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Metal Intoxication: General Aspects and Chelating Agents
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Metal Intoxication: General Aspects and Chelating Agents

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

Deadline for manuscript submissions: closed (31 July 2022) | Viewed by 9440

Special Issue Editors

Dr. Massimiliano F. Peana

E-Mail Website
Guest Editor
Department of Chemical, Physical, Mathematical and Natural Sciences, University of Sassari, Via Vienna 2, 07100 Sassari, Italy
Interests: coordination chemistry; spectroscopy; NMR spectroscopy; transition metals; toxic metals; neurodegeneration; metal complexes; peptides; amino acids; proteins; metal interaction; chelation therapy; chelating agents
Dr. Christos T. Chasapis

E-Mail Website1 Website2
Guest Editor
1. NMR Center, Instrumental Analysis Laboratory, School of Natural Sciences, University of Patras, Patras, Greece
2. Institute of Chemical Engineering Sciences (ICE-HT), Foundation for Research and Technology, Hellas (FORTH), Patras, Greece
Interests: biochemistry; structural biology; NMR spectroscopy; transition metals; biotechnology; proteins; metal interaction; Wilson’s disease; coordination chemistry; bioinformatic

Special Issue Information

Dear Colleagues,

Several metals, such as sodium, potassium, magnesium, calcium, iron, manganese, cobalt, copper, zinc, and molybdenum, are essential for human health. They are indispensable elements for life, playing important roles in a wide variety of biological processes. Essential transition metals, like Fe, Mn, Cu, and Zn, participate in controlling various metabolic and signaling pathways. The human body needs appropriate amounts and their concentration has to be finely regulated, as any imbalance in their homeostasis can induce abnormalities.

Additionally, humans are also exposed to non-essential and toxic metals. Large environmental amounts of such chemicals come from both natural and anthropogenic sources, with the latter being predominant because of extensive metal mining and smelting, several industrial activities, incinerators, and the combustion of fossil fuel.

The dissipation of toxic metals, such as lead, mercury, arsenic, cadmium, aluminum, uranium, and tungsten contaminate water, air, soil, and food, causing a series of chronic and acute syndromes.

The characteristic coordination ability, dimension, and chemical properties of such metals make them, in particular circumstances, able to interact with protein sites other than those that are eventually tailored to them, by displacing other essential metals from their natural binding sites, leading to cell malfunctions and toxicity. Some of them (essential and not) possess redox properties and are a key inducer of reactive oxygen species, leading to oxidative stress and several cellular damage. If the doses of exposure exceed the capacity of the detoxification and homeostatic control, a sequence of cascade key events will occur at progressively higher levels of organization—from a cellular level (altered cell physiology, cycle and growth, cytotoxicity, genotoxicity, inflammation, altered mitochondria, and chloroplast function) to organ level (altered metabolism, altered organ physiology, altered nutrient dynamics, altered growth, and maintenance), until the whole organism responses (cancer, neurodegenerative disorders, organ failure, etc.). Clinical experience has demonstrated that acute and chronic metal intoxications can be treated efficiently using chelation therapy.

This clinical intervention involves the administration of chelating agents—molecules rationally designed to have a relatively higher affinity and selectivity for specific toxic metal ions, able to remove specific toxic metals from the body and maintain a safe and proper concentration at physiological levels for essential metals. They must form chemically inert and non-toxic metal complexes, and should not disturb the homeostasis of the essential biological metal ions. Moreover, chelating agents should enter the cell membrane to remove intracellular toxic metals, and should be rapidly and easily excreted from the body. An effective and safe chelating agent specific for each toxic metal ion, without side effects, is a challenging target. In addition, most available chelators do not cross the blood–brain barrier; consequently, they have a limited ability to remove metals from the brain tissue. The actual research is focused on evaluating the available chelating agents, improving their performances, and the development of new chelators and applications for clinical treatments.

This Special ssue aims to exploit heavy metal toxicity in humans, the chelation approach for their removal from the body, and to present the reader with the latest progress in the development of chelating strategies to treat chronic and acute metal intoxication. Submissions focusing on all aspects of chelation treatment (alone or in combination), including nutritional interventions, are welcome. Related and similar topics are also encouraged.

Potential topics include, but are not limited to, the following:

  • Chemical characterization of novel metal chelators for chronic and/or acute specific metal intoxication
  • Potential metal chelators in human diseases
  • Advances in chelation strategies and chelating agents in medicine
  • Exploration of the molecular mechanism of metal toxicity and the mechanisms of action for their removal
  • Studies devoted to the design and development of chelating agents’ functionalization for sensing or targeting purposes
  • Studies on the metal chelators’ properties, i.e., absorption, distribution, metabolism, and excretion
  • Potential nutritional intervention for metal detoxification.

