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In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine

A special issue of International Journal of Molecular Sciences (ISSN 1422-0067). This special issue belongs to the section "Biochemistry".

Deadline for manuscript submissions: 30 September 2024 | Viewed by 5466

Special Issue Editors

Prof. Dr. Roberta Bertani

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Guest Editor
Department of Industrial Engineering, Università degli Studi di Padova, Padua, Italy
Interests: organometallic and coordination systems; platinum systems; catalysis; bioactive inorganic materials; nanomaterials; magnetic materials; magnetic hyperhermia; hybrid materials; multifunctional polymer composites and nanocomposites
Prof. Dr. Francesco Paolo Fanizzi

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Guest Editor
Department of Biological and Environmental Sciences and Technologies (DISTEBA), University of Salento, Lecce, Italy
Interests: transition metals (specially platinum) coordination organometallic; bioinorganic chemistry; applications of high field NMR Spectroscopy in the fields of chemistry, biology, pharmaceutical and food sciences
Dr. Nicola Margiotta

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Guest Editor
Dipartimento di Chimica, Università degli Studi di Bari Aldo Moro, Via E. Orabona 4, 70125 Bari, Italy
Interests: medicinal inorganic chemistry; organometallic chemistry; metal-based complexes; antitumor platinum drugs; drug delivery of antitumor drugs by inorganic nanocarriers
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Special Issue Information

Dear Colleagues, 

Giovanni Natile was born in November 1944 in Putignano (Bari, Italy). After graduating in Chemistry in 1968 from the University of Padua, he devoted himself to general and inorganic chemistry as the foundation for a better knowledge of the biochemical and biological processes to be translated in medicinal applications. Chemistry, in this area, has in fact contributed to the understanding of some physiological and pathological processes and to the development of modern pharmacology. Since 1981, he has been a Professor of General and Inorganic Chemistry in the Faculty of Pharmaceutical Sciences at the University of Bari, Italy. As President of the Italian Chemical Society (SCI), Giovanni Natile has worked devotedly to strengthen its editorial policy and to encourage the collaboration with other European chemical societies to improve their partnership and initiated actions to promote the diffusion of chemical knowledge at all levels of society. As European Chemical Society (EuChemS) President (2005-2008), Giovanni Natile chaired its launch event at the European Parliament in 2006, bringing together representatives of the Parliament and the Commission with guests from the key European organizations involved in chemical sciences. With his support, EuCheMS, having signed a declaration on sustainable development, played a prominent role in developing policies, holding meetings in Brussels to publicize reports on energy and sustainable water management. He supported the creation of the European Young Chemists Network and the launch of the European Young Chemist Award. He led EuCheMS in strengthening its links with sister organizations, including the European Chemical Industry Council (CEFIC) and the European Physical Society (EPS). He is Professor Emeritus at the University of Bari.

Giovanni Natile has offered an invaluable contribution to the development and understanding of bioinorganic chemistry of anticancer transition metal organometallic complexes, authoring more than 300 papers. His research activity, which ranges from the first trans-platinum systems with cytotoxic activity, the antitumor activity of Pt(IV) compounds, to the occurrence and overcoming of resistance, metal interference, and the mechanisms of metals’ cellular uptake, has proved the importance of interdisciplinary collaboration in science.

This anniversary Special Issue, entitled “In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine”, aims to honor his scientific career by collecting papers concerning the chemistry of metals in biological systems and in medicine, dealing with metalloenzymes and metal-based drugs, retracing the path that, from cisplatin, led to the discovery of new metal compounds in cancer therapy and the understanding of metals’ role in the tumors' development.

