Journal of Materials Science

, Volume 53, Issue 1, pp 613–625 | Cite as

Preparation of TiO2/graphene composite with appropriate N-doping ratio for humic acid removal

Composites
First Online:
Received:
Accepted:

Abstract

Humic acid (HA), which contains abundant carboxyl groups and hydroxyl groups, is one of the major constituents of dissolved organic matter. The increase of HA in natural waters worldwide has caused great trouble in water treatment and water health. Photocatalysis is a promising technology for degrading HA. In this study, graphene oxide, TiO2 and different amounts of urea (nitrogen source) were mixed to dope nitrogen into TiO2 and RGO simultaneously and form N-TG to remove HA from aqueous solution. To confirm the effect of the N-doping and determine the best N-doping ratio for N-TG, various characterization and HA removal tests using different samples were conducted, we found the best N-doping ratio is ~1.46 at.%. The influences of the initial HA concentration, temperature and pH on HA removal performance were measured and discussed, notably, temperature range of 25–35 °C and neutral solution are more fitable for HA removal. HA removal is in the synergistic effect of adsorption and degradation. The presence of RGO almost doubles the adsorption ability of the composite, which does have a significant improvement on HA removal efficiency. Pretreated in darkness has an extra 2% improvement on HA removal efficiency.

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

Notes

Acknowledgements

This work was supported by the National Natural Science Foundation of China (Nos. 51678213 and 51578209), and a Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions.

Compliance with ethical standards

Conflict of interest

The authors declare that they have no conflict of interest.

Supplementary material

10853_2017_1509_MOESM1_ESM.docx (96 kb)
Supplementary material 1 (DOCX 96 kb)

