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  4. Classical and non-classical phosphine-Ru(ii)-hydrides in aqueous solutions: many, various, and useful
 
research article

Classical and non-classical phosphine-Ru(ii)-hydrides in aqueous solutions: many, various, and useful

Papp, Gábor
•
Horváth, Henrietta
•
Laurenczy, Gábor  
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2013
Dalton Transactions

Hydrogenation of the water-soluble [{RuCl2(mtppms)(2)}(2)] (mtppms = monosulfonated triphenylphosphine) was studied in aqueous solutions in the presence of excess mtppms both with H-2 and with aqueous HCOONa. Depending on the reductant, the pH and H-2 pressure altogether nine hydride species were identified. In acidic solutions at 1 bar H-2 pressure the known [RuHCl(mtppms)(3)] (1) and [{RuHCl-(mtppms)(2)}(2)] (3) were formed, however, elevated pressure led to the formation of trans-[RuH2(mtppms)(4)] (11). In basic solutions at atmospheric pressure cis-fac-[RuH2(H2O)(mtppms)(3)] (12) was observed which was readily replaced by [RuH2(eta(2)-H-2)(mtppms)(3)] (13) at higher H-2 pressures. 13 is the first water-soluble and stable eta(2)-H-2 Ru(II)-complex stabilized only by monodentate phosphine ligands. [RuHBr(mtppms)(3)] (9) and [RuHI(mtppms)(3)] (10) were obtained analogously to 1. In concentrated aqueous HCOONa solutions (often used in H-transfer hydrogenations) the major species was trans-RuH2(HCOO)(mtppms) (14) while in dilute solutions trans-[RuH2(H2O)(mtppms)(3)] (15) could be observed. Formation of these various hydride species offers an explanation for the earlier observed pH and pressure dependence of the rates and selectivities in hydrogenation of unsaturated aldehydes catalyzed by [{RuCl2(mtppms)(2)}(2)] + mtppms.

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Type
research article
DOI
10.1039/c2dt31793a
Web of Science ID

WOS:000312219800028

Author(s)
Papp, Gábor
Horváth, Henrietta
Laurenczy, Gábor  
Szatmári, Imre
Kathó, Ágnes
Joó, Ferenc
Date Issued

2013

Publisher

Royal Soc Chemistry

Published in
Dalton Transactions
Volume

42

Issue

2

Start page

521

Editorial or Peer reviewed

NON-REVIEWED

Written at

OTHER

EPFL units
LCOM  
Available on Infoscience
December 7, 2012
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/87322
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