Catalysis underpins the £3,500B/year global chemical industry, enabling new routes to synthesising new antibiotics, removing air pollution from the air we breathe, or turning industrial waste into useful products such as plastics. In short, without catalysis, many of the products, drugs, fuels and materials we take for granted would simply not exist. Unfortunately, the design of new catalysts with targeted properties remains an enormous challenge to industry and academia. The key reason is complexity; contemporary heterogeneous and nanoparticle catalysts can exhibit a mind-boggling range of reaction sites and pathways, and catalyst activity can depend (often in an ill-defined manner) on a wide range of features such as structure, composition, support interactions, temperature, pressure, reactant phase constituents, and by-product poisoning. This enormous chemical complexity is a direct barrier to the traditional trial-and-error synthetic approaches to catalyst design used the world over. But, what if we could teach computers to automatically design new, better, catalytic species instead? This would have a transformative impact on catalysis research, both in academia and industry; using computers to accurately predict the optimal catalyst for a reaction would cut down time wasted in trial-and-error synthesis, accelerate catalyst discovery and improve sustainability. However, automated computational design of catalysts has proven elusive to date; again, the same issue of chemical complexity which dogs experimental catalyst design similarly hinders computational methods. This project aims to change this situation, pushing us towards development of a "black box" strategy for computational catalyst design. Specifically, we will begin to address this challenge using path-constrained molecular dynamics (PCMD), a new computational approach developed recently by the PI. PCMD is a connectivity-driven sampling strategy which enables rapid generation of reaction paths connecting large numbers of different chemical species; combined with quantum-chemical calculations of reaction rates and kinetic modelling, PCMD underpins a hierarchical strategy which can predict trends in rate laws, selectivities and product yields arising as a result of changes to catalyst features. To the best of our knowledge, PCMD was the first automated "black box" strategy shown capable of predicting the emergent mechanism and rate law of complex catalytic transformations such as alkene hydroformylation. In the first industrial application of PCMD, we will seek to generate new insights into the reactive chemistry of nanoparticle and heterogeneous catalytic systems for exhaust emissions control. In collaboration with Johnson Matthey, a world-leader in emissions control technologies, we will use PCMD to develop a 'roadmap' of reaction mechanisms, thermodynamics and kinetics of key exhaust gas reactions on nanoparticle and heterogeneous catalysts, specifically carbon monoxide oxidation and nitrogen oxide reduction on metallic nanoparticles and in Cu-promoted zeolites. In addition, building new collaborations with Warwick Data Science Institute and The Alan Turing Institute, we will apply 'big data' statistical analyses of the (potentially enormous) reaction-path datasets generation by PCMD; this leads to the new concept of reaction-path data mining (RDM), which will transform reaction-path datasets into tangible insights and descriptors of catalyst function. Overall, our PCMD/RDM strategy represents a new direction for computational catalysis; by dramatically accelerating the development and application of this strategy, this project will be a critical milestone towards our ultimate long-term goal, namely the "black box" computational design of new catalysts, molecular and other functional chemical systems.

This is an extension of the original Fellowship "Spectroscopy-driven design of an efficient photocatalyst for CO2 reduction" There is sufficient solar energy incident on the UK to provide for all of our energy needs. However the insolation level varies hugely both within a day and on a seasonal level. For any energy technology to be viable it is essential that it is reliable. A route to overcoming the intermittency of supply issue is to use the solar energy to drive the production of a chemical fuel which can be stored and transported to be available when and where it is needed. Sustainable carbon-based solar fuels and feedstocks (e.g. CH4, CH3OH, CO) can be produced by the coupling of light driven water oxidation to the reduction of CO2. This is an exciting prospect but to realise the goal of low carbon-intensity fuel economy breakthroughs are required for both fuel generation and utilisation systems. Current materials for CO2 reduction and water oxidation do not achieve the required level of efficiency and stability at a viable cost. Similarly the most promising clean technologies for electricity generation on demand from carbon fuels, fuel cells, often suffer from relatively low efficiencies and intolerances to impurities in the fuel feed. The original fellowship has been highly successful in delivering new low-cost catalysts that can either be driven directly by sunlight (photocatalysts) or indirectly using electrical energy (which could in principle come from a PV panel) to reduce CO2 to CO, an important liquid fuel precursor. Part of the original fellowship developed new capabilities within the UK for a highly sensitive surface sensitive spectroscopy, IR-Vis Sum Frequency Generation Spectroscopy. This experiment has been used to identify with an incredible level of detail the mechanisms of catalysts at surfaces. These, and our wider spectroscopic studies, have been critical in guiding our own catalyst design programme. But the need for mechanistic insights extends beyond our own synthetic programme. A lack of understanding of the mechanisms of catalysis occurring on the surface of electrodes and photoelectrodes is a limiting factor for the entire field preventing the rational development of new materials. Therefore our spectroscopy driven programme will be expanded to address both the crucial reactions of fuel generation (water oxidation and CO2 reduction) as well as to fuel utilisation chemistry, through the study of state of the art metal-oxide fuel cells. The project is ambitious, aiming not just to provide the first identification of all key intermediates during water oxidation on the most commonly studied photoelectrode (hematite), but also to explore how secondary interactions with water and electrolyte salts control the activity. A similar level of mechanistic detail is also sought from leading CO2 reduction catalysts and fuel cell electrodes. This level of mechanistic detail that we aim to deliver could be transformative to our own, collaborators and the wider communities programmes of material development. The delivery of scalable, efficient materials for solar fuels production and utilisation is a challenging goal but the potential impact is enormous. An improved understanding of surface mechanisms on current materials would represent an important step towards this ambition.

