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Layered Double Hydroxides

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

Deadline for manuscript submissions: closed (30 April 2020) | Viewed by 54722

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Dr. Giuseppe Prestopino

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Dipartimento di Ingegneria Industriale Via del Politecnico 1, Università di Roma "Tor Vergata", I-00133 Roma, Italy
Interests: thin film technology; chemical vapor deposition synthesis; synthetic diamond; self-assembled nanomaterials; layered double hydroxides; electrical and optical properties
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Giuseppe Arrabito

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Department of Physics and Chemistry - Emilio Segrè, Viale delle Scienze Ed. 17, University of Palermo, 90128 Palermo, Italy
Interests: Molecular printing; 3D Printing; Dip Pen Nanolithography; Atomic Force Microscopy; Microfluidics; Nanowires; Fluorescence lifetime; nanomaterials/DNA/aptamer-based sensor; POC devices; DNA/aptamer; enzymes; biosensor design; medical applications; food and environmental applications

Special Issue Information

Dear Colleagues,

Two-dimensional (2D) materials constitute a versatile platform for the realization of a new class of functional systems showing unique enhanced surface effects and unprecedented tuneable confinement and geometry-related properties which can open up important applications in very different fields, namely surface chemistry and catalysis, band-gap engineering, photovoltaics, energy storage, harvesting and conversion, nanomedicine, spintronics and valleytronics. Many 2D materials with very different natures have been described in detail for these applications, such as graphene, silicene, phosphorene, hexagonal boron nitride (h-BN), transition metal dichalcogenides (TMDs), metal organic frameworks (MOFs), layered oxides and hydroxides, and DNA origami. Although the proof-of-principle for their outstanding functionality has been demonstrated, the ultimate hurdle for 2D materials to be implementable in technological applications is the ability to find reproducible, green-chemistry, environment friendly and low-cost approaches for their synthesis and subsequent functionalization at large scale and low cost. Among the up-to-date 2D materials, layered double hydroxides (LDHs) have attracted a huge research interest in the last years, with more than 2000 papers published in the last five years. LDHs are low-cost materials, and can be easily synthetized as self-assembled hierarchical nanosheet thin films and exfoliated up to the monolayer limit. LDHs are therefore a playground for exciting new research covering all of the most intriguing features of 2D materials and more.

The aim of this Special Issue is to provide a unique international platform that can enable scientists to publish the latest advancements on the following topics:

- Novel approaches to the controlled synthesis of inorganic, organic and biomolecular 2D materials (green chemistry, low temperature), with particular emphasis on the implementation of large-scale fabrication of devices, wet-chemistry and water-dispersible 2D material formulations.

- The synthesis, characterization, and functionalization of LDHs, including all contributions focusing on properties and applications of self-assembled hierarchical LDH nanosheet thin films and LDH exfoliation to monolayers, according to a multidisciplinary approach.

- Other 2D material monolayers, layered materials, Van der Waals heterostructures.

- Physical, chemical, and optical characterization of 2D materials and exploitation of their outstanding features for device fabrication and integration in complex systems.

Dr. Giuseppe Prestopino
Dr. Giuseppe Arrabito
Guest Editors

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Keywords

green chemistry
surface chemistry
hydrothermal synthesis
catalysis
energy conversion
layered double hydroxides
LDHs
2D materials
bottom-up, top-down, exfoliation
heterostructures and layered composites
quantum confinement
ionic conductivity

Published Papers (10 papers)

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Editorial

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3 pages, 162 KiB

Open AccessEditorial

Layered Double Hydroxides

by Giuseppe Prestopino and Giuseppe Arrabito

Crystals 2020, 10(11), 1050; https://doi.org/10.3390/cryst10111050 - 19 Nov 2020

Cited by 4 | Viewed by 2663

Abstract

The impact of layered double hydroxides (LDHs) within the multidisciplinary fields of materials sciences, physics, chemistry, and biology is rapidly growing, given their easiness of synthesis, flexibility in composition, tunable biocompatibility and morphology [...] Full article

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

Research

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15 pages, 5035 KiB

Open AccessArticle

Resveratrol-Loaded Solid Lipid Nanoparticle Supplementation Ameliorates Physical Fatigue by Improving Mitochondrial Quality Control

by Jingyu Sun, Yunhe Zhou, Yajuan Su, Sheng Li, Jingmei Dong, Qing He, Yang Cao, Tianfeng Lu and Lili Qin

