Development of Catalytic Processes for Carbon Dioxide Utilization
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Authors
Lu, Mi
Issue Date
2016
Type
Dissertation
Language
Keywords
amine , catalyst , CO2 , Heterogenous , hydrogen , hydrogenation
Alternative Title
Abstract
The increase in CO2 emissions contributes to the increase in global temperatures and climate change due to the ‘greenhouse effect.' The utilization of CO2 as a raw material in the synthesis of chemicals and liquid energy carriers offers a direct way to mitigate the increasing CO2 build-up. However, high-energy reagents and harsh reaction conditions are typically required for transforming CO2 into other chemicals. Renewable hydrogen is a high-energy material that can be stored by hydrogenating CO2 to valuable secondary energy carriers, such as methane, methanol, and formic acid. Indeed, formic acid/formate has been widely used in agriculture and the leather and dye industries and is the potential hydrogen storage material for fuel cells applications. Therefore, the aims of this dissertation are: (1) to develop a process of hydrogenating liquid ammonia or amines captured CO2 over supported palladium nanocatalysts, to produce value-added formate by utilizing the CO2 derivatives in the commercial Bioenergy with Carbon Capture and Storage (BECCS) process; (2) to further develop the rechargeable “hydrogen battery” based on the redox equilibrium between liquid ammonia captured CO2 / ammonium formates, as well as amine captured CO2 / formate amine adducts. The stored hydrogen can be catalytically released under mild conditions as the feed to fuel cells for regenerating electricity. The strategies of the process development will focus on the efficiency (rate of CO2 hydrogenation and dehydrogenation reaction) and energy use (the amount of energy required to utilize CO2 in existing products, i.e., reaction temperature and pressure). This development also includes gaining insight into the relationships among the various structures of amines, solvent effect, distribution of intermediates, catalytic performance, and reaction mechanism.
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In Copyright(All Rights Reserved)