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Hydrocarbon Utilization

Plasma Reforming of Carbon Oxides Robert Geiger, Sreekar Parami , David Staack Texas A&M, Mechanical Engineering . Hydrocarbon Utilization. CO2. Plasma Dissociation . H=393.5 kJ/mol CO2 H=241 kJ/mol H2O. CO. H2O. Combustion. Combustion Fischer Tropsch Ethanol Hydrogen. CO. H2.

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Hydrocarbon Utilization

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  1. Plasma Reforming of Carbon OxidesRobert Geiger, SreekarParami, David StaackTexas A&M, Mechanical Engineering

  2. Hydrocarbon Utilization CO2 Plasma Dissociation H=393.5 kJ/mol CO2 H=241 kJ/mol H2O CO H2O Combustion • Combustion • Fischer Tropsch • Ethanol • Hydrogen CO H2 CH4 (CxHy) Partial Combustion H=110 kJ/mol CO2 1/2 Plasma Polymerization Upgrading Carbon Oxide Polymers Higher Hydrocarbons Petrochemicals (Matthias Ballauff, et. al Angew. Chem. Int. Ed. 2004, 43)

  3. Experimental Setup • Power Supply: • Vmax ~ 10 kV • Imax ~ 40 mA • Freq ~ 25 – 30 kHz • P ~ 40W-150W

  4. DBD Reactor Color Variations

  5. Deposition Rate

  6. Increasing FlowFlow appears to change power density distribution 1700 sccm 870 sccm 180 sccm Gas temperature and surface temperature do not cause the different film colors. Increasing Power Power increases deposition rate and film darkness ~ 30W ~50W ~100W

  7. FTIR – Comparison with High Pressure Film (High Pressure Film FTIR data taken from: Lipp M J et al 2005 Nat. Mater. 4 211)

  8. Film Properties Hydration • C:O ~ 1.5 - 3.5 (XPS) • Solubility • Water (Hydrates) • Insoluble • Acetone • Ethanol • Solubility allows for spin coating • and layer by layer film growth Before After C:O ~ 1.9 1.7

  9. Kinetic Model in Development Proposed Mechanism for C3O3 Polymer Formation Kinetic Model of Carbon Monoxide Plasma Still need to add • CO* reactions • C(s) reactions • Surface reactions McTaggart FK PIasma Chemistry in Electrical Discharges (1967) Simulation

  10. Emission Spectroscopy C2 Swan Fit

  11. Future Work • CO Plasma • Determine the polymer structures (NMR) and chain length • Characterize polymers and determine their properties • Energy Balances • Complete the kinetic model and compare with experimental • Determine optimum production parameters • CO2 Plasma • Optical Emmsion for gas temperature and temperature gradients • Optimize systems • Residence times • Surface to volume ratios • Specific input power • Power supply efficiencies • Compare Systems

  12. Conclusion • CO Plasma • Interesting films can be formed as fast as 1 mg/min at 50W with solely carbon and oxygen atoms • These films appear similar in structure to high pressure CO polymers not C3O2 • Increased power darkens the film and increases deposition rate • Color changes do not alter the FTIR • A kinetic model in under development • The C2 swan, CO angstrom and CO Herzberg bands enables temperature measurements in the visible range • CO2 Plasma • Micro-glow discharge showed best results • High power density and rapid quenching are thought to be desirable

  13. References • Lipp M J et al 2005 Nat. Mater.4 211 • V V Brazhkin 2006 J. Phys.: Condens. Matter 18 9643 • McTaggart FK PIasma Chemistry in Electrical Discharges (1967) • P.C.Cosby, J. Chem. Phys. 98,9560(1993). • K.M.D’Amico,and A.L.S.Smith, J.Phys.D: Appl. Phys. 10,261 (1977) Email: rpg32@tamu.edu

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