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Article

Geochemical Behaviour of Trace Elements in Diesel Oil-Contaminated Soil During Remediation Assisted by Mineral and Organic Sorbents

by
Mirosław Wyszkowski
* and
Natalia Kordala
Department of Agricultural and Environmental Chemistry, University of Warmia and Mazury in Olsztyn, Łódzki 4 Sq., 10-727 Olsztyn, Poland
*
Author to whom correspondence should be addressed.
Appl. Sci. 2025, 15(15), 8650; https://doi.org/10.3390/app15158650 (registering DOI)
Submission received: 13 June 2025 / Revised: 1 August 2025 / Accepted: 3 August 2025 / Published: 5 August 2025
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Abstract

The topic of environmental pollution by petroleum products is highly relevant due to rapid urbanisation, including industrial development, road infrastructure and fuel distribution. Potential threat areas include refineries, fuel stations, pipelines, warehouses and transshipment bases, as well as sites affected by accidents or fuel spills. This study aimed to determine whether organic and mineral materials could mitigate the effects of diesel oil pollution on the soil’s trace element content. The used materials were compost, bentonite and calcium oxide. Diesel oil pollution had the most pronounced effect on the levels of Cd, Ni, Fe and Co. The levels of the first three elements increased, while the level of Co decreased by 53%. Lower doses of diesel oil (2.5 and 5 cm3 per kg of soil) induced an increase in the levels of the other trace elements, while higher doses caused a reduction, especially in Cr. All materials applied to the soil (compost, bentonite and calcium oxide) reduced the content of Ni, Cr and Fe. Compost and calcium oxide also increased Co accumulation in the soil. Bentonite had the strongest reducing effect on the Ni and Cr contents of the soil, reducing them by 42% and 53%, respectively. Meanwhile, calcium oxide had the strongest reducing effect on Fe and Co accumulation, reducing it by 12% and 31%, respectively. Inverse relationships were recorded for Cd (mainly bentonite), Pb (especially compost), Cu (mainly compost), Mn (mainly bentonite) and Zn (only compost) content in the soil. At the most contaminated site, the application of bentonite reduced the accumulation of Pb, Zn and Mn in the soil, while the application of compost reduced the accumulation of Cd. Applying various materials, particularly bentonite and compost, limits the content of certain trace elements in the soil. This has a positive impact on reducing the effect of minor diesel oil pollution on soil properties and can promote the proper growth of plant biomass.
Keywords:
diesel oil; soil; materials; Cd; Pb; Cr; Ni; Zn; Cu; Fe; Mn; Co

