Abstract
Green bio-flocculants from renewable biomass resources have received the widespread attention for wastewater treatment, which are promising alternatives to petroleum-based synthetic flocculants. In this paper, sustainable cationic cellulose bio-flocculants with various amino group contents were successfully prepared by a feasible chemical crosslinking with polyethyleneimine (PEI). The flocculation performances of diverse PEI-grafting cellulose (CE-PEI) were evaluated to purify turbid Kaolin suspension. Further, the flocculation kinetics and flocculation mechanism were investigated. Benefiting from the high surface positive charges and supramolecular structure, CE-PEI bio-flocculants with amino group contents of 17.5 mmol/g displayed the best turbidity removal efficiency. The residual turbidity of Kaolin suspension decreased from the initial 480–8.6 NTU, a 98.2% reduction with CE-PEI dosage of 0.15 mg/mL, sedimentation time of 30 min at pH 7.0. Flocculation kinetic results indicated that interaction of aggregation and collision between CE-PEI bio-flocculants and Kaolin particles was sufficient for the flocculation process at the optimal CE-PEI dosage. Moreover, charge neutralization was the dominant mechanism for the flocculation of CE-PEI on Kaolin. Thus, this work not only exploits a promising application of cellulose as a bio-flocculant, but also provides a feasible approach to efficiently purify high turbidity wastewater.
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Carvalho AJF, Trovatti E, Casale CA (2018) Polystyrene and cellulose nanofibril composites: fiber dispersion driven by nanoemulsion flocculation in the presence of a fiber or nanofiber suspension. J Mol Liq 272:387–394. https://doi.org/10.1016/j.molliq.2018.09.089
Chen X, Liu L, Luo ZH, Shen JY, Ni QQ, Yao JM (2018) Facile preparation of a cellulose-based bio-adsorbent modified by hPEI in heterogeneous system for high-efficiency removal of multiple types of dyes. React Funct Polym 125:77–83. https://doi.org/10.1016/j.reactfunctpolym.2018.02.009
Chen Y, Tian GW, Zhai BY, Zhang HL, Liang YN, Liang HB (2019) Cationic starch-grafted-cationic polyacrylamide based graphene oxide ternary composite flocculant for the enhanced flocculation of oil sludge suspension. Compos Part B-Eng. https://doi.org/10.1016/j.compositesb.2019.107416
Chen FJ, Jin XK, Jia DD, Cao YL, Duan HM, Long MQ (2020a) Efficient treament of organic pollutants over Cds/graphene composites photocatalysts. Appl Surf Sci. https://doi.org/10.1016/j.apsusc.2019.144422
Chen J, Xu XJ, Nie R, Feng L, Li XH, Liu BZ (2020b) Chitosan modified cationic polyacrylamide initiated by UV-H2O2 for sludge flocculation and new insight on the floc characteristics study. Polymers-Basel 12(11):2738–2746. https://doi.org/10.3390/polym12112738
Cheng M, Qin Z, Liu Y, Qin Y, Li T, Chen L, Zhu M (2014) Efficient extraction of carboxylated spherical cellulose nanocrystals with narrow distribution through hydrolysis of lyocell fibers by using ammonium persulfate as an oxidant. J Mater Chem a 2:251–258
Dong LJ, Zhu ZL, Qiu YL, Zhao JF (2016) Removal of lead from aqueous solution by hydroxyapatite/manganese dioxide composite. Front Environ Sci Eng 10:28–36
Donia AM, Atia AA, Abouzayed FI (2012) Preparation and characterization of nanomagnetic cellulose with fast kinetic properties towards the adsorption of some metalions. Chem Eng J 191:22–30. https://doi.org/10.1016/j.cej.2011.08.034
Essandoh M, Garcia RA, Nieman CM (2018) Chemical and enzymatic protein cross-linking to improve flocculant properties. ACS Sustain Chem Eng 6(10):12946–12952
Fu Q, Sutherland A, Gustafsson E, Ali MM, SoleymaniOrcid L, Pelton R (2017) Relating redox properties of polyvinylamine-g-tempo/laccase hydrogel complexes to cellulose oxidation. Langmuir 33(32):7854–7861. https://doi.org/10.1021/acs.langmuir.7b01460
