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Transition Metal Complexes and Their Applications
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Transition Metal Complexes and Their Applications

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Smart Materials".

Deadline for manuscript submissions: closed (20 November 2022) | Viewed by 22160

Special Issue Editor

Prof. Dr. Piotr Smoleński

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Guest Editor
Faculty of Chemistry, University of Wrocław, Wrocław, Poland
Interests: coordination and supramolecular chemistry; catalysis in aqueous (aqueous/organic) media; photocatalysis; crystal engineering for synthesis and characterization of MOF’s and CP’s; luminescent properties; reversible sensors; antiviral, antimicrobial and antitumor properties; synthesis a new water-soluble ligands
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Since the Nobel Prize in Chemistry for Swiss scientist Alfred Werner in 1913, coordination compounds have developed to an important class of new materials which are engaged in biomedical and catalytic applications and in many other areas. For this Special Issue, we are interested in original research papers covering the novel synthetic methods of coordination compounds and coordination polymers, including frequently used strategies for the molecular design, the important conditions of syntheses that have influences on the self-assembly and crystallization, as well as solvothermal reactions for coordination compounds, especially coordination polymers (CPs) and metal–organic frameworks (MOFs). An important advantage of this type of compounds is their rich applications. Therefore, for this Special Issue, we welcome contributions related to the potential applications of the transition–metal complexes in catalysis, molecular recognition and sensing, host–guest chemistry, electrical, biomedical applications, and as luminescent and magnetic materials.                                                                                       

Prof. Piotr Smoleński
Guest Editor

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Keywords

  • transition–metal complex
  • coordination polymer
  • metal–organic framework
  • crystal engineering
  • catalysis
  • biological activity
  • medical diagnostics
  • molecular recognition and sensing
  • composites
  • luminescent activity
  • magnetic properties

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Published Papers (8 papers)

