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Advances in Coordination Chemistry 2.0

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

Deadline for manuscript submissions: 31 December 2024 | Viewed by 12746

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Prof. Dr. Juan Niclós-Gutiérrez

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Department of Inorganic Chemistry, Faculty of Pharmacy, University of Granada, 18071 Granada, Spain
Interests: coordination chemistry; molecular recognition; metal complexes with purine nucleic bases or their synthetic nucleosides; crystal growth/structure; mixed ligand-metal complexes; interligand interactions; pi-stacking; C-H/pi interactions and other weak contributions to molecular and supramolecular crystal structures; DFT-calculations

Dr. Miquel Barceló-Oliver

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Departament de Química, Universitat de les Illes Balears, Crta de Valldemossa km 7.7, 07122 Palma de Mallorca, Spain
Interests: coordination chemistry; nucleic acids; riboswitch; i-motifs; crystallography; isothermal titration calorimetry; bioinorganic chemistry
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Dear Colleagues,

The use of coordination compounds dates back to prehistoric times. The earliest documented use is probably that of alizarin, hydroxyanthraquinone, a textile dye that produces a bright red colour in combination with aluminium ions [Kaufmann, G.B. Coordination Chemistry: History. In Encyclopedia of Inorganic Chemistry; Scott, R.A., Ed.; Wiley: New York; USA, 2006]. A milestone in the evolution of coordination chemistry is the revolutionary theory proposed by Alfred Werner in 1893, which laid foundations for modern coordination chemistry. Today, IUPAC defines a coordination compound as any compound that is composed of a central atom, usually that of a metal, to which is attached a surrounding array of other atoms or groups of atoms, each of which is called a ligand [IUPAC Recommendations 2005]. Active sites in many enzymes that regulate biological processes are coordination compounds, as well as many catalysts used in the transformation of organic substances. Studies of interactions between metal ions and ligands may provide insights into catalysed reactions. The field of coordination chemistry is broad, with almost each metal ion or ligand making up its own subfield. The abundant reports in recent literature show that interest in coordination chemistry remains unwaning and that focus has shifted from comprehensive theories of bonding towards the application and synthesis of compounds designed for specific use. We will dedicate this Special Issue to all aspects of coordination chemistry.

Any study related to the original or mini-review in Coordination Chemistry has a place in this Special issue. Thus the Keywords are broad suggestions, so that any contribution that fully or partially matches one or more of these suggestions will be well received.

Prof. Dr. Juan Niclós-Gutiérrez
Dr. Miquel Barceló-Oliver
Guest Editors

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Keywords

synthesis strategies for novel coordination compounds
coordination compounds with tailor-made ligands for specific applications
coordination compounds with multitopic ligands
single crystal XRD-structures and dimensionality of metal complexes
metal organic frameworks and its applications
molecular recognition in mixed-ligand metal complexes, at molecular and/or supra-molecular levels
model metal complexes from the bioinorganic frontier of biological chemistry
DFT and other theoretical approaches for interligand interactions in metal complexes

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Published Papers (12 papers)

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Research

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9 pages, 2288 KiB

Open AccessArticle

Gold/DNA-Cu²⁺ Complex Nanozyme-Based Aptamer Lateral Flow Assay for Highly Sensitive Detection of Kanamycin

by Xiuping Li, Rui Chang, Shengmei Tai, Minxin Mao and Chifang Peng

Molecules 2024, 29(19), 4569; https://doi.org/10.3390/molecules29194569 - 26 Sep 2024

Viewed by 621

Abstract

Aptamer-based lateral flow analysis (Apt-LFAs) has promising applications in many fields. Nanozymes have demonstrated high potential in improving the performance of Apt-LFAs and have been increasingly utilized in recent studies. In this study, we developed a nanozyme-based Apt-LFA for the rapid and sensitive detection of kanamycin by using a novel dual-functionalized AuNPs@polyA-DNA/GpG-Cu²⁺ nanozyme as a nanoprobe. In the nanoprobe design, the polyA-cDNA strand can discriminate a kanamycin aptamer from the kanamycin/aptamer complex, and the GpG-Cu²⁺ complex can amplify the detection signal by catalyzing the chromogenic reaction. The nanozyme Apt-LFA can quantify kanamycin in the range of 1–250 ng/mL with an LOD of 0.08 ng/mL, which demonstrated a 4-fold sensitivity improvement and had a wider linear range than the conventional AuNP-based LFA. The Apt-LFA was successfully applied to the detection of kanamycin in honey with good recoveries. Our dual-functionalized AuNP nanoprobe is easily prepared and can be highly compatible with the conventional AuNP-DNA-based LFA platform; thus, it can be extended to the application of Apt-LFAs for other small molecules. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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18 pages, 3884 KiB

