Accepted Manuscript Microwave assisted extraction as an efficient approach for biosynthesis of zinc oxide nanoparticles: Synthesis, characterization, and biological properties
Hamid Reza Rajabi, Asghar Naghiha, Mansoure Kheirizdeh, Hamed Sadatfaraji, Ali Mirzaei, Zinab Moradi Alvand PII: DOI: Reference:
S0928-4931(16)32164-6 doi: 10.1016/j.msec.2017.03.090 MSC 7601
To appear in:
Materials Science & Engineering C
Received date: Revised date: Accepted date:
12 November 2016 5 March 2017 12 March 2017
Please cite this article as: Hamid Reza Rajabi, Asghar Naghiha, Mansoure Kheirizdeh, Hamed Sadatfaraji, Ali Mirzaei, Zinab Moradi Alvand , Microwave assisted extraction as an efficient approach for biosynthesis of zinc oxide nanoparticles: Synthesis, characterization, and biological properties. The address for the corresponding author was captured as affiliation for all authors. Please check if appropriate. Msc(2017), doi: 10.1016/j.msec.2017.03.090
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ACCEPTED MANUSCRIPT Microwave assisted extraction as an efficient approach for biosynthesis of zinc oxide nanoparticles: Synthesis, characterization,
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and biological properties
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Hamid Reza Rajabia,*, Asghar Naghihab, Mansoure Kheirizdeha, Hamed Sadatfarajic, Ali Mirzaeid, Zinab Moradi Alvanda
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a Chemistry Department, Yasouj University, Yasouj, 75918-74831, Iran.
b Department of Animal Sciences, Faculty of Agriculture, Yasouj University, Yasouj 75918-74831, Iran.
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c Department of Chemistry, University of Golestan, Gorgan, Iran
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d Medicinal Plant Research Center, Yasouj University of Medical sciences, Yasouj, Iran.
*Corresponding author. Tel. /Fax: +98 741 2242164. E-mail address:
[email protected],
[email protected] (H.R. Rajabi).
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ACCEPTED MANUSCRIPT ABSTRACT In the present study, microwave assisted extraction (MAE) was applied as an efficient, green and rapid approach to prepare the aqueous extract of Suaeda aegyptiaca (SA) plant. The obtained aqueous extracts at two different irradiation power (90 and 270 W; 15 min) in MAE process as
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well as maceration method (24 h) were used in a green and eco-friendly approach for the
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synthesis of zinc oxide nanoparticles (ZnO NPs). The synthesized ZnO NPs have been
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characterized via different techniques including UV-Vis absorption; fluorescence and Fourier transform infrared (FT-IR) spectroscopices, scanning electron microscopy (SEM), and X-ray
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diffraction (XRD). According to the results, the average size of the prepared ZnO particles was
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estimated around 60 nm. A broad absorption band around 382 nm in UV-Vis absorption spectrum and a maximum emission at wavelength of 458 nm in fluorescence spectrum clarified
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the successful biosynthesis of ZnO NPs. Moreover, the biological properties of the extracts and
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biosynthesized ZnO NPs were investigated by antimicrobial tests (i.e. Well-diffusion, minimum inhibitory concentration (MIC), minimum bactericidal concentration (MBC) tests), antifungal
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and antioxidant tests (total phenolic and flovonoid content, antioxidant activity against dipheny-
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picrylhydrazyl (DPPH), and ethylbenzothiazolin-6sulphonic acid (ABTS+)). Finally, DNA
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cleavage potential of the samples was studied, too.
Keywords: Microwave, Biosynthesis, ZnO nanoparticles, Antimicrobial tests, Antioxidant activity.
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ACCEPTED MANUSCRIPT 1. Introduction Recently, green synthesis of new nano-scaled materials has been considered as one of the most attractive synthetic methods, since they are eco-friendly, convenient, cheap and time saving, non-toxic [1]. Lately, plant extract based synthetic method is preferred as a promising
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and favorable single-pot biosynthesis strategy over other methods [2-4]. In spite of the chemical
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and physical methods which are needed the use of high temperature, pressure, energy and toxic
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chemicals, the biosynthetic methods are rapid, environment-friendly, non-pathogenic, and economic [5,6]. In comparison with traditional and/or some modern extraction methods,
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microwave assisted extraction (MAE) has been accepted as a potential and powerful alternative
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for the extraction of organic compounds from plant materials [7]. For example, Soxhlet extraction is the most common and is still used as a standard in all cases. However, a typical
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Soxhlet extraction, by conductive heating mechanism, will be completed in 5-6 h [8]; while,
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closed vessel extractions by microwave heating can be completed in 15 minutes [9]. Take supercritical fluid extraction (SFE) as another example; it is expensive, highly sophisticated,
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requires high pressure and perfect operator [10]. Beside, in comparison with ultrasound assisted
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extraction (UAE), MAE possessed higher efficiency and smaller solvent volume requirement for the extraction of some secondary metabolites [11].
