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Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II

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A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Analytical Chemistry".

Deadline for manuscript submissions: closed (31 October 2023) | Viewed by 15969

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Prof. Dr. Giuseppe Scarponi

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Department of Life and Environmental Sciences, Università Politecnica delle Marche, Via Brecce Bianche, 60131 Ancona, Italy
Interests: analytical chemistry; electroanalytical chemistry; polarography and voltammetry; inductively coupled plasma–mass spectrometry; unmanned aerial vehicles for atmospheric analysis; chemometrics; environmental analytical chemistry; trace heavy metals; atmospheric aerosol; seawater; snow; ice
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Prof. Dr. Cristina Truzzi

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Department of Life and Environmental Sciences, Università Politecnica delle Marche, Via Brecce Bianche, 60131 Ancona, Italy
Interests: analytical chemistry; gas chromatography–mass spectrometry; high-performance liquid chromatography; atomic absorption spectroscopy; environmental analytical chemistry; food chemistry; heavy metals in marine organisms and insects; trace heavy metals in natural waters; chemical composition of food; multivariate statistical analysis applied to environmental and food data

Prof. Dr. Anna Annibaldi

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Department of Life and Environmental Sciences, Università Politecnica delle Marche, Via Brecce Bianche, 60131 Ancona, Italy
Interests: analytical chemistry, voltammetry for environmental analysis; atomic absorption spectroscopy; gas chromatography–mass spectrometry; inductively coupled plasma – mass spectrometry; environmental monitoring; heavy metals and organic contaminants in marine organisms; trace elements in seawater and marine sediments; heavy metals in insects; mineral water; river water
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Prof. Dr. Silvia Illuminati

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Department of Life and Environmental Sciences, Università Politecnica delle Marche, Via Brecce Bianche, 60131 Ancona, Italy
Interests: analytical and environmental chemistry; voltammetry and in-situ voltammetry; atomic absorption spectroscopy; inductively coupled plasma–mass spectrometry; unmanned aerial vehicles for atmospheric analysis; atmospheric depositions; chemical composition of atmospheric aerosol; metal speciation in seawater; environmental chemometrics
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Following the great success of the first Special Issue of the international journal Molecules dedicated to the topic “Determination of Trace Heavy Metals and Metalloids in Environmental Samples”, which hosted 18 high-quality articles from colleagues all around the world (URL https://www.mdpi.com/si/molecules/determination_metals_environmental), in cooperation with the editors of the journal, we have decided to edit a second Special Issue on the same topic, expanding the collection’s focus to include the subject of analytical chemistry of food.

This Special Issue has the broad scope to provide an overview of the current trends in analytical methods to determine heavy metal(loid)s in environmental matrices and food. Contributions, in the form of original research or review articles, are expected to include fundamental studies on the set-up of specific analytical methods, as well as real-case multidisciplinary investigations. Applications can extend to extreme environments (such as Polar Regions, high-altitude lands, deserts, stratosphere, ocean depths and floors), inaccessible sites (using unmanned vehicles), all kinds of biota, food and beverages, etc. In addition to “heavy” metal(loid)s, we expect that authors will also consider other major and minor constituents and limited organic compounds, so to provide a full characterization of matrices, when appropriate, and thorough studies. Multivariate statistical analyses applied to the reported applications are also welcome.

We believe that this Special Issue will present challenging scientific approaches and propose recent and emerging issues, as well as visions for the future. It will discuss, though not exclusively, new analytical methods and instrumental techniques, new sample treatments and instrumental set-ups, novel analytical applications in both abiotic and biotic matrices, case studies on environmental monitoring and on novels foods (such as insects) for the determination of trace heavy metal(loid)s.

