Effect of the reduction-preparation method on the surface states and catalytic properties of supported-nickel particles

被引:14
作者
Cerro-Alarcon, M.
Bachiller-Baeza, B.
Guerrero-Ruiz, A.
Rodriguez-Ramos, I.
机构
[1] CSIC, Inst Catalisis & Petr Quim, Madrid 28049, Spain
[2] Univ Nacl Educ Distancia, Grp Diseno & Aplicac Catalizadores Heterogeneos, Unidad Asociada ICP, CSIC, E-28040 Madrid, Spain
[3] Univ Nacl Educ Distancia, Dept Quim Inorgan & Quim Tecn, Fac Ciencias, E-28040 Madrid, Spain
关键词
carbon-supported metal catalysts; high surface area-graphite; nickel; hydrazine; surface characterisation; CO adsorption; microcalorimetry; XPS; citral hydrogenation;
D O I
10.1016/j.molcata.2006.05.056
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
Several high surface area graphite-supported Ni catalysts were prepared and reduced by different methods. Samples were prepared by impregnation of the support and then submitted to traditional H-2 flow reduction at high temperature or to reduction with aqueous hydrazine at low temperature, and compared with a sample prepared by the deposition-precipitation method by means of the reduction of the dissolved Ni precursor by hydrazine at low temperature. The surface of these catalysts was characterised by means of CO adsorption microcalorimetry and by X-ray photoelectron spectroscopy (XPS), and a correlation of the results obtained with those on the selective hydrogenation of citral can be done. In this sense, only Ni-0 sites were detected at the surface of the Ni catalysts prepared by reduction with hydrogen leading to high catalytic activities and selectivity towards citronellal formation, while Ni oxidised species are also present (and are major) for catalysts prepared by reduction with hydrazine, what leads to an enhanced selectivity towards the formation of the unsaturated alcohols, geraniol and nerol. The oxidation of these latter catalysts seems to be only superficial, as suggested by the absence of H-2 consumption peaks in the TPR experiments. The presence of Ni-0 sites over these latter catalysts was not detected by XPS, thus our study proves that CO adsorption microcalorimetry is a very powerful tool for surface characterisation of heterogeneous catalysts. (c) 2006 Elsevier B.V. All rights reserved.
引用
收藏
页码:221 / 230
页数:10
相关论文
共 46 条
[1]   ADSORPTION MICROCALORIMETRY AND STICKING PROBABILITIES ON METAL SINGLE-CRYSTAL SURFACES [J].
ALSARRAF, N ;
STUCKLESS, JT ;
WARTNABY, CE ;
KING, DA .
SURFACE SCIENCE, 1993, 283 (1-3) :427-437
[2]   CALORIMETRIC ADSORPTION HEATS ON LOW-INDEX NICKEL SURFACES [J].
ALSARRAF, N ;
KING, DA .
SURFACE SCIENCE, 1994, 307 :1-7
[3]  
ANDERSEN PJ, 1994, CATALYSIS, V11, P441
[4]  
Anderson J.R., 1975, STRUCTURE METALLIC C, P289
[5]   Interaction of carbon dioxide with the surface of zirconia polymorphs [J].
Bachiller-Baeza, B ;
Rodriguez-Ramos, I ;
Guerrero-Ruiz, A .
LANGMUIR, 1998, 14 (13) :3556-3564
[6]   Hydrogenation of citral on activated carbon and high-surface-area graphite-supported ruthenium catalysts modified with iron [J].
Bachiller-Baeza, B ;
Guerrero-Ruiz, A ;
Wang, P ;
Rodríguez-Ramos, I .
JOURNAL OF CATALYSIS, 2001, 204 (02) :450-459
[7]   Influence of Mg and Ce addition to ruthenium based catalysts used in the selective hydrogenation of α,β-unsaturated aldehydes [J].
Bachiller-Baeza, B ;
Rodríguez-Ramos, I ;
Guerrero-Ruiz, A .
APPLIED CATALYSIS A-GENERAL, 2001, 205 (1-2) :227-237
[8]   Platinum/graphite nanofiber catalysts of various structure:: Characterization and catalytic properties [J].
Baker, RTK ;
Rodriguez, N ;
Mastalir, A ;
Wild, U ;
Schlögl, R ;
Wootsch, A ;
Paál, Z .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (38) :14348-14355
[9]   Adsorption of CO and NO on NiO(111)/Ni(111) surface studied by infrared-visible sum frequency generation spectroscopy [J].
Bandara, A ;
Dobashi, S ;
Kubota, J ;
Onda, K ;
Wada, A ;
Domen, K ;
Hirose, C ;
Kano, SS .
SURFACE SCIENCE, 1997, 387 (1-3) :312-319
[10]   ESCA STUDY OF TERMINATION OF PASSIVATION OF ELEMENTAL METALS [J].
BARR, TL .
JOURNAL OF PHYSICAL CHEMISTRY, 1978, 82 (16) :1801-1810