Gd/HZSM-5 catalyst for conversion of methanol to hydrocarbons: Effects of amounts of the Gd loading and catalyst preparation method

被引:42
作者
Kim, Sungtak [1 ]
Park, Gyungah [1 ]
Kim, Seok Ki [1 ,2 ]
Kim, Yong Tae [1 ,2 ]
Jun, Ki-Won [1 ,2 ]
Kwak, Geunjae [1 ,2 ]
机构
[1] Korea Res Inst Chem Technol, Carbon Resources Convers Catalyt Res Ctr, POB 107,Gajeongro 141, Yuseong 34114, Daejeon, South Korea
[2] Univ Sci & Technol, Adv Mat & Chem Engn, Daejeon 34113, South Korea
关键词
Gadolinium; Coke; ZSM-5; Deactivation; Methanol-to-hydrocarbons; COKE FORMATION; REACTION-MECHANISM; AROMATIC-HYDROCARBONS; TO-HYDROCARBONS; ZEOLITE; ZSM-5; OLEFINS; DEACTIVATION; CRACKING; COKING;
D O I
10.1016/j.apcatb.2017.08.056
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
In this work, the effect of the gadolinium (Gd) content and preparation method on the characteristics of Gd-modified HZSM-5 catalysts and their reactivity in a methanol-to-hydrocarbons (MTH) reaction has been studied in detail. Gd/HZSM-5 catalysts with Gd contents of 1 wt% (1GdHZ), 5 wt% (5GdHZ), and 10 wt% (1OGdHZ) were prepared by an incipient wet impregnation method, and another Gd-modified HZSM-5 catalyst (GdHZ_JE) was prepared by an ion exchange method. It was found that increasing the Gd content in the catalysts prepared via the impregnation method with uniformly distributed nano-sized particles and thin films of Gd2O3 directly influenced the crystallinity, surface area, pore volume, acid-base properties, and reactivity of the catalysts. In particular, the amount of Lewis acid sites (LAS) on the catalyst determine the selectivity of light olefins and aromatics during the MTH reaction. In contrast, the GdHZ_IE catalyst possess a larger number of strong LAS and show higher aromatic selectivities compared with the bare HZSM-5 catalyst. Regardless of the preparation method, the catalyst modification by Gd inhibited the formation of polycondensed aromatic species on the catalyst surface and reduced the amount of carbon deposition by more than 50%. As the increasing amounts of Gd reduced the amount of carbon deposition, the lifetimes of the Gd/HZSM-5 catalysts were also prolonged.
引用
收藏
页码:191 / 201
页数:11
相关论文
共 53 条
[1]   The contribution of the methanol-to-aromatics reaction to benzene methylation over ZSM-5 catalysts [J].
Adebajo, MO ;
Long, MA .
CATALYSIS COMMUNICATIONS, 2003, 4 (02) :71-76
[2]  
[Anonymous], 2017, CHEM CAT CHEM, DOI [DOI 10.1016/j.comcom.2017.09.001, DOI 10.3390/NU9030293]
[3]  
Bal R., 2014, COKE RESISTANT SOLID
[4]   The role of lanthana loading on the catalytic properties of Pd/Al2O3-La2O3 in the NO reduction with H2 [J].
Barrera, A ;
Viniegra, M ;
Fuentes, S ;
Díaz, G .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 56 (04) :279-288
[5]   COKE FORMATION IN HIGH-SILICA ZEOLITES [J].
BIBBY, DM ;
HOWE, RF ;
MCLELLAN, GD .
APPLIED CATALYSIS A-GENERAL, 1992, 93 (01) :1-34
[6]   The methanol-to-hydrocarbons reaction:: insight into the reaction mechanism from [12C]benzene and [13C]methanol coreactions over zeolite H-beta [J].
Bjorgen, M ;
Olsbye, U ;
Petersen, D ;
Kolboe, S .
JOURNAL OF CATALYSIS, 2004, 221 (01) :1-10
[7]  
Broach R.W., 2010, Zeolites in industrial separation and catalysis, DOI DOI 10.1002/9783527629565
[8]   Insights into the coke deposited on HZSM-5, Hβ and HY zeolites during the cracking of polyethylene [J].
Castano, Pedro ;
Elordi, Gorka ;
Olazar, Martin ;
Aguayo, Andres T. ;
Pawelec, Barbara ;
Bilbao, Javier .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2011, 104 (1-2) :91-100
[9]   A methanol to olefins review: Diffusion, coke formation and deactivation SAPO type catalysts [J].
Chen, D. ;
Moljord, K. ;
Holmen, A. .
MICROPOROUS AND MESOPOROUS MATERIALS, 2012, 164 :239-250
[10]   Propane dehydrogenation catalyzed by gallosilicate MFI zeolites with perturbed acidity [J].
Choi, Seung-Won ;
Kim, Wun-Gwi ;
So, Jung-Seob ;
Moore, Jason S. ;
Liu, Yujun ;
Dixit, Ravindra S. ;
Pendergast, John G. ;
Sievers, Carsten ;
Sholl, David S. ;
Nair, Sankar ;
Jones, Christopher W. .
JOURNAL OF CATALYSIS, 2017, 345 :113-123