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Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications

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A special issue of Nanomaterials (ISSN 2079-4991). This special issue belongs to the section "Synthesis, Interfaces and Nanostructures".

Deadline for manuscript submissions: closed (31 December 2020) | Viewed by 38940

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Prof. Dr. Rafał Jakub Wiglusz

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1. Institute of Low Temperature and Structure Research, Polish Academy of Sciences, 00-901 Warszawa, Poland
2. Department of Organic Chemistry, Bioorganic Chemistry and Biotechnology, Faculty of Chemistry, Silesian University of Technology, 44100 Gliwice, Poland
Interests: biomaterials; biomimetics; biopolymers; hydrogels; nanomedicine
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Dear Colleagues,

In recent years, inorganic nanocrystalline materials activated by rare-earth ions (RE³⁺) have attracted a great deal of attention due to their potential applications as luminophores, up-converting materials, laser materials, and immunologic scavengers, as well as biomedical materials.

The goals of Special Issue of "Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications" will be achieved by the preparation of nanometer-sized materials doped and co-doped with rare earth ions followed by the creation of periodically ordered nanostructures based on single nanoparticles. A small particle size implies high sensitivity and selectivity. These new effects and possibilities are mainly due to quantum effects that are a result of the increasing ratio of surface to volume atoms in low-dimensional systems. An important factor in this context so far has been the design and fabrication of nanocomponents with/displaying new functionalities and characteristics for the improvement of existing materials; including photonic materials, conductive materials, polymers and biocomposites. With this concept of nanotechnology in mind, the aim of the Special Issue should be covered by innovative products and application options in electronics and biomedicine, based solely on nanoscale technology.

Topics to be covered in this Special Issue include:

Technology and applications of nanomaterials with rare earth ions,
Advanced physicochemical properties, characterization and modification of nanomaterials with rare earth ions,
Novel active materials, especially organic and inorganic materials, nanocrystalline materials, nanoceramics doped and co-doped with rare-earth ions with bio-related and emerging applications
Magnetic properties of nano-sized rare-earth compounds;
Applications of nano-sized rare earth doped and co-doped optical materials

Prof. Dr. Rafał Jakub Wiglusz
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Nanomaterials is an international peer-reviewed open access semimonthly journal published by MDPI.

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Keywords

Organic and Inorganic Nanomaterials
Rare earth ions
Biofunctionalization and Biomodification
Synthesis and Preparation
Bioimaging
Biosensors
Cytotoxicity
Energy transfer
Luminescence
Nanocomposites
Nanoceramics
Phosphors
Spectroscopic and optical properties
Magnetic nanomaterials
Thin films
Up-conversion
Down-conversion

Published Papers (12 papers)

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Editorial

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6 pages, 241 KiB

Open AccessEditorial

Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications

by Rafal J. Wiglusz

Nanomaterials 2021, 11(7), 1848; https://doi.org/10.3390/nano11071848 - 16 Jul 2021

Cited by 3 | Viewed by 1836

Abstract

The success of nanotechnology in the field of physical, chemical and medical sciences has started revolutionizing the drug delivery science and theranostics (therapy and diagnostics) [...] Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

Research

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17 pages, 4973 KiB

Open AccessArticle

Quenching of the Eu³⁺ Luminescence by Cu²⁺ Ions in the Nanosized Hydroxyapatite Designed for Future Bio-Detection

by Katarzyna Szyszka, Sara Targońska, Agnieszka Lewińska, Adam Watras and Rafal J. Wiglusz

Nanomaterials 2021, 11(2), 464; https://doi.org/10.3390/nano11020464 - 11 Feb 2021

