290 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 A B S T R A C T The intense use of pesticides can be harmful to the environment and human health, being necessary to monitor the environmental concentrations of pesticides. The legislation on drinking water for human consumption is one of the guiding regulations about monitoring priority. Therefore, a systematic review was carried out to compile information on the contamination of surface water, groundwater, and treated water in Brazil. Thereby, we selected those pesticides which, although they are authorized for use and are among the top- selling pesticides, are not regulated by GM Ordinance of the Ministry of Health (GM/MS) No. 888, of May 4, 2021. The databases used were PubMed, Scielo, Science Direct, Scopus, and Web of Science. Of the 122 pesticides in the market, 11 were selected. Analyses of environmental dynamics, concentration, and health effects were carried out. The Goss methodology and the Groundwater Ubiquity Score (GUS) index were used to estimate the risk of surface water and groundwater contamination, respectively. The concentrations found were compared with the values provided for in the guidelines adopted by international agencies, determining the Brazilian population’s margin of exposure (MOE) to the target pesticides. The results indicate a high probability of finding imidacloprid and hexazinone in the water, the prevalence of studies on surface waters, and the need to conduct additional studies as papers on some of the target pesticides were not found. It is concluded that the pesticides studied pose a low risk to human health, however, further studies are still required. Keywords: legislation; microcontaminants; health; agrochemicals. R E S U M O O intenso uso de agrotóxicos pode ser prejudicial ao meio ambiente e à saúde humana, tornando necessário o monitoramento de suas concentrações ambientais. Como um dos dispositivos norteadores sobre a prioridade de monitoramento é a legislação de água potável para consumo humano, foi realizada uma revisão sistemática da literatura com o objetivo de compilar informações sobre a contaminação das águas superficiais, subterrâneas e tratadas por agrotóxicos. Foram considerados os agrotóxicos mais vendidos em território brasileiro entre 2009 e 2019 e que possuem autorização de uso, mas que não são regulamentados pela Portaria GM do Ministério da Saúde nº 888, de 4 de maio de 2021. Dos 122 agrotóxicos comercializados, 11 foram selecionados. Analisaram- se a dinâmica ambiental, concentração em águas e efeitos na saúde humana. Na estimativa do risco de contaminação das águas superficiais e subterrâneas, empregou-se a metodologia Goss e o índice Groundwater Ubiquity Score (GUS), respectivamente. Uma comparação crítica sobre as concentrações encontradas e os valores-guia adotados por agências internacionais foi realizada, determinando-se a margem de exposição da população brasileira aos agrotóxicos. Os resultados do trabalho mostraram a maior probabilidade de que imidacloprido e hexazinona sejam encontrados em águas; a prevalência de estudos realizados em águas superficiais; e a necessidade de que mais trabalhos sejam realizados, uma vez que não foram encontrados artigos sobre alguns dos compostos-alvo. Conclui-se que os agrotóxicos estudados apresentam baixo risco à saúde, todavia se vê a necessidade de que mais estudos sejam desenvolvidos. Palavras-chave: legislação; microcontaminantes; saúde; pesticidas. Priority pesticides not covered by GM Ordinance of the Ministry of Health No. 888, of 2021, on water potability standard in Brazil Agrotóxicos prioritários não abordados pela Portaria GM do Ministério da Saúde nº 888, de 2021, sobre padrão de potabilidade da água no Brasil Beatriz Corrêa Thomé de Deus1,2 , Emanuel Manfred Freire Brandt2,3 , Renata de Oliveira Pereira2,3 1Programa de Pós-Graduação em Biodiversidade e Conservação da Natureza, Universidade Federal de Juiz de Fora – Juiz de Fora (MG), Brazil. 2Departamento de Engenharia Ambiental e Sanitária, Universidade Federal de Juiz de Fora – Juiz de Fora (MG), Brazil. 3Programa de Pós-Graduação em Engenharia Civil, Universidade Federal de Juiz de Fora – Juiz de Fora (MG), Brazil. Correspondence address: Beatriz Corrêa Thomé de Deus – Departamento de Engenharia Ambiental e Sanitária, Universidade Federal de Juiz de Fora – Rua José Lourenço Kelmer, s/n – Campus Universitário – São Pedro – CEP: 36036-900 – Juiz de Fora (MG), Brazil. E-mail: beatriz.correa@ engenharia.ufjf.br Conflicts of interest: the authors declare no conflicts of interest. Funding: none. Received on: 03/10/2021. Accepted on: 02/03/2022 https://doi.org/10.5327/Z2176-94781077 Revista Brasileira de Ciências Ambientais Brazilian Journal of Environmental Sciences Revista Brasileira de Ciências Ambientais Brazilian Journal of Environmental Sciences ISSN 2176-9478 Volume 56, Number 1, March 2021 This is an open access article distributed under the terms of the Creative Commons license. https://orcid.org/0000-0003-1858-1889 http://orcid.org/0000-0002-9009-1940 https://orcid.org/0000-0002-3414-7292 mailto:beatriz.correa@engenharia.ufjf.br