Open AccessArticle

Towards Nickel–NHC Fluoro Complexes—Synthesis of Imidazolium Fluorides and Their Reactions with Nickelocene

by Siobhan S. Wills, Corinne Bailly and Michael J. Chetcuti

Molecules 2024, 29(18), 4493; https://doi.org/10.3390/molecules29184493 - 21 Sep 2024

Viewed by 877

Abstract

While hundreds of complexes of the general formula [Ni(η⁵-C₅H₅)(NHC)(X)] exist (NHC = a N-heterocyclic carbene, X = Cl, Br, I), none is yet known with X = F. We attempted to prepare such a species by reacting nickelocene with imidazolium fluorides. Three imidazolium fluorides (ImH)⁺ F⁻ [Im = (N,N′-bis-(R)-imidazolium: 1a, IMe, R = Me; 1b, IMes, R = 2,4,6-trimethylphenyl; 1c, IPr, R = 2,6-diisopropylphenyl)] were prepared and characterized by spectroscopic methods. In addition, the salts 1b [(IMesH)⁺ F⁻] and 1c [(IPrH)⁺ F⁻] were subjected single-crystal X-ray diffraction experiments. The reactions of these imidazolium fluorides with nickelocene did not lead to [Ni(η⁵-C₅H₅)(NHC)(F)] species. Instead, the reaction of 1a [(IMeH)⁺ F⁻] and 1b [(IMesH)⁺ F⁻] with nickelocene led to the salt 2 [Ni(η⁵-C₅H₅)(IMe)₂]⁺ F⁻ and to the square planar complex 3atrans-[NiF₂(IMes)₂] respectively. Both complexes were characterized spectroscopically and by single crystal X-ray diffraction. All four X-ray diffraction studies reveal hydrogen bonding and hydrogen interactions with the F atom or anion, and in some cases with solvent molecules of crystallization, and these phenomena are all discussed. Complex 2, in particular, exhibited a wide range of interesting H-bonded interactions in the solid state. Complexes 2 and 3a were tested as catalysts for Suzuki–Miyaura coupling but were not promising: complex 2 was inactive, and while 3a did indeed catalyze the reaction, it gave widely diverging results owing to its instability in solution. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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12 pages, 10424 KiB

Open AccessArticle

Structural and Magnetic Properties of Dimeric Capsule Assemblies Formed by Cyclic Trinuclear Complexes

by Masahiro Muto, Kousuke Morinaga, Momoko Nishihashi, Yasunori Yamada and Masayuki Koikawa

Molecules 2024, 29(18), 4307; https://doi.org/10.3390/molecules29184307 - 11 Sep 2024

Viewed by 524

Abstract

Cyclic trinuclear homo-metal complexes, [{Fe(L³⁺²Br)py}₃] (1) and [{Mn(L³⁺²Br)}₃(py)₂ MeOH] (2), along with a hetero-metal complex, [FeMn₂(L³⁺²H)₃(DMF)₃] (3), were synthesized using asymmetric ditopic ligands (H₃L³⁺²H: 2-(2-hydroxyphenyl)-6-ol-5-(salicylideneamino)benzoxazole, H₃L³⁺²Br: 2-(2-hydrox-5-bromoyphenyl)-6-ol-5-(5-bromosalicylideneamino)benzoxazole). The molecular structure of 1 is characterized by a tripod structure with three-fold symmetry, where an enantiomer pair forms a dimeric capsule with dimensions of approximately 3 × 1.6 × 1.6 nm³. Complexes 2 and 3, which lack three-fold symmetry, exhibit similar molecular structures to previously reported complexes with these ligands, but do not form a capsule structure. Magnetic measurements of 1–3 reveal the presence of significantly weak antiferromagnetic interactions between the metal ions. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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11 pages, 2752 KiB

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Determination of Dipicolinic Acid through the Antenna Effect of Eu(III) Coordination Polymer

by Jing Li, Yu Liang, Chun Tian, Hongyan Zou, Lei Zhan, Lijuan Wang, Chengzhi Huang and Chunmei Li

Molecules 2024, 29(17), 4259; https://doi.org/10.3390/molecules29174259 - 8 Sep 2024

