Journal Article

FZJ-2017-03011

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Dicyclohexylmethane as a Liquid Organic Hydrogen Carrier: A Model Study on the Dehydrogenation Mechanism over Pd(111)

Amende, M. ; Gleichweit, C. ; Xu, T. ; Höfert, O. ; Wasserscheid, P.FZJ* ; Steinrück, H.-P. ; Papp, C. (Corresponding author) ; Libuda, J. ; Koch, M.

2016
Springer Science + Business Media B.V Dordrecht [u.a.]

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Please use a persistent id in citations: doi:10.1007/s10562-016-1711-z

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.

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Contributing Institute(s):

1. Helmholtz-Institut Erlangen-Nürnberg Erneuerbare Energien (IEK-11)

Research Program(s):

1. 134 - Electrolysis and Hydrogen (POF3-134) (POF3-134)

Appears in the scientific report 2017

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Database coverage:
; Current Contents - Engineering, Computing and Technology ; Current Contents - Physical, Chemical and Earth Sciences ; Ebsco Academic Search ; IF < 5 ; JCR ; Nationallizenz ; No Authors Fulltext ; SCOPUS ; Science Citation Index ; Science Citation Index Expanded ; Thomson Reuters Master Journal List ; Web of Science Core Collection

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