PEPR - A centre for Pulse Electron Paramagnetic Resonance spectroscopy at Imperial College

Lead Research Organisation: Imperial College London
Department Name: Chemistry

Abstract

Unpaired electrons play vital roles in e.g. respiration and photosynthesis, are associated with human diseases including cancer and Alzheimer's disease and are at the basis of the modern computer and many industrially used catalysts. We propose to set up a new research facility at Imperial College London which employs a powerful technique called ulse Electron Paramagnetic Resonance (EPR) spectroscopy, to identify and characterise such unpaired electrons (free radicals) and gain detailed insight into the structure and dynamics of paramagnetic compounds. The facility (PEPR) will therefore contribute to solving grand, societal challenges such as healthy aging, sustainable energy generation and storage, greener and more effective catalytic solutions for chemical manufacturing and developing a new generation of electronic devices.

PEPR will encompass state-of-the-art pulse EPR instrumentation and in partnership with University College London we will develop new instrumentation and methodology to push the boundaries of what is possible with EPR today and widen the applications of this already extremely versatile technique. We will do this by combining EPR spectroscopy with electrochemistry, a powerful method for investigating oxidation-reduction processes that often lie at the heart of systems with unpaired electrons and by enabling pulse EPR investigations of paramagnetic compounds that cannot be accumulated in sufficiently large quantities to be studied with current commercially-available instrumentation. PEPR will therefore bring new capabilities to the UK, build on the existing research strengths and infrastructure at Imperial College and engage new academic users and research centres across London, regionally and UK-wide.

The research facilitated by PEPR will have an immediate impact on UK science, with academic beneficiaries in a diverse range of research disciplines, and a significant people-pipeline through the many affiliated PhD students and PDRAs. Moreover, the facility's location at Imperial College's newly-established and growing innovation campus at White City provides a unique opportunity to encourage academia and industry to collaborate more closely on common, global challenges. Access to the wider community will be provided through outreach events such as the Great Exhibition Road Festival and the Imperial Lates, as well as by including the facility into the tours that are already taking place regularly in the Molecular Sciences Research Hub where PEPR will be located.

Planned Impact

We propose to create an internationally-renowned research facility (PEPR) that enables the elucidation and exploitation of unpaired electrons across a wide range of disciplines, building on existing research strengths at Imperial College and beyond:

The study of unpaired electrons has already had an impact on our society on many levels, such as in IT and communication (e.g. the modern computer) and in our fundamental understanding of the mechanisms of enzymes underpinning disease or bioinspired technology. PEPR will contribute to what may be some of the next breakthroughs, such as quantum computing, artificial photosynthesis and green and efficient energy production and storage. We will capitalise on the existing research strengths at Imperial College across Chemistry, Physics, Life Sciences, Engineering, Medicine and Materials Sciences, such as in e.g. catalysis, battery research and protein biophysics. The unique combination of state-of-the-art pulse EPR techniques with electrochemistry and instrument development to push the boundaries of signal to noise and trap previously elusive paramagnetic intermediates will enable new and unprecedented approaches and insights into these diverse research areas and address some of the EPSRC-aligned Grand Challenges in Quantum Physics for New Quantum Technologies, Nanoscale Design of Functional Materials, Understanding the Physics of Life, Directed Assembly of Extended Structures with Targeted Properties, Systems Chemistry: Exploring the Chemical Roots of Biological Organisation.

The research to be carried out at PEPR underpins at least 13 CDTs and spans nearly 80 research groups at Imperial, London-wide, regionally, UK-wide and internationally. In addition to the outcome of a highly skilled and trained researcher working across all areas of science (PEPR's facility manager), PEPR will thus have a significant impact on people and hence on the next generation of scientists and engineers. By opening up PEPR to the wider community (up to 30% external usage) we will further extend the impact of the facility. This is especially true given PEPR's location in a multidisciplinary research building adjoining the Translation and Innovation Hub where emergent SMEs (e.g. Polymateria) are already engaging in collaborative opportunities, in additional to large companies (e.g. Shell). Imperial has an excellent track-record in working with industry and any relevant IP will be managed via well-established routes for technology translation through Imperial's Industry Partnership and Commercialisation team. Dedicated and expert support through the facility manager and the scientifically diverse management team will ensure that new users will get the most out of their experiments at PEPR.

