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Heterogeneous photocatalytic degradation of pesticides using decatungstate intercalated macroporous layered double hydroxides

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Abstract

Decatungstate W10O32 4− was efficiently intercalated between the layers of three-dimensionally ordered macroporous Mg2Al-layered double hydroxide. The structural and textural properties of as-prepared intercalated compound were characterized using different solid-state characterization techniques such as X-ray powder diffraction, FTIR and Raman spectroscopies and electronic microscopy. The photocatalytic properties of immobilized W10O32 4− within Mg2Al structure were investigated using 2-(1-naphthyl) acetamide (NAD) as a model of pesticide. The influence of different parameters such as amount of catalyst, pH and oxygen concentration were investigated. An optimal NAD degradation was obtained for a photocatalyst concentration of 60 mg l−1. Under our experimental conditions, this heterogeneous photocatalyst induces photodegradation of 60 % of NAD after 17 h of irradiation at 365 nm and at pH 6.6. Interestingly, pesticide photodegradation leads to the mineralization of substrates to H2O and CO2 and the photocatalyst can be recycled and reused without any loss of activity over four cycles.

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References

  • Allaoui A, Malouki MA, Wong Wah Chung P (2011) Efficient degradation of methabenzthiazuron photoinduced by decatungstate anion in water: kinetics and mechanistic studies. Chemosphere 85:558–564

    Article  CAS  Google Scholar 

  • Andreozzi R, Caprio V, Insola A, Marotta R (1999) Advanced oxidation processes (AOP) for water purification and recovery. Catal Today 53:51–59

    Article  CAS  Google Scholar 

  • Antonaraki S, Triantis TM, Papaconstantinou E (2010) Photocatalytic degradation of lindane by polyoxometalates: intermediates and mechanistic studies. Catal Today 151:119–124

    Article  CAS  Google Scholar 

  • Bonchio M, Carraro M, Scorrano G, Fontanova E, Drioli E (2003) Heterogeneous photooxidation membranes incorporating decatungstate. Adv Synth Catal 345:1119–1126

    Article  CAS  Google Scholar 

  • Burrows HD, Canle LM, Santabella JA, Steenken S (2002) Reaction pathways and mechanisms of photodegradation of pesticides. J Photochem Photobiol B Biol 67:71–108

    Article  CAS  Google Scholar 

  • Carja G, Nakajima A, Dranca S, Dranca C, Okada K (2010) TiO2/ZnLDH as a self-assembled nanocomposite with photoresponsive properties. J Phys Chem C 114:14722–14728

    Article  CAS  Google Scholar 

  • Centi G, Perathoner S (2003) Remediation of water contamination using catalytic technologies. Appl Catal B Environ 41:15–29

    Article  CAS  Google Scholar 

  • Chiron S, Fernandez-Alba A, Rodriguez A, Garcia-Calvo E (2000) Pesticide chemical oxidation: state-of-the-art. Water Res 34:366–377

    Article  CAS  Google Scholar 

  • Clarke AE, Lombard PM, Edmundson WC (1941) Seed-setting in potatoes as affected by spraying with α-naphthaleneacetamide and by light. Am Potato J 18:273–279

    Article  Google Scholar 

  • Da Silva ES, Wong Wah-Chung P, Burrows HD, Sarakha M (2013) Photochemical degradation of the plant growth regulator 2-(1-naphthyl) acetamide in aqueous solution upon UV irradiation. Photochem Photobiol 89:560–570

    Article  Google Scholar 

  • Duan X, Evans DG (eds) (2006) Structure and bonding: layered double hydroxides. In: Struct. Bonding 119. Springer, Berlin

  • Duncan DC, Netzel TL, Hill CL (1995) Early-time dynamics and reactivity of polyoxometalate excited states. Identification of a short-lived LMCT excited state and a reactive long-lived charge-transfer intermediate following picosecond flash excitation of [W10O32]4− in acetonitrile. Inorg Chem 34:4640–4646

    Article  CAS  Google Scholar 

  • Dvininov E, Ignat M, Barvinschi P, Smithers MA, Popovici E (2010) New SnO2/MgAl-layered double hydroxide composites as photocatalysts for cationic dyes bleaching. J Hazard Mater 177:150–158