mailto:beatriz.correa@engenharia.ufjf.br https://doi.org/10.5327/Z2176-94781077 http://www.rbciamb.com.br http://abes-dn.org.br/ https://creativecommons.org/licenses/by/4.0/ Priority pesticides not covered by GM Ordinance of the Ministry of Health No. 888, of 2021, on water potability standard in Brazil 291 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 Introduction Pesticides are used to modify the composition of flora or fauna to preserve them from the action of harmful living beings (Brasil, 1989). Historically, since there were problems related to the cultivation pro- cess, the Brazilian agricultural production model was based on pesti- cides (Wahlbrinck et al., 2017). Since 2008 Brazil has been one of the world’s largest agricultural producers, the second top exporter of pesti- cides (Pignati et al., 2017). According to the Brazilian Institute for the Environment and Natural Resources (IBAMA), in 2009, the accumu- lated sales in Brazil were approximately 270,000 tons of Active Ingredi- ents (AI). In 2019, it was over 560,000, corresponding to a percentage increase of around 108% (IBAMA, 2021). The current model of agriculture requires the use of pesti- cides, as they help increase crop productivity (Sharma et  al., 2019). However,  when they are used excessively, pesticides can be harmful to the environment and contaminate aquatic matrices, the air, and the soil (Lorenzatto et  al., 2020). Contamination of aquatic matrices can occur through soil runoff, spray drift, or improper disposal of pesti- cide containers (Olisah et al., 2020). Once in the aquatic environment, pesticides can bioaccumulate in organisms (Belchior et al., 2014) and may have deleterious effects on the aquatic biota, such as fish (Améri- co-Pinheiro et  al., 2019, 2020). In addition, it is noted that pesticides can evaporate, infiltrate the soil, or be carried through rivers (Souza et al., 2020) and, depending on their properties, they can be transport- ed through the atmospheric process and reach new areas, extending the degree of contamination (Carvalho, 2017). The population can be exposed to the risks of pesticides mainly through food, as humans are at the top of the food chain and depend on resources (i.e., water, land, air) for survival (Belchior et al., 2014). Considering the aforementioned, it is necessary to analyze the risks associated with human exposure to pesticides. In this context, the risk assessment (RA) methodology stands out. This methodology aims to identify the risks associated with a chemical agent through four steps: • Hazard identification; • Dose (concentration) – response (effect) relation; • Exposure assessment; • Risk characterization (UNEP, 1999). The RA methodology is used to establish water potability stan- dards and guidelines worldwide (WHO, 2017), as well as the standards reviewing process (Vigiagua, 2020). Usually, substances are considered potential candidates to integrate the potability standard according to factors like the pattern of occurrence in springs, toxicity, environmen- tal dynamics, persistence/mobility in environmental matrices, and re- moval in water treatment plants (WTPs). In Brazil, water quality control for human consumption is regu- lated by Annex XX, of Consolidation Ordinance No. 5, of September 28, 2017, amended by GM Ordinance of the Ministry of Health (MS) No.  888, of May 4, 2021, in which pesticides and other substances harmful to humans are listed (Brasil, 2021). It is worth mentioning that some pesticides, even though they are not listed in the Ordinance, deserve attention. Especially the top-selling ones whose properties in- crease their occurrence in water matrices. Therefore, in this study, we aimed to carry out a risk assessment, based on a systematic literature review, of pesticides found in water for human consumption in Brazil, including exposure factors (commer- cialization, environmental dynamics, and occurrence on the surface, groundwater, and treated water) and chronic toxicity data. To this end, we focused on the top-selling authorized pesticides in Brazil but not listed in the water potability standard. Material and Methods Pesticide selection To identify the top-selling pesticides in Brazil, the data available in IBAMA’s current Marketing Reports were compiled (2009-2019) (IBA- MA, 2021). Our exclusion criteria were: • pesticide covered by GM/MS Ordinance No. 888 of 2021 (Brasil, 2021) because the purpose of this study is to evaluate the pesticides not covered by the Brazilian potability ordinance; • unauthorized pesticides or those that do not have a monograph at the Brazilian Health Surveillance Agency (ANVISA, 2021); • pesticides with a low percentage of sales — the 70th percentile was applied to the accumulated sales data, and the corresponding value was adopted as the cutoff point; • adjuvant compounds (those that are used in association with the AI to improve application). Environmental dynamics To analyze the probability of pesticides reaching the water, we verified their physicochemical properties: coefficient of adsorption in organic matter (Koc);  typical half-life (DT50) in the soil and water phase; solubility in water; octanol-water