(602g) Low Temperature Hydrogenation of Amine Captured CO2

Low-temperature Hydrogenation of Amine Captured CO₂

Ji Su, Mi Lu, Lisha Yang, Hongfei Lin*

Chemical & Materials Engineering, University of Nevada, Reno, NV 89557, USA

HongfeiL@unr.edu

Climate change resulting from the emission of CO₂ has become a widespread concern in the recent years. Though various CO₂ capture technologies have been proposed, chemical absorption and adsorption are currently believed to be the most suitable ones for post-combustion power plants.¹ Carbon Capture and Storage (Sequestration) (CCS) is a promising technology that has the potential to address the 40% of emission emanating from large-point sources such as power plants.^2–7 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^8,9 and catalytic reduction of CO₂ to fuels or value added chemicals is one of the greatest challenges facing today's society.^8–12 Recently, increasing efforts have been devoted to the transformation of CO₂ into value added substances such as formic acid or formate, which can be conveniently obtained by hydrogenation of CO₂ and is highly attractive as an important chemical used as preservative and antibacterial agent as well as a clean source for H₂ generation.^13–21

Herein, effective low temperature processes for hydrogenating amine captured CO₂ to formate over supported transition metal nano-catalysts has been developed in this study.  Five representative amine monoethanolamine (MEA), diethanolamine (DEA), Triethanolamine (TEA), 2-amino-2-methyl-1-propanol (AMP) and Piperazine (PZ) were used to capture CO₂ and then the solution were conducted to hydrogenation reaction over different metal on carbon catalysts.  The effect of amine structure and co-solvent was investigated. At the optimized reaction conditions, a high yield of formate, >99%, was achieved by the reduction of AMP captured CO₂ over the carbon supported Pd nanoparticles catalyst.  The stability of the Pd on carbon catalyst was tested and the possible reaction mechanism was proposed.  The effects of amine structure, solubility, and functional group were profound on the conversion of amine-CO₂ adducts.  The yield of formates is highly dependent on the bicarbonate and alkyl carbonate ion intermediates in an solution of amine captured CO₂.

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