Halide Anions as Shape-Directing Agents for Obtaining High-Quality Anisotropic Gold Nanostructures

DuChene, Joseph S.; Niu, Wenxin; Abendroth, John M.; Sun, Qi; Zhao, Wenbo; Huo, Fengwei; Wei, W. David

doi:10.1021/cm3020397

Cited by 187 publications

(206 citation statements)

References 67 publications

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“…These observations indicate the following: (i) The three corners are not equally active initially. This could be attributed to the heterogeneous imperfections of these corners (31,32). However, over time all three corners show similar reactivity (Fig.…”

Section: Significancementioning

confidence: 95%

Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity

Zhang

Lucas

Song

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

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For the practical application of nanocatalysts, it is desirable to understand the spatiotemporal fluctuations of nanocatalytic activity at the single-nanoparticle level. Here we use time-lapsed superresolution mapping of single-molecule catalysis events on individual nanoparticles to observe time-varying changes in the spatial distribution of catalysis events on Sb-doped TiO 2 nanorods and Au triangle nanoplates. Compared with the active sites on well-defined surface facets, the defects of the nanoparticle catalysts possess higher intrinsic reactivity but lower stability. Corners and ends are more reactive but also less stable than flat surfaces. Averaged over time, the most stable sites dominate the total apparent activity of single nanocatalysts. However, the active sites with higher intrinsic activity but lower stability show activity at earlier time points before deactivating. Unexpectedly, some active sites are found to recover their activity ("selfhealing") after deactivation, which is probably due to desorption of the adsorbate. Our superresolution measurement of different types of active catalytic sites, over both space and time, leads to a more comprehensive understanding of reactivity patterns and may enable the design of new and more productive heterogeneous catalysts.single-molecule nanocatalysis | optical superresolution imaging | photocatalysis | surface restructuring A ll kinds of nanoparticles, such as metals, metal oxides, and even nonmetals, are used as catalysts in a variety of chemical processes (1). In support of developing better and less-expensive nanoparticle catalysts, single-molecule mapping of nanocatalyst activity using superresolution imaging at the single-nanoparticle level can determine active site locations on nanoparticles and which structures are most reactive (2-5). For example, defects, corners, and edges on nanoparticle surfaces have been shown by singlemolecule, superresolution imaging of single nanocatalysts to be more active than other sites. The relative abundance of these sites on nanoparticle catalysts is important for explaining their observed reactivity (2, 4, 6-13).However, prior reports are based on longtime integrations of catalytic activity and thus do not provide information about any dynamic changes in catalytic activity, such as the time-dependent evolution of different active sites. Studies of time-varying catalytic activity are thus arguably more informative than time-averaged observations.The temporal fluctuation of catalytic activity on nanocatalysts or electrodes has been previously observed in situ at both the ensemble and single-nanoparticle level (14-17). More recently, superresolution imaging techniques have been applied to identify the spatial distribution of catalytic activity on a few different nanocatalysts including Au@SiO 2 nanorods, Au@SiO 2 nanotriangles (2, 4) and Au-CdS nanohybrids (6). The observed spatial variations in catalytic activity between different catalysts were merely attributed to possible reaction-driven surface reconstruction of...

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Section: Significancementioning

confidence: 95%

Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity

Zhang

Lucas

Song

et al. 2015

Proc. Natl. Acad. Sci. U.S.A.

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“…Of special importance is the method developed by in organic media [35,36], and those involving anisotropic systems [24,[37][38][39][40][41][42][43]. In the method proposed by Brust et al, the gold precursor complex (HAuCl 4 ) is dissolved in water and transferred to the organic phase using a suitable phase-transfer agent, such as tetraoctylammonium bromide [35].…”

Section: Gold Nanoparticlesmentioning

confidence: 99%

The SERS effect in coordination chemistry

Grasseschi

Toma

2017

Coordination Chemistry Reviews

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“…It is well known that halide ions (Cl À , Br À and I À ) have an affinity for Pd and are highly effective for tuning the growth of Pd nanostructures. [54][55][56][57][58][59][60][61][62][63][64] For the above three ions, their affinities for noble metal atoms or ions follows this order:…”

Section: 53mentioning

confidence: 99%

Rational selection of halide ions for synthesizing highly active Au@Pd nanobipyramids

Liu

Hao

et al. 2017

RSC Adv.

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Pd-based nanostructures with stepped facets possess potential applications in many fields, particularly in catalysis. Generally, crystal growth often only allows the formation of nanostructures with energetically non-stepped facets, so it is desirable to develop methods that can be used to prepare Pd-based nanostructures bounded by stepped facets. Herein, penta-fold twinned (PFT) Au@Pd nanobipyramids (NBs) with stepped {100} facets were synthesized through growing Pd on Au decahedral nanoparticles (NPs) in polyol. During the growth of Au@Pd NBs, Br À was a critical factor, because it has appropriate affinity for the Pd atom and adjusted the growth rate ratio along h110i and h100i, resulting in the formation of Au@Pd NBs with stepped {100} facets. The product shape and size could be tailored by controlling the reaction conditions. Transmission electron microscopy (TEM), high resolution transmission electron microscopy (HRTEM), energy dispersive spectroscopy (EDS), high angle annular dark field (HAADF) imaging and scanning transmission electron microscopy EDS (STEM-EDS) were used to investigate the structure and growth of the Au@Pd NBs. A growth mechanism involving two stages was elucidated. In the first stage, the growth of Pd clearly occurred along both h110i and h100i. In the second stage, the growth along h110i was faster than that along h100i. Furthermore, we also demonstrated that the as-prepared Au@Pd NBs had high catalytic activity, compared with Pd nanocubes and Pd-Au-Pd segmental nanorods.

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Halide Anions as Shape-Directing Agents for Obtaining High-Quality Anisotropic Gold Nanostructures

Cited by 187 publications

References 67 publications

Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity

Superresolution fluorescence mapping of single-nanoparticle catalysts reveals spatiotemporal variations in surface reactivity

The SERS effect in coordination chemistry

Rational selection of halide ions for synthesizing highly active Au@Pd nanobipyramids

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