Structural and textural properties of Fe2O3/γ-Al2O3 catalysts and their importance in the catalytic reforming of CH4 with H2S for hydrogen production

被引:26
作者
Galindo-Hernandez, Felix [1 ]
Dominguez, J. M. [1 ]
Portales, Benjamin [1 ]
机构
[1] IMP, Col San Bartolo Atepehua 07730, DF, Mexico
关键词
Hematite; gamma-Al2O3; Molecular hardness; Hydrogen; Carbon disulfide; Methane reforming; SOFT ACIDS; DISTRIBUTIONS; SULFIDE; AREA; HARD; GAS;
D O I
10.1016/j.jpowsour.2015.04.015
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
Newer catalysts for the methane reforming with H2S are designed, which are based on Fe2O3/gamma-Al2O3, nanocrystalline gamma-Al2O3 supports, and 1.0 to 6.0 wt% Fe. The main phases are identified as hematite and gamma-Al2O3, with sizes of about 2-4 nm. The structural features are characterized by X-ray diffraction, Rietveld's Refinement and Radial Distribution Function analysis. The textural properties of these catalysts are determined by N-2 sorption and surface fractal dimension calculations. Also, the electronic states are inferred by Mossbauer and UV-Vis (diffuse reflectance) spectroscopies. The activity of Fe2O3/gamma-Al2O3 catalysts in the methane reforming is tested in a fixed bed type reactor. Further calculations indicate that Fe2O3/gamma-Al2O3 catalysts go through a charge transfer decrease, which depends on the iron content, i.e., from 1.08 to 0.88 eV; Mossbauer spectroscopy reveals that Fe3+ ions adopt a tetrahedral coordination, which coincides with their higher activity for hydrogen production, with respect to catalysts having octahedral coordination. The specific surface area of these catalysts is about 84 m(2) g(-1), with a mean pore diameter of 2.5 nm. A mechanism for the methane reforming with H2S is proposed herein. (C) 2015 Elsevier B.V. All rights reserved.
引用
收藏
页码:13 / 24
页数:12
相关论文
共 46 条
[1]  
Agullo-Lopez F., 1988, POINT DEFECTS MAT
[2]   KINETIC-STUDY FOR THERMAL PRODUCTION OF HYDROGEN FROM H2S BY HETEROGENEOUS CATALYSIS OF VANADIUM SULFIDE IN A FLOW SYSTEM [J].
ALSHAMMA, LM ;
NAMAN, SA .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 1989, 14 (03) :173-179
[3]  
[Anonymous], IND STAT AN
[4]  
[Anonymous], 1991, 832S91100 EPA OFF WA
[5]  
[Anonymous], 2012, OIL GAS J
[6]   THE DETERMINATION OF PORE VOLUME AND AREA DISTRIBUTIONS IN POROUS SUBSTANCES .1. COMPUTATIONS FROM NITROGEN ISOTHERMS [J].
BARRETT, EP ;
JOYNER, LG ;
HALENDA, PP .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1951, 73 (01) :373-380
[7]   IMPROVING THE VALIDITY OF HYPERFINE FIELD DISTRIBUTIONS FROM MAGNETIC-ALLOYS .1. UNPOLARIZED SOURCE [J].
BRAND, RA .
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION B-BEAM INTERACTIONS WITH MATERIALS AND ATOMS, 1987, 28 (03) :398-416
[8]  
Brinker C.J., 2013, Sol-gel science: the physics and chemistry of sol-gel processing, DOI 10.1016/C2009-0-22386-5
[9]  
Cerna K., 2000, MATER STRUCT, V7, P6
[10]  
COELHO AA, 2007, TOPAS ACAD V4 1 COEL