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From Molecular Complexes to Complex Metallic Nanostructures-H-2 Solid-State NMR Studies of Ruthenium-Containing Hydrogenation Catalysts

Gutmann, T. and del Rosal, I. and Chaudret, B. and Poteau, R. and Limbach, H. H. and Buntkowsky, G. (2013):
From Molecular Complexes to Complex Metallic Nanostructures-H-2 Solid-State NMR Studies of Ruthenium-Containing Hydrogenation Catalysts.
In: Chemphyschem, pp. 3026-3033, 14, (13), [Online-Edition: http://apps.webofknowledge.com/full_record.do?product=WOS&se...],
[Article]

Abstract

In the last years, the combination of H-2 solid-state NMR techniques with quantum-chemical calculations has evolved into a powerful spectroscopic tool for the characterization of the state of hydrogen on the surfaces of heterogeneous catalysts. In the present minireview, a brief summary of this development is given, in which investigations of the structure and dynamics of hydrogen in molecular complexes, clusters and nanoparticle systems are presented, aimed to understand the reaction mechanisms on the surface of hydrogenation catalysts. The surface state of deuterium/hydrogen is analyzed employing a combination of variable-temperature H-2 static and magic-angle spinning (MAS) solid-state NMR techniques, in which the dominant quadrupolar interactions of deuterium give information on the binding situation and local symmetry of deuterium/hydrogen on molecular species. Using a correlation database from molecular complexes and clusters, the possibility to distinguish between terminal RuD, bridged Ru2D, three-fold Ru3D, and interstitial Ru6D is demonstrated. Combining these results with quantum-chemical density functional theory (DFT) calculations allows the interpretation of H-2 solid-state data of complex real world nanostructures, which yielded new insights into reaction pathways at the molecular level.

Item Type: Article
Erschienen: 2013
Creators: Gutmann, T. and del Rosal, I. and Chaudret, B. and Poteau, R. and Limbach, H. H. and Buntkowsky, G.
Title: From Molecular Complexes to Complex Metallic Nanostructures-H-2 Solid-State NMR Studies of Ruthenium-Containing Hydrogenation Catalysts
Language: English
Abstract:

In the last years, the combination of H-2 solid-state NMR techniques with quantum-chemical calculations has evolved into a powerful spectroscopic tool for the characterization of the state of hydrogen on the surfaces of heterogeneous catalysts. In the present minireview, a brief summary of this development is given, in which investigations of the structure and dynamics of hydrogen in molecular complexes, clusters and nanoparticle systems are presented, aimed to understand the reaction mechanisms on the surface of hydrogenation catalysts. The surface state of deuterium/hydrogen is analyzed employing a combination of variable-temperature H-2 static and magic-angle spinning (MAS) solid-state NMR techniques, in which the dominant quadrupolar interactions of deuterium give information on the binding situation and local symmetry of deuterium/hydrogen on molecular species. Using a correlation database from molecular complexes and clusters, the possibility to distinguish between terminal RuD, bridged Ru2D, three-fold Ru3D, and interstitial Ru6D is demonstrated. Combining these results with quantum-chemical density functional theory (DFT) calculations allows the interpretation of H-2 solid-state data of complex real world nanostructures, which yielded new insights into reaction pathways at the molecular level.

Journal or Publication Title: Chemphyschem
Volume: 14
Number: 13
Uncontrolled Keywords: solid-state nmr catalysis density functional theory nanoparticles transition metal complexes parahydrogen-induced polarization fischer-tropsch synthesis x-ray-structure dihydrogen complexes h-2 nmr surface reactivity immobilized catalysts quantum dynamics spin conversion mas nmr
Divisions: 07 Department of Chemistry
07 Department of Chemistry > Physical Chemistry
Date Deposited: 27 Oct 2014 20:40
Official URL: http://apps.webofknowledge.com/full_record.do?product=WOS&se...
Additional Information:

Sp. Iss. SI 216WE Times Cited:4 Cited References Count:111

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