Twinning Engineering of Platinum/Iridium Nanonets as Turing-Type Catalysts for Efficient Water Splitting.

The twin boundary, a common lattice plane of mirror-symmetric crystals, may have high reactivity due to special atomic coordination. However, twinning platinum and iridium nanocatalysts are grand challenges due to the high stacking fault energies that are nearly 1 order of magnitude larger than those of easy-twinning gold and silver. Here, we demonstrate that Turing structuring, realized by selective etching of superthin metal film, provides 14.3 and 18.9 times increases in twin-boundary densities for platinum and iridium nanonets, comparable to the highly twinned silver nanocatalysts. The Turing configurations with abundant low-coordination atoms contribute to the formation of nanotwins and create a large active surface area. Theoretical calculations reveal that the specific atom arrangement on the twin boundary changes the electronic structure and reduces the energy barrier of water dissociation. The optimal Turing-type platinum nanonets demonstrated excellent hydrogen-evolution-reaction performance with a 25.6 mV overpotential at 10.0 mA·cm-2 and a 14.8-fold increase in mass activity. And the bifunctional Turing iridium catalysts integrated in the water electrolyzer had a mass activity 23.0 times that of commercial iridium catalysts. This work opens a new avenue for nanocrystal twinning as a facile paradigm for designing high-performance nanocatalysts.

Turing structuring with multiple nanotwins to engineer efficient and stable catalysts for hydrogen evolution reaction.

Low-dimensional nanocrystals with controllable defects or strain modifications are newly emerging active electrocatalysts for hydrogen-energy conversion and utilization; however, a crucial challenge remains in insufficient stability due to spontaneous structural degradation and strain relaxation. Here we report a Turing structuring strategy to activate and stabilize superthin metal nanosheets by incorporating high-density nanotwins. Turing configuration, realized by constrained orientation attachment of nanograins, yields intrinsically stable nanotwin network and straining effects, which synergistically reduce the energy barrier of water dissociation and optimize the hydrogen adsorption free energy for hydrogen evolution reaction. Turing PtNiNb nanocatalyst achieves 23.5 and 3.1 times increase in mass activity and stability index, respectively, compared against commercial 20% Pt/C. The Turing PtNiNb-based anion-exchange-membrane water electrolyser with a low Pt mass loading of 0.05 mg cm-2 demonstrates at least 500 h stability at 1000 mA cm-2, disclosing the stable catalysis. Besides, this new paradigm can be extended to Ir/Pd/Ag-based nanocatalysts, illustrating the universality of Turing-type catalysts.

Focus on perovskite emitters in blue light-emitting diodes.

Blue perovskite light-emitting diodes (PeLEDs) are essential in pixels of perovskite displays, while their progress lags far behind their red and green counterparts. Here, we focus on recent advances of blue PeLEDs and systematically review the noteworthy strategies, which are categorized into compositional engineering, dimensional control, and size confinement, on optimizing microstructures, energy landscapes, and charge behaviors of wide-bandgap perovskite emitters (bandgap >2.5 eV). Moreover, the stability of perovskite blue emitters and related devices is discussed. In the end, we propose a technical roadmap for the fabrication of state-of-the-art blue PeLEDs to chase and achieve comparable performance with the other two primary-color devices.

Mechanism of HMBR in Reducing Membrane Fouling under Different SRT: Effect of Sludge Load on Microbial Properties.