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Research

15 pages, 2546 KiB  
Article
Trigonally Distorted Hexacoordinate Co(II) Single-Ion Magnets
by Ivan Nemec, Ondřej F. Fellner, Berenika Indruchová and Radovan Herchel
Materials 2022, 15(3), 1064; https://doi.org/10.3390/ma15031064 - 29 Jan 2022
Cited by 11 | Viewed by 2900
Abstract
By simple reactions involving various cobalt(II) carboxylates (acetate and in situ prepared pivalate and 4-hydroxybenzoate salts) and neocuproine (neo), we were able to prepare three different carboxylate complexes with the general formula [Co(neo)(RCOO)2] (R = –CH3 for 1, (CH [...] Read more.
By simple reactions involving various cobalt(II) carboxylates (acetate and in situ prepared pivalate and 4-hydroxybenzoate salts) and neocuproine (neo), we were able to prepare three different carboxylate complexes with the general formula [Co(neo)(RCOO)2] (R = –CH3 for 1, (CH3)3C– for 2, and 4OH-C4H6– for 3). The [Co(neo)(RCOO)2] molecules in the crystal structures of 1–3 adopt a rather distorted coordination environment, with the largest trigonal distortion observed for 1, whereas 2 and 3 are similarly distorted from ideal octahedral geometry. The combined theoretical and experimental investigations of magnetic properties revealed that the spin Hamiltonian formalism was not a valid approach and the L-S Hamiltonian had to be used to reveal very large magnetic anisotropies for 1–3. The measurements of AC susceptibility showed that all three compounds exhibited slow-relaxation of magnetization in a weak external static magnetic field, and thus can be classified as field-induced single-ion magnets. It is noteworthy that 1 also exhibits a weak AC signal in a zero-external magnetic field. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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29 pages, 17106 KiB  
Article
Copper(II) Perfluorinated Carboxylate Complexes with Small Aliphatic Amines as Universal Precursors for Nanomaterial Fabrication
by Iwona B. Szymańska, Katarzyna Madajska, Aleksandra Butrymowicz and Magdalena Barwiołek
Materials 2021, 14(23), 7451; https://doi.org/10.3390/ma14237451 - 4 Dec 2021
Cited by 4 | Viewed by 2565
Abstract
Copper(II) carboxylate compounds with ethylamine and isopropylamine of the general formula [Cu2(RNH2)2(µ-O2CRf)4], where R = Et, iPr, and Rf = CnF2n+1, n = 1–6, were [...] Read more.
Copper(II) carboxylate compounds with ethylamine and isopropylamine of the general formula [Cu2(RNH2)2(µ-O2CRf)4], where R = Et, iPr, and Rf = CnF2n+1, n = 1–6, were characterised in the condensed and gas phases by electron impact mass spectrometry (EI MS), IR spectroscopy, and thermal analysis. A mass spectra analysis confirmed the presence of metallated species in the gas phase. Among the observed fragments, the pseudomolecular ions [Cu2(RNH2)2(µ-O2CRf)3]+ were found, which suggests the dimeric structure of the studied complexes with axially N-coordinated ethyl- or isopropylamine molecules and bridging perfluorinated carboxylates. TGA studies demonstrated that copper transfer to the gas phase occurs even under atmospheric pressure. The temperature range of the [Cu2(RNH2)2(µ-O2CRf)4] and other copper carriers detection, observed in variable temperature infrared spectra, depends on the type of amine. The possible mechanisms of the decomposition of the tested compounds are proposed. The copper films were produced without additional reducing agents despite using Cu(II) CVD precursors in the chemical vapor deposition experiments. The layers of the gel-like complexes were fabricated in both spin- and dip-coating experiments, resulting in copper or copper oxide materials when heated. Dinuclear copper(II) carboxylate complexes with ethyl- and isopropylamine [Cu2(RNH2)2(µ-O2CRf)4] can be applied for the formation of metal or metal oxide materials, also in the nanoscale, by vapour and ‘wet’ deposition methods. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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9 pages, 1412 KiB  
Article
Unprecedented Use of NHC Gold (I) Complexes as Catalysts for the Selective Oxidation of Ethane to Acetic Acid
by Ana P. C. Ribeiro, Inês A. S. Matias, Poorya Zargaran, A. Stephen K. Hashmi and Luísa M. D. R. S. Martins
Materials 2021, 14(15), 4294; https://doi.org/10.3390/ma14154294 - 31 Jul 2021
Cited by 5 | Viewed by 2225
Abstract
The highly efficient eco-friendly synthesis of acetic acid (40% yield) directly from ethane is achieved by the unprecedented use of N-heterocyclic carbene (NHC) and N-heterocyclic oxo-carbene (NHOC) gold(I) catalysts in mild conditions. This is a selective and promising protocol to generate directly acetic [...] Read more.
The highly efficient eco-friendly synthesis of acetic acid (40% yield) directly from ethane is achieved by the unprecedented use of N-heterocyclic carbene (NHC) and N-heterocyclic oxo-carbene (NHOC) gold(I) catalysts in mild conditions. This is a selective and promising protocol to generate directly acetic acid from ethane, in comparison with the two most used methods: (i) the three-step, capital- and energy-intensive process based on the high-temperature conversion of methane to acetic acid; (ii) the current industrial methanol carbonylation processes, based in iridium and expensive rhodium catalysts. Green metrics determinations highlight the environmental advantages of the new ethane oxidation procedure. Comparison with previous reported published catalysts is performed to highlight the features of this remarkable protocol. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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24 pages, 6903 KiB  
