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Preparation and Properties of Cellulose Nanocomposite Fabrics with in situ Generated Silver Nanoparticles by Bioreduction Method

  • The aim of the present study was to develop antibacterial cellulose (cotton) nanocomposite fabrics (CNCFs) with in situ generated silver nanoparticles using medicinal plant Vitex leaf extract. The developed CNCFs were characterized by scanning electron microscope (SEM), Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD) and antibacterial tests. Further, these CNCFs possessed good antibacterial activities. These CNCFs prepared using simple and environmentally friendly method can be considered for medical applications in, such as, surgical aprons, wound cleaning, wound dressing, and hospital bed materials.
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    Cady, N. C. , Behnke, J. L. , Strickland, A. D. , 2011. Copper-based nanostructured coatings on natural cellulose: nanocomposites exhibiting rapid and efficient inhibition of a multi-drug resistant wound pathogen. A. baumannii, and mammalian cell biocompatibility in vitro. Adv. Funct. Mater. 21, 2506-2514
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    Heera, P. , Shanmugam, S. , Ramachandran, J. , 2015. Green synthesis of copper nanoparticles. Int. J. Curr. Res. and Acad. Rev. 3, 268-275.
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    Ibrahim, H. M. M. , 2015. Green synthesis and characterization of silver nanoparticles using banana peel extract and their antimicrobial activity against representative microorganisms. J. Radiat. Res. Appl. Sci. 8, 265-275. doi: 10.1016/j.jrras.2015.01.007
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    Jamshidi, A. , Jahangiri, M. , 2014. Synthesis of copper nanoparticles and its antibacterial activity against Escherichia coli. Asian J. Biol. Sci. 7, 183-186. doi: 10.3923/ajbs.2014.183.186
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    Kathireswari, P. , Gomathi, S. , Saminathan, K. , 2014. Green synthesis of silver nanoparticles using Vitex negundo and its antimicrobial activity against human pathogens. Int. J. Curr. Microbiol. App. Sci. 3, 614-621.
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    Kulkarni. V. D. , Kulkarni, P. S. , 2013. Green synthesis of copper nanoparticles using Ocimum sanctum leaf extract. Inter. J. Chem. Stud. 1, 1-4.
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    Kumar Trivedi, M. , 2015. The potential impact of biofield energy treatment on the physical and thermal properties of silver oxide powder. Int. J. Biomed. Sci. Eng. 3, 62. doi: 10.11648/j.ijbse.20150305.11
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    Li, R. , He, M. , Li, T. , Zhang, L. N. , 2015. Preparation and properties of cellulose/silver nanocomposite fibers. Carbohydr. Polym. 115, 269-275. doi: 10.1016/j.carbpol.2014.08.046
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    Logeswari, P. , Silambarasan, S. , Abraham, J. , 2013. Eco friendly synthesis of silver nanoparticles from commercially available plant powders and their antibacterial properties. Sci. Iran. 20, 1049-1054.
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    Mahdieh, M. , Zolanvari, A. , Azimee, A. S. , Mahdieh, M. , 2012. Green biosynthesis of silver nanoparticles by Spirulina platensis. Sci. Iran. 19, 926-929. doi: 10.1016/j.scient.2012.01.010
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    Muthulakshmi, L. , Rajini, N. , Nellaiah, H. , Kathiresan, T. , Jawaid, M. , Rajulu, A. V. , 2017a. Preparation and properties of cellulose nanocomposite films with in situ generated copper nanoparticles using Terminalia catappa leaf extract. Int. J. Biol. Macromol. 95, 1064-1071. doi: 10.1016/j.ijbiomac.2016.09.114
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    Muthulakshmi, L. , Rajini, N. , Nellaiah, H. , Kathiresan, T. , Jawaid, M. , Varada Rajulu, A. , 2017b. Experimental investigation of cellulose/silver nanocomposites using in situ generation method. J. Polym. Environ. 25, 1021-1032. doi: 10.1007/s10924-016-0871-7
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    Sadanand, V. , Rajini, N. , Satyanarayana, B. , Varada Rajulu, A. , 2016a. Preparation and properties of cellulose/silver nanoparticle composites with in situ-generated silver nanoparticles using Ocimum sanctum leaf extract. Int. J. Polym. Anal. Charact. 21, 408-416. doi: 10.1080/1023666X.2016.1161100
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    Sadanand, V. , Rajini, N. , Varada Rajulu, A. , Satyanarayana, B. , 2016b. Preparation of cellulose composites with in situ generated copper nanoparticles using leaf extract and their properties. Carbohydr. Polym. 150, 32-39. doi: 10.1016/j.carbpol.2016.04.121
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Preparation and Properties of Cellulose Nanocomposite Fabrics with in situ Generated Silver Nanoparticles by Bioreduction Method

