BaCu, a Two-Dimensional Electride with Cu Anions.

The electron-rich characteristic and low work function endow electrides with excellent performance in (opto)electronics and catalytic applications; these two features are closely related to the structural topology, constituents, and valence electron concentration of electrides. However, the synthesized electrides, especially two-dimensional (2D) electrides, are limited to specific structural prototypes and anionic p-block elements. Here we synthesize and identify a distinct 2D electride of BaCu with delocalized anionic electrons confined to the interlayer spaces of the BaCu framework. The bonding between Cu and Ba atoms exhibits ionic characteristics, and the adjacent Cu anions form a planar honeycomb structure with metallic Cu-Cu bonding. The negatively charged Cu ions are revealed by the theoretical calculations and experimental X-ray absorption near-edge structure. Physical property measurements reveal that BaCu electride has a high electronic conductivity (ρ = 3.20 µΩ cm) and a low work function (2.5 eV), attributed to the metallic Cu-Cu bonding and delocalized anionic electrons. In contrast to typical ionic 2D electrides with p-block anions, density functional theory calculations find that the orbital hybridization between the delocalized anionic electrons and BaCu framework leads to unique isotropic physical properties, such as mechanical properties, and work function. The freestanding BaCu monolayer with half-metal conductivity exhibits low exfoliation energy (0.84 J/m2) and high mechanical/thermal stability, suggesting the potential to achieve low-dimensional BaCu from the bulk. Our results expand the space for the structure and attributes of 2D electrides, facilitating the discovery and potential application of novel 2D electrides with transition metal anions.

Superatomic-Charge-Density-Wave in Cluster-Assembled Au6Te12Se8 Superconductors.

Superatomic crystals are a class of hierarchical materials composed of atomically precise clusters assembled via van der Waals or covalent-like interactions. Au6Te12Se8, an all-inorganic superatomic superconductor exhibiting superatomic-charge-density-wave (S-CDW), provides the first platform to study the response of its collective quantum phenomenon to the external pressure in superatomic crystals. We reveal a competition between S-CDW and superconductivity in an ultra-narrow pressure range. Distinct from conventional CDW ordering, S-CDW shows the lowest threshold (0.1 GPa) toward external pressure that is 1-2 orders of magnitude lower than other atomic compounds. Prominently, a second superconducting phase emerges above 7.3 GPa with a threefold enhancement in the transition temperature (Tc) to 8.5 K, indicating a switch of the conduction channel from the a- to b-axis. In situ synchrotron diffractions and theoretical calculations reveal a pressure-mediated mesoscopic slip of the superatoms and a 2D-3D transition of the Fermi surface topology, which well explains the observed dimensional crossover of conductivity and re-entrant superconductivity.

Hydrostatic pressure effect of photocarrier dynamics in GaAs probed by time-resolved terahertz spectroscopy.

Pressure effects on photocarrier dynamics such as interband relaxations and intraband cooling in GaAs have been investigated using in situ time-resolved terahertz spectroscopy with a diamond anvil cell. The interband photocarrier lifetime significantly decreases by nearly two orders of magnitude as the external hydrostatic pressure is increased up to 10 GPa. Considerable pressure tuning for the intervalley scattering processes has also been observed, and the time constants under different pressures are extracted based on the three-state rate model. This work provides new perspectives on tailoring nonequilibrium carrier dynamics in semiconductors using hydrostatic pressure and may serve as the impetus for the development of high-pressure terahertz spectroscopy.

Investigation on the mental health status of pregnant women in China during the Pandemic of COVID-19.

PURPOSE: To evaluate the anxiety and depression in pregnant women in China, and its influencing factors during the corona virus disease 2019 (COVID-19) pandemic. METHODS: From February 22 to February 27, a questionnaire survey was conducted on 156 pregnant women, including demographic characteristics, a self-rating anxiety scale (SAS), and a self-depression rating scale (SDS). RESULTS: A total of 13 non-homologous end-joining (8.3%, 13/156) patients were anxious, 79 patients (50.6%, 79/156) were depressed, and 13 patients (8.3%, 13/156) suffered from both anxiety and depression. The SAS score of pregnant women was 40.55 ± 6.09, and the SDS score was 50.42 ± 11.64. For the SAS score, only 8.3% of all patients (13/156) were in a light anxiety state. For the SDS score, 46.79% (73/156) of patients was normal, 23.72% of patients (37/156) showed mild depression, 22.44% (35/156) showed moderate depression, and 4.49% (7/156) showed severe depression. No significant changes were observed in SAS and SDS scores between patients from different regions within China, health state, gestational week, educational background, and living condition (P > 0.05). Moreover, no significant differences were observed between diagnosed/suspected patients and the normal control group (P > 0.05), and between pregnant women in Wuhan compared to other regions (P > 0.05). CONCLUSION: During the COVID-19 epidemic, the anxiety level of pregnant women was the same as that before the epidemic, while the level of depression was significantly higher. Pregnant women who lived in Wuhan, the epicenter of the epidemic, were not more anxious or depressed compared to pregnant women in other regions during the COVID-19 epidemic. Furthermore, the mental health status of pregnant women with COVID-19 was not more severe.

