With high quality and in high yield: The synthesis presented here affords CdSe and CdTe semiconductor nanocrystals without the need of a precursor injection. It allows the detailed control of the size and shape of the nanocrystals, as can be seen from the tetrahedral CdSe nanocrystals that have been prepared (TEM image). The method is suitable for industrial‐scale preparations.
Colloidal superparticles are nanoparticle assemblies in the form of colloidal particles. The assembly of nanoscopic objects into mesoscopic or macroscopic complex architectures allows bottom-up fabrication of functional materials. We report that the self-assembly of cadmium selenide-cadmium sulfide (CdSe-CdS) core-shell semiconductor nanorods, mediated by shape and structural anisotropy, produces mesoscopic colloidal superparticles having multiple well-defined supercrystalline domains. Moreover, functionality-based anisotropic interactions between these CdSe-CdS nanorods can be kinetically introduced during the self-assembly and, in turn, yield single-domain, needle-like superparticles with parallel alignment of constituent nanorods. Unidirectional patterning of these mesoscopic needle-like superparticles gives rise to the lateral alignment of CdSe-CdS nanorods into macroscopic, uniform, freestanding polymer films that exhibit strong photoluminescence with a striking anisotropy, enabling their use as downconversion phosphors to create polarized light-emitting diodes.
Hybrid materials of the metal−organic framework (MOF), chromium(III) terephthalate (MIL-101), and phosphotungstic acid (PTA) were synthesized in aqueous media in the absence of hydrofluoric acid. XRD analysis of the MIL101/PTA composites indicates the presence of ordered PTA assemblies residing in both the large cages and small pores of MIL-101, which suggests the formation of previously undocumented structures. The MIL101/PTA structure enables a PTA payload 1.5−2 times higher than previously achieved. The catalytic performance of the MIL101/PTA composites was assessed in the Baeyer condensation of benzaldehyde and 2-naphthol, in the three-component condensation of benzaldehyde, 2-naphthol, and acetamide, and in the epoxidation of caryophyllene by hydrogen peroxide. The catalytic efficiency was demonstrated by the high (over 80−90%) conversion of the reactants under microwave-assisted heating. In four consecutive reaction cycles, the catalyst recovery was in excess of 75%, whereas the product yields were maintained above 92%. The simplicity of preparation, exceptional stability, and reactivity of the novel composites indicate potential in utilization of these catalytic matrices in a multitude of catalytic reactions and engineering processes.
Quality and quantity: A non‐injection synthesis of high‐quality CdSe nanocrystals can be conducted in air, that is without the need for any oxygen‐free manipulation. The synthesis, which uses SeO2 as the selenium precursor, is suitable for the large‐scale industrial synthesis of high‐quality nanocrystals at low cost and has been generalized for the formation of other metal selenides, such as PbSe and Pd4.5Se nanocrystals.
A supramolecular chemistry approach is used to make supercrystalline spherical colloidal superparticles (SPs, see picture) from nanoparticles. Detailed mechanistic studies show that the formation of the SPs is a two‐step process. The major driving force for superparticle formation is the solvophobic interaction between nanoparticle building blocks and the growth solution; fine‐tuning the interaction led to a size‐controlled synthesis.
In this paper, we report an approach for using solvophobic interactions to synthesize well-defined colloidal superparticles from nonpolar-solvent-dispersible Fe3O4 nanoparticle artificial atoms. These colloidal superparticles possess a “single-supercrystal” structure, of which Fe3O4 artificial atoms occupy the lattice points of a face-centered cubic superlattice. In addition, these superparticles exhibit superlattice fringes under a low-resolution TEM, providing an interesting analogue to the lattice fringes of colloidal nanocrystals under a high-resolution TEM. Moreover, these superparticles can be further assembled into close-packed solid structures, demonstrating their role as a new type of building block in nanoscience.
Two-dimensional single-crystal PbS nanosheets were synthesized by deviatoric stress-driven orientation and attachment of nanoparticles (NPs). In situ small- and wide-angle synchrotron X-ray scattering measurements on the same spot of the sample under pressure coupled with transmission electron microscopy enable reconstruction of the nucleation route showing how enhanced deviatoric stress causes ordering NPs into single-crystal nanosheets with a lamellar mesostructure. At the same time that deviatoric stress drives SC(110) orientation in a face-centered-cubic supercrystal (SC), rocksalt (RS) NPs rotate and align their RS(200) and RS(220) planes within the SC(110) plane. When NPs approach each other along the compression axis, enhanced deviatoric stress drives soft ligands passivated at RS(200) and RS(220) surfaces to reorient from a group of SC(110) in-planes to the interspace of SC[110]-normal planes. While the internal NP structure starts a rocksalt-to-orthorhombic transition at 7.1 GPa, NPs become aligned on RS(220) and RS(200) and thus become attached at those faces. The transition-catalyzed surface atoms accelerate the inter-NP coalescing process and the formation of low-energy structure nanosheet. Above 11.6 GPa, the nucleated single-crystal nanosheets stack into a lamellar mesostructure that has a domain size comparable to the starting supercrystal.
The design and formation of a linear assembly of gold nanorods using a biomolecular recognition system are described. Anti-mouse IgG was immobilized on the {111} end faces of gold nanorods through a thioctic acid containing a terminal carboxyl group. The biofunctionalized nanorods can be assembled with the desired length using mouse IgG for biorecognition and binding. The gold nanorods can be assembled to extended nanorod chains, which can be as long as 3 microm. These assembled nanostructures may be used as the precursors for future nanodevices.
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