    Corresponding author: Anumakonda Varada Rajulu, avaradarajulu@gmail.com
  • a. Department of Chemical Engineering, Osmania University, Hyderabad-500007, India
  • b. Department of Chemistry, Osmania University, Hyderabad-500007, India
  • c. Departmentof Biochemistry, Kalasalingam University, Anand Nagar, Krishnankovil-626126, India
  • d. Centre for Composite Materials, International Research Centre, Kalasalingam University, Anand Nagar, Krishnankovil-626126, India

Abstract: The aim of the present study was to develop antibacterial cellulose (cotton) nanocomposite fabrics (CNCFs) with in situ generated silver nanoparticles using medicinal plant Vitex leaf extract. The developed CNCFs were characterized by scanning electron microscope (SEM), Fourier transform infrared (FT-IR) spectroscopy, X-ray diffraction (XRD) and antibacterial tests. Further, these CNCFs possessed good antibacterial activities. These CNCFs prepared using simple and environmentally friendly method can be considered for medical applications in, such as, surgical aprons, wound cleaning, wound dressing, and hospital bed materials.

1.   Introduction
  • Due to their unique properties such as higher surface area and antibacterial activity, the silver nanoparticles (AgNPs) and copper nanoparticles (CuNPs) were found many applications in packaging and medical fields (Cady et al., 2011; Bindhani and Panigrahi, 2015). Though there are many methods of generating metal nanoparticles from metal salts, the chemical and biological methods are simple (Sadanand et al., 2016b). Recently, many leaf extracts were used to reduce the metal salts into their respective nanoparticles. For instance, tea leaf and coffee powder (Sutradhar et al., 2014), plant tea (Brumbaugh et al., 2014), Ocimum sanctum (Kulkarni and Kulkarni, 2013), Gymnema sylvestre (Heera et al., 2015) were used as reducing agents to generate AgNPs and CuNPs. Some researchers dispersed the generated metal nanoparticles in polymer matrices to make polymer nanocomposites. However, the dispersion of nanoparticles in polymer matrices often leads to their agglomeration (Jamshidi and Jahangiri, 2014). In order to overcome this problem, some researchers in situ generated AgNPs and CuNPs in cellulose matrix (Sadanand et al., 2016a; 2016b; Muthulakshmi et al., 2017a; 2017b) using different leaf extracts as reducing agents. In the present study, the authors made an attempt to in situ generate AgNPs in cellulose (cotton) fabrics using Vitex leaf extract as a reducing agent. The Vitex leaf extract was selected as it has many medicinal applications as a carminative, an antispasmodic, antiseptic, a diuretic etc. and in the treatment of stomach ache, headache, influenza and diarrhea (Zoghbi et al., 1999; Kathireswari et al., 2014). Further, it was already proved that Vitex leaf extract could reduce the silver nitrate into AgNPs (Kathireswari et al., 2014). The cellulose nanocomposite fabrics (CNCFs) were characterized by Fourier transform infrared (FT-IR) spectroscopy, scanning electron microscope (SEM), X-ray diffraction (XRD) and antibacterial activity tests. The main aim of the present work was to develop antibacterial cotton fabrics with in situ generated AgNPs by simple and low-cost method using medicinal leaf extract as a reducing agent for medical applications such as surgical aprons, wound healing and wound cleaning materials, hospital bed spreads.

