Special Issue "Layered Double Hydroxide-Based Nanomaterials – From Fundamentals to Applications"

A special issue of Nanomaterials (ISSN 2079-4991).

Deadline for manuscript submissions: closed (31 December 2018).

Special Issue Editor

Dr. István Szilágyi
Website
Guest Editor
Department of Physical Chemistry and Materials Science, Faculty of Science and Informatics, University of Szeged, 1 Rerrich Béla tér, 6720 Szeged, Hungary
Interests: nanoparticle; polyelectrolyte; biocatalysis; ionic liquid; colloidal stability
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Special Issue Information

Dear Colleagues,

In the past decades, layered double hydroxides (LDHs) and their derivatives became one of the most important inorganic nanomaterials due to their biocompatibility, compositional diversity and possible delamination into two-dimensional unilamellar nanosheets. They are multifunctional materials, applications include sensing, catalysis, biomedical delivery, water treatment and development of novel hybrid nanocomposites. Due to the widespread contemporary interest in LDH-based materials in the scientific and technological communities, major efforts are being made on investigating the fundamental properties of these materials in order to optimize their use in more applied disciplines.The aim of this Special Issue is to present the most recent results concerning the synthesis, characterization and application of LDH-based nanomaterials. The targeted topics involve, but are not limited to, the following:

  • Synthesis of novel LDHs of diverse composition
  • Fundamental properties of LDHs in dispersion and solid state
  • Novel methodologies to study the structure of LDH materials
  • Colloid chemistry of LDHs
  • Development of polymer-LDH nanocomposites
  • Delamination of LDHs into unilamellar nanosheets
  • Preparation of LDH hybrids by intercalation
  • Design of LDH-based bionanomaterials
  • Interaction of LDHs with constituents of biological systems
  • Application of LDHs and their composites

Dr. István Szilágyi
Guest Editor

Manuscript Submission Information

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Keywords

  • layered double hydroxide
  • intercalation
  • delamination
  • aggregation
  • anion exchange
  • application
  • synthesis
  • nanocomposite
  • biomaterials
  • surface modification

Published Papers (8 papers)

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Editorial

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Open AccessEditorial
Layered Double Hydroxide-Based Nanomaterials-From Fundamentals to Applications
Nanomaterials 2019, 9(8), 1174; https://doi.org/10.3390/nano9081174 - 16 Aug 2019
Abstract
Layered double hydroxides (LDHs) and their composites with various substances represent an important class of materials suitable for several existing and future applications in biological, chemical, and environmental processes [...] Full article

