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Issue 10, 2014
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Distinguishing homogeneous from nanoparticle asymmetric iron catalysis

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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

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Publication details

The article was received on 11 Apr 2014, accepted on 04 Jun 2014 and first published on 05 Jun 2014


Article type: Perspective
DOI: 10.1039/C4CY00468J
Citation: Catal. Sci. Technol., 2014,4, 3426-3438

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    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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