Abstract
Pectin (Pec) and mucin (Muc) were incorporated into a pure cellulose hydrogel network prepared in a urea/NaOH solvent system and cross-linked with epichlorohydrin to create cellulose-based superabsorbent hydrogels. Hydrogels were also tested for pH-responsive swelling capacity and in vitro drug release behavior. It was observed that swelling ratios increased several folds for the Pec/Muc-modified hydrogels compared to pure cellulose hydrogel and the maximum swelling ratio was 2781% at pH 10 for Pec-modified hydrogel. Besides, different drug release profiles were observed in different pH mediums, where a highly swollen and less eroded matrix showed a slower release due to a larger diffusion path. The incremented swelling ratio of modified hydrogels was attributed to numerous functional groups present on the backbone of the polymers, which aided in forming excessive hydrogen bonds with water. Structural characterization and possible interactions among cellulose and incorporated materials inside the hydrogels were confirmed by attenuated total reflection Fourier transform infrared spectroscopy, field emission scanning electron microscope, and simultaneous thermal analysis. Moreover, the mechanical properties of the Pec and Muc incorporated hydrogels were significantly improved. Owing to the tunable pH-sensitive water absorption, drug release behavior, and improved mechanical properties, Pec/Muc-modified cellulose hydrogels present a wide range of possibilities for further expansion in controlled drug delivery systems and other biomedical applications.
Graphical abstract
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
References
Abdulhameed A, Mbuvi HM, Changamu EO (2020) Synthesis of cellulose-based superabsorbent hydrogel from rice husk using a microwave. Am J Mater Sci 10:1–8. https://doi.org/10.5923/j.materials.20201001.01
Adrian G, Mihai M, Vodnar DC (2019) The use of chitosan, alginate, and pectin in the biomedical and food sector-biocompatibility, bioadhesiveness, and biodegradability. Polymers 11:1837. https://doi.org/10.3390/polym11111837
Alam MN, Christopher LP (2018) Natural cellulose-chitosan cross-linked superabsorbent hydrogels with superior swelling properties. ACS Sustain Chem Eng 6:8736–8742. https://doi.org/10.1021/acssuschemeng.8b01062
Anagha B, George D, Maheswari PU, Begum KMMS (2019) Biomass derived antimicrobial hybrid cellulose hydrogel with green ZnO nanoparticles for curcumin delivery and its kinetic modelling. J Polym Environ 27:2054–2067. https://doi.org/10.1007/s10924-019-01495-y
Ashfaq M, Khan S, Verma N (2014) Synthesis of PVA-CAP-based biomaterial in situ dispersed with Cu nanoparticles and carbon micro-nanofibers for antibiotic drug delivery applications. Biochem Eng J 90:79–89. https://doi.org/10.1016/j.bej.2014.05.016
Bachmann B, Spitz S, Schädl B, Teuschl AH, Redl H, Nürnberger S, Ertl P (2020) Stiffness matters: fine-tuned hydrogel elasticity alters chondrogenic redifferentiation. Front Bioeng Biotechnol 8:373. https://doi.org/10.3389/fbioe.2020.00373
Baishya H, Gouda R, Qing Z (2017) Application of mathematical models in drug release kinetics of carbidopa and levodopa ER tablets. J Dev Drugs 6:1–8. https://doi.org/10.4172/2329-6631.1000171
Bansil R, Turner BS (2006) Mucin structure, aggregation, physiological functions, and biomedical applications. Curr Opin Colloid Interface Sci 11:164–170. https://doi.org/10.1016/j.cocis.2005.11.001
Bansil R, Stanley E, LaMont JT (1995) Mucin biophysics. Annu Rev Physiol 57:635–657. https://doi.org/10.1146/annurev.ph.57.030195.003223
