COLL 132 |
| Krijn P. de Jong, A. Jos van Dillen, J. Harry Bitter, Marjolein L. Toebes, and Martijn K. van der Lee. Department of Inorganic Chemistry, Utrecht University, Sorbonnelaan 16, P.O. Box 80083, 3508 TB Utrecht, Netherlands |
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Homogeneous deposition precipitation (HDP) is a versatile tool to prepare a metal(oxide)-on-support catalyst characterized by narrow particle size distributions and high loadings. Originally HDP has been developed for oxidic supports. Using the decomposition of urea, in the past nickel-on-silica catalyst have been prepared with loadings up to 50 wt% Ni. The deposition process mostly involved quite strong interactions during precipitation between the aqueous metal precursor and the support which often led to a mixed-compound formation such as nickel hydrosilicates. In this work we have carried out a fundamental study whether or not HDP can be used with graphite-like support such as carbon nanofibers (CNF) and carbon nanotubes (CNT). The key problem of these supports is that they are chemically very inert and even hydrophobic due to the non-polar surface. Therefore, treatment of the CNF in nitric acid at reflux conditions was used to introduce carboxylic acid groups (1-3 nm-2). Using nickel nitrate and urea hydrolysis in a suspension of CNF led to nucleation of Ni(OH)2 at the CNF surface. Loadings were varied in the range 10-50 wt% Ni. After reduction in H2 metallic nickel particles of 5-9 nm very uniformly distributed over the carbon nanofibers were obtained. Chemical or thermal removal of the –COOH groups from the surface of the CNF led to precipitation of large Ni(OH)2 platelets separate from the CNF support. Clearly, the interaction between the carboxylic acid groups and the nickel precursor is gentle but crucial in HDP using graphitic supports. In this talk it is shown that next to nickel also noble metals (Pt, Ru) can be deposited using HDP which gives rise to very small metal particles (1-2 nm) that are extremely thermally stable (~1000 K) on the CNF support. |
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The Science and Engineering of Catalyst Preparation
8:30 AM-11:55 AM, Monday, March 29, 2004 Marriott -- Orange County 3, Oral
Division of Colloid and Surface Chemistry |