Abstract
Sodium alginate-based hydrogels are particularly attractive because of their special properties such as biocompatibility, biodegradability, renewability, and ion exchange properties, and their mechanical performance can be greatly improved through forming semi-interpenetrating networks. Herein, a pH/temperature-sensitive semi-interpenetrating network hydrogel was fabricated by photopolymerization of N, N-dimethylacrylamide, N-isopropylacrylamide, and N, N'-methylenebisacrylamide in the presence of sodium alginate. The swelling ratio of the hydrogels reached 3263% in distilled water when the molar ratio of monomer to crosslinker was 150:1 and mass concentration of sodium alginate was 2%. The hydrogels were pH/temperature sensitive, and their swelling behavior had good cycling performance. Selective adsorption experiments showed that the hydrogel had good adsorption selectivity for the cationic methylene blue in binary dye systems. The maximum adsorption capacity was 151.79 mg/g with 250 mg/L methylene blue solution, 35 °C and pH = 10. The adsorption behavior could be well described by Langmuir isothermal model and pseudo-second-order kinetic model, suggesting that methylene blue adsorption was monolayer chemisorption. The adsorption capacity was still 75.91% of the initial adsorption capacity after five consecutive adsorption–desorption cycles, revealing that the adsorbent possessed good regeneration capacity. The efficient adsorbent described here was prepared by a facile strategy, so it holds great potential in wastewater treatment.
Similar content being viewed by others
Data availability
All data generated during this study are included in this published article and its supplementary information files.
References
Abasalizadeh F, Moghaddam SV, Alizadeh E et al (2020) Alginate-based hydrogels as drug delivery vehicles in cancer treatment and their applications in wound dressing and 3D bioprinting. J Biol Eng 14:8. https://doi.org/10.1186/s13036-020-0227-7
Adel M, Ahmed MA, Mohamed AA (2020) Effective removal of cationic dyes from aqueous solutions using reduced graphene oxide functionalized with manganese ferrite nanoparticles. Compos Commun 22:100450. https://doi.org/10.1016/j.coco.2020.100450
Ahamad T, Naushad M, Eldesoky GE et al (2019) Effective and fast adsorptive removal of toxic cationic dye (MB) from aqueous medium using amino-functionalized magnetic multiwall carbon nanotubes. J Mol Liq 282:154–161. https://doi.org/10.1016/j.molliq.2019.02.128
Al-Ghouti MA, Da’ana DA (2020) Guidelines for the use and interpretation of adsorption isotherm models: a review. J Hazard Mater 393:122383. https://doi.org/10.1016/j.jhazmat.2020.122383
Al-Shemy MT, Al-Sayed A, Dacrory S (2022) Fabrication of sodium alginate/graphene oxide/nanocrystalline cellulose scaffold for methylene blue adsorption: kinetics and thermodynamics study. Sep Purif Technol 290:120825. https://doi.org/10.1016/j.seppur.2022.120825
Anastopoulos I, Hosseini-Bandegharaei A, Fu J et al (2017) Use of nanoparticles for dye adsorption: review. J Dispersion Sci Technol 39:836–847. https://doi.org/10.1080/01932691.2017.1398661
Bashir S, Hina M, Iqbal J et al (2020) Fundamental concepts of hydrogels: synthesis, properties, and their applications. Polymers (basel) 12:2702. https://doi.org/10.3390/polym12112702
Bhattacharyya R, Ray SK (2015) Adsorption of industrial dyes by semi-IPN hydrogels of Acrylic copolymers and sodium alginate. J Ind Eng Chem 22:92–102. https://doi.org/10.1016/j.jiec.2014.06.029
Cheng Y, Zang J, Zhao X et al (2022) Nanocellulose-enhanced organohydrogel with high-strength, conductivity, and anti-freezing properties for wearable strain sensors. Carbohydr Polym 277:118872. https://doi.org/10.1016/j.carbpol.2021.118872
Dahlan NA, Lee LW, Pushpamalar J et al (2019) Adsorption of methylene blue onto carboxymethyl sago pulp-immobilized sago waste hydrogel beads. Int J Environ Sci Te 16:2047–2058. https://doi.org/10.1007/s13762-018-1789-5