1. Introduction

Due to rapid urbanisation, industrial development and the construction of road infrastructure and fuel distribution systems, the topic of environmental pollution by petroleum products is highly relevant [1]. Potentially threatening locations include refineries, fuel stations, pipelines, warehouses and transshipment bases, as well as sites affected by accidents or fuel spills [2]. Petroleum substances are complex mixtures of aliphatic (both saturated and unsaturated) and aromatic hydrocarbons, as well as heterocyclic compounds that contain oxygen, nitrogen or sulphur atoms, and trace amounts of trace element ions, including iron, lead, tin, arsenic, mercury, antimony and vanadium [3,4]. Crude oil and its derivatives have a negative impact on the physical, chemical and biological properties of soil, reducing its fertility and limiting crop production [5]. Soil contaminated with hydrocarbons loses its colloidal structure [6], and both its primary (e.g., compactness, porosity and bulk weight) and secondary (e.g., water, heat and air) physical properties are disturbed [7,8]. The partial filling of soil pores by petroleum products reduces the soil’s water-holding capacity and impedes water percolation and subsoiling. It also reduces air exchange between the soil and the atmosphere [9] and increases oxygen demand and consumption [10]. When soil is subjected to pressure from oil derivatives, denitrification and processes that release hydrogen sulfide intensify [11]. These processes lead to the formation of compounds that are toxic to plant roots and soil microorganisms [12]. The exchange capacity of magnesium, sodium, calcium and potassium is impaired, reducing the availability of these macronutrients [13,14]. Due to the presence of numerous organic groups present in petroleum pollutants, the carbon-to-nitrogen ratio is altered, which affects soil fertility, the composition and content of organic matter, and the exchange of nutrients between plant roots and soil [15]. The presence of petroleum derivatives alters the composition and activity of soil microorganisms, thereby limiting the growth of certain strains [16] and destabilising the soil’s enzymatic activity [17]. This also alters nutrient and energy conditions. These changes contribute to the depletion of biodiversity and the degradation of ecosystems in areas contaminated with these substances [8]. Numerous studies [18,19,20] have demonstrated the adverse effects of petroleum products on the soil environment. A particularly dangerous and permanent threat to human health and the ecological functions of agricultural soils is contamination with polycyclic aromatic hydrocarbons (PAHs), a group of petroleum hydrocarbons [21]. This is due to their mutagenic and carcinogenic effects [22], as well as their ability to bioaccumulate. This can result in PAHs building up in the food chain downstream and eventually entering the human body [23]. Additionally, harmful trace elements (TEs) are introduced into the soil alongside petroleum substances [24], negatively affecting food security and soil quality [25]. According to Wang et al. [26], industrial activities at petrochemical plants lead to the accumulation of cadmium, copper, chromium, arsenic, zinc, lead and nickel in the soil.
In November 2021, the European Commission presented the European Parliament with the ‘Soil Strategy for 2030: Reaping the benefits of healthy soils for people, food, nature and climate’. The document indicated a significant increase in activities concerning the remediation of contaminated sites in the medium term (until 2030). The long-term goal for 2050 is to reduce soil contamination to levels that are harmless to human health and natural ecosystems, thereby creating a toxin-free environment [27]. According to a report by the European Environment Agency, 60–70% of EU soils are currently ‘unhealthy’, which could lead to problems with European Union (EU) food security in the future. Furthermore, the cost of soil degradation in the EU exceeds EUR 50 billion per year [28]. Therefore, seeking environmentally friendly and economically viable technological solutions to mitigate the harmful effects of oil pollution on soils is fully justified and in line with the EU’s climate and economic initiatives. In terms of protecting the soil environment, a preventive approach would be to replace conventional fossil fuels with biofuels wherever possible. Studies suggest that biodiesel is significantly more biodegradable than conventional diesel oil [29] and less toxic [30], thanks to its hydrocarbon-free composition and low particulate emissions [31]. This alternative fuel can be used by various indigenous soil microorganisms as a source of carbon and energy [32]. However, its higher density and viscosity compared to conventional diesel oil [33] result in reduced mobility in the soil profile, which may limit its dispersion in the environment. Despite its superior environmental properties, biodiesel can still cause soil contamination [34], especially in the event of a large spill [30], negatively affecting soil pH, the number of microorganisms and their relative composition, as well as the quantitative indicators of microbial processes [29,35]. The ecotoxicity profile of biodiesel depends largely on the dose, the type of feedstock used and the type of alcohol used during the production and further processing of the biofuel [31]. Methods for remediating contaminated soils can be categorised as physical methods (including storage, thermal desorption, vitrification and electrokinetics), chemical methods (including washing, solidification, redox transformation and stabilisation) and biological methods (including bioremediation, phytoextraction, phytovolatilisation and rhizofiltration) [36,37]. Undoubtedly, chemical methods have many advantages, including in situ stabilisation. These include low economic cost, simple implementation, the absence of secondary waste, applicability even to heavily contaminated sites and rapid results [37]. In situ chemical stabilisation technology uses a combination of inorganic (e.g., calcium- and phosphate-based compounds, fly ash and clay minerals) and organic (e.g., sewage sludge, compost and biocarbon) materials to treat contaminated soils. These materials immobilise contaminants by increasing soil pH and improving soil structure, water capacity and nutrient status [38,39], and increasing sorption capacity and/or improving soil microbial activity [40].
The mechanism by which contaminants are immobilised following the application of these soil additives involves a combination of adsorption, complexation and precipitation processes [41]. This reduces the mobility and availability of contaminants, as well as their vertical migration and surface runoff with rainwater [42]. Trace elements are primarily immobilised by precipitation when calcium compounds are applied due to the resulting elevated pH levels [43]. Concurrently, the availability of trace elements is diminished by the formation of insoluble organometallic complexes when compost is applied [42]. Additionally, Lu et al. [44] reported that introducing alkaline materials into contaminated soil significantly improves microbial diversity in the soil and encourages the growth of beneficial bacterial communities. This also increases catalase and urease activity, indicating its role in improving soil health and biochemical properties. The application of clay materials such as bentonite reduces the amount of trace elements available to plants in the soil due to their adsorption to the material’s surface and edges, as well as intercalation (i.e., the replacement of a cation in the interlayer space) [45]. It also increases the soil’s sorption capacity [46] and microbial and enzymatic activity [47]. The main component of bentonite is the clay mineral montmorillonite, which belongs to the smectite group of layered silicates and has very small particle sizes [48]. Consequently, it has a large specific surface area, a high permanent negative charge and a high cation exchange capacity (CEC) [49]. Numerous authors have proven the usefulness of bentonite in the adsorption of various trace elements, including lead (Pb) [50] and cadmium (Cd) [50,51], copper (Cu) [51], and chromium (Cr) [52]. Studies by Czaban et al. [53] showed that adding bentonite to loamy sand increased the organic carbon and nitrogen content, thereby improving soil fertility. Due to its properties, namely its large sorptive surface area and high CEC, bentonite improves a soil’s ability to retain water [54], increases its nutrient content and retention, and improves the structure of sandy soils [55].
Soils play a vital role in the functioning of terrestrial ecosystems. They provide key ecosystem services, facilitate the cycling of elements, regulate water relations, support biodiversity and mitigate climate change [56]. Therefore, improving the quality of degraded land is essential for protecting biodiversity and enhancing the capacity of ecosystems to deliver essential services for sustaining life on Earth and to ensure human well-being [57]. In 2018, stabilisation and solidification methods accounted for 48.5% of engineering applications [58], demonstrating their potential for dealing with trace elements in overburdened soils.
Accordingly, a study was conducted to determine the potential of the organic and mineral materials used to mitigate the effects of diesel oil pollution on the content of trace elements in the soil. Compost, bentonite and calcium oxide were used as materials. This study is notable for comparing the effectiveness of organic and mineral sorbents under the controlled conditions of a pot experiment. The results can be translated into specific remediation measures under environmental conditions.

