This paper investigates the impact of reducing feature-vector dimensionality on the performance of machine learning(ML)models.Dimensionality reduction and feature selection techniques can improve computational efficie...This paper investigates the impact of reducing feature-vector dimensionality on the performance of machine learning(ML)models.Dimensionality reduction and feature selection techniques can improve computational efficiency,accuracy,robustness,transparency,and interpretability of ML models.In high-dimensional data,where features outnumber training instances,redundant or irrelevant features introduce noise,hindering model generalization and accuracy.This study explores the effects of dimensionality reduction methods on binary classifier performance using network traffic data for cybersecurity applications.The paper examines how dimensionality reduction techniques influence classifier operation and performance across diverse performancemetrics for seven ML models.Four dimensionality reduction methods are evaluated:principal component analysis(PCA),singular value decomposition(SVD),univariate feature selection(UFS)using chi-square statistics,and feature selection based on mutual information(MI).The results suggest that direct feature selection can be more effective than data projection methods in some applications.Direct selection offers lower computational complexity and,in some cases,superior classifier performance.This study emphasizes that evaluation and comparison of binary classifiers depend on specific performance metrics,each providing insights into different aspects of ML model operation.Using open-source network traffic data,this paper demonstrates that dimensionality reduction can be a valuable tool.It reduces computational overhead,enhances model interpretability and transparency,and maintains or even improves the performance of trained classifiers.The study also reveals that direct feature selection can be a more effective strategy when compared to feature engineering in specific scenarios.展开更多
In dynamic problems the electric and magnetic fields are inseparable. At the same time, a multitude of electrostatic and magnetostatic effects permit mutually independent description. This separation appears to be pos...In dynamic problems the electric and magnetic fields are inseparable. At the same time, a multitude of electrostatic and magnetostatic effects permit mutually independent description. This separation appears to be possible and thermodynamically consistent when the bulk energy density depends only on the polarization density or, alternatively, on the magnetization density. However, when the bulk energy density depends simultaneously on the both densities, then, the electrostatic and magnetostatic effects should be studied together. There appear interesting cross-effects;among those are the change of the internal electrostatic field inside a specimen under the influence of the external magnetic fields, and vice versa. Below, in the framework of thermodynamic approach the boundary value problem for magnetoelectric plate is formulated and analyzed. The exact solution is established for the isotropic pyroelectric plate.展开更多
Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above proble...Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above problems are poorly understood. Studying the cycling and float-charging characteristics of Li/NCM811 cells in high voltage conditions(4.5 V and 4.7 V, respectively), in this work we find that nearly all known problems with NCM811 material can be attributed to the oxidation of lattice oxygen occurring in the capacity region corresponding to H2 → H3 phase transition. While contributing to overall capacity,the oxidation of lattice oxygen results in a loss of oxygen through oxygen evolution and relative reactions between active oxygen evolution intermediates and electrolyte solvents. It is the loss of oxygen that results in irreversible layered-spinel-rocksalt phase transition, secondary particle cracking, and performance degradation. The conclusions of this work suggest that the priority for further research on NCM811 material should give to the suppression of oxygen evolution, followed by the use of the anti-oxygen electrolyte being chemically stable against the active oxygen evolution intermediates.展开更多
The oxygen evolution reaction(OER)is the essential module in energy conversion and storage devices such as electrolyzer,rechargeable metal–air batteries and regenerative fuel cells.The adsorption energy scaling relat...The oxygen evolution reaction(OER)is the essential module in energy conversion and storage devices such as electrolyzer,rechargeable metal–air batteries and regenerative fuel cells.The adsorption energy scaling relations between the reaction intermediates,however,impose a large intrinsic overpotential and sluggish reaction kinetics on OER catalysts.Developing advanced electrocatalysts with high activity and stability based on non-noble metal materials is still a grand challenge.Central to the rational design of novel and high-efficiency catalysts is the development and understanding of quantitative structure–activity relationships,which correlate the catalytic activities with structural and electronic descriptors.This paper comprehensively reviews the benchmark descriptors for OER electrolysis,aiming to give an in-depth understanding on the origins of the electrocatalytic activity of the OER and further contribute to building the theory of electrocatalysis.Meanwhile,the cutting-edge research frontiers for proposing new OER paradigms and crucial strategies to circumvent the scaling relationship are also summarized.Challenges,opportunities and perspectives are discussed,intending to shed some light on the rational design concepts and advance the development of more efficient catalysts for enhancing OER performance.展开更多
