Comprehension-driven design of advanced multi-block single-ion conducting polymer electrolytes for high-performance lithium-metal batteries

The continuously growing importance of batteries for powering(hybrid)electric vehicles and storing renewable energy has prompted a renewed focus on lithium-metal batteries(LMBs)in recent years,as its high theoretical specific capacity of about 3860 mA h g^(-1) and very low redox potential(-3.04 V vs.the standard hydrogen electrode)promise substantially higher energy densities compared to current lithium-ion batteries(LIBs)[1].However,lithium metal electrodes face severe challenges associated with the risk of dendritic lithium deposition and the high reactivity with traditional organic liquid electrolytes,resulting in a continuous loss of electrochemically active lithium and a relatively low Coulombic efficiency[2].To address these challenges,solid inorganic and polymer electrolytes have emerged as a potentially saferalternative.

Demonstrating grating-based phase-contrast imaging of laser-driven shock waves

Single-shot X-ray phase-contrast imaging is used to take high-resolution images of laser-driven strong shock waves.Employing a two-grating Talbot interferometer,we successfully acquire standard absorption,differential phase-contrast,and dark-field images of the shocked target.Good agreement is demonstrated between experimental data and the results of two-dimensional radiation hydrodynamics simulations of the laser-plasma interaction.The main sources of image noise are identified through a thorough assessment of the interferometer’s performance.The acquired images demonstrate that grating-based phase-contrast imaging is a powerful diagnostic tool for high-energy-density science.In addition,we make a novel attempt at using the dark-field image as a signal modality of Talbot interferometry to identify the microstructure of a foam target.

Activation of 2D MoS_(2) electrodes induced by high-rate lithiation processes

MoS_(2) is a highly promising material for application in lithium-ion battery anodes due to its high theoretical capacity and low cost.However,problems with a fast capacity decay over cycling,especially at the first cycles,and poor rate performance have deterred its practical implementation.Herein,electrodes comprised solely of few-layers 2D MoS_(2) nanosheets have been manufactured by scalable liquid-phase exfoliation and spray deposition methods.The long-standing controversy questioning the reversibility of conversion processes of MoS_(2)-based electrodes was addressed.Raman studies revealed that,in 2D MoS_(2) electrodes,conversion processes are indeed reversible,where nanostructure played a key role.Cycling of the electrodes at high current rates revealed an intriguing phenomenon consisting of a continuously increasing capacity after ca.100-200 cycles.This phenomenon was comprehensively addressed by a variety of electrochemical and microscopy methods that revealed underlying physical activation mechanisms that involved a range of profound electrode structural changes.Activation mechanisms delivered a capacitive electrode of a superior rate performance and cycling stability,as compared to the corresponding pristine electrodes,and to MoS_(2) electrodes previously reported.Herein,we have devised a methodology to overcome the problem of cycling stability of 2D MoS_(2) electrodes.Moreover,activation of electrodes constitutes a methodology that could be applied to enhance the energy storage performance of electrodes based on other 2D nanomaterials,or combinations thereof,strategically combining chemistries to engineer electrodes of superior energy storage properties.

Nano-additive manufacturing of multilevel strengthened aluminum matrix composites

Nanostructured materials are being actively developed,while it remains an open question how to rapidly scale them up to bulk engineering materials for broad industrial applications.This study propose an industrial approach to rapidly fabricate high-strength large-size nanostructured metal matrix composites and attempts to investigate and optimize the deposition process and strengthening mechanism.Here,advanced nanocrystalline aluminum matrix composites(nanoAMCs)were assembled for the first time by a novel nano-additive manufacturing method that was guided by numerical simulations(i.e.the in-flight particle model and the porefree deposition model).The present nanoAMC with a mean grain size<50 nm in matrix exhibited hardness eight times higher than the bulk aluminum and shows the highest hardness among all Al–Al2O3 composites reported to date in the literature,which are the outcome of controlling multiscale strengthening mechanisms from tailoring solution atoms,dislocations,grain boundaries,precipitates,and externally introduced reinforcing particles.The present high-throughput strategy and method can be extended to design and architect advanced coatings or bulk materials in a highly efficient(synthesizing a nanostructured bulk with dimensions of 50×20×4 mm^(3) in 9 min)and highly flexible(regulating the gradient microstructures in bulk)way,which is conducive to industrial production and application.