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On the other hands, nano-structured zinc oxide (ZnO) particles, as nontoxic metal oxides, have been taken in deep consideration owing to their applications in various fields such as biomolecular detection [12], diagnostics [13] and micro electronics [14]. Moreover, due to the some specific properties of ZnO NPs such as microbial growth inhibition, [15] catalytic activity [16], photochemical properties [17], strong adsorption ability [18], carriers of antibiotics [19], strong antibacterial [20] and killing activities [21], this kind of NPs were used in different
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ACCEPTED MANUSCRIPT studies. It was proven that biological properties of ZnO are dependent in particle size; so that their antibacterial activities improved with decreasing their particle size to nano-scale [22]. Hence, with the above back ground information, in the present study a simple method has been improved for the biosynthesis of ZnO NPs, by aqueous extract of Suaeda aegyptiaca (SA) plant.
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SA is a well-known genus which also is known as Seablites as well as Seepweed. It usually
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grows in saline or alkaline soil habitats like coastal salt-flats [23]. Like many desert plants, SA is
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low shrub to 60 cm high, often sprawling (Fig.1). In addition leaves linear to fusiform, terete, tip acute progressively reduced along flowering stems. Some advantageous aspects of this halophyte
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plant are its high growth rate, high biomass production, and copious seed production in natural
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condition. Some of medicinal applications of SA such as its application for tooth and gum infections, as snuff for dizziness, headaches, hysteria, nausea, and nervous system was reported
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by Qasem [24]. The expression pattern of proteins and discuss their possible roles in adaptation
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of SA to salt treatments was evaluated firstly by Askari et al [25]. It was reported that expression of cyanase from SA can be induced by salt stress. The quantitative determination of some
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elements in the leaves of SA obtained from different regions of southern Iran after microwave-
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assisted acid digestion was reported by Chamkouri et al [26]. The aim of this work was to develop a green, simple, and eco-friendly approach for the synthesis
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of nano-sized ZnO particles. The synthetic method has been designed based on the plantmediated biological synthesis using aqueous microwave extract of SA. Previously, biosynthesis of ZnO NPs by various plants such as Aloe vera [6], Cinnamomum camphora [27], Azadirachta indica [28], cotton [29], Ruta graveolens [30] emblicaofficianalis [31], and Trifolium pretense [32] have been reported; however; to the best of our knowledge there is no wide studies concerning the biosynthesis of ZnO nanostructures by using MAE extract of SA as well as their
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ACCEPTED MANUSCRIPT biological properties, in literature. After characterization of the synthesized ZnO NPs by various techniques, the biological properties of the extracts and ZnO NPs were examined by different biological tests against some Gram-negative and Gram-positive bacteria and also against two funguses, comparatively. Finally, the interaction of the samples with DNA was investigated by
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electrophoresis method.
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2. Experimental
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Fig. 1: Photographical images of Suaeda aegyptiaca plant.
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2.1. Materials and apparatus The safe leaves of Suaeda aegyptiaca were collected and dried in dark at room temperature for few days and then homogenized to fine powder by a mechanical grinder. The grinded pieces stored in airtight bottles. All reagents and solvents required for the biological and antioxidant tests were purchased from Aldrich and Merck companies and used without further purification. For biological tests, the solid medium of nutrient agar (Merck, Germany) was used for preparing the nutrient plates while Mueller Hinton Broth (Scharlab) was applied as the liquid 5
ACCEPTED MANUSCRIPT culture media. Sabouraub dextrose agar (Oxoid, Hampshire, England) was used as solid media for preparing the plates in antifungal studies. The Escherichia coli (ATCC 25922), Pseudomonas aereuguinosa (ATCC 9027), Staphylococcus aureus (ATCC 6538) and Bacillus subtilis (ATCC 6633) were used as Gram-negative or positive bacterial strains in antibacterial activity
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evaluations.
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In MAE process, a microwave device (model of KOC-9N8T, DAEWOO Company, Korea) was
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used to carry out the extraction step. The FT-IR spectra of the samples were recorded on a JASCO-680 apparatus in the spectral range of 4000–400 cm-1, using KBr disks. UV–Vis
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absorption spectra of all samples were measured by a Perkin-Elmer lambda 25
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spectrophotometer. All fluorescence spectra were obtained by a Cary Eclipse fluorescence spectrophotometer (Varian). SEM images were recorded on a Philips XL30 series instrument
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using a gold film for loading the dried particles on the instrument. The X-ray diffraction (XRD)
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pattern was obtained using STOE-Stidy-mp Diffractometer with Cu Kα source (λ=1.541786 Å).
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2.2. Preparation of plant extracts
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2.2.1. Conventional extraction
20 g of the dried and powdered leaves of SA was mixed with 250 ml double distilled water in a
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Meyer flask and kept in darkness, at room temperature, for 48 h. The obtained extract was filtered and placed into oven for 48 h, at 40 °C.
2.2.2. Microwave assisted extraction (MAE) The plant powder (20 g) were mixed with 250 ml double distilled water, in Round-bottom flask and then irradiated under different power (90W and 270W), for 15 minutes using a home-made
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2.3. Biosynthesis of ZnO NPs
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For the biosynthesis of ZnO NPs, 50 ml of obtained aqueous extracts were reacted with 50 ml of
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0.002 mol.L-1 Zn(NO)3.4(H2O) and stirred at constant temperature (70 °C) for 3 h. The
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precipitated particles were collected through centrifugation at 4000 rpm for 10 minute. Then, product washed with distilled water carefully and dried at 100 °C overnight. To remove the plant
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impurities from ZnO NPs, the samples were heated at 450 °C for 4 h [34].