ZnO Quantum Dots Coupled with Graphene toward Electrocatalytic N2 Reduction: Experimental and DFT Investigations.

Electrochemical reduction of N2 to NH3 is a promising method for artificial N2 fixation, but it requires efficient and robust electrocatalysts to boost the N2 reduction reaction (NRR). Herein, a combination of experimental measurements and theoretical calculations revealed that a hybrid material in which ZnO quantum dots (QDs) are supported on reduced graphene oxide (ZnO/RGO) is a highly active and stable catalyst for NRR under ambient conditions. Experimentally, ZnO/RGO was confirmed to favor N2 adsorption due to the largely exposed active sites of ultrafine ZnO QDs. DFT calculations disclosed that the electronic coupling of ZnO with RGO resulted in a considerably reduced activation-energy barrier for stabilization of *N2 H, which is the rate-limiting step of the NRR. Consequently, ZnO/RGO delivered an NH3 yield of 17.7 µg h-1 mg-1 and a Faradaic efficiency of 6.4 % in 0.1 m Na2 SO4 at -0.65 V (vs. RHE), which compare favorably to those of most of the reported NRR catalysts and thus demonstrate the feasibility of ZnO/RGO for electrocatalytic N2 fixation.

Wavelet Packet Decomposition-Based Multiscale CNN for Fault Diagnosis of Wind Turbine Gearbox.

This article presents an intelligent fault diagnosis method for wind turbine (WT) gearbox by using wavelet packet decomposition (WPD) and deep learning. Specifically, the vibration signals from the gearbox are decomposed using WPD and the decomposed signal components are fed into a hierarchical convolutional neural network (CNN) to extract multiscale features adaptively and classify faults effectively. The presented method combines the multiscale characteristic of WPD with the strong classification capacity of CNNs, and it does not need complex manual feature extraction steps as usually adopted in existing results. The presented CNN with multiple characteristic scales based on WPD (WPD-MSCNN) has three advantages: 1) the added WPD layer can legitimately process the nonstationary vibration data to obtain components at multiple characteristic scales adaptively, it takes full advantage of WPD and, thus, enables the CNN to extract multiscale features; 2) the WPD layer directly sends multiscale components to the hierarchical CNN to extract rich fault information effectively, and it avoids the loss of useful information due to hand-crafted feature extraction; and 3) even if the scale changes, the lengths of components remain the same, which shows that the proposed method is robust to scale uncertainties in the vibration signals. Experiments with vibration data from a production wind farm provided by a company using condition monitoring system (CMS) show that the presented WPD-MSCNN method is superior to traditional CNN and multiscale CNN (MSCNN) for fault diagnosis.

Facile construction of agar-based fire-resistant aerogels: A synergistic strategy via in situ generations of magnesium hydroxide and cross-linked Ca-alginate.

Biomass-based aerogel materials have many advantages, such as low thermal conductivity and non-toxicity. These materials are environmentally friendly and have broad development potential in the fields of packaging, cushioning and green building insulation. However, defects, such as low mechanical strength and poor fire safety, greatly limit the application of these materials. In this work, the agar/polyvinyl alcohol composite aerogel modified by the magnesium hydroxide (MH)/sodium alginate (SA) composite flame retardant system was developed by using a freeze-dried technology and the strategy of in-situ generation of MH and crosslinking of SA. The results showed that the MH/SA dramatically enhanced the mechanical and thermal stability of the composites. The compression modulus of AP-M35S15 was 2.37 MPa, which was 152.13 % higher than that of AP-M50. The limiting oxygen index value of AP-M35S15 was 34.1 % and reached V-0 level in the vertical burning test, which was better than those of the samples with a single MH effect. The cone calorimetric test showed that the MH/SA composite flame retardant system performed better in extending the ignition time, slowing down the heat release rate and reducing the total heat release and had a more complete dense carbon structure after burning.

