A General Design Strategy Enabling the Synthesis of Hydrolysis-Resistant, Water-Stable Titanium(IV) Complexes.

Autor: Koller AJ; Department of Chemistry, Stony Brook University, Stony Brook, NY 11794, USA., Saini S; Department of Radiology, University of Alabama at Birmingham, Birmingham, AL 25294, USA., Chaple IF; Department of Radiology, University of Alabama at Birmingham, Birmingham, AL 25294, USA., Joaqui-Joaqui MA; Department of Chemistry, University of Minnesota, Minneapolis, MN 55455, USA., Paterson BM; School of Biomedical Engineering and Imaging Sciences, King's College London, St. Thomas Hospital, London, SE1 7EH, UK., Ma MT; School of Biomedical Engineering and Imaging Sciences, King's College London, St. Thomas Hospital, London, SE1 7EH, UK., Blower PJ; School of Biomedical Engineering and Imaging Sciences, King's College London, St. Thomas Hospital, London, SE1 7EH, UK., Pierre VC; Department of Chemistry, University of Minnesota, Minneapolis, MN 55455, USA., Robinson JR; Department of Chemistry, Brown University, Providence, RI 02912, USA., Lapi SE; Department of Radiology, University of Alabama at Birmingham, Birmingham, AL 25294, USA., Boros E; Department of Chemistry, Stony Brook University, Stony Brook, NY 11794, USA.
Jazyk: angličtina
Zdroj: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2022 May 23; Vol. 61 (22), pp. e202201211. Date of Electronic Publication: 2022 Mar 29.
DOI: 10.1002/anie.202201211
Abstrakt: Despite its prevalence in the environment, the chemistry of the Ti 4+ ion has long been relegated to organic solutions or hydrolyzed TiO 2 polymorphs. A knowledge gap in stabilizing molecular Ti 4+ species in aqueous environments has prevented the use of this ion for various applications such as radioimaging, design of water-compatible metal-organic frameworks (MOFs), and aqueous-phase catalysis applications. Herein, we show a thorough thermodynamic screening of bidentate chelators with Ti 4+ in aqueous solution, as well as computational and structural analyses of key compounds. In addition, the hexadentate analogues of catechol (benzene-1,2-diol) and deferiprone (3-hydroxy-1,2-dimethyl-4(1H)-pyridone), TREN-CAM and THP Me respectively, were assessed for chelation of the 45 Ti isotope (t 1/2 =3.08 h, β + =85 %, E β+ =439 keV) towards positron emission tomography (PET) imaging applications. Both were found to have excellent capacity for kit-formulation, and [ 45 Ti]Ti-TREN-CAM was found to have remarkable stability in vivo.
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Databáze: MEDLINE