Adopting the Committee on Climate Change's recommendation to net zero emissions by 2050 demonstrates a clear commitment to leadership in the face of climate emergency. If this is to be achieved, decarbonising the industrial sector represents a critical challenge. However, at present, decarbonisation solutions are not economically competitive. It is critical to the UK's international competitiveness that this is underpinned by implementation of world-leading innovation, and therefore, ensuring research and innovation communities work together for timely industrial implementation. This project focuses on engaging academia, industry, policymakers and other stakeholders to develop an interdisciplinary consortium and subsequent proposal for the Industrial Decarbonisation Research and Innovation Centre (IDRIC). I will facilitate collaboration between researchers to foster co-creation of new interdisciplinary research and innovation programmes. The transformative innovation proposed here will be developed to address head on complex social and environmental challenges and contribute to low-cost transitions to new socio-technical systems. The Centre's agenda will be shaped initially by consultations, as well as network analysis, mapping and market analysis. Collaborative events and virtual environments will develop the co-creation of the cross-cutting challenges. I will embed EDI principles in the design of the Centre's engagement strategy.

Platinum group metals (PGMs) are exceptionally rare, high value metals that have important roles in electronics and industrial goods. One-quarter of all manufactured goods either contain a platinum group metal, or require a platinum group metal during the production process. The PGMs are extremely costly to produce, with the majority of PGM mining production in South Africa and Russia. The high price and low abundance of PGMs in natural environments means that recycling from waste electronic and industrial devices is a potentially economically viable mechanism to return valuable materials back into usage as part of a circular economy. Bacteria have the potential to recover PGMs from waste streams, as they can transform metals into different states using electrons that are released by the bacteria during metabolism. Adding electrons to a metal is a process known as reduction and changes the properties of the metal, causing it to aggregate into a solid mass known as a nanoparticle. Nanoparticles can be used as catalysts in important industrial reactions and are a valuable product in themselves. Often metal reduction processes happen inside the bacterium, which limits the size of the nanoparticle and can harm the cell, limiting its ability to survive. However, some bacteria can reduce metals on the surface of the cell, through a process known as Extracellular Electron Transfer (EET). This is adventitious as it makes the nanoparticles easier to harvest while not interfering with the internal metabolism of the cell or limiting the size of the nanoparticle. The bacterial family known as Shewanella are used for studies on PGM reduction because their surfaces are coated with proteins known as cytochromes, which makes them highly efficient at EET and metal reduction. The cytochromes that coat Shewanella can be grouped into four different clades, and these four groups have shown varying affinities for different metals suggesting that the overall specificity of Shewanella for different metals can be tuned depending on the types of cytochrome expressed on the cell surface. In this project we aim to extensively characterise the different interactions between these cell surface cytochromes and PGMs, specifically the metals iridium, platinum and palladium. These high value metals are present at low concentrations in waste effluent produced during the recycling of electronic devices. Our proposal aims to identify how soluble PGM interact with the different cytochromes (Objective 1), and understand how these interactions lead to the formation of nanoparticles in different waste streams (Objective 2). We will also use these findings to maximise PGM recovery from industrial waste streams (Objective 3). In Objective 1 we will determine where and how these precious metals associate to the different cytochrome. This will be achieved by first measuring the rate of electron exchange between cytochrome and PGMs at different metal concentrations. Objective 2 will use techniques developed in our laboratory to study these cell surface cytochromes. A light sensitive chemical bound to the cytochrome provides a continuous supply of electrons into the cytochrome. This will be used to study the different stages of PGM reduction on the cytochrome surface and study for the first time the initial steps of nanoparticle formation. We will also use synthetic membrane systems called vesicles to reduce the cytochromes and use these to explore the mechanism of formation of larger PGM nanoparticles. Finally in objective 3 we will use Shewanella cells optimised for enhanced cytochrome expression to improve the reduction and recovery of specific PGMs in different metal mixtures. These research objectives will show how Shewanella cytochromes can be used to capture different PGMs, and provide routes for further research around improving specificity as well as engineering systems for use in recovering metals from different waste streams.

One of the major current scientific and technological challenges concerns the conversion of carbon dioxide to fuels and useful products in effective and economically viable manner. This proposal responds to the major challenge of developing low energy routes to convert carbon dioxide to fuels and useful chemicals. The project has the following four main strands: (i) The use of electricity generated by renewable technologies to reduce CO2 electrocatalytically, where we will develop new approaches involving the use of ionic liquid solvents to activate the CO2 (ii) The use of hydrogen in the catalytic reduction of CO2, where we will apply computational procedures to predict new materials for this key catalytic process and subsequently test them experimentally (iii) The development of new materials for use in the efficient solar generation of hydrogen which will provide the reductant for the catalytic CO2 reduction (iv) A detailed life cycle analysis which will assess the extent to which the new technology achieves the overall objective of developing low carbon fuels. Our approach aims, therefore, to exploit renewably generated energy directly via the electrocatalytic route or indirectly via the solar generated hydrogen in CO2 utilisation for the formation of fuels and/or chemicals. The different components of the approach will be fully integrated to achieve coherent, new low energy technologies for this key process, while the rigorous life-cycle analysis will ensure that it satisfies the need for a low energy technology.