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Carbon Formation in Autothermal Reforming

 

Photographs of a rich flame (1:2 O2/CH4) in the annular burner at low (upper) and high (lower) steam-to-carbon ratios at 300 psi. Note the distinct orange incandescence from the soot being formed in the upper photo.

Autothermal reforming is an effective and energy-efficient way to produce hydrogen or synthesis gas for ammonia production and gas-to-liquids processes. However, soot formation at elevated pressures is a drawback. Sandia is investigating the formation of soot in a fuel-rich burner at high pressure and high temperature designed to mimic the conditions in the inlet burner of an autothermal reformer.

The experimental apparatus uses an annular co-flow burner configuration at pressures ranging from 250–1000 psi at various oxidation stoichiometries and steam-to-carbon ratios. A unique high-pressure optical cell is used to identify soot formation by measuring the attenuation of transmitted light.

Using pure methane as the feed fuel, recent results have revealed carbon dioxide content does not affect the soot formation process as much as originally presumed. The primary controlling factors are oxidation stoichiometry and fuel-steam ratio independent of total carbon. At these elevated pressures, the effect of additional CO2 in the system is small with respect to soot formation.

 The attenuation of transmitted light through the cell at two burner conditions at 250 psi. The burner is operated for three minutes after which the O2 is turned off.
A) CH4(1.0):O2(0.6):H2O(0.74),
B) CH4(1.0):O2(0.6):H2O(0.37).
The initial attenuation in B is due to soot formation in the gas flow and is about twice the initial attenuation in A. The sustained drop in signal from t = 142 to t = 145 in B is due to accumulation of deposits on the cell window. The O2 is turned off at t = 145. The recovery from t = 145 to t = 157 is due to steam cleaning of the windows. The final recovery to full transmittance at t = 157 is due to the addition of O2 in the absence of CH4.

 




Contact:
Steve Rice
sfrice@sandia.gov
(925) 294-1353