partition coefficient (Kow); and Henry’s law constant (KH). These properties were obtained through the Pesticides Properties Database  (PPDB) (IUPAC, 2020) and, in cases when the information was absent, using the Oregon State University (OSU) Extension Pesticide Properties Database (NPIC, 2020). The contamination potential of surface water and groundwater was estimated using the Goss methodology (Goss, 1992) and the GUS In- dex (Gustafson, 1989), respectively. A systematic review of environmental concentrations in surface water, groundwater, and treated water A systematic review was carried out using the PRISMA methodol- ogy (Moher et al., 2009). We searched for studies concerning the target pesticides in Brazil- ian waters using PubMed, Scielo, Science Direct, Scopus, and Web of Science platforms since there is broad literature regarding the subject Deus, B.C.T. 292 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 of this study. The following search codes were used: (pesticides AND water AND Brazil) and ((clomazone OR hexazinone OR “monosodi- um methyl arsenate” OR MSMA OR tebuthiuron OR cypermethrin OR imidacloprid OR “lambda-cyhalothrin” OR “lambda cyhalothrin” OR methomyl OR azoxystrobin OR “thiophanate-methyl” OR “thio- phanate methyl” OR ethephon) AND water AND Brazil). The pres- ent review considers articles in English or Portuguese language, pub- lished by October 4, 2021. We did not consider review articles since it is expected that the original ones have already been contemplated through the search made. After excluding duplicate articles, screening was performed on two levels: first, by analyzing the title, abstract, and keywords; and second, by reading the entire content of each one of the articles. We excluded those articles in which at least one of the following pieces of information was absent: • limit of detection (LOD) and limit of quantitation (LOQ); • number of samples in which there was detection or quantitation; • individual concentration of each sample and no information about the frequency of detection/quantitation or the average value. Also, we did not consider articles that quantified pesticides in mixtures (i.e., with metabolites or other compounds); and when it was not possible to identify the analysis matrix (e.g., raw or treated water). For papers that did not specify the individual environmental concen- trations but presented the average and the frequency of detection and/ or quantitation, we determined the individual concentrations as fol- lows: concentration = average ÷ number of samples. Due to the occur- rence of censored data, lower than the limit of detection (< LOD) or not detected (ND) and/or lower than the limit of quantitation (<  LOQ), the substitution method for censored data was applied (Sanford et al., 1993). Therefore, when elaborating the graphical representation of pes- ticide occurrence, in those studies where the environmental concen- tration was reported as < LOD or ND, we used LOD/2; and when the concentration was reported as < LOQ, we used LOQ/2. We also con- sidered as outliers (higher concentrations) the values that were at least 1.5 times the interquartile range (Q 3  - Q1), from the edge of the box (Minitab, 2020), which were not represented due to the graphic scale. Pesticide occurrence in surface water, groundwater, and treated water Based on the occurrence data of pesticides in surface water, groundwater, and treated water, we carried out an analysis to identify the most abundant pesticide in each of them. Also, we correlated the detection frequency with the pesticide’s position in IBAMA’s sales rank, considering total sales from 2009 to 2019. Human health effects To analyze the potential effects of pesticides on human health, we gathered information about chronic toxicity data from the Internation- al Agency for Research on Cancer (IARC, 2020a) and the United States Environmental Protection Agency (USEPA, 2020a). Critical comparison of environmental occurrence and maximum acceptable values in drinking water We searched for information about the target pesticides presence on international agencies and guidelines for drinking water quality to obtain the maximum acceptable values (MAV) on drinking wa- ter. We  selected USEPA and the World Health Organization (WHO) guidelines, as they are considered the main references used on drink- ing water standards in several countries (Araújo, 2018); New Zealand, Canada, and Australia guidelines that are also international references and employ the risk assessment methodology; and the European En- vironmental Agency (EEA), considering its high restrictiveness (Souza et al., 2019). Based on the occurrence data and the MAV in drinking water, we made a critical comparison of the environmental concen- trations to identify its potential risk for human health. According to USEPA, the occurrence value (OV) can be obtained by the 90th, 95th or 99th percentile of the concentrations found or through the maximum value detected in drinking water (USEPA, 2016a). On the other hand, the Australian Drinking Water Guidelines use only the maximum val- ue found in drinking water (NHMRC, 