Abstract
Capping ligands are crucial to synthesizing colloidal nanoparticles with functional properties. However, the synergistic effect between different ligands and their distribution on crystallographic surfaces of nanoparticles during colloidal synthesis is still unclear despite powerful spectroscopic techniques, due to a lack of direct imaging techniques. In this study, atom probe tomography is adopted to investigate the three-dimensional atomic-scale distribution of two of the most common types of these ligands, cetrimonium (C19H42N) and halide (Br and Cl) ions, on Pd nanoparticles. The results, validated using density functional theory, demonstrate that the Br anions adsorbed on the nanoparticle surfaces promote the adsorption of the cetrimonium cations through electrostatic interactions, stabilizing the Pd {111} facets. In contrast, the Cl anions are not strongly adsorbed onto the Pd surfaces. The high density of adsorbed cetrimonium cations for Br anion additions results in the formation of multiple-twinned nanoparticles with superior oxidation resistance.
Highlights
Capping ligands are crucial to synthesizing colloidal nanoparticles with functional properties
Among the several nanomaterials reported to date, colloidal nanoparticles (NPs) are attractive since they can be synthesized in large quantities at reasonable costs and their size, shape, and properties can be carefully tailored through optimized growth recipes[5]
Capping ligands are indispensable for synthesizing colloidal NPs, little is known about their adsorption behavior on different crystallographic facets, especially at the atomic scale
Summary
Capping ligands are crucial to synthesizing colloidal nanoparticles with functional properties. The research on nanomaterials was largely driven by their intriguing physical and chemical properties, such as the outstanding luminescence of semiconductor nanocrystals[1], the excellent energy storage performance of two-dimensional nanosheets[2], and the remarkable catalytic activity and selectivity of noble metal nanocatalysts[3,4]. These properties are usually ascribed to the limited size and high surface-to-volume ratio of nanomaterials, compared with their bulk counterparts. The lack of experimental data is attributed to limited spatial resolution and/or detection sensitivity of many of the analytical techniques used[30]
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