2.   Materials and Methods
  • In the present work, silver nitrate obtained from Aldrich Chemicals Ltd. was used as received without further purification. The white cellulose fabrics used in this work were purchased from local market (Hyderabad City, India) and washed twice with double distilled water and air dried. The Vitex leaves were procured from the local area.

  • The cleaned Vitex leaves were cut into small pieces and 10 wt% of leaves were added to distilled water maintained at 80 ℃ for 20 min. The decant was separated, filtered and stored till further use. To make the CNCFs with in situ generated AgNPs, initially, aqueous AgNO3 solutions of 1, 2, 3, 4 and 5 mmol/L concentrations were prepared separately. The cleaned and dried cotton fabrics were immersed in Vitex leaf extract and allowed the diffusion of this leaf extract into the fabrics. The leaf extract infused cotton fabrics were then kept in aq. AgNO3 solutions of different concentrations. The color of these fabrics changed slowly on immersion into light brown and the color deepened slowly. After 24 h, the CNCFs were thoroughly washed with distilled water and air dried.

  • The FT-IR spectra of cellulose fabric (Matrix) and CNCFs with in situ generated AgNPs were recorded on a smart iTR ATR Nicolet is 10 FT-IR spectrophotometer in the range of 4000-500 cm-1 with 32 scans in each case at a resolution of 4 cm-1. In order to examine the presence of AgNPs and their particle size distribution in the CNCFs, SEM images were recorded using Zeiss EVO 18 scanning electron microscope operated at an accelerating voltage of 10 kV. The energy-dispersive X-ray (EDX) spectra of the samples were recorded with the same instrument. The samples were gold sputter coated before recording the images. The XRD of the matrix and CNCFs with in situ generated AgNPs were recorded using a Bruker Eco D8 XRD diffractometer in the 2θ range of 10°-90° operated at a voltage of 40 kV and current 25 mA. The antibacterial activity of the matrix and the CNCFs with in situ generated AgNPs was tested against two gram negative (Pseudomonas and Escherichia coli) and two gram positive (Bassilus subtils and Stephylococus areus) bacteria by disc method following the procedure described elsewhere (Varaprasad et al., 2011). The observed inhibition zones were photographed and the zone diameter in each case was measured.

3.   Results and Discussion
  • The digital images of cellulose fabric, matrix and the CNCFs using 1-5 mmol/L aq. AgNO3 solutions were photographed and are presented in Fig. 1. From Fig. 1, it is evident that cellulose fabric was white in color while the Vitex leaf extract infused cotton fabric (matrix) appeared light brown. On the other hand, the color of the CNCFs varied from medium brown to dark brown with an increasing concentration of the source solution. The color change preliminarily indicates the in situ generation of the AgNPs in the matrix. Similar observation was made by Logeswari et al. (2013) and Banerjee et al. (2014) in the generation of metal nanoparticles by some leaf extracts. In order to visualize the formed AgNPs, the SEM images of the CNCFs were recorded. As an example, the SEM images of the CNCFs using 1 mmol/L (minimum) and 5 mmol/L (maximum) aq. AgNO3 solutions are presented in Fig. 2. The EDX spectra recorded simultaneously for the corresponding SEM images are also presented in the same figure. Using the micrographs, the particle size distribution in both these cases was determined and is presented in the same figure. From the SEM images (Fig. 2a and 2b), it is clearly evident that the formed AgNPs were spherical in shape. From Fig. 2c and 2d, the EDX spectra confirmed the presence of silver particles. It can be further seen that the intensity of the EDX peak corresponding to Ag element for CNCF using 5 mmol/L source solution was higher than that formed using 1 mmol/L source solution. It clearly indicates that larger number of AgNPs was generated when higher concentrated source solution was used. The particle size distribution of the prepared CNCFs using 1 mmol/L and 5 mmol/L source solution is presented in Fig. 2e and 2f, respectively. From the distribution curves, it is evident that in both cases, maximum numbers of generated AgNPs were in the particle range of 91-100 nm. However, the average size of the formed AgNPs in the CNCFs made using 1 mmol/L and 5 mmol/L source solutions was found to be 86 nm and 102 nm, respectively. This may be due to the agglomeration of some of the nanoparticles formed when higher concentrated source solutions were used. In the case of the CNCFs made using other concentrated source solutions (2, 3 and 4 mmol/L), the average particle size was found to be between these two values.

