Liu, Jiquan ; Fasel, Claudia ; Braga-Groszewicz, Pedro ; Rothermel, Niels ; Thankamony, Aany Sofia Lilly ; Sauer, Grit ; Xu, Yeping ; Gutmann, Torsten ; Buntkowsky, Gerd (2016)
Heterogeneous self-supported dirhodium(ii) catalysts with high catalytic efficiency in cyclopropanation – a structural study.
In: Catal. Sci. Technol., 6 (21)
doi: 10.1039/C6CY00915H
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
Catalytically active dirhodium sheet-like coordination polymers are synthesized from their precursors via ligand exchange. The individual lamellae of the dirhodium-bdc frameworks are stacked as parallel sheets, which are randomly oriented or slightly ordered. As inorganic building blocks Rh2(TFA)4 and Rh2(OAc)4, and as organic linker benzene 1,4-dicarboxylate (bdc) are employed. The successful synthesis of the Rh2-bdc(Tf) and Rh2-bdc(Ac) catalysts is proven by ATR-IR, XPS and 13C CP MAS NMR. Residual trifluoroacetate species are investigated by quantitative 19F MAS NMR which further reflects the configuration of trifluoroacetate in the obtained Rh2-bdc(Tf), and defects in the structure. DR-UV-vis and XPS demonstrate that the oxidation state and the Rh–Rh single bond in the dirhodium node are maintained during the ligand substitution process. The stability and reusability of the catalysts are verified by TG-DTA measurements and leaching tests. The catalysts show similar catalytic efficiency as the homogeneous catalyst in the model cyclopropanation between ethyl diazoacetate (EDA) and styrene.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2016 |
| Autor(en): | Liu, Jiquan ; Fasel, Claudia ; Braga-Groszewicz, Pedro ; Rothermel, Niels ; Thankamony, Aany Sofia Lilly ; Sauer, Grit ; Xu, Yeping ; Gutmann, Torsten ; Buntkowsky, Gerd |
| Art des Eintrags: | Bibliographie |
| Titel: | Heterogeneous self-supported dirhodium(ii) catalysts with high catalytic efficiency in cyclopropanation – a structural study |
| Sprache: | Englisch |
| Publikationsjahr: | 21 September 2016 |
| Verlag: | Royal Society of Chemistry |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Catal. Sci. Technol. |
| Jahrgang/Volume einer Zeitschrift: | 6 |
| (Heft-)Nummer: | 21 |
| DOI: | 10.1039/C6CY00915H |
| Kurzbeschreibung (Abstract): | Catalytically active dirhodium sheet-like coordination polymers are synthesized from their precursors via ligand exchange. The individual lamellae of the dirhodium-bdc frameworks are stacked as parallel sheets, which are randomly oriented or slightly ordered. As inorganic building blocks Rh2(TFA)4 and Rh2(OAc)4, and as organic linker benzene 1,4-dicarboxylate (bdc) are employed. The successful synthesis of the Rh2-bdc(Tf) and Rh2-bdc(Ac) catalysts is proven by ATR-IR, XPS and 13C CP MAS NMR. Residual trifluoroacetate species are investigated by quantitative 19F MAS NMR which further reflects the configuration of trifluoroacetate in the obtained Rh2-bdc(Tf), and defects in the structure. DR-UV-vis and XPS demonstrate that the oxidation state and the Rh–Rh single bond in the dirhodium node are maintained during the ligand substitution process. The stability and reusability of the catalysts are verified by TG-DTA measurements and leaching tests. The catalysts show similar catalytic efficiency as the homogeneous catalyst in the model cyclopropanation between ethyl diazoacetate (EDA) and styrene. |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Disperse Feststoffe 07 Fachbereich Chemie |
| Hinterlegungsdatum: | 25 Okt 2016 12:28 |
| Letzte Änderung: | 02 Aug 2021 09:57 |
| PPN: | |
| Sponsoren: | Financial support by the Deutsche Forschungsgemeinschaft DFG under contract Bu 911-22-1, and by the Hessen State Ministry of Higher Education, Research and the Arts in the frame of the LOEWE project iNAPO is gratefully acknowledged |
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