Polyelectrolyte-assisted soft reduced process for Pt-Cu nanoclusters with enhanced electrocatalytic activity for the methanol oxidation reaction
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A fundamental understanding of the structural growth of thiolate-protected gold nanoclusters not only benefits experimental synthesis but also will advance the methodology for structural predictions and for rational design of highly stable nanoclusters. Herein, we report numerous new structures (11 total) of thiolate-protected gold nanoclusters predicted from theoretical modulation of the double-helical cores of experimentally determined nanoclusters. Among these newly predicted structures, Au32(SR)22, Au40(SR)26, and Au48(SR)30 are obtained by adding a defective layer containing 4 gold atoms on a structural sequence of experimentally crystallized nanoclusters, namely, Au28(SR)20, Au36(SR)24, and Au44(SR)28. The generic growth pattern underlying this sequence of nanoclusters can be viewed as adding the highly stable tetrahedral Au4 unit on the double-helical cores. Likewise, the other eight newly predicted structures, including two groups of isomeric structures corresponding to the sequence of experimentally determined Au28(SR)20, Au36(SR)24, Au44(SR)28, and Au52(SR)32 nanoclusters, are successfully predicted. Density functional theory calculations show that these 11 newly predicted nanoclusters exhibit large highest occupied molecular orbital-lowest unoccupied molecular orbital gaps and all-positive harmonic vibrational frequencies, suggesting their high chemical stabilities. Additional analyses on the structures and properties suggest that these newly predicted nanoclusters are very likely to be synthesized in the laboratory. Confirmation by experiments would validate the new strategy for structural prediction of thiolate-protected gold nanoclusters by taking advantage of a large structure database of crystallized ligand-protected gold nanoclusters with a variety of gold cores.
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The electrochemical behavior of the methanol oxidation on the platinum electrode with different concentration H2SO4 solution was studied by using cycl ic voltammetry. The solution acidity scarcely affected the oxidation characteris tic of methanol on platinum. The peak potentials for methanol oxidation changed little, and reached 0.17 V and -0.03 V(vs. Hg / Hg2SO4) for potential forward an d backward scan respectively. However, the solution acidity affected the rate of methanol oxidation on platinum. The current of methanol oxidation increased wit h the decreasing of the solution acidity. This phenomenon could be explained by the difference of the formation of platinum oxide on platinum.
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Data on the structures and properties of nanoclusters and nanocluster systems are analysed. A classification of nanoclusters and nanosystems based on the method of their preparation is proposed. Methods for assembling nanoclusters to give nanostructures, the main principles of assembling and the types of nanosystems are described. The appearance of new properties upon combination of nanoclusters into a nanosystem is noted. The bibliography includes 274 references.
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Abstract It has been found that the bimetallic nanoclusters often have so-called core/shell structure if they are prepared by alcohol-reduction of two kinds of noble metal ions in the presence of a water-soluble polymer like poly(N-vinyl-2-pyrolidone)(PVP), and that the core/ shell structured bimetallic nanoclusters have much higher catalytic activity than the corresponding monometallic nanoclusters. Here, several kinds of monometallic and bimetallic nanoclusters are synthesized by the similar method, and the catalyses are measured. Thus, the colloidal dispersions of Au, Pt, Pd, Rh, and Ru monometallic, and Au/Pt, Au/Pd, Au/Rh, and Pt/Ru bimetallic nanoclusters were synthesized and applied as the catalysts for visible-light- induced hydrogen generation. The core/shell structures are analyzed mainly by UV–vis spectra. The rate of electron transfer from the methyl viologen cation radical to the metal nanoclusters is proportional to the hydrogen generation rate at the steady state. All the electrons accepted by the metal nanoclusters are used for the hydrogen generation. Both electron transfer and hydrogen generation rates increase when the bimetallic nanoclusters are used in place of the corresponding monometallic nanoclusters. The most active catalysts were Au/Rh and Pt/Ru bimetallic nanoclusters.
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Atomically precise noble metal nanoclusters are ultrasmall particles that are typically composed of tens to hundreds of metal atoms in the core (equivalent sizes 1–3 nm). This new class of nanomaterials is unique in that they are atomically precise and possess uniform structures, high stability, and attractive properties. Built on the significant success of Au nanoclusters, Ag nanoclusters have recently received increasing attention. The majority of reported silver nanocluster sizes exhibit molecular-like properties, whereas larger ones exhibit plasmons characteristic of metallic state (as opposed to molecular state in smaller sizes). Both molecular (i.e., nonmetallic) and metallic nanoclusters hold promise in a wide range of applications. To deepen the understanding of their physical and chemical properties, precise control over size and determination of the crystal structure are the top priorities. In recent developments, dozens of silver nanoclusters with definite formulas have been prepared through various strategies, albeit the structural determination still lags behind. In this short Review, we summarize the recent progress in ligand-protected silver nanoclusters, including the size-focusing synthetic methods, new sizes, structures, and properties.
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