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Communication

On the Scarce Occurrence of Arsenic in Vineyard Soils of Castilla La Mancha: Between the Null Tolerance of Vine Plants and Clean Vineyards

by
Raimundo Jiménez-Ballesta
1,*,
Francisco J. García-Navarro
2,
José A. Amorós
2,
Caridad Pérez-de-los-Reyes
2 and
Sandra Bravo
2
1
Department of Geology and Geochemistry, Autónoma University of Madrid, 28049 Madrid, Spain
2
High Technical School of Agricultural Engineers of Ciudad Real, University of Castilla-La Mancha, 13071 Ciudad Real, Spain
*
Author to whom correspondence should be addressed.
Pollutants 2023, 3(3), 351-359; https://doi.org/10.3390/pollutants3030024
Submission received: 26 May 2023 / Revised: 19 July 2023 / Accepted: 22 July 2023 / Published: 26 July 2023
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Abstract

:
Arsenic (As), a widely distributed metalloid in the Earth’s crust, constitutes one of the most significant environmental contaminants today. This study was carried out to determine As concentrations in the soils of a Castilla La Mancha (CLM; Spain) benchmark collection that represents all the soil orders (soil taxonomy) in this territory. It also examined vine plant tolerance to As in relation to soil concentration. For this purpose, soils and leaves from vineyards were collected from 10 locations in the CLM community. The bioconcentration factor (BCF) of As in vineyards was assessed. The results of the present study show that As content in soils is widely variable, and is fundamentally related to soil type and parent material. The most surprising point is that, although some vineyards have been treated with As derivatives, the vast majority of them do not accumulate any amount of As. This important finding must be used to enhance the quality of the final obtained product: wine. In other words, CLM wines are not at risk of As contamination and must, therefore, be clean wines. Our results suggest that CLM vineyards are clean of contamination by As because this element in leaves reveals null vine capacity to accumulate As, a process that derives from scarce As in soils and the traditional practices carried out by winegrowers.

