AI Article Synopsis
- Understanding the adsorption mechanism of dodecanethiol ligands on 3.3 nm gold nanocrystals (Au NCs) is crucial for optimizing their properties.
- The study uses in situ X-ray absorption techniques to reveal a two-step adsorption process, starting with a rapid increase in ligand coverage followed by a slower approach towards saturation.
- The first stage involves quick adsorption at corner and edge sites, leading to significant changes in Au-Au bond lengths, while the second stage fits a Langmuir kinetic model, indicating preferred adsorption at specific surface sites.
Article Abstract
Understanding the kinetic mechanism during ligand adsorption on gold nanocrystals is important for designing and fine-tuning their properties and implications. Here, we report a kinetic study on the adsorption process of dodecanethiol ligands on Au nanocrystals of 3.3 nm by an in situ time-resolved X-ray absorption fine structure technique. A two-step process of dodecanethiol adsorption on Au NC surfaces is proposed based on the obtained ligand coverage, which shows a quick increase from 0 to 0.40 within the first 20 min, followed by a much slower increase to the limiting value of 0.94. In-depth analysis suggests that the first stage involves the quick adsorption of dodecanethiol to the corner and edge sites of Au NCs surfaces, leading to remarkable surface Au-Au bond length relaxation (from 2.79 to 2.81 Å) and pronounced gold-to-ligand charge transfer. The second step that corresponds to the much slower adsorption process to the surface facets could be described by the Langmuir kinetics equation with an adsorption rate constant of 0.0132 min(-1) and an initial coverage of 0.41, in good agreement with the initially preferable adsorption of thiols to the most favorable sites.
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| http://dx.doi.org/10.1039/c3nr04020h | DOI Listing |
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