An intense laser pulse focused onto a plasma can excite nonlinear plasma waves.Under appropriate conditions,electrons from the background plasma are trapped in the plasma wave and accelerated to ultra-relativistic vel...An intense laser pulse focused onto a plasma can excite nonlinear plasma waves.Under appropriate conditions,electrons from the background plasma are trapped in the plasma wave and accelerated to ultra-relativistic velocities.This scheme is called a laser wakefield accelerator.In this work,we present results from a laser wakefield acceleration experiment using a petawatt-class laser to excite the wakefields as well as nanoparticles to assist the injection of electrons into the accelerating phase of the wakefields.We find that a 10-cm-long,nanoparticle-assisted laser wakefield accelerator can generate 340 pC,10±1.86 GeV electron bunches with a 3.4 GeV rms convolved energy spread and a 0.9 mrad rms divergence.It can also produce bunches with lower energies in the 4–6 GeV range.展开更多
Solar Wind Charge eXchange X-ray(SWCX) emission in the heliosphere and Ea rth’s exosphere is a hard to avoid signal in soft Xray obse rvations of astrophysical targets.On the other hand,the X-ray imaging possibilitie...Solar Wind Charge eXchange X-ray(SWCX) emission in the heliosphere and Ea rth’s exosphere is a hard to avoid signal in soft Xray obse rvations of astrophysical targets.On the other hand,the X-ray imaging possibilities offered by the SWCX process has led to an increasing number of future dedicated space missions for investigating the solar wind-terrestrial inte ractions and magnetospheric interfaces.In both cases,accurate modelling of the SWCX emission is key to correctly interpret its signal,and remove it from obse rvations,when needed.In this paper,we compile solar wind abundance measurements from ACE for different solar wind types,and atomic data from literature,including charge exchange cross-sections and emission probabilities,used fo r calculating the compound cross-section a for the SWCX X-ray emission.We calculate a values for charge-exchange with H and He,relevant to soft X-ray energy bands(0.1-2.0 keV)for various solar wind types and solar cycle conditions.展开更多
In this paper,an NMOS output-capacitorless low-dropout regulator(OCL-LDO)featuring dual-loop regulation has been proposed,achieving fast transient response with low power consumption.An event-driven charge pump(CP)loo...In this paper,an NMOS output-capacitorless low-dropout regulator(OCL-LDO)featuring dual-loop regulation has been proposed,achieving fast transient response with low power consumption.An event-driven charge pump(CP)loop with the dynamic strength control(DSC),is proposed in this paper,which overcomes trade-offs inherent in conventional structures.The presented design addresses and resolves the large signal stability issue,which has been previously overlooked in the event-driven charge pump structure.This breakthrough allows for the full exploitation of the charge-pump structure's poten-tial,particularly in enhancing transient recovery.Moreover,a dynamic error amplifier is utilized to attain precise regulation of the steady-state output voltage,leading to favorable static characteristics.A prototype chip has been fabricated in 65 nm CMOS technology.The measurement results show that the proposed OCL-LDO achieves a 410 nA low quiescent current(IQ)and can recover within 30 ns under 200 mA/10 ns loading change.展开更多
Solar wind charge exchange(SWCX)is the process of solar wind high-valence ions exchanging charges with neutral components and generating soft X-rays.Recently,detecting the SWCX emission from the magnetosphere is propo...Solar wind charge exchange(SWCX)is the process of solar wind high-valence ions exchanging charges with neutral components and generating soft X-rays.Recently,detecting the SWCX emission from the magnetosphere is proposed as a new technique to study the magnetosphere using panoramic soft X-ray imaging.To better prepare for the data analysis of upcoming magnetospheric soft X-ray imaging missions,this paper compares the magnetospheric SWCX emission obtained by two methods in an XMM-Newton observation,during which the solar wind changed dramatically.The two methods differ in the data used to fit the diffuse X-ray background(DXB)parameters in spectral analysis.The method adding data from the ROSAT All-Sky Survey(RASS)is called the RASS method.The method using the quiet observation data is called the Quiet method,where quiet observations usually refer to observations made by the same satellite with the same target but under weaker solar wind conditions.Results show that the spectral compositions of magnetospheric SWCX emission obtained by the two methods are very similar,and the changes in intensity over time are highly consistent,although the intensity obtained by the RASS method is about 2.68±0.56 keV cm^(-2)s^(-1)sr^(-1)higher than that obtained by the Quiet method.Since the DXB intensity obtained by the RASS method is about 2.84±0.74 keV cm^(-2)s^(-1)sr^(-1)lower than that obtained by the Quiet method,and the linear correlation coefficient between the difference of SWCX and DXB obtained by the two methods in diffe rent energy band is close to-1,the diffe rences in magnetospheric SWCX can be fully attributed to the diffe rences in the fitted DXB.The difference between the two methods is most significant when the energy is less than 0.7 keV,which is also the main energy band of SWCX emission.In addition,the difference between the two methods is not related to the SWCX intensity and,to some extent,to solar wind conditions,because SWCX intensity typically va ries with the solar wind.In summary,both methods are robust and reliable,and should be considered based on the best available options.展开更多
