Granulometric and Geochemical Distribution of Arsenic in a Mining Environmental Liability in a Semi-arid Area

doi:10.21203/rs.3.rs-4421727/v1

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Granulometric and Geochemical Distribution of Arsenic in a Mining Environmental Liability in a Semi-arid Area

https://doi.org/10.21203/rs.3.rs-4421727/v1

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published 06 Nov, 2024

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The present study refers to the "El Lavadero" tailings deposit, considered a mining environmental liability (MEL), located near San Felipe de Jesús town, Sonora, in northwest Mexico; the objective was to determine the total arsenic (As) content, its granulometric and geochemical distribution, and its mobilization capacity and bioavailability. The results in the oxidized and unoxidized tailings indicated low pH (potential of hydrogen) values (2.4–5.7) and elevated concentrations of total arsenic (8235–36,004 mg kg^− 1), which predominated in the finer granulometric fractions (< 0.05 mm). Arsenic also prevails in agricultural soil's finest fraction (> 2 mm). The above may represent adverse environmental effects because these particles can be transported and suspended in water media. Regarding the effluent sediments, arsenic prevails in the coarsest fraction (> 2 mm). A significant percentage of As (5–40%) was observed in the tailings (oxidized and unoxidized) distributed in the non-residual geochemical fraction (fraction I + fraction II + fraction III) (1106–7675 mg kg-1), indicating a potential for mobilization and bioavailability. Depending on the environmental conditions (redox potential (Eh) and pH), As can redissolve and present high mobility in abiotic media, potentially having a final impact on the environment and possible effects on human health. Based on the above, it is essential to rehabilitate the "El Lavadero" MEL to avoid a more significant environmental impact. Additionally, the quality of the water from the supply sources surrounding the "El Lavadero" MEL is recommended to be periodically monitored.

Studies on mining environment liabilities are essential to evaluate the environmental impact, specifically in water, sediment, and soil resources. Particularly in Mexico, many studies of this type currently focus on abandoned mining environmental liabilities in humid environments, so the geochemical mechanisms in these zones are well documented. Otherwise, only a few investigations exist in arid and semi-arid environments. This study is novel because it takes place in a semi-arid zone in the state of Sonora, México, particularly in the “El Lavadero” tailing deposit where the geochemical and granulometric association of arsenic is not known. It could represent a danger for the nearby water bodies and the environment in general because arsenic mobility can be regulated by the association of arsenic with the different compounds of the soil, tailings, and sediments, as well as the diverse particle sizes.

Mining is one of the activities that contribute the most to nations' economies (Dorin et al. 2014). Mining-metallurgical processes involve the separation of rocks and minerals that lack economic value from those that are valuable, producing a large amount of waste called mining tailings (Shengo 2021). Due to the lack of environmental regulations to control the closure of mines in the past, numerous mining environmental liabilities (MEL) were created where mining waste was accumulated over the years (Bennett 2016). MELs are substantial sources of pollution because they are usually formed from mining waste with high concentrations of Potentially Toxic Elements (PTE) (Reyes et al. 2021). These sites represent a significant environmental concern when they have high levels of PTE, such as arsenic (As) because they can be leached by meteoric water, causing water transport over long distances and contaminating the surrounding environment (Mukherjee et al. 2021). PTEs can severely impact the environment's natural resources, flora, fauna, and humans. They are considered one of the most significant hazards to the health of living beings due to their high persistence, non-degradability, toxicity, bioavailability, and adverse environmental effects (Mishra et al. 2019; León-García et al. 2021). When PTEs are present in nature as soluble complexes, they can mobilize and distribute to ecosystems to enter the food chain (Londoño-Franco et al. 2016).

Arsenic is widely distributed in nature, mainly as the sulfide; mineral deposits containing realgar, orpiment, and arsenopyrite maintain it naturally. (Peregrino-Ibarra 2016). It is a pervasive chemical element in rocks and soils and can be mobilized into the environment through natural processes such as weathering, biological activity, volcanic emissions, and anthropogenic processes such as mining (Alarcón et al. 2013). High levels of arsenic in water, soil, and crops in many regions of the world endanger the health of living beings (WHO 2018).

Water is the primary source of arsenic; access into the human body can occur through oral, respiratory, and skin routes (Ayejoto et al. 2022). Arsenic toxicity in humans manifests in skin, liver, neurological, hematological, cardiac changes, and even death. It also accumulates and is gradually eliminated from the body through urine, hair, nails, and skin. Patients who suffer from arsenic poisoning present different symptoms that can range from anorexia and nausea to melanosis and skin cancer (WHO 2018).

Arsenic also can cause harmful effects on aquatic and terrestrial fauna, including carcinogenic effects and death (Rehman et al. 2021). Regardless of the amount ingested, the entry and retention of As in living beings depends on its bioavailability, specifically on the physicochemical forms present in food, water, rocks, soil, and air. Furthermore, its toxicity depends on the oxidation state and the attached radical (Abbas et al. 2018). Inorganic compounds are more toxic than organic ones. Concerning the oxidation state, the trivalent form As (III) is more toxic than the pentavalent form As (V) (Jomova et al. 2011; Abbas et al. 2018).

Regarding arsenic present in rocks and minerals, its mobility depends on the attached geochemical phase. In nature, diverse environmental parameters such as pH and Eh govern As's mobility, bioavailability, and distribution towards the environment. Arsenic can be attached to readily soluble fractions in natural aqueous media and to phases that could never be solubilized (Bakhat et al. 2019; Srithongkul et al. 2019).

Arsenic mobility in tailings, soils, and sediments depends mainly on the granulometric form, its association with the different components of the soil (geochemical form), and the environmental conditions (Méndez and Armienta 2003). High levels of arsenic do not imply they represent a potential environmental risk because they must be in available fractions to be mobilized, contaminate other abiotic media, or be absorbed by living organisms (bioavailability). In assessing arsenic's mobility and leaching potential, it is necessary to determine the distribution of its chemical species in the different textural and physicochemical fractions and its association with the different soil constituents. This distribution (fractionation) directly relates to the geochemical behavior and mobility of PTEs under natural conditions. Sequential extraction and granulometric association procedures provide qualitative information to predict the mobilization, transport, and possible bioavailability hazards of PTEs (Ramos-Gómez et al. 2012).

In San Felipe de Jesús, Sonora, Mexico, the "El Lavadero" tailings deposit, a mining environmental liability, is adjacent to agricultural soils and streams that discharge into the Sonora River. In different periods of the 20th century, metallic minerals such as lead and zinc were processed at this site from regional mining activity, and it has not been in operation since the early 1980s (Campa-Robles 2015; Mora-Sánchez 2021). The tailings storage started approximately in 1920; there is no exact historical record of the daily volume of processed material, but it is estimated that it was approximately 100 tons of Pb, Zn, Cu, and Ag ores per day; due to the lack of environmental regulations in these years, the mining waste was abandoned. The absence of vegetation and orange-yellowish color characterizes now the site. (Roldan-Quintana 1979; Del Río-Salas et al. 2019; Loredo-Portales et al. 2020; Mora-Sánchez 2021). Studies on this MEL have reported high total concentrations of As in mining waste of up to 30,000 mg kg^− 1 (Del Río-Salas et al. 2019; Loredo-Portales et al. 2020).

