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

TY - JOUR

T1 - In Situ Ternary Adduct Formation of Yttrium Polyaminocarboxylates Leads to Small Molecule Capture and Activation

AU - Duckett, Simon B.

AU - Tickner, Benjamin

AU - Angelovski, Goran

AU - Platas-Iglesias, Carlos

PY - 2022/10/13

Y1 - 2022/10/13

N2 - 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] (H3DO3A – 1,4,7,10-tetraazacyclododecane-1,4,7-tricarboxylic acid) and [Y(EDTA)(H2O)2] (H4EDTA – ethylenediaminetetraacetic acid) 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 13C 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.

AB - 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] (H3DO3A – 1,4,7,10-tetraazacyclododecane-1,4,7-tricarboxylic acid) and [Y(EDTA)(H2O)2] (H4EDTA – ethylenediaminetetraacetic acid) 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 13C 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.

U2 - 10.1002/chem.202201780

DO - 10.1002/chem.202201780

M3 - Article

SN - 0947-6539

VL - 28

JO - Chemistry : A European Journal

JF - Chemistry : A European Journal

IS - 57

M1 - e202201780

ER -