    Figure 1.  Digital photographs of cellulose fabric (a); matrix (b) and CNCFs with in situ generated AgNPs using 1 mmol/L (c); 2 mmol/L (d); 3 mmol/L (e); 4 mmol/L (f) and 5 mmol/L (g) source solutions.

    Figure 2.  Scanning electron microscope (SEM) micrographs (a, b); energy-dispersive X-ray (EDX) spectra (c, d) and particle size distribution (e, f) of cellulose nanocomposite fabrics (CNCFs) with in situ generated silver nanoparticles (AgNPs) using 1 mmol/L and 5 mmol/L aq. AgNO3 solutions respectively.

    In order to examine the interaction between the cotton fabric and the Vitex leaf extract, their FT-IR spectra are presented in Fig. 3a. From Fig. 3a, it is evident that both the spectra had similar peaks indicating similar chemical groups in them. However, the intensity of the peaks at 3337 cm-1 (OH st. vibration) and 1022 cm-1 (C-O-C st. vibration) of the matrix was higher than that of the cotton fabric, indicating that additional OH and C-O-C groups were contributed by the leaf extract. In order to examine the influence of in situ generated AgNPs on the chemical structure of matrix, the FT-IR spectra of the matrix and the CNCFs using 1-5 mmol/L, source solutions are presented in Fig. 3b. For clarity, the spectra of matrix and the CNCF using 5 mmol/L source solution are presented separately in Fig. 3c. From Fig. 3b and 3c, it is evident that no major changes were observed except the lowering of intensity of the bands corresponding to O-H, C-O groups in the case of nano composites fabrics. This clearly indicates the role of O-H and C-O groups of the matrix in reducing the silver salts into AgNPs. The other common bands appearing at 2905 cm-1 (CH st.), 1640 cm-1 (crystallization of water) 1425 cm-1 (CH2 b.), 1359 and 1313 cm-1 (CH2 wagging) and 878 cm-1 (β-glucosidic linkage) indicate the cellulosic structure in both the matrix and the CNCFs. Similar observation was made in the case of synthesis of AgNPs using banana peel extract (Ibrahim et al., 2015) and cellulose nanofibers (Li et al., 2015). Though the OH and CO groups presented in cellulose can act as mild reducing agents (Vainio et al., 2007), their increased number by the leaf extract is expected to increase the reducing capacity of silver salts to AgNPs.

    Figure 3.  Fourier transform infrared (FT-IR) spectra of cotton fabric and matrix (a); matrix and CNCFs with in situ generated AgNPs using 1-5 mmol/L aq. AgNO3 source solutions (b) and matrix and cotton nanocomposite fabric with in situ generated AgNPs using 5 mmol/L source solution (c).

    In order to examine the effect of AgNPs on the crystallinity of the nanocomposite fabrics, the X-ray diffractograms of the cotton fabric, matrix and the nanocomposite cotton fabrics with in situ generated AgNPs using 1-5 mmol/L aq. AgNO3 solutions were recorded and are presented in Fig. 4a. As the overlapped diffractograms did not yield much information, the diffractograms corresponding to the matrix and the CNCF using 5 mmol/L aq. AgNO3 solution are shown separately in Fig. 4b. From Fig. 4b, it is clearly evident that the intensity of the CNCF was slightly higher than that of the matrix indicating a slight increase in the crystallinity of the CNCFs due to the presence of AgNPs. As the presence of AgNPs is hard to observe in the overlapped diffractograms (due to the higher intensity of the peak corresponding to the matrix), the diffractogram of the CNCF using 5 mmol/L aq. AgNO3 was expanded in 2θ = 30°-67° and is presented in Fig. 4c. From Fig. 4c, it is evident that there are several peaks in the diffractograms of which the peaks at 2θ = 38.1°, 45.1° and 63.6° corresponding to the reflections from (111), (200) and (220) planes of AgNPs (Mahdieh et al., 2012). The other prominent peaks observed at 2θ = 32.0°, 38.1°, 54.8° and 65.3° correspond to the reflections from (111), (200), (220) and (311) planes of Ag-O nanoparticles (Kumar Trivedi, 2015), respectively. Thus in the developed CNCFs, both AgNPs and AgO nanoparticles were generated. These results indicate the in situ generation of AgNPs and AgO nanoparticles in the matrix.

