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Highly Efficient Blue OLEDs Based on Metal‐Assisted Delayed Fluorescence Pd(II) Complexes
Abstract A series of metal‐assisted delayed fluorescence (MADF) palladium(II) complexes, PdN1N, PdN1N‐dm, and PdN6N, are studied. Their 77 K photoluminescence emission spectra show a narrow primary emission peak at 464, 466, and 470 nm, respectively, with small vibronic peaks characteristic of many phosphorescent emitters. At room temperature (300 K), the dominant emission peaks for PdN1N, PdN1N‐dm, and PdN6N are slightly redshifted to 472, 470, and 476 nm, respectively. In the meantime, a broad sideband is also shown between 410 and 450 nm due to the MADF process. A blue device employing PdN1N‐dm demonstrates an electroluminescence emission peak at 476 nm and the maximum external quantum efficiency (EQE) of 25.1%. The high maximum EQE of the blue organic light‐emitting diode (OLED) device indicates that both the phosphorescence and the delayed fluorescence are very efficient. In addition, a stable OLED device of PdN1N‐dm gives a maximum EQE of 9.8% and the estimated operational lifetime LT 70 of 350 h at the practical luminance of 100 cd m −2 .
Solvent-Assisted Linker Exchange: An Alternative to the De Novo Synthesis of Unattainable Metal-Organic Frameworks
Metal-organic frameworks (MOFs) have gained considerable attention as hybrid materials—in part because of a multitude of potential useful applications, ranging from gas separation to catalysis and light harvesting. Unfortunately, de novo synthesis of MOFs with desirable function–property combinations is not always reliable and may suffer from vagaries such as formation of undesirable topologies, low solubility of precursors, and loss of functionality of the sensitive network components. The recently discovered synthetic approach coined solvent-assisted linker exchange (SALE) constitutes a simple to implement strategy for circumventing these setbacks; its use has already led to the generation of a variety of MOF materials previously unobtainable by direct synthesis methods. This Review provides a perspective of the achievements in MOF research that have been made possible with SALE and examines the studies that have facilitated the understanding and broadened the scope of use of this invaluable synthetic tool.
Laser-Assisted Metal–Organic Chemical Vapor Deposition of Gallium Nitride
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Mechanisms of Hydrogen-Assisted Magnesiothermic Reduction of TiO{sub 2}
Direct reduction of TiO{sub 2} powder has been attempted for decades by researchers in an effort to decrease titanium (Ti) metal production costs. The main objective has been to avoid energy-intensive steps involved in production of primary Ti by the Kroll process. The emerging hydrogen-assisted magnesiothermic reduction process, which uses Mg to directly reduce TiO{sub 2} powder under a H{sub 2} atmosphere, has been shown to have the potential to compete directly with the Kroll process. The present studies represent an effort to understand the reduction reaction mechanisms of this process. Phase transformations and the reaction pathways are examined by SEM/EDX analysis of partially reduced powder cross-sectional, X-ray diffraction, and other analytical techniques. The results show important morphological changes, the prominent intermediate and final phases under the H{sub 2} atmosphere, as well as the local deposition behavior of the MgO byproduct. The effect of the specific surface areas of the initial particles is also discussed.
