The Haber-Bosch Process Revisited: On the Real Structure and Stability of "Ammonia Iron" under Working Conditions

被引:593
作者
Kandemir, Timur [1 ]
Schuster, Manfred E. [1 ]
Senyshyn, Anatoliy [2 ]
Behrens, Malte [1 ]
Schloegl, Robert [1 ]
机构
[1] Max Planck Gesell, Fritz Haber Inst, Abt Anorgan Chem, D-14195 Berlin, Germany
[2] Tech Univ Munich, Forsch Neutronenquelle Heinz Maier Leibnitz FRM 2, D-85747 Garching, Germany
关键词
catalyst microstructure; Haber-Bosch process; heterogeneous catalysis; iron nitridation; neutron diffraction; LONG-RANGE ORDER; IN-SITU; NEUTRON-DIFFRACTION; MAGNETIC-PROPERTIES; SURFACE; NITROGEN; CATALYST; DECOMPOSITION; MECHANISM; POWDER;
D O I
10.1002/anie.201305812
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
In situ neutron diffraction was used to study the structural properties of an industrial ammonia synthesis catalyst under working conditions similar to those of the Haber-Bosch process. Despite favorable thermodynamics, no indications of reversible bulk nitridation of the iron catalyst was observed in a self-generated ammonia concentration of 12 vol % at 425 °C and 75 bar after 88 h on stream. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
引用
收藏
页码:12723 / 12726
页数:4
相关论文
共 45 条
[1]   The interaction of nitrogen with the (111) surface of iron at low and at elevated pressures [J].
Alstrup, I ;
Chorkendorff, I ;
Ullmann, S .
JOURNAL OF CATALYSIS, 1997, 168 (02) :217-234
[2]  
Apodaca L. E., 2011, US GEOLOGICAL SURVEY
[3]  
Appl M., 2000, ULLMANNS ENCY IND CH, P139
[4]   KINETICS OF ACTIVATION OF THE INDUSTRIAL AND MODEL FUSED IRON CATALYSTS FOR AMMONIA-SYNTHESIS [J].
BARANSKI, A ;
KOTARBA, A ;
LAGAN, JM ;
PATTEKJANCZYK, A ;
PYRCZAK, E ;
REIZER, A .
APPLIED CATALYSIS A-GENERAL, 1994, 112 (01) :13-36
[5]   CATALYTIC DECOMPOSITION OF NITROGEN-15-LABELED HYDRAZINE ON MGO-SUPPORTED IRON [J].
BLOCK, J ;
SCHULZEK.G .
JOURNAL OF CATALYSIS, 1973, 30 (02) :327-329
[6]   THE TEXTURAL PROMOTION OF METALLIC IRON BY ALUMINA [J].
BORGHARD, WS ;
BOUDART, M .
JOURNAL OF CATALYSIS, 1983, 80 (01) :194-206
[7]   KINETICS AND MECHANISM OF AMMONIA-SYNTHESIS [J].
BOUDART, M .
CATALYSIS REVIEWS-SCIENCE AND ENGINEERING, 1981, 23 (1-2) :1-15
[8]   SURFACE, CATALYTIC AND MAGNETIC-PROPERTIES OF SMALL IRON PARTICLES .1. PREPARATION AND CHARACTERIZATION OF SAMPLES [J].
BOUDART, M ;
DELBOUILLE, A ;
DUMESIC, JA ;
KHAMMOUMA, S ;
TOPSOE, H .
JOURNAL OF CATALYSIS, 1975, 37 (03) :486-502
[9]   INTERACTION OF NITROGEN WITH IRON SURFACES .1. FE(100) AND FE(111) [J].
BOZSO, F ;
ERTL, G ;
GRUNZE, M ;
WEISS, M .
JOURNAL OF CATALYSIS, 1977, 49 (01) :18-41
[10]   SURFACE, CATALYTIC AND MAGNETIC-PROPERTIES OF SMALL IRON PARTICLES .3. NITROGEN INDUCED SURFACE RECONSTRUCTION [J].
DUMESIC, JA ;
TOPSOE, H ;
BOUDART, M .
JOURNAL OF CATALYSIS, 1975, 37 (03) :513-522