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    Experimental Microkinetic Approach of De-NO x by NH 3 on V 2 O 5 /WO 3 /TiO 2 Catalysts. 4. Individual Heats of Adsorption of Adsorbed H 2 O Species on Sulfate-Free and Sulfated TiO 2 Supports

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    Type
    Article
    Authors
    Giraud, François
    Couble, Julien
    Geantet, Christophe
    Guilhaume, Nolven
    Puzenat, Eric
    Gros, Sébastien
    Porcheron, Lynda
    Kanniche, Mohamed
    Bianchi, Daniel
    Date
    2015-07
    Online Publication Date
    2015-07
    Print Publication Date
    2015-07-16
    Permanent link to this record
    http://hdl.handle.net/10754/598285
    
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    Abstract
    © 2015 American Chemical Society. The present study is a part of an experimental microkinetic approach of the removal of NOx from coal-fired power plants by reduction with NH3 on V2O5/WO3/TiO2 catalysts (NH3-selective catalytic reduction, NH3-SCR). It is dedicated to the characterization of the heats of adsorption of molecularly adsorbed H2Oads species formed on sulfate-free and sulfated TiO2 supports. Water, which is always present during the NH3-SCR, may be in competition and/or react (formation of NH4$^{+}$) with the adsorbed NH3 species controlling the coverage of the adsorbed intermediate species of the reaction. Mainly, an original experimental procedure named adsorption equilibrium infrared spectroscopy (AEIR) previously used for the adsorption of NH3 species on the same solids is adapted for the adsorption of H2O. At Ta = 300 K and for PH2 O ≤ 1 kPa, three main H2Oads species are formed (associated with a minor amount of dissociated H2O species) on the two TiO2 solids. The species are identified by the positions of their IR bands in the 3750-3000 cm$^{-1}$ range. Considering the decreasing order of stability, they are (a) coordinated to strong (L2) and weak (L1) Lewis sites and denoted H2O ads-L2 and H2Oads-L1, respectively, and (b) hydrogen bonded to the H2Oads-L species and on O$^{2-}$/OH sites of the solids (denoted H2Owads). The three species have a common well-defined δH2O IR band at a position in the range 1640-1610 cm$^{-1}$ according to the total coverage of the surface. According to the AEIR method, the evolution of the intensity of this IR band during the increase in the adsorption temperature Ta in isobaric condition provides the evolution of the average coverage of the three species and then to their individual heats of adsorption as a function of their coverage. It is shown that there are no significant differences on the two TiO2 solids. In particular, the heat of adsorption of the H2Oads-L2 species varies from ∼114 to 61 kJ/mol at low and high coverages respectively, indicating that it can be present in the experimental conditions of the NH3-SCR. In a forthcoming article, the competitive chemisorptions and reaction between adsorbed H2O and NH3 species are studied and modeled on the TiO2 supports and model and commercial V2O5/WO3/TiO2 catalysts.
    Citation
    Giraud F, Couble J, Geantet C, Guilhaume N, Puzenat E, et al. (2015) Experimental Microkinetic Approach of De-NO x by NH 3 on V 2 O 5 /WO 3 /TiO 2 Catalysts. 4. Individual Heats of Adsorption of Adsorbed H 2 O Species on Sulfate-Free and Sulfated TiO 2 Supports . The Journal of Physical Chemistry C 119: 16089–16105. Available: http://dx.doi.org/10.1021/acs.jpcc.5b04147.
    Sponsors
    We thank Eva Diaz-Marti from Millenium Inorganic Chemicals, a Crystal Global company, for providing the TiO2-DT51 sample. D.B. thanks the “Institut de Chimie de Lyon” for the purchase of the mass spectrometer in the framework of the “Contrat de Projets Etat-Région” Rhône-Alpes (2007–2013). Thanks are due to King Abdullah University of Science and Technology (KAUST, Saudi Arabia) for the financial support (Award No. UK-C0017) of J.C.’s postdoctoral grant in the framework of the CADENCED project.
    Publisher
    American Chemical Society (ACS)
    Journal
    The Journal of Physical Chemistry C
    DOI
    10.1021/acs.jpcc.5b04147
    ae974a485f413a2113503eed53cd6c53
    10.1021/acs.jpcc.5b04147
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