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Advanced Composite Biomaterials

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: closed (30 November 2020) | Viewed by 40738

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Guest Editor
1. Advanced Polymer Materials Group, Faculty of Applied Chemistry and Materials Science, University Politehnica of Bucharest, Bucharest, Romania
2. Department of Analytical Chemistry and Environmental Engineering, Faculty of Chemistry and Materials Science, University Politehnica of Bucharest, 011061 Bucharest, Romania
Interests: synthesis and characterisation of polymeric membranes; biomedical applications of polymeric membranes; functionalization and derivatization of carbon-based nanospecies
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Guest Editor
Faculty of Material Science and Engineering, Metallic Material Science and Physical Metallurgy Department, Politehnica University of Bucharest, 313 Splaiul Independentei, 060042 Bucharest, Romania
Interests: thermal properties; mechanical properties; composites; materials characterization; microscopy

Special Issue Information

Dear Colleagues,

In recent years, there has been an increasing interest in biomedical engineering, which has to respond to more and more challenges, in particular related to changes in lifestyle and environmental factors. If two or three decades ago this domain was limited to a small number of applications, there are now a number of niche domains such as tissue engineering, polymeric materials for osteointegration, artificial organs, devices for the controlled release of drugs and the new materials must respond to all the challenges that have arisen. Among the new synthesized materials, one can distinguish the composites with carbon or graphite nanotubes, the filler having both the role of refining and improvement of some properties such as conductivity, adsorption or release of various substances capacities. The present Special Issue is dedicated to composite biomaterials with carbon nanotubes or graphene applicable in tissue engineering, osteointegration etc. The domains addressed by this issue are:

  • Polymer-carbon nanotube composite biomaterials;
  • Polymer-graphene composite biomaterials;
  • Ceramic-carbon nanotubes composite biomaterials;
  • Applications of carbon-nanotube composite biomaterials;
  • Applications of graphene composite biomaterials;
  • Characterization methods for carbon nanotube composite biomaterials;
  • Characterization methods for graphene composite biomaterials.

Prof. Stefan Ioan Voicu
Prof. Marian Miculescu
Guest Editors

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Keywords

  • Composite biomaterials
  • Carbon nanotube
  • Graphene
  • Characterization methods
  • Polymer-carbon nanotube composites
  • Polymer-graphene composites
  • Biomaterials

Published Papers (12 papers)

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Editorial

Jump to: Research, Review

3 pages, 403 KiB  
Editorial
Advanced Composite Biomaterials
by Stefan Ioan Voicu and Marian Miculescu
Materials 2021, 14(3), 625; https://doi.org/10.3390/ma14030625 - 01 Feb 2021
Viewed by 1522
Abstract
“Biomaterials” is one of the most important fields of study in terms of its development in the 21st century [...] Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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Research

