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Metal-Based Complexes in Cancer 2.0
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Metal-Based Complexes in Cancer 2.0

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

Deadline for manuscript submissions: 31 July 2024 | Viewed by 11597

Special Issue Editors

Dr. Claudia Riccardi

E-Mail Website
Guest Editor
Department of Chemical Sciences, University of Naples Federico II, 80126 Naples, Italy
Interests: ruthenium complexes; platinum complexes; benzodifuran compounds; oligonucleotides; G-quadruplex; aptamers; thrombin binding aptamers; nanosystems; nanomaterials
Special Issues, Collections and Topics in MDPI journals
Dr. Marialuisa Piccolo

E-Mail Website
Guest Editor
Department of Pharmacy, School of Medicine, University of Naples Federico II, 80131 Naples, Italy
Interests: preclinical investigation of anticancer compounds: antiproliferative and antimetastatic potential; evaluation of inflammatory pathways on cancer onset; xenobiotics effects on human cells
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

This is a continued collection of the hot topic of Metal-Based Complexes in Cancer. We already have done a successful special issue which received interesting contributions and discussions: https://www.mdpi.com/journal/ijms/special_issues/metal_based_complexes.

Metal-based drugs have attracted growing interest in biomedicine due to their potential value for both therapeutic and diagnostic applications in different diseases, especially in cancer.

Metal-based complexes are endowed with an impressive chemical diversity and versatility, depending on the metal of choice, its oxidation state, the number and type of coordinating ligands, and specific magnetic and/or optical properties.

This Special Issue of the International Journal of Molecular Sciences will include both regular articles and reviews focused on the most recent advances in metal-based complexes used in cancer therapy and diagnostics.

Contributions dealing with the design, synthesis, and characterization of novel metal-based compounds with biological activities, their mechanism of action, and innovative metal-based drug delivery systems are particularly welcome.

Topics of interest for this Special Issue include, but are not limited to, the following:

  • chemistry of metal-based anticancer drugs;
  • synthesis/improvement of metal-based complexes;
  • identification of the mechanism of action/biological targets;
  • interactions of metal-based complexes with proteins and/or nucleic acids;
  • uptake, toxicity, and resistance of metal-based anticancer agents;
  • metal-based complexes in targeted drug delivery systems;
  • metal-based drugs in cancer combinatorial therapy.

Dr. Claudia Riccardi
Dr. Marialuisa Piccolo
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. International Journal of Molecular Sciences is an international peer-reviewed open access semimonthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. There is an Article Processing Charge (APC) for publication in this open access journal. For details about the APC please see here. 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-based drugs
  • metal-based drug delivery systems
  • metal–protein interactions
  • metal–nucleic acid interactions
  • mechanism of action
  • anticancer activity

Published Papers (7 papers)