Prof. Dr. Giuseppe Scarponi
Prof. Dr. Cristina Truzzi
Prof. Dr. Anna Annibaldi
Prof. Dr. Silvia Illuminati
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Molecules is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 2700 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

environmental analytical chemistry
trace heavy metals and metalloids
chemical speciation
instrumental analysis
new analytical methods and techniques
sample pre-treatment
extreme environments
case studies of environmental monitoring
reviews
emerging environmental issues
food and “novel foods”
insects

Related Special Issue

Determination of Trace Heavy Metals and Metalloids in Environmental Samples in Molecules (19 articles)

Published Papers (9 papers)

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Research

11 pages, 1428 KiB

Open AccessArticle

Advancements in Portable Voltammetry: A Promising Approach for Iron Speciation Analysis

by Paolo Inaudi, Ornella Abollino, Monica Argenziano, Mery Malandrino, Caterina Guiot, Stefano Bertinetti, Laura Favilli and Agnese Giacomino

Molecules 2023, 28(21), 7404; https://doi.org/10.3390/molecules28217404 - 03 Nov 2023

Viewed by 697

Abstract

Iron, a crucial element in our environment, plays a vital role in numerous natural processes. Understanding the presence and concentration of iron in the environment is very important as it impacts various aspects of our planet’s health. The on-site detection and speciation of iron are significant for several reasons. In this context, the present work aims to evaluate the applicability of voltammetry for the on-site determination of iron and its possible speciation using a portable voltammetric analyzer. Voltammetry offers the advantage of convenience and cost-effectiveness. For iron (III) determination, the modification of a glassy carbon electrode (GCE) with an antimony-bismuth film (SbBiFE) using the acetate buffer (pH = 4) as a supporting electrolyte was used. The technique adopted was Square Wave Adsoptive Cathodic Stripping Voltammetry (SW-AdCSV), and we used 1-(2-piridylazo)-2-naphthol (PAN) as the iron (III) ligand. Linearity, repeatability, detection limit, and accuracy were determined using synthetic solutions; then, a Standard Reference Material (SRM) of 1643f Trace Elements in Water (iron content: 93.44 ± 0.78 µg L⁻¹) was used for validation measurements in the real matrix. the accuracy of this technique was found to be excellent since we obtained a recovery of 103.16%. The procedure was finally applied to real samples (tap, lake, and seawater), and the results obtained were compared via Inductively Coupled Plasma-Optical Emission Spectroscopy (ICP-OES). The amount of iron found was 207.8 ± 6.6 µg L⁻¹ for tap water using voltammetry and 200.9 ± 1.5 µg L⁻¹ with ICP-OES. For lake water, 171.7 ± 3.8 µg L⁻¹, 169.8 ± 4.1 µg L⁻¹, and 187.5 ± 5.7 µg L⁻¹ were found using voltammetry in the lab both on-site and using ICP-OES, respectively. The results obtained demonstrate the excellent applicability of the proposed on-site voltammetric procedure for the determination of iron and its speciation in water. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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14 pages, 2440 KiB

Open AccessArticle

On-Chip Antifouling Gel-Integrated Microelectrode Arrays for In Situ High-Resolution Quantification of the Nickel Fraction Available for Bio-Uptake in Natural Waters

by Sébastien Creffield, Mary-Lou Tercier-Waeber, Tanguy Gressard, Eric Bakker and Nicolas Layglon

Molecules 2023, 28(3), 1346; https://doi.org/10.3390/molecules28031346 - 31 Jan 2023

Cited by 1 | Viewed by 1366

Abstract

We aimed to monitor in situ nickel (Ni(II)) concentrations in aquatic systems in the nanomolar range. To achieve this, we investigated whether an analytical protocol for the direct quantification of cobalt (Co(II)) using adsorptive cathodic sweep voltammetry (Ad-CSV) on antifouling gel-integrated microelectrode arrays (GIME) we recently developed is also suitable for direct Ni(II) quantification. The proposed protocol consists of the reduction of the complex formed between Ni(II) (or Ni(II) and Co(II)) and nioxime adsorbed on the surface of the GIME-sensing element. The GIME enables to (i) avoid fouling, (ii) control the metal complex mass transport and, when interrogated by Ad-CSV, (iii) selectively determine the dynamic (kinetically labile Ni-nioxime) fraction that is potentially bioavailable. The nioxime concentration and pH were optimized. A temperature correction factor was determined. The limit of detection established for 90 s of accumulation time was 0.43 ± 0.06 in freshwater and 0.34 ± 0.02 nM in seawater. The sensor was integrated in a submersible probe in which the nioxime-containing buffer and the sample were mixed automatically. In situ field measurements at high resolution were successfully achieved in Lake Geneva during a diurnal cycle. The determination of the kinetically labile Ni-nioxime fraction allows one to estimate the potential ecotoxicological impact of Ni(II) in Lake Geneva. Additional Ni fractions were measured by ICP-MS and coupled to the in situ Ad-CSV data to determine the temporal Ni(II) speciation. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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12 pages, 8443 KiB

