Please use this identifier to cite or link to this item:
Title: Cooperative interplay between a flexible PNN-Ru(II) complex and a NaBH4 additive in the efficient catalytic hydrogenation of esters
Authors: Wang, Zheng
Chen, Xiangyang
Liu, Bo
Liu, Qing-Bin
Solan, Gregory A.
Yang, Xinzheng
Sun, Wen-Hua
First Published: 2-Feb-2017
Publisher: Royal Society of Chemistry
Citation: Catalysis Science and Technology, 2017, 7, 1297-1304
Abstract: A catalyst loading of between 0.001–0.05 mol% of the PNN-bearing ruthenium(II) complex [fac-PNN]RuH(PPh3)(CO) (PNN = 8-(2-diphenylphosphinoethyl)amidotrihydroquinoline), in combination with 5 mol% NaBH4, efficiently catalyzes the hydrogenation of esters to their corresponding alcohols under mild pressures of hydrogen. Both aromatic and aliphatic esters can be converted with high values of TON or TOF achievable. Mechanistic investigations using both DFT calculations and labeling experiments highlight the cooperative role of NaBH4 in the catalysis while the catalytically active species has been established as trans-dihydride [mer-PNHN]RuH2(CO) (PNHN = 8-(2-diphenylphosphinoethyl)aminotrihydroquinoline). The stereo-structure of the PNHN-ruthenium species greatly affects the activity of the catalyst, and indeed the cis-dihydride isomer [fac-PNHN]RuH2(CO) is unable to catalyze the hydrogenation of esters until ligand reorganization occurs to give the trans isomer.
DOI Link: 10.1039/c6cy02413k
ISSN: 2044-4753
eISSN: 2044-4761
Version: Post-print
Status: Peer-reviewed
Type: Journal Article
Rights: Copyright © 2017, Royal Society of Chemistry. Deposited with reference to the publisher’s open access archiving policy.
Description: The file associated with this record is under embargo until 12 months after publication, in accordance with the publisher's self-archiving policy. The full text may be available through the publisher links provided above.
Appears in Collections:Published Articles, Dept. of Chemistry

Files in This Item:
File Description SizeFormat 
170119_GAS manuscript.pdfPost-review (final submitted author manuscript)337.09 kBAdobe PDFView/Open

Items in LRA are protected by copyright, with all rights reserved, unless otherwise indicated.