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

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 25056

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Laboratory of Functional Dyes and Related Materials, National Institute for Research and Development in Chemistry and Petrochemistry, ICECHIM, 060021 Bucharest, Romania
Interests: dyes; organic synthesis; hybrid materials; smart textile; coatings; luminescent materials; nanomaterials
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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

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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  
Editorial
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://doi.org/10.3390/cryst12091273 - 7 Sep 2022
Viewed by 1266
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.
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 the environmental protection and human health—related topics [...] Full article

Research

Jump to: Editorial

15 pages, 3980 KiB  
Article
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://doi.org/10.3390/cryst12071005 - 20 Jul 2022
Cited by 2 | Viewed by 1597
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 [...] Read more.
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
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28 pages, 7359 KiB  
Article
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://doi.org/10.3390/cryst12060838 - 14 Jun 2022
Cited by 5 | Viewed by 1856
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, [...] Read more.
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
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9 pages, 3496 KiB  
Article
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://doi.org/10.3390/cryst12040545 - 13 Apr 2022
Cited by 6 | Viewed by 2110
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 [...] Read more.
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
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12 pages, 2695 KiB  
Article
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://doi.org/10.3390/cryst12040501 - 4 Apr 2022
Cited by 14 | Viewed by 1881
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 [...] Read more.
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
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18 pages, 6702 KiB  
Article
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://doi.org/10.3390/cryst12040440 - 22 Mar 2022
Cited by 9 | Viewed by 2098
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 [...] Read more.
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
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7 pages, 1538 KiB  
Article
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://doi.org/10.3390/cryst12030385 - 13 Mar 2022
Cited by 1 | Viewed by 1972
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 [...] Read more.
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
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22 pages, 7569 KiB  
Article
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://doi.org/10.3390/cryst12030380 - 11 Mar 2022
Cited by 8 | Viewed by 2457
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 [...] Read more.
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
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13 pages, 27252 KiB  
Article
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://doi.org/10.3390/cryst12020214 - 31 Jan 2022
Cited by 8 | Viewed by 2331
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), [...] Read more.
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
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9 pages, 3211 KiB  
Article
Modification of FA0.85MA0.15Pb(I0.85Br0.15)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://doi.org/10.3390/cryst11121544 - 10 Dec 2021
Cited by 3 | Viewed by 2277
Abstract
The surface composition and morphology of FA0.85MA0.15Pb(I0.85Br0.15)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 [...] Read more.
The surface composition and morphology of FA0.85MA0.15Pb(I0.85Br0.15)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 FA0.85MA0.15Pb(I0.85Br0.15)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
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7 pages, 3858 KiB  
Communication
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://doi.org/10.3390/cryst11121480 - 29 Nov 2021
Cited by 1 | Viewed by 1537
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 [...] Read more.
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)}33-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
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11 pages, 3379 KiB  
Article
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://doi.org/10.3390/cryst11111375 - 11 Nov 2021
Cited by 9 | Viewed by 2619
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. [...] Read more.
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 24 possess yellow emission under visible excitation (λex = 460 nm) with the tuning of the characteristic wavelength by the coordination environment of the metal center. Full article
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