Jump to: Editorial, Review

16 pages, 4102 KiB  
Article
The Interplay between Whey Protein Fibrils with Carbon Nanotubes or Carbon Nano-Onions
by Ning Kang, Jin Hua, Lizhen Gao, Bin Zhang and Jiewen Pang
Materials 2021, 14(3), 608; https://doi.org/10.3390/ma14030608 - 28 Jan 2021
Cited by 8 | Viewed by 2305
Abstract
Whey protein isolate (WPI) fibrils were prepared using an acid hydrolysis induction process. Carbon nanotubes (CNTs) and carbon nano-onions (CNOs) were made via the catalytic chemical vapor deposition (CVD) of methane. WPI fibril–CNTs and WPI fibril–CNOs were prepared via hydrothermal synthesis at 80 [...] Read more.
Whey protein isolate (WPI) fibrils were prepared using an acid hydrolysis induction process. Carbon nanotubes (CNTs) and carbon nano-onions (CNOs) were made via the catalytic chemical vapor deposition (CVD) of methane. WPI fibril–CNTs and WPI fibril–CNOs were prepared via hydrothermal synthesis at 80 °C. The composites were characterized by SEM, TEM, FTIR, XRD, Raman, and TG analyses. The interplay between WPI fibrils and CNTs and CNOs were studied. The WPI fibrils with CNTs and CNOs formed uniform gels and films. CNTs and CNOs were highly dispersed in the gels. Hydrogels of WPI fibrils with CNTs (or CNOs) could be new materials with applications in medicine or other fields. The CNTs and CNOs shortened the WPI fibrils, which might have important research value for curing fibrosis diseases such as Parkinson’s and Alzheimer’s diseases. The FTIR revealed that CNTs and CNOs both had interactions with WPI fibrils. The XRD analysis suggested that most of the CNTs were wrapped in WPI fibrils, while CNOs were partially wrapped. This helped to increase the biocompatibility and reduce the cytotoxicity of CNTs and CNOs. HR-TEM and Raman spectroscopy studies showed that the graphitization level of CNTs was higher than for CNOs. After hybridization with WPI fibrils, more defects were created in CNTs, but some original defects were dismissed in CNOs. The TG results indicated that a new phase of WPI fibril–CNTs or CNOs was formed. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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12 pages, 2727 KiB  
Article
Tearable and Fillable Composite Sponges Capable of Heat Generation and Drug Release in Response to Alternating Magnetic Field
by Koichiro Hayashi, Atsuto Tokuda, Jin Nakamura, Ayae Sugawara-Narutaki and Chikara Ohtsuki
Materials 2020, 13(16), 3637; https://doi.org/10.3390/ma13163637 - 17 Aug 2020
Cited by 6 | Viewed by 2659
Abstract
Tearable and fillable implants are used to facilitate surgery. The use of implants that can generate heat and release a drug in response to an exogenous trigger, such as an alternating magnetic field (AMF), can facilitate on-demand combined thermal treatment and chemotherapy via [...] Read more.
Tearable and fillable implants are used to facilitate surgery. The use of implants that can generate heat and release a drug in response to an exogenous trigger, such as an alternating magnetic field (AMF), can facilitate on-demand combined thermal treatment and chemotherapy via remote operation. In this study, we fabricated tearable sponges composed of collagen, magnetite nanoparticles, and anticancer drugs. Crosslinking of the sponges by heating for 6 h completely suppressed undesirable drug release in saline at 37 °C but allowed drug release at 45 °C. The sponges generated heat immediately after AMF application and raised the cell culture medium temperature from 37 to 45 °C within 15 min. Heat generation was controlled by switching the AMF on and off. Furthermore, in response to heat generation, drug release from the sponges could be induced and moderated. Thus, remote-controlled heat generation and drug release were achieved by switching the AMF on and off. The sponges destroyed tumor cells when AMF was applied for 15 min but not when AMF was absent. The tearing and filling properties of the sponges may be useful for the surgical repair of bone and tissue defects. Moreover, these sponges, along with AMF application, can facilitate combined thermal therapy and chemotherapy. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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18 pages, 4192 KiB  
Article
Ligno-Cellulosic Fibre Sized with Nucleating Agents Promoting Transcrystallinity in Isotactic Polypropylene Composites
by Armin Thumm, Regis Risani, Alan Dickson and Mathias Sorieul
Materials 2020, 13(5), 1259; https://doi.org/10.3390/ma13051259 - 10 Mar 2020
Cited by 9 | Viewed by 2746
Abstract
The mechanical performance of composites made from isotactic polypropylene reinforced with natural fibres depends on the interface between fibre and matrix, as well as matrix crystallinity. Sizing the fibre surface with nucleating agents to promote transcrystallinity is a potential route to improve the [...] Read more.