2. Materials and Methods

2.1. Pot Vegetative Experiment

The present study was carried out in a vegetation hall belonging to the University of Warmia and Mazury in Olsztyn (Poland). The experiments were carried out in a two-factor pot experimental setup on soil taken from Eutric Cambisol topsoil [59]. Soil properties are included in Table 1. The soil had high concentrations of Fe and Mn.
The concentration of trace elements in materials (sorbents) was varied and amounted to the following: compost: Cd—0.058 mg per kg, Pb—1.86 mg per kg, Cr—1.24 mg per kg, Ni—0.49 mg per kg, Zn—32.86 mg per kg, Cu—39.56 mg per kg, Mn—54.4 mg per kg, Fe—229 mg per kg, and Co—0.49 mg per kg; bentonite: Cd—0.298 mg per kg, Pb—9.78 mg per kg, Cr—2.82 mg per kg, Ni—2.44 mg per kg, Zn—14.44 mg per kg, Cu—12.92 mg per kg, Mn—147.5 mg per kg, Fe—4236 mg per kg, and Co—0.30 mg per kg; and calcium oxide: Cd—3.487 mg per kg, Pb—2.92 mg per kg, Cr—3.36 mg per kg, Ni—3.54 mg per kg, Zn—4.36 mg per kg, Cu—2.28 mg per kg, Mn—158.3 mg per kg, Fe—424 mg per kg, and Co—1.73 mg per kg. The compost was composted over a period of six months using a mixture of waste materials from a farm, including leaves from various trees (e.g., cherry, apple, maple, plum trees), cattle manure and garden peat. Analysis revealed that the compost had the highest concentrations of Zn and Cu, while the calcium oxide had the highest concentrations of Mn, Cd, Cr, Ni and Co, and the bentonite had the highest concentrations of Pb and Fe. Furthermore, the compost sample had the lowest concentrations of Cd, Pb, Cr, Ni, Mn, Fe and Co, while the calcium oxide sample had the lowest concentrations of Zn and Cu.
The first-order factor was simulated soil pollution with diesel oil, applied at the following doses: 0, 2.5, 5 and 10 cm3 per kg. The second-order factor pertained to the application of organic and mineral materials, including compost, bentonite and 50% calcium oxide (CaO), to the soil at the following rates: 30 g, 20 g and 1.47 g per kg of soil, respectively. The diesel oil doses are low and may occur incidentally under real-world conditions. The levels of diesel oil and sorbent doses have been established based on previous studies [60]. Furthermore, the below quantities of nitrogen (N), phosphorus (P), potassium (K), magnesium (Mg), manganese (Mn), molybdenum (Mo) and boron (B) were added to all pots. The following substances were used: 150 mg of N as urea 46% (NH2)(CO)2, Grupa Azoty Zakłady Azotowe Puławy S.A, Poland; 30 mg of P as KH2PO4 (analytical purity), Avantor Performance Materials Poland, Gliwice, Poland; 75 mg of K as KH2PO4 + KCl (analytical purity), Avantor Performance Materials Poland, Gliwice, Poland; 50 mg of Mg as MgSO4·7H2O (analytical purity), Avantor Performance Materials Poland S.A., Gliwice, Poland; 5 mg of Mn as MnCl2·4H2O (analytical purity), Avantor Performance Materials Poland, Gliwice, Poland; 5 mg of Mo as (NH4)6Mo7O24·4H2O (analytical purity), Avantor Performance Materials Poland, Gliwice, Poland; and 0.33 mg of B per kg of soil as H3BO3 (analytical purity), Avantor Performance Materials Poland, Gliwice, Poland. The soil was thoroughly mixed with diesel oil and the aforementioned nutrients and minerals (in accordance with the experimental scheme), after which it was transferred to 9 kg plastic pots. Oats (Avena sativa L.) were then sown. In order to ensure the reliability of the obtained results, each experimental object was conducted four times. During the period of oat vegetation, the plants were irrigated in order to maintain constant soil moisture. The harvesting of the oats was conducted at the panicle stage, and concurrently, samples of the soil were obtained for trace element analysis in a chemical laboratory. The soil samples were taken on the 68th day after the start of the experiment.