2.4. Biological activities
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2.4.1. Antibacterial activity
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Antibacterial activity of the obtained samples was examined against four bacteria including E. coli (ATCC: 25922) and P. aeruginosa (ATCC: 9027) as Gram-negative bacteria and
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Staphylococcus aureus (ATCC: 6538) and Bacillus subtilis (ATCC: 6635) as Gram-positive
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bacteria by disk diffusion method using nutrient agar as medium [35]. In this method, the samples with different concentrations (15 and 7.5 and 3.75 mg/mL) were prepared in dimethyl
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sulfoxide (DMSO). Then, a sterile paper disk impregnated with a solution of the compounds was placed on the surface of agar plates that have been inoculated with pathogen bacteria. The resulting plates were incubated for 24 h at 37 °C, then; the diameters of the inhibition zones around the disks were measured.
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ACCEPTED MANUSCRIPT 2.4.1.1. Well Diffusion Test Well diffusion method was used to determine in vitro antibacterial activities of SA aqueous extracts as well as ZnO NPs against four bacteria strain including E. coli (ATCC: 25922) and P. aeruginosa (ATCC: 9027) as Gram-negative bacteria and Staphylococcus aureus (ATCC:
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6538) and Bacillus subtilis (ATCC: 6635), as Gram-positive bacteria. In brief, 0.1 ml of each
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organism was spread uniformly using a sterile swab on the Muller Hinton Agar medium. Since,
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it was reported that DMSO has not significant biological effect against the selected bacteria [36], it was considered as a negative control test. Different concentrations of samples (i.e. 25,
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50, and 100mg/ml) were prepared in DMSO, respectively, then, 50 µl of samples poured on the
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plates. After incubation (24 h, 37 °C), the diameter of inhibition zone (mm) surrounding the
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well was considered as antibacterial activities measure of the samples.
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2.4.1.2. Minimum inhibitory concentration (MIC) test In MIC, antibacterial activities of the samples were evaluated by means of Broth dilution
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method [37]. By the serial dilution procedure, the various sample solutions were prepared in the
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concentration range of 0.0024-12.5 mg/ml in the sterilized conditions. Then, 0.65 ml of Muller Hinton Broth and 0.1 ml of the microorganism were added to each tube containing 0.25 ml of
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the sample. After incubation (24 h, 37 °C), the minimum sample concentration which prevent the growth of the microorganism was considered as MIC.
2.4.1.4. Minimum bactericidal concentration (MBC) test In MBC screening, a loop full of diluted sample solutions (from 0.0024 mg/mL to 12.5 mg/ml) was sub-cultured onto the Muller Hinton Agar medium and incubated at 37 °C for 24 h. The
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2.4.1.5. Antifungal activity test
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Antifungal activity of the samples was tested through the well diffusion technique, against two
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funguses including Candida albicans and Aspergillus oryzae, by various concentrations of the
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samples (25, 50 and 100 mg/ml) which prepared in DMSO [39]. In Brief, 0.1 ml of each fungus was speared on to the Sabouraud agar medium, then, 50 μl of the sample was dumped in wells
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made in Plate. After incubation the plates at 37 °C for 24 h and at 32 °C for 3 days, respectively,
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the inhibition zone (mm) was measured and recorded as the antifungal activity of the samples.
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2.5. Determination of total phenolic and flavonoid contents
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measured using the Folin-Ciocalteau reagent with slight change, the results were expressed as
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Gallic acid equivalent/g extract, at maximum wavelength of 765 nm [40]. The total falavonoid contents of the samples were also determined with aluminum chloride (AlCl3), in terms of Rutin
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equivalents/g extract, at 510 nm according to the literature [41].
2.6. Determination of antioxidant activity based on dipheny-picrylhydrazyl (DPPH) and ethylbenzothiazolin-6sulphonic acid (ABTS+) The antioxidant activities of the samples were examined using two assays: (1) 1,1-diphenyl-2picrilhydrazyl (DPPH) radical [42], and (2) ethylbenzothiazolin-6sulphonic acid (ABTS+) [43]. In DPPH and ABTS+ methods, the absorbance of the final solution samples was recorded by 9
ACCEPTED MANUSCRIPT UV-Vis absorption spectrophotometric technique at 517, 734 nm, respectively. The inhibition percentage of DPPH and ABTS+ free radicals were free radical was calculated by following equation [44]: Inhibition (%) = [(A0-A1)/A0]×100
(Eq.1)
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Where A0 is the absorbance of control and A1 is the absorbance of the tested samples.
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2.7. DNA interaction study
Pure DNA was extracted with CinaPure DNA kit, DNA cleavage process and agarose gel for gel
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electrophoresis method was perfomed according to previous reports [45, 46].
