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Multifunctional Oxide-Based Materials: From Synthesis to Application

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A special issue of Materials (ISSN 1996-1944).

Deadline for manuscript submissions: closed (15 May 2019) | Viewed by 43785

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Special Issue Editors

Prof. Dr. Teofil Jesionowski

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Institute of Chemical Technology and Engineering, Faculty of Chemical Technology, Poznan University of Technology, Berdychowo 4, PL-60965 Poznan, Poland
Interests: biopolymers; synthesis, characterization, and applications of advanced functional materials; functional fillers and polymer composites; (bio)additives and eco-friendly fillers; biomineralization-inspired syntheses and extreme biomimetics; biocomposites and biomaterials; removal of wastewater pollutants via adsorption; photocatalysis or precipitation methods; pigment composites; enzyme immobilization
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Dr. Filip Ciesielczyk

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Poznan University of Technology, Faculty of Chemical Technology, Institute of Chemical Technology and Engineering, Berdychowo 4, PL-60965 Poznan, Poland
Interests: multicomponent oxide systems; hybrid inorganic/organic materials; biomaterialsurface chemistry; inorganic pigments; catalysts; adsorption processes; environmental protection

Special Issue Information

Dear Colleagues,

The study and development of novel, oxide-based multifunctional materials with unique properties has become one of the most expanding fields in materials chemistry in recent years. The reason for this is that there are numerous inorganic/inorganic, as well as inorganic/organic, combinations that can be synthesized via different methods. The resulting mono-oxide and multicomponent systems or hybrids often possess exciting new properties for future materials, technological and environmental applications. This fact acts as a driving force for research and development of such systems. Even more importantly, these properties can be easily modified via the selection of hybrid components or via a typical functionalization process with the use of specific modifiers. Consequently, oxide-based hybrids have been widely applied in adsorption, catalysis (e.g., photocatalysis), polymer processing, optics, photoelectronics, electrochemistry, medicine, etc. This Special Issue focuses on recent advances in the synthesis, functionalization and application of oxide-based hybrids.

Proposed scope of this Special Issue is:

Synthesis of multifunctional oxide-based materials
Synthesis of hybrid inorganic/organic materials
Surface treatment (modification/grafting/immobilization)
Surface chemistry and functionality
Physicochemical characterization of oxide-based materials
Applications of oxide-based hybrids in electrochemistry, optics and biomedicine
Applications of oxide-based hybrids in environmental protection as catalysts (e.g., photocatalysts) or adsorbents of harmful inorganic and/or organic pollutants

Prof. Dr. Teofil Jesionowski
Dr. Filip Ciesielczyk
Guest Editors

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Keywords

inorganic oxides
hybrid materials
multicomponent systems
catalysts (photocatalysts)
synthesis routes
surface chemistry
modification
adsorption
immobilization
characterization techniques
environmental protection
electrochemistry
medical application
catalysis (photocatalysis)

Published Papers (9 papers)

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Research

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14 pages, 6318 KiB

Open AccessArticle

Modification of Ti6Al4V Titanium Alloy Surface Layer in the Ozone Atmosphere

by Mariusz Kłonica and Józef Kuczmaszewski

Materials 2019, 12(13), 2113; https://doi.org/10.3390/ma12132113 - 30 Jun 2019

Cited by 17 | Viewed by 2350

Abstract

The paper reports the results of a study on the Ti6Al4V titanium alloy involving the XPS (X-ray photoelectron spectroscopy) photoelectron spectroscopy method. The position of bands in the viewing spectrum serves as a basis for the qualitative identification of atoms forming the surface layer, while their intensity is used to calculate the aggregate concentration of these atoms in the analyzed layer. High-resolution spectra are used to determine the type of chemical bonds based on characteristic numerical values of the chemical shift. The paper also presents the 3D results of surface roughness measurements obtained from optical profiling, as well as the results of energy state measurements of the Ti6Al4V titanium alloy surface layer after ozone treatment. It was shown that the ozone treatment of the Ti6Al4V titanium alloy removes carbon and increases concentrations of Ti and V ions at higher oxidation states at the expense of metal atoms and lower valence ions. The modification of the surface layer in ozone atmosphere caused a 30% increase in the Ti element concentration in the surface layer compared to the samples prior to ozone treatment. The carbon removal rate from the Ti6Al4V titanium alloy samples amounted to 35%, and a 13% increase was noted in oxides. The tests proved that the value of the surface free energy of the Ti6Al4V titanium alloy increased as a result of ozone treatment. The highest increase in the surface free energy was observed for Variant 4 samples, and amounted to 17% compared to the untreated samples, while the lowest increase was equal to 14%. For the analyzed data, the maximum value of standard deviation was 0.99 [mJ/m²]. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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16 pages, 2858 KiB