Gao LF, Li C, Huang WC, Mei S, Lin H, Ou Q, Zhang Y, Guo J, Zhang F, Xu SX, Zhang H (2020) Mxene/polymer membranes: synthesis, properties, and emerging applications. Chem Mater 32(5):1703–1747. https://doi.org/10.1021/acs.chemmater.9b04408
Ge H, Huang H, Xu M, Chen Q (2016) Cellulose/poly (ethylene imine) composites as efficient and reusable adsorbents for heavy metal ions. Cellulose 23:2527–2537
Guo WJ, Fu ZY, Wang H, Liu SS, Wu FC, Giesy JP (2018) Removal of antimonate (Sb(V)) and antimonite (Sb (III)) from aqueous solutions by coagulation-flocculation-sedimentation (CFS): dependence on influencing factors and insights into removal mechanisms. SCI Total Environ 644:1277–1285. https://doi.org/10.1016/j.scitotenv.2018.07.034
Hena S, Znad H, Heong KT, Judd S (2018) Dairy farm wastewater treatment and lipid accumulation by Arthrospira platensis. Water Res 128:267–277. https://doi.org/10.1016/j.watres.2017.10.057
Jamshidifard S, Koushkbaghi S, Hosseini S, Rezaei S, Karamipour A, Jafari A, Irani M (2019) Incorporation of UiO-66-NH2 MOF into the PAN/chitosan nanofibers for adsorption and membrane filtration of Pb(II), Cd(II) and Cr(VI) ions from aqueous solutions. J Hazard Mater 368:10–20. https://doi.org/10.1016/j.jhazmat.2019.01.024
Li HJ, Cai T, Yuan B, Li RH, Yang H, Li A (2015) Flocculation of both kaolin and hematite suspensions using the starch-based flocculants and their floc properties. Ind Eng Chem Res 54(1):59–67. https://doi.org/10.1021/ie503606y
Li C, Ma HY, Venkateswaran S, Hsiao BS (2020) Highly efficient and sustainable carboxylated cellulose filters for removal of cationic dyes/heavy metals ions. Chem Eng J 389:123458. https://doi.org/10.1016/j.cej.2019.123458
Liu M, Jia LD, Zhao ZX, Han Y, Li YX, Peng QM (2020) Fast and robust lead (II) removal from water by bioinspired amyloid lysozyme fibrils conjugated with polyethyleneimine (PEI). Chem Eng J 390:124667–124676. https://doi.org/10.1016/j.cej.2020.124667
Nakamura A, Sato H, Sato Y, Murakami KJ (2020) Effects of calcium chloride and poly (N, N-dimethylaminoethyl methacrylate) on the filtration rate of a bentonite suspension and the examination of the filtration mechanism. Colloid Surf A. https://doi.org/10.1016/j.colsurfa.2020.125265
Noor MHM, Ngadi N, Inuwa IM, Opotu LA (2020) Synthesis and application of polyacrylamide grafted magnetic cellulose flocculant for palm oil wastewater treatment. J Environ Chem Eng 8(4):104014. https://doi.org/10.1016/j.jece.2020.104014
Park JH, Choi HM, Oh KW (2014) Simultaneous crosslinking and cationization of cotton cellulose by using dialdehyde and choline chloride: comparison between the pad-dry-cure and microwave irradiation process. Cellulose 21:3107–3119. https://doi.org/10.1007/s10570-014-0326-z
Peng P, Garnier G (2010) Effect of cationic polyacrylamide adsorption kinetics and ionic strength on precipitated calcium carbonate flocculation. Langmuir 26(22):16949–16957
Pourabdollah K (2021) Simultaneous ε-Keggin Al13 chloride salt and anionic polyacrylamide coagulation-flocculation system for agglomeration of trimetallic Cr-Ni-Fe doped core-shell microspheres of graphitized coke. Chem Eng J. https://doi.org/10.1016/j.cej.2021.128583
Rodríguez K, Renneckar S, Gatenholm P (2011) Biomimetic calcium phosphate crystal mineralization on electrospun cellulose-based scaffolds. ACS Appl Mater Inter 3(3):681–689
Salehizadeh H, Yan N, Farnood R (2018) Recent advances in polysaccharide bio-based flocculants. Biotechnol Adv 36(1):92–119. https://doi.org/10.1016/j.biotechadv.2017.10.002
Shahadat M, Teng TT, Rafatullah M, Shaikh ZA, Sreekrishnan TR, Ali SW (2017) Bacterial bioflocculants: a review of recent advances and perspectives. Chem Eng J 328:1139–1152. https://doi.org/10.1016/j.cej.2017.07.105
Shak KPY, Pang YL, Mah SK (2018) Nanocellulose: Recent advances and its prospects in environmental remediation. Beilstein J Nanotechnol 9:2479–2498. https://doi.org/10.3762/bjnano.9.232