This paper introduces a model-free reinforcement learning technique that is used to solve a class of dynamic games known as dynamic graphical games. The graphical game results from to make all the agents synchronize t...This paper introduces a model-free reinforcement learning technique that is used to solve a class of dynamic games known as dynamic graphical games. The graphical game results from to make all the agents synchronize to the state of a command multi-agent dynamical systems, where pinning control is used generator or a leader agent. Novel coupled Bellman equations and Hamiltonian functions are developed for the dynamic graphical games. The Hamiltonian mechanics are used to derive the necessary conditions for optimality. The solution for the dynamic graphical game is given in terms of the solution to a set of coupled Hamilton-Jacobi-Bellman equations developed herein. Nash equilibrium solution for the graphical game is given in terms of the solution to the underlying coupled Hamilton-Jacobi-Bellman equations. An online model-free policy iteration algorithm is developed to learn the Nash solution for the dynamic graphical game. This algorithm does not require any knowledge of the agents＇ dynamics. A proof of convergence for this multi-agent learning algorithm is given under mild assumption about the inter-connectivity properties of the graph. A gradient descent technique with critic network structures is used to implement the policy iteration algorithm to solve the graphical game online in real-time.展开更多
Traumatic injury is one of the leading causes of death, with uncontrolled hemorrhage from coagulation dysfunction as one of the main potentially preventable causes of the mortality. Hypothermia, acidosis, and resuscit...Traumatic injury is one of the leading causes of death, with uncontrolled hemorrhage from coagulation dysfunction as one of the main potentially preventable causes of the mortality. Hypothermia, acidosis, and resuscitative hemodilution have been considered as the significant contributors to coagulation manifestations following trauma, known as the lethal triad. Over the past decade, clinical observations showed that coagulopathy may be present as early as hospital admission in some severely injured trauma patients. The hemostatic dysfunction is associated with higher blood transfusion requirements, longer hospital stay, and higher mortality. The recognition of this early coagulopathy has initiated tremendous interest and effort in the trauma community to expand our understanding of the underlying pathophysiology and improve clinical treatments. This review discusses the current knowledge of coagulation complications following trauma.展开更多
AIM： To investigate the therapeutic potential of an RNA ligand （aptamer） specific for the catalytic ricin A-chain （RTA）, the protective effects of a 31-nucleo- tide RNA aptamer （31RA）, which formed a high affin...AIM： To investigate the therapeutic potential of an RNA ligand （aptamer） specific for the catalytic ricin A-chain （RTA）, the protective effects of a 31-nucleo- tide RNA aptamer （31RA）, which formed a high affinity complex with RTA, against ricin-induced toxicity in cell- based luciferase translation and cell cytotoxicity assays were evaluated. METHODS： To test the therapeutic potential of anti- RTA aptamers in Chinese hamster ovary （CliO） AA8 cells stably transfected with a tetracycline regulatable promoter, ricin ribotoxicity was measured us- ing luciferase and ricin-induced cytotoxicity was ascertained by MTS cell proliferation assay with tet- razolium compound [3-（4,5-dimethylthiazol-2-yl）- 5-（3-carboxymethoxyphenyl）-2-（4-sulfophenyl）-2H- tetrazolium]. RESULTS： Inhibition of protein synthesis by ricin in CliO AA8 cells resulted in diminished luciferase activity and treatment with polyclonal antibody against degly- cosylated RTA （dgA） neutralized the inhibitory effects of ricin on luciferase activity and protected against ricin-induced cytotoxicity as measured by MTS assay. The 31RA anti-RTA aptamer inhibited the translation of luciferase mRNA in cell-free reticulocyte translation assay. 31RA aptamer also partially neutralized the inhibitory effects of ricin on luciferase activity and partially protected against ricin-induced cytotoxicity in CliO AA8 cells. CONCLUSION： We have shown that anti-RTA RNA aptamer can protect against ricin ribotoxicity in cell- based luciferase and cell cytotoxicity assays. Hence, RNA aptamer that inhibits RTA enzymatic activity represents a novel class of nucleic acid inhibitor that has the potential to be developed as a therapeutic agent for the treatment of ricin intoxication.展开更多
A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)i...A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)ion,1-aza-12-crown-4-ether(A12C4)with cavity size well matched manganese(Ⅱ)ion is used in this work as electrolyte additive.Theoretical and experimental results show that stable complex forms between A12C4 and manganese(II)ions in the electrolyte,which does not affect the solvation of Li ions.The strong binding effect of A12C4 additive reduces the charge density of manganese(II)ion and inhibits its destruction of the PF_(6)^(-)structure in the electrolyte,leading to greatly improved thermal stability of manganese(II)ions-containing electrolyte.In addition to bulk electrolyte,A12C4 additive also shows capability in preventing Mn^(2+) from degrading SEI on graphite surface.Such bulk and interphasial stability introduced by A12C4 leads to significantly improved cycling performance of LIBs.展开更多