Cited by 17 | Viewed by 2509

Abstract

The hydroxyapatite nanopowders of the Eu³⁺-doped, Cu²⁺-doped, and Eu³⁺/Cu²⁺-co-doped Ca₁₀(PO₄)₆(OH)₂ were prepared by a microwave-assisted hydrothermal method. The structural and morphological properties of the products were investigated by X-ray powder diffraction (XRD), transmission electron microscopy techniques (TEM), and infrared spectroscopy (FT-IR). The average crystal size and the unit cell parameters were calculated by a Rietveld refinement tool. The absorption, emission excitation, emission, and luminescence decay time were recorded and studied in detail. The ⁵D₀ → ⁷F₂ transition is the most intense transition. The Eu³⁺ ions occupied two independent crystallographic sites in these materials exhibited in emission spectra: one Ca(1) site with C₃ symmetry and one Ca(2) sites with C_s symmetry. The Eu³⁺ emission is strongly quenched by Cu²⁺ ions, and the luminescence decay time is much shorter in the case of Eu³⁺/Cu²⁺ co-doped materials than in Eu³⁺-doped materials. The luminescence quenching mechanism as well as the schematic energy level diagram showing the Eu³⁺ emission quenching mechanism using Cu²⁺ ions are proposed. The electron paramagnetic resonance (EPR) technique revealed the existence of at least two different coordination environments for copper(II) ion. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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13 pages, 1894 KiB

Open AccessArticle

Mechanistic Insight of Sensing Hydrogen Phosphate in Aqueous Medium by Using Lanthanide(III)-Based Luminescent Probes

by Jashobanta Sahoo, Santlal Jaiswar, Pabitra B. Chatterjee, Palani S. Subramanian and Himanshu Sekhar Jena

Nanomaterials 2021, 11(1), 53; https://doi.org/10.3390/nano11010053 - 28 Dec 2020

Cited by 5 | Viewed by 2596

Abstract

The development of synthetic lanthanide luminescent probes for selective sensing or binding anions in aqueous medium requires an understanding of how these anions interact with synthetic lanthanide probes. Synthetic lanthanide probes designed to differentiate anions in aqueous medium could underpin exciting new sensing tools for biomedical research and drug discovery. In this direction, we present three mononuclear lanthanide-based complexes, EuLCl₃ (1), SmLCl₃ (2), and TbLCl₃ (3), incorporating a hexadentate aminomethylpiperidine-based nitrogen-rich heterocyclic ligand L for sensing anion and establishing mechanistic insight on their binding activities in aqueous medium. All these complexes are meticulously studied for their preferential selectivities towards different anions such as HPO₄²⁻, SO₄²⁻, CH₃COO⁻, I⁻, Br⁻, Cl⁻, F⁻, NO₃⁻, CO₃²⁻/HCO₃⁻, and HSO₄⁻ at pH 7.4 in aqueous HEPES (2-[4-(2-hydroxyethyl)piperazin-1-yl]ethanesulfonic acid) buffer. Among the anions scanned, HPO₄²⁻ showed an excellent luminescence change with all three complexes. Job’s plot and ESI-MS support the 1:2 association between the receptors and HPO₄²⁻. Systematic spectrophotometric titrations of 1–3 against HPO₄²⁻ demonstrates that the emission intensities of 1 and 2 were enhanced slightly upon the addition of HPO₄²⁻ in the range 0.01–1 equiv and 0.01–2 equiv., respectively. Among the three complexes, complex 3 showed a steady quenching of luminescence throughout the titration of hydrogen phosphate. The lower and higher detection limits of HPO₄²⁻ by complexes 1 and 2 were determined as 0.1–4 mM and 0.4–3.2 mM, respectively, while complex 3 covered 0.2–100 μM. This concludes that all complexes demonstrated a high degree of sensitivity and selectivity towards HPO₄²⁻. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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15 pages, 5881 KiB

Open AccessArticle

Investigation of Physicochemical Properties of the Structurally Modified Nanosized Silicate-Substituted Hydroxyapatite Co-Doped with Eu³⁺ and Sr²⁺ Ions

by Sara Targonska and Rafal J. Wiglusz

Nanomaterials 2021, 11(1), 27; https://doi.org/10.3390/nano11010027 - 24 Dec 2020

Cited by 8 | Viewed by 1769

Abstract

In this paper, a series of structurally modified silicate-substituted apatite co-doped with Sr²⁺ and Eu³⁺ ions were synthesized by a microwave-assisted hydrothermal method. The concentration of Sr²⁺ ions was set at 2 mol% and Eu³⁺ ions were established in the range of 0.5–2 mol% in a molar ratio of calcium ion amount. The XRD (X-ray powder diffraction) technique and infrared (FT-IR) spectroscopy were used to characterize the obtained materials. The Kröger–Vink notation was used to explain the possible charge compensation mechanism. Moreover, the study of the spectroscopic properties (emission, emission excitation and emission kinetics) of the obtained materials as a function of optically active ions and annealing temperature was carried out. The luminescence behavior of Eu³⁺ ions in the apatite matrix was verified by the Judd–Ofelt (J-O) theory and discussed in detail. The temperature-dependent emission spectra were recorded for the representative materials. Furthermore, the International Commission on Illumination (CIE) chromaticity coordinates and correlated color temperature were determined by the obtained results. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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21 pages, 6756 KiB

