Advancing Biotechnologies for Fuel Generation: Exploiting Transmembrane Cytochromes for Solar Energy Conversion
Lead Research Organisation:
University of Cambridge
Department Name: Chemistry
Abstract
Abstracts are not currently available in GtR for all funded research. This is normally because the abstract was not required at the time of proposal submission, but may be because it included sensitive information such as personal details.
Technical Summary
Most artificial homogeneous photosynthetic systems suffer a major drawback: a short-lived charge separated state, which is due to the failure to spatially decouple the reductive and the oxidative sites required to sustain charge separation. Inspired by membrane bilayers as Nature's solution to spatially decouple reduction and photoexcitation/oxidation, we propose to utilise synthetic biology to develop a novel approach that adopts the principles of natural photosynthesis; light harvesting, charge separation and catalysis. Our photocatalysts will exploit the outer-membrane spanning, cytochrome-based electron-transfer conduits produced naturally by Shewanella oneidensis MR-1. We will establish methods to attach photosensitisers, e.g., dye-sensitised TiO2 and CdS nanoparticles, to the external cytochrome of this conduit in a manner that allows for a rapid charge separation across the membrane creating a long-lived charge separated state. We will develop methods to deliver electrons from the internal face of the conduit to redox catalysts. As a proof-of-principle, the conduit will be coupled to hydrogen-evolving catalysts that will include a [NiFeSe]-hydrogenase, a synthetic cobaloxime catalyst that evolves hydrogen in pH neutral conditions, and colloidal platinum, well-known for its hydrogen evolving properties. Voltammetric and spectroscopic methods together with quantification of hydrogen evolution by gas-chromatography will define the solar conversion efficiencies, electron transfer rate and catalytic properties of these systems. Conditions will then be established to combine systems with the desired properties as hybrid photocatalysts in the bilayers of liposomes and also in S. oneidensis MR-1. Two methods will be employed to deliver the electrons required to sustain hydrogen evolution, sacrificial electron donors such as triethanolamine and electrodes. The latter is explored as it offers opportunities for simultaneous production of electricity.
Planned Impact
Societal impact
The aim of this project is to use biotechnological, biophysical, (bio)nanotechnological and synthetic biological approaches to study and exploit Shewenella sp. and Shewanella proteins. In particular, we aim to exploit Shewenalla sp. and their respiratory proteins to harvest solar energy and produce carbon-neutral fuels such as hydrogen. A renewable energy cycle is recognized as a top national strategic priority in the UK (UK White Paper on Energy). In the last 18 months, several incidents have demonstrated the fragility of the global energy supply: the sharp rise in oil prices following the outbreak of conflicts and civil wars in the Middle-East and the ecological and humanitarian threat of a nuclear meltdown in Fukushima, Japan. The search for alternative energy sources is therefore of major importance to THE GLOBAL SOCIETY. A solution to this problem has to be sought by combining a multitude of 'alternative' energy sources; this research will contribute to this progress.
A new academic partnership & training of new leaders in the energy sector
This project will establish a new academic partnership between Butt, Clarke, Richardson at Univ. East Anglia, Jeuken at Univ. Leeds and Reisner at Univ. Cambridge. The strong ties through this BBSRC project will allow us to form a nucleus around which future networks and collaborations will be built. Within this project we will also provide top-quality cross-disciplinary training for three BBSRC PDRAs, to provide expertise in the development of alternative energy biotechnologies, an area of critical scientific, technological and economic importance for the future.
Contribution to technology of alternative energy sources
Of particular interest for the studies proposed here are the multi-heme proteins in Shewanella which mediate electron transfer to the outside of the cell or to inorganic substrates. Shewanella serve as an important model system for mediator-less microbial fuel cells that run on waste carbon sources (such as in waste water) to produce electricity or hydrogen. Research into the electron transport of Shewanella will increase our understanding of their capabilities in microbial fuel cells. At this stage, these are basic research aims, with academic beneficiaries. However, after successful completion of this project, we propose that our work will contribute to the future design of such microbial fuel cells, in particular where future work aims to genetically of synthetically modifying the microbes to enhance electron transfer rates to the anode (i.e., increase electrical current). Furthermore, this BBSRC proposal explores a novel and innovative approach in which the natural electron transfer pathway is reversed. Instead of generating electricity by respiring hydrogen or a carbon source, we propose to use solar energy to produce hydrogen. Although the overall concept of this proposal is the harvesting of solar energy and the storage of energy (in the form of hydrogen), the fact that electricity can be used by microbes to make 'higher-energy' organic molecules, including hydrogen and a variety of hydrocarbons, is of major economic value. Microbes as catalysts are ideal as they relatively cheap to make and maintain (i.e., they grow and regenerate). This makes them ideal catalyst to synthesise organic molecules, such as formate, using electricity and CO2.