Extracellular polymeric substances (EPS) are the main causative agents of membrane fouling, and the use of a hybrid membrane bioreactor (HMBR) can mitigate this by reducing the EPS content. Four bench scale sets of HMBRs were used simultaneously to treat domestic wastewater. The effect of sludge retention times (SRT) on membrane fouling in HMBRs and the underlying mechanism were investigated by comparing and analyzing the changes in sludge load, microbial characteristics, EPS distribution characteristics, and transmembrane pressure under different SRTs. Results revealed that, among the four SRTs (10 d, 20 d, 30 d, and 60 d), the best removal rates of chemical oxygen demand and total nitrogen were observed for an SRT of 30 d, with average removal rates of 95.0% and 57.1%, respectively. The best results for ammonia nitrogen and total phosphorus removal were observed at an SRT of 20 d, with average removal rates of 84.3% and 99.5%, respectively. SRT can affect sludge load by altering the biomass, which significantly impacts the microbial communities. The highest microbial diversity was observed at an SRT of 30 d (with a BOD sludge load of 0.0310 kg/kg∙d), with Sphingobacteriales exhibiting the highest relative abundance at 19.6%. At this SRT setting, the microorganisms produced the least amount of soluble EPS and loosely bond EPS by metabolism, 3.41 mg/g and 4.52 mg/g, respectively. Owing to the reduced EPS content, membrane fouling was effectively controlled and the membrane module working cycle was effectively enhanced up to 99 d, the longest duration among the four SRTs.

Study on Creep-Fatigue Mechanical Behavior and Life Prediction of Ti2AlNb-Based Alloy.

Low-cycle fatigue, creep and creep-fatigue tests of Ti2AlNb-based alloy were carried out at 550 °C. Compared with low-cycle fatigue, a creep-fatigue hysteresis loop has larger area and smaller average stress. The introduction of creep damage will greatly reduce the cycle life, and change the fatigue crack initiation point and failure mechanism. Based on the linear damage accumulation rule, the fatigue damage and creep damage were described by the life fraction method and the time fraction method, respectively, and the creep-fatigue life of the Ti2AlNb-based alloy is predicted within an error band of ±2 times.

The Application Value of Three-Dimensional Power Doppler Ultrasound in Fetal Growth Restriction.

In this study, the application value of three-dimensional power Doppler ultrasound (3D-PDU) in fetal growth restriction (FGR) is explored. The retrospective cohort study enrolled pregnant women (with a gestational week of 11-13 + 6 weeks) who received routine health care in the obstetrics and gynecology clinic of our hospital from January 2020 to January 2021. The placentae were scanned using 3D-PDU, and the subjects were followed up until delivery. The fetuses were divided into the control group (n = 322) and FGR group (n = 44) according to their birth weight. There was no significant difference in nuchal translucency (NT), crown-rump length (CRL), and placental volume (PV) during the first trimester between the two groups (P > 0.05). Compared with the control group, the FGR group showed significantly lower levels of vascularisation index (VI), flow index (FI), and vascularisation flow index (VFI) and a higher incidence of fetal distress and neonatal asphyxia (P < 0.05). The FGR group showed a longer gestational week at birth, a higher probability of cesarean section, and a lower 5-minute Apgar score than the control group (P < 0.05). The VI, FI, and VFI of the control group were significantly higher than those of the FGR group. Pearson analysis showed that birth weight was positively correlated with VI and FI (P < 0.05). 3D-PDU assesses the blood perfusion of the fetus and placenta in the first trimester and predicts the pregnancy outcome, which shows great potential in the early diagnosis of FGR.

Pressure-Quenched Superconductivity in Weyl Semimetal NbP Induced by Electronic Phase Transitions under Pressure.

The TaAs family (NbAs, TaAs, NbP, TaP) are kinds of Weyl semimetals with lots of novel properties, thus attracting considerable attention in recent years. Here, we systematically studied the Weyl semimetal NbP up to 72 GPa through the resistivity, Raman spectra, X-ray diffraction measurements, and first-principles density functional theory (DFT) calculations. A pressure-induced semimetal-metal transition was observed at ∼36 GPa, which was further confirmed by the DFT calculations. With further compression up to 52 GPa, a superconducting state was observed. Interestingly, the Tc increases significantly upon decompression and shows a dome-shaped trend as a function of pressure. Surprisingly, the pressure-induced superconductivity can be quenched to ambient pressure, and all transitions under pressure do not involve any structural change. Our work not only depicts a phase diagram of the NbP system under high pressure but also provides a new experimental insight for superconductivity in Weyl semimetals.

Design, Synthesis, Anti-Tomato Spotted Wilt Virus Activity, and Mechanism of Action of Thienopyrimidine-Containing Dithioacetal Derivatives.

