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Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular...
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Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular Fluids

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

Deadline for manuscript submissions: closed (31 December 2021) | Viewed by 12271

Special Issue Editors

Dr. Andre Silva

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Guest Editor
LAQV-REQUIMTE, Departmento de Química e Bioquímica, Faculdade de Ciências, Universidade do Porto, Porto, Portugal
Interests: inorganic biochemistry; metal ions in biology; iron biochemistry; protein post-translational modifications
Special Issues, Collections and Topics in MDPI journals
Dr. Maria Rangel

E-Mail Website
Guest Editor
LAQV/REQUIMTE, Instituto de Ciências Biomédicas de Abel Salazar, Universidade do Porto, 4099-003 Porto, Portugal
Interests: bioinorganic chemistry; metal ions in biology; iron chelators; EPR spectroscopy; membranes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear colleagues,

Transition metal ions are essential for life. Metalloenzymes correspond to over a third of all enzymes, and they play an essential role in fundamental biological processes such as DNA synthesis and replication, oxygen transport, mitochondrial respiration and photosynthesis. However, there is an inherent toxicity problem which emanates from intrinsic reactivity under biological conditions. In order to prevent the deleterious effects resulting either from the deficit of these micronutrients or their toxic surplus, organisms have to tightly regulate metal ion levels and control their speciation in different compartments. In higher organisms (Animals and Plants) this tight regulation also means controlling both transport to the various organs and bioavailability to different tissues and cells.

In this context, understanding the solution chemistry of metal ions in extracellular biological fluids is fundamental both to understand their cellular bioavailability and toxicity. Having a clear knowledge about metal ion ligands, stability constants and redox potentials may provide the means to identify cellular import pathways and biochemical regulatory mechanisms.

In addition, several metal ion chelates (metallodrugs) are used as medicines and supplements, such as some radiopharmaceuticals, insulin mimetic drugs and iron formulations to fight anaemia. An important step in comprehending their safety and efficacy is to realise their stability, distribution and association with proteins in biological fluids (blood serum, cerebrospinal fluid, etc..).

This Special Issue of Molecules is dedicated to original research and review articles that cover the latest findings on metal ion chemistry in extracellular biological fluids. We will welcome speciation or redox studies in biological samples or model systems providing relevant insights for biological conditions. Results concerning association with proteins or on how protein expression levels or modifications influence metal ions distribution or bioavailability will be accepted. Description of quantification methods for individual species by chemical or spectroscopic methods will also be considered.


Dr. Andre Silva
Prof. Dr. Maria Rangel
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

  • Metal ion speciation
  • Metal ion complex stability
  • Metallodrugs
  • Blood plasma
  • Interstitial fluid
  • Cerebrospinal fluid
  • Xylem sap
  • Phloem sap
  • Apoplast
  • Metal ion chelates
  • Metal ion protein binding
  • Protein modifications

Published Papers (4 papers)

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Research

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16 pages, 1325 KiB  
Article
Comparative Evaluation of Intestinal Absorption and Functional Value of Iron Dietary Supplements and Drug with Different Delivery Systems
by Paolo Pastore, Marco Roverso, Erik Tedesco, Marta Micheletto, Etienne Mantovan, Michela Zanella and Federico Benetti
Molecules 2020, 25(24), 5989; https://doi.org/10.3390/molecules25245989 - 17 Dec 2020
Cited by 6 | Viewed by 2943
Abstract
Iron is a fundament micronutrient, whose homeostasis is strictly regulated. Iron deficiency anemia is among the most widespread nutritional deficiencies and its therapy, based on dietary supplement and drugs, may lead to severe side effects. With the aim of improving iron bioavailability while [...] Read more.
Iron is a fundament micronutrient, whose homeostasis is strictly regulated. Iron deficiency anemia is among the most widespread nutritional deficiencies and its therapy, based on dietary supplement and drugs, may lead to severe side effects. With the aim of improving iron bioavailability while reducing iron oral therapy side effects, novel dietary supplements based on innovative technologies—microencapsulation, liposomes, sucrosomes—have been produced and marketed. In the present work, six iron dietary supplements for different therapeutic targets were compared in terms of bioaccessibility, bioavailability, and safety by using an integrated in vitro approach. For general-purpose iron supplements, ME + VitC (microencapsulated) showed a fast, burst intestinal iron absorption kinetic, which maintained iron bioavailability and ferritin expression constant over time. SS + VitC (sucrosomes), on the other side, showed a slower, time-dependent iron absorption and ferritin expression trend. ME + Folate (microencapsulated) showed a behavior similar to that of ME + VitC, albeit with a lower bioavailability. Among pediatric iron supplements, a time-dependent bioavailability increase was observed for LS (liposome), while PIC (polydextrose-iron complex) bioavailability is severely limited by its poor bioaccessibility. Finally, except for SS + VitC, no adverse effects on intestinal mucosa vitality and barrier integrity were observed. Considering obtained results and the different therapeutic targets, microencapsulation-based formulations are endowed with better performance compared to the other formulations. Furthermore, performances of microencapsulated products were obtained with a lower iron daily dose, limiting the potential onset of side effects. Full article
(This article belongs to the Special Issue Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular Fluids)
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12 pages, 1413 KiB  
Article
Novel Insights into Mercury Effects on Hemoglobin and Membrane Proteins in Human Erythrocytes
by Marina Piscopo, Rosaria Notariale, Fabiana Tortora, Gennaro Lettieri, Giancarlo Palumbo and Caterina Manna
Molecules 2020, 25(14), 3278; https://doi.org/10.3390/molecules25143278 - 19 Jul 2020
Cited by 20 | Viewed by 2533
Abstract
Mercury (Hg) is a global environmental pollutant that affects human and ecosystem health. With the aim of exploring the Hg-induced protein modifications, intact human erythrocytes were exposed to HgCl2 (1–60 µM) and cytosolic and membrane proteins were analyzed by SDS-PAGE and AU-PAGE. [...] Read more.
Mercury (Hg) is a global environmental pollutant that affects human and ecosystem health. With the aim of exploring the Hg-induced protein modifications, intact human erythrocytes were exposed to HgCl2 (1–60 µM) and cytosolic and membrane proteins were analyzed by SDS-PAGE and AU-PAGE. A spectrofluorimetric assay for quantification of Reactive Oxygen Species (ROS) generation was also performed. Hg2+ exposure induces alterations in the electrophoretic profile of cytosolic proteins with a significant decrease in the intensity of the hemoglobin monomer, associated with the appearance of a 64 kDa band, identified as a mercurized tetrameric form. This protein decreases with increasing HgCl2 concentrations and Hg-induced ROS formation. Moreover, it appears resistant to urea denaturation and it is only partially dissociated by exposure to dithiothreitol, likely due to additional protein–Hg interactions involved in aggregate formation. In addition, specific membrane proteins, including band 3 and cytoskeletal proteins 4.1 and 4.2, are affected by Hg2+-treatment. The findings reported provide new insights into the Hg-induced possible detrimental effects on erythrocyte physiology, mainly related to alterations in the oxygen binding capacity of hemoglobin as well as decreases in band 3-mediated anion exchange. Finally, modifications of cytoskeletal proteins 4.1 and 4.2 could contribute to the previously reported alteration in cell morphology. Full article
(This article belongs to the Special Issue Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular Fluids)
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Review

