Abdulhussain, S. ; Breitzke, H. ; Ratajczyk, T. ; Grünberg, A. ; Srour, M. ; Arnaut, D. ; Weidler, H. ; Kunz, U. ; Kleebe, H.-J. ; Bommerich, U. ; Bernarding, J. ; Gutmann, T. ; Buntkowsky, G. (2014):
Synthesis, Solid-State NMR Characterization, and Application for Hydrogenation Reactions of a Novel Wilkinson's-Type Immobilized Catalyst.
In: Chemistry - A European Journal, 20 (4), pp. 1159-1166. Wiley, ISSN 0947-6539,
DOI: 10.1002/chem.201303020,
[Article]
Abstract
Silica nanoparticles (SiNPs) were chosen as a solid support material for the immobilization of a new Wilkinson's-type catalyst. In a first step, polymer molecules (poly(triphenylphosphine)ethylene (PTPPE); 4-diphenylphosphine styrene as monomer) were grafted onto the silica nanoparticles by surface-initiated photoinferter-mediated polymerization (SI-PIMP). The catalyst was then created by binding rhodium (Rh) to the polymer side chains, with RhCl(3)xH(2)O as a precursor. The triphenylphosphine units and rhodium as Rh-I provide an environment to form Wilkinson's catalyst-like structures. Employing multinuclear (P-31, Si-29, and C-13) solid-state NMR spectroscopy (SSNMR), the structure of the catalyst bound to the polymer and the intermediates of the grafting reaction have been characterized. Finally, first applications of this catalyst in hydrogenation reactions employing para-enriched hydrogen gas (PHIP experiments) and an assessment of its leaching properties are presented.
| Item Type: | Article |
|---|---|
| Erschienen: | 2014 |
| Creators: | Abdulhussain, S. ; Breitzke, H. ; Ratajczyk, T. ; Grünberg, A. ; Srour, M. ; Arnaut, D. ; Weidler, H. ; Kunz, U. ; Kleebe, H.-J. ; Bommerich, U. ; Bernarding, J. ; Gutmann, T. ; Buntkowsky, G. |
| Title: | Synthesis, Solid-State NMR Characterization, and Application for Hydrogenation Reactions of a Novel Wilkinson's-Type Immobilized Catalyst |
| Language: | English |
| Abstract: | Silica nanoparticles (SiNPs) were chosen as a solid support material for the immobilization of a new Wilkinson's-type catalyst. In a first step, polymer molecules (poly(triphenylphosphine)ethylene (PTPPE); 4-diphenylphosphine styrene as monomer) were grafted onto the silica nanoparticles by surface-initiated photoinferter-mediated polymerization (SI-PIMP). The catalyst was then created by binding rhodium (Rh) to the polymer side chains, with RhCl(3)xH(2)O as a precursor. The triphenylphosphine units and rhodium as Rh-I provide an environment to form Wilkinson's catalyst-like structures. Employing multinuclear (P-31, Si-29, and C-13) solid-state NMR spectroscopy (SSNMR), the structure of the catalyst bound to the polymer and the intermediates of the grafting reaction have been characterized. Finally, first applications of this catalyst in hydrogenation reactions employing para-enriched hydrogen gas (PHIP experiments) and an assessment of its leaching properties are presented. |
| Journal or Publication Title: | Chemistry - A European Journal |
| Volume of the journal: | 20 |
| Issue Number: | 4 |
| Publisher: | Wiley |
| Uncontrolled Keywords: | Heterogeneous catalysis para-hydrogen-induced polarization polymer support rhodium solid-state nmr parahydrogen-induced polarization transition-metal-complexes inorganic hybrid materials mesoporous silica heterogeneous hydrogenation recyclable catalyst enantioselective catalysts reusable catalysts spectroscopy nanoparticles |
| Divisions: | 07 Department of Chemistry 07 Department of Chemistry > Physical Chemistry |
| Date Deposited: | 27 Oct 2014 20:33 |
| DOI: | 10.1002/chem.201303020 |
| Additional Information: | 287NG Times Cited:2 Cited References Count:88 |
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