Crystals 2019, 9(11), 559; https://doi.org/10.3390/cryst9110559 - 25 Oct 2019

Cited by 9 | Viewed by 3014

Abstract

Resveratrol (RSV) has various pharmacological effects; however, few studies have directly addressed the possible antifatigue effects of long-term endurance exercise. The clinical use of RSV is limited by its poor water solubility and extremely short plasma half-life. Solid lipid nanoparticles (SLNs) are considered as reasonable drug delivery systems to overcome some of these drawbacks and expand its applications. In this study, RSV-SLNs were successfully prepared through emulsification and low-temperature solidification. Results showed that RSV-SLN supplementation effectively enhanced endurance performance. RSV-SLN supplementation might enhance mitochondrial function by ameliorating mitochondrial quality control (QC), which was superior to RSV application. These results revealed an unexpected role of RSV-SLN compared with RSV in terms of linking nutrient deprivation to mitochondrial oxidant production through mitochondrial QC. A mitochondrion-mediated pathway was likely involved in RSV-SLN, thereby improving endurance performance. Overall, this study highlighted new possibilities for anti-physical-fatigue strategies. Full article

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

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16 pages, 5454 KiB

Open AccessArticle

Synthesis of MgFe Layered Double Hydroxide from Iron-Containing Acidic Residual Solution and Its Adsorption Performance

by Alin Golban, Lavinia Lupa, Laura Cocheci and Rodica Pode

Crystals 2019, 9(10), 514; https://doi.org/10.3390/cryst9100514 - 03 Oct 2019

Cited by 16 | Viewed by 3549

Abstract

The paper presents a new method of layered double hydroxide (LDH) synthesis starting from secondary sources, namely acidic residual solutions. The iron content of the acidic solution resulting from the pickling step of the hot-dip galvanizing process make it suitable to be used as an iron precursor in LDH synthesis. Here, Mg₄Fe–LDH synthesized through the newly proposed method presented structural and morphological characteristics similar to the properties of layered double hydroxides synthesized from analytical-grade reagents. Moreover, the as-synthesized LDH and its calcined product presented efficient adsorption properties in the removal process of Mo(VI) from aqueous solutions. The adsorption studies are discussed from the equilibrium, kinetic, and thermodynamic points of view. The proposed novel technologies present both economic and environmental protection benefits. Full article

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17 pages, 2397 KiB

Open AccessArticle

Antimonate Removal from Polluted Mining Water by Calcined Layered Double Hydroxides

by Elisabetta Dore, Franco Frau and Rosa Cidu

Crystals 2019, 9(8), 410; https://doi.org/10.3390/cryst9080410 - 06 Aug 2019

Cited by 11 | Viewed by 2918

Abstract

Calcined layered double hydroxides (LDHs) can be used to remove Sb(V), in the Sb(OH)₆⁻ form, from aqueous solutions. Sorption batch experiments showed that the mixed MgAlFe oxides, obtained from calcined hydrotalcite-like compound (3HT-cal), removed Sb(OH)₆⁻ through the formation of a non-LDH brandholzite-like compound, whereas the mixed ZnAl oxides, resulting from calcined zaccagnaite-like compound (2ZC-cal), trapped Sb(OH)₆⁻ in the interlayer during the formation of a Sb(V)-bearing LDH (the zincalstibite-like compound). The competition effect of coexistent anions on Sb(OH)₆⁻ removal was HAsO₄²⁻ >> HCO₃⁻ ≥ SO₄²⁻ for 2ZC-cal and HAsO₄²⁻ >> HCO₃⁻ >> SO₄²⁻ for 3HT-cal. Considering the importance of assessing the practical use of calcined LDHs, batch experiments were also carried out with a slag drainage affected by serious Sb(V) pollution (Sb = 9900 μg/L) sampled at the abandoned Su Suergiu mine (Sardinia, Italy). Results showed that, due to the complex chemical composition of the slag drainage, dissolved Sb(OH)₆⁻ was removed by intercalation in the interlayer of carbonate LDHs rather than through the formation of brandholzite-like or zincalstibite-like compounds. Both 2ZC-cal and 3HT-cal efficiently removed very high percentages (up to 90–99%) of Sb(V) from the Su Suergiu mine drainage, and thus can have a potential application for real polluted waters. Full article

