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Recent Research Advance in the Halloysite Nanotubes Field

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (28 February 2023) | Viewed by 24840

Special Issue Editors

Department of Chemistry, University of Catania, Via Andrea Doria, 6, 95125 Catania, Italy
Interests: organic chemistry; synthesis; drug delivery; coniugates; hallosyte nanotubes; carrier systems; nanomaterials; biocompatible materials
Special Issues, Collections and Topics in MDPI journals
Department of Biological, Chemical and Pharmaceutical Sciences and Technologies, University of Palermo, Palermo, Italy
Interests: clay minerals; halloysite nanotubes; surface modification
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Halloysite (HNT) is a promising natural nanosized tubular clay mineral that has many important uses in different industrial fields. It is naturally occurring, biocompatible, and available in thousands of tons at low cost. As a consequence of a hollow cavity, HNT is mainly used as nanocontainer for the controlled release of several chemicals. The surface chemistry of HNTs is versatile for the targeted chemical modification of the inner lumen and outer surface and opens up several strategies to obtain novel nanomaterials of potential practical interest.

This Special Issue is focused on current research on halloysite-based nanomaterial from the state-of-the-art to the most recent advancements, with a special focus on the design of modified halloysite hybrids and their applications in biomedical, bioremediation, food packaging, and polymeric fields. Original contributions addressing the synthesis and characterization of HNT hybrids and related mechanisms involved in adsorption and release of active molecules, and/or metal nanoparticles as well as practical biological, industrial, or environmental applications, in the form of full papers or communications, are welcome. Mini-reviews presenting an overview of the state-of-the-art with projections on future perspectives and trends in this domain will also be considered.

Assoc. Prof. Dr. Serena Riela
Dr. Marina Massaro
Guest Editors

Manuscript Submission Information

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Keywords

  • Halloysite nanotubes
  • HNT modification
  • Catalytic supports
  • Drug carrier and delivery
  • Filler for polymeric matrices

Published Papers (5 papers)

