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Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi

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

Deadline for manuscript submissions: 31 July 2024 | Viewed by 13404

Special Issue Editor

Prof. Dr. Franca Morazzoni

E-Mail Website
Guest Editor
Laboratory of Inorganic and Hybrid Materials, Department of Materials Science, University of Milano-Bicocca, 20125 Milano, Italy
Interests: sensor materials; photocatalysis materials; inorganic-organic interphases; spectromagnetic characterization

Special Issue Information

Dear Colleagues,

Supramolecular chemistry is concerned with systems composed of a discrete number of molecules, held together by noncovalent interactions. Noncovalent interactions include van der Waals forces, hydrogen bonding, electrostatic effects, and metal–ligand interactions. Such interactions are characterized by different energies, varying from fractions to several tens of kcal mol-1, but possess a common feature: quick reversibility. They form and break according to fast and uncomplicated steps, which, following a trial and error mechanism, may allow the achievement of complex and sophisticated architectures. This means that noncovalent chemistry is thermodynamically controlled, whereas covalent (organic) chemistry is controlled by kinetics.

Metal–ligand interactions are especially versatile. This is firstly because metal ions represent the widest range of chemical individuals of the Periodic Table. It is no coincidence that supramolecular chemistry is conventionally considered to begin with the awarding of the Nobel Prize to Cram, Lehn, and Pedersen for their research on the novel coordination chemistry of alkali metal ions (1987); in particular, the different behavior of a homogeneous group of spherical ions, from Li+ to Cs+, promoted the design of “molecules with structure-specific interactions of high selectivity”. Soon thereafter, transition metal ions came into play, bringing their distinctive properties of color, magnetism, redox behavior, varying coordination geometry, and photophysical and photochemical activity, dramatically extending and enriching the discipline. Some of the most investigated topics include molecular switches, control of molecular motions, molecular machines and motors, transition metal directed self-assembly, anion recognition, photoinduced electron transfer sensing and switching, molecular logic, metal–organic frameworks for recognition and catalysis, supramolecular materials with photonic and/or conductor properties, and templating motifs for the formation of interpenetrated host–guest species.

Prof. Dr. Franca Morazzoni
Guest Editor

Manuscript Submission Information

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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

  • supramolecular chemistry
  • noncovalent interactions
  • metal-promoted self-assembly
  • molecular recognition
  • molecular switches

Published Papers (7 papers)

