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Naphthalene on Ni(111): Experimental and Theoretical Insights into Adsorption, Dehydrogenation, and Carbon Passivation
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemical Engineering.ORCID iD: 0000-0002-5395-599X
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2017 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 121, no 40, p. 22199-22207Article in journal (Refereed) Published
Abstract [en]

An attractive solution to mitigate tars and also to decompose lighter hydrocarbons in biomass gasification is secondary catalytic reforming, converting hydrocarbons to useful permanent gases. Albeit that it has been in use for a long time in fossil feedstock catalytic steam reforming, understanding of the catalytic processes is still limited. Naphthalene is typically present in the biomass gasification gas and to further understand the elementary steps of naphthalene transformation, we investigated the temperature dependent naphthalene adsorption, dehydrogenation and passivation on Ni(111). TPD (temperature-programmed desorption) and STM (scanning tunneling microscopy) in ultrahigh vacuum environment from 110 K up to 780 K, combined with DFT (density functional theory) were used in the study. Room temperature adsorption results in a flat naphthalene monolayer. DFT favors the dibridge[7] geometry but the potential energy surface is rather smooth and other adsorption geometries may coexist. DFT also reveals a pronounced dearomatization and charge transfer from the adsorbed molecule into the nickel surface. Dehydrogenation occurs in two steps, with two desorption peaks at approximately 450 and 600 K. The first step is due to partial dehydrogenation generating active hydrocarbon species that at higher temperatures migrates over the surface forming graphene. The graphene formation is accompanied by desorption of hydrogen in the high temperature TPD peak. The formation of graphene effectively passivates the surface both for hydrogen adsorption and naphthalene dissociation. In conclusion, the obtained results on the model naphthalene and Ni(111) system, provides insight into elementary steps of naphthalene adsorption, dehydrogenation, and carbon passivation, which may serve as a good starting point for rational design, development and optimization of the Ni catalyst surface, as well as process conditions, for the aromatic hydrocarbon reforming process.

Place, publisher, year, edition, pages
American Chemical Society , 2017. Vol. 121, no 40, p. 22199-22207
Keywords [en]
Adsorption, Aromatic hydrocarbons, Catalytic reforming, Charge transfer, Dehydrogenation, Density functional theory, Design for testability, Desorption, Gas adsorption, Gasification, Graphene, Hydrocarbons, Nickel, Passivation, Potential energy, Quantum chemistry, Scanning tunneling microscopy, Steam reforming, Temperature programmed desorption, Adsorption geometries, Attractive solutions, Catalytic steam reforming, Desorption of hydrogen, Hydrocarbon reforming, Naphthalene adsorption, Naphthalene transformation, Temperature dependent, Naphthalene
National Category
Chemical Process Engineering
Identifiers
URN: urn:nbn:se:kth:diva-227088DOI: 10.1021/acs.jpcc.7b07757Scopus ID: 2-s2.0-85031329487OAI: oai:DiVA.org:kth-227088DiVA, id: diva2:1206014
Funder
Swedish Research CouncilSwedish Energy Agency
Note

QC 20180515

Available from: 2018-05-15 Created: 2018-05-15 Last updated: 2018-05-15Bibliographically approved

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Moud, Pouya H.Engvall, Klas

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