Microstructural, chemical and textural characterization of ZnO nanorods synthesized by aerosol assisted chemical vapor deposition
ZnO nanorods were synthesized by aerosol assisted chemical vapor deposition onto TiO{sub 2} covered borosilicate glass substrates. Deposition parameters were optimized and kept constant. Solely the effect of different nozzle velocities on the growth of ZnO nanorods was evaluated in order to develop a dense and uniform structure. The crystalline structure was characterized by conventional X-ray diffraction in grazing incidence and Bragg–Brentano configurations. In addition, two-dimensional grazing incidence synchrotron radiation diffraction was employed to determine the preferred growth direction of the nanorods. Morphology and growth characteristics analyzed by electron microscopy were correlated with diffraction outcomes. Chemical composition was established by X-ray photoelectron spectroscopy. X-ray diffraction results and X-ray photoelectron spectroscopy showed the presence of wurtzite ZnO and anatase TiO{sub 2} phases. Morphological changes noticed when the deposition velocity was lowered to the minimum, indicated the formation of relatively vertically oriented nanorods evenly distributed onto the TiO{sub 2} buffer film. By coupling two-dimensional X-ray diffraction and computational modeling with ANAELU it was proved that a successful texture determination was achieved and confirmed by scanning electron microscopy analysis. Texture analysis led to the conclusion of a preferred growth direction in [001] having a distribution width Ω = 20° ± 2°. - Highlights: • Uniform and pure single-crystal ZnO nanorods were obtained by AACVD technique. • Longitudinal and transversal axis parallel to the [001] and [110] directions, respectively. • Texture was determined by 2D synchrotron diffraction and electron microscopy analysis. • Nanorods have its [001] direction distributed close to the normal of the substrate. • Angular spread about the preferred orientation is 20° ± 2°.
Investigation of water assisted phase transformation process from AlPO4-5 to AlPO4-tridymite
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Magnesium Alloy ZK60 Tubing made by Shear Assisted Processing and Extrusion (ShAPE)
ZK60 Magnesium tubing has been friction extruded from as-cast billets and T5 conditioned bars using Shear Assisted Processing and Extrusion (ShAPE). Tubes having an outer diameter of 50.8 mm and wall thickness of 1.9 mm were extruded with >20 times less ram force compared to conventional extrusion due to the unique shearing conditions and tooling inherent to ShAPE. Microstructures of the as-cast billet and T5 bar feedstock materials were significantly different from each other in terms of grain size, texture, and second phase distribution; yet the resulting microstructures after ShAPE were remarkably similar. An average grain size of 4-5 microns, 20o tilt of basal texture away from the extrusion axis, and refined second phases having a uniform distribution were achieved independent of the feedstock material. Hardness for as-extruded and artificially aged tubes are presented with isotropic behavior explained by detailed microstructural analysis. This work suggests that bulk ZK60 magnesium alloys extrusions may be fabricated in a single step, with microstructures that are unobtainable with conventional extrusion.
Rapid microwave-assisted preparation of binary and ternary transition metal sulfide compounds
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Template-Assisted, Seed-Mediated Synthesis of Hierarchically Mesoporous Core–Shell UiO-66: Enhancing Adsorption Capacity and Catalytic Activity through Iterative Growth
A hierarchically mesoporous (HM) UiO-66-F 4 shell with ~8 nm mesopores can be iteratively grown on top of UiO-66 nanoparticle (NP) seeds over several cycles templated by Pluronic F-127 micelles. Presumably, the Pluronic micelles that were formed in water can surround UiO-66 NPs to facilitate the overgrowth of an HM-UiO-66-F 4 shell in the presence of Zr IV precursors and BDC-F 4 linkers. The UiO-66 NP seeds play an important role in directing the continuous growth of the HM-UiO-66-F 4 shell, as only a nonporous phase was obtained in their absence. Furthermore, this template-assisted, seed-mediated method can be extended to produce other UiO-66-X (X = (OH) 2 , (COOH) 2 , etc.) shells, demonstrating its generality for the UiO-66 family of metal–organic frameworks. Notably, the incorporation of mesopores into the thrice-overgrown UiO-66@HM|3rd-UiO-66-F 4 materials leads to impressive enhancements in the per-mass uptake capacity of Direct Blue 86, a large anionic dye: 320% better than the parent UiO-66 seeds and 150% better than that for a [UiO-66 + UiO-66-F 4 ] physical mixture at the same mass proportion. Similar enhancements were also observed in the catalyzed oxidation of thioanisole.