The mechanical performance of composites made from isotactic polypropylene reinforced with natural fibres depends on the interface between fibre and matrix, as well as matrix crystallinity. Sizing the fibre surface with nucleating agents to promote transcrystallinity is a potential route to improve the mechanical properties. The sizing of thermo-mechanical pulp and regenerated cellulose (Tencel™) fibres with α- and β-nucleating agents, to improve tensile strength and impact strength respectively, was assessed in this study. Polarised microscopy, electron microscopy and differential scanning calorimetry (DSC) showed that transcrystallinity was achieved and that the bulk crystallinity of the matrix was affected during processing (compounding and injection moulding). However, despite substantial changes in crystal structure in the final composite, the sizing method used did not lead to significant changes regarding the overall composite mechanical performance. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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16 pages, 9763 KiB  
Article
Ultralight Industrial Bamboo Residue-Derived Holocellulose Thermal Insulation Aerogels with Hydrophobic and Fire Resistant Properties
by Hanxiao Huang, Yunshui Yu, Yan Qing, Xiaofeng Zhang, Jia Cui and Hankun Wang
Materials 2020, 13(2), 477; https://doi.org/10.3390/ma13020477 - 19 Jan 2020
Cited by 19 | Viewed by 3732
Abstract
In this study, water-soluble ammonium polyphosphate- (APP) and methyl trimethoxysilane (MTMS)-modified industrial bamboo residue (IBR)-derived holocellulose nanofibrils (HCNF/APP/MTMS) were used as the raw materials to prepare aerogels in a freeze-drying process. Synthetically modified aerogels were confirmed by Fourier transform infrared spectroscopy, X-ray diffraction, [...] Read more.
In this study, water-soluble ammonium polyphosphate- (APP) and methyl trimethoxysilane (MTMS)-modified industrial bamboo residue (IBR)-derived holocellulose nanofibrils (HCNF/APP/MTMS) were used as the raw materials to prepare aerogels in a freeze-drying process. Synthetically modified aerogels were confirmed by Fourier transform infrared spectroscopy, X-ray diffraction, and thermal stability measurements. As-prepared HCNF/APP/MTMS aerogels showed themselves to be soft and flexible. The scanning electron microscopy (SEM) analysis showed that the foam-like structure translates into a 3D network structure from HCNF aerogels to HCNF/APP/MTMS aerogels. The compressive modules of the HCNF/APP/MTMS aerogels were decreased from 38 kPa to 8.9 kPa with a density in the range of 12.04–28.54 kg/m3, which was due to the structural change caused by the addition of APP and MTMS. Compared with HCNF aerogels, HCNF/APP/MTMS aerogels showed a high hydrophobicity, in which the water contact angle was 130°, and great flame retardant properties. The peak of heat release rate (pHRR) and total smoke production (TSP) decreased from 466.6 to 219.1 kW/m2 and 0.18 to 0.04 m2, respectively, meanwhile, the fire growth rate (FIGRA) decreased to 8.76 kW/s·m2. The thermal conductivity of the HCNF/APP/MTMS aerogels was 0.039 W/m·K. All results indicated the prepared aerogels should be expected to show great potential for thermally insulative materials. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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13 pages, 4248 KiB  
Article
Synthesis and Characterization of PLA-Micro-structured Hydroxyapatite Composite Films
by Andreea Madalina Pandele, Andreea Constantinescu, Ionut Cristian Radu, Florin Miculescu, Stefan Ioan Voicu and Lucian Toma Ciocan
Materials 2020, 13(2), 274; https://doi.org/10.3390/ma13020274 - 08 Jan 2020
Cited by 77 | Viewed by 4790
Abstract
This article presents a facile synthesis method used to obtain new composite films based on polylactic acid and micro-structured hydroxyapatite particles. The composite films were synthesized starting from a polymeric solution in chloroform (12 wt.%) in which various concentrations of hydroxyapatite (1, 2, [...] Read more.
This article presents a facile synthesis method used to obtain new composite films based on polylactic acid and micro-structured hydroxyapatite particles. The composite films were synthesized starting from a polymeric solution in chloroform (12 wt.%) in which various concentrations of hydroxyapatite (1, 2, and 4 wt.% related to polymer) were homogenously dispersed using ultrasonication followed by solvent evaporation. The synthesized composite films were morphologically (through SEM and atomic force microscopy (AFM)) and structurally (through FT-IR and Raman spectroscopy) characterized. The thermal behavior of the composite films was also determined. The SEM and AFM analyses showed the presence of micro-structured hydroxyapatite particles in the film’s structure, as well as changes in the surface morphology. There was a significant decrease in the crystallinity of the composite films compared to the pure polymer, this being explained by a decrease in the arrangement of the polymer chains and a concurrent increase in the degree of their clutter. The presence of hydroxyapatite crystals did not have a significant influence on the degradation temperature of the composite film. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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19 pages, 4304 KiB  