3. Results and Discussion
3.1.1. Spectroscopic studies
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3.1. Characterization of the biosynthesized ZnO NPs
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The optical properties of biosynthesized ZnO NPs were investigated using UV-Vis absorption and fluorescence spectroscopic methods. UV-Vis absorption spectroscopy is a useful and
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beneficial technique for investigation of the optical properties of nano-scaled particles [47].
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Figure 2 shows the absorption spectra of the prepared ZnO NPs. As it can be seen from Fig.2, a sharp absorption band around the wavelength of 400 nm is clear in UV-Vis absorption spectra which can be attributed to the electron transitions from the valence band to the conduction band (O2p-Zn3d) assign to the basic band gap energy of ZnO crystals [48, 49]. Besides, from the excitonic absorption peak, it is possible to calculate the direct optical band gap energy (Eg) of the semiconductor nanoparticles [50] (Fig.2; inside). The Eg were obtained from extrapolation of the plot of (αhʋ)2 vs the photoenergy (hʋ) to zero[51]. The Eg values of 4.05, 3.93 and 2.02 eV were
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ACCEPTED MANUSCRIPT obtained for ZnO NPs synthesized by the aqueous extracts obtained using MAE at 90, 270 w and maceration methods, respectively, which the results were in agreement with the previous report [45]. It is worth to note that the obtained Eg values for ZnO NPs synthesized by MAE aqueous extract is more than that of synthesized by maceration method. Since, the optical band gap value
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of materials is related to the particle size [52], it can be concluded that the MAE method can
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Fig.2. UV-Vis absorption spectra of the prepared ZnO NPs prepared by MAE at (a) 90, (b) 270
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w and (c) maceration of Sa; the respective plot of (αhʋ)2 vs. hʋ
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Figure 3 shows the photoluminescence spectra of ZnO NPs prepared by different SA aqueous extract, at room temperature (Fig.3). Photoluminescence analysis shows a maximum emission
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peak at 458 nm. It was reported that the blue emission wavelength at around 460 nm is due to the
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intrinsic defects such as oxygen and zinc interstitials, as well as the presence of singly ionized oxygen vacancies [53]. The blue emission is caused by the radiative recombination of a
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photogenerated hole with an electron occupying the oxygen vacancy [54].
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Fig.3. PL spectra of the prepared ZnO NPs by maceration and MAE at 90 and 270 w.
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Figure 4 indicates the recorded FT-IR spectra of ZnO NPs by using various extracts. The detected peaks in FT-IR results of the samples can be corresponded to the presence of some
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phytoconstituents like alcohol (3394 cm-1), aldehyde (1627 cm-1), and amine (3394, 1396 cm-1).
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Moreover, the presence of a distinguish peak around 500 cm-1 may be related to ZnO NPs [55,56]. Indeed, these phytochemicals are able to interact with the surface of particles; subsequently, facilitate the stabilization of ZnO NPs. In other word, probably, the various secondary metabolites in the matrix of SA plant can act as natural stabilizing agents, in the biosynthesis procedure of ZnO NPs.
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Fig.4. FT-IR spectra of the prepared ZnO NPs by MAE at (a) 90, (b) 270 w and (c) maceration.
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3.1.3. Crystal structure and morphology
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In addition, characterization of the biosynthesized ZnO NPs was carried out by XRD and SEM techniques. Based on XRD patterns (Fig. 5), the observed peaks at 2θ position of 31.87, 45.59,
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56.63, 66.35 can be related to reflection from (1 0 0), (1 0 2), (1 1 0), (2 0 0) crystal planes
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confirm that ZnO NPs were produced in Wurtzite structure [57,58]. In addition, it shows some unidentifiable peaks which differ from ZnO NPs. They may be related to remained organic matter or amorphous impurities [59].
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Fig. 6. SEM images of the prepared ZnO NPs by (a) maceration, MAE at (b) 90 and (c) 270 w.
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Figure 6 shows SEM images of ZnO NPs prepared by both mentioned routes. As it is quite clear,
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the morphology and size of the particles prepared by the two methods is differs from each other. SEM micrographs visualize the effect of various synthesis conditions on the morphology of the nanoparticles. In comparison with maceration, MAE process can result in the uniform particles ( ZnO (macerated)~ E (270 w). The low antioxidant properties of
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the macerated extracts may be as a result of destroying impact of light as well as O2 on some extract’s components during the long extraction time (48 h) [67]. It was reported that the
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Fig. 9. According to the results, inhibitory (%) of the extract samples were founded as the following order: E (90 w)> E (macerated)> E (270 w); while, the order changed for ZnO NPs as:
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ACCEPTED MANUSCRIPT and organic medium, while DPPH is merely soluble in organic solvents; subsequently, it would
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Fig. 9. The results of antioxidant capacity by (a) DPPH, (b) ABTS+ assays of the samples and (c) photographical of (ABTS(+ test of the sample (A) in the absence, (B) presence of ABTS+ solution and (C) the sample in the presence of ABTS+ solution after 6 minutes
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ACCEPTED MANUSCRIPT 4. Conclusion The present study was reported a green, reusable, reproducible and nontoxic route for biosynthesis ZnO NPs using the aqueous extract of the Suaeda aegyptiaca plant, by maceration and microwave assisted extraction methods. The current study suggests that MAE can be
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NPs. By optimizing the extraction conditions as well as the applied irradiation power, it is
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possible to perform the microwave extraction for more completed extractions and it may be provided a more beneficial medium for the synthesis of nanoparticles with high biological effect,
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in comparison with other conventional methods. The aqueous extract of SA obtained by MAE
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References
[1] C. Vidya, S. Hiremath, M.N. Chandraprabha, M.A.L. Antonyraj, I.V. Gopal, A. Jain, K.
