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Lanthanide and actinide redox chemistry as a tool to study covalency


   Department of Chemistry

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  Dr Conrad Goodwin  No more applications being accepted  Funded PhD Project (Students Worldwide)

About the Project

Redox chemistry is an intrinsic property of every element, and while transition metal oxidation/reduction (redox) chemistry is fundamental to life, the redox chemistry of many of the f-elements is underdeveloped. The last 20 years has seen a renaissance in the redox chemistry of molecular lanthanide and actinide systems, with examples of M2+ for Th, U, Np, Pu, and all lanthanides save Pm; along with the first examples of Pr4+ and Tb4+.[1-3]

The stability of a given oxidation state is dictated by orbital energies and their involvement in forming bonds – certain donor types and geometries favour higher or lower oxidation states. Despite the redox advances above, the range of elements with verified bonds to actinides beyond U is extremely small. The first structurally authenticated metal-carbon bonds for Np, Pu, and Am came in 2017–2019,[4] and bonds to softer main-group elements such as Se are likewise extremely rare.[5] By expanding to new donors, and studying the effect of oxidation state on metal-donor interactions (e.g. M–S bonds with M5+/4+/3+), we can advance our understanding of f-block periodicity.

In this project we will synthesize stereochemically conserved molecular lanthanide and actinide systems where donor types are varied (e.g. consistent geometry across donors); and redox series with single donors to probe the metal-ligand interaction as a function of oxidation state. Finally, we will compare isoelectronic series between adjacent actinides such as U4+ and Np5+, which are both [Xe]5f26d0. Together these comparisons will revolutionise our understanding of periodicity in the early actinides.

You will be trained in synthetic air-free inorganic/organometallic techniques, and characterisation methods such as single-crystal X-ray crystallography. You will also receive training in the handling and chemistry of actinides such as U, Np, and Pu.

Academic background of candidates 

Applicants are expected to hold, or about to obtain, a minimum upper second-class undergraduate degree (or the overseas equivalent) in Chemistry. A Master’s degree in a relevant subject and experience in synthetic inorganic chemistry is desirable. Candidates with an interest in inorganic/organometallic air-free synthesis with actinide elements and/or experience in air/moisture-free chemistry are encouraged to apply.

Equality, diversity and inclusion is fundamental to the success of The University of Manchester, and is at the heart of all of our activities. We know that diversity strengthens our research community, leading to enhanced research creativity, productivity and quality, and societal and economic impact. We actively encourage applicants from diverse career paths and backgrounds and from all sections of the community, regardless of age, disability, ethnicity, gender, gender expression, sexual orientation and transgender status.

We also support applications from those returning from a career break or other roles. We consider offering flexible study arrangements (including part-time: 50%, 60% or 80%, depending on the project/funder).

All appointments are made on merit.

Contact for further Information

Please contact Dr Conrad Goodwin ([Email Address Removed] including a CV) for informal discussions before application.

For more information on the group visit: https://www.capgoodwin.com

Follow us on Twitter: @ConradGoodwin / @GoodwinRadChem

Department of Chemistry, Centre for Radiochemistry Research (CRR): https://www.chemistry.manchester.ac.uk/crr/


Funding Notes

This is a 3.5 year funded studentship, covering fees and stipend (£15,609 in 2021-22).
Open to all students.
We have start dates available in January, April, and September 2022.

References

[1] J. C. Wedal, W. J. Evans, J. Am. Chem. Soc. 2021, DOI: https://doi.org/10.1021/jacs.1021c08288.
[2] T. P. Gompa, A. Ramanathan, N. T. Rice, H. S. La Pierre, Dalton Trans. 2020, 49, 15945-15987.
[3] C. T. Palumbo, I. Zivkovic, R. Scopelliti, M. Mazzanti, J. Am. Chem. Soc. 2019, 141, 9827-9831.
[4] C. A. P. Goodwin, J. Su, T. E. Albrecht-Schmitt, A. V. Blake, E. R. Batista, S. R. Daly, S. Dehnen, W. J. Evans, A. J. Gaunt, S. A. Kozimor, N. Lichtenberger, B. L. Scott, P. Yang, Angew. Chem., Int. Ed. 2019, 58, 11695-11699.
[5] C. A. P. Goodwin, A. W. Schlimgen, T. E. Albrecht-Schönzart, E. R. Batista, A. Gaunt, M. T. Janicke, S. A. Kozimor, B. L. Scott, L. M. Stevens, F. D. White, P. Yang, Angew. Chem., Int. Ed. 2021, 60, 9459-9466.

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