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Article

Groundwater Contamination by Gas Stations in Two Eastern Amazonian Towns (Northern Brazil)

by
Pedro Chira
1,*,
Rosivaldo Mendes
2,
Stephen Ferrari
3,
Cassia Rocha
2,
Elisama da Silva
1,
Jarlana Farias
1 and
Raerida do Carmo
1
1
Instituto de Estudos Costeiros, (IECOS), Universidade Federal do Pará, Bragança 68600-000, Pará, Brazil
2
Instituto Evandro Chagas/Ministério da Saúde (IEC/SVS/MS), Ananindeua 67030-000, Pará, Brazil
3
Department of Ecology, Universidade Federal de Sergipe, São Cristóvão 49000-100, SE, Brazil
*
Author to whom correspondence should be addressed.
Appl. Sci. 2024, 14(13), 5529; https://doi.org/10.3390/app14135529
Submission received: 14 April 2024 / Revised: 22 May 2024 / Accepted: 18 June 2024 / Published: 26 June 2024
(This article belongs to the Section Environmental Sciences)
Browse Figures
Versions Notes

Abstract

:
The present study analyzed the presence of the principal volatile compounds of the BTEX type (benzene, toluene, ethylbenzene, and xylene [o-, m- and p-xylene]) in samples of water from wells located at residences and gas stations in two Amazonian towns—Tracuateua and Augusto Corrêa—in the Amazon region of northern Brazil. This innovative study is extremely relevant to the Amazonian towns surveyed, given that they lack systematic policies for the environmental control of gas stations and any municipal regulations on the quality of water destined for human consumption. A combination of mass spectrometry (MS) and gas chromatography (CG) techniques was applied to analyze these contaminants in 150 samples of local groundwater collected between 2020 and 2024. One of the four BTEX compounds (toluene) was identified in seven of the samples collected (4.66% of the total) at concentrations of 0.14–2.10 µg L−1. The concentrations of contaminants were low, in general. None of the water samples analyzed here presented any critical loss of water quality for human consumption according to the Brazilian legislation concerning BTEX concentrations. Neither of the two towns surveyed in the present study has remediation programs for environmental contamination. The GC-MS approach produced satisfactory results for the assessment of the contamination of underground water reserves by gas stations in both study towns. Further research (e.g., geophysical methods) will be necessary to determine the source of the contamination and its connection with the levels of toluene identified in the underground water sampled in these Amazonian towns.

1. Introduction

Water is a vital resource for humans and is present in most aspects of modern life, ranging from the basic physiological needs of human beings to economic activities, such as farming, industrial production, and the generation of electricity [1]. Conflicts over land and access to water, the indiscriminate exploitation of underground water sources, the lack of basic sanitation, and the inadequate management of forestry resources are all part of the major environmental problems in the northern Amazonian region of Brazil [2].
In the specific case of the northern Brazilian state of Pará, the past few decades have been marked by the progressive growth in the exploitation of natural resources. While anthropogenic modifications have yet to have irreversible impacts on the availability of water in the Brazilian Amazon region, the progressive growth of the pressures that affect the vulnerable local ecosystems area has been increasingly restrictive of the potential for social development and environmental sustainability [3].
The hydrographic basin of the Caeté River is located in the northeastern extreme of Pará and partially drains the areas of seven municipalities—Bonito, Santa Luzia do Pará, Ourém, Capanema, Tracuateua, Bragança, and Augusto Corrêa. The Caeté basin encompasses a number of potential sources of pollution, including (i) open-air refuse disposal; (ii) the lack of a sanitation system or effluent treatment plants; (iii) the discharge of the water used to clean the filters and decanters of the water treatment plant of the town of Bragança directly into the municipality’s primary source of drinking water; and (iv) the lack of adequate measures of environmental control of the gas stations located on the margins of the Caeté River [3].
The principal problems generated by the inadequate management of the gas stations located at or near the margins of the Caeté River include the dilution and dispersal of contaminants derived from petroleum, such as monoaromatic hydrocarbons [4], which affect both underground reservoirs and terrestrial bodies of water and have the potential to affect large areas [3]. Gas stations are important local sources of contamination of the soil and underground water, which occurs primarily in urban areas [5]. The seepage of the hydrocarbons derived from petroleum into the soil is a significant environmental problem, due to the widespread occurrence of leaks and the highly toxic nature of the contaminants that reach the underground waters used for human consumption [5,6]. These sources of contamination, contaminants derived from gasoline in particular, may also affect large numbers of workers and local residents in the area surrounding the gas stations [7,8,9,10].
Leaks at gas stations, caused by problems with the underground storage tanks and their pipes (ruptures, corrosion) or during the transportation of petroleum products, may cause serious environmental problems [11,12,13,14,15,16,17,18]. Even minor fuel leaks may contaminate shallow underground water sources [19]. These leaks may also arise due to the constant and almost uninterrupted handling of fuels [3,7,20].
The principal volatile organic compounds found in the soil and groundwater as the result of leaks from gas stations are the monoaromatic hydrocarbons or BTEX compounds (benzene, toluene, ethylbenzene, and xylene [o-, m- and p-xylene]) [21]. These substances are abundant in petroleum (e.g., fuel oil and gasoline) and petrochemical products [21,22,23].
BTEX substances are extremely toxic, and, once they are released into the environment, they evaporate rapidly into the air. These substances, as well as numerous other petroleum products, represent the fraction of crude oil that is most mobile and soluble in water [24,25,26,27,28]. BTEX petroleum products spread easily from sources of contamination [21]. A number of different types of detectors have been employed to determine the BTEX concentrations in field samples, in particular gas chromatography (GC) and mass spectrometry (MS) [29,30,31,32].
In 2022, Brazil had 43,266 gas stations officially in operation. Approximately 8.3% of these stations were operating in the north of Brazil, and 3.3% (1442 stations) were in the state of Pará [33]. In addition to these official statistics, it seems likely that a number of illegal establishments also operate in the country and would obviously not be included in the statistics. These gas stations may be contaminating the soil and bodies of water, causing profound impacts on the local environment [14,34].
In Brazil, gas stations are typically located in commercial or residential zones, where they may have a direct effect on the health of the residents living in adjacent areas [35]. Ordinance number 888/2021 of the Brazilian Health Ministry [36] defines the maximum permissible concentrations of organic substances in drinking water that represent a risk to public health.
The present study provides an innovative analysis of the potential contamination of underground water reserves by gas stations in the towns of Tracuateua and Augusto Corrêa in eastern Brazilian Amazonia, where no environmental control measures are employed by the local authorities for the regulation of gas stations. Samples of underground water collected from gas stations and their surroundings in these towns were studied using mass spectrometry (MS) and gas chromatography (GC) to identify possible contamination by monoaromatic hydrocarbons (BTEX compounds).

