Journal ArticleDOI
Single-molecule nanocatalysis reveals heterogeneous reaction pathways and catalytic dynamics
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The results exemplify the power of the single-molecule approach in revealing the interplay of catalysis, heterogeneous reactivity and surface structural dynamics in nanocatalysis.Abstract:
Nanoparticles are important catalysts for many chemical transformations. However, owing to their structural dispersions, heterogeneous distribution of surface sites and surface restructuring dynamics, nanoparticles are intrinsically heterogeneous and challenging to characterize in ensemble measurements. Using a single-nanoparticle single-turnover approach, we study the redox catalysis of individual colloidal Au nanoparticles in solution, using single-molecule detection of fluorogenic reactions. We find that for product generation, all Au nanoparticles follow a Langmuir-Hinshelwood mechanism but with heterogeneous reactivity; and for product dissociation, three nanoparticle subpopulations are present that show heterogeneous reactivity between multiple dissociation pathways with distinct kinetics. Correlation analyses of single-turnover waiting times further reveal activity fluctuations of individual Au nanoparticles, attributable to both catalysis-induced and spontaneous dynamic surface restructuring that occurs at different timescales at the surface catalytic and product docking sites. The results exemplify the power of the single-molecule approach in revealing the interplay of catalysis, heterogeneous reactivity and surface structural dynamics in nanocatalysis.read more
Citations
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Kinetic Analysis of Catalytic Reduction of 4-Nitrophenol by Metallic Nanoparticles Immobilized in Spherical Polyelectrolyte Brushes
TL;DR: In this article, a study on the catalytic reduction of 4-nitrophenol by sodium borohydride in the presence of metal nanoparticles is presented, where the nanoparticles are embedded in spherical polyelectrolyte brushes.
Journal ArticleDOI
Synthesis and catalytic properties of metal nanoparticles: Size, shape, support, composition, and oxidation state effects
TL;DR: In this paper, the authors examine the role played by the particle structure and morphology (size and shape), its chemical composition and oxidation state, and the effect of the cluster support.
Journal ArticleDOI
Optical detection of single non-absorbing molecules using the surface plasmon resonance of a gold nanorod.
TL;DR: The plasmonic detection of single molecules in real time without the need for labelling or amplification is reported, and the binding of single proteins is detected by monitoring the plAsmon resonance of the nanorod with a sensitive photothermal assay.
Journal ArticleDOI
Basic concepts and recent advances in nitrophenol reduction by gold- and other transition metal nanoparticles
TL;DR: In this paper, the basic concepts and recent developments and advances of gold nanoparticle (AuNP)-catalyzed 4-nitrophenol (4-NP) reduction to 4-aminophenol by sodium borohydride, including the catalytic mechanism, the variety of stabilizers, and dendritic, natural and heterogeneous AuNP supports are presented.
Journal ArticleDOI
Molecular and Supramolecular Networks on Surfaces: From Two-Dimensional Crystal Engineering to Reactivity
TL;DR: Recent developments in the design and functionality of supramolecular surface patterns are highlighted, with special attention paid to those networks which are chiral or contain a high degree of porosity as well as to the reactivity, which is one of the most important recent developments in supramolescular surface chemistry.
References
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Journal ArticleDOI
Chemistry and properties of nanocrystals of different shapes.
TL;DR: The interest in nanoscale materials stems from the fact that new properties are acquired at this length scale and, equally important, that these properties are equally important.
Journal ArticleDOI
Shape-Controlled Synthesis of Gold and Silver Nanoparticles
Yugang Sun,Younan Xia +1 more
TL;DR: Monodisperse samples of silver nanocubes were synthesized in large quantities by reducing silver nitrate with ethylene glycol in the presence of poly(vinyl pyrrolidone) (PVP), characterized by a slightly truncated shape bounded by {100, {110}, and {111} facets.
Journal ArticleDOI
Identification of active edge sites for electrochemical H2 evolution from MoS2 nanocatalysts.
Thomas F. Jaramillo,Kristina Pilt Jørgensen,Jacob Lindner Bonde,Jane Hvolbæk Nielsen,Sebastian Horch,Ib Chorkendorff +5 more
TL;DR: The active site for hydrogen evolution, a reaction catalyzed by precious metals, on nanoparticulate molybdenum disulfide (MoS2) is determined by atomically resolving the surface of this catalyst before measuring electrochemical activity in solution.
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