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Abstract

Bacillus anthracis is a Gram-positive bacterium that can cause acute infection and anthracnose, which is a serious concern for human health. Determining Bacillus anthracis through its spore biomarker dipicolinic acid (DPA) is crucial, and there is a strong need for a method that is rapid, sensitive, and selective. Here, we created Eu(III)-coordination polymers (Eu-CPs) with surfaces that have abundant carboxyl and hydroxyl groups. This was achieved by using citric acid and europium nitrate hexahydrate as precursors in a straightforward one-pot hydrothermal process. These Eu-CPs were then successfully utilized for highly sensitive DPA determination. The fluorescence (FL) emission of Eu-CPs, which is typically weak due to the coordination of Eu(III) with water molecules, was significantly enhanced in the presence of DPA. This enhancement is attributed to the competitive binding between DPA’s carboxyl or hydroxyl groups and water molecules. As a result, the absorbed energy of DPA, when excited by 280 nm ultraviolet light, is transferred to Eu-CPs through an antenna effect. This leads to the emission of the characteristic red fluorescence of Eu³⁺ at 618 nm. A strong linear relationship was observed between the enhanced FL intensity and DPA concentration in the range of 0.5–80 μM. This relationship allowed for a limit of detection (LOD) of 15.23 nM. Furthermore, the Eu-CPs we constructed can effectively monitor the release of DPA from Bacillus subtilis spores, thereby further demonstrating the potential significance of this strategy in the monitoring and management of anthrax risk. This highlights the novelty of this approach in practical applications, provides a valuable determination technique for Bacillus anthracis, and offers insights into the development cycle of microorganisms. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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22 pages, 7074 KiB

Open AccessArticle

Characterization and Cytotoxic Assessment of Bis(2-hydroxy-3-carboxyphenyl)methane and Its Nickel(II) Complex

by Ayman H. Ahmed, Ibrahim O. Althobaiti, Ebtsam K. Alenezy, Yazeed M. Asiri, Sobhy Ghalab and Omar A. Hussein

Molecules 2024, 29(17), 4239; https://doi.org/10.3390/molecules29174239 - 6 Sep 2024

Viewed by 651

Abstract

A condensation reaction of salicylic acid with formaldehyde in the presence of sulfuric acid led to the synthesization of the bis(2-hydroxy-3-carboxyphenyl)methane (BHCM) ligand, which was subsequently allowed to bind with nickel (II) ions. In light of the information obtained from the elemental analyses (C, H, and M), spectral (IR, MS, ¹H-NMR, and UV–Vis) and thermal and magnetic measurements, the most likely structures of the ligand and complex have been identified. It has been suggested that the BHCM coordinates in a tetradentate manner with two Ni(II) ions to produce an octahedral binuclear complex. The SEM and TEM morphology of the compounds showed spherical shapes. An X-ray diffraction analysis indicated a considerable difference in the diffraction patterns between BHCM (crystalline) and Ni–BHCM (amorphous), and the Scherrer equation was used to calculate the crystallite size. Some optical characteristics were estimated from UV–Vis spectra. The ligand and its nickel(II) complex underlie the range of semiconductors. It was verified that for human lung (A-549) cancer, the BHCM compound displayed a significant barrier to the proliferation test in noncancerous cells (human lung fibroblasts, WI-38), which was also undertaken. To demonstrate the binding affinities of the chosen compounds (BHCM and Ni–BHCM) in the receptor protein’s active site [PDB ID: 5CAO], a molecular docking (MD) study was carried out. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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14 pages, 5203 KiB

Open AccessArticle

Synthesis and Electrochemical Study of Gold(I) Carbene Complexes

by Andrea Rodríguez-Rubio, Álvaro Yuste, Tomás Torroba, Gabriel García-Herbosa and José V. Cuevas-Vicario

Molecules 2024, 29(17), 4081; https://doi.org/10.3390/molecules29174081 - 28 Aug 2024

Viewed by 550

Abstract

In this work, we have prepared and characterized some gold compounds wearing a N-heterocyclic carbene (NHC) ligand as well as alkynyl derivatives with different substituents. The study of their electrochemical behavior reveals that these complexes show an irreversible wave at potentials ranging between −2.79 and −2.91 V, referenced to the ferrocenium/ferrocene pair. DFT calculations indicate that the reduction occurs mainly on the aryl−C≡C fragment. The cyclic voltammetry experiments under CO₂ atmosphere show an increase in the faradaic current of the reduction wave compared to the experiments under argon atmosphere, indicating a possible catalytic activity towards the carbon dioxide reduction reaction (CO₂RR). Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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13 pages, 7253 KiB

