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Title: Carbon Dioxide Fixation and Utilization
Keywords: carbon dioxide, utilization, green chemistry, hydrothiolation, hydrosilylation
Issue Date: 22-Feb-2012
Citation: SITI NURHANNA BINTE RIDUAN (2012-02-22). Carbon Dioxide Fixation and Utilization. ScholarBank@NUS Repository.
Abstract: This thesis describes our efforts towards the fixation and utilization of CO2 as a feedstock, to yield fuels and synthetically useful intermediates. The fixation and utilization of carbon dioxide as a feedstock to form methanol was realized by the reduction of CO2 with hydrosilanes, over N-heterocyclic carbene (NHC) organocatalysts. Close examination of the reaction system revealed that the reaction took place with a three-step cascade reaction. The first hydrosilylation step was the rate-determining step, and explained the high selectivity and yield of methanol in excess of 95%. The extension of the homogeneous reaction system to a heterogeneous one was also realized with the use of polymeric NHC catalyst particles. The use of CO2 as a tool for organic transformations was also explored. A simple procedure for the stereoselective coupling of terminal alkynes and thiols has been developed under CO2 atmosphere. The reaction system was robust and utilizes inexpensive, readily available catalysts and substrates. Under the optimum reaction conditions, good to high yields and excellent stereoselecitvities were achieved for a broad range of aryl alkynes and thiols.
Appears in Collections:Ph.D Theses (Open)

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