Dr. Massimiliano F. Peana
Dr. Christos T. Chasapis
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

  • Chelation therapy
  • Chelating agents
  • Acute and chronic metal intoxication
  • Heavy metals
  • Toxic metals

Published Papers (4 papers)

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Research

20 pages, 12627 KiB  
Article
Confirming the Molecular Basis of the Solvent Extraction of Cadmium(II) Using 2-Pyridyl Oximes through a Synthetic Inorganic Chemistry Approach and a Proposal for More Efficient Extractants
by Anastasia Routzomani, Zoi G. Lada, Varvara Angelidou, Catherine P. Raptopoulou, Vassilis Psycharis, Konstantis F. Konidaris, Christos T. Chasapis and Spyros P. Perlepes
Molecules 2022, 27(5), 1619; https://doi.org/10.3390/molecules27051619 - 28 Feb 2022
Cited by 5 | Viewed by 2717
Abstract
The present work describes the reactions of CdI2 with 2-pyridyl aldoxime (2paoH), 3-pyridyl aldoxime (3paoH), 4-pyridyl aldoxime (4paoH), 2-6-diacetylpyridine dioxime (dapdoH2) and 2,6-pyridyl diamidoxime (LH4). The primary goal was to contribute to understanding the molecular basis of the [...] Read more.
The present work describes the reactions of CdI2 with 2-pyridyl aldoxime (2paoH), 3-pyridyl aldoxime (3paoH), 4-pyridyl aldoxime (4paoH), 2-6-diacetylpyridine dioxime (dapdoH2) and 2,6-pyridyl diamidoxime (LH4). The primary goal was to contribute to understanding the molecular basis of the very good liquid extraction ability of 2-pyridyl ketoximes with long aliphatic chains towards toxic Cd(II) and the inability of their 4-pyridyl isomers for this extraction. Our systematic investigation provided access to coordination complexes [CdI2(2paoH)2] (1), {[CdI2(3paoH)2]}n (2), {[CdI2(4paoH)2]}n (3) and [CdI2(dapdoH2)] (4). The reaction of CdI2 and LH4 in EtOH resulted in a Cd(II)-involving reaction of the bis(amidoxime) and isolation of [CdI2(L’H2)] (5), where L’H2 is the new ligand 2,6-bis(ethoxy)pyridine diimine. A mechanism of this transformation has been proposed. The structures of 1, 2, 3, 4·2EtOH and 5 were determined by single-crystal X-ray crystallography. The complexes have been characterized by FT-IR and FT-Raman spectra in the solid state and the data are discussed in terms of structural features. The stability of the complexes in DMSO was investigated by 1H NMR spectroscopy. Our studies confirm that the excellent extraction ability of 2-pyridyl ketoximes is due to the chelating nature of the extractants leading to thermodynamically stable Cd(II) complexes. The monodentate coordination of 4-pyridyl ketoximes (as confirmed in our model complexes with 4paoH and 3paoH) seems to be responsible for their poor performance as extractants. Full article
(This article belongs to the Special Issue Metal Intoxication: General Aspects and Chelating Agents)
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10 pages, 1247 KiB  
Article
Structural Identification of Metalloproteomes in Marine Diatoms, an Efficient Algae Model in Toxic Metals Bioremediation
by Christos T. Chasapis, Massimiliano Peana and Vlasoula Bekiari
Molecules 2022, 27(2), 378; https://doi.org/10.3390/molecules27020378 - 7 Jan 2022
Cited by 11 | Viewed by 2266
Abstract
The biosorption of pollutants using microbial organisms has received growing interest in the last decades. Diatoms, the most dominant group of phytoplankton in oceans, are (i) pollution tolerant species, (ii) excellent biological indicators of water quality, and (iii) efficient models in assimilation and [...] Read more.
The biosorption of pollutants using microbial organisms has received growing interest in the last decades. Diatoms, the most dominant group of phytoplankton in oceans, are (i) pollution tolerant species, (ii) excellent biological indicators of water quality, and (iii) efficient models in assimilation and detoxification of toxic metal ions. Published research articles connecting proteomics with the capacity of diatoms for toxic metal removal are very limited. In this work, we employed a structural based systematic approach to predict and analyze the metalloproteome of six species of marine diatoms: Thalassiosira pseudonana, Phaeodactylum tricornutum, Fragilariopsis cylindrus, Thalassiosira oceanica, Fistulifera solaris, and Pseudo-nitzschia multistriata. The results indicate that the metalloproteome constitutes a significant proportion (~13%) of the total diatom proteome for all species investigated, and the proteins binding non-essential metals (Cd, Hg, Pb, Cr, As, and Ba) are significantly more than those identified for essential metals (Zn, Cu, Fe, Ca, Mg, Mn, Co, and Ni). These findings are most likely related to the well-known toxic metal tolerance of diatoms. In this study, metalloproteomes that may be involved in metabolic processes and in the mechanisms of bioaccumulation and detoxification of toxic metals of diatoms after exposure to toxic metals were identified and described. Full article
(This article belongs to the Special Issue Metal Intoxication: General Aspects and Chelating Agents)
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30 pages, 6522 KiB  
Article
