dc.contributor |
Háskóli Íslands |
dc.contributor |
University of Iceland |
dc.contributor.author |
Gutmann, Torsten |
dc.contributor.author |
Liu, Jiquan |
dc.contributor.author |
Rothermel, Niels |
dc.contributor.author |
Xu, Yeping |
dc.contributor.author |
Jaumann, Eva |
dc.contributor.author |
Werner, Mayke |
dc.contributor.author |
Breitzke, Hergen |
dc.contributor.author |
Sigurdsson, Snorri |
dc.contributor.author |
Buntkowsky, Gerd |
dc.date.accessioned |
2020-08-10T14:01:09Z |
dc.date.available |
2020-08-10T14:01:09Z |
dc.date.issued |
2015-01-23 |
dc.identifier.citation |
T. Gutmann; J. Liu; N. Rothermel; Y. Xu; E. Jaumann; M. Werner; H. Breitzke; S. Th. Sigurdsson; G. Buntkowsky, „Natural Abundance 15N NMR by Dynamic Nuclear Polarization: Fast Analysis of Binding Sites of a Novel Amine‐Carboxyl‐Linked Immobilized Dirhodium Catalyst,“ in Chemistry - A European Journal, vol.21, no.9, pp. 3798-3805 doi: 10.1002/chem.201405043 |
dc.identifier.issn |
0947-6539 |
dc.identifier.issn |
1521-3765 (eISSN) |
dc.identifier.uri |
https://hdl.handle.net/20.500.11815/1955 |
dc.description |
Post-print (lokagerð höfundar) |
dc.description.abstract |
A novel heterogeneous dirhodium catalyst has been synthesized. This stable catalyst is constructed from dirhodium acetate dimer (Rh2(OAc)4) units, which are covalently linked to amine‐ and carboxyl‐bifunctionalized mesoporous silica (SBA‐15NH2COOH). It shows good efficiency in catalyzing the cyclopropanation reaction of styrene and ethyl diazoacetate (EDA) forming cis‐ and trans‐1‐ethoxycarbonyl‐2‐phenylcyclopropane. To characterize the structure of this catalyst and to confirm the successful immobilization, heteronuclear solid‐state NMR experiments have been performed. The high application potential of dynamic nuclear polarization (DNP) NMR for the analysis of binding sites in this novel catalyst is demonstrated. Signal‐enhanced 13C CP MAS and 15N CP MAS techniques have been employed to detect different carboxyl and amine binding sites in natural abundance on a fast time scale. The interpretation of the experimental chemical shift values for different binding sites has been corroborated by quantum chemical calculations on dirhodium model complexes. |
dc.description.sponsorship |
This work has been supported by the Deutsche Forschungsgemeinschaft (DFG) under contract Bu-911-20-1, which gave us the opportunity to set up the DNP spectrometer, and Bu-911-12-2, and the Islandic Research Fund (141062-051). We further thank Bruker Biospin Germany and France for technical installation and support of the DNP spectrometer. Particular acknowledgement is given to the technicians N. Mathieu, F. Rohe, and F. Aussenac from Bruker France for their excellent technical support on the DNP. We thank Dr. R. Meusinger from the organic chemistry department (TU Darmstadt) for measuring the 2D liquid-state NMR spectra. |
dc.format.extent |
3798-3805 |
dc.language.iso |
en |
dc.publisher |
Wiley |
dc.relation.ispartofseries |
Chemistry - A European Journal;21(9) |
dc.rights |
info:eu-repo/semantics/openAccess |
dc.subject |
Dynamic nuclear polarization |
dc.subject |
Heterogeneous catalysis |
dc.subject |
Hyperpolarization |
dc.subject |
Immobilized catalyst |
dc.subject |
NMR spectroscopy |
dc.subject |
Litrófsgreining |
dc.subject |
Kjarnsýrur |
dc.title |
Natural Abundance 15N NMR by Dynamic Nuclear Polarization: Fast Analysis of Binding Sites of a Novel Amine-Carboxyl-Linked Immobilized Dirhodium Catalyst |
dc.type |
info:eu-repo/semantics/article |
dcterms.license |
This is the peer reviewed version of the following article: Chemistry - A European Journal, which has been published in final form at https://doi.org/10.1002/chem.201405043. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Use of Self-Archived Versions. |
dc.description.version |
Peer reviewed |
dc.identifier.journal |
Chemistry - A European Journal |
dc.identifier.doi |
10.1002/chem.201405043 |
dc.relation.url |
https://api.wiley.com/onlinelibrary/tdm/v1/articles/10.1002%2Fchem.201405043 |
dc.contributor.department |
Raunvísindadeild (HÍ) |
dc.contributor.department |
Faculty of Physical Sciences (UI) |
dc.contributor.school |
Verkfræði- og náttúruvísindasvið (HÍ) |
dc.contributor.school |
School of Engineering and Natural Sciences (UI) |