The copper(II)-mediated ring opening/alkynylation of cyclopropanol by employing inexpensive and commercially available terminal alkyne is developed. The reactions proceeded efficiently to afford ...synthetically useful alk-4-yn-1-ones in moderate to good yields with good functional group tolerance. Control experiments showed that the reaction presumably proceeds via the formation of intermediates of copper homoenolate and/or alkynylcopper species.
Sodium‐ion batteries have gained much attention for their potential application in large‐scale stationary energy storage due to the low cost and abundant sodium sources in the earth. However, the ...electrochemical performance of sodium‐ion full cells (SIFCs) suffers severely from the irreversible consumption of sodium ions of cathode during the solid electrolyte interphase (SEI) formation of hard carbon anode. Here, a high‐efficiency cathode sodiation compensation reagent, sodium oxalate (Na2C2O4), which possesses both a high theoretical capacity of 400 mA h g−1 and a capacity utilization as high as 99%, is proposed. The implementation of Na2C2O4 as sacrificial sodium species is successfully realized by decreasing its oxidation potential from 4.41 to 3.97 V through tuning conductive additives with different physicochemical features, and the corresponding mechanism of oxidation potential manipulation is analyzed. Electrochemical results show that in the full cell based on a hard carbon anode and a P2‐Na2/3Ni1/3Mn1/3Ti1/3O2 cathode with Na2C2O4 as a sodium reservoir to compensate for sodium loss during SEI formation, the capacity retention is increased from 63% to 85% after 200 cycles and the energy density is improved from 129.2 to 172.6 W h kg−1. This work can provide a new avenue for accelerating the development of SIFCs.
The development of sodium‐ion batteries has been hindered so far by the irreversible consumption of sodium ions of the cathode during the solid electrolyte interphase formation. Therefore, in search of a safe, cost‐effective, and highly efficient cathode sodiation reagent, the feasibility of Na2C2O4 as a sodium reservoir source for enhancing the performance of sodium‐ion batteries is investigated.
Graphs naturally appear in numerous application domains, ranging from social analysis, bioinformatics to computer vision. The unique capability of graphs enables capturing the structural relations ...among data, and thus allows to harvest more insights compared to analyzing data in isolation. However, it is often very challenging to solve the learning problems on graphs, because (1) many types of data are not originally structured as graphs, such as images and text data, and (2) for graph-structured data, the underlying connectivity patterns are often complex and diverse. On the other hand, the representation learning has achieved great successes in many areas. Thereby, a potential solution is to learn the representation of graphs in a low-dimensional Euclidean space, such that the graph properties can be preserved. Although tremendous efforts have been made to address the graph representation learning problem, many of them still suffer from their shallow learning mechanisms. Deep learning models on graphs (e.g., graph neural networks) have recently emerged in machine learning and other related areas, and demonstrated the superior performance in various problems. In this survey, despite numerous types of graph neural networks, we conduct a comprehensive review specifically on the emerging field of graph convolutional networks, which is one of the most prominent graph deep learning models. First, we group the existing graph convolutional network models into two categories based on the types of convolutions and highlight some graph convolutional network models in details. Then, we categorize different graph convolutional networks according to the areas of their applications. Finally, we present several open challenges in this area and discuss potential directions for future research.
The advent of intense ultrashort optical pulses spanning a frequency range from terahertz to the visible has opened a new era in the experimental investigation and manipulation of quantum materials. ...The generation of strong optical field in an ultrashort time scale enables the steering of quantum materials nonadiabatically, inducing novel phenomenon or creating new phases which may not have an equilibrium counterpart. Ultrafast time‐resolved optical techniques have provided rich information and played an important role in characterization of the nonequilibrium and nonlinear properties of solid systems. Here, some of the recent progress of ultrafast optical techniques and their applications to the detection and manipulation of physical properties in selected quantum materials are reviewed. Specifically, the new development in the detection of the Higgs mode and photoinduced nonequilibrium response in the study of superconductors by time‐resolved terahertz spectroscopy are discussed.
