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Abstract

Acceptorless dehydrogenation of ethane was achieved in the gas phase via a two-step catalytic cycle involving ternary cationic metal hydrides, [(phen)M(H)]+, 1, and metal ethides, [(phen)M(CH2CH3)]+, 2, (where M = Ni, Pd, or Pt, and phen = 1,10-phenanthroline). Species 1 and 2 were generated and their reactivity studied in a quadrupole ion trap mass spectrometer. It was found that 1 readily reacted with ethane releasing H2 and forming 2, with the relative reactivity being Pt > Ni ≫ Pd. Density functional theory (DFT) calculations for this metathesis reaction agree with the experimental reactivity order. Species 2 can in turn be converted into 1 and release ethylene when sufficient energy is supplied via collision-induced dissociation. DFT calculations also provided insight into competing side reactions (e.g., dehydrogenation of 2 and formation of protonated phen ligand) that become competitive during this endothermic step. The catalytic cycle can be repeated in the mass spectrometer several times. Multiple entry points into the cycle have been identified and discussed.

Item Type:	Article
Authors/Creators:	Parker, K and Weragoda, GK and Canty, AJ and Polyzos, A and Ryzhov, V and O'hair, RAJ
Keywords:	palladium, catalysis, mass spectrometry, computation, DFT, organometallic
Journal or Publication Title:	Organometallics
Publisher:	Amer Chemical Soc
ISSN:	0276-7333
DOI / ID Number:	https://doi.org/10.1021/acs.organomet.0c00598
Copyright Information:	Copyright 2020 American Chemical Society
Related URLs:	UTAS Profile: Canty, AJ
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