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

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.

doi:10.1021/acs.jpcc.6b12285

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

Journal Article · Wed Mar 15 00:00:00 EDT 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.6b12285· OSTI ID:1347370

Luo, Si; Barrio, Laura; Nguyen-Phan, Thuy-Duong;

; Johnston-Peck, Aaron C.; Xu, Wenqian; Stach, Eric A.; Rodriguez, José A.;

CO₂ and H₂ production from the water–gas shift (WGS) reaction was studied over Pt/CeO_x–TiO₂ 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 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.

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Research Organization:: Brookhaven National Lab. (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1347370

Report Number(s):: BNL-113651-2017-JA; R&D Project: CO009; KC0302010

Journal Information:: Journal of Physical Chemistry. C, Vol. 121, Issue 12; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 16 works

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N ‐Methylation of N ‐Methylaniline with Carbon Dioxide and Molecular Hydrogen over a Heterogeneous Non‐Noble Metal Cu/TiO ₂ Catalyst Liu, Ke; Zhao, Zhenbo; Lin, Weiwei ChemCatChem, Vol. 11, Issue 16 https://doi.org/10.1002/cctc.201900582	journal	May 2019
Black TiO _2−x with stable surface oxygen vacancies as the support of efficient gold catalysts for water-gas shift reaction Li, Lei; Song, Li; Zhu, Longfeng Catalysis Science & Technology, Vol. 8, Issue 5 https://doi.org/10.1039/c7cy02429k	journal	January 2018

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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