Effect of ruthenium precursor on hydrogen-treated active carbon supported ruthenium catalysts for ammonia synthesis

被引:60
作者
Zhong, ZH [1 ]
Aika, K [1 ]
机构
[1] Tokyo Inst Technol, Interdisciplnary Grad Sch Sci & Engn, Dept Environm Chem & Engn, Midori Ku, Yokohama, Kanagawa 226, Japan
关键词
ruthenium complexes; active carbon supported complexes; ammonia synthesis; catalysis;
D O I
10.1016/S0020-1693(98)00202-3
中图分类号
O61 [无机化学];
学科分类号
070301 ; 081704 ;
摘要
Active carbon (A.C.), after treatment at 1123 K with hydrogen for more than 24 h, was found to be very effective as a support for ruthenium catalysts in ammonia synthesis. The activity of barium promoted Ru catalysts supported on this treated A.C, is affected remarkably by the Ru precursor. Ru-3(CO)(12) was found previously to be the most effective Ru precursor for oxide supports such as Al2O3, MgO, and CeO2 in ammonia synthesis. However, in this study, the Ru-BaO/A.C. catalyst prepared from Ru(acac)(3) was found to yield the highest activity, while the catalyst prepared from Ru-3(CO)(12) resulted in the lowest activity among several precursors. Transmission electron microscopy and hydrogen chemisorption showed that the particle size of Ru obtained from the decomposition of Ru(acac)(3) on hydrogen-treated A.C, is smaller than the particle size of Ru obtained from the decomposition of Ru-3(CO)(12). Additionally, RuCl3 was found to be an effective precursor for Ru/A.C, catalyst. It has been suggested that chlorine ions can be removed easily from A.C. by hydrogen reduction at 773 K, and that this results in the high activity. (C) 1998 Elsevier Science S.A. All rights reserved.
引用
收藏
页码:183 / 188
页数:6
相关论文
共 25 条
[1]   ACTIVATION OF NITROGEN BY ALKALI-METAL PROMOTED TRANSITION-METAL .1. AMMONIA SYNTHESIS OVER RUTHENIUM PROMOTED BY ALKALI-METAL [J].
AIKA, K ;
OZAKI, A ;
HORI, H .
JOURNAL OF CATALYSIS, 1972, 27 (03) :424-&
[2]   PREPARATION AND CHARACTERIZATION OF CHLORINE-FREE RUTHENIUM CATALYSTS AND THE PROMOTER EFFECT IN AMMONIA-SYNTHESIS .3. A MAGNESIA-SUPPORTED RUTHENIUM CATALYST [J].
AIKA, K ;
TAKANO, T ;
MURATA, S .
JOURNAL OF CATALYSIS, 1992, 136 (01) :126-140
[3]  
AIKA K, 1990, B CHEM SOC JPN, V63, P1225
[4]   CHARACTERIZATION AND AMMONIA-SYNTHESIS ACTIVITY OF RUTHENIUM ZEOLITE CATALYSTS [J].
CISNEROS, MD ;
LUNSFORD, JH .
JOURNAL OF CATALYSIS, 1993, 141 (01) :191-205
[5]   Ammonia synthesis catalyzed by ruthenium supported on basic zeolites [J].
Fishel, CT ;
Davis, RJ ;
Garces, JM .
JOURNAL OF CATALYSIS, 1996, 163 (01) :148-157
[6]  
Foster A. I., 1979, US Patent, Patent No. 4163775
[7]   SURFACE CHARACTERIZATION OF THE RU3(CO)12/AL2O3 SYSTEM .2. STRUCTURE AND REACTIVITY OF THE SURFACE CARBONYLIC COMPLEXES [J].
GUGLIELMINOTTI, E ;
ZECCHINA, A ;
BOSSI, A ;
CAMIA, M .
JOURNAL OF CATALYSIS, 1982, 74 (02) :240-251
[8]   SURFACE CHARACTERIZATION OF THE RU3(CO)12/AL2O3 SYSTEM .3. SURFACE-PROPERTIES AFTER FULL DECARBONYLATION AND REDUCTION [J].
GUGLIELMINOTTI, E ;
ZECCHINA, A ;
BOSSI, A ;
CAMIA, M .
JOURNAL OF CATALYSIS, 1982, 74 (02) :252-265
[9]   The kinetics of ammonia synthesis over Ru-based catalysts .1. The dissociative chemisorption and associative desorption of N-2 [J].
Hinrichsen, O ;
Rosowski, F ;
Hornung, A ;
Muhler, M ;
Ertl, G .
JOURNAL OF CATALYSIS, 1997, 165 (01) :33-44
[10]  
KHAJA MS, 1991, J MOL CATAL, V67, pL1