Open AccessArticle

The Influence of Ozonated Olive Oil-Loaded and Copper-Doped Nanohydroxyapatites on Planktonic Forms of Microorganisms

by Wojciech Zakrzewski, Maciej Dobrzynski, Joanna Nowicka, Magdalena Pajaczkowska, Maria Szymonowicz, Sara Targonska, Paulina Sobierajska, Katarzyna Wiglusz, Wojciech Dobrzynski, Adam Lubojanski, Sebastian Fedorowicz, Zbigniew Rybak and Rafal J. Wiglusz

Nanomaterials 2020, 10(10), 1997; https://doi.org/10.3390/nano10101997 - 10 Oct 2020

Cited by 10 | Viewed by 2877

Abstract

The research has been carried out with a focus on the assessment of the antimicrobial efficacy of pure nanohydroxyapatite, Cu²⁺-doped nanohydroxyapatite, ozonated olive oil-loaded nanohydroxyapatite, and Cu²⁺-doped nanohydroxyapatite, respectively. Their potential antimicrobial activity was investigated against Streptococcus mutans, Lactobacillus rhamnosus, and Candida albicans. Among all tested materials, the highest efficacy was observed in terms of ozonated olive oil. The studies were performed using an Ultraviolet–Visible spectrophotometry (UV-Vis), electron microscopy, and statistical methods, by determining the value of Colony-Forming Units (CFU/mL) and Minimal Inhibitory Concentration (MIC). Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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14 pages, 3911 KiB

Open AccessFeature PaperArticle

Preparation and Characterization of Self-Assembled Poly(l-Lactide) on the Surface of β-Tricalcium Diphosphate(V) for Bone Tissue Theranostics

by Jan A. Zienkiewicz, Adam Strzep, Dawid Jedrzkiewicz, Nicole Nowak, Justyna Rewak-Soroczynska, Adam Watras, Jolanta Ejfler and Rafal J. Wiglusz

Nanomaterials 2020, 10(2), 331; https://doi.org/10.3390/nano10020331 - 15 Feb 2020

Cited by 5 | Viewed by 2684

Abstract

This work was aimed to obtain and characterize the well-defined biocomposites based on β-tricalcium diphosphate(V) (β-TCP) co-doped with Ce³⁺ and Pr³⁺ ions modified by poly(l-lactide) (PLLA) with precise tailored chain length and different phosphate to polymer ratio. The composites as well as β-tricalcium diphosphate(V) were spectroscopically characterized using emission spectroscopy and luminescence kinetics. Morphological and structural properties were studied using X-Ray Diffraction (XRD) and Scanning Electron Microscopy (SEM). The self-assembled poly(l-lactide) in a shape of rose flower has been successfully polymerized on the surface of the β-tricalcium diphosphate(V) nanocrystals. The studied materials were evaluated in vitro including cytotoxicity (MTT assay) and hemolysis tests. The obtained results suggested that the studied materials may find potential application in tissue engineering. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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17 pages, 4246 KiB

Open AccessArticle

Investigation of Pyrophosphates KYP₂O₇Co-Doped with Lanthanide Ions Useful for Theranostics

by Adam Watras, Marta Wujczyk, Michael Roecken, Katarzyna Kucharczyk, Krzysztof Marycz and Rafal J. Wiglusz

Nanomaterials 2019, 9(11), 1597; https://doi.org/10.3390/nano9111597 - 11 Nov 2019