Open AccessArticle

Synthesis and Characterization of Transition Metal Complexes Supported by Phosphorus Ligands Obtained Using Hydrophosphination of Cyclic Internal Alkenes

by Victoria Mechrouk, Damien Bissessar, Julien Egly, Jordan Parmentier and Stéphane Bellemin-Laponnaz

Molecules 2024, 29(16), 3946; https://doi.org/10.3390/molecules29163946 - 21 Aug 2024

Viewed by 680

Abstract

The design and study of rich, bulky phosphorus ligands is a key area of research for homogeneous catalysis. Here, we describe an original strategy using a hydrophosphination reaction to produce phosphines of interest for coordination chemistry and homogenous catalysis. In particular, the phosphine obtained by reacting diphenylphosphine with acenaphthylene (ligand 2) gives a ligand that adopts an unusual spatial geometry. The coordination chemistry of the ligand has been investigated with Au(I), Ag(I), Cu(I), and Pd(II), for which a complete characterization could be made, particularly in X-ray diffraction studies. The reactivity of some of these complexes has been demonstrated, particularly in Pd-catalyzed cross-coupling reactions and Au-catalyzed hydroaminations and in the hydration of alkynes. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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17 pages, 6243 KiB

Open AccessArticle

Influence of Diluent on Extraction Parameters of Systems for Separation Am(III) and Ln(III) Based on 1,10-Phenanthroline-2,9-Diamide

by Mikhail A. Gerasimov, Petr I. Matveev, Mariia V. Evsiunina, Enni. K. Khult, Paulina Kalle, Valentine S. Petrov, Pavel S. Lemport, Vladimir G. Petrov, Galina V. Kostikova, Yuri A. Ustynyuk and Valentine G. Nenajdenko

Molecules 2024, 29(15), 3548; https://doi.org/10.3390/molecules29153548 - 28 Jul 2024

Viewed by 1210

Abstract

A systematic study of extraction systems for the separation of f-elements using the tetradentate N,O-donor diamide of 1,10-phenanthroline-2,9-dicarboxylic acid (L) in various molecular and ionic solvents was performed. It was demonstrated that the nature of a diluent has a significant impact on solvent extraction of Am(III) and Ln(III) and the stoichiometry of formed complexes with f-elements. The mechanism of complexation and forms of complexes in different diluents were investigated by radiometric methods, UV-vis titration, and XRD. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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12 pages, 2335 KiB

Open AccessArticle

[Fe(µ₂-OH)₆]³⁻ Linked Fe₃O Triads: Mössbauer Evidence for Trigonal µ₃-O²⁻ or µ₃-OH⁻ Groups in Bridged versus Unbridged Complexes

by D. Nirosha T. De Silva, Tyson N. Dais, Geoffrey B. Jameson, Casey G. Davies, Guy N. L. Jameson and Paul G. Plieger

Molecules 2024, 29(13), 3218; https://doi.org/10.3390/molecules29133218 - 7 Jul 2024

Viewed by 1139

Abstract

The syntheses, coordination chemistry, and Mössbauer spectroscopy of hepta-iron(III) complexes using derivatised salicylaldoxime ligands from two categories; namely, ‘single-headed’ (H₂L) and ‘double-headed’ (H₄L) salicylaldoximes are described. All compounds presented here share a [Fe₃-µ₃-O] core in which the iron(III) ions are µ₃-hydroxo-bridged in the complex C1 and µ₃-oxo-bridged in C2 and C3. Each compound consists of 2 × [Fe₃-µ₃-O] triads that are linked via a central [Fe(µ₂-OH)₆]³⁻ ion. In addition to the charge balance and microanalytical evidence, Mössbauer measurements support the fact that the triads in C1 are µ₃-OH bridged and are µ₃-O bridged in C2 and C3. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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14 pages, 2936 KiB

Open AccessArticle

Synthesis and Performance of Deep-Red Phosphorescent Iridium Complexes with Pyrone as an Auxiliary Ligand

by Wen Jiang, Wenming Hou, Caixian Yan, Zhifeng Nie, Qiaowen Chang, Xiangguang Li and Weiping Liu

Molecules 2024, 29(13), 3183; https://doi.org/10.3390/molecules29133183 - 3 Jul 2024