CE
Bansal, Green synthesis of ZnO nanoparticles by Calotropis Gigantea. Inter. J. Current Eng.
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Technol. (2013) 118-120.
[2] R. Yuvakkumar, J. Suresh, A. Joseph Nathanael, M. Sundrarajan, S.I. Hong, Novel green synthetic strategy to prepare ZnO nanocrystals using rambutan (Nephelium lappaceum L.) peel extract and its antibacterial applications, Mater. Sci.Eng. C 41 (2014)17-27. [3] R. Yuvakkumar, J. Suresh, B. Saravanakumar, A. Joseph Nathanael, Sun Ig Hong, V. Rajendran, Rambutan peels promoted biomimetic synthesis of bioinspired zinc oxide nanochains for biomedical applications, Spectrochim. Acta Part A 137 (2015) 250-258.
32
ACCEPTED MANUSCRIPT [4] H.J. Prabu, I. Johnson, Plant-mediated biosynthesis and characterization of silver nanoparticles by leaf extracts of Tragia involucrata, Cymbopogon citronella, Solanum verbascifolium and Tylophora ovate, Karbala Intern. J. Modern Sci. 1 (2015) 237–246. [5] S. Ahmed, M. Ahmad, B. Lal Swami, S. Ikram, A review on plants extract mediated
T
synthesis of silver nanoparticles for antimicrobial applications: A green expertise, J. Adv. Res. 7
IP
(2016) 17-28.
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[6] K. Ali, S. Dwivedi, , A. Azam, Q. Saqui, M. S. Al-Said, A.A. Alkhedhairy, J. Musarrat, Aloe vera extract functionalized zinc oxide nanoparticles as nanoantibiotics against multi-drug
US
resistant clinical bacterial isolates, J. Colloid. Interf. Sci. 472 (2016) 145–156.
AN
[7] L. Yuan, H. Li, R. Ma, X. Xu, C. Zhao, Z. Wang, F. Chen, X. Hu, Effect of energy density and citric acid concentration on anthocyanins yield and solution temperature of grape peel in
M
microwave-assisted extraction process, J. Food. Eng. 109 (2012) 274–280
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[8] J.P. Fan, R.F. Zhang, J.H. Zhu, Optimization of microwave-assisted extraction of total
(2010) 3487–3500.
PT
triterpenoid in Diospyros kaki leaves using response surface methodology. Asian J. Chem. 22
CE
[9] C.E. Meloan, Chemical Separations: Principles, Techniques and Experiments, Wiley (1999). [10] C-H. Chan, R Yusoff, G-C. Ngoh, FW-L. Kung Microwave-assisted extractions of active
AC
ingredients from plants, J. Chromatogr. A 1218 (2011) 6213–6225. [11] J. Li, Y-G. Zu, Y-J. Fu, Y-C. Yang, S-M. Li, Z-N. Li, M. Wink, Optimization of microwave-assisted extraction of triterpene saponins from defatted residue of yellow horn (Xanthoceras sorbifolia Bunge.) kernel and evaluation of its antioxidant activity. Innov. Food Sci. Emerg. Technol. 11 (2010) 637–664
33
ACCEPTED MANUSCRIPT [12] A. Choi, K. Kim, H.I. Jung, S.Y. Lee, ZnO nanowire biosensors for detection of biomolecular interactions in enhancement mode, Sensor Actuat. B-Chem. 148 (2010) 577-582. [13] R.D. Munje, S. Muthukumar, S. Prasad, Lancet-free and label-free diagnostics of glucose in sweat using Zinc Oxide based flexible bioelectronics, Sensor Actuat. B-Chem. 238 (2017) 482-
T
490.
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[14] A.C. Mofor, A.S. Bakin, B. Postels, M. Suleiman, A. Elshaer, A. Waag, Growth
CR
of ZnO layers for transparent and flexible electronics, Thin Solid Films. 516 (2008) 1401-1404. [15] S. Azizi, M. Rosfarizan, A. Bahadoran., S. Bayat, R. Abdul Rahim, A. Ariff, W.Z. Saad,
US
Effect of annealing temperature on antimicrobial and structural properties of bio-synthesized
AN
zinc oxide nanoparticles using flower extract of Anchusa italic, J. Photochem. Photobio. B 161 (2016) 441–449.
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[16] L. Soto-Vázquez, M. Cotto, C. Morant, J. Duconge, F. Márquez, Facile synthesis of ZnO
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nanoparticles and its photocatalytic activity in the degradation of 2-phenylbenzimidazole-5sulfonic acid, J. Photochem. Photobio. A332 (2017) 331–336.