In this study, phosphorus(P) sorption of thirteen light-weight aggregates(LWAs) from USA was compared during batch equilibrium experiments in order to identify those materials which had the highest P sorption capacity...In this study, phosphorus(P) sorption of thirteen light-weight aggregates(LWAs) from USA was compared during batch equilibrium experiments in order to identify those materials which had the highest P sorption capacity for further study. Seven different levels of sorption activity were observed, which were broadly grouped into three categories—high performing, middle performing, and low performing aggregates. Chemical analysis of Ca, Al, Fe, and Mg was used to describe the differences between LWAs. There was a significant correlation between cation(especially Al, Ca, Fe, and Mg) content and P sorbed. Langmuir isotherms were used to describe P sorption maximum and binding affinity for four of the top five performing LWAs, Universal, Stalite "D", Stalite "Mix", and TXI.The fifth aggregate, Lehigh, exhibited more complex sorption, and was better described by the Freundlich isotherm. Universal had a mean P sorption at the highest concentration of 824 mg kg-1, well above its calculated sorption maximum(702 mg kg-1), and also had the highest binding affinity(1.1 L mg-1). This experiment suggests that the top performing LWA(Universal) may perform poorly in column and field studies due to observed precipitates, which could degrade constructed wetland performance. Other LWAs may exhibit superior field performance due to their high calculated sorption maxima. In general, these results highlight the importance of batch experiments as a first step in identifying materials suitable for column and field experiments.展开更多
Fast charging of Li-ion cells faces two aspects of challenges,1)accelerated capacity fade and 2)inferior charging capability.It is commonly believed that the former is due to Li plating and its resultant reactions wit...Fast charging of Li-ion cells faces two aspects of challenges,1)accelerated capacity fade and 2)inferior charging capability.It is commonly believed that the former is due to Li plating and its resultant reactions with electrolyte at the graphite anode,which results in a loss in the inventory of Li+ions and an increase in the cell’s impedance.While the latter is ascribed to the high voltage polarization in relation to the slow transport of Li+ions between two electrodes.However,there are many other hidden facts that essentially affect the fast charging performances of Li-ion cells.This commentary intends,from the view of materials,to uncover these hidden factors,including failure of the solid electrolyte interphase and exfoliation of the graphite structure at the anode,structural degradation of the Ni-rich layered cathode materials,as well as the high solvation and desolvation activation energies of Li+ions in the electrolyte.Meanwhile,some solutions to the fast-charging problems of Li-ion cells are proposed based on the understanding of these hidden factors.展开更多
Hydroelectric facilities impact water temperature; low velocities in a reservoir increase residence time and enhance heat exchange in surface layers. In this study, an unsteady three-dimensional model was developed to...Hydroelectric facilities impact water temperature; low velocities in a reservoir increase residence time and enhance heat exchange in surface layers. In this study, an unsteady three-dimensional model was developed to predict the temperatm＇e dynamics in the McNary Dam forebay. The model is based on the open-source code OpenFOAM. RANS equations with the Boussinesq approximation were used to solve the flow field. A： realizable k-ε model that accounts for the production of wind turbulence was developed. Solar radiation and convective heat transfer at the free surface were included. The result of the model was compared with the field data collected on August 18, 2004. Changes in diurnal stratification were adequately predicted by the model. Observed vertical and lateral temperature distributions were accurately captured. Results indicate that the model can be used as a numerical tool to assess structural and operational alternatives to reduce the forebay temperature.展开更多
The non-flammability and high oxidation stability of sulfolane(SL)make it an excellent electrolyte candidate for lithium-ion batteries(LIBs).However,its incompatibility with graphitic anode prevents the realization of...The non-flammability and high oxidation stability of sulfolane(SL)make it an excellent electrolyte candidate for lithium-ion batteries(LIBs).However,its incompatibility with graphitic anode prevents the realization of these advantages.To understand how this incompatibility arises on molecular level so that it can be suppressed,we combined theoretical calculation and experimental characterization and reveal that the primary Li^(+) solvation sheath in SL is depleted of fluorine source.Upon reduction,SL in such fluorine-poor solvation sheath generates insoluble dimer with poor electronic insulation,hence leading to slow but sustained parasitic reactions.When fluorine content in Li^(+)-SL solvation sheath is increased via salt concentration,a high stability LiF-rich interphase on graphite can be formed.This new understanding of the failure mechanism of graphite in SL-based electrolyte is of great significance in unlocking many possible electrolyte solvent candidates for the high-voltage cathode materials for next-generation LIBs.展开更多
Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption ...Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption property of the core-shell nanorods were well characterized with XRD and TEM. The catalytic activity and stability were electrochemically evaluated with a rotating disk electrode, a rotating ring-disk electrode, and chronopotentiometric methods. The Ru@RuO2 nanorods reveal excellent bifunctional catalytic activity and robust stability for both oxygen evolution reaction(OER) and hydrogen evolution reaction(HER). The overpotentials for OER and HER are 320 m V and 137 m V at the current density of10 m A cm-2, respectively. The catalytic activity of Ru@RuO2 nanorods for OER is 6.5 times higher than that of the state-of-the-art catalyst IrO2 according to the catalytic current density measured at 1.60 V(versus RHE).The catalytic activity of Ru@RuO2 nanorods for HER is comparable to 40%Pt/C by comparing the catalytic current densities at à0.2 V.展开更多
