Abstract
In this study, Gum Arabic Aldehyde (GAA) and polyvinyl alcohol (PVA) were used to develop pH-sensitive and self-healable hydrogels. The PVA and GAA based hydrogels have the advantages of non-toxicity, water-solubility, eco-friendly, biodegradability, and pH sensitivity. However, poor stiffness, low mechanical strength, and hydrophilicity limit their applications. Graphene oxide (GO), gelatin, and boric acid were used to improve the limitations of GAA/PVA hydrogels through cross-linking, Schiff-base reaction between aldehyde groups of GAA and amino groups of gelatin, and hydrogen bonding between PVA chains and boric acid. The prepared hydrogels demonstrated high mechanical properties, good self-healing properties, and pH sensitivity, which facilitate their application as favorable biomaterials for drug delivery. The swelling behavior, degradation, mechanical properties, and rheological behaviors were studied for hydrogels. The hydrogels demonstrated well mechanical properties and well pH sensitivity during controlled release investigation of rivastigmine (RIV) drug under intestinal (~ 83% at pH 7.4) media. Incorporating GO in the hydrogel network, enhanced the mechanical properties, self-healing properties, drug entrapment efficiency, and ensure the controlled release of the entrapped drug. The self-healing properties, swelling behavior, degradation, tensile and compressive tests, rheological behaviors, and in vitro drug release behavior were studied to monitor the effect of GO on the hydrogel properties. Our results illustrated that the self-healing nanocomposite hydrogel was expected to be a platform for drug delivery in pH 7.4.
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Rahmani Z, Ghaemy M, Olad A (2021) Preparation of nanogels based on kappa-carrageenan/chitosan and N-doped carbon dots: study of drug delivery behavior. Polym Bull 78(5):2709–2726
Sarker B, Papageorgiou DG, Silva R, Zehnder T, Gul-E-Noor F, Bertmer M, Kaschta J, Chrissafis K, Detsch R, Boccaccini AR (2014) Fabrication of alginate–gelatin crosslinked hydrogel microcapsules and evaluation of the microstructure and physico-chemical properties. J Mater Chem B 2(11):1470–1482
Olad A, Gharekhani H, Mirmohseni A, Bybordi A (2017) Synthesis, characterization, and fertilizer release study of the salt and pH-sensitive NaAlg-g-poly (AA-co-AAm)/RHA superabsorbent nanocomposite. Polym Bull 74(8):3353–3377
Olad A, Eslamzadeh M, Katiraee F, Mirmohseni A (2020) Evaluation of in vitro anti-fungal properties of allicin loaded ion cross-linked poly (AA-co-AAm)/PVA/Cloisite 15A Nanocomposite hydrogel films as wound dressing materials. J Polym Res 27(4):1–10
Mahdavinia GR, Rahmani Z, Karami S, Pourjavadi A (2014) Magnetic/pH-sensitive κ-carrageenan/sodium alginate hydrogel nanocomposite beads: preparation, swelling behavior, and drug delivery. J Biomater Sci Polym Ed 25(17):1891–1906
Yu L, Ding J (2008) Injectable hydrogels as unique biomedical materials. Chem Soc Rev 37(8):1473–1481
McKay CS, Finn M (2014) Click chemistry in complex mixtures: bioorthogonal bioconjugation. Chem Biol 21(9):1075–1101
Trask R, Williams H, Bond I (2007) Self-healing polymer composites: mimicking nature to enhance performance. Bioinspir Biomim 2(1):1–9
Liu S, Kang M, Li K, Yao F, Oderinde O, Fu G, Xu L (2018) Polysaccharide-templated preparation of mechanically-tough, conductive and self-healing hydrogels. Chem Eng Sci 334:2222–2230
Wang Y, Adokoh CK, Narain R (2018) Recent development and biomedical applications of self-healing hydrogels. Expert Opin Drug Deliv 15(1):77–91
