Recieve Jute

Journal of Vinyl and Additive Technology
Removal of toxic heavy metal ions from aqueous solutions

using grafted Jute fibers with acrylic acid by gamma
irradiation
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Journal: Journal of Vinyl and Additive Technology
Manuscript ID VNL-16-161
Wiley - Manuscript type: Research Article

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Date Submitted by the Author: 13-Dec-2016

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Complete List of Authors: Hassan, Mahmoud; National Centre for Radiation Research and
Technology, Radiation Chemistry;
Zohdy, maged
er
Keywords: adsorption, copolymerization, fibers, functional polymers, radiation

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Page 1 of 25 Journal of Vinyl and Additive Technology
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3 Removal of toxic heavy metal ions from aqueous solutions using
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6 grafted Jute fibers with acrylic acid by gamma irradiation
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9 Mahmoud S. Hassan* and Maged H. Zohdy
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14 -Mahmoud S. Hassan (corresponding author)
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16 Asst. Prof Dr., Department of Radiation Chemistry, National Center for Radiation Research
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and Technology (NCRRT), Atomic Energy Authority. Tel.: +202 22748246; fax: +202
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21 22749298.
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25 -Maged H. Zohdy
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Dr., Department of Radiation Chemistry, National Center for Radiation Research and
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30 Technology (NCRRT), Atomic Energy Authority. Tel.: +202 22748246; fax: +202
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32 22749298.
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36 Acknowledgements
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The authors would like to thank the National Center for Radiation Research and
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40 Technology (NCRRT), Egyptian Atomic Energy Authority for providing the facilities and
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42 financial support throughout this work.
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Journal of Vinyl and Additive Technology Page 2 of 25
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3 Removal of toxic heavy metal ions from aqueous solutions using
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6 grafted Jute fibers with acrylic acid by gamma irradiation
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9 Mahmoud S. Hassan* and Maged H. Zohdy
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11 Radiation Chemistry Department, National Center for Radiation Research and Technology, Atomic Energy
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13 Authority, B.O. Box 29 Nasr City, Cairo, Egypt.
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17 ABSTRACT
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19 Jute fibers were grafted with acrylic acid by using the direct gamma irradiation
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technique, which used as an adsorbent substrate for the toxic heavy metal ions such as
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24 Hg2+and Pb2+ metal ions from their aqueous solutions. The treated Jute fibers were
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26 characterized by using of Fourier-transform infrared spectroscopy (FTIR) and X-ray
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28 diffraction (XRD). The effect of pH range of the metal ion solutions, contact time and the
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adsorption kinetics of the adsorption process were investigated. The effect of the initial
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concentration of dissolved metal ions and the adsorption isotherm for both of Langmuir and
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35 Freundlich adsorption models were also investigated. From the results, it can be concluded
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37 that the adsorption process obeys the second order kinetic reaction, and follows the Langmuir
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39 adsorption isotherm model, while, the higher adsorption capacities were at pH 5 and pH 6 for
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Pb2+ and Hg2+ metal ions, respectively.
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46 Keywords: Jute fibers; Gamma irradiation; Metal ion adsorption; Adsorption kinetics;
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48 Adsorption isotherm
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3 INTRODUCTION
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5 Heavy metal pollution can cause serious environmental problems as a result of their
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toxicity and carcinogenic effects on the natural environment and its accumulation in living
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10 organisms [1]. The toxicity of heavy metals might be caused by blocking essential functional
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12 groups of biomolecules and by disrupting the integrity of bio-membranes [2]. Mercury and
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14 lead are two the most famous toxic heavy metals, which are responsible for the water
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16 pollution of industrial effluents.
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Mercury pollution usually comes from different industries such as chloroalkali, paint,
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21 pharmaceutical, pulp and paper. Lead pollution comes as a result of the batteries storage and
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23 plating industries [3]. The increasing of lead concentrations in the drinking water can cause
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25 undesirable effects on the mental development of children and can cause the increasing of the
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blood pressure in adults. On the other hand, the presence of mercury in water in higher
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30 quantities can cause the damage of the central nervous system and chromosomes, and can
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32 cause the chest pain [4]. Because of increased environmental awareness, the development of
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34 cost effective methods for the removal of lead and mercury from aqueous solutions has
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36 gained great importance. Different techniques can be used for removing of the undesirable
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39 dissolved heavy metal ions from aqueous solutions, conventional techniques such as chemical
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41 precipitation, ion exchange, reverse osmosis, membrane separation and electrochemical
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43 treatments processes [5-7]. These techniques are often costly or ineffective, especially in
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45 removing heavy metal ions at low concentrations [8], while the adsorption methods are more
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effective for removing the undesirable heavy metals without producing unwanted by-
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50 products. Different materials were used as dye adsorbents such as: activated carbon [9],
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52 carboxylated cellulose nanocrystals [10], fly ash [11], Soy protein hollow microspheres [12],