2.2. Analytical Methodologies

Samples of soil material dried in the natural state (in the air) were passed through a sieve and then subjected to aqueous digestion [61]. In the resulting solutions, the content of trace elements was determined [62]. The atomic absorption spectrometry (AAS) method [62] was used to quantify trace elements in soil and materials (sorbents) after wet digestion of samples using the USEPA3051 method [61]. Details of the extractants used, the certified reference material (CRM), the standard materials and the apparatus used for trace element analyses in the soil are provided in Figure 1. The fundamental properties of the initial soil were also determined [63,64,65,66,67]. The following properties were determined in the initial soil: pH potentiometrically [63], HAC and CEC using the Kappen method [64], TOC using an analyser [65], the available P and K content using the Egner–Riehm method [66] and Mg using the Schachtschabel method [67]. A comprehensive description of the associated soil properties is provided in Figure 1.

2.3. Statistical Methods

The significance of the influence of the studied factors on soil properties was calculated with Statistica 13.3 software [68] using analysis of variance (ANOVA), Tukey’s HSD test, standard deviation, principal component analysis (PCA) and determination of the percentage of observed variability (by ANOVA method with η2 coefficient) for diesel oil pollution of soil, application of various materials and interaction of the studied factors. Cluster analysis using multivariate exploratory techniques (single bond and Pearson’s r correlation) was performed to show the relationships between the studied factors and the soil’s trace element content [68]. Subsequent to the collection of the test results, statistical analyses were performed for a significance level of p ≤ 0.01.

3. Results

3.1. Trace Elements in Soil

The pollution of soil with diesel oil has been demonstrated to induce substantial alterations in the composition of trace elements within the soil post-oat harvest (Figure 2 and Figure 3). In the initial series of experiments, in which no neutralising substances were employed, the presence of diesel oil pollution up to a dose of 10 cm3 per kilogramme of soil resulted in a 50% increase in cadmium, a 42% increase in nickel, a 41% decrease in iron and a 53% decrease in cobalt. In the case of the other trace elements, lower doses of diesel oil resulted in an increase in their content in the soil. Consequently, the lowest dose of this petroleum substance (2.5 cm3 per kg of soil) resulted in a 32% increase in the content of lead and 12% increase in that of chromium in the soil. In contrast, the average dose of diesel oil (5 cm3 per kg of soil) resulted in a 16% increase in copper, 19% increase in manganese and 25% increase in zinc in the soil. The increase in some trace elements in the soil under the influence of small doses of diesel oil is undoubtedly due to the fact that they can act as organic solvents. This allows them to partially decompose organic matter and release previously bound trace elements (e.g., Cr) into the soil solution, increasing their availability. Lower diesel oil rates increased trace element content as a result of lower soil pH, redox potential and reduced availability of organic ligands, which may have led to increased mobilisation of trace elements associated with less stable fractions [69]. The application of higher doses of diesel oil had a reducing effect on the content of these elements in the soil, especially chromium, whose concentration in the soil with the highest diesel oil dose was 21% lower than in the control site (without this petroleum substance).
Higher levels of diesel oil pollution inhibit the growth of soil microorganisms and consequently hinder the biogeochemical processes responsible for element mobilisation. They also restrict the availability of oxygen and water, which can lead to the immobilisation of some elements or their transformation into insoluble forms and adsorption of metals by oil particles, reducing their availability. Higher diesel oil doses increase soil acidification, which may favour the reduction of Cr(VI) to Cr(III). This is a less mobile cationic molecule due to its low solubility, high adsorption and complexation [69].
The application of all substances to the soil resulted in a limiting effect on nickel, chromium and iron. Furthermore, the application of compost and calcium oxide to the soil also resulted in a reducing effect on cobalt (Figure 2, Figure 3 and Figure 4). However, it is noteworthy that bentonite exhibited the most pronounced effect on nickel and chromium, while calcium oxide demonstrated the strongest impact on iron and cobalt, reducing their concentration in the soil by 42%, 53%, 12% and 31%, respectively. Conversely, the levels of cadmium, lead, copper and manganese exhibited an increase following the introduction of the materials into the soil. For cadmium and manganese, bentonite exhibited the most significant impact, while lead and copper demonstrated sensitivity to the effects of compost. It is evident that compost had an analogous effect on the zinc content of the soil. However, it should be noted that compost contributed to the reduction in cadmium, while bentonite contributed to the reduction in lead, zinc and manganese in the object with the highest diesel oil pollution (10 cm3 per kg of soil). Changes in the content of trace elements in the soil were probably associated with the beneficial effects of compost, bentonite and especially calcium oxide on other soil properties, in particular related to the neutralisation of its acidity [60].

