Elsevier

Particuology

Volume 40, October 2018, Pages 141-151
Particuology

Antimicrobial activity of metal-substituted cobalt ferrite nanoparticles synthesized by sol–gel technique

https://doi.org/10.1016/j.partic.2017.12.001Get rights and content

Highlights

  • Zn, Cu, and Mn substituted cobalt ferrite nanoparticles were synthesized by sol–gel method.

  • Antimicrobial activity of the ferrites against selected pathogens was studied.

  • Of the prepared ferrites, zinc cobalt ferrite (ZCFO) possessed strongest antimicrobial activity.

  • Irradiation at 150 kGy decreased ZCFO particle size and elevated its antimicrobial potential.

Abstract

Metal-substituted cobalt ferrites [MxCo(1−x)Fe2O4 (M = Zn, Cu, Mn; x = 0.0, 0.25, 0.5, and 0.75)] were synthesized via a sol–gel technique. The ferrite structures were confirmed by X-ray diffraction, Fourier transform infrared spectroscopy, scanning electron microscopy, surface analysis using the Brunauer–Emmett–Teller method, and energy-dispersive X-ray spectroscopy. Antimicrobial activity of these ferrites against selected pathogenic microbes was determined. The structures remained cubic spinel phases after substitution of metals. Substitution strongly influenced the microstructure and homogeneous grain distribution. The particle size of the ferrites increased linearly with increase in their annealing temperature. The surface area of zinc cobalt ferrite nanoparticles (ZCFO) was 52.56 m2/g, the average pore size was 1.84 nm, and pore volume was 0.136 mL/g. All ferrites showed antimicrobial activity toward all pathogens selected. Of these, the most powerful was ZCFO, showing zones of inhibition of 13.0 mm against Bacillus subtilis and Staphylococcus aureus and 12.0 mm against Candida albicans. Gamma-irradiated ZCFO nanoparticles (150.0 kGy) maintained higher antimicrobial activity than non-irradiated particles, e.g. being active toward S. aureus (16.0 mm). ZCFO is proposed as a candidate material for industrial and biomedical purposes.

Introduction

The utilization of metal and metal-oxide nanoparticles for antimicrobial performance is attracting much attention, as several of these suggest superior activity toward resistant microorganisms (El-Batal, El-Sayyad, El-Ghamery, & Gobara, 2017; El-Batal, El-Sayyad, El-Ghamry, Agaypi, et al., 2017; El-Batal, ElKenawy, Yassin, & Amin, 2015; Žalnėravičius, Paškevičius, Kurtinaitiene, & Jagminas, 2016). Ferrites are ferromagnetic compounds that are typically oxides of different transition metals, including iron (Farid et al., 2017); for example, MnFe2O4 and Zn–Mn ferrite can form unions of the formula MnxZn1−xFe2O4 (Dar & Varshney, 2017). They are frequently insulators in nature and, similar to most another ceramics, solid and fragile (Amirabadizadeh, Salighe, Sarhaddi, & Lotfollahi, 2017). In phases with magnetic characteristics, ferrites are usually categorized as soft or hard, which leads to respective decreased or increased magnetic coercivity (Pour, Shaterian, Afradi, & Yazdani-Elah-Abadi, 2017).

Spinel ferrite nanoparticles have well-known novel optical, photoelectric, and magnetic features. These nanoparticles possess high permeability, high overload magnetization, and have no preferred route of magnetization (Sharma, Thakur, Sharma, & Sharma, 2017). Spinel ferrites are magnetic semiconductors and are amongst compounds able to generate magnetic nanospheres that are widely accepted because they are non-toxic and simply prepared (Tomitaka, Hirukawa, Yamada, Morishita, & Takemura, 2009).

Ferrites are used in applications such as magnetic ingredients in microelectronics (Alcalá, Briceño, Brämer-Escamilla, & Silva, 2017). Most ferrites used in manufacturing magnetic liquids are of the spinel composition (Sharma et al., 2017, Yan and Luo, 2017). Additionally, there are different and diverse applications of ferrites in unique technological sectors, such as electronic designs, humidity sensors, microwave reflection, drug-delivery processes, magnetic resonance imaging, and inductors. Ferrites are also used as high-density data-storage materials, converters, catalysts, and antenna bodies (Anupama, Rudraswamy, & Dhananjaya, 2017; El Moussaoui et al., 2016; Niu, Zong, Hu, & Wu, 2017; Patil, Pawar, Tilekar, & Ladgaonkar, 2016; Samoila et al., 2017, Winder, 2016).