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Research

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17 pages, 5247 KiB  
Article
Cell Membrane-Coated Halloysite Nanotubes for Target-Specific Nanocarrier for Cancer Phototherapy
by Cuiying Tan, Jingqi Zheng, Yue Feng and Mingxian Liu
Molecules 2021, 26(15), 4483; https://doi.org/10.3390/molecules26154483 - 25 Jul 2021
Cited by 11 | Viewed by 2199
Abstract
Naturally-occurring halloysite nanotubes (HNTs) have many advantages for constructing target-specific delivery of phototherapeutic agents. Here, HNTs were labeled with fluorescein isothiocyanate (FITC) and loaded with the type-II photosensitizer indocyanine green (ICG) for phototherapy. HNTs-FITC-ICG was structurally stable due to presence of HNTs as [...] Read more.
Naturally-occurring halloysite nanotubes (HNTs) have many advantages for constructing target-specific delivery of phototherapeutic agents. Here, HNTs were labeled with fluorescein isothiocyanate (FITC) and loaded with the type-II photosensitizer indocyanine green (ICG) for phototherapy. HNTs-FITC-ICG was structurally stable due to presence of HNTs as the nanocarrier and protective agent. The nanocarrier was further wrapped with red blood cell membrane (RBCM) to enhance the biocompatibility. The HNTs-FITC-ICG-RBCM nanocarrier show high cytocompatibility and hemocompatibility. Due to the photothermal effect of ICG, a significant temperature rising was achieved by irradiation of the nanocarrier using 808 nm laser. The photothermal temperature rising was used to kill the cancer cells effectively. The HNTs-FITC-ICG-RBCM nanocarrier was further linked with anti-EpCAM to endow it with targeting therapy performance against breast cancer, and the anti-EpCAM-conjugated nanocarrier exhibited significantly tumor-specific accumulation. The RBCM-coated and biocompatible HNTs nanocarrier is a promising candidate for target-specific therapy of cancer. Full article
(This article belongs to the Special Issue Recent Research Advance in the Halloysite Nanotubes Field)
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9 pages, 3259 KiB  
Article
Theoretical Study of Retinol, Niacinamide and Glycolic Acid with Halloysite Clay Mineral as Active Ingredients for Topical Skin Care Formulations
by Ana Borrego-Sánchez, Claro Ignacio Sainz-Díaz, Luana Perioli and César Viseras
Molecules 2021, 26(15), 4392; https://doi.org/10.3390/molecules26154392 - 21 Jul 2021
Cited by 8 | Viewed by 5562
Abstract
The adsorption of retinol, niacinamide and glycolic acid active ingredients on the internal surface of halloysite in an aqueous environment was explored at the molecular level by means of calculations based on quantum mechanics and force fields from empirical interatomic potentials. These active [...] Read more.
The adsorption of retinol, niacinamide and glycolic acid active ingredients on the internal surface of halloysite in an aqueous environment was explored at the molecular level by means of calculations based on quantum mechanics and force fields from empirical interatomic potentials. These active ingredients are stably adsorbed on the internal surface of halloysite forming hydrogen bonds between the hydrogen, oxygen and nitrogen atoms with the hydroxyl groups of the inner surface of the halloysite. In addition, electrostatic interaction between these active ingredients with the water molecules was observed. Therefore, the theoretical results indicate that the adsorption of these active principles is favourable in the halloysite nanotube, which allows directing future experimental investigations for the development and design of retinol, niacinamide and glycolic acid with halloysite nanotubes systems, which may be topical formulations for skincare. Full article
(This article belongs to the Special Issue Recent Research Advance in the Halloysite Nanotubes Field)
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19 pages, 2960 KiB  
Article
Facile Fabrication of Natural Polyelectrolyte-Nanoclay Composites: Halloysite Nanotubes, Nucleotides and DNA Study
by Svetlana Batasheva, Marina Kryuchkova, Ramil Fakhrullin, Giuseppe Cavallaro, Giuseppe Lazzara, Farida Akhatova, Läysän Nigamatzyanova, Vladimir Evtugyn, Elvira Rozhina and Rawil Fakhrullin
Molecules 2020, 25(15), 3557; https://doi.org/10.3390/molecules25153557 - 04 Aug 2020
Cited by 22 | Viewed by 3826
Abstract
Complexation of biopolymers with halloysite nanotubes (HNTs) can greatly affect their applicability as materials building blocks. Here we have performed a systematic investigation of fabrication of halloysite nanotubes complexes with nucleotides and genomic DNA. The binding of DNA and various nucleotide species (polyAU, [...] Read more.