A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in th...A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in the breech chamber,and the other is arranged in the barrel.The breech chamber charge was ignited first,and the charges in the auxiliary chambers were ignited by the high-temperature,highpressure combustible gas trailing the projectile.In this way,the combustible gas in the auxiliary chambers could compensate for the pressure drop caused by the movement of the projectile.The proposed device features the advantage of launching a projectile with high muzzle velocity without exceeding the maximum pressure in the chamber.In order to obtain some internal ballistic characteristics of the launch system,some critical structure,such as the length of the filter cartridge auxiliary charge,the combustion degree of the propellant in the chamber,and the length of the barrel,are discussed.The experimental results show that with the increased auxiliary charge length,a pressure plateau or even a secondary peak pressure can be formed,which is less than the peak pressure.The projectile velocity increased by 23.57%,14.64%,and 7.65%when the diaphragm thickness was 0 mm,1 mm,and2 mm,respectively.The muzzle velocity of the projectile can be increased by 13.42%by increasing the length of the barrel.Under the same charge condition,with the increase of barrel length,the energy utilization rate of propellant increases by 28.64%.展开更多
This paper proposes a type of double-layer charge liner fabricated using chemical vapor deposition(CVD)that has tungsten as its inner liner.The feasibility of this design was evaluated through penetration tests.Double...This paper proposes a type of double-layer charge liner fabricated using chemical vapor deposition(CVD)that has tungsten as its inner liner.The feasibility of this design was evaluated through penetration tests.Double-layer charge liners were fabricated by using CVD to deposit tungsten layers on the inner surfaces of pure T2 copper liners.The microstructures of the tungsten layers were analyzed using a scanning electron microscope(SEM).The feasibility analysis was carried out by pulsed X-rays,slug-retrieval test and static penetration tests.The shaped charge jet forming and penetration law of inner tungsten-coated double-layer liner were studied by numerical simulation method.The results showed that the double-layer liners could form well-shaped jets.The errors between the X-ray test results and the numerical results were within 11.07%.A slug-retrieval test was found that the retrieved slug was similar to a numerically simulated slug.Compared with the traditional pure copper shaped charge jet,the penetration depth of the double-layer shaped charge liner increased by 11.4% and>10.8% respectively.In summary,the test results are good,and the numerical simulation is in good agreement with the test,which verified the feasibility of using the CVD method to fabricate double-layer charge liners with a high-density and high-strength refractory metal as the inner liner.展开更多
The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first ti...The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.展开更多
pH-responsive charge reversal loaded miRNA nanocomposite was prepared by electrostatic self-assembly.The morphology,particle size and zeta potential of the nanocomposites were analyzed by transmission electron microsc...pH-responsive charge reversal loaded miRNA nanocomposite was prepared by electrostatic self-assembly.The morphology,particle size and zeta potential of the nanocomposites were analyzed by transmission electron microscopy and dynamic light scattering.The synthesis of the polymer was analyzed by^(1)H-NMR.The zeta-potential changes and cellular uptake effects of the nanocomplexes under different pH environments were investigated.The experimental results show that the surface morphology of the nanocomposite is spherical,and the average particle size is about 135 nm.As the pH value of the solution gradually decreases,the surface charge of the nanocomposite reverses from negative charge to positive charge(from-9.4 to+17.1 mV).Cellular uptake mediated by pH-responsive nanocomposite is selective for tumor cells,and the cellular uptake effect in tumor cells at pH 6.5 was approximately 3 times higher than that at pH 7.4.This pH responsive charge reversal nanocomposite has promising application prospects for gene delivery in the weak acid environment of tumors.展开更多
Reactive armour is a very efficient add-on armour against shaped charge threats.Explosive reactive armour consists of one or several plates that are accelerated by an explosive.Similar but less violent acceleration of...Reactive armour is a very efficient add-on armour against shaped charge threats.Explosive reactive armour consists of one or several plates that are accelerated by an explosive.Similar but less violent acceleration of plates can also be achieved in a completely inert reactive armour.To be efficient against elongated jets,the motion of the plates needs to be inclined against the jet such that a sliding contact between the jet and the plates is established.This sliding contact causes a deflection and thinning of the jet.Under certain circumstances,the contact will become unstable,leading to severe disturbances on the jet.These disturbances will drastically reduce the jet penetration performance and it is therefore of interest to study the conditions that leads to an unstable contact.Previous studies on the interaction between shaped charge jets and flyer plates have shown that it is mainly the forward moving plate in an explosive reactive armour that is effective in disturbing the jet.This is usually attributed to the higher plate-to-jet mass flux ratio involved in the collision of the forward moving plate compared to the backward moving plate.For slow moving plates,as occurs in inert reactive armour,the difference in mass flux for the forward and backward moving plate is much lesser,and it is therefore of interest to study if other factors than the mass flux influences on the protection capability.In this work,experiments have been performed where a plate is accelerated along its length,interacting with a shaped charge jet that is fired at an oblique angle to the plate’s normal,either against or along the plate’s velocity.The arrangement corresponds to a jet interacting with a flyer plate from a reactive armour,with the exception that the collision velocity is the same for both types of obliquities in these experiments.The experiments show that disturbances on the jet are different in the two cases even though the collision velocities are the same.Numerical simulations of the interaction support the observation.The difference is attributed to the character of the contact pressure in the interaction region.For a backward moving plate,the maximum contact pressure is obtained at the beginning of the interaction zone and the contact pressure is therefore higher upstream than downstream of the jet while the opposite is true for a forward moving plate.A negative interface pressure gradient with respect to the jet motion results in a more stable flow than a positive,which means that the jet-plate contact is more stable for a backward moving plate than for a forward moving plate.A forward moving plate is thus more effective in disturbing the jet than a backward moving plate,not only because of the higher jet to plate mass flux ratio but also because of the character of the contact with the jet.展开更多
Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in superca...Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.展开更多
To study the effects of the initiation position on the damage and fracture characteristics of linear-charge blasting, blasting model experiments were conducted in this study using computed tomography scanning and thre...To study the effects of the initiation position on the damage and fracture characteristics of linear-charge blasting, blasting model experiments were conducted in this study using computed tomography scanning and three-dimensional reconstruction methods. The fractal damage theory was used to quantify the crack distribution and damage degree of sandstone specimens after blasting. The results showed that regardless of an inverse or top initiation, due to compression deformation and sliding frictional resistance, the plugging medium of the borehole is effective. The energy of the explosive gas near the top of the borehole is consumed. This affects the effective crushing of rocks near the top of the borehole, where the extent of damage to Sections Ⅰ and Ⅱ is less than that of Sections Ⅲ and Ⅳ. In addition, the analysis revealed that under conditions of top initiation, the reflected tensile damage of the rock at the free face of the top of the borehole and the compression deformation of the plug and friction consume more blasting energy, resulting in lower blasting energy efficiency for top initiation. As a result, the overall damage degree of the specimens in the top-initiation group was significantly smaller than that in the inverse-initiation group. Under conditions of inverse initiation, the blasting energy efficiency is greater, causing the specimen to experience greater damage. Therefore, in the engineering practice of rock tunnel cut blasting, to utilize blasting energy effectively and enhance the effects of rock fragmentation, using the inverse-initiation method is recommended. In addition, in three-dimensional(3D) rock blasting, the bottom of the borehole has obvious end effects under the conditions of inverse initiation, and the crack distribution at the bottom of the borehole is trumpet-shaped. The occurrence of an end effect in the 3D linear-charge blasting model experiment is related to the initiation position and the blocking condition.展开更多
Ultrafast charge exchange recombination spectroscopy(UF-CXRS)has been developed on the EAST tokamak(Yingying Li et al 2019 Fusion Eng.Des.146522)to measure fast evolutions of ion temperature and toroidal velocity.Here...Ultrafast charge exchange recombination spectroscopy(UF-CXRS)has been developed on the EAST tokamak(Yingying Li et al 2019 Fusion Eng.Des.146522)to measure fast evolutions of ion temperature and toroidal velocity.Here,we report the preliminary diagnostic measurements after relative sensitivity calibration.The measurement results show a much higher temporal resolution compared with conventional CXRS,benefiting from the usage of a prismcoupled,high-dispersion volume-phase holographic transmission grating and a high quantum efficiency,high-gain detector array.Utilizing the UF-CXRS diagnostic,the fast evolutions of the ion temperature and rotation velocity during a set of high-frequency small-amplitude edgelocalized modes(ELMs)are obtained on the EAST tokamak,which are then compared with the case of large-amplitude ELMs.展开更多
Launch safety of explosive charges has become an urgent problem to be solved by all countries in the world aslaunch situation of ammunition becomes consistentlyworse.However, the existing numericalmodels have differen...Launch safety of explosive charges has become an urgent problem to be solved by all countries in the world aslaunch situation of ammunition becomes consistentlyworse.However, the existing numericalmodels have differentdefects. This paper formulates an efficient computational model of the combustion of an explosive charge affectedby a bottom gap in the launch environment in the context of the material point method. The current temperatureis computed accurately from the heat balance equation, and different physical states of the explosive charges areconsidered through various equations of state. Microcracks in the explosive charges are described with respectto the viscoelastic statistical crackmechanics (Visco–SCRAM) model. Themethod for calculating the temperatureat the bottomof the explosive charge with respect to the bottomgap is described. Based on this combustionmodel,the temperature history of a Composition B (COMB) explosive charge in the presence of a bottom gap is obtainedduring the launch process of a 155-mm artillery. The simulation results show that the bottom gap thickness shouldbe no greater than 0.039 cm to ensure the safety of the COM B explosive charge in the launch environment. Thisconclusion is consistent with previous results and verifies the correctness of the proposed model. Ultimately, thispaper derives amathematical expression for themaximumtemperature of the COMB explosive chargewith respectto the bottomgap thickness (over the range of 0.00–0.039 cm), and establishes a quantitative evaluationmethod forthe launch safety of explosive charges.The research results provide some guidance for the assessment and detectionof explosive charge safety in complex launch environments.展开更多
The extended kernel ridge regression(EKRR)method with odd-even effects was adopted to improve the description of the nuclear charge radius using five commonly used nuclear models.These are:(i)the isospin-dependent A^(...The extended kernel ridge regression(EKRR)method with odd-even effects was adopted to improve the description of the nuclear charge radius using five commonly used nuclear models.These are:(i)the isospin-dependent A^(1∕3) formula,(ii)relativistic continuum Hartree-Bogoliubov(RCHB)theory,(iii)Hartree-Fock-Bogoliubov(HFB)model HFB25,(iv)the Weizsacker-Skyrme(WS)model WS*,and(v)HFB25*model.In the last two models,the charge radii were calculated using a five-parameter formula with the nuclear shell corrections and deformations obtained from the WS and HFB25 models,respectively.For each model,the resultant root-mean-square deviation for the 1014 nuclei with proton number Z≥8 can be significantly reduced to 0.009-0.013 fm after considering the modification with the EKRR method.The best among them was the RCHB model,with a root-mean-square deviation of 0.0092 fm.The extrapolation abilities of the KRR and EKRR methods for the neutron-rich region were examined,and it was found that after considering the odd-even effects,the extrapolation power was improved compared with that of the original KRR method.The strong odd-even staggering of nuclear charge radii of Ca and Cu isotopes and the abrupt kinks across the neutron N=126 and 82 shell closures were also calculated and could be reproduced quite well by calculations using the EKRR method.展开更多
Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy...Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.展开更多
Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charg...Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charges(SOCs)has significant implications for reinforcing the thermal safety design of the lithium-ion battery module.This study first investigates the thermal safety boundary(TSB)correspondence at the cells and modules level under the guidance of a newly proposed concept,safe electric quantity boundary(SEQB).A reasonable thermal runaway propagation(TRP)judgment indicator,peak heat transfer power(PHTP),is proposed to predict whether TRP occurs.Moreover,a validated 3D model is used to quantitatively clarify the TSB at different SOCs from the perspective of PHTP,TR trigger temperature,SOC,and the full cycle life.Besides,three different TRP transfer modes are discovered.The interconversion relationship of three different TRP modes is investigated from the perspective of PHTP.This paper explores the TSB of LIBs under different SOCs at both cell and module levels for the first time,which has great significance in guiding the thermal safety design of battery systems.展开更多
The initial shape of the secondary arc considerably influences its subsequent shape.To establish the model for the arcing time of the secondary arc and modify the single-phase reclosing sequence,theoretical and experi...The initial shape of the secondary arc considerably influences its subsequent shape.To establish the model for the arcing time of the secondary arc and modify the single-phase reclosing sequence,theoretical and experimental analysis of the evolution process of the short-circuit arc to the secondary arc is critical.In this study,an improved charge simulation method was used to develop the internal-space electric-field model of the short-circuit arc.The intensity of the electric field was used as an independent variable to describe the initial shape of the secondary arc.A secondary arc evolution model was developed based on this model.Moreover,the accuracy of the model was evaluated by comparison with physical experimental results.When the secondary arc current increased,the arcing time and dispersion increased.There is an overall trend of increasing arc length with increasing arcing time.Nevertheless,there is a reduction in arc length during arc ignition due to short circuits between the arc columns.Furthermore,the arcing time decreased in the range of 0°-90°as the angle between the wind direction and the x-axis increased.This work investigated the method by which short-circuit arcs evolve into secondary arcs.The results can be used to develop the secondary arc evolution model and to provide both a technical and theoretical basis for secondary arc suppression.展开更多
Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR)...Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.展开更多
Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipat...Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like structures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.展开更多
基金supported by the Air Force Office of Scientific Research Grant No.FA9550-17-1-0264supported by the DOE,Office of Science,Fusion Energy Sciences under Contract No.DE-SC0021125+2 种基金supported by the U.S.Department of Energy Grant No.DESC0011617.D.A.Jarozynski,E.Brunetti,B.Ersfeld,and S.Yoffe would like to acknowledge support from the U.K.EPSRC(Grant Nos.EP/J018171/1 and EP/N028694/1)the European Union’s Horizon 2020 research and innovation program under Grant Agreement No.871124 Laserlab-Europe and EuPRAXIA(Grant No.653782)funded by the N8 research partnership and EPSRC(Grant No.EP/T022167/1).
文摘An intense laser pulse focused onto a plasma can excite nonlinear plasma waves.Under appropriate conditions,electrons from the background plasma are trapped in the plasma wave and accelerated to ultra-relativistic velocities.This scheme is called a laser wakefield accelerator.In this work,we present results from a laser wakefield acceleration experiment using a petawatt-class laser to excite the wakefields as well as nanoparticles to assist the injection of electrons into the accelerating phase of the wakefields.We find that a 10-cm-long,nanoparticle-assisted laser wakefield accelerator can generate 340 pC,10±1.86 GeV electron bunches with a 3.4 GeV rms convolved energy spread and a 0.9 mrad rms divergence.It can also produce bunches with lower energies in the 4–6 GeV range.
文摘Solar Wind Charge eXchange X-ray(SWCX) emission in the heliosphere and Ea rth’s exosphere is a hard to avoid signal in soft Xray obse rvations of astrophysical targets.On the other hand,the X-ray imaging possibilities offered by the SWCX process has led to an increasing number of future dedicated space missions for investigating the solar wind-terrestrial inte ractions and magnetospheric interfaces.In both cases,accurate modelling of the SWCX emission is key to correctly interpret its signal,and remove it from obse rvations,when needed.In this paper,we compile solar wind abundance measurements from ACE for different solar wind types,and atomic data from literature,including charge exchange cross-sections and emission probabilities,used fo r calculating the compound cross-section a for the SWCX X-ray emission.We calculate a values for charge-exchange with H and He,relevant to soft X-ray energy bands(0.1-2.0 keV)for various solar wind types and solar cycle conditions.
基金supported by the National Natural Science Foundation of China under Grant 62274189the Natural Science Foundation of Guangdong Province,China,under Grant 2022A1515011054the Key Area R&D Program of Guangdong Province under Grant 2022B0701180001.