The advent of ultrashort optical pulses has provided unprecedented opportunities to probe and manipulate physical properties of quantum materials. There have been rapid growing discoveries of photoinduced new phenomena and nonlinear properties. A review on recent progress of ultrafast optical characterization and manipulation of quantum states, specifically in systems with broken‐symmetry states or phase transitions, and prospects are provided.
Low‐cost and stable sodium‐layered oxides (such as P2‐ and O3‐phases) are suggested as highly promising cathode materials for Na‐ion batteries (NIBs). Biphasic hybridization, mainly involving P2/O3 ...and P2/P3 biphases, is typically used to boost their electrochemical performances. Herein, a P3/O3 intergrown layered oxide (Na2/3Ni1/3Mn1/3Ti1/3O2) as high‐rate and long‐life cathode for NIBs via tuning the amounts of Ti substitution in Na2/3Ni1/3Mn2/3−xTixO2 (x = 0, 1/6, 1/3, 2/3) is demonstrated. The X‐ray diffraction (XRD) Rietveld refinement and aberration‐corrected scanning transmission electron microscopy show the co‐existence of P3 and O3 phases, and density functional theory calculation corroborates the appearance of the anomalous O3 phase at the Ti substitution amount of 1/3. The P3/O3 biphasic cathode delivers an unexpected rate capability (≈88.7% of the initial capacity at a high rate of 5 C) and cycling stability (≈68.7% capacity retention after 2000 cycles at 1 C), superior to those of the sing phases P3‐Na2/3Ni1/3Mn2/3O2, P3‐Na2/3Ni1/3Mn1/2Ti1/6O2, and O3‐Na2/3Ni1/3Ti2/3O2. The highly reversible structural evolution of the P3/O3 integrated cathode observed by ex situ XRD, ex situ X‐ray absorption spectra, and the rapid Na+ diffusion kinetics, underpin the enhancement. These results show the important role of P3/O3 biphasic hybridization in designing and engineering layered oxide cathodes for NIBs.
P3/O3 biphasic Na2/3Ni1/3Mn1/3Ti1/3O2 cathode material is prepared for Na‐ion batteries by tuning the Ti amounts. This P3/O3 intergrown cathode delivers superior rate capability and cycling stability to those of the pristine P3 and O3 phases, which are underpinned by the observed highly reversible structural transition of P3/O3 biphase and the rapid Na+ diffusion kinetics.
Lithium metal anodes (LMAs) are promising for next‐generation batteries but have poor compatibility with the widely used carbonate‐based electrolytes, which is a major reason for their severe ...dendrite growth and low Coulombic efficiency (CE). A nitrate additive to the electrolyte is an effective solution, but its low solubility in carbonates is a problem that can be solved using a crown ether, as reported. A rubidium nitrate additive coordinated with 18‐crown‐6 crown ether stabilizes the LMA in a carbonate electrolyte. The coordination promotes the dissolution of NO3− ions and helps form a dense solid electrolyte interface that is Li3N‐rich which guides uniform Li deposition. In addition, the Rb (18‐crown‐6)+ complexes are adsorbed on the dendrite tips, shielding them from Li deposition on the dendrite tips. A high CE of 97.1% is achieved with a capacity of 1 mAh cm−2 in a half cell, much higher than when using the additive‐free electrolyte (92.2%). Such an additive is very compatible with a nickel‐rich ternary cathode at a high voltage, and the assembled full battery with a cathode material loading up to 10 mg cm−2 shows an average CE of 99.8% over 200 cycles, indicating a potential for practical use.
A rubidium nitrate (RbNO3) additive coordinated with 18‐crown‐6 crown ether is proposed to stabilize the lithium metal anode in the carbonate electrolyte. A coordination reaction between them promotes the dissolution of NO3− ions to form a dense and Li3N‐rich solid electrolyte interface and generates the Rb(18‐crown‐6)+ complexes as stable shielding ions to suppress dendrite growth.
