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Title: Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes

Abstract

Support plays a complex role in catalysis by supported metal oxides and the exact support effect still remains elusive. One of the approaches to gain fundamental insights into the support effect is to utilize model support systems. In this study, we employed for the first time titania nanoshapes as the model supports and investigated how the variation of surface structure of the support (titania, TiO2) impacts the catalysis of supported oxide (vanadia, VOx). TiO2 truncated rhombi, spheres and rods were synthesized via hydrothermal method and characterized with XRD and TEM. These TiO2 nanoshapes represent different mixtures of surface facets including [1 0 1], [0 1 0] and [0 0 1] and were used to support vanadia. The structure of supported VOx species was characterized in detail with in situ Raman spectroscopy as a function of loading on the three TiO2 nanoshapes. Oxidative dehydrogenation (ODH) of isobutane to isobutene was used as a model reaction to test how the support shape influences the activity, selectivity and activation energy of the surface VOx species. It was shown that the shape of TiO2 support does not pose evident effect on either the structure of surface VOx species or the catalytic performance of surfacemore » VOx species in isobutane ODH reaction. Finally, this insignificant support shape effect was ascribed to the small difference in the surface oxygen vacancy formation energy among the different TiO2 surfaces and the multi-faceting nature of the TiO2 nanoshapes.« less

Authors:
 [1];  [1];  [1];  [1]; ;  [1];  [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Energy Frontier Research Centers (EFRC) (United States). Center for Understanding and Control of Acid Gas-induced Evolution of Materials for Energy (UNCAGE-ME)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1286865
Alternate Identifier(s):
OSTI ID: 1252539
Grant/Contract Number:  
AC05-00OR22725; SC0012577
Resource Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 263; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Titania; Vanadia; Support effect; Nanoshapes; Surface facets; Surface structure; Oxygen vacancy formation energy; Isobutane oxidative dehydrogenation; Raman spectroscopy

Citation Formats

Kraemer, Shannon K., Rondinone, Adam Justin, Tsai, Yu-Tung, Schwartz, Viviane, Steven H. Overbury, Idrobo, Juan-Carlos, and Wu, Zili. Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes. United States: N. p., 2015. Web. https://doi.org/10.1016/j.cattod.2015.09.049.
Kraemer, Shannon K., Rondinone, Adam Justin, Tsai, Yu-Tung, Schwartz, Viviane, Steven H. Overbury, Idrobo, Juan-Carlos, & Wu, Zili. Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes. United States. https://doi.org/10.1016/j.cattod.2015.09.049
Kraemer, Shannon K., Rondinone, Adam Justin, Tsai, Yu-Tung, Schwartz, Viviane, Steven H. Overbury, Idrobo, Juan-Carlos, and Wu, Zili. Mon . "Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes". United States. https://doi.org/10.1016/j.cattod.2015.09.049. https://www.osti.gov/servlets/purl/1286865.
@article{osti_1286865,
title = {Oxidative dehydrogenation of isobutane over vanadia catalysts supported by titania nanoshapes},
author = {Kraemer, Shannon K. and Rondinone, Adam Justin and Tsai, Yu-Tung and Schwartz, Viviane and Steven H. Overbury and Idrobo, Juan-Carlos and Wu, Zili},
abstractNote = {Support plays a complex role in catalysis by supported metal oxides and the exact support effect still remains elusive. One of the approaches to gain fundamental insights into the support effect is to utilize model support systems. In this study, we employed for the first time titania nanoshapes as the model supports and investigated how the variation of surface structure of the support (titania, TiO2) impacts the catalysis of supported oxide (vanadia, VOx). TiO2 truncated rhombi, spheres and rods were synthesized via hydrothermal method and characterized with XRD and TEM. These TiO2 nanoshapes represent different mixtures of surface facets including [1 0 1], [0 1 0] and [0 0 1] and were used to support vanadia. The structure of supported VOx species was characterized in detail with in situ Raman spectroscopy as a function of loading on the three TiO2 nanoshapes. Oxidative dehydrogenation (ODH) of isobutane to isobutene was used as a model reaction to test how the support shape influences the activity, selectivity and activation energy of the surface VOx species. It was shown that the shape of TiO2 support does not pose evident effect on either the structure of surface VOx species or the catalytic performance of surface VOx species in isobutane ODH reaction. Finally, this insignificant support shape effect was ascribed to the small difference in the surface oxygen vacancy formation energy among the different TiO2 surfaces and the multi-faceting nature of the TiO2 nanoshapes.},
doi = {10.1016/j.cattod.2015.09.049},
journal = {Catalysis Today},
number = ,
volume = 263,
place = {United States},
year = {2015},
month = {11}
}

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