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Catalytically highly active top gold atom on palladium nanocluster

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TLDR
The 'crown-jewel' concept for preparation of catalytically highly Au-based colloidal catalysts is presented and results indicate that the genesis of the high activity of the catalysts could be ascribed to the presence of negatively charged top Au atoms.
Abstract
Catalysis using gold is emerging as an important field of research in connection with 'green' chemistry. Several hypotheses have been presented to explain the markedly high activities of Au catalysts. So far, the origin of the catalytic activities of supported Au catalysts can be assigned to the perimeter interfaces between Au nanoclusters and the support. However, the genesis of the catalytic activities of colloidal Au-based bimetallic nanoclusters is unclear. Moreover, it is still a challenge to synthesize Au-based colloidal catalysts with high activity. Here we now present the 'crown-jewel' concept (Supplementary Fig. S1) for preparation of catalytically highly Au-based colloidal catalysts. Au-Pd colloidal catalysts containing an abundance of top (vertex or corner) Au atoms were synthesized according to the strategy on a large scale. Our results indicate that the genesis of the high activity of the catalysts could be ascribed to the presence of negatively charged top Au atoms.

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Citations
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Single-atom catalysts: a new frontier in heterogeneous catalysis.

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Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles.

TL;DR: This Review will compare the results obtained from different systems and try to give a picture on how different types of metal species work in different reactions and give perspectives on the future directions toward better understanding of the catalytic behavior of different metal entities in a unifying manner.
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Single Cobalt Atoms with Precise N-Coordination as Superior Oxygen Reduction Reaction Catalysts

TL;DR: Durability tests revealed that the Co single atoms exhibit outstanding chemical stability during electrocatalysis and thermal stability that resists sintering at 900 °C, which could facilitate new discoveries at the atomic scale in condensed materials.
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Atomically Precise Clusters of Noble Metals: Emerging Link between Atoms and Nanoparticles

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References
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Journal ArticleDOI

Shape-Controlled Synthesis of Gold and Silver Nanoparticles

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.
Book

Electron Energy-Loss Spectroscopy in the Electron Microscope

TL;DR: In this article, the authors present an overview of the basic principles of energy-loss spectroscopy, including the use of the Wien filter, and the analysis of the inner-shell of the detector.
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Solvent-Free Oxidation of Primary Alcohols to Aldehydes Using Au-Pd/TiO2 Catalysts

TL;DR: It is shown that Au/Pd-TiO2 catalysts give very high turnover frequencies (up to 270,000 turnovers per hour) for the oxidation of alcohols, including primary alkyl alcohols and the addition of Au to Pd nanocrystals improved the overall selectivity.
Journal ArticleDOI

Identification of Active Gold Nanoclusters on Iron Oxide Supports for CO Oxidation

TL;DR: High catalytic activity for carbon monoxide oxidation is correlated with the presence of bilayer clusters that are ∼0.5 nanometer in diameter and contain only ∼10 gold atoms, consistent with that demonstrated previously with the use of model catalyst systems.
Journal ArticleDOI

When Gold Is Not Noble: Nanoscale Gold Catalysts

TL;DR: In this article, temperature-programmed reaction studies of the catalyzed combustion of CO on size-selected small monodispersed Aun (n ≤ 20) gold clusters supported on magnesia, and first-principle simulations reveal the microscopic origins of the observed unusual catalytic activity, with Au8 being the smallest catalytically active size.
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