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Effects of Pressure on the Properties of Coal Char Under Gasification Conditions at High Initial Heating RatesShurtz, Randy C. 23 September 2011 (has links)
The effects of elevated pressure and high heating rates on coal pyrolysis and gasification were investigated. A high-pressure flat-flame burner (HPFFB) was designed and built to conduct these studies. The HPFFB was designed to provide an environment with laminar, dispersed entrained flow, with particle heating rates of ~10^5 K/s, pressures of up to 15 atm, and gas temperatures of up to 2000 K. Residence times were varied from 30 to 700 ms in this study. Pyrolysis experiments were conducted at particle heating rates of ~10^5 K/s and maximum gas temperatures of ~1700 K at pressures of 1 to 15 atm. A new coal swelling correlation was developed that predicts the effects of heating rate, pressure, and coal rank on the swelling ratio at heating rates above ~10^4 K/s. A coal swelling rank index system based on 13C-NMR chemical structural parameters was devised. The empirical swelling model requires user inputs of the coal ultimate and proximate analyses and the use of a transient particle energy balance to predict the maximum particle heating rate. The swelling model was used to explain differences in previously reported bituminous coal swelling ratios that were measured in facilities with different heating rates. Char gasification studies by CO2 were conducted on a subbituminous coal and 4 bituminous coals in the HPFFB. Pressures of 5, 10, and 15 atmospheres were used with gas compositions of 20, 40, and 90 mole % CO2. Gas conditions with peak temperatures of 1700 K to 2000 K were used, which resulted in char particle temperatures of 1000 K to 1800 K. Three gasification models were developed to fit and analyze the gasification data. A simple 1st-order model was used to show that the measured gasification rates were far below the film-diffusion limit. The other two models, designated CCK and CCKN, were based on three versions of the CBK models. CCKN used an nth-order kinetic mechanism and CCK used a semi-global Langmuir-Hinshelwood kinetic mechanism. The two CCK models fit the HPFFB gasification data better than the 1st-order model. The fits of the gasification data with CCK and CCKN were comparable to each other. The fit of the data in CCK suggests that Knudsen diffusion may have influenced the gasification rates in the HPFFB experiments. The gasification rate parameters in each of the three models were correlated with coal rank. 13C-NMR parameters were used to estimate a structural parameter of the coal char. Char-CO2 gasification rate coefficients correlated better with this NMR-based char structure index than it did with the carbon and oxygen content of the parent coal.
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