3.2. Relations Between Variables

As illustrated in Figure 5, the interrelationships between the trace elements under scrutiny in the soil have been elucidated through PCA. PC1 and PC2 explained 43.55% and 23.97% of the variance, respectively. PCA 1 was dominated by chromium, cobalt, nickel and iron, while PCA 2 was primarily composed of cadmium and zinc. The arrangement of vector variables was found to allow for the conclusion that there was a positive correlation between copper content and manganese, albeit a weaker correlation with cadmium. Meanwhile, zinc content demonstrated a slightly weaker correlation with lead and iron. Furthermore, positive correlations were identified between nickel and cobalt and chromium, as well as between manganese and cadmium. The soil exhibited negative correlations between cadmium and nickel, and chromium and cobalt, and very weak correlations between cobalt and copper and manganese.
Cluster analysis using multivariate exploratory techniques (single bond and 1-r Pearson’s) confirms the effect of diesel oil pollution and the application of materials on trace element content in soil. As shown in Figure 6, the dendrogram indicates that diesel oil, being at the edge of the diagram, had a relatively low correlation with most heavy metals (based on results from all test series). The materials used had a more uniform effect on the content than diesel oil did, which was particularly significant for cadmium, chromium and copper. Zinc and lead, which are the most distant from each other in the dendrogram, were the least affected by both factors. The distribution of points in Figure 7 indicates that bentonite had a slightly greater impact on the content of the analysed trace elements in the soil than calcium oxide and organic matter in the form of compost.
The analysis of the percentage of observed variation confirmed the hypothesis that the type of used materials had a more significant effect than diesel oil pollution on the content of trace elements in the soil (Figure 8). The impact of these materials was dominant for the contents of cadmium (58.21%), manganese (60.13%), chromium (61.30%) and lead (74.40%). It was also significant for nickel (33.13%), copper (37.57%) and zinc (40.97%). The impact of soil pollution by diesel oil on the content of trace elements in the soil was found to be minimal, with its dominance being observed only for copper (47.38%) and cobalt (83.94%). However, it was found to be significant for nickel (28.63%) and chromium (32.57%). Furthermore, a significant proportion of the interaction between applied materials and diesel oil pollution was found to influence the content of trace elements in the soil. The highest concentrations were observed in nickel (37.79%), zinc (51.87%) and iron (75.90%).