    Figure 4.  The X-ray diffractograms (XRD) of cotton cloth, matrix and the CNCFs made using 1-5 mmol/L aq. AgNO3 as source solutions (a); matrix and CNCF using 5 mmol/L source solution (b) and CNCF using 5 mmol/L solution expanded in the 2θ = 30°-67° (c).

    In order to examine the antibacterial activities of the prepared CNCFs using different concentrated source solutions, the disc method was used against two gram negative (Pseudomonas and E. coli) and two gram positive (Bassilus subtils and Stephylococus areus) bacteria. For comparison, the test for cotton fabric and the matrix was also carried. The photographs of the petri dishes in which the test was conducted are presented in Fig. 5. The cotton cloth and the matrix were designated as A and B whereas the CNCFs using 1, 2, 3, 4 and 5 mmol/L were designated as H, I, J, K and L respectively in the images. Using the Image J program, the diameter of the clear zones was calculated and is presented in Table 1.

    Figure 5.  Antibacterial activity of cotton fabric (A); matrix (B); CNCFs with in situ generated AgNPs using 1 mmol/L (H), 2 mmol/L (I), 3 mmol/L (J), 4 mmol/L (K) and 5 mmol/L (L) aq. AgNO3 source solutions and Vitex leaf extract as a reducing agent against Pseudomonas (a); Escherichia coli (b); Bassilus subtils (c) and Stephylococus areus (d) bacteria.

    Concentration of aq. AgNO3 solution used Diameter (mm)
    Pseudomonas E. coli Bassilus subtils Stephylococus areus
    Cotton Fabric (A) - - - -
    Matrix (B) - - - -
    1 mmol/L (H) 12.9 11.0 12.9 11.1
    2 mmol/L (I) 12.6 11.1 14.1 11.4
    3 mmol/L (J) 13.7 13.1 15.1 13.8
    4 mmol/L (K) 13.7 14.4 14.3 14.7
    5 mmol/L (L) 14.4 14.0 13.4 16.3

    Table 1.  Diameter of the clear zones observed for cotton fabric, matrix and CNCFs using 1-5 mmol/L aq. AgNO3 solutions against gram negative (Pseudomonas and Escherichia coli) and gram positive (Bassilus subtils and Stephylococus areus).

    From Fig. 5 and Table 1, it is evident that both cotton fabric and matrix did not show any antibacterial activity. However, the CNCFs with in situ generated AgNPs using different concentrated source solutions and Vitex leaf extract as a reducing agent exhibite good antibacterial activities against gram negative and gram positive bacteria. In all the cases, the clear zone diameters varied between 11.0 mm and 16.3 mm and in most of the cases, incresed with increasing concentration of the source solutions. These observations indicate that the CNCFs can be used in medical applications as antibacterial materials.

4.   Conclusions
  • The matrix was formed by cellulose fabrics infused with Vitex leaf extracts. Using this matrix and 1-5 mmol/L aq. AgNO3 as the source solutions, AgNPs were in situ generated and the resulting CNCFs were characterized by SEM, FT-IR, XRD and antibacterial tests. The OH and CO groups in the matrix (due to the Vitex leaf extract) were found to be responsible for reducing the silver salt solution into AgNPs in the composites as indicated by the FT-IR spectral analysis. The CNCFs had spherical AgNPs with size increasing with increasing concentration of the source solutions. Further, the CNCFs exhibted good antibacterial activities against both the gram negative and gram positive bacteria. Hence, these CNCFs due to their antibacterial activity can be considered for applications in the medical field such as surgical aprons, wound cleaning and wound dressing materials and bed spreads for patients.

Conflict of Interest
  • The authors have no competing interest to decare.

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