We developed a colloidal synthesis of CsPbBr perovskite nanocrystals (NCs) at a relative low temperature (90 °C) for the bright blue emission which differs from the original green emission (∼510 nm) of CsPbBr nanocubes as reported previously. Shapes of the obtained CsPbBr NCs can be systematically engineered into single and lamellar-structured 0D quantum dots, as well as face-to-face stacking 2D nanoplatelets and flat-lying 2D nanosheets via tuning the amounts of oleic acid (OA) and oleylamine (OM). They exhibit sharp excitonic PL emissions at 453, 472, 449, and 452 nm, respectively. The large blue shift relative to the emission of CsPbBr bulk crystal can be ascribed to the strong quantum confinement effects of these various nanoshapes. PL decay lifetimes are measured, ranging from several to tens of nanoseconds, which infers the higher ratio of exciton radiative recombination to the nonradiative trappers in the obtained CsPbBr NCs. These shape-controlled CsPbBr perovskite NCs with the bright blue emission will be widely used in optoelectronic applications, especially in blue LEDs which still lag behind compared to the better developed red and green LEDs.
Magnesium ions (Mg 2+ ) are widely present in biological fluids, and they are suggested as the vital factors that inhibit spontaneous hydroxyapatite (HAP) precipitation in nature. However, the regulation mechanisms of Mg 2+ on HAP crystallization are still under intensive debates. We find that a typical precipitation of HAP from supersaturated solutions should include five stages: s1, formation of ion clusters and amorphous calcium phosphate (ACP); s2, stabilization of ACP; s3, transformation from ACP to HAP via dissolution and crystallization; s4, classical crystal growth of HAP; s5, HAP aging under a near equilibrium state. Actually, Mg 2+ ions exhibit different inhibitory effects on these stages. The ions have a negligible influence on the kinetics of initial ACP formation in solutions (s1) and final aging of crystals (s5). Rather, the ions can either adsorb onto or incorporate into the ACP precursor particles during s1. In s2, the lifetime of ACP in solution is extended significantly by both two types of Mg 2+ ions. However, the absorbed ones are more effective than the incorporated ones on the inhibition of the phase transformation from ACP to HAP in this s2. In stages of s3 and s4, it is only surface Mg 2+ ions that retard crystal growth of HAP and the incorporated Mg 2+ become inert. These detailed findings reveal how Mg 2+ ions affect the crystallization process of HAP mineralization from supersaturation. Such a detailed understanding can provide a chemical strategy for precise regulation of HAP formation kinetics in intermediate phase mediated crystallization.
The creation of an artificial superhydrophobic surface with micro- and nanostructures has been demonstrated using a block copolymer micelle solution and silica nanoparticles. The unique technique of a nanoparticle-supported micelle stabilization together with changes in the solvent power guarantees the precise morphology control of certain block copolymer-mediated surfaces. The approaches presented here provide a new strategy for the fabrication of a wettability-controlled organic-inorganic hybrid or organic coatings.
Large-area amorphous calcium carbonate (ACC) films in air are shown to be transformed into crystalline calcium carbonate (CaCO(3)) films via two modes-dissolution-recrystallization and solid-solid phase transition-depending on the relative humidity of the air and the temperature. Moisture in the air promotes the transformation of ACC into crystalline forms via a dissolution-recrystallization process. Increasing the humidity increases the rate of ACC crystallization and gives rise to films with numerous large pores. As the temperature is increased, the effect of moisture in the air is reduced and solid-solid transition by thermal activation becomes the dominant transformation mechanism. At 100 and 120 degrees C, ACC films are transformed into predominantly (110) oriented crystalline films. Collectively, the results show that calcium carbonate films with different morphologies, crystal phases, and structures can be obtained by controlling the humidity and temperature. This ability to control the transformation of ACC should assist in clarifying the role of ACC in the biomineralization of CaCO(3) and should open new avenues for preparing CaCO(3) films with oriented and fine structure.
A new and simple method for preparing large-area and continuous calcium carbonate films
under mild conditions is described. Amorphous calcium carbonate (ACC) films have been
formed both in the presence and absence of a poly(acrylic acid) inhibitor. The transformation
from ACC to crystalline vaterite/calcite has been observed by optical microscopy and
confirmed by external reflection infrared spectroscopy. We have shown that the inhibiting
effects of substrates and inhibitors on the transformation of ACC result in the formation of
good CaCO3 films. From our results, we suggested that ACC precipitates are initially formed
from highly supersaturated solutions, which then deposit as films through the cooperation
between an insoluble matrix and a soluble inhibitor. The matrix and inhibitor were also
found to affect the growth, morphology, and structure of CaCO3 crystal by influencing the
phase transformation of ACC into crystalline forms. It has been shown that ACC plays an
important role in the biomineralization and crystallization of calcium carbonate.
The regulation mechanism of organic additives on the crystallization of inorganic crystal is fundamentally important in biomineralization. Experimentally, it was found that the amino acids glycine (Gly) and glutamic acid (Glu) could lead to the formation of rod- and plate-like hydroxyapatite (HAP) crystallites, respectively. The detailed adsorption behavior of Gly and Glu on HAP crystal faces was studied by molecular dynamics (MD) simulation. The specific adsorption sites and patterns of Gly and Glu on the (100) and (001) faces of HAP crystals were revealed at the atomic level. The amino acids adsorbed on the HAP (001) and (100) faces with their positive amino groups occupied vacant calcium sites, and their negative carboxylate groups occupied vacant P or OH sites precisely and formed an ordered adsorption layer. The atomic force microscopy pulling simulation and free energy calculation showed that Glu was much more difficult to depart from the HAP (001) face than that from the (100) face. This result indicated that Glu preferred to adsorb strongly onto the HAP (001) face, which resulted in the formation of plate-like HAP. However, Gly did not show any significantly preferential adsorption between these two HAP faces. Thus, the habits of HAP, rod-like crystallites, were not altered during the HAP crystallization in the presence of Gly. Combined with experimental results, our study demonstrated that the MD simulation of interfacial structures could improve our understanding of biological regulation in mineralization processes at the atomic level.
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