Public Abstract

DE-SC0025543: Investigation of Reaction Pathways and Temperature Inhibition in Methane DBD Plasmas at the Princeton Collaborative Research Facility (PCRF)

Award Status: Active

Institution: University of Notre Dame du Lac, Notre Dame, IN
UEI: FPU6XGFXMBE9
DUNS: 824910376

Most Recent Award Date: 09/06/2024
Number of Support Periods: 1
PM: Podder, Nirmol

Current Budget Period: 09/01/2024 - 08/31/2025
Current Project Period: 09/01/2024 - 08/31/2025
PI: Go, David

Supplement Budget Period: N/A

Public Abstract

The conversion of light hydrocarbons into higher-order hydrocarbons, such as olefins, can have tremendous industrial impact as these products are often the building blocks used for a number of industrial products, including synthetic rubbers and fibers. Furthermore, combining light hydrocarbons with other chemical species, such as nitrogen, can yield valuable carbon-nitrogen (C-N) compounds that are relevant to industries such as pharmaceuticals. Production flaring is the on-site burning of light hydrocarbons that escape from crude oil and other extraction processes, producing not only vast amounts of pollution but wasting valuable natural resources. Electrically driven plasma processes, often in combination with catalysts, have the potential to address this waste issue by facilitating on-site conversion of light hydrocarbons rather than flaring using renewable electricity as the primary energy resource. The effective design of reactors and processing systems, however, requires a detailed understanding of the underlying plasma chemistry in order to establish rationale design strategies to control the yield and selectivity toward desired products. The goal of this research is to advance understanding of plasma-driven chemical conversion of light hydrocarbons using dielectric barrier discharges (DBDs) and methane (CH4) as a model system. This project will use the Princeton Collaborative Research Facility (PCRF) at Princeton Plasma Physics Laboratory (PPPL) to measure the products of a temperature-controlled methane DBD using Fourier transform infrared absorption spectroscopy (FTIR-AS). In particular, this work will use a heated FTIR cell to inhibit recombination of plasma products as the gas effluent from the DBD reactor cools. There are two objectives: (i) experimentally determine decomposition products of the gas effluent of CH4 plasmas across a range of temperatures and correlate these to plasma properties and (ii) conduct plasma simulations to predict product distributions for CH4 plasmas across a range of conditions. At the outcome of this work, there will be greater clarity on how the concentration of decomposition products varies with reaction temperature and whether these correlate with the electrical properties of the DBD, and in particular the plasma mode, or alternatively, if they are due solely to the reaction kinetics of various intermediates. If successful, this fundamental understanding of methane plasma behavior will inform the design of plasma reactor systems to facilitate the conversion of methane to higher-order hydrocarbons such as olefins and C-N compounds, and more broadly, advance understanding of the inherent relationships between reaction and plasma conditions for hydrocarbon plasmas.

The conversion of light hydrocarbons into higher-order hydrocarbons, such as olefins, can have tremendous industrial impact as these products are often the building blocks used for a number of industrial products, including synthetic rubbers and fibers. Furthermore, combining light hydrocarbons with other chemical species, such as nitrogen, can yield valuable carbon-nitrogen (C-N) compounds that are relevant to industries such as pharmaceuticals. Production flaring is the on-site burning of light hydrocarbons that escape from crude oil and other extraction processes, producing not only vast amounts of pollution but wasting valuable natural resources. Electrically driven plasma processes, often in combination with catalysts, have the potential to address this waste issue by facilitating on-site conversion of light hydrocarbons rather than flaring using renewable electricity as the primary energy resource. The effective design of reactors and processing systems, however, requires a detailed understanding of the underlying plasma chemistry in order to establish rationale design strategies to control the yield and selectivity toward desired products. The goal of this research is to advance understanding of plasma-driven chemical conversion of light hydrocarbons using dielectric barrier discharges (DBDs) and methane (CH4) as a model system. This project will use the Princeton Collaborative Research Facility (PCRF) at Princeton Plasma Physics Laboratory (PPPL) to measure the products of a temperature-controlled methane DBD using Fourier transform infrared absorption spectroscopy (FTIR-AS). In particular, this work will use a heated FTIR cell to inhibit recombination of plasma products as the gas effluent from the DBD reactor cools. There are two objectives: (i) experimentally determine decomposition products of the gas effluent of CH4 plasmas across a range of temperatures and correlate these to plasma properties and (ii) conduct plasma simulations to predict product distributions for CH4 plasmas across a range of conditions. At the outcome of this work, there will be greater clarity on how the concentration of decomposition products varies with reaction temperature and whether these correlate with the electrical properties of the DBD, and in particular the plasma mode, or alternatively, if they are due solely to the reaction kinetics of various intermediates. If successful, this fundamental understanding of methane plasma behavior will inform the design of plasma reactor systems to facilitate the conversion of methane to higher-order hydrocarbons such as olefins and C-N compounds, and more broadly, advance understanding of the inherent relationships between reaction and plasma conditions for hydrocarbon plasmas.