The present investigation consisted of a physicochemical characterization study of arsenic in the tailings of the "El Lavadero" MEL, adjacent agricultural soil, and sediments of the MEL primary effluent that discharges into the Sonora River, as well as its granulometric and geochemical distribution, to estimate As mobility, bioavailability, and degree of impact on the environment (water, soil, and biota). The aim is to define the potential impact of arsenic from "El Lavadero" MEL on the surrounding environment and contribute to developing environmental research on MELs in arid and semi-arid areas of northwest Mexico due to scarce existing research.

Study Area

The "El Lavadero" MEL is a few meters from San Felipe de Jesús town. This town has approximately 600 inhabitants and is located in the center of the State of Sonora (Fig. 1). It is located at an elevation of 853 meters above sea level, bordering to the north Banámichi and Huepac, south with Aconchi, and west with Opodepe (INEGI 2009; Mora-Sánchez 2021). The MEL has an irregular fan shape that opens towards the north, with an approximate diameter of 210 m and an area of approximately 17,000 m². It has heights between 2 and 5 meters, weighing approximately 210,000 tons (Espinoza-Madero 2012). Lead and zinc sulfide minerals were concentrated in this place, with copper and silver values, mainly from the Santa Rosa and las Lamas mines in the Mining District of San Felipe de Jesús. The process used was selective flotation, producing Zn and Cu, Pb, and Ag concentrates (Roldan-Quintana 1979). The reddish and grayish color predominates in the area, corresponding to many oxides and sulfides. (Fig. 2) (Del Río-Salas et al. 2019; Loredo-Portales et al. 2020; Mora-Sánchez 2021). The MEL is adjacent to agricultural lands where forage is grown and serves as food for the region's livestock (Fig. 2) (SAGARHPA 2017; Loredo-Portales et al. 2020). In addition, the primary effluent from mining waste forms a stream that discharges into the Sonora River (Fig. 2). In the study area, the predominant economic activities are livestock, agriculture, and mining. (Mora-Sánchez 2021).

Sampling and Sample Preparation

The methodology recommended by Mudroch and Azcue (1995) was used to collect and prepare the tailing, soil, and effluent sediment samples. Systematic and judgmental sampling was performed based on a regular geometric pattern to ensure the area of interest was covered uniformly, and the samples represented the site. Samples were collected manually, introducing clean and decontaminated plastic nucleators to a maximum depth of 20 cm. A total of 21 sampling stations were contemplated: ten samples of tailings (five correspond to oxidized tailings and five to unoxidized tailings), five samples of the surrounding agricultural soil, and five samples of sediments from the MEL primary effluent (stream) that discharge into the Sonora River (Fig. 1).

In addition, a blank field sample was collected at a sampling station on a hill 0.5 km away from the "El Lavadero" MEL (Figs. 1 and 2) to compare the results obtained in the present study with a site not visually impacted by the MEL. The material used in collecting the samples was previously washed with HNO₃ at 20% v/v and rinsed with deionized water. All the samples were placed in plastic containers and immediately transported to the laboratory for their corresponding physicochemical characterization. In the laboratory, the samples (mine tailings, soils, and sediments) were dried at room temperature for five days and reduced in volume using the coning and quartering method to obtain representative samples. Subsequently, pulverizing was carried out using a porcelain mortar until a size of less than 0.177 mm was obtained (Mudroch and Azcue 1995).

Physicochemical Analysis

The granulometric classification of the mine tailing, soil, and sediment samples was carried out through the percentage determination of the gravel, sand, silt, and clay fractions by the mesh and pipette method (Folk 1980; Lozano-Rivas 2018). The mineralogical characterization of the tailings, soil, and sediments was determined using X-ray diffraction (XRD) analysis. Samples were homogenized and pulverized in an agate mortar, sieved (< 75 microns), and placed in a double-loaded aluminum sample holder (non-oriented fractions). The measurement was carried out in the angular range (2θ) of 5° to 80° in step scanning with a "step scan" of 0.02° (2θ) and an integration time of 0.6 seconds per step, using an X-ray diffractometer (Bruker model D8 advance eco) equipped with copper source and nickel filter. Diffractogram identifications were obtained using the Xpert HighScore software, the ICSD (Inorganic Crystal Structure database), and the ICDD (International Center for Diffraction Data) databases (Goldstein et al. 2018).

On the other hand, the detection of major elements and morphology analysis were carried out by scanning electron microscopy (SEM). This analysis was carried out on tailings, soils, and sediments using a JEOL model 5410LV scanning electron microscope equipped with an X-ray energy dispersion system (EDS), operated at an acceleration voltage of 20 kV and a working distance of 20 mm. The study was carried out to identify primary elements in the sample (elemental semi-quantification) and to detect other EPTs bound to particles in the presence of arsenic. In addition, the morphology of the studied particles was analyzed (Goldstein et al. 2018).

The Eh was determined in the field during sample collection for each sampling station using a potentiometer (Thermo Electron Corporation model Orion 3 Star). The procedure involved introducing the electrode and verifying the contact with the sample. Once the thermal equilibrium is reached, the temperature and values of Eh in mV were recorded when the reading had stabilized (Mudroch and Azcue 1995). The potentiometer was constantly calibrated using Zobell's standard solution.

Regarding the potential of hydrogen (pH), a potentiometer (Thermo Electron Corporation model Orion 3 Star) was employed. The measurement was carried out in an aqueous extract prepared with the tailing, soil, and sediment samples in contact with deionized water in a 1:5 ratio (solid-liquid) previously stirred for one hour. For this analysis, the equipment calibration was constantly verified with three buffer solutions of different pH (4, 7, and 10) (Mudroch and Azcue 1995).

Concerning electrical conductivity (E.C.) determination, a Hanna conductivity meter model HI98130 was utilized. The measurement was carried out on an aqueous extract obtained with deionized water in a 1:5 ratio (solid-liquid) filtered with the Whatman 42 filter paper. A standard solution of 1413 µS cm^− 1 was used to calibrate the equipment constantly (Mudroch and Azcue 1995).

Total arsenic levels in the samples were calculated according to the methodology established by Van Loon and Barefoot (1989) and Gómez-Álvarez (2004). Sample digestions were carried out using concentrated mineral acids (HNO₃, H₂SO₄). The acid extracts were recovered in 1% H₂SO₄ and analyzed using the flame atomic absorption spectroscopy technique in the tailings. The agricultural soils and sediments were analyzed using the hydride generation atomic absorption spectroscopy. The atomic absorption equipment used was Perkin-Elmer PinAAcle 900T coupled with a hydride generator (FIAS 100). This procedure and equipment were also carried out in the different granulometric fractions.

