Sains Malaysiana 47(6)(2018): 1189–1197

http://dx.doi.org/10.17576/jsm-2018-4706-14

Influence of Poly (Ethylene Glycol) on the Characteristics of γ Radiation-Crosslinked Poly (Vinyl Pyrrolidone)-Low Molecular Weight Chitosan Network Hydrogels

(Kesan Poli(etilena glikol) ke atas Ciri-ciri Jaringan Hidrogel Kitosan Berjisim Molekul
Rendah-Poli(vinil pirolidon)Tertautsilang melalui Teknik Sinar Gamma)

MAZNAH MAHMUD^1,2*, RUSLI DAIK¹ & ZAINAH ADAM ²

¹School of Chemical Sciences and Food Technology, Universiti Kebangsaan Malaysia

43600 UKM Bangi, Selangor Darul Ehsan, Malaysia

²Radiation Processing Technology Division, Malaysian Nuclear Agency

43000 Kajang, Selangor Darul Ehsan, Malaysia

³Medical Technology Division, Malaysian Nuclear Agency, 43000 Kajang, Selangor Darul Ehsan

Malaysia

Received: 9 June 2017/Accepted: 8 January 2018  

ABSTRACT

PEG at compositions of 10, 15 and 20 g were added into the initial formulation of hydrogel L, which was composed of 6 g low molecular weight chitosan (LMC) and 14 g poly (vinyl pyrrolidone) in 100 g of 2% lactic acid. The mixtures were moulded and exposed to γ radiation at 7 kGy. The hydrogels obtained were characterized in term of gel fraction, swelling property, syneresis effect, FTIR, XRD and cross section morphology. The results indicated PEG reduces almost 27% crosslinking density of the LMC-PVP hydrogel yet increased hydrogel’s water holding capacity from 450% and 480% to 750% and 650% in phosphate buffer solution (PBS) at pH5.5 and pH7.0, respectively. Also PEG enhanced the ability of LMC-PVP hydrogel to retain its moisture from dehydration at body temperature. The morphological study showed PEG developed thick pores wall and reduced the pores size of the hydrogels’ network.

Keywords: Covalent-crosslink; plasticizer; porosity; swelling-equilibrium; syneresis

ABSTRAK

PEG dengan komposisi yang pelbagai iaitu 10, 15 dan 20 g telah ditambah ke dalam formulasi asal hidrogel L yang telah disediakan melalui pengadunan 6 g kitosan berjisin molekul rendah (LMC) dengan 14 g poli (vinil pirolidon) dan 100 g asid laktik berkepekatan 2%. Semua adunan dimasukkan dalam acuan dan didedahkan kepada sinar γ pada dos 7kGy. Hidrogel yang diperoleh dibuat pencirian daripada aspek kandungan gel, sifat pembengkakan, kesan sineresis, FTIR, XRD dan morfologi hidrogel menggunakan mikroskop imbasan elektron (SEM). Keputusan pencirian menunjukkan 10 g PEG telah mengurangkan ketumpatan jaringan taut silangan hidrogel sebanyak 14% tetapi meningkatkan keupayaan memegang air daripada 450% dan 480% kepada 750% dan 650% masing-masing dalam larutan penimbal fosfat (PBS) pada pH5.5 dan pH7.0. PEG juga meningkatkan keupayaan hidrogel LMC-PVP untuk mengekalkan kelembapannya daripada terhidrat pada suhu badan. Kajian morfologi juga menunjukkan PEG telah membentuk satu jaringan hidrogel berliang lebih kecil dengan dinding liang yang lebih tebal.

Kata kunci: Keliangan; pembengkakan ekuilibrium; pemplastik; sineresis; taut silang kovalen

REFERENCES

Abad, L.V., Relleve, L.S., Aranilla, C.T. & Rosa, A.M.D. 2003. Properties of radiation synthesized PVP-kappa carrageenan hydrogel blends. Radiation Physics and Chemistry 68: 901-908. http://doi.org/10.1016/S0969-806X(03)00164-6.