Manipulation of nonlinear optical responses in layered ferroelectric niobium oxide dihalides.

Realization of highly tunable second-order nonlinear optical responses, e.g., second-harmonic generation and bulk photovoltaic effect, is critical for developing modern optical and optoelectronic devices. Recently, the van der Waals niobium oxide dihalides are discovered to exhibit unusually large second-harmonic generation. However, the physical origin and possible tunability of nonlinear optical responses in these materials remain to be unclear. In this article, we reveal that the large second-harmonic generation in NbOX2 (X = Cl, Br, and I) may be partially contributed by the large band nesting effect in different Brillouin zone. Interestingly, the NbOCl2 can exhibit dramatically different strain-dependent bulk photovoltaic effect under different polarized light, originating from the light-polarization-dependent orbital transitions. Importantly, we achieve a reversible ferroelectric-to-antiferroelectric phase transition in NbOCl2 and a reversible ferroelectric-to-paraelectric phase transition in NbOI2 under a certain region of external pressure, accompanied by the greatly tunable nonlinear optical responses but with different microscopic mechanisms. Our study establishes the interesting external-field tunability of NbOX2 for nonlinear optical device applications.

Valley-dimensionality locking of superconductivity in cubic phosphides.

Two-dimensional superconductivity is primarily realized in atomically thin layers through extreme exfoliation, epitaxial growth, or interfacial gating. Apart from their technical challenges, these approaches lack sufficient control over the Fermiology of superconducting systems. Here, we offer a Fermiology-engineering approach, allowing us to desirably tune the coherence length of Cooper pairs and the dimensionality of superconducting states in arsenic phosphides AsxP1-x under hydrostatic pressure. We demonstrate how this turns these compounds into tunable two-dimensional superconductors with a dome-shaped phase diagram even in the bulk limit. This peculiar behavior is shown to result from an unconventional valley-dimensionality locking mechanism, driven by a delicate competition between three-dimensional hole-type and two-dimensional electron-type energy pockets spatially separated in momentum space. The resulting dimensionality crossover is further discussed to be systematically controllable by pressure and stoichiometry tuning. Our findings pave a unique way to realize and control superconducting phases with special pairing and dimensional orders.

In situ nanoarchitectonics of magnesium hydroxide particles for property regulation of carboxymethyl cellulose/poly(vinyl alcohol) aerogels.

Carboxymethyl cellulose (CMC)-based aerogels with low density, low thermal conductivity, and biodegradability are promising candidates for environmentally friendly heat-insulating materials. However, the application of CMC-based aerogels as insulation materials in building exterior walls is limited by the high water sensitivity, poor mechanical properties and high flammability of these aerogels. In this work, a simple hydration method was used to generate magnesium hydroxide (MH) directly from CMC/polyvinyl alcohol (PVA) mixed sol with active MgO obtained by calcined magnesite as the raw material. A series of composite aerogels with different MH contents were prepared through the freeze-drying method. Scanning electron microscopy showed that nanoflower-like MH was successfully synthesised in situ in the 3D porous polymer aerogel matrix. Compared with the mechanical properties and water resistance of the original CMC/PVA composite aerogels, those of the composite aerogels were significantly improved. In addition, the flame retardancy of the CMC/PVA composite aerogels was greatly enhanced by the introduction of MH into the polymer matrix, and the limiting oxygen index reached 35.5% when the MH loading was 60%.

Significantly improve the water and chemicals resistance of alginate-based nanocomposite films by a simple in-situ surface coating approach.

Biopolymers have shown great application prospects due to their advantages of being biodegradable, renewable, non-toxic, safe and inexpensive. However, the innate hydrophilicity of biopolymers means the materials prepared from them easily swell or disintegrate in aqueous media, limiting their applications. Herein, on the basis of improving the mechanical performance of a sodium alginate/poly(vinyl alcohol) (SA/PVA) film by introducing palygorskite (Pal) nanorods, the hydrophobicity of the obtained SA/PVA/Pal film was improved further by surface coating with methyltrichlorosilane (MTCS) through a vapor deposition-surface polycondensation reaction. MTCS nanofilaments, with a size of approximately 50 nm, were formed on the film surface by the silanization reaction between MTCS and hydroxyls, resulting in an improvement in surface hydrophobicity characterized by a contact angle (111.8°) higher than that of SA/PVA/Pal film (72.7°). Therefore, the obtained films maintained their original shape and strength after soaking for a long time in aqueous solutions containing acid, alkaline, and electrolyte, also in organics, while the uncoated film dissolved quickly and lost its original shape. Moreover, the surface coating also increased the film's tensile strength from 11.43 to 28.69 MPa. This demonstrates a simple, universal and effective way to improve the resistance of biopolymer-derived materials to water and various chemicals.

