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Article

Biogenic Synthesis of Silver-Iron Oxide Nanoparticles Using Kulekhara Leaves Extract for Removing Crystal Violet and Malachite Green Dyes from Water

by
Haradhan Kolya
* and
Chun-Won Kang
*
Department of Housing Environmental Design, Research Institute of Human Ecology, College of Human Ecology, Jeonbuk National University, Jeonju 54896, Republic of Korea
*
Authors to whom correspondence should be addressed.
Sustainability 2022, 14(23), 15800; https://doi.org/10.3390/su142315800
Submission received: 6 October 2022 / Revised: 22 November 2022 / Accepted: 24 November 2022 / Published: 28 November 2022
(This article belongs to the Special Issue Wastewater Treatment and Purification)
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Abstract

:
Crystal violet and malachite green, cationic dyes, are widely used in various industries. Water-containing dye molecules affect human health and aquatic life. Here, we synthesized silver-iron oxide nanoparticles using an aqueous extract of kulekhara leaves. The main advantage of this synthesis is that no iron salts were used to prepare Ag-iron oxide nanoparticles. Iron-rich Kulekhara leaves provide iron oxide during the in situ formation of silver nanoparticles. Synthesized Ag-Fe2O3 nanoparticles were characterized by UV-Vis, FTIR, XRD, and STEM-Cs. The dye-degradation studies were performed using synthesized nanoparticles in the presence of sodium borohydride. In the catalytic reaction, the color of crystal violet and malachite green disappeared (100%) within three minutes, and the same results were obtained in their mixtures (1:1 v/v). The presence of Fe2O3 in AgNPs may boost the rapid reduction in azo bonds due to the higher exposed surface area. The color changes were monitored using UV-Vis spectroscopy. Comparative literature studies showed that the performance of Ag-Fe2O3 is superior regarding the degradation of malachite green and crystal violet. These findings could entice researchers to design and develop various dye degradation using this eco-friendly process.

Graphical Abstract

1. Introduction

A constant supply of pure water is required in the home and industrial sectors. Waterways, lakes, and subsurface resources provide most water for domestic and industrial use. Freshwater resources are decreasing and becoming more and more contaminated as the global population and industrialization increase. Industries frequently use clean, sweet water while polluting rivers and seas. Crystal violet (CV) and malachite green (MG) dyes are commonly used in the textile, leather, wood, and paper industries [1,2]. Some dyes are loosely bound with textiles but may seep out of clothes when washed [3]. Therefore, textile industries produce coloring effluents and discharge them into rivers or seawater without proper treatment.
On the other hand, the aqueous dye solutions used to stain microorganisms are often discharged directly into the drain water [4,5]. Dye molecules in water cause several toxicities in marine life and human health [6]. Dyes, in this case, crystal violet and malachite green, which are hydrosoluble, would hinder the penetration of sunlight into the deep, reduce the solubility of oxygen in water, and thus hamper the ecosystem in water bodies [7]. However, most synthetic dyes create various public health diseases such as headaches, hypertension, red blood cell breakdown, skin allergy, central nervous system disorder, and cancer [8]. Therefore, research into removing dyes from water is crucial for ecological sustainability.
Several wastewater treatment technologies are available for removing dyes and other pollutants from wastewater, such as adsorption [9,10,11], membrane filtration [12], flocculation [13], advanced oxidation, bacterial degradation [14], and catalytic degradation [15,16]. The inexpensive process cost and less sludge generation/regeneration adsorption [17,18] and catalytic degradation methods [19] entice researchers in these studies. At present, biopolymer-based adsorbents are an attractive research area for wastewater treatment [20]. In addition, nanoparticles and magnetic-nanoparticles or magnetic polymer nanocomposites materials [21,22,23] are attracting attention among researchers in catalytic degradation [24,25] and adsorption processes [26] due to their easy regeneration, reusability, low cost, and less sludge [27,28,29,30].
Catalytic reduction in sodium borohydride has received particular attention for degrading dye molecules [31,32]. Sodium borohydride plays an essential catalytic role as a co-catalyst that can provide electrons and hydrogen in the catalytic dye degradation [33]. Furthermore, variations in color intensity might be easily monitored using UV-Vis spectroscopy. The azo bonds in azo dye molecules could be readily cleaved by hydrogenation, resulting in the dye molecules changing into less hazardous and environmentally friendly products. Researchers used various catalytic systems for azo bond cleavage, especially metal/metal oxide nanoparticles [34,35].
On the other hand, many surfactants and reactants are utilized to form and stabilize metal nanoparticles [36]. These chemicals are hazardous to the environment and humans. Therefore, environmentally friendly processes should produce and use metal nanoparticles. Researchers have recently used various fruit extracts [37], leaf extracts [38], and flower extracts [39] to prepare silver nanoparticles. Silver nanoparticles have unacceptable toxic effects on human health and the environment, in addition to their antimicrobial activity [40].
In this study, we synthesized silver-iron oxide nanoparticles using kulekhara leaves (Hygrophila auriculata) extract. This is an eco-friendly, facile, and low-cost approach. Kulekhara leaves are used as traditional medicinal plants in India [41,42]. Kulekhara leaves contain iron (Fe+2) and vitamin C are higher than common greens such as spinach, lettuce, and coriander. The leaves also contain many phytochemicals: flavonoids, glycosides, phenolic components, tannins, etc. [43]. These phytochemicals usually act as reducing and stabilizing agents to form metal nanoparticles [44]. In addition, Fe+2 has an essential role in forming naturally occurring silver nanoparticles [45]. As a result, dissolved Fe+2, and Ag+ transformed into Fe+3 and Ag0, respectively. The presence of phenolic-rich components in the leaf extract results in forming Fe2O3 simultaneously [46]. Synthesized materials were characterized by UV-Vis spectroscopy, FTIR spectroscopy, XRD, and STEM-Cs; the findings are discussed below.

