Writing through catalysis: A tape-reading molecular catalyst

Lead Research Organisation: University of Manchester
Department Name: Chemistry

Abstract

In 1936 Alan Turing published a concept for an automatic machine for abstract computing. Nowadays called a 'Turing machine', his proposal envisaged a device that featured a 'head' that could read and write symbols while moving along a tape. This influential thought experiment sparked the development of computer science. Although modern computers use a different design that employs random access memory, the resemblance of Turing's 'automatic machine' to information processing in biology is striking (the reading and writing of information by the ribosome, for example. Recently, the Leigh group reported an artificial molecular machine that is transported directionally along a molecular tape by chemical fuelling, changing the conformation of the reading head in response to chiral centres on the tape it encounters along the way. The conformational change results in changes to the circular dichroism response of the head, and so the sequence of symbols on the molecular tape can be read out as a string of data according to the changing CD response (+ve Cotton effect at 280 nm corresponds to the digit +1; -ve Cotton effect to -1, no Cotton effect to 0).
This project will seek to extend this concept to the writing of information through catalysis, using the change in conformation to alter the handedness of asymmetric catalysis by the reading head as it moves along the track. We will first investigate this concept through step-wise operations (e.g. with Trost-like ligands, as depicted below) and, ultimately, extend it to the synthesis of polymers with encoded sequence information, a task analogous to that performed by the ribosome.
The development of an artificial catalyst that changes the stereochemical outcome of catalytic transformations as it moves directionally along an information-encoded track would be a landmark achievement for the fields of both artificial molecular machinery and catalysis. It would enable the translation of molecular information from one form (the original tape) to another. This would be analogous to the function performed by the ribosome, but in a wholly artificial system not limited to peptides and featuring the reading of stereochemistry rather than nucleotide codons. The knowledge gained in this project will have impact in different areas. In addition to potentially improving the design of synthetic catalysts, the results may lead to the design of new, artificial, enzyme-like catalysts.

Planned Impact

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.

Publications

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Studentship Projects

Project Reference Relationship Related To Start End Student Name
EP/S023755/1 01/04/2019 30/09/2027
2752685 Studentship EP/S023755/1 01/10/2022 30/09/2026 Yuanshu Jiang