Trace-element geochemistry and S–O isotopes in the fluorite-barite mineralization of Merguechoum,Moroccan eastern Meseta:insights into ore genesis to the Pangea rifting

The Merguechoum fluorite-barite mineralization,located in the Eastern Meseta of Morocco,is hosted in the Late Hercynian granite.The ore consists of fine crystals of fluorite 1,massive barite 1,euhedral crystals of fluorite 2,and barite 2 with calcite and minor quartz and sulfides.The Merguechoum ore deposits have never been investigated.This study was the first contribution that studied the genesis of fluorite and barite.The ore occurs as dissemination within granite intrusion and also fills the NE-SWtrending meter-sized fractures and faults.The values of the total Rare Earth Elements and Yttrium(REY)and the ratios of LREY/HREY,Y/Ho,Tb/Ca,and Tb/La indicate that the Merguechoum fluorite precipitated from hydrothermal fluids,likely basinal brines,which interacted with the Hercynian granite.The REY data indicate that the ore-forming fluids of the early stage have intensely interacted with the Hercynian granite compared to those of the late ore stage.The gradual decrease in the europium(Eu/Eu^(*)),yttrium(Y/Y^(*)),and cerium(Ce/Ce^(*))anomalies and a low concentration ofΣREY observed in the second ore stage compared to the first ore stage suggest an increase in p H and fO_(2)and by inference a decrease in temperature during the evolution of the hydrothermal system.This evolution could be explained by fluid mixing between the ascending basinal hydrothermal fluids and the diluted sulfate-rich meteoric water barite separates from selected samples reveal that the dissolved sulfates(SO_(4)^(2-))were derived from Permian–Triassic sulfates and/or coeval poreseawater sulfates.The proposed fluid mixing triggered the precipitation of an early-stage F-Ba assemblage followed by the second-stage F-Ba mineralization.Geologic fieldwork,REY inventories,and isotope data point to the ore genesis during the Permian–Triassic extensional tectonic activity concerning the Pangea rifting.This extensional tectonic environment is likely the driving force that mobilized a large amount of the ore-forming basinal brines along the available faults and fractures to the loci of ore deposition.

Stepwise optimization of single-ion conducting polymer electrolytes for high-performance lithium-metal batteries

Single-ion conducting polymer electrolytes(SIPEs)are promising candidates for high-energy and highsafety lithium-metal batteries(LMBs).However,their insufficient ionic conductivity and electrochemical stability hinder their practical application.Herein,three new SIPEs,i.e.,poly(1,4-phenylene ether ether sulfone)-Li(PEES-Li),polysulfone-Li(PSF-Li),and hexafluoropolysulfone-Li(6FPSF-Li),all containing covalently tethered perfluorinated ionic side chains,have been designed,synthesized,and compared to investigate the influence of the backbone chemistry and the concentration of the ionic group on their electrochemical properties and cell performance.Especially,the trifluoromethyl group in the backbone and the concentration of the ionic function appear to play an essential role for the charge transport and stability towards oxidation,and the combination of both yields the best-performing SIPE with high ionic conductivity of ca.2.5×10^(-4)S cm^(-1),anodic stability of more than 4.8 V,and the by far highest capacity retention in Li‖LiNi0.6Co0.2Mn0.2O2cells.

