(87e) Developing Tunable Nanoscale Hybrid Electrolytes for Combined CO2 Capture and Conversion

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 design 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 talk, the current status of electrochemical CO2 conversion will be outlined through a brief discussion of relevant performance metrics, challenges and process requirements. The focus of this work is the development of Nanoparticle Organic Hybrid Materials (NOHMs)-based fluids as hybrid electrolyte systems that are capable of combined CO2 capture and conversion, without the need for a separate solvent regeneration step. Due to the complexity of these systems, a fundamental investigation of the structuring and organization of these nanoscale fluids is required. It has been observed that physical properties such as hydrodynamic size, viscosity and diffusion coefficient are highly dependent on the chemical nature and size of the secondary fluid molecule. Additionally, it was discovered that relevant transport properties of the untethered polymer were found to scale according to theoretical predictions. Interestingly, this behavior was not observed for NOHMs-based fluids. Lastly, the CO2 solubility of various 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. These findings provide important insights into the design and development of a novel reactive medium that is capable of performing combined CO2 capture and conversion.