Destruction of Aqueous Phase Organic Pollutants Using Ultraviolet Light-Emitting Diodes and Photocatalysis

  • Morgan M. Russell
  • David M. Kempisty
  • Sushil R. Kanel
  • Sudarshan Kurwadkar
  • Seth W. Brittle
  • Ioana Sizemore
  • Lester Yaal
Article

Abstract

The photocatalytic degradation of dyes (Allura Red AC and Brilliant Blue FCF) in water using ultraviolet light-emitting diodes (UV-LED) and an immobilized titanium dioxide (TiO2) as a photocatalyst was investigated using a novel bench-top Teflon® reactor. This reactor has been uniquely designed to contain low-powered UV-LEDs combined with TiO2 immobilized substrates. A sol-gel method was used to anneal TiO2 to three different substrates: standard microscope quartz slides, quartz cylinders, and borosilicate beads. Scanning electron microscopy (SEM), Raman spectroscopy, and mass comparisons techniques were performed for TiO2 characterization. High-resolution images confirmed the presence and morphology of TiO2 on the substrates. These analyses demonstrated the TiO2 coating was uniform and predominantly had the anatase crystalline phase structure. The slide had the largest individual TiO2 surface area of 0.187 mg cm−2. Results indicated the size, shape, packing, and stirring properties were factors that determine overall photocatalytic properties and degradation inside the reactor. The adjusted rate constants for an ideal completely mixed batch reactor (CMBR) were 1.69 * 10−3, 5.39 * 10−3, and 4.46 * 10−3 min−1 for the slides, beads, and cylinders, respectively. Beads were the best-performing substrate as determined by the greatest degradation rate for the model organic compound, Allura Red AC. The beads and cylinders showed 58 and 51% degradation of Allura Red AC, respectively. Actinometry experiments revealed cylinders had the largest fluence rate of 0.0782 J·L−1 s−1. Optimization of the sol-gel application method and reactor operating parameters was performed to maximize the degradation rate and the overall degradation of Allura Red AC. Electric energy per order (EEO) was calculated and optimized at 9.20, 10.5, and 12.7 kWh·m−3 order−1 for the glass beads, cylinders, and slides, respectively.

Graphical abstract

Keywords

UV-light-emitting diode (UV-LED) Photocatalysis Organic dye Titanium dioxide Thin film Electrical energy per order (EEO

Notes

Acknowledgements

The authors gratefully acknowledge the support of staff and other student assistants throughout this study. Dr. Kurwadkar was a key contributor from the beginning and throughout this research. SEM imaging and EDS analysis would not have been possible without John Kelley from the Air Force Research Laboratory (AFRL) Materials Characterization Facility at Wright-Patterson Air Force Base. Dr. Magnuson, Office of Research and Development, United States Environmental Protection Agency supported this work.

