Green synthesis of Fe-ZnO nanoparticles with improved sunlight photocatalytic performance for polyethylene film deterioration and bacterial inactivation

doi:10.1016/j.mssp.2020.105574

Materials Science in Semiconductor Processing

Volume 123, 1 March 2021, 105574

https://doi.org/10.1016/j.mssp.2020.105574 Get rights and content

Highlights

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Green synthesized Fe-ZnO nanoparticles using hibiscus rosa-sinensis leaf extracts.
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Fe dopant boosted light harvesting capability and possessed smaller particle size.
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High weight loss of LDPE/Fe-ZnO film was found under sunlight irradiation.
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LDPE/Fe-ZnO film also revealed antibacterial activity towards E. coli.
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Carbonyl peak detection and texture change signified polymer matrix degradation.

Abstract

Massive utilization and improper handling of plastics urge us to seek an applicable and efficient treatment method to reduce the plastic wastes. Herein, iron-doped ZnO (Fe-ZnO) nanoparticle was synthesized via a hibiscus rosa-sinensis leaf-assisted green method, and subsequently employed for low density polyethylene (LDPE) plastic degradation as well as Escherichia coli (E. coli) inactivation under sunlight irradiation. Myriad characterization techniques were used to investigate the structural, optical and electronic properties of green synthesized samples. The weight loss results presented that the photocatalytic performance of the LDPE/Fe-ZnO film was higher than those of pure LDPE and LDPE/un-doped ZnO films. The Fe-ZnO (2 wt%) nanoparticle demonstrated a greater photocatalytic deterioration of LDPE owing to its boosted optical absorption and the effective suppression of photogenerated charge carriers. The presence of carbonyl groups as the degradation product of LDPE was confirmed by Fourier transform infrared (FTIR) analysis. Field-emission scanning electron microscopy (FESEM) images also witnessed the formation of pores at the interface between polymer matrix and Fe-ZnO. Additionally, the LDPE/Fe-ZnO film exhibited an obvious antibacterial effect against E. coli as compared to LDPE/un-doped ZnO film. The current work put forward the construction of eco-friendly photocatalyst as a green strategy to tackle the challenges of plastic pollution.

Introduction

Plastics are synthetic organic polymers which considered as ideal materials because of their remarkable traits, such as light weight, transparent, ease of availability, durability and relatively low cost. Owing to their widespread commercial and industrial applications [1,2], many plastic materials discharged into the surface water bodies, including stream, river, sea as well as ocean. These plastics can accumulate and persist in the aquatic environment for years due to their high resistant against weathering and ageing degradation. Recent reports have shown that there might be over 5.3 trillion plastic debris, which are presently floating on the sea [3,4]. These plastics included polystyrene, polyethylene, polyurethane, terephthalate, polyvinyl chloride which massively utilized in our daily life and industries [5,6]. In particular, the polyethylene plastic fragments have garnered tremendous attention due to their abrasion damages that possessed to marine life and public health hazards [7].

Advanced oxidation processes (AOPs) are promising techniques for the decomposition of refractory and persistent pollutants including plastics. Heterogeneous photocatalysis is an effective environmental-friendly process among AOPs because of its potential exploitation of sunlight irradiation. ZnO nanoparticles owing of their exceptional characteristics strongly suit for this technique. These nanoparticles have been utilized in a broad spectrum of applications, including electronics, piezoelectric, spintronics, catalysis and solar cells [[8], [9], [10], [11]]. The efficiency and functionality of ZnO can be further boosted by modifying and improving its surface area through incorporation of several dopants, such as biomolecules and transition metal ions (Fe, Cu, Ni, Co) [[12], [13], [14]]. Among the transition metals, iron (Fe) is preferred as dopant because of its d-orbital electron easily overlapped with the ZnO valence band [13]. When Fe was doped on ZnO nanoparticles, an enhancement of optical and magnetic properties for environmental applications have been observed [14]. Doping of ZnO nanoparticles with Fe can also decrease the particle size and increase the amount of catalytically active sites, which was highly conducive for adsorption processes in photocatalytic reaction [15]. Therefore, the synthesis of Fe-doped ZnO nanoparticles with fascinating electronic and optical traits has turned up to be a major topic among the researchers.

To date, a broad spectrum of synthesis methods has been explored for the unmodified ZnO and transition metal ion-doped ZnO nanoparticles [[16], [17], [18]]. These approaches included the utilization of high cost, abundant surfactants, and toxic chemical reagents that impacted deplorably on the environment. Recently, green techniques for the fabrication of metal oxide nanomaterials have garnered tremendous attention with the assistance of plant extracts. It was noteworthy that plant extracts comprised of numerous biomolecule compounds, such as polyphenols, flavonoids, carbonyl and proteins compounds [19,20]. These biomolecule compounds could serve as green capping agents and templates, and accordingly could play as pivotal roles in the fabrication process.