Lithium-rich oxide is one of the most promising cathodes that meet high energy density requirement for batteries of the future, but its phase transformation from layer to spinel structure caused by the lattice instabi...Lithium-rich oxide is one of the most promising cathodes that meet high energy density requirement for batteries of the future, but its phase transformation from layer to spinel structure caused by the lattice instability presents severe challenge to cycling stability and the actually accessible capacity. The currently available approaches to suppress this undesired irreversible process often resort to limit the high voltages that lithium-rich oxide is exposed to. However, cycling stability thus improved is at the expense of the eventual energy output. In this work, we identified a new mechanism that is directly responsible for the lithium-rich oxide phase transformation and established a clear correlation between the successive consumption of Li+on anode due to incessant interphase repairing and the over-delithiation of lithium-rich oxide cathode. This new mechanism enables a simple but effective solution to the cathode degradation, in which an electrolyte additive is used to build a dense and protective interphase on anode with the intention to minimize Li depletion at cathode. The application of this new interphase effectively suppresses both electrolyte decomposition at anode and the phase transformation of lithium-rich oxide cathode, leading to high capacity and cycling stability.展开更多
Using ab initio molecular dynamics(AIMD)simulations,classical molecular dynamics(CMD)simulations,small-angle X-ray scattering(SAXS),and pulsed-field gradient nuclear magnetic resonance(PFG-NMR),the solvation structure...Using ab initio molecular dynamics(AIMD)simulations,classical molecular dynamics(CMD)simulations,small-angle X-ray scattering(SAXS),and pulsed-field gradient nuclear magnetic resonance(PFG-NMR),the solvation structure and ion dynamics of magnesium bis(trifluoromethanesulfonyl)imide(Mg(TFSI)_(2))aqueous electrolyte at 1,2,and 3 m concentrations are investigated.From AIMD and CMD simulations,the first solvation shell of an Mg;ion is found to be composed of six water molecules in an octahedral configuration and the solvation shell is rather rigid.The TFSI^(-)ions prefer to stay in the second solvation shell and beyond.Meanwhile,the comparable diffusion coefficients of positive and negative ions in Mg(TFSI)_(2)aqueous electrolytes have been observed,which is mainly due to the formation of the stable[Mg(H_(2)O_(6))_(2)]^(+)complex,and,as a result,the increased effective Mg ion size.Finally,the calculated correlated transference numbers are lower than the uncorrelated ones even at the low concentration of 2 and 3 m,suggesting the enhanced correlations between ions in the multivalent electrolytes.This work provides a molecular-level understanding of how the solvation structure and multivalency of the ion affect the dynamics and transport properties of the multivalent electrolyte,providing insight for rational designs of electrolytes for improved ion transport properties.展开更多
We analyze the propagation of electromagnetic fronts in unbounded electric conductors. Our analysis is based on the Maxwell model of electromagnetism that includes the displacement current and Ohm’s law in its simple...We analyze the propagation of electromagnetic fronts in unbounded electric conductors. Our analysis is based on the Maxwell model of electromagnetism that includes the displacement current and Ohm’s law in its simplest forms. A weak electromagnetic front is a propagating interface at which the electromagnetic field remains continuous while its first- and higher-order derivatives experience finite jump discontinuities. Remarkably, analysis of such fronts can be performed autonomously, <em>i</em>.<em>e</em>. strictly in terms of the quantities defined on the front. This property opens the possibility of establishing exact analytical solutions of the exact Maxwell system along with the evolution of the front.展开更多
Simple and double layers first appeared in electrostatics and later found various applications in mathematical physics. In this paper, we present the jump discontinuity conditions for their second-order spatial deriva...Simple and double layers first appeared in electrostatics and later found various applications in mathematical physics. In this paper, we present the jump discontinuity conditions for their second-order spatial derivatives.展开更多
In-bore yaw of a projectile in a gun tube has been shown to result in range loss if the yaw is significant. An attempt was made to determine if relationships between in-bore yaw and projectile First Maximum Yaw(FMY) w...In-bore yaw of a projectile in a gun tube has been shown to result in range loss if the yaw is significant. An attempt was made to determine if relationships between in-bore yaw and projectile First Maximum Yaw(FMY) were observable. Experiments were conducted in which pressure transducers were mounted near the muzzle of a 155 mm cannon in three sets of four. Each set formed a cruciform pattern to obtain a differential pressure across the projectile. These data were then integrated to form a picture of what the overall pressure distribution was along the side of the projectile. The pressure distribution was used to determine a magnitude and direction of the overturning moment acting on the projectile. This moment and its resulting angular acceleration were then compared to the actual first maximum yaw observed in the test. The degree of correlation was examined using various statistical techniques. Overall uncertainty in the projectile dynamics was between 20% and 40% of the mean values of FMY.展开更多
Convection and its ensuing severe weather, such as heavy rainfall, hail, tornado, and high wind, have significant im- pacts on our society and economy （e.g., Cao et al., 2004; Fritsch and Carbone, 2004; Verbout et al...Convection and its ensuing severe weather, such as heavy rainfall, hail, tornado, and high wind, have significant im- pacts on our society and economy （e.g., Cao et al., 2004; Fritsch and Carbone, 2004; Verbout et al., 2006; Ashley and Black, 2008; Cao, 2008; Cao and Ma, 2009; Zhang et al., 2014）. Due to its localized and transient nature, the initiation of convection or convective initiation remains one of the least understood aspects of convection in the scientific communi- ties, and it is a significant challenge to accurately predict the exact timing and location of convective initiation （e.g., Cai et al., 2006; Wilson and Roberts, 2006; Xue and Martin, 2006; Cao and Zhang, 2016）.展开更多