2. Materials and Methods

The present study was conducted in two towns located in eastern Brazilian Amazonia. These towns—Tracuateua, and Augusto Corrêa—are both within the Northeastern Pará Mesoregion in northern Brazil (Figure 1). The town of Tracuateua (01°05′26″ S, 46°54′34″ W) has an estimated population of 28,595 inhabitants, while Augusto Corrêa (01°01′19″ S, 46°38′42″ W) has a population of approximately 44,573 inhabitants [37].
Rainfall levels fluctuate considerably over the year in Pará, which has a rainy season lasting from December to May in most locations and a less rainy (or dry) season that is generally from June to November, with October having the least rainfall. The region has mean rainfall levels ranging from 965 to 2744 mm (rainy season) and from 230 to 666 mm in the dry season [38].
The towns that were the focus of the present study are located on the Bragança coastal plain, in the northeastern extreme of Pará state, and have an Am2 type climate, in the Köppen classification system, which is hot and humid [39], with a moderate water deficiency between July and December. Temperatures range annually between 18 °C (minimum) and 33 °C (maximum), with a general mean of 27 °C. Temperatures are typically highest between August and October. The principal local winds are the trade winds, which blow predominantly from the northeast, reaching maximum speeds of up to 7.5 m s−1 [40].
Applsci 14 05529 g001
Figure 1. Study areas surveyed in two Amazonian towns, in northern Brazil. Sources [41,42].
Figure 1. Study areas surveyed in two Amazonian towns, in northern Brazil. Sources [41,42].
Applsci 14 05529 g001

2.1. Collection of the Water Samples and the BTEX Detection Procedures

Samples of groundwater were collected during 10 different campaigns at gas stations and their surrounding areas in both Amazonian towns during 2020, 2021 (rainy and dry seasons), 2022, 2023 (rainy, rainy–dry, and dry seasons), and 2024 (rainy season). In the present study, 150 water samples were collected (30 in Tracuateua and 120 in Augusto Corrêa, Figure 1) for the analysis of the concentrations of BTEX contaminants.
The water samples were collected from boreholes with faucets installed, which were located at gas stations and in the areas surrounding these stations. The available database [43] and informal interviews with local well-diggers confirmed that the water table of the two study areas was located at a depth of approximately 10 m.
For the collection of a sample, the borehole faucet was opened for approximately 2–3 min to eliminate the standing water in the pipes and to remove the dirt, air, and other residues present in the piping. Prior to being turned on, the faucets were disinfected with sodium hypochlorite solution (100 mg L−1) and then washed to remove any residues of this disinfectant before the collection of the water samples.
The samples of underground water were collected in 100 mL amber glass flasks, which had been washed, sterilized, sealed, labeled, and stored in sterilized coolers containing ice gel packs for transportation to the laboratory, to ensure that the monoaromatic hydrocarbons were not volatilized unintentionally. These flasks were sent within 24 h for analysis at the Toxicology Laboratory of the Environment Sector of the Evandro Chagas Institute (Brazilian Ministry of Health) in the city of Belém, the Pará state capital. The procedures of the 21st edition of the Standard Methods for the Examination of Water and Wastewater, method SM-6010 B [44], and the National Waters Agency/Brazilian Ministry of the Environment [45] were adopted for the preservation of the samples collected here.
Gas chromatography (GC) is the principal technique used to separate and analyze volatile compounds. This procedure has been used to analyze gases, liquids, and solids, although the latter are generally dissolved in some type of volatile solvent. Both organic and inorganic substances can be analyzed using GC [46]. The principal detectors used for gaseous-phase chromatography are flame ionization, thermal conductibility, electron capture, mass spectrometry, photoionization, flame photometry, nitrogen-phosphorus detection, and atomic emission detection [47,48]. The combination of GC with mass spectrometry (GC/MS) is often considered to be ideal for the detection and quantification of volatile and semi-volatile organic compounds, including the concentrations of petroleum-based volatile organic hydrocarbon compounds (pH-VOCs) and BTEX compounds in samples of water [29,31,46,49,50].

2.2. Experimental Procedures

The automated headspace (HS) method, based on the D 6040 procedure [51], was applied to extract the BTEX compounds from the samples of underground water collected in the field. An aliquot of 15 mL was extracted from the 100 mL of each sample and placed in a 20 mL flask, which was sealed with an aluminum seal and Teflon septum. The samples were then wrapped in aluminum blocks, placed in a Triplus RSH autosampler (Thermo Scientific, Waltham, MA, USA), and heated to 80 °C for 10 min.
The BTEX compounds were quantified with a Trace 1300 gas chromatograph (Thermo Scientific, Waltham, MA, USA) coupled to a TSQ 8000 mass spectrometer (Thermo Scientific). A TG-5 MS column (Thermo Scientific) was used here, which was composed of 5% phenyl and 95% dimethyl siloxane, with a 30 m × 0.32 mm × 0.25 µm film. The oven temperature of the column was 40 °C for 1 min, raised to 70 °C, at 5 °C per minute, and finally to 70–220 °C at 30 °C per minute.
The carrier gas was helium (99.999% pure) used at a flow rate of 1.0 mL min−1. The injector was operated at 280 °C in split mode. The transfer line temperature was 250 °C, and the ion source was present at 230 °C. A 1000 µL aliquot of the sample contained in the headspace was injected into the chromatograph.
The quantification limits (QLs) for the BTEX contaminants were 0.05 μg L−1 for B, E, and X, and 0.1 μg L−1 for T.

