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Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health

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A special issue of Crystals (ISSN 2073-4352). This special issue belongs to the section "Hybrid and Composite Crystalline Materials".

Deadline for manuscript submissions: closed (30 June 2022) | Viewed by 23309

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Special Issue Editors

Dr. Radu Claudiu Fierascu

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Guest Editor

National Institute for Research and Development in Chemistry and Petrochemistry, ICECHIM, 060021 Bucharest, Romania
Interests: nanoparticles phytosynthesis; natural extracts; biological properties
Special Issues, Collections and Topics in MDPI journals

Dr. Florentina Monica Raduly

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Guest Editor

Laboratory of Functional Dyes and Related Materials, National Institute for Research and Development in Chemistry and Petrochemistry, ICECHIM, Bucharest, Romania
Interests: dyes; organic synthesis; hybrid materials; smart textiles; coatings; luminescent materials; natural dyes
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

A Special Issue titled "Hybrid Organic–Inorganic Materials Used to Improve the Environment and Human Health” is being launched to collect and disseminate original, theoretical, and applied scientific research in various fields of use of hybrid and composite crystalline materials.

In recent years, due to climate change, there has been increasing interest in the development of hybrid and nanocomposite materials. The state-of-the-art technology leads to the realization of many environmentally friendly materials or properties that help reduce pollution factors. Most applications are found in the automotive, textile, and food industries. These are reflected in the general state of human health. Another important factor that contributes to this condition is the development and application of nanomaterials in medicine. The research focuses mainly on the design and engineering of these materials, which include metal-organic frameworks; covalent organic frameworks; zeolite materials; organic–inorganic hybrids; composites based on graphene or carbon nitride, as well as those based on metal, metal oxides, or polymers, and their applications.

Original research and review papers that will be published in this Special Issue will cover various topics including but not limited to the following:

Preparative and processing techniques;
Structure and morphology;
Tailored optical properties;
Dressings and biomaterials carrying drugs;
Advanced catalyst systems;
Natural pesticides;
Smart packaging;
Bioactive coatings;
Electrochemical sensors.

Dr. Radu Claudiu Fierascu
Dr. Florentina Monica Raduly
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. Crystals is an international peer-reviewed open access monthly 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 2600 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

composite materials
functional materials
structural and morphological characterization
medical applications
solar cells
(photo)catalysts
luminescent materials
X-ray diffraction
optical properties
thermodynamic properties

Published Papers (12 papers)

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Editorial

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2 pages, 195 KiB

Open AccessEditorial

Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health

by Florentina Monica Raduly and Radu Claudiu Fierăscu

Crystals 2022, 12(9), 1273; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12091273 - 07 Sep 2022

Viewed by 1135

Abstract

The Special Issue on “Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health” is a collection of 11 original articles (including one communication paper) dedicated to theoretical and experimental research works providing new insights and practical findings in the fields of [...] Read more.

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

Research

Jump to: Editorial

15 pages, 3980 KiB

Open AccessArticle

Influence of Organic-Modified Inorganic Matrices on the Optical Properties of Palygorskite–Curcumin-Type Hybrid Materials

by Florentina Monica Raduly, Valentin Rădițoiu, Radu Claudiu Fierăscu, Alina Rădițoiu, Cristian Andi Nicolae and Violeta Purcar

Crystals 2022, 12(7), 1005; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12071005 - 20 Jul 2022

Cited by 2 | Viewed by 1460

Abstract

Clays are very important from an economic and application point of view, as they are suitable hosts for organic compounds. In order to diversify the fields of application, they are structurally modified by physical or chemical methods with cationic species, and/or different bifunctional compounds, such as organosilanes. In this study, palygorskite was modified with (3-Aminopropyl) triethoxysilane, which was subsequently modified at the amino group by grafting an acetate residue. By using this strategy, two types of host hybrid materials were obtained on which curcumin derivatives were deposited. The composites obtained were structurally characterized and their photophysical properties were investigated in relation to the structure of the host matrices and interactions with curcumin-type visiting species. The hybrid composites have different colors (orange, yellow, pink), depending on the polarity of the inorganic matrices modulated by different organic groups grafted at the surface. Fluorescence emission in the visible range is characterized by the presence of two emission maxima, one belonging to the chromophore and the other influenced by the physical interactions between auxochromes and host matrices. These hybrid materials, compared to other composite structures, are obtained by a simple adsorption process. They are temperature stable in aggressive environments (acid/base) and render the fluorescent properties of dyes redundant, with improved luminescent performance compared to them. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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28 pages, 7359 KiB

