Skip to main content
Log in

Synthesis of nano-scale zero-valent iron-reduced graphene oxide-silica nano-composites for the efficient removal of arsenic from aqueous solutions

  • Research Article
  • Published:
Environmental Science and Pollution Research Aims and scope Submit manuscript

Abstract

Design and synthesis of arsenic adsorbents with high performance and excellent stability has been still a significant challenge. In this study, we anchored nano-zero-valent iron (NZVI) on the surface of graphene-silica composites (GS) with high specific surface area, forming the NZVI/GS nano-composite. The prepared nano-materials were used to remove As(III) and As(V) through adsorption from aqueous solutions. The results indicated that NZVI particles were dispersed well on the surface of GS, and the NZVI/GS showed great potential to remove As(III) and As(V). Adsorption performance of NZVI/GS for As(III) and As(V) highly depended on the pH of solutions. The experimental data fitted well with the pseudo-second-order kinetic model and the Langmuir isotherm model. The calculated maximum adsorption capacities of NZVI/GS for As(III) and As(V) were up to 45.57 mg/g and 45.12 mg/g at 298 K, respectively, and the adsorption equilibrium could be reached within 60 min. The residual concentrations of As(III) and As(V) after treatment with 0.4 g/L NZVI/GS can meet with the drinking water standard of WHO when the initial concentrations were below 4 mg/L and 3 mg/L, respectively. Moreover, the as-prepared NZVI/GS had excellent anti-interference ability during the process of As removal in the presence of foreign ions. During the As removal process, As(III) was oxidized to As(V), which could be removed through adsorption by electrostatic attraction and complexation. These results indicated that the as-synthesized NZVI/GS composite is a promising adsorbent for the removal of arsenic from aqueous solutions.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6

Similar content being viewed by others

References

  • Ali I, Asim M, Khan TA (2012) Arsenite removal from water by electro-coagulation on zinc–zinc and copper–copper electrodes. International Journal of Environmental Science and Technology 10:377–384

    Article  CAS  Google Scholar 

  • Ali I, Al-Othman ZA, Alwarthan A, Asim M, Khan TA (2014) Removal of arsenic species from water by batch and column operations on bagasse fly ash. Environmental science and pollution research international 21:3218–3229

    Article  CAS  Google Scholar 

  • Ali I, Alharbi OML, Tkachev A, Galunin E, Burakov A, Grachev VA (2018) Water treatment by new-generation graphene materials: hope for bright future. Environmental science and pollution research international 25:7315–7329

    Article  CAS  Google Scholar 

  • Ali I, Basheer AA, Mbianda XY, Burakov A, Galunin E, Burakova I, Mkrtchyan E, Tkachev A, Grachev V (2019) Graphene based adsorbents for remediation of noxious pollutants from wastewater. Environ Int 127:160–180

    Article  CAS  Google Scholar 

  • Alotaibi KM, Shiels L, Lacaze L, Peshkur TA, Anderson P, Machala L, Critchley K, Patwardhan SV, Gibson LT (2017) Iron supported on bioinspired green silica for water remediation. Chemical Science 8:567–576

    Article  CAS  Google Scholar 

  • Bai Y, Yang T, Liang J, Qu J (2016) The role of biogenic Fe-Mn oxides formed in situ for arsenic oxidation and adsorption in aquatic ecosystems. Water Res. 98:119–127

    Article  CAS  Google Scholar 

  • Bang S, Korfiatis GP, Meng XG (2005) Removal of arsenic from water by zero-valent iron. J. Hazard. Mater. 121:61–67

    Article  CAS  Google Scholar 

  • Bhowmick S, Chakraborty S, Mondal P, Van Renterghem W, Van den Berghe S, Roman-Ross G, Chatterjee D, Iglesias M (2014) Montmorillonite-supported nanoscale zero-valent iron for removal of arsenic from aqueous solution: kinetics and mechanism. Chemical Engineering Journal 243:14–23

    Article  CAS  Google Scholar 

  • Bui TH, Kim C, Hong SP, Yoon J (2017) Effective adsorbent for arsenic removal: core/shell structural nano zero-valent iron/manganese oxide. Environmental science and pollution research international 24:24235–24242