Pressure-stabilized divalent ozonide CaO3 and its impact on Earth's oxygen cycles.

High pressure can drastically alter chemical bonding and produce exotic compounds that defy conventional wisdom. Especially significant are compounds pertaining to oxygen cycles inside Earth, which hold key to understanding major geological events that impact the environment essential to life on Earth. Here we report the discovery of pressure-stabilized divalent ozonide CaO3 crystal that exhibits intriguing bonding and oxidation states with profound geological implications. Our computational study identifies a crystalline phase of CaO3 by reaction of CaO and O2 at high pressure and high temperature conditions; ensuing experiments synthesize this rare compound under compression in a diamond anvil cell with laser heating. High-pressure x-ray diffraction data show that CaO3 crystal forms at 35 GPa and persists down to 20 GPa on decompression. Analysis of charge states reveals a formal oxidation state of -2 for ozone anions in CaO3. These findings unravel the ozonide chemistry at high pressure and offer insights for elucidating prominent seismic anomalies and oxygen cycles in Earth's interior. We further predict multiple reactions producing CaO3 by geologically abundant mineral precursors at various depths in Earth's mantle.

Effect of removing coloring metal ions from the natural brick-red palygorskite on properties of alginate/palygorskite nanocomposite film.

Natural palygorskite (Pal) nanorods have huge application prospect as a reinforcing filler of polymer material, but the presence of variable coloring metal ions (i.e., Fe(III)) in natural Pal may affect the comprehensive properties of polymer materials. In order to reveal the effects of removing coloring metal ions on the structure and mechanical, transparency and anti-aging performance of the polymer, a series of sodium alginate/Pal (SA/Pal) nanocomposite films were prepared using natural brick-red Pal (RPal) and white acid-leached Pal (HPal) as fillers, and their properties were investigated comparatively. Results indicate removal of partial metal ions in Pal greatly improved the mechanical, transmittance, water-resistance and anti-aging properties of SA/HPal film in contrast to the SA/RPal film, due to the intensified interaction between HPal and SA. After exposure in UV condition for 72 h, the SA/RPal film becomes brittle with a great decrease of tensile strength from 11.05 to 6.71 MPa; but the SA/HPal film still keeps good flexibility with only a slight decrease of tensile strength from 14.66 to 12.09 MPa, indicating a passive effect of removing Fe(III) on improving anti-aging performance of SA/Pal film. This research paves a theoretical foundation to extend the application of naturally abundant Pal in polymer materials.

Effect of Natural Nanostructured Rods and Platelets on Mechanical and Water Resistance Properties of Alginate-Based Nanocomposites.

A series of biopolymer-based nanocomposite films were prepared by incorporating natural one-dimensional (1D) palygorskite (PAL) nanorods, and two-dimensional (2D) montmorillonite (MMT) nanoplatelets into sodium alginate (SA) film by a simple solution casting method. The effect of different dimensions of nanoclays on the mechanical, water resistance, and light transmission properties of the SA/PAL or MMT nanocomposite films were studied. The field-emission scanning electron microscopy (FE-SEM) result showed that PAL can disperse better than MMT in the SA matrix in the case of the same addition amount. The incorporation of both PAL and MMT into the SA film can enhance the tensile strength (TS) and water resistance capability of the film. At a high content of nanoclays, the SA/PAL nanocomposite film shows relatively higher TS, and better water resistance than the SA/MMT nanocomposite film. The SA/MMT nanocomposite films have better light transmission than SA/PAL nanocomposite film at the same loading amount of nanoclays. These results demonstrated that 1D PAL nanorods are more suitable candidate of inorganic filler to improve the mechanical and water resistance properties of biopolymers/nanoclays nanocomposites.

Synergistic Effect of Halloysite Nanotubes and Glycerol on the Physical Properties of Fish Gelatin Films.