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Research

13 pages, 2587 KiB  
Article
Efficient Removal of Pb(Ⅱ) by Highly Porous Polymeric Sponges Self-Assembled from a Poly(Amic Acid)
by Ying Leng, Kai Jin, Tian Wang, Xiaoyong Lai and Hui Sun
Molecules 2023, 28(7), 2897; https://doi.org/10.3390/molecules28072897 - 23 Mar 2023
Cited by 1 | Viewed by 1119
Abstract
Lead (II) (Pb(II)) is widespread in water and very harmful to creatures, and the efficient removal of it is still challenging. Therefore, we prepared a novel sponge-like polymer-based absorbent (poly(amic acid), PAA sponge) with a highly porous structure using a straightforward polymer self-assembly [...] Read more.
Lead (II) (Pb(II)) is widespread in water and very harmful to creatures, and the efficient removal of it is still challenging. Therefore, we prepared a novel sponge-like polymer-based absorbent (poly(amic acid), PAA sponge) with a highly porous structure using a straightforward polymer self-assembly strategy for the efficient removal of Pb(II). In this study, the effects of the pH, dosage, adsorption time and concentration of Pb(II) on the adsorption behavior of the PAA sponge are investigated, revealing a rapid adsorption process with a removal efficiency up to 89.0% in 2 min. Based on the adsorption thermodynamics, the adsorption capacity increases with the concentration of Pb(II), reaching a maximum adsorption capacity of 609.7 mg g−1 according to the Langmuir simulation fitting. Furthermore, the PAA sponge can be efficiently recycled and the removal efficiency of Pb(II) is still as high as 93% after five adsorption–desorption cycles. Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy analyses reveal that the efficient adsorption of Pb(II) by the PAA sponge is mainly due to the strong interaction between nitrogen-containing functional groups and Pb(II), and the coordination of oxygen atoms is also involved. Overall, we propose a polymer self-assembly strategy to easily prepare a PAA sponge for the efficient removal of Pb(II) from water. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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12 pages, 4215 KiB  
Article
Synthesis, Crystal Structure, and Characterization of Energetic Salts Based on 3,5-Diamino-4H-Pyrazol-4-One Oxime
by Wen-Shuai Dong, Lu Zhang, Wen-Li Cao, Zu-Jia Lu, Qamar-un-Nisa Tariq, Chao Zhang, Xiao-Wei Wu, Zong-You Li and Jian-Guo Zhang
Molecules 2023, 28(1), 457; https://doi.org/10.3390/molecules28010457 - 03 Jan 2023
Cited by 2 | Viewed by 2240
Abstract
In order to broaden the study of energetic cations, a cation 3,5-diamino-4H-pyrazol-4-one oxime (DAPO) with good thermal stability was proposed, and its three salts were synthesized by a simple and efficient method. The structures of the three salts were verified by [...] Read more.
In order to broaden the study of energetic cations, a cation 3,5-diamino-4H-pyrazol-4-one oxime (DAPO) with good thermal stability was proposed, and its three salts were synthesized by a simple and efficient method. The structures of the three salts were verified by infrared spectroscopy, mass spectrometry, elemental analysis, and single crystal X-ray diffraction. The thermal stabilities of the three salts were verified by differential scanning calorimetry and thermos-gravimetric analysis. DAPO-based energetic salts are analysed using a variety of theoretical techniques, such as 2D fingerprint, Hirshfeld surface, and non-covalent interaction. Among them, the energy properties of perchlorate (DAPOP) and picrate (DAPOT) were determined by EXPLO5 program combined with the measured density and enthalpy of formation. These compounds have high density, acceptable detonation performance, good thermal stability, and satisfactory sensitivity. The intermolecular interactions of the four compounds were studied by Hirshfeld surface and non-covalent interactions, indicating that hydrogen bonds and π–π stacking interactions are the reasons for the extracellular properties of perchlorate (DAPOP) and picrate (DAPOT), indicating that DAPO is an optional nitrogen-rich cation for the design and synthesis of novel energetic materials with excellent properties. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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22 pages, 43443 KiB  
Article
From Gas Phase Observations to Solid State Reality: The Identification and Isolation of Trinuclear Salicylaldoximato Copper Complexes
by Benjamin D. Roach, Ross S. Forgan, Eduardo Kamenetzky, Simon Parsons, Paul G. Plieger, Fraser J. White, Sidney Woodhouse and Peter A. Tasker
Molecules 2022, 27(19), 6421; https://doi.org/10.3390/molecules27196421 - 29 Sep 2022
Cited by 1 | Viewed by 1207
Abstract
Conditions have been identified in which phenolic aldoximes and ketoximes of the types used in commercial solvent extraction processes can be doubly deprotonated and generate polynuclear Cu complexes with lower extractant:Cu molar ratios than those found in commercial operations. Electrospray mass spectrometry has [...] Read more.
Conditions have been identified in which phenolic aldoximes and ketoximes of the types used in commercial solvent extraction processes can be doubly deprotonated and generate polynuclear Cu complexes with lower extractant:Cu molar ratios than those found in commercial operations. Electrospray mass spectrometry has provided an insight into the solution speciation in extraction experiments and has identified conditions to allow isolation and characterization of polynuclear Cu-complexes. Elevation of pH is effective in enhancing the formation of trinuclear complexes containing planar {Cu3-μ3-O}4+ or {Cu3-μ3-OH}5+ units. DFT calculations suggest that such trinuclear complexes are more stable than other polynuclear species. Solid structures of complexes formed by a salicylaldoxime with a piperidino substituent ortho to the phenolic OH group (L9H2) contain two trinuclear units in a supramolecular assembly, {[Cu3OH(L9H)3(ClO4)](ClO4)} 2, formed by H-bonding between the central {Cu3-μ3-OH}5+ units and oxygen atoms in the ligands of an adjacent complex. Whilst the lower ligand:Cu molar ratios provide more efficient Cu-loading in solvent extraction processes, the requirement to raise the pH of the aqueous phase to achieve this will make it impractical in most commercial operations because extraction will be accompanied by the precipitation (as oxyhydroxides) of Fe(III) which is present in significant quantities in feed solutions generated by acid leaching of most Cu ores. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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13 pages, 2151 KiB  