文摘In this paper,an NMOS output-capacitorless low-dropout regulator(OCL-LDO)featuring dual-loop regulation has been proposed,achieving fast transient response with low power consumption.An event-driven charge pump(CP)loop with the dynamic strength control(DSC),is proposed in this paper,which overcomes trade-offs inherent in conventional structures.The presented design addresses and resolves the large signal stability issue,which has been previously overlooked in the event-driven charge pump structure.This breakthrough allows for the full exploitation of the charge-pump structure's poten-tial,particularly in enhancing transient recovery.Moreover,a dynamic error amplifier is utilized to attain precise regulation of the steady-state output voltage,leading to favorable static characteristics.A prototype chip has been fabricated in 65 nm CMOS technology.The measurement results show that the proposed OCL-LDO achieves a 410 nA low quiescent current(IQ)and can recover within 30 ns under 200 mA/10 ns loading change.
基金supported by NNSFC grants 42322408,42188101 and 42074202the Strategic Pioneer Program on Space Science,CAS Grant nos.XDA15350201+3 种基金in part by the Research Fund from the Chinese Academy of Sciencesthe Specialized Research Fund for State Key Laboratories of China.supported by the Young Elite Scientists Sponsorship Program(CAST-Y202045)supported by Royal Society grant DHFR1211068。
文摘Solar wind charge exchange(SWCX)is the process of solar wind high-valence ions exchanging charges with neutral components and generating soft X-rays.Recently,detecting the SWCX emission from the magnetosphere is proposed as a new technique to study the magnetosphere using panoramic soft X-ray imaging.To better prepare for the data analysis of upcoming magnetospheric soft X-ray imaging missions,this paper compares the magnetospheric SWCX emission obtained by two methods in an XMM-Newton observation,during which the solar wind changed dramatically.The two methods differ in the data used to fit the diffuse X-ray background(DXB)parameters in spectral analysis.The method adding data from the ROSAT All-Sky Survey(RASS)is called the RASS method.The method using the quiet observation data is called the Quiet method,where quiet observations usually refer to observations made by the same satellite with the same target but under weaker solar wind conditions.Results show that the spectral compositions of magnetospheric SWCX emission obtained by the two methods are very similar,and the changes in intensity over time are highly consistent,although the intensity obtained by the RASS method is about 2.68±0.56 keV cm^(-2)s^(-1)sr^(-1)higher than that obtained by the Quiet method.Since the DXB intensity obtained by the RASS method is about 2.84±0.74 keV cm^(-2)s^(-1)sr^(-1)lower than that obtained by the Quiet method,and the linear correlation coefficient between the difference of SWCX and DXB obtained by the two methods in diffe rent energy band is close to-1,the diffe rences in magnetospheric SWCX can be fully attributed to the diffe rences in the fitted DXB.The difference between the two methods is most significant when the energy is less than 0.7 keV,which is also the main energy band of SWCX emission.In addition,the difference between the two methods is not related to the SWCX intensity and,to some extent,to solar wind conditions,because SWCX intensity typically va ries with the solar wind.In summary,both methods are robust and reliable,and should be considered based on the best available options.
基金financially supported by the National Natural Science Foundation of China under Project No.51874267 and No.12272374the Fundamental Research Funds for the Central Universities under Project Nos.WK2480000008,WK2480000007,and WK2320000049。
文摘A launching system with a filter cartridge structure was proposed to improve the muzzle velocity of the projectile.The combustion chamber of the launching system is divided into two fixed chambers,one is located in the breech chamber,and the other is arranged in the barrel.The breech chamber charge was ignited first,and the charges in the auxiliary chambers were ignited by the high-temperature,highpressure combustible gas trailing the projectile.In this way,the combustible gas in the auxiliary chambers could compensate for the pressure drop caused by the movement of the projectile.The proposed device features the advantage of launching a projectile with high muzzle velocity without exceeding the maximum pressure in the chamber.In order to obtain some internal ballistic characteristics of the launch system,some critical structure,such as the length of the filter cartridge auxiliary charge,the combustion degree of the propellant in the chamber,and the length of the barrel,are discussed.The experimental results show that with the increased auxiliary charge length,a pressure plateau or even a secondary peak pressure can be formed,which is less than the peak pressure.The projectile velocity increased by 23.57%,14.64%,and 7.65%when the diaphragm thickness was 0 mm,1 mm,and2 mm,respectively.The muzzle velocity of the projectile can be increased by 13.42%by increasing the length of the barrel.Under the same charge condition,with the increase of barrel length,the energy utilization rate of propellant increases by 28.64%.
基金funded by the China Postdoctoral Science Foundation(Grant No.2022M721614)the opening project of State Key Laboratory of Explosion Science and Technology,Beijing Institute of Technology(Grant No.KFJJ23-07M)。
文摘This paper proposes a type of double-layer charge liner fabricated using chemical vapor deposition(CVD)that has tungsten as its inner liner.The feasibility of this design was evaluated through penetration tests.Double-layer charge liners were fabricated by using CVD to deposit tungsten layers on the inner surfaces of pure T2 copper liners.The microstructures of the tungsten layers were analyzed using a scanning electron microscope(SEM).The feasibility analysis was carried out by pulsed X-rays,slug-retrieval test and static penetration tests.The shaped charge jet forming and penetration law of inner tungsten-coated double-layer liner were studied by numerical simulation method.The results showed that the double-layer liners could form well-shaped jets.The errors between the X-ray test results and the numerical results were within 11.07%.A slug-retrieval test was found that the retrieved slug was similar to a numerically simulated slug.Compared with the traditional pure copper shaped charge jet,the penetration depth of the double-layer shaped charge liner increased by 11.4% and>10.8% respectively.In summary,the test results are good,and the numerical simulation is in good agreement with the test,which verified the feasibility of using the CVD method to fabricate double-layer charge liners with a high-density and high-strength refractory metal as the inner liner.
