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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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Die Kombination von Strategien der chemischen mit solchen der genetischen Optimierung (also Chemogenetik) ermöglicht die Erzeugung künstlicher Hydrogenasen auf der Grundlage der Biotin-Avidin-Technik. Wie bei Enzymen wird über Wechselwirkungen in der zweiten Koordinationssphäre zwischen dem Wirtprotein (Streptavidin) und dem Substrat (einem Olefin) die Selektivität gezielt in Richtung der R- oder S-Hydrierungsprodukte gesteuert.

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