Two-dimensional transition metal carbides(MXenes) have been demonstrated to be promising supports for single-atom catalysts(SACs) to enable efficient oxygen evolution reaction(OER).However,the rational design of MXene...Two-dimensional transition metal carbides(MXenes) have been demonstrated to be promising supports for single-atom catalysts(SACs) to enable efficient oxygen evolution reaction(OER).However,the rational design of MXene-based SACs depends on an experimental trial-and-error approach.A theoretical guidance principle is highly expected for the efficient evaluation of MXene-based SACs.Herein,highthroughput screening was performed through first-principles calculations and machine learning techniques.Ti_(3)C_(2)(OH)_(x),V_(3)C_(2)(OH)_(x),Zr_(3)C_(2)(OH)_(x),Nb_(3)C_(2)(OH)_(x),Hf_(3)C_(2)(OH)_(x),Ta_(3)C_(2)(OH)_(x),and W_(3)C_(2)(OH)_(x) were screened out based on their excellent stability.Zn,Pd,Ag,Cd,Au,and Hg were proposed to be promising single atoms anchored in MXenes based on cohesive energy analysis.Hf_(3)C_(2)(OH)_(x) with a Pd single atom delivers a theoretical overpotential of 81 mV.Both moderate electron-deficient state and high covalency of metal-carbon bonds were critical features for the high OER reactivity.This principle is expected to be a promising approach to the rational design of OER catalysts for metal-air batteries,fuel cells,and other OER-based energy storage devices.展开更多
In high-altitude nuclear detonations,the proportion of pulsed X-ray energy can exceed 70%,making it a specific monitoring signal for such events.These pulsed X-rays can be captured using a satellite-borne X-ray detect...In high-altitude nuclear detonations,the proportion of pulsed X-ray energy can exceed 70%,making it a specific monitoring signal for such events.These pulsed X-rays can be captured using a satellite-borne X-ray detector following atmospheric transmission.To quantitatively analyze the effects of different satellite detection altitudes,burst heights,and transmission angles on the physical processes of X-ray transport and energy fluence,we developed an atmospheric transmission algorithm for pulsed X-rays from high-altitude nuclear detonations based on scattering correction.The proposed method is an improvement over the traditional analytical method that only computes direct-transmission X-rays.The traditional analytical method exhibits a maximum relative error of 67.79% compared with the Monte Carlo method.Our improved method reduces this error to within 10% under the same conditions,even reaching 1% in certain scenarios.Moreover,its computation time is 48,000 times faster than that of the Monte Carlo method.These results have important theoretical significance and engineering application value for designing satellite-borne nuclear detonation pulsed X-ray detectors,inverting nuclear detonation source terms,and assessing ionospheric effects.展开更多
A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-spee...A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-speed camera technique and the flash X-ray radiography technique.Based on dynamic analysis,one-dimensional characteristics analysis and some numerical simulations on the propagating processes of blast waves before the container shell rupturing,further and detailed analyses of the experimental results are presented.The effects of the liquid viscosity on the dynamic dispersing flow are also analyzed,and the spall fracture mechanism is explored.Thus,the dominating forces determining the dispersing liquid flow are revealed,that is,the stretching and shearing action due to the interaction of two reflecting rarefaction waves in opposite propagating directions.The influence of container shell strength on the dispersing liquid flow is also investigated,and the characters of cavitation layered in liquid before shell rupturing are uncovered.Results revealed that different shell material results in different cavitating layers.Then the different cavitating layers drive the different dynamic liquid dispersing process coming into being.The metastable liquid states caused by pressure drop and cavitation generation are discussed.展开更多
