Clean and sustainable hydrogen will have a major impact in the future of several sectors of our economy - from industrial processes (e.g. steel and concrete manufacturing), domestic and industrial heating, to the transportation sector (e.g. fuel cells and combustion engines), hydrogen offers many pathways to decarbonisation. This has been clearly articulated recently in the UK Government's Hydrogen Strategy. However, to enable hydrogen to fulfil its potential, it must be produced by renewable power, without carbon-emissions. Splitting water into hydrogen and oxygen with electricity (electrolysis) is one of the most promising technologies to meet this challenge. Indeed, commercialised electrolysers exist today that generate "green" hydrogen at industrially relevant scales. However, to date, 96% of hydrogen is produced from fossil fuel derived processes resulting in carbon-emissions. While a portfolio of electrolyser technologies will likely play important roles in the long term, proton exchange membrane electrolysers (PEM-ELs) are widely anticipated to provide the base capacity in the short and medium term. Despite this expectation, the high cost of green hydrogen from PEM-EL is a major barrier. PEM-ELs today require precious and scarce iridium and platinum-based catalysts. Indeed, technoeconomic analyses show that when manufactured at scale, the PEM-EL stack is the most expensive component of the electrolyser, and the anode electrodes (iridium catalyst and transport layers) will account for the majority of the stack cost. Diversification of catalyst composition (i.e. to move away from pure iridium catalysts) thus, represents a substantial opportunity that could enable significant growth in green hydrogen generation using PEM-Els. This proposal offers a novel and unified strategy to develop synthetic methods and utilise advanced materials characterisations to feed-forward into the design of reduced iridium-content catalysts. We will explore our electrocatalysts through a translational approach, from "model system" thin films, to nanopowdered studies and commercially relevant testing, providing insight into which properties (conductivity, intrinsic activity, durability) dictate and control catalyst performance across these different testing beds. Furthermore, our synthesis methods, including co-sputtering from multi-magnetron systems will enable precision and great flexibility in catalyst composition. Working with our industrial partner, Johnson Matthey, the most active nanopowder catalysts will be benchmarked against commercial materials using industrial testing protocols. Throughout the project, we will leverage an array of advanced materials characterisation techniques to correlate structural and chemical properties to the catalyst performance, mimicking the operating conditions within a working electrolyser. In summary, the proposed work herein will implement catalysts with nanometer precision, uncovering design strategies and characterising catalysts under operating conditions and therefore accelerating the development of cost-effective catalysts for sustainable hydrogen production.

The combination of computer simulation with experiment is fundamental to achieving new understanding in chemistry, and to delivering advances that can address the most pressing societal challenges. The integration of computer simulation into research across the chemical sciences has been accelerated by the accessibility of high-performance computing infrastructure and tailored software that can harness the distributed architectures. New materials and chemical processes can be predicted by models of atoms and electrons using this infrastructure, with periodic density functional theory (DFT) at the forefront of the field of applied materials simulation. However, the efficacy of these modelling paradigms is proportional to the degrees of freedom in the system, which means that big models with lots of electrons, such as when considering catalytic processes, become very expensive to simulate. To address these shortcomings, this Fellowship looks to improve the capability and accessibility of methods that can provide high-level accuracy for electronic structure simulations, necessary for bond-breaking or bond-forming reactions, with reduced degrees of freedom, which means simulations can be performed quicker. This Fellowship is delivering new multiscale modelling paradigms, and the aim of this renewal is to make these paradigms more accessible through easier to use frameworks, and to extend our capabilities by integrating new machine-learning models into the simulation workflow, with the potential for acceleration in accurately resolving aspects of the system wavefunction. The new capabilities will continue to be developed in internationally leading software packages (FHI-aims, ChemShell) with collaborative partners distributed globally in academia and government research laboratories. The Fellowship will simultaneously look to demonstrate the potential of these new methods, with aims to resolve key mechanistic aspects of the synthesis of renewable fuel in collaboration with experimental partners in academia, notably at the host institution (Cardiff Catalysis Institute, Cardiff University) and via collaborations through the UK Catalysis Hub, as well as industry (Johnson Matthey, bp). The Fellowship aims to provide new knowledge of how the catalytic active site structure defines reactivity and selectivity in processes relating to photo- and electro-catalytic H2 generation; and also to explore how the structure of support materials influences thermally driven catalytic transformation of waste to sustainable aviation fuel. Finally, the Fellowship has complementary aims to support the transition of the research team from emergent researchers to influential and authoritative research leaders who can support the development of both new research domains and the next generation of researchers. The research team will be supported in developing, practising, and reflecting on their leadership activities, so they can deliver lasting impact in their sphere of influence.