4. Discussion

In our study, increasing doses of diesel oil were found to significantly increase the content of most of the analysed elements in the soil, such as Pb, Cu, Mn, Zn, Cd, Ni and Fe. However, the highest dose (10 cm3 per kg) was found to reduce chromium and cobalt content. An increase in the content of selected trace elements in soil following contamination by petroleum products was demonstrated by the studies of Nadal et al. [70] and Osawaru et al. [71]. Osawaru et al. [71] reported the greatest changes for Fe (568% increase), Mn (280% increase) and Cr (276% increase). Jamrah et al. [72] conducted a study to characterise the content of trace elements in the soil surrounding an oil field in Fahud, Oman. Soil analysis has revealed an elevated presence of zinc, copper, lead and vanadium, compared to uncontaminated soil. Soil contamination with petroleum products affects its physical and chemical properties, including lowering the pH level of the soil [71] and reducing the total amount of base-exchangeable cations, the soil’s base saturation and its cation exchange capacity [73]. These changes determine the mobility of trace elements and their ability to move through the soil profile [74]. As reported by Devatha et al. [75], soil contaminated with 10% petroleum had a lower pH (6.54 versus 6.95) and increased electrical conductivity than uncontaminated soil. This can lead to disruption of the environment’s ionic balance and a reduction in soil permeability. Trace element mobility increases as soil pH decreases [76]. At low pH, trace elements exist in more bioavailable free ionic forms, primarily due to reduced adsorption onto mineral or organic surfaces and reduced formation of poorly soluble phosphates and carbonates [77]. Petroleum derivatives also affect the oxidoreductive potential of the soil, leading to its reduction [78]. Under these conditions, the solubility of Fe-Mn hydroxides, to which TEs are bound, increases, resulting in the remobilisation of biologically available TEs [79,80]. Due to their chemical composition, petroleum pollutants contribute to the co-contamination of soil with TEs [81], which could explain the elevated levels of cadmium, nickel and iron observed in the samples containing the highest dosage of diesel oil in the present study.
Of the soil materials compared in this study, bentonite and calcium oxide were found to be the most effective at reducing the negative effects of diesel oil on soil. At the site with the highest level of petroleum contamination (10 cm3 per kg), the application of bentonite reduced the soil content of Pb, Zn and Mn. The favourable effect of bentonite in reducing the content of TEs under conditions of soil contamination by petroleum substances can be explained by its strong sorptive properties with respect to petroleum products (0.20–0.50 g of petroleum products per g of sorbent) [82]. Thanks to its significant sorptive surface area (both external and internal), bentonite plays a major role in soil chemical processes, affecting the mobility and availability of trace elements [83]. Additionally, the high content of silicon dioxide, magnesium oxide and calcium oxide reduces the acidity of the soil upon introduction of bentonite [84], which may also explain the limited accumulation of Ni, Cr and Fe in the series with the addition of this material in this study. Similar observations were made by Kumararaja et al. [85], who evaluated the suitability of bentonite as an immobilising agent in the remediation of trace element-contaminated soil. Following the application of 2.5% bentonite to the soil, reduced accumulation of zinc (by 15.8%), nickel (by 31.6%) and copper (by 18.6%) was recorded relative to the control sample (without bentonite addition). This reduction in the bioavailability of trace elements was related to the properties of the bentonite, specifically its strong sorption capacity and the large number of adsorption sites within the interlayer space, on the outer surface and on the edges. Introducing the sorbent into the soil also increased the pH (from 8.30 to 8.53), promoting the precipitation of TEs in the form of hydroxides. Gao and Li [83] confirmed the usefulness of bentonite in immobilising nickel and copper in mining-contaminated soils. They demonstrated that adding 10% bentonite reduced the exchangeable fraction of nickel by 56% compared to the control object (without the additive) and increased the fraction bound to organic matter and Fe and Mn oxides by 69% and 73%, respectively. In the case of copper, the exchangeable fraction was reduced by more than 2.7-fold compared to the control sample, while the fraction bound to organic matter increased by 68%, and the fraction bound to Fe-Mn oxides increased by 91%. According to the researchers, applying bentonite also reduced soil acidity (pH 7.9 versus 7.2). Under alkaline soil conditions, the adsorption of trace elements onto the surface of Fe-Mn oxides increases [49], as does the stability of the soil organic matter–metal complex [86]. At the same time, the concentration of iron, aluminium and magnesium ions decreases, facilitating the adsorption of the ions of trace elements on soil colloid surfaces [83].
The main mechanism of action of liming is an increase in soil pH, leading to the precipitation of trace elements in the form of less soluble and bioavailable hydroxides, carbonates and phosphates [87]. In our study, adding calcium oxide reduced the accumulation of Co, Fe, Ni and Cr in the soil. Hong et al. [88] conducted a comprehensive analysis of the effects of various calcium compounds on cadmium immobilisation in soils affected by gold mining activities. Of the alkaline materials tested (CaCO3, Ca(OH)2, CaSO4·2H2O and oyster shell meal), hydrated lime (Ca(OH)2) was found to be the most effective at increasing soil pH and the net negative charge, and at reducing the concentration of extractable Cd. Adding 8 Mg ha−1 reduced the bioavailability of cadmium by 54% relative to the control. An increase in the net negative charge, which is associated with the dissociation of H+ from the weakly acidic functional groups of organic matter and some clay minerals, increases the adsorption of TE cations onto soil colloids. Additionally, liming reduces Cd mobility by precipitating it as carbonates, phosphates, hydroxides and oxides at a high soil pH [89]. Lahori et al. [90] evaluated the effect of hydrated lime on the immobilisation and phytoavailability of trace elements in soils contaminated by zinc smelter operations. They demonstrated that adding 1% (w/w) of Ca(OH)2 reduced the mobility, toxicity and bioavailability of Pb (by 21.6–31.7%), Cd (by 22.2–57.6%), Cu (by 29.8–50.0%) and Zn (by 40.8–61.3%) compared to the control soil without the additive. Garau et al. [91] showed that liming with CaCO3 (0.4% w/w) significantly reduced the leachability of Cd, Pb and Zn from mining-contaminated soil. They confirmed that the immobilising effect of calcium compounds on soluble trace element content is mainly due to an increase in soil pH (from 4.23 to 7.14). This increase in pH promotes the precipitation of TEs in less accessible forms and increases their adsorption onto colloids of different charges, such as organic matter or iron oxides and aluminium oxides. Furthermore, the authors state that liming significantly increases microbial and enzymatic soil activity. The slightly different results of our study compared to those of the cited authors in terms of the effect of the liming process on the immobilisation of specific TEs may be due to differences in the form of the calcium compound, the granulometric composition of the soil and the nature of the contamination studied. The positive effects of in situ stabilisation of contaminated soils using calcium compounds were also confirmed by Zhou et al. [92] and Zeng et al. [93].
As a source of dissolved organic carbon, compost increases the organic matter content of the soil, thereby improving its sorption capacity [94] and increasing the retention of TEs [95]. In our own research, applying compost reduced the accumulation of Cd, Co, Ni, Cr and Fe in the soil. Similar results were obtained by Medyńska-Juraszek et al. [96], who noted a reduction in the mobility and bioavailability of Cd, Pb, and Ni when 10% green waste compost was added to industrial soil from a copper smelter site. The researchers observed an increase in the proportion of TE fractions associated with organic matter, compared to their exchangeable forms. Humus substances, which constitute a significant proportion of the organic matter in compost, can reduce the solubility of TEs by forming stable complexes with them [97]. Additionally, the surface of the compost is rich in functional groups such as carboxyl and phenolic groups, which provide sites for adsorption and electrostatic interactions with TE cations [98]. Liu et al. [99] conducted a study assessing the effect of poultry manure and rice husk compost applications on the immobilisation and biotoxicity of Cd in contaminated soils. In the most contaminated series (50 mg Cd per kg), adding compost at a rate of 120 g per kg reduced the amount of soluble/exchangeable Cd by 95.7%. Under the same conditions, the authors also observed significant increases in the fraction of Cd bound to organic matter (7.8-fold) and inorganic sludge (1.5-fold). Introducing compost into soil increases its pH, promoting the precipitation of trace element hydroxides and carbonates [100], and stimulating soil microbial activity. This can result in the transformation of TEs into geochemically more stable forms [101]. Farrell et al. [102] and Tang et al. [103] also demonstrated the effectiveness of compost in reducing the availability of TEs in contaminated soils. Further advantages of using compost for soil remediation include increased soil fertility and biological activity in the soil, long-term protection and a sustainable, closed-loop approach [104].
The immobilisation efficiency of soil additives depends on soil properties, including initial pH and cation exchange capacity (CEC). Soils with a high CEC have a higher retention capacity for trace element cations [105] and better stabilisation of introduced sorbents [106]. Soil pH determines the surface loading of soil colloids and sorbents [107]. In an alkaline environment (pH > 7), negatively charged surfaces predominate, increasing the soil’s retention capacity for cationic compounds [108] and leading to increased adsorption of trace elements onto soil colloids. Soil pH controls the solubility of trace element combinations and affects the availability of organic ligands [109]. At a pH level that is neutral to slightly alkaline, the carboxylic and phenolic groups in humic substances become deprotonated and negatively charged. This allows for the efficient formation of complexes with trace element cations through electrostatic forces [110]. Although complexation with organic matter provides long-term immobilisation efficiency of TEs over a wider pH range, it is sensitive to changes in redox potential [40]. Elements immobilised by precipitation are most stable under alkaline conditions but can be remobilised when the pH decreases [111].
Compared to biological alternatives (e.g., bioremediation and phytoremediation), the in situ stabilisation method for contaminated soils produces faster results, enabling earlier site development [37]. It is also characterised by its independence from climatic and seasonal conditions, its applicability to a wide range of soil types and contaminants, predictable results, and an absence of secondary waste generation [112]. Phytoremediation, on the other hand, is a process that takes a very long time (even decades) to achieve satisfactory results, and is limited to the depth to which the applied plants’ root systems penetrate [113]. The effectiveness of phytoremediation depends on climatic conditions, the type of plants and the concentration of contaminants [114]. At too high a concentration, phytotoxic effects may limit the application of this remediation method [37]. Additionally, the management of contaminated biomass can pose a risk of contaminating trophic networks [113]. Bioremediation allows environmental toxins to be neutralised through the metabolic activity of microorganisms and their enzymes. However, it too has its limitations [115]. The main issues include sensitivity to weather and climatic conditions, a slow degradation rate (of several years) [116], a risk of secondary contamination, limited suitability for certain pollutants and highly contaminated soils [37] and a high cost. The process also requires continuous monitoring of biotic parameters, pH values, temperature, moisture and nutrient availability in order to maintain consistent performance [16]. Therefore, the in situ stabilisation method proposed in this study, which uses bentonite, calcium oxide and compost, represents an optimal compromise between the efficiency, implementation time and costs associated with the remediation of contaminated soils.
In situ stabilisation is an effective, economical and sustainable method of remediating soils contaminated with petroleum derivatives, particularly in areas where other methods would be difficult or impractical to implement. This study therefore expands our knowledge of the suitability and effectiveness of using bentonite, calcium oxide and compost to treat oil-contaminated soils. The controlled conditions of the experiment ensure that the resulting data can be used to inform the design of full-scale remediation interventions under real environmental conditions.

