The role of CO 2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst
Abstract
Catalytic performance and the nature of surface adsorbates were investigated for high-surface-area ceria during ethylbenzene oxidative dehydrogenation (ODH) reaction using CO2 as a soft oxidant. A template assisted method was used to synthesize the high-surface-area ceria. The interactions between ethylbenzene, styrene and CO2 on the surface of ceria and the role of CO2 for the ethylbenzene ODH reaction have been investigated in detail by using activity test, in situ Diffuse Reflectance Infrared and Raman spectroscopy. Not only did CO2 as an oxidant favor the higher yield of styrene, but it also inhibited the deposition of coke during the ethylbenzene ODH reaction. Ethylbenzene ODH reaction over ceria followed a two-step pathway: Ethylbenzene is first dehydrogenated to styrene with H2 formed simultaneously, and then CO2 reacts with H2 via the reverse water gas shift. The styrene produced can easily polymerize to form polystyrene, a key intermediate for coke formation. In the absence of CO2, the polystyrene transforms into graphite-like coke at temperatures above 500 °C, which leads to catalyst deactivation. While in the presence of CO2, the coke deposition can be effectively removed via oxidation with CO2.
- Authors:
-
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Ames Lab., Ames, IA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1222559
- Alternate Identifier(s):
- OSTI ID: 1234459; OSTI ID: 1287018
- Report Number(s):
- IS-J-8866
Journal ID: ISSN 2155-5435; ED2801000; CEED500
- Grant/Contract Number:
- AC05-00OR22725; AC02-07CH11358
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Catalysis
- Additional Journal Information:
- Journal Volume: 5; Journal Issue: 10; Journal ID: ISSN 2155-5435
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; high-surface-area ceria; oxidative dehydrogenation; ethylbenzene; styrene; CO2; infrared spectroscopy; Raman spectroscopy; coking; CO2
Citation Formats
Zhang, Li, Wu, Zili, Nelson, Nicholas, Sadow, Aaron D., Slowing, Igor I., and Overbury, Steven H. The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst. United States: N. p., 2015.
Web. doi:10.1021/acscatal.5b01519.
Zhang, Li, Wu, Zili, Nelson, Nicholas, Sadow, Aaron D., Slowing, Igor I., & Overbury, Steven H. The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst. United States. doi:10.1021/acscatal.5b01519.
Zhang, Li, Wu, Zili, Nelson, Nicholas, Sadow, Aaron D., Slowing, Igor I., and Overbury, Steven H. Tue .
"The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst". United States. doi:10.1021/acscatal.5b01519. https://www.osti.gov/servlets/purl/1222559.
@article{osti_1222559,
title = {The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst},
author = {Zhang, Li and Wu, Zili and Nelson, Nicholas and Sadow, Aaron D. and Slowing, Igor I. and Overbury, Steven H.},
abstractNote = {Catalytic performance and the nature of surface adsorbates were investigated for high-surface-area ceria during ethylbenzene oxidative dehydrogenation (ODH) reaction using CO2 as a soft oxidant. A template assisted method was used to synthesize the high-surface-area ceria. The interactions between ethylbenzene, styrene and CO2 on the surface of ceria and the role of CO2 for the ethylbenzene ODH reaction have been investigated in detail by using activity test, in situ Diffuse Reflectance Infrared and Raman spectroscopy. Not only did CO2 as an oxidant favor the higher yield of styrene, but it also inhibited the deposition of coke during the ethylbenzene ODH reaction. Ethylbenzene ODH reaction over ceria followed a two-step pathway: Ethylbenzene is first dehydrogenated to styrene with H2 formed simultaneously, and then CO2 reacts with H2 via the reverse water gas shift. The styrene produced can easily polymerize to form polystyrene, a key intermediate for coke formation. In the absence of CO2, the polystyrene transforms into graphite-like coke at temperatures above 500 °C, which leads to catalyst deactivation. While in the presence of CO2, the coke deposition can be effectively removed via oxidation with CO2.},
doi = {10.1021/acscatal.5b01519},
journal = {ACS Catalysis},
number = 10,
volume = 5,
place = {United States},
year = {2015},
month = {9}
}
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