Unraveling the Origin of Photocatalytic Deactivation in CeO 2 /Nb 2 O 5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species
| Autor: | Tomasz Grzyb, Kirill Kovnir, Colin P. Harmer, Hanen Abdelli, Mohamad El-Roz, Lukasz Wolski, Marco Daturi, Oleg I. Lebedev |
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| Přispěvatelé: | Laboratoire catalyse et spectrochimie (LCS), Centre National de la Recherche Scientifique (CNRS)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Université de Caen Normandie (UNICAEN), Normandie Université (NU), Laboratoire de cristallographie et sciences des matériaux (CRISMAT), Université de Caen Normandie (UNICAEN), Normandie Université (NU)-Normandie Université (NU)-École Nationale Supérieure d'Ingénieurs de Caen (ENSICAEN), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS)-Institut de Recherche sur les Matériaux Avancés (IRMA), Normandie Université (NU)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Normandie Université (NU)-Institut national des sciences appliquées Rouen Normandie (INSA Rouen Normandie), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Université de Rouen Normandie (UNIROUEN), Institut National des Sciences Appliquées (INSA)-Normandie Université (NU)-Institut National des Sciences Appliquées (INSA)-Centre National de la Recherche Scientifique (CNRS), Iowa State University (ISU), Normandie Université (NU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS) |
| Jazyk: | angličtina |
| Rok vydání: | 2021 |
| Předmět: |
Photoluminescence
Materials science chemistry.chemical_element 02 engineering and technology 010402 general chemistry 01 natural sciences Article X-ray photoelectron spectroscopy Physisorption [CHIM]Chemical Sciences Physical and Theoretical Chemistry ComputingMilieux_MISCELLANEOUS business.industry Heterojunction 021001 nanoscience & nanotechnology 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials Cerium General Energy Semiconductor chemistry Chemical engineering Photocatalysis Charge carrier 0210 nano-technology business |
| Zdroj: | Journal of Physical Chemistry C Journal of Physical Chemistry C, American Chemical Society, 2021, 125 (23), pp.12650-12662. ⟨10.1021/acs.jpcc.1c02812⟩ Journal of Physical Chemistry C, 2021, 125 (23), pp.12650-12662. ⟨10.1021/acs.jpcc.1c02812⟩ The Journal of Physical Chemistry. C, Nanomaterials and Interfaces |
| ISSN: | 1932-7447 1932-7455 |
| DOI: | 10.1021/acs.jpcc.1c02812⟩ |
| Popis: | The study provides deep insight into the origin of photocatalytic deactivation of Nb2O5 after modification with ceria. Of particular interest was to fully understand the role of ceria species in diminishing the photocatalytic performance of CeO2/Nb2O5 heterostructures. For this purpose, ceria was loaded on niobia surfaces by wet impregnation. The as-prepared materials were characterized by powder X-ray diffraction, nitrogen physisorption, UV-visible spectroscopy, X-ray photoelectron spectroscopy, high-resolution transmission electron microscopy, and photoluminescence measurements. Photocatalytic activity of parent metal oxides (i.e., Nb2O5 and CeO2) and as-prepared CeO2/Nb2O5 heterostructures with different ceria loadings were tested in methanol photooxidation, a model gas-phase reaction. Deep insight into the photocatalytic process provided by operando-IR techniques combined with results of photoluminescence studies revealed that deactivation of CeO2/Nb2O5 heterostructures resulted from increased recombination of photo-excited electrons and holes. The main factor contributing to more efficient recombination of the charge carriers in the heterostructures was the ultrafine size of the ceria species. The presence of such highly dispersed ceria species on the niobia surface provided a strong interface between these two semiconductors, enabling efficient charge transfer from Nb2O5 to CeO2. However, the ceria species supported on niobia exhibited a high defect site concentration, which acted as highly active recombination centers for the photo-induced charge carriers. |
| Databáze: | OpenAIRE |
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