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14 pages, 1014 KiB  
Review
The (Bio)Chemistry of Non-Transferrin-Bound Iron
by André M. N. Silva and Maria Rangel
Molecules 2022, 27(6), 1784; https://doi.org/10.3390/molecules27061784 - 09 Mar 2022
Cited by 19 | Viewed by 3692
Abstract
In healthy individuals, virtually all blood plasma iron is bound by transferrin. However, in several diseases and clinical conditions, hazardous non-transferrin-bound iron (NTBI) species occur. NTBI represents a potentially toxic iron form, being a direct cause of oxidative stress in the circulating compartment [...] Read more.
In healthy individuals, virtually all blood plasma iron is bound by transferrin. However, in several diseases and clinical conditions, hazardous non-transferrin-bound iron (NTBI) species occur. NTBI represents a potentially toxic iron form, being a direct cause of oxidative stress in the circulating compartment and tissue iron loading. The accumulation of these species can cause cellular damage in several organs, namely, the liver, spleen, and heart. Despite its pathophysiological relevance, the chemical nature of NTBI remains elusive. This has precluded its use as a clinical biochemical marker and the development of targeted therapies. Herein, we make a critical assessment of the current knowledge of NTBI speciation. The currently accepted hypotheses suggest that NTBI is mostly iron bound to citric acid and iron bound to serum albumin, but the chemistry of this system remains fuzzy. We explore the complex chemistry of iron complexation by citric acid and its implications towards NTBI reactivity. Further, the ability of albumin to bind iron is revised and the role of protein post-translational modifications on iron binding is discussed. The characterization of the NTBI species structure may be the starting point for the development of a standardized analytical assay, the better understanding of these species’ reactivity or the identification of NTBI uptake mechanisms by different cell types, and finally, to the development of new therapies. Full article
(This article belongs to the Special Issue Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular Fluids)
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Other

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17 pages, 2452 KiB  
Perspective
Toxic Metal Species and ‘Endogenous’ Metalloproteins at the Blood–Organ Interface: Analytical and Bioinorganic Aspects
by Tristen G. Bridle, Premkumari Kumarathasan and Jürgen Gailer
Molecules 2021, 26(11), 3408; https://doi.org/10.3390/molecules26113408 - 04 Jun 2021
Cited by 12 | Viewed by 2520
Abstract
Globally, human exposure to environmental pollutants causes an estimated 9 million deaths per year and it could also be implicated in the etiology of diseases that do not appear to have a genetic origin. Accordingly, there is a need to gain information about [...] Read more.
Globally, human exposure to environmental pollutants causes an estimated 9 million deaths per year and it could also be implicated in the etiology of diseases that do not appear to have a genetic origin. Accordingly, there is a need to gain information about the biomolecular mechanisms that causally link exposure to inorganic environmental pollutants with distinct adverse health effects. Although the analysis of blood plasma and red blood cell (RBC) cytosol can provide important biochemical information about these mechanisms, the inherent complexity of these biological matrices can make this a difficult task. In this perspective, we will examine the use of metalloentities that are present in plasma and RBC cytosol as potential exposure biomarkers to assess human exposure to inorganic pollutants. Our primary objective is to explore the principal bioinorganic processes that contribute to increased or decreased metalloprotein concentrations in plasma and/or RBC cytosol. Furthermore, we will also identify metabolites which can form in the bloodstream and contain essential as well as toxic metals for use as exposure biomarkers. While the latter metal species represent useful biomarkers for short-term exposure, endogenous plasma metalloproteins represent indicators to assess the long-term exposure of an individual to inorganic pollutants. Based on these considerations, the quantification of metalloentities in blood plasma and/or RBC cytosol is identified as a feasible research avenue to better understand the adverse health effects that are associated with chronic exposure of various human populations to inorganic pollutants. Exposure to these pollutants will likely increase as a consequence of technological advances, including the fast-growing applications of metal-based engineering nanomaterials. Full article
(This article belongs to the Special Issue Molecular and Spectroscopic Insights into Metal Ions Speciation in Extracellular Fluids)
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