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Immobilization and Characterization of RuCl₂(PPh₃)₃ Mesoporous Silica SBA-3

Grünberg, Anna ; Gutmann, Torsten ; Rothermel, Niels ; Yeping, Xu ; Breitzke, Hergen ; Buntkowsky, Gerd (2021)
Immobilization and Characterization of RuCl₂(PPh₃)₃ Mesoporous Silica SBA-3.
In: Zeitschrift für Physikalische Chemie, 227 (6-7)
doi: 10.26083/tuprints-00019685
Article, Secondary publication, Publisher's Version

Abstract

The five-fold coordinated ruthenium (II) catalyst RuCl₂(PPh₃)₃ is heterogenized on the surface of amine functionalized mesoporous silica material SBA-3 and studied by BET, XRD and ³¹P CP-MAS solid-state NMR. The spectra indicate the replacement of one or two of the triphenyl-phosphine groups in the course of the grafting. To distinguish between both possibilities two-dimensional J-resolved ³¹P MAS solid-state NMR combined with quantum chemical calculations is employed. The changes of the scalar coupling pattern between the neat catalyst and the immobilized catalyst suggest the replacement of two of the PPh₃-groups by coordinative bonds to the amine-functions of the linker. DFT calculations reveal the absence of two chemically and magnetically equivalent phosphines and confirm the replacement of two PPh₃-groups. This finding is similar to the results observed for the binding of the rhodium in the Wilkinson’s catalyst, despite the different coordination of the metals (four-fold versus five-fold), the presence of two chlorine ligands and the different transition metal.

Item Type: Article
Erschienen: 2021
Creators: Grünberg, Anna ; Gutmann, Torsten ; Rothermel, Niels ; Yeping, Xu ; Breitzke, Hergen ; Buntkowsky, Gerd
Type of entry: Secondary publication
Title: Immobilization and Characterization of RuCl₂(PPh₃)₃ Mesoporous Silica SBA-3
Language: English
Date: 2021
Publisher: De Gruyter
Journal or Publication Title: Zeitschrift für Physikalische Chemie
Volume of the journal: 227
Issue Number: 6-7
DOI: 10.26083/tuprints-00019685
URL / URN: https://tuprints.ulb.tu-darmstadt.de/19685
Corresponding Links:
Origin: Secondary publication service
Abstract:

The five-fold coordinated ruthenium (II) catalyst RuCl₂(PPh₃)₃ is heterogenized on the surface of amine functionalized mesoporous silica material SBA-3 and studied by BET, XRD and ³¹P CP-MAS solid-state NMR. The spectra indicate the replacement of one or two of the triphenyl-phosphine groups in the course of the grafting. To distinguish between both possibilities two-dimensional J-resolved ³¹P MAS solid-state NMR combined with quantum chemical calculations is employed. The changes of the scalar coupling pattern between the neat catalyst and the immobilized catalyst suggest the replacement of two of the PPh₃-groups by coordinative bonds to the amine-functions of the linker. DFT calculations reveal the absence of two chemically and magnetically equivalent phosphines and confirm the replacement of two PPh₃-groups. This finding is similar to the results observed for the binding of the rhodium in the Wilkinson’s catalyst, despite the different coordination of the metals (four-fold versus five-fold), the presence of two chlorine ligands and the different transition metal.

Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-196853
Additional Information:

Keywords: RuCl₂(PPh₃)₃ / Heterogeneous Catalysis / Solid-State-NMR / MAS / Scalar Interactions / Quantum-chemical Calculations

Classification DDC: 500 Science and mathematics > 540 Chemistry
Divisions: 07 Department of Chemistry
07 Department of Chemistry > Eduard Zintl-Institut > Physical Chemistry
Date Deposited: 01 Oct 2021 11:26
Last Modified: 04 Oct 2021 05:57
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