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Controlled Ligand Exchange Between Ruthenium Organometallic Cofactor Precursors and a Naïve Protein Scaffold Generates Artificial Metalloenzymes Catalysing Transfer Hydrogenation.

التفاصيل البيبلوغرافية
العنوان: Controlled Ligand Exchange Between Ruthenium Organometallic Cofactor Precursors and a Naïve Protein Scaffold Generates Artificial Metalloenzymes Catalysing Transfer Hydrogenation.
المؤلفون: Biggs GS; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK., Klein OJ; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.; Department of Biochemistry, University of Cambridge, Tennis Court Road, Cambridge, CB2 1GA, UK., Maslen SL; MRC Laboratory of Molecular Biology, Francis Crick Avenue, Cambridge Biomedical Campus, Cambridge, CB2 0QH, UK., Skehel JM; MRC Laboratory of Molecular Biology, Francis Crick Avenue, Cambridge Biomedical Campus, Cambridge, CB2 0QH, UK., Rutherford TJ; MRC Laboratory of Molecular Biology, Francis Crick Avenue, Cambridge Biomedical Campus, Cambridge, CB2 0QH, UK., Freund SMV; MRC Laboratory of Molecular Biology, Francis Crick Avenue, Cambridge Biomedical Campus, Cambridge, CB2 0QH, UK., Hollfelder F; Department of Biochemistry, University of Cambridge, Tennis Court Road, Cambridge, CB2 1GA, UK., Boss SR; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK., Barker PD; Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge, CB2 1EW, UK.
المصدر: Angewandte Chemie (International ed. in English) [Angew Chem Int Ed Engl] 2021 May 03; Vol. 60 (19), pp. 10919-10927. Date of Electronic Publication: 2021 Mar 26.
نوع المنشور: Journal Article; Research Support, Non-U.S. Gov't
اللغة: English
بيانات الدورية: Publisher: Wiley-VCH Country of Publication: Germany NLM ID: 0370543 Publication Model: Print-Electronic Cited Medium: Internet ISSN: 1521-3773 (Electronic) Linking ISSN: 14337851 NLM ISO Abbreviation: Angew Chem Int Ed Engl Subsets: MEDLINE
أسماء مطبوعة: Publication: <2004-> : Weinheim : Wiley-VCH
Original Publication: Weinheim/Bergstr. : New York, : Verlag Chemie ; Academic Press, c1962-
مواضيع طبية MeSH: Metalloproteins/*metabolism , Organometallic Compounds/*chemistry , Ruthenium/*chemistry, Catalysis ; Fluorine ; Hydrogenation ; Ligands ; Magnetic Resonance Spectroscopy ; Metalloproteins/chemistry ; Molecular Structure ; Organometallic Compounds/metabolism ; Ruthenium/metabolism
مستخلص: Many natural metalloenzymes assemble from proteins and biosynthesised complexes, generating potent catalysts by changing metal coordination. Here we adopt the same strategy to generate artificial metalloenzymes (ArMs) using ligand exchange to unmask catalytic activity. By systematically testing Ru II (η 6 -arene)(bipyridine) complexes designed to facilitate the displacement of functionalised bipyridines, we develop a fast and robust procedure for generating new enzymes via ligand exchange in a protein that has not evolved to bind such a complex. The resulting metal cofactors form peptidic coordination bonds but also retain a non-biological ligand. Tandem mass spectrometry and 19 F NMR spectroscopy were used to characterise the organometallic cofactors and identify the protein-derived ligands. By introduction of ruthenium cofactors into a 4-helical bundle, transfer hydrogenation catalysts were generated that displayed a 35-fold rate increase when compared to the respective small molecule reaction in solution.
(© 2021 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.)
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معلومات مُعتمدة: MC_U105184326 United Kingdom MRC_ Medical Research Council
فهرسة مساهمة: Keywords: direct coordination; ligand exchange; metalloenzymes; ruthenium; transfer hydrogenation
المشرفين على المادة: 0 (Ligands)
0 (Metalloproteins)
0 (Organometallic Compounds)
284SYP0193 (Fluorine)
7UI0TKC3U5 (Ruthenium)
تواريخ الأحداث: Date Created: 20210222 Date Completed: 20210809 Latest Revision: 20240402
رمز التحديث: 20240402
مُعرف محوري في PubMed: PMC8251807
DOI: 10.1002/anie.202015834
PMID: 33616271
قاعدة البيانات: MEDLINE
الوصف
تدمد:1521-3773
DOI:10.1002/anie.202015834