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The Quest for Accurate Theoretical Models of Metalloenzymes: An Aid to Experiment

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Transition Metals in Coordination Environments

Part of the book series: Challenges and Advances in Computational Chemistry and Physics ((COCH,volume 29))

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Abstract

Enzymes are versatile oxidants in Nature that catalyze a range of reactions very efficiently. Experimental studies on the mechanism of enzymes are sometimes difficult due to the short lifetime of catalytic cycle intermediates. Theoretical modeling can assist and guide experiment and elucidate mechanisms for fast reaction pathways. Two key computational approaches are in the literature, namely quantum mechanics /molecular mechanics (QM/MM) on complete enzyme structures and QM cluster models on active site structures only. These two approaches are reviewed here. We give examples where the QM cluster approach worked well and, for instance, enabled the bioengineering of an enzyme to change its functionality. In addition, several examples are given, where QM cluster models were insufficient and full QM/MM structures were needed to establish regio-, chemo-, and stereoselectivities.

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Acknowledgements

This work is partially supported as part of an EPSRC low carbon fuels grant (EP/N009533/1).

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Authors and Affiliations

  1. School of Chemistry, Cardiff University, Main Building, Park Place, Cardiff, CF10 3AT, UK

    Matthew G. Quesne

  2. The Manchester Institute of Biotechnology and School of Chemical Engineering and Analytical Science, The University of Manchester, 131 Princess Street, Manchester, M1 7DN, UK

    Sam P. de Visser

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Correspondence to Matthew G. Quesne .

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  1. Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Kraków, Poland

    Ewa Broclawik

  2. Jerzy Haber Institute of Catalysis and Surface Chemistry, Polish Academy of Sciences, Kraków, Poland

    Tomasz Borowski

  3. Faculty of Chemistry, Jagiellonian University, Kraków, Poland

    Mariusz Radoń

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Quesne, M.G., de Visser, S.P. (2019). The Quest for Accurate Theoretical Models of Metalloenzymes: An Aid to Experiment. In: Broclawik, E., Borowski, T., Radoń, M. (eds) Transition Metals in Coordination Environments. Challenges and Advances in Computational Chemistry and Physics, vol 29. Springer, Cham. https://doi.org/10.1007/978-3-030-11714-6_14

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