基金funded by US Army Combat Capabilities Development Command(CCDC)Aviation&Missile Center,https://www.avmc.army.mil/(accessed on 5 February 2024),CONTRACT NUMBER:W31P4Q-18-D-0002 through Georgia Tech Research Institute and AAMU-RISE。
文摘This paper investigates the impact of reducing feature-vector dimensionality on the performance of machine learning(ML)models.Dimensionality reduction and feature selection techniques can improve computational efficiency,accuracy,robustness,transparency,and interpretability of ML models.In high-dimensional data,where features outnumber training instances,redundant or irrelevant features introduce noise,hindering model generalization and accuracy.This study explores the effects of dimensionality reduction methods on binary classifier performance using network traffic data for cybersecurity applications.The paper examines how dimensionality reduction techniques influence classifier operation and performance across diverse performancemetrics for seven ML models.Four dimensionality reduction methods are evaluated:principal component analysis(PCA),singular value decomposition(SVD),univariate feature selection(UFS)using chi-square statistics,and feature selection based on mutual information(MI).The results suggest that direct feature selection can be more effective than data projection methods in some applications.Direct selection offers lower computational complexity and,in some cases,superior classifier performance.This study emphasizes that evaluation and comparison of binary classifiers depend on specific performance metrics,each providing insights into different aspects of ML model operation.Using open-source network traffic data,this paper demonstrates that dimensionality reduction can be a valuable tool.It reduces computational overhead,enhances model interpretability and transparency,and maintains or even improves the performance of trained classifiers.The study also reveals that direct feature selection can be a more effective strategy when compared to feature engineering in specific scenarios.
文摘In dynamic problems the electric and magnetic fields are inseparable. At the same time, a multitude of electrostatic and magnetostatic effects permit mutually independent description. This separation appears to be possible and thermodynamically consistent when the bulk energy density depends only on the polarization density or, alternatively, on the magnetization density. However, when the bulk energy density depends simultaneously on the both densities, then, the electrostatic and magnetostatic effects should be studied together. There appear interesting cross-effects;among those are the change of the internal electrostatic field inside a specimen under the influence of the external magnetic fields, and vice versa. Below, in the framework of thermodynamic approach the boundary value problem for magnetoelectric plate is formulated and analyzed. The exact solution is established for the isotropic pyroelectric plate.
文摘Inferior cycling stability, poor safety, and gas generation are long lasting problems of Ni-rich Li Ni0.80 Co0.10 Mn0.10 O2(NCM811) cathode material. Although much effort has been made, mechanisms for the above problems are poorly understood. Studying the cycling and float-charging characteristics of Li/NCM811 cells in high voltage conditions(4.5 V and 4.7 V, respectively), in this work we find that nearly all known problems with NCM811 material can be attributed to the oxidation of lattice oxygen occurring in the capacity region corresponding to H2 → H3 phase transition. While contributing to overall capacity,the oxidation of lattice oxygen results in a loss of oxygen through oxygen evolution and relative reactions between active oxygen evolution intermediates and electrolyte solvents. It is the loss of oxygen that results in irreversible layered-spinel-rocksalt phase transition, secondary particle cracking, and performance degradation. The conclusions of this work suggest that the priority for further research on NCM811 material should give to the suppression of oxygen evolution, followed by the use of the anti-oxygen electrolyte being chemically stable against the active oxygen evolution intermediates.
基金support from the U.S.Department of the Army and U.S.Army Future Commandsupport from the U.S.Army Research Laboratory Senior Research Fellowship Program。
文摘The oxygen evolution reaction(OER)is the essential module in energy conversion and storage devices such as electrolyzer,rechargeable metal–air batteries and regenerative fuel cells.The adsorption energy scaling relations between the reaction intermediates,however,impose a large intrinsic overpotential and sluggish reaction kinetics on OER catalysts.Developing advanced electrocatalysts with high activity and stability based on non-noble metal materials is still a grand challenge.Central to the rational design of novel and high-efficiency catalysts is the development and understanding of quantitative structure–activity relationships,which correlate the catalytic activities with structural and electronic descriptors.This paper comprehensively reviews the benchmark descriptors for OER electrolysis,aiming to give an in-depth understanding on the origins of the electrocatalytic activity of the OER and further contribute to building the theory of electrocatalysis.Meanwhile,the cutting-edge research frontiers for proposing new OER paradigms and crucial strategies to circumvent the scaling relationship are also summarized.Challenges,opportunities and perspectives are discussed,intending to shed some light on the rational design concepts and advance the development of more efficient catalysts for enhancing OER performance.