Decontamination of 2-chloroethyl ethyl sulfide （2-CEES, CH_3CH_2SCH_2CH_2C1） by pulsed corona plasma was investigated. The results show that 212.6 mg/m^3 of 2-CEES, with the gas flow rate of 2 m^3/h, can be decontam...Decontamination of 2-chloroethyl ethyl sulfide （2-CEES, CH_3CH_2SCH_2CH_2C1） by pulsed corona plasma was investigated. The results show that 212.6 mg/m^3 of 2-CEES, with the gas flow rate of 2 m^3/h, can be decontaminated to 0.09 mg/m^3. According to the variation of the inlet and outlet concentration of 2-CEES vapor with retention time, it is found that the reaction of 2-CEES in a pulsed corona plasma system follows the first order reaction, with the reaction rate constant of 0.463 s^-1. The decontamination mechanism is discussed based on an analysis of the dissociation energy of chemical bonds and decontamination products. The C-S bond adjacent to the C1 atom will be destroyed firstly to form CH3CH2S. and .CH2CH2C1 radicals. CH3CH2S. can be decomposed to .C_2H_5 and .S..S can be oxidized to SO_2, while .C_2H_5 can be finally oxidized to CO_2 and H_2O. The C-Cl bond in the .CH_2CH_2C1 radical can be destroyed to form .CH_2CH_2. and .C1, which can be mineralized to CO_2, H_2O and HCl. The H atom in the .CH_2CH_2C1 radical can also be substituted by -C1 to form CHCl_2-CHCl_2.展开更多
Low-temperature plasma is a green and high-efficiency technology for chemical warfare agent(CWA)decontamination.However,traditional plasma devices suffer from the problems of highpower composition and large power-supp...Low-temperature plasma is a green and high-efficiency technology for chemical warfare agent(CWA)decontamination.However,traditional plasma devices suffer from the problems of highpower composition and large power-supply size,which limit their practical applications.In this paper,a self-driven microplasma decontamination system,induced by a dielectric-dielectric rotary triboelectric nanogenerator(dd-r TENG),was innovatively proposed for the decontamination of CWA simulants.The microplasma was characterized via electrical measurements,optical emission spectra and ozone concentration detection.With an output voltage of-3460 V,the dd-r TENG can successfully excite microplasma in air.Reactive species,such as OH,O(1D),Hαand O3were detected.With input average power of 0.116 W,the decontamination rate of 2-chloroethyl ethyl sulfide reached 100%within 3 min of plasma treatment,while the decontamination rates of malathion and dimethyl methylphosphonate reached(65.92±1.65)%and(60.88±1.92)%after 7 min of plasma treatment,respectively.In addition,the decontamination rates gradually decreased with the increase in the simulant concentrations.Typical products were identified and analyzed.This study demonstrates the broad spectrum and feasibility of the dd-r TENG-microplasma for CWA elimination,which provides significant guidance for their practical applications in the future.展开更多
In this letter,the streamer propagation in the atmospheric pressure helium plasma jet with afloating electrode nozzle driven by the kHz AC power supply is investigated.The current signal induced by the space charges a...In this letter,the streamer propagation in the atmospheric pressure helium plasma jet with afloating electrode nozzle driven by the kHz AC power supply is investigated.The current signal induced by the space charges and the mean propagation velocity of the guided ionization waves are measured by the capacitive probe method in the discharge region.The space charges in the guided ionization waves are found to increase with the applied voltage,which enhances both the electric field near the streamer head and the propagation velocity.The applicability of the streamer mechanism to the propagation of the guided ionization waves is validated by this electrical diagnostic method.展开更多
Aiming at the Four-Dimensional Variation source term inversion algorithm proposed earlier,the observation error regularization factor is introduced to improve the prediction accuracy of the diffusion model,and an impr...Aiming at the Four-Dimensional Variation source term inversion algorithm proposed earlier,the observation error regularization factor is introduced to improve the prediction accuracy of the diffusion model,and an improved Four-Dimensional Variation source term inversion algorithm with observation error regularization(OER-4DVAR STI model)is formed.Firstly,by constructing the inversion process and basic model of OER-4DVAR STI model,its basic principle and logical structure are studied.Secondly,the observation error regularization factor estimation method based on Bayesian optimization is proposed,and the error factor is separated and optimized by two parameters:error statistical time and deviation degree.Finally,the scientific,feasible and advanced nature of the OER-4DVAR STI model are verified by numerical simulation and tracer test data.The experimental results show that OER-4DVAR STI model can better reverse calculate the hazard source term information under the conditions of high atmospheric stability and flat underlying surface.Compared with the previous inversion algorithm,the source intensity estimation accuracy of OER-4DVAR STI model is improved by about 46.97%,and the source location estimation accuracy is improved by about 26.72%.展开更多
