Abstract
Defects can induce drastic changes of the electronic properties of two-dimensional transition metal dichalcogenides and influence their applications. It is still a great challenge to ...characterize small defects and correlate their structures with properties. Here, we show that tip-enhanced Raman spectroscopy (TERS) can obtain distinctly different Raman features of edge defects in atomically thin MoS
2
, which allows us to probe their unique electronic properties and identify defect types (e.g., armchair and zigzag edges) in ambient. We observed an edge-induced Raman peak (396 cm
−1
) activated by the double resonance Raman scattering (DRRS) process and revealed electron–phonon interaction in edges. We further visualize the edge-induced band bending region by using this DRRS peak and electronic transition region using the electron density-sensitive Raman peak at 406 cm
−1
. The power of TERS demonstrated in MoS
2
can also be extended to other 2D materials, which may guide the defect engineering for desired properties.
Designing and modulating the local structure of metal sites is the key to gain the unique selectivity and high activity of single metal site catalysts. Herein, we report strain engineering of curved ...single atomic iron‐nitrogen sites to boost electrocatalytic activity. First, a helical carbon structure with abundant high‐curvature surface is realized by carbonization of helical polypyrrole that is templated from self‐assembled chiral surfactants. The high‐curvature surface introduces compressive strain on the supported Fe−N4 sites. Consequently, the curved Fe−N4 sites with 1.5 % compressed Fe−N bonds exhibit downshifted d‐band center than the planar sites. Such a change can weaken the bonding strength between the oxygenated intermediates and metal sites, resulting a much smaller energy barrier for oxygen reduction. Catalytic tests further demonstrate that a kinetic current density of 7.922 mA cm−2 at 0.9 V vs. RHE is obtained in alkaline media for curved Fe−N4 sites, which is 31 times higher than that for planar ones. Our findings shed light on modulating the local three‐dimensional structure of single metal sites and boosting the catalytic activity via strain engineering.
Compressive strain engineering of curved single atomic iron‐nitrogen sites could boost the catalytic activity for electrocatalytic oxygen reduction reaction.
Grain size is an important component trait of grain yield, which is frequently threatened by abiotic stress. However, little is known about how grain yield and abiotic stress tolerance are regulated. ...Here, we characterize GSA1, a quantitative trait locus (QTL) regulating grain size and abiotic stress tolerance associated with metabolic flux redirection. GSA1 encodes a UDP-glucosyltransferase, which exhibits glucosyltransferase activity toward flavonoids and monolignols. GSA1 regulates grain size by modulating cell proliferation and expansion, which are regulated by flavonoid-mediated auxin levels and related gene expression. GSA1 is required for the redirection of metabolic flux from lignin biosynthesis to flavonoid biosynthesis under abiotic stress and the accumulation of flavonoid glycosides, which protect rice against abiotic stress. GSA1 overexpression results in larger grains and enhanced abiotic stress tolerance. Our findings provide insights into the regulation of grain size and abiotic stress tolerance associated with metabolic flux redirection and a potential means to improve crops.
Osteoarthritis (OA), the most prevalent age-related joint disorder, is characterized by chronic inflammation, progressive articular cartilage destruction, and subchondral bone sclerosis. Accumulating ...evidences indicate that circular RNAs (circRNAs) play a critical role in various diseases, but the function of circRNAs in OA remains largely unknown. Here we showed that circRNA.33186 was significantly upregulated in IL-1β)-treated chondrocytes and in cartilage tissues of a destabilized medial meniscus (DMM)-induced OA mouse model. Knockdown of circRNA.33186 increased anabolic factor (type II collagen) expression and decreased catabolic factor (MMP-13) expression. Knockdown of circRNA.33186 also promoted proliferation and inhibited apoptosis in IL-1β-treated chondrocytes. Silencing of circRNA.33186 in vivo markedly alleviated DMM-induced OA. Mechanistic study showed that circRNA.33186 directly binds to and inhibits miR-127-5p, thereby increasing MMP-13 expression, and contributes to OA pathogenesis. Taken together, our findings demonstrated a fundamental role of circRNA.33186 in OA progression and provide a potential drug target in OA therapy.
Zhu and colleagues demonstrate that circRNA.33186 regulates chondrocyte functions, including ECM catabolism, proliferation, and apoptosis. Silencing of circRNA.33186 alleviated OA by acting as a sponge of miR-127-5p. These findings reveal a fundamental role of circRNA.33186 in OA progression and provide a potential drug target in OA therapy.