The aim of this project is to use biotechnological, biophysical, (bio)nanotechnological and synthetic biological approaches to study and exploit Shewenella sp. and Shewanella proteins. In particular, we aim to exploit Shewenalla sp. and their respiratory proteins to harvest solar energy and produce carbon-neutral fuels such as hydrogen. A renewable energy cycle is recognized as a top national strategic priority in the UK (UK White Paper on Energy). In the last 18 months, several incidents have demonstrated the fragility of the global energy supply: the sharp rise in oil prices following the outbreak of conflicts and civil wars in the Middle-East and the ecological and humanitarian threat of a nuclear meltdown in Fukushima, Japan. The search for alternative energy sources is therefore of major importance to THE GLOBAL SOCIETY. A solution to this problem has to be sought by combining a multitude of 'alternative' energy sources; this research will contribute to this progress.
A new academic partnership & training of new leaders in the energy sector
This project will establish a new academic partnership between Butt, Clarke, Richardson at Univ. East Anglia, Jeuken at Univ. Leeds and Reisner at Univ. Cambridge. The strong ties through this BBSRC project will allow us to form a nucleus around which future networks and collaborations will be built. Within this project we will also provide top-quality cross-disciplinary training for three BBSRC PDRAs, to provide expertise in the development of alternative energy biotechnologies, an area of critical scientific, technological and economic importance for the future.
Contribution to technology of alternative energy sources
Of particular interest for the studies proposed here are the multi-heme proteins in Shewanella which mediate electron transfer to the outside of the cell or to inorganic substrates. Shewanella serve as an important model system for mediator-less microbial fuel cells that run on waste carbon sources (such as in waste water) to produce electricity or hydrogen. Research into the electron transport of Shewanella will increase our understanding of their capabilities in microbial fuel cells. At this stage, these are basic research aims, with academic beneficiaries. However, after successful completion of this project, we propose that our work will contribute to the future design of such microbial fuel cells, in particular where future work aims to genetically of synthetically modifying the microbes to enhance electron transfer rates to the anode (i.e., increase electrical current). Furthermore, this BBSRC proposal explores a novel and innovative approach in which the natural electron transfer pathway is reversed. Instead of generating electricity by respiring hydrogen or a carbon source, we propose to use solar energy to produce hydrogen. Although the overall concept of this proposal is the harvesting of solar energy and the storage of energy (in the form of hydrogen), the fact that electricity can be used by microbes to make 'higher-energy' organic molecules, including hydrogen and a variety of hydrocarbons, is of major economic value. Microbes as catalysts are ideal as they relatively cheap to make and maintain (i.e., they grow and regenerate). This makes them ideal catalyst to synthesise organic molecules, such as formate, using electricity and CO2.
Organisations
People |
ORCID iD |
Erwin Reisner (Principal Investigator) |
Publications
Ainsworth EV
(2016)
Photoreduction of Shewanella oneidensis Extracellular Cytochromes by Organic Chromophores and Dye-Sensitized TiO2.
in Chembiochem : a European journal of chemical biology
Andrei V
(2020)
Bias-free solar syngas production by integrating a molecular cobalt catalyst with perovskite-BiVO4 tandems.
in Nature materials
Hutton GA
(2016)
Carbon Dots as Versatile Photosensitizers for Solar-Driven Catalysis with Redox Enzymes.
in Journal of the American Chemical Society
Hwang ET
(2015)
A Decaheme Cytochrome as a Molecular Electron Conduit in Dye-Sensitized Photoanodes.
in Advanced functional materials
Hwang ET
(2017)
Exploring Step-by-Step Assembly of Nanoparticle:Cytochrome Biohybrid Photoanodes.
