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Structural and Kinetic Study of the Reduction of CuO–CeO2/Al2O3 by Time-Resolved X-ray Diffraction

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Abstract

The crystallographic structure of (11 wt.%)CuO–(6 wt.%)CeO2/γ-Al2O3 has been studied and compared with (11 wt.%)CuO/γ-Al2O3 under reducing conditions, using time-resolved in situ X-ray diffraction in the temperature range 25–800 °C. In CuO–CeO2/Al2O3, H2-TPR reduces the CuO phase to Cu, while in C3H8-TPR reduction follows a two-step pathway via Cu2O. A thermal treatment in He also induces reduction for CuO, albeit at higher temperature. In addition to CuO reduction, the CeO2 promoter in CuO–CeO2/Al2O3 is also partially reduced, without crystallographic transition, regardless of the atmosphere and at similar temperature where reduction of CuO occurs. Supported CuO as in CuO–CeO2/Al2O3 or CuO/Al2O3, is more readily reduced by thermal treatment in He than unsupported CuO and Cu2O. Moreover, the addition of CeO2 to the CuO–CeO2/Al2O3 catalyst allows for enhanced reducibility of CuO, compared to CuO/Al2O3. The CuO phase in CuO–CeO2/Al2O3 is reduced to Cu2O and partly to Cu at 700 °C and mainly to Cu at 800 °C in He flow. The thermal reduction of CuO–CeO2/Al2O3 requires an apparent activation energy of 216 kJ/mol.

Graphical Abstract

An isothermal reduction treatment at 800 oC in He reduces CuO–CeO2/Al2O3, as demonstrated by time-resolved in situ X-ray diffraction. Supported CuO are more easily reduced by thermal treatment compared to unsupported CuO and Cu2O. The CuO phase in CuO–CeO2/Al2O3 is reduced to Cu2O and partly to Cu at 700 °C and mainly to Cu at 800 °C in He flow (see figure)

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References

  1. Armor JN (1992) Appl Catal B 1:221–256

    Article  CAS  Google Scholar 

  2. Everaert K, Baeyens J (2004) J Hazard Mater 109:113–139

    Article  CAS  Google Scholar 

  3. Christopher JGI, Heyes J, Hilary J, Moss JARL (1982) J Chem Technol Biotechnol 32:1025–1033

    Google Scholar 

  4. Larsson P-O, Andersson A (1998) J Catal 179:72–89

    Article  CAS  Google Scholar 

  5. Wang C-H, Lin S-S, Chen C-L, Weng H-S (2006) Chemosphere 64:503–509

    Article  CAS  Google Scholar 

  6. Heynderickx PM, Thybaut JW, Poelman H, Poelman D, Marin GB (2010) J Catal 272:109–120

    Article  CAS  Google Scholar 

  7. Alexopoulos K, Anilkumar M, Reyniers M-F, Poelman H, Cristol S, Balcaen V, Heynderickx PM, Poelman D, Marin GB (2010) Appl Catal B 97:381–388

    Article  CAS  Google Scholar 

  8. Huang T-J, Tsai D-H (2003) Catal Lett 87:173–178

    Article  CAS  Google Scholar 

  9. Doornkamp C, Ponec V (2000) J Mol Catal A 162:19–32

    Article  CAS  Google Scholar 

  10. Grzybowska-Świerkosz B (2000) Top Catal 11–12:23–42

    Article  Google Scholar 

  11. Busca G, Daturi M, Finocchio E, Lorenzelli V, Ramis G, Willey RJ (1997) Catal Today 33:239–249

    Article  CAS  Google Scholar 

  12. Balcaen V, Roelant R, Poelman H, Poelman D, Marin GB (2010) Catal Today 157:49–54

    Article  CAS  Google Scholar 

  13. Rubio O, Herguido J, Menéndez M (2003) Chem Eng Sci 58:4619–4627

    Article  CAS  Google Scholar 

  14. Haber J, Turek W (2000) J Catal 190:320–326

    Article  CAS  Google Scholar 

  15. Liu D-J, Robota HJ (1993) Catal Lett 21:291–301

    Article  CAS  Google Scholar 

  16. Amano F, Tanaka T, Funabiki T (2004) J Mol Catal A 221:89–95

    Article  CAS  Google Scholar 

  17. Iwamoto M, Yahiro H, Tanda K, Mizuno N, Mine Y, Kagawa S (1991) J Phys Chem 95:3727–3730

    Article  CAS  Google Scholar 

  18. Llabres i Xamena FX, Fisicaro P, Berlier G, Zecchina A, Palomino GT, Prestipino C, Bordiga S, Giamello E, Lamberti C (2003) J Phys Chem. B 107: 7036–7044