基金Project supported by the National Key Research and Development Program of China(Grant No.2017YFA0402400)the National Natural Science Foundation of China(Grant Nos.11974358 and 11934004)+1 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB34020000)the Heavy Ion Research Facility in Lanzhou(HIRFL).
文摘The state-selective cross section data are useful for understanding and modeling the x-ray emission in celestial observations.In the present work,using the cold target recoil ion momentum spectroscopy,for the first time we investigated the state-selective single electron capture processes for S^(q+)–He and H_(2)(q=11–15)collision systems at an impact energy of q×20 keV and obtained the relative state-selective cross sections.The results indicate that only a few principal quantum states of the projectile energy level are populated in a single electron capture process.In particular,the increase of the projectile charge state leads to the population of the states with higher principal quantum numbers.It is also shown that the experimental averaged n-shell populations are reproduced well by the over-barrier model.The database is openly available in Science Data Bank at 10.57760/sciencedb.j00113.00091.
基金Funded by the National Key R&D Program of China(No.2023YFC2412300)the Natural Science Foundation of Hubei Province(No.2022CFB386)the National Natural Science Foundation of China(No.52073222)。
文摘pH-responsive charge reversal loaded miRNA nanocomposite was prepared by electrostatic self-assembly.The morphology,particle size and zeta potential of the nanocomposites were analyzed by transmission electron microscopy and dynamic light scattering.The synthesis of the polymer was analyzed by^(1)H-NMR.The zeta-potential changes and cellular uptake effects of the nanocomplexes under different pH environments were investigated.The experimental results show that the surface morphology of the nanocomposite is spherical,and the average particle size is about 135 nm.As the pH value of the solution gradually decreases,the surface charge of the nanocomposite reverses from negative charge to positive charge(from-9.4 to+17.1 mV).Cellular uptake mediated by pH-responsive nanocomposite is selective for tumor cells,and the cellular uptake effect in tumor cells at pH 6.5 was approximately 3 times higher than that at pH 7.4.This pH responsive charge reversal nanocomposite has promising application prospects for gene delivery in the weak acid environment of tumors.
基金funded by the Swedish Armed Forces under Contract No AT.9220620。
文摘Reactive armour is a very efficient add-on armour against shaped charge threats.Explosive reactive armour consists of one or several plates that are accelerated by an explosive.Similar but less violent acceleration of plates can also be achieved in a completely inert reactive armour.To be efficient against elongated jets,the motion of the plates needs to be inclined against the jet such that a sliding contact between the jet and the plates is established.This sliding contact causes a deflection and thinning of the jet.Under certain circumstances,the contact will become unstable,leading to severe disturbances on the jet.These disturbances will drastically reduce the jet penetration performance and it is therefore of interest to study the conditions that leads to an unstable contact.Previous studies on the interaction between shaped charge jets and flyer plates have shown that it is mainly the forward moving plate in an explosive reactive armour that is effective in disturbing the jet.This is usually attributed to the higher plate-to-jet mass flux ratio involved in the collision of the forward moving plate compared to the backward moving plate.For slow moving plates,as occurs in inert reactive armour,the difference in mass flux for the forward and backward moving plate is much lesser,and it is therefore of interest to study if other factors than the mass flux influences on the protection capability.In this work,experiments have been performed where a plate is accelerated along its length,interacting with a shaped charge jet that is fired at an oblique angle to the plate’s normal,either against or along the plate’s velocity.The arrangement corresponds to a jet interacting with a flyer plate from a reactive armour,with the exception that the collision velocity is the same for both types of obliquities in these experiments.The experiments show that disturbances on the jet are different in the two cases even though the collision velocities are the same.Numerical simulations of the interaction support the observation.The difference is attributed to the character of the contact pressure in the interaction region.For a backward moving plate,the maximum contact pressure is obtained at the beginning of the interaction zone and the contact pressure is therefore higher upstream than downstream of the jet while the opposite is true for a forward moving plate.A negative interface pressure gradient with respect to the jet motion results in a more stable flow than a positive,which means that the jet-plate contact is more stable for a backward moving plate than for a forward moving plate.A forward moving plate is thus more effective in disturbing the jet than a backward moving plate,not only because of the higher jet to plate mass flux ratio but also because of the character of the contact with the jet.
基金We are grateful to National Natural Science Foundation of China(Grant No.22375056,52272163)the Key R&D Program of Hebei(Grant No.216Z1201G)+1 种基金Natural Science Foundation of Hebei Province(Grant No.E2022208066,B2021208014)Key R&D Program of Hebei Technological Innovation Center of Chiral Medicine(Grant No.ZXJJ20220105).