Dariani RS, Esmaeili A, Mortezaali A et al (2016) Photocatalytic reaction and degradation of methylene blue on TiO2 nano-sized particles. Optik 127:7143–7154. https://doi.org/10.1016/j.ijleo.2016.04.026
Ding Y, Tang R, Feng Y et al (2022) Synthesis and characterisation of high resilience collagen-polyacrylamide semi-interpenetrating network hydrogel. Mater Today Commun 32:103955. https://doi.org/10.1016/j.mtcomm.2022.103955
Fan X, Wang X, Cai Y et al (2022) Functionalized cotton charcoal/chitosan biomass-based hydrogel for capturing Pb(2+), Cu(2+) and MB. J Hazard Mater 423:127191. https://doi.org/10.1016/j.jhazmat.2021.127191
Gallastegui A, Spesia MB, dell’Erba IE et al (2019) Controlled release of antibiotics from photopolymerized hydrogels: Kinetics and microbiological studies. Mater Sci Eng C Mater Biol Appl 102:896–905. https://doi.org/10.1016/j.msec.2019.04.027
Gohr MS, Abd-Elhamid AI, El-Shanshory AA et al (2022) Adsorption of cationic dyes onto chemically modified activated carbon: Kinetics and thermodynamic study. J Mol Liq 346:118227. https://doi.org/10.1016/j.molliq.2021.118227
Hasanpour M, Hatami M (2020) Photocatalytic performance of aerogels for organic dyes removal from wastewaters: review study. J Mol Liq 309:113094. https://doi.org/10.1016/j.molliq.2020.113094
Hassan MM, Carr CM (2021) Biomass-derived porous carbonaceous materials and their composites as adsorbents for cationic and anionic dyes: a review. Chemosphere 265:129087. https://doi.org/10.1016/j.chemosphere.2020.129087
Hu X, Cheng W, Nie W et al (2015) Synthesis and characterization of a temperature-sensitive hydrogel based on sodium alginate and N-isopropylacrylamide. Polym Adv Technol 26:1340–1345. https://doi.org/10.1002/pat.3682
Hu S, Zhi Y, Shan S et al (2022) Research progress of smart response composite hydrogels based on nanocellulose. Carbohydr Polym 275:118741. https://doi.org/10.1016/j.carbpol.2021.118741
Huang T, Tu ZC, Wang H et al (2017) Pectin and enzyme complex modified fish scales gelatin: rheological behavior, gel properties and nanostructure. Carbohydr Polym 156:294–302. https://doi.org/10.1016/j.carbpol.2016.09.040
Huang X, Li J, Luo J et al (2021) Research progress on double-network hydrogels. Mater Today Commun 29:102757. https://doi.org/10.1016/j.mtcomm.2021.102757
Jalababu R, Veni SS, Reddy KVNS (2018) Synthesis and characterization of dual responsive sodium alginate-g-acryloyl phenylalanine-poly N -isopropyl acrylamide smart hydrogels for the controlled release of anticancer drug. J Drug Deliv Sci Technol 44:190–204. https://doi.org/10.1016/j.jddst.2017.12.013
Jang JW, Park JH, Kim IJ et al (2020) Preparation and characterization of thermoresponsive poly(N-isopropylacrylamide-co-N-isopropylmethacrylamide) hydrogel materials for smart windows. J Appl Polym Sci 138:49788. https://doi.org/10.1002/app.49788
Jayaramudu T, Varaprasad K, Sadiku ER et al (2019) Temperature-sensitive semi-IPN composite hydrogels for antibacterial applications. Colloids Surf A Physicochem Eng Asp 572:307–316. https://doi.org/10.1016/j.colsurfa.2019.04.012
Jiang M, Niu N, Chen L (2022) A template synthesized strategy on bentonite-doped lignin hydrogel spheres for organic dyes removal. Sep Purif Technol 285:120376. https://doi.org/10.1016/j.seppur.2021.120376
Kailasa SK, Joshi DJ, Kateshiya MR et al (2022) Review on the biomedical and sensing applications of nanomaterial-incorporated hydrogels. Mater Today Chem 23:100746. https://doi.org/10.1016/j.mtchem.2021.100746
Kang S, Zhao Y, Wang W et al (2018) Removal of methylene blue from water with montmorillonite nanosheets/chitosan hydrogels as adsorbent. Appl Surf Sci 448:203–211. https://doi.org/10.1016/j.apsusc.2018.04.037
Kang S, Qin L, Zhao Y et al (2020) Enhanced removal of methyl orange on exfoliated montmorillonite/chitosan gel in presence of methylene blue. Chemosphere 238:124693. https://doi.org/10.1016/j.chemosphere.2019.124693