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11 pages, 1262 KiB

Open AccessArticle

Mg-Fe Layered Double Hydroxides Enhance Surfactin Production in Bacterial Cells

by Pei-Hsin Chang, Si-Yu Li, Tzong-Yuan Juang and Yung-Chuan Liu

Crystals 2019, 9(7), 355; https://doi.org/10.3390/cryst9070355 - 12 Jul 2019

Cited by 4 | Viewed by 2990

Abstract

In this study, four additives—montmorillonite, activated carbon, and the layered double hydroxides (LDHs), Mg₂Fe–LDH and Mg₂Al–LDH—were tested for their ability to promote surfactin production in a Bacillus subtilis ATCC 21332 culture. Among these tested materials, the addition of 4 g/L of the Mg-Fe LDH, which featured an Mg/Fe molar ratio of 2:1, produced the highest surfactin yield of 5280 mg/L. During the time course of B. subtilis cultivation with the added LDH, two phases of cell growth were evident: Growth and decay. In the growth phase, the cells grew slowly and secreted a high amount of surfactin; in the decay phase, the cells degraded rapidly. The production in the presence of the Mg₂Fe–LDH had three characteristics: (i) High surfactin production at low biomass, indicating a high specific surfactin yield of 3.19 g/g DCW; (ii) rapid surfactin production within 24 h, inferring remarkably high productivity (4660 mg/L/d); and (iii) a lower carbon source flux to biomass, suggesting an efficient carbon flux to surfactin, giving a high carbon yield of 52.8%. The addition of Mg₂Fe–LDH is an effective means of enhancing surfactin production, with many potential applications and future industrial scale-up. Full article

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10 pages, 9549 KiB

Open AccessArticle

Rapid Removal and Efficient Recovery of Tetracycline Antibiotics in Aqueous Solution Using Layered Double Hydroxide Components in an In Situ-Adsorption Process

by Kwanjira Panplado, Maliwan Subsadsana, Supalax Srijaranai and Sira Sansuk

Crystals 2019, 9(7), 342; https://doi.org/10.3390/cryst9070342 - 04 Jul 2019

Cited by 15 | Viewed by 3661

Abstract

This work demonstrates a simple approach for the efficient removal of tetracycline (TC) antibiotic from an aqueous solution. The in situ-adsorption removal method involved instant precipitation formation of mixed metal hydroxides (MMHs), which could immediately act as a sorbent for capturing TC from an aqueous solution, by employing layered double hydroxide (LDH) components including magnesium and aluminum ions in alkaline conditions. By using this approach, 100% removal of TC can be accomplished within 4 min under optimized conditions. The fast removal possibly resulted from an instantaneous adsorption of TC molecules onto the charged surface of MMHs via hydrogen bonding and electrostatically induced attraction. The results revealed that our removal technique was superior to the use of LDH as a sorbent in terms of both removal kinetics and efficiency. Moreover, the recovery of captured TC was tested under the influence of various common anions. It was found that 98% recovery could be simply achieved by using phosphate, possibly due to its highly charged density. Furthermore, this method was successful for efficient removal of TC in real environmental water samples. Full article

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14 pages, 3033 KiB

Open AccessEditor’s ChoiceArticle

The Fabrication of Calcium Alginate Beads as a Green Sorbent for Selective Recovery of Cu(Ⅱ) from Metal Mixtures

by Niannian Yang, Runkai Wang, Pinhua Rao, Lili Yan, Wenqi Zhang, Jincheng Wang and Fei Chai

Crystals 2019, 9(5), 255; https://doi.org/10.3390/cryst9050255 - 17 May 2019

Cited by 52 | Viewed by 5797

Abstract

Calcium alginate (CA) beads as a green sorbent were easily fabricated in this study using sodium alginate crosslinking with CaCl₂, and the crosslinking pathway was the exchange between the sodium ion of α-L-guluronic acid and Ca(II). The experimental study was conducted on Cu(II), Cd(II), Ni(II) and Zn(II) as the model heavy metals and the concentration was determined by inductively coupled plasma optical emission spectrometry (ICP-OES). The characterization and sorption behavior of the CA beads were analyzed in detail via using scanning electron microscopy (SEM), fourier transform infrared spectroscopy (FTIR) and X-ray photoelectron spectroscopy (XPS). The adsorption experiments demonstrated that the CA beads exhibited a high removal efficiency for the selective adsorption of Cu(II) from the tetra metallic mixture solution and an excellent adsorption capacity of the heavy metals separately. According to the isotherm studies, the maximum uptake of Cu(II) could reach 107.53 mg/g, which was significantly higher than the other three heavy metal ions in the tetra metallic mixture solution. Additionally, after five cycles of adsorption and desorption, the uptake rate of Cu(II) on CA beads was maintained at 92%. According to the properties mentioned above, this material was assumed to be applied to reduce heavy metal pollution or recover valuable metals from waste water. Full article