Open AccessArticle

Laccase Immobilized onto Zirconia–Silica Hybrid Doped with Cu²⁺ as an Effective Biocatalytic System for Decolorization of Dyes

by Katarzyna Jankowska, Filip Ciesielczyk, Karolina Bachosz, Jakub Zdarta, Ewa Kaczorek and Teofil Jesionowski

Materials 2019, 12(8), 1252; https://doi.org/10.3390/ma12081252 - 16 Apr 2019

Cited by 33 | Viewed by 4251

Abstract

Nowadays, novel and advanced methods are being sought to efficiently remove dyes from wastewaters. These compounds, which mainly originate from the textile industry, may adversely affect the aquatic environment as well as living organisms. Thus, in presented study, the synthesized ZrO₂–SiO₂ and Cu²⁺-doped ZrO₂–SiO₂ oxide materials were used for the first time as supports for laccase immobilization, which was carried out for 1 h, at pH 5 and 25 °C. The materials were thoroughly characterized before and after laccase immobilization with respect to electrokinetic stability, parameters of the porous structure, morphology and type of surface functional groups. Additionally, the immobilization yields were defined, which reached 86% and 94% for ZrO₂–SiO₂–laccase and ZrO₂–SiO₂/Cu²⁺–laccase, respectively. Furthermore, the obtained biocatalytic systems were used for enzymatic decolorization of the Remazol Brilliant Blue R (RBBR) dye from model aqueous solutions, under various reaction conditions (time, temperature, pH). The best conditions of the decolorization process (24 h, 30 °C and pH = 4) allowed to achieve the highest decolorization efficiencies of 98% and 90% for ZrO₂–SiO₂–laccase and ZrO₂–SiO₂/Cu²⁺–laccase, respectively. Finally, it was established that the mortality of Artemia salina in solutions after enzymatic decolorization was lower by approx. 20% and 30% for ZrO₂–SiO₂–laccase and ZrO₂–SiO₂/Cu²⁺–laccase, respectively, as compared to the solution before enzymatic treatment, which indicated lower toxicity of the solution. Thus, it should be clearly stated that doping of the oxide support with copper ions positively affects enzyme stability, activity and, in consequence, the removal efficiency of the RBBR dye. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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9 pages, 3651 KiB

Open AccessArticle

Self-Propagating Synthesis and Characterization Studies of Gd-Bearing Hf-Zirconolite Ceramic Waste Forms

by Kuibao Zhang, Dan Yin, Kai Xu and Haibin Zhang

Materials 2019, 12(1), 178; https://doi.org/10.3390/ma12010178 - 07 Jan 2019

Cited by 14 | Viewed by 3249

Abstract

Synroc is recognized as the second-generation waste matrice for nuclear waste disposal. Zirconolite is one of the most durable Synroc minerals. In this study, Gd and Hf were selected as the surrogates of trivalent and tetravalent actinide nuclides. Gd-bearing Hf-zirconolite (Ca_1−xHf_1−xGd_2xTi₂O₇) ceramic waste forms were rapidly synthesized from a self-propagating technique using CuO as the oxidant. The results indicate that Gd can concurrently replace the Ca and Hf sites. However, Gd₂O₃ could not completely be incorporated into the lattice structure of zirconolite when the x value is higher than 0.8. The aqueous durability of selected Gd-Hf codoped sample (Hf-Gd-0.6) was tested, where the 42 days normalized leaching rates (LR_i) of Ca, Cu, Gd and Hf are measured to be 1.57, 0.13, 4.72 × 10⁻⁷ and 1.59 × 10⁻⁸ g·m⁻²·d⁻¹. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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18 pages, 3275 KiB

Open AccessFeature PaperArticle

Development of Alumina–Mesoporous Organosilica Hybrid Materials for Carbon Dioxide Adsorption at 25 °C

by Chamila Gunathilake, Rohan S. Dassanayake, Chandrakantha S. Kalpage and Mietek Jaroniec

