Skip to main content
SpringerLink
Log in

Preparation of CuOx@ZnFe-LDH composites and photocatalytic degradation of 4-nitrophenol by activated persulfate

  • Published:
Journal of Materials Science: Materials in Electronics Aims and scope Submit manuscript

Abstract

In order to meet the current challenges of wastewater treatment, a novel, environment-friendly, efficient and economical treatment method has always been an ideal choice for the degradation of organic pollutants. In this work, active and stable CuOx@ZnFe-LDH composite was prepared via co-precipitation method. A series of characterization methods were used to investigate the structural characteristics of the obtained products. The photocatalytic performance of the prepared composites were evaluate by degrading 4-nitrophenol under mild conditions. Besides, with the addition of persulfate, the photocatalytic degradation activity was greatly enhanced due to the synergistic effect of catalysts and ultraviolet light on persulfate activation. The results showed that CuOx@ZnFe-LDH composite obtained the best photocatalytic performance compared with ZnFe-LDH and ZnFe-CLDH, which could completely degrade 10 mg/L of 4-nitrophenol in less than 60 min. After four consecutive cycles CuOx@ZnFe-LDH composite could still remain remarkable reusability and stability. In addition, a possible photocatalytic degradation mechanism was proposed according to the characterization and experimental results. The CuOx@ZnFe-LDH composite was expected to be an efficient catalyst for energy conversion and environmental treatment. This work also was expected to provide a new idea for designing new type of catalysts for organic pollutants treatment.

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

Access this article

Log in via an institution

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
Fig. 7
Fig. 8
Fig. 9
Fig. 10
Fig. 11
Fig. 12
Fig. 13

Similar content being viewed by others

References

  1. P. Hu, M. Long, Cobalt-catalyzed sulfate radical-based advanced oxidation: A review on heterogeneous catalysts and applications. Appl. Catal. B 181, 103–117 (2016)

    Article  CAS  Google Scholar 

  2. A.R. Ribeiro, O.C. Nunes, M.F. Pereira, A.M. Silva, An overview on the advanced oxidation processes applied for the treatment of water pollutants defined in the recently launched Directive. Environ. Int. 75, 33–51 (2015)

    Article  CAS  Google Scholar 

  3. F. Crapulli, D. Santoro, M.R. Sasges, A.K. Ray, Mechanistic modeling of vacuum UV advanced oxidation process in an annular photoreactor. Water Res. 64, 209–225 (2014)

    Article  CAS  Google Scholar 

  4. M.X. Luo, L. Lv, G.W. Deng, W. Yao, Y. Ruan, X.X. Li, A.H. Xu, The mechanism of bound hydroxyl radical formation and degradation pathway of Acid Orange II in Fenton-like Co2+-HCO3 – system. Appl. Catal. A 469, 198–205 (2014)

    Article  CAS  Google Scholar 

  5. L.A. De, R.F. Dantas, S. Esplugas, Assessment of iron chelates efficiency for photo-Fenton at neutral PH. Water Res 61, 232–242 (2014)

    Article  Google Scholar 

  6. S.A. Messele, O.S.G.P. Soares, J.J.M. Órfão, C. Bengoa, F. Stüber, A. Fortuny, A. Fabregat, J. Font, Effect of activated carbon surface chemistry on the activity of ZVI/AC catalysts for Fenton-like oxidation of phenol. Catal. Today 240, 73–79 (2015)

    Article  CAS  Google Scholar 

  7. Y.F. Huang, Y.H. Huang, Identification of produced powerful radicals involved in the mineralization of bisphenol A using a novel UV-Na2S2O8/H2O2-Fe(II,III) two-stage oxidation process. J. Hazard. Mater. 162, 1211–1216 (2009)

    Article  CAS  Google Scholar 

  8. Y.Q. Gao, N.Y. Gao, Y. Deng, D.Q. Yin, Y.S. Zhang, Degradation of florfenicol in water by UV/Na2S2O8 process. Environ. Sci. Pollut. Res. 22, 8693–8701 (2015)

