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Surprising Differences of Alkane C‐H Activation Catalyzed by Ruthenium Nanoparticles: Complex Surface‐Substrate Recognition?
Author(s) -
Rothermel Niels,
Bouzouita Donia,
Röther Tobias,
de Rosal Iker,
Tricard Simon,
Poteau Romuald,
Gutmann Torsten,
Chaudret Bruno,
Limbach HansHeinrich,
Buntkowsky Gerd
Publication year - 2018
Publication title -
chemcatchem
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 1.497
H-Index - 106
eISSN - 1867-3899
pISSN - 1867-3880
DOI - 10.1002/cctc.201801022
Subject(s) - cyclopentane , ruthenium , cyclohexane , catalysis , chemistry , butane , alkane , reactivity (psychology) , photochemistry , ligand (biochemistry) , substrate (aquarium) , nanoparticle , stereochemistry , organic chemistry , materials science , nanotechnology , medicine , biochemistry , alternative medicine , receptor , oceanography , pathology , geology
The activation of C−H bonds of alkanes remains a major challenge for chemistry. In a series of deuteration experiments with D 2 in contact with bis‐(diphenylphosphino) butane (dppb) stabilized ruthenium nanoparticles (liquid substrates, 60 °C, 6 bar D 2 ) we have observed a surprisingly large reactivity of cyclopentane as compared to cyclohexane and other alkanes. DFT calculations using a ligand‐free Ru 13 H 17 model cluster as catalyst indicate oxidative C−H cleavage of the bound substrates as rate limiting reaction step. They also indicate similar binding and activation enthalpies of reactions of cyclopentane and cyclohexane.