Builders PF, Kunle OO, Okpaku LC, Builders MI, Attama AA, Adikwu MU (2008) Preparation and evaluation of mucinated sodium alginate microparticles for oral delivery of insulin. Eur J Pharm Biopharm 70:777–783. https://doi.org/10.1016/j.ejpb.2008.06.021
Caccavo D, Cascone S, Lamberti G, Barba AA, Larsson A (2016) Swellable hydrogel-based systems for controlled drug delivery. Smart Drug Deliv Syst 10:237–303. https://doi.org/10.5772/61792
Chen EYT, Wang YC, Chen CS, Chin WC (2010) Functionalized positive nanoparticles reduce mucin swelling and dispersion. PLoS One 5:e15434. https://doi.org/10.1371/journal.pone.0015434
Chen W, Yuan S, Shen J, Chen Y, Xiao Y (2021) A composite hydrogel based on pectin/cellulose via chemical cross-linking for hemorrhage. Front Bioeng Biotechnol 8:1582. https://doi.org/10.3389/fbioe.2020.627351
Cheng Y, Lu J, Liu S, Zhao P, Lu G, Chen J (2014) The preparation, characterization, and evaluation of regenerated cellulose/collagen composite hydrogel films. Carbohydr Polym 107:57–64. https://doi.org/10.1016/j.carbpol.2014.02.034
Dafe A, Etemadi H, Dilmaghani A, Mahdavinia GR (2017) Investigation of pectin/starch hydrogel as a carrier for oral delivery of probiotic bacteria. Int J Biol Macromol 97:536–543. https://doi.org/10.1016/j.ijbiomac.2017.01.060
Deka C, Deka D, Bora MM, Jha DK, Kakati DK (2018) Investigation of pH-sensitive swelling and curcumin release behavior of chitglc hydrogel. J Polym Environ 26:4034–4045. https://doi.org/10.1007/s10924-018-1272-x
Duffy CV, David L, Crouzier T (2015) Covalently-crosslinked mucin biopolymer hydrogels for sustained drug delivery. Acta Biomater 20:51–59. https://doi.org/10.1016/j.actbio.2015.03.024
El-Hag AA, AlArifi A (2009) Characterization and in vitro evaluation of starch based hydrogels as carriers for colon specific drug delivery systems. Carbohydr Polym 78:725–730. https://doi.org/10.1016/j.carbpol.2009.06.009
Fu Y, Kao WJ (2010) Drug release kinetics and transport mechanisms of non-degradable and degradable polymeric delivery systems. Expert Opin Drug Deliv 7:429–444. https://doi.org/10.1517/17425241003602259
Fu LH, Qi C, Ma MG, Wan P (2019) Multifunctional cellulose-based hydrogels for biomedical applications. J Mater Chem B 7:1541–1562. https://doi.org/10.1039/c8tb02331j
Ghorbani M, Roshangar L, Soleimani Rad J (2020) Development of reinforced chitosan/pectin scaffold by using the cellulose nanocrystals as nanofillers: an injectable hydrogel for tissue engineering. Eur Polym J 130:109697. https://doi.org/10.1016/j.eurpolymj.2020.109697
Gnanasambandam R, Proctor A (2000) Determination of pectin degree of esterification by diffuse reflectance Fourier transform infrared spectroscopy. Food Chem 68:327–332. https://doi.org/10.1016/S0308-8146(99)00191-0
Gunathilake GTMSU, Ching YC, Chuah CH (2017) Enhancement of curcumin bioavailability using nanocellulose reinforced chitosan hydrogel. Polymers 9:64. https://doi.org/10.3390/polym9020064
He M, Chen H, Zhang X, Wang C, Xu C, Xue Y, Wang J, Zhou P, Zhao Q (2018) Construction of novel cellulose/chitosan composite hydrogels and films and their applications. Cellulose 25:1987–1996. https://doi.org/10.1007/s10570-018-1683-9
Hirakawa B (2005) Epichlorohydrin. In: Encyclopedia of toxicology, 2nd edn, pp 228–229. https://doi.org/10.1016/B0-12-369400-0/00377-X
Huber T, Feast S, Dimartino S, Cen W, Fee C (2019) Analysis of the effect of processing conditions on physical properties of thermally set cellulose hydrogels. Materials 12:1–20. https://doi.org/10.3390/ma12071066
Isobe N, Komamiya T, Kimura S, Kim UJ, Wada M (2018) Cellulose hydrogel with tunable shape and mechanical properties: from rigid cylinder to soft scaffold. Int J Biol Macromol 117:625–631. https://doi.org/10.1016/j.ijbiomac.2018.05.071