基金supported by the Deanship of Scientific Research at King Fahd University of Petroleum & Minerals Project(No.JF141002)the National Science Foundation(No.ECCS-1405173)+3 种基金the Office of Naval Research(Nos.N000141310562,N000141410718)the U.S. Army Research Office(No.W911NF-11-D-0001)the National Natural Science Foundation of China(No.61120106011)the Project 111 from the Ministry of Education of China(No.B08015)
文摘This paper introduces a model-free reinforcement learning technique that is used to solve a class of dynamic games known as dynamic graphical games. The graphical game results from to make all the agents synchronize to the state of a command multi-agent dynamical systems, where pinning control is used generator or a leader agent. Novel coupled Bellman equations and Hamiltonian functions are developed for the dynamic graphical games. The Hamiltonian mechanics are used to derive the necessary conditions for optimality. The solution for the dynamic graphical game is given in terms of the solution to a set of coupled Hamilton-Jacobi-Bellman equations developed herein. Nash equilibrium solution for the graphical game is given in terms of the solution to the underlying coupled Hamilton-Jacobi-Bellman equations. An online model-free policy iteration algorithm is developed to learn the Nash solution for the dynamic graphical game. This algorithm does not require any knowledge of the agents＇ dynamics. A proof of convergence for this multi-agent learning algorithm is given under mild assumption about the inter-connectivity properties of the graph. A gradient descent technique with critic network structures is used to implement the policy iteration algorithm to solve the graphical game online in real-time.
文摘Traumatic injury is one of the leading causes of death, with uncontrolled hemorrhage from coagulation dysfunction as one of the main potentially preventable causes of the mortality. Hypothermia, acidosis, and resuscitative hemodilution have been considered as the significant contributors to coagulation manifestations following trauma, known as the lethal triad. Over the past decade, clinical observations showed that coagulopathy may be present as early as hospital admission in some severely injured trauma patients. The hemostatic dysfunction is associated with higher blood transfusion requirements, longer hospital stay, and higher mortality. The recognition of this early coagulopathy has initiated tremendous interest and effort in the trauma community to expand our understanding of the underlying pathophysiology and improve clinical treatments. This review discusses the current knowledge of coagulation complications following trauma.
基金Supported by Grant from the National Institutes of Health (Tchou-Wong), No. ES-000260 and No. AI-059476
文摘AIM： To investigate the therapeutic potential of an RNA ligand （aptamer） specific for the catalytic ricin A-chain （RTA）, the protective effects of a 31-nucleo- tide RNA aptamer （31RA）, which formed a high affinity complex with RTA, against ricin-induced toxicity in cell- based luciferase translation and cell cytotoxicity assays were evaluated. METHODS： To test the therapeutic potential of anti- RTA aptamers in Chinese hamster ovary （CliO） AA8 cells stably transfected with a tetracycline regulatable promoter, ricin ribotoxicity was measured us- ing luciferase and ricin-induced cytotoxicity was ascertained by MTS cell proliferation assay with tet- razolium compound [3-（4,5-dimethylthiazol-2-yl）- 5-（3-carboxymethoxyphenyl）-2-（4-sulfophenyl）-2H- tetrazolium]. RESULTS： Inhibition of protein synthesis by ricin in CliO AA8 cells resulted in diminished luciferase activity and treatment with polyclonal antibody against degly- cosylated RTA （dgA） neutralized the inhibitory effects of ricin on luciferase activity and protected against ricin-induced cytotoxicity as measured by MTS assay. The 31RA anti-RTA aptamer inhibited the translation of luciferase mRNA in cell-free reticulocyte translation assay. 31RA aptamer also partially neutralized the inhibitory effects of ricin on luciferase activity and partially protected against ricin-induced cytotoxicity in CliO AA8 cells. CONCLUSION： We have shown that anti-RTA RNA aptamer can protect against ricin ribotoxicity in cell- based luciferase and cell cytotoxicity assays. Hence, RNA aptamer that inhibits RTA enzymatic activity represents a novel class of nucleic acid inhibitor that has the potential to be developed as a therapeutic agent for the treatment of ricin intoxication.
基金supported by the National Natural Science Foundation of China(21972049)the Guangdong Program for Distinguished Young Scholar(2017B030306013)the Science and Technology Planning Project of Guangdong Province(2017B090901020)。
文摘A once overlooked source of electrolyte degradation incurred by dissolved manganese(Ⅱ)species in lithium-ion batteries has been identified recently.In order to deactivate the catalytic activity of such manganese(II)ion,1-aza-12-crown-4-ether(A12C4)with cavity size well matched manganese(Ⅱ)ion is used in this work as electrolyte additive.Theoretical and experimental results show that stable complex forms between A12C4 and manganese(II)ions in the electrolyte,which does not affect the solvation of Li ions.The strong binding effect of A12C4 additive reduces the charge density of manganese(II)ion and inhibits its destruction of the PF_(6)^(-)structure in the electrolyte,leading to greatly improved thermal stability of manganese(II)ions-containing electrolyte.In addition to bulk electrolyte,A12C4 additive also shows capability in preventing Mn^(2+) from degrading SEI on graphite surface.Such bulk and interphasial stability introduced by A12C4 leads to significantly improved cycling performance of LIBs.
