期刊
CHEMISTRY-A EUROPEAN JOURNAL
卷 22, 期 9, 页码 2964-2971出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.201504403
关键词
astatine; competition experiments; hydrolysis constants; Pourbaix diagrams; quantum mechanical calculations
资金
- French National Agency for Research [ANR-2010-BLAN-0807]
- Investissements d'Avenir [ANR-11-EQPX-0004, ANR-11-LABX-0018]
- Region Pays de la Loire (NUCSAN project)
- GENCI-CINES/IDRIS grant [2015-c2015085117]
It is generally assumed that astatide (At-) is the predominant astatine species in basic aqueous media. This assumption is questioned in non-complexing and non-reductive aqueous solutions by means of high-pressure anion-exchange chromatography. Contrary to what is usually believed, astatide is found to be a minor species at pH=11. A different species, which also bears a single negative charge, becomes predominant when the pH is increased beyond 7. Using competition experiments, an equilibrium constant value of 10(-6.9) has been determined for the formation of this species from AtO(OH) with the exchange of one proton. The identification of this species, AtO(OH)(2)(-), is achieved through relativistic quantum mechanical calculations, which rule out the significant formation of the AtO2- species, while leading to a hydrolysis constant of AtO(OH) in excellent agreement with experiment when the AtO(OH)(2)(-) species is considered. Beyond the completion of the Pourbaix diagram of astatine, this new information is of interest for the development of At-211 radiolabeling protocols.
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