Journal
INORGANIC CHEMISTRY
Volume 59, Issue 19, Pages 13923-13932Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.inorgchem.0c01553
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- French National Agency for Research with Investissements d'Avenir [ANR-11-EQPX-0004, ANR-11-LABX-0018]
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The affinity of AtO+ for around 20 model ligands (L), carrying functionalized oxygen, sulfur, and nitrogen atoms, has been assessed through a combined experimental and theoretical methodology. Significant equilibrium constants (K-L similar to 10(4)) have been measured for sulfur-containing compounds, in agreement with the previously highlighted, relatively stable radiolabeling of SH-containing proteins with At-211. Conversely, no interaction occurs in the aqueous phase for their oxygenated counterparts, but higher affinities (K-L > 10(6)) have been determined for nitrogen-based ligands, including aromatic nitrogen heterocycles. The quantum mechanical calculations definitively ruled out any rationale based on either the metallic character of astatine or its guessed softness; the favored interactions all involve specifically the oxygen atom of AtO+, leading to the formation of covalent O-S or O-C single bonds.
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