Green synthesis of Zirconia nanoparticles based on ginger root extract: Optimization of reaction conditions, application in dentistry

 

Thyagarajan R.*, Narendrakumar G., Rameshkumar V., Varshiney M.

Department of Biotechnology, School of Bio and Chemical Engineering,

Sathyabama Institute of Science and Technology, Chennai – 600119.

 

ABSTRACT:

Zirconia nano particles were synthesized from Zirconium oxychloride octahydrate using the extract of Zingiber officinale by Green synthesis. The synthesis was confirmed by the color change from pale yellow to pink. The synthesized nano particles were characterized by UV-visible spectrophotometer, Fourier Transform Infrared Spectroscopy (FT-IR), Scanning Electron Microscopy (SEM), X-ray Diffraction (XRD). The nanoparticles were found to be tetragonal with the XRD results. As an application in Dentistry, the activity of the zirconia nanoparticles were checked using well diffusion method with an oral bacterium, Streptococci mutans, and found the nano particles were inhibiting the growth of the bacterium.

 

 

1. INTRODUCTION

The production of nanometer-sized metals has been the emphasis of much attention in industry and academia due to their significant properties (physical, chemical and biological)^1-4. Recently, the production of nanoparticles using plant materials has boosted the  significance because of simple, cost-effective, environmentally friendly, and dependable approaches^5-9. The recent approach to improve the properties of acrylic resins is the addition of zirconium oxide (zirconia, ZrO2) as filler. Studies have shown that zirconia is biocompatible and additional advantage of zirconia as filler over other metal fillers is superior esthetics¹⁰.  Zirconia is an oxide extensively used in structural (complex polymorphism with cubic, tetragonal, orthorhombic and monoclinic) and functional roles such as heat stabilizers ^11,12 catalyst ^13-16 dental prosthetics ^17-21 and Photocatalytic water decontamination ²². This refractory material exhibits relatively high toughness and oxidation resistance, making it suitable in applications ranging from cutting tools, bone prostheses to thermal barrier coatings.

 

 

Its high ionic conductivity has led to its widespread use as an oxygen sensor in automobile emissions systems and as an electrolyte in solid-oxide fuel-cells ^23-26. The chemical constituents of plant extracts act as reducing agents as well as stabilizing agent for the nano-particle synthesis^27-29. Biomolecules from plant extracts reduces metal ions to nanoparticles in a single step^30-32. The process is quick, easy and can readily be scaled up. The process also has an added advantage of being eco-friendly and to explore importance of medicinal    plants^33-36.

 

In the present study, Zirconium nanoparticles (ZrNp) were firstly synthesized using extracts of Zingiber officinale roots, which is plentifully available in Tamilnadu, India. Characterizations such as FT-IR, SEM and XRD were exercised to analysis the prepared material in terms of dimensions, morphology, arrangement and structure. Furthermore, based on the  Spectrophotometric and FT-IR analysis, a possible production method was proposed. Finally, they were used to evaluate their activity against dental pathogens.

 

2. MATERIALS AND METHODS:

2.1 Materials:

The root of Zingiber officinale was collected from the markets of Chennai, Tamilnadu, India. Botanist in Sathyabama Institute of Science and technology confirmed their biological properties. The analytical grade zirconyl chloride octahydrate (ZrOCl₂·8H₂O) used was purchased from Sigma Aldrich.

 

2.2 Zingiber officinale extract preparation:

The ginger root was washed many times with tap water followed by distilled water. After drying using homogenizer the extract was separated from the biomass.  

 

2.3 Response surface methodology:

The synthesis conditions were determined from a Central composite design with three central points^37-40. The factors and levels varied are shown in Table 1.

 

The general polynomial equation was used

Equation Y= β₀ + β₁ X₁ + β₂X₂ + β₃X₃ + β₁₁X²₁ + β₂₂X²₂ + β₃₃X²₃ + β₁₂X₁X₂ + β₁₃X₁X₃ + β₂₃X₂X₃                   (1)

 

where Y is predicted response; X₁, X₂, X₃ are independent variables; β0 is an offset term; β₁, β₂, β₃ are coefficients of linear effects; β₁₁, β₂₂, β₃₃ are coefficients of squared effects; β₁₂, β₁₃, β₂₃ are coefficients of interaction terms

Table-1 Factors and levels of the design applied to the synthesis of zirconia nanoparticles using Zingiber officinale root extracts.

 

2.4 Green synthesis of zirconia nanoparticles:

According to the Table-2 design of experiment (DoE) from design Expert version 7.0.0 different combination of 0.3M of Zirconium oxychloride [ZrOCl₂.8H₂O] solution (in distilled water) and ginger extract was added with different time interval. The color changed from pale yellow to mild pink indication the reduction reaction and the FT-IR results confirmed the presence of Zirconia.