Prof. Dr. Roberta Bertani
Prof. Dr. Francesco Paolo Fanizzi
Dr. Nicola Margiotta
Guest Editors

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Published Papers (4 papers)

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Research

15 pages, 7083 KiB  
Article
Metal Ion Binding to Human Glutaminyl Cyclase: A Structural Perspective
by Giusy Tassone, Cecilia Pozzi and Stefano Mangani
Int. J. Mol. Sci. 2024, 25(15), 8279; https://doi.org/10.3390/ijms25158279 - 29 Jul 2024
Viewed by 478
Abstract
Glutaminyl-peptide cyclotransferases (QCs) convert the N-terminal glutamine or glutamate residues of protein and peptide substrates into pyroglutamate (pE) by releasing ammonia or a water molecule. The N-terminal pE modification protects peptides/proteins against proteolytic degradation by amino- or exopeptidases, increasing their stability. Mammalian QC [...] Read more.
Glutaminyl-peptide cyclotransferases (QCs) convert the N-terminal glutamine or glutamate residues of protein and peptide substrates into pyroglutamate (pE) by releasing ammonia or a water molecule. The N-terminal pE modification protects peptides/proteins against proteolytic degradation by amino- or exopeptidases, increasing their stability. Mammalian QC is abundant in the brain and a large amount of evidence indicates that pE peptides are involved in the onset of neural human pathologies such as Alzheimer’s and Huntington’s disease and synucleinopathies. Hence, human QC (hQC) has become an intensively studied target for drug development against these diseases. Soon after its characterization, hQC was identified as a Zn-dependent enzyme, but a partial restoration of the enzyme activity in the presence of the Co(II) ion was also reported, suggesting a possible role of this metal ion in catalysis. The present work aims to investigate the structure of demetallated hQC and of the reconstituted enzyme with Zn(II) and Co(II) and their behavior in the presence of known inhibitors. Furthermore, our structural determinations provide a possible explanation for the presence of the mononuclear metal binding site of hQC, despite the presence of the same conserved metal binding motifs present in distantly related dinuclear aminopeptidase enzymes. Full article
(This article belongs to the Special Issue In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine)
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12 pages, 2351 KiB  
Communication
Description of a Non-Canonical AsPt Blue Species Originating from the Aerobic Oxidation of AP-1 in Aqueous Solution
by Damiano Cirri, Tiziano Marzo, Piero Mastrorilli, Valentina Petrelli, Stefano Todisco, Elvira De Giglio, Cristina Gellini, Marilena Ricci, Alessandro Pratesi and Luigi Messori
Int. J. Mol. Sci. 2024, 25(13), 7408; https://doi.org/10.3390/ijms25137408 - 5 Jul 2024
Viewed by 550
Abstract
The peculiar behavior of arsenoplatin-1, ([Pt(µ-NHC(CH3)O)2ClAs(OH)2], AP-1), in aqueous solution and the progressive appearance of a characteristic and intense blue color led us to carry out a more extensive investigation to determine the nature of this elusive [...] Read more.
The peculiar behavior of arsenoplatin-1, ([Pt(µ-NHC(CH3)O)2ClAs(OH)2], AP-1), in aqueous solution and the progressive appearance of a characteristic and intense blue color led us to carry out a more extensive investigation to determine the nature of this elusive chemical species, which we named “AsPt blue”. A multi-technique approach was therefore implemented to describe the processes involved in the formation of AsPt blue, and some characteristic features of this intriguing species were revealed. Full article
(This article belongs to the Special Issue In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine)
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13 pages, 1702 KiB  
Article
Synthesis and Characterisation of Platinum(II) Diaminocyclohexane Complexes with Pyridine Derivatives as Anticancer Agents
by Brondwyn S. McGhie, Jennette Sakoff, Jayne Gilbert, Christopher P. Gordon and Janice R. Aldrich-Wright
Int. J. Mol. Sci. 2023, 24(24), 17150; https://doi.org/10.3390/ijms242417150 - 5 Dec 2023
Cited by 1 | Viewed by 1383
Abstract
Cisplatin-type covalent chemotherapeutics are a cornerstone of modern medicinal oncology. However, these drugs remain encumbered with dose-limiting side effects and are susceptible to innate and acquired resistance. The bulk of platinum anticancer research has focused on Cisplatin and its derivatives. Here, we take [...] Read more.
