Iridium N-heterocyclic carbene complexes as efficient catalysts for magnetization transfer from para-hydrogen

M.J. Cowley, Ralph W. Adams, Kevin Atkinson, Martin Charles Roy Cockett, Simon Duckett, Gary George Reginald Green, J.A.B. Lohman, R Kerssebaum, D Kilgour, Ryan Edward Mewis

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While the characterization of materials by NMR is hugely important in the physical and biological sciences, it also plays a vital role in medical imaging. This success is all the more impressive because of the inherently low sensitivity of the method. We establish here that [Ir(H)(2)(IMes)(py)(3)]Cl undergoes both pyridine (py) loss as well as the reductive elimination of H(2). These reversible processes bring para-H(2) and py into contact in a magnetically coupled environment, delivering an 8100-fold increase in (1)H NMR signal strength relative to non-hyperpolarized py at 3 T. An apparatus that facilitates signal averaging has been built to demonstrate that the efficiency of this process is controlled by the strength of the magnetic field experienced by the complex during the magnetization transfer step. Thermodynamic and kinetic data combined with DFT calculations reveal the involvement of [Ir(H)(2)(eta(2)-H(2))(IMes)(py)(2)](+), an unlikely yet key intermediate in the reaction. Deuterium labeling yields an additional 60% improvement in signal, an observation that offers insight into strategies for optimizing this approach.
Original languageEnglish
Pages (from-to)6134-6137
Number of pages4
JournalJournal of the American Chemical Society
Issue number16
Early online date6 Apr 2011
Publication statusPublished - 27 Apr 2011
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    Simon B. Duckett (Invited speaker)

    1 Jul 2012

    Activity: Participating in or organising an eventConference participation

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