in ChemElectroChem
Description | The grant allowed close collaboration with Lars Jeuken (Leeds), Julea Butt (Norwich) and Erwin Reisner (Cambridge) groups. During that collaboration, we could use a decaheme cytochrome (MtrC) from Shewanella oneidensis for different purposes on metal oxides (ITO) electrode surfaces. It enabled the efficient electronic wiring of redox enzymes, namely a hydrogenase (H2ase) and a fumarate reductase (FccA) for H2 electrooxidation and fumarate electroreduction respectively. Using spectroelectrochemistry we could show that the electronic communication between the electrode and enzyme remained efficient in the presence of an MtrC layer, showing the excellent ability of this electron transfer protein to shuttle electron from an electrode surface to an enzyme and vice versa. During this collaboration, we also found out that MtrC was capable of peroxidase activity. On electrode surface and in solution assay the protein was compared to the benchmark catalyst for hydrogen peroxide reduction Horseradish Peroxidase (HRP). In solution, the activity of MtrC remained lower than the natural catalyst HRP, however, once immobilised on electrode, MtrC showed a much higher electrocatalytic activity that was attributed to the excellent electronic wiring of MtrC, due to its 10 hemes. Spectroelectrochemistry (UV-vis and Raman) allowed to explained this unexpected activity by the presence of a heme owing a loosely bond histidine as 6th ligand creating the possibility for the heme to have a vacant space for the catalysis. The results of this award have contributed to the preparation of an ERC (MatEnSAP) and more recently a BBSRC grant (BB/S00159X/1). |
Exploitation Route | The findings from this project are currently researched further with funding from an ERC (MatEnSAP) and more recently a BBSRC grant (BB/S00159X/1). |
Sectors | Energy Environment |
URL | http://www-reisner.ch.cam.ac.uk/ |
Description | Contribution to the "Solar Fuels Vision Statement" |
Geographic Reach | National |
Policy Influence Type | Membership of a guideline committee |
Description | ECH2020 EUROPEAN RESEARCH COUNCIL - MATENSAP: Semi-artificial photosynthesis with wired enzymes |
Amount | € 1,715,252 (EUR) |
Funding ID | 682833 |
Organisation | European Research Council (ERC) |
Sector | Public |
Country | Belgium |
Start | 09/2016 |
End | 11/2021 |
Description | UKRI Circular Economy Approaches to Eliminate Plastic Waste - University of Cambridge |
Amount | £1,035,067 (GBP) |
Funding ID | EP/S025308/1 |
Organisation | Engineering and Physical Sciences Research Council (EPSRC) |
Sector | Public |
Country | United Kingdom |
Start | 01/2019 |
End | 06/2020 |
Title | Raw Data Supporting Article: Bias-free Solar Syngas Production by Integrating a Molecular Cobalt Catalyst with Perovskite-BiVO4 Tandems |
Description | |
Type Of Material | Database/Collection of data |
Year Produced | 2019 |
Provided To Others? | Yes |
URL | https://www.repository.cam.ac.uk/handle/1810/299205 |
Title | Raw data supporting publication: High Performance Reduction of H2O2 with an Electron Transport Decaheme Cytochrome on a Porous ITO Electrode |
Description | Raw Data supporting JACS publication: High Performance Reduction of H2O2 with an Electron Transport Decaheme Cytochrome on a Porous ITO Electrode |
Type Of Material | Database/Collection of data |
Year Produced | 2017 |
Provided To Others? | Yes |
Title | Research Data Supporting "Competing charge transfer pathways at the photosystem II-electrode interface" |
Description | Raw data and supplementary information supporting publication : 'Competing charge transfer pathways at the photosystem II-electrode interface' |
Type Of Material | Database/Collection of data |
Year Produced | 2016 |
Provided To Others? | Yes |
URL | https://www.repository.cam.ac.uk/handle/1810/256813 |
Title | Research data supporting "Carbon Dots as Versatile Photosensitizers for Solar-Driven Catalysis with Redox Enzymes" |
Description | Raw Data (e.g. NMR Messurements) supporting article: Carbon Dots as Versatile Photosensitizers for Solar-Driven Catalysis with Redox Enzymes |
Type Of Material | Database/Collection of data |
Year Produced | 2016 |
Provided To Others? | Yes |
Title | Research data supporting "Photoelectrochemical H2 Evolution with a Hydrogenase Immobilized on a TiO2-protected Silicon Electrode" |
Description | Experimental Raw data supporting publication: Photoelectrochemical H2 Evolution with a Hydrogenase Immobilized on a TiO2-protected Silicon Electrode |
Type Of Material | Database/Collection of data |
Year Produced | 2016 |
Provided To Others? | Yes |
URL | https://www.repository.cam.ac.uk/handle/1810/254578 |
Title | Research data supporting "Poly(cobaloxime)-carbon nanotube electrode: a freestanding buckypaper with polymer-enhanced H2 evolution performance" |
Description | Caractarisation and experimental data supporting publication: Poly(cobaloxime)-carbon nanotube electrode: a freestanding buckypaper with polymer-enhanced H2 evolution performance |
Type Of Material | Database/Collection of data |
Year Produced | 2016 |
Provided To Others? | Yes |
URL | https://www.repository.cam.ac.uk/handle/1810/253645 |
