In Situ Ternary Adduct Formation of Yttrium Polyaminocarboxylates Leads to Small Molecule Capture and Activation

In this work the chemistry of yttrium complexes is exploited for small molecule capture and activation. Nuclear magnetic resonance (NMR) and density functional theory (DFT) studies were used to investigate the in situ formation of solution state ternary yttrium-acetate, yttrium-bicarbonate, and yttrium-pyruvate adducts with a range of polyaminocarboxylate chelates. These studies reveal that [Y(DO3A)(H2O)(2)] (H(3)DO3A - 1,4,7,10-tetraazacyclododecane-1,4,7-tricarboxylic acid) and [Y(EDTA)(H2O)(q)](-) (H(4)EDTA - ethylenediaminetetraacetic acid, q = 2 and 3) are able to form ternary adducts with bicarbonate and pyruvate. In the latter, unusual decarboxylation of pyruvate to form acetic acid and CO2 was observed and further studied using SABRE-hyperpolarised C-13 NMR (SABRE - signal amplification by reversible exchange) to provide information about the reaction timescale and lifetime of intermediates involved in this conversion. The work presented demonstrates that yttrium complexes can capture and activate small molecules, which may lead to novel and useful applications of this metal in catalysis and medical imaging.

Automated summary

This work explores the capture and activation of small molecules using yttrium complexes. It investigates the in situ formation of ternary yttrium-acetate, yttrium-bicarbonate, and yttrium-pyruvate adducts with polyaminocarboxylate chelates using NMR and DFT. The study reveals the ability of yttrium complexes to form adducts with bicarbonate and pyruvate, and the unusual decarboxylation reaction of pyruvate to form acetic acid and CO2.