A Bottom-Up Formation Mechanism of Solid Electrolyte Interphase Revealed by Isotope-Assisted Time-of-Flight Secondary Ion Mass Spectrometry
Understanding the solid electrolyte interphase (SEI) formation mechanism is critically important for the performance and durability of lithium-ion batteries. However, the details of how SEI builds up into a nanometer-thick layer from molecular level reduction reactions on negative electrodes are missing. Here, isotope-assisted time-of-flight secondary ion mass spectrometry analyses were designed to answer this fundamental question. By investigating the isotope ratio profile in SEI during the initial SEI formation cycle, it is discovered that the topmost SEI near the electrolyte formed first and the SEI near the electrode formed later. Furthermore, this new “bottom-up” SEI growth mechanism was then correlated to the electrolyte one-electron and two-electron reduction reaction dynamics, which in turn explains the formation of the two-layered organic–inorganic SEI composite structure.
Ammonia-Assisted Light Alkane Anti-coke Reforming on Isolated ReO x Sites in Zeolite
The conventional reforming produces H 2 with stoichiometric amounts of CO and CO 2 from hydrocarbons. Here, we show that CO x -free H 2 can be produced from ammonia-assisted reforming (ammoreforming) of natural gas liquids (C n H 2n+2 + nNH 3 = nHCN + (2n + 1) H 2 , n = 2 or 3) at the same conditions as the steam reforming. Such a process co-produces HCN, which can be easily separated from H 2 and used as value-added chemicals or for NH 3 recycling through hydrolysis. In addition, the ammoreforming of ethane and propane was realized over the Re-modified HZSM-5 zeolite rather than the traditional Pt-based catalyst for the BMA process (methane ammoreforming). The specific activity of the Re/HZSM-5 catalysts at 650 °C is up to 1 mol H2 /g Re /min (or 180 min –1 ) during ethane ammoreforming. The catalyst is highly coke resistant and shows only slight deactivation with a time-on-stream up to 20 h. Characterization of the fresh and used catalysts by X-ray absorption and Raman spectroscopies suggested that the isolated ReO x site grafted by AlO 4 – tetrahedral in the zeolite framework is responsible for the outstanding catalytic activity and coke resistibility.
CO[subscript 2]-Assisted Oxidative Dehydrogenation of Propane over VO[subscript x]/In[subscript 2]O[
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Ce x Zr 1– x O 2 -Supported CrO x Catalysts for CO 2 -Assisted Oxidative Dehydrogenation of Propane–Probing the Active Sites and Strategies for Enhanced Stability
CO 2 -assisted oxidative dehydrogenation of propane (CO 2 -ODH) represents an attractive approach for propylene production and CO 2 utilization. As a soft oxidant, CO 2 can minimize overoxidation of the hydrocarbons to enhance the propylene selectivity while increasing the equilibrium yield. However, a major challenge of CO 2 -ODH is the rapid deactivation of the catalysts. The current study focuses on designing Ce x Zr 1–x O 2 -mixed oxide-supported CrO x catalysts for CO 2 -ODH with enhanced product selectivity and catalyst stability. By doping 0–30% Ce in the Ce x Zr 1–x O 2 mixed oxide support, propane conversion of 53–79% was achieved at 600 °C, with propylene selectivity up to 82%. Compared to the pure ZrO 2 -supported catalyst (i.e., 5 wt %Cr/ZrO 2 ), 20–30 %Ce doped catalysts (i.e., 5 wt %Cr/Ce 0.2 Zr 0.8 O 2 and 5 wt %Cr/Ce 0.3 Zr 0.7 O 2 ) inhibited the formation of CH 4 and ethylene and improved propylene selectivity from 57 to 77–82%. Detailed characterizations of the 5%Cr/Ce 0.2 Zr 0.8 O 2 catalyst and density functional theory (DFT) calculations indicated that Cr 3+ is the active species during the CO 2 -ODH reaction, and the reaction follows a non-redox dehydrogenation pathway. Coke formation was determined to be the primary reason for catalyst deactivation, and the addition of Ce to the ZrO 2 support greatly enhanced the coke resistance, leading to superior stability. Furthermore, coke removal by oxidizing the catalyst in air is effective in restoring its activity.