EAGER: Towards Sustainable Carbon-Negative Chemical Manufacturing by Creating Synergy between Carbon Dioxide Utilization and Biorefinery

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The development of economically viable techniques for manufacturing carbon-negative fuels and commodity chemicals from atmospheric carbon dioxide and renewable energy is a grand challenge with important societal and environmental sustainability implications. This research project explores the synergy between carbon dioxide utilization and biorefining operations for producing a particular class of chemicals, formates. Carbon dioxide is released from biorefining operations, so this "biogenic" carbon dioxide is being explored as a feedstock. The research project project aims to systematically explore and model the process chemistry of integrated carbon dioxide capture and conversion into formates. In addition to disseminating the results of this research to a broader audience via publications and presentations, the researchers will recruit undergraduate from the Pacific Northwest Louis Stokes Alliance for Minority Participation program (PNW LSAMP). The mission of LSAMP is to increase pathways to college for underrepresented minorities. The research group also commits to offering two summer internships for community college students to do research associated with this project.The main objective of this research project is to investigate the reactivity of carbonate ions, formed by capturing carbon dioxide with amines or ammonia in aqueous ethanol solutions, for the production of formates by catalytic hydrogenation. The research project focuses on studying the process chemistry and reaction mechanism of the integrated carbon dioxide capture and hydrogenation process, in which ethyl carbonate ions are the key intermediates for the highly selective production of formates in amine-bioethanol-water solvents at near ambient temperatures. The mechanism of the formation of ethyl carbonate ions during the carbon dioxide capture process is being elucidated through theoretical and experimental studies. The structure-activity relationship of carbon supported palladium nano-catalysts is being explored using advanced experimental tools, such as in-situ nuclear magnetic resonance spectroscopy and Fourier-transform infrared spectroscopy. In particular, the influence of the surface facets of palladium nanocrystals on the activation of biocarbonate and ethyl carbonate adsorbates in the carbon dioxide-amine-ethanol-water systems is being studied. By creating synergy between value-added carbon utilization and biorefining processes, this research approach may lead to the development of new technologies for manufacturing carbon-negative chemicals.