pH-Dependent Coordination of AgI Ions by Histidine: Experiment, Theory, and a Model for SilE

Authors

  • Laurent Mirolo,

    1. Department of Chemistry, Fribourg Center for Nanomaterials, University of Fribourg, Chemin du musée 9, 1700 Fribourg (Switzerland), Fax: (+41) 26-300-97-38
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    • These authors contributed equally to this work.

  • Tobias Schmidt,

    1. Department of Chemistry, University of Basel, Klingelbergstrasse 80, 4056 Basel (Switzerland)
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    • These authors contributed equally to this work.

  • Dr. Sonja Eckhardt,

    1. Department of Chemistry, Fribourg Center for Nanomaterials, University of Fribourg, Chemin du musée 9, 1700 Fribourg (Switzerland), Fax: (+41) 26-300-97-38
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    • These authors contributed equally to this work.

  • Prof. Dr. Markus Meuwly,

    1. Department of Chemistry, University of Basel, Klingelbergstrasse 80, 4056 Basel (Switzerland)
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  • Prof. Dr. Katharina M. Fromm

    Corresponding author
    1. Department of Chemistry, Fribourg Center for Nanomaterials, University of Fribourg, Chemin du musée 9, 1700 Fribourg (Switzerland), Fax: (+41) 26-300-97-38
    • Department of Chemistry, Fribourg Center for Nanomaterials, University of Fribourg, Chemin du musée 9, 1700 Fribourg (Switzerland), Fax: (+41) 26-300-97-38
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Abstract

Artificial implants and biomaterials lack the natural defense system of our body and, thus, have to be protected from bacterial adhesion and biofilm formation. In addition to the increasing number of implanted objects, the resistance of bacteria is also an important problem. Silver ions are well-known for their antimicrobial properties, yet not a lot is known about their mode of action. Silver is expected to interact on many levels, thus the development of silver resistance is very difficult. Nevertheless, some bacteria are able to resist silver, even at higher concentrations. One such defense mechanism of bacteria against heavy-metal intoxication includes an efflux system. SilE, a periplasmic silver-binding protein that is involved in this defense mechanism, has been shown to possess numerous histidine functions, which strongly bind to silver atoms, as demonstrated by ourselves previously. Herein, we address the question of how histidine binds to silver ions as a function of pH value. This property is important because the local proton concentration in cells varies. Thus, we solved the crystal structures of histidine–silver complexes at different pH values and also investigated the influence of the amino-acid configuration. These results were completed by DFT calculations on the binding strength and packing effects and led to the development of a model for the mode of action of SilE.

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