Abstract
Adsorption plays vital roles in many processes including catalysis, sensing, and nanomaterials design. However, quantifying molecular adsorption, especially at the nanoscale, is challenging, hindering the exploration of its utilization on nanomaterials that possess heterogeneity across different length scales. Here we map the adsorption of nonfluorescent small molecule/ion and polymer ligands on gold nanoparticles of various morphologies in situ under ambient solution conditions, in which these ligands are critical for the particles’ physiochemical properties. We differentiate at nanometer resolution their adsorption affinities among different sites on the same nanoparticle and uncover positive/negative adsorption cooperativity, both essential for understanding adsorbate-surface interactions. Considering the surface density of adsorbed ligands, we further discover crossover behaviors of ligand adsorption between different particle facets, leading to a strategy and its implementation in facet-controlled synthesis of colloidal metal nanoparticles by merely tuning the concentration of a single ligand.
Highlights
Adsorption plays vital roles in many processes including catalysis, sensing, and nanomaterials design
Using COMPEITS (COMPetition-Enabled Imaging Technique with Super-resolution) that is capable of imaging nonfluorescent surface processes in situ and at nanometer resolution[11], we map the adsorption of small molecule/ion and polymer ligands on individual gold (Au) nanoparticles of various morphologies under ambient solution conditions (Fig. 1a)
We first examined the adsorption of cetyltrimethylammonium bromide (CTAB), a ligand widely used in Au nanoparticle synthesis and surface modification[5,18], on pseudospherical 5-nm Au nanoparticles using COMPEITS
Summary
Adsorption plays vital roles in many processes including catalysis, sensing, and nanomaterials design. Using COMPEITS (COMPetition-Enabled Imaging Technique with Super-resolution) that is capable of imaging nonfluorescent surface processes in situ and at nanometer resolution[11], we map the adsorption of small molecule/ion and polymer ligands on individual gold (Au) nanoparticles of various morphologies under ambient solution conditions (Fig. 1a). These ligands play critical roles in the shape-controlled synthesis, solution stabilization, surface functionalization, and catalytic poisoning of nanoparticles of various compositions[3,4,5,6,12]. If L adsorption is cooperative, h deviates from 1 and is the Hill coefficient of cooperativity: h > 1 for positive cooperativity; h < 1 for negative cooperativity[16,17]
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