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The Development of Artificial Metalloenzymes


Department of Chemistry

York United Kingdom Biochemistry Inorganic Chemistry Organic Chemistry Synthetic Chemistry

About the Project

Background: As natural biocatalysts, enzymes have evolved over billions or years to be highly efficient and selective. Their application in both bioconversions and chemical syntheses is attractive because of their sustainability and environmental compatibility. However, for many applications, suitable naturally occurring enzymes are not available. Tailor-made artificial metalloenzymes, on the other hand, can combine the selectivity and biocompatibility of proteins with the reactivity and the reaction scope of synthetic catalysts and thus have the potential to expand the range of applications in which biocatalysts can be used, for example by making new-to-nature transformations accessible.

Aim: The aim of the project is to develop modular and recyclable artificial metalloenzymes to enhance the scope and sustainability of biocatalysis.

Experimental Approach: The project will apply a catch-and-release approach to artificial enzyme design that provides new opportunities for biocatalysis. Inspired by the way bacteria acquire essential iron, we have developed a new iron-based anchor unit that connects synthetic catalysts to protein scaffolds, creating artificial enzymes, but on chemical reduction of the iron centre, the anchor unit disconnects and triggers the disassembly of the artificial enzymes. Hence both the protein and the synthetic catalyst can be recovered and recycled.

By using this redox-controlled catch-and-release approach, a flexible toolbox for the preparation of artificial metalloenzymes will be developed that allows catalysts, protein scaffolds and solid supports to be mixed, matched and recycled, for us and others to use, adapt and explore further, both in batch processes and in continuous flow.

Training: The project is multi-disciplinary and will provide comprehensive hands-on training in a wide range of techniques, including synthetic organometallic chemistry, protein handling and immobilisation techniques, HPLC methods and catalytic activity studies. In addition, the student will take a selection of suitable training courses, which, depending on their background , will complement lab-based training. The student will be provided with a number of other opportunities to network and present their work as a poster or oral presentation both within and external to the University. The student will be encouraged to attend two major international conferences during their PhD.

All Chemistry research students have access to our innovative Doctoral Training in Chemistry (iDTC): cohort-based training to support the development of scientific, transferable and employability skills: https://www.york.ac.uk/chemistry/postgraduate/training/idtc/

The candidate must have a background in synthetic chemistry and be willing to learn the other aspects of the project. You should hold or expect to achieve the equivalent of at least a UK upper second class degree in Chemistry or a related subject. Please check the entry requirements for your country: https://www.york.ac.uk/study/international/your-country/

The Department of Chemistry holds an Athena SWAN Gold Award and is committed to supporting equality and diversity for all staff and students. The Department strives to provide a working environment which allows all staff and students to contribute fully, to flourish, and to excel: https://www.york.ac.uk/chemistry/ed/.

For more information about the project, click on the supervisor’s name above to email the supervisor. For more information about the application process or funding, please click on email institution


Funding Notes

This project is available to students from any country who can fund their own studies. The Department of Chemistry at the University of York is pleased to offer Wild Fund Scholarships. Applications are welcomed from those who meet the PhD entry criteria from any country outside the UK. Scholarships will be awarded on supervisor support, academic merit, country of origin, expressed financial need and departmental strategy. For further details and deadlines, please see our website: View Website

References

Key reference: Redox-switchable siderophore anchor enables reversible artificial metalloenzyme assembly, Nature Catalysis, D. J. Raines, J. E. Clarke, E. V. Blagova, E. J. Dodson, K. S. Wilson, A.-K. Duhme-Klair, Nature Catalysis, (2018), 1, 680. SharedIt link: https://rdcu.be/4RgH.

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