The goal of this partnership is to create new catalysts for chemical reactions that are sustainable and help produce important chemicals and intermediates. Catalysts are essential substances that make chemical reactions happen more efficiently, and they are fundamental to many of the key processes that support our modern society. Without effective catalysts, many of the products and processes that we rely on would not be possible. At present, the chemical industry primarily uses fossil carbon sources like natural gas, oil, and coal. However, this approach is not sustainable in the long term, and it contributes to climate change and other environmental problems. As a result, researchers are looking for new ways to make chemicals that rely on green and sustainable carbon sources. Acetylene is one such molecule that has the potential to be an essential intermediate for a sustainable chemical industry. Acetylene chemistry was well developed over a century ago, but it was displaced as a central chemical intermediate by readily available ethene derived from oil. As a result, acetylene chemistry is currently an underexplored field. However, it is possible to produce acetylene from methane, which from biogas is a renewable source of carbon. Therefore, acetylene could become a crucial central intermediate for a new green chemical industry. We aim to design and understand catalysts based on Au, Pt, and AuPt that will act as a new class of catalysts to produce key chemicals and intermediates from acetylene. The partnership will bring together world-leading and complementary catalysis expertise, with the Cardiff Catalysis Institute (CCI collaborating with the UK Catalysis Hub (Harwell), the Max Planck Institute fur Kohlenforschung (KOFO, Mulheim), the Instituto de Tecnologia Quimica (ITQ), and the Fritz-Haber-Institute of the Max Planck Society (FHI, Berlin). A key benefit of this partnership is the additionality that it provides. By pooling expertise and resources, researchers can tackle grand challenge problems more effectively. The collaborative project brings together centres with unique and crucial expertise, such as the high-pressure facilities for acetylene catalysis at MPI KOFO, the fundamental surface science and advanced characterization techniques available at Harwell and FHI, the advanced computational methodologies of the FHI and the synthetic expertise concerning nanoparticles of ITQ. This partnership will enable UK researchers to access this expertise and cutting-edge facilities to tackle the complex challenge of making and characterizing new catalysts. The research will focus on gaining a fundamental understanding of what controls the activity of these catalysts in specific reactions, such as acetylene hydrochlorination and acetylene hydrogenation. Supported Au and Pt catalysts display a range of morphologies and often have individual atoms/cations, clusters, and nanoparticles. In some reactions, it is the well-dispersed Au+ cations that are active, while in others, nanoparticles are active. The research will seek to gain a deeper understanding of what controls the activity in these reactions and use this knowledge to design new and improved catalysts. To achieve these goals, we will use in situ/operando techniques and complementary capabilities available through the partnership to study these new catalysts. The team of experts assembled has worked together previously in various combinations, which will facilitate effective collaboration and communication. The ultimate goal of this partnership is to create new catalysts that will enable the sustainable production of important chemicals and intermediates, contributing to the development of a more sustainable and environmentally friendly chemical industry.

The Cardiff Catalysis Institute, UK Catalysis Hub, Netherlands Centre for Multiscale Catalytic Energy Conversion (MCEC, Utrecht), and the Fritz-Haber-Institute of the Max Planck Society (FHI, Berlin) will use a novel theory-led approach to the design of new trimetallic nanoparticle catalysts. Supported metal nanoparticles have unique and fascinating physical and chemical properties that lead to wide ranging applications. A nanoparticle, by definition, has a diameter in the range one to one hundred nanometres. For such small structures, particularly towards the lower end of the size range, every atom can count as the properties of the nanoparticle can be changed upon the addition or removal of just a few atoms. Thus, properties of metal nanoparticles can be tuned by changing their size (number of atoms), morphology (shape) and composition (atom types and stoichiometry, i.e., including elemental metals, pure compounds, solid solutions, and metal alloys) as well as the choice of the support used as a carrier for the nanoparticle. The constituent atoms of a nanoparticle that are either part of, or are near the surface, can be exposed to light, electrons and X-rays for characterisation, and this is the region where reactions occur. Our lead application will be catalysis, which is a strategic worldwide industry of huge importance to the UK and global economy. Many catalysts comprise supported metal nanoparticles and this is now a rapidly growing field of catalysis. Metallic NPs already have widespread uses e.g., in improving hydrogen fuel cells and biomass reactors for energy generation, and in reducing harmful exhaust pollutants from automobile engines. Many traditional catalysts contain significant amounts of expensive precious metals, the use of which can be dramatically reduced by designing new multi-element nanocatalysts that can be tuned to improve catalytic activity, selectivity, and lifetime, and to reduce process and materials costs. A major global challenge in