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Process Intensification by a One-Step, Plasma-Assisted Synthesis of Liquid Chemicals from Light Hydrocarbons
Project Number
DE-FE0031862
Last Reviewed Dated
Goal

The goal of this project is to use plasma stimulation of a light hydrocarbon resource to synthesize value-added liquid chemicals. This work will evaluate the hypothesis that the plasma will serve multiple roles in this transformative chemistry, including activation of Carbon - Hydrogen (C-H) bonds at low bulk gas temperature and pressure, providing a fast response for immediate startup and shutdown, enhancing the lifetime of the catalyst through plasma-assisted removal of surface impurities, and providing a means to activate Nitrogen (N2) to allow for the direct formation of chemicals containing nitrogen–carbon (N-C) bonds. In addition, the project will explore the potential for exploiting these processes more broadly, by building on recent discoveries using plasma-assisted methods to convert hydrogen and N2 feeds.

Performer(s)

University of Notre Dame – Notre Dame, IN 46556

Background

Flaring light hydrocarbons from wells and refineries amounts to a global, annual loss of >140 billion m3 of natural gas. Not only are valuable, non-renewable hydrocarbons misused during this process, but flaring also contributes more than 400 metric tons of CO2 to the environment. The implementation of chemical processing technology that directly converts light gases to liquid products will relieve the strain associated with gas separations and gas compression at the source.

Impact

The project offers the opportunity to assess a potential mechanism to reduce quantities of flared gas at oil and gas production sites, where gas transport options are insufficient or do not exist, by converting the gas to energy-dense liquid products. In addition to providing a value-added pathway for use of the gas, the proposed technology will also offer environmental and economic benefits through the reduction of CO2 emissions caused by the flaring of light hydrocarbon feeds and through the direct use of CO2 as a soft oxidant. All of these factors offer the potential to meaningfully contribute to ensuring U.S. security and prosperity by addressing energy and environmental challenges through transformative science and technology solutions.

Accomplishments (most recent listed first)
  • Design, construction, and safe operation of three plasma-stimulated reactor systems that are leak-free and operated with reproducible experimental data collection.
  • Validation and demonstration of hydrocarbon — N2 coupling under plasma stimulation, and liquid production.
  • Development of experimental procedures to identify and quantify products. 
  • Development and ongoing population of data structures to capture known/measured operating and performance parameters of reactors and materials. Validated through selected replication of experiments based off parameters in the database. 
  • Identification of surface-adsorbed intermediates from plasma stimulation using the in-situ/operando spectroscopy plasma reactor.
  • Experimental evidence of product selectivity control via plasma-simulated catalysis at lower bulk temperatures than thermal catalysis.
  • Patent Application: Production of Nitrogen-Containing Liquids from Hydrocarbon and N2 Feeds. File Date: 4/3/2020. Application #: 63/004,676.
Current Status

The project entered Budget Period (BP) 3 in March 2022. Year 2 (BP2) activities were focused on evaluating process conditions to improve the selectivities of desired products and the effects of possible shale gas contaminants in the feed system on product distribution.  In BP3, the project team will determine the appropriate catalyst to facilitate C-N coupling and/or liquid production by combining reaction performance results, in situ/operando characterization, and predictive modeling.  The team is using in situ spectroscopy to identify surfaces species formed from plasma stimulation and to determine if these species participate in C-N coupling pathways.  Additionally, the project team is evaluating alternative plasmas (e.g., gliding arc) to activate gas phase species to facilitate the production of liquid products.

PMIRAS
Image depicting a newly designed multimodal spectroscopic instrument combining polarization modulation infrared reflection-absorption spectroscopy (PMIRAS), mass spectrometry, and optical emission spectroscopy (OES) for the investigation of plasma−surface interactions.  Work published in ACS Appl. Mater. Interfaces 2021, 13, 47, 56242–56253.
Project Start
Project End
DOE Contribution

$999,954.00

Performer Contribution

$250,044

Contact Information

NETL – Robert Noll (robert.noll@netl.doe.gov or 412-386-7597)
University of Notre Dame – Jason Hicks (jhicks3@nd.edu or 574-631-3661)