Restricted Research - Award List, Note/Discussion Page

Fiscal Year: 2021

179  University of North Texas  (84475)

Principal Investigator: Marshall,Paul

Total Amount of Contract, Award, or Gift (Annual before 2011): $ 315,290

Exceeds $250,000 (Is it flagged?): Yes

Start and End Dates: - 8/31/23

Restricted Research: YES

Academic Discipline: Chemistry

Department, Center, School, or Institute: College of Science

Title of Contract, Award, or Gift: Chemistry of ammonia-based fuels

Name of Granting or Contracting Agency/Entity: U.S. Department of Energy
CFDA Link: DOE
81.049

Program Title: N/A
CFDA Linked: Office of Science Financial Assistance Program

Note:

1.1.1 (SAM); Novel ammonia and ammonia/hydrocarbon mixtures are possible fuels that can be created using renewable energy and would reduce emissions of carbon dioxide. The gas-phase chemical kinetics of reactions relevant to their combustion will be investigated both experimentally and computationally. Phase 1 of the work will focus on the characterization of elementary processes by experimental and theoretical methods. Most experiments will be based on generation of reactive intermediates by ultraviolet laser photolysis of precursors combined with time-resolved electronic spectroscopy to monitor short-lived reactants in real time with microsecond resolution, at temperatures up to 1100 K. An alternative approach will be relative rate methods, where photoinitiated chemistry is monitored by infrared spectroscopy which allows detection of products as well as reactants, on a 100-1000 s time scale. The computational work will rely on density functional theory and coupled cluster methods to develop potential energy surfaces for chemical reactions, in order to deduce rate constants and product branching ratios. Transition state unimolecular rate theories, with allowance for anharmonic effects and multiple low-energy configurations, will be applied to derive kinetic information to help interpret experiments and to extrapolate to inaccessible conditions. In Phase 2 a jet-stirred reactor will be employed to monitor thermally-initiated chemistry at elevated temperatures on a ca. 1 second time scale, with infrared detection. The time profiles of reactants and products will reflect the impact of multiple reactions. An overall multireaction mechanism, incorporating the new results for elementary steps, will be developed in Phase 3 and validated by comparison with literature data and the new multireaction experiments. Likely outcomes are quantitative data for elementary reactions, improved understanding of the fundamental kinetics of species important in hydrocarbon-ammonia oxidation, and development of an overall chemical mechanism that will permit efficient design of new fuel and combustion engine systems, all with the ultimate goal of reducing harmful emissions and environmental impact.

Discussion: No discussion notes

 

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