Currently, there is insufficient viricide to effectively control tomato spotted wilt virus (TSWV). To address this pending issue, a series of thienopyrimidine-containing dithioacetal derivatives were prepared and tested for their anti-TSWV activities. A subsequent three-dimensional quantitative structure-activity relationship was constructed to indicate the development of optimal compound 35. The obtained compound 35 had excellent anti-TSWV curative, protective, and inactivating activities (63.0, 56.6, and 74.1%, respectively), and the EC50 values of protective and inactivating activities of compound 35 were 252.8 and 113.5 mg/L, respectively, better than those of ningnanmycin (284.8 and 144.7 mg/L) and xiangcaoliusuobingmi (624.9 and 300.0 mg/L). In addition, the anti-TSWV activity of compound 35 was associated with defense-related enzyme activities, enhanced photosynthesis, and reduced stress response, thereby enhancing disease resistance.

Precise Modeling of Thermal and Strain Rate Effect on the Hardening Behavior of SiC/Al Composite.

Temperature and strain rate have significant effects on the mechanical behavior of SiC/Al 2009 composites. This research aimed to precisely model the thermal and strain rate effect on the strain hardening behavior of SiC/Al composite using the artificial neural network (ANN). The mechanical behavior of SiC/Al 2009 composites in the temperature range of 298-623 K under the strain rate of 0.001-0.1 s-1 was investigated by a uniaxial tension experiment. Four conventional models were adopted to characterize the plastic flow behavior in relation to temperature, strain rate, and strain. The ANN model was also applied to characterize the flow behavior of the composite at different strain rates and temperatures. Experimental results showed that the plastic deformation behavior of SiC/Al 2009 composite possesses a coupling effect of strain, strain rate, and temperature. Comparing the prediction error of these models, all four conventional models could not provide satisfactory modeling of flow curves at different strain rates and temperatures. Compared to the four conventional models, the suggested ANN structure dramatically improved the prediction accuracy of the flow curves at different strain rates and temperatures by reducing the prediction error to a maximum of 4.0%. Therefore, the ANN model is recommended for precise modeling of the thermal and strain rate effect on the flow curves of SiC/Al composites.

Effects of Strength and Distribution of SiC on the Mechanical Properties of SiCp/Al Composites.

In this paper, considering the strength and geometric discrete distribution characteristics of composite reinforcement, by introducing the discrete distribution function of reinforcement, the secondary development of ABAQUS is realized by using the Python language, the parametric automatic generation method of representative volume elements of particle-reinforced composites is established, and the tensile properties of silicon carbide particle-reinforced aluminum matrix composites are analyzed. The effects of particle strength, particle volume fraction, and particle random distribution on the mechanical properties of SiCp/Al composites are studied. The results show that the random distribution of particles and the change in particle strength have no obvious influence on the stress-strain relationship before the beginning of material damage, but have a great influence on the damage stage, maximum strength, and corresponding failure strain. With the increase in particle volume fraction, the damage intensity of the model increases, and the random distribution of particles has a great influence on the model with a large particle volume fraction. The results can provide a reference for the design, preparation, and characterization of particle-reinforced metal matrix composites.

Chemical Polishing of Perovskite Surface Enhances Photovoltaic Performances.

The benefits of excess PbI2 on perovskite crystal nucleation and growth are countered by the photoinstability of interfacial PbI2 in perovskite solar cells (PSCs). Here we report a simple chemical polishing strategy to rip PbI2 crystals off the perovskite surface to decouple these two opposing effects. The chemical polishing results in a favorable perovskite surface exhibiting enhanced luminescence, prolonged carrier lifetimes, suppressed ion migration, and better energy level alignment. These desired benefits translate into increased photovoltages and fill factors, leading to high-performance mesostructured formamidinium lead iodide-based PSCs with a champion efficiency of 24.50%. As the interfacial ion migration paths and photodegradation triggers, dominated by PbI2 crystals, were eliminated, the hysteresis of the PSCs was suppressed and the device stability under illumination or humidity stress was significantly improved. Moreover, this new surface polishing strategy can be universally applicable to other typical perovskite compositions.

Mechanochemistry Advances High-Performance Perovskite Solar Cells.