Open AccessArticle

Parametric Analyses of the Influence of Temperature, Load Duration, and Interlayer Thickness on a Laminated Glass Structure Exposed to Out-of-Plane Loading

by Mirela Galić, Gabrijela Grozdanić, Vladimir Divić and Pavao Marović

Crystals 2022, 12(6), 838; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12060838 - 14 Jun 2022

Cited by 4 | Viewed by 1724

Abstract

One of today’s most-used glass products is a composite made of at least two glass panels connected with a soft polymeric interlayer—laminated glass. The mechanical properties of such elements are influenced by interlayer properties and the type of glass used. In this work, experimental and numerical analyses of laminated glass panels exposed to four-point bending are performed to observe and compare the stresses and displacements caused by different parameters, such as temperature, load duration, the thickness and type of the interlayers, as well as the symmetrical and nonsymmetrical disposition of the glass plates’ thickness. The numerical analysis was verified by four-point bending experimental tests. After validation, a parametric study on these influences was performed. To obtain the relationship between the load duration, temperature, and thickness of the interlayer compared to the maximal displacement (as a measure of flexural stiffness) and tension stress in the bottom glass plate, an analytical polynomial of a sixth total order is proposed. Isosurfaces are created, showing the dependence of stresses and displacements on the specified parameters as well as clearly showing differences in the behavior of laminated glass panels for the same conditions but with different interlayers. Based on the findings of the parametric study, conclusions are derived about the flexural stiffness and stress distribution in two-plate laminated glass with PVB and ionoplast interlayers. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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9 pages, 3496 KiB

Open AccessArticle

Comparative Study of Cu/ZSM-5 Catalysts Synthesized by Two Ion-Exchange Methods

by Dalia Santa Cruz-Navarro, Miguel Torres-Rodríguez, Mirella Gutiérrez-Arzaluz, Violeta Mugica-Álvarez and Sibele Berenice Pergher

Crystals 2022, 12(4), 545; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12040545 - 13 Apr 2022

Cited by 5 | Viewed by 1876

Abstract

As catalysis is one of the pillars of green chemistry, this work aimed at continuing the development of synthesized catalysts under controlled conditions that allow the attainment of materials with the best physicochemical properties for the process for which they were designed. Based on this, the synthesis, characterization, and comparison of copper-based catalysts supported on ammonium and acidic ZSM-5-type zeolite by two ion exchange methods, liquid phase and solid state, are presented. The catalysts obtained were characterized by SEM/EDS, FTIR, XRD, and TPR to study the effect of the synthesis method on the physicochemical properties of each catalyst. The SEM/EDS results showed a homogeneous distribution of copper in the zeolite and the TPR led to determining the temperature ranges for the reduction of Cu²⁺ → Cu⁺ → Cu⁰. Furthermore, the X-ray results showed no modification of the structure of the zeolite after ion exchange, heat treatment, and TPR analysis. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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12 pages, 2695 KiB

Open AccessArticle

Gas-Sensing Properties of a Carbyne-Enriched Nanocoating Deposited onto Surface Acoustic Wave Composite Substrates with Various Electrode Topologies

by Mariya Aleksandrova, Georgi Kolev, Andrey Brigadin and Alexander Lukin

Crystals 2022, 12(4), 501; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12040501 - 04 Apr 2022

