In-depth Understanding of Catalytic Activation of Carbon Dioxide for Value-added Products

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In the foreseeable future, the use of fossil fuels for energy is inevitable and so is the emission of carbon dioxide (CO2) from it. To avoid the predicted climate change from the increase of CO2 concentration in the atmosphere, in addition to the technologies of CO2 capture and storage (CCS), which are passive from a strategic point of view, conversion of the emitted CO2 into useful and value-added chemicals or products (CO2 capture and utilization or CCU in short) is inherently important, and catalyst development for CO2 conversion plays a vital role in these technology advances. Building on the successful research and development of a catalyst for CO2 reforming of methane (CH4), this proposed research program focuses on the understanding of the mechanisms of C-O bond breakage and C-H bond formation in catalytic conversion of CO2, aiming to extend fundamental knowledge of catalyst structures that is necessary to the development of new and powerful catalysts for CO2 conversion to achieve desired CO2 utilization.******The methodology includes using the atomic layer deposition (ALD) method to prepare the model catalysts with known and uniform structures and using advanced instrumental characterization such as in situ and/or operando spectroscopic characterizations at the Canadian Light Source (CLS) for the catalytic mechanism studies. Density functional theory (DFT) calculations will also be used to help confirm the understanding. The short-term objectives of this program are to establish the relationship between the catalyst structures and catalytic performance on C-O bond breakage in CO2 reforming of CH4 reaction system and on C-H bond formation in CO2 hydrogenation for methanol. The long-term goal is to understand the catalyst structures of the complex, natural CO2 conversion processes such as photosynthesis and mimic the natural catalytic processes for CO2 utilization. The highly qualified personnel (HQP) training plan in the proposed research program includes PhD and MSc students in the fields of catalyst preparation using ALD technology and catalytic mechanism studies with CLS synchrotron technologies as well as the DFT calculations.