The Effect of Metal Cations on the Aqueous Behavior of Dopamine. Thermodynamic Investigation of the Binary and Ternary Interactions with Cd2+, Cu2+ and UO22+ in NaCl at Different Ionic Strengths and Temperatures
by Antonio Gigliuto, Rosalia Maria Cigala, Anna Irto, Maria Rosa Felice, Alberto Pettignano, Concetta De Stefano and Francesco Crea
Molecules 2021, 26(24), 7679; https://doi.org/10.3390/molecules26247679 - 19 Dec 2021
Cited by 3 | Viewed by 2138
Abstract
The interactions of dopamine [2-(3,4-Dihydroxyphenyl)ethylamine, (Dop−)] with cadmium(II), copper(II) and uranyl(VI) were studied in NaCl(aq) at different ionic strengths (0 ≤ I/mol dm−3 ≤ 1.0) and temperatures (288.15 ≤ T/K ≤ 318.15). From the elaboration of the experimental [...] Read more.
The interactions of dopamine [2-(3,4-Dihydroxyphenyl)ethylamine, (Dop−)] with cadmium(II), copper(II) and uranyl(VI) were studied in NaCl(aq) at different ionic strengths (0 ≤ I/mol dm−3 ≤ 1.0) and temperatures (288.15 ≤ T/K ≤ 318.15). From the elaboration of the experimental data, it was found that the speciation models are featured by species of different stoichiometry and stability. In particular for cadmium, the formation of only MLH, ML and ML2 (M = Cd2+; L = dopamine) species was obtained. For uranyl(VI) (UO22+), the speciation scheme is influenced by the use of UO2(acetate)2 salt as a chemical; in this case, the formation of ML2, MLOH and the ternary MLAc (Ac = acetate) species in a wide pH range was observed. The most complex speciation model was obtained for the interaction of Cu2+ with dopamine; in this case we observed the formation of the following species: ML2, M2L, M2L2, M2L2(OH)2, M2LOH and ML2OH. These speciation models were determined at each ionic strength and temperature investigated. As a further contribution to this kind of investigation, the ternary interactions of dopamine with UO22+/Cd2+ and UO22+/Cu2+ were investigated at I = 0.15 mol dm−3 and T = 298.15K. These systems have different speciation models, with the MM’L and M2M’L2OH [M = UO22+; M’ = Cd2+ or Cu2+, L = dopamine] common species; the species of the mixed Cd2+ containing system have a higher stability with respect the Cu2+ containing one. The dependence on the ionic strength of complex formation constants was modelled by using both an extended Debye–Hückel equation that included the Van’t Hoff term for the calculation of the formation enthalpy change values and the Specific Ion Interaction Theory (SIT). The results highlighted that, in general, the entropy is the driving force of the process. The quantification of the effective sequestering ability of dopamine towards the studied cations was evaluated by using a Boltzmann-type equation and the calculation of pL0.5 parameter. The sequestering ability was quantified at different ionic strengths, temperatures and pHs, and this resulted, in general, that the pL0.5 trend was always: UO22+ > Cu2+ > Cd2+. Full article
(This article belongs to the Special Issue Metal Intoxication: General Aspects and Chelating Agents)
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19 pages, 3124 KiB  
Article
Bifunctional 3-Hydroxy-4-Pyridinones as Potential Selective Iron(III) Chelators: Solution Studies and Comparison with Other Metals of Biological and Environmental Relevance
by Anna Irto, Paola Cardiano, Karam Chand, Rosalia Maria Cigala, Francesco Crea, Concetta De Stefano and Maria Amélia Santos
Molecules 2021, 26(23), 7280; https://doi.org/10.3390/molecules26237280 - 30 Nov 2021
Cited by 4 | Viewed by 1451
Abstract
The binding ability of five bifunctional 3-hydroxy-4-pyridinones towards Cu2+ and Fe3+ was studied by means of potentiometric and UV–Vis spectrophotometric measurements carried out at I = 0.15 mol L−1 in NaCl(aq),T = 298.15 K and 310.15 K. The [...] Read more.
The binding ability of five bifunctional 3-hydroxy-4-pyridinones towards Cu2+ and Fe3+ was studied by means of potentiometric and UV–Vis spectrophotometric measurements carried out at I = 0.15 mol L−1 in NaCl(aq),T = 298.15 K and 310.15 K. The data treatments allowed us to determine speciation schemes featured by metal-ligand species with different stoichiometry and stability, owing to the various functional groups present in the 3-hydroxy-4-pyridinones structures, which could potentially participate in the metal complexation, and in the Cu2+ and Fe3+ behaviour in aqueous solution. Furthermore, the sequestering ability and metal chelating affinity of the ligands were investigated by the determination of pL0.5 and pM parameters at different pH conditions. Finally, a comparison between the Cu2+ and Fe3+/3-hydroxy-4-pyridinones data herein presented with those already reported in the literature on the interaction of Zn2+ and Al3+ with the same ligands showed that, from the thermodynamic point of view, the 3-hydroxy-4-pyridinones are particularly selective towards Fe3+ and could therefore be considered promising iron-chelating agents, also avoiding the possibility of competition, and eventually the depletion, of essential metal cations of biological and environmental relevance, such as Cu2+ and Zn2+. Full article
(This article belongs to the Special Issue Metal Intoxication: General Aspects and Chelating Agents)
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