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Research

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17 pages, 3672 KiB  
Article
Impact of Conventional and Potential New Metal-Based Drugs on Lipid Metabolism in Osteosarcoma MG-63 Cells
by Daniela S. C. Bispo, Marlene Correia, Tatiana J. Carneiro, Ana S. Martins, Aliana A. N. Reis, Ana L. M. Batista de Carvalho, Maria P. M. Marques and Ana M. Gil
Int. J. Mol. Sci. 2023, 24(24), 17556; https://doi.org/10.3390/ijms242417556 - 16 Dec 2023
Cited by 1 | Viewed by 780
Abstract
This work investigated the mechanisms of action of conventional drugs, cisplatin and oxaliplatin, and the potentially less deleterious drug Pd2Spermine (Spm) and its Pt(II) analog, against osteosarcoma MG-63 cells, using nuclear-magnetic-resonance metabolomics of the cellular lipidome. The Pt(II) chelates induced different [...] Read more.
This work investigated the mechanisms of action of conventional drugs, cisplatin and oxaliplatin, and the potentially less deleterious drug Pd2Spermine (Spm) and its Pt(II) analog, against osteosarcoma MG-63 cells, using nuclear-magnetic-resonance metabolomics of the cellular lipidome. The Pt(II) chelates induced different responses, namely regarding polyunsaturated-fatty-acids (increased upon cisplatin), suggesting that cisplatin-treated cells have higher membrane fluidity/permeability, thus facilitating cell entry and justifying higher cytotoxicity. Both conventional drugs significantly increased triglyceride levels, while Pt2Spm maintained control levels; this may reflect enhanced apoptotic behavior for conventional drugs, but not for Pt2Spm. Compared to Pt2Spm, the more cytotoxic Pd2Spm (IC50 comparable to cisplatin) induced a distinct phospholipids profile, possibly reflecting enhanced de novo biosynthesis to modulate membrane fluidity and drug-accessibility to cells, similarly to cisplatin. However, Pd2Spm differed from cisplatin in that cells had equivalent (low) levels of triglycerides as Pt2Spm, suggesting the absence/low extent of apoptosis. Our results suggest that Pd2Spm acts on MG-63 cells mainly through adaptation of cell membrane fluidity, whereas cisplatin seems to couple a similar effect with typical signs of apoptosis. These results were discussed in articulation with reported polar metabolome adaptations, building on the insight of these drugs’ mechanisms, and particularly of Pd2Spm as a possible cisplatin substitute. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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27 pages, 4279 KiB  
Article
Synthesis, Structural Characterization, Cytotoxicity, and Protein/DNA Binding Properties of Pyridoxylidene-Aminoguanidine-Metal (Fe, Co, Zn, Cu) Complexes
by Violeta Jevtovic, Munirah Sulaiman Othman Alhar, Dejan Milenković, Zoran Marković, Jasmina Dimitrić Marković and Dušan Dimić
Int. J. Mol. Sci. 2023, 24(19), 14745; https://doi.org/10.3390/ijms241914745 - 29 Sep 2023
Cited by 5 | Viewed by 856
Abstract
Pyridoxylidene-aminoguanidine (PLAG) and its transition metal complexes are biologically active compounds with interesting properties. In this contribution, three new metal-PLAG complexes, Zn(PLAG)(SO4)(H2O)].∙H2O (Zn-PLAG), [Co(PLAG)2]SO4∙2H2O (Co-PLAG), and [Fe(PLAG)2]SO4∙2H [...] Read more.
Pyridoxylidene-aminoguanidine (PLAG) and its transition metal complexes are biologically active compounds with interesting properties. In this contribution, three new metal-PLAG complexes, Zn(PLAG)(SO4)(H2O)].∙H2O (Zn-PLAG), [Co(PLAG)2]SO4∙2H2O (Co-PLAG), and [Fe(PLAG)2]SO4∙2H2O) (Fe-PLAG), were synthetized and characterized by the X-ray crystallography. The intermolecular interactions governing the stability of crystal structure were compared to those of Cu(PLAG)(NCS)2 (Cu-PLAG) within Hirshfeld surface analysis. The structures were optimized at B3LYP/6-31+G(d,p)(H,C,N,O,S)/LanL2DZ (Fe,Co,Zn,Cu), and stability was assessed through Natural Bond Orbital Theory and Quantum Theory of Atoms in Molecules. Special emphasis was put on investigating the ligand’s stability and reactivity. The binding of these compounds to Bovine and Human serum albumin was investigated by spectrofluorometric titration. The importance of complex geometry and various ligands for protein binding was shown. These results were complemented by the molecular docking study to elucidate the most important interactions. The thermodynamic parameters of the binding process were determined. The binding to DNA, as one of the main pathways in the cell death cycle, was analyzed by molecular docking. The cytotoxicity was determined towards HCT116, A375, MCF-7, and A2780 cell lines. The most active compound was Cu-PLAG due to the presence of PLAG and two thiocyanate ligands. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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24 pages, 8875 KiB  
Article
The Effect of Metal Ions (Fe, Co, Ni, and Cu) on the Molecular-Structural, Protein Binding, and Cytotoxic Properties of Metal Pyridoxal-Thiosemicarbazone Complexes
by Violeta Jevtovic, Asma K. Alshamari, Dejan Milenković, Jasmina Dimitrić Marković, Zoran Marković and Dušan Dimić
Int. J. Mol. Sci. 2023, 24(15), 11910; https://doi.org/10.3390/ijms241511910 - 25 Jul 2023
Cited by 13 | Viewed by 1744
Abstract
Thiosemicarbazones and their transition metal complexes are biologically active compounds and anticancer agents with versatile structural properties. In this contribution, the structural features and stability of four pyridoxal-thiosemicarbazone (PLTSC) complexes with Fe, Co, Ni, and Cu were investigated using the density functional theory [...] Read more.
Thiosemicarbazones and their transition metal complexes are biologically active compounds and anticancer agents with versatile structural properties. In this contribution, the structural features and stability of four pyridoxal-thiosemicarbazone (PLTSC) complexes with Fe, Co, Ni, and Cu were investigated using the density functional theory and natural bond orbital approach. Special emphasis was placed on the analysis of the donor atom−metal interactions. The geometry of compounds and crystallographic structures were further examined by Hirshfeld surface analysis, and the main intermolecular interactions were outlined. It has been shown that the geometry and the number of PLTSC units in the structure determine the type and contribution of the specific interactions. The binding of all four complexes to bovine and human serum albumin was investigated through spectrofluorometric titration. The dependency of the thermodynamic parameters on the present metal ion and geometry was explained by the possible interactions through molecular docking simulations. The binding of complexes to DNA, as one of the possible ways the compounds could induce cell death, was examined by molecular docking. The cytotoxicity was measured towards HCT116, A375, MCF-7, A2780, and MCF5 cell lines, with Cu-PLTSC being the most active, as it had the highest affinity towards DNA and proteins. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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22 pages, 3915 KiB  
