Integrated Direct Air Capture and H2-Free CO2 Valorization

The emission of CO2 represents one of the most pressing environmental challenges. Addressing this challenge requires a multi-faceted approach that involves a vigorous move to renewable energy and negative emission technologies (NETs). Direct air capture (DAC) is arguably the most challenging NET. Conversion of CO2 into valuable chemical products could promote DAC deployment. However, a significant cost reduction is needed and could be realized by designing highly efficient, integrated CO2 capture and conversion processes that leverage the resources available at the existing infrastructure. This project aims to advance the fundamental understanding of a novel integrated DAC and CO2 conversion process that converts CO2 without using external H2. The work involves the design and development task-specific ionic liquids (ILs) for DAC and subsequently conversion of CO2 to chemicals (ethylene, CO, and polyketones) using ethane as input for a tandem catalytic processes. Advanced characterization and theoretical studies are employed to decipher the interactions between ILs and single-site catalysts with CO2 and to elucidate the CO2 capture and conversion mechanisms. Data science-driven predictive computation methods accelerate the design of new ILs and catalysts. The methodology has four critical components: 1) efficient CO2 capture, 2) H2-free CO2 conversion , 3) operando characterization, and 4) data science-driven predictive computation. Hence, this work will strengthen the foundation for technological advancement for the production of value-added materials, such as polyketones, from ambient CO2.