Dicyclohexylmethane as a Liquid Organic Hydrogen Carrier: A Model Study on the Dehydrogenation Mechanism over Pd(111)

Beitrag in einer Fachzeitschrift
(Originalarbeit)


Details zur Publikation

Autor(en): Amende M, Gleichweit C, Xu T, Höfert O, Koch M, Wasserscheid P, Steinrück HP, Papp C, Libuda J
Zeitschrift: Catalysis Letters
Jahr der Veröffentlichung: 2016
Seitenbereich: 1-10
ISSN: 1572-879X


Abstract


Abstract: We have studied the dehydrogenation of the liquid organic hydrogen carrier (LOHC) dicyclohexylmethane (DCHM) to diphenylmethane (DPM) and its side reactions on a Pd(111) single crystal surface. The adsorption and thermal evolution of both DPM and DCHM was measured in situ in ultrahigh vacuum (UHV) using synchrotron radiation-based high-resolution X-ray photoelectron spectroscopy (HR-XPS). We found that after deposition at 170 K, the hydrogen-lean DPM undergoes C-H bond scission at the methylene bridge at 200 K and, starting at 360 K, complete dehydrogenation of the phenyl rings occurs. Above 600 K, atomic carbon incorporates into the Pd bulk. For the hydrogen-rich DCHM, the first stable dehydrogenation intermediate, a double π-allylic species, forms already at 190 K. Until 340 K, further dehydrogenation of the phenyl rings and of the methylene bridge occurs, yielding the same intermediate that is formed upon heating of DPM to this temperature, that is, DPM dehydrogenated at the methylene bridge. The onset for the complete dehydrogenation of this intermediate occurs at a much higher temperature than after adsorption of DPM. This behavior is mainly attributed to coadsorbed hydrogen from DCHM dehydrogenation. The results are discussed in comparison to our previous study of DPM and DCHM on Pt(111) revealing strong material dependencies. Graphical Abstract: [Figure not available: see fulltext.]



FAU-Autoren / FAU-Herausgeber

Amende, Maximilian
Lehrstuhl für Physikalische Chemie II
Gleichweit, Christoph
Lehrstuhl für Physikalische Chemie II
Höfert, Oliver
Lehrstuhl für Physikalische Chemie II
Koch, Marcus
Lehrstuhl für Chemische Reaktionstechnik
Libuda, Jörg Prof. Dr.
Professur für Physikalische Chemie
Papp, Christian PD Dr.
Lehrstuhl für Physikalische Chemie II
Steinrück, Hans-Peter Prof. Dr.
Lehrstuhl für Physikalische Chemie II
Wasserscheid, Peter Prof. Dr.
Lehrstuhl für Chemische Reaktionstechnik
Xu, Tao
Professur für Physikalische Chemie


Zusätzliche Organisationseinheit(en)
Exzellenz-Cluster Engineering of Advanced Materials


Zitierweisen

APA:
Amende, M., Gleichweit, C., Xu, T., Höfert, O., Koch, M., Wasserscheid, P.,... Libuda, J. (2016). Dicyclohexylmethane as a Liquid Organic Hydrogen Carrier: A Model Study on the Dehydrogenation Mechanism over Pd(111). Catalysis Letters, 1-10. https://dx.doi.org/10.1007/s10562-016-1711-z

MLA:
Amende, Maximilian, et al. "Dicyclohexylmethane as a Liquid Organic Hydrogen Carrier: A Model Study on the Dehydrogenation Mechanism over Pd(111)." Catalysis Letters (2016): 1-10.

BibTeX: 

Zuletzt aktualisiert 2018-12-12 um 13:50