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IC4 FUNDED PROJECTS trodes with dissolved pyridines was also studied. There were clear indica- tions that adsorbed pyridine was involved – a finding that supports the con- cept of chemically binding the catalyst to the silicon surface. The experimental work with homogeneous catalysts and on semiconductor surfaces were corroborated by theoretical studies. The calculations carried out in the Rösch group concerning a heterogeneous reaction mechanism focused initially on the reaction energies and activation barriers of the first two reaction steps. The calculations showed that on a ruthenium surface the CO2 inserted preferentially either via the C atom or simultaneously via a C- and an O-centre, but not via an O atom alone, thus enabling initial hydride transfer to CO2. The pathways to the next important intermediates HCO and H2CO are assumed to proceed via the formate, for which the highest relative activation barrier is 97 kJ/mol. The highest barriers on the alternative pa- thways via CO are 110 kJ/mol (to form HCO) and 167 kJ/mol (to form COH), both of which are significantly higher than that for the formate-mediated path. Once H2CO has been formed, only two hydrogenation steps are needed to synthesise methanol with activation barriers of 49 kJ/mol and 127 kJ/mol respectively. In summary, the path via the formate is slightly energetical- ly favoured compared with the direct route. These results provide a readily apparent explanation as to why HCOO- and CO- species are predominantly found on the surface. The Department of Physical Chemistry focused on examining the photo- chemical properties of hybrid systems of metal clusters and semiconduc- tors. A platform was developed that enabled the synthesis, characterisati- on and photocatalytic study of nanostructured semiconductors containing metal clusters of atomically precise composition. It could be shown that under the same loading conditions, the size of the cluster had a significant effect on the photocatalytic activity of the system. A conceptual model was also developed that can describe these effects and can be used in the design of customised photocatalysts. 2.5.2 Exploitation, commercialisation and dissemination of results AdCOO Over the short- to medium-term, the adsorptive systems currently availa- ble will not be as cost-effective at capturing CO2 from power plant flue gas streams as the wet scrubbing methods and solvents presently used. If a suita- ble adsorbent were to become available in future, adsorptive capture would reduce operating costs resulting in significantly lower carbon capture costs over the long-term. 159PDF Image | Chemical Processes and Use of CO2
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