References

  1. Balachandran, U., & Eror, N. G. (1982). Raman spectra of titanium dioxide. Journal of Solid State Chemistry, 42(3), 276–282.  https://doi.org/10.1016/0022-4596(82)90006-8.CrossRefGoogle Scholar
  2. Behnajady, M. A., Vahid, B., Modirshahla, N., & Shokri, M. (2009). Evaluation of electrical energy per order (EEO) with kinetic modeling on the removal of Malachite Green by US/UV/H2O2 process. Desalination, 249(1), 99–103.  https://doi.org/10.1016/j.desal.2008.07.025.CrossRefGoogle Scholar
  3. Bolton, J. R., Bircher, K. G., Tumas, W., & Tolman, C. A. (2001). Figures-of- merit for the technical development and application of advanced oxidation technologies for both electric- and solar-driven systems (IUPAC Technical Report). Pure and Applied Chemistry, 73(4), 627–637.  https://doi.org/10.1351/pac200173040627.CrossRefGoogle Scholar
  4. Chen, J., Kim, J., & Loeb, S. (2017). LED Revolution: fundamentals and prospects for UV disinfection applications. Environmental Science: Water Research & Technology, 2017(3), 188–202.  https://doi.org/10.1039/C6EW00241B.Google Scholar
  5. Cho, M., Chung, H., Choi, W., & Yoon, J. (2004). Linear correlation between inactivation of E. coli and OH radical concentration in TiO2 photocatalytic disinfection. Water Research, 38(4), 1069–1077.  https://doi.org/10.1016/j.watres.2003.10.029.CrossRefGoogle Scholar
  6. Choi, H., Stathatos, E., & Dionysiou, D. D. (2006). Sol-gel preparation of mesoporous photocatalytic TiO2 films and TiO2/Al2O3 composite membranes for environmental applications. Applied Catalysis B: Environmental, 63(1–2), 60–67.  https://doi.org/10.1016/j.apcatb.2005.09.012.CrossRefGoogle Scholar
  7. Dariani, R. S., Esmaeili, A., Mortezaali, A., & Dehghanpour, S. (2016). Photocatalytic reaction and degradation of methylene blue on TiO2 nano-sized particles. Optik, 127(18), 7143–7154.  https://doi.org/10.1016/j.ijleo.2016.04.026.CrossRefGoogle Scholar
  8. Dominguez, S., Rivero, M. J., Gomez, P., Ibanez, R., & Ortiz, I. (2015). Kinetic modeling and energy evaluation of sodium dodecylbenzenesulfonate photocatalytic degradation in a new LED reactor. Journal of Industrial and Engineering Chemistry, 37, 237–242.  https://doi.org/10.1016/j.jiec.2016.03.031.CrossRefGoogle Scholar
  9. Eskandarloo, H., Badiei, A., Behnajady, M. A., & Ziarani, G. M. (2015). UV-LEDs assisted preparation of silver-deposited TiO2 catalyst bed inside microchannels as a high efficiency microphotoreactor for cleaning polluted water. Chemical Engineering Journal, 270, 158–167.  https://doi.org/10.1016/j.cej.2015.01.117.CrossRefGoogle Scholar
  10. Fang, W., Dappozze, F., Guillard, C., Zhou, Y., Xing, M., Mishra, S., Daniele, S., & Zhang, J. (2017). Zn-assisted TiO2 − x Photocatalyst with efficient charge separation for enhanced photocatalytic activities. Journal of Physical Chemistry C, 121, 17,068–17,076.CrossRefGoogle Scholar
  11. Ghosh, J. P., Sui, R., Langford, C. H., Achari, G., & Berlinguette, C. P. (2009). A comparison of several nanoscale photocatalysts in the degradation of a common pollutant using LEDs and conventional UV light. Water Research, 43(18), 4499–4506.  https://doi.org/10.1016/j.watres.2009.07.027.CrossRefGoogle Scholar
  12. Government Accountability Office, U. S. (2005). Groundwater contamination: DOD uses and develops a range of remediation technologies to clean up military sites. Report to Congressional Committees.Google Scholar
  13. Habibi, M. H., & Mikhak, M. (2012). Titania/zinc oxide nanocomposite coatings on glass or quartz substrate for photocatalytic degradation of direct blue 71. Applied Surface Science, 258(18), 6745–6752.  https://doi.org/10.1016/j.apsusc.2012.03.042.CrossRefGoogle Scholar
  14. Hales, M. C., Steinberg, T. A., & Martens, W. N. (2014). Synthesis and characterization of titanium sol-gels in varied gravity. Journal of Non-Crystalline Solids, 396–397, 13–19.  https://doi.org/10.1016/j.jnoncrysol.2014.04.010.CrossRefGoogle Scholar
  15. Han, C., Pelaez, M., Likodimos, V., Kontos, A. G., Falaras, P., O’Shea, K., & Dionysiou, D. D. (2011). Innovative visible light-activated sulfur doped TiO2 films for water treatment. Applied Catalysis B: Environmental, 107(1–2), 77–87.  https://doi.org/10.1016/j.apcatb.2011.06.039.CrossRefGoogle Scholar
  16. Kent, F. C., Montreuil, K. R., Brookman, R. M., Sanderson, R., Dahn, J. R., & Gagnon, G. A. (2011). Photocatalytic oxidation of DBP precursors using UV with suspended and fixed TiO 2. Water Research, 45(18), 6173–6180.  https://doi.org/10.1016/j.watres.2011.09.013.CrossRefGoogle Scholar