Materials 2018, 11(11), 2301; https://doi.org/10.3390/ma11112301 - 16 Nov 2018

Cited by 15 | Viewed by 4491

Abstract

Two series of alumina (Al₂O₃)–mesoporous organosilica (Al–MO) hybrid materials were synthesized using the co-condensation method in the presence of Pluronic 123 triblock copolymer. The first series of Al–MO samples was prepared using aluminum nitrate nanahydrate (Al–NN) and aluminum isopropoxide (Al–IP) as alumina precursors, and organosilanes with three different bridging groups, namely tris[3-(trimethoxysilyl)propyl]isocyanurate, 1,4-bis(triethoxysilyl)benzene, and bis(triethoxysilyl)ethane. The second series was obtained using the aforementioned precursors in the presence of an amine-containing 3-aminopropyltriethoxysilane to introduce, also, hanging groups. The Al–IP-derived mesostructures in the first series showed the well-developed porosity and high specific surface area, as compared to the corresponding mesostructures prepared in the second series with 3-aminopropyltriethoxysilane. The materials obtained from Al–NN alumina precursor possessed enlarged mesopores in the range of 3–17 nm, whereas the materials synthesized from Al–IP alumina precursor displayed relatively low pore widths in the range of 5–7 nm. The Al–IP-derived materials showed high CO₂ uptakes, due to the enhanced surface area and microporosity in comparison to those observed for the samples of the second series with AP hanging groups. The Al–NN- and Al–IP-derived samples exhibited the CO₂ uptakes in the range of 0.73–1.72 and 1.66–2.64 mmol/g at 1 atm pressure whereas, at the same pressure, the Al–NN and Al–IP-derived samples with 3-aminopropyl hanging groups showed the CO₂ uptakes in the range of 0.72–1.51 and 1.70–2.33 mmol/g, respectively. These data illustrate that Al–MO hybrid materials are potential adsorbents for large-scale CO₂ capture at 25 °C. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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14 pages, 1946 KiB

Open AccessArticle

Thermal and Mechanical Properties of Silica–Lignin/Polylactide Composites Subjected to Biodegradation

by Aleksandra Grząbka-Zasadzińska, Łukasz Klapiszewski, Sławomir Borysiak and Teofil Jesionowski

Materials 2018, 11(11), 2257; https://doi.org/10.3390/ma11112257 - 13 Nov 2018

Cited by 24 | Viewed by 3563

Abstract

In this paper, silica–lignin hybrid materials were used as fillers for a polylactide (PLA) matrix. In order to simulate biodegradation, PLA/hybrid filler composite films were kept in soil of neutral pH for six months. Differential scanning calorimetry (DSC) allowed analysis of nonisothermal crystallization behavior of composites, thermal analysis provided information about their thermal stability, and scanning electron microscopy (SEM) was applied to define morphology of films. The influence of biodegradation was also investigated in terms of changes in mechanical properties and color of samples. It was found that application of silica–lignin hybrids as fillers for PLA matrix may be interesting not only in terms of increasing thermal stability, but also controlled biodegradation. To the best knowledge of the authors, this is the first publication regarding biodegradation of PLA composites loaded with silica–lignin hybrid fillers. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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19 pages, 5512 KiB

Open AccessArticle

TiO₂-ZnO Binary Oxide Systems: Comprehensive Characterization and Tests of Photocatalytic Activity

by Katarzyna Siwińska-Stefańska, Adam Kubiak, Adam Piasecki, Joanna Goscianska, Grzegorz Nowaczyk, Stefan Jurga and Teofil Jesionowski

Materials 2018, 11(5), 841; https://doi.org/10.3390/ma11050841 - 18 May 2018

Cited by 99 | Viewed by 6299

Abstract

A series of TiO₂-ZnO binary oxide systems with various molar ratios of TiO₂ and ZnO were prepared using a sol-gel method. The influence of the molar ratio and temperature of calcination on the particle sizes, morphology, crystalline structure, surface composition, porous structure parameters, and thermal stability of the final hybrids was investigated. Additionally, to confirm the presence of characteristic surface groups of the material, Fourier transform infrared spectroscopy was applied. It was found that the crystalline structure, porous structure parameters, and thermal stability were determined by the molar ratio of TiO₂ to ZnO and the calcination process for the most part. A key element of the study was an evaluation of the photocatalytic activity of the TiO₂-ZnO hybrids with respect to the decomposition of C.I. Basic Blue 9, C.I. Basic Red 1, and C.I. Basic Violet 10 dyes. It was found that the TiO₂-ZnO material obtained with a molar ratio of TiO₂:ZnO = 9:1 and calcined at 600 °C demonstrates high photocatalytic activity in the degradation of the three organic dyes when compared with pristine TiO₂. Moreover, an attempt was made to describe equilibrium aspects by applying the Langmuir-Hinsherlwood equation. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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14 pages, 5919 KiB