The characteristic properties of ferrites can be improved by conjugation of other divalent metallic ions in their chemical structure; for example, the addition of cobalt ions to ferrite improves coercivity, due to enhanced magneto-crystalline anisotropy that results from the coupling of the spins of the cobalt and iron ions (Ghafoor et al., 2016). Cobalt ferrite (CoFe2O4; CFO) has attracted significant study in the last five decades due to its unique and tunable physical characteristics (Tatarchuk, Bououdina, Paliychuk, Yaremiy, & Moklyak, 2017). These qualities give CFO tremendous potential in several technologies, such as data storage, as a microwave absorber, high-sensitivity sensors, magneto-electronics, optoelectronics, catalyst investigations, and nanobiotechnology (Kumar, Singh, Zope, & Kar, 2017; Samavati and Ismail, 2017, Tatarchuk et al., 2017). Some investigations (Kumar, Reddy, Devi, & Sathiyaraj, 2016) have evaluated dielectric, structural, and gas-sensing performance of metal-substituted spinel (MFe2O4; M = Zn, Cu, Ni, and Co) ferrite nanoparticles. NiFe2O4, CuFe2O4, CoFe2O4, and ZnFe2O4 are commercially employed to sense liquefied petroleum gas.

Of the various ferrites, CFO possesses novel fascinating and physical characteristics that have led to extensive attention regarding potential biomedical applications (Sanpo, Berndt, Wen, & Wang, 2016), including its increased drug solubility and stability and decreased side effects (Gupta & Gupta, 2005). It has been used for magnetic orientation in drug delivery (Nasongkla et al., 2006), imaging factors and therapy of brain tumors (Reddy et al., 2006), as a drug-delivery vehicle in biomedical approaches (Byrappa, Ohara, & Adschiri, 2008), for advanced bacterial action of a drug carrier (Sun et al., 2004), and as the vector in drug delivery to the kidney and brain (Buteică et al., 2010; Thankachan, Kurian, Nair, Xavier, & Mohammed, 2014). Conjugation of metals to cobalt ferrite may produce new composite substances with improved antimicrobial action (Samavati & Ismail, 2017). In recent times, experimentation on antibacterial characteristics of ferrites has been very successful (Samavati & Ismail, 2017); most researchers have improved antibacterial quality by replacing copper by cobalt in CFO, manufacturing CuxCo1−xFe2O4 using a co-precipitation method. Substitution of cobalt by copper in CFO nanoparticles significantly changed the microstructure, crystal composition, and particle diameter and further developed the antibacterial activity (Samavati & Ismail, 2017).

This study investigated the structure of multifunctional nanoferrites with the nominal formula MxCo1−xFe2O4 (M = Zn, Cu, and Mn; x = 0.0, 0.25, 0.5, and 0.75) produced by the sol–gel method to improve their physical characteristics. Moreover, it aimed to recognize the potential of ferrite nanoparticles before and after gamma irradiation on selected pathogenic microbes, as possible candidates in various fields of biomedical applications.

Section snippets

Materials

All media components were purchased from Oxoid (UK) and Difco (USA). All reagents were of analytical grade. The chemicals used in the manufacture of the ferrites included ferric nitrate nonahydrate (Fe(NO3)3·9H2O, 98%), cobalt nitrate hexahydrate (Co(NO3)2·6H2O, 99.5%), copper nitrate hexahydrate (Cu(NO3)2·6H2O), manganese nitrate tetrahydrate (Mn(NO3)2·4H2O, 98%), zinc sulfate heptahydrate (ZnSO4·7H2O, 99%), citric acid (99.57%), and ethylene glycol (C2H6O2, 99.8%).

Synthesis of nanoferrites

A sol–gel technique was

X-ray diffraction analysis

Typical X-ray diffraction patterns of CFO nanoparticles, as-obtained and after annealing at different temperatures, are shown in Fig. 1. The most intense peaks, observed at 2θ values of 30.12°, 35.54°, 37.12°, 43.13°, 53.41°, 56.89°, and 62.62°, were indexed as the (220), (311), (222), (400), (442), (511), and (440) reflection planes, respectively, indicating the presence of a cubic spinel phase with the Fd3¯m space group (El-Batal, Gharib, Ghazi, Hegazi, & Hafz, 2016). The observed diffraction

Conclusions

The integration of metals such as zinc, copper, and manganese into CFO nanoparticles was studied. The sol–gel manufacturing technique used eco-friendly and cost-effective citric acid and ethylene glycol to initiate gel formation and subsequent nanoparticle formation. Complete identification and analysis revealed the surface structural morphology, elemental compositions, surface area, pore and pore volume sizes, crystallinity, and functional groups of the synthesized nanoferrites. The

Acknowledgments

The authors thank the Nanotechnology Research Unit (P.I. Prof. Dr. Ahmed I. El-Batal), Drug Microbiology Laboratory, Drug Radiation Research Department, National Center for Radiation Research and Technology, Egypt, for financing and supporting this study under the project Nutraceuticals and Functional Foods Production by using Nano/Biotechnological and Irradiation Processes. The authors also thank Dr. Mohamed Gobara (Military Technical College) and the Zeiss microscopy team in Cairo for their

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