Iron Coordination Properties of Gramibactin as Model for the New Class of Diazeniumdiolate Based Siderophores

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Abstract

Gramibactin (GBT) is an archetype for the new class of diazeniumdiolate siderophores, produced by Paraburkholderia graminis, a cereal-associated rhizosphere bacterium, for which a detailed solution thermodynamic study exploring the iron coordination properties is reported. The acid-base behavior of gramibactin as well as its complexing ability toward Fe3+ was studied over a wide range of pH values (2≤pH≤11). For the latter the ligand-competition method employing EDTA was used. Only two species are formed: [Fe(GBT)]− (pH 2 to 9) and [Fe(GBT)(OH)2]3− (pH≥9). The formation of [Fe(GBT)]− and its occurrence in real systems was confirmed by LC-HRESIMS analysis of the bacteria culture broth extract. The sequestering ability of gramibactin was also evaluated in terms of the parameters pFe and pL0.5. Gramibactin exhibits a higher sequestering ability toward Fe3+ than EDTA and of the same order of magnitude as hydroxamate-type microbial siderophores, but smaller than most of the catecholate-type siderophores and much higher than the most known phytosiderophores.

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Gama, S., Hermenau, R., Frontauria, M., Milea, D., Sammartano, S., Hertweck, C., & Plass, W. (2021). Iron Coordination Properties of Gramibactin as Model for the New Class of Diazeniumdiolate Based Siderophores. Chemistry - A European Journal, 27(8), 2724–2733. https://doi.org/10.1002/chem.202003842

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