Article
New Volatile Perfluorinated Amidine–Carboxylate Copper(II) Complexes as Promising Precursors in CVD and FEBID Methods
by Katarzyna Madajska and Iwona Barbara Szymańska
Materials 2021, 14(12), 3145; https://doi.org/10.3390/ma14123145 - 8 Jun 2021
Cited by 3 | Viewed by 3101
Abstract
In the present study, we have synthesised and characterised newly copper(II) complexes with the general formula [Cu2(NH2(NH=)CC2F5)2(µ–O2CRF)4], where RF = CF3, C2F [...] Read more.
In the present study, we have synthesised and characterised newly copper(II) complexes with the general formula [Cu2(NH2(NH=)CC2F5)2(µ–O2CRF)4], where RF = CF3, C2F5, C3F7, C4F9. Infrared spectroscopy, mass spectrometry with electron ionisation (EI MS), and density-functional theory (DFT) calculations were used to confirm compounds’ composition and structure. The volatility of the compounds was studied using thermal analysis (TGA), EI MS mass spectrometry, variable temperature infrared spectroscopy (VT IR), and sublimation experiments. Research has revealed that these compounds are the source of metal carriers in the gas phase. The thermal decomposition mechanism over reduced pressure was proposed. TGA studies demonstrated that copper transfer to the gaseous phase occurs even at atmospheric pressure. Two selected complexes [Cu2(NH2(NH=)CC2F5)2(µ–O2CC2F5)4] and [Cu2(NH2(NH=)CC2F5)2(µ–O2CC3F7)4] were successful used as chemical vapour deposition precursors. Copper films were deposited with an evaporation temperature of 393 K and 453 K, respectively, and a decomposition temperature in the range of 573–633 K without the use of hydrogen. The microscopic observations made to investigate the interaction of the [Cu2(NH2(NH=)CC2F5)2(µ–O2CC2F5)4] with the electron beam showed that the ligands are completely lost under transmission electron microscopy analysis conditions (200 keV), and the final product is copper(II) fluoride. In contrast, the beam energy in scanning electron microscopy (20 keV) was insufficient to break all coordination bonds. It was shown that the Cu-O bond is more sensitive to the electron beam than the Cu-N bond. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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19 pages, 5965 KiB  
Article
Novel H-Bonded Synthons in Copper Supramolecular Frameworks with Aminoethylpiperazine-Based Ligands. Synthesis, Structure and Catalytic Activity
by Oksana V. Nesterova, Armando J. L. Pombeiro and Dmytro S. Nesterov
Materials 2020, 13(23), 5435; https://doi.org/10.3390/ma13235435 - 29 Nov 2020
Cited by 8 | Viewed by 2037
Abstract
New Schiff base complexes [Cu2(HL1)(L1)(N3)3]∙2H2O (1) and [Cu2L2(N3)2]∙H2O (2) were synthesized. The crystal structures of 1 and [...] Read more.
New Schiff base complexes [Cu2(HL1)(L1)(N3)3]∙2H2O (1) and [Cu2L2(N3)2]∙H2O (2) were synthesized. The crystal structures of 1 and 2 were determined by single-crystal X-ray diffraction analysis. The HL1 ligand results from the condensation of salicylaldehyde and 1-(2-aminoethyl)piperazine, while a new organic ligand, H2L2, was formed by the dimerization of HL1 via a coupling of two piperazine rings of HL1 on a carbon atom coming from DMF solvent. The dinuclear building units in 1 and 2 are linked into complex supramolecular networks through hydrogen and coordination bondings, resulting in 2D and 1D architectures, respectively. Single-point and broken-symmetry DFT calculations disclosed negligible singlet–triplet splittings within the dinuclear copper fragments in 1 and 2. Catalytic studies showed a remarkable activity of 1 and 2 towards cyclohexane oxidation with H2O2 in the presence of nitric acid and pyridine as promoters and under mild conditions (yield of products up to 21%). Coordination compound 1 also acts as an active catalyst in the intermolecular coupling of cyclohexane with benzamide using di-tert-butyl peroxide (tBuOOtBu) as a terminal oxidant. Conversion of benzamide at 55% was observed after 24 h reaction time. By-product patterns and plausible reaction mechanisms are discussed. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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9 pages, 2220 KiB  
Article
Nitridated Ca2NaMg2V3O12: Eu3+ Vanadate Garnet Phosphor-in-Glass
by Damian Pasinski and Jerzy Sokolnicki
Materials 2020, 13(13), 2996; https://doi.org/10.3390/ma13132996 - 6 Jul 2020
Cited by 11 | Viewed by 2027
Abstract
In this study, Ca2NaMg2V3O12 coordination compound undoped and doped with Eu3+ obtained in the air and ammonia atmosphere by solid-state reaction was investigated. Ca2NaMg2V3O12: Eu3+ obtained [...] Read more.
