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• W1986811838 endingPage "3303" @default.
• W1986811838 startingPage "3297" @default.
• W1986811838 abstract "The knowledge of intramolecular dynamics, geo-metric confinement, and structure of surface-bound ligands are important factors for understanding surface chemistry, catalysis, and design of catalytically optimized nanoparticles. In this report, intramolecular dynamics of perdeuterated triphenylphosphine ligands, d15-(PPh3), bound to the surface of gold nanoparticles (AuNPs) are characterized by pulsed deuteron nuclear magnetic resonance (2H NMR) in the solid state. The 2H quadrupolar echo Fourier transform NMR line shapes indicate fast 180° flip dynamics (π flip) of phenyl rings in surface-bound d15-(PPh3) ligands about the P−C bond at the rate of k ≥ 7 × 107 s−1. In contrast, the d15-(PPh3)AuCl complex, a model compound that is also present in this nanoparticle system, does not exhibit measurable π flips on the time scale sampled by the experiment (∼10−5 s). Its phenyl rings appear rigid from ambient temperature up to 386 K. The experimental 2H NMR line shape results are consistent with a theoretical model of phenyl rings undergoing rapid π flips. The deuterons of the phenyl ring experiencing the rapid motion of surface-bound d15-(PPh3) ligands in a high magnetic field exhibit substantially shortened spin−lattice (T1) relaxation times of 44 ms in the ortho and meta positions and 2.5 s for the para position in comparison to the very long T1 time in excess of 103 s observed in the rigid d15-(PPh3)AuCl complex. The difference in T1 by several orders of magnitude further confirms the rapid phenyl ring dynamics of ligands bound through gold−phosphorus bond on the surfaces. The observation of uninterrupted rapid motion in phenyl rings suggests the presence of well-separated ligands and availability of low-coordinated surface gold atoms. These parameters are critically important in the catalytic activity of ligand-capped nanoparticles." @default.
• W1986811838 created "2016-06-24" @default.
• W1986811838 creator A5003847596 @default.
• W1986811838 creator A5053925403 @default.
• W1986811838 creator A5073730354 @default.
• W1986811838 date "2011-02-04" @default.
• W1986811838 modified "2023-09-27" @default.
• W1986811838 title "Intramolecular Ligand Dynamics in <i>d</i>₁₅-(PPh₃)-Capped Gold Nanoparticles Investigated by ²H NMR" @default.
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• W1986811838 doi "https://doi.org/10.1021/jp110686a" @default.
• W1986811838 hasPublicationYear "2011" @default.
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