Abstract
This research describes the swelling behavior of cellulose nanocrystal-graft-polyacrylic acid/polyvinyl alcohol (CNC-g-PAA/PVA) hydrogels produced via a semi-interpenetrating network (semi-IPN) approach. To improve the dispersion of cellulose nanocrystals (CNCs) in the hydrogel system, the CNCs were embedded into the PAA polymer structure via grafting with AA monomers and polymerization processes. The produced CNC-g-PAA was further developed into a semi-IPN system with polyvinyl alcohol (PVA) to study the effect of CNC content on the water absorption and retention properties. The physical and chemical properties of the semi-IPN hydrogels were characterized using Fourier transform infrared spectroscopy (FTIR), field emission scanning electron microscopy (FESEM), thermogravimetric analysis (TGA), and rheometer. The data revealed that an increased CNC content significantly improved the swelling ratio and swelling kinetics of the hydrogels at room temperature. Moreover, a higher pH and temperature also enhanced the swelling performance of the hydrogels. These improvements demonstrate the potential utility of CNC-g-PAA/PVA hydrogels in agricultural and horticultural applications.
This is a preview of subscription content, log in via an institution to check access.
Similar content being viewed by others
Data availability
Not applicable.
References
Ahmed EM (2015) Hydrogel: Preparation, characterization, and applications: a review. J Adv Res 6(2):105–121. https://doi.org/10.1016/j.jare.2013.07.006
Auad ML, Contos VS, Nutt S, Aranguren MI, Marcovich NE (2008) Characterization of nanocellulose- reinforced shape memory polyurethanes. Polym Int 57(4):651–659. https://doi.org/10.1002/pi.2394
Bai H, Li Z, Zhang S, Wang W, Dong W (2018) Interpenetrating polymer networks in polyvinyl alcohol/cellulose nanocrystals hydrogels to develop absorbent materials. Carbohyd Polym 200:468–476. https://doi.org/10.1016/j.carbpol.2018.08.041
Bao Y, Ma J, Li N (2011) Synthesis and swelling behaviors of sodium carboxymethyl cellulose-g-poly(AA-co-AM-co-AMPS)/MMT superabsorbent hydrogel. Carbohyd Polym 84(1):76–82. https://doi.org/10.1016/j.carbpol.2010.10.061
Chen Q, Zhu L, Zhao C, Wang Q, Zheng J (2013) A robust, one-pot synthesis of highly mechanical and recoverable double network hydrogels using thermoreversible sol-gel polysaccharide. Adv Mater 25(30):4171–4176. https://doi.org/10.1002/adma.201300817
Dragan ES (2014) Design and applications of interpenetrating polymer network hydrogels. A review. Chem Eng J 243:572–590. https://doi.org/10.1016/j.cej.2014.01.065
Elliott JE, Macdonald M, Nie J, Bowman CN (2004) Structure and swelling of poly(acrylic acid) hydrogels: Effect of pH, ionic strength, and dilution on the crosslinked polymer structure. Polymer 45(5):1503–1510. https://doi.org/10.1016/j.polymer.2003.12.040
Erizal E, Abbas B, Sukaryo SG, Barleany DR (2015) Synthesis and characterization superabsorbent hydrogels of partially neutralized acrylic acid prepared using gamma irradiation: swelling and thermal behavior. Indones J Chem 15(3):281–281. https://doi.org/10.22146/ijc.21197
Essawy HA, Ghazy MB, El-Hai FA, Mohamed MF (2016) Superabsorbent hydrogels via graft polymerization of acrylic acid from chitosan-cellulose hybrid and their potential in controlled release of soil nutrients. Int J Biol Macromol 89:144–151. https://doi.org/10.1016/j.ijbiomac.2016.04.071
Haraguchi K, Li HJ (2006) Mechanical properties and structure of polymer – clay nanocomposite gels with high clay content. Macromolecules 39(5):1898–1905. https://doi.org/10.1021/ma052468y
Jayaramudu T, Raghavendra GM, Varaprasad K, Sadiku R, Raju KM (2013) Development of novel biodegradable au nanocomposite hydrogels based on wheat: for inactivation of bacteria. Carbohyd Polym 92:2193–2200. https://doi.org/10.1016/j.carbpol.2012.12.006
Jayaramudu T, Ko HU, Kim HC, Kim JW, Muthoka RM, Kim J (2018) Electroactive hydrogels made with polyvinyl alcohol/cellulose nanocrystals. Materials 11(9):1615. https://doi.org/10.3390/ma11091615
Jayaramudu T, Ko HU, Kim HC, Kim JW, Kim J (2019) Swelling behavior of polyacrylamide–cellulose nanocrystal hydrogels: swelling kinetics, temperature, and pH effects. Materials 12(13):2080. https://doi.org/10.3390/ma12132080