    Article  CAS  Google Scholar 

  • Fox MA, Dulay MT (1995) Heterogeneous photocatalysis. Chem Rev 83:341–357

    Google Scholar 

  • Furusawa K, Norde W, Lyklema J (1972) A method for preparing surfactant-free polystyrene latices of high surface charge. Kolloid Z Z Polym 250:908

    Article  CAS  Google Scholar 

  • Gardner FE (1941) Practical applications of plant growth substances in horticulture. Proc Fla State Hortic Soc 54:20–26

    Google Scholar 

  • Gaya UI, Abdullah AH (2008) Heterogeneous photocatalytic degradation of organic contaminants over titanium dioxide: a review of fundamentals, progress and problems. J Photochem Photobiol C Photochem Rev 9:1–12

    Article  CAS  Google Scholar 

  • Geraud E, Prevot V, Ghanbaja J, Leroux F (2006) Macroscopically ordered hydrotalcite-type materials using self-assembled colloidal crystal template. Chem Mater 18:238–240

    Article  CAS  Google Scholar 

  • Geraud E, Bouhent M, Derriche Z, Leroux F, Prevot V, Forano C (2007) Texture effect of layered double hydroxides on chemisorption of Orange II. J Phys Chem Solids 68:818–823

    Article  CAS  Google Scholar 

  • Geraud E, Rafqah S, Sarakha M, Forano C, Prevot V, Leroux F (2008) Three dimensionally ordered macroporous layered double hydroxides: preparation by templated impregnation/coprecipitation and pattern stability upon calcination. Chem Mater 20:1116–1125

    Article  CAS  Google Scholar 

  • Gomes-Silva C, Bouizi Y, Fornes V, Garcia H (2009) Layered double hydroxides as highly efficient photocatalysts for visible light oxygen generation from water. J Am Chem Soc 131:13833–13839

    Article  CAS  Google Scholar 

  • Guo Y, Li D, Hu C, Wang Y, Wang E, Zhou Y, Feng S (2001) Photocatalytic degradation of aqueous organochlorine pesticide on the layered double hydroxide pillared by paratungstate A ion, Mg12Al6(OH)36(W7O24)·4H2O. Appl Catal B 30:337–349

    Article  CAS  Google Scholar 

  • Legrini O, Oliveros E, Braun AM (1993) Photochemical processes for water treatment. Chem Rev 93:671–698

    Article  CAS  Google Scholar 

  • Maldotti A, Molinari A, Amadelli R (2002) Photocatalysis with organized systems for the oxofunctionalization of hydrocarbons by O2. Chem Rev 102:3811

    Article  CAS  Google Scholar 

  • Mills A, LeHunte S (1997) An overview of semiconductor photocatalysis. J Photochem Photobiol A 108:1–35

    Article  CAS  Google Scholar 

  • Molinari A, Bratovcic A, Magnacca G, Maldotti A (2010) Matrix effects on the photocatalytic oxidation of alcohols by [nBu4N]4W10O32 incorporated into sol–gel silica. Dalton Trans 39:7826–7833

    Article  CAS  Google Scholar 

  • Molinari A, Maldotti A, Bratovcic A, Magnacca G (2013) Photocatalytic properties of sodium decatungstate supported on sol–gel silica in the oxidation of glycerol. Catal Today 206:46–52

    Article  CAS  Google Scholar 

  • Niu P, Hao J (2013) Photocatalytic degradation of methyl orange by titanium dioxide–decatungstate nanocomposite films supported on glass slides. Colloids Surf A 431:127–132

    Article  CAS  Google Scholar 

  • Parida K, Mohapatra L, Baliarsingh N (2012) Effect of Co2+ substitution in the framework of carbonate intercalated Cu/Cr LDH on structural, electronic, optical, and photocatalytic properties. J Phys Chem C 116:22417–22424

    Article  CAS  Google Scholar 

  • Paušová Š, Krýsa J, Jirkovský J, Mailhot G, Prevot V (2012) Photocatalytic behavior of nanosized TiO2 immobilized on layered double hydroxides by delamination/restacking process. Environ Sci Pollut Res 19:3709–3718

    Article  Google Scholar 

  • Rafqah S, Wong Wah Chung P, Nelieu S, Einhorn J, Sarakha M (2006) Phototransformation of triclosan in the presence of TiO2 in aqueous suspension: mechanistic approach. Appl Catal B Environ 66:119–125

    Article  CAS  Google Scholar 

  • Rafqah S, Wong Wah Chung P, Forano C, Sarakha M (2008) Photocatalytic degradation of metsulfuron methyl in aqueous solution by decatungstate anions. J Photochem Photobiol A Chem 199:297–302