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54 sawdust [13], polyrhodanine-encapsulated magnetic nanoparticles [14] and chitosan
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56 entrapped CM-cellulose hydrogels [7]. Moreover, the grafted substrates polyacrylic acid, due
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3 to the characteristic chelating ability of the crosslinked polyacrylic acid upon different
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5 substrates towards different heavy metal ions [15,16].
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The irradiation technique is known to be an effective technique for altering the properties
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10 of matters; graft copolymerization by using the direct irradiation technique was used over the
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12 past decades for polymer treatments, in which, new side chains could be introduced to the
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14 polymer backbone by covalent bonding [17-19]. In this regards, the radiation was induced the
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16 grafting polymerization to produce high performance chemically active polymer materials for
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adsorption and separation processes. As an example, the grafting process with poly acrylic
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21 acid, which act as a chelating polymer have a considerable attention in the separation of
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23 heavy metals due to its ability to form chelates [15].
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25 Jute is one of the most affordable natural fibers and is the second to cotton in amount
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produced and variety of its raw material extracted from vegetable fibers. It also cheap,
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30 contains huge interspaces and can be used easily as a wastewater effluent filtration. Jute
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32 fibers are lignocelluloses natural fibers, composed mainly of cellulose, hemicellulose (82–85
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34 %) and lignin [20]. Jute fibers are also known for its durability, and eco-friendly properties,
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36 so they are ideal for the different adsorption applications.
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39 The present work dealt with the grafting of Jute fibers with acrylic acid monomer by
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41 using mutual gamma radiation technique, which used as an adsorbent substrate as for some
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43 toxic heavy metal ions such as: Pb2+ and Hg2+. The grafted Jute fibers were characterized by
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45 using FTIR and XRD. The effect of different parameters on adsorption capacity of grafted
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Jute fibers for metal ions such as contact time, pH range and the initial concentrations of the
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50 metal ion solutions were investigated. The Kinetic parameters and the adsorption isotherm of
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52 adsorption process were also investigated.
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3 EXPERIMENTAL AND TECHNIQUES
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5 Materials
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Acrylic acid (AAc) was used as received and it was supplied by Fluka. Jute fibers
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10 were supplied by the Egyptian Company for Jute Production, Egypt. Ammonium hydroxide,
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12 Ammonium chloride, Sodium hydroxide, EDTA and Glacial acetic acid were supplied by El-
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14 Nasr Pharmaceutical Chemicals Co., Egypt. Lead nitrate [Pb(NO3)2] (Mwt; 331.2) and
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16 mercuric chloride [HgCl2] (Mwt; 271.52) were supplied by Alpha Chemika Co., India. All
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chemical reagents used were all of analytical grade and all the solutions were prepared with
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21 distilled water.
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23 Grafting of Jute fibers with acrylic acid
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25 Jute fibers were pre-swelled swelled for 24 h in NaOH solution (20%), then they
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washed, neutralized with diluted acetic acid and then the dried samples were weighted (Wo).
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30 The grafting process of Jute fibers were done by immersing of the pre-swelled fibers into
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32 glass tubes containing acrylic acid monomer, solvent and ferrous ammonium sulphate as an
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34 inhibitor for the homopolymer formation, then they irradiated at different doses of direct
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36 gamma radiation source. The grafted fibers were then washed to extract the residual
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39 monomer and homopolymer. The homogenous grafted samples were dried and weighed
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41 (Wg). The degree of grafting was calculated as shown in Eq. 1:
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43 Graft yield (%) = [(Wg – Wo)/Wo] x 100 (1)
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45 Irradiation to the required doses was carried out at a Co60 gamma cell of dose rate 2.5
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kGy/ h (made in India) installed at the National Center for Radiation Research and
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50 Technology, Cairo, Egypt.
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52 Characterization of grafted Jute fibers with PAAc
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54 The prepared grafted Jute fibers were analyzed by Fourier transform infrared (FTIR),
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56 in a wide range wavenumber (400 - 4000 cm-1), and in solid state using Mattson 5000 FTIR
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3 spectrometer (Mattson Instruments, Madison, WI). X-ray diffraction (XRD) studies were
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5 performed using Philips (PW 1390) equipment, using Nickel- filtered Cu-Kα radiation.
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Determination of metal ions adsorption capacity grafted Jute fibers
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10 The adsorption capacity (q) of Jute fibers towards the different metal ions was
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12 determined. A constant weight of dry treated Jute fibers (0.2 g) was immersed in a definite
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14 volume (50 ml) of metal salts solutions from HgCl2 or Pb(NO3)2, at a constant concentration
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16 of (0.1 M) for all, in flasks under shaking. The remaining metal ions concentrations were
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determined by using standard solution of EDTA [21]. The adsorption capacity, the amount of
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21 ions adsorbed per mass unit of treated Jute fibers q (mg/g) was evaluated was calculated
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23 using Eq. 2:
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25 q= (Co – Ce) V/ W (2)