2.3. Data Analysis

All the samples were analyzed in duplicate, and the mean BTEX concentration is used to represent each sample. The concentrations of the BTEX contaminants analyzed in the present study were compared with the maximum value allowed (MVA) in drinking water in accordance with ordinance No. 888/2021 of the Brazilian Health Ministry [36]. The MVAs are 5 μg L−1 for B, 30 μg L−1 for T, 300 μg L−1 for E, and 500 μg L−1 for X [36].

3. Results

A total of 150 water samples were collected during each sampling period over the course of the present study between 2020 and 2024 (Table 1). Only 7 of the 150 samples were contaminated with BTEX.
A total of 15 samples were collected in December 2020 (rainy season). The first three samples were obtained from the area adjacent to two gas stations in Tracuateua. In Augusto Corrêa, a further 12 samples were collected from four gas stations for the evaluation of potential contamination by BTEX. All the concentrations were below the QL in all the samples collected in this first session. None of the samples from this period can be considered to have been contaminated in excess.
A total of 45 samples were collected in 2021 (from both study towns) in March (rainy season, 15 samples), July (the rainy–dry transition, 15 samples), and October 2021 (dry season, 15 samples), although all the samples were below the QL for any BTEX compound in the combined GC/MS. Once again, contamination was not confirmed in any of the samples according to the MVAs of the Brazilian Health Ministry [36].
In the fifth sampling session (15 samples, January 2022, rainy season), toluene (2.10 µg L−1) was detected by GC/MS in 1 sample, A07, from gas station P14 (1°01′33.01″ S, 46°38′48.06″ W) in Augusto Corrêa. This sample was above the QL, but contamination was not confirmed in terms of the MVA defined by Brazilian legislation [36]. BTEX were not detected in any of the other samples collected from the two study towns during this season.
In Tracuateua, during the sixth sampling session (12 samples collected) in July 2022 (rainy–dry transition), 2 samples, A24 (0.141 µg L−1) and A25 (0.167 µg L−1), from gas station P12 contained toluene (Table 2). Neither of these samples exceeded the maximum values permitted by the Brazilian legislation [36].
Three of the samples collected in Augusto Corrêa (sample A06 from gas station P14, and samples A10 and A11 from station P15, July 2022) had toluene concentrations that were above the QL, between 0.14 µg L−1 and 0.236 µg L−1 (Table 3). None of the samples collected in Augusto Corrêa during this period exceeded the permitted thresholds for any of these substances [36].
In the seventh sampling session (15 samples, November 2022, dry season), toluene (0.664 µg L−1) was detected by GC/MS in a single sample, A06, from a residence near gas station P14 (1°01′32.84″ S, 46°38’48.59″ W) in Augusto Corrêa. This sample was above the QL but below the Brazilian legal MVA [36]. No other BTEX contaminants were detected in the other water samples collected from either of the two Amazonian towns during this period. The chromatogram of sample A06 (Figure 2) presents a clear toluene signal (retention time: 8.72 min). All the other samples presented values below the quantification limit.
In the eighth, ninth, and tenth sessions, conducted in April and August 2023 and March 2024, in the towns of Tracuateua and Augusto Corrêa, all the samples were found to be below the quantification limits for BTEX using the combined CG/MS technique.

4. Discussion

BTEX compounds are the contaminants found most frequently in environmental disasters. These compounds are commonly found in gasoline and other derivatives of petroleum and make up a major part of its soluble fraction [11,52,53]. The percentage per weight of BTEX in gasoline is 11% benzene, 26% toluene, 11% ethylbenzene, 31% meta-xylene, 12% ortho-xylene, and 9% para-xylene [54].
One of the principal sources of contamination of the subsoil and underground waters is the accidental release of petroleum-based fuels from storage tanks or pipelines [11,55]. These highly toxic compounds tend to enter the environment through spills or leaks and then spread rapidly. These accidental discharges typically occur in the vicinity of oil and gas wells, fuel stations, and storage tanks, e.g., [14,16,17,56,57,58].
These substances are highly volatile and are extremely similar to one another in their physicochemical characteristics (e.g., solubility, volatility) and their dispersal routes into the environment [22,59]. The maximum BTEX concentrations (mg L−1) that can dissolve in pure water at a specific temperature (25 °C) are 1740–1860 mg L−1 of benzene, 500–627 mg L−1 of toluene, 131–208 mg L−1 of ethylbenzene, and 167–196 mg L−1 of xylene, e.g., [16,22,60]. The solubility of these substances in water greatly affects their movement and their dispersal through the soil and underground water [54]. BTEX contaminants are dangerous substances, given their enormous capacity for movement through water, the ground, and the air, due to the density, solubility, and molecular weight of these compounds [61].
Each compound may provoke a specific type of toxicological damage, with benzene, for example, having deleterious impacts on the hematopoietic, central nervous, and reproductive systems, while toluene may provoke damage to the hematopoietic and reproductive systems. Ethylbenzene and xylene, in turn, may cause disorders of the respiratory and neurological systems [9]. Benzene is considered to be the most toxic and dangerous compound of the BTEX group and is a major risk factor for the development of cancer [7].
In a study of underground water reserves in northern Fortaleza, a city in northeastern Brazil [62], samples were collected from tubular wells at gas stations and in the surrounding area. In this study, ethylbenzene and o-xylene had the highest concentrations of the compounds analyzed.
Ref. [63] applied the CG/SM approach in their investigation of contamination by BTEX at six points, using samples of underground water collected from wells excavated at a gas station with a history of leaks in the metropolitan region of Yogyakarta, in Indonesia. In this study, the majority of the BTEX components were found in the samples at concentrations of between 0.008 and 25.631 µg L−1. The concentration of benzene at one of the sampling points exceeded the threshold for drinking water established by both the Indonesian government and the WHO.
Ref. [64] investigated the existence of BTEX in samples of shallow underground water from 16 wells monitored in the region of Songyuan, in the basin of the Songhua River in China. The mean BTEX concentrations were 1.53 µg L−1 (B), 1.76 µg L−1 (T), 2.11 µg L−1 (E), and 0.30 µg L−1 (X).
Ref. [65] also applied the GC/MS approach to analyze the occurrence of BTEX contaminants in samples of underground and surface waters in the city of Guangzhou, in the Chinese province of Guangdong, but found that the samples were within the legal thresholds. A proportion (14.63%) of the samples was contaminated, with concentrations of less than 9.5 µg L−1. Toluene (12.20% of the samples) and benzene (3.65%) were the predominant contaminants.
Ref. [66] evaluated the degree of contamination of the subsoil in the vicinity of an oil spill in the town of Osubi, in Okpe, the Delta state, in southeastern Nigeria. The study integrated the geoelectrical resistivity method (1D, 2D, and 3D techniques) with the geochemical approach and detected plumes of contamination provoked by the spillage of oil and total petroleum hydrocarbons (TPHs), poly-aromatic hydrocarbons (PAHs), and BTEX contaminants at high concentrations in the samples of underground water collected from the study site.
Ref. [67] evaluated the occurrence of BTEX contamination in the subsoil of gas stations and adjacent residences in the eastern Amazonian town of Bragança, combining ground-penetrating radar (GPR) with GC/MS. That study identified the presence of the BTEX contaminants benzene, toluene, ethylbenzene, and/or xylene in 13 of the samples of underground water (19.7% of the total) and found evidence of the possible existence of plumes of BTEX contamination in the subsurface of the gas stations, confirming that leaks in the storage tanks were the source of the contamination.
While toluene was the only BTEX contaminant detected in the present study, the concentrations were low and within the MVAs established for this compound by the Brazilian Health Ministry. Even so, it is important to consider that even a minimal level of contamination serves as a warning call, which highlights the need for continued monitoring. Further research is also needed to identify the source of the contamination of the subsurface in the two study towns, using, for example, geophysical tools, which have been shown to be highly effective for the identification of underground plumes of BTEX contamination, contributing to the verification of possible sources of contamination, e.g., [66,67].