    Article  CAS  Google Scholar 

  • Calderon B, Fullana A (2015) Heavy metal release due to aging effect during zero valent iron nanoparticles remediation. Water Res 83:1–9

    Article  CAS  Google Scholar 

  • Chandra V, Park J, Chun Y, Lee JW, Hwang I-C, Kim KS (2010) Water-dispersible magnetite-reduced graphene oxide composites for arsenic removal. Acs Nano 4:3979–3986

    Article  CAS  Google Scholar 

  • Cohen SM, Chowdhury A, Arnold LL (2016) Inorganic arsenic: a non-genotoxic carcinogen. J Environ Sci (China) 49:28–37

    Article  Google Scholar 

  • Cui L, Wang Y, Gao L, Hu L, Wei Q, Du B (2015) Removal of Hg(II) from aqueous solution by resin loaded magnetic beta-cyclodextrin bead and graphene oxide sheet: synthesis, adsorption mechanism and separation properties. J. Colloid Interface Sci. 456:42–49

    Article  CAS  Google Scholar 

  • Davodi B, Jahangiri M (2014) Determination of optimum conditions for removal of As (III) and As (V) by polyaniline/polystyrene nanocomposite. Synth. Met. 194:97–101

    Article  CAS  Google Scholar 

  • Du Q, Zhang S, Pan B, Lv L, Zhang W, Zhang Q (2013) Bifunctional resin-ZVI composites for effective removal of arsenite through simultaneous adsorption and oxidation. Water Res 47:6064–6074

    Article  CAS  Google Scholar 

  • Fakhri A, Kahi DS (2017) Synthesis and characterization of MnS2/reduced graphene oxide nanohybrids for with photocatalytic and antibacterial activity. J Photochem Photobiol B 166:259–263

    Article  CAS  Google Scholar 

  • Fakhri A, Naji M (2017) Degradation photocatalysis of tetrodotoxin as a poison by gold doped PdO nanoparticles supported on reduced graphene oxide nanocomposites and evaluation of its antibacterial activity. J Photochem Photobiol B 167:58–63

    Article  CAS  Google Scholar 

  • Fang W, Jiang X, Luo H, Geng J (2018) Synthesis of graphene/SiO2@polypyrrole nanocomposites and their application for Cr(VI) removal in aqueous solution. Chemosphere 197:594–602

    Article  CAS  Google Scholar 

  • Geim AK (2009) Graphene: Status and Prospects. Science 324:1530–1534

    Article  CAS  Google Scholar 

  • Gihring TM, Druschel GK, McCleskey RB, Hamers RJ, Banfield JF (2001) Rapid arsenite oxidation by Thermus aquaticus and Thermus thermophilus: field and laboratory investigations. Environmental Science & Technology 35:3857–3862

    Article  CAS  Google Scholar 

  • Goldberg S, Johnston CT (2001) Mechanisms of arsenic adsorption on amorphous oxides evaluated using macroscopic measurements, vibrational spectroscopy, and surface complexation modeling. J. Colloid Interface Sci. 234:204–216

    Article  CAS  Google Scholar 

  • Guo XJ, Chen FH (2005) Removal of arsenic by bead cellulose loaded with iron oxyhydroxide from groundwater. Environmental Science & Technology 39:6808–6818

    Article  CAS  Google Scholar 

  • Guo H, Jiao T, Zhang Q, Guo W, Peng Q, Yan X (2015a) Preparation of graphene oxide-based hydrogels as efficient dye adsorbents for wastewater treatment. Nanoscale Research Letters 10:931

    Google Scholar 

  • Guo L, Ye P, Wang J, Fu F, Wu Z (2015b) Three-dimensional Fe3O4-graphene macroscopic composites for arsenic and arsenate removal. J. Hazard. Mater. 298:28–35

    Article  CAS  Google Scholar 

  • Jia YF, Demopoulos GP (2005) Adsorption of arsenate onto ferrihydrite from aqueous solution: influence of media (sulfate vs nitrate), added gypsum, and pH alteration. Environmental Science & Technology 39:9523–9527

    Article  CAS  Google Scholar 

  • Kanel SR, Manning B, Charlet L, Choi H (2005) Removal of arsenic(III) from groundwater by nanoscale zero-valent iron. Environmental Science & Technology 39:1291–1298

