One step green synthesis of larvicidal, and azo dye degrading antibacterial nanoparticles by response surface methodology

https://doi.org/10.1016/j.jphotobiol.2018.11.020Get rights and content

Highlights

  • Iron oxide and manganese oxide nanoparticles were synthesized using Acorus calamus.

  • Polyphenol compounds were responsible for bio-reduction and stabilization.

  • Showed excellent photocatalytic activities in reducing dyes at 0.03%.

  • Nanoparticles showed larvicidal activity at 30 μg/ml concentration.

  • Nanoparticles inhibited P. aeruginosa and A. flavus at 40 μg/ml concentration.

Abstract

The present study explored the one step extracellular green synthesis of Iron oxide (FexOy) and manganese oxide nanoparticles (MnNPs) using aqueous extract of Acorus calamus rhizome. The organic chemicals including polyphenol compounds responsible for bio-reduction and stabilization from the polyphenol enriched microwave irradiated aqueous extract of Acorus calamus were studied using GC–MS analysis. Further, their synthesis conditions were optimized using response surface methodology (RSM) and central composite design (CCD) using three variables. The green synthesized Iron oxide and Manganese oxide NPs were characterized by UV, FTIR, XRD, TEM and SEM. Results indicated that the Iron oxide NPs and mixture of iron and manganese NPs showed photocatalytic excellent activities in reducing dyes like methylene blue (0.1%) and Congo red (0.25%) at 0.03% NPs. However, Mn NPs showed moderate activity. On a contrary, manganese showed better larvicidal activity compared to Iron oxide NPs against the phytopathogens commonly affecting the vegetable crops. The present finding showed that high mortality rate at 30 μg/ml concentration of manganese NPs was comparatively interesting. In addition, NPs overall had appreciable activity with P. aeruginosa being more sensitive to Iron oxide NPs (22 ± 2 mm zone of inhibition) and manganese NPs (13 ± 2 mm zone of inhibition) and Iron oxide NPs completely inhibited the growth of A. flavus at 40 μg/ml concentration.

Introduction

Nanoparticle research is of great interest worldwide due to unique characteristics [1]. Classical way of synthesizing nanoparticle like attrition and pyrolysis have several negatives in them such as defective surface formation, low productivity, ever increasing manufacturing cost, and require large amount of energy. Also, chemical synthesis methods involve the utilization of chemicals which are toxic, further leads to the formation of hazardous by products chemicals [2]. As a result, that there is an ever increasing need to establish and follow clean, nontoxic, and environment-benign procedures for synthesis of nanoparticles (NPs). Synthesis of NPs by green technology is emerging as an efficient method enabling to impart steric stabilization eliminating aggregation concerns. It helps to end the negative effects of using sodium borohydride and several other hazardous chemicals as a reducing agent in conventional synthesis [3]. The utilization of environmentally friendly materials like plant, bacteria, and fungi for the synthesis of NPs gives various advantages of eco-friendliness and extraordinary compatibility for various applications of industrial, pharmaceutical and biomedical importance [4]. In the green synthesis of NPs, plant extracts are more advantageous as they eliminates the laborious process involving cell cultures and can be easily scaled-up for large-scale synthesis under nonaseptic conditions, Plants secrete molecules of functional ability for the reaction, in accordance with the principles of green chemistry [5]. The potent plant extract we have used, Acorus calamus is a natural medicinal plant [6].