Ako, K. 2015. Influence of elasticity on the syneresis properties of Kappa-carrageenan gels. Carbohydrate Polymers 115:408-414. http://doi.org/10.1016/j.carbpol.2014.08.109.

Archana, D., Singh, B.K., Dutta, J. & Dutta, P.K. 2013. In vivo evaluation of chitosan – PVP – titanium dioxide nanocomposite as wound dressing material. Carbohydrate Polymers 95: 530-539. http://doi.org/10.1016/j.carbpol.2013.03.034.

Berger, J., Reist, M., Mayer, J.M., Felt, O., Peppas, N.A. & Gurny, R. 2004. Structure and interactions in covalently and ionically crosslinked chitosan hydrogels for biomedical applications. European Journal of Pharmaceutics and Biopharmaceutics 57: 19-34. http://doi.org/10.1016/S0939-6411(03)00161-9.

Can, H.K. 2005. Synthesis of persulfate containing poly (N -vinyl-2-pyrrolidone) (PVP) hydrogels in aqueous solutions by g -induced radiation. Radiation Physics and Chemistry 72: 703–710. http://doi.org/10.1016/j. radphyschem.2004.04.028.

Das, A., Gupta, B.K. & Nath, B. 2012. Mucoadhesive polymeric hydrogels for nasal delivery of Penciclovir. Journal of Applied Pharmaceutical Science 2: 158-166. http://doi.org/10.7324/JAPS.2012.21228.

De Kruif, C.G.K., Anema, S.G., Zhu, C., Havea, P. & Coker, C. 2015. Food hydrocolloids water holding capacity and swelling of casein hydrogels. Food Hydrocolloids 44: 372-379. http://doi.org/10.1016/j.foodhyd.2014.10.007.

Dergunov, S.A. & Mun, G.A. 2009. γ-irradiated chitosanpolyvinyl pyrrolidone hydrogels as pH-sensitive proteindelivery system. Radiation Physics and Chemistry 78: 65-68. http://doi.org/10.1016/j.radphyschem.2008.07.003.

Dergunov, S.A., Nam, I.K., Mun, G.A., Nurkeeva, Z.S. & Shaikhutdinov, E.M. 2005. Radiation synthesisand characterization of stimuli-sensitive chitosan–polyvinyl pyrrolidone hydrogels. Radiation Physics and Chemistry 72: 619–623. http://doi.org/10.1016/j. radphyschem.2004.03.011.

Divoux, T., Mao, B. & Snabre, P. 2015. Syneresis and delayed detachment of agar plates. Soft Matter 11: 3677-3685. http:// doi.org/10.1039/C5SM00433K.

Duy, N.N., Phu, D., Van Anh, N.T. & Hien, Q.N. 2011. Synergistic degradation to prepare oligochitosan by g -irradiation of chitosan solution in the presence of hydrogen peroxide.Radiation Physics and Chemistry 80: 848-853. http://doi.org/10.1016/j.radphyschem.2011.03.012.

El-sherbiny, I.M. & Smyth, H.D.C. 2012. Poly (ethyleneglycol)– carboxymethyl chitosan-based pH-responsive hydrogels: Photo-induced synthesis, characterization, swelling, and in vitro evaluation as potential drug carriers. Carbohydrate Research 345: 2004-2012. http://doi. org/10.1016/j.carres.2010.07.026.

Farag, R.K. & Mohamed, R.R. 2012. Synthesis and characterization of carboxymethyl chitosan nanogels for swelling studies and antimicrobial activity.Molecules 18: 190-203. http://doi. org/10.3390/molecules18010190.

Hashemi, A., Mirzadeh, H., Imani, M. & Samadi, N. 2013. Chitosan/polyethylene glycol fumarate blend film: Physical and antibacterial properties. Carbohydrate Polymers 92: 48-56. http://doi.org/10.1016/j.carbpol.2012.09.002.