Graphical Abstract

1. Introduction

Globally speaking, soil is an important compartment of the environment, in which anthropogenic loading of potential toxic elements (PTEs) poses a health risk for ecosystems and their inhabitants. Accumulation of PTE trace metals in soil has the potential to restrain soil functions, cause plant toxicity and enter the food chain [1]. Therefore, knowledge of PTEs in the environment is an essential requirement within various regulatory frameworks that aim to ensure a high level of protection for human health and the environment through safe, sustainable chemical use.
Arsenic (As) is the 20th most abundant naturally occurring element in the Earth’s crust, and is widely dispersed in the environment. Primarily associated with igneous and sedimentary rocks, As is naturally found in soils because of natural processes, including the weathering of As-enriched minerals, volcanic emissions and biological activities [2]. It is generally joined to or mixed with other elements, but has a particular affinity for sulfur and can, thus, also be joined to sulfur [3].
According to the OIV (International Organisation of Vine and Wine) [4], As is a metalloid that is present in the Earth’s crust at levels as high as 3.4 mg kg−1, although Bowen [5] suggests a lower value of 1.5 mg kg−1. It can fall within different concentration ranges in soil [4,6]. In line with Kabata-Pendias [7], the total As concentration in uncontaminated soils varies from 0.1 to 95 mg kg−1, with a mean of <10 mg kg−1. However, As appears in both edaphic processes (from parent material), and in anthropic processes.
Arsenic is toxic, and has been used as a pesticide, fungicide and herbicide for a long time [8]. Indeed metalloid As, a natural environmental contaminant that shares properties of metals and nonmetals, was the commonest form of pesticide until World War II, and was still used in the 1970s and 1980s [9]. The use of organic arsenical pesticides began in the 1950s and has continued practically to the present day [10]. However, they were forbidden at the end of the twentieth century [11].
Natural As content in soils globally ranges from 0.01 to >600 mg kg−1, with a mean of about 2–20 mg kg−1 [12]. In soils, pentavalent As predominates, due to the oxidation of trivalent arsenicals [13]. According to [14], however, many studies have shown that the relative oral As bioavailability (defined as the fraction of ingested arsenic absorbed across the gastrointestinal barrier and available for systemic distribution and metabolism) in soils, is less than 50%. In any case, vineyards with high contents can respond to geochemical anomalies and are, therefore, natural causes [15]. There are also anthropogenic causes induced from applying pesticides, among other factors. In fact, prior to its use in vineyards, As had a similar history to many other naturally occurring elements now known to be lethal, including lead. Arsenic predominating as a treatment in vineyards dates back to remote times, when it was necessary to control molds and pests in vineyards. The best-known treatments include organic and inorganic As compounds like monosodium methanearsonate, calcium arsenate, lead arsenate and copper arsenate. At this point, it is worth highlighting the well-known Paris Green (copper arsenate), which was used to rid vineyards of molds [10].
Experience has shown the need to eliminate As use in vineyards, although it is important to note that As still occurs naturally in earth [2]. The EPA (Environmental Protection Agency) [16] has set a standard level of inorganic As in drinking water at a maximum value of 10 parts per billion (ppb). The mechanism by which As can be incorporated into vine is through grapevine roots and leaf tissue. It should be noted that only a minimal amount of As relocates to the skin, pulp and seeds of berries in grapevines [17]. Thus, some studies suggest that the accumulation of heavy metals in plant tissues could inhibit significant plant enzymatic activity, which would result in a wide range of adverse effects, such as photosynthetic processes [18].
The bioconcentration factor (BCF) and the bioaccumulation factor (BAF) are used as criteria for bioaccumulation when identifying and classifying hazardous substances for the environment [19]. It is understood that the BCF is a calculated value that indicates the ability of plants to remove metal compounds from soil. Therefore, the BCF is an important parameter that is employed in the feasibility study of heavy metals, plant remediation potential and phytoremediation. According to Usman et al. [20], plants with a BCF of >1 can be used as bioaccumulators, while BCF values of >2 can be considered high bioaccumulators. Therefore, a BCF value of >1 indicates that a plant is an accumulator, whereas a value <1 implies that the plant cannot be used as an accumulator.
Although many factors can influence the chemical composition of wine, including grape variety, soil type, climate and winemaking practices, currently the quality of wine and its aroma/flavor characteristics are discussed in relation to its chemical composition As is interesting for its toxicity. Despite the studies carried out on As, scarce information is available on the BCFs of this element in Castilla La Mancha (CLM) vines. In a preliminary study, Jiménez-Ballesta et al. [21] found that the As in the vineyard soils of the Valdepeñas PDO contained different concentrations. However, to the best of our knowledge, this is the first study to examine specific As tolerance and tissue accumulation capacity in relation to the background As concentration in soil. Consequently, the present work was carried out to determine the BCF values of vine (Vitis vinífera L.) from CLM, to find out if As bioaccumulated in vine leaves or not. The ultimate goal was to protect consumers from exposure to As toxicity as a result of regular consumption. With all this in mind, the main objectives of this study were to conduct fieldwork to understand As contents in vineyard soils, look for the vertical distribution in the vineyard soil profiles in the CLM community and, at the same time, analyze As contents in leaves. The ratios of As contents in leaves to those in vineyard soils were calculated, to determine the BCF of As. Hence, the present work aimed to provide the accumulation capacity of bioconcentration or bioexclusion (this last understood as external biosecurity, which involves preventing the introduction of new diseases into a population from an outside source) of As in the vines collected in CLM.

