Visible-Light-Driven Mitigation of Rhodamine B and Disinfection of E. coli Using Magnetic Recyclable Copper–Nitrogen Co-doped Titania/Strontium Ferrite/Diatomite Heterojunction Composite

  • Yan Chen
  • Qiong Wu
  • Jun WangEmail author
  • Youtao SongEmail author


The researches on the development of novel powdery photocatalysts have been conducted for decades, yet their low reusability in suspension system is still the bottleneck which hinders their large-scale application. An alternative method to overcome this issue is developing magnetic recyclable photocatalytic composite. In this work, we fabricated copper-nitrogen co-doped titania/strontium ferrite/diatomite (CN-TSD) ternary composite via sol–gel route. The physicochemical properties of the composite were characterized and analyzed, and its photocatalytic activity was investigated via the decomposition of organic dye Rhodamine B and disinfection of bacteria Escherichia coli under visible light illumination. Charge transfer occurred at the heterojunction interface between titania and strontium ferrite lowered the recombination of charge carriers, and thus promoted photodecomposition efficiency. The photodecomposition rate was further accelerated by the high adsorption performance of diatomite, due to the adsorption and decomposition synergism between photocatalytic components and diatomite. The best doping amount and catalyst dosage are determined, and the corresponding catalyst sample showed its photo-decomposition percentage as 97.1% after 2.5 h, and showed its photo-disinfection percentage of 94.0% after 2 h. CN-TSD composite could simply be separated from waterbody via an external magnet. After five turns of repetition tests, only slightly decrease of decomposition or disinfection efficiency could be observed. This composite was promising to be applied in wastewater remediation process, due to its good visible-light-driven photocatalytic activity, as well as its good reusability and stability.


Escherichia coli Rhodamine B Magnetic recyclable Diatomite Strontium ferrite 



The authors greatly acknowledge the National Science Foundation of China (31570154), Major science and technology project of water pollution control and management in China (2015ZX07202-012).

Supplementary material

10904_2019_1253_MOESM1_ESM.doc (250 kb)
Supplementary material 1 (DOC 250 kb)