基金Supported by the Soil Characterization Laboratory,University of Masachusetts,Amherst,MA,USA
文摘In this study, phosphorus(P) sorption of thirteen light-weight aggregates(LWAs) from USA was compared during batch equilibrium experiments in order to identify those materials which had the highest P sorption capacity for further study. Seven different levels of sorption activity were observed, which were broadly grouped into three categories—high performing, middle performing, and low performing aggregates. Chemical analysis of Ca, Al, Fe, and Mg was used to describe the differences between LWAs. There was a significant correlation between cation(especially Al, Ca, Fe, and Mg) content and P sorbed. Langmuir isotherms were used to describe P sorption maximum and binding affinity for four of the top five performing LWAs, Universal, Stalite "D", Stalite "Mix", and TXI.The fifth aggregate, Lehigh, exhibited more complex sorption, and was better described by the Freundlich isotherm. Universal had a mean P sorption at the highest concentration of 824 mg kg-1, well above its calculated sorption maximum(702 mg kg-1), and also had the highest binding affinity(1.1 L mg-1). This experiment suggests that the top performing LWA(Universal) may perform poorly in column and field studies due to observed precipitates, which could degrade constructed wetland performance. Other LWAs may exhibit superior field performance due to their high calculated sorption maxima. In general, these results highlight the importance of batch experiments as a first step in identifying materials suitable for column and field experiments.
文摘Fast charging of Li-ion cells faces two aspects of challenges,1)accelerated capacity fade and 2)inferior charging capability.It is commonly believed that the former is due to Li plating and its resultant reactions with electrolyte at the graphite anode,which results in a loss in the inventory of Li+ions and an increase in the cell’s impedance.While the latter is ascribed to the high voltage polarization in relation to the slow transport of Li+ions between two electrodes.However,there are many other hidden facts that essentially affect the fast charging performances of Li-ion cells.This commentary intends,from the view of materials,to uncover these hidden factors,including failure of the solid electrolyte interphase and exfoliation of the graphite structure at the anode,structural degradation of the Ni-rich layered cathode materials,as well as the high solvation and desolvation activation energies of Li+ions in the electrolyte.Meanwhile,some solutions to the fast-charging problems of Li-ion cells are proposed based on the understanding of these hidden factors.
基金supported by Hydro Research Foundation (Grant No. DE-EE0002668)
文摘Hydroelectric facilities impact water temperature; low velocities in a reservoir increase residence time and enhance heat exchange in surface layers. In this study, an unsteady three-dimensional model was developed to predict the temperatm＇e dynamics in the McNary Dam forebay. The model is based on the open-source code OpenFOAM. RANS equations with the Boussinesq approximation were used to solve the flow field. A： realizable k-ε model that accounts for the production of wind turbulence was developed. Solar radiation and convective heat transfer at the free surface were included. The result of the model was compared with the field data collected on August 18, 2004. Changes in diurnal stratification were adequately predicted by the model. Observed vertical and lateral temperature distributions were accurately captured. Results indicate that the model can be used as a numerical tool to assess structural and operational alternatives to reduce the forebay temperature.
基金supported by the National Natural Science Foundation of China(21972049)the Guangdong Program for Distinguished Young Scholar(2017B030306013)the Science and Technology Planning Project of Guangdong Province(2017B090901020)。
文摘The non-flammability and high oxidation stability of sulfolane(SL)make it an excellent electrolyte candidate for lithium-ion batteries(LIBs).However,its incompatibility with graphitic anode prevents the realization of these advantages.To understand how this incompatibility arises on molecular level so that it can be suppressed,we combined theoretical calculation and experimental characterization and reveal that the primary Li^(+) solvation sheath in SL is depleted of fluorine source.Upon reduction,SL in such fluorine-poor solvation sheath generates insoluble dimer with poor electronic insulation,hence leading to slow but sustained parasitic reactions.When fluorine content in Li^(+)-SL solvation sheath is increased via salt concentration,a high stability LiF-rich interphase on graphite can be formed.This new understanding of the failure mechanism of graphite in SL-based electrolyte is of great significance in unlocking many possible electrolyte solvent candidates for the high-voltage cathode materials for next-generation LIBs.
基金the U.S.Department of the ArmyU.S.Army Materiel Command for supporting this work
文摘Ru@RuO2 core-shell nanorods were successfully synthesized by heat-treating Ru nanorods with air oxidation through an accurate control of the temperature and time. The structure, composition, dimension, and adsorption property of the core-shell nanorods were well characterized with XRD and TEM. The catalytic activity and stability were electrochemically evaluated with a rotating disk electrode, a rotating ring-disk electrode, and chronopotentiometric methods. The Ru@RuO2 nanorods reveal excellent bifunctional catalytic activity and robust stability for both oxygen evolution reaction(OER) and hydrogen evolution reaction(HER). The overpotentials for OER and HER are 320 m V and 137 m V at the current density of10 m A cm-2, respectively. The catalytic activity of Ru@RuO2 nanorods for OER is 6.5 times higher than that of the state-of-the-art catalyst IrO2 according to the catalytic current density measured at 1.60 V(versus RHE).The catalytic activity of Ru@RuO2 nanorods for HER is comparable to 40%Pt/C by comparing the catalytic current densities at à0.2 V.