Kharat M, Du Z, Zhang G, McClements DJ (2017) Physical and chemical stability of curcumin in aqueous solutions and emulsions: impact of pH, temperature, and molecular environment. J Agric Food Chem 65:1525–1532. https://doi.org/10.1021/acs.jafc.6b04815
Kowalski G, Kijowska K, Witczak M, Kuterasiński L, Lukasiewicz M (2019) Synthesis and effect of structure on swelling properties of hydrogels based on high methylated pectin and acrylic polymers. Polymers 11:1–16. https://doi.org/10.3390/polym11010114
Koyano T, Koshizaki N, Umehara H, Nagura M, Minoura N (2000) Surface states of PVA/chitosan blended hydrogels. Polymer 41:4461–4465. https://doi.org/10.1016/S0032-3861(99)00675-8
Kumar BA, Nayak RR (2019) Supramolecular phenoxy-alkyl maleate-based hydrogels and their enzyme/pH-responsive curcumin release. New J Chem 43:5559–5567. https://doi.org/10.1039/C8NJ05796F
Laurén P, Somersalo P, Pitkänen I, Lou YR, Urtti A, Partanen J, Seppälä J, Madetoja M, Laaksonen T, Mäkitie A, Yliperttula M (2017) Nanofibrillar cellulose-alginate hydrogel coated surgical sutures as cell-carrier systems. PLoS One 12:e0183487. https://doi.org/10.1371/journal.pone.0183487
Li DQ, Wang SY, Meng YJ, Guo ZW, Cheng MM, Li J (2021) Fabrication of self-healing pectin/chitosan hybrid hydrogel via diels-alder reactions for drug delivery with high swelling property, pH-responsiveness, and cytocompatibility. Carbohydr Polym 268:118244. https://doi.org/10.1016/j.carbpol.2021.118244
Liu LS, Kost J, Yan F, Spiro RC (2012) Hydrogels from biopolymer hybrid for biomedical, food, and functional food applications. Polymers 4:997–1011. https://doi.org/10.3390/polym4020997
Mahmud M, Zaman S, Perveen A, Jahan RA, Islam F, Arafat MT (2019) Controlled release of curcumin from electrospun fiber mats with antibacterial activity. J Drug Deliv Sci Technol 55:101386. https://doi.org/10.1016/j.jddst.2019.101386
Menchicchi B, Fuenzalida JP, Hensel A, Swamy MJ, David L, Rochas C, Goycoolea FM (2015) Biophysical analysis of the molecular interactions between polysaccharides and mucin. Biomacromol 16:924–935. https://doi.org/10.1021/bm501832y
Navarra MA, Dal Bosco C, Moreno JS, Vitucci FM, Paolone A, Panero S (2015) Synthesis and characterization of cellulose-based hydrogels to be used as gel electrolytes. Membranes 5:810–823. https://doi.org/10.3390/membranes5040810
Pandey M, Amin MCIM, Ahmad N, Abeer MM (2013) Rapid synthesis of superabsorbent smart-swelling bacterial cellulose/acrylamide-based hydrogels for drug delivery. Int J Polym Sci. https://doi.org/10.1155/2013/905471
Patel MM, Smart JD, Nevell TG, Ewen RJ, Eaton PJ, Tsibouklis J (2003) Mucin/poly(acrylic acid) interactions: a spectroscopic investigation of mucoadhesion. Biomacromol 4:1184–1190. https://doi.org/10.1021/bm034028p
Pei Y, Yang J, Liu P, Xu M, Zhang X, Zhang L (2013) Fabrication, properties and bioapplications of cellulose/collagen hydrolysate composite films. Carbohydr Polym 92:1752–1760. https://doi.org/10.1016/j.carbpol.2012.11.029
Petrou G, Crouzier T (2018) Mucins as multifunctional building blocks of biomaterials. Biomater Sci 6:2282–2297. https://doi.org/10.1039/c8bm00471d
Ranganathan N, Joseph Bensingh R, Abdul Kader M, Nayak SK (2019) Synthesis and properties of hydrogels prepared by various polymerization reaction systems. In: Mondal M (ed) Cellulose-based superabsorbent hydrogels. Polymers and polymeric composites: a reference series. Springer, Cham
Raschip IE, Fifere N, Varganici CD, Dinu MV (2020) Development of antioxidant and antimicrobial xanthan-based cryogels with tuned porous morphology and controlled swelling features. Int J Biol Macromol 156:608–620. https://doi.org/10.1016/j.ijbiomac.2020.04.086
