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

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

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

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

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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: http://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.