    Article  CAS  Google Scholar 

  9. M.H. Nie, Y. Yang, Z.J. Zhang, C.X. Yan, X.N. Wang, H.J. Li, W.B. Dong, Degradation of chloramphenicol by thermally activated persulfate in aqueous solution. Chem. Eng. J. 246, 373–382 (2014)

    Article  CAS  Google Scholar 

  10. X.G. Duan, C. Su, L. Zhou, H.Q. Sun, A. Suvorova, T.W. Odedairo, Z.H. Zhu, Z.P. Shao, S.B. Wang, Surface controlled generation of reactive radicals from persulfate by carbocatalysis on nanodiamonds. Appl. Catal. B: Environ. 194, 7–15 (2016)

    Article  CAS  Google Scholar 

  11. A. Jawad, J. Lang, Z.W. Liao, A. Khan, J. Ifthikar, Z.N. Lv, S.J. Long, Z.L. Chen, Z.Q. Chen, Activation of persulfate by CuOx@Co-LDH: a novel heterogeneous system for contaminant degradation with broad pH window and controlled leaching. Chem. Eng. J. 335, 548–559 (2017)

    Article  Google Scholar 

  12. C. Gong, F. Chen, Q. Yang, K. Luo, F.B. Yao, S.N. Wang, X.L. Wang, J.W. Wu, X.M. Li, D.B. Wang, G.M. Zeng, Heterogeneous activation of peroxymonosulfate by Fe-Co layered doubled hydroxide for efficient catalytic degradation of Rhoadmine B. Chem. Eng. J. 321, 222–232 (2017)

    Article  CAS  Google Scholar 

  13. Y.P. Zhu, R.L. Zhu, G.Q. Zhu, M.M. Wang, Y.N. Chen, J.X. Zhu, Y.F. Xi, H.P. He, Plasmonic Ag coated Zn/Ti-LDH with excellent photocatalytic activity. Appl. Surf. Sci. 433, 458–467 (2017)

    Article  Google Scholar 

  14. Y.H. Guan, J. Ma, X.C. Li, J.Y. Fang, L.W. Chen, Influence of pH on the formation of sulfate and hydroxyl radicals in the UV/peroxymonosulfate system. Environ. Sci. Technol. 45, 9308–9314 (2011)

    Article  CAS  Google Scholar 

  15. M. Pagano, A. Volpe, A. Lopez, G. Mascolo, R. Ciannarella, Degradation of chlorobenzene by Fenton-like processes using zero-valent iron in the presence of Fe3+ and Cu2+. Environ. Technol. 32, 155–165 (2011)

    Article  CAS  Google Scholar 

  16. W.C. Cheng, C.C. Ding, X.X. Wang, Z.Y. Wu, Y.B. Sun, S.H. Yu, T.T. Hayat, X.K. Wang, Competitive sorption of As(V) and Cr(VI) on carbonaceous nanofibers. Chem. Eng. J. 293, 311–318 (2016)

    Article  CAS  Google Scholar 

  17. X. Huang, M. Su, J.Z. Zhou, W.K. Shu, Z.F. Huang, N.Y. Gao, G.R. Qian, Novel activation of persulfate by its intercalation into Mg/Al-layered double hydroxide: Enhancement of non-radical oxidation. Chem. Eng. J. 328, 66–73 (2017)

    Article  CAS  Google Scholar 

  18. Y. Yang, G.L. Fan, F. Li, Synthesis of novel marigold-like carbonate-type Mg–Al layered double hydroxide micro-nanostructures via a two-step intercalation route. Mater. Lett. 116, 203–205 (2014)

    Article  CAS  Google Scholar 

  19. A. Jawad, X. Lu, Z. Chen, G. Yin, Degradation of chlorophenols by supported Co-Mg-Al layered double hydrotalcite with bicarbonate activated hydrogen peroxide. J. Phys. Chem. A 118, 10028–10035 (2014)