The extraction of toxic constituents soluble in water test was carried out to estimate the danger of tailings due to their toxicity. The technique refers to the "test to carry out the extraction of As in tailings, with water in equilibrium with CO₂", a procedure that utilizes distilled water in equilibrium with CO₂ as extractant under standard conditions (carbonic acid, pH = 5.5) prepared at the moment of use (SEMARNAT 2003). In the aqueous extract obtained, the arsenic regulated in the Mexican Regulations (SEMARNAT 2009) is quantified by hydride generation atomic absorption spectroscopy technique.

Regarding the arsenic sequential extraction, the BCR method was carried out (Rauret et al. 2000). The study consisted of a sequential separation of three geochemical fractions in the tailings, agricultural soil, and sediments: fraction 1: exchangeable arsenic and soluble fraction; fraction 2: arsenic bound to Fe and Mn oxides; fraction 3: arsenic bound to organic matter and sulfides; residual fraction: arsenic bound to the residual fraction. The BCR method consists of three extraction stages, based on the difference in the extractant power applied in each of them, with the first extractant being the weakest (0.11 M acetic acid), followed by a 0.5 M hydroxylamine hydrochloride solution, as well as the last stage where arsenic is extracted first with 8.8 M hydrogen peroxide, and subsequently with 1 M ammonium acetate. Arsenic concentration in the residual fraction is determined by the acid digestion of the residue in aqua regia. The quantification of arsenic is subsequently determined by the atomic absorption spectroscopy technique for each geochemical fraction.

Geoaccumulation Index (Igeo)

The Igeo was calculated in the tailings, soils, and sediments to determine the degree of contamination by As (Li et al. 2016). It is widely used to assess contamination numerically through the relationship of the present concentration versus the reference values through the following equation:

$$\text{I}\text{g}\text{e}\text{o} ={ \text{l}\text{o}\text{g}}_{2}\left(\frac{\text{C}\text{n}}{1.5\text{B}\text{n}}\right)$$

C_n is the As concentration in the samples, and B_n is the average background geochemical As values. The following scale proposed by Müller (1969) was utilized to interpret the obtained results (Table 1).

Table 1

Igeo interpretation (Müller 1969)
Igeo Value	Interpretation of Quality (Tailing, Soil, or Sediment)
> 5	Extremely polluted
4–5	Strongly to extremely polluted
3–4	Strongly polluted
2–3	Moderately to strongly polluted
1–2	Moderately polluted
0–1	Unpolluted to moderately polluted
0	Unpolluted

Quality Control

In order to validate the accuracy and precision of the methodology employed in the arsenic analysis, a certified MESS-4 standard (Marine Sediment Certified Reference Material) was utilized and treated similarly to the tailing, soil, and sediment samples (USEPA 1992; Skoog et al. 2015; NMX 2016). The results of the triplicate analysis indicated acceptable accuracy, with recovery percentages between 90 and 105%. In addition, reactive blanks were analyzed in triplicate and subjected to the same treatments and extractions as the other samples. The detection limits (DL) (mg kg^− 1) for total arsenic were 0.04 for flame atomic absorption spectroscopy and 0.0003 for the hydride generation. The sampling equipment (plastic nucleators) and laboratory materials were soaked in a 20% (v/v) HCl solution for three days and subsequently rinsed with deionized water before use (NMX 2001). The reagents utilized were of analytical grade (Baker and Merck). Deionized water was used in all experiments.

Granulometric Analysis

The results of the granulometric analysis are presented in Tables 2 and 3. Sampling stations 1A and 2A of the oxidized tailings present fine textural characteristics, with silt and clay predominating in more than 50%. In the other tailing stations (unoxidized and oxidized), the proportion of sand is greater than 50% (Table 2). The oxidized tailings presented finer textures than the unoxidized tailings because the oxidation processes develop more quickly and efficiently in mining wastes with a greater exposed surface area (Salas-Urviola et al. 2020). The particle size of a mineral decisively influences its oxidation rate; it is favored when the particle is finely divided due to the broader reaction surface exposed to the medium (Fernández-Rubio 2016). Regarding agricultural soil, station 5B (station located in the primary water discharge of the tailings) presented a predominance of sandy particles (> 90%) (Table 3). In contrast, in the remaining four stations, the sand is less than 56%, in addition to presenting proportions of gravel. Similar to most agricultural soils, the effluent sediments were characterized by the predominance of sand and gravel (Table 3).

The results indicate that the finest particles are found in mine tailings, with sand, silt, and clay prevailing, favoring the release of arsenic into the environment due to the considerable surface area (Lundgren and Silver 1980; Fernández-Rubio 2016). The differences in granulometric classification between the various sampling stations corresponding to the tailings can be associated with variations in milling conditions, as well as differences between the geological characteristics of the deposit they came from because minerals from various mines in the sector were concentrated in the "El Lavadero" MEL (Roldan-Quintana 1979). On the other hand, the agricultural soil and the effluent sediments presented a coarser granulometry, with gravel, sand, and mud prevailing. Granulometry studies in the "El Lavadero" MEL and agricultural soil have reported similar results (Espinoza-Madero 2012). Likewise, similar results of granulometric analysis have been reported in mining tailings deposits in southern Mexico and other regions of the world (García-Balboa 1998; Corona-Chávez et al. 2017; Salas-Urviola et al. 2020).

Table 2

Granulometric analysis results in the tailings of the "El Lavadero" MEL (oxidized and unoxidized)
Parameter	Oxidized Tailings					Unoxidized Tailings
Parameter	1A	1B	1C	2A	3B	2B	3A	3C	4A	4B
Sand (%)	37.13	56.95	72.92	42.30	62.19	73.43	80.92	55.50	75.53	80.78
Silt (%)	52.06	28.67	18.83	29.18	21.96	13.14	7.86	29.16	16.27	11.45
Clay (%)	10.80	14.38	8.25	28.52	15.85	13.43	11.22	15.34	8.20	7.77
Granulometry	Sandy silt	Muddy sand	Silty sand	Sandy mud	Muddy sand	Muddy sand	Muddy sand	Muddy sand	Muddy sand	Muddy sand

Table 3

Granulometric analysis results in agricultural soil and effluent sediments
Parameter	Agricultural Soil					Effluent Sediments
Parameter	5A	5B	5C	6A	6B	EF1	EF2	EF3	EF4	EF5	BC
Gravel (%)	15.95		10.03	7.82	19.09	31.43	39.17	32.57	39.43	40.39	53.66
Sand (%)	45.82	92.25	64.29	56.01	54.40	67.58	59.30	66.64	59.91	58.87	40.65
Silt (%)		5.57
Clay (%)		2.18
Silt + Clay (%)	38.22		25.68	36.17	26.51	0.99	1.53	0.79	0.66	0.75	5.69
Granulometry	Gravelly muddy sand	Sand	Gravelly muddy sand	Gravelly muddy sand	Gravelly muddy sand	Sandy gravel	Sandy gravel	Sandy gravel	Sandy gravel	Sandy gravel	Muddy Sandy gravel

Mineralogical Characterization

Table 4 presents the results of the mineralogical characterization carried out by the XRD technique in the unoxidized tailings (2B and 3A), oxidized tailings (1A and 2A), agricultural soil (5A and 5B), sediments (EF1 and EF5 ), and the blank field station (BC). These sampling stations were contemplated because they are the most representative of the "El Lavadero" MEL, as they have higher concentrations of arsenic. In the case of unoxidized tailings, they are characterized by the predominance of quartz, arsenopyrite, pyrite, sphalerite, lead arsenate, clinomimetite, hydronium-jarosite and gypsum (Table 4). The oxidized tailings contain quartz, pyrite, sphalerite, hydronium-jarosite, gypsum, jarosite, beudantite, and copiapite (Table 4). In the tailings (oxidized and unoxidized), primary minerals such as quartz, iron sulfides, zinc, and arsenic, and secondary minerals such as arsenates and sulfates are present. Secondary species, such as jarosite, gypsum, copiapite, and clinomimetite, can be generated due to the oxidation of sulfurous mining waste, depending on its composition and alteration conditions (Lottermoser 2010; Murciego et al. 2019).