2. Material and Methods

2.1. Sample Collections

Soil and leaf samples were collected from the five provinces of the CLM Community (Figure 1). Profiles were opened using a caterpillar machine in 2012 and 2015. Soils were described according to the criteria defined by the FAO [22].
Soil samples (n = 20) were collected from the corresponding 10 soil vineyard profiles (Table 1), generally a horizon of type A and another of type B. In the soils under study, horizon A usually develops between 0 and 40 cm maximum, while horizon B is usually between 40 and 90 cm deep. Around each profile, 20 leaves approximately from the center of the shoot were collected before harvest. Subsequently, in the laboratory, leaf samples were oven-dried for 7 days at 36 °C.
In general, the Tempranillo variety grafted onto the 110 Richter rootstock is that used and, therefore, most samples were collected in the vineyards of this type.

2.2. Analytical Procedures

In the laboratory, soil samples were dried to a constant weight and homogenized and, after grinding, were passed through an 80-mesh sieve to obtain very fine particles. Homogenization was performed using quartering and pulverization procedures. X-ray fluorescence (XRF) spectrometers are widely used to determine trace elements [25,26,27,28,29,30]. XRF measurements were taken by a PHILIPS PW (2404) spectrometer in the solid mode in a powdered aliquot of each sample. The pearls of soil samples were analyzed at a maximum power of 4 kW (set of crystal analyzers for LiF220, LiF200, Ge, PET and PX1, flow detector and twinkle detector). An analysis of samples was carried out with pearls of lithium borate. Quality control was achieved using Certified Reference Materials for soils (NIST 2710, CRM 039, BCR 62, SMR 1573A, SMR 1515). The precision and reproducibility of the method were determined by analyzing four replicates of one representative sample and calculating the coefficient of variation. The lower limit of detection (LLD) was 0.3. The quality assurance and acceptable precision of the level of standard deviation was 3.7. According to these results, the method can be considered reproducible and precise.

2.3. Determining the Bioaccumulation Factor

The BCF is the ratio of the concentration of heavy metals in plants and soils. It is an indicator of a plant’s capacity to accumulate heavy metals [16]. The BCF was used to assess the transfer of As from soil to vine plant, calculated with the equation 1 as below:
BCF = Cc/Cs
where Cc represents As content (as dry matter) in plants and Cs depicts the element concentration in the corresponding soils.

