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X-ray absorption spectroscopic investigation of Fe(II)-peplomycin and peplomycin derivatives: the effect of axial ligation on Fe-pyrimidine back-bonding

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Abstract.

X-ray absorption spectroscopy (XAS) is used to study ferrous complexes of a bleomycin (BLM) congener, peplomycin (PEP), and two of its derivatives, iso-peplomycin (ISO) and depyruvamide peplomycin (DP), in which potential axial ligands have been perturbed and removed, respectively. Application of extended X-ray absorption fine structure analysis shows an elongation of the short-distance component of the first coordination sphere in DP and ISO relative to PEP. The XAS pre-edge intensity concomitantly decreases with increased axial perturbation. The short-distance component of PEP is correlated to the Fe-pyrimidine bond and is related to the amount of π-back-bonding. Thus, the XAS analysis of these complexes provides structural information relevant to their differences in O2 reactivity.

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Authors and Affiliations

  1. Department of Chemistry, Stanford University, Stanford, California 94305, USA

    Erik C. Wasinger, Kelly Zaleski & Edward I. Solomon

  2. Department of Chemistry, Stanford University and Stanford Synchrotron Radiation Laboratory, SLAC, Stanford University, Stanford, California 94309, USA

    Britt Hedman & Keith O. Hodgson

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  1. Erik C. Wasinger
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  2. Kelly Zaleski
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  3. Britt Hedman
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  4. Keith O. Hodgson
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  5. Edward I. Solomon
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Wasinger, E.C., Zaleski, K., Hedman, B. et al. X-ray absorption spectroscopic investigation of Fe(II)-peplomycin and peplomycin derivatives: the effect of axial ligation on Fe-pyrimidine back-bonding. J Biol Inorg Chem 7, 157–164 (2002). https://doi.org/10.1007/s007750100283

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  • DOI: https://doi.org/10.1007/s007750100283

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