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Title: Importance of Low Dimensional CeO x Nanostructures in Pt/CeO x –TiO 2 Catalysts for the Water–Gas Shift Reaction

Abstract

CO 2 and H 2 production from the water–gas shift (WGS) reaction was studied over Pt/CeO x–TiO 2 catalysts with incremental loadings of CeO x, which adopts variations in the local morphology. The lowest loading of CeO x (1 wt % to 0.5 at. %) that is configured in its smallest dimensions exhibited the best WGS activity over larger dimensional structures. We attribute this to several factors including the ultrafine dispersed one-dimensional nanocluster geometry, a large concentration of Ce 3+ and enhanced reducibility of the low loadings. We utilized several in situ experiments to monitor the active state of the catalyst during the WGS reaction. X-ray diffraction (XRD) results showed lattice expansion that indicated reduced ceria was prevalent during the WGS reaction. On the surface, Ce 3+ related hydroxyl groups were identified by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The enhanced reducibility of the catalyst with the introduction of ceria was further revealed by H 2-temperature programed reduction (H 2-TPR) and good thermal stability was confirmed by in situ environmental transmission electron microscopy (ETEM). Finally, we also investigated the formation of the low dimensional structures during catalyst preparation, through a two-stage crystal growth of ceria crystallite on TiO 2more » nanoparticle: fine crystallites ~1D formed at ~250 °C, followed by crystal growth into 2D chain and 3D particle from 250–400 °C.« less

Authors:
; ; ; ORCiD logo; ; ; ; ; ORCiD logo
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1347370
Report Number(s):
BNL-113651-2017-JA
Journal ID: ISSN 1932-7447; R&D Project: CO009; KC0302010
Grant/Contract Number:  
SC00112704
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 121; Journal Issue: 12; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Luo, Si, Barrio, Laura, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Johnston-Peck, Aaron C., Xu, Wenqian, Stach, Eric A., Rodriguez, José A., and Senanayake, Sanjaya D. Importance of Low Dimensional CeO x Nanostructures in Pt/CeO x –TiO 2 Catalysts for the Water–Gas Shift Reaction. United States: N. p., 2017. Web. doi:10.1021/acs.jpcc.6b12285.
Luo, Si, Barrio, Laura, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Johnston-Peck, Aaron C., Xu, Wenqian, Stach, Eric A., Rodriguez, José A., & Senanayake, Sanjaya D. Importance of Low Dimensional CeO x Nanostructures in Pt/CeO x –TiO 2 Catalysts for the Water–Gas Shift Reaction. United States. doi:10.1021/acs.jpcc.6b12285.
Luo, Si, Barrio, Laura, Nguyen-Phan, Thuy-Duong, Vovchok, Dimitriy, Johnston-Peck, Aaron C., Xu, Wenqian, Stach, Eric A., Rodriguez, José A., and Senanayake, Sanjaya D. Wed . "Importance of Low Dimensional CeO x Nanostructures in Pt/CeO x –TiO 2 Catalysts for the Water–Gas Shift Reaction". United States. doi:10.1021/acs.jpcc.6b12285. https://www.osti.gov/servlets/purl/1347370.
@article{osti_1347370,
title = {Importance of Low Dimensional CeO x Nanostructures in Pt/CeO x –TiO 2 Catalysts for the Water–Gas Shift Reaction},
author = {Luo, Si and Barrio, Laura and Nguyen-Phan, Thuy-Duong and Vovchok, Dimitriy and Johnston-Peck, Aaron C. and Xu, Wenqian and Stach, Eric A. and Rodriguez, José A. and Senanayake, Sanjaya D.},
abstractNote = {CO2 and H2 production from the water–gas shift (WGS) reaction was studied over Pt/CeOx–TiO2 catalysts with incremental loadings of CeOx, which adopts variations in the local morphology. The lowest loading of CeOx (1 wt % to 0.5 at. %) that is configured in its smallest dimensions exhibited the best WGS activity over larger dimensional structures. We attribute this to several factors including the ultrafine dispersed one-dimensional nanocluster geometry, a large concentration of Ce3+ and enhanced reducibility of the low loadings. We utilized several in situ experiments to monitor the active state of the catalyst during the WGS reaction. X-ray diffraction (XRD) results showed lattice expansion that indicated reduced ceria was prevalent during the WGS reaction. On the surface, Ce3+ related hydroxyl groups were identified by diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS). The enhanced reducibility of the catalyst with the introduction of ceria was further revealed by H2-temperature programed reduction (H2-TPR) and good thermal stability was confirmed by in situ environmental transmission electron microscopy (ETEM). Finally, we also investigated the formation of the low dimensional structures during catalyst preparation, through a two-stage crystal growth of ceria crystallite on TiO2 nanoparticle: fine crystallites ~1D formed at ~250 °C, followed by crystal growth into 2D chain and 3D particle from 250–400 °C.},
doi = {10.1021/acs.jpcc.6b12285},
journal = {Journal of Physical Chemistry. C},
number = 12,
volume = 121,
place = {United States},
year = {Wed Mar 15 00:00:00 EDT 2017},
month = {Wed Mar 15 00:00:00 EDT 2017}
}

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