The increasing threat posed by climate change has made energy storage more important than ever before. Lithium-ion batteries (LIB) have revolutionised portable electronics and have growing impact in electric vehicles. This success is due to their high energy densities which permit small light batteries to power increasingly small and complicated electronic devices. However, new generations of battery materials are required which combine high energy and power densities with low cost and high safety, for applications such as electric vehicles or static energy storage. The need to reduce CO2 emissions prioritises the use of renewable energy sources as opposed to the burning of fossil fuels. The intermittent nature of these renewable energy sources and the need to match supply with demand requires the storage of excess energy generated at peak production so that it may be released at times of peak demand. Electrochemical energy storage represents one of the more attractive solutions to this challenge. Polyoxyanion compounds are receiving considerable interest as alternative cathodes to conventional oxides. The strong binding of the oxygen in polyoxyanions enhances stability and thus safety, compared with layered transition metal oxides and raises the voltage via the inductive effect. The aim of this work is to investigate new polyanion systems, particularly oxalates, including the incorporation of highly electronegative fluorine which is beneficial for improving the electrochemical performance and raising the voltage. In a particularly exciting development, our preliminary studies indicate that in addition to conventional transition metal redox activity, the oxalate group itself may show redox behaviour. By employing a combination of experimental and computational techniques we will be able to obtain a fuller understanding of these materials and develop them towards possible application. In order to achieve this we have assembled a strong team of collaborators. These include academic partners for both computational (DFT) and experimental (Mossbauer and X-ray absorption spectroscopy) studies, together with industrial support from Faradion and Johnson Matthey. Our approach will maximise the opportunity to combine transition metal and oxalate redox and thereby obtain higher capacities, beyond the conventional metal-only redox activity.

This user-need CDT will equip graduates with the skills needed by the UK formulation industry to manufacture the next generation of formulated products at net zero, addressing the decarbonisation needs for the sector and aligning with this EPSRC priority. Formulated products, including foods, battery electrodes, pharmaceuticals, paints, catalysts, structured ceramics, thin films and coatings, cosmetics, detergents and agrochemicals, are central to UK prosperity (sector size > £95bn GVA in 2021) and Formulation Engineering is concerned with the design and manufacture of these products whose effectiveness is determined by the microstructure of the material. Containing complex soft materials: structured solids, soft solids or structured liquids, whose nano- to micro-scale physical and chemical structures are highly process dependent and critical to product function, their manufacture poses common challenges across different industry sectors. Moving towards Net Zero manufacture thus needs systems thinking underpinned by interdisciplinary understanding of chemistry, processing and materials science pioneered by the CDT for Formulation Engineering at the University of Birmingham over the past twenty years, with a proven delivery of industrial impact evidenced by our partner's letters of support and three Impact Case Studies ranked at 4* in the recent Research Excellence Framework in 2021. A new CDT strategy has been co-created with our industry partners, where we address new user-led research challenges through our theme of Formulation for Net Zero ('FFN0), articulated in two research areas: 'Manufacturing Net Zero (MN0)', and 'Towards 4.0rmulation'. Formulation engineering is not taught in first degree courses, so training is needed to develop the future leaders in this area. This was the industry need that led to the creation of the CDT in Formulation Engineering, based within the School of Chemical Engineering at Birmingham. The CDT leads the field: we won for the University one of the 2011 Diamond Jubilee Queen's Anniversary Prizes, demonstrating the highest national excellence. The UK is a world-leader in Formulation; many multinational formulation companies base research and manufacture in the UK, and the supply of trained graduates, and open innovation research partnerships facilitated by the CDT are critical to their success. The CDT receives significant industry funding (>£650k pa), supported by 31 industry partners including multinationals: P&G, Colgate, Unilever, Diageo, Devro, Fonterra, Samworth Bros., Jacobs Douwe Egberts, Nestle, Pepsico, Mondelez, GSK, AZ, Lonza, Novartis, BMS, BASF, Celanese, Croda, Innospec, Linde/BOC, Origen, Imerys, Johnson Matthey, Rolls-Royce/HTRC, JLR Lucideon and SMEs: Aquapak, CALGAVIN and ITS/StreamSensing. Intra and cross cohort training is central to our strategy, through our taught programme and twice-yearly internal conferences, industry partner-led regional research meetings, student-led technical and soft skills workshops and social events and inter CDT meetings. We have embedded diversity and inclusion into all of our projects and processes, including blind CV recruitment. Since 2018 our cohorts have been > 50% female and >35% BAME. We will co-create training and research partnerships with other CDTs, Catapult Centres, and industry, and train at least 50 EngD and PhD graduates with the skills needed to enhance the UK's leading international position in this critical area. The taught programme delivers a common foundation in formulation engineering, specialist technical training, modules on business, entrepreneurship and soft skills including a course in Responsible Research in Formulation. We have obtained promises of significant industry and University funding, with 67 offers of projects already. EPSRC costs will be 44% of the cash total for the CDT, and ca. £27% of the whole cost when industry in-kind funding is included.

Hydrogen will play a central role in the clean economy and in meeting ambitious climate targets. However, to realise its full potential, we must enable low cost, widespread production of zero-carbon H2 by water electrolysis, powered using renewable energy. Underlying this challenge is improved understanding of these complex systems from atoms to cells under real world operating conditions. AMPERE brings together experts from academia, national laboratories and industry to diagnose and understand degradation and performance-limiting processes in electrolysers. Crucially, this project will address the effects of system dynamics, a key but often overlooked aspect of operation when using intermittent energy sources such as solar and wind. We will leverage a unique toolbox of state-of-the-art measurement techniques, spanning length scales from ionic motion in the polymer membrane, to local electrochemical activity across electrode assemblies, water management and bubble formation. This will produce the definitive picture of multi-scale electrolyser dynamics and our focus on realistic production rates and in-situ/operando methods will ensure these insights will have practical relevance. Thus, the outputs of AMPERE will help usher in zero-carbon H2 at scale, as a chemical feedstock and energy vector for clean power generation, heating and transportation.