PT
[17] A. Chapel, S. Ben Dkhil, S. Therias, J-L. Gardette, D. Hannani, G. Poize, M. Gaceur, S-M.
CE
Shah, P.W.W. Chung, C. Videlot-Ackermann, O. Margeat, A. Rivaton, Effect of ZnO nanoparticles on the photochemical and electronic stability of P3HT used in polymer solar cells.
AC
Sol. Energ. Mat. Sol. C 155 (2016) 79–87. [18] F. Zhang, X. Chen, F. Wu, Y. Ji, High adsorption capability and selectivity of ZnO nanoparticles for dye removal, J. Colloid Surface A 509 (2016) 474-483. [19] C. Saikia, M. K. Das, A. Ramteke, T. K. Maji, Evaluation of folic acid tagged aminated starch/ZnO coated iron oxide nanoparticles as targeted curcumin delivery system, Carbohyd. Polym. 157 (2016) 391–399.
34
ACCEPTED MANUSCRIPT [20] D. Wu., Z. Chen., K. Cai, D. Zhuo, J. Chen, B. Jiang, Investigation into the antibacterial activity of monodisperse BSA-conjugated zinc oxide nanoparticles, Curr. Appl. Phys. 14 (2014) 1470–1475. [21] G.D. Venkatasubbu , R. Baskar , T. Anusuya, CA. Seshan, R. Chelliah, Toxicity mechanism
T
of titanium dioxide and zinc oxide nanoparticles against food pathogens, Colloid Surface B 148
IP
(2016) 600–606
CR
[22] H. Kaya, F. Aydın, M. Gürkan, S. Yılmaz, M. Ates, V. Demir, Z. Arslan, A comparative toxicity study between small and large size zinc oxide nanoparticles in tilapia
AN
parameters, Chemosphere 144 (2016) 571–582.
US
(Oreochromisniloticus): Organ pathologies, osmoregulatory responses and immunological
[23] J.P. Fan, R.F. Zhang, J.H. Zhu, Optimization of microwave assisted extraction of total
M
triterpenoid in diospyros kaki leaves using response surface methodology, J. Chem. 22 (2010)
ED
3487–3500.
[24] J.R. Qasem, Pak. J. Bot. 47 (2015) 551-570.
PT
[25] H. Askari, J. Edqvist, M. Hajheidari, M. Kafi, G. Hosseini Salekdeh, Proteomics 6 (2006)
CE
2542–2554.
[26] N. Chamkouri, M. Torabpour, F. Ghafarizadeh, J. Bas. Res. Med. Sci. 2 (2015) 49-56.
AC
[27] Y. Qian, J. Yao, M. Russel, K. Chen, X. Wang, Characterization of green synthesized nanoformulation (ZnO–A. vera) and their antibacterial activity against pathogens, Environ. Toxicol. Phar. 39 (2015) 736-746. [28] J. Huang, Q. Li, D. Sun, Y. Lu, Y. Su, X. Yang, H. Wang, Y. Wang, W.S hao, N. He, Biosynthesis of silver and gold nanoparticles by novel sundried Cinnamomum camphora leaf, Nanotechnology 18 (2007) 105104.
35
ACCEPTED MANUSCRIPT [29]
R.
Aladpoosh,
M.
Montazer,
in biosynthesis of ZnO nanorods
The
producing
role
of
cellulosic
multifunctional
chains
properties:
of
cotton
Mechanism,
characterizations and features, Carbohyd. Polym. 126 (2015) 122-129. [30]
K. Lingaraju,
H. Raja
K. Manjunath,
R. B. Basavaraj,
H. Nagabhushana,
K. Lingaraju, H. Raja Naika, K. Manjunath, R. B. Basavaraj,
T
G. Nagaraju, D. Suresh,
Naika,
IP
H. Nagabhushana, G. Nagaraju, D. Suresh, Biogenic synthesis of zinc oxide nanoparticles
CR
using Ruta graveolens (L.) and their antibacterial and antioxidant activities, Appl. Nanosci. 6 (2016) 703–710.
US
[31] B. Ankamwar, D. Chinmay, A. Absar, S. Murali, Biosynthesis of gold and silver
AN
nanoparticles using emblica officinalisfruit extract, their phase transfer and transmetallation in an organic solution, J. Nanosci. Nanotechnol. 10 (2005) 1665–1671.
M
[32] R. Dobrucka, J. Długaszewska, Biosynthesis and antibacterial activity of ZnO nanoparticles
ED
using Trifolium pratense flower extract, Saudi J. Biolog. Sci. 23 (2016) 517-523. [33] H.R. Rajabi, H. Deris, H. Sadat Faraji, Facile and green biosynthesis of silver
PT
nanostructures by aqueous extract of suaeda acuminata afer microwave assisted extraction,
CE
Nanochem. Res. 1 (2016) 36-41.
[34] S. Azizi, M.B. Ahmad, F. Namvar, R. Mohamad, Green biosynthesis and characterization of
AC
zinc oxide nanoparticles using brown marine macroalga Sargassum muticum aqueous extract, Mater. Lett. 116 (2013) 275-277. [35] J. Zhishen, T. Mengcheng, W. Jianming, The determination of flavonoid contents in mulberry and their scavenging effects on superoxide radicals, Food Chem. 64 (1999) 555-559.