基金National Natural Science Foundation of China (22209094, 22209093)Research Funds of Institute of Zhejiang University-Quzhou (No. IZQ2023RCZX032)+2 种基金USTB Mat Com of Beijing Advanced Innovation Center for Materials Genome EngineeringMinistry of Education, Youth and Sports of the Czech Republic through the e-INFRA CZ (ID:90254)project Quantum materials for applications in sustainable technologies (QM4ST), funded as project No. CZ.02.01.01 /00/22_008/0004572。
文摘Two-dimensional transition metal carbides(MXenes) have been demonstrated to be promising supports for single-atom catalysts(SACs) to enable efficient oxygen evolution reaction(OER).However,the rational design of MXene-based SACs depends on an experimental trial-and-error approach.A theoretical guidance principle is highly expected for the efficient evaluation of MXene-based SACs.Herein,highthroughput screening was performed through first-principles calculations and machine learning techniques.Ti_(3)C_(2)(OH)_(x),V_(3)C_(2)(OH)_(x),Zr_(3)C_(2)(OH)_(x),Nb_(3)C_(2)(OH)_(x),Hf_(3)C_(2)(OH)_(x),Ta_(3)C_(2)(OH)_(x),and W_(3)C_(2)(OH)_(x) were screened out based on their excellent stability.Zn,Pd,Ag,Cd,Au,and Hg were proposed to be promising single atoms anchored in MXenes based on cohesive energy analysis.Hf_(3)C_(2)(OH)_(x) with a Pd single atom delivers a theoretical overpotential of 81 mV.Both moderate electron-deficient state and high covalency of metal-carbon bonds were critical features for the high OER reactivity.This principle is expected to be a promising approach to the rational design of OER catalysts for metal-air batteries,fuel cells,and other OER-based energy storage devices.
文摘In high-altitude nuclear detonations,the proportion of pulsed X-ray energy can exceed 70%,making it a specific monitoring signal for such events.These pulsed X-rays can be captured using a satellite-borne X-ray detector following atmospheric transmission.To quantitatively analyze the effects of different satellite detection altitudes,burst heights,and transmission angles on the physical processes of X-ray transport and energy fluence,we developed an atmospheric transmission algorithm for pulsed X-rays from high-altitude nuclear detonations based on scattering correction.The proposed method is an improvement over the traditional analytical method that only computes direct-transmission X-rays.The traditional analytical method exhibits a maximum relative error of 67.79% compared with the Monte Carlo method.Our improved method reduces this error to within 10% under the same conditions,even reaching 1% in certain scenarios.Moreover,its computation time is 48,000 times faster than that of the Monte Carlo method.These results have important theoretical significance and engineering application value for designing satellite-borne nuclear detonation pulsed X-ray detectors,inverting nuclear detonation source terms,and assessing ionospheric effects.
基金the support of National Nature Science Foundation of China, the support numbers are No. 10572149 and No.10676120the National Key Research and Development program of China (subject no. 2017YFC0209901) for its support to the work of this paper
文摘A systematic investigation on the mechanism of dynamic liquid dispersing process via theoretical and experimental approach is presented.The experiments include weak and strong constrained scenarios using the high-speed camera technique and the flash X-ray radiography technique.Based on dynamic analysis,one-dimensional characteristics analysis and some numerical simulations on the propagating processes of blast waves before the container shell rupturing,further and detailed analyses of the experimental results are presented.The effects of the liquid viscosity on the dynamic dispersing flow are also analyzed,and the spall fracture mechanism is explored.Thus,the dominating forces determining the dispersing liquid flow are revealed,that is,the stretching and shearing action due to the interaction of two reflecting rarefaction waves in opposite propagating directions.The influence of container shell strength on the dispersing liquid flow is also investigated,and the characters of cavitation layered in liquid before shell rupturing are uncovered.Results revealed that different shell material results in different cavitating layers.Then the different cavitating layers drive the different dynamic liquid dispersing process coming into being.The metastable liquid states caused by pressure drop and cavitation generation are discussed.