A prerequisite for commercializing perovskite photovoltaics is to develop a swift and eco-friendly synthesis route, which guarantees the mass production of halide perovskites in the industry. Herein, a green-solvent-assisted mechanochemical strategy is developed for fast synthesizing a stoichiometric δ-phase formamidinium lead iodide (δ-FAPbI3 ) powder, which serves as a high-purity precursor for perovskite film deposition with low defects. The presynthesized δ-FAPbI3 precursor possesses high concentration of micrometer-sized colloids, which are in favor of preferable crystallization by spontaneous nucleation. The resultant perovskite films own preferred crystal orientations of cubic (100) plane, which is beneficial for superior carrier transport compared to that of the films with isotropic crystal orientations using "mixture of PbI2 and FAI" as precursors. As a result, high-performance perovskite solar cells with a maximum power conversion efficiency of 24.2% are obtained. Moreover, the δ-FAPbI3 powder shows superior storage stability for more than 10 months in ambient environment (40 ± 10% relative humidity), being conducive to a facile and practical storage for further commercialization.

Determining the Mechanical Strength of Ultra-Fine-Grained Metals.

The mechanical strengthening of metals is the long-standing challenge and popular topic of materials science in industries and academia. The size dependence of the strength of the nanometals has been attracting a lot of interest. However, characterizing the strength of materials at the lower nanometer scale has been a big challenge because the traditional techniques become no longer effective and reliable, such as nano-indentation, micropillar compression, tensile, etc. The current protocol employs radial diamond-anvil cell (rDAC) X-ray diffraction (XRD) techniques to track differential stress changes and determine the strength of ultrafine metals. It is found that ultrafine nickel particles have more significant yield strength than coarser particles, and the size strengthening of nickel continues down to 3 nm. This vital finding immensely depends on effective and reliable characterizing techniques. The rDAC XRD method is expected to play a significant role in studying and exploring nanomaterial mechanics.

Effect of Surface Integrity on Hot Fatigue Life of Ti2AlNb Intermetallic Alloy.

The effect of surface integrity on the hot fatigue performance of Ti2AlNb alloy was investigated. A turning process was used to prepare the standard specimens for hot fatigue tests. The surface integrity characterization and axial fatigue tests were performed. The results show that the influence of surface roughness on the hot fatigue performance of the Ti2AlNb alloy is a secondary factor. The compressive residual stress and enhanced microhardness in the surface layer has a significant effect on the hot fatigue life and they are dominant in the hot fatigue behavior of the Ti2AlNb alloy. Through the investigation on the characteristics of the fatigue fractures, the fatigue propagation process was significantly suppressed because of the strong residual compressive stress and microhardness distribution on the surface layer of the Ti2AlNb specimen.

Influencing Factors on the Healing Performance of Microcapsule Self-Healing Concrete.

The amounts of the components in a microcapsule self-healing system significantly impact the basic performance and self-healing performance of concrete. In this paper, an orthogonal experimental design is used to investigate the healing performance of microcapsule self-healing concrete under different pre-damage loads. The strength recovery performance and sound speed recovery performance under extensive damage are analyzed. The optimum factor combination of the microcapsule self-healing concrete is obtained. Scanning electron microscopy (SEM) and energy dispersive spectroscopy (EDS) are carried out on the concrete samples before and after healing to determine the healing mechanism. The results show that the healing effect of self-healing concrete decreases with an increase in the pre-damage load, and the sound speed recovery rate increases with an increase in the damage degree. The influence of the sodium silicate content on the compressive strength and compressive strength recovery rate of the self-healing concrete increases, followed by a decrease. The optimum combination of factors of the microcapsule self-healing system is 3% microcapsules, 30% sodium silicate, and 15% sodium fluosilicate. The results can be used for the design and preparation of self-healing concrete.

Evolution of Structural and Electronic Properties in NbTe2 under High Pressure.