    Article  CAS  Google Scholar 

  • Katsoyianni IA, Ruettimann T, Hug SJ (2009) Response to comment on “pH dependence of fenton reagent generation and As(III) oxidation and removal by corrosion of zero valent iron in aerated water”. Environmental Science & Technology 43:3980–3981

    Article  CAS  Google Scholar 

  • Katsoyiannis IA, Zouboulis AI (2002) Removal of arsenic from contaminated water sources by sorption onto iron-oxide-coated polymeric materials. Water Res. 36:5141–5155

    Article  CAS  Google Scholar 

  • Katsoyiannis IA, Ruettimann T, Hug SJ (2008) pH dependence of Fenton reagent generation and As(III) oxidation and removal by corrosion of zero valent iron in aerated water. Environmental Science & Technology 42:7424–7430

    Article  CAS  Google Scholar 

  • Kim J, Benjamin MM (2004) Modeling a novel ion exchange process for arsenic and nitrate removal. Water Res. 38:2053–2062

    Article  CAS  Google Scholar 

  • Kim KS, Zhao Y, Jang H, Lee SY, Kim JM, Kim KS, Ahn J-H, Kim P, Choi J-Y, Hong BH (2009) Large-scale pattern growth of graphene films for stretchable transparent electrodes. Nature 457:706–710

    Article  CAS  Google Scholar 

  • Li F (2013) Layer-by-layer loading iron onto mesoporous silica surfaces: synthesis, characterization and application for As(V) removal. Microporous and Mesoporous Materials 171:139–146

    Article  CAS  Google Scholar 

  • Li D, Mueller MB, Gilje S, Kaner RB, Wallace GG (2008) Processable aqueous dispersions of graphene nanosheets. Nature Nanotechnology 3:101–105

    Article  CAS  Google Scholar 

  • Li Y, Ye Z, Zhou J, Liu J, Song G, Zhang K, Ye B (2012) A new voltammetric sensor based on poly(L-arginine)/graphene-Nafion composite film modified electrode for sensitive determination of Terbutaline sulfate. J. Electroanal. Chem. 687:51–57

    Article  CAS  Google Scholar 

  • Li F, Geng D, Cao Q (2014) Adsorption of As(V) on aluminum-, iron-, and manganese-(oxyhydr)oxides: equilibrium and kinetics. Desalination and Water Treatment 56:1829–1838

    Article  CAS  Google Scholar 

  • Li J, Chen C, Zhang R, Wang X (2015) Nanoscale zero-valent iron particles supported on reduced graphene oxides by using a plasma technique and their application for removal of heavy-metal ions. Chemistry-an Asian Journal 10:1410–1417

    Article  CAS  Google Scholar 

  • Liang Q, Luo H, Geng J, Chen J (2018) Facile one-pot preparation of nitrogen-doped ultra-light graphene oxide aerogel and its prominent adsorption performance of Cr(VI). Chemical Engineering Journal 338:62–71

    Article  CAS  Google Scholar 

  • Monique Bissena FHF (2003) Arsenic – a review.Part I: Occurrence, Toxicity, Speciation, Mobility. Acta Hydroch. Hydrob. 31:9–18

    Article  Google Scholar 

  • Nguyen DCT, Zhu L, Zhang Q, Cho KY, Oh W-C (2018) A new synergetic mesoporous silica combined to CdSe-graphene nanocomposite for dye degradation and hydrogen evolution in visible light. Materials Research Bulletin 107:14–27

    Article  CAS  Google Scholar 

  • Parashar K, Ballav N, Debnath S, Pillay K, Maity A (2016) Rapid and efficient removal of fluoride ions from aqueous solution using a polypyrrole coated hydrous tin oxide nanocomposite. J. Colloid Interface Sci. 476:103–118

    Article  CAS  Google Scholar 

  • Ristein J, Zhang W, Speck F, Ostler M, Ley L, Seyller T (2010) Characteristics of solution gated field effect transistors on the basis of epitaxial graphene on silicon carbide. Journal of Physics D-Applied Physics 43:345303

    Article  CAS  Google Scholar 

  • Sun X, Hu C, Qu J (2013) Preparation and evaluation of Zr-beta-FeOOH for efficient arsenic removal. Journal of Environmental Sciences 25:815–822