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Where Co and Ce are the initial and equilibrium metal ion solution concentrations (mg/l),
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30 respectively, W is the weight of treated Jute fibers (g), V is the volume of metal salt solution
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32 (L).
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36 RESULTS AND DISCUSIONS
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39 Graft copolymerization of Jute fibers with acrylic acid
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41 Jute fiber is known to be stiff fiber with rough textured surface, with high crystalline
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43 proportion as a result of the high lignin percent and hemicelluose ratios. To overcome this
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45 drawback, the alkali impregnation of the fibers was used as a pretreatment, to decrease the
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crystalline fraction related to the amorphous portion. This consequently leads to the increase
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50 in the chemical reaction possibilities of the Jute fibers [22,23]. In the grafting of individual
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52 monomers by radiation, it is easy to control the grafting process by controlling the factors
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54 affecting the graft yield. From previous works [24], it was found that the grafting solution was
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56 preferred to be includes H2O/MeOH (90:10), 0.1% of ammonium ferrous sulphate as inhibitor
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3 for homopolymer formation. The effect of irradiation dose and monomer concentration on the
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5 obtained graft yield was investigated as shown in Fig. 1, in which the grafting yield increases
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with increasing of the irradiation dose, as a result of the free radicals formation, which leads to
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10 the increase in the grafting yield [25]. It was found also that the grafting yield increases with
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12 increasing of the AAc monomer concentration up to 30%, which give 28% grafting yield at 30
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14 (kGy) irradiation doses. By increasing AAc monomer concentration further more 30%, the
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16 grafting yield tends to level off as a result of homopolymer formation of PAAc [26].
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Characterization of Jute fibers
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21 Fourier-transform infrared (FTIR)
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23 FTIR spectroscopic analysis was used to confirm the formation of graft
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25 copolymerization of PAAc onto Jute fibers. Fig. 2 shows the IR spectra of ungrafted and
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grafted Jute fibers with PAAc (28% grafting yield). As illustrated, the FTIR spectrum of Jute
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30 fibers before grafting, as an example of cellulosic materials showed a characteristic absorption
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32 band at 3448 cm-1 assigned to the stretching vibration of –OH, the vibration band at 2923cm-1
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34 confirms the presence of C-H stretching, the vibration band at 1650-1640cm-1 due to the water
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36 associated with cellulose. In addition, absorption bands at 1375-1320 cm-1 and at 1047-1004cm-
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39 confirms the presence of C-H bending of cellulose, and the stretching vibration of C-O,
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41 respectively. On the other hand, the FTIR spectrum of grafted Jute fibers with PAAc showed
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43 the same characteristic vibration bands of Jute fibers were found beside new characteristic
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45 absorbed bands for –CO of carboxylic acid at 1320-1210 cm-1, –C=O of carboxylic acid at 1720-
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1700 cm-1, accompanied with increasing of –OH broad band of carboxylic acid at 3448 cm-1.
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50 These findings prove the introduction of PAAc grafted chains onto the backbone of Jute
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52 fibers [27].
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3 X-ray diffraction (XRD)
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The XRD spectra of untreated Jute and Jute-g-PAAc were studied as shown in Fig. 3.
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8 The Jute fibers showed a definite characteristic peak at 2θ = 22.45o. A sharp peak was
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10 observed, which represents the high crystallinity nature of Jute fibers (intensity ~908 Kcps).
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12 This could be attributed to the great crystalline lignin [22] in the Jute fibres composition.
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14 After grafting with PAAc, the intensity of the characterized peak of Jute fibers was decreased
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17 (intensity ~620 Kcps), which could be attributed to the dilution of the crystalline fraction by
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Adsorption mechanism of metal ions by grafted Jute fibers with PAAc
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24 The mechanism of the metal ions adsorption processes is not fully understood but
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26 several mechanisms were suggested for metal ion binding to the grafted polymer chains
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28 including ion exchange, complexation , co-ordination/ chelation , electrostatic interactions,
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acid-base interactions, hydrogen bonding, hydrophobic interactions, physisorption and