Cisplatin-type covalent chemotherapeutics are a cornerstone of modern medicinal oncology. However, these drugs remain encumbered with dose-limiting side effects and are susceptible to innate and acquired resistance. The bulk of platinum anticancer research has focused on Cisplatin and its derivatives. Here, we take inspiration from the design of platinum complexes and ligands used successfully with other metals to create six novel complexes. Herein, the synthesis, characterization, DNA binding affinities, and lipophilicity of a series of non-traditional organometallic Pt(II)-complexes are described. These complexes have a basic [Pt(PL)(AL)]Cl2 molecular formula which incorporates either 2-pyrrolidin-2-ylpyridine, 2-(1H-Imidazol-2-yl)pyridine, or 2-(2-pyridyl)benzimidazole as the PL; the AL is resolved diaminocyclohexane. Precursor [Pt(PL)(Cl)2] complexes were also characterized for comparison. While the cytotoxicity and DNA binding properties of the three precursors were unexceptional, the corresponding [Pt(PL)(AL)]2+ complexes were promising; they exhibited different DNA binding interactions compared with Cisplatin but with similar, if not slightly better, cytotoxicity results. Complexes with 2-pyrrolidin-2-ylpyridine or 2-(2-pyridyl)benzimidazole ligands had similar DNA binding properties to those with 2-(1H-Imidazol-2-yl)pyridine ligands but were not as cytotoxic to all cell lines. The variation in activity between cell lines was remarkable and resulted in significant selectivity indices in MCF10A and MCF-7 breast cancer cell lines, compared with previously described similar Pt(II) complexes such as 56MESS. Full article
(This article belongs to the Special Issue In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine)
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13 pages, 2890 KiB  
Article
Wireframe DNA Origami for the Cellular Delivery of Platinum(II)-Based Drugs
by Erik De Luca, Yang Wang, Igor Baars, Federica De Castro, Marco Lolaico, Danilo Migoni, Cosimo Ducani, Michele Benedetti, Björn Högberg and Francesco Paolo Fanizzi
Int. J. Mol. Sci. 2023, 24(23), 16715; https://doi.org/10.3390/ijms242316715 - 24 Nov 2023
Viewed by 1610
Abstract
The DNA origami method has revolutionized the field of DNA nanotechnology since its introduction. These nanostructures, with their customizable shape and size, addressability, nontoxicity, and capacity to carry bioactive molecules, are promising vehicles for therapeutic delivery. Different approaches have been developed for manipulating [...] Read more.
The DNA origami method has revolutionized the field of DNA nanotechnology since its introduction. These nanostructures, with their customizable shape and size, addressability, nontoxicity, and capacity to carry bioactive molecules, are promising vehicles for therapeutic delivery. Different approaches have been developed for manipulating and folding DNA origami, resulting in compact lattice-based and wireframe designs. Platinum-based complexes, such as cisplatin and phenanthriplatin, have gained attention for their potential in cancer and antiviral treatments. Phenanthriplatin, in particular, has shown significant antitumor properties by binding to DNA at a single site and inhibiting transcription. The present work aims to study wireframe DNA origami nanostructures as possible carriers for platinum compounds in cancer therapy, employing both cisplatin and phenanthriplatin as model compounds. This research explores the assembly, platinum loading capacity, stability, and modulation of cytotoxicity in cancer cell lines. The findings indicate that nanomolar quantities of the ball-like origami nanostructure, obtained in the presence of phenanthriplatin and therefore loaded with that specific drug, reduced cell viability in MCF-7 (cisplatin-resistant breast adenocarcinoma cell line) to 33%, while being ineffective on the other tested cancer cell lines. The overall results provide valuable insights into using wireframe DNA origami as a highly stable possible carrier of Pt species for very long time-release purposes. Full article
(This article belongs to the Special Issue In Honor of Giovanni Natile’s 80th Birthday: Metals in Biology and Medicine)
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