Viewed by 962

Abstract

Two bis-cyclometalated heteroleptic iridium complexes incorporating 1-phenylisoquinoline (piq) as the main cyclometalating ligand and 3-hydroxy-2-methyl-4-pyrone (ma) or 2-ethyl-3-hydroxy-4H-pyran-4-one (ema) as the auxiliary ligand, namely Ir(piq)₂(ma) (Ir-1) and Ir(piq)₂(ema) (Ir-2), were developed and applied as deep-red phosphors in organic light-emitting diodes (OLEDs). The two auxiliary ligands had similar influences on the photophysical, electrochemical, and electroluminescent properties of the iridium complexes. Ir(piq)₂(ma) (Ir-1) showed better luminescence performance in a simple phosphorescent OLED compared to the traditional red iridium complex Ir(piq)₂(acac) and exhibited a current efficiency of 9.39 cd A⁻¹ (EQE of 12.09%). In contrast, Ir(piq)₂(ema) exhibited an efficiency of 8.6 cd A⁻¹ (EQE of 10.19%). Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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21 pages, 5458 KiB

Open AccessArticle

Synthesis, Structural Characterisation, and Electrochemical Properties of Copper(II) Complexes with Functionalized Thiosemicarbazones Derived from 5-Acetylbarbituric Acid

by Alfonso Castiñeiras, Nuria Fernández-Hermida, Isabel García-Santos, Lourdes Gómez-Rodríguez, Antonio Frontera and Juan Niclós-Gutiérrez

Molecules 2024, 29(10), 2245; https://doi.org/10.3390/molecules29102245 - 10 May 2024

Viewed by 828

Abstract

The reaction between 5-acetylbarbituric acid and 4-dimethylthiosemicarbazide or 4-hexamethyleneiminyl thiosemicarbazide produces 5-acetylbarbituric-4-dimethylthiosemicarbazone (H₂AcbDM) and 5-acetylbarbituric-4N-hexamethyleneiminyl thiosemicarbazone (H₂Acbhexim). Eight new complexes with different copper(II) salts have been prepared and characterized using elemental analysis, molar conductance, UV–Vis, ESI-HRMS, FT-IR, magnetic moment, EPR, and cyclic voltammetry. In addition, three-dimensional molecular structures of [Cu(HAcbDM)(H₂O)₂](NO₃)·H₂O (3a), [Cu(HAcbDM)(H₂O)₂]ClO₄ (4), and [Cu(HAcbHexim)Cl] (6) were determined by single crystal X-ray crystallography, and an analysis of their supramolecular structure was carried out. The H-bonded assemblies were further studied energetically using DFT calculations and MEP surface and QTAIM analyses. In these complexes, the thiosemicarbazone coordinates to the metal ion in an ONS-tridentate manner, in the O-enolate/S-thione form. The electrochemical behavior of the thiosemicarbazones and their copper(II) complexes has been investigated at room temperature using the cyclic voltammetry technique in DMFA. The Cu(II)/Cu(I) redox system was found to be consistent with the quasi-reversible diffusion-controlled process. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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Review

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39 pages, 3357 KiB

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Hybrid Hydroxyapatite–Metal Complex Materials Derived from Amino Acids and Nucleobases

by Alondra Jiménez-Pérez, Marta Martínez-Alonso and Javier García-Tojal

Molecules 2024, 29(18), 4479; https://doi.org/10.3390/molecules29184479 - 20 Sep 2024

Viewed by 2004

Abstract

Calcium phosphates (CaPs) and their substituted derivatives encompass a large number of compounds with a vast presence in nature that have aroused a great interest for decades. In particular, hydroxyapatite (HAp, Ca₁₀(OH)₂(PO₄)₆) is the most abundant CaP mineral and is significant in the biological world, at least in part due to being a major compound in bones and teeth. HAp exhibits excellent properties, such as safety, stability, hardness, biocompatibility, and osteoconductivity, among others. Even some of its drawbacks, such as its fragility, can be redirected thanks to another essential feature: its great versatility. This is based on the compound’s tendency to undergo substitutions of its constituent ions and to incorporate or anchor new molecules on its surface and pores. Thus, its affinity for biomolecules makes it an optimal compound for multiple applications, mainly, but not only, in biological and biomedical fields. The present review provides a chemical and structural context to explain the affinity of HAp for biomolecules such as proteins and nucleic acids to generate hybrid materials. A size-dependent criterium of increasing complexity is applied, ranging from amino acids/nucleobases to the corresponding macromolecules. The incorporation of metal ions or metal complexes into these functionalized compounds is also discussed. Full article

(This article belongs to the Special Issue Advances in Coordination Chemistry 2.0)

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