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EASTBIO The development of salen-based artificial metalloenzymes for sustainable chemistry


   School of Chemistry

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  Dr A Jarvis, Dr Jennifer Garden  No more applications being accepted  Funded PhD Project (Students Worldwide)

About the Project

Project Details:

Artificial metalloenzymes (ArMs) combine transition metal reactivity with the selectivity of enzymes to introduce new catalytic reactions into the biocatalytic toolbox.1 A classic group of transition metal catalysts are the salen and salophen-type complexes that exhibit catalytic activity for a range of synthetic reactions, including epoxidation, C-H bond oxidation and amination, small molecule activation such as water splitting, and polymerisation reactions for green plastics.

The first examples of salen-based ArMs emerged in early 2000s when transition metal-bound salen ligands were used along with myoglobin (apo-Mb) scaffolds to yield selective biocatalysts for oxidation of thiols.2,3. Despite a number of subsequent reports, the reaction scope of these ArMs has not been explored beyond sulfoxidation, even though salen catalysts are highly versatile.

Ongoing work within the Jarvis group has shown we can improve the stability of these ArMs by exploring both the salen ligand structure and rational design of the active site. The use of different transition metal complexes permits access to high-valent metal intermediate species, such as Fe(IV)=O, and functionalisation of the salen ligand backbone alongside protein engineering allows for fine-tuning of the electronic properties of the metal.

 This project will build on this work to explore the catalytic activity of these new ArMs beyond sulfoxidation reactions. Due to the wide variety of reactions that can be catalysed by salen-based complexes, the student will have the opportunity to develop the project depending on their interests. Potential directions include:

1. The development of selective oxidation reactions and in depth structural and kinetic studies.

2. Development of a green and biocompatible water-splitting catalyst.

3. New catalysts for the synthesis/recycling of biodegradable plastics (in collaboration with Dr Jenni Garden).

 The project would suit a student with an interest in improving the sustainability of chemical production, and working at the interface of two disciplines – chemistry and biology. Depending on the student’s background, training will be provided in molecular biology (i.e. the growth, expression and purification of proteins, genetic optimisation via either site-directed or random mutagenesis), structural biology and bioinorganic chemistry (understanding metal binding of the proteins using methods such as UV-vis, crystallography, NMR), and in the organic chemistry needed for catalytic testing (both synthesis and analysis i.e. HPLC, GC).

 The group has a number of ongoing collaborations to support this work, and there will be the opportunity to spend time in other groups to acquire the additional skills and data.

Application Process:

To apply for an EASTBIO PhD studentship, follow the instructions below:

 ·        Informal enquiries should be addressed to Dr Amanda Jarvis. To apply, please send a cover letter outlining your previous research experience and reasons for applying, alongside an up-to-date CV to [Email Address Removed]

 ·        After you have discussed the projects of interest to you with Dr Amanda Jarvis., download and complete our Equality, Diversity and Inclusion survey and then fill in the EASTBIO Application Form and submit to Dr Jarvis.

 ·        Send the EASTBIO Reference Form to your two academic/professional referees, and ask your referees to submit your references directly to Dr Amanda Jarvis [Email Address Removed]

We anticipate that our first set of interviews will be held 6th – 10th February 2023.

If you have further queries about the application/recruitment process please contact EASTBIO

The School of Chemistry holds a Silver Athena SWAN award in recognition of our commitment to advance gender equality in higher education. The University is a member of the Race Equality Charter and is a Stonewall Scotland Diversity Champion, actively promoting LGBT equality. The University has a range of initiatives to support a family friendly working environment. See our University Initiatives website for further information. University Initiatives website: https://www.ed.ac.uk/equality-diversity/help-advice/family-friendly


Funding Notes

UKRI-funded studentships are open to students worldwide and will cover tuition fees at the UK rate, plus a stipend to support living costs and an annual research grant of £5,000 for the first three years of the PhD research. Please note that UKRI has recently announced an increase of its minimum stipend levels in response to the ongoing cost of living crisis. The increased stipend of £17,668 full time equivalent has come into effect from the 1st of October 2022 and will apply, with annual increments, to the new intake of students starting in autumn 2023.

References

1. a) F. Schwizer et al. Chem. Rev., 2018, 118, 142-231. b) A.G. Jarvis, Curr. Opin. Chem. Biol. 2020, 58, 63.
2. M. Ohashi, T. Koshiyama, T. Ueno, M. Yanase, H. Fujii, Y. Watanabe, Angew. Chem. Int. Ed., 2003, 42, 1005-1008.
3. T. Ueno et al. J. Am. Chem. Soc., 2005, 127, 6556-6562.

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