Hezaveh, H. & Muhamad, I.I. 2013. Controlled drug release via minimization of burst release in pH-response kappacarrageenan/ polyvinyl alcohol hydrogels. Chemical Engineering Research and Design 91: 508-519. http://doi.morg/10.1016/j.cherd.2012.08.014.

Hill, D.J.T., Whittaker, A.K. & Zainuddin. 2011. Water diffusion into radiation crosslinked PVA – PVP network hydrogels. Radiation Physics and Chemistry 80: 213-218. http://doi. org/10.1016/j.radphyschem.2010.07.035.

Jin, S., Liu, M., Zhang, F., Chen, S. & Niu, A. 2006. Synthesis and characterization of pH-sensitivity semi-IPN hydrogel based on hydrogen bond between poly (N-vinylpyrrolidone) and poly (acrylic acid).Polymer 47: 1526–1532. http://doi. org/10.1016/j.polymer.2006.01.009.

Mahmud, M., Daik, R. & Adam, Z. 2015. Properties of radiationsynthesized poly(vinyl pyrrolidone)/chitosan hydrogel blends. AIP Conference Proceedings. DOI: 10.1063/1.4931310.

Makuuchi, K. 2010. Critical review of radiation processing of hydrogel and polysaccharide.Radiation Physics and Chemistry 79: 267-271. http://doi.org/10.1016/j. radphyschem.2009.10.011.

Meena, R., Prasad, K. & Siddhanta, A.K.Ã. 2009. Food hydrocolloids development of a stable hydrogel network based on agar–kappa-carrageenan blend cross-linked with genipin. Food Hydrocolloids 23: 497-509. http://doi. org/10.1016/j.foodhyd.2008.03.008.

Nguyen, N. & Liu, J. 2013. Fabrication and characterization of poly (vinyl alcohol)/ chitosan hydrogel thin films via UV irradiation. European Polymer Journal 49: 4201-4211. http:// doi.org/10.1016/j.eurpolymj.2013.09.032.

Park, J., Kim, H., Choi, J., Gwon, H., Shin, Y., Young, M., Lim, M., Khill, M.S. & Nho, Y. 2012. Effects of annealing and the addition of PEG on the PVA based hydrogel by gamma ray. Radiation Physics and Chemistry 81: 857-860. http://doi. org/10.1016/j.radphyschem.2012.02.005.

Park, K.R. & Nho, Y.C. 2003. Synthesis of PVA/PVP hydrogels having two-layer by radiation and their physical properties.Radiation Physics and Chemistry 67: 361-365. http://doi.  org/10.1016/S0969-806X(03)00067-7.

Park, S., Nah, J. & Park, Y. 2011. pH-Dependent mode of antibacterial actions of low molecular weight watersoluble chitosan (LMWSC) against various pathogens. Macromolecular Research 19: 853-860. http://doi. org/10.1007/s13233-011-0812-1.

Pasanphan, W., Rimdusit, P., Choofong, S., Thananchai, P. & Nilsuwankosit, S. 2010. Systematic fabrication of chitosan nanoparticle by gamma irradiation. Radiation Physics and Chemistry 79: 1095-1102. http://doi.org/10.1016/j.radphyschem.2010.04.003.

Pollock, J.F. & Healy, K.E. 2010. Mechanical and swelling characterization of poly ( N -isopropyl acrylamide-comethoxy poly (ethylene glycol) methacrylate) sol – gels. Acta Biomaterialia 6: 1307-1318. http://doi.org/10.1016/j. actbio.2009.11.027.

Pu, X., Wei, K. & Zhang, Q. 2013. In situ forming chitosan /hydroxyapatite rods reinforced via genipin crosslinking. Materials Letters 94: 169-171. http://doi.org/10.1016/j. matlet.2012.12.009.

Riva, R., Ragelle, H., Rieux, des A., Duhem, N., Jerome, C. & Preat, V. 2011. Chitosan and chitosan derivatives in drug delivery and tissue engineering. Advance Polymer Science 244: 19-44. http://doi.org/10.1007/12.