5. Conclusions

In the present innovative study in two towns of northeastern Pará (Brazil), one contaminant (toluene) was detected in approximately 4.66% of the samples of underground water analyzed. This contaminant was recorded, in varying proportions, in both towns. Overall, 6.66% of the samples collected in Tracuateua contained toluene and 4.16% in Augusto Corrêa. The combination of analytical techniques (GC-MS) provided satisfactory results, which revealed the presence of only one of the monoaromatic hydrocarbons (toluene), contrasting with the findings of the Amazonian town of Bragança, where all the BTEX compounds were recorded.
The Amazonian towns studied here lack effective environmental control measures for their gas stations, which represent an important potential source of contamination due to the existence of storage tanks varying in age from 11 to 15 years in Augusto Corrêa and from 7 to 21 years in Tracuateua, as well as the continuous and almost uninterrupted handling of fuels, which may contribute to the contamination of the local subsoil and sources of water.
Even so, the occurrence of BTEX contaminants recorded in the present study was low, and no critical loss of water quality was detected. The concentrations were within the values permitted by the Brazilian legislation for BTEX in drinking water. The presence of these compounds in the water is nevertheless worrisome and highlights the need for additional monitoring, given the potential risks of exposure for both gas station employees and local residents where the presence of BTEX was detected.
Given the growing need for adequate criteria for the evaluation of water quality, the continued monitoring of the towns surveyed in the present study will be extremely important, as will the adequate supervision of local environmental agencies, to ensure their capacity to remediate future spills of petroleum compounds, either from leaks from existing storage tanks or accidents during the installation of new infrastructure.
Monitoring is necessary and recommended to identify the status of the subsoil of gas stations and the surrounding areas. This monitoring will ensure the detection of possible changes in the contamination levels in the areas in which BTEX compounds have been detected.
Ultimately, the eventual application of integrated geophysical methods (e.g., GPR, Vertical Electrical Surveying [VES], and Resistive Electrical Tomography [ERT]) to the analysis of the subsurface of the gas stations surveyed here would help to determine whether the contamination is in fact derived from the underground storage tanks and establish a connection with the levels of toluene recorded in the present study.

Author Contributions

Conceptualization, P.C., R.M., S.F. and C.R.; methodology: P.C., R.M. and C.R.; validation: P.C., R.M. and C.R.; formal analysis: P.C., R.M., S.F., C.R., E.d.S., J.F. and R.d.C.; investigation: P.C., R.M. and C.R.; resources: P.C. and R.M.; data curation: P.C.; writing—original draft: P.C., R.M., S.F. and C.R.; writing—review and editing: P.C., R.M., S.F., C.R., E.d.S., J.F. and R.d.C.; supervision: P.C. and R.M. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by the Dean of Research and Posgraduation Studies—PROPESP/Federal University of Pará—UFPA (Brazil).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The original contributions presented in the study are included in the article, further inquiries can be directed to the corresponding author.

Acknowledgments

The authors would like to thank the Dean’s Office of Research and Graduate Studies (PROPESP) of the Federal University of Pará (UFPA) for financial support through the concession of scholarships for the fieldwork in the two eastern Amazonian towns in northern Brazil.

Conflicts of Interest

The authors declare no conflicts of interest.

