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Enzyme Control Over Ferric Iron Magnetostructural Properties.


ABSTRACT: Fe3+ complexes in aqueous solution can exist as discrete mononuclear species or multinuclear magnetically coupled species. Stimuli-driven change to Fe3+ speciation represents a powerful mechanistic basis for magnetic resonance sensor technology, but ligand design strategies to exert precision control of aqueous Fe3+ magnetostructural properties are entirely underexplored. In pursuit of this objective, we rationally designed a ligand to strongly favor a dinuclear μ-oxo-bridged and antiferromagnetically coupled complex, but which undergoes carboxylesterase mediated transformation to a mononuclear high-spin Fe3+ chelate resulting in substantial T1 -relaxivity increase. The data communicated demonstrate proof of concept for a novel and effective strategy to exert biochemical control over aqueous Fe3+ magnetic, structural, and relaxometric properties.

SUBMITTER: Wang H 

PROVIDER: S-EPMC8935392 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Enzyme Control Over Ferric Iron Magnetostructural Properties.

Wang Huan H   Cleary Michael B MB   Lewis Luke C LC   Bacon Jeffrey W JW   Caravan Peter P   Shafaat Hannah S HS   Gale Eric M EM  

Angewandte Chemie (International ed. in English) 20211202 3


Fe<sup>3+</sup> complexes in aqueous solution can exist as discrete mononuclear species or multinuclear magnetically coupled species. Stimuli-driven change to Fe<sup>3+</sup> speciation represents a powerful mechanistic basis for magnetic resonance sensor technology, but ligand design strategies to exert precision control of aqueous Fe<sup>3+</sup> magnetostructural properties are entirely underexplored. In pursuit of this objective, we rationally designed a ligand to strongly favor a dinuclear  ...[more]

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