Romero et al. (2007) and Yucel and Baba (2016), report that secondary minerals such as jarosite and gypsum are typical of environments where acid mine drainage is formed. A study has reported that "El Lavadero" MEL is a generator of acid drainage, favoring the mobility of EPT, such as arsenic (Mora-Sánchez 2021). The majority of the species previously reported, such as sulfides and quartz, correspond to those registered by Roldan-Quintana (1979) within the mineralogy of the San Felipe de Jesús deposits. On the other hand, species from the carbonate group were not detected. Carbonate minerals attenuate the acidity generated, helping to precipitate metallic compounds (Mora-Sánchez 2021).

Agricultural soil is characterized by quartz, albite, ferric sanidine, and calcium albite. At station 5B, iron sulfate hydroxide and iron, magnesium, and sodium sulfates were also detected (Table 4). These minerals are classified within the group of silicates, except the latter two, which are common in MELs in oxidizing environments (Durocher and Schindler 2011). These minerals (sulfates formed in the oxidation processes of the sulfides detected in the tailings) are present in the surrounding agricultural soil due to water transport from the tailings deposit. It is essential to mention that arsenic was not detected in the agricultural soil because the XRD technique cannot identify minerals at elemental concentrations less than 2% (Sánchez et al. 2018).

Table 4

Mineralogical characterization by XRD of the "El Lavadero" MEL sampling stations, surrounding agricultural soil, and effluent sediments
Mineral	Formula	Sampling Stations
Mineral	Formula	1A	2A	2B	3A	5A	5B	EF1	EF5	BC
Calcite	CaCO₃									+
Ankerite	Ca(Fe²⁺,Mg)(CO₃)₂							+	+
Quartz	SiO₂	+	+	+	+	+	+	+	+	+
Albite	NaAlSi₃O₈					+		+	+	+
Sanidine	(K_0.93,Na_0.07)(AlSi₃O₈)								+
Potassium feldspar	KAlSi₃O₈									+
Intermediate plagioclase	(Na,Ca)(Si,Al)₄O₈									+
Muscovite	KAl₂(Al,Si)₄O₁₀(OH,F)₂									+
Kaolinite	Al₂(OH)₄Si₂O									+
Ferric sanidine	KFe_0.28Al_0.72Si₃O₈					+
Calcium albite	(Na_0.84Ca_0.16)Al_1.16Si_2.84O₈						+
Lead arsenate	PbAs₂O₆			+	+
Arsenopyrite	FeAsS			+	+
Pyrite	FeS₂		+	+	+
Sphalerite	ZnS	+			+
Hydronium-jarosite	Fe₃(SO₄)₂(OH)₅·2H₂O	+			+
Iron, magnesium and sodium sulfate	NaMgFe(SO₄)₃						+
Iron sulfate hydroxide	2Fe(OH)SO₄						+
Clinomimetite	Pb₅(AsO₄)₃Cl				+
Gypsum	CaSO₄·2H₂O	+	+		+
Jarosite	KFe³⁺ ₃(OH)₆(SO₄)₂		+
Beudantite	KFe³⁺ ₃(OH)₆(SO₄)₂		+	+
Copiapite	Fe ²⁺Fe^3 + ₄(SO₄)₆(OH)₂·20(H₂O)		+

The effluent sediments are formed by ankerite, quartz, albite, and sanidine, corresponding to the silicate group. The mineralogical composition detected by XRD in the present study is similar to other studies in freshwater sediments (Maity and Maiti 2016; León-García et al. 2021). In the case of the field blank station (BC), quartz, intermediate plagioclase, calcite, potassium feldspar, diopside, muscovite, and kaolinite were detected (Table 4). The previous mineralogy is significantly different than found in the tailings and the agricultural soil, indicating no impact of the "El Lavadero" MEL.

Scanning Electron Microscopy

Figure 3 indicates the results obtained from the unoxidized tailings of stations 2B and 3A, where arsenic was detected bound to particles with a predominance of iron and sulfur. In the case of station 3A, the particle studied may be arsenopyrite according to its percentage composition and crystalline morphology (Table 4). The dissolution of arsenic sulfides, such as arsenopyrite, releases iron, sulfur, and arsenic under certain geochemical conditions. Under neutral and oxidizing conditions, arsenic can precipitate, forming iron oxyhydroxides, but if the conditions are more acidic, secondary species such as arsenates could be generated, favoring the mobility of arsenic (Asta et al. 2013; Battistel et al. 2021). Concerning the oxidized tailings (stations 1A and 2A), arsenic was detected to be bound to particles where iron, lead, and sulfur predominate. In the case of station 1A, it was probably clinomimetite, a secondary species of the arsenate group, reported in the present investigation by X-ray diffraction. The interaction of arsenates with other species in soils is frequent, even at low concentrations of arsenic in solution, mainly through adsorption with the oxides of iron, aluminum, manganese, clay minerals, and organic matter (Bundschuh et al. 2008). The above contributes to maintaining lower solubility and toxicity than arsenites.

Regarding the surrounding agricultural soil, no arsenic was detected. The above does not mean that arsenic is not present; the study carried out by SEM does not detect concentrations of less than 2% of elements (Melgarejo et al. 2010). The particle studied at station 5A corresponds to quartz because it was characterized by the predominance of oxygen and silicon, presenting a hexagonal habit. Sulfur and manganese in small quantities were detected in the soil of the discharge station (5B). According to the elemental composition, the particle studied corresponds to a mineral from the silicate group, such as modernite or intermediate plagioclase, as reported by previous studies in the study area (Del Río-Salas et al. 2019; Mora-Sánchez 2021). In the case of the effluent sediments, the presence of PTEs (including arsenic) was not detected; only the presence of iron and a predominance of oxygen and silicon were detected, indicating they are minerals from the silicate group, such as albite. (Table 4).

