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  Mechanochemistry and the mechanical bond – sustainable methods for the synthesis of functional rotaxanes and catenanes


   School of Chemistry

  ,  Applications accepted all year round  Funded PhD Project (UK Students Only)

About the Project

Background

Molecules are mechanically bonded if they are composed of two covalent subcomponents that are threaded through one another such that they can never separate even though there is no covalent bond between them. Such structures have been proposed to have various applications, from molecular machines to catalysts, materials, and in medicine. However, their synthesis remains challenging and environmentally burdensome – if they are to deliver on their promise, a step change in their sustainable synthesis is needed.

Mechanochemistry is the use of mechanical force to initiate and control chemical reactions, which has many advantages over classical solution-phase synthesis, including the ability to conduct reactions at lower temperatures, overcome issues with solubility, as well as resulting in less waste. Mechanochemistry can now be performed as a continuous, scalable, manufacturing process via the use of Twin Screw Extrusion (TSE), which was highlighted by IUPAC as one of the top 10 technologies that will change the world, making it the ideal solution to many synthetic chemistry problems.

The project

The Goldup Group have demonstrated the potential of mechanically bonded molecules in catalysis (https://doi.org/10.1002/anie.202115961), sensing (https://doi.org/10.1002/anie.201712931), biochemistry (https://doi.org/10.1021/jacs.0c01670) and as ligands (https://doi.org/10.1002/anie.202103596). Although they have developed methods to synthesise such molecules in high yield (https://doi.org/10.1021/jacs.6b08958) these solution-phase syntheses can never achieve the efficiency required for large scale applications. The Crawford Group (https://www.birmingham.ac.uk/staff/profiles/chemistry/crawford-deborah.aspx) have pioneered the use of extrusion (https://onlinelibrary.wiley.com/doi/abs/10.1002/adma.201505352) and other mechanochemical methods (https://doi.org/10.1002/ange.201706723) for the synthesis of complex molecules (https://doi.org/10.1039/D1DT01751A), including the components of supramolecular species (https://doi.org/10.1039/C4SC03217A).

The successful candidate will combine methods developed by the Goldup and Crawford Groups to demonstrate that mechanochemical methods can solve the sustainability problem inherent in the chemistry of the mechanical bond by developing sustainable methods for the synthesis of functional interlocked molecules, setting the stage for the next phase of the chemistry of the mechanical bond.

Relevant reviews:

The chemistry of interlocked molecules: Goldup, Chem. Commun. 2014, https://doi.org/10.1039/C3CC47842D

Recent developments in mechanochemical materials synthesis by extrusion: Crawford, Adv. Mater. 2016, https://doi.org/10.1002/adma.201505352

Training and mentoring

Training will be provided in syntheticc and supramolecular chemistry by the Goldup Group, and mechanochemistry and related concepts by the Crawford Group. They will gain experience of analytical techniques including advanced NMR analysis, single crystal x-ray diffraction and HPLC. They will be mentored by to improve their writing, presentation skills and ability to design and execute new projects. Completing a PhD under the supervision of Goldup and Crawford will prepare students for leadership roles in scientific research, as well as positions across the scientific sector more generally.

The Goldup Group

Research in the Goldup Group (https://golduplab.org/) focusses on the synthesis, properties and applications of mechanically interlocked molecules such as rotaxanes and catenanes.

The Crawford Group

Research in the Crawford Group (https://www.birmingham.ac.uk/staff/profiles/chemistry/crawford-deborah.aspx) focuses on solvent-free routes to sustainable synthesis, including TSE, the first technique that scales-up solvent-free synthesis.

Funding

This studentship is fully funded for 3.5 years and includes a tax-free annual stipend (currently £18,622) and fees (currently £4,712) at the UK home rate. Due to funding restrictions, applicants not eligible for UK home fee status will only be considered in exceptional circumstances.

Application process

Candidates should contact Professor Goldup by email () with a CV and a covering letter. The School of Chemistry is keen to achieve a gender and diversity balance across the School and welcome applicants from all backgrounds. The School holds an Athena SWAN Bronze Award, which recognises its work in promoting women’s careers in science, technology, engineering, mathematics and medicine (STEM).

Chemistry (6)

References


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