Rashidzadeh A, Olad A, Hejazi MJ (2017) Controlled release systems based on intercalated paraquat onto montmorillonite and clinoptilolite clays encapsulated with sodium alginate. Adv Polym Technol 36(2):177–185
Posocco B, Dreussi E, De Santa J, Toffoli G, Abrami M, Musiani F, Grassi M, Farra R, Tonon F, Grassi G (2015) Polysaccharides for the delivery of antitumor drugs. Materials 8(5):2569–2615
Zohuriaan-Mehr MJ, Motazedi Z, Kabiri K, Ershad-Langroudi A (2005) New super-absorbing hydrogel hybrids from Gum Arabic and acrylic monomers. J Macromol Sci Part A 42(12):1655–1666
Mittal H, Maity A, Ray SS (2015) Gum ghatti and poly (acrylamide-co-acrylic acid) based biodegradable hydrogel-evaluation of the flocculation and adsorption properties. Polym Degrad Stab 120:42–52
Dai L, Zhang L, Wang B, Yang B, Khan I, Khan A, Ni Y (2017) Multifunctional self-assembling hydrogel from guar gum. Chem Eng Sci 330:1044–1051
Chang M, Liu X, Meng L, Wang X, Ren J (2018) Xylan-based hydrogels as a potential carrier for drug delivery: effect of pore-forming agents. Pharmaceutics 10(4):261
Shariatinia Z, Jalali AM (2018) Chitosan-based hydrogels: preparation, properties and applications. Int J Biol Macromol 115:194–220
Rahmani Z, Sahraei R, Ghaemy M (2018) Preparation of spherical porous hydrogel beads based on ion-crosslinked gum tragacanth and graphene oxide: study of drug delivery behavior. Carbohydr Polym 194:34–42
Mahdavinia GR, Rahmani Z, Mosallanezhad A, Karami S, Shahriari M (2016) Effect of magnetic laponite RD on swelling and dye adsorption behaviors of κ-carrageenan-based nanocomposite hydrogels. Desalin Water Treat 57(43):20582–20596
Xu Z, Li Z, Jiang S, Bratlie KM (2018) Chemically modified gellan gum hydrogels with tunable properties for use as tissue engineering scaffolds. ACS Omega 3(6):6998–7007
Patel S, Goyal A (2015) Applications of natural polymer Gum Arabic: a review. Int J Food Prop 18(5):986–998
Dave PN, Gor A (2018) Natural polysaccharide-based hydrogels and nanomaterials: recent trends and their applications, Ch. 3 In: Handbook of nanomaterials for industrial applications (ISBN: 9780128133514), Dimensions, pp. 36–66
Mekkawy AI, El-Mokhtar MA, El-Shanawany SM, Ibrahim EH (2016) Silver nanoparticles-loaded hydrogels, a potential treatment for resistant bacterial infection and wound healing: a review. Br J Pharm Res 14(2):1–19
Ramanathan T, Abdala A, Stankovich S, Dikin D, Herrera-Alonso M, Piner R, Adamson D, Schniepp H, Chen X, Ruoff R (2008) Functionalized graphene sheets for polymer nanocomposites. Nat Nanotechnol 3(6):327–331
Wang A, Pu K, Dong B, Liu Y, Zhang L, Zhang Z, Duan W, Zhu Y (2013) Role of surface charge and oxidative stress in cytotoxicity and genotoxicity of graphene oxide towards human lung fibroblast cells. J Appl Toxicol 33(10):1156–1164
Pandit AH, Mazumdar N, Imtiyaz K, Rizvi MMA, Ahmad S (2019) Periodate-modified Gum Arabic cross-linked PVA hydrogels: a promising approach toward photoprotection and sustained delivery of folic acid. ACS Omega 4(14):16026–16036
Afinjuomo F, Fouladian P, Parikh A, Barclay TG, Song Y, Garg S (2019) Preparation and characterization of oxidized inulin hydrogel for controlled drug delivery. Pharmaceutics 11(7):356
Wei J, Du C, Liu H, Chen Y, Yu H, Zhou Z (2016) Preparation and characterization of aldehyde-functionalized cellulosic fibers through periodate oxidization of bamboo pulp. Bioresources 11(4):8386–8395
Ali A, Ganie SA, Mazumdar N (2018) A new study of iodine complexes of oxidized Gum Arabic: an interaction between iodine monochloride and aldehyde groups. Carbohydr Polym 180:337–347
