English
 
Help Privacy Policy Disclaimer
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT

Released

Journal Article

Size Dependent H2 Adsorption on AlnRh+ (n = 1–12) Clusters

MPS-Authors
/persons/resource/persons21548

Gewinner,  Sandy
Molecular Physics, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons22079

Schöllkopf,  Wieland
Molecular Physics, Fritz Haber Institute, Max Planck Society;

/persons/resource/persons21506

Fielicke,  André
Molecular Physics, Fritz Haber Institute, Max Planck Society;

External Resource
No external resources are shared
Fulltext (restricted access)
There are currently no full texts shared for your IP range.
Fulltext (public)
There are no public fulltexts stored in PuRe
Supplementary Material (public)
There is no public supplementary material available
Citation

Jia, M., Vanbuel, J., Ferrari, P., Fernández, E. M., Gewinner, S., Schöllkopf, W., et al. (2018). Size Dependent H2 Adsorption on AlnRh+ (n = 1–12) Clusters. The Journal of Physical Chemistry C, 122(22), 18247-18255. doi:10.1021/acs.jpcc.8b04332.


Cite as: https://hdl.handle.net/21.11116/0000-0002-1871-4
Abstract
The interaction of hydrogen with singly rhodium doped aluminum clusters AlnRh+ (n = 1–12) is investigated experimentally by a combination of time-of-flight mass spectrometry and infrared multiple photon dissociation (IRMPD) spectroscopy. Density functional theory (DFT) is employed to optimize the geometric and electronic structures of bare and hydrogenated AlnRh+ clusters and the obtained infrared spectra of hydrogenated clusters are compared with the corresponding IRMPD spectra. The reactivity of the AlnRh+ clusters toward H2 is found to be strongly size-dependent, with n = 1–3, and 7 being the most reactive. Furthermore, it is favorable for H2 to adsorb molecularly on Al2Rh+ and Al3Rh+, while it prefers dissociative adsorption on other sizes. The initial molecular adsorption of H2 is identified as the determining step for hydrogen interaction with the AlnRh+ clusters, because the calculated molecular adsorption energies of H2 correlate well with the experimental abundances of the hydrogenated clusters. Natural charge populations and properties of the AlnRh+ clusters are analyzed to interpret the observed size-dependent reactivity.