Article
Preparation and Performance of Radiata-Pine-Derived Polyvinyl Alcohol/Carbon Quantum Dots Fluorescent Films
by Li Xu, Yushu Zhang, Haiqing Pan, Nan Xu, Changtong Mei, Haiyan Mao, Wenqing Zhang, Jiabin Cai and Changyan Xu
Materials 2020, 13(1), 67; https://doi.org/10.3390/ma13010067 - 21 Dec 2019
Cited by 38 | Viewed by 3480
Abstract
In this study, the low-cost processing residue of Radiata pine (Pinus radiata D. Don) was used as the lone carbon source for synthesis of CQDs (Carbon quantum dots) with a QY (The quantum yield of the CQDs) of 1.60%. The CQDs [...] Read more.
In this study, the low-cost processing residue of Radiata pine (Pinus radiata D. Don) was used as the lone carbon source for synthesis of CQDs (Carbon quantum dots) with a QY (The quantum yield of the CQDs) of 1.60%. The CQDs were obtained by the hydrothermal method, and +a PVA-based biofilm was prepared by the fluidized drying method. The effects of CQDs and CNF (cellulose nanofibers) content on the morphology, optical, mechanical, water-resistance, and wettability properties of the PVA/CQDs and PVA/CNF/CQDs films are discussed. The results revealed that, when the excitation wavelength was increased from 340 to 390 nm, the emission peak became slightly red-shifted, which was induced by the condensation between CQDs and PVA. The PVA composite films showed an increase in fluorescence intensity with the addition of the CNF and CQDs to polymers. The chemical structure of prepared films was determined by the FTIR spectroscopy, and no new chemical bonds were formed. In addition, the UV transmittance was inversely proportional to the change of CQDs content, which indicated that CQDs improved the UV barrier properties of the films. Furthermore, embedding CQDs Nano-materials and CNF into the PVA matrix improved the mechanical behavior of the Nano-composite. Tensile modulus and strength at break increased significantly with increasing the concentration of CQDs Nano-materials inside the Nano-composite, which was due to the increased in the density of crosslinking behavior. With the increase of CQDs content (>1 mL), the water absorption and surface contact angle of the prepared films decreased gradually, and the water-resistance and surface wettability of the films were improved. Therefore, PVA/CNF/CQDs bio-nanocomposite films could be used to prepare anti-counterfeiting, high-transparency, and ultraviolet-resistant composites, which have potential applications in ecological packaging materials. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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13 pages, 3531 KiB  
Article
Preparation and Characterization of Dyed Corn Straw by Acid Red GR and Active Brilliant X-3B Dyes
by Yanchen Li, Beibei Wang, Yingni Yang, Yi Liu and Hongwu Guo
Materials 2019, 12(21), 3483; https://doi.org/10.3390/ma12213483 - 24 Oct 2019
Cited by 3 | Viewed by 1913
Abstract
Corn straw is a kind of biomass material with huge reserves, which can be used in plate processing, handicraft manufacturing, indoor decoration, and other fields. To investigate the dyeing mechanism of corn straw with different dyes, corn straw was pretreated and dyed with [...] Read more.
Corn straw is a kind of biomass material with huge reserves, which can be used in plate processing, handicraft manufacturing, indoor decoration, and other fields. To investigate the dyeing mechanism of corn straw with different dyes, corn straw was pretreated and dyed with Acid Red GR and Brilliant Red X-3B. The dyeing properties and light resistance of the two dyes were analyzed by dyeing rate, photochromaticity, FTIR, SEM, and water-washing firmness. The results showed that the structure and stability of the dyes were the main factors which influenced fading. A bleaching pretreatment could remove the waxiness of the corn straw epidermis and increase the porosity on the surface of the straw, which accelerated the photochromic coloring of the corn straw skin. The corn straw dyed with both dyes had good light resistance, but the straw dyed with Reactive Brilliant Red X-3B had higher dyeing rate, brighter color, and higher photochromaticity than the straw dyed with Acid Red GR. FTIR and water-washing firmness showed that Acid Red GR mainly bound to lignin, while Reactive Brilliant Red X-3B mainly bound to cellulose, hemicellulose, and lignin in corn straw through covalent bonds, which increased the coloring rate. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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11 pages, 9730 KiB  
Article
Combined Effects of Color and Elastic Modulus on Antifouling Performance: A Study of Graphene Oxide/Silicone Rubber Composite Membranes
by Huichao Jin, Wei Bing, Limei Tian, Peng Wang and Jie Zhao
Materials 2019, 12(16), 2608; https://doi.org/10.3390/ma12162608 - 16 Aug 2019
