RESEARCH ARTICLE

Immobilization of nano-zero-valent irons by carboxylated cellulose nanocrystals for wastewater remediation

  • Bangxian Peng 1 ,
  • Rusen Zhou 2 ,
  • Ying Chen 1 ,
  • Song Tu 1 ,
  • Yingwu Yin 1 ,
  • Liyi Ye , 1
Expand
  • 1. Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China
  • 2. School of Chemistry, Physics and Mechanical Engineering, Queensland University of Technology, Brisbane, QLD 4000, Australia

Received date: 07 Nov 2019

Accepted date: 24 Jan 2020

Published date: 15 Dec 2020

Copyright

2020 Higher Education Press and Springer-Verlag GmbH Germany, part of Spring Nature

Abstract

Nano-zero-valent irons (nZVI) have shown great potential to function as universal and low-cost magnetic adsorbents. Yet, the rapid agglomeration and easy surface corrosion of nZVI in solution greatly hinders their overall applicability. Here, carboxylated cellulose nanocrystals (CCNC), widely available from renewable biomass resources, were prepared and applied for the immobilization of nZVI. In doing so, carboxylated cellulose nanocrystals supporting nano-zero-valent irons (CCNC-nZVI) were obtained via an in-situ growth method. The CCNC-nZVI were characterized and then evaluated for their performances in wastewater treatment. The results obtained show that nZVI nanoparticles could attach to the carboxyl and hydroxyl groups of CCNC, and well disperse on the CCNC surface with a size of ~10 nm. With the CCNC acting as corrosion inhibitors improving the reaction activity of nZVI, CCNC-nZVI exhibited an improved dispersion stability and electron utilization efficacy. The Pb(II) adsorption capacity of CCNC-nZVI reached 509.3 mg·g1 (298.15 K, pH= 4.0), significantly higher than that of CCNC. The adsorption was a spontaneous exothermic process and could be perfectly fitted by the pseudo-second-order kinetics model. This study may provide a novel and green method for immobilizing magnetic nanomaterials by using biomass-based resources to develop effective bio-adsorbents for wastewater decontamination.

Cite this article

Bangxian Peng , Rusen Zhou , Ying Chen , Song Tu , Yingwu Yin , Liyi Ye . Immobilization of nano-zero-valent irons by carboxylated cellulose nanocrystals for wastewater remediation[J]. Frontiers of Chemical Science and Engineering, 2020 , 14(6) : 1006 -1017 . DOI: 10.1007/s11705-020-1924-y

Acknowledgements

This work was supported by the Key Planning Project of Science and Technology of Fujian Province, China (Grant No. 2018N0032). The authors declare no existing conflicts of interest.

Electronic Supplementary Material

Supplementary material is available in the online version of this article at https://doi.org/10.1007/s11705-020-1924-y and is accessible for authorized users.
1
Ouni L, Ramazani A, Taghavi Fardood S. An overview of carbon nanotubes role in heavy metals removal from wastewater. Frontiers of Chemical Science and Engineering, 2019, 13(2): 274–295

DOI

2
Fu R B, Yang Y P, Xu Z, Zhang X, Guo X P, Bi D S. The removal of chromium (VI) and lead (II) from groundwater using sepiolite-supported nanoscale zero-valent iron (S-NZVI). Chemosphere, 2015, 138: 726–734

DOI

3
Chen B, Zhu C, Fei J, Jiang Y, Yin C, Su W, He X, Li Y, Chen Q, Ren Q, Chen Y. Reaction kinetics of phenols and p-nitrophenols in flowing aerated aqueous solutions generated by a discharge plasma jet. Journal of Hazardous Materials, 2019, 363: 55–63

DOI

4
Nahata M, Seo C Y, Krishnakumar P, Schwank J. New approaches to water purification for resource-constrained settings: Production of activated biochar by chemical activation with diammonium hydrogenphosphate. Frontiers of Chemical Science and Engineering, 2018, 12(1): 194–208