    Google Scholar 

  19. Menon U, Galvita VV, Marin GB J Catal. 283:1–9

  20. http://www.numpy.org

  21. http://www.scipy.org

  22. Wang X, Hanson JC, Frenkel AI, Kim J-Y, Rodriguez JA (2004) J Phys Chem B 108:13667–13673

    Article  CAS  Google Scholar 

  23. Kim JY, Rodriguez JA, Hanson JC, Frenkel AI, Lee PL (2003) J Am Chem Soc 125:10684–10692

    Article  CAS  Google Scholar 

  24. Kim JY, Hanson JC, Frenkel AI, Lee PL, Rodriguez JA (2004) J Phys Condens Matter 16:S3479–S3484

    Article  CAS  Google Scholar 

  25. Yamaguchi A, Shido T, Inada Y, Kogure T, Asakura K, Nomura M, Iwasawa Y (2001) Bull Chem Soc Jpn 74:801–808

    Article  CAS  Google Scholar 

  26. Reitz TL, Lee PL, Czaplewski KF, Lang JC, Popp KE, Kung HH (2001) J Catal 199:193–201

    Article  CAS  Google Scholar 

  27. Oguchi H, Kanai H, Utani K, Matsumura Y, Imamura S (2005) Appl Cat A 293:64–70

    Article  CAS  Google Scholar 

  28. Smith ML, Campos A, Spivey JJ (2012) Catal Today 182:60–66

    Google Scholar 

  29. Silversmit G, Poelman H, Balcaen V, Heynderickx PM, Olea M, Nikitenko S, Bras W, Smet PF, Poelman D, De Gryse R, Reniers MFO, Marin GB (2009) J Phys Chem Solids 70:1274–1284

    Article  CAS  Google Scholar 

  30. Aneggi E, Boaro M, de Leitenburg C, Dolcetti G, Trovarelli A (2006) J Alloys Compd 408–412:1096–1102

    Article  Google Scholar 

  31. Martinez-Arias A, Gamarra D, Fernandez-Garcia M, Wang XQ, Hanson JC, Rodriguez JA (2006) J Catal 240:1–7

    Article  CAS  Google Scholar 

  32. Cao Y, Casenas B, Pan W-P (2006) Energy Fuels 20:1845–1854

    Article  CAS  Google Scholar 

  33. Malinin GV, Tolmachev YM (1975) Russ Chem Rev 44:392

    Article  Google Scholar 

  34. Kirsch PD, Ekerdt JG (2001) J Appl Phys 90:4256

    Article  CAS  Google Scholar 

  35. Bera P, Aruna ST, Patil KC, Hegde MS (1999) J Catal 186:36–44

    Article  CAS  Google Scholar 

  36. Shapovalov V, Metiu H (2007) J Catal 245:205–214

    Article  CAS  Google Scholar 

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Acknowledgments

This work was supported by the ‘Long Term Structural Methusalem Funding by the Flemish Government’.

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Authors and Affiliations

  1. Laboratory for Chemical Technology, Ghent University, Krijgslaan 281, S5, 9000, Ghent, Belgium

    Vladimir V. Galvita, Hilde Poelman & Guy B. Marin

  2. Department of Solid State Sciences, Ghent University, Krijgslaan 281, S1, 9000, Ghent, Belgium

    Geert Rampelberg, Bob De Schutter & Christophe Detavernier

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  1. Vladimir V. Galvita
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  2. Hilde Poelman
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  3. Geert Rampelberg
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  4. Bob De Schutter
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  5. Christophe Detavernier
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  6. Guy B. Marin
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Correspondence to Vladimir V. Galvita.

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Galvita, V.V., Poelman, H., Rampelberg, G. et al. Structural and Kinetic Study of the Reduction of CuO–CeO2/Al2O3 by Time-Resolved X-ray Diffraction. Catal Lett 142, 959–968 (2012). https://doi.org/10.1007/s10562-012-0859-4

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