References

  1. Gusmão, L.H.A.; Homma, A.K.O.; Watrin, O.S. Análise cartográfica da concentração do cultivo de mandioca no estado do Pará, Amazônia brasileira. Geogr. Ensino Pesqui. 2016, 20, 51–62. [Google Scholar] [CrossRef]
  2. BRASIL Ministério do Meio Ambiente. Caderno da Região Hidrográfica Amazônica; BRASIL Ministério do Meio Ambiente: Brasília, Brazil, 2006; 132p. [Google Scholar]
  3. Gorayeb, A.; Pereira, L.C.C. Análise Integrada das Paisagens de Bacias Hidrográficas na Amazônia Oriental; Imprensa Universitária da Universidade Federal do Ceará (UFC): Fortaleza, Brazil, 2014; 108p. [Google Scholar]
  4. BRASIL Ministério da Saúde. Sistema de Informação da Atenção Básica—SIAB: Indicadores 2004; Ministério da Saúde: Brasília, Brazil, 2005. [Google Scholar]
  5. Bertolo, R.; Alves, C.C.; Maximiano, A. Áreas contaminadas. In Geologia de Engenharia e Ambiental: Aplicações, 1st ed.; Oliveira, A.M.S., Monticeli, J.J., Eds.; ABGE—Associação Brasileira de Geologia de Engenharia e Ambiental: São Paulo, Brazil, 2018; Volume 3, pp. 227–252. [Google Scholar]
  6. Caetano, M.O.; Schneider, I.A.H.; Gomes, L.P.; Kieling, A.G.; Miranda, L.A.S. A compact remediation system for the treatment of groundwater contaminated with BTEX and TPH. Environ. Technol. 2017, 38, 1408–1420. [Google Scholar] [CrossRef] [PubMed]
  7. Figueiredo, V.O.; Carvalho, L.V.B.D.; Borges, R.M.; Costa-Amaral, I.C.; Santos, M.V.C.D.; Rosa, A.C.S.; Menezes, M.A.C.D.; Mattos, R.D.C.O.D.C.; Sarcinelli, P.N.; Alves, S.R.; et al. Avaliação da exposição a BTEX em postos de revenda de combustíveis no Rio de Janeiro, Brasil, e os riscos à saúde do trabalhador. Cad. Saúde Pública 2021, 37, e00351520. [Google Scholar] [CrossRef]
  8. Amaral, I.C.C.; Carvalho, L.V.B.D.; Pimentel, J.N.D.S.; Pereira, A.C.; Vieira, J.A.; Castro, V.S.D.; Borges, R.M.; Alves, S.R.; Nogueira, S.M.; Tabalipa, M.D.M.; et al. Avaliação ambiental de BTEX (benzeno, tolueno, etilbenzeno, xilenos) e biomarcadores de genotoxicidade em trabalhadores de postos de combustíveis. Rev. Bras. Saude Ocup. 2017, 42, e8s. [Google Scholar] [CrossRef]
  9. Tunsaringkarn, T.; Siriwong, W.; Rungsiyothin, A.; Nopparatbundit, S. Occupational exposure of gasoline station workers to BTEX compounds in Bangkok, Thailand. Int. J. Occup. Environ. Med. 2012, 3, 117–125. [Google Scholar]
  10. Österreicher-Cunha, P.; do Amaral Vargas, E., Jr.; Guimarães, J.R.D.; de Campos, T.M.P.; Nunes, C.M.F.; Costa, A.; dos Santos Antunes, F.; da Silva, M.I.P.; Mano, D.M. Evaluation of bioventing on a gasoline-ethanol contaminated undisturbed residual soil. J. Hazard. Mater. 2004, 110, 63–76. [Google Scholar] [CrossRef]
  11. Bian, Y.; Zhang, Y.; Zhou, Y.; Feng, X.-S. BTEX in the environment: An update on sources, fate, distribution, pretreatment, analysis, and removal techniques. Chem. Eng. J. 2022, 435, 134825. [Google Scholar] [CrossRef]
  12. Popitanu, C.; Cioca, G.; Copolovici, L.; Iosif, D.; Munteanu, F.D.; Copolovici, D. The easonality impact of the BTEX pollution on the atmosphere of arad city, Romania. Int. J. Environ. Res. Public Health 2021, 18, 4858. [Google Scholar] [CrossRef]
  13. Baghani, A.N.; Sorooshian, A.; Heydari, M.; Sheikhi, S.; Golbaz, Q.; Ashournejad, M.; Kermani, F.; Golkhorshidi, A.; Barkhordari, A.J.; Jafari, M.; et al. A case study of BTEX characteristics and health effects by major point sources of pollution during winter in Iran. Environ. Pollut. 2019, 247, 607–617. [Google Scholar] [CrossRef]
  14. Lins, E.A.M.; de Souza, R.B.R. Btex contaminated area diagnosis and mapping: Case study. Int. J. Dev. Res. 2019, 9, 31548–31553, ISSN 2230-9926. [Google Scholar]
  15. Hadei, M.; Hopke, P.K.; Rafiee, M.; Rastkari, N.; Yarahmadi, M.; Kermani, M.; Shahsavani, A. Indoor and outdoor concentrations of BTEX and formaldehyde in Tehran, Iran: Effects of building characteristics and health risk assessment. Environ. Sci. Pollut. Res. 2018, 25, 27423–27437. [Google Scholar] [CrossRef] [PubMed]
  16. Fayemiwo, O.M.; Daramola, M.O.; Moothi, K. BTEX compounds in water—Future trends and directions for water treatment. Water SA 2017, 43, 602–613. [Google Scholar] [CrossRef]
  17. Rao, S.M.; Joshua, R.E.; Arkenadan, L. BTEX contamination of Bengaluru aquifers, Karnataka, India. J. Environ. Eng. Sci. 2017, 12, 56–61. [Google Scholar] [CrossRef]
  18. IARC—International Agency for Research on Cancer. World Cancer Report 2014; Stewart, B.W., Wild, C.P., Eds.; World Health Organization: Genève, Switzerland, 2014; 630p. [Google Scholar]
  19. Day, M.J.; Reinke, R.F.; Thomson, J.A.M. Fate and Transport of Fuel Components Below Slightly Leaking Underground Storage Tanks Technical Note. Environ. Forensics 2001, 2, 21–28. [Google Scholar] [CrossRef]
  20. Su, F.; Lu, C.; Johnston, K.R.; Hu, S. Kinetics, Thermodynamics, and Regeneration of BTEX Adsorption in Aqueous Solutions via NaOCl-Oxidized Carbon Nanotubes. In Environanotechnology; Fan, M., Huang, C.-P., Bland, A.E., Wang, Z., Slimane, R., Wright, I., Eds.; Elsevier B.V.: Amsterdam, The Netherlands, 2010; pp. 71–97. [Google Scholar] [CrossRef]