Cited by 25 | Viewed by 3017
Abstract
Biofouling is a significant maritime problem because the growth of fouling organisms on the hulls of ships leads to very high economic losses every year. Inspired by the soft skins of dolphins, we prepared graphene oxide/silicone rubber composite membranes in this study. These [...] Read more.
Biofouling is a significant maritime problem because the growth of fouling organisms on the hulls of ships leads to very high economic losses every year. Inspired by the soft skins of dolphins, we prepared graphene oxide/silicone rubber composite membranes in this study. These membranes have low surface free energies and adjustable elastic moduli, which are beneficial for preventing biofouling. Diatom attachment studies under static conditions revealed that color has no effect on antifouling behavior, whereas the studies under hydrodynamic conditions revealed that the combined effects of color and elastic modulus determine the antifouling performance. The experimental results are in accordance with the “harmonic motion effect” theory proposed by us, and we also provide a supplement to the theory in this paper. On the basis of the diatom attachment test results, the membrane with 0.36 wt % of graphene oxide showed excellent antifouling performance, and is promising in practical applications. The results confirmed that the graphene oxide and graphene have similar effect to enhance silicone rubber antifouling performance. This study provides important insight for the design of new antifouling coatings; specifically, it indicates that lighter colors and low Young’s moduli provide superior performance. In addition, this study provides a reference for the application of graphene oxide as fillers to enhance the composite antifouling performance. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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14 pages, 2172 KiB  
Article
Investigating the Mechanical Properties of ZrO2-Impregnated PMMA Nanocomposite for Denture-Based Applications
by Saleh Zidan, Nikolaos Silikas, Abdulaziz Alhotan, Julfikar Haider and Julian Yates
Materials 2019, 12(8), 1344; https://doi.org/10.3390/ma12081344 - 25 Apr 2019
Cited by 74 | Viewed by 5139
Abstract
Acrylic resin PMMA (poly-methyl methacrylate) is used in the manufacture of denture bases but its mechanical properties can be deficient in this role. This study investigated the mechanical properties (flexural strength, fracture toughness, impact strength, and hardness) and fracture behavior of a commercial, [...] Read more.
Acrylic resin PMMA (poly-methyl methacrylate) is used in the manufacture of denture bases but its mechanical properties can be deficient in this role. This study investigated the mechanical properties (flexural strength, fracture toughness, impact strength, and hardness) and fracture behavior of a commercial, high impact (HI), heat-cured denture base acrylic resin impregnated with different concentrations of yttria-stabilized zirconia (ZrO2) nanoparticles. Six groups were prepared having different wt% concentrations of ZrO2 nanoparticles: 0% (control), 1.5%, 3%, 5%, 7%, and 10%, respectively. Flexural strength and flexural modulus were measured using a three-point bending test and surface hardness was evaluated using the Vickers hardness test. Fracture toughness and impact strength were evaluated using a single edge bending test and Charpy impact instrument. The fractured surfaces of impact test specimens were also observed using a scanning electron microscope (SEM). Statistical analyses were conducted on the data obtained from the experiments. The mean flexural strength of ZrO2/PMMA nanocomposites (84 ± 6 MPa) at 3 wt% zirconia was significantly greater than that of the control group (72 ± 9 MPa) (p < 0.05). The mean flexural modulus was also significantly improved with different concentrations of zirconia when compared to the control group, with 5 wt% zirconia demonstrating the largest (23%) improvement. The mean fracture toughness increased in the group containing 5 wt% zirconia compared to the control group, but it was not significant. However, the median impact strength for all groups containing zirconia generally decreased when compared to the control group. Vickers hardness (HV) values significantly increased with an increase in ZrO2 content, with the highest values obtained at 10 wt%, at 0 day (22.9 HV0.05) in dry conditions when compared to the values obtained after immersing the specimens for seven days (18.4 HV0.05) and 45 days (16.3 HV0.05) in distilled water. Incorporation of ZrO2 nanoparticles into high impact PMMA resin significantly improved flexural strength, flexural modulus, fracture toughness and surface hardness, with an optimum concentration of 3–5 wt% zirconia. However, the impact strength of the nanocomposites decreased, apart from the 5 wt% zirconia group. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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Review