Kaya-Özkiper K, Uzun A, Soyer-Uzun S (2022) A novel alkali activated magnesium silicate as an effective and mechanically strong adsorbent for methylene blue removal. J Hazard Mater 424:127256. https://doi.org/10.1016/j.jhazmat.2021.127256
Kubra KT, Salman MS, Hasan MN (2021) Enhanced toxic dye removal from wastewater using biodegradable polymeric natural adsorbent. J Mol Liq 328:115468. https://doi.org/10.1016/j.molliq.2021.115468
Li W, Wei H, Liu Y et al (2021) Fabrication of novel starch-based composite hydrogel microspheres combining Diels-Alder reaction with spray drying for MB adsorption. J Environ Chem Eng 9:105929. https://doi.org/10.1016/j.jece.2021.105929
Li IC, Chen YH, Chen YC (2022) Sodium alginate-g-poly(sodium acrylate) hydrogel for the adsorption- desorption of ammonium nitrogen from aqueous solution. J Water Process Eng 49:102999. https://doi.org/10.1016/j.jwpe.2022.102999
Liu Z, Wei H, Liu Y et al (2022) Fabrication and characterization of interpenetrating network hydrogels based on sequential amine-anhydride reaction and photopolymerization in water. Polym Eng Sci 62:917–928. https://doi.org/10.1002/pen.25896
Loffredo E, Carnimeo C, Silletti R et al (2021) Use of the solid by-product of anaerobic digestion of biomass to remove anthropogenic organic pollutants with endocrine disruptive activity. Processes 9:2018. https://doi.org/10.3390/pr9112018
Luo J, Ma X, Zhou X et al (2021) Construction of physically crosslinked cellulose nanofibrils/alkali lignin/montmorillonoite/polyvinyl alcohol network hydrogel and its application in methylene blue removal. Cellulose 28:5531–5543. https://doi.org/10.1007/s10570-021-03847-1
Ma J, Zhang M, Ji M et al (2021) Magnetic graphene oxide-containing chitosan sodium alginate hydrogel beads for highly efficient and sustainable removal of cationic dyes. Int J Biol Macromol 193:2221–2231. https://doi.org/10.1016/j.ijbiomac.2021.11.054
Nicol E (2021) Photopolymerized porous hydrogels. Biomacromol 22:1325–1345. https://doi.org/10.1021/acs.biomac.0c01671
Ortega-Garcia A, Martinez-Bernal BG, Ceja I et al (2022) Drug delivery from stimuli-responsive Poly(N-isopropylacrylamide-co-N-isopropylmethacrylamide)/Chitosan Core/Shell Nanohydrogels. Polymers 14:522. https://doi.org/10.3390/polym14030522
Pashaei-Fakhri S, Peighambardoust SJ, Foroutan R et al (2021) Crystal violet dye sorption over acrylamide/graphene oxide bonded sodium alginate nanocomposite hydrogel. Chemosphere 270:129419. https://doi.org/10.1016/j.chemosphere.2020.129419
Pettignano A, Aguilera DA, Tanchoux N et al (2019) Alginate: a versatile biopolymer for functional advanced materials for catalysis. Stud Surf Sci Catal 178:357–375. https://doi.org/10.1016/B978-0-444-64127-4.00017-3
Qu RJ, Wang Y, Li D et al (2021) Rheological behavior of nanocellulose gels at various calcium chloride concentrations. Carbohydr Polym 274:118660. https://doi.org/10.1016/j.carbpol.2021.118660
Rahmatpour A, Soleimani P, Mirkani A (2022) Eco-friendly poly(vinyl alcohol)/partially hydrolyzed polyacrylamide/graphene oxide semi-IPN nanocomposite hydrogel as a reusable and efficient adsorbent of cationic dye methylene blue from water. React Funct Polym 175:105290. https://doi.org/10.1016/j.reactfunctpolym.2022.105290
Rather RA, Bhat MA, Shalla AH (2022) Multicomponent interpenetrating metal based Alginate-Carrageenan biopolymer hydrogel beads substantiated by graphene oxide for efficient removal of methylene blue from waste water. Chem Eng Res Des 182:604–615. https://doi.org/10.1016/j.cherd.2022.04.017
Saleh TA, Al-Ruwayshid SH, Sari A et al (2020) Synthesis of silica nanoparticles grafted with copolymer of acrylic acrylamide for ultra-removal of methylene blue from aquatic solutions. Eur Polym J 130:109698. https://doi.org/10.1016/j.eurpolymj.2020.109698
Sari Yilmaz M (2022) Graphene oxide/hollow mesoporous silica composite for selective adsorption of methylene blue. Microporous Mesoporous Mater. https://doi.org/10.1016/j.micromeso.2021.111570
