Issue 10, 2014

Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

Abstract

This perspective will examine the use of a wide range of techniques for differentiating homogeneous from nanoparticle asymmetric catalysis as it pertains to two highly active systems developed within our group. The 6,5,6 and 5,5,5-precatalysts, trans-[Fe(NCMe)CO(PPh2C6H4CH[double bond, length as m-dash]NCHPh–)2][BF4]2 and trans-[Fe(CO)Br(PR2CH2CH[double bond, length as m-dash]NCHPh–)2][BF4], respectively, are highly active and selective asymmetric transfer hydrogenation (ATH) catalysts. Here, we will review the series of tests that were undertaken to support the idea that the 6,5,6-precatalyst forms iron nanoparticles (Fe NPs) during catalysis, whereas the 5,5,5-system remains homogeneous. Techniques include the use of NMR and DFT to investigate intermediates and activation steps, reaction profile and induction period analysis, substoichiometric poisoning, electron microscopy imaging, dynamic light scattering (DLS), X-ray photoelectron microscopy (XPS), magnetometry, and multiphasic analysis. We also elaborate on the wider applicability of these and other tests to probe the true nature of an active catalyst, with emphasis on the importance of using a wide range of techniques for insightful mechanistic evaluations.

Graphical abstract: Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

Article information

Article type
Perspective
Submitted
11 四月 2014
Accepted
04 六月 2014
First published
05 六月 2014

Catal. Sci. Technol., 2014,4, 3426-3438

Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

J. F. Sonnenberg and R. H. Morris, Catal. Sci. Technol., 2014, 4, 3426 DOI: 10.1039/C4CY00468J

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