In this study, Ca2NaMg2V3O12 coordination compound undoped and doped with Eu3+ obtained in the air and ammonia atmosphere by solid-state reaction was investigated. Ca2NaMg2V3O12: Eu3+ obtained in the ammonia atmosphere was then investigated as a phosphor-in-glass (PiG). Annealed Ca2NaMg2V3O12: Eu3+ phosphor forms a single phase with the cubic garnet structure and Ia3d space group. Nitridation in ammonia causes a widening of a VO43− group emission band on the low energy side and it red-shifts by 20 nm. The emission of Eu3+ is extended as compared to the non-nitridated phosphor. Ca2NaMg2V3O12: Eu3+ after nitridation shows higher emission quantum yield (QY): 49 vs. 45 and lower correlated color temperature (CCT) and 4179 vs. 4998 as compared to phosphor without nitridation. The QY for PiG is 55. The thermal stability of nitridated phosphors is superior to phosphor obtained in the air atmosphere and is further enhanced for PiG. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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16 pages, 4715 KiB  
Article
Tethering (Arene)Ru(II) Acylpyrazolones Decorated with Long Aliphatic Chains to Polystyrene Surfaces Provides Potent Antibacterial Plastics
by Corrado Di Nicola, Fabio Marchetti, Riccardo Pettinari, Alessia Tombesi, Claudio Pettinari, Iolanda Grappasonni, Paul J. Dyson and Stefania Scuri
Materials 2020, 13(3), 526; https://doi.org/10.3390/ma13030526 - 22 Jan 2020
Cited by 7 | Viewed by 2707
Abstract
The acylpyrazolone proligands HQR (HQR in general, in detail: HQCy = 1-phenyl-3-methyl-4-carbonylcyclohexyl-5-pyrazolone, 4-C(O)-phenyl, HQPh = 1-phenyl-3-methyl-4-benzoyl-5-pyrazolone, HQC17 = 1-phenyl-3-methyl-4-stearoyl-5-pyrazolone, HQC17,Ph = 1-phenyl-3-stearyl-4-benzoyl-5-pyrazolone) were synthesized and reacted with (arene)Ru(II) acceptors affording complexes [(arene)Ru(QR)Cl] (arene = cymene [...] Read more.
The acylpyrazolone proligands HQR (HQR in general, in detail: HQCy = 1-phenyl-3-methyl-4-carbonylcyclohexyl-5-pyrazolone, 4-C(O)-phenyl, HQPh = 1-phenyl-3-methyl-4-benzoyl-5-pyrazolone, HQC17 = 1-phenyl-3-methyl-4-stearoyl-5-pyrazolone, HQC17,Ph = 1-phenyl-3-stearyl-4-benzoyl-5-pyrazolone) were synthesized and reacted with (arene)Ru(II) acceptors affording complexes [(arene)Ru(QR)Cl] (arene = cymene (cym) or hexamethylbenzene (hmb)). The complexes were characterized by elemental analyses, thermogravimetric analysis-Differntial Thermal Analysis (TGA-DTA), IR spectroscopy, ESI-MS and 1H, and 13C NMR spectroscopy. Complexes [(arene)Ru(QR)Cl] where QR = QC17 and QC17,Ph, due to the long aliphatic chain in the ligand, afford nanometric dispersions in methanol via self-assembly into micellar aggregates of dimensions 50–200 nm. The antibacterial activity of the complexes was established against Escherichia coli and Staphylococcus aureus, those containing the ligands with a long aliphatic chain being the most effective. The complexes were immobilized on polystyrene by a simple procedure, and the resulting composite materials showed to be very effective against E. coli and S. aureus. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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18 pages, 1616 KiB  
Article
Pentafluorophenyl Platinum(II) Complexes of PTA and Its N-Allyl and N-Benzyl Derivatives: Synthesis, Characterization and Biological Activity
by Paolo Sgarbossa, Urszula Śliwińska-Hill, M. Fátima C. Guedes da Silva, Barbara Bażanów, Aleksandra Pawlak, Natalia Jackulak, Dominik Poradowski, Armando J. L. Pombeiro and Piotr Smoleński
Materials 2019, 12(23), 3907; https://doi.org/10.3390/ma12233907 - 26 Nov 2019
Cited by 7 | Viewed by 2755
Abstract
From the well-known 1,3,5-triaza-phosphaadamantane (PTA, 1a), the novel N-allyl and N-benzyl tetrafuoroborate salts 1-allyl-1-azonia-3,5-diaza-7-phosphaadamantane (APTA(BF4), 1b) and 1-benzyl-1-azonia-3,5-diaza-7-phosphaadamantane (BzPTA(BF4), 1c) were obtained. These phosphines were then allowed to react with (Pt(μ-Cl)(C6F5)(tht))2 [...] Read more.
From the well-known 1,3,5-triaza-phosphaadamantane (PTA, 1a), the novel N-allyl and N-benzyl tetrafuoroborate salts 1-allyl-1-azonia-3,5-diaza-7-phosphaadamantane (APTA(BF4), 1b) and 1-benzyl-1-azonia-3,5-diaza-7-phosphaadamantane (BzPTA(BF4), 1c) were obtained. These phosphines were then allowed to react with (Pt(μ-Cl)(C6F5)(tht))2 (tht = tetrahydrothiophene) affording the water soluble Pt(II) complexes trans-(PtCl(C6F5)(PTA)2) (2a) and its bis-cationic congeners trans-(PtCl(C6F5)(APTA)2)(BF4)2 (2b) and trans-(PtCl(C6F5)(BzPTA)2)(BF4)2 (2c). The compounds were fully characterized by multinuclear NMR, ESI-MS, elemental analysis and (for 2a) also by single crystal X-ray diffraction, which proved the trans configuration of the phosphine ligands. Furthermore, in order to evaluate the cytotoxic activities of all complexes the normal human dermal fibroblast (NHDF) cell culture were used. The antineoplastic activity of the investigated compounds was checked against the human lung carcinoma (A549), epithelioid cervix carcinoma (HeLa) and breast adenocarcinoma (MCF-7) cell cultures. Interactions between the complexes and human serum albumin (HSA) using fluorescence spectroscopy and circular dichroism spectroscopy (CD) were also investigated. Full article
(This article belongs to the Special Issue Transition Metal Complexes and Their Applications)
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