Big data with its vast volume and complexity is increasingly concerned, developed and used for all professions and trades. Remote sensing, as one of the sources for big data, is generating ...earth-observation data and analysis results daily from the platforms of satellites, manned/unmanned aircrafts, and ground-based structures. Agricultural remote sensing is one of the backbone technologies for precision agriculture, which considers within-field variability for site-specific management instead of uniform management as in traditional agriculture. The key of agricultural remote sensing is, with global positioning data and geographic information, to produce spatially-varied data for subsequent precision agricultural operations. Agricultural remote sensing data, as general remote sensing data, have all characteristics of big data. The acquisition, processing, storage, analysis and visualization of agricultural remote sensing big data are critical to the success of precision agriculture. This paper overviews available remote sensing data resources, recent development of technologies for remote sensing big data management, and remote sensing data processing and management for precision agriculture. A five-layer-fifteenlevel (FLFL) satellite remote sensing data management structure is described and adapted to create a more appropriate four-layer-twelve-level (FLTL) remote sensing data management structure for management and applications of agricultural remote sensing big data for precision agriculture where the sensors are typically on high-resolution satellites, manned aircrafts, unmanned aerial vehicles and ground-based structures. The FLTL structure is the management and application framework of agricultural remote sensing big data for precision agriculture and local farm studies, which outlooks the future coordination of remote sensing big data management and applications at local regional and farm scale.
Engineering single-atom electrocatalysts with high-loading amount holds great promise in energy conversion and storage application. Herein, we report a facile and economical approach to achieve an ...unprecedented high loading of single Ir atoms, up to ∼18wt%, on the nickel oxide (NiO) matrix as the electrocatalyst for oxygen evolution reaction (OER). It exhibits an overpotential of 215 mV at 10 mA cm–2 and a remarkable OER current density in alkaline electrolyte, surpassing NiO and IrO2 by 57 times and 46 times at 1.49 V vs RHE, respectively. Systematic characterizations, including X-ray absorption spectroscopy and aberration-corrected Z-contrast imaging, demonstrate that the Ir atoms are atomically dispersed at the outermost surface of NiO and are stabilized by covalent Ir–O bonding, which induces the isolated Ir atoms to form a favorable ∼4+ oxidation state. Density functional theory calculations reveal that the substituted single Ir atom not only serves as the active site for OER but also activates the surface reactivity of NiO, which thus leads to the dramatically improved OER performance. This synthesis method of developing high-loading single-atom catalysts can be extended to other single-atom catalysts and paves the way for industrial applications of single-atom catalysts.
With the improvement of the quality of human life, various industries utilize deep learning technology to meet the needs of users. In this paper, after exploring the deep temporal model and deep ...forest algorithm (DF) model in extracting the characteristics of user behavior features, we propose a user behavior prediction model based on CNN-LSTM and add a front embedding layer as well as a feature fusion layer to improve it and increase the prediction accuracy. The weighted average method is used to integrate CNN-LSTM with DF for algorithmic model fusion, aiming to improve the robustness and stability of the model and achieve accurate predictions of user behavior. In the empirical analysis, the correct rate of the fusion model proposed in this paper exceeds the proper rate of several other models by 11.75-15.73%, and it can reach 11.2% recall at k=20. Meanwhile, the lower the user behavior level is, the higher the prediction accuracy of the CNNLSTM+DF algorithm is, which can reach up to 95.20%. The lower the average relative error and average absolute error are, which can reach 13.45% and 3.92min respectively, which verifies the validity of the fusion model proposed in this paper, and provides a reference for the research in the related fields.
