期刊
CHEMISTRY OF MATERIALS
卷 20, 期 16, 页码 5218-5228出版社
AMER CHEMICAL SOC
DOI: 10.1021/cm8004198
关键词
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资金
- Robert A. Welch Foundation [F-1288]
- National Science Foundation [053 1030]
- DOE-BES [DE-FG0203ER15468, DE-FG02-03ER15468, DE-FG02-03ER15476]
- DOE [DE-FG02-05ER15688, DE-AC02-98CH10886, W-31-109-ENG-38]
- CMU [REF 60628]
- SPRING
In this article, we provide a detailed description of the synthesis and properties of Pt dendrimer-encapsulated nanoparticles (DENs) prepared using sixth-generation, hydroxyl-terminated, poly(amidoamine) (PAMAM) dendrimers (G6-OH) and three different PtCl42-/G6-OH ratios: 55, 147, and 240. Results obtained from UV-vis spectroscopy, X-ray photoelectron spectroscopy, electron microscopy, X-ray absorption spectroscopy, and high-energy X-ray diffraction show that only a fraction of the Pt2+/dendrimer precursors are reduced by BH4- and that the reduction process is highly heterogeneous. That is, after reduction each Pt2+/dendrimer precursor complex is either fully reduced, to yield a DEN having a size and structure consistent with the original PtCl42-/dendrimer ratio used for the synthesis, or the precursor is not reduced at at all. This result is consistent with an autocatalytic process that entails slow formation of a nascent catalytic Pt seed within the dendrimer, followed by rapid, catalytic reduction of nearby Pt2+ ions. Details concerning the formation of the Pt2+/dendrimer precursor are also discussed.
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