5. Conclusions

In order to determine the potential of organic and mineral materials in mitigating the effects of diesel oil pollution on the trace element content of soil, a test was conducted using three different remediation additives. Specifically, the test materials used were compost, which is a source of organic matter with high sorption capacity; bentonite, which is a clay mineral with immobilising properties; and calcium oxide, which is an alkaline additive capable of stabilising soil pH and precipitating trace elements in less accessible forms.
The content of trace elements in the soil was clearly correlated with the diesel oil pollution and the materials used to mitigate its impact. Diesel oil pollution had the greatest effect on cadmium, nickel, iron and cobalt levels. The contents of the first three elements increased by 50% (Cd), 42% (Ni) and 41% (Fe), while the concentration of the last element decreased by 53% (Co). Lower doses of diesel oil (2.5 and 5 cm3 per kg of soil) increased the content of the other trace elements in the soil, particularly chromium, whereas higher doses decreased it. All the materials applied to the soil (compost, bentonite and calcium oxide) clearly reduced the content of nickel, chromium and iron. Additionally, the application of compost and calcium oxide reduced the accumulation of cobalt in the soil. Bentonite had the strongest reducing effect on the nickel and chromium content of the soil, while calcium oxide had the strongest reducing effect on iron and cobalt accumulation. Inverse relationships were noted for cadmium (mainly bentonite), lead (especially compost), copper (mainly compost), manganese (mainly bentonite) and zinc (only compost) content. Bentonite limited the accumulation of lead, zinc and manganese in the most contaminated object, while compost had the same effect on cadmium.
Using various materials, particularly bentonite and compost, limits the content of certain trace elements in the soil. This positively impacts the effect of minor diesel oil pollution on soil properties and can result in improved plant biomass growth.
Future research will assess the influence of different soil types (with varying organic matter content, pH and mineralogical composition) on observed trace element mobility phenomena. It will also be crucial to carry out experiments under field conditions to confirm the relationships obtained in a natural soil environment.