DOI

5
Yan Y, Huang P, Zhang H P. Preparation and characterization of novel carbon molecular sieve membrane/PSSF composite by pyrolysis method for toluene adsorption. Frontiers of Chemical Science and Engineering, 2019, 13(4): 772–783

DOI

6
Tao Q Q, Zhang X, Prabaharan K, Dai Y. Separation of cesium from wastewater with copper hexacyanoferrate film in an electrochemical system driven by microbial fuel cells. Bioresource Technology, 2019, 278: 456–459

DOI

7
Zhou R S, Zhou R W, Zhang X H, Bazaka K, Ostrikov K. Continuous flow removal of acid fuchsine by dielectric barrier discharge plasma water bed enhanced by activated carbon adsorption. Frontiers of Chemical Science and Engineering, 2019, 13(2): 340–349

DOI

8
Fu F L, Dionysiou D D, Liu H. The use of zero-valent iron for groundwater remediation and wastewater treatment: A review. Journal of Hazardous Materials, 2014, 267: 194–205

DOI

9
Yang F, Zhang S S, Sun Y Q, Cheng K, Li J S, Tsang D C W. Fabrication and characterization of hydrophilic corn stalk biochar-supported nanoscale zero-valent iron composites for efficient metal removal. Bioresource Technology, 2018, 265: 490–497

DOI

10
Cai Z Q, Fu J, Du P H, Zhao X, Hao X D, Liu W, Zhao D Y. Reduction of nitrobenzene in aqueous and soil phases using carboxymethyl cellulose stabilized zero-valent iron nanoparticles. Chemical Engineering Journal, 2018, 332: 227–236

DOI

11
Dhar P, Kumar A, Katiyar V. Fabrication of cellulose nanocrystal supported stable Fe(0) nanoparticles: A sustainable catalyst for dye reduction, organic conversion and chemo-magnetic propulsion. Cellulose (London, England), 2015, 22(6): 3755–3771

DOI

12
Zhao X, Liu W, Cai Z Q, Han B, Qian T W, Zhao D Y. An overview of preparation and applications of stabilized zero-valent iron nanoparticles for soil and groundwater remediation. Water Research, 2016, 100: 245–266

DOI

13
Mu Y, Jia F, Ai Z H, Zhang L Z. Iron oxide shell mediated environmental remediation properties of nano zero-valent iron. Environmental Science. Nano, 2017, 4(1): 27–45

DOI

14
Liu W, Tian S T, Zhao X, Xie W B, Gong Y Y, Zhao D Y. Application of stabilized nanoparticles for in situ remediation of metal-contaminated soil and groundwater: A critical review. Current Pollution Reports, 2015, 1(4): 280–291

DOI

15
Shi L N, Lin Y M, Zhang X, Chen Z L. Synthesis, characterization and kinetics of bentonite supported nZVI for the removal of Cr (VI) from aqueous solution. Chemical Engineering Journal, 2011, 171(2): 612–617

DOI

16
Horzum N, Demir M M, Nairat M, Shahwan T. Chitosan fiber-supported zero-valent iron nanoparticles as a novel sorbent for sequestration of inorganic arsenic. RSC Advances, 2013, 3(21): 7828–7837

DOI

17
Dong H R, Deng J M, Xie Y K, Zhang C, Jiang Z, Cheng Y J, Hou K J, Zeng G M. Stabilization of nanoscale zero-valent iron (nZVI) with modified biochar for Cr (VI) removal from aqueous solution. Journal of Hazardous Materials, 2017, 332: 79–86

DOI

18
Cai Z Q, Fu J, Du P H, Zhao X, Hao X D, Liu W, Zhao D Y. Reduction of nitrobenzene in aqueous and soil phases using carboxymethyl cellulose stabilized zero-valent iron nanoparticles. Chemical Engineering Journal, 2018, 332: 227–236

DOI

19
Lv X S, Xu J, Jiang G M, Xu X H. Removal of chromium (VI) from wastewater by nanoscale zero-valent iron particles supported on multiwalled carbon nanotubes. Chemosphere, 2011, 85(7): 1204–1209

