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X-Ray Structure and Designed Evolution of an Artificial Transfer Hydrogenase

Authors

  • Marc Creus Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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    • These authors contributed equally to this work.

  • Anca Pordea,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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    • These authors contributed equally to this work.

  • Thibaud Rossel,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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  • Alessia Sardo,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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  • Christophe Letondor Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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  • Anita Ivanova Dr.,

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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  • Isolde LeTrong Dr.,

    1. Departments of Biological Structure and Biochemistry and the Biomolecular Structure Center, University of Washington, Box 357420 Seattle, WA 98195-7420, USA, Fax:(+1) 206-543-1524
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  • Ronald E. Stenkamp Prof.,

    1. Departments of Biological Structure and Biochemistry and the Biomolecular Structure Center, University of Washington, Box 357420 Seattle, WA 98195-7420, USA, Fax:(+1) 206-543-1524
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    • Corresponding authors: Prof. Stenkamp for the X-ray structure, Prof. Ward for all other matters.

  • Thomas R. Ward Prof.

    1. Institute of Chemistry, University of Neuchâtel, Av. Bellevaux 51, CP 158, 2009 Neuchâtel, Switzerland, Fax: (+41) 32-718-2511
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    • Corresponding authors: Prof. Stenkamp for the X-ray structure, Prof. Ward for all other matters.


  • This work was funded by the Swiss National Science Foundation (Grants FN 200021-105192 and 200020-113348), the Roche Foundation as well as the FP6 Marie Curie Research Training network (MRTN-CT-2003-505020) and the Canton of Neuchâtel. We thank Umicore Precious Metals Chemistry for a loan of ruthenium. We thank C. R. Cantor for the streptavidin gene.

Abstract

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A structure is worth a thousand words: Guided by the X-ray structure of an S-selective artificial transfer hydrogenase, designed evolution was used to optimize the selectivity of hybrid catalysts. Fine-tuning of the second coordination sphere of the ruthenium center (see picture, orange sphere) by introduction of two point mutations allowed the identification of selective artificial transfer hydrogenases for the reduction of dialkyl ketones.

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