Cited by 3 | Viewed by 2277

Abstract

Diphosphate compounds (KYP₂O₇) co-doped with Yb³⁺ and Er³⁺ ions were obtained by one step urea assisted combustion synthesis. The experimental parameters of synthesis were optimized using an experimental design approach related to co-dopants concentration and heattreatment as well as annealing time. The obtained materials were studied with theinitial requirements showing appropriate morphological (X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM)) and spectroscopic properties (emission, luminescence kinetics). Moreover, the effect of Er³⁺ and Yb³⁺ ions doped KYP₂O₇ on morphology, proliferative and metabolic activity and apoptosis in MC3T3-E1 osteoblast cell line and 4B12osteoclasts cell line was investigated. Furthermore, the expression of the common pro-osteogenic markers in MC3T3-E1 osteoblast as well as osteoclastogenesis related markers in 4B12 osteoclasts was evaluated. The extensive in vitro studies showed that KYP₂O₇ doped with 1 mol% Er³⁺ and 20 mol% Yb³⁺ ions positively affected the MC3T3-E1 and 4B12 cells activity without triggering their apoptosis. Moreover, it was shown that an activation of mTOR and Pi3k signaling pathways with 1 mol% Er³⁺, 20 mol% Yb³⁺: KYP₂O₇ can promote the MC3T3-E1 cells expression of late osteogenic markers including RUNX and BMP-2. The obtained data shed a promising light for KYP₂O₇ doped with Er³⁺ and Yb³⁺ ions as a potential factors improving bone fracture healing as well as in bioimaging (so-called in theranostics). Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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14 pages, 3487 KiB

Open AccessArticle

SmS/EuS/SmS Tri-Layer Thin Films: The Role of Diffusion in the Pressure Triggered Semiconductor-Metal Transition

by Andreas Sousanis, Dirk Poelman and Philippe F. Smet

Nanomaterials 2019, 9(11), 1513; https://doi.org/10.3390/nano9111513 - 24 Oct 2019

Cited by 2 | Viewed by 3067

Abstract

While SmS thin films show an irreversible semiconductor-metal transition upon application of pressure, the switching characteristics can be modified by alloying with other elements, such as europium. This manuscript reports on the resistance response of tri-layer SmS/EuS/SmS thin films upon applying pressure and on the correlation between the resistance response and the interdiffusion between the layers. SmS thin films were deposited by e-beam sublimation of Sm in an H₂S atmosphere, while EuS was directly sublimated by e-beam from EuS. Structural properties of the separate thin films were first studied before the deposition of the final nanocomposite tri-layer system. Piezoresistance measurements demonstrated two sharp resistance drops. The first drop, at lower pressure, corresponds to the switching characteristic of SmS. The second drop, at higher pressure, is attributed to EuS, partially mixed with SmS. This behavior provides either a well-defined three or two states system, depending on the degree of mixing. Depth profiling using x-ray photoelectron spectroscopy (XPS) revealed partial diffusion between the compounds upon deposition at a substrate temperature of 400 °C. Thinner tri-layer systems were also deposited to provide more interdiffusion. A higher EuS concentration led to a continuous transition as a function of pressure. This study shows that EuS-modified SmS thin films are possible systems for piezo-electronic devices, such as memory devices, RF (radio frequency) switches and piezoresistive sensors. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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16 pages, 3289 KiB

Open AccessArticle

The Comprehensive Approach to Preparation and Investigation of the Eu³⁺ Doped Hydroxyapatite/poly(L-lactide) Nanocomposites: Promising Materials for Theranostics Application

by Katarzyna Szyszka, Sara Targonska, Malgorzata Gazinska, Konrad Szustakiewicz and Rafal J. Wiglusz

Nanomaterials 2019, 9(8), 1146; https://doi.org/10.3390/nano9081146 - 10 Aug 2019

Cited by 19 | Viewed by 2988

Abstract

In response to the need for new materials for theranostics application, the structural and spectroscopic properties of composites designed for medical applications, received in the melt mixing process, were evaluated. A composite based on medical grade poly(L-lactide) (PLLA) and calcium hydroxyapatite (HAp) doped with Eu³⁺ ions was obtained by using a twin screw extruder. Pure calcium Hap, as well as the one doped with Eu³⁺ ions, was prepared using the precipitation method and then used as a filler. XRPD (X-ray Powder Diffraction) and IR (Infrared) spectroscopy were applied to investigate the structural properties of the obtained materials. DSC (Differential Scanning Calorimetry) was used to assess the Eu³⁺ ion content on phase transitions in PLLA. The tensile properties were also investigated. The excitation, emission spectra as well as decay time were measured to determine the spectroscopic properties. The simplified Judd–Ofelt (J-O) theory was applied and a detailed analysis in connection with the observed structural and spectroscopic measurements was made and described. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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Review

