Nanofiltration & Reverse Osmosis Technical Assessment for Pesticides Removal

Nanofiltration & Reverse Osmosis Technical Assessment for Pesticides Removal | 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 Case Report Nanofiltration & Reverse Osmosis Technical Assessment for Pesticides Removal Rubén Rodríguez-Alegre, Laura Pérez Megías, Sonia Sanchis, Carlos Andecochea Saiz, and 1 more This is a preprint; it has not been peer reviewed by a journal. https://doi.org/ 10.21203/rs.3.rs-3991503/v1 This work is licensed under a CC BY 4.0 License Status: Under Review Version 1 posted 7 You are reading this latest preprint version Abstract The increasing food demand for a growing population has resulted in the intensification and modernization of agriculture leading to an increasing use of pesticides to protect crops against insects, weeds, fungi, and other pests. However, these chemical compounds can cause adverse effects on the environment due to their low biodegradability and toxicity. This study assesses the use of DuPont FilmTec™ NF270 and FilmTec™ XLE membranes for the removal of six pesticides (atrazine, simazine, isoproturon, metolachlor ESA, 2,4-D, and chlorothalonil) in aqueous streams. The results reported average rejection rates of 29.25–89.36% and > 97% in the nanofiltration and reverse osmosis membranes respectively, showcasing that membrane technology is effective for the removal of these pollutants from wastewater streams. However, a customised selection of the membrane (nanofiltration/reverse osmosis) should be performed depending on the targeted pollutants in order to balance the pesticide rejection and energy consumption for each market application. Pesticides nanofiltration reverse osmosis membrane processes wastewater treatment Figures Figure 1 Figure 2 Figure 3 1. Introduction The growing global population, which could reach 9.7 billion people by 2050 according to United Nations data [ 1 ], poses a challenge for food production and supply chain. This has translated into the intensification of agricultural activities, both in terms of land expansion and the use of resources to maximize food production, including water, fertilizers, and pesticides, among others [ 2 , 3 ]. Pesticides, defined by the World Health Organization (WHO) as agents used to protect crops against insects, weeds, and fungi, are considered contaminants of emerging concern (CEC) [ 4 ] due to their complexity and low biodegradability. Pesticide application in agricultural soils has a great impact not only on the environment but on human health as well [ 5 ]. Once the pesticide is applied on the field, they have the potential to be transferred through adsorption, leaching, volatilization, and runoff [ 3 ]. At water level, as a result of their continuous use, thousands of different compounds originating from the use of these chemicals have been found in rivers, groundwater, and coastal areas worldwide, and their degradation gives place to another set of different compounds which can have diverse effects at different levels [ 6 , 7 ]. Besides, the uptake of these compounds by humans comes both from food and fresh water, producing several adverse effects such as asthma and respiratory affections, cancer, diabetes, and Parkinson’s disease, among others [ 8 ]. For this study, some of the most common pesticides have been selected. Atrazine and simazine belong to the group of triazines, widely used herbicides worldwide, which are currently under scrutiny due to water contamination, particularly for the immunotoxic effect of atrazine. Similarly, isoproturon is an herbicide known for its toxicity to organisms other than its intended targets [ 9 ]. Metolachlor ESA is an herbicide that has been extensively studied and shown to have negative effects on aquatic organisms [ 10 ]. 2,4-Dichlorophenoxyacetic acid (2,4-D) is the most widely used herbicide globally and a key component of various synthetic pesticides. Recent evidence has linked its presence in groundwater to cancer development [ 11 ]. Lastly, chlorothalonil is a broad-spectrum fungicide that has been used in agriculture for decades and has been banned in numerous countries in the recent past due to its carcinogenic potential [ 12 ]. Traditional wastewater treatment systems are not effective in the removal of pesticides and, given the hazardous nature of these compounds, the need to find new pathways to minimize their presence in the environment becomes imperative [ 13 ]. For decades, membrane processes have become a standard in the treatment of a wide range of liquid effluents with the aim of reducing their pollutant load in diverse sectors, including industrial, urban, and agricultural [ 14 ]. Size exclusion processes such as microfiltration (MF), ultrafiltration (UF), nanofiltration (NF), and reverse osmosis (RO) have been extensively studied, and their application in real environments has demonstrated outstanding results [ 15 ]. These technologies are also suitable for the treatment of streams containing emerging contaminants such as pesticides [ 16 ]. Specifically, among the aforementioned processes, nanofiltration, and reverse osmosis are the best suited for treating streams with pesticides, as they allow for their rejection due to their more restrictive cut-off [ 17 ], resulting in high-quality effluents [ 18 ]. In detail, nanofiltration membranes have a molecular weight cut-off ranging from 100 to 1000 Da. These membranes are usually targeted towards softening of water, being partially effective in removing dissolved ions [ 19 ]. Previous studies have reported pesticide removal efficiencies ranging from 30.00% to greater than 90.00% for phenylurea, phenoxyacetic acid, triazines, dithiolane pesticides organophosphate or synthetic auxin classes [ 20 – 24 ]. Meanwhile, reverse osmosis membranes have a molecular cut-off smaller than 100 Da [ 25 ] and are the standard on desalination processes. In this case, previous studies present pesticide retention rates ranging from 72.00% up to 98.00% in some pesticide families such as triazines, phenoxyacetic acid, organophosphates, conazoles or organochlorides [ 21 , 23 , 26 – 28 ]. Dupont has commercially a wide range of membranes for water treatment which can be used for pesticides removal. The FilmTec™ NF270 membrane is renowned for its ability to effectively remove contaminants at very low levels while allowing the passage of water and dissolved solutes, making it suitable for nanofiltration applications. On the other hand, the FilmTec™ XLE membrane is characterized by its high productivity and energy efficiency, making it suitable for reverse osmosis applications where reduced energy consumption is desired. Both membranes are highly regarded for their quality and performance, and are extensively utilized in potable water treatment, wastewater treatment, desalination, and various other water treatment applications [ 29 ]. Originally developed for applications such as desalination and wastewater treatment, these membranes have garnered widespread acclaim for their ability to effectively remove contaminants at minimal levels while facilitating the passage of water and dissolved solutes [ 30 ]. However, the application of these membranes for the removal of pesticides presents a compelling shift in their utilization. By harnessing their selective filtration properties, particularly noteworthy in the NF270 membrane, DuPont membranes offer a promising solution to the pressing issue of pesticide contamination in water sources. This strategic adaptation underscores the adaptability and efficacy of DuPont membranes, showcasing their potential to address emerging environmental challenges beyond conventional water treatment applications. This study aims to assess the performance of DuPont FilmTec™ NF270 and FilmTec™ XLE membranes for the removal of pesticides, namely atrazine, simazine, isoproturon, metholachlor ESA, 2,4-D, and chlorothalonil from a synthetic aqueous solution. Furthermore, a benchmark with previous works is presented to ease the decision making in membrane process application for this field. 