Elucidating the interaction between Ni and CeOx in ethanol steam reforming catalysts: A perspective of recent studies over model and powder systems
Abstract
Bulk metallic nickel is a poor catalyst for the reforming of oxygenates being deactivated by the deposition of coke. In contrast, Ni-ceria is an active system for the catalytic extraction of H2 from the ethanol steam reforming reaction (ESR, C2H5OH + 3H2O ↔ 2CO2 + 6H2). Numerous studies, with model (well-defined crystal surfaces) and technical (high surface area powders) catalysts, have been devoted to understand the fundamental role of each catalyst component, the performance of adjacent sites in the metal-oxide interface, and the complex mechanistic steps that convert two oxygenated reactants (ethanol and H2O) into H2. The size and low loading of Ni on ceria facilitate metal-oxide support interactions that probably enhance the reactivity of the system. To establish the precise role of both Ni and Ce is challenging. However it is clear that both Ni and Ce are associated with the dissociation of H2O (OH + H), while ceria readily adsorbs and partially dissociates ethanol (i.e. ethoxy formation). The most difficult step of Csingle bondC bond dissociation likely occurs only on Ni or at the Ni-Ce interface. H2O and OH remain as important agents for the prevention of excess C build up during the Csingle bondH/Csingle bondC dissociation process.more »
- Authors:
-
- Brookhaven National Lab. (BNL), Upton, NY (United States); SUNY Stony Brook, Stony Brook, NY (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1377056
- Alternate Identifier(s):
- OSTI ID: 1331071; OSTI ID: 1397032
- Report Number(s):
- BNL-114203-2017-JA; BNL-113171-2016-JA
Journal ID: ISSN 0926-3373; R&D Project: CO040; KC0302010
- Grant/Contract Number:
- SC00112704; SC0012704
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Applied Catalysis B: Environmental
- Additional Journal Information:
- Journal Volume: 197; Journal Issue: C; Journal ID: ISSN 0926-3373
- Publisher:
- Elsevier
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Ceria; Nickel; Ethanol steam reforming; Hydrogen generation; Water
Citation Formats
Liu, Zongyuan, Senanayake, Sanjaya D., and Rodriguez, Jose A. Elucidating the interaction between Ni and CeOx in ethanol steam reforming catalysts: A perspective of recent studies over model and powder systems. United States: N. p., 2016.
Web. doi:10.1016/j.apcatb.2016.03.013.
Liu, Zongyuan, Senanayake, Sanjaya D., & Rodriguez, Jose A. Elucidating the interaction between Ni and CeOx in ethanol steam reforming catalysts: A perspective of recent studies over model and powder systems. United States. https://doi.org/10.1016/j.apcatb.2016.03.013
Liu, Zongyuan, Senanayake, Sanjaya D., and Rodriguez, Jose A. Tue .
"Elucidating the interaction between Ni and CeOx in ethanol steam reforming catalysts: A perspective of recent studies over model and powder systems". United States. https://doi.org/10.1016/j.apcatb.2016.03.013. https://www.osti.gov/servlets/purl/1377056.
@article{osti_1377056,
title = {Elucidating the interaction between Ni and CeOx in ethanol steam reforming catalysts: A perspective of recent studies over model and powder systems},
author = {Liu, Zongyuan and Senanayake, Sanjaya D. and Rodriguez, Jose A.},
abstractNote = {Bulk metallic nickel is a poor catalyst for the reforming of oxygenates being deactivated by the deposition of coke. In contrast, Ni-ceria is an active system for the catalytic extraction of H2 from the ethanol steam reforming reaction (ESR, C2H5OH + 3H2O ↔ 2CO2 + 6H2). Numerous studies, with model (well-defined crystal surfaces) and technical (high surface area powders) catalysts, have been devoted to understand the fundamental role of each catalyst component, the performance of adjacent sites in the metal-oxide interface, and the complex mechanistic steps that convert two oxygenated reactants (ethanol and H2O) into H2. The size and low loading of Ni on ceria facilitate metal-oxide support interactions that probably enhance the reactivity of the system. To establish the precise role of both Ni and Ce is challenging. However it is clear that both Ni and Ce are associated with the dissociation of H2O (OH + H), while ceria readily adsorbs and partially dissociates ethanol (i.e. ethoxy formation). The most difficult step of Csingle bondC bond dissociation likely occurs only on Ni or at the Ni-Ce interface. H2O and OH remain as important agents for the prevention of excess C build up during the Csingle bondH/Csingle bondC dissociation process. Often, deactivation upon C build up, is a direct result of Ni sintering and decoupling of the Ni-Ce interactions. One strategy to maintain good activity and stability is to protect the Ni-Ce interaction, and this can be achieved through the use of solid solutions (Ce1–xNixO2–y) or by employing stabilizing agents such as W (NixWyCezO2). In this paper, we present and discuss the most recent work for the ESR reaction and show the important role of ceria which participates directly in the reaction and also enhances catalytic activity through metal-support interactions.},
doi = {10.1016/j.apcatb.2016.03.013},
journal = {Applied Catalysis B: Environmental},
number = C,
volume = 197,
place = {United States},
year = {Tue Mar 08 00:00:00 EST 2016},
month = {Tue Mar 08 00:00:00 EST 2016}
}
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Works referencing / citing this record:
Growth and structure of ultrathin praseodymium oxide layers on ruthenium(0001)
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Dry Reforming of Shale Gas and Carbon Dioxide with Ni-Ce-Al 2 O 3 Catalyst: Syngas Production Enhanced over Ni-CeO x Formation
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- ChemCatChem, Vol. 10, Issue 20