ABSTRACT

Platform chemicals are the essential building blocks used by the chemical processing industries to produce high-value chemical products. Conversion of greenhouse gases (GHG) such as CO2 and CH4 to platform precursors could significantly reduce atmospheric GHG while producing oxygenated chemical feedstocks and fuels. Current production of oxygenated chemicals from GHG requires large-scale, complex, high-pressure reaction processes, and manufacturing operations with significant carbon footprints. Therefore, there is a critical need to explore more sustainable routes to dry methane reforming (DMR), the reaction between CO2 and CH4 to produce highly reactive hydrogen and carbon monoxide. Non-thermal (low temperature) plasma-catalysis processes have recently emerged as an alternative to current DMR. This electrically driven approach will be investigated for one-step production of oxygenated species from GHG under mild conditions, making use of renewable and decentralized electrical power sources, potentially expanding US employment and regional business opportunities. This research program will study the fundamental chemical and physical mechanisms at work in plasma-enhanced conversion of GHG with the goal of reaching chemical processing conditions that are energy flexible and efficient. Over the next five years the research team will focus on understanding plasma chemistry reaction mechanisms and the systematic design of plasma-catalytic membrane reactor concepts capable of on-demand use of renewable electricity. Education and outreach activities include developing an undergraduate/graduate level plasma catalysis class and continuing a STEM Camp for Girl Scouts.

In this project, atmospheric low-temperature plasma catalysis will be investigated as an alternative to conventional thermally activated reaction routes to oxygenated fuels and chemical products based on high pressure Dry Methane Reforming (DMR). The key feature of plasma-catalysis is the synergy between the plasma and the catalyst, where the non-equilibrium plasma creates radicals and charged plasma-phase species which react at the catalyst surface to form the chemical product species; however, little is known in terms of fundamental understanding of plasma/catalyst interactions and surface processes. This research will address this knowledge gap by focusing on perovskite catalysts, selected for their unique dielectric and polarization properties. The interaction between the charged species in the plasma and perovskite catalysts may lead to drastic changes in the perovskite structural and surface electronic properties, potentially leading to unprecedented oxygenated species production rates. The in situ diagnostic capabilities of the research team will make possible the systematic synthesis of plasma-enhanced perovskite catalysts designed to operate at low temperature (<200 deg C) and atmospheric pressure, opening the door to decentralized and modular production of oxygenated fuels and chemicals from CO2 and CH4. To further improve process performance, the catalyst will be fabricated as a unique macroporous perovskite membrane with the objective of improving selectivity to methanol. The proposed membrane reactor offers the advantages of significantly reduced pressure drop typically found in packed bed reactors enhancing process throughput. Specific research plans focus on: (1) Designing nanocrystalline perovskite membranes for the synthesis of oxygenated chemicals and fuels; (2) Fine tuning the catalytic active sites of selected perovskites for the synthesis of methanol; (3) Evaluating the catalytic performance of perovskite membranes under low-temperature plasma in the conversion of CO2/CH4 mixtures to methanol; (4) Elucidation and understanding of the synergism in plasma-catalyst systems for the synthesis of oxygenated chemical species.

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.

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