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Recent Breakthroughs with Layered Double Hydroxides

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A special issue of Inorganics (ISSN 2304-6740). This special issue belongs to the section "Inorganic Solid-State Chemistry".

Deadline for manuscript submissions: closed (30 June 2018) | Viewed by 21314

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Special Issue Editors

Prof. Dr. Domenica Tonelli

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Department Industrial Chemistry "Toso Montanari", University of Bologna, Viale Risorgimento 4, 40136 Bologna, Italy
Interests: analytical chemistry; sensors; biosensors; materials characterization; food analysis; environmental analysis; electrochemical devices; chemically modified electrodes; layered double hydroxides; conducting polymers; electrosynthesis; nanomaterials; metal nanoparticles; nanocomposites; energy storage; energy conversion
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Dr. Erika Scavetta

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Dipartimento di Chimica Industriale ‘Toso Montanari’, Università di Bologna, Viale Risorgimento 4, 40136 Bologna, Italy
Interests: material chemistry; electrochemistry; organic electrochemical transistors; electrochemical sensors; conducting polymers; electrocatalysis
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Layered double hydroxides (LDHs) are a family of anionic clays consisting of positively-charged brucite-like layers among which are located anions and water molecules. It is possible to synthesize LDHs containing a lot of combinations of bivalent and trivalent cations, the only limitation being their radium which must be not too different from those of Mg²⁺ and Al³⁺. LDHs are two-dimensional materials with widely tunable properties since many organic or inorganic species can be easily intercalated inside the interlayers, thus inducing changes in their porosity, morphology, charge transport, hydrophilicity/hydrophobicity, etc. Furthermore, LDHs are low-cost materials with water-resistant structures, good thermal stabilities, and environmentally-friendly natures and biocompatibilities.

All these characteristics make possible LDH utilization in many different fields, such as adsorbents for removing harmful anions, catalysis, separation technology, and photochemistry, as polymer additives, as anticorrosion coatings, drug carriers for pharmaceutically active compounds and in cancer therapy. Furthermore, LDHs are attractive materials for the fabrication of sensors and biosensors, and, when containing electroactive species, they exhibit promising pseudocapacitive properties.

This Special Issue aims to highlight the most recent applications involving LDHs with particular interest in the fields of energy storage, photocatalysis, electrocatalysis, heterogeneous catalysis, and sensing.

Prof. Dr. Domenica Tonelli
Prof. Dr. Erika Scavetta
Guest Editors

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Keywords

Layered double hydroxides
Synthesis routes
Structural, chemical and physical properties
Energy storage
Catalysis
Sensors

Published Papers (5 papers)

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Research

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17 pages, 3772 KiB

Open AccessArticle

AgCl-ZnAl Layered Double Hydroxides as Catalysts with Enhanced Photodegradation and Antibacterial Activities

by Morena Nocchetti, Monica Pica, Berardo Ridolfi, Anna Donnadio, Elisa Boccalon, Giulia Zampini, Donatella Pietrella and Mario Casciola

Inorganics 2019, 7(10), 120; https://doi.org/10.3390/inorganics7100120 - 03 Oct 2019

Cited by 11 | Viewed by 2892

Abstract

Surface-modified ZnAl layered double hydroxides (LDHs) were prepared by reaction of AgNO₃, with both ZnAlCl (LDH1) and ZnAlCO₃ exchanged on the surface with chloride anions (LDH3). In this way, AgCl nanoparticles with crystalline domains ranging from 40 to 100 nm were grown on the LDH surface. An additional sample was prepared by partial reduction of silver to obtain Ag@AgCl-LDH (LDH2). The composites were tested as catalysts in Rhodamine B (RhB) degradation, wherein LDH2 showed complete cleavage of RhB after 45 min of irradiation versus 70 min needed in the presence of AgCl. This time decreased to 35 min for LDH1 and 15 min for LDH3, underlining the role of the AgCl dimensions and anion in the interlayer region. Studies on the reactive species involved in the degradation process revealed that, for all catalysts, O₂·⁻ was the main active species, while, to some extent, holes contribute to the activity of the LDH3. Finally, the composites showed high bactericidal activity, under irradiation, against Escherichia coli, comparable with that of Gentamicin, the positive control. A synergic effect of silver released from the composites and the production of reactive oxygen species was considered. Full article

(This article belongs to the Special Issue Recent Breakthroughs with Layered Double Hydroxides)

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22 pages, 2940 KiB

Open AccessArticle

Ketone Formation via Decarboxylation Reactions of Fatty Acids Using Solid Hydroxide/Oxide Catalysts

by Benjamin Smith, Li Li, Diego D. Perera-Solis, Louise F. Gildea, Vladimir L. Zholobenko, Philip W. Dyer and H. Christopher Greenwell

Inorganics 2018, 6(4), 121; https://doi.org/10.3390/inorganics6040121 - 08 Nov 2018

Cited by 7 | Viewed by 5575

Abstract

A sustainable route to ketones is described where stearone is produced via ketonic decarboxylation of stearic acid mediated by solid base catalysts in yields of up to 97%, at 250 °C. A range of Mg/Al layered double hydroxide (LDH) and mixed metal oxide (MMO) solid base catalysts were prepared with Mg/Al ratios of between 2 and 6 via two synthetic routes, co-precipitation and co-hydration, with each material tested for their catalytic performance. For a given Mg/Al ratio, the LDH and MMO materials showed similar reactivity, with no correlation to the method of preparation. The presence of co-produced oxide phases in the co-hydration catalysts had negligible impact on reactivity. Full article

