Advertisement

Photocatalytic Activity of La-Containing Mixed- Metal Oxides Derived from Layered Double Hydroxides to Degrade Methylene Blue in the Presence of H2O2

  • Minhong XuEmail author
  • Mengxia Qian
  • Guoxiang Pan
  • Yuhua Guo
  • Tao Wu
Article
  • 10 Downloads

Abstract

Photocatalytic degradation of polluted water by means of minerals, such as clays and oxides, which have surfaces that exhibit catalytic properties, has been suggested to be a useful new strategy to promote both organic and inorganic pollutant degradation. Nevertheless, much still remains to be studied about the capability of mixed metal oxides derived from lanthanum-containing layered double hydroxides to promote pollutant removal by means of photocatalytic degradation with the mineral surfaces. The objective of the present study was to investigate the synthesis of ternary MgAlLa mixed-metal oxides (MgAlLa-M) with various Mg/Al/La molar ratios through a hydrotalcite-like precursor route by co-precipitation of appropriate amounts of metal salts from homogeneous solution, followed by calcination at 600°C. The crystal structure, surface morphology, and optical properties of the samples were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), Fourier-transform infrared spectroscopy (FTIR), and UV-Vis diffuse reflectance spectroscopy (DRS). Analysis by XRD showed that MgO, La2O3, MgAl2O4, and La10Al4O21 phases coexisted in calcined samples as MgAlLa-M. The samples showed a small band gap of 3.11–3.35 eV according to DRS. The photocatalytic activities of the samples were evaluated by degradation of methylene blue (MB) under visible light irradiation. MgAlLa-M had better photocatalytic properties than hydrotalcite precursors, and the MgAlLa-0.5-M possessed the best photocatalytic activity. The photocatalytic degradation efficiency of MB dye with MgAlLa-0.5-M under visible light irradiation for 1 h was 99.89% in the presence of H2O2, which exceeded the binary MgAl-M (84.06%) under the same conditions. The high photocatalytic activity of the sample was attributed to the addition of La(III). In addition, the possible mechanism of photocatalytic degradation of MB by MgAlLa-M was discussed. The results showed that •O2 plays a major role in the MgAlLa-0.5-M/H2O2 system.

Keywords

Co-precipitation method Hydrotalcites Methylene Blue Mixed metal oxides Photocatalytic activity 

Notes

Acknowledgements

This work was supported financially by the Zhejiang Provincial Natural Science Foundation of China (LQ19E040001 and LY14B060006).