Jump to: Editorial, Research

24 pages, 5171 KiB  
Review
Cellulose Composites with Graphene for Tissue Engineering Applications
by Madalina Oprea and Stefan Ioan Voicu
Materials 2020, 13(23), 5347; https://doi.org/10.3390/ma13235347 - 25 Nov 2020
Cited by 37 | Viewed by 3593
Abstract
Tissue engineering is an interdisciplinary field that combines principles of engineering and life sciences to obtain biomaterials capable of maintaining, improving, or substituting the function of various tissues or even an entire organ. In virtue of its high availability, biocompatibility and versatility, cellulose [...] Read more.
Tissue engineering is an interdisciplinary field that combines principles of engineering and life sciences to obtain biomaterials capable of maintaining, improving, or substituting the function of various tissues or even an entire organ. In virtue of its high availability, biocompatibility and versatility, cellulose was considered a promising platform for such applications. The combination of cellulose with graphene or graphene derivatives leads to the obtainment of superior composites in terms of cellular attachment, growth and proliferation, integration into host tissue, and stem cell differentiation toward specific lineages. The current review provides an up-to-date summary of the status of the field of cellulose composites with graphene for tissue engineering applications. The preparation methods and the biological performance of cellulose paper, bacterial cellulose, and cellulose derivatives-based composites with graphene, graphene oxide and reduced graphene oxide were mainly discussed. The importance of the cellulose-based matrix and the contribution of graphene and graphene derivatives fillers as well as several key applications of these hybrid materials, particularly for the development of multifunctional scaffolds for cell culture, bone and neural tissue regeneration were also highlighted. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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23 pages, 3717 KiB  
Review
Recent Advances in Applications of Cellulose Derivatives-Based Composite Membranes with Hydroxyapatite
by Madalina Oprea and Stefan Ioan Voicu
Materials 2020, 13(11), 2481; https://doi.org/10.3390/ma13112481 - 29 May 2020
Cited by 40 | Viewed by 4389
Abstract
The development of novel polymeric composites based on cellulose derivatives and hydroxyapatite represents a fascinating and challenging research topic in membranes science and technology. Cellulose-based materials are a viable alternative to synthetic polymers due to their favorable physico-chemical and biological characteristics. They are [...] Read more.
The development of novel polymeric composites based on cellulose derivatives and hydroxyapatite represents a fascinating and challenging research topic in membranes science and technology. Cellulose-based materials are a viable alternative to synthetic polymers due to their favorable physico-chemical and biological characteristics. They are also an appropriate organic matrix for the incorporation of hydroxyapatite particles, inter and intramolecular hydrogen bonds, as well as electrostatic interactions being formed between the functional groups on the polymeric chains surface and the inorganic filler. The current review presents an overview on the main application fields of cellulose derivatives/hydroxyapatite composite membranes. Considering the versatility of hydroxyapatite particles, the hybrid materials offer favorable prospects for applications in water purification, tissue engineering, drug delivery, and hemodialysis. The preparation technique and the chemical composition have a big influence on the final membrane properties. The well-established membrane fabrication methods such as phase inversion, electrospinning, or gradual electrostatic assembly are discussed, together with the various strategies employed to obtain a homogenous dispersion of the inorganic particles in the polymeric matrix. Finally, the main conclusions and the future directions regarding the preparation and applications of cellulose derivatives/hydroxyapatite composite membranes are presented. Full article
(This article belongs to the Special Issue Advanced Composite Biomaterials)
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