Roy DS, Rohera BD (2002) Comparative evaluation of rate of hydration and matrix erosion of HEC and HPC and study of drug release from their matrices. Eur J Pharm Sci 16:193–199. https://doi.org/10.1016/S0928-0987(02)00103-3
Spiridon I, Anghel N, Dinu MV, Vlad S, Bele A, Ciubotaru BI, Verestiuc L, Pamfil D (2020) Development and performance of bioactive compounds-loaded cellulose/collagen/ polyurethane materials. Polymers 12:1191. https://doi.org/10.3390/POLYM12051191
Sriamornsak P, Thirawong N, Weerapol Y, Nunthanid J, Sungthongjeen S (2007) Swelling and erosion of pectin matrix tablets and their impact on drug release behavior. Eur J Pharm Biopharm 67:211–219. https://doi.org/10.1016/j.ejpb.2006.12.014
Svensson O, Arnebrant T (2010) Mucin layers and multilayers: physicochemical properties and applications. Curr Opin Colloid Interface Sci 15:395–405. https://doi.org/10.1016/j.cocis.2010.05.015
Wach RA, Mitomo H, Yoshii F, Kume T (2002) Hydrogel of radiation-induced cross-linked hydroxypropylcellulose. Macromol Mater Eng 287:285–295. https://doi.org/10.1002/1439-2054(20020401)287:4%3c285::AID-MAME285%3e3.0.CO;2-3
Yadollahi M, Gholamali I, Namazi H, Aghazadeh M (2015) Synthesis and characterization of antibacterial carboxymethyl cellulose/ZnO nanocomposite hydrogels. Int J Biol Macromol 74:136–141. https://doi.org/10.1016/j.ijbiomac.2014.11.032
Yang F, He W, Li H, Zhang X, Feng Y (2019a) Role of acid treatment combined with the use of urea in forming cellulose hydrogel. Carbohydr Polym 223:115059. https://doi.org/10.1016/j.carbpol.2019.115059
Zhang X, Morits M, Jonkergouw C, Ora A, Delgado JJV, Farooq M, Ajdary R, Huan S, Linder M, Rojas O, Sipponen MH, Österberg M (2020) Three-dimensional printed cell culture model based on spherical colloidal lignin particles and cellulose nanofibril-alginate hydrogel. Biomacromol 21:1875–1885. https://doi.org/10.1021/acs.biomac.9b01745
Zhao Y, He M, Zhao L, Wang S, Li Y, Gan L, Li M, Xu L, Chang PR, Anderson DP, Chen Y (2016) Epichlorohydrin-cross-linked hydroxyethyl cellulose/soy protein isolate composite films as biocompatible and biodegradable implants for tissue engineering. ACS Appl Mater Interfaces 8:2781–2795. https://doi.org/10.1021/acsami.5b11152
Zhou J, Chang C, Zhang R, Zhang L (2007) Hydrogels prepared from unsubstituted cellulose in NaOH/urea aqueous solution. Macromol Biosci 7:804–809. https://doi.org/10.1002/mabi.200700007
Zykwinska AW, Ralet MCJ, Garnier CD, Thibault JFJ (2005) Evidence for in vitro binding of pectin side chains to cellulose. Plant Physiol 139:397–407. https://doi.org/10.1104/pp.105.065912
Acknowledgments
The research project was funded by the Bangladesh University of Engineering and Technology (BUET) under Grant No: DAERS/CASR/R-1/2020/DR-330(53).
Author information
Authors and Affiliations
Corresponding author
Ethics declarations
Conflict of interest
The authors declare no potential conflicts of interest relevant to the authorship, research, and publication of this article.
Consent to participate
All authors participated in this research.
Consent to publish
All authors have given their permission for this manuscript to be published.
Additional information
Publisher's Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
About this article
Cite this article
Islam, F., Wong, S.Y., Li, X. et al. Pectin and mucin modified cellulose-based superabsorbent hydrogel for controlled curcumin release. Cellulose 29, 5207–5222 (2022). https://doi.org/10.1007/s10570-022-04600-y
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-022-04600-y