Publication, presentation, lunchtime seminars and engagement innovation activities at White City (e.g. with Upstream, a partnership between Hammersmith & Fulham Council and Imperial College London) will ensure that the impact generated through access to PEPR is disseminated effectively and without delay. Our symposium in year 4 will draw experts, in academia and industry, and further publicise the work of PEPR on an international level. We will engage in numerous outreach opportunities at Imperial including the Great Exhibition Road Festival (targeting all ages) and the Imperial Lates (for adults) where the PEPR management team already have an existing track record.

Publications

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Barluzzi L (2022) Identification of Oxidation State +1 in a Molecular Uranium Complex. in Journal of the American Chemical Society

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Richardson KH (2021) Functional basis of electron transport within photosynthetic complex I. in Nature communications

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Seif-Eddine M (2022) Following the evolution of paramagnetic species during catalysis: film-electrochemical EPR spectroscopy in Biochimica et Biophysica Acta (BBA) - Bioenergetics

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Webster L (2022) Synthesis and reactivity of titanium 'POCOP' pincer complexes in Dalton Transactions

 
Description As a result of the new methodology developed as part of PEPR (film-electrochemical EPR), we have been able to make a discovery in the area of electrocatalysis. Because we are now able to monitor radicals in real time during electrocatalysis, we have been able to trap a key intermediate in the electrocatalytic oxidation of alcohols by nitroxides, an industrially relevant reaction. The paper is currently under review. The methodology is currently being used and extended more widely other projects within PEPR.
Exploitation Route Users of PEPR are currently able to use the methodology in collaboration with PI Roessler. In the future, it is envisaged to make this methodology more widely applicable to PEPR users and beyond.
Sectors Chemicals,Energy,Environment

 
Description The capabilities at PEPR are also available to use by industry - local SMEs as well as major companies. PEPR has been and is involved in several industry projects and Syngenta is now co-funding two PhD project supervised by PEPR PI Roessler and that are making extensive use of the PEPR facility. Because many of the projects are under non-disclosure agreement details cannot be provided, but in all cases the research carried out at PEPR has led to further the goals of the respective companies.
First Year Of Impact 2021
Sector Agriculture, Food and Drink,Chemicals
Impact Types Societal,Economic

 
Description Spins and superconducting circuits for advanced spectroscopy (SpinSUPER)
Amount £1,063,137 (GBP)
Funding ID EP/W005794/1 
Organisation Engineering and Physical Sciences Research Council (EPSRC) 
Sector Public
Country United Kingdom
Start 08/2022 
End 08/2025
 
Description Synchronized Structure and Dynamics Investigations of Ionic Liquids by Pulse EPR
Amount £313,708 (GBP)
Funding ID RPG-2021-383 
Organisation The Leverhulme Trust 
Sector Charity/Non Profit
Country United Kingdom
Start 03/2022 
End 09/2024
 
Title In situ and operando electrochemical EPR spectroscopy 
Description With this methodology it is possible to monitor the evolution of radicals in real time during an electrochemical reaction, including electrocatalysis. 
Type Of Material Improvements to research infrastructure 
Year Produced 2023 
Provided To Others? No  
Impact The publication describing the method is currently under review. Impact is currently mainly in the form of conference dissemination and PI Roessler invited to discuss the technique at summer schools. 
 
Description Collaboration with Dr F. Mark Chadwick 
Organisation Imperial College London
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution The EPR measurements and the analysis/interpretation of some of the experimental results are performed at the PEPR facility.
Collaborator Contribution The Chadwick group synthesises the investigated metal complexes and aids with the interpretation of the spectroscopic results in the light of the properties of the studied molecules.
Impact 2 primary research articles (DOI: 10.1039/D2DT03291K and 10.26434/chemrxiv-2022-dndhp).
Start Year 2021
 