Physicochemical parameters

The results of the physicochemical parameters are presented in Tables 5 and 6. The Eh ranged from 303.9 to 517.6 mV in the oxidized tailings, from 255 to 462 mV in the unoxidized tailings, from 259.2 to 349 mV in the agricultural soil, and from 227.4 to 291.6 mV in the effluent sediments. In all cases, an oxidizing environment is present, favoring the formation of arsenic species in its oxidized form, such as arsenates (Pérez-Míngez 2015). In oxidizing environments, the formation of acid mine drainage is favored, resulting in the release and subsequent transport of arsenic to the surrounding environment (Mora-Sánchez 2021). The oxidizing Eh can promote oxidation reactions, causing the arsenic in mineral sulfides (Table 4) to be released into the environment through physicochemical processes (Al-Abed et al. 2007). Eh and pH are the most important environmental parameters that regulate the physicochemical form of arsenic (precipitated state, forming a secondary mineral, or in solution) (Craw and Bowell 2014).

Concerning pH, the results fluctuated from 2.1 to 4.6 in the oxidized tailings, from 4.1 to 5.7 in the unoxidized tailings, from 3.9 to 6.8 in the surrounding agricultural soil, and from 6.2 to 7 in the effluent sediments (Tables 5 and 6). Both tailings (unoxidized and oxidized) presented the lowest pH values, with the oxidized tailings being lower. The oxidized tailings (stations 1A, 1B, 2A) presented pH values lower than 4, which are classified as dangerous for the environment (Huillcañahui 2007; SEMARNAT 2009). The oxidized tailings presented lower pH values than the unoxidized tailings because the former oxidation events released acidity into the medium, consuming alkalinity species, such as calcite (CaCO₃). Likewise, in oxidized waste, the presence of secondary minerals such as sulfates (jarosite, gypsum, beudantite) is more significant than in unoxidized waste; these species, when solubilized in water, cause additional acidity (Lottermoser 2010; Mora-Sánchez 2021).

Regarding agricultural soil, station 5B has a pH value of less than four because it is located in the primary water discharge from the tailings (Fig. 1c). Due to the above, agricultural soil is classified as dangerous due to its low pH value (SEMARNAT 2009). The rest of the stations on the surrounding agricultural soil presented pH values between 6.3 and 6.7 (slightly acidic). Similar pH values have been detected in other studied MELs (Corrales-Pérez and Martín-Romero 2018; Gallardo-Martínez et al. 2020). Concerning effluent sediments, increasing pH values are observed as the sampling stations move further away from the "El Lavadero" MEL; however, the pH values are generally slightly acidic. It is essential to mention that pH influences the speciation and mobility of PTEs, including arsenic, favoring its transport at acidic pH values (Hoagland et al. 2021).

Concerning E.C., values greater than 5000 µS cm^− 1 can be seen in the tailings (oxidized and unoxidized) (Tables 5 and 6). In the case of agricultural soil and effluent sediments, only the E.C. value from station 5B (4750 µS cm^− 1) highlights, which is the most impacted by tailings as it receives acidic waste with high PTE values, including arsenic. (Fig. 1c). This agricultural soil is classified as saline soil, so it is not of sufficient quality for farming (SEMARNAT 2000). Regarding effluent sediment, levels were below 370 µS cm^− 1; these values are similar to the field blank (BC). The elevated E.C. values detected in tailings (oxidized and unoxidized) and agricultural soil (station 5B) are probably caused by significant amounts of hydrogen ions, PTEs, and arsenic salts dissolved in an acidic medium (Lech et al. 2016). Acid drainage solutions from MELs generally maintain E.C. values similar to those found in the tailings (oxidized and unoxidized) in the present study (Yang et al. 2006; Ramírez-Serrano et al. 2017). On the other hand, a direct relationship is observed between the decrease in pH and the increase in E.C. at all sampling stations, indicating the increase in solubility under acidic conditions.

Table 5

Physicochemical parameters (Eh, pH, and E.C.) in the tailings of the "El Lavadero" MEL
Parameter	Oxidized Tailings					Unoxidized Tailings
Parameter	1A	1B	1C	2A	3B	2B	3A	3C	4A	4B
Eh (mV)	517.6	415.9	429.5	450.6	303.9	279.6	462	277.4	255	272.8
pH	2.4	2.5	4.2	2.1	4.6	4.8	4.1	5.6	5.4	5.7
E.C. (µS cm^− 1)	12,650	12,400	5425	70,150	13,900	20,150	29,700	14,000	9200	6650
SEMARNAT (2009)^a (pH)	4	4	4	4	4	4	4	4	4	4

^a A pH limit value for mine tailings to be considered dangerous (SEMARNAT 2009).

Table 6

Physicochemical parameters (Eh, pH, and E.C.) in the agricultural soil and effluent sediments
Parameter	Agricultural Soil					Effluent Sediments
Parameter	5A	5B^a	5C	6A	6B	EF1	EF2	EF3		EF4		EF5		BC^c
Eh (mV)	349	290	310.2	259.2	287.8	291.6	239.3	235.2	257.2		227.4		292.8
pH	6.3	3.9	6.4	6.8	6.5	6.2	6.2	6.6	6.7		7.0		7.1
E.C. (µS cm^− 1)	336	4750	326	310.5	258.5	142.5	167.5	267.5	370.5		215		350
SEMARNAT (2009)^b (pH)	4	4	4	4	4	4	4	4		4		4		4

^a Agricultural soil station located at the primary water discharge site from the tailings; ^b pH limit value for mine tailings to be considered dangerous (SEMARNAT 2009); ^c Field blank station.

Total Arsenic

The results of total As are presented in Table 7. In the oxidized tailings, the content of total As fluctuated from 8235 to 35,470 mg kg^− 1, in the unoxidized tailings from 9134 to 36,004 mg kg^− 1, in the agricultural soil from 223 to 1311 mg kg^− 1, and in the effluent sediments from 160 to 179 mg kg^− 1. The behavior of the total arsenic concentration: unoxidized tailings > oxidized tailings > agricultural soil > effluent sediments. Station 5B (agricultural soil) presented the most elevated concentration of total arsenic in the soil, which is logical since it is located in the primary water discharge zone of the "El Lavadero" MEL (Fig. 2c). On the other hand, both the agricultural soil and the effluent sediments presented more elevated values concerning the blank field station (132.88 mg kg^− 1), so an impact from the tailings can be attributed. In general terms, the concentrations of arsenic in mining tailings (oxidized and unoxidized) are similar to those reported by previous studies in the MEL (Del Río-Salas et al. 2019; Loredo-Portales et al. 2020) and much more elevated than the average concentration of other MELs in Mexico (Cervantes-Macedo 2014; Magdaleno-Rico 2014; Salas-Urviola et al. 2020).

In Mexican regulations, a permissible limit value of total arsenic of 100 mg kg^− 1 is contemplated for mining waste; if exceeded, it is considered hazardous waste (SEMARNAT 2009). Regarding tailings (oxidized and unoxidized), all presented values were more elevated than the permissible limit and classified as dangerous due to their toxicity. In Mexico, SEMARNAT (2004) establishes the permissible limit value for total As (22 mg kg^− 1) in agricultural soils, which was exceeded in all sampling stations of agricultural soil. Therefore, soil is not considered appropriate for farming. Regarding the effluent sediments, the New Zealand sediment quality guide (ANZECC and ARMCANZ 2000) establishes a permissible limit value of 70 mg kg^− 1, which was widely exceeded by all the sampling stations associated with sediments from the effluent, demonstrating the water transport of arsenic, which could be dragged from the MEL to form part of the stream sediments.