Production of palmitoleic acid by oleaginous yeast Scheffersomyces segobiensis DSM 27193 using systematic dissolved oxygen regulation strategy

Palmitoleic acid(POA)can be naturally found only in few oil seeds and has significant applications in pharmaceutical industry.Recently,the isolated oleaginous yeast Scheffersomyces segobiensis DSM 27193 was identified with high content of POA in its intracellular lipid(13.80%).In this study,process optimization focused on dissolved oxygen regulation to improve POA production was conducted.Dynamic agitation was found to do significant enhancement on POA-rich lipid production than aeration regulation.Under the best condition of 1000 r·min^(-1)of agitation and 1 vvm(airvolume/culture volume/min)of aeration,no ethanol was detected during the whole fermentation process,while a dry biomass concentration of 44.80 g·L^(-1)with 13.43 g·L^(-1)of lipid and 2.93 g·L^(-1)of POA was achieved.Transcription analysis revealed that the ethanol synthetic pathway was downregulated under the condition of high agitation,while the expression of the key enzymes responsible for lipid and POA accumulation were enhanced.

Non-crossing Quantile Regression Neural Network as a Calibration Tool for Ensemble Weather Forecasts

Despite the maturity of ensemble numerical weather prediction(NWP),the resulting forecasts are still,more often than not,under-dispersed.As such,forecast calibration tools have become popular.Among those tools,quantile regression(QR)is highly competitive in terms of both flexibility and predictive performance.Nevertheless,a long-standing problem of QR is quantile crossing,which greatly limits the interpretability of QR-calibrated forecasts.On this point,this study proposes a non-crossing quantile regression neural network(NCQRNN),for calibrating ensemble NWP forecasts into a set of reliable quantile forecasts without crossing.The overarching design principle of NCQRNN is to add on top of the conventional QRNN structure another hidden layer,which imposes a non-decreasing mapping between the combined output from nodes of the last hidden layer to the nodes of the output layer,through a triangular weight matrix with positive entries.The empirical part of the work considers a solar irradiance case study,in which four years of ensemble irradiance forecasts at seven locations,issued by the European Centre for Medium-Range Weather Forecasts,are calibrated via NCQRNN,as well as via an eclectic mix of benchmarking models,ranging from the naïve climatology to the state-of-the-art deep-learning and other non-crossing models.Formal and stringent forecast verification suggests that the forecasts post-processed via NCQRNN attain the maximum sharpness subject to calibration,amongst all competitors.Furthermore,the proposed conception to resolve quantile crossing is remarkably simple yet general,and thus has broad applicability as it can be integrated with many shallow-and deep-learning-based neural networks.

Insights into the hydrogen evolution reaction in vanadium redox flow batteries:A synchrotron radiation based X-ray imaging study

The parasitic hydrogen evolution reaction(HER)in the negative half-cell of vanadium redox flow batteries(VRFBs)causes severe efficiency losses.Thus,a deeper understanding of this process and the accompanying bubble formation is crucial.This benchmarking study locally analyzes the bubble distribution in thick,porous electrodes for the first time using deep learning-based image segmentation of synchrotron X-ray micro-tomograms.Each large three-dimensional data set was processed precisely in less than one minute while minimizing human errors and pointing out areas of increased HER activity in VRFBs.The study systematically varies the electrode potential and material,concluding that more negative electrode potentials of-200 m V vs.reversible hydrogen electrode(RHE)and lower cause more substantial bubble formation,resulting in bubble fractions of around 15%–20%in carbon felt electrodes.Contrarily,the bubble fractions stay only around 2%in an electrode combining carbon felt and carbon paper.The detected areas with high HER activity,such as the border subregion with more than 30%bubble fraction in carbon felt electrodes,the cutting edges,and preferential spots in the electrode bulk,are potential-independent and suggest that larger electrodes with a higher bulk-to-border ratio might reduce HER-related performance losses.The described combination of electrochemical measurements,local X-ray microtomography,AI-based segmentation,and 3D morphometric analysis is a powerful and novel approach for local bubble analysis in three-dimensional porous electrodes,providing an essential toolkit for a broad community working on bubble-generating electrochemical systems.

