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Solar photocatalytic gas-phase degradation of n-decane—a comparative study using cellulose acetate monoliths coated with P25 or sol-gel TiO2 films

  • Advanced Oxidation Technologies: Advances and Challenges in IberoAmerican Countries
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Abstract

Cellulose acetate monoliths (CAM) were used as the substrate for the deposition of TiO2 films to produce honeycombed photoactive structures to fill a tubular photoreactor equipped with a compound parabolic collector. By using such a setup, an efficient single-pass gas-phase conversion was achieved in the degradation of n-decane, a model volatile organic compound. The CAM three-dimensional, gas-permeable transparent structure with a rugged surface enables a good adhesion of the catalytic coating. It also provides a rigid structure for packing the tubular photoreactor, and maximizing the illuminated catalyst surface. The efficiency of the photocatalytic oxidation (PCO) process on n-decane degradation was evaluated under different operating conditions, such as feeding concentration (73 and 146 ppm), gas stream flow rate (73, 150, and 300 mL min−1), relative humidity (3 and 25 %), and UV irradiance (18.9, 29.1, and 38.4 WUV m−2). The results show that n-decane degradation by neat photolysis is negligible, but mineralization efficiencies of 86 and 82 % were achieved with P25-CAM and SG-CAM, respectively, for parent pollutant conversions above 95 %, under steady-state conditions. A mass transfer model, considering the mass balance to the plug-flow packed photoreactor, and PCO reaction given by a Langmuir-Hinshelwood bimolecular non-competitive two types of sites equation, was able to predict well the PCO kinetics under steady-state conditions, considering all the operational parameters tested. Overall, the performance of P25-CAM was superior taking into account mineralization efficiency, cost of preparation, surface roughness, and robustness of the deposited film.

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References

  • Aris A (1956) On the dispersion of a solute in a fluid flowing through a tube. P Roy Soc Lond A Mat 235:67–77

    Article  Google Scholar 

  • Augugliaro V, Coluccia S, Loddo V, Marchese L, Martra G, Palmisano L, Schiavello M (1999) Photocatalytic oxidation of gaseous toluene on anatase TiO2 catalyst: mechanistic aspects and FT-IR investigation. Appl Catal B Environ 20:15–27

    Article  CAS  Google Scholar 

  • Bosc F, Edwards D, Keller N, Keller V, Ayral A (2006) Mesoporous TiO2-based photocatalysts for UV and visible light gas-phase toluene degradation. Thin Solid Films 495:272–279

    Article  CAS  Google Scholar 

  • Boulamanti AK, Philippopoulos CJ (2009) Photocatalytic degradation of C5–C7 alkanes in the gas-phase. Atmos Environ 43:3168–3174

    Article  CAS  Google Scholar 

  • Debono O, Thévenet F, Gravejat P, Héquet V, Raillard C, Le Coq L, Locoge N (2013) Gas phase photocatalytic oxidation of decane at ppb levels: removal kinetics, reaction intermediates and carbon mass balance. J Photochem Photobiol A Chem 258:17–29

    Article  CAS  Google Scholar 

  • Djeghri N, Formenti M, Juillet F, Teichner SJ (1974) Photointeraction on the surface of titanium dioxide between oxygen and alkanes. Farad Discuss Chem Soc 58:185

    Article  Google Scholar 

  • Fuller EN, Giddings JC (1965) A comparison of methods for predicting gaseous diffusion coefficients. J Chromatogr Sci 3:222–227

    Article  CAS  Google Scholar 

  • Fuller EN, Schettler PD, Giddings JC (1966) New method for prediction of binary gas-phase diffusion coefficients. Ind Eng Chem 58:18–27

    Article  CAS  Google Scholar 

  • Fuller EN, Ensley K, Giddings JC (1969) Diffusion of halogenated hydrocarbons in helium. The effect of structure on collision cross sections. J Phys Chem 73:3679–3685

    Article  CAS  Google Scholar 

  • Gallego E, Roca FJ, Perales JF, Sánchez G, Esplugas P (2012) Characterization and determination of the odorous charge in the indoor air of a waste treatment facility through the evaluation of volatile organic compounds (VOCs) using TD–GC/MS. Waste Manag 32:2469–2481

    Article  CAS  Google Scholar 

  • International Organization for Standardization (2004) ISO 16000-6. Determination of volatile organic compounds in indoor and test chamber air by active sampling on Tenax TA sorbent, thermal desorption and gas chromatography using MS or MS/FID

  • Järnström H, Saarela K, Kalliokoski P, Pasanen AL (2006) Reference values for indoor air pollutant concentrations in new, residential buildings in Finland. Atmos Environ 40:7178–7191

    Article  Google Scholar 

  • Kjærgaard S, Mølhave L, Pedersen OF (1989) Human reactions to indoor air pollutants: n-decane. Environ Int 15:473–482