3. Results and Discussion

Elemental as Concentrations in Soils

Table 2 summarizes the elemental As concentrations for the soil samples collected from 10 wine subregions. Concentrations were calculated to express their values as oven-dried weights of soils. The As concentration in soils ranged from 0 to 24.8 mg kg−1, with a mean of 7.3 mg kg−1 on surface horizons and 8.2 mg kg−1 on subsurface horizons. The mean total was 7.8 mg kg−1. Whether soil horizons showed higher As concentrations than the deeper horizon, and vice versa, was not detected. This homogeneity may be attributed to mixing for tillage. However, a marked drop in As concentrations was observed at depth in two soil profiles: case profiles 1 and 6. Only in case profile 10 did As content exceed the reference values (16.1 mg kg−1) proposed by [22,31].
The As content of a given soil is primarily determined by that soil’s parent materials and by anthropogenic inputs [12]. In CLM, pedological processes also intervene, but there is rarely anthropogenic input. The different soil types are attributed to various processes such as partial weathering, accumulation of carbonates, argiluviation, rubefaction, gypsum accumulation, etc. Finally, there are two singular processes of slight territorial importance, salification and gleyzation. In any case, delving into the processes, it is worth noting that the local climate, which is characterized by marked differences between the dry and rainy seasons, should also favor the release of iron from primary Fe-bearing minerals—after their hydrolysis, oxidation and crystallization of residuals—in the form of hydroxides and oxyhydroxides (hematite and other related mineral phases), which are responsible for the characteristic red color of these soils. The studied soils did not show eluvial horizons, whereas clay rainfall and accumulation of iron oxides (red color) were commonly observed.
We obtained a surprising result for As content in leaves: there was no evidence for As concentrations. In the literature, some research studies, like those of [24,32], report marked As accumulation in plants growing in strongly contaminated sites (affected by mining activity). This was not the case of the CLM studied soils. Therefore, calculating the BCF (to assess whether vines could be categorized as accumulators) did not prove valuable in the case study.
Arsenic contents in vineyard soils vary, mainly according to soil type and parent materials. It is understood that parent material is the initial state of the solid matter making up a soil. It can consist of consolidated rocks, and it can also include unconsolidated deposits such as river alluvium, lake or marine sediments, glacial tills, loess, etc. Parent materials influence soil formation through their mineralogical composition, their texture, and their stratification (occurrence in layers). Dark-colored ferromagnesian (iron- and magnesium-containing) rocks, for example, can produce soils with a high content of iron compounds and of clay minerals in the kaolin or smectite groups, whereas light-colored siliceous (silica-containing) rocks tend to produce soils that are low in iron compounds and that contain clay minerals in the illite or vermiculite groups. The coarse texture of granite rocks leads to a coarse, loamy soil texture, and promotes the development of E horizons (the leached lower regions of the topmost soil layer). The fine texture of basaltic rocks, on the other hand, yields soils with a loam or clay-loam texture, and hinders the development of E horizons.
In soils, the baseline As concentration is generally in the order of 5-10 mg kg−1 [33]. The mean amount of As in soils in European topsoil is 7.0 mg kg−1 [34]. Therefore, the studied soils fell within the European range. In any case, the As content in the topsoil did not exceed the optimum value recommended by the new Dutchlist (29 mg kg−1 As) (http://www.contaminatedland.co.uk/std-guid/dutch-l.htm, accessed on 24 June 2023). In Asian countries, As concentrations generally range from 5 to >50 mg kg−1 [35], but tend to be comparatively higher in mining areas [36,37,38,39,40].
In soil and related environments, the transformation and mobility of As are governed by abiotic and biotic processes [41]. Abiotic processes include sorption, desorption, precipitation, dissolution and redox reactions. Soil components, which are able to sorb ions in soil, include phyllosilicates, allophanes, imogolite, carbonates, and Fe, Al and Mn oxides, organic matter (OM) and microorganisms [42]. In the studied soils, Amoros et al. [43] highlighted abundant carbonates, and also phyllosilicates and Fe oxides, so the As mobility in these soils can be interpreted as low.
Arsenate (V) is the thermodynamically stable form of As under aerobic conditions, and interacts strongly with the solid matrix. Movement of As in soils depends on the adsorption–desorption reactions in the solid phase. In semi-arid areas, like those studied, where reddish brown earth soil is present, well or moderately well-drained conditions prevail. Under these conditions, red soils with argillic horizons were observed (profiles 3, 6, 7 and 10). In these cases, clays (<2 µm) and iron oxides can absorb As, because of their edge [33].
If we take into account the fact that concentrations of > 50 mg kg−1 are also considered dangerous in several countries, and soil remediation procedures are recommended above this threshold [44], the first results obtained in this study indicate that there is no risk of As presence in the soils and vine leaves of this region.
Globally speaking, high As levels in soils are often of geogenic origin, and related to natural processes (i.e., weathering of minerals). Currently, soil enrichment with As at levels far above the reference values results from anthropogenic activities, and thus agricultural soils are slightly to moderately contaminated by heavy metal toxicity. Here, the interpretation is that it could be due to long-term use of phosphatic fertilizers, sewage sludge applications, industrial waste and inadequate watering practices [45,46].
The BCF is one of the metrics used to evaluate the potential of a substance to bioaccumulate in organisms. Based on the obtained results, although [47] have stated the presence of As and other strata elements in Croatian wines, and some authors like [48,49,50], have indicated that the application of pesticides, fungicides and fertilizers containing Cd, Cu, Mn, Pb and Zn compounds leads to larger amounts of these metals in wine, it is unlikely that the constitution of the wines from CLM is affected by the presence of As.
The BCF is provided in numerous articles [50,51,52,53,54,55]. However, the accumulation of heavy metals from soil to plants is a complex process that is affected by multiple factors, which intervene through several mechanisms, including soil pH, soil organic matter content, plant species, climatic conditions, etc. In particular, clay minerals and other soil colloids can also influence the bioavailability of heavy metals. Zhou and Li [29] suggested that for a given soil pH, increasing the proportion of clay particles (<2 µm) can enhance the soil’s zinc (Zn) adsorption capacity, therefore limiting Zn transfer to plants. In addition, the bacteria and fungi surrounding plant roots can promote plants’ uptake of As, and also of heavy metals, by changing their activity. It is known that some bacteria can reduce As, while others can oxidize As [56].

