Hybrid organic-inorganic metal halide perovskites have fascinating electronic properties and have already been implemented in various devices. Although the behavior of bulk metal halide perovskites has been widely studied, the properties of perovskite nanocrystals are less well-understood because synthesizing them is still very challenging, in part because of stability. Here we demonstrate a simple and versatile method to grow monodisperse CHNHPbBrI perovskite nanocrystals inside mesoporous silica templates. The size of the nanocrystal is governed by the pore size of the templates (3.3, 3.7, 4.2, 6.2, and 7.1 nm). In-depth structural analysis shows that the nanocrystals maintain the perovskite crystal structure, but it is slightly distorted. Quantum confinement was observed by tuning the size of the particles via the template. This approach provides an additional route to tune the optical bandgap of the nanocrystal. The level of quantum confinement was modeled taking into account the dimensions of the rod-shaped nanocrystals and their close packing inside the channels of the template. Photoluminescence measurements on CHNHPbBr clearly show a shift from green to blue as the pore size is decreased. Synthesizing perovskite nanostructures in templates improves their stability and enables tunable electronic properties via quantum confinement. These structures may be useful as reference materials for comparison with other perovskites, or as functional materials in all solid-state light-emitting diodes.
The discovery of lead-free hybrid double perovskites provides a viable approach in the search for stable and environmentally benign photovoltaic materials as alternatives to lead-containing systems such as MAPbX 3 (X = Cl, Br, or I). Following our recent reports of (MA) 2 KBiCl 6 and (MA) 2 TlBiBr 6 , we have now synthesized a hybrid double perovskite, (MA) 2 AgBiBr 6 , that has a low band gap of 2.02 eV and is relatively stable and nontoxic. Its electronic structure and mechanical and optical properties are investigated with a combination of experimental studies and density functional theory calculations.
Two-dimensional (2D) materials are promising for applications in a wide range of fields because of their unique properties. Hydrogen boride sheets, a new 2D material recently predicted from theory, exhibit intriguing electronic and mechanical properties as well as hydrogen storage capacity. Here, we report the experimental realization of 2D hydrogen boride sheets with an empirical formula of HB, produced by exfoliation and complete ion-exchange between protons and magnesium cations in magnesium diboride (MgB) with an average yield of 42.3% at room temperature. The sheets feature an sp-bonded boron planar structure without any long-range order. A hexagonal boron network with bridge hydrogens is suggested as the possible local structure, where the absence of long-range order was ascribed to the presence of three different anisotropic domains originating from the 2-fold symmetry of the hydrogen positions against the 6-fold symmetry of the boron networks, based on X-ray diffraction, X-ray atomic pair distribution functions, electron diffraction, transmission electron microscopy, photo absorption, core-level binding energy data, infrared absorption, electron energy loss spectroscopy, and density functional theory calculations. The established cation-exchange method for metal diboride opens new avenues for the mass production of several types of boron-based 2D materials by countercation selection and functionalization.
Hard carbon possesses the ability to store Li, Na, and K ions between stacked sp 2 carbon layers and voids (micropores). We have explored hard carbon as a candidate for negative electrode materials for Li-ion, Na-ion, and K-ion batteries. Hard carbon samples have been prepared by carbonizing sucrose at different heat treatment temperatures (HTTs) in the range of 700−2000 °C to make them structurally suitable for reversible Li, Na, and K insertion. Structures and particle morphology of the hard carbon samples synthesized at different HTTs were systematically characterized using X-ray diffraction, small-angle X-ray scattering, pair distribution function analysis, electron microscopy, Raman spectroscopy, and electron spin resonance spectroscopy. All these characterizations of hard carbon samples have revealed advanced ordering of carbons and reduction of carbon defects with increasing HTT. Thus, the average stacked carbon interlayer distance decreases, the number of the stacking layers increases, the layered domains grow in the in-plane direction, and interstitial voids enlarge. Electrochemical properties of the hard carbons were examined in nonaqueous Li, Na, and K cells. Potential profiles and reversible capacities upon galvanostatic charge/discharge processes in nonaqueous cells are significantly different depending on HTTs and different alkali metal ions. On the basis of these findings, strategies to design high-capacity hard carbon negative electrodes for high-energy-density Li-ion, Na-ion, and K-ion batteries are discussed.
Single metal-organic frameworks (MOFs), constructed from the coordination between one-fold metal ions and organic linkers, show limited functionalities when used as precursors for nanoporous carbon materials. Herein, we propose to merge the advantages of zinc and cobalt metals ions into one single MOF crystal (i.e., bimetallic MOFs). The organic linkers that coordinate with cobalt ions tend to yield graphitic carbons after carbonization, unlike those bridging with zinc ions, due to the controlled catalytic graphitization by the cobalt nanoparticles. In this work, we demonstrate a feasible method to achieve nanoporous carbon materials with tailored properties, including specific surface area, pore size distribution, degree of graphitization, and content of heteroatoms. The bimetallic-MOF-derived nanoporous carbon are systematically characterized, highlighting the importance of precisely controlling the properties of the carbon materials. This can be done by finely tuning the components in the bimetallic MOF precursors, and thus designing optimal carbon materials for specific applications.
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