2. Materials & Method 2.1. Reagents & equipment Synthetic solutions were prepared by using the studied six pesticides standards (see Table 1 ) provided by Sigma-Aldrich (Spain). The rejection tests of the NF and RO membranes were performed using MgSO 4 ·7H 2 O and NaCl provided by Scharlab (Spain). Table 1 Characteristics of the pesticides studied in the present work Pesticide Formula CAS number Molecular weigh (g mol − 1 ) Solubility (mg L − 1 ) Atrazine C 8 H 14 ClN 5 1912-24-9 215.68 33.00** Simazine C 7 H 12 ClN 5 122-34-9 201.66 6.20* Isoproturon C 12 H 18 N 2 O 34123-59-6 206.28 65.00** Metolachlor ESA C 15 H 22 NNaO 5 S 171118-09-5 329.40 530.00* 2,4-Dichlorophenoxyacetic acid C 8 H 6 Cl 2 O 3 94-75-7 221.04 667.00** Chlorothalonil C 8 Cl 4 N 2 1897-45-6 265.92 0.81** * Solubility in water at 20ºC ** Solubility in water at 25ºC The analysis of pesticides concentration was carried out by duplicate using High-Performance Liquid Chromatography coupled with a photodiode array and mass spectrometry system (ACQUITY UHPLC-PDA-SQ, Waters, Spain). The pesticide removal experiments were conducted in duplicate using two spiral-wound polyamide NF membranes (FilmTec™ NF270) and two polyamide brackish water RO membranes (FilmTec™ XLE), both provided in 1812 element format by DuPont Water Solutions (USA). The characteristics of both membranes are presented in Table 2 . These membranes were implemented in an SW-18 filtration plant (MMSX, Switzerland), operating in a tangential flow in batch mode. Table 2 Assessed membrane characteristics Parameter FilmTec™ NF270 FilmTec™ XLE Membrane process Nanofiltration Reverse osmosis Manufacturer DuPont DuPont Membrane material Piperazine based polyamide m-Phenylene diamine based polyamide Membrane configuration Spiral wound (1812) Spiral wound (1812) Active membrane area (m 2 ) 0.54 0.54 Permeate flow rate (LMH) 52.00 52.00 Minimum salts rejection (%) 97.00 (MgSO 4 ) 97.00 (NaCl) pH range 3.00–10.00 2.00–11.00 Maximum operating temperature (ºC) 45.00 45.00 Maximum operating pressure (Bar) 41.00 41.00 2.2. Filtration tests As feed water for the experiments, synthetic solutions were prepared by dissolving proper amounts of pesticides in deionised water for obtaining stock solutions containing 0.20 mg L − 1 atrazine, 0.20 mg L − 1 simazine, 0.20 mg L − 1 isoproturon, 0.20 mg L − 1 metolachlor ESA, 0.20 mg L − 1 2,4-D, and 0.40 mg L − 1 chlorothalonil. All solutions were prepared at 50°C with constant stirring for 5 h to ensure maximum solubilisation. Pesticides concentrations were selected according to HPLC quantification limit for each compound (0.01 mg L − 1 for atrazine, simazine, isoproturon and metolachlor ESA; 0.10 mg L − 1 for chlorothalonil) considering a maximum rejection rate of 99%. Firstly, membranes integrity tests were performed by replicating the working conditions reported in elements technical data sheet (see Table 3 ) and comparing salt rejection results. This stablishes a salts rejection reference value for each membrane capabilities. Afterwards, pesticides removal tests were carried out twice for each membrane (with fresh membrane and after a water wash) to assess their performance reproducibility. For pesticides removal tests, MgSO 4 and NaCl were added to the synthetic solution for NF and RO filtrations, respectively, for performing an additional assessment of salts rejection compared with the stablished reference value. A summary of the performed experiments and operating conditions are shown in Table 3 . The rejection of salts and pesticides (R) by the membranes was calculated using Eq. 1: \(R\left(\%\right)= \left(1-\frac{{C}_{p}}{{C}_{f}}\right)· 100\) Eq. 1 Where C p and C f are the concentrations of salts and pesticides in the permeate and the feed sample, respectively. 3. Results & Discussion In this study, the pesticide rejection capacity of nanofiltration and reverse osmosis membranes is evaluated to reduce the discharge of these contaminants into natural water bodies and wastewater treatment plants. 3.1. Salts rejection tests Initial salt tests showed an average salt rejection of 97.71 ± 0.03% and 95.22 ± 0.01% for NF270 and XLE, respectively. Although the experimental salt rejection was slightly lower than what is established by the supplier, the difference could be caused by some analytical deviations, but not to membrane deficiencies that would cause more significant differences. In addition, as can be seen in Fig. 1 , salt rejection during pesticide filtration tests remained quite constant and in range with what was obtained during membrane integrity tests. Therefore, by using this parameter as control, the good performance of the membranes can be assured, corroborating the reliability of the obtained pesticide rejection results. 3.2. Pesticides adsorption onto membranes surface After the first filtration with pesticides, mass balance assessment showed that solutes contained in permeate and retentate streams were significantly lower than in feed. This can be explained as some pesticides can be adsorbed onto the surface of membranes, as observed by Plakas & Karabelas (2008) and Nikbakht Fini et al. (2019). Therefore, feed solution was recirculated through the membranes until no pesticides concentration was observed in the feed solution in order to (i) equilibrate the membranes surface in terms of adsorption of pesticides and (ii) quantify the specific adsorption for each pesticide by using Eq. 2. \(A=\frac{{V}_{f}{C}_{f}-{V}_{p}{C}_{p}-{V}_{r}{C}_{r}}{S}\) (Eq. 2) Where A is the adsorption in mg of pesticides per m 2 of membrane, S is the membrane’s surface area in m 2 , V f , V p and V r are the volume of feed, permeate and retentate in L, respectively, and C f , C p and C r are the pesticides concentration in the feed, permeate and retentate in mg L − 1 , respectively. The specific adsorption of pesticides onto the surface of the membranes is shown in Fig. 2 . As reported in previous studies, the amount of adsorbed compounds on NF and RO membranes is strongly correlated with the relative membrane and pesticide hydrophobicity, but also with thin layer density [ 21 ]. Results for chlorothanolil are not shown since, due to its low solubility in water, it remained as solid particles in the solutions during membrane adsorption and rejection tests. As can be seen, both membranes reported pesticides adsorption, being the adsorption significantly greater when using NF270 than for XLE. This fact can be explained by NF and RO active layers being composed of piperazine-based polyamide and m-phenylene diamine-based polyamide, respectively, resulting in a higher hydrophobicity in the case of NF membrane, which promotes the adsorption of highly hydrophobic and low dipolar moment species. Although all studied substances have relatively similar octanol-water partition coefficients (log P) around 3 (2.61, 2.18, 2.90, 2.80 and 3.10 for atrazine, simazine, isoproturon, 2,4-D, and metolachlor, respectively), atrazine, simazine, and isoproturon reported significantly higher specific adsorption values. This fact can be explained by a lower dipolar moment compared with 2,4-D (O-H bond from the acidic group) and metolachlor (Cl-C bond). Moreover, according to Goh et al., (2022), substances low spatial complexity could also facilitate the adsorption onto membrane active surface. 3.3. Membrane filtration assessment for pesticides rejection Analysing the pesticides passage through the membrane (see Fig. 3 ), both NF270 and XLE membranes demonstrated the capability to partially reject the tested pesticides. Chlorothalonil, as mentioned in the previous section, appeared as suspended solids due to its low solubility in water, thus facilitating its rejection in both NF and RO membranes (> 99.90%). However, this fact difficulted its proper quantification by LC-MS, since samples must be filtered by a 0.45µm filter prior its analysis. By using NF270, the average passage rates obtained for atrazine, simazine, isoproturon, and 2,4-D were found to be 68.72 ± 0.05%, 70.76 ± 0.05%, 67.10 ± 0.04%, and 56.47 ± 0.04%, respectively. The relatively low rejection rates could be explained by the similarity of the pesticide’s molecular weight with the membrane's nominal molecular weight cut-off (200 Da), resulting in a partial rejection of these substances while a portion of these pesticides can be still found in the permeate stream. In the case of metolachlor ESA, it reported an average passage of 10.64 ± 0.01%, significantly lower than the rest of substances, due to its high molecular weight (329.40 g mol − 1 ), which facilitates its rejection by the nanofiltration membrane. The XLE reverse osmosis membrane demonstrated a higher capability to retain the tested pesticides, achieving up to 97.63% rejection in the case of 2,4-D. The average passage rates for all studied pesticides were found to be lower than 2.50%, resulting in a much lower pesticides concentration in permeate, potentially suitable for being further treated for pesticides degradation prior discharge. 