Abstract
A novel PEI-grafted magnetic cellulose (Fe3O4/MCC-PEI) with high amino density was prepared by grafting PEI onto the surface of magnetic cellulose in NaOH/urea aqueous solvent. The embedding of Fe3O4 into cellulose provided excellent magnetic responsiveness for recycling the adsorbent in the magnetic field. The adsorbent for Cr(VI) removal from aqueous solution overcame the disadvantages of adsorbent like difficult recycling, poor regeneration performance and low removal rate at low Cr(VI) concentration. Therefore, the as-prepared Fe3O4/MCC-PEI showed high Cr(VI) adsorption capacity (198.8 mg/g) which could achieve adsorption equilibrium within 10 min, and the removal rate could reach 100% at low Cr(VI) concentration (less than 1.0 mg/L), demonstrating that the high amino density (7.85 mmol/g) and magnetic responsiveness of the adsorbent can greatly promote adsorption capacity and removal efficiency. The adsorbent also showed promising regeneration performance, and the adsorption capacity remained above 96% after six cycles.
Graphical Abstract
Similar content being viewed by others
References
Abbas A, Hussain MA, Sher M, Irfan MI, Tahir MN, Tremel W (2017) Design, characterization and evaluation of hydroxyethylcellulose based novel regenerable supersorbent for heavy metal ions uptake and competitive adsorption. Int J Biol Macromol 102:170–180. https://doi.org/10.1016/j.ijbiomac.2017.04.024
Carpenter AW, De Lannoy CF, Wiesner MR (2015) Cellulose nanomaterials in water treatment technologies. Environ Sci Technol 49:5277–5287. https://doi.org/10.1021/es506351r
Chen H, Lin J, Zhang N, Chen L, Zhong S, Wang Y, Zhang W, Ling Q (2018) Preparation of MgAl-EDTA-LDH based electrospun nanofiber membrane and its adsorption properties of copper(II) from wastewater. J Hazard Mater 345:1–9. https://doi.org/10.1016/j.jhazmat.2017.11.002
Ching TW, Haritos V, Tanksale A (2018) Ultrasound-assisted conversion of cellulose into hydrogel and functional carbon material. Cellulose 25:2629–2645. https://doi.org/10.1007/s10570-018-1746-y
Cui Y, Atkinson JD (2017) Tailored activated carbon from glycerol: role of acid dehydrator on physiochemical characteristics and adsorption performance. J Mater Chem A 5:16812–16821. https://doi.org/10.1039/c7ta02898a
Dinari M, Soltani R, Mohammadnezhad G (2017) Kinetics and thermodynamic study on novel modified-mesoporous silica MCM-41/polymer matrix nanocomposites: effective adsorbents for trace Cr(VI) removal. J Chem Eng Data 62:2316–2329. https://doi.org/10.1021/acs.jced.7b00197
Dong Z, Zhao J, Du J, Li C, Zhao L (2016) Radiation synthesis of spherical cellulose-based adsorbent for efficient adsorption and detoxification of Cr(VI). Radiat Phys Chem 126:68–74. https://doi.org/10.1016/j.radphyschem.2016.05.013
Dwivedi AD, Sanandiya ND, Singh JP, Husnain SM, Chae KH, Hwang DS, Chang YS (2017) Tuning and characterizing nanocellulose interface for enhanced removal of dual-sorbate (AsV and CrVI) from water matrices. ACS Sustain Chem Eng 5:518–528. https://doi.org/10.1021/acssuschemeng.6b01874
El-Korashy SA, Elwakeel KZ, Abd El-Hafeiz A (2016) Fabrication of bentonite/thiourea-formaldehyde composite material for Pb(II), Mn(VII) and Cr(VI) sorption: a combined basic study and industrial application. J Clean Prod 137:40–50. https://doi.org/10.1016/j.jclepro.2016.07.073
Ghasimi S, Landfester K, Zhang KAI (2016) Water compatible conjugated microporous polyazulene networks as visible-light photocatalysts in aqueous. Medium Chemcatchem 8:694–698. https://doi.org/10.1002/cctc.201501102
Hajeeth T, Sudha PN, Vijayalakshmi K (2015) Removal of Cr(VI) from aqueous solution using graft copolymer of cellulose extracted from sisal fibre with acrylic acid monomer. Cellul Chem Technol 49:891–900
He H, Hou X, Ma B, Zhuang L, Li C, He S, Chen S (2016a) The oxidation of viscose fiber optimized by response surface methodology and its further amination with PEI for CO2 adsorption. Cellulose 23:2539–2548. https://doi.org/10.1007/s10570-016-0955-5
He H, Zhuang L, Chen S, Liu H, Li Q (2016b) Structure design of a hyperbranched polyamine adsorbent for CO2 adsorption. Green Chem 18:5859–5869. https://doi.org/10.1039/c6gc01416j
