Interrogating the catalytic mechanism of nanoparticle mediated Stille coupling reactions employing bio-inspired Pd nanocatalysts.
| Autor: | Pacardo DB; Department of Chemistry, University of Kentucky, 101 Chemistry-Physics Building, Lexington, Kentucky 40506-0055, USA., Slocik JM, Kirk KC, Naik RR, Knecht MR |
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| Jazyk: | angličtina |
| Zdroj: | Nanoscale [Nanoscale] 2011 May; Vol. 3 (5), pp. 2194-201. Date of Electronic Publication: 2011 Apr 01. |
| DOI: | 10.1039/c1nr10089k |
| Abstrakt: | To address issues concerning the global environmental and energy state, new catalytic technologies must be developed that translate ambient and efficient conditions to heavily used reactions. To achieve this, the structure/function relationship between model catalysts and individual reactions must be critically discerned to identify structural motifs responsible for the reactivity. This is especially true for nanoparticle-based systems where this level of information remains limited. Here we present evidence indicating that peptide-capped Pd nanoparticles drive Stille C-C coupling reactions via Pd atom leaching. Through a series of reaction studies, the materials are shown to be optimized for reactivity under ambient conditions where increases in temperature or catalyst concentration deactivate reactivity due to the leaching process. A quartz crystal microbalance analysis demonstrates that Pd leaching occurs during the initial oxidative addition step at the nanoparticle surface by aryl halides. Together, this suggests that peptide-based materials may be optimally suited for use as model systems to isolate structural motifs responsible for the generation of catalytically reactive materials under ambient synthetic conditions. (© The Royal Society of Chemistry 2011) |
| Databáze: | MEDLINE |
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