期刊
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
卷 169, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.jaap.2022.105820
关键词
Catalytic pyrolysis; Sulcis low-rank coal; Olivine and Ni/gamma-Al2O3 catalyst; Quantitative gas distribution; Isoconversional method
This study investigated the catalytic pyrolysis of Sulcis low-rank coal with the presence of a catalyst, and analyzed the properties of the products. The results showed that the addition of a catalyst significantly improved the yield of gas products during coal pyrolysis, and the nickel catalyst had a positive effect on the production of H2.
Catalytic pyrolysis of Sulcis low-rank coal over naturally occurring olivine, and home-made 15 wt%Ni/gamma-Al2O3 catalyst was conducted for the upgrading of coal pyrolysis volatile gases in the temperature range ambient900 degrees C under atmospheric pressure. Raw coal and mixtures of coal-additive (90:10 wt%) were slowly heated in temperature programmed mode using a laboratory-scale quartz furnace coupled in parallel to Fourier transform infrared (FTIR) spectrometer and GC chromatograph for quantitative analysis of flue gas. Coal pyrolysis with and without additives was also conducted by TG/DTG/DSC analysis at different heating rate (beta = 15, 20, 30 degrees Cmin(-1)). DSC results clearly indicated some extra exothermic events during catalytic coal pyrolysis. Quantitative gaseous products distribution with temperature showed yields significantly and selectively improved with additives. Generally, more CO and CO2 were emitted under catalytic coal pyrolysis. Meanwhile, nickel catalyst exerted a marked positive effect on H-2 yield overall in the temperature range 400-500 degrees C. The light hydrocarbons such as methane, ethane, propane and n-hexane substantially remaining unchanged, whereas a remarkable increase of emitted ethene was originated from catalytic pyrolysis. A deeper SO2 evolution was observed over olivine, whereas the N-containing compounds (NH3, NOx) were also modified in catalytic pyrolysis. Formaldehyde was also monitored, which represents a fragment originating from polycyclic aromatic side chains. Reaction kinetic study by a model-free isoconversional method indicated a complex multiple-step mechanism of coal pyrolysis, exception made for conversion values between 5% and 50% where a single-step reaction path was operating. The calculated average Ea and the pre-exponential factor were markedly reduced by the presence of additives. Meanwhile the compensation effect was also existing.
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