4. Conclusions

The present study was conducted to determine As contents, which is an essential element, but is toxic at high concentrations, in the soils and leaves of CLM vineyards. The As concentration in soils ranged from 0 to 24.8 mg kg−1, with a mean of 7.3 mg kg−1 on surface horizons and 8.2 mg kg−1 on subsurface horizons. The average total As was 7.8 mg kg−1. This study reports null As concentrations in vine leaves, because the BCF of As in leaves revealed null vine capacity to accumulate that element, a process that derives from As scarcity in soils. In addition, usual viticultural practices are reasonably carried out by winegrowers. Therefore, our results suggest that CLM vineyards are clean of contamination by As, so it can be concluded that consuming the wine from these vineyards cannot be considered a toxicological risk.

Author Contributions

R.J.-B. conceived and designed this study; F.J.G.-N., R.J.-B., C.P.-d.-l.-R. and J.A.A. participated in the collection of soil samples. Software, S.B.; formal analysis, S.B.; writing—original draft preparation, R.J.-B., writing—reviewing and editing, R.J.-B., F.J.G.-N. and S.B. All authors have read and agreed to the published version of the manuscript.

Funding

This research was funded by the Gobierno de Castilla La Mancha (Government of Castilla-La Mancha) research project ‘Vineyard Soils of Castilla La Mancha: influence on grape composition’.

Data Availability Statement

The data and materials will be made available from the corresponding author(s) upon reasonable request.

Acknowledgments

The authors wish to acknowledge the financial support given by the Regional Government of Castilla-La Mancha (Spain).

Conflicts of Interest

The authors declare no conflict of interest.

