Conversion of methyl mercaptan and methanol to hydrocarbons over solid acid catalysts - A comparative study

被引:67
作者
Hulea, Vasile [1 ]
Huguet, Edouard [1 ,2 ]
Cammarano, Claudia [1 ]
Lacarriere, Antoine [1 ]
Durand, Robert [1 ]
Leroi, Catherine [3 ]
Cadours, Renaud [2 ]
Coq, Bernard [1 ]
机构
[1] UMR 5253 CNRS ENSCM UM2 UM1, Inst Charles Gerhardt Montpellier, F-34296 Montpellier 5, France
[2] TOTAL SA, Explorat & Prod, F-92078 Paris, La Defense, France
[3] TOTAL SA, Explorat & Prod, F-64018 Pau, France
关键词
Methylmercaptan; Methanol; Zeolites; Catalysis; Desulfurization; ZEOLITE CATALYSTS; MECHANISM; OLEFINS; TRANSFORMATION; DEACTIVATION; COKING; ZSM-5; MTO;
D O I
10.1016/j.apcatb.2013.07.056
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
This study demonstrates that CH3SH (a harmful impurity in natural gas) can be selectively converted into H2S and hydrocarbons (M2TH process) on H-zeolite/zeotype with diverse topologies. The catalytic activity varied as follows: H-ZSM-5>H-Y>H-FER>H-BEA>H-MOR>H-SAPO-34. In addition, H-ZSM-5 was the most stable catalyst toward deactivation by coke. The effect of the carrier gas (nitrogen or methane) and the role of water on the catalytic behavior of zeolites were explored under different conditions. Similar performances were obtained using CH3SH/N-2 or CH3SH/CH4 mixtures, but the amount of coke drastically decreased and the catalyst lifetime increased when 2% of water was added into the reaction. M2TH was compared with the well-known MTH (methanol to hydrocarbons) process. Although there are similarities between the two processes, significant differences were also observed, essentially regarding the products formed and distributed. These aspects are discussed taking into account the reaction pathway involved in each process. (C) 2013 Elsevier B.V. All rights reserved.
引用
收藏
页码:547 / 553
页数:7
相关论文
共 26 条
[11]  
Froment GF., 1992, Catalysis, V9, P1, DOI DOI 10.1039/9781847553218-00001
[12]   COKING AND DEACTIVATION OF ZEOLITES - INFLUENCE OF THE PORE STRUCTURE [J].
GUISNET, M ;
MAGNOUX, P .
APPLIED CATALYSIS, 1989, 54 (01) :1-27
[13]   The mechanism of methanol to hydrocarbon catalysis [J].
Haw, JF ;
Song, WG ;
Marcus, DM ;
Nicholas, JB .
ACCOUNTS OF CHEMICAL RESEARCH, 2003, 36 (05) :317-326
[14]   A highly efficient process for transforming methyl mercaptan into hydrocarbons and H2S on solid acid catalysts [J].
Huguet, Edouard ;
Coq, Bernard ;
Durand, Robert ;
Leroi, Catherine ;
Cadours, Renaud ;
Hulea, Vasile .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2013, 134 :344-348
[15]   Mechanism of the Catalytic Conversion of Methanol to Hydrocarbons [J].
Ilias, Samia ;
Bhan, Aditya .
ACS CATALYSIS, 2013, 3 (01) :18-31
[16]   STUDY OF STABILITY AND SELECTIVITY OF CATALYTIC ACTION OF ZSM-TYPE ZEOLITES IN METHANOL TRANSFORMATION [J].
IONE, KG ;
ECHEVSKII, GV ;
NOSYREVA, GN .
JOURNAL OF CATALYSIS, 1984, 85 (01) :287-294
[17]   A new approach to the modeling of deactivation in the conversion of methanol on zeolite catalysts [J].
Janssens, Ton V. W. .
JOURNAL OF CATALYSIS, 2009, 264 (02) :130-137
[18]   Methanol to hydrocarbons over zeolites with MWW topology: Effect of zeolite texture and acidity [J].
Lacarriere, Antoine ;
Luck, Francis ;
Swierczynski, Dariusz ;
Fajula, Francois ;
Hulea, Vasile .
APPLIED CATALYSIS A-GENERAL, 2011, 402 (1-2) :208-217
[19]   CATALYTIC CONVERSION OF METHANOL TO LIGHT ALKENES ON SAPO MOLECULAR-SIEVES [J].
MARCHI, AJ ;
FROMENT, GF .
APPLIED CATALYSIS, 1991, 71 (01) :139-152
[20]   DECOMPOSITION OF ALKANETHIOLS TO DIALKYL SULFIDES AND HYDROGEN-SULFIDE [J].
MASHKINA, AV ;
GRUNVALD, VR ;
NASTEKA, VI ;
BORODIN, BP ;
YAKOVLEVA, VN ;
KHAIRULINA, LN .
REACTION KINETICS AND CATALYSIS LETTERS, 1990, 41 (02) :357-362