2021). Given the impossibility of calculating the percentile for some pesticides due to the reduced amount of data, we chose to use the recommendation proposed by the Australian guidelines, with some modifications. Thus, to obtain the MOE, we calculated the ratio between MAV and OV in each of the matrices — and not only for drinking water, as the methodology pro- poses. This approach was adopted considering a conservative view on those cases in which the water resources are used for public supply and considering that water treatment would not effectively remove residual pesticides. The OV of each pesticide was obtained using the maximum concentration found in each matrix (disregarding  outliers). In cases where more than one MAV was available, we used the most restrictive one. From the values obtained, the MOE was stipulated: MOE ≤ 1: the pesticide poses a risk to human health;  1 ≤ MOE ≤ 10: the pesticide deserves attention since its occurrence is in the same order of magni- tude as the concentrations that would represent a risk to human health; and MOE ≥ 10: the pesticide is less likely to cause adverse health effects. Results and Discussion Pesticide selection The research started with 122 pesticides and, based on the ap- plication of the criteria, 111 were excluded: 32 according to criteria 1 (covered by GM/MS Ordinance No. 888 of 2021);  8 according to criteria 2 (ANVISA monograph absent/excluded);  66 based on cri- teria 3 (total sales were less than 12128t);  and 5 according to criteria 4 (adjuvants).  Finally, a total of 11 pesticides remained in the study: clomazone, hexazinone, monosodium methyl arsonate (MSMA), and Priority pesticides not covered by GM Ordinance of the Ministry of Health No. 888, of 2021, on water potability standard in Brazil 293 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 tebuthiuron (herbicides);  cypermethrin, imidacloprid, lambda-cy- halothrin and methomyl (insecticides);  azoxystrobin and thiophan- ate-methyl (fungicides); and ethephon (growth regulator). Environmental dynamics The physicochemical properties of the pesticides influence their environmental dynamics, defining major or minor tendencies to reach water matrices. Using the International Union of Pure and Applied Chemistry (IUPAC, 2020) and OSU (NPIC, 2020) data, we evaluated the water contamination potential of pesticides. Among the regarded pesticides, hexazinone and imidacloprid have greater contamination probability, as they have high solubility (33,000 and 2,500 mg/L, re- spectively), showing a tendency for surface runoff (Elias et al., 2018) and high DT50 (soil) (105 and 191 days, respectively). These properties, although being influenced by soil type and climate conditions (New Zealand, 2020), indicate that these pesticides are persistent in the en- vironment. Furthermore, hexazinone and imidacloprid have low Koc (54 and 13 ml/g, respectively), i.e., they are poorly retained on soil particles (Pérez-Lucas et  al., 2021); low Kow (1.17 and 0.57, respec- tively), an indication that they can easily pass into the aqueous phase (Yang et  al., 2018), and low KH (1.10 x 10-⁷ and 1.7 x 10-¹⁰ Pa m³/ mol, respectively), which means they do not volatilize easily, remain- ing in the aquatic environment for longer periods (Chao et al., 2017). In addition, methomyl has high solubility (55,000 mg/L) and low Koc (72 ml/g); MSMA is strongly retained on soil particles (200 days) and shows low log Kow (-3.1), an indication that it has a higher affinity to the water phase. Otherwise, some pesticides did not show a tendency for contami- nation: cypermethrin, which has low solubility (0.009 mg/L), is strongly adsorbed to the soil matrix (3 x 105 ml/g), shows volatilization tendency (0.31 Pa m³/mol), and has high log Kow (5.55), with a less pronounced hydrophilic characteristic; lambda-cyhalothrin shows low solubility (0.005 mg/L) and is strongly retained to the soil (Koc  =  283,707  ml/g and DT50 (soil) = 175 days); methomyl, which in addition to having high solubility (55,000 mg/L) and low Koc (72 ml/g), shows low DT50 (water) (2.9 days), an indication that it is poorly persistent in the environment; tebuthiuron that despite showing high soil permanency (400 days) and low log Kow (1.79), tends to volatilize (KH = 2.47  x  10 -5 Pa m³/mol); clomazone and ethephon are not persistent in the soil since they have DT50 (soil) equal to 22.6 and 13.1 days, respectively. Also, ethephon is poorly persistent in the water matrix (DT50 (water) = 2.4 days). It is worth mentioning the fungicide class, since both azoxystrob- in and thiophanate-methyl have low solubility (6.7 and 18.5 mg/L, re- spectively) and are slightly mobile on the solid surface (Koc = 589 and 1830 ml/g, respectively), tending to remain retained to the soil matrix. Also, they have DT50 (water) equal to 6.1 and 3 days, respectively, indicat- ing that they are slightly persistent in the water matrix. According to the Goss methodology (Goss, 1992), hexazinone, tebuthiuron, and azoxystrobin have a high potential for water con- tamination, considering their transportation as dissolved in the water; and lambda-cyhalothrin is a potential