2. Materials and Methods

2.1. Materials

Silver nitrate and borohydride were purchased from Sigma Aldrich, Korea. MG and CV dyes were procured from Daejung Chemicals & Metals Co. Ltd., Siheung, Republic of Korea. Distilled water was used for the entire synthesis process, and tap water (pH 6.9, turbidity 0.1 NTU) was used to prepare a stock solution of 100 mg/L, MG, and CV dyes. Kulekhara leaves were obtained from Indian marketplaces.

2.2. Preparation of Nanoparticles

Green kulekhara leaves were collected from Rajabazar market, Midnapore, West Bengal, India. Green leaves were dried under sunlight, and drying leaves were pulverized using a mixer grinder. The dust of leaves (500 mg) was poured into water (100 mL) and then boiled for about 10 min. After filtering the residue, the filtrate was collected in a stoppered conical flask and used to synthesize nanoparticles. About 50 mL (10−3 M) of silver nitrate aqueous solution was taken in a beaker, and then 2 mL of kulekhara leaves extract was mixed with the solution at room temperature (24 °C). The solution color changed from colorless to yellowish within 5 min, and then the yellowish color transformed to a deep radish yellow within 10 min. This solution was subjected to characterization using instrumental characterization techniques. A schematic of the synthesis process is shown in Figure 1.

2.3. Characterization

UV-Vis spectrophotometer (UV−1650PC, Shimadzu, Kyoto, Japan) was utilized to measure the optical characteristics of the colored solution. The absorbance spectra were collected in a 1 cm cuvette at an 800–200 nm wavelength. FTIR spectra (Thermo Scientific Nicolet iS20, Waltham, MA, USA) in the wavelength range 4000–400 cm−1 were used to investigate the change in chemical functionality and nanoparticle formation using KBr pellets. The colloidal solution was centrifuged, and the residue was dried on glass plates in a vacuum oven at 80 °C. The dried materials were structurally examined using an X-ray diffractometer (Miniflex, Rigaku, Japan), Cu Kα radiation at a scan rate of 1° min−1 in the 10–80° range. The drop-casting technique was used to obtain sufficient material for TEM analysis on a lacey F/C 300 mesh Cu grid. High-resolution transmittance electron spectroscopy (STEM-Cs, JEOL/JEM-ARM200F) at 200 kV was used for morphological investigation and EDS analysis.