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possibly precipitation. In the case of Jute grafted with acrylic acid, the hydrogen atom in
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35 carboxylic group of acrylic acid can be exchanged by metal ion and then, the carboxyl groups
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37 have two lone pair of electrons on the oxygen can be form a chelate with metal ion [29]. Two
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39 carboxyl groups are required to form a chelate with divalent metal ions. The Jute-g-PAAc
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was used as an adsorbent matrix for some toxic divalent heavy metal ions such as Pb2+ and
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44 Hg2+. Previous reports [30] proved that the carboxylic groups of AAc act as strong
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46 complexing agent for the metal ions as shown in Eqs. 3 and 4:
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Jute-g-COO- + Pb2+ → [Jute-g-COO] 2 Pb (complex) (3)
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53 Jute-g-COO- + Hg2+ → [Jute-g-COO] 2 Hg (complex) (4)
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3 Effect of pH
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5 The influence of the initial dye solutions pH on the amount of adsorbed metal ions (q)
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by the grafted Jute fibers with PAAc was illustrated as shown in Fig. 4. The binding of metal
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10 ions to the adsorbent as a function of pH, using of 0.1 M as an initial concentration for both
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12 of two metal salts, at temperature of (30oC), after 60 min of soaking under shaking is
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14 represented in Fig. 4. It is clear that the metal binding is strongly pH dependent and
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16 maximum adsorption occurs at pH 5 for lead and pH 6 for mercury. The increase in metal
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removal (%) with increase in pH is due to a decrease in competition between proton and
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21 metal ions for the surface sites and by the decrease in positive surface charge. Meanwhile, the
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23 metal removal was decreased at low pH values as a result of the protonation effect and the
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25 increasing competition of protons for the same binding sites that metal can use. A slight
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decrease in adsorption was observed above pH 5 for lead and at pH 6, Pb2+ started
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30 precipitating as Pb(OH)2. Hence pH experiments at alkaline ranges were avoided. Hg2+
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32 adsorption at higher pH may be attributed to the electrostatic attraction between Hg(OH)+
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34 ions and the negatively charged adsorbent surface [31].
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36 Effect of contact time
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39 The effect of contact time on the adsorption efficiency (%) of Jute-g-PAAc fibres towards
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41 the different metal ions, at constant pH (5) and temperature (30oC) was studied as shown in
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43 Fig. 5. It can be seen that the absorption capacity of treated Jute fibres towards the different
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metal ions increased significantly after 10 min, and it tended to increase with lower rate with
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48 increasing the time up to 60 min. Above 60 min, the adsorption capacity tended to level off.
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50 The rapid initial adsorption was due to the abundant available chelating PAAc sites on the
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52 surface of treated Jute fibres and the high concentration of metal ions [32], with increasing the
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54 contact time, the adsorption rate decreased and finally reached equilibrium, due to limited
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57 vacant adsorption sites available on the treated Jute fibres. It was found also that, at the same
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3 conditions that the adsorption efficiency was grater in case of Pb2+ metal ions than it in the case
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5 of Hg2+ metal ions. This could be attributed the change in their binding capacity, which it was
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(7.18) and (6.75) for Pb2+ and Hg2+ metal ions, respectively. [33]. Also, the metal ion atomic
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10 number plays an important role [34-36], in which the Pb2+ metal ions posses the higher atomic
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12 number and the smaller hydrated ionic radii, which increase its adsorption possibility upon the
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17 Adsorption Kinetics
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21 of the metal ions. The pseudo first-order model [37,38] was used according to Eq. 5:
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log(qe - qt) = log qe – kpf / 2:303t (5)
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26 Where, qe is the adsorbed amount of metal ions (mg/g) at equilibrium, qt is the
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28 adsorbed amount of metal ions (mg/g) at time t and the pseudo first order rate constant kpf
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30 (min-1). The slopes and intercepts of plots of log (qe–qt) versus time (t), were used to
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32 determine kpf and qe as illustrated in Fig. 6. The data of qm, b and correlation coefficient (r2)
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35 were summarized in Table 1. On the other hand, the pseudo second-order model [39] was
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37 used according to Eq. 6:

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39 t/qt =1/K2q2e + t/qe (6)
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41 Where, k2 is the rate constant of pseudo second order adsorption (g/mg/min), qe is the
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adsorbed amount of metal ions (mg/g) at equilibrium and qt is the adsorbed amount of metal
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46 ions (mg/g) at time t. The slopes and intercepts of plots of (t/qt) versus time (t) were used to
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48 determine k2 and qe as illustrated in Fig. 6. The data of k2, qe and correlation coefficient (r2)
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50 were summarized in Table 1.
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52 As shown in Table 1, which summarize the obtained data for both of the adsorption
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55 kinetic models, the correlation coefficients were found to be 0.7882 for both of Pb2+ and Hg2+
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57 metal ions according to the pseudo first order model, while they were 0.9991 for both of Pb2+
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3 and Hg2+ metal ions according to the pseudo second order model, which indicate sharply that
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5 the adsorption processes for both of Pb2+ and Hg2+ metal ions by the treated Jute fibers obey
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the pseudo second order model.
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10 Effect of initial concentration
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12 The influence of the initial dye concentrations (Co) on the amount of adsorbed Hg2+,
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14 Pb2+ metal ions at equilibrium (qe) by the grafted Jute fibers with PAAc was illustrated as
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16 shown in Fig.7. It can be seen that the adsorption capacity at equilibrium increases with
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increasing of the initial concentrations of the metal ion concentration, for both of Pb2+ and
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21 Hg2+. This could be attributed to the acceleration of the metal ion diffusion into the
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23 polymeric network, in which, at higher concentrations, the driving force increases which
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25 overcome the mass transfer resistance between solid- liquid phases [40].
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Adsorption isotherms
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30 The adsorption isotherms are important for the discussion of the interaction of the
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32 adsorbent molecules with the adsorbent surface [41,42]. Two common adsorption isotherm
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34 models can be used to describe the experimental data; Langmuir and Freundlich models. The
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36 Langmuir adsorption isotherm assumes that the adsorption process occurs at specific
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39 homogeneous sites on the Jute-g-PAAc and is the most commonly used for monolayer
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41 adsorption process, as shown in Eq.7:
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43 Ce/qe = 1/bqm + Ce/qm (7)
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46 Where, qe is the equilibrium adsorption capacity of metal ions on Jute-g-PAAc (mg/ g), Ce is
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48 the equilibrium metal ion concentration (M), qm is the monolayer adsorption capacity and b is
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the Langmuir adsorption constant (L/mg). The slopes and intercepts of plots of Ce/qe versus
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53 Ce were used to determine qm and b as illustrated in Fig. 8. The data of qm, b and correlation
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3 The Freundlich adsorption isotherm assumes that the adsorption process occurs at
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5 specific heterogeneous systems and is the most commonly used for adsorption process, as
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shown in Eq. 8:
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10 ln qe = ln Kf+ 1/n ln Ce (8)
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13 Where, qe is the equilibrium adsorption capacity of metal ions on Jute-g-PAAc (mg/ g), Ce is
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15 the equilibrium metal ion concentration (M), Kf is Freundlich constant and 1/n is the
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17 heterogeneity factor. The slopes and intercepts of plots of ln qe versus ln Ce were used to
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determine Kƒ and n as shown in Fig. 8 [43]. The data of Kf , n and correlation coefficient (r2)
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As shown in Table 2, which summarize the obtained data for both of the two isotherm
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27 models, the values of r2 for the adsorption of both two metal ions (Pb2+ and Hg2+), according
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31 dye qm was 16.67 and 15.63 for Pb2+ and Hg2+, respectively. Mainwhile, r2 for both two metal
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33 ions, according to the Freundlich equation were found to be 0.9765. According to the values
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36 of the determined correlation coefficients (r2), it can be seen that the Langmuir equation has a
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38 nearest fit to the experimental data than the Freundlich equation. So, it can be concluded that
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42 does not follow the Freundlich model.