    Article  CAS  Google Scholar 

  • Renneke RF, Pasqual MI, Hill CL (1990) Polyoxometalate systems for the catalytic selective production of non thermodynamic alkenes form alkanes. Nature of excited-state deactivation processes and control of subsequent thermal processes in polyoxometalate photoredox chemistry. J Am Chem Soc 112:6585–6594

    Article  CAS  Google Scholar 

  • Rives V (2001) Layered double hydroxides: present and future. Nova Science, New York, p 439

    Google Scholar 

  • Rives V, Ulibarri MA (1999) Layered double hydroxides (LDH) intercalated with metal coordination compounds and oxometalates. Coord Chem Rev 181:61–120

    Article  CAS  Google Scholar 

  • Sattari D, Hill CL (1993) Catalytic carbon–halogen bond cleavage chemistry by redox-active polyoxometalates. J Am Chem Soc 115:4649–4657

    Article  CAS  Google Scholar 

  • Schroden RC, Stein A (2004) 3D ordered macroporous materials. In: Caruso F (ed) Colloids and colloid assemblies. Wiley, 465–493

  • Shao M, Han J, Wei M, Evans DG, Duan X (2011) The synthesis of hierarchical Zn–Ti layered double hydroxide for efficient visible-light photocatalysis. Chem Eng J 168:519–524

    Article  CAS  Google Scholar 

  • Stein A, Wilson BE, Rudisill SG (2013) Design and functionality of colloidal-crystal-templated materials. Chem Soc Rev 42:2763–2803

    Article  CAS  Google Scholar 

  • Taviot-Gueho C, Prevot V, Forano C (2013) Layered double hydroxides. In: Bergaya F, Theng BKG, Lagaly G (eds) Handbook of clay science, 2nd edn. Elsevier, Amsterdam

    Google Scholar 

  • Tzirakis MD, LykakisIoannis N, Orfanopoulos M (2009) Decatungstate as an efficient photocatalyst in organic chemistry. Chem Soc Rev 38:2609–2621

    Article  CAS  Google Scholar 

  • Woodford JJ, Dacquin J-P, Wilson K, Lee AF (2012) Better by design: nanoengineered macroporous hydrotalcites for enhanced catalytic biodiesel production. Energy Environ Sci 5:6145–6150

    Article  CAS  Google Scholar 

  • Zhi Y, Li Y, Zhang Q, Wang H (2010) ZnO nanoparticles immobilized on flaky layered double hydroxides as photocatalysts with enhanced adsorptivity for removal of Acid Red G. Langmuir 26:15546–15553

    Article  CAS  Google Scholar 

Download references

Acknowledgments

Eliana S. Da Silva acknowledges the Portuguese Science Foundation (FCT) for the PhD grant (BD/SFRH/BD/43171/2008) he received under the framework of the Portuguese POPH/FEDER/QREN program.

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Authors and Affiliations

  1. Clermont Université, Université Blaise Pascal, Institut de Chimie de Clermont-Ferrand, BP 10448, 63000, Clermont-Ferrand, France

    Eliana S. Da Silva, Vanessa Prevot, Claude Forano, Pascal Wong-Wah-Chung & Mohamed Sarakha

  2. CNRS, UMR 6296, ICCF, 63171, Aubiere, France

    Eliana S. Da Silva, Vanessa Prevot, Claude Forano, Pascal Wong-Wah-Chung & Mohamed Sarakha

  3. Department of Chemistry, University of Coimbra, Rua Larga, 3004-535, Coimbra, Portugal

    Eliana S. Da Silva & Hugh D. Burrows

Authors
  1. Eliana S. Da Silva
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  2. Vanessa Prevot
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  3. Claude Forano
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  4. Pascal Wong-Wah-Chung
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  5. Hugh D. Burrows
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  6. Mohamed Sarakha
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Corresponding authors

Correspondence to Vanessa Prevot or Mohamed Sarakha.

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Responsible editor: Philippe Garrigues

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Da Silva, E.S., Prevot, V., Forano, C. et al. Heterogeneous photocatalytic degradation of pesticides using decatungstate intercalated macroporous layered double hydroxides. Environ Sci Pollut Res 21, 11218–11227 (2014). https://doi.org/10.1007/s11356-014-2971-z

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