Chen X, Fan M, Tan H, Ren B, Yuan G, Jia Y, Li J, Xiong D, Xing X, Niu X (2019) Magnetic and self-healing chitosan-alginate hydrogel encapsulated gelatin microspheres via covalent cross-linking for drug delivery. Mater Sci Eng C 101:619–629
Al Dalaty A, Karam A, Najlah M, Alany RG, Khoder M (2016) Effect of non-cross-linked calcium on characteristics, swelling behaviour, drug release and mucoadhesiveness of calcium alginate beads. Carbohydr Polym 140:163–170
Lee DH, Arisaka Y, Tonegawa A, Kang TW, Tamura A, Yui N (2019) Cellular orientation on repeatedly stretching gelatin hydrogels with supramolecular cross-linkers. Polymers 11(12):2095
Kumaraswamy S, Babaladimath G, Badalamoole V, Mallaiah SH (2017) Gamma irradiation synthesis and in vitro drug release studies of ZnO/PVA hydrogel nanocomposites. Adv Mater Lett 8(4):546–552
Tiong ACY, Tan IS, Foo HCY, Lam MK, Mahmud HB, Lee KT (2022) Facile asymmetric modification of graphene nanosheets using κ-carrageenan as a green template. J Colloid Interface Sci 607(2):1131–1141
Pagar K, Vavia P (2013) Rivastigmine-loaded l-lactide-depsipeptide polymeric nanoparticles: decisive formulation variable optimization. Sci Pharm 81(3):865–888
Patil S, Babbar A, Mathur R, Mishra A, Sawant K (2010) Mucoadhesive chitosan microspheres of carvedilol for nasal administration. J Dr Targ 18(4):321–331
Reddy P, Eswaramma S, Krishna Rao K, Lee YI (2014) Dual responsive pectin hydrogels and their silver nanocomposites: swelling studies, controlled drug delivery and antimicrobial applications. Bull Korean Chem Soc 35(8):2391–2399
Nath J, Chowdhury A, Dolui SK (2018) Chitosan/graphene oxide-based multifunctional pH-responsive hydrogel with significant mechanical strength, self-healing property, and shape memory effect. Adv Polym Technol 37(8):3665–3679
Mansur HS, Sadahira CM, Souza AN, Mansur AA (2008) FTIR spectroscopy characterization of poly (vinyl alcohol) hydrogel with different hydrolysis degree and chemically crosslinked with glutaraldehyde. Mater Sci Eng C 28(4):539–548
Pan C, Liu L, Chen Q, Zhang Q, Guo G (2017) Tough, stretchable, compressive novel polymer/graphene oxide nanocomposite hydrogels with excellent self-healing performance. ACS Appl Mater Interfaces 9(43):38052–38061
Jing Z, Xian X, Huang Q, Chen Q, Hong P, Li Y, Shi A (2020) Biocompatible double network poly (acrylamide-co-acrylic acid)-Al3+/poly (vinyl alcohol)/graphene oxide nanocomposite hydrogels with excellent mechanical properties, self-recovery and self-healing ability. New J Chem 44:10390–10403
Zhu J, Guo P, Chen D, Xu K, Wang P, Guan S (2018) Fast and excellent healing of hydroxypropyl guar gum/poly (N, N-dimethyl acrylamide) hydrogels. J Polym Sci B Polym Phys 56(3):239–247
Devi VKA, Shyam R, Palaniappan A, Jaiswal AK, Oh T-H, Nathanael AJ (2021) Self-healing hydrogels: preparation, mechanism and advancement in biomedical applications. Polymers 13(21):3782
Pettignano A, Häring M, Bernardi L, Tanchoux N, Quignard F, Díaz DD (2017) Self-healing alginate–gelatin biohydrogels based on dynamic covalent chemistry: elucidation of key parameters. Mater Chem Front 1(1):73–79
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Rahmani, S., Olad, A. & Rahmani, Z. Preparation of self-healable nanocomposite hydrogel based on Gum Arabic/gelatin and graphene oxide: study of drug delivery behavior. Polym. Bull. 80, 4117–4138 (2023). https://doi.org/10.1007/s00289-022-04247-6
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DOI: https://doi.org/10.1007/s00289-022-04247-6