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Tailoring the Active Site of Chemzymes by Using a Chemogenetic-Optimization Procedure: Towards Substrate-Specific Artificial Hydrogenases Based on the Biotin–Avidin Technology

Authors

  • Gérard Klein Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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    • Both authors contributed equally to the work.

  • Nicolas Humbert,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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    • Both authors contributed equally to the work.

  • Julieta Gradinaru Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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  • Anita Ivanova,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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  • François Gilardoni Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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  • Untung E. Rusbandi,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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  • Thomas R. Ward Prof.

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 2, 2007 Neuchâtel, Switzerland, Fax: (+41) 327-182-511
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  • We thank Professor C. R. Cantor for the streptavidin gene and Professors P. Schürmann and J.-M. Neuhaus for their help in setting up the protein production. This work was funded by the Swiss National Science Foundation (Grants FN 620-57866.99 and FN 200021-105192/1 as well as NRP 47 “Supramolecular Functional Materials”), CERC3 (Grant FN20C321-101071), the Roche Foundation, the Canton of Neuchâtel, as well as the FP6 Marie Curie Research Training Network (MRTN-CT-2003-505020). Umicore Precious Metals Chemistry is acknowledged for a loan of rhodium.

Abstract

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The combination of chemical- with genetic-optimization strategies (i.e. chemogenetic) allows the production of artificial hydrogenases based on the biotin–avidin technology. In the spirit of enzymes, second-coordination-sphere interactions between the host protein (streptavidin) and the substrate (an olefin) allow fine-tuning of the selectivity to produce either R or S hydrogenation products.

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