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231224s2016 xx |||||o 00| ||eng c |
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|a 10.1021/acs.langmuir.6b00013
|2 doi
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|a pubmed24n0863.xml
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|a (DE-627)NLM259092118
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|a (NLM)27046305
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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| 100 |
1 |
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|a Özkar, Saim
|e verfasserin
|4 aut
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| 245 |
1 |
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|a Palladium(0) Nanoparticle Formation, Stabilization, and Mechanistic Studies
|b Pd(acac)₂ as a Preferred Precursor, [Bu₄N]₂HPO₄ Stabilizer, plus the Stoichiometry, Kinetics, and Minimal, Four-Step Mechanism of the Palladium Nanoparticle Formation and Subsequent Agglomeration Reactions
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|c 2016
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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|a ƒa Online-Ressource
|b cr
|2 rdacarrier
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|a Date Completed 29.08.2016
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|a Date Revised 19.04.2016
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a Palladium(0) nanoparticles continue to be important in the field of catalysis. However, and despite the many prior reports of Pd(0)n nanoparticles, missing is a study that reports the kinetically controlled formation of Pd(0)n nanoparticles with the simple stabilizer [Bu4N]2HPO4 in an established, balanced formation reaction where the kinetics and mechanism of the nanoparticle-formation reaction are also provided. It is just such studies that are the focus of the present work. Specifically, the present studies reveal that Pd(acac)2, in the presence of 1 equiv of [Bu4N]2HPO4 as stabilizer in propylene carbonate, serves as a preferred precatalyst for the kinetically controlled nucleation following reduction under 40 ± 1 psig initial H2 pressure at 22.0 ± 0.1 °C to yield 7 ± 2 nm palladium(0) nanoparticles. Studies of the balanced stoichiometry of the Pd(0)n nanoparticle-formation reaction shows that 1.0 Pd(acac)2 consumes 1.0 equiv of H2 and produces 1.0 equiv of Pd(0)n while also releasing 2.0 ± 0.2 equiv of acetylacetone. The inexpensive, readily available HPO4(2-) also proved to be as effective a Pd(0)n nanoparticle stabilizer as the more anionic, sterically larger, "Gold Standard" stabilizer P2W15Nb3O62(9-). The kinetics and associated minimal mechanism of formation of the [Bu4N]2HPO4-stabilized Pd(0)n nanoparticles are also provided, arguably the most novel part of the present studies, specifically the four-step mechanism of nucleation (A → B, rate constant k1), autocatalytic surface growth (A + B → 2B, rate constant k2), bimolecular agglomeration (B + B → C, rate constant k3), and secondary autocatalytic surface growth (A + C → 1.5C, rate constant k4), where A is Pd(acac)2, B represents the growing, smaller Pd(0)n nanoparticles, and C represents the larger, most catalytically active Pd(0)n nanoparticles. Additional details on the mechanism and catalytic properties of the resultant Pd(0)n·HPO4(2-) nanoparticles are provided in this work
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|a Journal Article
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|a Research Support, Non-U.S. Gov't
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|a Research Support, U.S. Gov't, Non-P.H.S.
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| 700 |
1 |
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|a Finke, Richard G
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Langmuir : the ACS journal of surfaces and colloids
|d 1992
|g 32(2016), 15 vom: 19. Apr., Seite 3699-716
|w (DE-627)NLM098181009
|x 1520-5827
|7 nnns
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| 773 |
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|g volume:32
|g year:2016
|g number:15
|g day:19
|g month:04
|g pages:3699-716
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|u http://dx.doi.org/10.1021/acs.langmuir.6b00013
|3 Volltext
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