36
ACCEPTED MANUSCRIPT [36] M. Montazerozohori, S.A. Musavi, A. Naghih., S. Veyseh, Some new IIB group complexes of an imidazolidine ligand: Synthesis, spectral characterization, electrochemical, thermal and antimicrobial properties, J. Iran. Chem. Sco. 126 (2014)227–238. [37] S. Ravikumar, R. Gokulakrishnan, J. Anandha Raj, Nanoparticles as a source for the
T
treatment of fish diseases, Asia Pac. J. Trop. Dis. 2 (2012) S703-S706.
IP
[38] S. Ravikumar, R. Gokulakrishnan, K. Selvanathan, S. Selvam, Antibacterial activity of
CR
metal oxide nanoparticles against ophthalmic pathogens, Int. J. Pharm. Res. Dev. 3 (2011) 122127.
US
[39] N. Raman, A. Sakthivel, K. Rajasekaran, Synthesis and Spectral Characterization of
[40]
AN
Antifungal Sensitive Schiff Base Transition Metal Complexes, Mycobiology 35 (2007) 150-153. A. Mirzaei, N. Mirzaei, Z. Salehpour, S.A. Khosravani, M. Amouei, Phenolic, ascorbic
M
contents and antioxidant activities of 21 Iranian Fruits. Life Sci. J. 10 (2013) 1240-1245.
ED
[41] I. Kosalec, M. Bakmaz, S. Pepeliniak, S. Vladimir-Knezevic, Quantitative analysis of the flavonoids in raw propolis from northern, Croatia, Acta Pharm. 54 (2004) 65-72.
PT
[42] A.V. Gadow, E. Joubert, C.F. Hansmann, Comparison of antioxidant activity of aspalathin
CE
with that of other plant phenols of Rooibosed tea (Aspalathon linearis),α-tocopherol, BHT and BHA. J Agric. Food Chem.45( 1997) 632-638.
AC
]43[ R. Re, N. Pallegrini, A. Proteggente, A. Pannala, M. Yang, C. Rice-Evans, Antioxidant activity applying an improved ABTS radical cation decolorization assay, Free Radic. Biol. Med. 26 (1999) 1231-1237. ]44[ M.A. Ebrahimzadeh, S.M. Nabavi, S.F. Nabavi, F. Bahramian , A.R. Bekhradnia, Antioxidant and free radical scavenging activity of H. officinalis L. var. angustifolius, V. odorata, B. hyrcana and C. speciosum, Pak. J. Pharm. Sci. 23 (2010) 29-34.
37
ACCEPTED MANUSCRIPT [45[ A.D. Khalaji, Gh. Grivani, M. Rezaei, K. Fejfarova, M. Dusek, Synthesis and spectral characterization of mercury(II) complexes with the bidentate Schiff base ligand N,N′-bis(2,3dimethoxybenzylidene)-1,2-diaminoethane: The crystal structures of [Hg((23-MeO-ba)2en)I2] and [Hg((23-MeO-ba)2en)Br2], Polyhedron 30 (2011) 27-90.
T
]46[ M. Montazerozohori, S. Mojahedi Jahromi, Naghiha A., Some new cadmium complexes:
IP
Antibacterial/antifungal activity and thermal behavior, J. Ind. Eng. Chem. 20 (2014) 2463-2470.
CR
]47[ H.R. Rajabi, M. Farsi, Study of capping agent effect on the structural, optical and
US
photocatalytic properties of zinc sulfide quantum dots, Mater. Sci. Semicon. Proc.48 (2016) 14– 22.
AN
]48[ K. Harish, R. Renu, Structural and Optical Characterization of ZnO Nanoparticles Synthesized by Microemulsion Route, Int. Lett. Chem. Phys. Astron. 14 (2013) 26-36.
M
]49[ D. H. Zhang, Z. Y. Xue, and Q. P. Wang, “Formation of ZnO nanoparticles by the reaction
ED
of zinc metal with aliphatic alcohols, J. Phys. Chem. D 35 (2002) 2837–2840.
PT
]50[ H.R. Rajabi, O. Khani, M. Shamsipur, V. Vatanpour, High-performance pure and Fe3+-ion doped ZnS quantum dots as green nanophotocatalysts for the removal of malachite green under
CE
UV-light irradiation, J. Hazard. Mater. 250–251 (2013) 370–378.
AC
]51[ M. Roushani, M. Shamsipur, H.R. Rajabi, Highly selective detection of dopamine in the presence of ascorbic acid and uric acid using thioglycolic acid capped CdTe quantum dots modified electrode, J. Electroanal. Chem. 712 (2014) 19–24. [52] O. Khani, H .R. Rajabi, M.H. Yousefi, A.A. Khosravi, M. Jannesari, M. Shamsipur, Synthesis and characterizations of ultra-small ZnS and Zn(1-x)FexS quantum dots in aqueous media
and
spectroscopic
study
of
their
Spectrochim. A 79 (2011) 361–369.
