EFFECTS OF IRON-OXYGEN PRECURSOR PHASE ON CARBON-CARBON BOND SCISSION IN NAPHTHYLBIBENZYLMETHANE

被引:14
作者
LINEHAN, JC
MATSON, DW
DARAB, JG
机构
[1] Pacific Northwest Lab, Richland, WA
关键词
D O I
10.1021/ef00043a010
中图分类号
TE [石油、天然气工业]; TK [能源与动力工程];
学科分类号
0807 ; 0820 ;
摘要
Eleven iron-oxygen compounds prepared using standard laboratory syntheses were tested as precursors for carbon-carbon bond scission catalysts with the coal model compound naphthylbibenzylmethane in the presence of elemental sulfur and a hydrogen-donating solvent. The structure of the iron-oxygen catalyst precursor was found to be the most significant factor determining the reactivity of the catalyst produced. The reactivity of the iron-oxygen compounds showed little : apparent correlation with surface area, iron content, or water content. The iron-containing single-phase materials with the best catalytic activity at 400 degrees C were determined to be ferric oxyhydroxysulfate (Fe8O8(OH)(8)SO4), six-line ferrihydrite, goethite ((alpha-FeOOH), and akaganeite (beta-FeOOH). The worst iron-oxygen compounds were found to be wustite (FeO), two-line ferrihydrite, magnetite (Fe3O4), and maghemite (gamma-Fe2O3). The general order of reactivity of the iron-oxygen compounds toward carbon-carbon bond scission was found to be proto-oxyhydroxides > oxyhydroxides > oxides. All of the iron-oxygen compounds tested were at least as active as metallic iron (alpha-Fe). All of the active I catalyst precursors produced similar distributions of organic reaction products from the model compound. The best catalyst precursor tested was ferric oxyhydroxysulfate, which formed a catalyst which selectively cleaved carbon-carbon bonds at the a-naphthyl-methylene (''a'') and the beta-naphthylmethylene (''b'') positions with a model compound consumption of greater than 90% under the test; conditions. The ferric oxyhydroxysulfate was found to contain a relatively large amount of water and small amount of iron, 18% and 43%, respectively, by weight.
引用
收藏
页码:56 / 62
页数:7
相关论文
共 39 条
[1]   CATALYSIS OF COAL HYDROLIQUEFACTION BY SYNTHETIC IRON CATALYSTS [J].
ANDRES, M ;
CHARCOSSET, H ;
CHICHE, P ;
DAVIGNON, L ;
DJEGAMARIADASSOU, G ;
JOLY, JP ;
PREGERMAIN, S .
FUEL, 1983, 62 (01) :69-72
[2]  
BI XX, 1991, ENERG FUEL, V5, P683
[3]  
BIGHAM JM, 1990, GEOCHIM COSMOCHIM AC, V54, P2743
[4]  
CUGINI AV, 1991, PREPR PAP AM CHEM SO, V36, P91
[5]  
DARAB JG, 1993, PREPR PAP AM CHEM SO, V38, P27
[6]   ROLE OF CATALYSIS IN COAL-LIQUEFACTION RESEARCH AND DEVELOPMENT [J].
DERBYSHIRE, F .
ENERGY & FUELS, 1989, 3 (03) :273-277
[7]   ACTIVATED RED MUD AS A CATALYST FOR THE HYDROGENATION OF COALS AND OF AROMATIC-COMPOUNDS [J].
EAMSIRI, A ;
JACKSON, WR ;
PRATT, KC ;
CHRISTOV, V ;
MARSHALL, M .
FUEL, 1992, 71 (04) :449-453
[8]   MODELING COAL-LIQUEFACTION .1. DECOMPOSITION OF 4-(1-NAPHYTYLMETHYL)BIBENZYL CATALYZED BY CARBON-BLACK [J].
FARCASIU, M ;
SMITH, C .
ENERGY & FUELS, 1991, 5 (01) :83-87
[9]   IRON COMPOUNDS AND IRON CATALYSTS - ACTIVITY IN REACTIONS RELEVANT TO DIRECT COAL-LIQUEFACTION [J].
FARCASIU, M ;
SMITH, C ;
PRADHAN, VR ;
WENDER, I .
FUEL PROCESSING TECHNOLOGY, 1991, 29 (03) :199-208
[10]  
FARCASIU M, 1993, PREP PAP AM CHEM SOC, V38, P53