  21. Ding, L.; Cupples, A.M. The effect of the potential fuel additive isobutanol on benzene, toluene, ethylbenzene, and p-xylene degradation in aerobic soil microcosms. Environ. Technol. 2015, 36, 237–244. [Google Scholar] [CrossRef] [PubMed]
  22. El-Naas, M.H.; Acio, J.A.; El Telib, A.E. Aerobic biodegradation of BTEX: Progresses and Prospects. J. Environ. Chem. Eng. 2014, 2, 1104–1122. [Google Scholar] [CrossRef]
  23. Lee, M.-R.; Chang, C.h.-M.; Dou, J. Determination of benzene, toluene, ethylbenzene, xylenes in water at sub-ng l−1 levels by solid-phase microextraction coupled to cryo-trap gas chromatography–mass spectrometry. Chemosphere 2007, 69, 1381–1387. [Google Scholar] [CrossRef]
  24. Wongbunmak, A.; Khiawjan, S.; Suphantharika, M.; Pongtharangkul, T. BTEX biodegradation by Bacillusamyloliquefaciens subsp. Plantarum W1 and its proposed BTEX biodegradation pathways. Sci. Rep. 2020, 10, 17408. [Google Scholar] [CrossRef]
  25. Ukoha, P.O.; Ekere, N.R.; Timothy, C.L.; Agbazue, V.E. Benzene, toluene, ethylybenzene and xylenes (btex) contamination of soils andwater bodies from alkyd resin and lubricants industrial production plant. J. Chem. Soc. Niger. 2015, 40, 51–55. [Google Scholar]
  26. Menghini, L.N.; da Silva, M.N.; Cariús, R.; Vidal, C.B.; Raulino, G.S.C.; Liberato, M.A.; Milhome, R.F.d.N. Validação de metodologia para análise de BTEX em água produzida por cromatografia a gás acoplado a espectrômetro de massas usando extração por headspace. Rev. Anal. 2014, 70, 70–86. [Google Scholar]
  27. Nadim, F.; Hoag, G.E.; Liu, S.; Carley, R.J.; Zack, P. Detection and remediation of soil and aquifer systems contaminated with petroleum products: An overview. Pet. Sci. Eng. 2000, 26, 169–178. [Google Scholar] [CrossRef]
  28. Saeed, T.; AI-Mutairi, M. Chemical composition of the water soluble fraction of the leaded gasolines in seawater. Environ. Int. 1999, 25, 17–129. [Google Scholar] [CrossRef]
  29. Wang, L.; Cheng, Y.; Wu, C.; Luo, F.; Lin, Z.; Naidu, N. Rapid on-site detection of underground petroleum pipeline leaks and risk assessment using portable gas chromatography-mass spectrometry and solid phase microextraction. J. Chromatogr. A 2023, 1696, 463980. [Google Scholar] [CrossRef] [PubMed]
  30. Agilent. Gas Chromatography Fundamentals. Available online: https://www.agilent.com/en/product/gas-chromatography/what-is-gas-chromatography (accessed on 20 April 2024).
  31. Pascale, R.; Bianco, G.; Calace, S.; Masi, S.; Mancini, I.M.; Mazzone, G.; Caniani, D. Method development and optimization for the determination of benzene, toluene, ethylbenzene and xylenes in water at trace levels by static headspace extraction coupled to gas chromatography–barrier ionization discharge detection. J. Chromatogr. A. 2018, 1548, 10–18. [Google Scholar] [CrossRef] [PubMed]
  32. Liaud, C.; Nguyen, N.T.; Nasreddine, R.; Le Calvé, S. Experimental performances study of a transportable GC-PID and two thermo-desorption based methods coupled to FID and MS detection to assess BTEX exposure at sub-ppb level in air. Talanta 2014, 127, 33–42. [Google Scholar] [CrossRef] [PubMed]
  33. ANP. Agência Nacional do Petróleo, Gás Natural e Biocombustíveis (Brasil). Anuário Estatístico Brasileiro do Petróleo, Gás Natural e Biocombustíveis. (Brazilian Statistical Yearbook of Petroleum, Natural Gas and Biofuels). Available online: http://www.anp.gov.br (accessed on 14 August 2023).
  34. ANP. Agência Nacional do Petróleo Gás Natural e Biocombustíveis. Anuário Estatístico de Petróleo e do Gás Natural 2017. 2018. Available online: http://www.anp.gov.br (accessed on 10 May 2024).
  35. Correa, S.M.; Arbilla, G.; Marques, M.R.C.; Oliveira, K.M.P.G. The impact of BTEX emissions from gas stations into the Atmosphere. Atmos. Pollut. Res. 2012, 3, 163–169. [Google Scholar] [CrossRef]
  36. BRASIL Ministério da Saúde (Brasil). Portaria no. 888, de 04 de maio de 2021. Dispõe sobre a alteração do Anexo XX da Portaria de Consolidação GM/MS nº 5, de 28 de setembro de 2017, para dispor sobre os procedimentos de controle e de vigilância da qualidade da água para consumo humano e seu padrão de potabilidade (Ministry of Health (Brazil). Ordinance no. 888, of May 4, 2021. Provides for the Amendment of Annex XX of the GM/MS Consolidation Ordinance No. 5, of September 28, 2017, to Provide for Control and Surveillance Procedures for the Quality of Water for Human Consumption and Its Potability Standard). Available online: https://www.in.gov.br/en/web/dou/-/portaria-gm/ms-n-888-de-4-de-maio-de-2021-318461562 (accessed on 7 February 2022).
  37. IBGE. Instituto Brasileiro de Geografia e Estatística, Cidades e Estados (Brazilian Institute of Geography and Statistics. Cities and States). Available online: https://www.ibge.gov.br/cidades-e-estados/pa/ (accessed on 15 March 2022).
  38. Moraes, B.C.D.; Costa, J.M.N.D.; Costa, A.C.L.D.; Costa, M.H. Spatial and temporal variation of precipitation in the state of Pará. Acta Amaz. 2005, 35, 207–214. [Google Scholar] [CrossRef]
