On the nature of nitrogen-containing carbonaceous deposits on coked fluid catalytic cracking catalysts

被引:34
作者
Barth, JO [1 ]
Jentys, A [1 ]
Lercher, JA [1 ]
机构
[1] Tech Univ Munich, Lehrstuhl Tech Chem 2, D-85747 Garching, Germany
关键词
D O I
10.1021/ie034163i
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
The regeneration of FCC catalysts leads to significant NOx emissions. Hence, the identification of surface deposits and reaction intermediates is important for understanding the mechanisms by which nitrogen-containing species are converted into NOx or N-2. Characterization of the feed and of carbonaceous deposits on spent FCC catalysts by IR and NMR spectroscopy as well as by (MA)LDI-TOF mass spectrometry showed that polyaromatic pyrrole derivatives (alkylcarbazoles, alkylbenzocarbazoles, alkylindoles) are the main source of nitrogen in the feed of FCC units. Consequently, (poly-)aromatic compounds (m/z = 350-850) such as carbazole and quinoline derivatives are the main nitrogen-containing components in the coke. During oxidative regeneration, these pregraphitic species are converted into smaller aromatic compounds similar to the nitrogen molecules originally present in the feedstock. With increasing temperature, nitrogen-containing coke species accumulate on the catalyst surface and can only be removed by oxidative regeneration at 550-700 degreesC.
引用
收藏
页码:2368 / 2375
页数:8
相关论文
共 27 条
[1]  
BARTH JO, IN PRESS IND ENG CHE
[2]  
BARTH JO, 2003, P 17 WORLD PETR C RI, V3, P445
[3]   Environmental fluid catalytic cracking technology [J].
Cheng, WC ;
Kim, G ;
Peters, AW ;
Zhao, X ;
Rajagopalan, K ;
Ziebarth, MS ;
Pereira, CJ .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1998, 40 (1-2) :39-79
[4]   IDENTIFICATION OF COMPLEX AROMATIC-MOLECULES IN INDIVIDUAL INTERPLANETARY DUST PARTICLES [J].
CLEMETT, SJ ;
MAECHLING, CR ;
ZARE, RN ;
SWAN, PD ;
WALKER, RM .
SCIENCE, 1993, 262 (5134) :721-725
[5]   NOx emissions in fluid catalytic cracking catalyst regeneration [J].
Dishman, KL ;
Doolin, PK ;
Tullock, LD .
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH, 1998, 37 (12) :4631-4636
[6]   Deactivation pathways in zeolite-catalyzed isobutane/butene alkylation [J].
Feller, A ;
Barth, JO ;
Guzman, A ;
Zuazo, I ;
Lercher, JA .
JOURNAL OF CATALYSIS, 2003, 220 (01) :192-206
[7]   Common mechanistic aspects of liquid and solid acid catalyzed alkylation of isobutane with n-butene [J].
Feller, A ;
Zuazo, I ;
Guzman, A ;
Barth, JO ;
Lercher, JA .
JOURNAL OF CATALYSIS, 2003, 216 (1-2) :313-323
[8]  
Guisnet M., 1997, HDB HETEROGENEOUS CA, V2, P626
[9]   Comment on "Real time characterization of the organic composition and size of individual diesel engine smoke particles" [J].
Haefliger, OP ;
Bucheli, TD ;
Zenobi, R .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1999, 33 (21) :3932-3932
[10]   Mass spectrometry of polymers and polymer surfaces [J].
Hanton, SD .
CHEMICAL REVIEWS, 2001, 101 (02) :527-569