Cited by 13 | Viewed by 1745

Abstract

The application of carbyne-enriched nanomaterials opens unique possibilities for enhancing the functional properties of several nanomaterials and unlocking their full potential for practical applications in high-end devices. We studied the ethanol-vapor-sensing performance of a carbyne-enriched nanocoating deposited onto surface acoustic wave (SAW) composite substrates with various electrode topologies. The carbyne-enriched nanocoating was grown using the ion-assisted pulse-plasma deposition technique. Such carbon nanostructured metamaterials were named 2D-ordered linear-chain carbon, where they represented a two-dimensionally packed hexagonal array of carbon chains held by the van der Waals forces, with the interchain spacing approximately being between 4.8 and 5.03 Å. The main characteristics of the sensing device, such as dynamic range, linearity, sensitivity, and response and recovery times, were measured as a function of the ethanol concentration. To the authors’ knowledge, this was the first time demonstration of the detection ability of carbyne-enriched material to ethanol vapors. The results may pave the path for optimization of these sensor architectures for the precise detection of volatile organic compounds, with applications in the fields of medicine, healthcare, and air composition monitoring. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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18 pages, 6702 KiB

Open AccessArticle

Synthesis, Molecular Structure, Thermal and Spectroscopic Analysis of a Novel Bromochalcone Derivative with Larvicidal Activity

by Pollyana P. Firmino, Jaqueline E. Queiroz, Lucas D. Dias, Patricia R. S. Wenceslau, Larissa M. de Souza, Ievgeniia Iermak, Wesley F. Vaz, Jean M. F. Custódio, Allen G. Oliver, Gilberto L. B. de Aquino and Hamilton B. Napolitano

Crystals 2022, 12(4), 440; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12040440 - 22 Mar 2022

Cited by 8 | Viewed by 1974

Abstract

Chalcones belong to the flavonoids family and are natural compounds which show promising larvicidal property against Aedes aegypti larvae. Aiming to obtain a synthetic chalcone derivative with high larvicidal activity, herein, a bromochalcone derivative, namely (E)-3-(4-butylphenyl)-1-(4-bromophenyl)-prop-2-en-1-one (BBP), was designed, synthesized and extensively characterized by ¹H- and ¹³C- nuclear magnetic resonance (NMR), infrared (IR), Raman spectroscopy, mass spectrometry (MS), ultraviolet–visible spectroscopy (UV-Vis), thermogravimetric analysis (TGA), differential scanning calorimetry (DSC), and X-ray diffraction. Further, the quantum mechanics calculations implemented at the B3LYP/6–311+G(d)* level of the theory indicate that the supramolecular arrangement was stabilized by C–H⋯O and edge-to-face C–H⋯π interactions. The EGAP calculated (3.97 eV) indicates a good reactivity value compared with other similar chalcone derivatives. Furthermore, the synthesized bromochalcone derivative shows promising larvicidal activity (mortality up to 80% at 57.6 mg·L⁻¹) against Ae. aegypti larvae. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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7 pages, 1538 KiB

Open AccessArticle

A Molten Salt Electrochemical Process for the Preparation of Cost-Effective p-Block (Coating) Materials

by Prabhat Kumar Tripathy and Kunal Mondal

Crystals 2022, 12(3), 385; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12030385 - 13 Mar 2022

Cited by 1 | Viewed by 1803

Abstract

Solar energy applications rely heavily on p-block elements and transition metals. Silicon is, by far, the most commonly used material in photovoltaic cells and accounts for about 85% of modules sold presently. Of late, thin film photovoltaic cells have gained momentum because of their higher efficiencies. Most of these thin film devices are made out of just five elements, namely, cadmium, tellurium, selenium, indium, gallium and copper. The present manuscript describes an elegant and inexpensive molten salt-based electrolytic process for fabricating a tellurium-coated metallic substrate. A three-electrode set up was employed to coat iridium with tellurium from a molten bath containing lithium chloride, lithium oxide and tellurium tetrachloride (LiCl-Li₂O-TeCl₄) at 650 °C for a duration ranging from 30 to 120 min under a galvanostatic mode. The tellurium coating was observed to be thick, uniform, smooth and homogeneous. Additionally, the deposited tellurium did not chemically react with the iridium substrate to form intermetallic compounds, which is a good feature from the standpoint of the device’s performance characteristics. The present process, being generic in nature, shows the potential for the manufacture of both the coated substates and high-purity elements not just for tellurium but also for other p-block elements. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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22 pages, 7569 KiB

Open AccessArticle

Isolation, Identification, Spectral Studies and X-ray Crystal Structures of Two Compounds from Bixa orellana, DFT Calculations and DNA Binding Studies

by Mehtab Parveen, Mohammad Azeem, Afroz Aslam, Mohammad Azam, Sharmin Siddiqui, Mohammad Tabish, Ali Mohammad Malla, Kim Min, Vitor Hugo Rodrigues, Saud I. Al-Resayes and Mahboob Alam

