The electrochemical conversion of CO2 to chemicals and fuels using carbon-free energy has recently been proposed as a pathway to achieving net carbon neutrality, due to the rapid cost reduction of renewable energies. Although there have been early successes in catalyst development and reactor design for CO2 reduction, it is also important to consider the development of electrolytes that can effectively deliver CO2 to electrodes with favorable product selectivity and reaction rates. Novel reactive materials are currently being employed as additives to aqueous and non-aqueous electrolytes in order to improve CO2 solubility, tune the selectivity of the CO2 reduction reaction and enhance reaction rates. In this study, Nanoparticle Organic Hybrid Materials (NOHMs)-based fluids have been designed as hybrid electrolyte systems that are capable of combined CO2 capture and conversion, thus eliminating the need for a separate solvent regeneration step. Therefore, NOHMs-based electrolytes are hypothesized to possess an energetic advantage when compared with conventional two-step CO2 capture and conversion processes. The development of NOHMs-based electrolytes requires a fundamental investigation into the structuring and organization of these complex nanoscale fluids. A study of the mixing behaviors of NOHMs with a variety of secondary fluids has revealed a non-linear relationship between the viscosity and the concentration of NOHMs; this non-linear relationship is significantly influenced by the chemistry and molecular size of the secondary fluid. Additionally, the CO2 solubility of NOHMs-based electrolytes has been measured and a change in the selectivity of the CO2 reduction reaction has been identified in the presence of these nanoscale electrolytes. The results of this work provide important insights into the design and development of a novel reactive medium that is capable of performing combined CO2 capture and conversion, thus improving the overall sustainability of the proposed CO2-to-chemicals and fuels pathways.

Tunable nanoscale hybrid electrolytes for combined CO2 capture and conversion

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

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