University: University of Southampton
University Supervisor: Prof. Simon J. Coles
University Group: Chemistry
Diamond Group: Beamline I19
Reactivity between solids and gases is the basis of many important chemical and catalytic processes, with numerous examples of structures at, before or after reaction determined to high levels of precision, providing new insights into important processes such as adsorption of small molecules in porous materials, e.g. methane, hydrogen. However, direct, mechanistic insight into the intermediates in catalytic processes is challenging as currently deployed, because the technique acquires an averaged, superpositional, picture of a final state or isolated intermediate with no temporal information on the changes in speciation under catalytic conditions.
This studentship will develop methods to determine real-time speciation of a single–crystalline catalyst while simultaneously measuring the kinetic profile of the substrates/products. Providing snapshots at precisely defined points in catalysis will give insight into resting states, decomposition pathways and microenvironment–derived selectivity. An opportunity to benchmark this new method comes from recently reported single-crystal to single–crystal transformations using solid/gas reactivity in Solid-state Molecular OrganoMetallic chemistry (SMOM). SMOM is based on unambiguously determining precise molecular structure, using single–crystal x-ray diffraction, of very reactive species that cannot even be observed using solution techniques.
This PhD will be highly collaborative, developing an in-operando approach by interfacing a single–crystal flow cell with a GC-MS and benchmarking with novel gas/solid catalysis. This will provide a step change in the ability to study catalytic reactions in the single crystal state and then be applied to understanding catalysis and gas separation/storage in extended (MOF) materials. The studentship will explore the transportability of the apparatus to other beamlines and engage the wider chemistry community. Apparatus will be initially developed at the National Crystallography Service (Southampton) before being transferred to Diamond. The application to catalysis will involve very close collaboration with the synthesis/catalysis groups of Weller (Oxford) and Rosseinsky (Liverpool): both non–supervisory roles.
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