  1. 1.
    R. Asahi, T. Morikawa, H. Irie, T. Ohwaki, Nitrogen-doped titanium dioxide as visible-light-sensitive photocatalyst: designs, developments, and prospects. Chem. Rev. 114, 9824–9852 (2014)CrossRefGoogle Scholar
  2. 2.
    R. Asahi, T. Morikawa, T. Ohwaki, K. Aoki, Y. Taga, Visible-light photocatalysis in nitrogen-doped titanium oxides. Science 293, 269–271 (2001)CrossRefGoogle Scholar
  3. 3.
    Y. Chen, K. Liu, Preparation and characterization of nitrogen-doped TiO2/diatomite integrated photocatalytic pellet for the adsorption-degradation of tetracycline hydrochloride using visible light. Chem. Eng. J. 302, 682–696 (2016)CrossRefGoogle Scholar
  4. 4.
    Y. Chen, K. Liu, Preparation of granulated N-doped TiO2/diatomite composite and its applications of visible light degradation and disinfection. Powder Technol. 303, 176–191 (2016)CrossRefGoogle Scholar
  5. 5.
    Y. Chen, K. Liu, Fabrication of magnetically recyclable Ce/N co-doped TiO2/NiFe2O4/diatomite ternary hybrid: Improved photocatalytic efficiency under visible light irradiation. J. Alloys Compd. 697, 161–173 (2017)CrossRefGoogle Scholar
  6. 6.
    Y. Chen, Q. Wu, N. Bu, J. Wang, Y. Song, Magnetic recyclable lanthanum-nitrogen co-doped titania/strontium ferrite/diatomite heterojunction composite for enhanced visible-light-driven photocatalytic activity and recyclability. Chem. Eng. J. 373, 192–202 (2019)CrossRefGoogle Scholar
  7. 7.
    Y. Chen, Q. Wu, L. Liu, J. Wang, Y. Song, The fabrication of floating Fe/N co-doped titania/diatomite granule catalyst with enhanced photocatalytic efficiency under visible light irradiation. Adv. Powder Technol. 30, 126–135 (2019)CrossRefGoogle Scholar
  8. 8.
    Y. Chen, Q. Wu, L. Liu, J. Wang, Y. Song, The fabrication of self-floating Ti3+/N co-doped TiO2/diatomite granule catalyst with enhanced photocatalytic performance under visible light irradiation. Appl. Surf. Sci. 467–468, 514–525 (2019)CrossRefGoogle Scholar
  9. 9.
    Y. Chen, Q. Wu, J. Wang, Y. Song, Visible-light-driven decomposition of antibiotic oxytetracycline and disinfection of Escherichia coli using magnetically recyclable lanthanum-nitrogen co-doped titania/calcium ferrite/diatomite heterojunction material. J. Ind. Eng. Chem. 77, 171–180 (2019)CrossRefGoogle Scholar
  10. 10.
    X.D. Dong, Z.M. Sun, X.W. Zhang, X. Li, S.L. Zheng, Synthesis and enhanced solar light photocatalytic activity of a C/N Co-doped TiO2/diatomite composite with exposed (001) facets. Aust. J. Chem. 71, 315–324 (2018)CrossRefGoogle Scholar
  11. 11.
    Q. Guo, Z. Zhang, X. Ma, K. Jing, M. Shen, N. Yu, J. Tang, D.D. Dionysiou, Preparation of N, F-codoped TiO2 nanoparticles by three different methods and comparison of visible-light photocatalytic performances. Sep. Purif. Technol. 175, 305–313 (2017)CrossRefGoogle Scholar
  12. 12.
    J.A. Jiménez-Miramontes, J.L. Domínguez-Arvizu, J.M. Salinas-Gutiérrez, M.J. Meléndez-Zaragoza, A. López-Ortiz, V. Collins-Martínez, Synthesis, characterization and photocatalytic evaluation of strontium ferrites towards H 2 production by water splitting under visible light irradiation. Int. J. Hydrog. Energy 42, 30257–30266 (2017)CrossRefGoogle Scholar
  13. 13.
    C.-S. Kim, J.-W. Shin, Y.-H. Cho, H.-D. Jang, H.-S. Byun, T.-O. Kim, Synthesis and characterization of Cu/N-doped mesoporous TiO2 visible light photocatalysts. Appl. Catal. A 455, 211–218 (2013)CrossRefGoogle Scholar
  14. 14.
    B. Li, H. Huang, Y. Guo, Y. Zhang, Diatomite-immobilized BiOI hybrid photocatalyst: facile deposition synthesis and enhanced photocatalytic activity. Appl. Surf. Sci. 353, 1179–1185 (2015)CrossRefGoogle Scholar
  15. 15.
    X. Liu, T. Zhang, L. Zhang, Microwave-induced catalytic application of magnetically separable strontium ferrite in the degradation of organic dyes: insight into the catalytic mechanism. Sep. Purif. Technol. 195, 192–198 (2018)CrossRefGoogle Scholar
  16. 16.
    C. Lu, Y. Chen, L. Tang, S. Wei, Y. Song, J. Wang, Preparation of Yb, N, and F doped Er3+:Y3Al5O12/TiO2 composite films for visible-light photocatalytic degradation of organic dyes. Russ. J. Phys. Chem. A 91, 1345–1357 (2017)CrossRefGoogle Scholar
  17. 17.
    K.S. Min, R.S. Kumar, J.H. Lee, K.S. Kim, S.G. Lee, Y.A. Son, Synthesis of new TiO2/porphyrin-based composites and photocatalytic studies on methylene blue degradation. Dyes Pigm. 160, 37–47 (2019)CrossRefGoogle Scholar
  18. 18.
    K.S. Min, R. Manivannan, Y.A. Son, Porphyrin Dye/TiO2 imbedded PET to improve visible-light photocatalytic activity and organosilicon attachment to enrich hydrophobicity to attain an efficient self-cleaning material. Dyes Pigm. 162, 8–17 (2019)CrossRefGoogle Scholar
  19. 19.
    N.G. Moustakas, A.G. Kontos, V. Likodimos, F. Katsaros, N. Boukos, D. Tsoutsou, A. Dimoulas, G.E. Romanos, D.D. Dionysiou, P. Falaras, Inorganic–organic core–shell titania nanoparticles for efficient visible light activated photocatalysis. Appl. Catal. B 130–131, 14–24 (2013)CrossRefGoogle Scholar