基金supported by State Key Laboratory of NBC Protection for Civilian,China
文摘Decontamination of 2-chloroethyl ethyl sulfide （2-CEES, CH_3CH_2SCH_2CH_2C1） by pulsed corona plasma was investigated. The results show that 212.6 mg/m^3 of 2-CEES, with the gas flow rate of 2 m^3/h, can be decontaminated to 0.09 mg/m^3. According to the variation of the inlet and outlet concentration of 2-CEES vapor with retention time, it is found that the reaction of 2-CEES in a pulsed corona plasma system follows the first order reaction, with the reaction rate constant of 0.463 s^-1. The decontamination mechanism is discussed based on an analysis of the dissociation energy of chemical bonds and decontamination products. The C-S bond adjacent to the C1 atom will be destroyed firstly to form CH3CH2S. and .CH2CH2C1 radicals. CH3CH2S. can be decomposed to .C_2H_5 and .S..S can be oxidized to SO_2, while .C_2H_5 can be finally oxidized to CO_2 and H_2O. The C-Cl bond in the .CH_2CH_2C1 radical can be destroyed to form .CH_2CH_2. and .C1, which can be mineralized to CO_2, H_2O and HCl. The H atom in the .CH_2CH_2C1 radical can also be substituted by -C1 to form CHCl_2-CHCl_2.
基金supported by National Natural Science Foundation of China(No.51877205)Fundamental Research Funds for the Central Universities(No.buct201906)+1 种基金the State Key Laboratory of NBC Protection for Civilian(No.SKLNBC2021-0X)Beijing Nova Program(No.2022015)。
文摘Low-temperature plasma is a green and high-efficiency technology for chemical warfare agent(CWA)decontamination.However,traditional plasma devices suffer from the problems of highpower composition and large power-supply size,which limit their practical applications.In this paper,a self-driven microplasma decontamination system,induced by a dielectric-dielectric rotary triboelectric nanogenerator(dd-r TENG),was innovatively proposed for the decontamination of CWA simulants.The microplasma was characterized via electrical measurements,optical emission spectra and ozone concentration detection.With an output voltage of-3460 V,the dd-r TENG can successfully excite microplasma in air.Reactive species,such as OH,O(1D),Hαand O3were detected.With input average power of 0.116 W,the decontamination rate of 2-chloroethyl ethyl sulfide reached 100%within 3 min of plasma treatment,while the decontamination rates of malathion and dimethyl methylphosphonate reached(65.92±1.65)%and(60.88±1.92)%after 7 min of plasma treatment,respectively.In addition,the decontamination rates gradually decreased with the increase in the simulant concentrations.Typical products were identified and analyzed.This study demonstrates the broad spectrum and feasibility of the dd-r TENG-microplasma for CWA elimination,which provides significant guidance for their practical applications in the future.
基金supported by National Natural Science Foundation of China(Nos.10775087 and51907190)the State Key Laboratory of NBC Protection for Civilian(SKLNBC 2019–16)。
文摘In this letter,the streamer propagation in the atmospheric pressure helium plasma jet with afloating electrode nozzle driven by the kHz AC power supply is investigated.The current signal induced by the space charges and the mean propagation velocity of the guided ionization waves are measured by the capacitive probe method in the discharge region.The space charges in the guided ionization waves are found to increase with the applied voltage,which enhances both the electric field near the streamer head and the propagation velocity.The applicability of the streamer mechanism to the propagation of the guided ionization waves is validated by this electrical diagnostic method.
基金Ministry of Science and Technology of the People’s Republic of China for its support and guidance(Grant No.2018YFC0214100)。
文摘Aiming at the Four-Dimensional Variation source term inversion algorithm proposed earlier,the observation error regularization factor is introduced to improve the prediction accuracy of the diffusion model,and an improved Four-Dimensional Variation source term inversion algorithm with observation error regularization(OER-4DVAR STI model)is formed.Firstly,by constructing the inversion process and basic model of OER-4DVAR STI model,its basic principle and logical structure are studied.Secondly,the observation error regularization factor estimation method based on Bayesian optimization is proposed,and the error factor is separated and optimized by two parameters:error statistical time and deviation degree.Finally,the scientific,feasible and advanced nature of the OER-4DVAR STI model are verified by numerical simulation and tracer test data.The experimental results show that OER-4DVAR STI model can better reverse calculate the hazard source term information under the conditions of high atmospheric stability and flat underlying surface.Compared with the previous inversion algorithm,the source intensity estimation accuracy of OER-4DVAR STI model is improved by about 46.97%,and the source location estimation accuracy is improved by about 26.72%.