Soluble As (Extraction Test of Toxic Constituents)

Table 8 indicates the results of the toxic constituent extraction test. SEMARNAT (2009) and USEPA (1983) establish a maximum permissible arsenic value of 5 mg L^− 1 for the aqueous extract obtained in the test. If this value is exceeded, the tailings are dangerous due to their toxicity (arsenic or PTEs are released into the aqueous phase). Station 2A, corresponding to the oxidized tailings, was the only one exceeding this value (9.165 mg L^− 1), classifying it as dangerous due to its toxicity concerning arsenic. Station 2A presented an acidic pH value (2.1), which contributes to the solubilization of arsenic because arsenic species are more soluble in acidic media (Craw and Bowell 2014). The results of agricultural soil and effluent sediments were below 1 mg L^− 1. The water solubility test is not sufficient to evaluate the mobility of arsenic toward the environment because, in nature, various parameters such as Eh and pH, can promote its mobility (Rauret et al. 2000; León-García et al. 2021).

Table 7

Total As concentration (average ± standard deviation) (mg kg^− 1) in the tailings of the "El Lavadero" MEL, agricultural soil, and effluent sediments
Sampling Station	Classification	Total As
1A	Oxidized tailing	35,470.83 ± 359.16
1B	Oxidized tailing	17,769.39 ± 378.15
1C	Oxidized tailing	8235.42 ± 776.76
2A	Oxidized tailing	29291.18 ± 63.37
3B	Oxidized tailing	16,986.27 ± 1446.76
2B	Unoxidized tailing	25,299.10 ± 1810.20
3A	Unoxidized tailing	36,004.07 ± 1241.04
3C	Unoxidized tailing	9134.22 ± 884.99
4A	Unoxidized tailing	22,594.38 ± 489.62
4B	Unoxidized tailing	12,940.81 ± 389.97
5A	Agricultural soil	234.36 ± 28.37
5B	Agricultural soil	1311.09 ± 42.08
5C	Agricultural soil	239.04 ± 77.97
6A	Agricultural soil	223.76 ± 19.20
6B	Agricultural soil	290.98 ± 6.40
EF1	Effluent sediment	236.22 ± 19.70
EF2	Effluent sediment	179.80 ± 6.98
EF3	Effluent sediment	168.87 ± 21.55
EF4	Effluent sediment	160.61 ± 53.45
EF5	Effluent sediment	193.75 ± 62.61
BC	Field blank	132.88 ± 36.02

Table 8

Mobility test results (extraction test of toxic constituents) in the tailings of the "El Lavadero" MEL, agricultural soil, and effluent sediments (SEMARNAT 2003)
Sampling Station	Classification	As (mg L^− 1)
1A	Oxidized tailing	0.785
1B	Oxidized tailing	0.464
1C	Oxidized tailing	0.283
2A	Oxidized tailing	9.165
3B	Oxidized tailing	0.744
2B	Unoxidized tailing	1.728
3A	Unoxidized tailing	3.3
3C	Unoxidized tailing	0.052
4A	Unoxidized tailing	0.15
4B	Unoxidized tailing	0.15
5A	Agricultural soil	0.039
5B	Agricultural soil	0.11
5C	Agricultural soil	0.021
6A	Agricultural soil	BDL
6B	Agricultural soil	BDL
EF1	Effluent sediment	BDL
EF2	Effluent sediment	BDL
EF3	Effluent sediment	BDL
EF4	Effluent sediment	BDL
EF5	Effluent sediment	BDL
BC	Field blank	BDL
SEMARNAT^a	MPV	5
USEPA^b	MPV	5

^a Maximum permissible value of As (Mg L^− 1) (SEMARNAT 2009) in the aqueous extract of the extraction test of toxic constituents, ^b Maximum permissible value of As (mg L^− 1) (USEPA 1983), MPV = Maximum permissible value, BDL = Below detection limit (mg L^− 1) (0.02).

As Distribution by Granulometric Fractions

Tables 9 and 10 present the results of total arsenic by granulometric fraction. Regarding unoxidized tailings (Table 9), a slight predominance of arsenic is observed in the mud fraction (silt + clay), except in stations 3A and 3C, where arsenic is distributed similarly in both sand and mud (Fig. 4). Concerning the oxidized tailings (Table 9), the predominance of arsenic in the fine fractions (clay + silt) is evident in all sampling stations; more than 50% of the arsenic concentration is associated with this fraction. Generally, arsenic prevails in fine fractions in tailings (oxidized and unoxidized), facilitating its mobility. Arsenic persists in a more elevated proportion in fine particle sizes because of the greater exposed surface area; this is due to natural oxidation processes continually favoring the release of solutions loaded with arsenic saturating these particles, and arsenic tends to adsorb to the surface area of fine minerals (Reimann et al. 2009). The arsenic contained in fine fractions is susceptible to re-solubilize to continue its transport in this way; the above will depend on its physicochemical form and the environmental conditions of Eh and pH present at the site (Gorny et al. 2018). Loredo-Portales et al. (2020) reported similar results from the distribution of arsenic in the tailings studied in the present investigation.

Concerning the percentage distribution of arsenic in the agricultural soil of station 5B (discharge station) (Table 9), a vast predominance is observed in the mud fraction (72%), demonstrating that the transport of contaminants is more effective in the case of the finer particles, which can be suspended in the water medium. In the case of the remaining sampling stations of agricultural soil (Table 10), arsenic is distributed in less than 45% in the gravel fraction and more than 54% in the sand + silt + clay fraction.

Regarding effluent sediments (Table 10), stations EF2 and EF3 present As in the coarsest fraction (gravel) in a proportion of approximately 90%. In the case of the remaining stations EF1, EF4, and EF5, a predominance of arsenic (more than 60%) is observed in the finest fraction (sand + silt + clay). The above could result from dragging particulate mining waste contaminated with As from the "El Lavadero" MEL. A study has reported similar results in river sediments, indicating the highest PTE contents in the coarse fractions (León-García et al. 2021). In general terms, the mobility of arsenic can be favored by bounding to fine fractions in the tailings, which are the focus of contamination.

