Merging transition metal-catalysis and electrochemistry for late stage functionalization of biologically active molecules

Transition-metal catalysed C-H functionalisation reactions have proven revolutionary in recent years, with thousands of publications describing myriad protocols including cross-coupling reactions, directed and non-directed regioselective C-C bond formation (achieving alkylation, alkenylation and arylation), and selective late-stage functionalisation of complex biologically active molecules. Electrochemistry has been utilised since the 1800s, but has largely been viewed by most synthetic chemists as obscure and inaccessible until only very recently. In the past 15 years, electrochemistry has enjoyed a surge of new-found interest within the synthesis community as electrochemistry equipment has become more standardised and accessible, with chemists discovering exciting novel transformations utilising electrochemical methods. Transition-metal catalysis integrated with electrochemistry has emerged as a versatile method for C-H functionalisation, and is at the forefront of research understanding, enabling previously unknown transformations while simultaneously removing the need for stoichiometric oxidants and reductants, improving the sustainability of synthetic chemistry. This thesis details work undertaken to contribute to this exciting modern field of chemistry, by developing new methods of electrochemical transition-metal catalysed C-H functionalisation for the late-stage functionalisation of biologically active molecules

iCAT will work with industry partners to create an holistic approach to the training of students in biocatalysis, chemocatalysis, and their process integration. Traditional graduate training typically focuses on one aspect of catalysis and this approach can severely restrict innovation and impact. Advances in technology and fundamental reaction discovery are rendering this silo-approach obsolete, and a new training modality is needed to produce the next generation of chemists and engineers who can operate across a far broader chemical continuum. iCAT will meet this challenge with a state-of-the-art CDT, equipping the next generation of scientists and engineers with the skills needed to develop future catalytic processes and create the functional molecules of tomorrow.

The UK has one of the world's top-performing chemical industries, achieving outstanding levels of growth, exports, productivity and international investment. The UK's chemical industry is a significant provider of jobs and creator of wealth, with a turnover in excess of £50 billion and a contribution of over £15 Billion of value to the UK economy [2015 figures]. iCAT will deliver highly skilled people to lead this industry across its various sectors, achieving impact through the following actions:

1. Equip the next generation of science and engineering leaders with the interdisciplinary skills and knowledge needed to work across the bio and chemo catalytic remit and build the functional molecules we need to structure society.

2. Provide a highly skilled workforce and research base, skilled in the latest methodologies, strategies and techniques of catalysis and engineering that is crucial for the UK's Chemical Industry.

3. Build the critical mass necessary to support effective cohort-based training in a world-class research environment.

4. Develop and disseminate new catalytic technologies and processes that will be taken up by industrial and academic teams around the world.

5. Encourage Industry to promote research challenges within the CDT that are of core relevance to their business.

6. Provide cohesion in the integration of biocatalysis, engineering and chemocatalysis to create a more unified voice for strategic dialogue with industry, funders and policy makers, and more generally outreach and public engagement.

7. Draw-in and bring together Industrial partners to facilitate future Industrial collaborations.

8. Benefit Industrial scientists through interactions with the CDT (e.g. training and supervisory experience, exposure to cutting-edge synthesis and catalysis etc).

9. Link with other activities in the landscape: bringing unique expertise in catalysis to, for example, externally-funded University-led initiatives, EPRSC Grand Challenge Networks, and the National Catalysis Hub.