Article
A Supramolecular Approach to Antimicrobial Surfaces
by Valentina Gazzola, Pietro Grisoli, Valeria Amendola, Giacomo Dacarro, Carlo Mangano, Piersandro Pallavicini, Antonio Poggi, Silvia Rossi, Barbara Vigani and Angelo Taglietti
Molecules 2022, 27(17), 5731; https://doi.org/10.3390/molecules27175731 - 05 Sep 2022
Viewed by 1548
Abstract
In this paper, we report on the preparation of Imidazole-functionalized glass surfaces, demonstrating the ability of a dinuclear Cu(II) complex of a macrocyclic ligand to give a “cascade” interaction with the deprotonated forms of grafted imidazole moieties. In this way, we realized a [...] Read more.
In this paper, we report on the preparation of Imidazole-functionalized glass surfaces, demonstrating the ability of a dinuclear Cu(II) complex of a macrocyclic ligand to give a “cascade” interaction with the deprotonated forms of grafted imidazole moieties. In this way, we realized a prototypal example of an antimicrobial surface based on a supramolecular approach, obtaining a neat microbicidal effect using low amounts of the described copper complex. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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20 pages, 2788 KiB  
Article
Fluorogenic Detection of Sulfite in Water by Using Copper(II) Azacyclam Complexes
by Carlo Ciarrocchi, Donatella Sacchi, Massimo Boiocchi, Maduka Lankani Weththimuni, Alessio Orbelli Biroli and Maurizio Licchelli
Molecules 2022, 27(6), 1852; https://doi.org/10.3390/molecules27061852 - 12 Mar 2022
Cited by 4 | Viewed by 2265
Abstract
Copper(II) azacyclam complexes (azacyclam = 1,3,5,8,12-pentaazacyclotetradecane) containing naphthyl or dansyl subunits can be prepared by template synthesis involving proper sulfonamide derivatives as locking fragments. The macrocyclic complexes are very poorly emissive due to the fluorescence-quenching behavior displayed by Cu2+ ions. However, the [...] Read more.
Copper(II) azacyclam complexes (azacyclam = 1,3,5,8,12-pentaazacyclotetradecane) containing naphthyl or dansyl subunits can be prepared by template synthesis involving proper sulfonamide derivatives as locking fragments. The macrocyclic complexes are very poorly emissive due to the fluorescence-quenching behavior displayed by Cu2+ ions. However, the fluorescence can be recovered as a result of the decomposition of the complexes, which induces the release of free light-emitting subunits to the solution. This reaction takes place very slowly in neutral water but its rate is increased by the presence of sulfite. Therefore, [Cu(azacyclam)]2+ derivatives have been investigated as simple chemical probes for the fluorogenic detection of sulfite both on laboratory and real samples. Preliminary tests performed on samples of white wine provided sulfite concentration values that are in agreement with those obtained by a standard analytical method. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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9 pages, 2622 KiB  
Article
Fluorogenic Detection of Human Serum Albumin Using Curcumin-Capped Mesoporous Silica Nanoparticles
by Ismael Otri, Serena Medaglia, Elena Aznar, Félix Sancenón and Ramón Martínez-Máñez
Molecules 2022, 27(3), 1133; https://doi.org/10.3390/molecules27031133 - 08 Feb 2022
Cited by 7 | Viewed by 1990
Abstract
Mesoporous silica nanoparticles loaded with rhodamine B and capped with curcumin are used for the selective and sensitive fluorogenic detection of human serum albumin (HSA). The sensing mesoporous silica nanoparticles are loaded with rhodamine B, decorated with aminopropyl moieties and capped with curcumin. [...] Read more.
Mesoporous silica nanoparticles loaded with rhodamine B and capped with curcumin are used for the selective and sensitive fluorogenic detection of human serum albumin (HSA). The sensing mesoporous silica nanoparticles are loaded with rhodamine B, decorated with aminopropyl moieties and capped with curcumin. The nanoparticles selectively release the rhodamine B cargo in the presence of HSA. A limit of detection for HSA of 0.1 mg/mL in PBS (pH 7.4)-acetonitrile 95:5 v/v was found, and the sensing nanoparticles were used to detect HSA in spiked synthetic urine samples. Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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8 pages, 2250 KiB  
Article
Reaction of Amino-Terminated PAMAM Dendrimers with Carbon Dioxide in Aqueous and Methanol Solutions
by Beijun Cheng and Angel E. Kaifer
Molecules 2022, 27(2), 540; https://doi.org/10.3390/molecules27020540 - 15 Jan 2022
Cited by 1 | Viewed by 1791
Abstract
Polyamines have been used as active materials to capture carbon dioxide gas based on its well-known reaction with amines to form carbamates. This work investigates the reactions between three amino-terminated poly(amidoamine) (PAMAM) dendrimers (G1, G3 and G5) and CO2(g) in aqueous [...] Read more.
Polyamines have been used as active materials to capture carbon dioxide gas based on its well-known reaction with amines to form carbamates. This work investigates the reactions between three amino-terminated poly(amidoamine) (PAMAM) dendrimers (G1, G3 and G5) and CO2(g) in aqueous (D2O) and methanolic (CD3OD) solutions. The reactions were monitored using 1H NMR spectroscopy, and yielded dendrimers with a combination of terminal carbamate and terminal ammonium groups. In aqueous media the reaction was complicated by the generation of soluble carbonate and bicarbonate ions. The reaction was cleaner in CD3OD, where the larger G5 dendrimer solution formed a gel upon exposure to CO2(g). All reactions were reversible, and the trapped CO2 could be released by treatment with N2(g) and mild heating. These results highlight the importance of the polyamine dendrimer size in terms of driving changes to the solution’s physical properties (viscosity, gel formation) generated by exposure to CO2(g). Full article
(This article belongs to the Special Issue Metal Ions in Supramolecular Chemistry: A Themed Issue in Honor of Professor Luigi Fabbrizzi)
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