Carbon Capture, Utilization and Storage (CCUS) has been proposed as a strategy to address the climate change that has been caused by the significant rise in the levels of anthropogenic CO2 in the atmosphere. With the rapid deployment of renewable energy in recent years, now there exists carbon-free energy (e.g., electricity from solar and wind) that can be used to activate CO2. Many researchers have been developing electrochemical processes that can convert CO2 to chemicals and fuels. While significant advances have been made in terms of catalysis, less studies have focused on the reactive medium (electrolyte). The CO2 solubility in typical aqueous electrolytes is limited, which can challenge the overall efficiency of CO2 conversion to chemicals and fuels via electrochemical reduction. Thus, a novel class of reactive materials has been developed for use as an electrolyte with improved CO2 solubility and these materials can perform combined CO2 capture and conversion. In this study, Nanoparticle Organic Hybrid Materials (NOHMs)-based fluids have been designed as hybrid electrolyte systems that are capable of capturing and converting CO2 without the need for a separate solvent regeneration step. As a result, NOHMs-based fluids have an energetic advantage when compared with conventional two step CO2 capture and conversion processes. The investigation into the mixing behavior of NOHMs-based fluids reveals a non-linear relationship between the viscosity and the concentration of NOHMs. This non-linear relationship is a result of the hierarchical structures that are present within NOHMs-based fluids, as determined by USAXS experiments. Additionally, this relationship suggests the presence of a critical concentration of NOHMs is one of the major design principles for tuning the viscosity and ion transport during CO2 capture and conversion. 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.

Unique mixing behaviors of novel nanoscale hybrid material systems enabling combined CO2 capture and conversion

256th National Meeting (2018)

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