    Article  CAS  Google Scholar 

  20. G.Q. Zhao, J. Zou, C.F. Li, J.G. Yu, X.Y. Jiang, Y.J. Zheng, W.J.H. Hu, F.P. Jiao, Enhanced photocatalytic degradation of rhodamine B, methylene blue and 4-nitrophenol under visible light irradiation using TiO2/MgZnAl layered double hydroxide. J. Mater. Sci. 29, 7002–7014 (2018)

    CAS  Google Scholar 

  21. G.Q. Zhao, C.F. Li, X. Wu, J.G. Yu, X.Y. Jiang, W.J.H. Hu, F.P. Jiao, Reduced graphene oxide modified NiFe-calcinated layered double hydroxides for enhanced photocatalytic removal of methylene blue. Appl. Surf. Sci. 434, 251–259 (2018)

    Article  CAS  Google Scholar 

  22. G. Carja, A. Nakajima, S. Dranca, C. Dranca, K. Okada, TiO2/ZnLDH as a Self-Assembled Nanocomposite with Photoresponsive Properties. J. Phys. Chem. C 114, 14722–14728 (2010)

    Article  CAS  Google Scholar 

  23. Y. Nie, Q. Yan, S. Chen, D. O’Hare, Q. Wang, CuTi-LDH derived NH3-SCR catalysts with highly dispersed CuO active phase and improved SO2, resistance. Catal. Commun. 97, 47–50 (2017)

    Article  CAS  Google Scholar 

  24. W. Zhao, C. Liang, S. Xing, Enhanced Photocatalytic and Fenton-Like Performance of CuOx Decorated ZnFe2O4, ACS Appl. Mater. Interfaces 9, 41927–41936 (2017)

    Article  CAS  Google Scholar 

  25. M. Mumtaz, S. Naeem, K. Nadeem, F. Naeem, A. Jabbar, Y.R. Zheng, NawazishA. Khan, M. Imran, Study of nano-sized (ZnFe2O4)y, particles/CuTl-1223 superconductor composites. Solid State Sci. 22, 21–26 (2013)

    Article  CAS  Google Scholar 

  26. Y. Lei, C.S. Chen, Y.J. Tu, Y. Ding, Heterogeneous degradation of organic pollutants by persulfate activated by CuO-Fe3O4: mechanism, stability and effects of pH and bicarbonate ions Environ. Sci. Technol. 49, 6838–6845 (2015)

    Article  CAS  Google Scholar 

  27. D. Fu, G. Han, C. Meng, Size-controlled synthesis and photocatalytic degradation properties of nano-sized ZnO nanorods. Mater. Lett. 72, 53–56 (2012)

    Article  CAS  Google Scholar 

  28. M. Abdel-Baki, A.M. Salem, F.A. Abdel-Wahab, F. EI-Diasty, Bond character, optical properties and ionic conductivity of Li2O/B2O3/SiO2/Al2O3, glass: Effect of structural substitution of Li2O for LiCl. J. Non-Cryst. Solids 354, 4527–4533 (2008)

    Article  CAS  Google Scholar 

  29. M.Y. Ding, M.H. Qiu, T.J. Wang, L.L. Ma, C.Z. Wu, J.G. Liu, Effect of iron promoter on structure and performance of CuMnZnO catalyst for higher alcohols synthesis. Appl. Energy 97, 543–547 (2012)

    Article  CAS  Google Scholar 

  30. S. Schnell, C. Mendoza, The condition for pseudo-first-order kinetics in enzymatic reactions is independent of the initial enzyme concentration. Biophys. Chem. 107, 165–174 (2004)

    Article  CAS  Google Scholar 

  31. G.H. Zhang, B.Z. Lin, Y.Q. Qiu, L.W. He, Y.L. Chen, B.F. Gao, Hightly efficient visible-light-driven photocatalytic hydrogen generation by immobilizing CdSe nanocrystals on ZnCr-layered double hydroxide nanosheets. Int. J. Hydrog. Energy 40, 4758–4765 (2015)

    Article  CAS  Google Scholar 

  32. G.Q. Zhao, D. Zhang, Y. Jin, Y. Xie, W.J.H. Hu, F.P. Jiao, Multi-walled carbon nanotubes modified Bi2S3 microspheres for enhanced photocatalytic decomposition efficiency. Ceram. Int. 43, 15080–15088 (2017)