Crystals 2022, 12(3), 380; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12030380 - 11 Mar 2022

Cited by 8 | Viewed by 2328

Abstract

4,6-Diacetylresorcinol (1) and 3-O-methylellagic acid dihydrate (2), both biologically significant compounds, were extracted from Bixa orellana and studied using IR, ¹H, and ¹³C NMR, and UV-vis spectroscopic techniques. X-ray crystallographic techniques were also used to establish the molecular structure of the isolated compounds 1 and 2. Geometric parameters, vibrational frequencies, and gauge including atomic orbital (GIAO) ¹H and ¹³C NMR of 1 and 2 in the ground state were computed by the density functional theory (DFT) using B3LYP/6-311G(d,p) basis set backing up experimental studies and established the correct structure of isolated compounds. The parameters obtained from the combined DFT, and X-ray diffraction studies are mutually agreed to establish correct structures of 1 and 2. In addition, an electrostatic potential map and HOMO−LUMO energy gap were made using the DFT calculation to determine the distribution of energy and the chemical reactivity region of the isolated compounds. The current study also provides further insights into the interaction of compound 2 with ct-DNA using numerous biophysical and in silico techniques. Moreover, in silico studies indicate that compound 2 binds to the DNA in the minor groove. Lipinski’s rule of five revealed a higher tendency of compound 2 towards drug-likeness. The bioavailability and synthetic accessibility score for compound 2 was found to be 0.55 and 3.21, suggesting that compound 2 could serve as an effective therapeutic candidate. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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13 pages, 27252 KiB

Open AccessArticle

Performance Enhancement of Self-Cleaning Cotton Fabric with ZnO NPs and Dicarboxylic Acids

by Xinlei Ji, Hong Li, Yuan Qin and Jun Yan

Crystals 2022, 12(2), 214; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst12020214 - 31 Jan 2022

Cited by 7 | Viewed by 2199

Abstract

In this paper, we explore the self-cleaning and washing durability of green-prepared ZnO NPs combined with cotton fabrics. Honeysuckle extract was used to prepare ZnO NPs with an average particle size of 15.3 nm. Cotton fabrics were then treated with oxalic acid (OA), tartaric acid (TA), and succinic acid (SA) as cross-linking agents, sodium hypophosphite as a catalyst, and after that, the ZnO NPs were applied to the cross-linked cotton fabrics by the padding to prepare the self-cleaning cotton fabrics. The morphology and structure of the fabric samples were characterized using FTIR, scanning electron microscopy (SEM), Energy-dispersive X-ray spectroscopy (EDS), and XRD. The optical properties of the cotton fabric samples were discussed by UV-vis diffuse reflectance spectrum, and the self-cleaning performance, wrinkle recovery angle and ultraviolet protection performance of the cotton fabric samples were analyzed. The results showed that the carboxyl groups of TA, OA, and SA were esterified with hydroxyl groups of the cotton fiber and formed a film on the surface of the cotton fabrics. ZnO NPs were successfully loaded onto the cotton fabrics by strong electrostatic interaction, causing the improvement of the washing resistance of the cross-linked fabrics. In addition, compared with uncross-linked fabrics, the wrinkle recovery performance of the cross-linked fabrics had also been greatly improved, and the UV protection factor reached 50+, thus obtaining an excellent self-cleaning, multifunctional cotton-based textile with anti-wrinkle and anti-ultraviolet properties. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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9 pages, 3211 KiB

Open AccessArticle

Modification of FA_0.85MA_0.15Pb(I_0.85Br_0.15)₃ Films by NH₂-POSS

by Yangyang Zhang, Na Liu, Haipeng Xie, Jia Liu, Pan Yuan, Junhua Wei, Yuan Zhao, Baopeng Yang, Jianhua Zhang, Shitan Wang, Han Huang, Dongmei Niu, Qi Chen and Yongli Gao

Crystals 2021, 11(12), 1544; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst11121544 - 10 Dec 2021

