Zirconium oxides dispersed on silica derived from Cp(2)ZrCl(2), [(i-PrCp)(2)ZrH(mu-H)](2), and Zr(OEt)(4) characterized by X-ray absorption fine structure and catalytic ketonization of acetic acid

被引:36
作者
Okumura, K [1 ]
Iwasawa, Y [1 ]
机构
[1] UNIV TOKYO, GRAD SCH SCI, DEPT CHEM, BUNKYO KU, TOKYO 113, JAPAN
关键词
D O I
10.1006/jcat.1996.0400
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
Newly dispersed Zr oxides on SiO2 were prepared from Cp(2)ZrCl(2), [(i-PrCp)(2)ZrH(mu-H)](2), and Zr(OEt)(4) precursors and were characterized by X-ray absorption fine structure (XAFS) and catalytic ketonization of acetic acid. ZrCp(2)Cl(2) and [(i-PrCp)(2)Zr(mu-H)](2) precursors yielded monomeric Zr oxides with unsaturated coordination in low loadings, whereas Zr(OEt)(4) yielded Zr-oxide assemblies in octahedral symmetry independent of Zr loading up to 15 wt% Zr. The former catalysts were more active than the latter catalyst for ketonization of acetic acid. The catalytic ketonization was suggested to proceed via bidentate acetates adsorbed on neighboring Zr sites. (C) 1996 Academic Press, Inc.
引用
收藏
页码:440 / 448
页数:9
相关论文
共 52 条
[1]   STRUCTURE OF ONE-ATOMIC-LAYER TITANIUM-OXIDE ON SILICON-OXIDE AND ITS PALLADIUM-MEDIATED RESTRUCTURING [J].
ASAKURA, K ;
INUKAI, J ;
IWASAWA, Y .
JOURNAL OF PHYSICAL CHEMISTRY, 1992, 96 (02) :829-834
[2]   SELECTIVE ISOPENTANE FORMATION FROM CH3OH ON A NEW ONE-ATOMIC LAYER ZrO2/ZSM-5 HYBRID CATALYST [J].
Asakura, Kiyotaka ;
Aoki, Mutsuto ;
Iwasawa, Yasuhiro .
CATALYSIS LETTERS, 1988, 1 (11) :395-403
[3]   THE SUPERACIDITY OF SULFATED ZIRCONIA - AN AB-INITIO QUANTUM-MECHANICAL STUDY [J].
BABOU, F ;
BIGOT, B ;
SAUTET, P .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (44) :11501-11509
[4]   ELECTROPHILIC CHLORINATION OF METHANE OVER SUPERACIDIC SULFATED ZIRCONIA [J].
BATAMACK, P ;
BUCSI, I ;
MOLNAR, A ;
OLAH, GA .
CATALYSIS LETTERS, 1994, 25 (1-2) :11-19
[5]   CHARACTERIZATION OF THE ACID STRENGTH OF SIO2-ZRO2 MIXED OXIDES [J].
BOSMAN, HJM ;
KRUISSINK, EC ;
VANDERSPOEL, J ;
VANDENBRINK, F .
JOURNAL OF CATALYSIS, 1994, 148 (02) :660-672
[6]   SUPERACID AND CATALYTIC PROPERTIES OF SULFATED ZIRCONIA [J].
CHEN, FR ;
COUDURIER, G ;
JOLY, JF ;
VEDRINE, JC .
JOURNAL OF CATALYSIS, 1993, 143 (02) :616-626
[7]   SYNTHESIS AND REACTIVITY OF NEW ACHIRAL AND CHIRAL SUBSTITUTED DIHYDRIDOZIRCONOCENES AND -HAFNOCENES [J].
COUTURIER, S ;
TAINTURIER, G ;
GAUTHERON, B .
JOURNAL OF ORGANOMETALLIC CHEMISTRY, 1980, 195 (03) :291-306
[8]   TPD AND HREELS INVESTIGATION OF THE REACTION OF FORMIC-ACID ON ZRO2(100) [J].
DILARA, PA ;
VOHS, JM .
JOURNAL OF PHYSICAL CHEMISTRY, 1993, 97 (49) :12919-12923
[9]   SKELETAL ISOMERIZATION OF HYDROCARBONS OVER ZIRCONIUM-OXIDE PROMOTED BY PLATINUM AND SULFATE ION [J].
EBITANI, K ;
KONISHI, J ;
HATTORI, H .
JOURNAL OF CATALYSIS, 1991, 130 (01) :257-267
[10]   STABILIZATION OF TETRAGONAL STRUCTURE IN ZIRCONIA MICROCRYSTALS [J].
GARVIE, RC .
JOURNAL OF PHYSICAL CHEMISTRY, 1978, 82 (02) :218-224