References

  1. 1.
    Delpla I, Jung AV, Baures E, Clement M, Thomas O (2009) Impacts of climate change on surface water quality in relation to drinking water production. Environ Int 35:1225–1233CrossRefGoogle Scholar
  2. 2.
    Wu X, Tan X, Yang S, Wen T, Guo H, Wang X, Xu A (2013) Coexistence of adsorption and coagulation processes of both arsenate and NOM from contaminated groundwater by nanocrystallined Mg/Al layered double hydroxides. Water Res 47:4159–4168CrossRefGoogle Scholar
  3. 3.
    Jiang Y, Goodwill JE, Tobiason JE, Reckhow DA (2016) Impacts of ferrate oxidation on natural organic matter and disinfection byproduct precursors. Water Res 96:114–125CrossRefGoogle Scholar
  4. 4.
    Broo AE, Berghult B, Hedberg T (1998) Copper corrosion in water distribution systems—the influence of natural organic matter (NOM) on the solubility of copper corrosion products. Corros Sci 40:1479–1489CrossRefGoogle Scholar
  5. 5.
    Zhang J, Gong J, Zenga G, Ou X, Jiang Y, Chang Y, Guo M, Zhang C et al (2016) Simultaneous removal of humic acid/fulvic acid and lead from landfill leachate using magnetic graphene oxide. Appl Surf Sci 370:335–350CrossRefGoogle Scholar
  6. 6.
    Xu H, Jiao R, Xiao F, Wang D (2014) Effects of different coagulants in treatment of TiO2-humic acid (HA) water and the aggregate characterization in different coagulation conditions. Colloid Surf A 446:213–223CrossRefGoogle Scholar
  7. 7.
    Dong C, Chen W, Liu C (2014) Preparation of novel magnetic chitosan nanoparticle and its application for removal of humic acid from aqueous solution. Appl Surf Sci 292:1067–1076CrossRefGoogle Scholar
  8. 8.
    Lin T, Lu Z, Chen W (2015) Interaction mechanisms of humic acid combined with calcium ions on membrane fouling at different conditions in an ultrafiltration system. Desalination 357:26–35CrossRefGoogle Scholar
  9. 9.
    Thuyavan YL, Anantharaman N, Arthanareeswaran G, Ismail AF (2014) Adsorptive removal of humic acid by zirconia embedded in a poly(ether sulfone) membrane. Ind Eng Chem Res 53:11355–11364CrossRefGoogle Scholar
  10. 10.
    Lim SM, Chiang K, Amal R, Fabris R, Chow C, Drikas M (2007) A study on the removal of humic acid using advanced oxidation processes. Sep Sci Technol 42:1391–1404CrossRefGoogle Scholar
  11. 11.
    Lee PF, Sun DD, Leckie JO (2007) Adsorption and photodegradation of humic acids by nano-structured TiO2 for water treatment. J Adv Oxid Technol 10:72–78Google Scholar
  12. 12.
    Birben NC, Uyguner-Demirel CS, Sen Kavurmaci S, Gurkan YY, Turkten N, Cinar Z, Bekbolet M (2017) Application of Fe-doped TiO2 specimens for the solar photocatalytic degradation of humic acid. Catal Today 281:78–84CrossRefGoogle Scholar
  13. 13.
    Liu Y, Pei F, Lu R, Xu S, Cao S (2014) TiO2/N-graphene nanocomposite via a facile in situ hydrothermal sol–gel strategy for visible light photodegradation of eosin Y. Mater Res Bull 60:188–194CrossRefGoogle Scholar
  14. 14.
    Zhang Y, Pan C (2011) TiO2/graphene composite from thermal reaction of graphene oxide and its photocatalytic activity in visible light. J Mater Sci 46:2622–2626. doi: 10.1007/s10853-010-5116-x CrossRefGoogle Scholar
  15. 15.
    Chen X, Mao SS (2007) Titanium dioxide nanomaterials: synthesis, properties, modifications, and applications. Chem Rev 107:2891–2959CrossRefGoogle Scholar
  16. 16.
    Chen W, Ye T, Xu H, Chen T, Geng N, Gao X (2017) An ultrafiltration membrane with enhanced photocatalytic performance from grafted N-TiO2/graphene oxide. Rsc Adv 7:9880–9887CrossRefGoogle Scholar
  17. 17.
    Johra FT, Jung W (2015) RGO–TiO2–ZnO composites: synthesis, characterization, and application to photocatalysis. Appl Catal A Gen 491:52–57CrossRefGoogle Scholar
  18. 18.
    Pelaez M, Nolan NT, Pillai SC, Seery MK, Falaras P, Kontos AG, Dunlop PSM, Hamilton JWJ et al (2012) A review on the visible light active titanium dioxide photocatalysts for environmental applications. Appl Catal B Environ 125:331–349CrossRefGoogle Scholar
  19. 19.
    Wang R, Wu Q, Lu Y, Liu H, Xia Y, Liu J, Yang D, Huo Z et al (2014) Preparation of nitrogen-doped TiO2/graphene nanohybrids and application as counter electrode for dye-sensitized solar cells. Acs Appl Mater Inter 6:2118–2124CrossRefGoogle Scholar
  20. 20.
    Li Z, Zhang H, Liu Q, Sun L, Stanciu L, Xie J (2013) Fabrication of high-surface-area graphene/polyaniline nanocomposites and their application in supercapacitors. Acs Appl Mater Inter 5:2685–2691CrossRefGoogle Scholar
  21. 21.
    Meyer JC, Geim AK, Katsnelson MI, Novoselov KS, Booth TJ, Roth S (2007) The structure of suspended graphene sheets. Nature 446:60–63CrossRefGoogle Scholar
  22. 22.
    Thuy-Duong N, Viet HP, Shin EW, Hai-Dinh P, Kim S, Chung JS, Kim EJ, Hur SH (2011) The role of graphene oxide content on the adsorption-enhanced photocatalysis of titanium dioxide/graphene oxide composites. Chem Eng J 170:226–232CrossRefGoogle Scholar
