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Abstract:

It is through the comparison of experimental results and theoretical calculations that the mechanistic details of several surface photoreactions initiated upon UV(A) illumination of adsorbed oxalic acid on rutile and anatase can be proposed. The absorption of light is found to be rather localized at surface Ti atoms and at the adsorbed species on both TiO2 polymorphs, respectively. Different surface complexes exhibit different photoreactivities, and consequently, each of them may follow a different reaction mechanism. Experimental data can be explained involving reactions such as the interconversion of monodentate into bidentate species which may further be oxidized to CO2 or may even produce OH radicals, while the reduction of monodentate species to the respective aldehyde results in combination with the oxidation of a neighbouring adsorbed OH group into the formation of an adsorbed OOH radical. On the basis of the results presented herein, it is concluded that the direct action of the photocatalytically produced electron-hole pairs on the adsorbed species is the primary step of the photocatalytic reaction, while the intermediate formation of free radical species followed by their reaction with an oxalate molecule can be regarded as a secondary process. Within the system described in this work, OH radicals only appear to be produced following the direct interaction of a hole with the adsorbed organic compound, but not with chemisorbed water molecules. © 2014 Elsevier Inc. All rights reserved.

Registro:

Documento: Artículo
Título:Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms
Autor:Mendive, C.B.; Bredow, T.; Schneider, J.; Blesa, M.; Bahnemann, D.
Filiación:Departamento de Química, Facultad de Ciencias Exactas y Naturales, Universidad Nacional de Mar Del Plata, B7600AYL, Dean Funes, Mar del Plata, Argentina
Institut für Technische Chemie, Leibniz Universität Hannover, Callinstr. 3, Hannover, Germany
Mulliken Center for Theoretical Chemistry, Institut für Physikalische und Theoretische Chemie, Universität Bonn, Beringstraße 4, Bonn, Germany
Postgraduate School, Universidad Nacional de General San Martín, 1 Piso B1650ANQ San Martín, Peatonal Belgrano, Buenos Aires, Argentina
Laboratory for Nanocomposite Materials, Department of Photonics, Faculty of Physics, Saint-Petersburg State University, Peterhof, Ulianovskaia str. 3, Saint-Petersburg, Russian Federation
Palabras clave:Oxalic acid; Photocatalysis; Surface complexes; Surface reactions; Titanium dioxide; Free radicals; Molecules; Organic acids; Oxalic acid; Oxide minerals; Photocatalysis; Photoreactivity; Reaction intermediates; Titanium dioxide; Direct interactions; Electron hole pairs; Free radical species; Intermediate formation; Photocatalytic reactions; Surface complex; Surface reaction mechanism; Theoretical calculations; Surface reactions
Año:2015
Volumen:322
Página de inicio:60
Página de fin:72
DOI: http://dx.doi.org/10.1016/j.jcat.2014.11.008
Título revista:Journal of Catalysis
Título revista abreviado:J. Catal.
ISSN:00219517
CODEN:JCTLA
Registro:https://bibliotecadigital.exactas.uba.ar/collection/paper/document/paper_00219517_v322_n_p60_Mendive

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Citas:

---------- APA ----------
Mendive, C.B., Bredow, T., Schneider, J., Blesa, M. & Bahnemann, D. (2015) . Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms. Journal of Catalysis, 322, 60-72.
http://dx.doi.org/10.1016/j.jcat.2014.11.008
---------- CHICAGO ----------
Mendive, C.B., Bredow, T., Schneider, J., Blesa, M., Bahnemann, D. "Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms" . Journal of Catalysis 322 (2015) : 60-72.
http://dx.doi.org/10.1016/j.jcat.2014.11.008
---------- MLA ----------
Mendive, C.B., Bredow, T., Schneider, J., Blesa, M., Bahnemann, D. "Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms" . Journal of Catalysis, vol. 322, 2015, pp. 60-72.
http://dx.doi.org/10.1016/j.jcat.2014.11.008
---------- VANCOUVER ----------
Mendive, C.B., Bredow, T., Schneider, J., Blesa, M., Bahnemann, D. Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms. J. Catal. 2015;322:60-72.
http://dx.doi.org/10.1016/j.jcat.2014.11.008