Article
Triple Negative Breast Cancer Preclinical Therapeutic Management by a Cationic Ruthenium-Based Nucleolipid Nanosystem
by Maria Grazia Ferraro, Marco Bocchetti, Claudia Riccardi, Marco Trifuoggi, Luigi Paduano, Daniela Montesarchio, Gabriella Misso, Rita Santamaria, Marialuisa Piccolo and Carlo Irace
Int. J. Mol. Sci. 2023, 24(7), 6473; https://doi.org/10.3390/ijms24076473 - 30 Mar 2023
Cited by 3 | Viewed by 1748
Abstract
Based on compelling preclinical evidence concerning the progress of our novel ruthenium-based metallotherapeutics, we are focusing research efforts on challenging indications for the treatment of invasive neoplasms such as the triple-negative breast cancer (TNBC). This malignancy mainly afflicts younger women, who are black, [...] Read more.
Based on compelling preclinical evidence concerning the progress of our novel ruthenium-based metallotherapeutics, we are focusing research efforts on challenging indications for the treatment of invasive neoplasms such as the triple-negative breast cancer (TNBC). This malignancy mainly afflicts younger women, who are black, or who have a BRCA1 mutation. Because of faster growing and spreading, TNBC differs from other invasive breast cancers having fewer treatment options and worse prognosis, where existing therapies are mostly ineffective, resulting in a large unmet biomedical need. In this context, we benefited from an experimental model of TNBC both in vitro and in vivo to explore the effects of a biocompatible cationic liposomal nanoformulation, named HoThyRu/DOTAP, able to effectively deliver the antiproliferative ruthenium(III) complex AziRu, thus resulting in a prospective candidate drug. As part of the multitargeting mechanisms featuring metal-based therapeutics other than platinum-containing agents, we herein validate the potential of HoThyRu/DOTAP liposomes to act as a multimodal anticancer agent through inhibition of TNBC cell growth and proliferation, as well as migration and invasion. The here-obtained preclinical findings suggest a potential targeting of the complex pathways network controlling invasive and migratory cancer phenotypes. Overall, in the field of alternative chemotherapy to platinum-based drugs, these outcomes suggest prospective brand-new settings for the nanostructured AziRu complex to get promising goals for the treatment of metastatic TNBC. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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19 pages, 2666 KiB  
Article
Development of Novel Pt(IV)-Carbohydrate Derivatives as Targeted Anticancer Agents against Osteosarcoma
by Eoin Moynihan, Silvia Panseri, Giada Bassi, Arianna Rossi, Elisabetta Campodoni, Eithne Dempsey, Monica Montesi, Trinidad Velasco-Torrijos and Diego Montagner
Int. J. Mol. Sci. 2023, 24(7), 6028; https://doi.org/10.3390/ijms24076028 - 23 Mar 2023
Cited by 2 | Viewed by 1722
Abstract
Despite the enormous importance of cisplatin as a chemotherapeutic agent, its application is impacted by dose-limiting side effects and lack of selectivity for cancer cells. Researchers can overcome these issues by taking advantage of the pro-drug nature of the platinum(IV) oxidation state, and [...] Read more.
Despite the enormous importance of cisplatin as a chemotherapeutic agent, its application is impacted by dose-limiting side effects and lack of selectivity for cancer cells. Researchers can overcome these issues by taking advantage of the pro-drug nature of the platinum(IV) oxidation state, and by modifying the coordination sphere of the metal centre with specific vectors whose receptors are overexpressed in tumour cell membranes (e.g., carbohydrates). In this paper we report the synthesis of four novel carbohydrate-modified Pt(IV) pro-drugs, based on the cisplatin scaffold, and their biological activity against osteosarcoma (OS), a malignant tumour which is most common in adolescents and young adults. The carbohydrate-targeting vectors and Pt scaffold are linked using copper-catalysed azide–alkyne cycloaddition (CuAAC) chemistry, which is synonymous with mild and robust reaction conditions. The novel complexes are characterised using multinuclear 1D-2D NMR (1H, 13C and 195Pt), IR, HR-MS, Elem. Analyses, and CV. Cytotoxicity on 2D and 3D and cell morphology studies on OS cell lines, as well as non-cancerous human foetal osteoblasts (hFOBs), are discussed. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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20 pages, 2268 KiB  
Article
Synthesis, Characterization and Biological Investigation of the Platinum(IV) Tolfenamato Prodrug–Resolving Cisplatin-Resistance in Ovarian Carcinoma Cell Lines
by Marie-Christin Barth, Norman Häfner, Ingo B. Runnebaum and Wolfgang Weigand
Int. J. Mol. Sci. 2023, 24(6), 5718; https://doi.org/10.3390/ijms24065718 - 16 Mar 2023
Cited by 3 | Viewed by 1583
Abstract
The research on the anticancer potential of platinum(IV) complexes represents one strategy to circumvent the deficits of approved platinum(II) drugs. Regarding the role of inflammation during carcinogenesis, the effects of non-steroidal anti-inflammatory drug (NSAID) ligands on the cytotoxicity of platinum(IV) complexes is of [...] Read more.
The research on the anticancer potential of platinum(IV) complexes represents one strategy to circumvent the deficits of approved platinum(II) drugs. Regarding the role of inflammation during carcinogenesis, the effects of non-steroidal anti-inflammatory drug (NSAID) ligands on the cytotoxicity of platinum(IV) complexes is of special interest. The synthesis of cisplatin- and oxaliplatin-based platinum(IV) complexes with four different NSAID ligands is presented in this work. Nine platinum(IV) complexes were synthesized and characterized by use of nuclear magnetic resonance (NMR) spectroscopy (1H, 13C, 195Pt, 19F), high-resolution mass spectrometry, and elemental analysis. The cytotoxic activity of eight compounds was evaluated for two isogenic pairs of cisplatin-sensitive and -resistant ovarian carcinoma cell lines. Platinum(IV) fenamato complexes with a cisplatin core showed especially high in vitro cytotoxicity against the tested cell lines. The most promising complex, 7, was further analyzed for its stability in different buffer solutions and behavior in cell cycle and cell death experiments. Compound 7 induces a strong cytostatic effect and cell line-dependent early apoptotic or late necrotic cell death processes. Gene expression analysis suggests that compound 7 acts through a stress-response pathway integrating p21, CHOP, and ATF3. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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Review