  23. 23.
    Duru I, Ege D, Kamali AR (2016) Graphene oxides for removal of heavy and precious metals from wastewater. J Mater Sci 51:6097–6116. doi: 10.1007/s10853-016-9913-8 CrossRefGoogle Scholar
  24. 24.
    Xue Z, Zhao S, Zhao Z, Li P, Gao J (2016) Thermodynamics of dye adsorption on electrochemically exfoliated graphene. J Mater Sci 51:4928–4941. doi: 10.1007/s10853-016-9798-6 CrossRefGoogle Scholar
  25. 25.
    Jia Z, Li H, Zhao Y, Frazer L, Qian B, Borguet E, Ren F, Dikin DA (2017) Electrical and mechanical properties of poly(dopamine)-modified copper/reduced graphene oxide composites. J Mater Sci 52:11620–11629. doi: 10.1007/s10853-017-1307-z CrossRefGoogle Scholar
  26. 26.
    Liu S, Sun H, Liu S, Wang S (2013) Graphene facilitated visible light photodegradation of methylene blue over titanium dioxide photocatalysts. Chem Eng J 214:298–303CrossRefGoogle Scholar
  27. 27.
    Pan X, Yang M, Tang Z, Xu Y (2014) Noncovalently functionalized graphene-directed synthesis of ultralarge graphene-based TiO2 nanosheet composites: tunable morphology and photocatalytic applications. J Phys Chem C 118:27325–27335CrossRefGoogle Scholar
  28. 28.
    Qian W, Greaney PA, Fowler S, Chiu S, Goforth AM, Jiao J (2014) Low-temperature nitrogen doping in ammonia solution for production of N-doped TiO2-hybridized graphene as a highly efficient photocatalyst for water treatment. Acs Sustain Chem Eng 2:1802–1810CrossRefGoogle Scholar
  29. 29.
    Li J, Chen LX, Li X, Zhang CC, Zeng FL (2015) Hollow organosilica nanospheres prepared through surface hydrophobic layer protected selective etching. Appl Surf Sci 340:126–131CrossRefGoogle Scholar
  30. 30.
    Barrejon M, Primo A, Gomez-Escalonilla MJ, Fierro JLG, Garcia H, Langa F (2015) Covalent functionalization of N-doped graphene by N-alkylation. Chem Commun 51:16916–16919CrossRefGoogle Scholar
  31. 31.
    Lherbier A, Botello-Mendez AR, Charlier J (2013) Electronic and transport properties of unbalanced sublattice N-doping in graphene. Nano Lett 13:1446–1450CrossRefGoogle Scholar
  32. 32.
    Meng F, Li J, Cushing SK, Zhi M, Wu N (2013) Solar hydrogen generation by nanoscale p–n junction of p-type molybdenum disulfide/n-type nitrogen-doped reduced graphene oxide. J Am Chem Soc 135:10286–10289CrossRefGoogle Scholar
  33. 33.
    Liu C, Zhang L, Liu R, Gao Z, Yang X, Tu Z, Yang F, Ye Z et al (2016) Hydrothermal synthesis of N-doped TiO2 nanowires and N-doped graphene heterostructures with enhanced photocatalytic properties. J Alloy Compd 656:24–32CrossRefGoogle Scholar
  34. 34.
    Dawlaty JM, Shivaraman S, Strait J, George P, Chandrashekhar M, Rana F, Spencer MG, Veksler D et al (2008) Measurement of the optical absorption spectra of epitaxial graphene from terahertz to visible. Appl Phys Lett 93:193–197CrossRefGoogle Scholar
  35. 35.
    Zhang H, Gu W, Li M, Fang W, Li Z, Tao W (2015) Influence of environmental factors on the adsorption capacity and thermal conductivity of silica nano-porous materials. J Nanosci Nanotechnol 15:3048–3054CrossRefGoogle Scholar
  36. 36.
    Pierrard JC, Rimbault J, Aplincourt M (2002) Experimental study and modelling of lead solubility as a function of pH in mixtures of ground waters and cement waters. Water Res 36:879–890CrossRefGoogle Scholar
  37. 37.
    Kosmulski M (2002) The significance of the difference in the point of zero charge between rutile and anatase. Adv Colloid Interface 99:255–264CrossRefGoogle Scholar
  38. 38.
    Kipton H, Powell J, Town RM (1992) Solubility and fractionation of humic acid: effect of pH and ionic medium. Anal Chim Acta 267:47–54CrossRefGoogle Scholar
  39. 39.
    Yuan R, Zhou B (2016) Effect of ion (Al, Fe and Zn) co-doped TiO2 nanotubes on photocatalytic degradation of humic acids under UV/ozonation for drinking water purification. Water Sci Tech W Sup 16:237–244CrossRefGoogle Scholar
  40. 40.
    Hidaka H, Honjo H, Horikoshi S, Serpone N (2003) Photocatalyzed degradations on a TiO2-coated quartz crystal microbalance. I. Adsorption/desorption processes in the degradation of phenol and catechol. New J Chem 27:1371–1376CrossRefGoogle Scholar
  41. 41.
    Zhou Q, Zhong Y, Chen X, Liu J, Huang X, Wu Y (2014) Adsorption and photocatalysis removal of fulvic acid by TiO2-graphene composites. J Mater Sci 49:1066–1075. doi: 10.1007/s10853-013-7784-9 CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC 2017

Authors and Affiliations

  1. 1.Ministry of Education Key Laboratory of Integrated Regulation and Resource Development on Shallow LakesHohai UniversityNanjingPeople’s Republic of China
  2. 2.College of EnvironmentHohai UniversityNanjingPeople’s Republic of China

Personalised recommendations