2.4. Removal of Malachite Green and Crystal Violet

In a 100 mL conical flask, 35 mL of MG (100 mg/L) and CV (100 mg/L) dyes were taken separately. The dye solution was then mixed with 1 mL of NaBH4 (0.5 mg/mL) by handshaking. After that, 0.5 mL of nanoparticle solution was added to the mixture. The azo bonds of the MG and CV dyes were rapidly destroyed, and the solution became colorless.
On the other hand, 3 mL of MG or CV dyes were taken in UV-cuvette, and then 20 μL of prepared NaBH4 solution was added. After that, 20 μL of nanoparticle solution was added and mixed quickly. Afterward, UV-Vis measurements were performed at an interval of 1 min in the 800–200 nm range (scan speed: fast, sampling interval: 0.5 nm). A mixture of these two dye solutions was prepared by mixing two equal volumes of each dye (1:1 v/v). The procedure, as mentioned earlier, was used to investigate the degradation of dyes in the mixture.

3. Results and Discussions

3.1. Synthesis and Characterization of Ag-Fe2O3 Nanoparticles

The nanoparticle solution had a specific color change compared to the extract solution, as illustrated in Figure 1. Figure 2a shows the UV-Vis spectra of nanoparticles, kulekhara extract, and silver nitrate solution.
The absorbance peak at 429 nm suggests the presence of silver nanoparticles. The formation of silver nanoparticles by Fe+2 was found to have significant absorbance between 350 nm and 700 nm, indicating a polydispersed distribution of AgNPs/Fe2O3 [45]. The peak at 290 nm suggests the presence of natural phenolic compounds (phytochemicals) in the kulekhara leaf extract [47,48].
The FTIR spectrum of the eco-friendly synthesized Ag/Fe2O3 nanoparticles is shown in Figure 2b. The O―H bond stretching in phenolic compounds appeared at 3436 cm−1. The peak at 2921 cm−1 and 1631 cm−1 corresponds to the ―CH stretching of the methylene group and C=C stretching, respectively. The high peak at 1385 cm−1 confirms the presence of silver nanoparticles [15]. The peak in the C―O stretching, O―H vibration, or C―O―C bond vibration is 1016 cm−1 [47]. Moreover, the Fe―O stretching band’s vibration coincides at 580 cm−1 and 619 cm−1 (Figure 2c) [25,49].
The crystalline nature of the synthesized nanoparticle using the XRD spectrum is shown in Figure 3.
The presence of amorphous peaks in the spectrum implies the green synthesis of nanoparticles. The peak at 10°–20° refers to organic components from the reaction medium responsible for stabilizing the formed nanoparticles [25]. The peaks at 38°, 43.4°, 65.5°, and 77.1° are formed by the lattice planes of face-centered cubic silver crystals (111), (200), (220), and (311), respectively. The obtained data were matched with the JCPDS database:04–0783 [50]. On the other hand, peaks at 24.5°, 33.6°, 41.0°, 51.5°, and 62.6° corresponds to the X-ray diffraction pattern of Fe2O3 and indicate lattice plane (012), (104), (113), (024) and (214) respectively [51]. Therefore, the XRD spectrum indicates the formation of Ag/Fe2O3 nanoparticles.
The morphology of the Ag/Fe2O3 nanoparticles was also investigated by STEM-Cs analysis. TEM images of nanoparticles are shown in Figure 4a,b at different magnifications. TEM analyses (Figure 4a,b) reveal that relatively spherical nanoparticles are formed with an average diameter of 10.42 ± 0.81 nm. The size distribution histogram is shown in Figure 4c. The HR-TEM image of AgNPs/Fe2O3 nanoparticles (Figure 4d) demonstrates the lattice fringes. The nearly smooth edges are also quite distinct from this image. Energy dispersive X-ray analysis (EDS) elemental mapping was used to identify the elements present in the prepared nanoparticles. The EDS mapping and layer image of elements O, Fe, and Ag are shown in Figure 4e–h. The EDS mapping demonstrates that oxygen and iron are associated with the particles on silver nanoparticles (Figure 4h). The overall analysis of TEM images indicates the formation of Ag-iron oxide nanoparticles by kulekhara leaves extract.