    Article  Google Scholar 

  • Li Puma G, Salvadó-Estivill I, Obee TN, Hay SO (2009) Kinetics rate model of the photocatalytic oxidation of trichloroethylene in air over TiO2 thin films. Sep Purif Technol 67:226–232

    Article  CAS  Google Scholar 

  • Lopes FVS, Monteiro RAR, Silva AMT, Silva GV, Faria JL, Mendes AM, Vilar VJP, Boaventura RAR (2012) Insights into UV-TiO2 photocatalytic degradation of PCE for air decontamination systems. Chem Eng J 204–206:244–257

    Article  Google Scholar 

  • Lopes FVS, Miranda SM, Monteiro RAR, Martins SDS, Silva AMT, Faria JL, Boaventura RAR, Vilar VJP (2013) Perchloroethylene gas-phase degradation over titania-coated transparent monoliths. Appl Catal B Environ 140–141:444–456

    Article  Google Scholar 

  • Malato S, Fernández-Ibáñez P, Maldonado MI, Blanco J, Gernjak W (2009) Decontamination and disinfection of water by solar photocatalysis: Recent overview and trends. Catal Today 147:1–59

    Article  CAS  Google Scholar 

  • Mickaël D, Bruno B, Valérie C, Murielle L, Cécile P, Jacques R, Severine K (2014) Indoor air quality and comfort in seven newly built, energy-efficient houses in France. Build Environ 72:173–187

    Article  Google Scholar 

  • Minabe T, Tryk DA, Sawunyama P, Kikuchi Y, Hashimoto K, Fujishima A (2000) TiO2-mediated photodegradation of liquid and solid organic compounds. J Photochem Photobiol A Chem 137:53–62

    Article  CAS  Google Scholar 

  • Mo J, Zhang Y, Yang R (2005) Novel insight into VOC removal performance of photocatalytic oxidation reactors. Indoor Air 15:291–300

    Article  CAS  Google Scholar 

  • Mo J, Zhang Y, Xu Q, Lamson JJ, Zhao R (2009) Photocatalytic purification of volatile organic compounds in indoor air: a literature review. Atmos Environ 43:2229–2246

    Article  CAS  Google Scholar 

  • Monteiro RAR, Lopes FVS, Silva AMT, Ângelo J, Silva GV, Mendes AM, Boaventura RAR, Vilar VJP (2014) Are TiO2-based exterior paints useful catalysts for gas-phase photooxidation processes? A case study on n-decane abatement for air detoxification. Appl Catal B Environ 147:988–999

    Article  CAS  Google Scholar 

  • Nakamura R, Sato S (2002) Oxygen species active for photooxidation of n-decane over TiO2 surfaces. J Phys Chem B 106:5893–5896

    Article  CAS  Google Scholar 

  • Narasimha Rao K (2003) Studies on thin film materials on acrylics for optical applications. Bull Mater Sci 26:239–245

    Article  Google Scholar 

  • Obee TN (1996) Photooxidation of sub-parts-per-million toluene and formaldehyde levels on titania using a glass-plate reactor. Environ Sci Technol 30:3578–3584

    Article  CAS  Google Scholar 

  • Obee TN, Brown RT (1995) TiO2 photocatalysis for indoor air applications: effects of humidity and trace contaminant levels on the oxidation rates of formaldehyde, toluene, and 1,3-butadiene. Environ Sci Technol 29:1223–1231

    Article  CAS  Google Scholar 

  • Obee TN, Hay SO (1997) Effects of moisture and temperature on the photooxidation of ethylene on titania. Environ Sci Technol 31:2034–2038

    Article  CAS  Google Scholar 

  • Ohura T, Amagai T, Shen X, Li S, Zhang P, Zhu L (2009) Comparative study on indoor air quality in Japan and China: characteristics of residential indoor and outdoor VOCs. Atmos Environ 43:6352–6359

    Article  CAS  Google Scholar 

  • Pelizzetti E, Minero C (1993) Mechanism of the photo-oxidative degradation of organic pollutants over TiO2 particles. Electrochim Acta 38:47–55

    Article  CAS  Google Scholar 

  • Peral J, Domènech X, Ollis DF (1997) Heterogeneous photocatalysis for purification, decontamination and deodorization of air. J Chem Technol Biot 70:117–140

    Article  CAS  Google Scholar 

  • Poling BE, Prausnitz JM, O’Connell JP (2001) The properties of gases and liquids. McGraw-Hill, New York

    Google Scholar 

  • Ruthven DM (1984) Principal of adsorption and adsorption processes. Wiley, New York

    Google Scholar 

  • Satterfield CN (1970) Mass transfer in heterogeneous catalysis. MIT Press, Massachusetts Institute of Technology, Cambridge

    Google Scholar 

  • Shang J, Du Y, Xu Z (2002) Photocatalytic oxidation of heptane in the gas-phase over TiO2. Chemosphere 46:93–99

    Article  CAS  Google Scholar 

  • Srivastava PK, Pandit GG, Sharma S, Mohan Rao AM (2000) Volatile organic compounds in indoor environments in Mumbai, India. Sci Total Environ 255:161–168