Fish gelatin (FG)/glycerol (GE)/halloysite (HT) composite films were prepared by casting method. The morphology of the composite films was observed by scanning electron microscopy (SEM). The effects of HT and GE addition on the mechanical properties, water resistance and optical properties of the composites were investigated. Results showed that with increasing GE content, the elongation at composite breaks increased significantly, but their tensile strength (TS) and water resistance decreased. SEM results showed that GE can partly promote HT dispersion in composites. TS and water resistance also increased with the addition of HTs. Well-dispersed HTs in the FG matrix decreased the moisture uptake and water solubility of the composites. All films showed a transparency higher than 80% across the visible light region (400⁻800 nm), thereby indicating that light transmittance of the resulting nanocomposites was slightly affected by GE and HTs.

Reducing Water Sensitivity of Chitosan Biocomposite Films Using Gliadin Particles Made by In Situ Method.

In order to sustain rapid expansion in the field of biocomposites, it is necessary to develop novel fillers that are biodegradable, and easy to disperse and obtain. In this work, gliadin particles (GPs) fabricated through an in situ method have been reported as fillers for creating chitosan (CS)-based biocomposite films. In general, the particles tend to agglomerate in the polymer matrix at high loading (approximately >10%) in the biopolymer/particles composites prepared by the traditional solution-blending method. However, the micrographs of biocomposites confirmed that the GPs are well dispersed in the CS matrix in all CS/GPs composites even at a high loading of 30% in this study. It was found that the GPs could improve the mechanical properties of the biocomposites. In addition, the results of moisture uptake and solubility in water of biocomposites showed that water resistance of biocomposites was enhanced by the introduction of GPs. These results suggested that GPs fabricated through an in situ method could be a good candidate for use in biopolymer-based composites.

One-step in situ fabrication of a granular semi-IPN hydrogel based on chitosan and gelatin for fast and efficient adsorption of Cu2+ ion.

The novel granular semi-IPN hydrogels were in situ prepared in an aqueous solution by the free-radical grafting and crosslinking reactions among chitosan (CTS), acrylic acid (AA), gelatin (GE) and N,N'-methylene-bis-acrylamide. The FTIR spectra and elemental analysis confirmed that the AA monomers were grafted onto CTS backbone, and the GE macromolecular chains interpenetrated through the CTS-g-PAA network. The hydrogels are granular, which are composed of numerous micro-spheres according to the scanning electron microscope observations. The gel strength, adsorption, reuse and recovery properties of the hydrogels for Cu(2+) ion were systematically investigated. The results indicate the hydrogel with 2 wt% GE has the highest adsorption capacity of 261.08 mg/g with the recovery ratio of 95.2%. And the incorporation of 10 wt% GE enhanced the storage modulus by 103.4% (ω=100 rad/s) and 115.1% (ω=0.1 rad/s), and the adsorption rate by 5.67%. Moreover, the adsorption capacity of the hydrogel is still as high as 153.9 mg/g, after five cycles of adsorption-desorption. It was found that the ion-exchange and complexation interactions between the functional groups (-COO(-) and -NH2) of the hydrogels and Cu(2+) ion are the predominant adsorption mechanisms.

Chitosan-g-poly(acrylic acid) hydrogel with crosslinked polymeric networks for Ni2+ recovery.

In this study, chitosan-g-poly(acrylic acid) (CTS-g-PAA) hydrogel with crosslinked polymeric networks was prepared from an aqueous dispersion polymerization and then used as the adsorbent to recover a valuable metal, Ni2+. The adsorption capacity of CTS-g-PAA for Ni2+ was evaluated and the adsorption kinetics was investigated using Voigt-based model and pseudo-second-order model. In addition, the effects of pH values and coexisting heavy metal ions such as Cu2+ and Pb2+ on the adsorption capacity were studied. The results indicate that the as-prepared adsorbent has faster adsorption rate and higher adsorption capacity for Ni2+ recovery, with the maximum adsorption capacity of 161.80 mg g(-1). In a wide pH range of 3-7, the adsorption capacity keeps almost the same, and even under competitive conditions, the adsorption capacity of CTS-g-PAA for Ni2+ is observed to be as high as 54.47 mg g(-1). Finally, the adsorption performance of CTS-g-PAA for Ni2+ in real water sample and the reusability of the as-prepared adsorbent were evaluated, and also the controlled adsorption mechanism was proposed.