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
Vakili M, Deng S, Cagnetta G, Wang W, Meng PP, Liu DC, Yu G (2019) Regeneration of chitosan-based adsorbents used in heavy metal adsorption: a review. Sep Purif Technol 224:373–387. https://doi.org/10.1016/j.seppur.2019.05.040
Wang JP, Chen YZ, Wang Y, Yuan SJ, Yu HQ (2011) Optimization of coagulation-flocculation process for pulp mill wastewater treatment using a combination of uniform design and response surface methodology. Water Res 45:5633–5640. https://doi.org/10.1016/j.watres.2011.08.023
Wang N, Ouyang XK, Yang LY, Omer MA (2017) Fabrication of a magnetic cellulose nanocrystal/metal-organic framework composite for removal of Pb(ii) from water. ACS Sustain Chem Eng. 5(11):10447–10458. https://doi.org/10.1021/acssuschemeng.7b02472
Wang Q, Xie D, Chen JJ, Liu G, Yu MG (2020) Facile fabrication of superhydrophobic and photoluminescent tempo-oxidized cellulose-based paper for anticounterfeiting application. ACS Sustain Chem Eng 8(35):13176–13184. https://doi.org/10.1021/acssuschemeng.0c01559
Wei H, Gao BQ, Ren J, Li AM, Yang H (2018) Coagulation/flocculation in dewatering of sludge: a review. Water Res. https://doi.org/10.1016/j.watres.2018.07.029
Witham MI, Grabsch AF, Owen AT, Fawell PD (2012) The effect of cations on the activity of anionic polyacrlamide flocculant solutions. Inter J Miner Process 114–117:51–62
Wong SS, Teng TT, Ahmad AL, Zuhairi A, Najafpour G (2006) Treatment of pulp and paper mill wastewater by polyacrylamide (PAM) in polymer induced flocculation. J Hazard Mater 135:378–388. https://doi.org/10.1016/j.jhazmat.2005.11.076
Yu KF, Li P, Li H, Zhang B, Yang J, Huang FY, Li R, He YL (2021) Potential of coagulation to remove particle-associated and free-living antibiotic resistome from wastewater. J Hazard Mater 406:124295. https://doi.org/10.1016/j.jhazmat.2020.124295
Zhang N, Zang GL, Shi C, Yu HQ, Sheng GP (2016) A novel adsorbent TEMPO mediated oxidized cellulose nanofifibrils modifified with PEI: preparation, characterization, and application for Cu (II) removal. J Hazard Mater 316:11–18. https://doi.org/10.1016/j.jhazmat.2016.05.018
Zhao DL, Japip S, Zhang Y, Weber M, Maletzko C, Chung TS (2020) Emerging thin-film nanocomposite (TFN) membranes for reverse osmosis: a review. Water Res. https://doi.org/10.1016/j.watres.2020.115557
Zhao CL, Zhou JY, Yan Y, Yang LW, Xing GH, Li HY, Wu P, Wang MY, Zheng HL (2021) Application of coagulation/flocculation in oily wastewater treatment: A review. Sci Total Environ 761:142795. https://doi.org/10.1016/j.scitotenv.2020.142795
Zhu HC, Zhang Y, Yang XG, Liu HY, Zhang XM, Yao JM (2015a) An eco-friendly one-step synthesis of dicarboxyl cellulose for potential application in flocculation. Ind Eng Chem Res 54:2825–2829. https://doi.org/10.1021/ie503020n
Zhu HC, Zhang Y, Yang XG, Liu HY, Shao L, Zhang XM, Yao JM (2015b) One-step green synthesis of non-hazardous dicarboxyl cellulose flocculant and its flocculation activity evaluation. J Hazard Mater 296:1–8. https://doi.org/10.1016/j.jhazmat.2015.04.029
Acknowledgements
The work was financially supported by the National Natural Science Foundation of China (51672251), and 521 Talent Project of Zhejiang Sci-Tech University.
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ZL Investigation, Data curation, Writing-original draft. WG Investigation, Data curation. XC Methodology. RM Format and layout. YD Characterization. LL Supervision, Review and editing, Funding acquisition. JY Conceptualization, Writing-review and editing.
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Li, Z., Gong, W., Chen, X. et al. Sustainable cationic cellulose for highly efficient flocculation of Kaolin suspension. Cellulose 28, 11097–11108 (2021). https://doi.org/10.1007/s10570-021-04211-z
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DOI: https://doi.org/10.1007/s10570-021-04211-z