Fiber Bundle Topology Optimization for Surface Flows

This paper presents a topology optimization approach for the surface flows on variable design domains.Via this approach,the matching between the pattern of a surface flow and the 2-manifold used to define the pattern can be optimized,where the 2-manifold is implicitly defined on another fixed 2-manifold named as the base manifold.The fiber bundle topology optimization approach is developed based on the description of the topological structure of the surface flow by using the differential geometry concept of the fiber bundle.The material distribution method is used to achieve the evolution of the pattern of the surface flow.The evolution of the implicit 2-manifold is realized via a homeomorphous map.The design variable of the pattern of the surface flow and that of the implicit 2-manifold are regularized by two sequentially implemented surface-PDE filters.The two surface-PDE filters are coupled,because they are defined on the implicit 2-manifold and base manifold,respectively.The surface Navier-Stokes equations,defined on the implicit 2-manifold,are used to describe the surface flow.The fiber bundle topology optimization problem is analyzed using the continuous adjoint method implemented on the first-order Sobolev space.Several numerical examples have been provided to demonstrate this approach,where the combination of the viscous dissipation and pressure drop is used as the design objective.

Recycled graphite for more sustainable lithium-ion batteries

The demand for lithium-ion batteries(LIBs)is driven largely by their use in electric vehicles,which is projected to increase dramatically in the future.This great success,however,urgently calls for the efficient recycling of LIBs at the end of their life.Herein,we describe a froth flotation-based process to recycle graphite—the predominant active material for the negative electrode—from spent LIBs and investigate its reuse in newly assembled LIBs.It has been found that the structure and morphology of the recycled graphite are essentially unchanged compared to pristine commercial anode-grade graphite,and despite some minor impurities from the recycling process,the recycled graphite provides a remarkable reversible specific capacity of more than 350 mAh g^(−1).Even more importantly,newly assembled graphite‖NMC532 cells show excellent cycling stability with a capacity retention of 80%after 1000 cycles,that is,comparable to the performance of reference full cells comprising pristine commercial graphite.

校外科学学习环境中的兴趣建模:系统性文献综述

校外科学学习环境丰富了许多国家的课堂教学。已有大量研究探讨了校外学习环境所带来的影响,尤其是校外学习环境促进兴趣养成的能力。由于这些研究中运用了不同的兴趣理论,迄今为止,还没有关于该研究领域的综述。因此,本文在全面系统回顾国际文献的基础上,详细分析了兴趣理论在校外学习环境研究中的应用。此外,本文还得出了关于在校外科学学习环境中促进情境兴趣和个体兴趣提升的推论,结果清晰表明,情境兴趣通过这类学习环境得以促进提升。结合不同兴趣理论所提出的影响因素,本文构建了校外学习环境中的学生兴趣模型,该模型可用于指导校外学习环境的开发和进一步完善。

环氧树脂涂层中添加含铝复合粉增强碳钢基材的防腐性

采用电化学阻抗谱(EIS)和电位极化(Tafel)试验,研究了在环氧树脂涂层中添加含铝粉末以增强碳钢基材的防腐性,含铝粉末包括纯铝、Al/CNT、Al/Al_(2)O_(3)、Al/CNT/Al_(2)O_(3)。用球磨法合成含2 wt.%碳纳米管、2 wt.%氧化铝纳米颗粒的复合粉末,然后以1 wt.%的浓度加入到环氧树脂涂层中。结果表明,由于环氧树脂复合涂层的防护性能增强,从而提高了其耐腐蚀性。研究还发现,Al/CNT/Al_(2)O_(3)复合添加剂的保护性能比其他添加剂更显著,因为其颗粒尺寸的减小和具有某些形状的颗粒,进一步减少了腐蚀环境通过涂层渗透的路径,避免了金属基底/涂层界面可能发生的反应。EP-Al/CNT/Al_(2)O_(3)保持了一次时间常数特性,并在整个暴露时间内表现出最高的阻抗和最强的稳定性。这些添加剂的存在增强了涂层,从而改善了涂层的屏障性能。