Open AccessArticle

Synthesis and Effect of Hierarchically Structured Ag-ZnO Hybrid on the Surface Antibacterial Activity of a Propylene-Based Elastomer Blends

by Pavel Bazant, Tomas Sedlacek, Ivo Kuritka, David Podlipny and Pavlina Holcapkova

Materials 2018, 11(3), 363; https://doi.org/10.3390/ma11030363 - 01 Mar 2018

Cited by 20 | Viewed by 4388

Abstract

In this study, a hybrid Ag-ZnO nanostructured micro-filler was synthesized by the drop technique for used in plastic and medical industry. Furthermore, new antibacterial polymer nanocomposites comprising particles of Ag-ZnO up to 5 wt % and a blend of a thermoplastic polyolefin elastomer (TPO) with polypropylene were prepared using twin screw micro-compounder. The morphology and crystalline-phase structure of the hybrid Ag-ZnO nanostructured microparticles obtained was characterized by scanning electron microscopy and powder X-ray diffractometry. The specific surface area of this filler was investigated by means of nitrogen sorption via the Brunauer-Emmet-Teller method. A scanning electron microscope was used to conduct a morphological study of the polymer nanocomposites. Mechanical and electrical testing showed no adverse effects on the function of the polymer nanocomposites either due to the filler utilized or the given processing conditions, in comparison with the neat polymer matrix. The surface antibacterial activity of the compounded polymer nanocomposites was assessed against Escherichia coli ATCC 8739 and Staphylococcus aureus ATCC 6538P, according to ISO 22196:2007 (E). All the materials at virtually every filler-loading level were seen to be efficient against both species of bacteria. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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Review

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32 pages, 4297 KiB

Open AccessReview

Removal of Hazardous Oxyanions from the Environment Using Metal-Oxide-Based Materials

by Ewelina Weidner and Filip Ciesielczyk

Materials 2019, 12(6), 927; https://doi.org/10.3390/ma12060927 - 20 Mar 2019

Cited by 73 | Viewed by 7033

Abstract

Scientific development has increased the awareness of water pollutant forms and has reawakened the need for its effective purification. Oxyanions are created by a variety of redox-sensitive metals and metalloids. These species are harmful to living matter due to their toxicity, nondegradibility, and mobility in aquatic environments. Among a variety of water treatment techniques, adsorption is one of the simplest, cheapest, and most effective. Since metal-oxide-based adsorbents poses a variety of functional groups onto their surface, they were widely applied in ions sorption. In this paper adsorption of harmful oxyanions by metal oxide-based materials according to literature survey was studied. Characteristic of oxyanions originating from As, V, B, W and Mo, their probable adsorption mechanisms and comparison of their sorption affinity for metal-oxide-based materials such as iron oxides, aluminum oxides, titanium dioxide, manganium dioxide, and various oxide minerals and their combinations are presented in this paper. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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52 pages, 6129 KiB

Open AccessReview

Titania-Based Hybrid Materials with ZnO, ZrO₂ and MoS₂: A Review

by Adam Kubiak, Katarzyna Siwińska-Ciesielczyk and Teofil Jesionowski

Materials 2018, 11(11), 2295; https://doi.org/10.3390/ma11112295 - 15 Nov 2018

Cited by 51 | Viewed by 6572

Abstract

Titania has properties that enable it to be used in a variety of applications, including self-cleaning surfaces, air and water purification systems, hydrogen evolution, and photoelectrochemical conversion. In order to improve the properties of titanium dioxide, modifications are made to obtain oxide/hybrid systems that are intended to have the properties of both components. In particular, zinc oxide, zirconia and molybdenum disulfide have been proposed as the second component of binary systems due to their antibacterial, electrochemical and photocatalytic properties. This paper presents a review of the current state of knowledge on the synthesis and practical utility of TiO₂-ZnO and TiO₂-ZrO₂ oxide systems and TiO₂-MoS₂ hybrid materials. The first part focuses on the hydrothermal method; then a review is made of the literature on the synthesis of the aforementioned materials using the sol-gel method. In the last section, the literature on the electrospinning method of synthesis is reviewed. The most significant physico-chemical, structural and dispersive-morphological properties of binary hybrid systems based on TiO₂ are described. A key aim of this review is to indicate the properties of TiO₂-ZnO, TiO₂-ZrO₂ and TiO₂-MoS₂ hybrid systems that have the greatest importance for practical applications. The variety of utilities of titania-based hybrid materials is emphasized. Full article

(This article belongs to the Special Issue Multifunctional Oxide-Based Materials: From Synthesis to Application)

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