References

  1. Ahmed, A. A. A., Talib, Z. A., Hussein, M. Z. B., & Zakaria, A. (2012). Improvement of the crystallinity and photocatalytic property of zinc oxide as calcination product of Zn–Al layered double hydroxide. Journal of Alloys and Compounds,539, 154–160.  https://doi.org/10.1016/j.jallcom.2012.05.093.CrossRefGoogle Scholar
  2. Baliarsingh, N., Mohapatra, L., & Parida, K. (2013). Design and development of a visible light harvesting Ni–Zn/Cr–CO3 2 LDH system for hydrogen evolution. Journal of Materials Chemistry A,13, 4236–4243.  https://doi.org/10.1039/C2TA00933A.CrossRefGoogle Scholar
  3. Carvalho, D. C., Ferreira, N. A., Filho, J. M., Ferreira, O. P., Soares, J. M., & Oliveira, A. C. (2015). Ni–Fe and Co–Fe binary oxides derived from layered double hydroxides and their catalytic evaluation for hydrogen production. Catalysis Today,250, 155–165.  https://doi.org/10.1016/j.cattod.2014.08.010.CrossRefGoogle Scholar
  4. Carja, G., Dartu, L., Okada, K., & Fortunato, E. (2013). Nanoparticles of copper oxide on layered double hydroxides and the derived solid solutions as wide spectrum active nano-photocatalysts. Chemical Engineering Journal,222, 60–66.  https://doi.org/10.1016/j.cej.2013.02.039.CrossRefGoogle Scholar
  5. Chen, Y., Zhou, S., Li, F., Wei, J., Dai, Y., & Chen, Y. (2011). Fluorescence and phase transitions of Mg-Al-Eu ternary layered double hydroxides-dependence on annealing. Clay Minerals,46, 487–493.  https://doi.org/10.1007/s10895-011-0857-8.CrossRefGoogle Scholar
  6. Chen, J., Lei, Z., Wang, A., Liu, J., Wu, X., Chang, T., Zhang, Y., & Li, M. (2015). Structure analysis and fluorescence of Mg-Al-Tb ternary layered double hydroxides and their calcined products. Journal of Metals,67, 354–360.  https://doi.org/10.1007/s11837-014-1210-x.CrossRefGoogle Scholar
  7. Curtius, H., & Ufer, K. (2007). Eu incorporation behavior of a Mg-Al-Cl layered double hydroxide. Clays and Clay Minerals,55, 354–360.  https://doi.org/10.1346/ccmn.2007.0550403.CrossRefGoogle Scholar
  8. Fan, G., Sun, W., Wang, H., & Li, F. (2011). Visible-light-induced heterostructured Zn–Al–In mixed metal oxide nanocomposite photocatalysts derived from a single precursor. Chemical Engineering Journal,174, 467–474.  https://doi.org/10.1016/j.cej.2011.09.054.CrossRefGoogle Scholar
  9. Ferreira, O. P., Alves, O. L., Gouveia, D. X., Filho, A. G. S., Paiva, J. A. C. D., & Filho, J. M. (2004). Thermal decomposition and structural reconstruction effect on Mg–Fe-based hydrotalcite compounds. Journal of Solid State Chemistry,177, 3058–3069.  https://doi.org/10.1016/j.jssc.2004.04.030.CrossRefGoogle Scholar
  10. Heredia, A. C., Oliva, M. I., Agú, U., Zandalazini, C. I., Marchetti, S. G., Herrero, E. R., & Crivello, M. E. (2013). Synthesis, characterization and magnetic behavior of Mg–Fe–Al mixed oxides based on layered double hydroxide. Journal of Magnetism and Magnetic Materials,342, 38–46.  https://doi.org/10.1016/j.jmmm.2013.04.057.CrossRefGoogle Scholar
  11. Hussain, M., Russo, N., & Saracco, G. (2011). Photocatalytic abatement of VOCs by novel optimized TiO2 nanoparticles. Chemical Engineering Journal,166, 138–149.  https://doi.org/10.1016/j.cej.2010.10.040.CrossRefGoogle Scholar
  12. Ishibashi, K. I., Fujishima, A., Watanabe, T., & Hashimoto, K. (2000). Quantum yields of active oxidative species formed on TiO2 photocatalyst. Journal of Photochemistry and Photobiology A-Chemistry,134, 139–142.  https://doi.org/10.1016/S1010-6030(00)00264-1.CrossRefGoogle Scholar
  13. Kong, Y., Li, Y., Hu, G., Jing, L., Pan, D., Dong, D., et al. (2018). Preparation of polystyrene-b-poly(ethylene/propylene)-b-polystyrene grafted glycidyl methacrylate and its compatibility with recycled polypropylene/recycled high impact polystyrene blends. Polymer,145, 232–241.  https://doi.org/10.1016/j.polymer.2018.05.017.CrossRefGoogle Scholar
  14. Lan, M., Fan, G., Yang, L., & Li, F. (2014). Enhanced visible-light-induced photocatalytic performance of a novel ternary semiconductor coupling system based on hybrid Zn–In mixed metal oxide/g-C3N4 composites. RSC Advances,5, 5725–5734.  https://doi.org/10.1039/C4RA07073A.CrossRefGoogle Scholar
  15. Li, S. D., Wang, H. S., Li, W. M., Wu, X. F., Tang, W. X., & Chen, Y. F. (2015). Effect of Cu substitution on promoted benzene oxidation over porous CuCo-based catalysts derived from layered double hydroxide with resistance of water vapor. Applied Catalysis B Environmental,166-167, 260–269.  https://doi.org/10.1016/j.apcatb.2014.11.040.CrossRefGoogle Scholar