3.4. Comparative study A comparison of the results obtained in the present study against previous works in terms of pesticides rejection using NF and RO membranes was done (Table 4 ). The efficiency of each treatment is presented as overall pesticide removal rate (%) for every work cited. Table 4 Previous works on pesticides removal using NF and RO Membrane process Reference Pesticides Removal rate (%) NF This work Atrazine, simazine, isoproturon, Metholachlor ESA, 2,4-D and chlorothalonil 29.25–89.36 [ 24 ] Atrazine & dimethoate 80.00–95.00 [ 21 ] Diuron & isoproturon 78.90–89.50 [ 23 ] (2-methyl-4-chlorophenoxy acetic acid (MCPA), 2-methyl-4-chlorophenoxy propionic acid, (MCPP), (2,6-dichlorobenzamide, (BAM) 30.00–82.00 [ 20 ] 2,4-D 97.00 [ 22 ] Atrazine & isoprothiolane 54.00–82.00 RO This work Atrazine, simazine, isoproturon, Metholachlor ESA, 2,4-D and chlorothalonil 97.64–99.99 [ 21 ] Cycluron > 95.00 [ 27 ] 158 pesticides 72.00–98.00 [ 23 ] (2-methyl-4-chlorophenoxy acetic acid (MCPA), 2-methyl-4-chlorophenoxy propionic acid, (MCPP), (2,6-dichlorobenzamide, (BAM) > 92.00 [ 26 ] Tributyl phosphate, irgarol, flutriafol & dicofol > 95.00 [ 28 ] 2-methyl-4-chlorophenoxyacetic acid (MCPA) 95.30 The NF membrane evaluated in the present study achieved a removal rate in the rage of 29.25–89.36% for the studied pesticides, due to their wide range of molecular weight. This result is in the range of the ones reported in previous studies, which are between 30.00 and 97.00%. The similar molecular weight of most of the studied pesticides with the tested membrane’s molecular weight cut-off allow the permeation of these compounds, which can be found in the permeate stream in small quantities. As can be observed in the previous table, NF reported partial rejection rates in almost all published studies; therefore, the technology is effective for pesticides which can be found as particles suspension or those with a medium molecular weight (> 300 Da). The RO membrane evaluated in the present study presented average removal rates between 97.64–99.99% for the different pesticides. This is slightly higher than some results reported in previous studies (72.00–98.00%). However, Fujioka et al., (2020) tested the RO rejection of a wide range of pesticides, including other ones with smaller molecular weight and chemical affinity (hydrophobicity), such as cycluron, carbendazim or aldicarb, which were also rejected. Almost all studies reported pesticides rejection > 90%, resulting in the presence of small quantities of pesticides in permeate, most of them below detection limit, which would potentially allow its direct discharge or with a smooth polishing treatment. 4. Conclusions In the present study, the rejection efficiency of a NF membrane (NF270) and a RO membrane (XLE) for the treatment of wastewater effluents containing pesticides has been investigated. The studied pesticides included atrazine, simazine, isoproturon, metolachlor ESA, 2,4-Dichlorophenoxyacetic acid, and chlorothalonil, widely used pesticides for crops and with toxic or carcinogenic effects on humans and the environment. Both membranes reported pesticides adsorption onto the polyamide active layer, which depends on substance’s hydrophobicity and dipolar moments. This should be considered for a proper assessment of pesticides rejection when a fresh membrane is used. However, there are only a few studies that assessed this phenomenon in depth, so it is important to perform more studies for stablishing a clear correlation between the membrane’s active layer material, substance’s physicochemical properties and their adsorption onto membranes. In the case of chlorothalonil, a full rejection was observed by using both NF and RO, since the compound was present in suspension due to its low solubility in water. Therefore, for those products that are delivered as suspension, ultrafiltration or microfiltration membranes could be assessed for its removal from wastewater effluents with lower energy consumption. Moreover, NF270 reported a wide range of rejection rates depending on the targeted pesticide, reporting efficient rejection for larger molecules (> 300 Da), while XLE filtration tests resulted in the rejection of > 95% for all the studied pesticides. Therefore, XLE can be used as efficient treatment for the rejection of pesticides in wastewaters. In this study, the feed solution contained higher pesticides concentration than the commonly present in agricultural leachates for proper quantification purposes, but further tests should be carried out considering lower concentration of these compounds for a better assessment of the membranes performance at relevant environment. Finally, the assessment of these membranes performance during a longer working period, integrating the implementation of a Clean-in-place (CIP) process should also be performed prior to the uptake of this technology at industrial scale. In this context, additional tests are required to optimize the utilization of these membranes on a real-scale basis by validating the technology using real waters. Declarations Acknowledgment This study was funded by DuPont Water Solutions and its Global Water Technology Center in Tarragona, Spain. Data availability The data supporting the findings of this study are available from the corresponding author. Competing interests. The authors declare no conflicts of interest. Author contribution statements Rubén Rodríguez-Alegre: in charge of conducting the analytical work, analyzing and interpreting the data, writing the first draft of the document: writing, reviewing, and editing – the original draft. Laura Pérez Megías: perform experiments; analytical work, to analyzing and interpreting the data, writing the first draft of the document: writing, reviewing, and editing – the original draft. Sonia Sanchis: editing & reviewing. 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Removal of herbicide 2-methyl-4-chlorophenoxyacetic acid (MCPA) from saline industrial wastewater by reverse osmosis and nanofiltration. Desalination 2020;496:114691. https://doi.org/10.1016/j.desal.2020.114691. Simonič M. Reverse Osmosis Treatment of Wastewater for Reuse as Process Water—A Case Study. Membranes 2021;11:976. https://doi.org/10.3390/membranes11120976. Massons G, Gilabert-Oriol G, Niewersch C. Nanofiltration innovation: performance of new DuPont TM FilmTec TM NF270-440 element in municipal wastewater operation. DWT 2023;309:149–53. https://doi.org/10.5004/dwt.2023.29886. Plakas KV, Karabelas AJ. Membrane retention of herbicides from single and multi-solute media: The effect of ionic environment. Journal of Membrane Science 2008;320:325–34. https://doi.org/10.1016/j.memsci.2008.04.016. Additional Declarations No competing interests reported. Cite Share Download PDF Status: Under Review Version 1 posted Editorial decision: Revision requested 02 Apr, 2024 Reviews received at journal 21 Mar, 2024 Reviewers agreed at journal 19 Mar, 2024 Reviewers invited by journal 19 Mar, 2024 Editor assigned by journal 14 Mar, 2024 Submission checks completed at journal 14 Mar, 2024 First submitted to journal 26 Feb, 2024 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. As a division of Research Square Company, we’re committed to making research communication faster, fairer, and more useful. We do this by developing innovative software and high quality services for the global research community. Our growing team is made up of researchers and industry professionals working together to solve the most critical problems facing scientific publishing. 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-3991503","acceptedTermsAndConditions":true,"allowDirectSubmit":false,"archivedVersions":[],"articleType":"Case Report","associatedPublications":[],"authors":[{"id":279492132,"identity":"a7964d29-e3a9-4ada-89a4-831d0cb9e856","order_by":0,"name":"Rubén Rodríguez-Alegre","email":"","orcid":"","institution":"Leitat Technological Center","correspondingAuthor":false,"prefix":"","firstName":"Rubén","middleName":"","lastName":"Rodríguez-Alegre","suffix":""},{"id":279492134,"identity":"3b18346a-248f-4737-ae01-15bfc045717d","order_by":1,"name":"Laura Pérez Megías","email":"","orcid":"","institution":"Leitat Technological Center","correspondingAuthor":false,"prefix":"","firstName":"Laura","middleName":"Pérez","lastName":"Megías","suffix":""},{"id":279492136,"identity":"a12ea968-1458-4b16-8b5b-27f1ddf02422","order_by":2,"name":"Sonia Sanchis","email":"","orcid":"","institution":"Leitat Technological Center","correspondingAuthor":false,"prefix":"","firstName":"Sonia","middleName":"","lastName":"Sanchis","suffix":""},{"id":279492137,"identity":"2fbb9dcf-3973-4264-9906-5ba3afeef159","order_by":3,"name":"Carlos Andecochea Saiz","email":"","orcid":"","institution":"Leitat Technological Center","correspondingAuthor":false,"prefix":"","firstName":"Carlos","middleName":"Andecochea","lastName":"Saiz","suffix":""},{"id":279492139,"identity":"9f14f903-890b-4fea-b107-c48af57dd6f8","order_by":4,"name":"Xialei You","email":"data:image/png;base64,iVBORw0KGgoAAAANSUhEUgAAAZAAAAAyAQMAAABI0h/eAAAABlBMVEX///8AAABVwtN+AAAACXBIWXMAAA7EAAAOxAGVKw4bAAAAu0lEQVRIiWNgGAWjYLCCDwUMPKTpYJxhwMDDw8BMghZmHgMGBuK1GNxIPiZtY2AjY89+/gDDxz21hLVIzkhLk84xSOPh4UkGuvDZccJa+CVyzIBaDgP9kgx04YFjhLWwgbRYGPzn4eF/TKQWsC0MBgd4eCTAttQQ4ZeeZ8mWPQbJPDw3HhscnHHgAGEtBseTD974UWFnz96f+PDBhwN1hLUwCCQg2EArDhOhhR/VKcTYMgpGwSgYBSMNAADa5DEj4lNxRwAAAABJRU5ErkJggg==","orcid":"","institution":"Leitat Technological Center","correspondingAuthor":true,"prefix":"","firstName":"Xialei","middleName":"","lastName":"You","suffix":""}],"badges":[],"createdAt":"2024-02-26 17:01:13","currentVersionCode":1,"declarations":"","doi":"10.21203/rs.3.rs-3991503/v1","doiUrl":"https://doi.org/10.21203/rs.3.rs-3991503/v1","draftVersion":[],"editorialEvents":[],"editorialNote":"","failedWorkflow":false,"files":[{"id":52924073,"identity":"5c5b1793-f148-479a-b59c-0facebdabc40","added_by":"auto","created_at":"2024-03-18 17:49:05","extension":"png","order_by":1,"title":"Figure 1","display":"","copyAsset":false,"role":"figure","size":9611,"visible":true,"origin":"","legend":"\u003cp\u003eSalts rejection assessment in the presence of pesticide (light shade) and without pesticide (drak shade) for NF270 and