Enzyme activity by design: an artificial rhodium hydroformylase for linear aldehydes

Jarvis, A. G., Obrecht, L., Deuss, P. J., Laan, W., Gibson, E. K. , Wells, P. P. and Kamer, P. C.J. (2017) Enzyme activity by design: an artificial rhodium hydroformylase for linear aldehydes. Angewandte Chemie (International Edition), 56(44), pp. 13596-13600. (doi: 10.1002/anie.201705753) (PMID:28841767) (PMCID:PMC5659135)

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Artificial metalloenzymes (ArMs) are hybrid catalysts that offer a unique opportunity to combine the superior performance of natural protein structures with the unnatural reactivity of transition‐metal catalytic centers. Therefore, they provide the prospect of highly selective and active catalytic chemical conversions for which natural enzymes are unavailable. Herein, we show how by rationally combining robust site‐specific phosphine bioconjugation methods and a lipid‐binding protein (SCP‐2L), an artificial rhodium hydroformylase was developed that displays remarkable activities and selectivities for the biphasic production of long‐chain linear aldehydes under benign aqueous conditions. Overall, this study demonstrates that judiciously chosen protein‐binding scaffolds can be adapted to obtain metalloenzymes that provide the reactivity of the introduced metal center combined with specifically intended product selectivity.

Item Type:Articles
Additional Information:This work was supported by the EU through NEST Adventure STREP Project Artizymes (FP6‐2003‐NEST‐B3 15471), Marie Curie Excellence Grants, Artizyme Catalysis (MEXT‐2004‐014320), and through a Marie Curie Individual Fellowship project ArtOxiZymes to A.G.J. (H2020‐MSCA‐IF‐2014‐657755). We thank the EPSRC for funding through the EPSRC critical mass grant “Clean catalysis for sustainable development” (EP/J018139/1) and Sasol (CASE studentship to P.J.D.). The UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium, which is funded by the EPSRC (EP/K014706/2, EP/K014668/1, EP/K014854/1, EP/K014714/1, and EP/M013219/1).
Glasgow Author(s) Enlighten ID:Gibson, Dr Emma
Authors: Jarvis, A. G., Obrecht, L., Deuss, P. J., Laan, W., Gibson, E. K., Wells, P. P., and Kamer, P. C.J.
College/School:College of Science and Engineering > School of Chemistry
Journal Name:Angewandte Chemie (International Edition)
ISSN (Online):1521-3773
Published Online:13 September 2017
Copyright Holders:Copyright © 2017 The Authors
First Published:First published in Angewandte Chemie (International Edition) 56(44): 13596-13600
Publisher Policy:Reproduced under a Creative Commons License
Data DOI:10.17630/03fa38f2-b858-4fff-a478-83e61672955c

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Project CodeAward NoProject NamePrincipal InvestigatorFunder's NameFunder RefLead Dept
654181Catalytic HDO (UK Catalysis hub)Samuel JacksonEngineering and Physical Sciences Research Council (EPSRC)EP/K014706/1CHEM - CHEMISTRY
652891Towards closing the chlorine cycle in large-scale chemical manufacturing processes (UK Catalysis hub)David LennonEngineering and Physical Sciences Research Council (EPSRC)EP/K014854/1CHEM - CHEMISTRY