文摘Free-standing covalent organic framework(COFs)nanofilms exhibit a remarkable ability to rapidly intercalate/de-intercalate Li^(+) in lithium-ion batteries,while simultaneously exposing affluent active sites in supercapacitors.The development of these nanofilms offers a promising solution to address the persistent challenge of imbalanced charge storage kinetics between battery-type anode and capacitor-type cathode in lithium-ion capacitors(LICs).Herein,for the first time,custom-made COFBTMB-TP and COFTAPB-BPY nanofilms are synthesized as the anode and cathode,respectively,for an all-COF nanofilm-structured LIC.The COFBTMB-TP nanofilm with strong electronegative–CF3 groups enables tuning the partial electron cloud density for Li^(+) migration to ensure the rapid anode kinetic process.The thickness-regulated cathodic COFTAPB-BPY nanofilm can fit the anodic COF nanofilm in the capacity.Due to the aligned 1D channel,2D aromatic skeleton and accessible active sites of COF nanofilms,the whole COFTAPB-BPY//COFBTMB-TP LIC demonstrates a high energy density of 318 mWh cm^(−3) at a high-power density of 6 W cm^(−3),excellent rate capability,good cycle stability with the capacity retention rate of 77%after 5000-cycle.The COFTAPB-BPY//COFBTMB-TP LIC represents a new benchmark for currently reported film-type LICs and even film-type supercapacitors.After being comprehensively explored via ex situ XPS,7Li solid-state NMR analyses,and DFT calculation,it is found that the COFBTMB-TP nanofilm facilitates the reversible conversion of semi-ionic to ionic C–F bonds during lithium storage.COFBTMB-TP exhibits a strong interaction with Li^(+) due to the C–F,C=O,and C–N bonds,facilitating Li^(+) desolation and absorption from the electrolyte.This work addresses the challenge of imbalanced charge storage kinetics and capacity between the anode and cathode and also pave the way for future miniaturized and wearable LIC devices.
基金supported by the National Natural Science Foundation of China (No.52204085)the Interdisciplinary Research Project for Young Teachers of USTB,Fundamental Research Funds for the Central Universities (No.FRF-IDRY-21-006).
文摘To study the effects of the initiation position on the damage and fracture characteristics of linear-charge blasting, blasting model experiments were conducted in this study using computed tomography scanning and three-dimensional reconstruction methods. The fractal damage theory was used to quantify the crack distribution and damage degree of sandstone specimens after blasting. The results showed that regardless of an inverse or top initiation, due to compression deformation and sliding frictional resistance, the plugging medium of the borehole is effective. The energy of the explosive gas near the top of the borehole is consumed. This affects the effective crushing of rocks near the top of the borehole, where the extent of damage to Sections Ⅰ and Ⅱ is less than that of Sections Ⅲ and Ⅳ. In addition, the analysis revealed that under conditions of top initiation, the reflected tensile damage of the rock at the free face of the top of the borehole and the compression deformation of the plug and friction consume more blasting energy, resulting in lower blasting energy efficiency for top initiation. As a result, the overall damage degree of the specimens in the top-initiation group was significantly smaller than that in the inverse-initiation group. Under conditions of inverse initiation, the blasting energy efficiency is greater, causing the specimen to experience greater damage. Therefore, in the engineering practice of rock tunnel cut blasting, to utilize blasting energy effectively and enhance the effects of rock fragmentation, using the inverse-initiation method is recommended. In addition, in three-dimensional(3D) rock blasting, the bottom of the borehole has obvious end effects under the conditions of inverse initiation, and the crack distribution at the bottom of the borehole is trumpet-shaped. The occurrence of an end effect in the 3D linear-charge blasting model experiment is related to the initiation position and the blocking condition.
基金supported by the National Magnetic Confinement Fusion Science Program of China (No. 2019YFE 03030004)National Natural Science Foundation of China (Nos. 11535013 and 11975232)
文摘Ultrafast charge exchange recombination spectroscopy(UF-CXRS)has been developed on the EAST tokamak(Yingying Li et al 2019 Fusion Eng.Des.146522)to measure fast evolutions of ion temperature and toroidal velocity.Here,we report the preliminary diagnostic measurements after relative sensitivity calibration.The measurement results show a much higher temporal resolution compared with conventional CXRS,benefiting from the usage of a prismcoupled,high-dispersion volume-phase holographic transmission grating and a high quantum efficiency,high-gain detector array.Utilizing the UF-CXRS diagnostic,the fast evolutions of the ion temperature and rotation velocity during a set of high-frequency small-amplitude edgelocalized modes(ELMs)are obtained on the EAST tokamak,which are then compared with the case of large-amplitude ELMs.
基金the Natural Science Foundation of Heilongjiang Province,China(LH2019A008).
文摘Launch safety of explosive charges has become an urgent problem to be solved by all countries in the world aslaunch situation of ammunition becomes consistentlyworse.However, the existing numericalmodels have differentdefects. This paper formulates an efficient computational model of the combustion of an explosive charge affectedby a bottom gap in the launch environment in the context of the material point method. The current temperatureis computed accurately from the heat balance equation, and different physical states of the explosive charges areconsidered through various equations of state. Microcracks in the explosive charges are described with respectto the viscoelastic statistical crackmechanics (Visco–SCRAM) model. Themethod for calculating the temperatureat the bottomof the explosive charge with respect to the bottomgap is described. Based on this combustionmodel,the temperature history of a Composition B (COMB) explosive charge in the presence of a bottom gap is obtainedduring the launch process of a 155-mm artillery. The simulation results show that the bottom gap thickness shouldbe no greater than 0.039 cm to ensure the safety of the COM B explosive charge in the launch environment. Thisconclusion is consistent with previous results and verifies the correctness of the proposed model. Ultimately, thispaper derives amathematical expression for themaximumtemperature of the COMB explosive chargewith respectto the bottomgap thickness (over the range of 0.00–0.039 cm), and establishes a quantitative evaluationmethod forthe launch safety of explosive charges.The research results provide some guidance for the assessment and detectionof explosive charge safety in complex launch environments.
基金This work was supported by the National Natural Science Foundation of China(Nos.11875027,11975096).
