ORGANIC NITROGEN CONVERSION DURING THE THERMAL DECOMPOSITION OF HUADIAN OIL SHALE OF CHINA

XIANGXIN HAN ； BIN CHEN ； QINGYOU LI ； JIANHUI TONG ； XIUMIN JIANG

《Oil Shale》 34卷2期 (2017/06) Pp. 97-109

https://doi.org/10.3176/oil.2017.2.01

摘要

Organic nitrogen plays an adverse role in the utilization of oil shale, deactivating catalysts in the shale oil refining process and forming NO_X in the combustion of oil shale and shale oil. To have a deep understanding of its thermochemical transformation during the decomposition of oil shale, the conversion of organic nitrogen is experimentally studied and a set of physical models of nitrogen-containing groups is constructed and solved using the quantum chemical transition state theory (TST) in the Gaussian 09, Revision A.02 package. The results obtained show that three principal nitrogen-containing species - pyrrolic nitrogen, pyridinic nitrogen and amino nitrogen - first crack to nitriles or amino species from the breakup of the C-N bond, and then to HCN and NH_3. If attacked by oxygen-containing groups, the nitrogen-containing products formed can be further converted into NO_X. Including also quaternary and chemisorbed NO_X in the study, the conversion history of five typical nitrogen-containing groups present in oil shale kerogen is summarized and illustrated.

關鍵字

oil shale pyrolysis ； organic nitrogen ； thermochemical conversion ； quantum chemistry ； transition state theory