Open AccessArticle

Multielement Determination in Turmeric (Curcuma longa L.) Using Different Digestion Methods

by Michaela Zeiner, Monika Šoltić, Ivan Nemet and Iva Juranović Cindrić

Molecules 2022, 27(23), 8392; https://doi.org/10.3390/molecules27238392 - 01 Dec 2022

Cited by 5 | Viewed by 1690

Abstract

The antioxidant, anti-inflammatory and antiseptic properties of turmeric (Curcuma longa L.) derive from its rich nutritional composition making it interesting for medicinal uses, besides being used as spice in cooking. To complete the picture on the composition of turmeric, not only the organic compounds need to be known, but also the elemental composition covering essential and potentially toxic elements. The samples were digested in a microwave assisted digestion system using different reagent mixtures. The best digestion mixture was semi-concentrated nitric acid combined with hydrogen peroxide. After optimization of the sample preparation method, the contents of Ag, Al, As, Ba, Be, Bi, Ca, Cd, Co, Cr, Cu, Fe, Ga, K, Li, Mg, Mn, Mo, Na, Ni, Pb, Rb, Se, Sr, Te, Tl, V and Zn in curcuma were determined by inductively coupled plasma atomic emission spectrometry (ICP-AES), as well as by inductively coupled plasma mass spectrometry (ICP-MS). Even if the general composition found is in line with the scarce data in literature, clear differences can be seen between the analyzed samples, considering provenience, production procedures, and harvesting year as potential influencing factors. Whereas all samples contained less As and Pb than regulated by WHO, one limit exceeding was found for Cd. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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12 pages, 750 KiB

Open AccessCommunication

Heavy Metal Depuration Steps for Gracilaria chilensis in Outdoor Culture Systems

by Jorge Rivas, Florentina Piña, Matías Araya, Nicolás Latorre-Padilla, Benjamín Pinilla-Rojas, Sofía Caroca, Francisca C. Bronfman and Loretto Contreras-Porcia

Molecules 2022, 27(20), 6832; https://doi.org/10.3390/molecules27206832 - 12 Oct 2022

Cited by 1 | Viewed by 1761

Abstract

Seaweed aquaculture is affected by natural and anthropogenic stressors, which put the biomass productivity of the cultures at risk. Seaweed biomass for commercial purposes, principally in pharmaceutical and/or nutraceutical applications, needs to be free of pollutants; therefore, controlled cultures have relevance in regulating the quality of biomass. The aim of this work was to demonstrate the successful utilization of controlled outdoor cultures to remove excess heavy metal accumulation in Gracilaria chilensis, an important commercial seaweed farming model. Specifically, we designed a simple and operational heavy metal depuration protocol, utilizing seawater and tap water removal, which permitted the concentration reduction of 10 heavy metals, including As, Cu, and Cd but not Zn, from the biomass at 7 days of culture. The percentage of depuration of the heavy metals ranged from 32 to 92% at 7 days, which was maintained throughout 21 days of culture. During the culture period, the monitored physicochemical parameters (temperature, salinity, and dissolved oxygen, among others) remained stable, with an increase in the daily growth rate (DGR% d⁻¹) of the biomass recorded after 14 days of culture. Consequently, the experimental setup was successful for heavy metal depuration, which highlights the importance of controlled outdoor cultures as important tools of sustainability. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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17 pages, 2335 KiB

Open AccessArticle

Lead Isotopic Constraints on the Provenance of Antarctic Dust and Atmospheric Circulation Patterns Prior to the Mid-Brunhes Event (~430 kyr ago)

by Changhee Han, Laurie J. Burn, Paul Vallelonga, Soon Do Hur, Claude F. Boutron, Yeongcheol Han, Sanghee Lee, Ahhyung Lee and Sungmin Hong

Molecules 2022, 27(13), 4208; https://doi.org/10.3390/molecules27134208 - 30 Jun 2022