DOI

20
Brinchi L, Cotana F, Fortunati E, Kenny J M. Production of nanocrystalline cellulose from lignocellulosic biomass: Technology and applications. Carbohydrate Polymers, 2013, 94(1): 154–169

DOI

21
Jiang S S, Daly H, Xiang H, Yan Y, Zhang H P, Hardacre C, Fan X L. Microwave-assisted catalyst-free hydrolysis of fibrous cellulose for deriving sugars and biochemical. Frontiers of Chemical Science and Engineering, 2019, 13(4): 718–726

DOI

22
Islam M S, Chen L, Sisler J, Tam K C. Cellulose nanocrystal (CNC)–inorganic hybrid systems: Synthesis, properties and applications. Journal of Materials Chemistry. B, Materials for Biology and Medicine, 2018, 6(6): 864–883

DOI

23
Maimaiti H, Awati A, Yisilamu G, Zhang D D, Wang S X. Synthesis and visible-light photocatalytic CO2/H2O reduction to methyl formate of TiO2 nanoparticles coated by aminated cellulose. Applied Surface Science, 2019, 466: 535–544

DOI

24
Zarei S, Niad M, Raanaei H. The removal of mercury ion pollution by using Fe3O4-nanocellulose: Synthesis, characterizations and DFT studies. Journal of Hazardous Materials, 2018, 344: 258–273

DOI

25
Liu H, Song J, Shang S B, Song Z Q, Wang D. Cellulose nanocrystal/silver nanoparticle composites as bifunctional nanofillers within waterborne polyurethane. ACS Applied Materials & Interfaces, 2012, 4(5): 2413–2419

DOI

26
Chen L, Cao W J, Quinlan P J, Berry R M, Tam K C. Sustainable catalysts from gold-loaded polyamidoamine dendrimer-cellulose nanocrystals. ACS Sustainable Chemistry & Engineering, 2015, 3(5): 978–985

DOI

27
Cheng M, Qin Z Y, Chen Y Y, Liu J M, Ren Z C. Facile one-step extraction and oxidative carboxylation of cellulose nanocrystals through hydrothermal reaction by using mixed inorganic acids. Cellulose (London, England), 2017, 24(8): 3243–3254

DOI

28
Avila Ramirez J A, Fortunati E, Kenny J M, Torre L, Foresti M L. Simple citric acid-catalyzed surface esterification of cellulose nanocrystals. Carbohydrate Polymers, 2017, 157: 1358–1364

DOI

29
Lu J, Askeland P, Drzal L T. Surface modification of microfibrillated cellulose for epoxy composite applications. Polymer, 2008, 49(5): 1285–1296

DOI

30
Zhou C J, Wu Q L, Yue Y Y, Zhang Q G. Application of rod-shaped cellulose nanocrystals in polyacrylamide hydrogels. Journal of Colloid and Interface Science, 2011, 353(1): 116–123

DOI

31
Yu X L, Tong S R, Ge M F, Wu L Y, Zuo J C, Cao C Y, Song W G. Adsorption of heavy metal ions from aqueous solution by carboxylated cellulose nanocrystals. Journal of Environmental Sciences (China), 2013, 25(5): 933–943

DOI

32
Zhang X, Lin S, Chen Z L, Megharaj M, Naidu R. Kaolinite-supported nanoscale zero-valent iron for removal of Pb2+ from aqueous solution: Reactivity, characterization and mechanism. Water Research, 2011, 45(11): 3481–3488

DOI

33
Wu L M, Liao L B, Lv G C, Qin F X, He Y J, Wang X Y. Micro-electrolysis of Cr (VI) in the nanoscale zero-valent iron loaded activated carbon. Journal of Hazardous Materials, 2013, 254-255: 277–283

DOI

34
Ling L, Pan B C, Zhang W X. Removal of selenium from water with nanoscale zero-valent iron: Mechanisms of intraparticle reduction of Se (IV). Water Research, 2015, 71: 274–281