Kong W, Li Q, Li X, Su Y, Yue Q, Gao B (2019) A biodegradable biomass-based polymeric composite for slow release and water retention. J Environ Manage 230:190–198. https://doi.org/10.1016/j.jenvman.2018.09.086
Li X, Li Q, Su Y, Yue Q, Gao B, Su Y (2015) A novel wheat straw cellulose-based semi-IPNs superabsorbent with integration of water-retaining and controlled-release fertilizers. J Taiwan Inst Chem E 55:170–179. https://doi.org/10.1016/j.jtice.2015.04.022
Li X, Li Q, Xu X, Su Y, Yue Q, Gao B (2016) Characterization, swelling and slow-release properties of a new controlled release fertilizer based on wheat straw cellulose hydrogel. J Taiwan Inst Chem E 60:564–572. https://doi.org/10.1016/j.jtice.2015.10.027
Loos W, Verbrugghe S, Goethals EJ, Du Prez FE, Bakeeva IV, Zubov VP (2003) Thermo-responsive organic/inorganic hybrid hydrogels based on poly(N-vinylcaprolactam). Macromol Chem Phys 204(1):98–103. https://doi.org/10.1002/macp.200290058
Memic A, Alhadrami HA, Hussain MA, Aldhahri M, Al Nowaiser F, Al-Hazmi F, Oklu R, Khademhosseini A (2016) Hydrogels 2.0: improved properties with nanomaterial composites for biomedical applications. Biomed Mater 11(1):014104. https://doi.org/10.1088/1748-6041/11/1/014104
Moon RJ, Martini A, Nairn J, Simonsen J, Youngblood J (2011) Cellulose nanomaterials review: structure, properties and nanocomposites. Chem Soc Rev 40(7):3941–3994. https://doi.org/10.1039/C0CS00108B
Oladosu Y, Rafii MY, Arolu F, Chukwu SC, Salisu MA, Fagbohun IK, Muftaudeen TK, Swaray S, Haliru BS (2022) Superabsorbent Polymer hydrogels for sustainable agriculture: a review. Horticulturae 8(7):605. https://doi.org/10.3390/horticulturae8070605
Palanivelu SD, Armir NA, Zulkifli A, Hair AH, Salleh KM, Lindsey K, Che-Othman MH, Zakaria S (2022) Hydrogel application in urban farming: potentials and limitations - a review. Polymers 14(13):2590. https://doi.org/10.3390/polym14132590
Rizwan M, Gilani SR, Durani AI, Naseem S (2021) Materials diversity of hydrogel: synthesis, polymerization process and soil conditioning properties in agricultural field. J Adv Res 33:15–40. https://doi.org/10.1016/j.jare.2021.03.007
Sennakesavan G, Mostakhdemin M, Dkhar LK, Seyfoddin A, Fatihhi SJ (2020) Acrylic acid/acrylamide based hydrogels and its properties - a review. Polym Degrad Stabil 180:109308. https://doi.org/10.1016/j.polymdegradstab.2020.109308
Tanan W, Panichpakdee J, Saengsuwan S (2019) Novel biodegradable hydrogel based on natural polymers: synthesis, characterization, swelling/reswelling and biodegradability. Eur Polym J 112:678–687. https://doi.org/10.1016/j.eurpolymj.2018.10.033
Varaprasad K, Mohan YM, Ravindra S, Reddy NN, Vimala K, Monika K, Sreedhar B, Raju KM (2010) Hydrogel–silver nanoparticle composites: a new generation of antimicrobials. J Appl Polym Sci 115(2):1199–1207. https://doi.org/10.1002/app.31249
Varaprasad K, Raghavendra GM, Jayaramudu T, Yallapu MM, Sadiku R (2017) A mini review on hydrogels classification and recent developments in miscellaneous applications. Mater Sci Eng C 79:958–971. https://doi.org/10.1016/j.msec.2017.05.096
Wan Ishak WH, Yong Jia O, Ahmad I (2020) pH-responsive gamma-irradiated poly(acrylic acid)-cellulose-nanocrystal-reinforced hydrogels. Polymers 12(9):1932. https://doi.org/10.3390/polym12091932
Wang W, Wang A (2010) Synthesis and swelling properties of pH-sensitive semi-IPN superabsorbent hydrogels based on sodium alginate-g-poly(sodium acrylate) and polyvinylpyrrolidone. Carbohyd Polym 80(4):1028–1036. https://doi.org/10.1016/j.carbpol.2010.01.020
Wang W, Yang S, Zhang A, Yang Z (2020) Preparation and properties of novel corn straw cellulose–based superabsorbent with water-retaining and slow-release functions. J Appl Polym Sci 137(32):48951. https://doi.org/10.1002/app.48951
Wang J, Chen H, Ma R, Shao J, Huang S, Liu Y, Jiang Y, Cheng D (2021a) Novel water- and fertilizer-management strategy: nutrient-water carrier. J Clean Prod 291:125961. https://doi.org/10.1016/j.jclepro.2021.125961
Wang W, Yang S, Zhang A, Yang Z (2021b) Synthesis of a slow-release fertilizer composite derived from waste straw that improves water retention and agricultural yield. Sci Total Environ 768:144978. https://doi.org/10.1016/j.scitotenv.2021.144978
