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Structural elucidation of supported Rh complexes derived from RhCl(PPh3)3 immobilized on surface-functionalized SBA-15 and their catalytic performance for C-heteroatom (S, O) bond formation
- Source :
- Journal of Catalysis. 365:43-54
- Publication Year :
- 2018
- Publisher :
- Elsevier BV, 2018.
-
Abstract
- The local structures of rhodium complexes derived from the immobilization of Wilkinson’s complex, RhCl(PPh3)3, on SBA-15 silica functionalized with primary–amine, secondary–amine, or diphenylphosphine groups within the mesoporous channels were characterized by a series of techniques including XRD, HR-TEM, multinuclear (13C/29Si/31P) solid-state NMR, 2D 31P{1H} HETCOR NMR, XPS, and Rh K-edge EXAFS. Immobilization of RhCl(PPh3)3 through covalent bond formation with different functional groups grafted to the silica surface lead to variations in the local structure of the Rh center that has important implications for catalysis. The immobilized Rh complexes demonstrated high activity for the addition of alkynes with thiols (hydrothiolation) or sulfonic acids (hydrosulfonation) with excellent regio- and stereoselectivity under mild reaction conditions. This work demonstrates the elucidation of the local structure of the immobilized Rh complexes requires a complimentary multi-technique characterization approach that probes both the metal center itself and surrounding ligands.
- Subjects :
- Diphenylphosphine
Extended X-ray absorption fine structure
010405 organic chemistry
Chemistry
Heteroatom
chemistry.chemical_element
010402 general chemistry
01 natural sciences
Catalysis
0104 chemical sciences
Rhodium
Metal
chemistry.chemical_compound
Covalent bond
visual_art
Polymer chemistry
visual_art.visual_art_medium
Physical and Theoretical Chemistry
Mesoporous material
Subjects
Details
- ISSN :
- 00219517
- Volume :
- 365
- Database :
- OpenAIRE
- Journal :
- Journal of Catalysis
- Accession number :
- edsair.doi...........f9867aaec97f8c82e8f241a703e961ba