Table 9

Distribution results of As by granulometric fraction in the tailings of the "El Lavadero" MEL and agricultural soil (station 5B)
Sampling Station	Classification	% Sand	% Mud (Silt + Clay)
1A	Oxidized Tailing	51.99	48.01
1B	Oxidized Tailing	22.24	77.76
1C	Oxidized Tailing	19.97	80.03
2A	Oxidized Tailing	40.56	59.44
3B	Oxidized Tailing	23.21	76.79
2B	Unoxidized Tailing	37.75	62.25
3A	Unoxidized Tailing	50.14	49.86
3C	Unoxidized Tailing	54.72	45.28
4A	Unoxidized Tailing	38.31	61.69
4B	Unoxidized Tailing	35.01	64.99
5B	Agricultural Soil	27.73	72.27

Table 10

Distribution results of As by granulometric fraction in the agricultural soil and effluent sediments
Sampling Station	Classification	% Gravel	% Sand + Silt + Clay
5A	Agricultural Soil	23.12	76.88
5C	Agricultural Soil	32.88	67.12
6A	Agricultural Soil	16.17	83.83
6B	Agricultural Soil	45.32	54.68
EF1	Effluent Sediment	36.72	63.28
EF2	Effluent Sediment	89.03	10.97
EF3	Effluent Sediment	90.30	9.70
EF4	Effluent Sediment	34.38	65.62
EF5	Effluent Sediment	39.72	60.28
BC	Field Blank	59.03	40.97

Arsenic in the Geochemical Fractions (Sequential Extraction)

The distribution of As in the different geochemical fractions (results of the sequential extraction study) is observed in Tables 11, 12, 13, and 14, as well as in Fig. 5. In fraction I (Exchangeable and Soluble), the minimum concentrations and maximum As (mg kg^− 1) were: unoxidized tailings (154–293), oxidized tailings (23–467), agricultural soil (0.82–16) and effluent sediments (0.05–0.11). The most elevated values occurred in the oxidized tailings, followed by the unoxidized tailings. The As contained in this fraction may be adsorbed to secondary species such as efflorescent salts produced by evapotranspiration, sulfates formed by acid mine drainage, or carbonates (Bravo et al. 2020).

Regarding agricultural soil, station 5B (primary water discharge zone) presented the highest value of As (16 mg kg^− 1) because tailings have been transported due to physical erosion. In the case of effluent sediments, the lowest As values were detected. Arsenic is weakly adsorbed and available to living beings in the exchangeable and soluble fraction (Méndez and Armienta 2003). It can be readily solubilized in meteoric water, facilitating its transport to the surrounding environment (Gómez-Álvarez 2008).

In fraction II (Fe and Mn Oxides), the minimum and maximum concentrations (mg kg^− 1) were: unoxidized tailings (402–1482), oxidized tailings (179–1053), agricultural soil (1.21–152) and sediment of effluent (0.15–0.4). The behavior of the As concentration was: tailings (oxidized and unoxidized) > agricultural soil > effluent sediments. In this fraction, more elevated values of As are detected than in fraction I; this may be due to the coprecipitation and adsorption of As in conjunction with the precipitation of iron oxides and hydroxides produced by changes in the pH of solids (Gómez-Álvarez 2008). In the Fe and Mn Oxide fraction, As can be adsorbed or coprecipitated, and in addition, it is usually unstable under reducing conditions, potentializing its mobilization when low values of redox potential occur (Aguilar-Hinojosa et al. 2016).

Regarding fraction III (Organic Matter and Sulfides), the As contents (mg kg^− 1) were: unoxidized tailings (537–6308), oxidized tailings (215–2893), agricultural soil (0.52–25) and effluent sediments (0.05–0.25). The behavior of the As concentration was as follows: oxidized tailings > unoxidized tailings > agricultural soil > effluent sediments. Both fractions III and II are considered among the most important in the adsorption of PTE (Aguilar-Hinojosa et al. 2016). In the case of tailings, organic matter is absent; however, there is a high presence of sulfides. The redox potential can affect the degradation and solubility of organic matter and sulfides, influencing the release of PTEs (Gómez-Álvarez 2008). Under oxidizing conditions, sulfides can be oxidized, causing the release of As (Bravo et al. 2020).

The Residual fraction presented the following minimum and maximum concentrations (mg kg^− 1): unoxidized tailings (3800–15999), oxidized tailings (2496–28299), agricultural soil (4–861), and effluent sediments (2–6). The As concentration is distributed as follows: residual fraction > fraction II > fraction III > fraction I (Fig. 5). In global terms, arsenic predominates in the residual fraction in more than 60%. This fraction contains the inert arsenic found within the crystalline structure of some primary and secondary minerals (Pagnanelli et al. 2004; Gómez-Álvarez 2008). The arsenic bound to this fraction is stable; it can not solubilize under normal environmental conditions and, therefore, could not impact the environment and be biologically available in a reasonable geological time (Gómez-Álvarez 2008).

In general terms, the As concentration behavior was: unoxidized tailings > oxidized tailings > agricultural soil > effluent sediments (Tables 11, 12, 13, and 14). Regarding tailings (oxidized and unoxidized), approximately 20% of the As concentration is encountered in the non-residual fraction (fraction I + fraction II + fraction III), being available and having mobilization capacity. Under environmental conditions, this may occur in a reasonable geological time (Bravo et al. 2020) (Fig. 5). The agricultural soil (station 5B), located in the "El Lavadero" MEL discharge, presented considerable amounts of As in the non-residual fraction (194 mg kg^− 1) (Table 12), and it has a potential for mobilization to the environment. Concerning the effluent sediment, less than 1 mg kg^− 1 of As is found in the non-residual fraction, predominating in the residual fraction (> 80%) (Fig. 5); therefore, the dissolution of As towards the aqueous phase could not represent a danger to the environment.

Based on the previous analysis, arsenic present in the first three fractions (non-residual fraction) (> 60%) can be released into the environment, which will depend on the environmental variations that may occur. They are the changes in the redox potential, pH, temperature, and others (Gorny et al. 2018). In the case of tailings, only the fraction of exchangeable and soluble arsenic exceeds the maximum permissible value (5 mg kg^− 1) established by Mexican regulations for total As (SEMARNAT 2009).

Table 11

As concentration (mg kg^− 1) in the geochemical fractions of unoxidized tailings (Sequential Extraction)
Fractions	Sampling Stations (Unoxidized Tailings)
Fractions	2B	3A	3C	4A	4B
I (Exchangeable and Soluble)	293.12	208.97	167.32	154.86	183.26
II ( Fe and Mn Oxides )	1482.19	1157.75	401.99	639.81	431.54
III (O.M. and sulfides)	2752.06	6308.43	537.46	1518.84	590.37
Residual	12,819.48	15,988.66	3799.65	10,758.07	5255.45
Total	17,346.85	23,663.82	4906.41	13,071.57	6460.62

Table 12

As concentration (mg kg^− 1) in the geochemical fractions of oxidized tailings (Sequential Extraction)
Fractions	Sampling Stations (Oxidized Tailings)
Fractions	1A	1B	1C	2A	3B
I (Exchangeable and Soluble)	367.85	23.77	24.11	466.96	124.69
II ( Fe and Mn Oxides )	735.50	495.73	179.19	1053.35	685.80
III (O.M. and sulfides)	215.24	284.34	169.82	2893.29	2367.69
Residual	28,298.92	10,094.14	2495.52	8147.97	5149.44
Total	29,617.50	10,897.99	2868.64	12,561.57	8327.62

Table 13

As concentration (mg kg^− 1) in the geochemical fractions of agricultural soil (Sequential Extraction)
Fractions	Sampling Stations (Agricultural Soil)
Fractions	5A	5B	5C	6A	6B
I (Exchangeable and Soluble)	4.45	16.30	2.06	0.83	0.82
II ( Fe and Mn Oxides )	8.85	151.53	5.06	1.48	1.21
III (O.M. and sulfides)	3.46	25.44	1.69	0.70	0.52
Residual	42.33	861.34	20.14	11.19	4.39
Total	59.09	1054.62	28.95	14.21	6.94

