Using topological design to develop defect-rich graphene-based substrates for single-atom catalysis

• Applicant: Dr. Benedikt P. Klein
• Subject Area: Physical Chemistry of Solids and Surfaces, Material Characterisation ; Theoretical Chemistry: Molecules, Materials, Surfaces
• Term: from 2020 to 2024
• Project identifier: Deutsche Forschungsgemeinschaft (DFG) - Project number 453278757

This proposal presents a unique joint experimental and theoretical effort to design and test a novel defect-rich graphene-like carbon network as a substrate for single atom catalysis (SAC). SAC provides a pathway towards new reactivities and the more efficient use of precious metals in future catalysts, both necessary for the transition to a sustainable energy industry. The graphene-based network, central to the proposal, will be produced using a new bottom-up approach utilising topological design to circumvent most problems of regular on-surface synthesis. We will exploit the massively enhanced interaction of topologically non-alternant aromatic molecules towards metal surfaces. The use of such precursors enables the one-step preparation of a graphene-like layer by dehydrogenative coupling. This layer will contain a high concentration of topological defects, and, while lacking long range crystallinity, will provide uniform distribution of anchor sites for the single metal adatoms forming a SAC. The best precursor molecules will be chosen by theoretical pre-screening, while theoretical modelling of the catalytic activity will guide the choice of a suitable metal atom species to combine with the synthesised graphene-like substrate. The joint experimental and theoretical characterisation of both the graphene-like substrate and the produced SAC will involve advanced synchrotron spectroscopic and lab-based microscopic techniques, providing sub-Ångström resolution in structure determination and various spectroscopic data. The thereby obtained spectra will be interpreted with the help of DFT-based calculations, for which improved spectroscopy simulation methods will be developed. The produced SAC will be subjected to proof-of-principle experiments showing its catalytic activity for the low-temperature oxidation of CO.The applicant will perform experimental and theoretical work, which is expected to show benefits in both fields by way of synergetic effects in both planning and interpretation of experimental and theoretical data. The work will result in the production of a new class of graphene-based substrates for SAC. By this process, it will facilitate further research into a field critically important for the future of sustainable energy economics and with the potential of changing many industrially relevant processes on a fundamental level.During this project, the applicant will extend his portfolio of experimental methods by the addition of scanning tunnelling microscopy and advanced synchrotron based techniques, while simultaneously gaining experience in performing cutting-edge DFT-based spectroscopic simulations. The resulting uniquely broad skill set will enable him to forge an independent career at the interface between theory and experiment in the future, while at the same time creating a wide and long-lasting network of collaborators.

• DFG Programme: WBP Fellowship
• International Connection: United Kingdom
• Hosts: Dr. David A Duncan; Professor Dr. Reinhard Maurer, Ph.D.