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Study of catalytic sites on ruthenium for hydrogenation of N-ethylcarbazole: Implications of hydrogen storage via reversible catalytic hydrogenation
Morawa Eblagon K.5; Tam K.3; Yu K.M.K.5; Zhao S.-L.4; Gong X.-Q.4; He H.2; Ye L.2; Wang L.-C.2; Ramirez-Cuesta A.J.1; Tsang S.C.5
2010-06-03
Source PublicationJournal of Physical Chemistry C
ISSN19327447 19327455
Volume114Issue:21Pages:9720-9730
Abstract

Hydrogen storage is a significant challenge for the development and viability of hydrogen-powered vehicles. Storage of molecular hydrogen in nitrogen-substituted polyunsaturated aromatic organic molecules through reversible catalytic hydrogenation and dehydrogenation is a promising approach. The success of developing a catalytic hydrogen storage concept is highly dependent on finding an efficient catalyst; however, understanding how molecules interact with metal catalytic sites is, at present, rather limited. In this work, a combined experimental and theoretical study is conducted to identify efficient catalytic sites on metallic surfaces and to understand the reaction mechanism for the forward hydrogenation reaction. It is clearly revealed from experimentation that hydrogenation of N-ethylcarbazole, a typical nitrogen-substituted polyunsaturated aromatic organic molecule, is taking place in a stepwise manner over metal catalysts. Because of steric constraints at terrace sites, the kinetically stable pyrrole intermediate, formed by partial hydrogenation of N-ethylcarbazole, cannot be readsorbed once desorbed into solution. Therefore further hydrogenation occurs at the low coordinated sites where no similar steric hindrance is encountered. Thus, the mechanism for hydrogenation involves an unusual shuttling of partially hydrogenated intermediates from terrace sites to higher indexed sites via solution. First-principles calculations confirm that the pyrrole intermediate can strongly adsorb to various low coordination sites, typically steps on the vicinal (109) surface, while the adsorption is extremely weak on flat (001) terraces. This work is the first example of catalytic site analysis to account for observed activity, selectivity and recyclability of a typical metal catalyst for catalytic hydrogen storage, which could lead to rational design of superior materials. © 2010 American Chemical Society.

DOI10.1021/jp908640k
URLView the original
Indexed BySCI
Language英语
WOS Research AreaChemistry ; Science & Technology - Other Topics ; Materials Science
WOS SubjectChemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary
WOS IDWOS:000278003700027
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Cited Times [WOS]:52   [WOS Record]     [Related Records in WOS]
Document TypeJournal article
CollectionFaculty of Health Sciences
Affiliation1.TOSCA
2.Fudan University
3.AstraZeneca
4.East China University of Science and Technology
5.University of Oxford
Recommended Citation
GB/T 7714
Morawa Eblagon K.,Tam K.,Yu K.M.K.,et al. Study of catalytic sites on ruthenium for hydrogenation of N-ethylcarbazole: Implications of hydrogen storage via reversible catalytic hydrogenation[J]. Journal of Physical Chemistry C,2010,114(21):9720-9730.
APA Morawa Eblagon K..,Tam K..,Yu K.M.K..,Zhao S.-L..,Gong X.-Q..,...&Tsang S.C..(2010).Study of catalytic sites on ruthenium for hydrogenation of N-ethylcarbazole: Implications of hydrogen storage via reversible catalytic hydrogenation.Journal of Physical Chemistry C,114(21),9720-9730.
MLA Morawa Eblagon K.,et al."Study of catalytic sites on ruthenium for hydrogenation of N-ethylcarbazole: Implications of hydrogen storage via reversible catalytic hydrogenation".Journal of Physical Chemistry C 114.21(2010):9720-9730.
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