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32 pages, 2358 KiB  
Review
The Lung Microbiome in COPD and Lung Cancer: Exploring the Potential of Metal-Based Drugs
by Megan O’Shaughnessy, Orla Sheils and Anne-Marie Baird
Int. J. Mol. Sci. 2023, 24(15), 12296; https://doi.org/10.3390/ijms241512296 - 01 Aug 2023
Cited by 5 | Viewed by 2345
Abstract
Chronic obstructive pulmonary disease (COPD) and lung cancer 17 are two of the most prevalent and debilitating respiratory diseases worldwide, both associated with high morbidity and mortality rates. As major global health concerns, they impose a substantial burden on patients, healthcare systems, and [...] Read more.
Chronic obstructive pulmonary disease (COPD) and lung cancer 17 are two of the most prevalent and debilitating respiratory diseases worldwide, both associated with high morbidity and mortality rates. As major global health concerns, they impose a substantial burden on patients, healthcare systems, and society at large. Despite their distinct aetiologies, lung cancer and COPD share common risk factors, clinical features, and pathological pathways, which have spurred increasing research interest in their co-occurrence. One area of particular interest is the role of the lung microbiome in the development and progression of these diseases, including the transition from COPD to lung cancer. Exploring novel therapeutic strategies, such as metal-based drugs, offers a potential avenue for targeting the microbiome in these diseases to improve patient outcomes. This review aims to provide an overview of the current understanding of the lung microbiome, with a particular emphasis on COPD and lung cancer, and to discuss the potential of metal-based drugs as a therapeutic strategy for these conditions, specifically concerning targeting the microbiome. Full article
(This article belongs to the Special Issue Metal-Based Complexes in Cancer 2.0)
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