    Article  CAS  Google Scholar 

  • Tang L, Feng H, Tang J, Zeng G, Deng Y, Wang J, Liu Y, Zhou Y (2017) Treatment of arsenic in acid wastewater and river sediment by Fe@Fe2O3 nanobunches: the effect of environmental conditions and reaction mechanism. Water Res 117:175–186

    Article  CAS  Google Scholar 

  • Wang C, Luo H, Zhang Z, Wu Y, Zhang J, Chen S (2014a) Removal of As(III) and As(V) from aqueous solutions using nanoscale zero valent iron-reduced graphite oxide modified composites. J. Hazard. Mater. 268:124–131

    Article  CAS  Google Scholar 

  • Wang C, Luo H, Zhang Z, Wu Y, Zhang J, Chen S (2014b) Removal of As(III) and As(V) from aqueous solutions using nanoscale zero valent iron-reduced graphite oxide modified composites. Journal of hazardous materials 268:124–131

    Article  CAS  Google Scholar 

  • Wu CC, Hus LC, Chiang PN, Liu JC, Kuan WH, Chen CC, Tzou YM, Wang MK, Hwang CE (2013) Oxidative removal of arsenite by Fe(II)- and polyoxometalate (POM)-amended zero-valent aluminum (ZVAl) under oxic conditions. Water Res. 47:2583–2591

    Article  CAS  Google Scholar 

  • Wu Y, Luo H, Wang H (2014) Removal of para-nitrochlorobenzene from aqueous solution on surfactant-modified nanoscale zero-valent iron/graphene nanocomposites. Environ. Technol. 35:2698–2707

    Article  CAS  Google Scholar 

  • Wu C, Tu J, Liu W, Zhang J, Chu S, Lu G, Lin Z, Dang Z (2017) The double influence mechanism of pH on arsenic removal by nano zero valent iron: electrostatic interactions and the corrosion of Fe0. Environmental Science: Nano 4:1544–1552

    CAS  Google Scholar 

  • Xu W, Wang J, Wang L, Sheng G, Liu J, Yu H, Huang X-J (2013) Enhanced arsenic removal from water by hierarchically porous CeO2–ZrO2 nanospheres: role of surface- and structure-dependent properties. J. Hazard. Mater. 260:498–507

    Article  CAS  Google Scholar 

  • Yamashita T, Hayes P (2008) Analysis of XPS spectra of Fe2+ and Fe3+ ions in oxide materials. Appl. Surf. Sci. 254:2441–2449

    Article  CAS  Google Scholar 

  • Yang S, Zhi L, Tang K, Feng X, Maier J, Muellen K (2012) Efficient synthesis of heteroatom (N or S)-doped graphene based on Ultrathin graphene oxide-porous silica sheets for oxygen reduction reactions. Adv. Funct. Mater. 22:3634–3640

    Article  CAS  Google Scholar 

  • Ye L, Liu W, Shi Q, Jing C (2017) Arsenic mobilization in spent nZVI waste residue: effect of Pantoea sp. IMH. Environmental pollution 230:1081–1089

    Article  CAS  Google Scholar 

  • Zhu H, Jia Y, Wu X, Wang H (2009) Removal of arsenic from water by supported nano zero-valent iron on activated carbon. J. Hazard. Mater. 172:1591–1596

    Article  CAS  Google Scholar 

Download references

Funding

We received financial support from the Social Development Fund of Guangdong Province (No.2017A020216018) and Guangzhou Science and Technology Project (No. 201904010319).

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Hanjin Luo.

Ethics declarations

Conflict of interest

The authors declare that they have no conflict of interest.

Additional information

Responsible editor: Tito Roberto Cadaval Jr

Publisher’s note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

Electronic supplementary material

ESM 1

(DOCX 34123 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Liu, P., Liang, Q., Luo, H. et al. Synthesis of nano-scale zero-valent iron-reduced graphene oxide-silica nano-composites for the efficient removal of arsenic from aqueous solutions. Environ Sci Pollut Res 26, 33507–33516 (2019). https://doi.org/10.1007/s11356-019-06320-6

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11356-019-06320-6

Keywords

Navigation