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Industrial and agricultural activities heavily constrain soil quality. Potentially Toxic Elements (PTEs) are a threat to public health and the environment alike. In this regard, the identification of areas that require remediation is crucial. In the herein research a geochemical dataset (230 samples) comprising 14 elements (Cu, Pb, Zn, Ag, Ni, Mn, Fe, As, Cd, V, Cr, Ti, Al and S) was gathered throughout eight different zones distinguished by their main activity, namely, recreational, agriculture/livestock and heavy industry in the Avilés Estuary (North of Spain). Then a stratified systematic sampling method was used at short, medium, and long distances from each zone to obtain a representative picture of the total variability of the selected attributes. The information was then combined in four risk classes (Low, Moderate, High, Remediation) following reference values from several sediment quality guidelines (SQGs). A Bayesian analysis, inferred for each zone, allowed the characterization of PTEs correlations, the unsupervised learning network technique proving to be the best fit. Based on the Bayesian network structure obtained, Pb, As and Mn were selected as key contamination parameters. For these 3 elements, the conditional probability obtained was allocated to each observed point, and a simple, direct index (Bayesian Risk Index-BRI) was constructed as a linear rating of the pre-defined risk classes weighted by the previously obtained probability. Finally, the BRI underwent geostatistical modeling. One hundred Sequential Gaussian Simulations (SGS) were computed. The Mean Image and the Standard Deviation maps were obtained, allowing the definition of High/Low risk clusters (Local G clustering) and the computation of spatial uncertainty. High-risk clusters are mainly distributed within the area with the highest altitude (agriculture/livestock) showing an associated low spatial uncertainty, clearly indicating the need for remediation. Atmospheric emissions, mainly derived from the metallurgical industry, contribute to soil contamination by PTEs.

When considering complex scenarios involving several attributes, such as in environmental characterization, a clearer picture of reality can be achieved through the dimensional reduction of data. In this context, maps facilitate the visualization of spatial patterns of contaminant distribution and the identification of enriched areas. A set, of 15 Potentially Toxic Elements (PTEs) – (As, Ba, Cd, Co, Cr, Cu, Hg,Mo, Ni, Pb, Sb, Se, Tl, V, and Zn), was measured in soil, collected in Langreo's municipality (80 km2), Spain. Relative enrichment (RE) is introduced here to refer to the proportion of elements present in a given context. Indeed, a novel approach is provided for research into PTE fate. This method involves studying the variability of PTE proportions throughout the study area, thereby allowing the identification of dissemination trends. Traditional geostatistical approaches commonly use raw data (concentrations) accepting that the elements analyzedmake up the entirety of the soil. However, in geochemical studies the analyzed elements are just a fraction of the total soil composition. Therefore, considering compositional data is pivotal. The spatial characterization of PTEs considering raw and compositional data together allowed a broad discussion about, not only the PTEs concentration's distribution but also to reckon possible trends of relative enrichment (RE). Transformations to open closed data are widely used for this purpose. Spatial patterns have an indubitable interest. In this study, the Centered Log-ratio transformation (clr) was used, followed by its back-transformation, to build a set of compositional data that, combined with raw data, allowed to establish the sources of the PTEs and trends of spatial dissemination.

The impact of mining activities on the environment is vast. In this regard, many mines were operating well before the introduction of environmental law. This is particularly true of cinnabar mines, whose activity has declined for decades due to growing public concern regarding Hg high toxicity. Here we present the exemplary case study of an abandoned Hg mine located in the Somiedo Natural Reserve (Spain). Until its closure in the 1970s, this mine operated under no environmental regulations, its tailings dumped in two spoil heaps, one of them located uphill and the other in the surroundings of the village of Caunedo. This study attempts to outline the degree to which soil and other environmental compartments have been affected by the two heaps. To this end, we used a novel combination of multivariate statistical, geostatistical and machine-learning The techniques used included principal component and clustering analysis, Bayesian networks, indicator kriging, and sequential Gaussian simulations. Our results revealed high concentrations of Hg and, secondarily, As in soil but not in water or sediments. The innovative methodology abovementioned allowed us to identify natural and anthropogenic associations between 25 elements and to conclude that soil pollution was attributable mainly to natural weathering of the uphill heap. Moreover, the probability of surpassing the threshold limits and the local backgrounds was found to 31 be high in a large extension of the area. The methodology used herein demonstrated to be effective for addressing complex pollution scenarios and therefore they are applicable to similar cases.

The impact of mining activities on the environment is vast. In this regard, many mines were operating well before the introduction of environmental law. This is particularly true of cinnabar mines, whose activity has declined for decades due to growing public concern regarding Hg high toxicity. Here we present the exemplary case study of an abandoned Hg mine located in the Somiedo Natural Reserve (Spain). Until its closure in the 1970s, this mine operated under no environmental regulations, its tailings dumped in two spoil heaps, one of them located uphill and the other in the surroundings of the village of Caunedo. This study attempts to outline the degree to which soil and other environmental compartments have been affected by the two heaps. To this end, we used a novel combination of multivariate statistical, geostatistical and machine-learning methodologies. The techniques used included principal component and clustering analysis, Bayesian networks, indicator kriging, and sequential Gaussian simulations. Our results revealed high concentrations of Hg and, secondarily, As in soil but not in water or sediments. The innovative methodology abovementioned allowed us to identify natural and anthropogenic associations between 25 elements and to conclude that soil pollution was attributable mainly to natural weathering of the uphill heap. Moreover, the probability of surpassing the threshold limits and the local backgrounds was found to be high in a large extension of the area. The methodology used herein demonstrated to be effective for addressing complex pollution scenarios and therefore they are applicable to similar cases.

Potentially Toxic Elements (PTEs) are contaminants with high toxicity and complex geochemical behaviour and, therefore, high PTEs contents in soil may affect ecosystems and/or human health. However, before addressing the measurement of soil pollution, it is necessary to understand what is meant by pollution-free soil. Often, this background, or pollution baseline, is undefined or only partially known. Since the concentration of chemical elements is compositional, as the attributes vary together, here we present a novel approach to build compositional indicators based on Compositional Data (CoDa) principles. The steps of this new methodology are: 1) Exploratory data analysis through variation matrix, biplots or CoDa dendrograms; 2) Selection of geological background in terms of a trimmed subsample that can be assumed as non-pollutant; 3) Computing the spread Aitchison distance from each sample point to the trimmed sample; 4) Performing a compositional balance able to predict the Aitchison distance computed in step 3. Identifying a compositional balance, including pollutant and non-pollutant elements, with sparsity and simplicity as properties, is crucial for the construction of a Compositional Pollution Indicator (CI). Here we explored a database of 150 soil samples and 37 chemical elements from the contaminated region of Langreo, Northwestern Spain. There were obtained three Cis: the first two using elements obtained through CoDa analysis, and the third one selecting a list of pollutants and non-pollutants based on expert knowledge and previous studies. The three indicators went through a Stochastic Sequential Gaussian simulation. The results of the 100 computed simulations are summarized through mean image maps and probability maps of exceeding a given threshold, thus allowing characterization of the spatial distribution and variability of the CIs. A better understanding of the trends of relative enrichment and PTEs fate is discussed.