  17. Kim, S. H., Lee, S. W., Lee, G. M., Lee, B. T., Yun, S. T., & Kim, S. O. (2016). Monitoring of TiO2-catalytic UV-LED photo-oxidation of cyanide contained in mine wastewater and leachate. Chemosphere, 143, 106–114.  https://doi.org/10.1016/j.chemosphere.2015.07.006.CrossRefGoogle Scholar
  18. Konstantinou, I. K., & Albanis, T. A. (2004). TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations: a review. Applied Catalysis B: Environmental, 49(1), 1–14.  https://doi.org/10.1016/j.apcatb.2003.11.010.CrossRefGoogle Scholar
  19. Muruganandham, M., Selvam, K., & Swaminathan, M. (2007). A comparative study of quantum yield and electrical energy per order (EEO) for advanced oxidative decolourization of reactive azo dyes by UV light. Journal of Hazardous Materials, 144(1–2), 316–322.  https://doi.org/10.1016/j.jhazmat.2006.10.035.CrossRefGoogle Scholar
  20. Natarajan, K., Natarajan, T. S., Bajaj, H. C., & Tayade, R. J. (2011). Photocatalytic reactor based on UV-LED/TiO 2 coated quartz tube for degradation of dyes. Chemical Engineering Journal, 178, 40–49.  https://doi.org/10.1016/j.cej.2011.10.007.CrossRefGoogle Scholar
  21. Naumenko, A., Gnatiuk, I., Smirnova, N., & Eremenko, A. (2012). Characterization of sol-gel derived TiO2/ZrO2 films and powders by Raman spectroscopy. Thin Solid Films, 520(14), 4541–4546.  https://doi.org/10.1016/j.tsf.2011.10.189.CrossRefGoogle Scholar
  22. Prusakova, V., Armellini, C., Carpentiero, A., Chiappini, A., Collini, C., Dirè, S., & Chiasera, A. (2015). Morphologic, structural, and optical characterization of sol- gel derived TiO2 thin films for memristive devices. Physica Status Solidi C, 12(1–2), 192–196.  https://doi.org/10.1002/pssc.201400101.CrossRefGoogle Scholar
  23. Rahn, R. O. (1997). Potassium iodide as a chemical actinometer for 254 nm radiation: use of lodate as an electron scavenger. Photochemistry and Photobiology, 66(4), 450–455.  https://doi.org/10.1111/j.1751-1097.1997.tb03172.x.CrossRefGoogle Scholar
  24. Rasoulifard, M., Fazli, M., & Eskandarian, M. (2014). Kinetic study for photocatalytic degradation of Direct Red 23 in UV–LED/nano-TiO2/S2O82− process: dependence of degradation kinetic on operational parameters. Journal of Industrial and Engineering Chemistry, 20(5), 3695–3702.  https://doi.org/10.1016/j.jiec.2013.12.068.CrossRefGoogle Scholar
  25. Swarnakar, P., Kanel, S. R., Nepal, D., Jiang, Y., Jia, H., Kerr, L., & Rakovan, J. (2013). Silver deposited titanium dioxide thin film for photocatalysis of organic compounds using natural light. Solar Energy, 88, 242–249.  https://doi.org/10.1016/j.solener.2012.10.014.CrossRefGoogle Scholar
  26. Thiam, A., Sirés, I., Garrido, J. A., Rodríguez, R. M., & Brillas, E. (2015). Decolorization and mineralization of Allura Red AC aqueous solutions by electrochemical advanced oxidation processes. Journal of Hazardous Materials, 290, 34–42.  https://doi.org/10.1016/j.jhazmat.2015.02.050.CrossRefGoogle Scholar
  27. Varshney, G., Kanel, S. R., Kempisty, D. M., Varshney, V., Agrawal, A., Sahle- Demessie, E., & Nadagouda, M. N. (2016). Nanoscale TiO2 films and their application in remediation of organic pollutants. Coordination Chemistry Reviews, 306(July), 43–64.  https://doi.org/10.1016/j.ccr.2015.06.011.CrossRefGoogle Scholar
  28. Vasuki, T., Saroja, M., & Venkatachalam, S. S. (2015). Synthesis and characterization of TiO2 thin film for photocatalytic degradation of textile dye effluent. International Journal of Recent Scientific Research, 6, 3511–3514.Google Scholar
  29. Wu, C.-Y., Lee, Y.-L., Lo, Y.-S., Lin, C.-J., & Wu, C.-H. (2013). Thickness- dependent photocatalytic performance of nanocrystalline TiO2 thin films prepared by sol–gel spin coating. Applied Surface Science, 280, 737–744.  https://doi.org/10.1016/j.apsusc.2013.05.053.CrossRefGoogle Scholar

Copyright information

© This is a U.S. Government work and not under copyright protection in the US; foreign copyright protection may apply 2018

Authors and Affiliations

  • Morgan M. Russell
    • 1
  • David M. Kempisty
    • 1
  • Sushil R. Kanel
    • 1
  • Sudarshan Kurwadkar
    • 2
  • Seth W. Brittle
    • 3
  • Ioana Sizemore
    • 3
  • Lester Yaal
    • 4
  1. 1.Department of Systems Engineering and ManagementAir Force Institute of TechnologyWright-Patterson AFBUSA
  2. 2.Department of Civil and Environmental EngineeringCalifornia State UniversityFullertonUSA
  3. 3.Department of ChemistryWright State UniversityDaytonUSA
  4. 4.Department of Advanced Material EngineeringAzrieli College of Engineering JerusalemJerusalemIsrael

Personalised recommendations