Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms
- Autores
- Mendive, Cecilia Beatriz; Bredow, Thomas; Schneider, Jenny; Blesa, Miguel Angel; Bahnemann, Detlef
- Año de publicación
- 2015
- Idioma
- inglés
- Tipo de recurso
- artículo
- Estado
- versión publicada
- Descripción
- 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.
Fil: Mendive, Cecilia Beatriz. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina. Leibniz Universitaet Hannover; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Bredow, Thomas. Universitaet Bonn; Alemania
Fil: Schneider, Jenny. Leibniz Universitaet Hannover; Alemania
Fil: Blesa, Miguel Angel. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de General Sarmiento; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina
Fil: Bahnemann, Detlef. Leibniz Universitaet Hannover; Alemania - Materia
-
Oxalic Acid
Photocatalysis
Surface Complexes
Surface Reactions
Titanium Dioxide - Nivel de accesibilidad
- acceso abierto
- Condiciones de uso
- https://creativecommons.org/licenses/by-nc-nd/2.5/ar/
- Repositorio
- Institución
- Consejo Nacional de Investigaciones Científicas y Técnicas
- OAI Identificador
- oai:ri.conicet.gov.ar:11336/37578
Ver los metadatos del registro completo
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Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanismsMendive, Cecilia BeatrizBredow, ThomasSchneider, JennyBlesa, Miguel AngelBahnemann, DetlefOxalic AcidPhotocatalysisSurface ComplexesSurface ReactionsTitanium Dioxidehttps://purl.org/becyt/ford/1.4https://purl.org/becyt/ford/1It 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.Fil: Mendive, Cecilia Beatriz. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina. Leibniz Universitaet Hannover; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Bredow, Thomas. Universitaet Bonn; AlemaniaFil: Schneider, Jenny. Leibniz Universitaet Hannover; AlemaniaFil: Blesa, Miguel Angel. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de General Sarmiento; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; ArgentinaFil: Bahnemann, Detlef. Leibniz Universitaet Hannover; AlemaniaAcademic Press Inc Elsevier Science2015-02info:eu-repo/semantics/articleinfo:eu-repo/semantics/publishedVersionhttp://purl.org/coar/resource_type/c_6501info:ar-repo/semantics/articuloapplication/pdfapplication/pdfhttp://hdl.handle.net/11336/37578Mendive, Cecilia Beatriz; Bredow, Thomas; Schneider, Jenny; Blesa, Miguel Angel; Bahnemann, Detlef; Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms; Academic Press Inc Elsevier Science; Journal of Catalysis; 322; 2-2015; 60-720021-9517CONICET DigitalCONICETenginfo:eu-repo/semantics/altIdentifier/doi/10.1016/j.jcat.2014.11.008info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0021951714003200info:eu-repo/semantics/openAccesshttps://creativecommons.org/licenses/by-nc-nd/2.5/ar/reponame:CONICET Digital (CONICET)instname:Consejo Nacional de Investigaciones Científicas y Técnicas2025-09-29T09:40:14Zoai:ri.conicet.gov.ar:11336/37578instacron:CONICETInstitucionalhttp://ri.conicet.gov.ar/Organismo científico-tecnológicoNo correspondehttp://ri.conicet.gov.ar/oai/requestdasensio@conicet.gov.ar; lcarlino@conicet.gov.arArgentinaNo correspondeNo correspondeNo correspondeopendoar:34982025-09-29 09:40:14.652CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicasfalse |
dc.title.none.fl_str_mv |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
title |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
spellingShingle |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms Mendive, Cecilia Beatriz Oxalic Acid Photocatalysis Surface Complexes Surface Reactions Titanium Dioxide |
title_short |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
title_full |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
title_fullStr |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