Description | 11th Hydrogen Conference, Marseille, France |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Plenary lecture |
Year(s) Of Engagement Activity | 2016 |
Description | 13th Nordic Photosynthesis Congress, Copenhagen, Denmark |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Plenary Talk The conference covered the following topics: • Structure and function of photosynthetic reaction centers and antennae complexes • Biogenesis of the photosynthetic membrane • Regulation and acclimation of photosynthesis • Synthetic biology and artificial photosynthesis • Evolution |
Year(s) Of Engagement Activity | 2016 |
Description | 5th National Symposium on Advances in Chemical Sciences. Amritsar, India |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Annual meeting of RSC and Chemical Research Society of India (CRSi) of about 10 researchers from both India and the UK |
Year(s) Of Engagement Activity | 2016 |
Description | Facebook account with information about the group |
Form Of Engagement Activity | Engagement focused website, blog or social media channel |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Other audiences |
Results and Impact | Facebook account with information about the group to make the wider public aware of research work done by the Reisner Group |
Year(s) Of Engagement Activity | 2013,2014,2015,2016 |
URL | https://www.facebook.com/ReisnerLab |
Description | Gordon Research Conference on Metallocofactors, Massachusetts, USA |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Postgraduate students |
Results and Impact | To provide a lecture in a session entitled Photosynthetic Cofactors in Biology at the kickoff Gordon Research Conference on the topic of Metallocofactors. There have been stimulating sessions on a range of topics (e.g., nitrogenase, CO-dehydrogenase, hydrogenases, PSII, etc..) Gordon Research Conferences provide an intimate setting to discuss the most recent and most exciting results in science |
Year(s) Of Engagement Activity | 2016 |
Description | Invited Lecture-29th Workshop on Quantum Solar Energy Conversion, Rauris, Austria |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Keynote Lecture at 29th Workshop on Quantum Solar Energy Conversion, Rauris, Austria. Knowledge transfer of experts on conversion of solar photons to electrical or chemical energy. |
Year(s) Of Engagement Activity | 2017 |
Description | Keynote Lecture at 14th International Symposium on Applied Bioinorganic Chemistry |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Keynote Lecture at the 14th International Symposium on Applied Bioinorganic Chemistry, Toulouse, France. |
Year(s) Of Engagement Activity | 2017 |
URL | https://isabc2017.sciencesconf.org/ |
Description | Keynote Lecture at XXIV International Symposium on Bioelectrochemistry and Bioenergetics, Lyon, France |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Keynote Lecture at XXIV Int. Symposium on Bioelectrochemistry and Bioenergetics, Lyon, France. Knowlege transfer on Bioelectrochemistry and Bioenergetics. |
Year(s) Of Engagement Activity | 2017 |
URL | http://www.bioelectrochemical-soc.org/general/meetings.php |
Description | Plenary Lecture - 'From Photosynthesis to solar fuels' symposium, College de France, Paris, France |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Prof. Reisner attended the 'From Photosynthesis to Solar Fuels' symposium as an invited pleanary speaker. The purpose was for knowledge exchange between PIs/researchers. |
Year(s) Of Engagement Activity | 2018 |
Description | Plenary Lecture - National meeting of the Norwegian Chemical Society, Lillestrøm, Norway |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Prof. Reisner attended the National Meeting of the Norwegian Chemical Society as an invited plenary speaker. The purpose was a knowledge exchange between PIs |
Year(s) Of Engagement Activity | 2018 |
Description | Plenary Lecture - XXV National Meeting of Portuguese Chemical Society, Lisbon, Portugal |
Form Of Engagement Activity | A talk or presentation |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Professional Practitioners |
Results and Impact | Plenary Lecture at XXV National Meeting of Portuguese Chemical Society, Lisbon, Portugal. |
Year(s) Of Engagement Activity | 2017 |
URL | http://xxvenspq.eventos.chemistry.pt/ |
Description | Twitter account for the Reisner Group |
Form Of Engagement Activity | Engagement focused website, blog or social media channel |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Other audiences |
Results and Impact | Twitter account to spread the news about the Reisner Group's work |
Year(s) Of Engagement Activity | 2014,2015,2016 |
URL | https://twitter.com/reisnerlab |
Description | Youtube Channel with Movies from the Reisner Group |
Form Of Engagement Activity | Engagement focused website, blog or social media channel |
Part Of Official Scheme? | No |
Geographic Reach | International |
Primary Audience | Other audiences |
Results and Impact | Presenting short video's about the Reisner Group's Research work on youtube to make the wider public aware of the work and research of the group |
Year(s) Of Engagement Activity | 2013,2014,2015,2016 |
URL | https://www.youtube.com/user/reisnerlab |