reforming and fixation of carbon oxides in atmospheric pressure non- thermal co/co 2 plasmas robert...
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Reforming and Fixation of Carbon Oxides in Atmospheric Pressure Non-
thermal CO/CO2 Plasmas
Robert Geiger
Advisor: Dr. David Staack
Texas A&M Mechanical Engineering
Plasma Engineering & Diagnostics Laboratory (PEDL)
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Outline
• Introduction
• Experimental Setup
• Results
• Future Work
• Conclusion
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Carbon Monoxide at Really High Pressures
Lipp M J et al 2005 Nat. Mater. 4 211
V V Brazhkin 2006 J. Phys.: Condens. Matter 18 9643
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EXPERIMENTAL SECTION
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Experimental Setup
Power Supply:•Vmax ~ 10 kV•Imax ~ 40 mA•Freq ~ 25 – 30 kHz•P ~ 40W-150W
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Low Power Setting (~60W)
Color Changes with Time and Power
30 min 60 min 120min 180min
Hi Power Setting (~130W, 180 min)
Low Power Setting (~60W, 180 min)
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FTIR – Comparison with High Pressure Film
(High Pressure Film FTIR data taken from: Lipp M J et al 2005 Nat. Mater. 4 211)
500 1000 1500 2000 2500 3000 3500cm-1
High Pressure CO
High Pressure COPlasma CO Film
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Film Properties
•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
Hydration
C:O ~ 1.9 1.7
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Kinetics
Proposed mechanism from several sources
McTaggart FK PIasma Chemistry in Electrical Discharges (1967)
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Kinetic Model in Development
Still need to add• CO* reactions• C(s) reactions• Surface reactions
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Kinetic Model in Development
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Kinetic Model in Development
CO
CO2
C3O2
C3O2(p)
•Const T•Te = 1 eV•ne = 1013 cm-3
•ne = const
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Emission Spectroscopy
300 350 400 450 500 550 600 650w (nm)
C2 - SPECAIRCO - Our ModelExperimental
Angstrom CO Bands (B1Σ+ – A1π)
C2 Swan Bands (d3π– a3π)
Herzberg CO Bands (C1Σ+ – A1π)
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Emission Spectroscopy - Temperature
471.5 472 472.5 473 473.5 474 474.5
0
0.5
1
wavelength (nm)
Inte
nsity
(A
.U.)
Trot
= 408K
Tvib
= 1962K
FWHM = 0.271nm
RMSE = 1.66%
ExperModel
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Future Work
• Characterize polymers and determine their properties
• Complete the kinetic model and compare with experimental
• Determine optimum production parameters
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Conclusion
• Interesting films can be formed with solely carbon and oxygen atoms
• These films appear similar in structure to high pressure CO polymers
• A kinetic model in under development• The C2 swan, CO angstrom and CO
Herzberg bands enables temperature measurements in the visible range
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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)
Questions?
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Solubility and Hydration
Before After
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CO CO2 + C(gr)
Metastability of CO
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• C/O ratios ranging from 1.5-3.5
XPS
Ref: INSERT REF
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