XLE\u003c/p\u003e","description":"","filename":"1.png","url":"https://assets-eu.researchsquare.com/files/rs-3991503/v1/3f7d9f9e3963b55eda0fd4a6.png"},{"id":52924072,"identity":"db2cf26e-25b1-40f5-875d-93cb45fbcaa7","added_by":"auto","created_at":"2024-03-18 17:49:05","extension":"png","order_by":2,"title":"Figure 2","display":"","copyAsset":false,"role":"figure","size":11581,"visible":true,"origin":"","legend":"\u003cp\u003ePesticides adsorption onto membranes Surface for NF270 (dark shade) and XLE (light shade)\u003c/p\u003e","description":"","filename":"2.png","url":"https://assets-eu.researchsquare.com/files/rs-3991503/v1/acdfa3542ae8996fddad6223.png"},{"id":52924071,"identity":"3585129e-dfc9-4005-882d-4349a65a997b","added_by":"auto","created_at":"2024-03-18 17:49:05","extension":"png","order_by":3,"title":"Figure 3","display":"","copyAsset":false,"role":"figure","size":12341,"visible":true,"origin":"","legend":"\u003cp\u003ePesticides passage through the NF270 membrane (dark shade) and XLE membrane (light shade)\u003c/p\u003e","description":"","filename":"3.png","url":"https://assets-eu.researchsquare.com/files/rs-3991503/v1/48b58dd40a2b01c9bf31235f.png"},{"id":52924908,"identity":"0f0eb4ef-cb1e-4952-90a0-10801e269667","added_by":"auto","created_at":"2024-03-18 17:57:06","extension":"pdf","order_by":0,"title":"","display":"","copyAsset":false,"role":"manuscript-pdf","size":362029,"visible":true,"origin":"","legend":"","description":"","filename":"manuscript.pdf","url":"https://assets-eu.researchsquare.com/files/rs-3991503/v1/2e4fe8ca-c742-4e54-9e69-e815208e1e85.pdf"}],"financialInterests":"No competing interests reported.","formattedTitle":"Nanofiltration \u0026 Reverse Osmosis Technical Assessment for Pesticides Removal","fulltext":[{"header":"1. Introduction","content":"\u003cp\u003eThe growing global population, which could reach 9.7\u0026nbsp;billion people by 2050 according to United Nations data [\u003cspan citationid=\"CR1\" class=\"CitationRef\"\u003e1\u003c/span\u003e], poses a challenge for food production and supply chain. This has translated into the intensification of agricultural activities, both in terms of land expansion and the use of resources to maximize food production, including water, fertilizers, and pesticides, among others [\u003cspan citationid=\"CR2\" class=\"CitationRef\"\u003e2\u003c/span\u003e, \u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e].\u003c/p\u003e \u003cp\u003ePesticides, defined by the World Health Organization (WHO) as agents used to protect crops against insects, weeds, and fungi, are considered contaminants of emerging concern (CEC) [\u003cspan citationid=\"CR4\" class=\"CitationRef\"\u003e4\u003c/span\u003e] due to their complexity and low biodegradability. Pesticide application in agricultural soils has a great impact not only on the environment but on human health as well [\u003cspan citationid=\"CR5\" class=\"CitationRef\"\u003e5\u003c/span\u003e]. Once the pesticide is applied on the field, they have the potential to be transferred through adsorption, leaching, volatilization, and runoff [\u003cspan citationid=\"CR3\" class=\"CitationRef\"\u003e3\u003c/span\u003e]. At water level, as a result of their continuous use, thousands of different compounds originating from the use of these chemicals have been found in rivers, groundwater, and coastal areas worldwide, and their degradation gives place to another set of different compounds which can have diverse effects at different levels [\u003cspan citationid=\"CR6\" class=\"CitationRef\"\u003e6\u003c/span\u003e, \u003cspan citationid=\"CR7\" class=\"CitationRef\"\u003e7\u003c/span\u003e]. Besides, the uptake of these compounds by humans comes both from food and fresh water, producing several adverse effects such as asthma and respiratory affections, cancer, diabetes, and Parkinson\u0026rsquo;s disease, among others [\u003cspan citationid=\"CR8\" class=\"CitationRef\"\u003e8\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eFor this study, some of the most common pesticides have been selected. Atrazine and simazine belong to the group of triazines, widely used herbicides worldwide, which are currently under scrutiny due to water contamination, particularly for the immunotoxic effect of atrazine. Similarly, isoproturon is an herbicide known for its toxicity to organisms other than its intended targets [\u003cspan citationid=\"CR9\" class=\"CitationRef\"\u003e9\u003c/span\u003e]. Metolachlor ESA is an herbicide that has been extensively studied and shown to have negative effects on aquatic organisms [\u003cspan citationid=\"CR10\" class=\"CitationRef\"\u003e10\u003c/span\u003e]. 2,4-Dichlorophenoxyacetic acid (2,4-D) is the most widely used herbicide globally and a key component of various synthetic pesticides. Recent evidence has linked its presence in groundwater to cancer development [\u003cspan citationid=\"CR11\" class=\"CitationRef\"\u003e11\u003c/span\u003e]. Lastly, chlorothalonil is a broad-spectrum fungicide that has been used in agriculture for decades and has been banned in numerous countries in the recent past due to its carcinogenic potential [\u003cspan citationid=\"CR12\" class=\"CitationRef\"\u003e12\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eTraditional wastewater treatment systems are not effective in the removal of pesticides and, given the hazardous nature of these compounds, the need to find new pathways to minimize their presence in the environment becomes imperative [\u003cspan citationid=\"CR13\" class=\"CitationRef\"\u003e13\u003c/span\u003e]. For decades, membrane processes have become a standard in the treatment of a wide range of liquid effluents with the aim of reducing their pollutant load in diverse sectors, including industrial, urban, and agricultural [\u003cspan citationid=\"CR14\" class=\"CitationRef\"\u003e14\u003c/span\u003e]. Size exclusion processes such as microfiltration (MF), ultrafiltration (UF), nanofiltration (NF), and reverse osmosis (RO) have been extensively studied, and their application in real environments has demonstrated outstanding results [\u003cspan citationid=\"CR15\" class=\"CitationRef\"\u003e15\u003c/span\u003e]. These technologies are also suitable for the treatment of streams containing emerging contaminants such as pesticides [\u003cspan citationid=\"CR16\" class=\"CitationRef\"\u003e16\u003c/span\u003e]. Specifically, among the aforementioned processes, nanofiltration, and reverse osmosis are the best suited for treating streams with pesticides, as they allow for their rejection due to their more restrictive cut-off [\u003cspan citationid=\"CR17\" class=\"CitationRef\"\u003e17\u003c/span\u003e], resulting in high-quality effluents [\u003cspan citationid=\"CR18\" class=\"CitationRef\"\u003e18\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eIn detail, nanofiltration membranes have a molecular weight cut-off ranging from 100 to 1000 Da. These membranes are usually targeted towards softening of water, being partially effective in removing dissolved ions [\u003cspan citationid=\"CR19\" class=\"CitationRef\"\u003e19\u003c/span\u003e]. Previous studies have reported pesticide removal efficiencies ranging from 30.00% to greater than 90.00% for phenylurea, phenoxyacetic acid, triazines, dithiolane pesticides organophosphate or synthetic auxin classes [\u003cspan additionalcitationids=\"CR21 CR22 CR23\" citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]. Meanwhile, reverse osmosis membranes have a molecular cut-off smaller than 100 Da [\u003cspan citationid=\"CR25\" class=\"CitationRef\"\u003e25\u003c/span\u003e] and are the standard on desalination processes. In this case, previous studies present pesticide retention rates ranging from 72.00% up to 98.00% in some pesticide families such as triazines, phenoxyacetic acid, organophosphates, conazoles or organochlorides [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e, \u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e, \u003cspan additionalcitationids=\"CR27\" citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e\u0026ndash;\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eDupont has commercially a wide range of membranes for water treatment which can be used for pesticides removal. The FilmTec\u0026trade; NF270 membrane is renowned for its ability to effectively remove contaminants at very low levels while allowing the passage of water and dissolved solutes, making it suitable for nanofiltration applications. On the other hand, the FilmTec\u0026trade; XLE membrane is characterized by its high productivity and energy efficiency, making it suitable for reverse osmosis applications where reduced energy consumption is desired. Both membranes are highly regarded for their quality and performance, and are extensively utilized in potable water treatment, wastewater treatment, desalination, and various other water treatment applications [\u003cspan citationid=\"CR29\" class=\"CitationRef\"\u003e29\u003c/span\u003e].