38
interactions
with bovine serum albumin,
ACCEPTED MANUSCRIPT ]53[ V. Viswanath, V. C. Janu, Synthesis, effect of capping agents, structural, optical and photoluminescence properties of ZnO nanoparticles A. K. Singh, J. Lumin. 129 (2009) 874–878. ]54[ S. Talam, S.R. Karumuri, N. Gunnam, Synthesis, Characterization, and Spectroscopic Properties of ZnO Nanoparticles, ISRN Nanotechnology 2012 (2012) 6 pages.
T
[55] R. Zamiri, A. Zakaria, H. Abbastabar Ahangar, M. Darroudi, A. Khorsand Zak, G.P.C.
IP
Drummen, J. Alloys Comp. 516 (2012) 41-48.
CR
[56] K.D. Bhatte, D.N. Sawant, D.V. Pinjari, A.B. Pandit, B.M. Bhanage, Material Lett. 77 (2012) 93-95.
US
[57] M.C.C. Silva, A.B.D. Silva, F.M. Teixeira, P.C.P.D. Sousa, M.M.R. Rondon, J.E.R.H.
AN
Júnior, L.R.L. Sampaio, S.L. Oliveira, A.N.M. Holonda, S.M.M.D. Vasconcelos, Asian Pacific J. Trop. Med. 3 (2010) 332-341.
M
[58] H. Thakuria, B.M. Borah, G. Das, ZnO Nanoparticles from a Metal-Organic Framework
ED
Containing ZnII Metallacycles, Eur. J. Inorg. Chem. (2007) 524–529. ]59[ Y. Mo, Y. Tang, S. Wang, J. Ling, H. Zhang, D. Luo, Green synthesis of silver
PT
nanoparticles using phlomis leaf extract and investigation of their antibacterial activity, Mat.
CE
Lett. 138 (2015) 251-254.
[60] H.R. Ghorbani, F. Parsa Mehr, H. Pazoki, B. Mosavar Rahmani, Synthesis of ZnO
AC
nanoparticles by precipitation method, Orient. J. Chem. 31 (2015) 1219-1221. ]61[ W. Waldeck, E. Heidenreich, G. Mueller, M. Wiessler, K. Tóth, K. Braun, ROS-mediated killing efficiency with visible light of bacteria carrying different red fluorochrome proteins, J. Photochem. Photobio. B 109 (2012) 28-33.
39
ACCEPTED MANUSCRIPT ]62[ M. J. Divya, C. Sowmia, K. Joona, K. P. Dhanya, synthesis of zinc oxide nanoparticle from hibiscus rosa-sinensis leaf extract and investigation of its antimicrobial activity, Res. J. Pharma. Biol .Chem. Sci. 4 (2013) 1137-1142. [63[ G.S. Watson, D.W. Green, L. Schwarzkopf, X. Li, B.W. Cribb, S. Myhra, Jolanta A.
T
Watson, A gecko skin micro/nano structure – A low adhesion, superhydrophobic, anti-wetting,
IP
self-cleaning, biocompatible, antibacterial surface, Acta Biomaterialia. 21 (2015) 109-122.
CR
]64[ S. Chakraborti, A.K. Mandal, S. Sarwar, P. Singh, R. Chakraborty, P. Chakrabarti, Bactericidal effect of polyethyleneimine capped ZnO nanoparticles on multiple antibiotic
US
resistant bacteriaharboring genes of high-pathogenicity island Colloids and Surfaces B:
AN
Biointerfaces. 121 (2014) 44-53.
]65[ Q. Yu, B. Zhang, J. Li, B. Zhang, H. Wang, M. Li, Endoplasmic reticulum-derived reactive
M
oxygen species (ROS) is involved in toxicity of cell wall stress to Candida albicans, Free Radical
ED
Biol. Med. 99 (2016) 572-583.
[66[ R.K. Salar, P. Sharma, N. Kumar, Enhanced antibacterial activity of streptomycin against
PT
some human pathogens using green synthesized silver nanoparticles, Resource-Efficient
CE
Technol. 1 (2015) 106-115.
[67] B.S. Reddy, S.V. Reddy, N.K. Reddy, Physical and magnetic properties of (Co, Ag) doped
AC
ZnO nanoparticles, J. Mater. Sci. Mter. Electron. 24 (2013) 5204–5210. [68] S.Z. Mohammadi, M. Khorasani-Motlagh, Sh. Jahani, M. Yosefi, Synthesis and Characterization of α-Fe2O3 nanoparticles by microwave method, Int. J. Nanosci. Nanotech. 8 (2012) 87-92. ]69[ P. Deepa, P.K. Kaleena, K. Valivittan, Antioxidant potential of Sansevieria roxburghiana Schult and Schult. f, Asian. J. Pharm. Clin. Res. 5 (2012) 166-169.
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Graphical abstract
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ACCEPTED MANUSCRIPT Highlights: ►New report on biosynthesis of ZnO NPs by plant extract based on microwave extraction ►Spectroscopic characterization of the prepared ZnO NPs.
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► Antimicrobial and antioxidant investigations of the prepared samples.
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