(This article belongs to the Special Issue Recent Breakthroughs with Layered Double Hydroxides)

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16 pages, 23022 KiB

Open AccessArticle

On the Rehydration of Organic Layered Double Hydroxides to form Low-Ordered Carbon/LDH Nanocomposites

by Eleonora Conterosito, Luca Palin, Diego Antonioli, Maria Pia Riccardi, Enrico Boccaleri, Maurizio Aceto, Marco Milanesio and Valentina Gianotti

Inorganics 2018, 6(3), 79; https://doi.org/10.3390/inorganics6030079 - 14 Aug 2018

Cited by 4 | Viewed by 4779

Abstract

Low-ordered carbon/layered double hydroxide (LDH) nanocomposites were prepared by rehydration of the oxides produced by calcination of an organic LDH. While the memory effect is a widely recognized effect on oxides produced by inorganic LDH, it is unprecedented from the calcination/rehydration of organic ones. Different temperatures (400, 600, and 1100 °C) were tested on the basis of thermogravimetric data. Water, instead of a carbonate solution, was used for the rehydration, with CO₂ available from water itself and/or air to induce a slower process with an easier and better intercalation of the carbonaceous species. The samples were characterized by X-ray powder diffraction (XRPD), infrared in reflection mode (IR), and Raman spectroscopies and scanning electron microscopy (SEM). XRPD indicated the presence of carbonate LDH, and of residuals of unreacted oxides. IR confirmed that the prevailing anion is carbonate, coming from the water used for the rehydration and/or air. Raman data indicated the presence of low-ordered carbonaceous species moieties and SEM and XRPD the absence of separated bulky graphitic sheets, suggesting an intimate mixing of the low ordered carbonaceous phase with reconstructed LDH. Organic LDH gave better memory effect after calcination at 400 °C. Conversely, the carbonaceous species are observed after rehydration of the sample calcined at 600 °C with a reduced memory effect, demonstrating the interference of the carbonaceous phase with LDH reconstruction and the bonding with LDH layers to form a low-ordered carbon/LDH nanocomposite. Full article

(This article belongs to the Special Issue Recent Breakthroughs with Layered Double Hydroxides)

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Graphical abstract

18 pages, 2610 KiB

Open AccessArticle

Oxidation of Benzylic Alcohols and Lignin Model Compounds with Layered Double Hydroxide Catalysts

by Justin K. Mobley, John A. Jennings, Tonya Morgan, Axel Kiefer and Mark Crocker

Inorganics 2018, 6(3), 75; https://doi.org/10.3390/inorganics6030075 - 31 Jul 2018

Cited by 4 | Viewed by 3930

Abstract

Alcohol oxidation to carbonyl compounds is one of the most commonly used reactions in synthetic chemistry. Herein, we report the use of base metal layered double hydroxide (LDH) catalysts for the oxidation of benzylic alcohols in polar solvents. These catalysts are ideal reagents for alcohol oxidations due to their ease of synthesis, tunability, and ease of separation from the reaction medium. LDHs synthesized in this study were fully characterized by means of X-ray diffraction, NH₃-temperature programmed desorption (TPD), pulsed CO₂ chemisorption, N₂ physisorption, electron microscopy, and elemental analysis. LDHs were found to effectively oxidize benzylic alcohols to their corresponding carbonyl compounds in diphenyl ether, using O₂ as the terminal oxidant. LDH catalysts were also applied to the oxidation of lignin β-O-4 model compounds. Typically, for all catalysts, only trace amounts of the ketone formed from benzylic alcohol oxidation were observed, the main products comprising benzoic acids and phenols arising from β-aryl ether cleavage. This observation is consistent with the higher reactivity of the ketones, resulting from weakening of the C_β–O₄ bond that was shown to be aerobically cleaved at 180 °C in the absence of a catalyst. Full article

(This article belongs to the Special Issue Recent Breakthroughs with Layered Double Hydroxides)

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Review

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18 pages, 4957 KiB

Open AccessReview

Hydrotalcite-Type Materials Electrodeposited on Open-Cell Metallic Foams as Structured Catalysts

by Phuoc Hoang Ho, Erika Scavetta, Domenica Tonelli, Giuseppe Fornasari, Angelo Vaccari and Patricia Benito

Inorganics 2018, 6(3), 74; https://doi.org/10.3390/inorganics6030074 - 29 Jul 2018

Cited by 1 | Viewed by 3533

Abstract

Structured catalysts based on hydrotalcite-derived coatings on open-cell metallic foams combine tailored basic/acidic sites, relatively high specific surface area and/or metal dispersion of the coating as well as low pressure drop and enhanced heat and mass transfer of the 3D metallic support. The properties of the resulting structured catalysts depend on the coating procedure. We have proposed the electro-base generation method for in situ and fast precipitation of Ni/Al and Rh/Mg/Al hydrotalcite-type materials on FeCrAlloy foams, which after calcination at high temperature give rise to structured catalysts for syngas (CO + H₂) production through Steam Reforming and Catalytic Partial Oxidation of CH₄. The fundamental understanding of the electrochemical-chemical reactions relevant for the electrodeposition and the influence of electrosynthesis parameters on the properties of the as-deposited coatings as well the resulting structured catalysts and, hence, on their catalytic performance, were summarized. Full article

(This article belongs to the Special Issue Recent Breakthroughs with Layered Double Hydroxides)

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