[article]
| Titre : |
Effects of O2 on characteristics of sulfur added to petroleum coke through reaction with SO2 |
| Type de document : |
texte imprimé |
| Auteurs : |
Eric A. Morris, Auteur ; Charles Q. Jia, Auteur |
| Année de publication : |
2011 |
| Article en page(s) : |
pp. 12709–12717 |
| Note générale : |
Chimie industrielle |
| Langues : |
Anglais (eng) |
| Mots-clés : |
Sulfur petroleum coke |
| Résumé : |
Alberta oil-sands petroleum coke is an abundant byproduct of the upgrading of bitumen. The current study aims to improve the current understanding of sulfur added to the surface of petroleum coke through reaction with sulfur dioxide (SO2) and how this is affected by a large excess of oxygen (O2). Particular focus is given to the distribution and speciation of sulfur within the coke particles, as well as its thermal stability. Petroleum coke was activated in SO2 with and without O2 in a packed bed reactor at 600−800 °C. The activated cokes were characterized with electron probe microanalysis (EPMA), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). Cross-sectional analysis with EPMA of activated coke particles revealed that sulfur-rich coke particles (i.e., SIAC) could be produced with and without O2. Under low SO2 (3%), high O2 (18%) conditions, however, O2 competitively reacted with coke at 600 °C, and SO2 only reacted to form a sulfur-rich layer after O2 had been depleted. Analysis with XPS suggested that the sulfur-rich layer of the coke particles was made up of thiophene from the coke plus carbon−sulfur surface complexes, mainly heterocyclic sulfide and disulfide, while the presence of aliphatic sulfide, thiolactone, and thiol could not be ruled out. TGA and DSC analyses confirmed that sulfur added to activated coke via reaction with SO2 was not elemental in nature. In both N2 and air, sulfur added via high-temperature reaction with SO2 is more thermally stable than that of a commercial SIAC sulfurized at lower temperatures. This may have beneficial implications if these SO2 activated cokes were to be used to capture mercury, since they could be thermally regenerated with minimal loss of active sulfur surface sites while the captured mercury is collected, avoiding the costly and potentially problematic landfill disposal of Hg-containing activated carbon. |
| DEWEY : |
660 |
| ISSN : |
0888-5885 |
| En ligne : |
http://pubs.acs.org/doi/abs/10.1021/ie101388q |
in Industrial & engineering chemistry research > Vol. 49 N° 24 (Décembre 2010) . - pp. 12709–12717
[article] Effects of O2 on characteristics of sulfur added to petroleum coke through reaction with SO2 [texte imprimé] / Eric A. Morris, Auteur ; Charles Q. Jia, Auteur . - 2011 . - pp. 12709–12717. Chimie industrielle Langues : Anglais ( eng) in Industrial & engineering chemistry research > Vol. 49 N° 24 (Décembre 2010) . - pp. 12709–12717
| Mots-clés : |
Sulfur petroleum coke |
| Résumé : |
Alberta oil-sands petroleum coke is an abundant byproduct of the upgrading of bitumen. The current study aims to improve the current understanding of sulfur added to the surface of petroleum coke through reaction with sulfur dioxide (SO2) and how this is affected by a large excess of oxygen (O2). Particular focus is given to the distribution and speciation of sulfur within the coke particles, as well as its thermal stability. Petroleum coke was activated in SO2 with and without O2 in a packed bed reactor at 600−800 °C. The activated cokes were characterized with electron probe microanalysis (EPMA), X-ray photoelectron spectroscopy (XPS), thermogravimetric analysis (TGA), and differential scanning calorimetry (DSC). Cross-sectional analysis with EPMA of activated coke particles revealed that sulfur-rich coke particles (i.e., SIAC) could be produced with and without O2. Under low SO2 (3%), high O2 (18%) conditions, however, O2 competitively reacted with coke at 600 °C, and SO2 only reacted to form a sulfur-rich layer after O2 had been depleted. Analysis with XPS suggested that the sulfur-rich layer of the coke particles was made up of thiophene from the coke plus carbon−sulfur surface complexes, mainly heterocyclic sulfide and disulfide, while the presence of aliphatic sulfide, thiolactone, and thiol could not be ruled out. TGA and DSC analyses confirmed that sulfur added to activated coke via reaction with SO2 was not elemental in nature. In both N2 and air, sulfur added via high-temperature reaction with SO2 is more thermally stable than that of a commercial SIAC sulfurized at lower temperatures. This may have beneficial implications if these SO2 activated cokes were to be used to capture mercury, since they could be thermally regenerated with minimal loss of active sulfur surface sites while the captured mercury is collected, avoiding the costly and potentially problematic landfill disposal of Hg-containing activated carbon. |
| DEWEY : |
660 |
| ISSN : |
0888-5885 |
| En ligne : |
http://pubs.acs.org/doi/abs/10.1021/ie101388q |
|
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