Transition metal dichalcogenides (TMDs) have attracted wide attention due to their quasi-two-dimensional layered structure and exotic properties. Plenty of efforts have been done to modulate the interlayer stacking manner for novel states. However, as an equally important element in shaping the unique properties of TMDs, the effect of intralayer interaction is rarely revealed. Here, we report a particular case of pressure-tuned re-arrangement of intralayer atoms in distorted 1T-NbTe2, which was demonstrated to be a new type of structural phase transition in TMDs. The structural transition occurs in the pressure range of 16-20 GPa, resulting in a transformation of Nb atomic arrangement from the trimeric to dimeric structure, accompanied by a dramatic collapse of unit cell volume and lattice parameters. Simultaneously, a charge density wave (CDW) was also found to collapse during the phase transition. The strong increase in the critical fluctuations of CDW induces a significant decline in the electronic correlation and a change of charge carrier type from hole to electron in NbTe2. Our finding reveals a new mechanism of structure evolution and expands the field of pressure-induced phase transition.

Purine Nucleoside Derivatives Containing a Sulfa Ethylamine Moiety: Design, Synthesis, Antiviral Activity, and Mechanism.

To find efficient and broad-spectrum viral agents, a series of purine nucleoside derivatives containing sulfa ethylamine moieties was designed and synthesized, and their antiviral activities against tobacco mosaic virus (TMV), cucumber mosaic virus (CMV), and potato virus Y (PVY) were evaluated. Some target compounds displayed good antiviral activities. Among them, compound 3 showed excellent protective activity against CMV and PVY with 50% effective concentration values (EC50) of 137 and 209 µg/mL, respectively, which were better than that of the control agent ningnanmycin (508 and 431 µg/mL). Moreover, the EC50 value of compound 3 for the inactivating activity against TMV was 48 µg/mL, which was better than that of ningnanmycin (88 µg/mL). In addition, compound 3 not only destroyed the structure of the TMV virus but also had a good interaction with the coat protein of the TMV virus. Therefore, compound 3 may further destroy the structure of the virus by binding to the coat protein of the TMV virus, thereby weakening the infectivity of the virus.

Facile synthesis of anionic porous organic polymer for ethylene purification.

The removal of acetylene from ethylene is of vital significance in the petroleum and chemical industry, the presence of trace acetylene impurities in ethylene polymerization process could lead to the interruption of ethylene polymerization. Herein, we construct a new anionic porous organic polymer using potassium tetraphenylborate via Friedel-Crafts alkylation reaction under mild conditions. The resulting material, APOP, possesses good thermal stability and a decent BET surface area, as exemplified by thermogravimetric analysis measurement and nitrogen gas sorption experiment. Acetylene and ethylene adsorption isotherms reveal that APOP has a higher adsorption capacity of acetylene than that of ethylene under same conditions. Ideal adsorbed solution theory calculations and breakthrough experiments both demonstrate that APOP is capable of selective adsorption of acetylene over ethylene. To the best of our knowledge, APOP represents the first anionic porous organic polymer material capable of selective adsorption of acetylene over ethylene, and the exploration of APOP may provide a new way for these key gas separations using ionic porous organic polymer materials.

Superior Carrier Lifetimes Exceeding 6 µs in Polycrystalline Halide Perovskites.

Lead halide perovskite films have witnessed rapid progress in optoelectronic devices, whereas polycrystalline heterogeneities and serious native defects in films are still responsible for undesired recombination pathways, causing insufficient utilization of photon-generated charge carriers. Here, radiation-enhanced polycrystalline perovskite films with ultralong carrier lifetimes exceeding 6 µs and single-crystal-like electron-hole diffusion lengths of more than 5 µm are achieved. Prolongation of charge-carrier activities is attributed to the electronic structure regulation and the defect elimination at crystal boundaries in the perovskite with the introduction of phenylmethylammonium iodide. The introduced electron-rich anchor molecules around the host crystals prefer to fill the halide/organic vacancies at the boundaries, rather than form low-dimensional phases or be inserted into the original lattice. The weakening of the electron-phonon coupling and the excitonic features of the photogenerated carriers in the optimized films, which together contribute to the enhancement of carrier separation and transportation, are further confirmed. Finally the resultant perovskite films in fully operating solar cells with champion efficiency of 23.32% are validated and a minimum voltage deficit of 0.39 V is realized.