  39. Martorano, L.G.; Pereira, L.C.; Cézar, E.G.M.; Pereira, I.C.B. Estudos Climáticos do Estado do Pará, Classificação Climática (Köppen) e Deficiência Hídrica (Thornthwhite, Mather); SUDAM/EMBRAPA, SNLCS: Belém, Brazil, 1993; 53p. [Google Scholar]
  40. INMET. Instituto Nacional de Meteorologia—Ministério da Agricultura, Pecuária e Abastecimento (National Institute of Meteorology—Ministry of Agriculture, Livestock and Supply). Available online: https://portal.inmet.gov.br/ (accessed on 2 August 2020).
  41. IBGE. Instituto Brasileiro de Geografia e Estatística, Cidades (Brazilian Institute of Geography and Statistics. Cities). Available online: http://cidades.ibge.gov.br/xtras/perfil.php?codmun=150010 (accessed on 13 January 2022).
  42. Google Earth Pro. Available online: https://www.google.com/earth/versions/ (accessed on 13 September 2022).
  43. SIAGAS. Sistema de Informações de Águas Subterrâneas—CPRM/Serviço Geológico do Brasil (SGB) (Groundwater Information System-CPRM/Geological Survey of Brazil (SGB)). Available online: https://siagasweb.sgb.gov.br/layout/index.php (accessed on 30 June 2022).
  44. APHA-AWWA-WEF—American Public Health Association/American Water Works Association/Water Environment Federation. Standard Methods for the Examination of Water and Wastewater, 1st ed.; APHA-AWWA-WEF: Washington, DC, USA, 2005. [Google Scholar]
  45. ANA. Agência Nacional de Águas—Ministério do Meio Ambiente (Brasil), Guia nacional de coleta e preservação de amostras (Ministry of the Environment, National Guide for Sample Collection and Preservation). Available online: https://cetesb.sp.gov.br/wp-content/uploads/2021/10/Guia-nacional-de-coleta-e-preservacao-de-amostras-2012.pdf (accessed on 14 April 2022).
  46. McNair, H.M.; Miller, J.M.; Snow, N.H. Basic Gas Chromatography, 3rd ed.; John Wiley & Sons, Inc.: Hoboken, NJ, USA, 2019; 265p. [Google Scholar]
  47. A3 ANALÍTICA. Princípios de Cromatografia a Gás. Available online: https://a3analitica.com.br/bloga3pharma/2019/01/08/principios-da-cromatografia-a-gas-gc/ (accessed on 22 January 2024).
  48. Skoog, D.A.; West, D.M.; Holler, J.; Crouch, S.R. Fundamentos de Química Analítica; Cengage Learning: Boston, MA, USA, 2006; 1124p. [Google Scholar]
  49. Pavón, J.L.P.; del Nogal Sánchez, M.; Laespada, M.E.F.; Cordero, B.M. Simultaneous determination of gasoline oxygenates and benzene, toluene, ethylbenzene and xylene in water samples using headspace-programmed temperature vaporization-fast gas chromatography–mass spectrometry. J. Chromatogr. A 2007, 1175, 106–111. [Google Scholar] [CrossRef] [PubMed]
  50. Bustillos, O.V. A cromatografia a gás acoplada à espectrometria de massas—GC/MS. Rev. Anal. 2020, 105, 28–30. Available online: https://revistaanalytica.com.br/analytica-ed-105/ (accessed on 12 May 2022).
  51. Wallace, R.; Stenerson, K. Method 6040D, Odors in Drinking Water, Using SPME on the Supelco SLB-5ms Capillary Column. Available online: https://www.chromatographyonline.com/view/method-6040d-odors-drinking-water-using-spme-supelco-slb-5ms-capillary-column (accessed on 13 January 2022).
  52. Rodrigo-Ilarri, J.; Rodrigo-Clavero, M.-E.; Capilla, J.E.; Romero-Ballesteros, L. Environmental Assessment of Soil and Groundwater Pollution by BTEX Leaching in Valencia Region (Spain). Water 2023, 15, 3279. [Google Scholar] [CrossRef]
  53. Miri, S.; Espejel-Pérez, J.A.; Kaur Brar, S.; Rouissi, T.; Martel, R. Sustainable production and co-immobilization of cold-active enzymes from Pseudomonas sp. for BTEX biodegradation. Environ. Pollut. 2021, 285, 117678. [Google Scholar] [CrossRef]
  54. Mitra, S.; Roy, P. BTEX: A Serious Ground-water Contaminant. Res. J. Environ. Sci. 2011, 5, 394–398. [Google Scholar] [CrossRef]
  55. Teramoto, E.H.; Chang, H.K. A Screening Model to Predict Entrapped LNAPL Depletion. Water 2020, 12, 334. [Google Scholar] [CrossRef]
  56. Almuhtaseb, R.M.; Bhagyaraj, S.; Krupa, I. A concise review on BTEX remediation from aqueous solutions by adsorption. Emergent Mater. 2024, 7, 695–719. [Google Scholar] [CrossRef]
  57. Doherty, V.E.; Otitoloju, A.A. Occurrence and distribution of monocyclic aromatic hydrocarbons (BTEX) and the impact on macrobenthic community structure in Lagos lagoon, Nigeria. Environ. Monit. Assess. 2016, 188, 571. [Google Scholar] [CrossRef]
  58. Yeh, C.H.; Lin, C.W.; Wu, C.H. A permeable reactive barrier for the bioremediation of BTEX-contaminated groundwater: Microbial community distribution and removal efficiencies. J. Hazard. Mater. 2010, 178, 74–80. [Google Scholar] [CrossRef]
  59. Esmaelnejad, F.; Hajizadeh, Y.; Pourzamani, H.; Amin, M. Monitoring of benzene, toluene, ethylbenzene, and xylene isomers emission from Shahreza gas stations in 2013. Int. J. Environ. Health Eng. 2015, 4, 17. [Google Scholar] [CrossRef]
  60. Alberici, R.M.; Zampronio, C.G.; Poppi, R.J.; Eberlin, M.N. Water solubilization of ethanol and BTEX from gasoline: On-line monitoring by membrane introduction mass spectrometry. Analyst 2002, 127, 230–234. [Google Scholar] [CrossRef]