基金supported by the National Natural Science Foundation of China(Grant No.21872058)the Key Project of Science and Technology in Guangdong Province(2017A010106006)
文摘Lithium-rich oxide is one of the most promising cathodes that meet high energy density requirement for batteries of the future, but its phase transformation from layer to spinel structure caused by the lattice instability presents severe challenge to cycling stability and the actually accessible capacity. The currently available approaches to suppress this undesired irreversible process often resort to limit the high voltages that lithium-rich oxide is exposed to. However, cycling stability thus improved is at the expense of the eventual energy output. In this work, we identified a new mechanism that is directly responsible for the lithium-rich oxide phase transformation and established a clear correlation between the successive consumption of Li+on anode due to incessant interphase repairing and the over-delithiation of lithium-rich oxide cathode. This new mechanism enables a simple but effective solution to the cathode degradation, in which an electrolyte additive is used to build a dense and protective interphase on anode with the intention to minimize Li depletion at cathode. The application of this new interphase effectively suppresses both electrolyte decomposition at anode and the phase transformation of lithium-rich oxide cathode, leading to high capacity and cycling stability.
基金supported by the Joint Center for Energy Storage Research(JCESR),a U.S.Department of Energy,Energy Innovation Hub。
文摘Using ab initio molecular dynamics(AIMD)simulations,classical molecular dynamics(CMD)simulations,small-angle X-ray scattering(SAXS),and pulsed-field gradient nuclear magnetic resonance(PFG-NMR),the solvation structure and ion dynamics of magnesium bis(trifluoromethanesulfonyl)imide(Mg(TFSI)_(2))aqueous electrolyte at 1,2,and 3 m concentrations are investigated.From AIMD and CMD simulations,the first solvation shell of an Mg;ion is found to be composed of six water molecules in an octahedral configuration and the solvation shell is rather rigid.The TFSI^(-)ions prefer to stay in the second solvation shell and beyond.Meanwhile,the comparable diffusion coefficients of positive and negative ions in Mg(TFSI)_(2)aqueous electrolytes have been observed,which is mainly due to the formation of the stable[Mg(H_(2)O_(6))_(2)]^(+)complex,and,as a result,the increased effective Mg ion size.Finally,the calculated correlated transference numbers are lower than the uncorrelated ones even at the low concentration of 2 and 3 m,suggesting the enhanced correlations between ions in the multivalent electrolytes.This work provides a molecular-level understanding of how the solvation structure and multivalency of the ion affect the dynamics and transport properties of the multivalent electrolyte,providing insight for rational designs of electrolytes for improved ion transport properties.
文摘We analyze the propagation of electromagnetic fronts in unbounded electric conductors. Our analysis is based on the Maxwell model of electromagnetism that includes the displacement current and Ohm’s law in its simplest forms. A weak electromagnetic front is a propagating interface at which the electromagnetic field remains continuous while its first- and higher-order derivatives experience finite jump discontinuities. Remarkably, analysis of such fronts can be performed autonomously, <em>i</em>.<em>e</em>. strictly in terms of the quantities defined on the front. This property opens the possibility of establishing exact analytical solutions of the exact Maxwell system along with the evolution of the front.
文摘Simple and double layers first appeared in electrostatics and later found various applications in mathematical physics. In this paper, we present the jump discontinuity conditions for their second-order spatial derivatives.
文摘In-bore yaw of a projectile in a gun tube has been shown to result in range loss if the yaw is significant. An attempt was made to determine if relationships between in-bore yaw and projectile First Maximum Yaw(FMY) were observable. Experiments were conducted in which pressure transducers were mounted near the muzzle of a 155 mm cannon in three sets of four. Each set formed a cruciform pattern to obtain a differential pressure across the projectile. These data were then integrated to form a picture of what the overall pressure distribution was along the side of the projectile. The pressure distribution was used to determine a magnitude and direction of the overturning moment acting on the projectile. This moment and its resulting angular acceleration were then compared to the actual first maximum yaw observed in the test. The degree of correlation was examined using various statistical techniques. Overall uncertainty in the projectile dynamics was between 20% and 40% of the mean values of FMY.
文摘Convection and its ensuing severe weather, such as heavy rainfall, hail, tornado, and high wind, have significant im- pacts on our society and economy （e.g., Cao et al., 2004; Fritsch and Carbone, 2004; Verbout et al., 2006; Ashley and Black, 2008; Cao, 2008; Cao and Ma, 2009; Zhang et al., 2014）. Due to its localized and transient nature, the initiation of convection or convective initiation remains one of the least understood aspects of convection in the scientific communi- ties, and it is a significant challenge to accurately predict the exact timing and location of convective initiation （e.g., Cai et al., 2006; Wilson and Roberts, 2006; Xue and Martin, 2006; Cao and Zhang, 2016）.