\u003c/p\u003e \u003cp\u003eOriginally developed for applications such as desalination and wastewater treatment, these membranes have garnered widespread acclaim for their ability to effectively remove contaminants at minimal levels while facilitating the passage of water and dissolved solutes [\u003cspan citationid=\"CR30\" class=\"CitationRef\"\u003e30\u003c/span\u003e]. However, the application of these membranes for the removal of pesticides presents a compelling shift in their utilization. By harnessing their selective filtration properties, particularly noteworthy in the NF270 membrane, DuPont membranes offer a promising solution to the pressing issue of pesticide contamination in water sources. This strategic adaptation underscores the adaptability and efficacy of DuPont membranes, showcasing their potential to address emerging environmental challenges beyond conventional water treatment applications.\u003c/p\u003e \u003cp\u003eThis study aims to assess the performance of DuPont FilmTec\u0026trade; NF270 and FilmTec\u0026trade; XLE membranes for the removal of pesticides, namely atrazine, simazine, isoproturon, metholachlor ESA, 2,4-D, and chlorothalonil from a synthetic aqueous solution. Furthermore, a benchmark with previous works is presented to ease the decision making in membrane process application for this field.\u003c/p\u003e"},{"header":"2. Materials \u0026 Method","content":"\u003cdiv id=\"Sec3\"\u003e\n \u003ch2\u003e2.1. Reagents \u0026amp; equipment\u003c/h2\u003e\n \u003cp\u003eSynthetic solutions were prepared by using the studied six pesticides standards (see Table \u003cspan\u003e1\u003c/span\u003e) provided by Sigma-Aldrich (Spain). The rejection tests of the NF and RO membranes were performed using MgSO\u003csub\u003e4\u003c/sub\u003e\u0026middot;7H\u003csub\u003e2\u003c/sub\u003eO and NaCl provided by Scharlab (Spain).\u003c/p\u003e\n \u003cdiv\u003e\n \u003ctable id=\"Tab1\" border=\"1\"\u003e\n \u003ccaption language=\"En\"\u003e\n \u003cdiv\u003eTable 1\u003c/div\u003e\n \u003cdiv\u003e\n \u003cp\u003eCharacteristics of the pesticides studied in the present work\u003c/p\u003e\n \u003c/div\u003e\n \u003c/caption\u003e\n \u003ccolgroup cols=\"5\"\u003e\u003c/colgroup\u003e\n \u003cthead\u003e\n \u003ctr\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003ePesticide\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eFormula\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eCAS number\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eMolecular weigh\u003c/p\u003e\n \u003cp\u003e(g mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eSolubility\u003c/p\u003e\n \u003cp\u003e(mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e)\u003c/p\u003e\n \u003c/th\u003e\n \u003c/tr\u003e\n \u003c/thead\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eAtrazine\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e8\u003c/sub\u003eH\u003csub\u003e14\u003c/sub\u003eClN\u003csub\u003e5\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e1912-24-9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e215.68\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e33.00**\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eSimazine\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e7\u003c/sub\u003eH\u003csub\u003e12\u003c/sub\u003eClN\u003csub\u003e5\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e122-34-9\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e201.66\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e6.20*\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eIsoproturon\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e12\u003c/sub\u003eH\u003csub\u003e18\u003c/sub\u003eN\u003csub\u003e2\u003c/sub\u003eO\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e34123-59-6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e206.28\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e65.00**\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMetolachlor ESA\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e15\u003c/sub\u003eH\u003csub\u003e22\u003c/sub\u003eNNaO\u003csub\u003e5\u003c/sub\u003eS\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e171118-09-5\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e329.40\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e530.00*\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e2,4-Dichlorophenoxyacetic acid\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e8\u003c/sub\u003eH\u003csub\u003e6\u003c/sub\u003eCl\u003csub\u003e2\u003c/sub\u003eO\u003csub\u003e3\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e94-75-7\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e221.04\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e667.00**\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eChlorothalonil\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eC\u003csub\u003e8\u003c/sub\u003eCl\u003csub\u003e4\u003c/sub\u003eN\u003csub\u003e2\u003c/sub\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e1897-45-6\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e265.92\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e0.81**\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\" colspan=\"5\"\u003e\n \u003cp\u003e* Solubility in water at 20\u0026ordm;C\u003c/p\u003e\n \u003cp\u003e** Solubility in water at 25\u0026ordm;C\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n \u003c/div\u003e\n \u003cp\u003eThe analysis of pesticides concentration was carried out by duplicate using High-Performance Liquid Chromatography coupled with a photodiode array and mass spectrometry system (ACQUITY UHPLC-PDA-SQ, Waters, Spain).\u003c/p\u003e\n \u003cp\u003eThe pesticide removal experiments were conducted in duplicate using two spiral-wound polyamide NF membranes (FilmTec\u0026trade; NF270) and two polyamide brackish water RO membranes (FilmTec\u0026trade; XLE), both provided in 1812 element format by DuPont Water Solutions (USA). The characteristics of both membranes are presented in Table \u003cspan\u003e2\u003c/span\u003e. These membranes were implemented in an SW-18 filtration plant (MMSX, Switzerland), operating in a tangential flow in batch mode.\u003c/p\u003e\n \u003cdiv\u003e\n \u003ctable id=\"Tab2\" border=\"1\"\u003e\n \u003ccaption language=\"En\"\u003e\n \u003cdiv\u003eTable 2\u003c/div\u003e\n \u003cdiv\u003e\n \u003cp\u003eAssessed membrane characteristics\u003c/p\u003e\n \u003c/div\u003e\n \u003c/caption\u003e\n \u003ccolgroup cols=\"3\"\u003e\u003c/colgroup\u003e\n \u003cthead\u003e\n \u003ctr\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eParameter\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eFilmTec\u0026trade; NF270\u003c/p\u003e\n \u003c/th\u003e\n \u003cth align=\"left\"\u003e\n \u003cp\u003eFilmTec\u0026trade; XLE\u003c/p\u003e\n \u003c/th\u003e\n \u003c/tr\u003e\n \u003c/thead\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMembrane process\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eNanofiltration\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eReverse osmosis\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eManufacturer\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eDuPont\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eDuPont\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMembrane material\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003ePiperazine based polyamide\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003em-Phenylene diamine based polyamide\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMembrane configuration\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eSpiral wound (1812)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eSpiral wound (1812)\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eActive membrane area (m\u003csup\u003e2\u003c/sup\u003e)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e0.54\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e0.54\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003ePermeate flow rate (LMH)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e52.00\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e52.00\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMinimum salts rejection (%)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e97.00 (MgSO\u003csub\u003e4\u003c/sub\u003e)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e97.00 (NaCl)\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003epH range\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e3.00\u0026ndash;10.00\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e2.00\u0026ndash;11.00\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMaximum operating temperature (\u0026ordm;C)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e45.00\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e45.00\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eMaximum operating pressure (Bar)\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e41.00\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e41.00\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n \u003c/div\u003e\n\u003c/div\u003e\n\u003cdiv id=\"Sec4\"\u003e\n \u003ch2\u003e2.2. Filtration tests\u003c/h2\u003e\n \u003cp\u003eAs feed water for the experiments, synthetic solutions were prepared by dissolving proper amounts of pesticides in deionised water for obtaining stock solutions containing 0.20 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e atrazine, 0.20 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e simazine, 0.20 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e isoproturon, 0.20 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e metolachlor ESA, 0.20 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e 2,4-D, and 0.40 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e chlorothalonil. All solutions were prepared at 50\u0026deg;C with constant stirring for 5 h to ensure maximum solubilisation. Pesticides concentrations were selected according to HPLC quantification limit for each compound (0.01 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for atrazine, simazine, isoproturon and metolachlor ESA; 0.10 mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e for chlorothalonil) considering a maximum rejection rate of 99%.