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Catalysis for CO2 activation reactions with light alkanes

CO<sub>2</sub>, without question, the most famous greenhouse gas, is known to have an increasing concentration in both the atmosphere and oceans. To slow down the pace not only of global warming but also the ocean acidification, several routes are proposed to effectively reduce the net emission of CO<sub>2</sub>. Compared to Carbon Capture and Sequestration/Storage (CCS), Carbon Capture and Utilisation (CCU) has much more potential because of the lower costs of scale up and higher profitability to potentially attract capital investment. Different from the conventional CCU route which is to reduce CO<sub>2</sub> to fuels with hydrogen generated via renewable-energy-driving electricity, two processes are investigated in this thesis; that of Dry Methane Reforming (DMR) and the DeHydrogenation of Propane by CO<sub>2</sub> (DHP by CO<sub>2</sub>). The projects on these two processes not only develop catalysts which would be suitable for the reaction performance, but also the ultimate aim is to link the processes with a renewable energy source (in the thesis we chose Solar Thermal Heating).Thermodynamic calculations and process simulations were also evaluated. The results of DMR unfortunately did not indicate a promising future to link with Solar Thermal Heating due to the very high temperature required during the process. However, the results of thermodynamic calculations and process simulations in DMR project illustrate a good opportunity to utilise flue gas in industry through the so-called Tri- Methane Reforming (TMR). In the DHP by CO<sub>2</sub> process, the catalysts developed were less promising than the ones in DMR due to the severe side-reactions occurred which significantly decreased the selectivity for the desired product. However - and importantly - through our thermodynamic calculations and process simulations, the DHP by CO<sub>2</sub> process has a bright future if the Solar Thermal Heating can be applied with the relative lower temperature requirement, making the CO<sub>2</sub> utilisation process much easier to be fulfilled than DMR.

Identiferoai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:730114
Date January 2016
CreatorsDu, Xian
ContributorsEdwards, Peter P.
PublisherUniversity of Oxford
Source SetsEthos UK
Detected LanguageEnglish
TypeElectronic Thesis or Dissertation
Sourcehttps://ora.ox.ac.uk/objects/uuid:924c17f7-5b71-4e70-b304-e0686d0413ea

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