 

2.5 Zirconia Characterization:

Characterization of the zirconium nanoparticles were done with UV-vis spectrophotometry (Cary Varian 300), Fourier Transform Infrared Spectroscopy, Scanning Electron Microscope, X-ray Diffraction.

 

2.6 Dental sample analysis:

Streptococci mutans strain was purchased from MTCC and sub culture of the organism according to the prescribed instructions.

i)      A lawn of the organism is made and well was cut and the sample was loaded and checked for activity using well diffusion method.

ii)     Zone of inhibition was found and noted.

 

Table-1 Factors and levels of the design applied to the synthesis of zirconia nanoparticles using Zingiber officinale root extracts

 

3. RESULTS:

From the ginger root, the extract was separated and used for the synthesis of zirconia. Using the design of experiment provided. On the basis of DoE, the combination was done and the results were analyzed using UV- Vis spectrophotometry (Figure -1) and further confirmed using FT-IR.

 

Figure -1 UV-VIS spectrometric results for Zirconia nanoparticles

 

Table 2 Design of Experiments with response (Actual and Predicted)

 

 

Figure 2. Contour plot showing different interaction between the factors

 

Optimization of process parameters on zirconia production using RSM:

The production of zirconia was optimized various parameter such as Factor 1 A: Concentration, Factor 2 B:Extract,  Factor 3 C:Time using response surface methodology (RSM) using Central composite design (CCD). The model used was quadratic and 20 runs trial was performed. The productivity was calculated for the design of experiment that was given by Design expert software (Table 2). The response was estimated by FT-IR was displayed as contour plot and surface plot.

 

R1= 7.629 + 0.0785A -0.112 B -0.1518 C-0.25AB -0.025AC+0.225+BC-0.549A²-0.4784 B² - 0.655 C²        (1)

 

The effect of concentration of the substrate (A) with respect to Extract concentration  (B) express that as the production of zirconia significantly (Figure 4a), the extract concentration plays an significant role in the zirconia production with respect to concentration of substrate (Figure 4b),

 

The R² value was 98.99% compared to Adjusted R² of 97.83% with respect to the predicted R² of  95.88% confirms the fitness of the test (Table 3).

 

Figure 3. FTIR of the ginger extract which was lyophilized over night. X-axis is the wavenumber and Y-axis is the % transmittance. Bands observed at 3313.71 cm^-1 and 1670 cm^-1 are assigned to the bending and stretching vibrations of the O-H bond due to absorbed water molecules. The band at 1336.67 cm^-1 is attributed to the absorption of non-bridging OH groups. The sharp band at 750.31 cm^-1 is the characteristic band/ peak of ZrO₂. ^25,32

 

 

 

 

 

Table 3. ANOVA Table

 

 

Figure 3. FT IR results

 

Figure 4 . Under 20000 X of magnification the size of the nano particles were measured

 

 

Figure 5. XRD results

 

The ultrafine particles (nano particles) were found to be in cubic phase ranging from 140nm to 585nm in size²⁷. Heinz et al., 2017³⁶ stated that the nanoparticles synthesized was 200nm range in size with spherical and irregular morphology because other phenomena like transparency, turbidity, stable dispersion etc., extends the upper limit are occasionally considered, the use of the prefix nano is accepted for dimensions smaller than 500nm, provided reference to the definition is indicated.)

Figure 5. (101) is the peak for zirconium nano particles obtained at 45º which this the particle size can be calculated Using Scherrer equation D=0.9λβcosθ (1) where θ is the angle, D is the size if the particle, β is the wave breadth, λ is the wavelength^{18, 24}. The peaks are overlapping because the sample is a tetragonal doublet.

 

Figure 6: Activity of  Zirconia  nanoparticles  against S. mutans (oral bacteria)

 

Figure  6 shows The zone of clearance appeared 24 hours after performing well diffusion method. The diameter of the well is 0.7cm and the diameter of the zone of clearance is 22mm. Area of the zone 10.318cm²

 

4. CONCLUSION:

The method proposed for the synthesis of zirconia nanoparticles using Zingiber officinale root extract was effective, and materials with monoclinic phases were obtained that was confirmed using XRD. The Central composite design showed significant composition of concentration of zirconium oxide, quantity of ginger root extract and time duration required for the formation of nanoparticle. The results were confirmed using FT-IR. The nanoparticles presented a crystallite size ranging from 295 to 583 nm using Scanning electron microscopy. After confirming the presence of the nano particles, it was subjected to Streptococci mutans to check the activity. The nano particles have acted on the S.mutans and they have lysed or inhibited the organism. This was performed with well diffusion method. Hence, zirconia nano particles can be used in dentistry to make temporary hollis.

 

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Accepted on 21.10.2021           © RJPT All right reserved

Research J. Pharm. and Tech 2022; 15(11):5314-5320.