contaminant considering its transportation in the soil. MSMA has a high contamination potential through both water and soil transportation. The other target pesticides have a moderate to low probability of surface water contamination. Regarding groundwater contamination, we verified that hexazi- none and tebuthiuron tend to contaminate groundwater, according to the GUS index (Gustafson, 1989). Moreover, clomazone, metho- myl, azoxystrobin, and ethephon can also be potential contaminants since they are at the transition state. The other pesticides have little contamination probability. However, it is worth noting that even those compounds that are unlikely to reach water matrices, given their prop- erties, could also be potential contaminants since climate and soil char- acteristics can be favorable to leach (Pérez-Lucas et al., 2019). We were not able to calculate the contamination probability of imidacloprid for both surface water and groundwater since its Koc value is absent in the PPDB (IUPAC, 2020), and this insecticide is not listed in the OSU Ex- tension Pesticide Properties Database (NPIC, 2020). A systematic review of concentrations in surface water, groundwater, and treated water A total of 1,775 articles were found (number of articles = N = 1,775), 104 from PubMed, 40 from Scielo, 197 from Science Direct, 870 from Scopus, and 564 from Web of Science (Figure 1). After screening, only 30 articles were included in our analysis based on the inclusion and exclusion criteria. Source: adapted from PRISMA (Moher et al., 2009). Figure 1 – Flowchart of the systematic review. Deus, B.C.T. 294 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 Among the target pesticides of this study, we observed that imidaclo- prid was the top-selling product and also the most detected in surface wa- ters (F = 27.3%). Likewise, the least selling, cypermethrin, was not detected (Figure 3). These results are in line with the expectations, as top-selling pesticides are more likely to have a higher detection percentage. Azoxystrobin is one of the most widely used fungicides worldwide (Uçkun and Öz, 2021) and it is applied mainly against brusone (Pyric- ularia oryzae), the main fungal disease that affects irrigated rice (Back et  al., 2016). Approximately 2900 tons of this fungicide are sold annu- ally in Brazil. Concentrations of this pesticide were found in the range of 0.001 to 0.125 μg L– 1 (Figure 3) in Rio Grande do Sul (RS) (Amaral et al., 2020; Severo et al., 2020) and São Paulo (SP) states (López-Doval et al., 2017; Montagner et al., 2014, 2019). In Montagner et al. (2019), an outlier of 0.431 μg L– 1 was observed in the sample collected in the city of Indaiatuba (SP). In the region of Londrina, Paraná (PR), azoxystrobin was quantified at an average concentration of 0.027 μg L– 1 in 15 of the 24 samples analyzed (Souza et al., 2019). In other studies carried out in the southern region of Brazil, it was not found at quantifiable levels (Amaral et al., 2018; Almeida et al., 2019) and it was not detected in the Camand- ucaia River and its tributaries (SP) (Barizon et al., 2020). Cypermethrin, a synthetic pyrethroid used against agricultural and domestic pests (Bhatt et al., 2020), has average annual sales in Brazil of about 1230 tons. It was not detected in any of the 10 samples collected in Minas Gerais (MG) in a study that showed relatively high LOD and LOQ (1.5 and 5 μg L– 1, respectively) (Rodrigues et al., 2018). Clomazone has average annual sales in Brazil of approximate- ly 5164 tons and it is widely used in rice crops (Guo et  al., 2021). Studies  on this herbicide were conducted in RS, PR, and SP, being found in quantifiable levels in 11 (Zanella et al., 2002; Bortoluzzi et al., 2006, 2007; Armas et  al., 2007; Silva et  al., 2009; Primel et  al., 2010; Marchesan et  al., 2007, 2010; Caldas et  al., 2013; Severo et  al., 2020; Guarda et al., 2020b) of the 16 articles considered in at least one sample analyzed in each of the studies, totaling 218 of 1064 samples (Figure 3). *2020 and 2021 sales data are still not available by IBAMA. Figure 2 – Annual sales (2009-2019) and Scientific production (2009- 2021)*. Usually, the articles found evaluated the occurrence of more than one pesticide in waters. The most studied pesticide was clomazone (N = 17), followed by imidacloprid (N = 12), azoxystrobin (N = 10), tebuthiuron (N = 5), hex- azinone (N = 4), and lambda-cyhalothrin (N = 2). Cypermethrin and methomyl were studied in only one article each. We did not find arti- cles regarding ethephon, MSMA, and thiophanate-methyl. About  57% of the studies referred to the occurrence of pesticides in surface water, approximately 3% in groundwater matrices, and the same percentage in drinking water. The remaining percentage referred to the occurrence in more than one matrix (e.g., surface and groundwater). We observe a larger number of studies related to both surface and treated water, ap- proximately 23%. Establishing a comparison between scientific production and com- mercialization over the years, it was possible to note a growing trend (Figure 2). It is worth noting that the 2020 and 2021 