Table 14

As concentration (mg kg^− 1) in the geochemical fractions of Effluent Sediments (Sequential Extraction)
Fractions	Sampling Stations (Effluent Sediments)
Fractions	EF1	EF2	EF3	EF4	EF5	BC
I (Exchangeable and Soluble)	0.11	0.08	0.11	0.05	0.07	0.09
II ( Fe and Mn Oxides )	0.22	0.26	0.36	0.40	0.15	0.52
III (O.M. and sulfides)	0.25	0.11	0.06	0.05	0.05	0.14
Residual	5.36	2.74	3.49	2.52	3.27	3.74
Total	5.94	3.18	4.03	3.03	3.54	4.49

Geoaccumulation Index (Igeo)

The Igeo results for arsenic are indicated in Table 15. All the tailings (oxidized and unoxidized) of the "El Lavadero" MEL present extreme contamination; this is coherent because the MEL was formed during different periods of the last century. Station 5B (water discharge zone from the tailings) is also classified as extremely polluted. The remaining agricultural soil and effluent sediment stations were classified as moderately to heavily polluted. The above highlights the impact produced by the MEL on its surrounding environment. These results agree with different contamination indices determined at the site in other studies (Espinoza-Madero 2012; Del Río-Salas et al. 2019; Loredo-Portales et al. 2020).

Table 15

Results of the Geoaccumulation Index (arsenic)
Station	Type of Sample	Igeo	Classification
1A	Oxidized Tailing	9.8	Extremely polluted
1B	Oxidized Tailing	8.8	Extremely polluted
1C	Oxidized Tailing	7.7	Extremely polluted
2A	Oxidized Tailing	9.6	Extremely polluted
3B	Oxidized Tailing	8.8	Extremely polluted
2B	Unoxidized Tailing	9.3	Extremely polluted
3A	Unoxidized Tailing	9.9	Extremely polluted
3C	Unoxidized Tailing	7.9	Extremely polluted
4A	Unoxidized Tailing	9.2	Extremely polluted
4B	Unoxidized Tailing	8.4	Extremely polluted
5A	Agricultural Soil	2.6	Moderately to strongly polluted
5B	Agricultural Soil	5.1	Extremely polluted
5C	Agricultural Soil	2.6	Moderately to strongly polluted
6A	Agricultural Soil	2.5	Moderately to strongly polluted
6B	Agricultural Soil	2.9	Moderately to strongly polluted
EF1	Effluent Sediment	2.6	Moderately to strongly polluted
EF2	Effluent Sediment	2.2	Moderately to strongly polluted
EF3	Effluent Sediment	2.1	Moderately to strongly polluted
EF4	Effluent Sediment	2.0	Moderately to strongly polluted
EF5	Effluent Sediment	2.3	Moderately to strongly polluted

Mining waste in areas surrounding San Felipe de Jesús town is considered a potential source of contaminants, including arsenic. The results indicate that arsenic prevails in the finest granulometric fractions (silt + clay, < 0.05 mm), harming the environment because these particles can be transported suspended in water media. Furthermore, its solubilization can be favored due to the greater exposed surface area. In a lesser proportion, arsenic is present in the sand fraction (0.05–2 mm).

In agricultural soil, As again predominated in the finest fraction (sand + silt + clay; < 2 mm), which may favor assimilation by plants due to the effective solubilization potential that this metalloid can present. Arsenic was detected mainly in the coarsest fraction (> 2 mm) in the effluent sediments, corresponding to gravel.

Regarding the As association in the different geochemical fractions, a large percentage of As (5–40%) is associated with the non-residual fraction (fraction I + fraction II + fraction III) in the tailings (oxidized and unoxidized), agricultural soil, and effluent sediments, indicating that depending on the environmental conditions (Eh, pH, temperature), As can be redissolved and present high mobility in abiotic media, potentially having a final impact in aquatic and terrestrial biota. The above is more critical in the tailings (oxidized and unoxidized) as well as in station 5B of agricultural soil as it presents high values of arsenic in the non-residual fraction (> 193 mg kg^− 1).

The high levels of arsenic detected and its degree of association by particle size and geochemical fraction establish that it has considerable mobilization potential and may be available for biota. The "El Lavadero" MEL represents a critical environmental contamination (water, air, soil), considering arsenic is a cumulative and highly toxic metalloid. High levels of arsenic can affect surrounding food crops intended for human and animal consumption, including the natural water supply sources of San Felipe de Jesús town and the effluents discharged into the Sonora River.

Based on the above, rehabilitating the "El Lavadero" MEL is important to avoid a more significant environmental impact. Additionally, the quality of the water from the supply sources surrounding the "El Lavadero" MEL is recommended to be periodically monitored.

Acknowledgements

The authors thank the Interdisciplinary Faculty of Engineering and the Department of Chemical Engineering and Metallurgy of the University of Sonora for supporting this research. We also acknowledge Dr. Francisco Brown Bojórquez Torres for their contribution in the XRD and SEM analysis.

Funding

This work was partially supported financially by the University of Sonora.

Competing Interests

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

Data Availability

This manuscript includes all the data generated and analyzed in the current investigation.

Author Contributions

Francisco Javier Mora-Sánchez: Experimental activity (field sampling, sample preparation, digestion, instrumental analysis of arsenic by atomic absorption techniques), data analysis, writing, translation (English), manuscript submission; Agustín Gómez-Álvarez: Experimental activity (field sampling, advice on preparation and digestion of tailings, soil, and sediment samples), instrumental analysis (analysis of total arsenic by atomic absorption techniques (flame and hydride generation), data analysis, corrections, and writing; Martin Antonio Encinas-Romero: Data analysis, translation support; Jesus Leobardo Valenzuela-García: Data analysis, translation support; Kareen Krizzan Encinas-Soto: Support in the analysis of arsenic by the flame atomic absorption technique and hydride generation; Martin Jara Marini: Field sampling, corrections, writing, and translation support; Arturo Israel Villalba-Atondo: Field sampling, granulometric analysis, and data interpretation; Guadalupe Dorame-Carreño: Support in the analysis of arsenic by the flame atomic absorption technique and hydride generation.

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Granulometric and Geochemical Distribution of Arsenic in a Mining Environmental Liability in a Semi-arid Area

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Abstract

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Introduction

Materials and Methods

Study Area

Sampling and Sample Preparation

Physicochemical Analysis

Geoaccumulation Index (Igeo)

Quality Control

Results and Discussion

Granulometric Analysis

Mineralogical Characterization

Scanning Electron Microscopy

Physicochemical parameters

Total Arsenic

Soluble As (Extraction Test of Toxic Constituents)

As Distribution by Granulometric Fractions

Arsenic in the Geochemical Fractions (Sequential Extraction)

Geoaccumulation Index (Igeo)

Conclusions

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