Cited by 1 | Viewed by 1411

Abstract

A lead (Pb) isotopic record, covering the two oldest glacial–interglacial cycles (~572 to 801 kyr ago) characterized by lukewarm interglacials in the European Project for Ice Coring in Antarctica Dome C ice core, provides evidence for dust provenance in central East Antarctic ice prior to the Mid-Brunhes Event (MBE), ~430 kyr ago. Combined with published post-MBE data, distinct isotopic compositions, coupled with isotope mixing model results, suggest Patagonia/Tierra del Fuego (TdF) as the most important sources of dust during both pre-MBE and post-MBE cold and intermediate glacial periods. During interglacials, central-western Argentina emerges as a major contributor, resulting from reduced dust supply from Patagonia/TdF after the MBE, contrasting to the persistent dominance of dust from Patagonia/TdF before the MBE. The data also show a small fraction of volcanic Pb transferred from extra-Antarctic volcanoes during post-MBE interglacials, as opposed to abundant transfer prior to the MBE. These differences are most likely attributed to the enhanced wet removal efficiency with the hydrological cycle intensified over the Southern Ocean, associated with a poleward shift of the southern westerly winds (SWW) during warmer post-MBE interglacials, and vice versa during cooler pre-MBE ones. Our results highlight sensitive responses of the SWW and the associated atmospheric conditions to stepwise Antarctic warming. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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11 pages, 1750 KiB

Open AccessArticle

On-Site Determination of Methylmercury by Coupling Solid-Phase Extraction and Voltammetry

by Paolo Inaudi, Elio Mondino, Ornella Abollino, Mery Malandrino, Monica Argenziano, Laura Favilli, Roberto Boschini and Agnese Giacomino

Molecules 2022, 27(10), 3178; https://doi.org/10.3390/molecules27103178 - 16 May 2022

Cited by 2 | Viewed by 1561

Abstract

A measurement and speciation procedure for the determination of total mercury (Hg_TOT), inorganic mercury (Hg_IN), and methylmercury (CH₃Hg) was developed and the applicability for on-site determination was demonstrated. A simple, portable sample pretreatment procedure was optimized to extract the analytes. Home-made columns, packed with a new sorbent material called CYXAD (CYPHOS 101 modified Amberlite XAD), were used to separate the two forms of the analyte. Hg_TOT and CH₃Hg were determined by anodic stripping voltammetry (ASV), using a solid gold electrode (SGE). Two certified reference materials (BCR-463 Tuna Fish and Tuna Fish ERM-CE 464) and eight fresh fishes were analyzed. Then, the results that were obtained following the optimized portable procedure were compared with the concentrations obtained, using a direct mercury analyzer (DMA). This quantification, using the two techniques, demonstrated the good performance of the proposed method. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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12 pages, 2426 KiB

Open AccessArticle

Influence of Soil Salinity on Selected Element Contents in Different Brassica Species

by Michaela Zeiner, Iva Juranović Cindrić, Ivan Nemet, Karla Franjković and Branka Salopek Sondi

Molecules 2022, 27(6), 1878; https://doi.org/10.3390/molecules27061878 - 14 Mar 2022

Cited by 8 | Viewed by 1907

Abstract

Climate changes in coastal regions cause increased soil salinity, a well-known type of environmental stress for a high number of agricultural crop species, including Brassicaceae, whose growth and development, and consequently the crop quality and yield, are affected by salinity stress. The aim of the present study is to investigate the effect of salt stress on micro- and macro-element homeostasis in different Brassica crops. Kale (Brassica oleracea var. acephala), white cabbage (B. oleracea var. capitata) and Chinese cabbage (B. rapa ssp. pekinensis) were grown hydroponically and treated with 200 mmol/L sodium chloride for 24 h to mimic short-term salt stress. The contents of Al, Ca, K, Mg, Na, B, Ba, Cd, Co, Cr, Cu, Fe, Mn, Ni, Pb, Sr, V and Zn were determined in the roots and leaves of the salt-treated plants and corresponding controls by inductively coupled plasma atomic emission spectrometry and inductively coupled plasma mass spectrometry. While Al, Ca, K, Mg and Na were determined in the mg/g range, the contents of the other elements were found at the µg/g level. A statistical analysis of the obtained data showed that the applied salt treatment significantly influenced the single-element contents in different plant parts. The major elements Ca, K and Mg were mainly unaffected in the more-salt-tolerant kale and white cabbage under salinity stress, while K and Mg were significantly decreased in the more-sensitive Chinese cabbage. The levels of micro-elements were found to be species/variety specific. In general, potentially toxic elements were accumulated in the roots of salt-treated plants to a higher extent than in the corresponding controls. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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13 pages, 3056 KiB