\u003c/p\u003e\n \u003cp\u003eFirstly, membranes integrity tests were performed by replicating the working conditions reported in elements technical data sheet (see Table \u003cspan\u003e3\u003c/span\u003e) and comparing salt rejection results. This stablishes a salts rejection reference value for each membrane capabilities. Afterwards, pesticides removal tests were carried out twice for each membrane (with fresh membrane and after a water wash) to assess their performance reproducibility. For pesticides removal tests, MgSO\u003csub\u003e4\u003c/sub\u003e and NaCl were added to the synthetic solution for NF and RO filtrations, respectively, for performing an additional assessment of salts rejection compared with the stablished reference value. A summary of the performed experiments and operating conditions are shown in Table \u003cspan\u003e3\u003c/span\u003e.\u003c/p\u003e\n \u003cdiv\u003e\n \u003ctable id=\"Tab3\" border=\"1\"\u003e\u003c/table\u003e\n \u003c/div\u003e\n \u003cp\u003e\u003cimg src=\"https://myfiles.space/user_files/122228_c8a1650c59388082/122228_custom_files/img1710760001.png\"\u003e\u003cbr\u003e\u003c/p\u003e\n \u003cp\u003eThe rejection of salts and pesticides (R) by the membranes was calculated using Eq. 1:\u003c/p\u003e\n \u003cdiv\u003e\n \u003ctable id=\"Taba\" border=\"1\"\u003e\n \u003ccolgroup cols=\"2\"\u003e\u003c/colgroup\u003e\n \u003ctbody\u003e\n \u003ctr\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003e\u003cspan\u003e\u003cspan\u003e\\(R\\left(\\%\\right)= \\left(1-\\frac{{C}_{p}}{{C}_{f}}\\right)\u0026middot; 100\\)\u003c/span\u003e\u003c/span\u003e\u003c/p\u003e\n \u003c/td\u003e\n \u003ctd align=\"left\"\u003e\n \u003cp\u003eEq.\u0026nbsp;1\u003c/p\u003e\n \u003c/td\u003e\n \u003c/tr\u003e\n \u003c/tbody\u003e\n \u003c/table\u003e\n \u003c/div\u003e\n \u003cp\u003eWhere C\u003csub\u003ep\u003c/sub\u003e and C\u003csub\u003ef\u003c/sub\u003e are the concentrations of salts and pesticides in the permeate and the feed sample, respectively.\u003c/p\u003e\n\u003c/div\u003e"},{"header":"3. Results \u0026 Discussion","content":"\u003cp\u003eIn this study, the pesticide rejection capacity of nanofiltration and reverse osmosis membranes is evaluated to reduce the discharge of these contaminants into natural water bodies and wastewater treatment plants.\u003c/p\u003e \u003cdiv id=\"Sec6\" class=\"Section2\"\u003e \u003ch2\u003e3.1. Salts rejection tests\u003c/h2\u003e \u003cp\u003eInitial salt tests showed an average salt rejection of 97.71\u0026thinsp;\u0026plusmn;\u0026thinsp;0.03% and 95.22\u0026thinsp;\u0026plusmn;\u0026thinsp;0.01% for NF270 and XLE, respectively. Although the experimental salt rejection was slightly lower than what is established by the supplier, the difference could be caused by some analytical deviations, but not to membrane deficiencies that would cause more significant differences.\u003c/p\u003e \u003cp\u003eIn addition, as can be seen in Fig.\u0026nbsp;\u003cspan refid=\"Fig1\" class=\"InternalRef\"\u003e1\u003c/span\u003e, salt rejection during pesticide filtration tests remained quite constant and in range with what was obtained during membrane integrity tests. Therefore, by using this parameter as control, the good performance of the membranes can be assured, corroborating the reliability of the obtained pesticide rejection results.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec7\" class=\"Section2\"\u003e \u003ch2\u003e3.2. Pesticides adsorption onto membranes surface\u003c/h2\u003e \u003cp\u003eAfter the first filtration with pesticides, mass balance assessment showed that solutes contained in permeate and retentate streams were significantly lower than in feed. This can be explained as some pesticides can be adsorbed onto the surface of membranes, as observed by Plakas \u0026amp; Karabelas (2008) and Nikbakht Fini et al. (2019).\u003c/p\u003e \u003cp\u003eTherefore, feed solution was recirculated through the membranes until no pesticides concentration was observed in the feed solution in order to (i) equilibrate the membranes surface in terms of adsorption of pesticides and (ii) quantify the specific adsorption for each pesticide by using Eq.\u0026nbsp;2.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"No\" id=\"Tabb\" border=\"1\"\u003e \u003ccolgroup cols=\"2\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\"\u003e \u003cp\u003e\u003cspan class=\"InlineEquation\"\u003e\u003cspan class=\"mathinline\"\u003e\\(A=\\frac{{V}_{f}{C}_{f}-{V}_{p}{C}_{p}-{V}_{r}{C}_{r}}{S}\\)\u003c/span\u003e\u003c/span\u003e\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e(Eq.\u0026nbsp;2)\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eWhere A is the adsorption in mg of pesticides per m\u003csup\u003e2\u003c/sup\u003e of membrane, S is the membrane\u0026rsquo;s surface area in m\u003csup\u003e2\u003c/sup\u003e, V\u003csub\u003ef\u003c/sub\u003e, V\u003csub\u003ep\u003c/sub\u003e and V\u003csub\u003er\u003c/sub\u003e are the volume of feed, permeate and retentate in L, respectively, and C\u003csub\u003ef\u003c/sub\u003e, C\u003csub\u003ep\u003c/sub\u003e and C\u003csub\u003er\u003c/sub\u003e are the pesticides concentration in the feed, permeate and retentate in mg L\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e, respectively.\u003c/p\u003e \u003cp\u003eThe specific adsorption of pesticides onto the surface of the membranes is shown in Fig.\u0026nbsp;\u003cspan refid=\"Fig2\" class=\"InternalRef\"\u003e2\u003c/span\u003e. As reported in previous studies, the amount of adsorbed compounds on NF and RO membranes is strongly correlated with the relative membrane and pesticide hydrophobicity, but also with thin layer density [\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]. Results for chlorothanolil are not shown since, due to its low solubility in water, it remained as solid particles in the solutions during membrane adsorption and rejection tests.\u003c/p\u003e \u003cp\u003eAs can be seen, both membranes reported pesticides adsorption, being the adsorption significantly greater when using NF270 than for XLE. This fact can be explained by NF and RO active layers being composed of piperazine-based polyamide and m-phenylene diamine-based polyamide, respectively, resulting in a higher hydrophobicity in the case of NF membrane, which promotes the adsorption of highly hydrophobic and low dipolar moment species.\u003c/p\u003e \u003cp\u003eAlthough all studied substances have relatively similar octanol-water partition coefficients (log P) around 3 (2.61, 2.18, 2.90, 2.80 and 3.10 for atrazine, simazine, isoproturon, 2,4-D, and metolachlor, respectively), atrazine, simazine, and isoproturon reported significantly higher specific adsorption values. This fact can be explained by a lower dipolar moment compared with 2,4-D (O-H bond from the acidic group) and metolachlor (Cl-C bond). Moreover, according to Goh et al., (2022), substances low spatial complexity could also facilitate the adsorption onto membrane active surface.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec8\" class=\"Section2\"\u003e \u003ch2\u003e3.3. Membrane filtration assessment for pesticides rejection\u003c/h2\u003e \u003cp\u003eAnalysing the pesticides passage through the membrane (see Fig.\u0026nbsp;\u003cspan refid=\"Fig3\" class=\"InternalRef\"\u003e3\u003c/span\u003e), both NF270 and XLE membranes demonstrated the capability to partially reject the tested pesticides. Chlorothalonil, as mentioned in the previous section, appeared as suspended solids due to its low solubility in water, thus facilitating its rejection in both NF and RO membranes (\u0026gt;\u0026thinsp;99.90%). However, this fact difficulted its proper quantification by LC-MS, since samples must be filtered by a 0.45\u0026micro;m filter prior its analysis.