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47 CONCLUSIONS
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49 This work was dealt with the grafting of Jute fibers with PAAc. The prepared Jute-g-
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51 PAAc was used as an adsorbent for different metal ions from their solutions. From the
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53 results, it can be concluded that the adsorption capacity of Jute-g-PAAc was enhanced at
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56 moderate pH range up to 5, 6 for Pb2+ and Hg2+, respectively. It can be concluded also that
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58 the adsorption kinetics of the adsorption process of Jute-g-PAAc towards the metal ions
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3 follow the pseudo second order rate and obey the Langmuir adsorption isotherm model. For
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5 all cases, the adsorption selectivity for Pb2+ was greater than it in the case of Hg2+, according
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to the change in their binding capacity.
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12 RERERENCES
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14 [1] C. Liu, R. Bai, and Q. S. Ly, Water Res., 42(6-7), 1511(2008).
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17 [2] G. Bayramoglu, M. Y. Arica, and S. Bektas, J. Appl. Polym. Sci., 106(1),169 (2007).
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19 [3] P. Shekinah, K. Kadirvelu, P. Kanmani, P. Senthilkumar, and V. Subburam, J. Chem.
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[5] R. Akkaya, and U. Ulusoy, J. Hazard. Mater., 151, 380 (2008).
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[6] S. H. Jang, Y. G. Jeonga, B. G. Min, W.S. Lyoo, and S.C. Lee, J. Hazard. Mater., 159(2-
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33 [7] L. Zhao, and H. Mitomo, J. Appl. Polym. Sci., 110(3), 1388 (2008).
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35 [8] R. Laus, and V. T. De Favere, Biosource- Technol., 102 (19), 8769 (2011).
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38 [9] M. Kobya,; E. Demirbas,; E. Senturk, and M. Ince, Bioresource Technol., 96(13), 1518
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42 [10] X. Yu, S. Tong, M. Ge, L. Wu, J. Zuo, C. Cao, and W. Song, J. Environ. Sci., 25(5), 933
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22 Monomer conc. Irradiation dose (kGy)
r
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24 Figure1. Effect of irradiation dose and AAc concentration on the graft yield of PAAc
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26 onto Jute fibers at constant solvent composition H2O/MeOH; 90/10) and
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1650
12 1375
13 0.4 3448
14 1047
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Transmittance (%)
17 Jute/PAAc
1.0
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Fo
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20 0.6
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Figure 3. XRD scans of untreated Jute and Jute-g-PAAc fibers.
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Figure 4. Effect of pH on the absorption of different metal ions by Jute-g-PAAc.
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24 Figure 5. Effect of contact time on the adsorption capacity of metal ions by Jute-g-
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Pb
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t/q t (min/(mg/g)
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Log(q e-q t )
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17 Pseudo first order Pseudo second order
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22 Figure 6. The pseudo-first and second order plots for the adsorption of the different
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qe (mg/g)
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17 Time: 60 min
3 Hg2+
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20 0.0 0.1 0.2 0.3 0.4 0.5 0.6
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Ce (M)
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24 Figure 7. Effect of initial ion concentrations on the adsorption capacity of metal ions
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Ce/qe
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14 0.02
1.2
15 1.0
16 Pb2+ Pb2+
0.01
17 Hg2+ 0.8 Hg2+
18 0.00 0.6
Fo
19 0.0 0.1 0.2 0.3 0.4 0.5 0.6 -4.0 -3.5 -3.0 -2.5 -2.0 -1.5 -1.0 -0.5
20 Ce (M) ln Ce
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Figure 8. The Langmuir and Freundlich plots for the adsorption of the different metal
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Pseudo first order Pseudo second order
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8 kinetic model kinetic model
9 Metal ions Kpf qe r2 Kps qe r2
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11 (min-1) (mg/g) (g/(mg/min)) (mg/g)
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Pb2+ 0.0657 1.1823 0.7882 0.0253 0.1519 0.9991
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14 Hg2+ 0.0707 1.1484 0.7882 0.0197 0.1519 0.9991
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Metal ions Langmuir model Freundlich model
8 qm b r2 Kƒ n r2
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10 Pb2+ 16.67 0.01 0.9954 0.751 0.776 0.9765
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12 Hg2+ 15.63 0.01 0.9954 0.746 0.748 0.9765
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Journal of Vinyl and Additive Technology

Removal of toxic heavy metal ions from aqueous solutions

Wiley - Manuscript type: Research Article

Date Submitted by the Author: 13-Dec-2016

Keywords: adsorption, copolymerization, fibers, functional polymers, radiation

John Wiley & Sons

25 q= (Co – Ce) V/ W (2)

37 used according to Eq. 6:

37 [27] Y. Zheng, and A. Wang, J. Macromol.Sci.A., 47(1), 33 (2009).

25 [41] E. L. Grabowska, and G. Gryglewicz, Dyes Pigm., 74, 34 (2007).

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