Description Collaboration with Dr Judy Hirst 
Organisation Medical Research Council (MRC)
Department MRC Mitochondrial Biology Unit
Country United Kingdom 
Sector Academic/University 
PI Contribution We are working in collaboration with the Hirst group in order to contribute to the elucidation of the mechanism of mitochondrial complex I through EPR spectroscopic methods.
Collaborator Contribution The Hirst group has contributed their extensive experience in working with bovine complex I, training members of my group to carry out the purification and thus enabling us to carry out the purification in house. We have also had access to unpublished work and benefited from the intellectual input to our publication.
Impact Judy Hirst and I have co-authored one review paper and another primary research article is submitted.
Start Year 2015
 
Description Collaboration with Dr Matthew Bidwell, Dr Ifan E. L. Stephens and Prof Magda Titirici 
Organisation Imperial College London
Department Department of Chemical Engineering
Country United Kingdom 
Sector Academic/University 
PI Contribution Measurements are being performed at the PEPR facility using its unique EPR film-spectroelectrochemical setup to investigate the properties of the system provided by the collaboration partners.
Collaborator Contribution The research partners provide the materials to be investigated and all the background knowledge required to perform the measurements.
Impact A primary research article is being currently drafted.
Start Year 2022
 
Description Collaboration with Dr Matthew Bidwell, Dr Ifan E. L. Stephens and Prof Magda Titirici 
Organisation Imperial College London
Department Department of Materials
Country United Kingdom 
Sector Academic/University 
PI Contribution Measurements are being performed at the PEPR facility using its unique EPR film-spectroelectrochemical setup to investigate the properties of the system provided by the collaboration partners.
Collaborator Contribution The research partners provide the materials to be investigated and all the background knowledge required to perform the measurements.
Impact A primary research article is being currently drafted.
Start Year 2022
 
Description Collaboration with Dr Rebecca Musgrave 
Organisation King's College London
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution The PEPR facility assists with the measurement and interpretation of EPR spectra; moreover, contributed to the EPR-related section of a joint publication draft.
Collaborator Contribution The Musgrave group synthesises the studied metal complexes and provides the required knowledge in the field of inorganic chemistry.
Impact The final draft of a primary research article is available.
Start Year 2022
 
Description Collaboration with Dr Rivka Isaacson 
Organisation King's College London
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution An EPR-based investigation is ongoing to characterise the change of the conformational space sampled by the homodimeric protein SGTA upon interaction with its binding partners. The input provided by the PEPR facility encompasses advising on how the research question can be addressed using EPR spectroscopy, performing and analysing the experimental measurements as well as devising a strategy to convert these results into a structural model. Moreover, the team at PEPR is assisting with writing the EPR-related sections of the research grants related to this collaboration.
Collaborator Contribution Dr Isaacson's research group is carrying forward the biology-related aspect of the collaboration, including the preparation of the samples to be analysed at the PEPR facility.
Impact Publication of a primary research article.
Start Year 2018
 
Description Collaboration with Prof Anthony Kucernak 
Organisation Imperial College London
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution Within the aim of understanding the speciation of Manganese during cycling of redox flow batteries, EPR measurements followed by the development of a data analysis protocol allowed to quantify the time-dependent concentration of Mn(II) species.
Collaborator Contribution The Kucernak group contributed their extensive knowledge in the field of battery electrochemistry to interpret the results of the EPR measurements.
Impact A primary research article is being currently drafted.
Start Year 2021
 
Description Collaboration with Prof Clare Grey 
Organisation University of Cambridge
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution The temperature-dependent electron spin relaxation behaviour of the samples provided by the Grey group is being investigated using pulse EPR spectroscopy; besides performing the measurements, support is provided with the analysis of the experimental traces to yield the temperature-dependent relaxation times.
Collaborator Contribution The Grey group provided the samples and performed the analysis of the temperature dependence of the relaxation times.
Impact A primary research article is being currently drafted.
Start Year 2021
 
Description Collaboration with Prof Erwin Reisner 
Organisation University of Cambridge
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution A spin-trapping EPR study has been proposed and performed to elucidate the mechanism of an electrooxidation reaction; besides running the measurements, the PEPR facility contributed scientific input by identifying the most suitable approach to detect the reaction intermediates using EPR spectroscopy.
Collaborator Contribution The Reisner group contributed specific knowledge on the studied system to interpret the results of the spin-trapping study within the more general context of the reaction mechanism under investigation.
Impact A primary research article has been published (DOI: 10.1021/acscatal.2c02689)
Start Year 2021
 