文摘The extended kernel ridge regression(EKRR)method with odd-even effects was adopted to improve the description of the nuclear charge radius using five commonly used nuclear models.These are:(i)the isospin-dependent A^(1∕3) formula,(ii)relativistic continuum Hartree-Bogoliubov(RCHB)theory,(iii)Hartree-Fock-Bogoliubov(HFB)model HFB25,(iv)the Weizsacker-Skyrme(WS)model WS*,and(v)HFB25*model.In the last two models,the charge radii were calculated using a five-parameter formula with the nuclear shell corrections and deformations obtained from the WS and HFB25 models,respectively.For each model,the resultant root-mean-square deviation for the 1014 nuclei with proton number Z≥8 can be significantly reduced to 0.009-0.013 fm after considering the modification with the EKRR method.The best among them was the RCHB model,with a root-mean-square deviation of 0.0092 fm.The extrapolation abilities of the KRR and EKRR methods for the neutron-rich region were examined,and it was found that after considering the odd-even effects,the extrapolation power was improved compared with that of the original KRR method.The strong odd-even staggering of nuclear charge radii of Ca and Cu isotopes and the abrupt kinks across the neutron N=126 and 82 shell closures were also calculated and could be reproduced quite well by calculations using the EKRR method.
基金funded by the National Key Research and Development Program of China(2018YFA0900702).
文摘Biocatalysis in organic solvents(OSs)has numerous important applications,but native enzymes in OSs often exhibit limited catalytic performance.Herein,we proposed a computation-aided surface charge engineering strategy to improve the catalytic performance of haloalkane dehalogenase DhaA in OSs based on the energetic analysis of substrate binding to the DhaA surface.Several variants with enhanced OS resistance were obtained by replacing negative charged residues on the surface with positive charged residue(Arg).Particularly,a four-substitution variant E16R/E93R/E121R/E257R exhibited the best catalytic performance(five-fold improvement in OS resistance and seven-fold half-life increase in 40%(vol)dimethylsulfoxide).As a result,the overall catalytic performance of the variant could be at least 26 times higher than the wild-type DhaA.Fluorescence spectroscopy and molecular dynamics simulation studies revealed that the residue substitution mainly enhanced OS resistance from four aspects:(a)improved the overall structural stability,(b)increased the hydrophobicity of the local microenvironment around the catalytic triad,(c)enriched the hydrophobic substrate around the enzyme molecule,and(d)lowered the contact frequency between OS molecules and the catalytic triad.Our findings validate that computationaided surface charge engineering is an effective and ingenious rational strategy for tailoring enzyme performance in OSs.
基金supported by the National Natural Science Foundation of China(No.U20A20310 and No.52176199)sponsored by the Program of Shanghai Academic/Technology Research Leader(No.22XD1423800)。
文摘Thermal runaway(TR)is a critical issue hindering the large-scale application of lithium-ion batteries(LIBs).Understanding the thermal safety behavior of LIBs at the cell and module level under different state of charges(SOCs)has significant implications for reinforcing the thermal safety design of the lithium-ion battery module.This study first investigates the thermal safety boundary(TSB)correspondence at the cells and modules level under the guidance of a newly proposed concept,safe electric quantity boundary(SEQB).A reasonable thermal runaway propagation(TRP)judgment indicator,peak heat transfer power(PHTP),is proposed to predict whether TRP occurs.Moreover,a validated 3D model is used to quantitatively clarify the TSB at different SOCs from the perspective of PHTP,TR trigger temperature,SOC,and the full cycle life.Besides,three different TRP transfer modes are discovered.The interconversion relationship of three different TRP modes is investigated from the perspective of PHTP.This paper explores the TSB of LIBs under different SOCs at both cell and module levels for the first time,which has great significance in guiding the thermal safety design of battery systems.
基金supported by National Natural Science Foundation of China(Nos.92066108 and 51277061)。
文摘The initial shape of the secondary arc considerably influences its subsequent shape.To establish the model for the arcing time of the secondary arc and modify the single-phase reclosing sequence,theoretical and experimental analysis of the evolution process of the short-circuit arc to the secondary arc is critical.In this study,an improved charge simulation method was used to develop the internal-space electric-field model of the short-circuit arc.The intensity of the electric field was used as an independent variable to describe the initial shape of the secondary arc.A secondary arc evolution model was developed based on this model.Moreover,the accuracy of the model was evaluated by comparison with physical experimental results.When the secondary arc current increased,the arcing time and dispersion increased.There is an overall trend of increasing arc length with increasing arcing time.Nevertheless,there is a reduction in arc length during arc ignition due to short circuits between the arc columns.Furthermore,the arcing time decreased in the range of 0°-90°as the angle between the wind direction and the x-axis increased.This work investigated the method by which short-circuit arcs evolve into secondary arcs.The results can be used to develop the secondary arc evolution model and to provide both a technical and theoretical basis for secondary arc suppression.
基金financially supported by the National Natural Science Foundation of China (52363028)the Natural Science Foundation of Guangxi Province (2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject (GUIKE AD23023004,GUIKE AD20297039)
文摘Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.
基金conducted by the Fundamental Research Center of Artificial Photosynthesis(FReCAP)financially supported by the National Natural Science Foundation of China(22172011 and 22088102)+1 种基金the National Key R&D Program of China(2022YFA0911904)the Fundamental Research Funds for the Central Universities(DUT22LK06,DUT22QN213 and DUT23LAB611)。
文摘Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like structures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.