There are reports of successful synthesis of iron NPs utilizing green tea leaf and sorghum bran extracts [7,8]. Nanosized iron particles are of huge value in environmental bioremediation. They are the most widely reported in specific applications of degradation of organic and inorganic pollutants [[9], [10], [11]]. In recent years iron oxide NPs have attracted much more attention due to their properties such as surface-to-volume ratio, superparamagnetism, easy separation methodology and greater surface area [12]. These iron oxide NPs have potential application in magnetic resonance imaging, waste treatment, catalysts, and environmental remediation [13]. Iron NPs are very important for abatement of environmental pollution such as degradation of chlorinated organic pollutants, organic dyes, and heavy metals removal. It was also reported that the green synthesized NPs catalyzed hydrogen perioxide for the degradation of the bromothymol blue [14,15]. Few reports of manganese oxide nanoparticle synthesis were reported for the electrochemical sensing of 4- Nitrophenol [[16], [17], [18]]. Statistical methods help in effective variables and the interaction between different important parameters [19]. Response surface methodology (RSM) is a widely used mathematical in combination with statistical analysis method which improves and optimizes processes through evaluation of the interaction effects among process variables [20,21]. An alarming increase in the use of synthetic complex organic dyes has been shown by the textile industry as coloring materials [22]. The two dyes Congo red and Methylene blue are cationic and anionic in nature, respectively [23]. These dyes are used extensively in textile, paper, rubber and plastic industries if they are discharged without any regulation can cause serious ecological damage. Therefore, the need for developing a simple more effective method for the degradation of dyes has gathered enormous significance. Metal nanoparticles, due to their relatively large surface-to-volume ratios along with their light absorbing properties known to exhibit better catalytic activity in reducing dyes [24].

Mosquito borne illnesses constitutes serious health problem causing various diseases including, Japanese encephalitis, malaria, chikungunya, lymphatic filariasis, fever and dengue fever and which are high prevalent in India. About 2.5 million malaria cases have been reported all around world, however, India being a tropical country alone have >75% of the malaria cases [25]. Larvicides derived from medicinal plants are promising category of natural pesticide, due to their green low level toxicity for non target organisms [26] and plant-derived larvicides contain a combination of various chemical compounds that work synergistically against targeting different biological processes, reducing the likelihood of resistance [26]. An alternative to botanic larvicides is the production of NPs synthesized using medicinal plant extracts as reducing agent [27,28]. Metallic NPs has very effective antimicrobial effects while to human cells it is non- toxic [29,30]. Further, potential of medicinal plants come more to the limelight, in green synthesis of NPs in an attempt is being made to synthesize metallic NPs as it also exemplifies the properties of the plant extract which act as the capping agent. Several reports are available for green synthesis of metal NPs for their antibacterial activity [31,32] antifungal activity [33,34] and larvicidal activity [[35], [36], [37], [38]]. Acorus calamus is a herbaceous perennial native to India and it is widely used as medicine as well as utilised for their perfume. Further, it contains b asarone and eugenol as chief phytoconstituents [39]. Here in this work, microwave irradiation for the preparation of extract is followed as highly localized temperature and pressure includes reducing extraction time with reproducible high purity final products and primarily suitable for separation of active ingredients from natural entities [40,41]. In this work, for the first time we are reporting, an environment-friendly and low-cost method to produce iron and manganese NPs using A. calamus aqueous extract. Further, their synthesis conditions were optimized using RSM. We also report their application antibacterial, antifungal, larvicidal and the photocatalytic activity degradation of methylene blue and congo red without addition of any external ROS generating agents.

Section snippets

Preparation of Extracts

The rhizome of A. calamus was collected as fresh from Western Ghats (Longitude 77.2182 and Latitude 8.29294), Kanyakumari District, Tamilnadu, India. Initially, the surfaces of the rhizomes were washed several times with distilled water. The rhizomes were shade dried for about 4 to 5 days and then finely powdered. An aqueous extracts of A. calamus were prepared as 10 g of powdered rhizome were packed down into the beaker containing 1000 ml of double-distilled water (DDW). The extraction was

Green Synthesis of NPs Using A. calamus Extract

The synthesis of Iron oxide NPs was initially observed by the instantaneous colour change from near colourless to black. The excitation of surface plasmon resonance vibrations is exemplified by the instantaneous colour to black. Similar results were observed in tea extract studied previously [47]. Initially, the colour of aqueous manganese metal ion solution looks transparent. On addition of A. calamus aqueous extract the manganese metal ion solution gradually changes to reddish dark brown in

Conclusions

Iron oxide and manganese oxide NPs were successfully synthesized by polyphenolics enriched microwave irradiated aqueous extract of A. calamus. The synthesized conditions were optimized using RSM. Thus, the present study shows the potential application of RSM in predicting the various parameters and its interactions enabling NP synthesis with unique characteristic features. These observations clearly indicated that it can be provide a path for design of bioprocess to provide large scale

Funding

The authors would like to extend their sincere appreciation to the Deanship of Scientific Research at King Saud University for its funding of this research through the Research Group Project No. RG-1435-071.

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