title_full_unstemmed |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
title_sort |
Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms |
dc.creator.none.fl_str_mv |
Mendive, Cecilia Beatriz Bredow, Thomas Schneider, Jenny Blesa, Miguel Angel Bahnemann, Detlef |
author |
Mendive, Cecilia Beatriz |
author_facet |
Mendive, Cecilia Beatriz Bredow, Thomas Schneider, Jenny Blesa, Miguel Angel Bahnemann, Detlef |
author_role |
author |
author2 |
Bredow, Thomas Schneider, Jenny Blesa, Miguel Angel Bahnemann, Detlef |
author2_role |
author author author author |
dc.subject.none.fl_str_mv |
Oxalic Acid Photocatalysis Surface Complexes Surface Reactions Titanium Dioxide |
topic |
Oxalic Acid Photocatalysis Surface Complexes Surface Reactions Titanium Dioxide |
purl_subject.fl_str_mv |
https://purl.org/becyt/ford/1.4 https://purl.org/becyt/ford/1 |
dc.description.none.fl_txt_mv |
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. Fil: Mendive, Cecilia Beatriz. Universidad Nacional de Mar del Plata. Facultad de Ciencias Exactas y Naturales. Departamento de Química; Argentina. Leibniz Universitaet Hannover; Alemania. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina Fil: Bredow, Thomas. Universitaet Bonn; Alemania Fil: Schneider, Jenny. Leibniz Universitaet Hannover; Alemania Fil: Blesa, Miguel Angel. Comisión Nacional de Energía Atómica; Argentina. Universidad Nacional de General Sarmiento; Argentina. Consejo Nacional de Investigaciones Científicas y Técnicas; Argentina Fil: Bahnemann, Detlef. Leibniz Universitaet Hannover; Alemania |
description |
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. |
publishDate |
2015 |
dc.date.none.fl_str_mv |
2015-02 |
dc.type.none.fl_str_mv |
info:eu-repo/semantics/article info:eu-repo/semantics/publishedVersion http://purl.org/coar/resource_type/c_6501 info:ar-repo/semantics/articulo |
format |
article |
status_str |
publishedVersion |
dc.identifier.none.fl_str_mv |
http://hdl.handle.net/11336/37578 Mendive, Cecilia Beatriz; Bredow, Thomas; Schneider, Jenny; Blesa, Miguel Angel; Bahnemann, Detlef; Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms; Academic Press Inc Elsevier Science; Journal of Catalysis; 322; 2-2015; 60-72 0021-9517 CONICET Digital CONICET |
url |
http://hdl.handle.net/11336/37578 |
identifier_str_mv |
Mendive, Cecilia Beatriz; Bredow, Thomas; Schneider, Jenny; Blesa, Miguel Angel; Bahnemann, Detlef; Oxalic acid at the TiO2/water interface under UV(A) illumination: Surface reaction mechanisms; Academic Press Inc Elsevier Science; Journal of Catalysis; 322; 2-2015; 60-72 0021-9517 CONICET Digital CONICET |
dc.language.none.fl_str_mv |
eng |
language |
eng |
dc.relation.none.fl_str_mv |
info:eu-repo/semantics/altIdentifier/doi/10.1016/j.jcat.2014.11.008 info:eu-repo/semantics/altIdentifier/url/https://www.sciencedirect.com/science/article/pii/S0021951714003200 |
dc.rights.none.fl_str_mv |
info:eu-repo/semantics/openAccess https://creativecommons.org/licenses/by-nc-nd/2.5/ar/ |
eu_rights_str_mv |
openAccess |
rights_invalid_str_mv |
https://creativecommons.org/licenses/by-nc-nd/2.5/ar/ |
dc.format.none.fl_str_mv |
application/pdf application/pdf |
dc.publisher.none.fl_str_mv |
Academic Press Inc Elsevier Science |
publisher.none.fl_str_mv |
Academic Press Inc Elsevier Science |
dc.source.none.fl_str_mv |
reponame:CONICET Digital (CONICET) instname:Consejo Nacional de Investigaciones Científicas y Técnicas |
reponame_str |
CONICET Digital (CONICET) |
collection |
CONICET Digital (CONICET) |
instname_str |
Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.name.fl_str_mv |
CONICET Digital (CONICET) - Consejo Nacional de Investigaciones Científicas y Técnicas |
repository.mail.fl_str_mv |
dasensio@conicet.gov.ar; lcarlino@conicet.gov.ar |
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1844613273319636992 |
score |
13.070432 |