Hokkanen S, Repo E, Lou S, Sillanpaa M (2015) Removal of arsenic(V) by magnetic nanoparticle activated microfibrillated cellulose. Chem Eng J 260:886–894. https://doi.org/10.1016/j.cej.2014.08.093
Hokkanen S, Bhatnagar A, Repo E, Lou S, Sillanpaa M (2016a) Calcium hydroxyapatite microfibrillated cellulose composite as a potential adsorbent for the removal of Cr(VI) from aqueous solution. Chem Eng J 283:445–452. https://doi.org/10.1016/j.cej.2015.07.035
Hokkanen S, Bhatnagar A, Sillanpaa M (2016b) A review on modification methods to cellulose-based adsorbents to improve adsorption capacity. Water Res 91:156–173. https://doi.org/10.1016/j.watres.2016.01.008
Iftekhar S, Srivastava V, Sillanpaa M (2017) Synthesis and application of LDH intercalated cellulose nanocomposite for separation of rare earth elements (REEs). Chem Eng J 309:130–139. https://doi.org/10.1016/j.cej.2016.10.028
Inoue K, Parajuli D, Ghimire KN, Biswas BK, Kawakita H, Oshima T, Ohto K (2017) Biosorbents for removing hazardous metals and metalloids. Mater (Basel Switz). https://doi.org/10.3390/ma10080857
Kera NH, Bhaumik M, Pillay K, Ray SS, Maity A (2017) Selective removal of toxic Cr(VI) from aqueous solution by adsorption combined with reduction at a magnetic nanocomposite surface. J Colloid Interface Sci 503:214–228. https://doi.org/10.1016/j.jcis.2017.05.018
Khan W, Wang Q, Jin X, Feng T (2017) The effect of sputtering parameters and doping of copper on surface free energy and magnetic properties of iron and iron nitride nano thin films on polymer substrate. Mater (Basel Switz) 10:217. https://doi.org/10.3390/ma10020217
Lippitz A, Hubert T (2005) XPS investigations of chromium nitride thin films. Surf Coat Technol 200:250–253. https://doi.org/10.1016/j.surfcoat.2005.02.091
Liu B, Dai W, Liang Z, Ye J, Ouyang L (2017a) Fe/N/C carbon nanotubes with high nitrogen content as effective non-precious catalyst for oxygen reduction reaction in alkaline medium. Int J Hydrogen Energy 42:5908–5915. https://doi.org/10.1016/j.ijhydene.2016.12.043
Liu C, Jin RN, Ouyang XK, Wang YG (2017b) Adsorption behavior of carboxylated cellulose nanocrystal-polyethyleneimine composite for removal of Cr(VI) ions. Appl Surf Sci 408:77–87. https://doi.org/10.1016/j.apsusc.2017.02.265
Lu W, Li J, Sheng Y, Zhang X, You J, Chen L (2017) One-pot synthesis of magnetic iron oxide nanoparticle-multiwalled carbon nanotube composites for enhanced removal of Cr(VI) from aqueous solution. J Colloid Interface Sci 505:1134–1146. https://doi.org/10.1016/j.jcis.2017.07.013
Maaz M, Elzein T, Bejjani A, Barroca-Aubry N, Lepoittevin B, Dragoe D (2017) Surface initiated supplemental activator and reducing agent atom transfer radical polymerization (SI-SARA-ATRP) of 4-vinylpyridine on poly(ethylene terephthalate). J Colloid Interface Sci 500:69–78. https://doi.org/10.1016/j.jcis.2017.03.115
Milosevic M, Saponjic Z, Nunney T, Deeks C, Radoicic M, Mitric M (2017) In situ photoreduction of Ag+-ions on the surface of titania nanotubes deposited on cotton and cotton/PET fabrics. Cellulose 24:1597–1610. https://doi.org/10.1007/s10570-017-1207-z
Nie S, Zhang K, Lin X, Zhang C, Yan D, Liang H, Wang S (2018) Enzymatic pretreatment for the improvement of dispersion and film properties of cellulose nanofibrils. Carbohydr Polym 181:1136–1142. https://doi.org/10.1016/j.carbpol.2017.11.020
Periyasamy S, Gopalakannan V, Viswanathan N (2017) Fabrication of magnetic particles imprinted cellulose based biocomposites for chromium(VI) removal. Carbohydr Polym 174:352–359. https://doi.org/10.1016/j.carbpol.2017.06.029
Pourfadakari S, Jorfi S, Ahmadi M, Takdastan A (2017) Experimental data on adsorption of Cr(VI) from aqueous solution using nanosized cellulose fibers obtained from rice husk. Data Brief 15:887–895. https://doi.org/10.1016/j.dib.2017.10.043
Rahimi K, Mirzaei R, Akbari A, Mirghaffari N (2018) Preparation of nanoparticle-modified polymeric adsorbent using wastage fuzzes of mechanized carpet and its application in dye removal from aqueous solution. J Clean Prod 178:373–383. https://doi.org/10.1016/j.jclepro.2017.12.213
