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Reactivity Aspects of SBA15-Based Doped Supported Catalysts: H2O2 Direct Synthesis and Disproportionation Reactions

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Abstract

Pd and PdAu catalysts supported on SBA15 and SiO2 were prepared and investigated for H2O2 direct synthesis in a batch autoclave (10 °C and 17.5 bar) and in the absence of halides and acids. The SiO2 supported catalysts exhibited inferior performances compared to the mesoporous ordered SBA15. A good control of both the catalysts dispersion and nanoparticle stability was achieved using SBA15. Catalysts were doped with bromine, a promoter in the H2O2 direct synthesis. Productivity and selectivity decreased when bromine was incorporated in the catalysts, thus indicating a possible poisoning due to the grafting process. A synergetic effect between Pd and Au was observed both in presence and absence of bromopropylsilane grafting on the catalyst surface. Three modifiers of the SBA15 support (Al, CeO2 and Ti) were chosen to elucidate the influence of the surface properties on metal dispersion and catalytic performance. Higher productivity and selectivity were achieved incorporating Al into the SBA15 framework, whereas neither Ti nor CeO2 improved H2O2 yields. The enhanced performance observed for the Prau/Al–SBA15 catalysts was attributed to the increased number of Brønsted acid sites. A modification of this catalyst with bromine was confirmed to impair both productivity and selectivity, possibly due to the broader particle size distribution and the poor stability of the metal nanoparticles, as demonstrate by transmission electron microscopy (TEM) images. H2O2 disproportionation was also investigated. A much slower reaction rate was observed compared to the H2O2 production, suggesting that the major contributor in the process of H2O2 destruction must be connected to the hydrogenation reaction.

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Acknowledgments

N. Gemo gratefully acknowledges the Cariparo Foundation and the Johan Gadolin Scholarship for financial support. P. Biasi gratefully acknowledges the Otto A. Malm Foundation for financial support. F. Menegazzo thanks INSTM (Florence) for postdoctoral fellowship. Prof. M. Modesti and Dr. S. Besco, Dipartimento di Ingegneria Industriale, University of Padova, are gratefully acknowledged for their precious help in the thermogravimetric analysis. This work is part of the activities at the Åbo Akademi Process Chemistry Centre (PCC) within the Finnish Centre of Excellence Programmes (2000–2005 and 2006–2011) by the Academy of Finland. In Sweden, the Bio4Energy programme and Kempe Foundations are acknowledged.

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Authors and Affiliations

  1. Dipartimento di Ingegneria Industriale, University of Padova, via Marzolo 9, 35131, Padua, Italy

    Nicola Gemo & Paolo Canu

  2. Department of Chemical Engineering, Process Chemistry Centre (PCC), Laboratory of Industrial Chemistry and Reaction Engineering, Åbo Akademi University, Biskopsgatan 8, 20500, Åbo-turku, Finland

    Nicola Gemo, Pierdomenico Biasi, Tapio O. Salmi & Jyri-Pekka Mikkola

  3. Department of Molecular Science and Nanosystems, Ca’ Foscari Venice University and Consortium INSTM UdR Ve, Dorsoduro 2137, Venetia, Italy

    Federica Menegazzo & Francesco Pinna

  4. Department of Chemistry, Chemical-Biochemical Centre (KBC), Technical Chemistry, Umeå University, 90187, Umeå, Sweden

    Ajaikumar Samikannu, Krisztián Kordás & Jyri-Pekka Mikkola

  5. Department of Electrical and Information Engineering, Microelectronics and Materials Physics Laboratories, University of Oulu, P.O. Box 4500, Oulu, 90014, Finland

    Krisztián Kordás

Authors
  1. Nicola Gemo
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  2. Pierdomenico Biasi
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  3. Paolo Canu
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  4. Federica Menegazzo
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  8. Tapio O. Salmi
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Corresponding authors

Correspondence to Pierdomenico Biasi or Jyri-Pekka Mikkola.

Additional information

Nicola Gemo and Pierdomenico Biasi contributed equally to the present work.

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Gemo, N., Biasi, P., Canu, P. et al. Reactivity Aspects of SBA15-Based Doped Supported Catalysts: H2O2 Direct Synthesis and Disproportionation Reactions. Top Catal 56, 540–549 (2013). https://doi.org/10.1007/s11244-013-0009-2

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