Green fabrication of chitosan/tragacanth gum bionanocomposite films having TiO2@Ag hybrid for bioactivity and antibacterial applications

doi:10.1016/j.ijbiomac.2020.06.163

International Journal of Biological Macromolecules

Volume 162, 1 November 2020, Pages 512-522

https://doi.org/10.1016/j.ijbiomac.2020.06.163 Get rights and content

Highlights

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TiO₂ NPs was doped with green synthesized Ag NPs using R. officinalis extracts.
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Bio-NC films were fabricated based on CS, GT, TiO₂ NPs, and TiO₂@Ag hybrid.
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TiO₂@Ag hybrid showed better dispersion than TiO₂ NPs in the CS-GT blend film.
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Loading of TiO₂@Ag hybrid increased the bioactivity of CS-GT blend matrix.
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The resulted bio-NC films showed antibacterial activity under UV irradiation.

Abstract

Common materials used in tissue engineering are not cost-effective and natural origin. Hence, we designed green, safe, and antibacterial bionanocomposite (bio-NC) films based on polysaccharides, chitosan (CS) and gum tragacanth (GT) for the bone tissue engineering. For this aim, different percentages of titanium dioxide nanoparticles (TiO₂ NPs) and green silver (Ag)-doped TiO₂ NPs (TiO₂@Ag hybrid) were employed as nanofiller to improve the properties of the CS-GT film. Moreover, the physicochemical characteristics of the bio-NC films were examined with a field-emission scanning electron microscope (FE-SEM), Fourier transform infrared, X-ray diffraction, and transmission electron microscopy (TEM). The FE-SEM images showed a rough surface for the CS-GT/TiO₂@Ag bio-NC films, and TEM images showed better dispersion of TiO₂@Ag hybrid than TiO₂ NPs into the CS-GT matrix. Also, these bio-NC films were considered for the bioactivity test and the results showed formation of hydroxyapatite on the surface of the prepared bio-NC films. Furthermore, addition of GT led to an increase in the bioactivity of the CS-GT blend. Finally, antibacterial behavior of the prepared bio-NC films was investigated against Escherichia coli and Staphylococcus aureus bacteria with/without ultraviolet irradiation and the results indicated better antibacterial performance for the CS-GT/TiO₂@Ag bio-NC film (TiO₂:Ag = 1:1) under both conditions.

Graphical abstract

Introduction

Over the past decade, materials based on chitosan (CS) have been using widely in wound healing and tissue engineering, because of their specific properties to prevent wound infections and bacterial growth [1,2] The CS is known for its unique features including best scaffold, antioxidant activity, nontoxicity, biocompatibility, and antibacterial properties [[3], [4], [5], [6], [7], [8], [9], [10]]. Also, this polysaccharide is made up of 2-amino 2-deoxyd-glucopyranose in deacetylated unit. So, CS is a good candidate for bioactivity and antibacterial applications, because it is biocompatible and promotes cells to migrate and adhere to its surface [1,11]. Moreover, CS blend with other polymers would be a good scaffold in tissue engineering to grow osteoblast [12]. So, another natural polysaccharide which was used in this study is gum tragacanth (GT). This anionic polymer consists of bassorin, and tragacanthic acid [13,14], and it has numerous applications in different areas like stabilizers and emulsifiers [[15], [16], [17]]. Jalali and co-workers [18] fabricated the novel bio-nanofibers of polyethylene terephthalate (PET)/GT through the electrospinning method. The manufactured PET/GT had excellent surface wettability. Presence of GT in these fibers enhanced the crystallinity of PET. However, the mechanical properties were decreased.

From both industrial and academic points of view, polymer-ceramic nanocomposites have been the subject of studies in the field of tissue engineering and wound [[19], [20], [21]]. Among different kinds of nanoparticles (NPs) like titanium dioxide (TiO₂) NPs have remarkable properties. TiO₂ NPs have high antibacterial activity, chemical stability, biocompatibility, and photocatalytic performance [[22], [23], [24], [25], [26]]. According to the band-gap energy of TiO₂ NPs, if these materials exposed to the ultraviolet (UV) irradiation, electron-hole pairs on their surface would be created. Therefore, these electrons can be used for the killing of bacteria [27]. Zhang and co-workers [28] prepared CS/TiO₂ bionanocomposite (bio-NC) films and studied antibacterial activities under UV irradiation. When TiO₂ NPs were added to the CS matrix, the wettability, antibacterial activity (under UV irradiation), and mechanical properties of bio-NC films were made improvements. The surface energy of TiO₂ NPs could be reduced when they were doped with other NPs. Therefore, it would prevent the agglomeration phenomena of TiO₂ NPs in the polymeric matrix [29,30]. Nair et al. [31] prepared silver (Ag)-doped TiO₂ (TiO₂@Ag hybrid) nanorods, and investigated the photocatalytic efficiency under exposed UV irradiation. Among the various worlds of NPs, Ag is more pay attention due to its antibacterial properties [[32], [33], [34]]. Further, Ag NPs were synthesized with the green method which they have been low-cost, eco-friendly, and safe in comparison with chemically [35,36]. Jatoi and coworkers [23] fabricated cellulose acetate nanofibers embedded with TiO₂@Ag hybrid. The results of the antibacterial test showed that these nanofibers had good antibacterial activity.

