Unraveling the Origin of Photocatalytic Deactivation in CeO2/Nb2O5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species
Abstract
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 activemore »
- Authors:
-
[1];
[3];
[3];
[4];
[2];
[2]
- Adam Mickiewicz Univ., Poznan (Poland). Faculty of Chemistry; Normandie Univ, Caen (France). Centre National de la Recherche Scientifique (CNRS). ENSICAEN. UNICAEN. Laboratoire Catalyse et Spectrochimie
- Normandie Univ, Caen (France). Centre National de la Recherche Scientifique (CNRS). ENSICAEN. UNICAEN. Laboratoire Catalyse et Spectrochimie
- Iowa State Univ., Ames, IA (United States). Dept. of Chemistry; Ames Lab., Ames, IA (United States)
- Adam Mickiewicz Univ., Poznan (Poland). Faculty of Chemistry. Dept. of Rare Earths
- Publication Date:
- Research Org.:
- Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
- OSTI Identifier:
- 1815462
- Grant/Contract Number:
- AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 125; Journal Issue: 23; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Oxides; Alcohols; Catalysts; Transition metals; Materials
Citation Formats
Wolski, Lukasz, Lebedev, Oleg I., Harmer, Colin P., Kovnir, Kirill, Abdelli, Hanen, Grzyb, Tomasz, Daturi, Marco, and El-Roz, Mohamad. Unraveling the Origin of Photocatalytic Deactivation in CeO2/Nb2O5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species. United States: N. p., 2021.
Web. doi:10.1021/acs.jpcc.1c02812.
Wolski, Lukasz, Lebedev, Oleg I., Harmer, Colin P., Kovnir, Kirill, Abdelli, Hanen, Grzyb, Tomasz, Daturi, Marco, & El-Roz, Mohamad. Unraveling the Origin of Photocatalytic Deactivation in CeO2/Nb2O5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species. United States. https://doi.org/10.1021/acs.jpcc.1c02812
Wolski, Lukasz, Lebedev, Oleg I., Harmer, Colin P., Kovnir, Kirill, Abdelli, Hanen, Grzyb, Tomasz, Daturi, Marco, and El-Roz, Mohamad. Wed .
"Unraveling the Origin of Photocatalytic Deactivation in CeO2/Nb2O5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species". United States. https://doi.org/10.1021/acs.jpcc.1c02812. https://www.osti.gov/servlets/purl/1815462.
@article{osti_1815462,
title = {Unraveling the Origin of Photocatalytic Deactivation in CeO2/Nb2O5 Heterostructure Systems during Methanol Oxidation: Insight into the Role of Cerium Species},
author = {Wolski, Lukasz and Lebedev, Oleg I. and Harmer, Colin P. and Kovnir, Kirill and Abdelli, Hanen and Grzyb, Tomasz and Daturi, Marco and El-Roz, Mohamad},
abstractNote = {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.},
doi = {10.1021/acs.jpcc.1c02812},
journal = {Journal of Physical Chemistry. C},
number = 23,
volume = 125,
place = {United States},
year = {Wed Jun 02 00:00:00 EDT 2021},
month = {Wed Jun 02 00:00:00 EDT 2021}
}
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