Electrostatic Catalysis

Lead Research Organisation: University of Oxford
Department Name: Oxford Chemistry

Abstract

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Description What were the most significant achievements from the awards?
Scientific:
a) We have elucidated and fully characterised the Micheal addition reaction inside the [Pd2L4]2+ cage. We showed computationally that catalysis arises due to entropy contribution, i.e., dual biding of the reactants instead of enthalpic stabilisation.
b) We have developed an automated method for parametrisation of the metal centre needed for workflow in studying the reaction in supramolecular cages. The publication is ready and will be submitted soon.
c) We developed a semi-automated approach for finding ground and transition states inside the cages for the C-C forming reaction bonds. This workflow will be extremely useful to speed up future work on the project.
d) We identified ground state stabilisation as a new strategy for optimising the catalytic activity of supramolecular cages. We are working closely with experimental colleagues to validate these findings experimentally.

The work done in the award has been presented in several meetings by both the PI and the PDRA

PDRA:
a) 2023 December: Macrocyclic and Supramolecular Chemistry Meeting, Birmingham, UK
(poster: "metallicious: Automated force-field parametrisation of covalently bound metals for supramolecular structures")
b) 2023 May, AI for enzyme instructed catalysts, Amsterdam, the Netherlands (poster: "Catalysis in [Fe4L6]8+ supramolecular cage")
c) 2022 December, Macrocyclic and Supramolecular Chemistry Meeting, Nottingham, UK (poster: "Dynamics and catalysis in [Fe4L6]8+ supramolecular cage")
d) 2022 September, Confinement-Controlled Chemistry Symposium (talk: "Exploring chemical reactions through automation and machine learning")

PDRA:
a) 2023 December: Macrocyclic and Supramolecular Chemistry Meeting, Birmingham, UK
(poster: "metallicious: Automated force-field parametrisation of covalently bound metals for supramolecular structures")
b) 2023 May, AI for enzyme instructed catalysts, Amsterdam, the Netherlands (poster: "Catalysis in [Fe4L6]8+ supramolecular cage")
c) 2022 December, Macrocyclic and Supramolecular Chemistry Meeting, Nottingham, UK (poster: "Dynamics and catalysis in [Fe4L6]8+ supramolecular cage")
d) 2022 September, Confinement-Controlled Chemistry Symposium (talk: "Exploring chemical reactions through automation and machine learning")

PI
a) (To come) May 2024, Keynote speaker at Girona Seminar 2024 dedicated to Supramolecular Chemistry
b) June 2023, Invited speaker at Physical Organic Gordon Research Conference. Holderness, USA
c) May 2-23, RSC Prize Tour at the Universities of Liverpool, Manchester and Edinburgh, UK May
d) May 2023, Invited speaker at AI4 Enzyme Instructed Catalysis Workshop. Amsterdam, NL
e) Dec 2022, Invited speaker at RSC Macrocyclic and Supramolecular Chemistry Meeting. Nottingham, UK
Exploitation Route We have open-source software that has significantly sped up the modelling process of systems containing metals. While our primary aim was an application for supramolecular cages, the developed tool can be used for a broad spectrum of systems, such as proteins, metalorganic frameworks and supramolecular knots. This work is completed, and the manuscript is in preparation. We expect this tool to be relevant for computational chemists across different fields.
Sectors Chemicals

Environment
 
Description Collaboration with the Martí Centelles grpoup in Spain 
Organisation Polytechnic University of Valencia
Country Spain 
Sector Academic/University 
PI Contribution We have worked together in the development of the computational tool, CageCavityCalc (C3), which enable calculating and visualizing cavities in molecular cages.
Collaborator Contribution Dr Marti-VCentelles developed the idea and we contributed with testing, feedback, etc. We are working together to implement this tool as part of cgbind.
Impact Preprint: https://chemrxiv.org/engage/chemrxiv/article-details/65c9f0bf9138d23161ecc7b7
Start Year 2022