Author Contributions

Conceptualisation, M.W.; methodology, M.W.; validation, M.W.; formal analysis, M.W. and N.K.; investigation, N.K.; resources, M.W.; data curation, M.W.; writing—original draft preparation, M.W. and N.K.; writing—review and editing, M.W. and N.K.; visualisation, M.W. and N.K.; supervision, M.W.; project administration, M.W.; funding acquisition, M.W. All authors have read and agreed to the published version of the manuscript.

Funding

The research was financed by the Department of Agricultural and Environmental Chemistry, Faculty of Agriculture and Forestry, University of Warmia and Mazury in Olsztyn (grant No. 30.610.004-110).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The data are contained within the article.

Conflicts of Interest

The authors declare no conflicts of interest. The funders had no role in the design of the study; in the collection, analyses, or interpretation of data; in the writing of the manuscript, or in the decision to publish the results.

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Figure 1. Soil analysis methods.
Figure 1. Soil analysis methods.
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Figure 2. Influence of different materials on the Cd, Pb, Cr, Ni, Zn and Cu content of soil contaminated with diesel oil, in mg per kg (averages ± standard deviations).
Figure 2. Influence of different materials on the Cd, Pb, Cr, Ni, Zn and Cu content of soil contaminated with diesel oil, in mg per kg (averages ± standard deviations).
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Figure 3. Influence of different materials on the Mn, Fe and Co content of soil contaminated with diesel oil, in mg per kg (averages ± standard deviations).
Figure 3. Influence of different materials on the Mn, Fe and Co content of soil contaminated with diesel oil, in mg per kg (averages ± standard deviations).
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Figure 4. Influence of different materials on trace element content in soil, in mg per kg (averages for all objects in series).
Figure 4. Influence of different materials on trace element content in soil, in mg per kg (averages for all objects in series).
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Figure 5. Relations between trace element contents in soil calculated with PCA method.
Figure 5. Relations between trace element contents in soil calculated with PCA method.
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Figure 6. Influence of diesel oil and different materials on trace element content in soil, presented as a tree diagram.
Figure 6. Influence of diesel oil and different materials on trace element content in soil, presented as a tree diagram.
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Figure 7. Relative influence of diesel oil and different materials on trace element content in soil calculated with PCA method.
Figure 7. Relative influence of diesel oil and different materials on trace element content in soil calculated with PCA method.
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Figure 8. Relative effect of factors on trace elements in soil (in percent).
Figure 8. Relative effect of factors on trace elements in soil (in percent).
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Table 1. Properties of soil.
Table 1. Properties of soil.
PropertiesSoil
Granulometric compositionsandy loam
Sand (1.0–0.1 mm) in %53
Clay (0.1–0.02 mm) in %8
Silt (1.0–0.1 mm) in %39
pHKCl5.10
Hydrolytic acidity (HAC) in mM per kg30.8
Total exchangeable bases (TEB) in mM per kg 88.0
Cation exchange capacity (CEC) in mM per kg 118.8
Base saturation (BS) in %74.1
Total organic carbon (TOC) in g per kg8.54
Available phosphorus in mg per kg34.35
Available potassium in mg per kg75.26
Available magnesium in mg per kg41.22
Total cadmium0.194
Total lead16.41
Total chromium12.72
Total nickel14.53
Total zinc21.07
Total copper2.95
Total manganese220.0
Total iron6897
Total cobalt3.05
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Wyszkowski, M.; Kordala, N. Geochemical Behaviour of Trace Elements in Diesel Oil-Contaminated Soil During Remediation Assisted by Mineral and Organic Sorbents. Appl. Sci. 2025, 15, 8650. https://doi.org/10.3390/app15158650

AMA Style

Wyszkowski M, Kordala N. Geochemical Behaviour of Trace Elements in Diesel Oil-Contaminated Soil During Remediation Assisted by Mineral and Organic Sorbents. Applied Sciences. 2025; 15(15):8650. https://doi.org/10.3390/app15158650

Chicago/Turabian Style

Wyszkowski, Mirosław, and Natalia Kordala. 2025. "Geochemical Behaviour of Trace Elements in Diesel Oil-Contaminated Soil During Remediation Assisted by Mineral and Organic Sorbents" Applied Sciences 15, no. 15: 8650. https://doi.org/10.3390/app15158650

APA Style

Wyszkowski, M., & Kordala, N. (2025). Geochemical Behaviour of Trace Elements in Diesel Oil-Contaminated Soil During Remediation Assisted by Mineral and Organic Sorbents. Applied Sciences, 15(15), 8650. https://doi.org/10.3390/app15158650

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