\u003c/p\u003e \u003cp\u003e \u003c/p\u003e \u003cp\u003eBy using NF270, the average passage rates obtained for atrazine, simazine, isoproturon, and 2,4-D were found to be 68.72\u0026thinsp;\u0026plusmn;\u0026thinsp;0.05%, 70.76\u0026thinsp;\u0026plusmn;\u0026thinsp;0.05%, 67.10\u0026thinsp;\u0026plusmn;\u0026thinsp;0.04%, and 56.47\u0026thinsp;\u0026plusmn;\u0026thinsp;0.04%, respectively. The relatively low rejection rates could be explained by the similarity of the pesticide\u0026rsquo;s molecular weight with the membrane's nominal molecular weight cut-off (200 Da), resulting in a partial rejection of these substances while a portion of these pesticides can be still found in the permeate stream. In the case of metolachlor ESA, it reported an average passage of 10.64\u0026thinsp;\u0026plusmn;\u0026thinsp;0.01%, significantly lower than the rest of substances, due to its high molecular weight (329.40 g mol\u003csup\u003e\u0026minus;\u0026thinsp;1\u003c/sup\u003e), which facilitates its rejection by the nanofiltration membrane.\u003c/p\u003e \u003cp\u003eThe XLE reverse osmosis membrane demonstrated a higher capability to retain the tested pesticides, achieving up to 97.63% rejection in the case of 2,4-D. The average passage rates for all studied pesticides were found to be lower than 2.50%, resulting in a much lower pesticides concentration in permeate, potentially suitable for being further treated for pesticides degradation prior discharge.\u003c/p\u003e \u003c/div\u003e \u003cdiv id=\"Sec9\" class=\"Section2\"\u003e \u003ch2\u003e3.4. Comparative study\u003c/h2\u003e \u003cp\u003eA comparison of the results obtained in the present study against previous works in terms of pesticides rejection using NF and RO membranes was done (Table\u0026nbsp;\u003cspan refid=\"Tab4\" class=\"InternalRef\"\u003e4\u003c/span\u003e). The efficiency of each treatment is presented as overall pesticide removal rate (%) for every work cited.\u003c/p\u003e \u003cp\u003e \u003cdiv class=\"gridtable\"\u003e\u003ctable float=\"Yes\" id=\"Tab4\" border=\"1\"\u003e \u003ccaption language=\"En\"\u003e \u003cdiv class=\"CaptionNumber\"\u003eTable 4\u003c/div\u003e \u003cdiv class=\"CaptionContent\"\u003e \u003cp\u003ePrevious works on pesticides removal using NF and RO\u003c/p\u003e \u003c/div\u003e \u003c/caption\u003e \u003ccolgroup cols=\"4\"\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c1\" colnum=\"1\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c2\" colnum=\"2\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c3\" colnum=\"3\"\u003e\u003c/div\u003e \u003cdiv align=\"left\" class=\"colspec\" colname=\"c4\" colnum=\"4\"\u003e\u003c/div\u003e \u003cthead\u003e \u003ctr\u003e \u003cth align=\"left\" colname=\"c1\"\u003e \u003cp\u003eMembrane process\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c2\"\u003e \u003cp\u003eReference\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c3\"\u003e \u003cp\u003ePesticides\u003c/p\u003e \u003c/th\u003e \u003cth align=\"left\" colname=\"c4\"\u003e \u003cp\u003eRemoval rate (%)\u003c/p\u003e \u003c/th\u003e \u003c/tr\u003e \u003c/thead\u003e \u003ctbody\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"5\" rowspan=\"6\"\u003e \u003cp\u003eNF\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThis work\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAtrazine, simazine, isoproturon, Metholachlor ESA, 2,4-D and chlorothalonil\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e29.25\u0026ndash;89.36\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR24\" class=\"CitationRef\"\u003e24\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAtrazine \u0026amp; dimethoate\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e80.00\u0026ndash;95.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eDiuron \u0026amp; isoproturon\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e78.90\u0026ndash;89.50\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e(2-methyl-4-chlorophenoxy acetic acid (MCPA), 2-methyl-4-chlorophenoxy propionic acid, (MCPP), (2,6-dichlorobenzamide, (BAM)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e30.00\u0026ndash;82.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR20\" class=\"CitationRef\"\u003e20\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2,4-D\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e97.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR22\" class=\"CitationRef\"\u003e22\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAtrazine \u0026amp; isoprothiolane\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e54.00\u0026ndash;82.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c1\" morerows=\"5\" rowspan=\"6\"\u003e \u003cp\u003eRO\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003eThis work\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eAtrazine, simazine, isoproturon, Metholachlor ESA, 2,4-D and chlorothalonil\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e97.64\u0026ndash;99.99\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR21\" class=\"CitationRef\"\u003e21\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eCycluron\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e\u0026gt;\u0026thinsp;95.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR27\" class=\"CitationRef\"\u003e27\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e158 pesticides\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e72.00\u0026ndash;98.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR23\" class=\"CitationRef\"\u003e23\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e(2-methyl-4-chlorophenoxy acetic acid (MCPA), 2-methyl-4-chlorophenoxy propionic acid, (MCPP), (2,6-dichlorobenzamide, (BAM)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e\u0026gt;\u0026thinsp;92.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR26\" class=\"CitationRef\"\u003e26\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003eTributyl phosphate, irgarol, flutriafol \u0026amp; dicofol\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e\u0026gt;\u0026thinsp;95.00\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003ctr\u003e \u003ctd align=\"left\" colname=\"c2\"\u003e \u003cp\u003e[\u003cspan citationid=\"CR28\" class=\"CitationRef\"\u003e28\u003c/span\u003e]\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c3\"\u003e \u003cp\u003e2-methyl-4-chlorophenoxyacetic acid (MCPA)\u003c/p\u003e \u003c/td\u003e \u003ctd align=\"left\" colname=\"c4\"\u003e \u003cp\u003e95.30\u003c/p\u003e \u003c/td\u003e \u003c/tr\u003e \u003c/tbody\u003e \u003c/colgroup\u003e \u003c/table\u003e\u003c/div\u003e \u003c/p\u003e \u003cp\u003eThe NF membrane evaluated in the present study achieved a removal rate in the rage of 29.25\u0026ndash;89.36% for the studied pesticides, due to their wide range of molecular weight. This result is in the range of the ones reported in previous studies, which are between 30.00 and 97.00%. The similar molecular weight of most of the studied pesticides with the tested membrane\u0026rsquo;s molecular weight cut-off allow the permeation of these compounds, which can be found in the permeate stream in small quantities. As can be observed in the previous table, NF reported partial rejection rates in almost all published studies; therefore, the technology is effective for pesticides which can be found as particles suspension or those with a medium molecular weight (\u0026gt;\u0026thinsp;300 Da).\u003c/p\u003e \u003cp\u003eThe RO membrane evaluated in the present study presented average removal rates between 97.64\u0026ndash;99.99% for the different pesticides. This is slightly higher than some results reported in previous studies (72.00\u0026ndash;98.00%). However, Fujioka et al., (2020) tested the RO rejection of a wide range of pesticides, including other ones with smaller molecular weight and chemical affinity (hydrophobicity), such as cycluron, carbendazim or aldicarb, which were also rejected. Almost all studies reported pesticides rejection\u0026thinsp;\u0026gt;\u0026thinsp;90%, resulting in the presence of small quantities of pesticides in permeate, most of them below detection limit, which would potentially allow its direct discharge or with a smooth polishing treatment.\u003c/p\u003e \u003c/div\u003e"},{"header":"4. Conclusions","content":"\u003cp\u003eIn the present study, the rejection efficiency of a NF membrane (NF270) and a RO membrane (XLE) for the treatment of wastewater effluents containing pesticides has been investigated. The studied pesticides included atrazine, simazine, isoproturon, metolachlor ESA, 2,4-Dichlorophenoxyacetic acid, and chlorothalonil, widely used pesticides for crops and with toxic or carcinogenic effects on humans and the environment.\u003c/p\u003e \u003cp\u003eBoth membranes reported pesticides adsorption onto the polyamide active layer, which depends on substance\u0026rsquo;s hydrophobicity and dipolar moments. This should be considered for a proper assessment of pesticides rejection when a fresh membrane is used. However, there are only a few studies that assessed this phenomenon in depth, so it is important to perform more studies for stablishing a clear correlation between the membrane\u0026rsquo;s active layer material, substance\u0026rsquo;s physicochemical properties and their adsorption onto membranes.