The high theoretical energy density (1274 Wh kg−1) and high safety enable the all‐solid‐state Na−S batteries with great promise for stationary energy storage system. However, the uncontrollable ...solid–liquid‐solid multiphase conversion and its associated sluggish polysulfides redox kinetics pose a great challenge in tunning the sulfur speciation pathway for practical Na−S electrochemistry. Herein, we propose a new design methodology for matrix featuring separated bi‐catalytic sites that control the multi‐step polysulfide transformation in tandem and direct quasi‐solid reversible sulfur conversion during battery cycling. It is revealed that the N, P heteroatom hotspots are more favorable for catalyzing the long‐chain polysulfides reduction, while PtNi nanocrystals manipulate the direct and full Na2S4 to Na2S low‐kinetic conversion during discharging. The electrodeposited Na2S on strongly coupled PtNi and N, P‐codoped carbon host is extremely electroreactive and can be readily recovered back to S8 without passivation of active species during battery recharging, which delivers a true tandem electrocatalytic quasi‐solid sulfur conversion mechanism. Accordingly, stable cycling of the all‐solid‐state soft‐package Na−S pouch cells with an attractive specific capacity of 876 mAh gS−1 and a high energy of 608 Wh kgcathode−1 (172 Wh kg−1, based on the total mass of cathode and anode) at 60 °C are demonstrated.
A new design methodology for matrix featuring separated bi‐catalytic sites that direct one‐step reversible sulfur conversion during battery cycling was proposed. And the tandem electrocatalysis manipulated tunable quasi‐solid sulfur redox chemistry smoothen the efficient entrapping‐catalysis‐conversion polysulfide speciation for practical all‐solid‐state Na−S batteries.
Peroxymonosulfate (PMS) is extensively used as an oxidant to develop the sulfate radical-based advanced oxidation processes in the decontamination of organic pollutants and various PMS activation ...methods have been explored. Visible-light-assisted PMS activation to construct a Fenton-like process has shown a great potential for pollution control. In our work, BiVO4 nanosheets were prepared using a hydrothermal process and used to activate PMS under visible light. A rapid degradation of ciprofloxacin (CIP) was achieved by dosing PMS (0.96 g/L), BiVO4 (0.32 g/L) under visible light with a reaction rate constant of 77.72-fold higher than that in the BiVO4/visible light process. The electron spin resonance and free radical quenching experiments indicate that reactive species of •O2−, h+, •OH and SO4•− all worked, where h+, •OH and SO4•− were found as the dominant contributors to the CIP degradation. The spectroscopic analyses further demonstrate that the photoinduced electrons were directly involved in the PMS activation process. The generated •O2− was partially utilized to activate PMS and more •OH was produced because of the chain reactions between SO4•− and H2O/OH−. In this process, PMS acted as an electron acceptor to transfer the photo-induced charges from the conduction band of BiVO4 and PMS was successfully activated to yield the high-powered oxidative species. From the degradation intermediates of CIP detected by a liquid-chromatography-mass spectrometer, the possible degradation pathways were proposed. The substantially decreased toxicity of CIP after the reaction was also observed. This work might provide new insights into the visible-light-assisted PMS activation mechanisms and is useful to construct environmentally-friendly catalytic processes for the efficient degradation of organic pollutants.
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•PMS was effectively activated by BiVO4 nanosheets for water purification under visible light.•Separation of electron/hole pairs and generation of oxidative species were enhanced.•Visible-light-assisted PMS activation Fenton-like mechanism was elucidated.•High mineralization and low biotoxicity validated the application potential of the system.
This article performs a systematic study to understand the dependence of the splitting of an initially axisymmetric storm on the various components of the Unified Model (UM) and Weather Research and ...Forecasting model (WRF). The models are adapted to keep their differences at a minimum. Results at km‐scale grid resolution show that the models differ significantly even under a controlled environment with no surface and radiative forcing. The initial storm in UM splits into two within the first hour. WRF also produces two separate updraughts, but it does not split entirely because of a secondary downdraught that falls just ahead of the original updraught. The cold pool from this downdraught converges with the oncoming winds at lower levels to generate a ring of updraughts connecting the two. UM also shows a similar secondary downdraught, but it is relatively weak. Experiments with the successive reduction in complexity of the microphysics scheme show that the models start to differ with the inclusion of rain processes. Sensitivity experiments with the magnitude of turbulent mixing length do not impact this aspect of model behaviour. Resolution sensitivity experiments show that the storm does not split in UM for a horizontal resolution of O(100 m), whereas WRF behaves consistently across all the resolutions. Through further analyses, we argue that the formal accuracy of the model dynamical core has no control in deciding whether the initial storm will undergo a split or not.
The life cycle of a thunderstorm is complex, and to correctly capture its evolution is vital for a numerical model. Here we have used two well‐established models (UM and WRF) to show that even in an idealized set‐up the models differ significantly (see image). Results demonstrate that the models start to differ with the inclusion of rain processes, which points to the physics–dynamics coupling as a potential cause for it.
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