  20. 20.
    A.M. Senol, O. Metin, Y. Onganer, A facile route for the preparation of silver nanoparticles-graphene oxide nanocomposites and their interactions with pyronin Y dye molecules. Dyes Pigm. 162, 926–933 (2019)CrossRefGoogle Scholar
  21. 21.
    Z.M. Sun, C.Q. Li, X. Du, S.L. Zheng, G.F. Wang, Facile synthesis of two clay minerals supported graphitic carbon nitride composites as highly efficient visible-light-driven photocatalysts. J. Colloid Interface Sci. 511, 268–276 (2018)CrossRefGoogle Scholar
  22. 22.
    Z.M. Sun, G.Y. Yao, M.Y. Liu, S.L. Zheng, In situ synthesis of magnetic MnFe2O4/diatomite nanocomposite adsorbent and its efficient removal of cationic dyes. J. Taiwan Inst. Chem. Eng. 71, 501–509 (2017)CrossRefGoogle Scholar
  23. 23.
    F. Tian, Z. Wu, Y. Yan, B.C. Ye, D. Liu, Synthesis of visible-light-responsive Cu and N-Codoped AC/TiO2 photocatalyst through microwave irradiation. Nanoscale Res. Lett. 11, 292 (2016)CrossRefGoogle Scholar
  24. 24.
    T. Vijayaraghavan, S.P. Suriyaraj, R. Selvakumar, R. Venkateswaran, A. Ashok, Rapid and efficient visible light photocatalytic dye degradation using AFe2O4 (A = Ba, Ca and Sr) complex oxides. Mater. Sci. Eng. B 210, 43–50 (2016)CrossRefGoogle Scholar
  25. 25.
    B. Wang, F.C. de Godoi, Z. Sun, Q. Zeng, S. Zheng, R.L. Frost, Synthesis, characterization and activity of an immobilized photocatalyst: natural porous diatomite supported titania nanoparticles. J. Colloid Interface Sci. 438, 204–211 (2015)CrossRefGoogle Scholar
  26. 26.
    B. Wang, G. Zhang, X. Leng, Z. Sun, S. Zheng, Characterization and improved solar light activity of vanadium doped TiO2/diatomite hybrid catalysts. J. Hazard. Mater. 285, 212–220 (2015)CrossRefGoogle Scholar
  27. 27.
    G. Wang, X. Ma, S. Wei, S. Li, J. Qiao, J. Wang, Y. Song, Highly efficient visible-light driven photocatalytic hydrogen production from a novel Z-scheme Er3+:YAlO3/Ta2O5-V5+||Fe3+-TiO2/Au coated composite. J. Power Sources 373, 161–171 (2018)CrossRefGoogle Scholar
  28. 28.
    Q. Wu, Z. Zhang, The fabrication of magnetic recyclable nitrogen modified titanium dioxide/strontium ferrite/diatomite heterojunction nanocomposite for enhanced visible-light-driven photodegradation of tetracycline. Int. J. Hydrog. Energy 44, 8261–8272 (2019)CrossRefGoogle Scholar
  29. 29.
    Q. Wu, Z. Zhang, The preparation of self-floating Sm/N co-doped TiO2/diatomite hybrid pellet with enhanced visible-light-responsive photoactivity and reusability. Adv. Powder Technol. 30, 415–422 (2019)CrossRefGoogle Scholar
  30. 30.
    Y. Xia, F. Li, Y. Jiang, M. Xia, B. Xue, Y. Li, Interface actions between TiO2 and porous diatomite on the structure and photocatalytic activity of TiO2-diatomite. Appl. Surf. Sci. 303, 290–296 (2014)CrossRefGoogle Scholar
  31. 31.
    T. Xie, L. Xu, C. Liu, Dielectric and magnetic response of Sr–Zn ferrite composite. Rsc Adv. 3, 15856–15865 (2013)CrossRefGoogle Scholar
  32. 32.
    T. Xie, L. Xu, C. Liu, X. Zhang, A novel magnetic heterojunction photocatalyst TiO2/SrFe12O19: synthesis strategy, photocatalytic activity, and unprecedented migration mechanism of photoexcited charge carrier. Mater. Technol. 33, 582–591 (2018)CrossRefGoogle Scholar
  33. 33.
    K. Yamanaka, T. Ohwaki, T. Morikawa, Charge-carrier dynamics in Cu- or Fe-loaded nitrogen-doped TiO2 powder studied by femtosecond diffuse reflectance spectroscopy. J. Phys. Chem. C 117, 16448–16456 (2013)CrossRefGoogle Scholar
  34. 34.
    D. Zhang, L. Zhang, Ultrasonic-assisted sol-gel synthesis of rugby-shaped SrFe2O4/reduced graphene oxide hybrid as versatile visible light photocatalyst. J. Taiwan Inst. Chem. Eng. 69, 156–162 (2016)CrossRefGoogle Scholar
  35. 35.
    G.X. Zhang, A.K. Song, Y.W. Duan, S.L. Zheng, Enhanced photocatalytic activity of TiO2/zeolite composite for abatement of pollutants. Microporous Mesoporous Mater. 255, 61–68 (2018)CrossRefGoogle Scholar
  36. 36.
    Z. Zhang, Y. Xu, X. Ma, F. Li, D. Liu, Z. Chen, F. Zhang, D.D. Dionysiou, Microwave degradation of methyl orange dye in aqueous solution in the presence of nano-TiO2-supported activated carbon (supported-TiO2/AC/MW). J. Hazard. Mater. 209–210, 271–277 (2012)CrossRefGoogle Scholar
  37. 37.
    X.D. Zhu, Y.J. Wang, R.J. Sun, D.M. Zhou, Photocatalytic degradation of tetracycline in aqueous solution by nanosized TiO2. Chemosphere 92, 925–932 (2013)CrossRefGoogle Scholar

Copyright information

© Springer Science+Business Media, LLC, part of Springer Nature 2019

Authors and Affiliations

  1. 1.College of EnvironmentLiaoning UniversityShenyangPeople’s Republic of China
  2. 2.College of ChemistryLiaoning UniversityShenyangPeople’s Republic of China

Personalised recommendations