Size Dependent H2 Adsorption on AlnRh+ (n = 1–12) Clusters
| Autor: | Minh Tho Nguyen, Meiye Jia, Piero Ferrari, Wieland Schöllkopf, Sandy Gewinner, Eva M. Fernández, André Fielicke, Jan Vanbuel, Ewald Janssens |
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| Rok vydání: | 2018 |
| Předmět: |
Technology
Hydrogen Infrared Materials Science Infrared spectroscopy chemistry.chemical_element Materials Science Multidisciplinary 02 engineering and technology TRANSITION-METAL CLUSTERS 010402 general chemistry 01 natural sciences Dissociation (chemistry) Adsorption Infrared multiphoton dissociation Nanoscience & Nanotechnology MOLECULE Physical and Theoretical Chemistry COMPLEX HYDRIDES Spectroscopy ZETA VALENCE QUALITY BASIS-SETS Science & Technology Chemistry Physical Chemistry CHEMISORPTION DISSOCIATION ALUMINUM 021001 nanoscience & nanotechnology REACTIVITY 0104 chemical sciences Surfaces Coatings and Films Electronic Optical and Magnetic Materials General Energy Physical Sciences HYDROGEN-STORAGE MATERIALS Science & Technology - Other Topics Physical chemistry Density functional theory 0210 nano-technology |
| Zdroj: | The Journal of Physical Chemistry C. 122:18247-18255 |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/acs.jpcc.8b04332 |
| Popis: | © 2018 American Chemical Society. 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. ispartof: JOURNAL OF PHYSICAL CHEMISTRY C vol:122 issue:32 pages:18247-18255 status: published |
| Databáze: | OpenAIRE |
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