Shao P, Xu P, Zhang L et al (2019) Non-chloride in situ preparation of nano-cuprous oxide and its effect on heat resistance and combustion properties of calcium alginate. Polymers 11:1760. https://doi.org/10.3390/polym11111760
Sharma S, Sharma G, Kumar A et al (2022) Adsorption of cationic dyes onto carrageenan and itaconic acid-based superabsorbent hydrogel: Synthesis, characterization and isotherm analysis. J Hazard Mater 421:126729. https://doi.org/10.1016/j.jhazmat.2021.126729
Shaziya HS (2018) The removal of Cu2+, Ni2+ and Methylene Blue (MB) from aqueous solution using Luffa Actangula Carbon: Kinetics, thermodynamic and isotherm and response methodology. Groundw Sustain Dev 6:141–149. https://doi.org/10.1016/j.gsd.2017.12.008
Soury R, Jabli M, Latif S et al (2022) Synthesis and characterization of a new meso-tetrakis (2,4,6-trimethylphenyl) porphyrinto) zinc(II) supported sodium alginate gel beads for improved adsorption of methylene blue dye. Int J Biol Macromol 202:161–176. https://doi.org/10.1016/j.ijbiomac.2022.01.087
Tan M, Zheng S, Lv H et al (2021) Rational design and synthesis of chitosan–quinoa polysaccharide composite aerogel and its adsorption properties for Congo red and methylene blue. New J Chem 45:9829–9837. https://doi.org/10.1039/d1nj01212f
Taşdelen B, Çifçi Dİ, Meriç S (2017) Preparation of N-isopropylacrylamide/itaconic acid/Pumice highly swollen composite hydrogels to explore their removal capacity of methylene blue. Colloids Surf A Physicochem Eng Asp 519:245–253. https://doi.org/10.1016/j.colsurfa.2016.11.003
Verma A, Thakur S, Mamba G et al (2020) Graphite modified sodium alginate hydrogel composite for efficient removal of malachite green dye. Int J Biol Macromol 148:1130–1139. https://doi.org/10.1016/j.ijbiomac.2020.01.142
Wang L, Zhang J, Wang A (2011) Fast removal of methylene blue from aqueous solution by adsorption onto chitosan-g-poly (acrylic acid)/attapulgite composite. Desalination 266:33–39. https://doi.org/10.1016/j.desal.2010.07.065
Wang B, Chi H, Hou Y et al (2020a) Enhancement of Pb(II) Adsorption and Antibacterial Performances of Sodium Alginate/Acrylic Acid Composite Hydrogel via Snowflake-like ZnO Modification. Polym-Plast Tech Mat 59:1010–1022. https://doi.org/10.1080/25740881.2020.1719140
Wang W, Ni J, Chen L et al (2020b) Synthesis of carboxymethyl cellulose-chitosan-montmorillonite nanosheets composite hydrogel for dye effluent remediation. Int J Biol Macromol 165:1–10. https://doi.org/10.1016/j.ijbiomac.2020.09.154
Wang X, Fan X, Xie H et al (2021) Polyacrylic acid/carboxymethyl cellulose/activated carbon composite hydrogel for removal of heavy metal ion and cationic dye. Cellulose 29:483–501. https://doi.org/10.1007/s10570-021-04286-8
Wang Z, Lu J, Wu C et al (2022) Efficient reclamation phosphate by alginate-g-BMOF using poly(N-isopropyl acrylamide-co-acrylamide) as coating for temperature-responsive slow-release P-fertilizer. Int J Biol Macromol 201:437–447. https://doi.org/10.1016/j.ijbiomac.2022.01.061
Xu S, Jin Y, Li R et al (2022) Amidoxime modified polymers of intrinsic microporosity/alginate composite hydrogel beads for efficient adsorption of cationic dyes from aqueous solution. J Colloid Interface Sci 607:890–899. https://doi.org/10.1016/j.jcis.2021.08.157
Yagub MT, Sen TK, Afroze S et al (2014) Dye and its removal from aqueous solution by adsorption: a review. Adv Colloid Interface Sci 209:172–184. https://doi.org/10.1016/j.cis.2014.04.002
Yan J, Li K (2021) A magnetically recyclable polyampholyte hydrogel adsorbent functionalized with β-cyclodextrin and graphene oxide for cationic/anionic dyes and heavy metal ion wastewater remediation. Sep Purif Technol 277:119469. https://doi.org/10.1016/j.seppur.2021.119469
