13C MAS NMR mechanistic study of the initial stages of propane activation over H-ZSM-5 zeolite

被引:40
作者
Ivanova, II [1 ]
Pomakhina, EB
Rebrov, AI
Derouane, EG
机构
[1] Moscow MV Lomonosov State Univ, Dept Chem, Moscow 119899, Russia
[2] RAS, Inst Petrochem Synth, Moscow 117012, Russia
[3] Univ Liverpool, Leverhulme Ctr Innovat Catalysis, Liverpool L69 3BX, Merseyside, England
关键词
propane activation; mechanism; zeolites; H-ZSM-5; MAS NMR; carbenium ions; carbonium ions;
D O I
10.1023/A:1019139111671
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
C-13 MAS NMR study of the early stages of propane 2-C-13 activation was performed over H-ZSM-5 catalysts with various content of protonic and aprotonic sites. The reaction mechanism was tested by addition of various probe-molecules (C3H6, C6H6, H-2, H2O and CO). The results on tracing the fate of 13C label during this experiments conclude to a monofunctional mechanism involving propane protonation on the strong Bronsted sites of H-ZSM-5 and the formation of carbonium ion type transition states, which further evolve in four different ways leading to C-13 scrambling in propane, cracking, dehydrogenation and disproportionation.
引用
收藏
页码:49 / 59
页数:11
相关论文
共 48 条
[1]   CRACKING REACTIONS OF C6 PARAFFINS ON HZSM-5 [J].
ABBOT, J .
APPLIED CATALYSIS, 1990, 57 (01) :105-125
[2]   REACTIONS OF 3-METHYLPENTANE AND 2,3-DIMETHYLBUTANE ON ALUMINOSILICATE CATALYSTS [J].
ABBOT, J .
JOURNAL OF CATALYSIS, 1990, 126 (02) :628-642
[3]   DIRECT OBSERVATION OF SHAPE SELECTIVITY IN ZEOLITE ZSM-5 BY MAGIC-ANGLE-SPINNING NMR [J].
ANDERSON, MW ;
KLINOWSKI, J .
NATURE, 1989, 339 (6221) :200-203
[4]   INFLUENCE OF FRAMEWORK AND NONFRAMEWORK ALUMINUM ON THE ACIDITY OF HIGH-SILICA, PROTON-EXCHANGED FAU-FRAMEWORK ZEOLITES [J].
BEYERLEIN, RA ;
MCVICKER, GB ;
YACULLO, LN ;
ZIEMIAK, JJ .
JOURNAL OF PHYSICAL CHEMISTRY, 1988, 92 (07) :1967-1970
[5]  
Breitmaier E., 1987, Carbon-13 NMR spectroscopy
[6]   DEHYDROGENATION - THE 1ST STEP IN THE CRACKING OF ISOPENTANE OVER SILICA-ALUMINA CRACKING CATALYSTS [J].
BRENNER, A ;
EMMETT, PH .
JOURNAL OF CATALYSIS, 1982, 75 (02) :410-415
[7]   ISOMERIZATION AND CRACKING OF C-13-LABELED HEXANES OVER H-MORDENITE .1. LABELING OF THE PRODUCTS AND GENERAL REACTION SCHEME [J].
DAAGE, M ;
FAJULA, F .
JOURNAL OF CATALYSIS, 1983, 81 (02) :394-404
[8]   THERMODYNAMIC AND MECHANISTIC STUDIES OF INITIAL-STAGES IN PROPANE AROMATIZATION OVER GA-MODIFIED H-ZSM-5 CATALYSTS [J].
DEROUANE, EG ;
HAMID, SBA ;
IVANOVA, II ;
BLOM, N ;
HOJLUNDNIELSEN, PE .
JOURNAL OF MOLECULAR CATALYSIS, 1994, 86 (1-3) :371-400
[9]  
ENGELHARDT G, 1987, HIGH RESOLUTION SOLI, P379
[10]   CONTRIBUTION TO THE UNDERSTANDING OF THE REACTION CHEMISTRY OF ISOBUTANE AND NEOPENTANE OVER ACID CATALYSTS, .1. [J].
ENGELHARDT, J ;
HALL, WK .
JOURNAL OF CATALYSIS, 1990, 125 (02) :472-487