Estimation of diaphragm wall deflections for deep braced excavation in anisotropic clays using ensemble learning

This paper adopts the NGI-ADP soil model to carry out finite element analysis,based on which the effects of soft clay anisotropy on the diaphragm wall deflections in the braced excavation were evaluated.More than one thousand finite element cases were numerically analyzed,followed by extensive parametric studies.Surrogate models were developed via ensemble learning methods(ELMs),including the e Xtreme Gradient Boosting(XGBoost),and Random Forest Regression(RFR)to predict the maximum lateral wall deformation(δhmax).Then the results of ELMs were compared with conventional soft computing methods such as Decision Tree Regression(DTR),Multilayer Perceptron Regression(MLPR),and Multivariate Adaptive Regression Splines(MARS).This study presents a cutting-edge application of ensemble learning in geotechnical engineering and a reasonable methodology that allows engineers to determine the wall deflection in a fast,alternative way.

Function spaces of Besov-type and Triebel-Lizorkin-type——a survey

This article is devoted to presenting a recapitulative introduction for the theory of Besov-type and Triebel-Lizorkin-type spaces developed in recent years.

Effects of Potassium and Manganese Promoters on Nitrogen-Doped Carbon Nanotube-Supported Iron Catalysts for CO_2 Hydrogenation

Nitrogen-doped carbon nanotubes （NCNTs） were used as a support for iron （Fe） nanoparticles applied in car- bon dioxide （CO_2） hydrogenation at 633 K and 25 bar （1 bar = 10-5 Pa）. The Fe/NCNT catalyst promoted with both potassium （K） and manganese （Mn） showed high performance in CO_2 hydrogenation, reaching 34.9% conversion with a gas hourly space velocity （GHSV） of 3.1 L-（g·h）-1. Product selectivities were high for olefin products and low for short-chain alkanes for the K-promoted catalysts. When Fe/NCNT catalyst was promot- ed with both K and Mn, the catalytic activity was stable for 60 h of reaction time. The structural effect of the Mn promoter was demonstrated by X-ray diffraction （XRD）, temperature-programmed reduction （TPR） with molecular hydrogen （H2）, and in situ X-ray absorption near-edge structure （XANES） analysis. The Mn pro- moter stabilized wtistite （FeO） as an intermediate and lowered the TPR onset temperature. Catalytic ammo- nia （NH_3） decomposition was used as an additional probe reaction for characterizing the promoter effects. The Fe/NCNT catalyst promoted with both K and Mn had the highest catalytic activity, and the Mn-promoted Fe/NCNT catalysts had the highest thermal stability under reducing conditions.

Reduction and carburization of iron oxides for Fischer–Tropsch synthesis

The activation of iron oxide Fischer–Tropsch Synthesis(FTS) catalysts was investigated during pretreatment: reduction in hydrogen followed by carburization in either CO or syngas mixture, or simultaneously reduction and carburization in syngas. A combination of different complementary in situ techniques was used to gain insight into the behavior of Fe-based FTS catalysts during activation. In situ XRD was used to identify the crystalline structures present during both reduction in hydrogen and carburization. An increase in reduction rate was established when increasing the temperature. A complete reduction was demonstrated in the ETEM and a grain size dependency was proven, i.e. bigger grains need higher temperature in order to reduce. XPS and XAS both indicate the formation of a small amount of carbonaceous species at the surface of the bulk metallic iron during carburization.