Research

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Open AccessArticle
Potential Sustainable Slow-Release Fertilizers Obtained by Mechanochemical Activation of MgAl and MgFe Layered Double Hydroxides and K2HPO4
Nanomaterials 2019, 9(2), 183; https://doi.org/10.3390/nano9020183 - 01 Feb 2019
Cited by 4
Abstract
This study describes the behavior of potential slow-release fertilizers (SRF), prepared by the mechanochemical activation of calcined Mg2Al-CO3 or Mg2Fe-CO3 layered double hydroxides (LDH) mixed with dipotassium hydrogen phosphate (K2HPO4). The effects of [...] Read more.
This study describes the behavior of potential slow-release fertilizers (SRF), prepared by the mechanochemical activation of calcined Mg2Al-CO3 or Mg2Fe-CO3 layered double hydroxides (LDH) mixed with dipotassium hydrogen phosphate (K2HPO4). The effects of LDH thermal treatment on P/K release behavior were investigated. Characterizations of the inorganic composites before and after release experiments combined X-Ray diffraction (XRD), Fourier-transform infra-red spectroscopy (FTIR), solid-state nuclear magnetic resonance (NMR), scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX). The best release profile (<75% in 28 days and at least 75% release) was obtained for MgAl/K2HPO4 (9 h milling, 2:1 molar ratio, MR). Compared to readily used K2HPO4, milling orthophosphate into LDH matrices decreases its solubility and slows down its release, with 60% and 5.4% release after 168 h for MgAl/K2HPO4 and MgFe/K2HPO4 composites, respectively. Mechanochemical addition of carboxymethylcellulose to the LDH/K2HPO4 composites leads to a noticeable improvement of P release properties. Full article
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Open AccessArticle
Enhancing PD-1 Gene Silence in T Lymphocytes by Comparing the Delivery Performance of Two Inorganic Nanoparticle Platforms
Nanomaterials 2019, 9(2), 159; https://doi.org/10.3390/nano9020159 - 28 Jan 2019
Cited by 29
Abstract
Suitable carriers are crucial to RNAi applications for cancer genotherapy and T-cell immunotherapy. In this research, we selected two extensively-investigated biocompatible inorganic nanoparticle carriers, i.e., layered double hydroxide (LDH) and lipid-coated calcium phosphate (LCP) and then compared their efficacy for siRNA delivery in [...] Read more.
Suitable carriers are crucial to RNAi applications for cancer genotherapy and T-cell immunotherapy. In this research, we selected two extensively-investigated biocompatible inorganic nanoparticle carriers, i.e., layered double hydroxide (LDH) and lipid-coated calcium phosphate (LCP) and then compared their efficacy for siRNA delivery in T cells, in order to understand which carrier is more efficient in delivering functional programmed cell death protein 1 siRNA (PD-1 siRNA) to suspended T lymphocytes. Both LDH and LCP nanoparticles quickly delivered gene segment to mouse T cell lines (EL4), while the LCP nanoparticles exhibited more cellular uptake and higher PD-1 gene silence efficiency. We further demonstrated that LCP nanoparticles successfully reduced the expression of PD-1 in human ex vivo tumor infiltrating lymphocytes (TILs). Thus, LCP nanoparticles can be used as a better nano-carrier for gene therapy in lymphocytes, especially in regards to TIL-related cancer immunotherapy. Full article
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Open AccessArticle
Effect of Polyelectrolyte Mono- and Bilayer Formation on the Colloidal Stability of Layered Double Hydroxide Nanoparticles
Nanomaterials 2018, 8(12), 986; https://doi.org/10.3390/nano8120986 - 28 Nov 2018
Cited by 5
Abstract
Sequential adsorption of polyelectrolytes on nanoparticles is a popular method to obtain thin films after deposition. However, the effect of polyelectrolyte multilayer formation on the colloidal stability of the nanoparticles has not been studied in detail. In the present work, layered double hydroxides [...] Read more.
Sequential adsorption of polyelectrolytes on nanoparticles is a popular method to obtain thin films after deposition. However, the effect of polyelectrolyte multilayer formation on the colloidal stability of the nanoparticles has not been studied in detail. In the present work, layered double hydroxides (LDH) were synthesized and interaction with oppositely and like-charged polyelectrolytes was investigated. Electrophoretic and light scattering measurements revealed that colloidal stability of LDH can be tuned by adsorption of poly(styrene sulfonate) (PSS) on the oppositely charged LDH surface in appropriate doses and thus, unstable or stable dispersions can be designed. Negatively charged LDH of adsorbed PSS monolayer was obtained and a poly(diallyldimethyl ammonium chloride) (PDADMAC) second layer was systematically built on the particles. The obtained polyelectrolyte bilayer provided high colloidal stability for the LDH-PSS-PDADMAC dispersions due to the presence of repulsive interparticle forces of electrostatic and steric origin. The results provide crucial quantitative information on designing highly stable particle-polyelectrolyte systems for the preparation of thin films or immobilization of guest substances between the layers for delivery processes. Full article
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Open AccessArticle
Enhanced Oxygen Vacancies in a Two-Dimensional MnAl-Layered Double Oxide Prepared via Flash Nanoprecipitation Offers High Selective Catalytic Reduction of NOx with NH3
Nanomaterials 2018, 8(8), 620; https://doi.org/10.3390/nano8080620 - 15 Aug 2018
Cited by 11
Abstract
A two-dimensional MnAl-layered double oxide (LDO) was obtained by flash nanoprecipitation method (FNP) and used for the selective catalytic reduction of NOx with NH3. The MnAl-LDO (FNP) catalyst formed a particle size of 114.9 nm. Further characterization exhibited rich oxygen [...] Read more.
A two-dimensional MnAl-layered double oxide (LDO) was obtained by flash nanoprecipitation method (FNP) and used for the selective catalytic reduction of NOx with NH3. The MnAl-LDO (FNP) catalyst formed a particle size of 114.9 nm. Further characterization exhibited rich oxygen vacancies and strong redox property to promote the catalytic activity at low temperature. The MnAl-LDO (FNP) catalyst performed excellent NO conversion above 80% at the temperature range of 100–400 °C, and N2 selectivity above 90% below 200 °C, with a gas hourly space velocity (GHSV) of 60,000 h−1, and a NO concentration of 500 ppm. The maximum NO conversion is 100% at 200 °C; when the temperature in 150–250 °C, the NO conversion can also reach 95%. The remarkable low-temperature catalytic performance of the MnAl-LDO (FNP) catalyst presented potential applications for controlling NO emissions on the account of the presentation of oxygen vacancies. Full article
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Open AccessArticle
The Adsorption of Dextranase onto Mg/Fe-Layered Double Hydroxide: Insight into the Immobilization
Nanomaterials 2018, 8(3), 173; https://doi.org/10.3390/nano8030173 - 19 Mar 2018
Cited by 5
Abstract
We report the adsorption of dextranase on a Mg/Fe-layered double hydroxide (Mg/Fe-LDH). We focused the effects of different buffers, pH, and amino acids. The Mg/Fe-LDH was synthesized, and adsorption experiments were performed to investigate the effects. The maximum adsorption occurred in pH 7.0 [...] Read more.
We report the adsorption of dextranase on a Mg/Fe-layered double hydroxide (Mg/Fe-LDH). We focused the effects of different buffers, pH, and amino acids. The Mg/Fe-LDH was synthesized, and adsorption experiments were performed to investigate the effects. The maximum adsorption occurred in pH 7.0 4-(2-hydroxyethyl)-1-piperazineethanesulfonic acid (HEPES) buffer, and the maximum dextranase adsorption uptake was 1.38 mg/g (416.67 U/mg); histidine and phenylalanine could affect the adsorption. A histidine tag could be added to the protein to increase the adsorption significantly. The performance features and mechanism were investigated with X-ray diffraction patterns (XRD) and Fourier transform infrared spectra (FTIR). The protein could affect the crystal structure of LDH, and the enzyme was adsorbed on the LDH surface. The main interactions between the protein and LDH were electrostatic and hydrophobic. Histidine and phenylalanine could significantly affect the adsorption. The hexagonal morphology of LDH was not affected after adsorption. Full article
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Review