\u003c/p\u003e \u003cp\u003eIn the case of chlorothalonil, a full rejection was observed by using both NF and RO, since the compound was present in suspension due to its low solubility in water. Therefore, for those products that are delivered as suspension, ultrafiltration or microfiltration membranes could be assessed for its removal from wastewater effluents with lower energy consumption.\u003c/p\u003e \u003cp\u003eMoreover, NF270 reported a wide range of rejection rates depending on the targeted pesticide, reporting efficient rejection for larger molecules (\u0026gt;\u0026thinsp;300 Da), while XLE filtration tests resulted in the rejection of \u0026gt;\u0026thinsp;95% for all the studied pesticides. Therefore, XLE can be used as efficient treatment for the rejection of pesticides in wastewaters.\u003c/p\u003e \u003cp\u003eIn this study, the feed solution contained higher pesticides concentration than the commonly present in agricultural leachates for proper quantification purposes, but further tests should be carried out considering lower concentration of these compounds for a better assessment of the membranes performance at relevant environment.\u003c/p\u003e \u003cp\u003eFinally, the assessment of these membranes performance during a longer working period, integrating the implementation of a Clean-in-place (CIP) process should also be performed prior to the uptake of this technology at industrial scale. In this context, additional tests are required to optimize the utilization of these membranes on a real-scale basis by validating the technology using real waters.\u003c/p\u003e"},{"header":"Declarations","content":"\u003cp\u003e\u003cstrong\u003eAcknowledgment\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThis study was funded by DuPont Water Solutions and its Global Water Technology Center in Tarragona, Spain.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eData availability\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003eThe data supporting the findings of this study are available from the corresponding author.\u003c/p\u003e\n\u003cp\u003eCompeting interests. The authors declare no conflicts of interest.\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eAuthor contribution statements\u003c/strong\u003e\u003c/p\u003e\n\u003cp\u003e\u003cstrong\u003eRub\u0026eacute;n Rodr\u0026iacute;guez-Alegre:\u003c/strong\u003e in charge of conducting the analytical work, analyzing and interpreting the data, writing the first draft of the document: writing, reviewing, and editing \u0026ndash; the original draft. \u003cstrong\u003eLaura P\u0026eacute;rez Meg\u0026iacute;as:\u003c/strong\u003e perform experiments; analytical work, to analyzing and interpreting the data, writing the first draft of the document: writing, reviewing, and editing \u0026ndash; the original draft. \u003cstrong\u003eSonia Sanchis:\u003c/strong\u003e editing \u0026amp; reviewing. \u003cstrong\u003eCarlos Andecochea Saiz:\u003c/strong\u003e funding acquisition, investigation, performing experiments, editing \u0026amp; reviewing. \u003cstrong\u003eXialei You:\u003c/strong\u003e funding acquisition, investigation, performing experiments, editing \u0026amp; reviewing.\u003c/p\u003e"},{"header":"References","content":"\u003col\u003e\n\u003cli\u003eClune T. 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Journal of Membrane Science 2020;595:117577. https://doi.org/10.1016/j.memsci.2019.117577.\u003c/li\u003e\n\u003cli\u003eZhang J, Weston G, Yang X, Gray S, Duke M. Removal of herbicide 2-methyl-4-chlorophenoxyacetic acid (MCPA) from saline industrial wastewater by reverse osmosis and nanofiltration. Desalination 2020;496:114691. https://doi.org/10.1016/j.desal.2020.114691.\u003c/li\u003e\n\u003cli\u003eSimonič M. Reverse Osmosis Treatment of Wastewater for Reuse as Process Water\u0026mdash;A Case Study. Membranes 2021;11:976. https://doi.org/10.3390/membranes11120976.\u003c/li\u003e\n\u003cli\u003eMassons G, Gilabert-Oriol G, Niewersch C. Nanofiltration innovation: performance of new DuPont\u003csup\u003eTM\u003c/sup\u003e FilmTec\u003csup\u003eTM\u003c/sup\u003e NF270-440 element in municipal wastewater operation. DWT 2023;309:149\u0026ndash;53. https://doi.org/10.5004/dwt.2023.29886.\u003c/li\u003e\n\u003cli\u003ePlakas KV, Karabelas AJ. Membrane retention of herbicides from single and multi-solute media: The effect of ionic environment. Journal of Membrane Science 2008;320:325\u0026ndash;34. https://doi.org/10.1016/j.memsci.2008.04.016.\u003c/li\u003e\n\u003c/ol\u003e"}],"fulltextSource":"","fullText":"","funders":[],"hasAdminPriorityOnWorkflow":false,"hasManuscriptDocX":true,"hasOptedInToPreprint":true,"hasPassedJournalQc":"","hasAnyPriority":false,"hideJournal":false,"highlight":"","institution":"","isAcceptedByJournal":true,"isAuthorSuppliedPdf":false,"isDeskRejected":"","isHiddenFromSearch":false,"isInQc":false,"isInWorkflow":false,"isPdf":false,"isPdfUpToDate":true,"isWithdrawnOrRetracted":false,"journal":{"display":true,"email":"[email protected]","identity":"discover-environment","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"Learn more about [Discover Environment](https://www.springer.com/44274/)","snPcode":"44274","submissionUrl":"https://submission.nature.com/new-submission/44274/3","title":"Discover Environment","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Discover Series","inReviewEnabled":true,"inReviewRevisionsEnabled":true},"keywords":"Pesticides, nanofiltration, reverse osmosis, membrane processes, wastewater treatment","lastPublishedDoi":"10.21203/rs.3.rs-3991503/v1","lastPublishedDoiUrl":"https://doi.org/10.21203/rs.3.rs-3991503/v1","license":{"name":"CC BY 4.0","url":"https://creativecommons.org/licenses/by/4.0/"},"manuscriptAbstract":"\u003cp\u003eThe increasing food demand for a growing population has resulted in the intensification and modernization of agriculture leading to an increasing use of pesticides to protect crops against insects, weeds, fungi, and other pests. However, these chemical compounds can cause adverse effects on the environment due to their low biodegradability and toxicity. This study assesses the use of DuPont FilmTec\u0026trade; NF270 and FilmTec\u0026trade; XLE membranes for the removal of six pesticides (atrazine, simazine, isoproturon, metolachlor ESA, 2,4-D, and chlorothalonil) in aqueous streams. The results reported average rejection rates of 29.25\u0026ndash;89.36% and \u0026gt;\u0026thinsp;97% in the nanofiltration and reverse osmosis membranes respectively, showcasing that membrane technology is effective for the removal of these pollutants from wastewater streams. However, a customised selection of the membrane (nanofiltration/reverse osmosis) should be performed depending on the targeted pollutants in order to balance the pesticide rejection and energy consumption for each market application.\u003c/p\u003e","manuscriptTitle":"Nanofiltration \u0026amp; Reverse Osmosis Technical Assessment for Pesticides Removal","msid":"","msnumber":"","nonDraftVersions":[{"code":1,"date":"2024-03-18 17:49:00","doi":"10.21203/rs.3.rs-3991503/v1","editorialEvents":[{"type":"communityComments","content":0},{"type":"decision","content":"Revision requested","date":"2024-04-02T09:04:55+00:00","index":"","fulltext":""},{"type":"editorInvitedReview","content":"","date":"2024-03-21T12:14:21+00:00","index":"hide","fulltext":""},{"type":"reviewerAgreed","content":"8d7b99eb-6e7d-4fb9-a0e0-5a1859810acd","date":"2024-03-19T19:13:10+00:00","index":"hide","fulltext":""},{"type":"reviewersInvited","content":"","date":"2024-03-19T09:39:25+00:00","index":"","fulltext":""},{"type":"editorAssigned","content":"","date":"2024-03-14T08:18:03+00:00","index":"","fulltext":""},{"type":"checksComplete","content":"","date":"2024-03-14T08:17:33+00:00","index":"","fulltext":""},{"type":"submitted","content":"Discover Environment","date":"2024-02-26T16:55:17+00:00","index":"","fulltext":""}],"status":"published","journal":{"display":true,"email":"[email protected]","identity":"discover-environment","isNatureJournal":false,"hasQc":true,"allowDirectSubmit":false,"externalIdentity":"","sideBox":"Learn more about [Discover Environment](https://www.springer.com/44274/)","snPcode":"44274","submissionUrl":"https://submission.nature.com/new-submission/44274/3","title":"Discover Environment","twitterHandle":"","acdcEnabled":true,"dfaEnabled":true,"editorialSystem":"stoa","reportingPortfolio":"Discover Series","inReviewEnabled":true,"inReviewRevisionsEnabled":true}}],"origin":"","ownerIdentity":"f8b8e4a3-65f8-4833-9bfb-ae0c8982bdf7","owner":[],"postedDate":"March 18th, 2024","published":true,"recentEditorialEvents":[],"rejectedJournal":[],"revision":"","amendment":"","status":"under-review","subjectAreas":[],"tags":[],"updatedAt":"2024-05-02T04:18:29+00:00","versionOfRecord":[],"versionCreatedAt":"2024-03-18 17:49:00","video":"","vorDoi":"","vorDoiUrl":"","workflowStages":[]},"version":"v1","identity":"rs-3991503","journalConfig":"researchsquare"},"__N_SSP":true},"page":"/article/[identity]/[[...version]]","query":{"redirect":"/article/rs-3991503","identity":"rs-3991503","version":["v1"]},"buildId":"qtupq5eGEP_6zYnWcrvyt","isFallback":false,"isExperimentalCompile":false,"dynamicIds":[84888],"gssp":true,"scriptLoader":[]}