Thermogravimetry, coupled with a mass spectrometer (TG-MS) was used to investigate
the catalytic effect potassium carbonate (K2CO3) and potassium chloride (KCl), on the char conversion and the product gas composition of chars derived from a South African inertinite-rich bituminous coal. Sequential leaching of the coal with HCl-HF-HCl was performed to reduce the mineral matter present in the coal. This was done in order to reduce possible undesirable interactions between the minerals and inorganic compounds in the coal during heat treatments. The leaching process substantially reduced the ash content from 21.5% to less than 3%.
K2CO3 and KCl [0.5, 1, 3, 5 K-wt %] were loaded to the demineralized coal, raw coal and
demineralized coal with added mineral mixture prior to charring. The mineral mixture was made up of kaolinite, quartz, pyrite, siderite, calcite, anastase and hydromagnesite. The ‘doped’ coal samples were then subjected to heat treatments in a CO2 atmosphere up to 1200 °C. The results obtained showed that both K2CO3 and KCl exhibit a catalytic effect on the char conversion during heat treatments in CO2 atmosphere and the char conversion was increased with increasing loadings up to 5 K-wt% of K2CO3 and KCl. The temperature ranges at which conversion occurred were found to be lower for K2CO3 than for KCl. Subsequently, char conversion occurred over a relatively narrower temperature range for K2CO3 than observed for KCl. The catalytic behaviour of K2CO3 and KCl was confirmed by the results obtained. The results also indicated that the catalytic influence of K2CO3 is greater than that of KCl and that KCl is more susceptible to deactivation by minerals and inorganic compounds present in the coal than K2CO3.
Different analytical techniques (XRF and XRD) were used to determine the extent of
interaction of the catalysts used with the char material in the 5 K-wt% ‘doped’ coal samples. From the XRF results, it was observed that the K2O content was reduced after heat treatments in CO2, however, no potassium crystalline phases were observed in the XRD results after heat treatments in CO2. The reduced K2O content may be attributed to the potassium been taken up in other mineral matter during char reaction with CO2, forming new amorphous inorganic complex compounds. Thus the potassium retained in the sample after heat treatment, indicated by the XRF results, may be in an amorphous phase.
Mass spectrometry (MS) indicated that temperatures at which the maximum rate of
evolution of gaseous species occurred were relatively lower for K2CO3 loaded char samples iv than observed for KCl loaded samples. In addition, no mass-to-charge ratio (m/z) peak at 39 atomic mass unit (amu) from the MS results was observed, indicating that no potassium was detected in the gaseous phases for all the char samples. The undetected potassium in the gaseous phase may be due to the detection limit of the MS equipment.
The MS results also indicated that addition of the catalyst facilitates the evolution of H2
from the coal char samples. Addition of the catalysts to the samples lowered the temperature at which maximum H2 was given off. The shift to lower temperatures was observed with increased catalyst loadings for both K2CO3 and KCl loaded samples. / Thesis (MSc (Chemistry))--North-West University, Potchefstroom Campus, 201
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:nwu/oai:dspace.nwu.ac.za:10394/8759 |
| Date | January 2012 |
| Creators | Leeuw, Kelebogile Ancient |
| Publisher | North-West University |
| Source Sets | South African National ETD Portal |
| Language | English |
| Detected Language | English |
| Type | Thesis |
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