Cited by 3 | Viewed by 2161

Abstract

The surface composition and morphology of FA_0.85MA_0.15Pb(I_0.85Br_0.15)₃ films fabricated by the spin-coating method with different concentrations of NH₂-POSS were investigated with atomic force microscopy (AFM), X-ray photoelectron spectroscopy (XPS), angle-resolved X-ray photoelectron spectroscopy (AR-XPS), and Fourier transform infrared spectroscopy (FTIR). It was found that the surface composition of the FA_0.85MA_0.15Pb(I_0.85Br_0.15)₃ films was changed regularly through the interaction between NH₂-POSS and the perovskite film. The corresponding surface morphological changes were also observed. When the concentration of NH₂-POSS exceeded 10 mg/mL, a lot of cracks on the surface of the perovskite film were observed and the surface morphology was damaged. The surface composition and its distribution can be adjusted by changing the concentration of NH₂-POSS and the proper concentration of NH₂-POSS can substantially improve the quality of perovskite film. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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7 pages, 3858 KiB

Open AccessCommunication

Atmospheric Carbon Dioxide Capture as Carbonate into a Luminescent Trinuclear Cd(II) Complex with Tris(2-aminoethyl)amine Tripodal Ligand

by Augustin M. Mădălan

Crystals 2021, 11(12), 1480; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst11121480 - 29 Nov 2021

Cited by 1 | Viewed by 1432

Abstract

Spontaneous atmospheric CO₂ capture as carbonate anion occurred in the synthesis of a trinuclear Cd(II) complex with tris(2-aminoethyl)amine ligand. In reaction two types of compounds were obtained and structurally characterized by X-ray diffraction on a single crystal: initially [{Cd(tren)}₃(tren)](ClO₄)₆·2H₂O (1) and subsequently [{Cd(tren)}₃(tren)][{Cd(tren)}₃(µ₃-ηCO₃)](ClO₄)₁₀ (2). The carbonate anion replaces partially the bridging tren molecule and coordinates in a µ₃ fashion. The luminescent properties of the compounds were investigated. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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11 pages, 3379 KiB

Open AccessEditor’s ChoiceArticle

Crystal Structures, Thermal and Luminescent Properties of Gadolinium(III) Trans-1,4-cyclohexanedicarboxylate Metal-Organic Frameworks

by Pavel A. Demakov, Alena A. Vasileva, Vladimir A. Lazarenko, Alexey A. Ryadun and Vladimir P. Fedin

Crystals 2021, 11(11), 1375; https://0-doi-org.brum.beds.ac.uk/10.3390/cryst11111375 - 11 Nov 2021

Cited by 9 | Viewed by 2481

Abstract

Four new gadolinium(III) metal-organic frameworks containing 2,2′-bipyridyl (bpy) or 1,10-phenanthroline (phen) chelate ligands and trans-1,4-cyclohexanedicarboxylate (chdc²⁻) were synthesized. Their crystal structures were determined by single-crystal X-ray diffraction analysis. All four coordination frameworks are based on the binuclear carboxylate building units. In the compounds [Gd₂(bpy)₂(chdc)₃]·H₂O (1) and [Gd₂(phen)₂(chdc)₃]·0.5DMF (2), the six-connected {Ln₂(L)₂(OOCR)₆} blocks form a 3D network with the primitive cubic (pcu) topology. In the compounds [Gd₂(NO₃)₂(phen)₂(chdc)₂]·2DMF (3) and [Gd₂Cl₂(phen)₂(chdc)₂]·0.3DMF·2.2dioxane (4), the four-connected {Ln₂(L)₂(X)₂OOCR)₄} units (where X = NO₃⁻ for 3 or Cl⁻ for 4) form a 2D square-grid (sql) network. The solid-state luminescent properties were investigated for the synthesized frameworks. Bpy-containing compound 1 shows no luminescence, possibly due to the paramagnetic quenching by Gd³⁺ cation. In contrast, the phenathroline-containing MOFs 2–4 possess yellow emission under visible excitation (λ_ex = 460 nm) with the tuning of the characteristic wavelength by the coordination environment of the metal center. Full article

(This article belongs to the Special Issue Hybrid Organic-Inorganic Materials Used to Improve the Environment and Human Health)

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