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11 pages, 1963 KiB

Open AccessArticle

Luminescent Layered Double Hydroxides Intercalated with an Anionic Photosensitizer via the Memory Effect

by Alexandre C. Teixeira, Alysson F. Morais, Ivan G.N. Silva, Eric Breynaert and Danilo Mustafa

Crystals 2019, 9(3), 153; https://doi.org/10.3390/cryst9030153 - 14 Mar 2019

Cited by 12 | Viewed by 6083

Abstract

Layered double hydroxides (LDHs) containing Eu³⁺ activators were synthesized by coprecipitation of Zn²⁺, Al³⁺, and Eu³⁺ in alkaline NO₃⁻-rich aqueous solution. Upon calcination, these materials transform into a crystalline ZnO solid solution containing Al and Eu. For suitably low calcination temperatures, this phase can be restored to LDH by rehydration in water, a feature known as the memory effect. During rehydration of an LDH, new anionic species can be intercalated and functionalized, obtaining desired physicochemical properties. This work explores the memory effect as a route to produce luminescent LDHs intercalated with 1,3,5-benzenetricarboxylic acid (BTC), a known anionic photosensitizer for Eu³⁺. Time-dependent hydration of calcined LDHs in a BTC-rich aqueous solution resulted in the recovery of the lamellar phase and in the intercalation with BTC. The interaction of this photosensitizer with Eu³⁺ in the recovered hydroxide layers gave rise to efficient energy transfer from the BTC antennae to the Eu³⁺ ions, providing a useful tool to monitor the rehydration process of the calcined LDHs. Full article

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Review

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29 pages, 6684 KiB

Open AccessReview

Layered Double Hydroxides in Bioinspired Nanotechnology

by Giuseppe Arrabito, Riccardo Pezzilli, Giuseppe Prestopino and Pier Gianni Medaglia

Crystals 2020, 10(7), 602; https://doi.org/10.3390/cryst10070602 - 11 Jul 2020

Cited by 15 | Viewed by 4835

Abstract

Layered Double Hydroxides (LDHs) are a relevant class of inorganic lamellar nanomaterials that have attracted significant interest in life science-related applications, due to their highly controllable synthesis and high biocompatibility. Under a general point of view, this class of materials might have played an important role for the origin of life on planet Earth, given their ability to adsorb and concentrate life-relevant molecules in sea environments. It has been speculated that the organic–mineral interactions could have permitted to organize the adsorbed molecules, leading to an increase in their local concentration and finally to the emergence of life. Inspired by nature, material scientists, engineers and chemists have started to leverage the ability of LDHs to absorb and concentrate molecules and biomolecules within life-like compartments, allowing to realize highly-efficient bioinspired platforms, usable for bioanalysis, therapeutics, sensors and bioremediation. This review aims at summarizing the latest evolution of LDHs in this research field under an unprecedented perspective, finally providing possible challenges and directions for future research. Full article

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43 pages, 7846 KiB

Open AccessEditor’s ChoiceReview

Layered Double Hydroxides: A Toolbox for Chemistry and Biology

by Giuseppe Arrabito, Aurelio Bonasera, Giuseppe Prestopino, Andrea Orsini, Alessio Mattoccia, Eugenio Martinelli, Bruno Pignataro and Pier Gianni Medaglia

Crystals 2019, 9(7), 361; https://doi.org/10.3390/cryst9070361 - 15 Jul 2019

Cited by 65 | Viewed by 17857

Abstract

Layered double hydroxides (LDHs) are an emergent class of biocompatible inorganic lamellar nanomaterials that have attracted significant research interest owing to their high surface-to-volume ratio, the capability to accumulate specific molecules, and the timely release to targets. Their unique properties have been employed for applications in organic catalysis, photocatalysis, sensors, drug delivery, and cell biology. Given the widespread contemporary interest in these topics, time-to-time it urges to review the recent progresses. This review aims to summarize the most recent cutting-edge reports appearing in the last years. It firstly focuses on the application of LDHs as catalysts in relevant chemical reactions and as photocatalysts for organic molecule degradation, water splitting reaction, CO₂ conversion, and reduction. Subsequently, the emerging role of these materials in biological applications is discussed, specifically focusing on their use as biosensors, DNA, RNA, and drug delivery, finally elucidating their suitability as contrast agents and for cellular differentiation. Concluding remarks and future prospects deal with future applications of LDHs, encouraging researches in better understanding the fundamental mechanisms involved in catalytic and photocatalytic processes, and the molecular pathways that are activated by the interaction of LDHs with cells in terms of both uptake mechanisms and nanotoxicology effects. Full article

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