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Pollutants 03 00024 g001 550
Figure 1. Schematic situation map of the Castilla La Mancha territory, including its five provinces. Coordinates: 41.778 (N); 0.866 (E); 37.892 (S); 41.778 (W).
Figure 1. Schematic situation map of the Castilla La Mancha territory, including its five provinces. Coordinates: 41.778 (N); 0.866 (E); 37.892 (S); 41.778 (W).
Pollutants 03 00024 g001
Table
Table 1. Description and edaphic characteristics of the studied soils. Soil Classification by means of Soil Survey Staff [23] and IUSS Working Group [24]. The grown grapes are Tempranillo.
Table 1. Description and edaphic characteristics of the studied soils. Soil Classification by means of Soil Survey Staff [23] and IUSS Working Group [24]. The grown grapes are Tempranillo.
Wine RegionsLocation (Coordinates)Parent MaterialDrainageMorphologySoil Type
IUSS Group/Soil Taxonomy
1Almansa
(Albacte)		(30 s) 665754 x–4308009 yGreen MarlsModerately well-drainedAp-Bw-2Cg1-2Cg2Endogleyic Cambisol (Calcaric, Novic)/
Aquic Haploxerept
2C. Calatrava (Ciudad Real)(30 s) 0412661 x–4322211 yFluvial sedimentsModerately well-drainedAp-Ckm1-Ckm2Petric Calcisol (Skeletic, Novic)/
Petrocalcic Calcixerept
3Mancha (Albacete) (30 s) 0525789 x–4304004 yLimestoneModerately well-drainedAp-Bt-RLeptic Luvisol (Clayic, Rhodic)/
Lithic Rhodoxeralf
4Mancha (Ciudad Real) (30 s) 500059 x–4339662 yMarlsModerately well-drainedAp-Bw-BC-CkHaplic Cambisol (Eutric, Arenic)/
Typic Haploxerept
5Mancha (Cuenca)(30 s) 514046 x–4361360 ySandsSomewhat excessively drainedAp-C1-C2Protic Arenosol (Eutric, Hyperochric)/
Typic Xeropsamment
6Mancha (Toledo) (30 s) 467601 x–4384620 yPoligenic sedimentsModerately well-drainedAp-Bt1-2Ck-3Bt2Calcic Luvisol (Siltic, Chromic)/
Calcic Haploxeralf
7Manchuela (Cuenca) (30 s) 0569515 x–4357046 yMarlsImperfectly drainedAp-Bw-CCalcic Luvisol (Clayic, Rhodic)/
Calcic Rhodoxeralf
8Méntrida Toledo)(30 s) 383622 x–4428093 yArkosesSomewhat excessively drainedAp-Bt-CHaplic Luvisol (Arenic, Chromic)/
Typic Haploxeralf
9Montes (Toledo) (30 s) 0406159 x–4428125 yQuartzite and shale sedimentsWell-drainedAp-Bw-CHaplic Cambisol (Dystric, Skeletic)/
Typic Dystroxerept
10Valdepeñas (Ciudad Real) (30 s) 473093 x–4296586 yColluviumModerately well-drainedAp-Bt-Bt/C-CCutanic Luvisol (Skeletic, Rhodic)/
Inceptic Rhodoxeralf
Table
Table 2. The results, ratios and bioconcentration factor of As in vineyards.
Table 2. The results, ratios and bioconcentration factor of As in vineyards.
Wine RegionsSurface Horizon
(Ap)		Subsurface Horizon
(B or C)		Surface/
Subsurface 		LeavesBCF
As (mg kg−1)As (mg kg−1)
11 Almansa
(Albacte) 		3.51.52.33<LLD0.0
22 C. Calatrava (Ciudad Real) 0.30.80.37<LLD0.0
33 Mancha (Albacete) 12.111.81.02<LLD0.0
44 Mancha (Ciudad Real)12.810.71.12<LLD0.0
55 Mancha (Cuenca) 0.01.90.0<LLD0.0
66 Mancha (Toledo) 6.47.03.76<LLD0.0
77 Manchuela (Cuenca) 7.710.40.74<LLD0.0
88 Méntrida (Toledo) 6.19.60.63<LLD0.0
99 Montes (Toledo) 4.24.11.02<LLD 0.0
1010 Valdepeñas (Ciudad Real) 18.024.80.72<LLD0.0
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Jiménez-Ballesta, R.; García-Navarro, F.J.; Amorós, J.A.; Pérez-de-los-Reyes, C.; Bravo, S. On the Scarce Occurrence of Arsenic in Vineyard Soils of Castilla La Mancha: Between the Null Tolerance of Vine Plants and Clean Vineyards. Pollutants 2023, 3, 351-359. https://doi.org/10.3390/pollutants3030024

AMA Style

Jiménez-Ballesta R, García-Navarro FJ, Amorós JA, Pérez-de-los-Reyes C, Bravo S. On the Scarce Occurrence of Arsenic in Vineyard Soils of Castilla La Mancha: Between the Null Tolerance of Vine Plants and Clean Vineyards. Pollutants. 2023; 3(3):351-359. https://doi.org/10.3390/pollutants3030024

Chicago/Turabian Style

Jiménez-Ballesta, Raimundo, Francisco J. García-Navarro, José A. Amorós, Caridad Pérez-de-los-Reyes, and Sandra Bravo. 2023. "On the Scarce Occurrence of Arsenic in Vineyard Soils of Castilla La Mancha: Between the Null Tolerance of Vine Plants and Clean Vineyards" Pollutants 3, no. 3: 351-359. https://doi.org/10.3390/pollutants3030024

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