Rapti S, Pournara A, Sarma D, Papadas IT, Armatas GS, Hassan YS (2016) Rapid, green and inexpensive synthesis of high quality UiO-66 amino-functionalized materials with exceptional capability for removal of hexavalent chromium from industrial waste. Inorgan Chem Front 3:635–644. https://doi.org/10.1039/c5qi00303b
Sakulthaew C, Chokejaroenrat C, Poapolathep A, Satapanajaru T, Poapolathep S (2017) Hexavalent chromium adsorption from aqueous solution using carbon nano-onions (CNOs). Chemosphere 184:1168–1174. https://doi.org/10.1016/j.chemosphere.2017.06.094
Shi T, Yang D, Yang H, Ye J, Cheng Q (2017) Preparation of chitosan crosslinked modified silicon material and its adsorption capability for chromium(VI). Appl Clay Sci 142:100–108. https://doi.org/10.1016/j.clay.2016.11.023
Sun X, Yang L, Li Q, Zhao J, Li X, Wang X, Liu H (2014) Amino-functionalized magnetic cellulose nanocomposite as adsorbent for removal of Cr(VI): synthesis and adsorption studies. Chem Eng J 241:175–183. https://doi.org/10.1016/j.cej.2013.12.051
Sun X, Li Q, Yang L, Liu H (2016) Removal of chromium(VI) from wastewater using weakly and strongly basic magnetic adsorbents: adsorption/desorption property and mechanism comparative studies. RSC Adv 6:18471–18482. https://doi.org/10.1039/c5ra27028f
Voisin H, Bergstrom L, Liu P, Mathew AP (2017) Nanocellulose-based materials for water purification. Nanomaterials 7:57. https://doi.org/10.3390/nano7030057
Wang S, Vincent T, Roux JC, Faur C, Guibal E (2017) Innovative conditioning of algal-based sorbents: macro-porous discs for palladium sorption. Chem Eng J 325:521–532. https://doi.org/10.1016/j.cej.2017.05.103
Wu SP, Dai XZ, Kan JR, Shilong FD, Zhu MY (2017) Fabrication of carboxymethyl chitosan-hemicellulose resin for adsorptive removal of heavy metals from wastewater. Chin Chem Lett 28:625–632. https://doi.org/10.1016/j.cclet.2016.11.015
Xu X, Gao BY, Tang X, Yue QY, Zhong QQ, Li Q (2011) Characteristics of cellulosic amine-crosslinked copolymer and its sorption properties for Cr(VI) from aqueous solutions. J Hazard Mater 189:420–426. https://doi.org/10.1016/j.jhazmat.2011.02.056
Yan Y, An Q, Xiao Z, Zheng W, Zhai S (2017) Flexible core-shell/bead-like alginate@PEI with exceptional adsorption capacity, recycling performance toward batch and column sorption of Cr(VI). Chem Eng J 313:475–486. https://doi.org/10.1016/j.cej.2016.12.099
You W, Hong M, Zhang H, Wu Q, Zhuang Z, Yu Y (2016) Functionalized calcium silicate nanofibers with hierarchical structure derived from oyster shells and their application in heavy metal ions removal. Phys Chem Chem Phys 18:15564–15573. https://doi.org/10.1039/c6cp01199c
Zhang C, Su J, Zhu H, Xiong J, Liu X, Li D (2017a) The removal of heavy metal ions from aqueous solutions by amine functionalized cellulose pretreated with microwave-H2O2. RSC Adv 7:34182–34191. https://doi.org/10.1039/c7ra03056h
Zhang F, Yan M, He J, Yin F (2017b) Microstructures and nano-mechanical properties of multilayer coatings prepared by plasma nitriding Cr-coated Al alloy. Vacuum 142:106–113. https://doi.org/10.1016/j.vacuum.2017.05.013
Zhu H, Kong Q, Cao X, He H, Wang J, He Y (2016) Adsorption of Cr(VI) from aqueous solution by chemically modified natural cellulose. Desalin Water Treat 57:20368–20376. https://doi.org/10.1080/19443994.2015.1108237
Acknowledgments
The authors gratefully acknowledge the financial support provided by the Guangxi Science and Technology Research Program (14251009), the Guangxi Youth Natural Science Fund (GXNSFBA053025), the National High Technology Research and Development Program (“863”Program) of China (2009AA06A416), the National Natural Science Foundation of China (51108261), the Natural Science Foundation of Guangxi (2013GXNSFFA019005), and the Director Fund Project of Guangxi Key Laboratory of Clean Pulp & Papermaking and Pollution Control (ZR201701).
Author information
Authors and Affiliations
Corresponding authors
Electronic supplementary material
Below is the link to the electronic supplementary material.
Rights and permissions
About this article
Cite this article
Li, Y., Zhu, H., Zhang, C. et al. PEI-grafted magnetic cellulose for Cr(VI) removal from aqueous solution. Cellulose 25, 4757–4769 (2018). https://doi.org/10.1007/s10570-018-1868-2
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1007/s10570-018-1868-2