In this paper, we propose an image enhancement algorithm combining non-subsampled shearlet transform and gradient-domain guided filtering to address the problems of low resolution, noise ...amplification, missing details, and weak edge gradient retention in the X-ray image enhancement process. First, we decompose histogram equalization and nonsubsampled shearlet transform to the original image. We get a low-frequency sub-band and several high-frequency sub-bands. Adaptive gamma correction with weighting distribution is used for the low-frequency sub-band to highlight image contour information and improve the overall contrast of the image. The gradient-domain guided filtering is conducted for the high-frequency sub-bands to suppress image noise and highlight detail and edge information. Finally, we reconstruct all the effectively processed sub-bands by the inverse non-subsampled shearlet transform and obtain the final enhanced image. The experimental results show that the proposed algorithm has good results in X-ray image enhancement, and its objective index also has evident advantages over some classical algorithms.
Lightweight structural materials with a unique combination of high stiffness, strength, toughness, and hardness, are highly desired yet challenging to be artificially fabricated. Biological ...structural materials, on the other hand, ingeniously integrate multiple mutually exclusive mechanical properties together relying on their hierarchically heterogeneous structures bonded with gradient interfaces. Here, a scalable bottom‐up approach combining continuous nanofiber‐assisted evaporation‐induced self‐assembly with laminating, pressure‐less sintering and resin infiltration is reported to fabricate bioinspired heterogeneous ceramic–resin composites with locally tunable microstructure to fulfill specific properties. A gradient interlayer is introduced to provide a gradual transition between adjacent heterogeneous layers, effectively alleviating their property mismatch. The optimized heterogeneous nacre‐like composite, as a demonstration, exhibits an attractive combination of low density (≈2.8 g cm−3), high strength (≈292 MPa), toughness (≈6.4 MPa m1/2), surface hardness (≈1144 kgf mm−2) and impact‐resistance, surpassing the overall performance of engineering alumina. This material‐independent approach paves the way for designing advanced bioinspired heterogeneous materials for diverse structural and functional applications.
By developing a simple bottom‐up assembly approach, nacre‐like ceramic–resin composites with tunable heterogeneous architectures are scalably manufactured. The composites are designed with a strong and tough nacre‐like main body, and a stiff and hard surface layer bonded by a gradient interlayer to alleviate property mismatch. This structural design achieves an impressive combination of low density and multiple desired mechanical properties.
Vast global declines of freshwater and marine fish diversity and population abundance pose serious threats to both ecosystem sustainability and human livelihoods. Environmental DNA (eDNA)‐based ...biomonitoring provides robust, efficient, and cost‐effective assessment of species occurrences and population trends in diverse aquatic environments. Thus, it holds great potential for improving conventional surveillance frameworks to facilitate fish conservation and fisheries management. However, the many technical considerations and rapid developments underway in the eDNA arena can overwhelm researchers and practitioners new to the field. Here, we systematically analysed 416 fish eDNA studies to summarize research trends in terms of investigated targets, research aims, and study systems, and reviewed the applications, rationales, methodological considerations, and limitations of eDNA methods with an emphasis on fish and fisheries research. We highlighted how eDNA technology may advance our knowledge of fish behaviour, species distributions, population genetics, community structures, and ecological interactions. We also synthesized the current knowledge of several important methodological concerns, including the qualitative and quantitative power eDNA has to recover fish biodiversity and abundance, and the spatial and temporal representations of eDNA with respect to its sources. To facilitate ecological applications implementing fish eDNA techniques, recent literature was summarized to generate guidelines for effective sampling in lentic, lotic, and marine habitats. Finally, we identified current gaps and limitations, and pointed out newly emerging research avenues for fish eDNA. As methodological optimization and standardization improve, eDNA technology should revolutionize fish monitoring and promote biodiversity conservation and fisheries management that transcends geographic and temporal boundaries.
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