3.2. Catalytic Activity of Ag-Iron Oxide Nanoparticles

The UV-Vis spectrophotometer was used to determine the catalytic activity of the synthesized nanoparticles for the hydrogenation reaction of azo bonds in crystal violet, malachite green, and their mixtures. The results are shown in Figure 5. Color changes and the UV-Vis spectra before and after the catalytic reaction are shown in Figure 5a. The maximum absorbance (λmax) of crystal violet appeared at 588 nm. After adding nanoparticles, its intensity slightly increases due to the interaction between dye molecules and nanoparticles. A new peak appeared at 420 nm as a result of the presence of Ag and Fe2O3 nanoparticles. After adding sodium borohydride, the peak intensity at 588 nm decreases very quickly, and the absorbance becomes almost zero within 3 minutes. A new peak appeared at 286 nm, which is due to the reduction in crystal violet and the formation of leucocrystal violet [52]. The degraded crystal violet, leucocrystal violet, did not show any toxicity in water, as confirmed by the studies of Sengan et al. [31] using the Zebrafish model.
On the other hand, the maximum absorbance peak in malachite green dye was observed at 619 nm, as shown in Figure 5b. The intensity of the peak pattern decreases, and the absorbance becomes zero after three minutes of adding nanoparticles and sodium borohydride solution. The peak appeared at 288 nm, suggesting the formation of leucomalachite green [53]. Similarly, the reduction in their (CV + MG; 1:1 v/v) mixture by nanoparticles in the presence of sodium borohydride exhibited complete reduction within 3 minutes (Figure 5c). However, a slow reduction reaction of azo bonds was observed using only sodium borohydride.
Additionally, there was no difference in absorption in the absence of sodium borohydride. Moreover, the reduction in azo bonds took place more quickly in the presence of Ag-Fe2O3 nanoparticles and NaBH4. This is due to the greater availability of exposed surface area of nanoparticles. The catalyst accepts electrons from BH4- ions and transfers them to electrophilic dyes, thereby initiating catalytic reduction. The donor is BH4- and the acceptor is the dye molecule. The dye molecules’ electrons are then transferred to the catalyst [54]. A probable mechanism is shown in Figure 6.

3.3. Discussion

A simple and environmentally friendly method was used to prepare silver–iron oxide nanoparticles. This study used kuleakhara leaf extract as a reducing agent and iron supplier in the reaction medium. As kulekhara leaves contain enough ferrous compounds, iron salts from outside are not used. On the other hand, phytochemicals and iron(II) in leaf extracts can reduce the silver ion [41,42]. The presence of phenolic-rich components and iron(II) in the leaf extract resulted in the formation of Fe2O3, as iron(II) was oxidized to iron(III), and silver(I) was reduced to silver(0) [46]. The UV-Vis, FTIR, XRD, and TEM characterization techniques confirmed the formation of these nanoparticle. The nanoparticles were used as a catalyst to reduce the azo bond in the dye molecules in the presence of sodium borohydride. We investigated the catalytic performance of Ag/Fe2O3 nanoparticles using two cationic dyes (malachite green and crystal violet) separately and in combination. Nanoparticles with NaBH4 cleaved azo bonds quickly, and discoloration was complete in three minutes. The formation of leucocrystal violet and leucomalachite green is recognized by the discoloration of the solutions [52,53]. However, there was no dye discoloration using nanoparticles without NaBH4. The reaction rate of sodium borohydride to reduce the azo bond of dye molecules is slow.
Furthermore, the reduction in azo bonds was accelerated in the presence of Ag-Fe2O3 nanoparticles. This is due to the increased availability of nanoparticle exposed surface area. The elemental composition of the treated dye mixture (supernatant liquid) was evaluated by EDS. The percent composition was as follows: C (89.01%), N (5.92%), O (4.92%), Fe (0.05%), and Ag (0.09%). It is difficult to separate the catalyst from the reaction medium and thus to test its reusability due to the low concentration of Ag and Fe in the treated solution. Further research is needed to study the magnetic properties of Ag-iron oxide nanoparticles.

