Kinetically-Guided Rational Design of Chemical Looping Reactors for Partial Oxidation Reactions

There is an urgent need to reduce energy use in catalytic chemical processes and to transition these processes toward use of plentiful natural gas reserves available in the United States and around the world. By advancing novel reactor configurations, this project will provide a template for that transition. As part of this project, the PIs will also advance workforce development in the Gulf Coast region by organizing and hosting workshops for working professionals and students focused on decarbonization of the chemical industry, and by developing and teaching a short course on modular processes to be offered to working professionals.

Dynamic reactor performance will be investigated by combining catalyst synthesis and characterization, transient kinetic studies including temporal analysis of products (TAP), and kinetic and reactor modeling to understand the impact of molecular-level features such as oxygen speciation and reactivity on reactor performance. Reactor models will, for the first time, be developed while taking into account different types of oxygen species and their reactivities in both desired and undesired reaction pathways during dynamic operation.

Rather than using chemical looping merely to minimize mixing of reductant and oxidant, this research will design from the bottom-up. The designed catalysts and reactors will provide inherent advantages in product selectivity conferred by non-steady state operation. A detailed, molecular-level understanding of oxygen speciation and reactivity will be developed using transient kinetic experiments including TAP.

This will be integrated into reactor scale models that account for coupling between reaction and transport. The investigators will also exploit mass transfer limitations – typically detrimental in sequential reaction networks – through forced dynamic operation enabled by the selective transient depletion of unselective oxygen relative to selective oxygen.

This multiscale, kinetically-guided approach will lead to the identification of catalysts and reactors with performance exceeding the state-of-the-art. It will also provide a framework for quantitatively analyzing chemical looping and non-steady state reactor performance that could be applied to partial oxidation reactions more broadly.

This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.