The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst

Zhang, Li; Wu, Zili; Nelson, Nicholas; Sadow, Aaron D.; Slowing, Igor I.; Overbury, Steven H.

doi:10.1021/acscatal.5b01519

Title: The role of CO₂ as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst

Journal Article · Tue Sep 22 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b01519· OSTI ID:1222559

Zhang, Li ^[1]; Wu, Zili ^[1]; Nelson, Nicholas ^[2]; Sadow, Aaron D. ^[2]; Slowing, Igor I. ^[2]; Overbury, Steven H. ^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Iowa State Univ., Ames, IA (United States); Ames Lab., Ames, IA (United States)

Catalytic performance and the nature of surface adsorbates were investigated for high-surface-area ceria during the ethylbenzene oxidative dehydrogenation (ODH) reaction using CO₂ as a soft oxidant. The high surface area ceria material was synthesized using a template-assisted method. The interactions among 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. CO₂ as an oxidant not only favored the higher yield of styrene but 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 produced styrene can easily undergo polymerization to form polystyrene, which is a key intermediate for coke formation. Furthermore, in the absence of CO₂, the produced polystyrene transforms into graphite-like coke at temperatures above 500°C, which leads to catalyst deactivation. In the presence of CO₂, the coke deposition can be effectively removed via oxidation with CO₂.

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Research Organization:: Ames Laboratory (AMES), Ames, IA (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: AC05-00OR22725; AC02-07CH11358

OSTI ID:: 1222559

Alternate ID(s):: OSTI ID: 1234459; OSTI ID: 1287018

Report Number(s):: IS-J-8866; ED2801000; CEED500

Journal Information:: ACS Catalysis, Vol. 5, Issue 10; ISSN 2155-5435

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 73 works

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
high-surface-area ceria
oxidative dehydrogenation
ethylbenzene
styrene
CO2
infrared spectroscopy
Raman spectroscopy
coking
CO2

Title: The role of CO2 as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst

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Title: The role of CO₂ as a soft oxidant for dehydrogenation of ethylbenzene to styrene over a high-surface-area ceria catalyst