Yan S, Ren X, Zhang F et al (2022) Comparative study of Pb2+, Ni2+, and methylene blue adsorption on spherical waste solid-based geopolymer adsorbents enhanced with carbon nanotubes. Sep Purif Technol 284:120234. https://doi.org/10.1016/j.seppur.2021.120234
Yu Y, Liu Y, Kong Y et al (2012) Synthesis and characterization of temperature-sensitive Poly(N-isopropylacryamide) hydrogel with comonomer and Semi-IPN material. Polym Plast Technol Eng 51:854–860. https://doi.org/10.1080/03602559.2012.671419
Yuan J, Yi C, Jiang H et al (2021) Direct ink writing of hierarchically porous cellulose/alginate monolithic hydrogel as a highly effective adsorbent for environmental applications. ACS Appl Polym Mater 3:699–709. https://doi.org/10.1021/acsapm.0c01002
Zhang H, Pang X, Qi Y (2015) pH-Sensitive graphene oxide/sodium alginate/polyacrylamide nanocomposite semi-IPN hydrogel with improved mechanical strength. RSC Adv 5:89083–89091. https://doi.org/10.1039/c5ra19637j
Zhang ZH, Xu JY, Yang X-L (2021) MXene/sodium alginate gel beads for adsorption of methylene blue. Mater Chem Phys 260:124123. https://doi.org/10.1016/j.matchemphys.2020.124123
Zhang Y, Hui C, Wei R et al (2022) Study on anionic and cationic dye adsorption behavior and mechanism of biofilm produced by Bacillus amyloliquefaciens DT. Appl Surf Sci 573:151627. https://doi.org/10.1016/j.apsusc.2021.151627
Zhou Q, Gao Q, Luo W et al (2015) One-step synthesis of amino-functionalized attapulgite clay nanoparticles adsorbent by hydrothermal carbonization of chitosan for removal of methylene blue from wastewater. Colloids Surf A Physicochem Eng Asp 470:248–257. https://doi.org/10.1016/j.colsurfa.2015.01.092
Zhou Y, Lu J, Zhou Y et al (2019) Recent advances for dyes removal using novel adsorbents: a review. Environ Pollut 252:352–365. https://doi.org/10.1016/j.envpol.2019.05.072
Acknowledgements
The authors acknowledge the support provided by Zhengzhou Science and Technology Bureau, Henan University of Technology. The authors would like to thank MogoEdit (https://www.mogoedit.com) for its English editing during the preparation of this manuscript.
Funding
The work was supported by Natural Science Project of Zhengzhou Science and Technology Bureau [grant number 21ZZXTCX14]; the Innovative Funds Plan of Henan University of Technology [grant number: 2021ZKCJ08]; the National Natural Science Foundation of China [grant number: U1904171]; and the Key Science and Technology Project of Henan Province, China [grant number: 212102210630].
Author information
Authors and Affiliations
Contributions
All authors contributed to the study conception and design; BYH was involved in methodology, investigation, and writing—original draft acquisition; HLW contributed to conceptualization, writing—review and editing, and funding acquisition; CWH was involved in methodology and data curation; YQZ contributed to methodology and data curation; SY provided software and was involved in data curation; GW contributed to resources and methodology; YMS was involved in supervision and funding acquisition; JJL contributed to project administration and writing—review and editing.
Corresponding author
Ethics declarations
Conflict of interest
The authors have no relevant financial or non-financial interests to disclose.
Ethics approval
Not applicable.
Consent to participate
Not applicable.
Consent for publication
All authors have agreed with the content, and all have given explicit consent to publish.
Additional information
Editorial responsibility: M. Abbaspour.
Supplementary Information
Below is the link to the electronic supplementary material.
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
Hua, B.Y., Wei, H.L., Hu, C.W. et al. Preparation of pH/temperature-sensitive semi-interpenetrating network hydrogel adsorbents from sodium alginate via photopolymerization for removing methylene blue. Int. J. Environ. Sci. Technol. 21, 227–244 (2024). https://doi.org/10.1007/s13762-022-04741-4
Received:
Revised:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s13762-022-04741-4