Thiolate adsorption on Au(${\bm {hkl}}$hkl) and equilibrium shape of large thiolate-covered gold nanoparticles

Barmparis, Georgios D.; Honkala, Karoliina; Remediakis, Ioannis N.

doi:10.1063/1.4790368

Cited by 36 publications

(55 citation statements)

References 63 publications

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“…The adsorption of alkylthiols onto stepped surfaces has been infrequently studied experimentally, but theoretical calculations indicate that in the limit of a small adsorbate (MeS), adsorption typically occurs on 2-fold or bridge sites on the stepped surfaces examined. 42 The differences in the adsorption energy are in-line with the desorption potentials measured here given that the resolution of binding energies are The self-assembly of alkylthiols onto gold shows an influence of the pzc (or dbb) and intermolecular interaction on the energetics of desorption. To demonstrate that the measurements made on these single crystal gold bead electrodes are indeed strongly influenced by the surface crystallography, the same analysis was performed on a SAM created from fluorophore labeled Aib peptides.…”

Section: ■ Results and Discussionmentioning

confidence: 60%

Influence of Surface Structure on Single or Mixed Component Self-Assembled Monolayers via in Situ Spectroelectrochemical Fluorescence Imaging of the Complete Stereographic Triangle on a Single Crystal Au Bead Electrode

Yu¹,

Casanova-Moreno²,

Guryanov

et al. 2014

J. Am. Chem. Soc.

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The use of a single crystal gold bead electrode is demonstrated for characterization of self-assembled monolayers (SAM)s formed on the bead surface expressing a complete set of face centered cubic (fcc) surface structures represented by a stereographic projection. Simultaneous analysis of many crystallographic orientations was accomplished through the use of an in situ fluorescence microscopic imaging technique coupled with electrochemical measurements. SAMs were prepared from different classes of molecules, which were modified with a fluorescent tag enabling characterization of the influence of electrical potential and a direct comparison of the influence of surface structure on SAMs adsorbed onto low index, vicinal and chiral surfaces. The assembly of alkylthiol, Aib peptide and DNA SAMs are studied as a function of the electrical potential of the interface revealing how the organization of these SAMs depend on the surface crystallographic orientation, all in one measurement. This approach allows for a simultaneous determination of SAMs assembled onto an electrode surface onto which the whole fcc stereographic triangle can be mapped, revealing the influence of intermolecular interactions as well as the atomic arrangement of the substrate. Moreover, this method enables study of the influence of the Au surface atom arrangement on SAMs that were created and analyzed, both under identical conditions, something that can be challenging for the typical studies of this kind using individual gold single crystal electrodes. Also demonstrated is the analysis of a SAM containing two components prepared using thiol exchange. The two component SAM shows remarkable differences in the surface coverage, which strongly depends on the surface crystallography enabling estimates of the thiol exchange energetics. In addition, these electrode surfaces enable studies of molecular adsorption onto the symmetry related chiral surfaces since more than one stereographic triangle can be imaged at the same time. The ability to observe a SAM modified surface that contains many complete fcc stereographic triangles will facilitate the study of the single and multicomponent SAMs, identifying interesting surfaces for further analysis.

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Section: ■ Results and Discussionmentioning

confidence: 60%

Influence of Surface Structure on Single or Mixed Component Self-Assembled Monolayers via in Situ Spectroelectrochemical Fluorescence Imaging of the Complete Stereographic Triangle on a Single Crystal Au Bead Electrode

Yu¹,

Casanova-Moreno²,

Guryanov

et al. 2014

J. Am. Chem. Soc.

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“…1). However, due to the fact given in brackets in point 2, the equilibrium shape rarely contains faces with indexes higher than three [17]. …”

Section: Reviewmentioning

confidence: 99%

Nanoparticle shapes by using Wulff constructions and first-principles calculations

Barmparis

Łodziana

López

et al. 2015

Beilstein J. Nanotechnol.

221

162

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Summary Background: The majority of complex and advanced materials contain nanoparticles. The properties of these materials depend crucially on the size and shape of these nanoparticles. Wulff construction offers a simple method of predicting the equilibrium shape of nanoparticles given the surface energies of the material. Results: We review the mathematical formulation and the main applications of Wulff construction during the last two decades. We then focus to three recent extensions: active sites of metal nanoparticles for heterogeneous catalysis, ligand-protected nanoparticles generated as colloidal suspensions and nanoparticles of complex metal hydrides for hydrogen storage. Conclusion: Wulff construction, in particular when linked to first-principles calculations, is a powerful tool for the analysis and prediction of the shapes of nanoparticles and tailor the properties of shape-inducing species.

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“…Fig. 5 presents the free energy for hydrogen adsorption on the terrace Au(111) (solid line) and few commonly studied stable stepped gold surfaces [53,54] (non-solid lines). The DG H* on the terrace Au(111) surface is calculated to be 0.45 eV following the work of Nørskov [16].…”

mentioning

confidence: 99%

Activation Effect of Electrochemical Cycling on Gold Nanoparticles towards the Hydrogen Evolution Reaction in Sulfuric Acid

Wang

Sun

Liao

et al. 2016

Electrochimica Acta

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A B S T R A C TThis article reports a study of electrochemical cycling effects on hydrogen evolution catalytic activity of gold nanoparticles in sulfuric acid. We found that after cycling within the double layer regime, up to 0.64 V vs RHE, there is a dramatic effect on the HER activity of gold nanoparticles: 128 mV drop of the overpotential, a decrease of 23 mV/dec for the Tafel slope as well as a nearly twenty times increase of the turn-over frequency (TOF). This enhanced activity is tentatively assigned to the formation of stepped like structures by the consecutive electrochemical cycling in the double layer region.

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Thiolate adsorption on Au(${\bm {hkl}}$hkl) and equilibrium shape of large thiolate-covered gold nanoparticles

Cited by 36 publications

References 63 publications

Influence of Surface Structure on Single or Mixed Component Self-Assembled Monolayers via in Situ Spectroelectrochemical Fluorescence Imaging of the Complete Stereographic Triangle on a Single Crystal Au Bead Electrode

Influence of Surface Structure on Single or Mixed Component Self-Assembled Monolayers via in Situ Spectroelectrochemical Fluorescence Imaging of the Complete Stereographic Triangle on a Single Crystal Au Bead Electrode

Nanoparticle shapes by using Wulff constructions and first-principles calculations

Activation Effect of Electrochemical Cycling on Gold Nanoparticles towards the Hydrogen Evolution Reaction in Sulfuric Acid

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