Complexation of biopolymers with halloysite nanotubes (HNTs) can greatly affect their applicability as materials building blocks. Here we have performed a systematic investigation of fabrication of halloysite nanotubes complexes with nucleotides and genomic DNA. The binding of DNA and various nucleotide species (polyAU, UMP Na2, ADP Na3, dATP Na, AMP, uridine, ATP Mg) by halloysite nanotubes was tested using UV-spectroscopy. The study revealed that binding of different nucleotides to the nanoclay varied but was low both in the presence and absence of MgCl2, while MgCl2 facilitated significantly the binding of longer molecules such as DNA and polyAU. Modification of the nanotubes with DNA and nucleotide species was further confirmed by measurements of ζ-potentials. DNA-Mg-modified nanotubes were characterized using transmission electron (TEM), atomic force (AFM) and hyperspectral microscopies. Thermogravimetric analysis corroborated the sorption of DNA by the nanotubes, and the presence of DNA on the nanotube surface was indicated by changes in the surface adhesion force measured by AFM. DNA bound by halloysite in the presence of MgCl2 could be partially released after addition of phosphate buffered saline. DNA binding and release from halloysite nanotubes was tested in the range of MgCl2 concentrations (10–100 mM). Even low MgCl2 concentrations significantly increased DNA sorption to halloysite, and the binding was leveled off at about 60 mM. DNA-Mg-modified halloysite nanotubes were used for obtaining a regular pattern on a glass surface by evaporation induced self-assembly process. The obtained spiral-like pattern was highly stable and resisted dissolution after water addition. Our results encompassing modification of non-toxic clay nanotubes with a natural polyanion DNA will find applications for construction of gene delivery vehicles and for halloysite self-assembly on various surfaces (such as skin or hair). Full article
(This article belongs to the Special Issue Recent Research Advance in the Halloysite Nanotubes Field)
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11 pages, 2802 KiB  
Article
Ruthenium-Loaded Halloysite Nanotubes as Mesocatalysts for Fischer–Tropsch Synthesis
by Anna Stavitskaya, Kristina Mazurova, Mikhail Kotelev, Oleg Eliseev, Pavel Gushchin, Aleksandr Glotov, Ruslan Kazantsev, Vladimir Vinokurov and Yuri Lvov
Molecules 2020, 25(8), 1764; https://doi.org/10.3390/molecules25081764 - 11 Apr 2020
Cited by 28 | Viewed by 4144
Abstract
Halloysite aluminosilicate nanotubes loaded with ruthenium particles were used as reactors for Fischer–Tropsch synthesis. To load ruthenium inside clay, selective modification of the external surface with ethylenediaminetetraacetic acid, urea, or acetone azine was performed. Reduction of materials in a flow of hydrogen at [...] Read more.
Halloysite aluminosilicate nanotubes loaded with ruthenium particles were used as reactors for Fischer–Tropsch synthesis. To load ruthenium inside clay, selective modification of the external surface with ethylenediaminetetraacetic acid, urea, or acetone azine was performed. Reduction of materials in a flow of hydrogen at 400 °C resulted in catalysts loaded with 2 wt.% of 3.5 nm Ru particles, densely packed inside the tubes. Catalysts were characterized by N2-adsorption, temperature-programmed desorption of ammonia, transmission electron microscopy, X-ray fluorescence, and X-ray diffraction analysis. We concluded that the total acidity and specific morphology of reactors were the major factors influencing activity and selectivity toward CH4, C2–4, and C5+ hydrocarbons in the Fischer–Tropsch process. Use of ethylenediaminetetraacetic acid for ruthenium binding gave a methanation catalyst with ca. 50% selectivity to methane and C2–4. Urea-modified halloysite resulted in the Ru-nanoreactors with high selectivity to valuable C5+ hydrocarbons containing few olefins and a high number of heavy fractions (α = 0.87). Modification with acetone azine gave the slightly higher CO conversion rate close to 19% and highest selectivity in C5+ products. Using a halloysite tube with a 10–20-nm lumen decreased the diffusion limitation and helped to produce high-molecular-weight hydrocarbons. The extremely small C2–C4 fraction obtained from the urea- and azine-modified sample was not reachable for non-templated Ru-nanoparticles. Dense packing of Ru nanoparticles increased the contact time of olefins and their reabsorption, producing higher amounts of C5+ hydrocarbons. Loading of Ru inside the nanoclay increased the particle stability and prevented their aggregation under reaction conditions. Full article
(This article belongs to the Special Issue Recent Research Advance in the Halloysite Nanotubes Field)
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Review

Jump to: Research

44 pages, 14772 KiB  
Review
Past, Present and Future Perspectives on Halloysite Clay Minerals
by Marina Massaro, Renato Noto and Serena Riela
Molecules 2020, 25(20), 4863; https://doi.org/10.3390/molecules25204863 - 21 Oct 2020
Cited by 86 | Viewed by 8189
Abstract
Halloysite nanotubes (HNTs), clay minerals belonging to the kaolin groups, are emerging nanomaterials which have attracted the attention of the scientific community due to their interesting features, such as low-cost, availability and biocompatibility. In addition, their large surface area and tubular structure have [...] Read more.
Halloysite nanotubes (HNTs), clay minerals belonging to the kaolin groups, are emerging nanomaterials which have attracted the attention of the scientific community due to their interesting features, such as low-cost, availability and biocompatibility. In addition, their large surface area and tubular structure have led to HNTs’ application in different industrial purposes. This review reports a comprehensive overview of the historical background of HNT utilization in the last 20 years. In particular it will focus on the functionalization of the surfaces, both supramolecular and covalent, following applications in several fields, including biomedicine, environmental science and catalysis. Full article
(This article belongs to the Special Issue Recent Research Advance in the Halloysite Nanotubes Field)
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