  61. AmbScience Engenharia. Conheça os Contaminantes do Grupo dos BTEX E Seus Malefícios Para o Meio Ambiente. Available online: https://ambscience.com/contaminantes/ (accessed on 20 April 2024).
  62. Freitas, E.V.C.; Barreto, F.M.S.á.; Neto, M.F.A.; Cavalcante, R.M. Avaliação do uso da cromatografia gasosa para detecção de hidrocarbonetos monoaromáticos na água subterrânea na região Norte do Município de Fortaleza (CE). (Evaluation of the use of gas chromatography to detect monoaromatic hydrocarbons in groundwater in the northern region of the Municipality of Fortaleza (CE). Águas Subterrâneas 2016, 30, 289–305. [Google Scholar] [CrossRef]
  63. Rahmawati, S.; Juliani, A.; Sari, W.P.; Bariroh, A. Investigation of Groundwater Pollution by Petroleum Hydrocarbon from Gas Station in Yogyakarta, Indonesia. J. Sains Dan Teknol. Lingkung. 2018, 10, 67–76. [Google Scholar] [CrossRef]
  64. Zhang, Z.; Teng, Y.; Guo, G.; Li, F.; Zhang, C. Risk assessment of BTEX in the groundwater of Songyuan region of Songhua River in China. Water Sci. Technol. Water Supply 2016, 16, 135–143. [Google Scholar] [CrossRef]
  65. Liu, C.-Y.; Sun, J.-C.; Jing, J.-H.; Zhang, Y.; Guo, W.X. Distribution characteristics and source of BTEX in groundwater in Guangzhou, Guangdong Province, P.R. China. J. Groundw. Sci. Eng. 2016, 4, 238–246. [Google Scholar] [CrossRef]
  66. Eze, S.U.; Ogagarue, D.O.; Nnorom, S.L.; Osung, W.E.; Ibitoye, T.A. Integrated geophysical and geochemical methods for environmental assessment of subsurface hydrocarbon contamination. Environ. Monit. Assess. 2021, 193, 451. [Google Scholar] [CrossRef] [PubMed]
  67. Gomes, K.J.M.; Oliva, P.A.C.; da Rocha, H.O.; de Alcantara Mendes, R.; da Costa, A.C.G.; dos Santos Miranda, C.; de Oliveira Almeida, N. Evaluation of the contamination of the subsurface and groundwater by monoaromatic hydrocarbons in an eastern Amazonian town in northern Brazil. Environ. Earth Sci. 2023, 82, 23. [Google Scholar] [CrossRef]
Applsci 14 05529 g002
Figure 2. Chromatogram of sample A06 from gas station P14, showing the BTEX concentrations (Augusto Corrêa, November 2022).
Figure 2. Chromatogram of sample A06 from gas station P14, showing the BTEX concentrations (Augusto Corrêa, November 2022).
Applsci 14 05529 g002
Table 1. Summary of the samples of underground water collected in the towns of Augusto Corrêa and Tracuateua, in northeastern Pará, Brazil, and the occurrence of contamination with BTEX.
Table 1. Summary of the samples of underground water collected in the towns of Augusto Corrêa and Tracuateua, in northeastern Pará, Brazil, and the occurrence of contamination with BTEX.
PeriodNumber of Samples Collected in:Number of Samples in Which BTEX Were Detected
Augusto CorrêaTracuateua
December 2020
(rainy season)		123-
March 2021
(rainy season)		123-
July 2021
(rainy–dry season)		123-
October 2021
(dry season)		123-
January 2022
(rainy season)		1231
July 2022
(rainy–dry season)		1235
November 2022
(dry season)		1231
Abril 2023
(rainy season)		123-
August 2023
(dry season)		123-
March 2024
(rainy season)		123-
Total120307
Table 2. The BTEX compounds recorded in the water samples collected in the present study (Tracuateua, in July 2022).
Table 2. The BTEX compounds recorded in the water samples collected in the present study (Tracuateua, in July 2022).
SampleSiteB
(µg L−1)		T
(µg L−1)		E
(µg L−1)		X
(µg L−1)
A24Market near gas station P12<QL0.141<QL<QL
A25Gas station P12<QL0.167<QL<QL
Table 3. The BTEX compounds recorded in the water samples collected from the area surrounding two gas stations (14 and 15) in Augusto Corrêa, in July 2022.
Table 3. The BTEX compounds recorded in the water samples collected from the area surrounding two gas stations (14 and 15) in Augusto Corrêa, in July 2022.
SampleSiteB
(µg L−1)		T
(µg L−1)		E
(µg L−1)		X
(µg L−1)
A06Residence near gas station P14<QL0.140<QL<QL
A10Residence near gas station P15<QL0.184<QL<QL
A11Residence near gas station P15<QL0.236<QL<QL
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Chira, P.; Mendes, R.; Ferrari, S.; Rocha, C.; da Silva, E.; Farias, J.; do Carmo, R. Groundwater Contamination by Gas Stations in Two Eastern Amazonian Towns (Northern Brazil). Appl. Sci. 2024, 14, 5529. https://doi.org/10.3390/app14135529

AMA Style

Chira P, Mendes R, Ferrari S, Rocha C, da Silva E, Farias J, do Carmo R. Groundwater Contamination by Gas Stations in Two Eastern Amazonian Towns (Northern Brazil). Applied Sciences. 2024; 14(13):5529. https://doi.org/10.3390/app14135529

Chicago/Turabian Style

Chira, Pedro, Rosivaldo Mendes, Stephen Ferrari, Cassia Rocha, Elisama da Silva, Jarlana Farias, and Raerida do Carmo. 2024. "Groundwater Contamination by Gas Stations in Two Eastern Amazonian Towns (Northern Brazil)" Applied Sciences 14, no. 13: 5529. https://doi.org/10.3390/app14135529

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