Wen P, Wu Z, He Y, Ye BC, Han Y, Wang J, Guan X (2016) Microwave-assisted synthesis of a semi-interpenetrating polymer network slow-release nitrogen fertilizer with water absorbency from cotton stalks. ACS Sustain Chem Eng 4(12):6572–6579. https://doi.org/10.1021/acssuschemeng.6b01466
Wen P, Han Y, Wu Z, He Y, Ye BC, Wang J (2017) Rapid synthesis of a corncob-based semi-interpenetrating polymer network slow-release nitrogen fertilizer by microwave irradiation to control water and nutrient losses. Arab J Chem 10(7):922–934. https://doi.org/10.1016/j.arabjc.2017.03.002
Wohlhauser S, Delepierre G, Labet M, Morandi G, Thielemans W, Weder C, Zoppe JO (2018) Grafting polymers from cellulose nanocrystals: synthesis, properties, and applications. Macromolecules 51(16):6157–6189. https://doi.org/10.1021/acs.macromol.8b00733
Yang J, Han CR, Duan JF, Xu F, Sun RC (2013) Mechanical and viscoelastic properties of cellulose nanocrystals reinforced poly(ethylene glycol) nanocomposite hydrogels. ACS Appl Mater Inter 5(8):3199–3207. https://doi.org/10.1021/am4001997
Yang W, Xu F, Ma X, Guo J, Li C, Shen S, Puglia D, Chen J, Xu P, Kenny J, Ma P (2021) Highly-toughened PVA/nanocellulose hydrogels with anti-oxidative and antibacterial properties triggered by lignin-Ag nanoparticles. Mater Sci Eng C 129:112385. https://doi.org/10.1016/j.msec.2021.112385
Yin OS, Ahmad I, Amin M (2015) Effect of cellulose nanocrystals content and pH on swelling behaviour of gelatin based hydrogel. Sains Malays 44(6):793–799
Zaharia A, Radu AL, Iancu S, Florea AM, Sandu T, Minca I, Fruth-Oprisan V, Teodorescu M, Sarbu A, Iordache TV (2018) Bacterial cellulose-poly (acrylic acid-co-N, N′-methylene-bis-acrylamide) interpenetrated networks for the controlled release of fertilizers. RSC Adv 8(32):17635–17644. https://doi.org/10.1039/C8RA01733F
Zainul Armir NA, Zulkifli A, Gunaseelan S, Palanivelu SD, Salleh KM, Che Othman MH, Zakaria S (2021) Regenerated cellulose products for agricultural and their potential: a review. Polymers 13:3586. https://doi.org/10.3390/polym13203586
Zainul Armir NA, Mohd Salleh K, Zulkifli A, Zakaria S (2022) pH-responsive ampholytic regenerated cellulose hydrogel integrated with carrageenan and chitosan. Ind Crop Prod 178:114588. https://doi.org/10.1016/j.indcrop.2022.114588
Zhang X, Liu Y, Lu P, Zhang M (2020) Preparation and properties of hydrogel based on sawdust cellulose for environmentally friendly slow release fertilizers. Green Process Synth 9(1):139–152. https://doi.org/10.1515/gps-2020-0015
Zhou T, Wang Y, Huang S, Zhao Y (2018) Synthesis composite hydrogels from inorganic-organic hybrids based on leftover rice for environment-friendly controlled-release urea fertilizers. Sci Total Environ 615:422–430. https://doi.org/10.1016/j.scitotenv.2017.09.084
Zhu B, Ma D, Wang J, Zhang S (2015) Structure and properties of semi-interpenetrating network hydrogel based on starch. Carbohyd Polym 133:448–455. https://doi.org/10.1016/j.carbpol.2015.07.037
Acknowledgments
The authors would like to thank the Ministry of Higher Education Malaysia for the project funding given (LRGS/1/2019/UKM-UKM/5/1).
Authors’ information (optional).
Not applicable.
Funding
This work was supported by the Ministry of Higher Education Malaysia (project grant number LRGS/1/2019/UKM-UKM/5/1).
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design. Material preparation was performed by NHH and KSL. Data collection and analysis were performed by NHH, KSL, NFJ, and NAG. The first draft of the manuscript was written by NHH and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
Corresponding author
Ethics declarations
Ethics approval and consent to participate
Not applicable.
Consent for publication
The authors agreed with the content, and all gave explicit consent to submit and publish the results presented in the article.
Competing interests
The authors declare no competing interests.
Additional information
Publisher’s Note
Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Halim, N.H., Lau, K.S., Jafri, N.F. et al. Cellulose nanocrystal-graft-polyacrylic acid /polyvinyl alcohol hydrogels: physicochemical properties and swelling behavior. Cellulose (2024). https://doi.org/10.1007/s10570-024-05968-9
Received:
Accepted:
Published:
DOI: https://doi.org/10.1007/s10570-024-05968-9