sales data were not plotted because they were not available yet (IBAMA, 2021). Although scientific production showed some periods of decline, a growth tendency is observed since 2018, as suggested by the trendline (Figure 2). Most of the studies were carried out in the South (N = 19) and Southeast (N = 8) regions of Brazil, where the trade of agricultural products is highly significant (Oliveira and Rodrigues, 2019). The Mid- west region showed two articles. The North and Northeast regions, which have little participation in the Brazilian agribusiness (Oliveira and Rodrigues, 2019), had only one study each. Pesticide occurrence in Brazilian surface water We found 27 articles related to surface water contamination in Brazil. Most of them was about clomazone (N = 16), imidacloprid (N = 11), and azoxystrobin (N = 9); followed by tebuthiuron (N = 5), hexazinone (N = 4), and lambda-cyhalothrin (N = 2). Cypermethrin and methomyl were reported by only one article each. Figure 3 shows pesticide concentration in Brazilian surface water. Figure 3 – Pesticide occurrence in Brazilian surface water. Priority pesticides not covered by GM Ordinance of the Ministry of Health No. 888, of 2021, on water potability standard in Brazil 295 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 Of this amount, about 41% were between 0.002 and 0.1 μg L– 1; and ap- proximately 50% were found between 0.15 and 1.72 μg L– 1. Outliers of 3.21 and 15.69 μg L– 1 were identified, associated with the increased use of this herbicide and reduced manual weed control (Bortoluzzi et al., 2007). Moreover, outliers between 5.4 and 23 μg L– 1 were found, pos- sibly because clomazone has high water stability and is widely used in the study area (Primel et al., 2010). There was no detection/quantita- tion in other studies (Vieira et al., 2016; López-Doval et al., 2017; Vieira et al., 2017; Souza et al., 2019; Barizon et al., 2020). Hexazinone, widely used in sugarcane crops (Acayaba et al., 2021), has average annual sales in Brazil of approximately 1374 tons. A study carried out in Mato Grosso (MT) identified this pesticide in two of the 18 samples collected, at concentrations of 0.009 and 0.02 μg L– 1 (Sposito et  al., 2018) (Figure 3). In PR, it was quantified in the range of 0.01 and 0.03 μg L– 1 (Figure 3) and outliers from 0.07 to 0.14 μg L– 1 (Almeida et  al., 2019). There was no detection in MT (Duarte et  al., 2016) and no quantitation in PR (Souza et al., 2019). Imidacloprid, of which about 7659 tons are sold per year in Brazil, is a neonicotinoid used against a variety of insects (Tuelher et al., 2018) and it was found at concentrations between 0.001 and 0.125 μg L– 1 in RS (Amaral et  al., 2018, 2020; Severo et  al., 2020), SP (López-Doval et al., 2017), MT (Sposito et al., 2018), PR (Almeida et al., 2019; Sou- za et  al., 2019) and Tocantins (TO) (Guarda et  al., 2020b) (Figure 3). Studies carried out in RS detected outliers between 0.38 and 2.18 μg L– 1 (Bortoluzzi et  al., 2006), from 0.55 to 2.59 μg L– 1 (Bortoluzzi et  al., 2007) and from 0.17 to 0.82 μg L– 1 (Severo et  al., 2020). In Bortolu- zzi et al. (2006, 2007), the high concentrations found were justified by the increase in the use of imidacloprid to replace other insecticides that were used in tobacco cultivation; whereas in Severo et al. (2020), although the meteorological conditions of the collection were not re- ported, it was possible that extreme rainfall events had occurred, since high concentrations can be recorded after heavy rainfall (Pérez et  al., 2017). There was no detection in a study carried out in SP (Barizon et al., 2020). Lambda-cyhalothrin, a synthetic pyrethroid insecticide that mim- ics the insecticidal properties of natural pyrethrin (Sharma et al., 2021), has annual sales in Brazil of approximately 1241 tons. It was detected in the region of Guaíra (SP) at concentrations of 0.1 and 0.2 μg L– 1 and an outlier of 5.66 μg L– 1 (Filizola et al., 2002). There was no detection in a study carried out in Sergipe (SE) (Pinheiro and Andrade, 2009). Methomyl is widely used due to its broad-spectrum properties (He  et  al., 2022) and has average annual sales in Brazil of 6106 tons. It was not detected in any of the 28 samples collected in Formoso River (PR) (Guarda et al., 2020c). Tebuthiuron, an herbicide widely used in sugarcane crops (Teixeira et al., 2018), has average annual sales in Brazil of 3475 tons. Its occur- rence was reported in SP (Monteiro et  al., 2014), PR (Almeida et  al., 2019), and MT (Sposito et  al., 2018) at concentrations between 0.01 and 0.05 μg L– 1 (Figure 3) and outliers from 0.06 to 0.18 μg L– 1 (Almei- da et al., 2019). There was no detection in another study carried out in SP (Barizon et al., 2020) and no quantitation in PR (Souza et al., 2019). Pesticide occurrence in Brazilian groundwater The risk of groundwater contamination depends on the physico- chemical properties of pesticides, soil properties, hydrological and cli- matic conditions, and the management practices adopted in the crops (Gaona et  al., 2019). We found a total of four studies carried out in groundwater matrices. Clomazone, hexazinone, and