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­­Paramagnetic lanthanide NMR probes signalling changes in zinc concentration by emission and chemical shift : a proof of concept study.

Parker, David and Harnden, Alice C. and Batsanov, Andrei S. (2019) '­­Paramagnetic lanthanide NMR probes signalling changes in zinc concentration by emission and chemical shift : a proof of concept study.', Angewandte Chemie., 25 (24). pp. 6212-6225.

Abstract

A zinc‐selective probe, based on a set of rare earth complexes of a modified DO3A macrocyclic ligand incorporating a tris‐pyridylamine (TPA) moiety has been structurally characterised in solution and in the solid‐state. One pyridine group possesses a tert‐butyl substituent to serve as an NMR reporter group. The mono‐capped square‐antiprismatic Dy complex has a long bond (2.83Å) to an apical N atom (pKa 5.70 Eu) and binds to one water molecule on zinc binding. Zinc binding is reversible, and involves all of the exocyclic ligand N donors; it is signalled by large (ratiometric) changes in Eu emission intensity, and by dramatic changes in the size (>50 ppm) and sign of the chemical shift of the paramagnetically shifted tBu resonances in Tb, Dy and Tm complexes. Slow trans‐metallation was observed, leading to formation of an unusual di‐zinc species in which one zinc ion is 7‐coordinate and the other is six‐coordinate.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Status:Peer-reviewed
Publisher Web site:https://doi.org/10.1002/chem.201900609
Publisher statement:This is the accepted version of the following article: Parker, David, Harnden, Alice C. & Batsanov, Andrei S. (2019). ­­Paramagnetic Lanthanide NMR Probes Signalling Changes in Zinc Concentration by Emission and Chemical Shift: A Proof of Concept Study. Angewandte Chemie 25(24): 6212-6225 which has been published in final form at https://doi.org/10.1002/chem.201900609. This article may be used for non-commercial purposes in accordance With Wiley Terms and Conditions for self-archiving.
Date accepted:11 March 2019
Date deposited:27 March 2019
Date of first online publication:04 April 2019
Date first made open access:04 April 2020

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