  16. Li, Y., Wu, X., Song, J., Li, J., Shao, Q., Cao, N., et al. (2017). Reparation of recycled acrylonitrile- butadiene-styrene by pyromellitic dianhydride: reparation performance evaluation and property analysis. Polymer,124, 41–47.  https://doi.org/10.1016/j.polymer.2017.07.042.CrossRefGoogle Scholar
  17. Liu, N., & Sun, G. (2011). Photo-degradation of methylene blue in the presence of 2-anthraquinone sulfonate and cyclohexanol presence. Dyes and Pigments,91, 215–224.  https://doi.org/10.1016/j.dyepig.2011.03.018.CrossRefGoogle Scholar
  18. Mao, N., Zhou, C. H., Tong, D. S., Yu, W. H., & Cynthia Lin, C. X. (2017). Exfoliation of layered double hydroxide solids into functional nanosheets. Applied Clay Science,144, 60–78.  https://doi.org/10.1016/j.clay.2017.04.021.CrossRefGoogle Scholar
  19. Muñoz, M., Moreno, S., & Molina, R. (2012). Synthesis of Ce and Pr-promoted Ni and Co catalysts from hydrotalcite type precursors by reconstruction method. International Journal of Hydrogen Energy,37, 18827–18842.  https://doi.org/10.1016/j.ijhydene.2012.09.132.CrossRefGoogle Scholar
  20. Nivangune, N. T., Ranade, V. V., & Kelkar, A. A. (2017). MgFeCe ternary layered double hydroxide as highly efficient and recyclable heterogeneous base catalyst for synthesis of dimethyl carbonate by transesterification. Catalysis Letters,147, 2558–2569.  https://doi.org/10.1007/s10562-017-2146-x.CrossRefGoogle Scholar
  21. Ömer, Ş., Kaya, M., & Saka, C. (2015). Plasma-surface modification on bentonite clay to improve the performance of adsorption of methylene blue. Applied Clay Science,116, 46–53.  https://doi.org/10.1016/j.clay.2015.08.015.CrossRefGoogle Scholar
  22. Özdemir, A., & Keskin, C. S. (2009). Removal of a binary dye mixture of congo red and malachite green from aqueous solutions using a bentonite adsorbent. Clays and Clay Minerals,57, 695–705.  https://doi.org/10.1346/CCMN.2009.0570603.CrossRefGoogle Scholar
  23. Pan, D., Ge, S., Zhao, J., Shao, Q., Guo, L., Zhang, X., et al. (2018). Synthesis, characterization and photocatalytic activity of mixed-metal oxides derived from NiCoFe ternary layered double hydroxides. Dalton Transactions,47, 65–78.  https://doi.org/10.1039/C8DT01045E.CrossRefGoogle Scholar
  24. Parida, K., Satpathy, M., & Mohapatra, L. (2012). Incorporation of Fe(III) into Mg/Al layered double hydroxide framework: effects on textural properties and photocatalytic activity for H2 generation. Journal of Materials Chemistry,22, 7350–7357.  https://doi.org/10.1039/c2jm15658j.CrossRefGoogle Scholar
  25. Sahu, R. K., Mohanta, B. S., & Das, N. N. (2013). Synthesis, characterization and photocatalytic activity of mixed oxides derived from ZnAlTi ternary layered double hydroxides. Journal of Physics and Chemistry of Solids,74, 1263–1270.  https://doi.org/10.1016/j.jpcs.2013.04.002.CrossRefGoogle Scholar
  26. Scavetta, E., Ballarin, B., Corticelli, C., Gualandi, I., Tonelli, D., Prevot, V., Forano, C., & Mousty, C. (2012). An insight into the electrochemical behavior of Co/Al layered double hydroxide thin films prepared by electrodeposition. Journal of Power Sources,201, 360–367.  https://doi.org/10.1016/j.jpowsour.2011.10.122.CrossRefGoogle Scholar
  27. Shi, L., Li, D., Wang, J., Li, S., Evans, D. G., & Duan, X. (2005). Synthesis, flame-retardant and smoke-suppressant properties of a borate-intercalated layered double hydroxide. Clays and Clay Minerals,53, 294–300.  https://doi.org/10.1346/ccmn.2005.0530309.CrossRefGoogle Scholar
  28. Shu, X., He, J., Chen, D., & Wang, Y. (2008). Tailoring of phase composition and photoresponsive properties of Ti-containing nanocomposites from layered precursor. The Journal of Physical Chemistry C,112, 4151–4158.  https://doi.org/10.1021/jp711091m.CrossRefGoogle Scholar
  29. Subhan, M. A., Ahmed, T., & Uddin, N. (2015). Synthesis, structure, Pl and photocatalytic activities of La2O2CO3·CeO2·ZnO fabricated by co-precipitation method. Spectrochimica Acta Part A Molecular and Biomolecular Spectroscopy,138, 827–833.  https://doi.org/10.1016/j.saa.2014.10.114.CrossRefGoogle Scholar
  30. Wang, Z., Fongarland, P., Lu, G., & Essayem, N. (2014). Reconstructed La-, Y-, Ce-modified MgAl-hydrotalcite as a solid base catalyst for aldol condensation: investigation of water tolerance. Journal of Catalysis,318, 108–118.  https://doi.org/10.1016/j.jcat.2014.07.006.CrossRefGoogle Scholar