    Article  CAS  Google Scholar 

  • Taylor GI (1953) Dispersion of soluble matter in solvent flowing slowly through a tube. P Roy Soc Lond A Mat 219:186–203

    Article  CAS  Google Scholar 

  • Teixeira JV, Miranda S, Monteiro RAR, Lopes FVS, Madureira J, Silva GV, Pestana N, Pinto E, Vilar VJP, Boaventura RAR (2013) Assessment of indoor airborne contamination in a wastewater treatment plant. Environ Monit Assess 185:59–72

    Article  CAS  Google Scholar 

  • Twesme TM, Tompkins DT, Anderson MA, Root TW (2006) Photocatalytic oxidation of low molecular weight alkanes: observations with ZrO2–TiO2 supported thin films. Appl Catal B Environ 64:153–160

    Article  CAS  Google Scholar 

  • Valdés-Solís T, Linders MJG, Kapteijn F, Marbán G, Fuertes AB (2004) Adsorption and breakthrough performance of carbon-coated ceramic monoliths at low concentration of n-butane. Chem Eng Sci 59:2791–2800

    Article  Google Scholar 

  • Wang K-H, Tsai H-H, Hsieh Y-H (1998) The kinetics of photocatalytic degradation of trichloroethylene in gas phase over TiO2 supported on glass bead. Appl Catal B-Environ 17:313–320

    Article  CAS  Google Scholar 

  • Wang S, Ang HM, Tade MO (2007) Volatile organic compounds in indoor environment and photocatalytic oxidation: state of the art. Environ Int 33:694–705

    Article  CAS  Google Scholar 

  • William Balcerski, Ryu SY, Hoffmann MR (2008) Gas-phase photodegradation of decane and methanol on TiO2: dynamic surface chemistry characterized by diffuse reflectance FTIR. Int J Photoenergy 2008

  • Yamazaki S, Tsukamoto H, Araki K, Tanimura T, Tejedor-Tejedor I, Anderson MA (2001) Photocatalytic degradation of gaseous tetrachloroethylene on porous TiO2 pellets. Appl Catal B Environ 33:109–117

    Article  CAS  Google Scholar 

  • Zhang P, Liu J (2004) Photocatalytic degradation of trace hexane in the gas phase with and without ozone addition: kinetic study. J Photochem Photobiol A Chem 167:87–94

    Article  CAS  Google Scholar 

Download references

Acknowledgments

Financial support for this work was mainly provided by project PTDC/EQU-EQU/100554/2008 supported by FCT—Fundação para a Ciência e a Tecnologia. This work was also supported by projects PEst-C/EQB/LA0020/2013 and NORTE-07-0162-FEDER-000050, financed by FEDER through COMPETE - Programa Operacional Factores de Competitividade, by FCT, QREN and ON2. V.J.P. Vilar and A.M.T. Silva acknowledge the FCT Investigator 2013 Programme (IF/01501/2013 and IF/00273/2013, respectively). F.V.S. Lopes gratefully acknowledge FCT for his Post-doc Research Fellowship, SFRH/BPD/73894/2010. C. Rodrigues-Silva gratefully acknowledges CAPES for providing Post-Doc research scholarship (8674/13-2) and the project CAPES/FCT 308/11 for financial support.

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Authors and Affiliations

  1. LSRE—Laboratory of Separation and Reaction Engineering, Associate Laboratory LSRE/LCM, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, Porto, 4200-465, Portugal

    Sandra M. Miranda, Filipe V. S. Lopes, Caio Rodrigues-Silva, Rui A. R. Boaventura & Vítor J. P. Vilar

  2. LCM—Laboratory of Catalysis and Materials, Associate Laboratory LSRE/LCM, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal

    Sandra M. Miranda, Adrián M. T. Silva & Joaquim L. Faria

  3. IDMEC—Institute of Mechanical Engineering, Faculdade de Engenharia, Universidade do Porto, Rua Dr. Roberto Frias, 4200-465, Porto, Portugal

    Susana D. S. Martins

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  1. Sandra M. Miranda
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  2. Filipe V. S. Lopes
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  3. Caio Rodrigues-Silva
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  4. Susana D. S. Martins
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  5. Adrián M. T. Silva
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  6. Joaquim L. Faria
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  7. Rui A. R. Boaventura
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  8. Vítor J. P. Vilar
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Corresponding authors

Correspondence to Adrián M. T. Silva or Vítor J. P. Vilar.

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Responsible editor: Philippe Garrigues

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Miranda, S.M., Lopes, F.V.S., Rodrigues-Silva, C. et al. Solar photocatalytic gas-phase degradation of n-decane—a comparative study using cellulose acetate monoliths coated with P25 or sol-gel TiO2 films. Environ Sci Pollut Res 22, 820–832 (2015). https://doi.org/10.1007/s11356-014-2952-2

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  • DOI: https://doi.org/10.1007/s11356-014-2952-2

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