagulation combined MOF process has the potential to be an effective method for the wastewater remediation.\u003c/p\u003e","manuscriptTitle":"A study on ZIF-67 augmented Electrocoagulation process for Wastewater Treatment","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2025-09-02 11:08:40","doi":"10.21203/rs.3.rs-7376258/v1","editorialEvents":[{"type":"communityComments","content":0}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"researchsquare","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":true,"externalIdentity":"","sideBox":"","snPcode":"","submissionUrl":"/submission","title":"Research Square","twitterHandle":"researchsquare","acdcEnabled":true,"dfaEnabled":false,"editorialSystem":"","reportingPortfolio":"","inReviewEnabled":false,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"62b40730-bf2a-45f5-a36b-d0ebd06c3e0e","owner":[],"postedDate":"September 2nd, 2025","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"posted","subjectAreas":[],"tags":[],"updatedAt":"2025-10-16T03:15:34+00:00","versionOfRecord":[],"versionCreatedAt":"2025-09-02 11:08:40","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-7376258","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-7376258","identity":"rs-7376258","version":["v1"]},"buildId":"8U1c8b4HqxoKbykW_rLl7","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}