3.4. Efficiency Comparison

The catalytic efficiency of Ag-iron oxide nanoparticles for the degradation of dyes’ molecules was compared to other metal nanoparticles and other dyes, as shown in Table 1. Methylene blue is the most reported dye in literature. The reduction in methylene blue with silver nanoparticles and NaBH4 is faster compared to catalytic reduction with silver nanoparticles only. Bentonite-AgNPs could remove 84.6% of malachite green in 5 min. However, Ag-Fe2O3 nanoparticles removed 100% of malachite green and crystal violet in 3 min. It is evident that the green synthesized Ag-iron oxide nanoparticles exhibited better efficiency than some other green synthesized silver nanoparticles using different leaf extracts.

4. Conclusions

Here, silver-iron oxide nanoparticles were synthesized using kulekhara leaves extract. The synthesis approach is simple, facile, low-cost, and eco-friendly. The synthesized nanoparticles were characterized by UV-Vis, FTIR, XRD, and STEM-Cs analysis. The findings proved the formation of Ag-Fe2O3 nanoparticles (10.42 ± 0.81 nm). The green nanoparticles were used to degrade azo bonds in crystal violet, malachite green, and their mixture in the presence of sodium borohydride. Results exhibited the rapid degradation of dye molecules (~100%) within three minutes. These findings could entice the researcher to design and develop the catalytic degradation of azo bonds of various dye molecules in wastewater.

Author Contributions

H.K.: Conceptualization, Formal analysis, Investigation, Writing: original draft, Writing: review and editing. C.-W.K.: Project administration, Funding acquisition, Writing: review and editing. All authors have read and agreed to the published version of the manuscript.

Funding

Basic Science Research Program supported this research through the National Research Foundation of Korea, funded by the Ministry of Education (NRF-2019R1I1A3A02059471) and was supported under the framework of an international cooperation program managed by the National Research Foundation of Korea (NRF-2020K2A9A2A08000181).

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

Not applicable.

Conflicts of Interest

The authors declare that they have no known competing financial interest or personal relationships that could have appeared to influence the work reported in this paper. Moreover, no animal studies or human participants are involved in this study.