imidacloprid had two articles each; azoxystrobin and tebuthiuron only one; and no ar- ticles were found on the other pesticides. Among the pesticides that are more likely to be found in groundwater due to their high leach- ing potential, clomazone, hexazinone, and tebuthiuron were detect- ed. Tebuthiuron was the most detected (F = 100%), although its total number of samples (n = 4) is much lower than the second most found, imidacloprid (F = 35%; n = 40) (Figure 4). Clomazone was quantified in the range of 0.001 to 0.008 μg L– 1 in the southern region of Brazil (Silva et al., 2011) (Figure 4) and in out- liers of 2.68 and 10.84 μg L– 1 (Bortoluzzi et al., 2007), possibly related to the expansion of tobacco farming in RS and the reduction of manual weed control (Bortoluzzi et al., 2007). Hexazinone was quantified in PR at concentrations of 0.04 to 0.11 μg L– 1 (Almeida et al., 2019), not being detected in a study carried out in MT, in which the LOD and LOQ were 2.65 and 8.04 μg L– 1, re- spectively (Duarte et al., 2016). Imidacloprid was detected in PR at concentrations between 0.05 and 0.16 μg L– 1 (Almeida et al., 2019); and in RS in 10 of the 36 samples analyzed, in which outliers between 0.67 and 6.22 μg L– 1 were identi- fied, possibly due to the increased use of this insecticide in the cultiva- tion of tobacco (Bortoluzzi et al., 2007) (Figure 4). The occurrence of tebuthiuron has been reported in PR at concen- trations between 0.01 and 0.02 μg L– 1 (Almeida et al., 2019) (Figure 4). Figure 4 – Pesticide occurrence in Brazilian groundwater. Deus, B.C.T. 296 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 Pesticide occurrence in Brazilian treated water Pesticides can be leached from soils (Singh et  al., 2018) and since conventional treatment processes are generally not effective enough in removing residual pesticides (Elfikrie et al., 2020), they may be found in drinking water. We found eight studies on the tar- get pesticides in treated water: azoxystrobin (N = 5); clomazone, imidacloprid, and tebuthiuron (N = 3); hexazinone (N = 2); and cypermethrin (N = 1). Cypermethrin data were not plotted because they comprise two samples only. No studies were found on the other pesticides. It is worth mentioning that the frequency of detection in treated water was lower than in the two environmental matrices previously addressed. The top-selling pesticide, imidacloprid, had the second-highest frequency of detection (F = 12.8%) and, as in surface water, it was ob- served that the least selling product, in this case, hexazinone, was not detected (Figure 5). Once again, these results were in line with the ex- pectations since less intense commercialization implies a lower proba- bility that the pesticide will be found in the environment. Azoxystrobin was found at concentrations between 0.001 and 0.002 μg L– 1 in PR (Souza et al., 2019) and SP states (Montagner et al., 2019). This fungicide was not quantified in other studies carried out in PR (Almeida et al., 2019), SP (Montagner et al., 2014), and RS (von Ameln Lovison et al., 2021) (Figure 5). Clomazone was quantified in RS at an average concentration of 0.063 μg L– 1 in 4 of the 10 samples analyzed (Caldas et al., 2013). It was not detected in other studies carried out in the southern region (Primel et al., 2010; Souza et al., 2019) (Figure 5). Hexazinone was not quantified in any of the 24 samples collected in the Tibagi River (PR) (Souza et al., 2019). Imidacloprid was found at concentrations between 0.01 and 0.02 μg L– 1 in studies carried out in PR (Almeida et al., 2019; Souza et al., 2019), and it was not quantified in RS (von Ameln Lovison et al., 2021) (Figure 5). Cypermethrin was not detected in any of the two samples collect- ed in MG (Rodrigues et al., 2018). Studies related to tebuthiuron were conducted in PR (Souza et  al., 2019) and SP (Monteiro et  al., 2014); however, it was only quantified in the SP study (at a concentration of 0.01 μg L– 1, in filtered water). After treatment, tebuthiuron was at levels lower than LOQ (Monteiro et al., 2014). Human health effects Pesticides are considered highly toxic as they persist in the environment and tend to accumulate in organisms (Porter et  al., 2018). In humans, the effects are diverse, such as cancer, mal- formation, and chromosomal alterations (Sabarwal et  al., 2018). Cypermethrin, an endocrine disruptor (IARC, 2020b) that poses risks to the gastrointestinal system (USEPA, 2020a), is a potential human carcinogen ( USEPA, 2016b). Ethephon can affect the ner- vous system, and thiophanate-methyl the endocrine and repro- ductive systems (USEPA, 2020a). Methomyl, although it can affect the urinary and immune systems (USEPA, 2020a), showed evi- dence of non-carcinogenicity in humans, as did hexazinone and tebuthiuron, which are non-carcinogenic (USEPA, 2020b). While it is not likely to be carcinogenic to humans, lambda-cyhalothrin is neurotoxic (USEPA, 2017). We did not find information on the other pesticides. Due to the adverse effects pesticides can have on human health, it is necessary to remove these contaminants before water is distributed to the population (Mekonen et al., 2016). However, most pesticides are not effectively removed in conventional WTPs (Elfikrie et  al., 2020). Therefore, advanced technologies are required, which must be chosen based on the characteristics of the contaminant (Rodriguez-Narvaez et al., 2017), such as zeolite coated with zero-valent iron nanoparticles (Rashtbari et al., 2020), gamma irradiation (Khedr et al., 2019), mem- brane filtration (Fini et al., 2019), advanced oxidative processes (Mala- kootian et al., 2020), adsorption (Salomão et al., 2021), and ozonation (Cruz-Alcalde et al., 2017). A critical comparison between environmental occurrence and maximum acceptable values in drinking water The compilation of pesticide occurrence data in Brazilian aquatic matrices showed that they are usually present at low con- centrations. However, even small concentrations can be harmful to the health of the population since the toxic potential of pesti- cides can be increased through bioaccumulation and/or biomag- nification (Guarda et al., 2020a). Thus, pesticide toxicity must be analyzed and reference values should be established for the Brazil- ian reality. The reference values for drinking water obtained from international water quality agencies and guidelines are shown in Table 1. Four of the target pesticides of this study are listed in at least one of the water quality agencies/guidelines considered (Table 1).Figure 5 – Pesticide occurrence in Brazilian treated water. Priority pesticides not covered by GM Ordinance of the Ministry of Health No. 888, of 2021, on water potability standard in Brazil 297 RBCIAMB | v.57 | n.2 | June 2022 | 290-301 - ISSN 2176-9478 Pesticides WHO US EPA EU Australia Canada NZ Surface water Groundwater Treated water MC MOE MC MOE MC MOE Cypermethrin * - - 200 - - ND WS ND Hexazinone - - - 400 - 400 0.03 13333.3 0.11 3636.36 NQ Methomyl * - - 20 - - ND WS WS Thiophanate methyl - - - 90 - - WS WS WS Table 1 – Reference Values (μg/L), maximum concentration found, and margin of exposure in drinking water. EU: European Union; NZ: New Zealand; MC: Maximum concentration found; MOE: Margin of exposure; -guide value not presented/not included in the legislation; *pesticide has no guide value as it is unlikely to be found in drinking water; ND: not detected; NQ: not quantified; WS: without studies in the matrix of interest. Source: WHO (2017), European Parliament (2020), Health Canada (2020), New Zealand (2020), NHMRC (2021) and USEPA (2021). MOE calculation was not possible for pesticides that did not have a MAV (azoxystrobin, clomazone, ethephon, imidacloprid, lambda-cy- halothrin, MSMA, and tebuthiuron). It is worth mentioning that in some cases, even when a MAV was available, we could not calculate the MOE in cases with no detection/quantitation (cypermethrin and methomyl); when the only detectable concentration referred to an out- lier; and when associated studies were lacking (thiophanate-methyl) (Table 1). It was only possible to establish the MOE for hexazinone and, for both surface water and groundwater, the values were above 10 (Table 1), indicating a small probability that adverse health effects will occur (USEPA, 2016a). This result is possibly due to concentrations as high as MAV were not reported and, for cases in which the occur- rence was higher, as for imidacloprid, no associated MAV was found. Considering that none of the OV exceeded the reference values, and the analysis referring to the MOE showed a satisfactory result, it would be possible to infer that the concentrations found would not be harm- ful to the population’s health. However, despite the occurrence at low levels having the potential to be dangerous, pesticides are not found alone in the environment, and the interaction between them and other substances can increase the adverse effects (Lei et al., 2015). Conclusions The systematic review showed more studies carried out on surface water, followed by treated water and groundwater. We noted that some pesticides had more studies than others, highlighting clomazone in the surface water matrix, and azoxystrobin in the treated water one. No monitoring data were found for ethephon and thiophanate-methyl, probably due to unfavorable environmental dynamics, which reduces their probability of environmental occurrence. Imidacloprid and hex- azinone are the most likely to be found in aquatic matrices. Howev- er, the MOE of the Brazilian population to hexazinone showed that this compound was not found at levels that would potentially cause harm to the population’s health. Nevertheless, it is recommended to continue monitoring this and other pesticides in the water and analyze the risks associated with a mixture of pesticides. We conclude that the target pesticides pose a low risk to human health. However, some objections must be raised, especially for cypermethrin, because it is a potential carcinogen. Due to MSMA’s favorable environmental dynamics, it is necessary to monitor it. Furthermore, it is important to carry out tox- icological studies for pesticides for which a MAV has not been found, such as imidacloprid. 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