the field of nanocatalysis is to find a route to design and fabricate nanocatalysts in a rational, reproducible and robust way, thus making them more amenable for commercial applications. Currently, most supported metal nanocatalysts comprise one or at most two metals as alloys, but this project seeks to explore more complex structures using trimetallics as we now have proof-of-concept studies which show that the introduction of just a small amount of a third metal can markedly enhance catalytic performance. We aim to use theory to predict the structures and reactivities of multi-metallic NPs and to validate these numerical simulations by their synthesis and experimental characterisation (e.g., using electron microscopy and X-ray spectroscopy), particularly using in-situ methodologies and catalytic testing on a reaction of immense current importance; namely the hydrogenation of carbon dioxide to produce liquid transportation fuels. The programme is set out so that the experimental validation will provide feedback into the theoretical studies leading to the design of greatly improved catalysts. The use of theory to drive catalyst design is a novel feature of this proposal and we consider that theoretical methods are now sufficiently well developed and tested to be able to ensure theory-led catalyst design can be achieved. To achieve these ambitious aims, we have assembled a team of international experts to tackle this key area who have a track record of successful collaboration. The research centres in this proposal have complementary expertise that will allow for the study of a new class of complex heterogeneous catalysts, namely trimetallic alloys. The award of this Centre-to-Centre grant will place the UK at the forefront of international catalytic research.

The Centre for Doctoral Training in "Molecular Modelling and Materials Science" (M3S CDT) at University College London (UCL) will deliver to its students a comprehensive and integrated training programme in computational and experimental materials science to produce skilled researchers with experience and appreciation of industrially important applications. As structural and physico-chemical processes at the molecular level largely determine the macroscopic properties of any material, quantitative research into this nano-scale behaviour is crucially important to the design and engineering of complex functional materials. The M3S CDT offers a highly multi-disciplinary 4-year doctoral programme, which works in partnership with a large base of industrial and external sponsors on a variety of projects. The four main research themes within the Centre are 1) Energy Materials; 2) Catalysis; 3) Healthcare Materials; and 4) 'Smart' Nano-Materials, which will be underpinned by an extensive training and research programme in (i) Software Development together with the Hartree Centre, Daresbury, and (ii) Materials Characterisation techniques, employing Central Facilities in partnership with ISIS and Diamond. Students at the M3S CDT follow a tailor-made taught programme of specialist technical courses, professionally accredited project management courses and generic skills training, which ensures that whatever their first degree, on completion all students will have obtained thorough technical schooling, training in innovation and entrepreneurship and managerial and transferable skills, as well as a challenging doctoral research degree. Spending >50% of their time on site with external sponsors, the students gain first-hand experience of the demanding research environment of a competitive industry or (inter)national lab. The global and national importance of an integrated computational and experimental approach to the Materials Sciences, as promoted by our Centre, has been highlighted in a number of policy documents, including the US Materials Genome Initiative and European Science Foundation's Materials Science and Engineering Expert Committee position paper on Computational Techniques, Methods and Materials Design. Materials Science research in the UK plays a key role within all of the 8 Future Technologies, identified by Science Minister David Willetts to help the UK acquire long-term sustainable economic growth. Materials research in UCL is particularly well developed, with a thriving Centre for Materials Research, a Materials Chemistry Centre and a new Centre for Materials Discovery (2013) with a remit to build close research links with the Catalysis Technology Hub at the Harwell Research Complex and the prestigious Francis Crick Institute for biomedical research (opening in 2015). The M3S will work closely with these centres and its academic and industrial supervisors are already heavily involved with and/or located at the Harwell Research Complex, whereas a number of recent joint appointments with the Francis Crick Institute will boost the M3S's already strong link with biomedicine. Moreover, UCL has perhaps the largest concentration of computational materials scientists in the UK, if not the world, who interact through the London-wide Thomas Young Centre for the Theory and Simulation of Materials. As such, UCL has a large team of well over 100 research-active academic staff available to supervise research projects, ensuring that all external partners can team up with an academic in a relevant research field to form a supervisory team to work with the Centre students. The success of the existing M3S CDT and the obvious potential to widen its research remit and industrial partnerships into topical new materials science areas, which lie at the heart of EPSRC's strategic funding priorities and address national skills gaps, has led to this proposal for the funding of 5 annual student cohorts in the new phase of the Centre.