  31. Wu, W., Huang, Z. H., & Lim, T. T. (2014). Recent development of mixed metal oxide anodes for electrochemical oxidation of organic pollutants in water. Applied Catalysis A: General,480, 58–78.  https://doi.org/10.1016/j.apcata.2014.04.035.CrossRefGoogle Scholar
  32. Xiang, X., Hima, H. I., Wang, H., & Li, F. (2008). Facile synthesis and catalytic properties of nickel-based mixed-metal oxides with mesopore networks from a novel hybrid composite precursor. Chemistry of Materials,20, 1173–1182.  https://doi.org/10.1021/cm702072t.CrossRefGoogle Scholar
  33. Xiang, Q., Yu, J., & Wong, P. K. (2011). Quantitative characterization of hydroxyl radicals produced by various photocatalysts. Journal of Colloid and Interface Science,357, 163–167.  https://doi.org/10.1016/j.jcis.2011.01.093.CrossRefGoogle Scholar
  34. Xiang, X., Xie, L., Li, Z., & Li, F. (2013). Ternary MgO/ZnO/In2O3 heterostructured photocatalysts derived from a layered precursor and visible-light-induced photocatalytic activity. Chemical Engineering Journal,221, 222–229.  https://doi.org/10.1016/j.cej.2013.02.030.CrossRefGoogle Scholar
  35. Xu, M., Pan, G., Meng, Y., Guo, Y., Wu, T., & Chen, H. (2019). Effect of Ce3+ on the photocatalytic activity of MAlCe ternary hydrotalcites-like compounds in methylene blue photodegradation. Applied Clay Science,170, 46–56.  https://doi.org/10.1016/j.clay.2019.01.011.CrossRefGoogle Scholar
  36. Yan, T., Zhu, H., Li, R., Li, Z., Liu, J., & Wang, G. (2013). Microwave synthesis of nickel/cobalt double hydroxide ultrathin flowerclusters with three-dimensional structures for high-performance supercapacitors. Electrochim Acta,111, 71–79.  https://doi.org/10.1016/j.electacta.2013.07.215.CrossRefGoogle Scholar
  37. Yan, L., Yang, K., Shan, R., Yan, T., Wei, J., Yu, S., Yu, H., & Du, B. (2015). Kinetic, isotherm and thermodynamic investigations of phosphate adsorption onto core–shell Fe3O4@ LDH composites with easy magnetic separation assistance. Journal of Colloid and Interface Science,448, 508–516.  https://doi.org/10.1016/j.jcis.2015.02.048.CrossRefGoogle Scholar
  38. Yang, R., Cui, Y., Yan, Q., Zhang, C., Qiu, L., O'Hare, D., & Wang, Q. (2017). Design of highly efficient NOx storage-reduction catalysts from layered double hydroxides for NOx emission control from naphtha cracker flue gases. Chemical Engineering Journal,326, 656–666.  https://doi.org/10.1016/j.cej.2017.06.016.CrossRefGoogle Scholar
  39. Zhao, X., Zhang, F., Xu, S., Evans, D. G., & Duan, X. (2010). From layered double hydroxides to ZnO-based mixed metal oxides by thermal decomposition: transformation mechanism and UV-blocking properties of the product. Chemistry of Materials,22, 3933–3942.  https://doi.org/10.1021/cm100383d.CrossRefGoogle Scholar
  40. Zhang, L., Dai, C. H., Zhang, X. X., Liu, Y. N., & Yan, J. H. (2016). Synthesis and highly efficient photocatalytic activity of mixed oxides derived from ZnNiAl layered double hydroxides. Transactions of Nonferrous Metals Society of China,26, 2380–2389.  https://doi.org/10.1016/S1003-6326(16)64360-1.CrossRefGoogle Scholar
  41. Zhou, C. H. (2010). Emerging trends and challenges in synthetic clay-based materials and layered double hydroxides. Applied Clay Science,48, 1–4.  https://doi.org/10.1016/j.clay.2009.12.018.CrossRefGoogle Scholar
  42. Zhou, C. H., & Keeling, J. (2013). Fundamental and applied research on clay minerals: from climate and environment to nanotechnology. Applied Clay Science,74, 3–9.  https://doi.org/10.1016/j.clay.2013.02.013.CrossRefGoogle Scholar
  43. Zhou, C. H., Li, Z. Z., Ai, Q. W., Tian, H. C., & Hong, P. H. (2016). Current fundamental and applied research into clay minerals in china. Applied Clay Science,119, 3–7.  https://doi.org/10.1016/j.clay.2015.07.043.CrossRefGoogle Scholar

Copyright information

© The Clay Minerals Society 2019
AE: Chun-Hui Zhou

Authors and Affiliations

  • Minhong Xu
    • 1
    Email author
  • Mengxia Qian
    • 2
  • Guoxiang Pan
    • 1
  • Yuhua Guo
    • 1
  • Tao Wu
    • 1
  1. 1.Department of Materials EngineeringHuzhou UniversityHuzhouChina
  2. 2.Key Laboratory of Advanced Textile Materials and Manufacturing Technology of Ministry of EducationZhejiang Sci-Tech UniversityHangzhouChina

Personalised recommendations