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Open AccessReview
Applications of Mechanochemically Prepared Layered Double Hydroxides as Adsorbents and Catalysts: A Mini-Review
Nanomaterials 2019, 9(1), 80; https://doi.org/10.3390/nano9010080 - 08 Jan 2019
Cited by 10
Abstract
Mechanochemically prepared layered double hydroxide (M-LDH), which usually possesses high surface chemical activity and a substantial amount of surface defects, has presented outstanding application performance especially in the area of environmental protection. Recently published works on the mechanochemical synthesis of LDH were first [...] Read more.
Mechanochemically prepared layered double hydroxide (M-LDH), which usually possesses high surface chemical activity and a substantial amount of surface defects, has presented outstanding application performance especially in the area of environmental protection. Recently published works on the mechanochemical synthesis of LDH were first introduced to provide a comprehensive summary on the preparation of the materials. Ensuing discussion provided an overview of recent research on the applications of M-LDH products as adsorbents and catalysts. The excellent adsorption performance and fast adsorption rate of the precursor of LDH produced by dry milling of raw materials was identified. The catalytic performances of M-LDH as catalysts, mainly photocatalysts, were then introduced. It is foreseeable that by rational utilization of mechanochemical processes and the unique chemical properties of M-LDH, increasing numbers of applications using M-LDH could be expected. Full article
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Open AccessReview
Research Progress of NiMn Layered Double Hydroxides for Supercapacitors: A Review
Nanomaterials 2018, 8(10), 747; https://doi.org/10.3390/nano8100747 - 20 Sep 2018
Cited by 24
Abstract
The research on supercapacitors has been attractive due to their large power density, fast charge/discharge speed and long lifespan. The electrode materials for supercapacitors are thus intensively investigated to improve the electrochemical performances. Various transition metal layered double hydroxides (LDHs) with a hydrotalcite-like [...] Read more.
The research on supercapacitors has been attractive due to their large power density, fast charge/discharge speed and long lifespan. The electrode materials for supercapacitors are thus intensively investigated to improve the electrochemical performances. Various transition metal layered double hydroxides (LDHs) with a hydrotalcite-like structure have been developed to be promising electrode materials. Earth-abundant metal hydroxides are very suitable electrode materials due to the low cost and high specific capacity. This is a review paper on NiMn LDHs for supercapacitor application. We focus particularly on the recent published papers using NiMn LDHs as electrode materials for supercapacitors. The preparation methods for NiMn LDHs are introduced first. Then, the structural design and chemical modification of NiMn LDH materials, as well as the composites and films derived from NiMn LDHs are discussed. These approaches are proven to be effective to enhance the performance of supercapacitor. Finally, the reports related to NiMn LDH-based asymmetric supercapacitors are summarized. A brief discussion of the future development of NiMn LDHs is also provided. Full article
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