    Article  CAS  Google Scholar 

  33. M.F.D. Almeida, C.R. Bellato, A.H. Mounteer, S.O. Ferreira, J.L. Milagres, L.D.L. Miranda, Enhanced photocatalytic activity of TiO2 -impregnated with MgZnAl mixed oxides obtained from layered double hydroxides for phenol degradation. Appl. Surf. Sci. 357, 1765–1775 (2015)

    Article  Google Scholar 

  34. C. Ma, F.H. Wang, C. Zhang, Z.G. Yu, J.J. Wei, Z.Z. Yang, Y.Q. Li, Z.H. Li, M.Y. Zhu, L.Q. Shen, G.M. Zeng, Photocatalytic decomposition of Congo red under visible light irradiation using MgZnCr-TiO2, layered double hydroxide. Chemosphere 168, 80–90 (2017)

    Article  CAS  Google Scholar 

  35. A. Wang, W. Guo, F. Hao, X. Yue, Y. Leng, Degradation of Acid Orange 7 in aqueous solution by zero-valent aluminum under ultrasonic irradiation. Ultrason. Sonochem. 21, 572–575 (2014)

    Article  CAS  Google Scholar 

  36. L.G. Devi, S.G. Kumar, K.M. Reddy, C. Munikrishnappa, Photo degradation of Methyl Orange an azo dye by Advanced Fenton Process using zero valent metallic iron: influence of various reaction parameters and its degradation mechanism. J. Hazard. Mater. 164, 459–467 (2009)

    Article  Google Scholar 

  37. P. Paja, M. Bensimon, U. Klehm, P. Albers, D. Laub, L. Kiwi-Minsker, A. Renken, J. Kiwi, Highly dispersed PTFE/Co3O4 flexible films as photocatalyst showing fast kinetic performance for the discoloration of azo-dyes under solar irradiation. J. Photochem. Photobiol. A 187, 332–338 (2007)

    Article  Google Scholar 

  38. G.D. Fang, D.D. Dionysiou, Y. Wang, S.R. Al-Abed, D.M. Zhou, Sulfate radical-based degradation of polychlorinated biphenyls: effects of chloride ion and reaction kinetics, J. Hazard. Mater. 227, 394–401 (2012)

    Google Scholar 

  39. X.L. Shi, C.L. Zou, G.H. Pan, H. Gong, L. Xu, Y. Zhou, Atomically smooth gallium nitride surface prepared by chemical-mechanical polishing with S2O8 2–-Fe2+ based slurry. Tribol. Int. 110, 441–450 (2016)

    Article  Google Scholar 

  40. D.P. Cassidy, V.J. Srivastava, F.J. Dombrowski, J.W. Lingle, Combining in situ, chemical oxidation, stabilization, and anaerobic bioremediation in a single application to reduce contaminant mass and leachability in soil. J. Hazard. Mater. 297, 347–355 (2015)

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 21476269, 21776319). The authors also thank the Fundamental Research Funds for the Central Universities of Central South University (No.2017zzts777, 2018zzts377) and the Open-End Fund for the Valuable and Precision Instruments of Central South University (No. CSUZC201832) for the financial supports of this work.

Author information

Authors and Affiliations

  1. School of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, People’s Republic of China

    Caifeng Li, Guoqing Zhao, Lukai Liu, Jingang Yu, Xinyu Jiang & Feipeng Jiao

Authors
  1. Caifeng Li
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Guoqing Zhao
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Lukai Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Jingang Yu
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Xinyu Jiang
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Feipeng Jiao
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Feipeng Jiao.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Li, C., Zhao, G., Liu, L. et al. Preparation of CuOx@ZnFe-LDH composites and photocatalytic degradation of 4-nitrophenol by activated persulfate. J Mater Sci: Mater Electron 29, 19461–19471 (2018). https://doi.org/10.1007/s10854-018-0076-z

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s10854-018-0076-z

Search

Navigation