DOI

35
Gong K D, Hu Q, Xiao Y Y, Cheng X, Liu H, Wang N, Qiu B, Guo Z H. Triple layered core-shell ZVI@carbon@polyaniline composite enhanced electron utilization in Cr(VI) reduction. Journal of Materials Chemistry. A, Materials for Energy and Sustainability, 2018, 6(24): 11119–11128

DOI

36
Su F C, Zhou H J, Zhang Y X, Wang G Z. Three-dimensional honeycomb-like structured zero-valent iron/chitosan composite foams for effective removal of inorganic arsenic in water. Journal of Colloid and Interface Science, 2016, 478: 421–429

DOI

37
Zhang X L, Lin Q L, Luo S Y, Ruan K Z, Peng K P. Preparation of novel oxidized mesoporous carbon with excellent adsorption performance for removal of malachite green and lead ion. Applied Surface Science, 2018, 442: 322–331

DOI

38
Khan A, Xing J, Elseman A M, Gu P C, Gul K, Ai Y J, Jehan R, Alsaedi A, Hayat T, Wang X K. A novel magnetite nanorod-decorated Si-Schiff base complex for efficient immobilization of U(VI) and Pb(II) from water solutions. Dalton Transactions (Cambridge, England), 2018, 43(33): 11327–11336

DOI

39
Huang X, Wei D, Zhang X W, Fan D W, Sun X, Du B, Wei Q. Synthesis of amino-functionalized magnetic aerobic granular sludge-biochar for Pb(II) removal: Adsorption performance and mechanism studies. Science of the Total Environment, 2019, 685: 681–689

DOI

40
Wang N, Yang D X, Wang X X, Yu S J, Wang H Q, Wen T, Song G, Yu Z M, Wang X K. Highly efficient Pb(II) and Cu(II) removal using hollow Fe3O4@PDA nanoparticles with excellent application capability and reusability. Inorganic Chemistry Frontiers, 2018, 5(9): 2174–2182

DOI

41
Liu X J, Lai D G, Wang Y. Performance of Pb(II) removal by an activated carbon supported nanoscale zero-valent iron composite at ultralow iron content. Journal of Hazardous Materials, 2019, 361: 37–48

DOI

42
Siahkamari M, Jamali A, Sabzevari A, Shakeri A. Removal of lead(II) ions from aqueous solutions using biocompatible polymeric nano-adsorbents: A comparative study. Carbohydrate Polymers, 2017, 157: 1180–1189

DOI

43
Zhao Z F, Zhang X, Zhou H J, Liu G, Kong M G, Wang G Z. Microwave-assisted synthesis of magnetic Fe3O4-mesoporous magnesium silicate core-shell composites for the removal of heavy metal ions. Microporous and Mesoporous Materials, 2017, 242: 50–58

DOI

44
Fu R B, Yang Y P, Xu Z, Zhang X, Guo X P, Bi D S. The removal of chromium (VI) and lead (II) from groundwater using sepiolite-supported nanoscale zero-valent iron (S-NZVI). Chemosphere, 2015, 138: 726–734

DOI

45
Rama Chandraiah M. Facile synthesis of zero valent iron magnetic biochar composites for Pb(II) removal from the aqueous medium. Alexandria Engineering Journal, 2016, 55: 619–625

DOI

46
Li X Q, Zhang W X. Equestration of metal cations with zerovalent iron nanoparticles—a study with high resolution X-ray photoelectron spectroscopy (HR-XPS). Journal of Physical Chemistry C, 2007, 111(19): 6939–6946

DOI

47
Abdel-Samad H W, Watson P R. An XPS study of the adsorption of chromate on goethite (α-FeOOH). Applied Surface Science, 1997, 108(3): 371–377

DOI

48
Noubactep C. A critical review on the process of contaminant removal in Fe0-H2O systems. Environmental Technology, 2008, 29(8): 909–920

DOI

49
Martin J E, Herzing A A, Yan W L, Li X Q, Koel B E, Kiely C J, Zhang W X. Determination of the oxide layer thickness in core-shell zerovalent iron nanoparticles. Langmuir, 2008, 24(8): 4329–4334

DOI

Outlines

/