Jump to: Editorial, Research

19 pages, 1100 KiB

Open AccessReview

Nanomaterials Application in Orthodontics

by Wojciech Zakrzewski, Maciej Dobrzynski, Wojciech Dobrzynski, Anna Zawadzka-Knefel, Mateusz Janecki, Karolina Kurek, Adam Lubojanski, Maria Szymonowicz, Zbigniew Rybak and Rafal J. Wiglusz

Nanomaterials 2021, 11(2), 337; https://doi.org/10.3390/nano11020337 - 28 Jan 2021

Cited by 23 | Viewed by 5800

Abstract

Nanotechnology has gained importance in recent years due to its ability to enhance material properties, including antimicrobial characteristics. Nanotechnology is applicable in various aspects of orthodontics. This scientific work focuses on the concept of nanotechnology and its applications in the field of orthodontics, including, among others, enhancement of antimicrobial characteristics of orthodontic resins, leading to reduction of enamel demineralization or control of friction force during orthodontic movement. The latter one enables effective orthodontic treatment while using less force. Emphasis is put on antimicrobial and mechanical characteristics of nanomaterials during orthodontic treatment. The manuscript sums up the current knowledge about nanomaterials’ influence on orthodontic appliances. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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30 pages, 2742 KiB

Open AccessReview

Application of Selected Nanomaterials and Ozone in Modern Clinical Dentistry

by Adam Lubojanski, Maciej Dobrzynski, Nicole Nowak, Justyna Rewak-Soroczynska, Klaudia Sztyler, Wojciech Zakrzewski, Wojciech Dobrzynski, Maria Szymonowicz, Zbigniew Rybak, Katarzyna Wiglusz and Rafal J. Wiglusz

Nanomaterials 2021, 11(2), 259; https://doi.org/10.3390/nano11020259 - 20 Jan 2021

Cited by 22 | Viewed by 4695

Abstract

This review is an attempt to summarize current research on ozone, titanium dioxide (TiO₂), silver (Ag), copper oxide CuO and platinum (Pt) nanoparticles (NPs). These agents can be used in various fields of dentistry such as conservative dentistry, endodontic, prosthetic or dental surgery. Nanotechnology and ozone can facilitate the dentist’s work by providing antimicrobial properties to dental materials or ensuring a decontaminated work area. However, the high potential of these agents for use in medicine should be confirmed in further research due to possible side effects, especially in long duration of observation so that the best way to apply them can be obtained. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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29 pages, 2374 KiB

Open AccessReview

Selected Nanomaterials’ Application Enhanced with the Use of Stem Cells in Acceleration of Alveolar Bone Regeneration during Augmentation Process

by Wojciech Zakrzewski, Maciej Dobrzynski, Zbigniew Rybak, Maria Szymonowicz and Rafal J. Wiglusz

Nanomaterials 2020, 10(6), 1216; https://doi.org/10.3390/nano10061216 - 22 Jun 2020

Cited by 29 | Viewed by 4387

Abstract

Regenerative properties are different in every human tissue. Nowadays, with the increasing popularity of dental implants, bone regenerative procedures called augmentations are sometimes crucial in order to perform a successful dental procedure. Tissue engineering allows for controlled growth of alveolar and periodontal tissues, with use of scaffolds, cells, and signalling molecules. By modulating the patient’s tissues, it can positively influence poor integration and healing, resulting in repeated implant surgeries. Application of nanomaterials and stem cells in tissue regeneration is a newly developing field, with great potential for maxillofacial bony defects. Nanostructured scaffolds provide a closer structural support with natural bone, while stem cells allow bony tissue regeneration in places when a certain volume of bone is crucial to perform a successful implantation. Several types of selected nanomaterials and stem cells were discussed in this study. Their use has a high impact on the efficacy of the current and future procedures, which are still challenging for medicine. There are many factors that can influence the regenerative process, while its general complexity makes the whole process even harder to control. The aim of this study was to evaluate the effectiveness and advantage of both stem cells and nanomaterials in order to better understand their function in regeneration of bone tissue in oral cavity. Full article

(This article belongs to the Special Issue Nanostructural Materials with Rare Earth Ions: Synthesis, Physicochemical Characterization, Modification and Applications)

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