Description Collaboration with Prof Mark R. Crimmin 
Organisation Imperial College London
Department Department of Chemistry
Country United Kingdom 
Sector Academic/University 
PI Contribution Advanced pulse EPR measurements (e.g., hyperfine sublevel correlation spectroscopy, HYSCORE, using the standard sequence or enhanced variants) are being performed to characterise the structure and the electron distribution of the metal complexes provided by the Crimmin group. The PEPR facility contributes to this research project by proposing the most suitable spectroscopic approaches, performing the measurements and analysing the results; based on the experimental observations, modifications of the metal complexes (e.g., isotope labelling) are proposed to maximise the amount of information that can be obtained from the spectroscopic investigation.
Collaborator Contribution The Crimmin group synthesises the samples, characterises them (e.g., by X-ray diffraction and DFT calculations) and helps in the interpretation of the experimental results in the light of what is know about the structure and properties of the metal complexes under investigation.
Impact A primary research article is being currently drafted.
Start Year 2022
 
Description Collaboration with Prof Sandrine Heutz 
Organisation Imperial College London
Department Department of Materials
Country United Kingdom 
Sector Academic/University 
PI Contribution Pulse EPR measurements have been performed at the PEPR facility to investigate the electron spin relaxation properties of materials used for spintronic devices. The experiments have only been possible thanks to the unique high-sensitivity setup (HEMT cryogenic preamplifier) available at PEPR.
Collaborator Contribution The Heutz group provided the materials and interpreted the experimental results.
Impact A primary research article is being currently drafted.
Start Year 2021
 
Description Great Exhibition Road Festival 2022 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Public/other audiences
Results and Impact The Great Exhibition Road Festival 2022 was a 2-days event with contributions from many institutions from both academic and non-academic environments.
Overall, more than 30,000 visitors attended. The PEPR facility and the research group led by PEPR PI Maxie Roessler shared a stand and proposed activities targeted to different age groups, ranging from practical workshops for the youngest participants to an introduction of the research themes dealt with at the PEPR facility and the used methodology. The stand was visited by more than 1,000 people, most of which engaged with us and asked questions about our work and research.
Year(s) Of Engagement Activity 2022
URL https://www.greatexhibitionroadfestival.co.uk
 
Description PEPR Launch Event 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach International
Primary Audience Postgraduate students
Results and Impact PEPR's launch was a hybrid online and in-person event aimed at showcasing the wide range of challenges that can be tackled with (pulse) electron paramagnetic resonance (EPR) spectroscopy and illustrating the unique capabilities and vision of the newly established research facility.
The programme featured short scientific talks given by PEPR's co-investigators and internationally leading EPR spectroscopists demonstrating applications of EPR in the research fields of Chemistry & Catalysis, Energy & Environment, Materials and Biology; short talks were delivered as well by industrial partners and funders.
The event gathered an audience of over 100 attendees and included opportunities for networking, among which the possibility to attend tours of the research facility laboratory and a drinks reception.
Year(s) Of Engagement Activity 2021
URL https://www.imperial.ac.uk/news/230915/facility-launched-study-complex-molecules-materials/
 
Description White City Ecosystem Events 2023 
Form Of Engagement Activity Participation in an activity, workshop or similar
Part Of Official Scheme? No
Geographic Reach Regional
Primary Audience Industry/Business
Results and Impact Two events took place at the beginning of 2023: the I-HUB Ecosystem Fair and the Jawdrop Life Sciences summit.
- The I-HUB Ecosystem Fair aimed at showcasing the services available to businesses working at Imperial College London's Translation & Innovation Hub (I-HUB). The PEPR Facility was part of the "Access to Equipment" table and presented its services to local SMEs; this interaction resulted in information exchange and the creation of potential collaborations.
- The Jawdrop Life Sciences summit aimed at bringing together leading scientists, tech specialists, researchers and decision-makers from across the White City area in London and beyond. The PEPR Facility was present at the Technology Showcase Event, taking place over lunch, and discussed with the attendees possible applications of (pulsed) electron paramangetic resonance to biology-related questions.
Year(s) Of Engagement Activity 2023
URL https://www.whitecityinnovationdistrict.org.uk/jawdrop-summit/