Open AccessArticle

The Design of Experiment as a Tool to Model Plant Trace-Metal Bioindication Abilities

by Mirko Salinitro, Alessandro Zappi, Sonia Casolari, Marcello Locatelli, Annalisa Tassoni and Dora Melucci

Molecules 2022, 27(6), 1844; https://doi.org/10.3390/molecules27061844 - 11 Mar 2022

Cited by 1 | Viewed by 1653

Abstract

Bioindicator plants are species that have the capacity to linearly uptake some elements (metal and metalloids) from the growing substrate, thus reflecting their concentration in the soil. Many factors can influence the uptake of these elements by plants, among which is the simultaneous presence of several metals, a common situation in contaminated or natural soils. A novel approach that can be used to validate the bioindication ability of a species growing on a polymetallic substrate is the design of experiment (DoE) approach. The aim of the present study was to apply the DoE in full factorial mode to model the Cu, Cd, Pb, Zn, and Cr bioindication capacity of Polygonum aviculare, used as the model plant. The results showed that P. aviculare has the ability to bioindicate Cd and Cr with a linear uptake (from 0.35 to 6.66, and 0.1 to 3.4 mg kg⁻¹, respectively) unaffected by the presence of other metals. Conversely, the uptake of Pb, Cu, and Zn is strongly influenced by the presence of all the studied metals, making their concentration in the plant shoot not proportional to that of the soil. In conclusion, these preliminary results confirmed that the DoE can be used to predict the bioindicator abilities of a plant for several elements at the same time and to evaluate the interactions that can be established between variables in the growing medium and in the plant itself. However, more studies including other plant species are needed to confirm the effectiveness of this method. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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21 pages, 1976 KiB

Open AccessArticle

New Eco-Sustainable Feed in Aquaculture: Influence of Insect-Based Diets on the Content of Potentially Toxic Elements in the Experimental Model Zebrafish (Danio rerio)

by Cristina Truzzi, Federico Girolametti, Leonardo Giovannini, Ike Olivotto, Matteo Zarantoniello, Giuseppe Scarponi, Anna Annibaldi and Silvia Illuminati

Molecules 2022, 27(3), 818; https://doi.org/10.3390/molecules27030818 - 26 Jan 2022

Cited by 3 | Viewed by 2818

Abstract

According to the concept of circular economy, insects represent good candidates as aquafeed ingredients. Nevertheless, there are some potential chemical risks linked with insect consumption. In this study, we reared the teleost Danio rerio, used as an experimental model, with five experimental diets characterized by increasing levels (0%, 25%, 50%, 75%, and 100%) of full-fat Hermetia illucens (Hi) prepupae, substituting for fish meal (FM) and fish oil (FO). We investigated the presence of potentially toxic elements (PTEs) Cd, Pb, Ni, As, and Hg in larval (20 days), juvenile (2 months), and adult (6 months) fish. Quantitative determinations of Cd, Pb, Ni, and As were made with an atomic absorption spectrometer; the total mercury content was determined by a direct mercury analyzer. The substitution of FM and FO with Hermetia illucens meal led to a reduction in the content of some PTEs, such as Pb, As, and Ni, in fishfeed, leading to concentrations below the legal limit of undesirable substances in animal feed. By increasing the Hi meal dietary content, we observed in the Danio rerio specimens an increase in Cd, Pb, and Ni content and a reduction in As content for all life stages. Moreover, a general increase in the content of Cd, Pb, Hg, and Ni from larvae to juvenile was measured, while the shift of Danio rerio from the juvenile to the adult stage involved a significant increase in the content of Pb, Hg, and Ni. Larvae had a reduced ability to bioaccumulate metal(loid)s compared to juveniles and adults. In conclusion, the content of PTEs in Danio rerio is influenced both by the type of diet administered and by the life stage of the animal itself. This research demonstrates the possibility of using Hi prepupae as an aquafeed ingredient without exposing fish to a chemical risk and, in perspective, allows applying these eco-sustainable diets for the breeding of edible fish species, without endangering human health. Full article

(This article belongs to the Special Issue Determination of Trace Heavy Metals and Metalloids in Environmental and Food Samples II)

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