Smart Transformer-based Medium Voltage Grid Support by Means of Active Power Control

In the last decades the voltage regulation has been challenged by the increase of power variability in the electric grid,due to the spread of non-dispatchable generation sources.This paper introduces a Smart Transformer(ST)-based Medium Voltage(MV)grid support by means of active power control in the ST-fed Low Voltage(LV)grid.The aim of the proposed strategy is to improve the voltage profile in MV grids before the operation of On-Load Tap Changer in the primary substation transformer,which needs tens of seconds.This is realized through reactive power injection by the AC/DC MV converter and simultaneous decrease of the active power consumption of voltage-dependent loads in ST-fed LV grid,controlling the ST output voltage.The last feature has two main effects:the first is to reduce the active power withdrawn from MV grid,and consequently the MV voltage drop caused by the active current component.At the same time,higher reactive power injection capability in the MV converter is unlocked,due to the lower active power demand.As result,the ST increases the voltage support in MV grid.The analysis and simulation results carried out in this paper show improvements compared to similar solutions,i.e.the only reactive power compensation.The impact of the proposed solution has been finally evaluated under different voltage-dependence of the loads in the LV grid.

The impact of nitrogen amendment and crop growth on dissolved organic carbon in soil solution

Dissolved organic carbon(DOC) is an important component of the terrestrial carbon cycle.However,the sources and controlling factors of DOC in soils remain uncertain.In this study,the effects of nitrogen(N) amendment and crop growth on DOC in soil solution were examined at a maize-wheat rotated field located in the central Sichuan Basin in southwestern China.Nitrogen treatments in this study included 150 kg N ha-1 season-1,200 kg N ha-1 season-1 and the control without any fertilizer application.During the whole experimental period,we observed significant decreases(p<0.05) in DOC concentrations in the sampled soil solutions associated with increase in N inputs at the bare soil plots,but no change in DOC at the plots with crop growth.The estimated average contributions of plantderived DOC were 16%,24% and 32% of total DOC in the summer maize season and 21%,32% and 38% in the winter wheat season along with the gradient of N fertilizer application rates.The results implied thatthe crop growth could play a key role in the soil DOC production,and the N input enhanced DOC production by increasing crop growth.The relationship between the DOC concentrations and the crop root biomass was statistically significant for both the maize and winter wheat seasons.Our observations indicated that crop growth exerted greater influence on the seasonal variability of DOC concentration in soil solutions at the experimental site,which overwhelmed the effect of soil native organic matter decomposition on DOC concentrations in soil solutions.

Assessing the microstructure and in vitro degradation behavior of Mg-xGd screw implants using μCT

Biodegradable implants are taking an increasingly important role in the area of orthopedic implants with the aim to replace permanent implants for temporary bone healing applications.During the implant preparation process,the material’s surface and microstructure are being changed by stresses induced by machining.Hence degradable metal implants need to be fully characterized in terms of the influence of machining on the resulting microstructure and corrosion performance.In this study,micro-computed tomography(μCT)is used for the quantification of the degradation rate of biodegradable implants.To our best knowledge,for the first time quantitative measures are introduced to describe the degradation homogeneity in 3D.This information enables a prediction in terms of implant stability during the degradation in the body.Two magnesium gadolinium alloys,Mg-5Gd and Mg-10 Gd(all alloy compositions are given in weight%unless otherwise stated),in the shape of M2 headless screws have been investigated for their microstructure and their degradation performance up to 56 days.During the microstructure investigations particular attention was paid to the localized deformation of the alloys,due to the machining process.In vitro immersion testing was performed to assess the degradation performance quantified by subsequent weight loss and volume loss(usingμCT)measurements.Although differences were observed in the degree of screw’s near surface microstructure being influenced from machining,the degradation rates of both materials appeared to be suitable for application in orthopedic implants.From the degradation homogeneity point of view no obvious contrast was detected between both alloys.However,the higher degradation depth ratios between the crests and roots of Mg-5Gd ratios may indicated a less homogeneous degradation of the screws of these alloys on contract to the ones made of Mg-10Gd alloys.Due to its lower degradation rates,its more homogeneous microstructure,its weaker texture and better degradation performance extruded Mg-10Gd emerged more suitable as implant material than Mg-5Gd.