Article (Scientific journals)
Detection of Intermediates in Dual Gold Catalysis Using High-Resolution Ion Mobility Mass Spectrometry
Greisch, J.-F.; Weis, P.; Brendle, K. et al.
2018In Organometallics, 37 (9), p. 1493-1500
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Keywords :
Benzene; Benzene refining; Catalysis; Catalysts; Chemical activation; Electrospray ionization; Gold; Ion mobility spectrometers; Mass spectrometry; Model structures; Reaction intermediates; Collision cross sections; Cooperative interactions; Density functional computations; Direct observations; High resolution; Ion mobility-mass spectrometry; Reaction mixture; Structural isomers; Isomers
Abstract :
[en] We have probed for reaction intermediates involved in the dual-gold-catalyzed activation of a conjugated 1,5-diyne substrate and its further coupling to benzene in the liquid phase. This was done by sampling the reaction mixture by electrospray ionization followed by high-resolution ion mobility mass spectrometry - under conditions allowing for the resolution of structural isomers differing in their collision cross sections by less than 0.5%. For the cationic mass corresponding to catalyst + diyne (activation stage) we resolve four isomers. At the mass corresponding to catalyst + diyne + benzene, two isomers are observed. By comparing the experimentally obtained cross sections to those inferred for model structures derived from density functional computations, we find our measurements to be consistent with the proposed solution mechanism. This constitutes the first direct observation of intermediates in dual gold catalysis and supports the previous inference that the mechanism involves cooperative interactions between two gold centers. © 2018 American Chemical Society.
Disciplines :
Chemistry
Author, co-author :
Greisch, J.-F.;  Institute of Physical Chemistry, KIT, Karlsruhe, Germany, Institute of Nanotechnology, KIT, Eggenstein-Leopoldshafen, Germany
Weis, P.;  Institute of Physical Chemistry, KIT, Karlsruhe, Germany
Brendle, K.;  Institute of Physical Chemistry, KIT, Karlsruhe, Germany
Kappes, M. M.;  Institute of Physical Chemistry, KIT, Karlsruhe, Germany, Institute of Nanotechnology, KIT, Eggenstein-Leopoldshafen, Germany
Haler, Jean ;  Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de spectrométrie de masse (L.S.M.)
Far, Johann  ;  Université de Liège - ULiège > Département de chimie (sciences) > Center for Analytical Research and Technology (CART)
De Pauw, Edwin  ;  Université de Liège - ULiège > Département de chimie (sciences) > Laboratoire de spectrométrie de masse (L.S.M.)
Albers, C.;  Bruker Daltonic GmbH, Bremen, Germany
Bay, S.;  Organic Chemistry Institute, Heidelberg University, Heidelberg, Germany
Wurm, T.;  Organic Chemistry Institute, Heidelberg University, Heidelberg, Germany
Rudolph, M.;  Organic Chemistry Institute, Heidelberg University, Heidelberg, Germany
Schulmeister, J.;  Organic Chemistry Institute, Heidelberg University, Heidelberg, Germany
Hashmi, A. S. K.;  Organic Chemistry Institute, Heidelberg University, Heidelberg, Germany
More authors (3 more) Less
Language :
English
Title :
Detection of Intermediates in Dual Gold Catalysis Using High-Resolution Ion Mobility Mass Spectrometry
Publication date :
2018
Journal title :
Organometallics
ISSN :
0276-7333
eISSN :
1520-6041
Publisher :
American Chemical Society
Volume :
37
Issue :
9
Pages :
1493-1500
Peer reviewed :
Peer Reviewed verified by ORBi
Funders :
Hector Fellow Academy
Hector Stiftung II
DFG - Deutsche Forschungsgemeinschaft [DE]
F.R.S.-FNRS - Fonds de la Recherche Scientifique [BE]
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