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Figure 1. Schematic of silver-iron oxide nanoparticle synthesis.
Figure 1. Schematic of silver-iron oxide nanoparticle synthesis.
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Figure 2. (a) UV-Vis spectra of silver/Fe2O3 nanoparticles, kulekhara extract, and silver nitrate solution, (b) FTIR spectra of Ag/Fe2O3 nanoparticles, and (c) zoom view of FTIR spectra of Ag/Fe2O3 nanoparticles.
Figure 2. (a) UV-Vis spectra of silver/Fe2O3 nanoparticles, kulekhara extract, and silver nitrate solution, (b) FTIR spectra of Ag/Fe2O3 nanoparticles, and (c) zoom view of FTIR spectra of Ag/Fe2O3 nanoparticles.
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Figure 3. XRD diffraction pattern of Ag/Fe2O3 nanoparticles by kulekhara leaves extract.
Figure 3. XRD diffraction pattern of Ag/Fe2O3 nanoparticles by kulekhara leaves extract.
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Figure 4. STEM-Cs images at different magnifications (a) 100 nm, (b) 50 nm, (c) histogram of size distribution using ImageJ and originPro 8.5 software, (d) HR-TEM single crystal at 5 nm, (e) mapping of O, (f) mapping of Ag, (g) mapping of Fe, and (h) EDS layer image of elements.
Figure 4. STEM-Cs images at different magnifications (a) 100 nm, (b) 50 nm, (c) histogram of size distribution using ImageJ and originPro 8.5 software, (d) HR-TEM single crystal at 5 nm, (e) mapping of O, (f) mapping of Ag, (g) mapping of Fe, and (h) EDS layer image of elements.
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Figure 5. Dye degradation studies (a) crystal violet, (b) malachite green, and (c) mixtures of crystal violet and malachite green.
Figure 5. Dye degradation studies (a) crystal violet, (b) malachite green, and (c) mixtures of crystal violet and malachite green.
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Figure 6. Reaction mechanism of azo bonds reduction using nanoparticles and sodium NaBH4, (a) crystal violet and (b) malachite green.
Figure 6. Reaction mechanism of azo bonds reduction using nanoparticles and sodium NaBH4, (a) crystal violet and (b) malachite green.
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Table
Table 1. Comparison of dye degradation time using silver nanoparticles.
Table 1. Comparison of dye degradation time using silver nanoparticles.
Sl No.NanoparticlesDyesReaction
Conditions		Removal
(%)		TimeRef.
1.MMT/iron oxide/AgRhodamine BCatalyst: 0.448 mg/mL; NaBH4: 27 mM; Dye: 0.08 mM.46.08 min[30]
2.Ag NPsMethylene blueCatalyst: 0.1 mg/mL; Dye: 10 mg/L.84.064 h[55]
3.Ag NPsSafraninCatalyst: 0.12 mg/mL; Dye: 10 mg/L.84.672 h[56]
4.Au-AgNPsMalachite greenCatalyst: 0.1 mg/mL; Dye: 40 mg/L.90.048 h[57]
5.Bentonite-Ag0Malachite greenCatalyst: 0.12 mg/mL; Dye: 5 × 10−5 M.86.45 min[58]
6.AgNPscrystal violetCatalyst: 10 mg/mL; Dye: NA. 90.024 h[59]
7.AgNPsMethylene blueCatalyst: 0.3 mg/mL; Dye: 3.1 × 10−5 M. NaBH4: 3.0 × 10−5 M.1001 min[60]
8.Au-Ag NPsCongo redCatalyst: 20 μL; Dye: 10−4 M. NaBH4: 20 μL.1006 min[32]
9.Ag NPsMethylene blueCatalyst: 2 mL; Dye: 10−3 M. NaBH4: 0.1 M10013 min[61]
10.Fe3O4 @PDA-AgMethylene blueCatalyst: 3 mg; Dye: 20 mg/L. NaBH4: 0.1 M92.67 min[62]
11.AS-AgNPsMethylene blueCatalyst: 0.05 mL; Dye: 100 μM. NaBH4: 100 mM97.027 min[63]
12.AgNPsMethylene blueCatalyst: 0.05 mL; Dye: 50 μM. NaBH4: 0.005 M99.020 min[64]
13.Ag-iron oxide NPsCrystal violet
Malachite green
Mixture (1:1 v/v) 		Catalyst: 0.5 mL; Dye: 100 mg/L. NaBH4: 0.5 mg/mL1003 minThis work
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Kolya, H.; Kang, C.-W. Biogenic Synthesis of Silver-Iron Oxide Nanoparticles Using Kulekhara Leaves Extract for Removing Crystal Violet and Malachite Green Dyes from Water. Sustainability 2022, 14, 15800. https://doi.org/10.3390/su142315800

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Kolya H, Kang C-W. Biogenic Synthesis of Silver-Iron Oxide Nanoparticles Using Kulekhara Leaves Extract for Removing Crystal Violet and Malachite Green Dyes from Water. Sustainability. 2022; 14(23):15800. https://doi.org/10.3390/su142315800

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Kolya, Haradhan, and Chun-Won Kang. 2022. "Biogenic Synthesis of Silver-Iron Oxide Nanoparticles Using Kulekhara Leaves Extract for Removing Crystal Violet and Malachite Green Dyes from Water" Sustainability 14, no. 23: 15800. https://doi.org/10.3390/su142315800

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