Not surprisingly, there has been a great interest in incorporating the green synthesized supported metal oxide material into the polymer matrix (including polyethylene) to improve its atmospheric degradation [21,22]. Moreover, combining photocatalyst and polymer film would be concurrently destroyed the pathogenic microorganisms present in the environment. Such polymer film can be broadly used for automotive accessories, military vehicles, medicals and textiles [23]. Thus, addition of antimicrobial agents in the form of polymer composite matrix can be an appealing strategy. Vast antibacterial polymer films have been revealed via the silver and copper materials [24,25]. Nonetheless, to the best of our knowledge, there has been no report on the incorporation of eco-friendly synthesized Fe-ZnO into the polymer film for dual applications in deteriorating the polymer matrix and inactivating the bacterial cell.

Inspired by the aforementioned consideration, we report a hibiscus rosa-sinensis leaf-assisted green method for the synthesis of Fe-doped ZnO (Fe-ZnO) nanoparticles. The prepared Fe-ZnO nanoparticles were integrated into the low density polyethylene (LDPE) as composite films and subsequently tested them under the sunlight irradiation. Additionally, antibacterial property of the developed LDPE samples was assessed against the Escherichia Coli (E. coli). The deterioration of polymer film was investigated via the weight loss, Fourier Transform Infrared (FTIR), field-emission scanning electron microscopy (FESEM) and thermogravimetric (TGA) tests. Finally, the mechanism involved in the photocatalytic deterioration of LDPE over the Fe-ZnO nanoparticles was also postulated.

Section snippets

Chemicals

Zinc acetate dihydrate (Zn(CH₃CO₂)₂·2H₂O) was obtained from Chem Soln. Iron (III) chloride (FeCl₃) and cyclohexane were acquired from R & M chemicals. Low density polyethylene (LDPE) particles with radius of about 2 mm were supplied by Sinopec Group. All the chemicals utilized in the present study were of analytical grade and without further treatment.

Preparation of hibiscus rosa-sinensis plant extract

Fresh leaves of hibiscus rosa-sinensis were collected around our university. The collected leaves were cleaned with water to wash away the dusts

Material characteristics

The functional group characteristics of undoped ZnO and Fe-ZnO samples prepared at different Fe loadings are shown in Fig. 2. The FTIR spectra showed that the ZnO absorption peak with Zn-O stretching mode was found at 490 cm⁻¹, which can be corresponded to hexagonal ZnO wurtzite structure (Fig. 2a). Apart from the distinct peak of Zn-O, weak absorption peaks observed at 601 cm⁻¹ can be denoted to the characteristic of Fe-O stretching mode [28]. The broad absorption band observed at 3436 cm⁻¹

Conclusion

In summary, Fe-ZnO nanoparticles were fabricated according to a simple and green method utilizing hibiscus rosa-sinensis leaf extract, and their sunlight photocatalytic deterioration of LDPE plastic and antibacterial activities were investigated for the first time. Microscopic analysis displayed that the Fe-ZnO had smaller particle sizes as compared to that of undoped ZnO. The UV–vis DRS exhibited a reduction of band gap value after the Fe doping, while excellent electronic property in Fe-ZnO

Author contribution statement

Assoc. Prof. Dr. Sze Mun Lam: Conceptualization, Formal analysis, Investigation & Writing - draft & editing. Assoc. Prof. Dr. Jin Chung Sin: Conceptualization, Funding acquisition. Prof. Dr. Honghu Zeng: Funding acquisition. Prof. Dr. Abdul Rahman Mohamed, Assoc. Prof. Dr. Lin Hua & Assoc. Prof. Dr. Haixiang Li: Resources & Software. Miss Yen Yi Chai & Mr. Choong Man Kit: Methodology.

Declaration of competing interest

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Acknowledgments

The research was supported by Ministry of Higher Education (MoHE) through Fundamental Research Grant Scheme (FRGS/1/2019/TK02/UTAR/02/4), Universiti Tunku Abdul Rahman (UTARRF/2020-C1/S04), Research funds of The Guangxi Key Laboratory of Theory and Technology for Environmental Pollution Control, China (1801K012 and 1801K013), and special funding for Guangxi “Bagui Scholar” construction project.

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Green synthesis of Fe-ZnO nanoparticles with improved sunlight photocatalytic performance for polyethylene film deterioration and bacterial inactivation

Highlights

Abstract

Introduction

Section snippets

Chemicals

Preparation of hibiscus rosa-sinensis plant extract

Material characteristics

Conclusion

Author contribution statement

Declaration of competing interest

Acknowledgments

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