Recently, the biomimetic technique has been becoming the subject of research, and study. For this reason, the bioactivity assay has been being a proper way to evaluate this technique in different materials. The bioactivity test could be assessed the probability to use artificial tissue, and suitable biomaterial scaffold which is a platform for cell growth, differentiation, attachment, and proliferation [19,37]. Another essential factor for bone tissue engineering is antibacterial property which prevents the growth of infection [38,39]. Moreover, several mechanisms are suggested for the antimicrobial activity of CS, which is related to the positively charged amino groups to stick the negatively charged surface of bacterial wall or plasma membrane [40,41]. The NPs may be more attractive for their antibacterial performance instead of antibiotics [42]. Some materials like GT have not been showing the antibacterial property. However, Ag NPs and some of the polymers have been composed of GT which could demonstrate the antibacterial defense against bacteria [43]. Rao and co-workers [44] prepared the GT-acrylamide/Ag bio-NC hydrogels and examined their antibacterial activity. When Ag NPs were embedded into the GT-acrylamide matrix, the inhibition zone against both Escherichia coli and Bacillus subtilis was observed.

Each year 6.3 billion tons of plastic wastes are produced in the world that only 9% of them are recycled [45]. Hence, this novel project addresses the expansion of artificial tissue and suitable biomaterial scaffold in tissue engineering which could use the scaffold to grow osteoblast without infections of the special parts. Furthermore, we used a high potent CS-GT polymer matrix which becomes reduce the consumption of petroleum products and also decreasing the production of polymer wastes. In addition, the different amounts of TiO₂@Ag hybrids with green synthesized Ag NPs were applied to this blend of the film. All of the novel bio-NCs films were fabricated via ultrasonic (US) irradiation which this method becomes low-cost, eco-friendly, safe, and non-toxic.

The present study is the first report of the bioactivity and antibacterial properties of the CS-GT polymer via TiO₂ NPs and TiO₂@Ag hybrids. The bioactivity test, all of the films were soaked in simulated body fluid (SBF) to 27 days. As well as, Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli) bacteria were used to study the antibacterial activity of bio-NC films with/without exposed to UV irradiation.

Section snippets

Materials

CS from crab shells with a molecular weight of 600,000–800,000 g·mol⁻¹, purity ≥90%, and the degree of deacetylation of 89.92% was bought from Acros Organics Company (USA). GT with the reported average molecular weight of 840,000 g·mol⁻¹ [46] was obtained from an Isfahanian local store, Iran. The TiO₂ NPs (with a particle size around 10–20 nm) with 78.8% anatase and 21.2% rutile crystalline phases were purchased by Neutrino chemical company at Tehran. Iran. Sodium chloride (NaCl,

Morphological studies

The surface morphology of NPs in the polymeric matrix for all samples was studied with the FE-SEM analysis. Figs. S1a and b show the morphology of pure CS and GT films, respectively. These images display a smooth surface for CS and GT films. Also, the FE-SEM image of the CS-GT blend film demonstrates the same surface morphology (Fig. S1c). When different amounts of TiO₂ NPs were embedded into the CS-GT blend film, the FE-SEM images showed different surface morphology on the surface of bio-NC

Conclusions

In this study, we prepared a novel CS-GT/TiO₂ and CS-GT/TiO₂@Ag bio-NC films with the aid of US irradiation and using solution casting method. The CS-GT/TiO₂ bio-NC film 5 wt% shows excellent dispersity of TiO₂ NPs. Next, the TiO₂@Ag hybrids were appended with 5 wt% total weight of the polymer to the CS-GT solution, and bio-NC films were prepared. The TEM micrographs of CS-GT/TiO₂@Ag (1.00:1.00) bio-NC film displayed the best dispersion of TiO₂@Ag hybrids in the CS-GT blend film. Finally, all

Author statements

Prof. Dr. Shadpour Mallakpour: Conceptualization, Methodology, Validation, Investigation, Visualization, Writing-review and editing, Resources, Supervision, Project administration, Funding acquisition.

Mr. Vahid Ramezanzade: Methodology, Investigation, Software, Formal analysis, Validation, Writing-original draft,

Declaration of competing interest

The authors declare no competing financial interest.

Acknowledgments

This research is financially supported by Research Affairs Division Isfahan University of Technology (IUT), Tehran, I. R. Iran, Centre of Excellence in Sensors and Green Chemistry Research, IUT, Isfahan, I. R. Iran, Isfahan, I. R. Iran, Iran Nanotechnology Initiative Council (INIC), and National Elite Foundation (NEF), Tehran, I. R. Iran. The authors' gratitude to Dr. F. Tabesh. Dr. F. Azimi, Dr. V. Behranvand, Dr. S. Rashidimoghadam, Dr. E. Khadem, Dr. M. Hatami, Miss. M. Naghdi, Miss. F.

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Green fabrication of chitosan/tragacanth gum bionanocomposite films having TiO2@Ag hybrid for bioactivity and antibacterial applications

Highlights

Abstract

Graphical abstract

Introduction

Section snippets

Materials

Morphological studies

Conclusions

Author statements

Declaration of competing interest

Acknowledgments

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Green fabrication of chitosan/tragacanth gum bionanocomposite films having TiO₂@Ag hybrid for bioactivity and antibacterial applications