دورية أكاديمية
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Exploiting the Fluxionality of Lanthanide Complexes in the Design of Paramagnetic Fluorine Probes.

التفاصيل البيبلوغرافية
العنوان: Exploiting the Fluxionality of Lanthanide Complexes in the Design of Paramagnetic Fluorine Probes.
المؤلفون: Wilharm RK; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Ramakrishnam Raju MV; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Hoefler JC; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States., Platas-Iglesias C; Centro de Investigacións Científicas Avanzadas and Departamento de Quıímica, Facultade de Ciencias, Universidade da Coruña, 15071 A Coruña, Galicia Spain., Pierre VC; Department of Chemistry, University of Minnesota, Minneapolis, Minnesota 55455, United States.
المصدر: Inorganic chemistry [Inorg Chem] 2022 Mar 07; Vol. 61 (9), pp. 4130-4142. Date of Electronic Publication: 2022 Feb 23.
نوع المنشور: Journal Article
اللغة: English
بيانات الدورية: Publisher: American Chemical Society Country of Publication: United States NLM ID: 0366543 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1520-510X (Electronic) Linking ISSN: 00201669 NLM ISO Abbreviation: Inorg Chem Subsets: PubMed not MEDLINE; MEDLINE
أسماء مطبوعة: Original Publication: [Easton, Pa.] American Chemical Society.
مستخلص: Fluorine-19 MRI is increasingly being considered as a tool for biomolecular imaging, but the very poor sensitivity of this technique has limited most applications. Previous studies have long established that increasing the sensitivity of 19 F molecular probes requires increasing the number of fluorine nuclei per probe as well as decreasing their longitudinal relaxation time. The latter is easily achieved by positioning the fluorine atoms in close proximity to a paramagnetic metal ion such as a lanthanide(III). Increasing the number of fluorine atoms per molecule, however, is only useful inasmuch as all of the fluorine nuclei are chemically equivalent. Previous attempts to achieve this equivalency have focused on designing highly symmetric and rigid fluorinated macrocyclic ligands. A much simpler approach consists of exploiting highly fluxional lanthanide complexes with open coordination sites that have a high affinity for phosphated and phosphonated species. Computational studies indicate that Ln III -TREN-MAM is highly fluxional, rapidly interconverting between at least six distinct isomers. In neutral water at room temperature, Ln III -TREN-MAM binds two or three equivalents of fluorinated phosphonates. The close proximity of the 19 F nuclei to the Ln III center in the ternary complex decreases the relaxation times of the fluorine nuclei up to 40-fold. Advantageously, the fluorophosphonate-bound lanthanide complex is also highly fluxional such that all 19 F nuclei are chemically equivalent and display a single 19 F signal with a small LIS. Dynamic averaging of fluxional fluorinated supramolecular assemblies thus produces effective 19 F MR systems.
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معلومات مُعتمدة: R01 DK124333 United States DK NIDDK NIH HHS
تواريخ الأحداث: Date Created: 20220223 Date Completed: 20220308 Latest Revision: 20230308
رمز التحديث: 20230308
مُعرف محوري في PubMed: PMC8966431
DOI: 10.1021/acs.inorgchem.1c03908
PMID: 35196450
قاعدة البيانات: MEDLINE
الوصف
تدمد:1520-510X
DOI:10.1021/acs.inorgchem.1c03908