In this study, we have successfully developed a facile method for the high-yield fabrication of Au-Pd core-shell heterostructures with an unusual tetrahexahedral (THH) morphology using Au nanocubes as the structure-directing cores. The lattice orientations of the Au nanocubes match those of the Pd shells. Structural analysis establishes that the THH nanocrystals are bounded by high-index {730} facets. A substantial lattice mismatch between Au and Pd, oxidative etching in the presence of chloride and oxygen, the use of cetyltrimethylammonium chloride (CTAC) surfactant, and the reaction temperature (30-60 °C) were identified to be key factors facilitating the formation of the THH core-shell nanocrystals. Intermediate products have also been examined to follow the growth process. By selecting cubic gold cores with sizes of 30-70 nm and varying the volume of the gold core solution used, THH Au-Pd core-shell nanocrystals with continuously adjustable sizes from 56 to 124 nm can be readily obtained. Their UV-vis spectra display progressive red-shifted bands. Interestingly, novel concave octahedral and octahedral Au-Pd core-shell nanocrystals can be prepared by lowering the reaction temperature and prolonging the reaction time. The concave octahedra show depressions on all the {111} faces. Electrocatalytic activity of the three Au-Pd core-shell structures for the oxidation of ethanol has been investigated. The THH nanocrystals with entirely high-index {730} facets were found to exhibit the best electrocatalytic activity. These size-tunable THH Au-Pd core-shell nanocrystals may be valuable for catalyzing other organic reactions.
We report the first synthesis of elongated penta-branched gold nanocrystals with a shape resembling that of a star fruit but with sharp ends by a seeding growth approach. Cetyltrimethylammonium bromide (CTAB) capping surfactant was used, and AgNO 3 was added to the last growth solution to promote the formation of the five side branches. Through an investigation of the products collected by adding AgNO 3 into first, second, third, or fourth growth solution, the penta-branched nanocrystals were found to be derived from pentagonal bipyramid-shaped nanocrystals. Side growth over the twin boundaries results in the formation of five elongated branches with the highest point of each branch bisecting the branch into two halves. Smaller penta-branched nanocrystals with sizes of 70-110 nm and more fully developed larger nanocrystals with sizes of 200-350 nm can be readily prepared. The branches possess singlecrystalline {111} faces. The intermediate products obtained at various time points were examined and their UV-vis absorption spectra recorded. By replacing CTAB with cetyltrimethylammonium chloride surfactant, and controlling the concentration of bromide ions in the solution, gold nanostars with five symmetrical branches and monodispersed sizes of 120-130 nm were synthesized for the first time.
Gold nanocubes, octahedra, and rhombic dodecahedra with roughly two sets of particle sizes have been successfully synthesized via a seed-mediated growth approach. All six samples were analyzed for comparative surface-enhanced Raman scattering (SERS) activity. All of these Au nanostructures were found to yield strong enhancement at a thiophenol concentration of 10(-7) M and are excellent SERS substrates. Rhombic dodecahedra with a rhombus edge length of 32 nm showed significantly better enhancement than the other samples and can reach a detection limit of 10(-8) M. Simulations of the binding energies of thiophenol on the different faces of gold and electric near-field intensities of these nanocrystals have been performed to evaluate the experimental results. Superior SERS activity of these nanocrystals can be expected toward the detection of many other molecules.
Nanopores have become an important tool for molecule detection at single molecular level. With the development of fabrication technology, synthesized solid-state membranes are promising candidate substrates in respect of their exceptional robustness and controllable size and shape. Here, a 30–60 (tip-base) nm conical nanopore fabricated in 100 nm thick silicon nitride (Si3N4) membrane by focused ion beam (FIB) has been employed for the analysis of λ-DNA translocations at different voltage biases from 200 to 450 mV. The distributions of translocation time and current blockage, as well as the events frequencies as a function of voltage are investigated. Similar to previously published work, the presence and configurations of λ-DNA molecules are characterized, also, we find that greater applied voltages markedly increase the events rate, and stretch the coiled λ-DNA molecules into linear form. However, compared to 6–30 nm ultrathin solid-state nanopores, a threshold voltage of 181 mV is found to be necessary to drive DNA molecules through the nanopore due to conical shape and length of the pore. The speed is slowed down ∼5 times, while the capture radius is ∼2 fold larger. The results show that the large nanopore in thick membrane with an improved stability and throughput also has the ability to detect the molecules at a single molecular level, as well as slows down the velocity of molecules passing through the pore. This work will provide more motivations for the development of nanopores as a Multi-functional sensor for a wide range of biopolymers and nano materials.
Nanopores have been used as a high throughput tool for characterizing individual biomolecules and nanoparticles. Here, we present the translocation of rigid rod-shaped tobacco mosaic virus (TMV) through solid-state nanopores. Interestingly, due to the high rigidity of TMV, three types of events with distinctive characteristics at the capture process and a strong current fluctuation during the translocation of TMV are observed. A kinetic model is then proposed to address the dynamics of the translocation, followed by corresponding dynamics simulations. The results reveal that TMV has to rotate to fit and pass the pore when it is captured by a nanopore with an angle larger than the maximum angle that allows it to pass through. Then, we investigate the dependence of the rotation of TMV on the conductance fluctuations at the blockade stage. The results show that the rotation of TMV during the passage through the pore affects the current signal significantly. This study gives a fundamental understanding of the dynamics of rod-shaped particles translocating through the nanopore and how the current responds to it. It opens a new possible way to characterize the rigidity of analytes by nanopores.
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