Shameli, K., Ahmad, M.B., Zamanian, A., Sangpour, P., Shabanzadeh, P., Abdollahi, Y. & Zargar, M. 2012. Green biosynthesis of silver nanoparticles using Curcuma longa tuber powder. International Journal of Nanomedicine 7: 5603-5610. http://doi.org/10.2147/IJN.S36786.

Simões, S., Figureueiras, A. & Veiga, F. 2012. Modular hydrogels for drug delivery. Journal of Biomaterials and Nanobiotechnology 3: 185-199.

Singh, B. & Pal, L. 2011. Radiation crosslinking polymerization of sterculia polysaccharide – PVA – PVP for making hydrogel wound dressings. International Journal of Biological Macromolecules 48: 501-510. http://doi.org/10.1016/j. ijbiomac.2011.01.013.

Sivaiah, K., Kumar, K.N., Naresh, V. & Buddhudu, S. 2011. Structural and optical properties of Li+: PVP & Ag+: PVP polymer films. Materials Sciences and Applications 2: 1688-1696. http://doi.org/10.4236/msa.2011.211225.

Soler, D.M., Rodriguez, Y., Correa, H., Moreno, A. & Carrizales, L. 2012. Pilot scale-up and shelf stability of hydrogel wound dressings obtained by gamma radiation. Radiation Physics and Chemistry 81: 1249-1253. http://doi.org/10.1016/j. radphyschem.2012.02.024.

Tahtat, D., Mahlous, M., Benamer, S., Khodja, A.N. & Youcef, S.L. 2012. Effect of molecular weight on radiation chemical degradation yield of chain scission of γ -irradiated chitosan in solid state and in aqueous solution. Radiation Physics and Chemistry 81: 659-665. http://doi.org/10.1016/j. radphyschem.2012.02.036.

Tanuma, H., Saito, T., Nishikawa, K., Dong, T., Yazawa, K. & Inoue, Y. 2010. Preparation and characterization of PEG-crosslinked chitosan hydrogel films with controllable swelling and enzymatic degradation behavior. Carbohydrate Polymers 80: 260-265. http://doi.org/10.1016/j.carbpol.2009.11.022.

Yang, C., Xu, L., Zhou, Y., Zhang, X., Huang, X. & Wang, M. 2010. A green fabrication approach of gelatin/CM-chitosan hybrid hydrogel for wound healing. Carbohydrate Polymers 82: 1297-1305. http://doi.org/10.1016/j.carbpol.2010.07.013.

Yuan, Y., Chesnutt, B.M., Utturkar, G., Haggard, W.O., Yang, Y., Ong, J.L. & Bumgardner, J.D. 2007. The effect of crosslinking of chitosan microspheres with genipin on protein release. Carbohydrate Polymers 68: 561-567. http://doi.org/10.1016/j.carbpol.2006.10.023.

Zhang, D., Zhou, W., Wei, B., Wang, X., Tang, R., Nie, J. & Wang, J. 2015a. Carboxyl-modified poly (vinyl alcohol)-crosslinked chitosan hydrogel films for potential wound dressing. Carbohydrate Polymers 125: 189-199. http://doi. org/10.1016/j.carbpol.2015.02.034.

Zhang, J., Han, J., Zhang, X., Jiang, J., Xu, M. & Zhang, D. 2015b. Polymeric nanoparticles based on chitooligosaccharide as drug carriers for co-delivery of all- trans -retinoic acid and paclitaxel. Carbohydrate Polymers 129: 25-34. shttp://doi. org/10.1016/j.carbpol.2015.04.036.

Zhao, L., Xu, L., Mitomo, H. & Yoshii, F. 2006. Synthesis of pH-sensitive PVP / CM-chitosan hydrogels with improved surface property by irradiation. Carbohydrate Polymers 64: 473-480. http://doi.org/10.1016/j.carbpol.2005.12.014.

*Corresponding author; email: maznah@nuclearmalaysia.gov.my