Assume that L is a non-negative self-adjoint operator on L^(2)(ℝ^(n))with its heat kernels satisfying the so-called Gaussian upper bound estimate and that X is a ball quasi-Banach function space onℝ^(n) satisfying som...Assume that L is a non-negative self-adjoint operator on L^(2)(ℝ^(n))with its heat kernels satisfying the so-called Gaussian upper bound estimate and that X is a ball quasi-Banach function space onℝ^(n) satisfying some mild assumptions.Let HX,L(ℝ^(n))be the Hardy space associated with both X and L,which is defined by the Lusin area function related to the semigroup generated by L.In this article,the authors establish various maximal function characterizations of the Hardy space HX,L(ℝ^(n))and then apply these characterizations to obtain the solvability of the related Cauchy problem.These results have a wide range of generality and,in particular,the specific spaces X to which these results can be applied include the weighted space,the variable space,the mixed-norm space,the Orlicz space,the Orlicz-slice space,and the Morrey space.Moreover,the obtained maximal function characterizations of the mixed-norm Hardy space,the Orlicz-slice Hardy space,and the Morrey-Hardy space associated with L are completely new.展开更多
Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batt...Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.展开更多
Combining the mean field Pozhar-Gubbins(PG)theory and the weighted density approximation,a novel method for local thermal conductivity of inhomogeneous fluids is proposed.The correlation effect that is beyond the mean...Combining the mean field Pozhar-Gubbins(PG)theory and the weighted density approximation,a novel method for local thermal conductivity of inhomogeneous fluids is proposed.The correlation effect that is beyond the mean field treatment is taken into account by the simulation-based empirical correlations.The application of this method to confined argon in slit pore shows that its prediction agrees well with the simulation results,and that it performs better than the original PG theory as well as the local averaged density model(LADM).In its further application to the nano-fluidic films,the influences of fluid parameters and pore parameters on the thermal conductivity are calculated and investigated.It is found that both the local thermal conductivity and the overall thermal conductivity can be significantly modulated by these parameters.Specifically,in the supercritical states,the thermal conductivity of the confined fluid shows positive correlation to the bulk density as well as the temperature.However,when the bulk density is small,the thermal conductivity exhibits a decrease-increase transition as the temperature is increased.This is also the case in which the temperature is low.In fact,the decrease-increase transition in both the small-bulk-density and low-temperature cases arises from the capillary condensation in the pore.Furthermore,smaller pore width and/or stronger adsorption potential can raise the critical temperature for condensation,and then are beneficial to the enhancement of the thermal conductivity.These modulation behaviors of the local thermal conductivity lead immediately to the significant difference of the overall thermal conductivity in different phase regions.展开更多
Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and selectivity.However...Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and selectivity.However,the underlying microscopic mechanism remains ambiguous.In this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or acrylonitrile.By analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy decrease.In addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions.展开更多
The process of entrainment-mixing between cumulus clouds and the ambient air is important for the development of cumulus clouds.Accurately obtaining the entrainment rate(λ)is particularly important for its parameteri...The process of entrainment-mixing between cumulus clouds and the ambient air is important for the development of cumulus clouds.Accurately obtaining the entrainment rate(λ)is particularly important for its parameterization within the overall cumulus parameterization scheme.In this study,an improved bulk-plume method is proposed by solving the equations of two conserved variables simultaneously to calculateλof cumulus clouds in a large-eddy simulation.The results demonstrate that the improved bulk-plume method is more reliable than the traditional bulk-plume method,becauseλ,as calculated from the improved method,falls within the range ofλvalues obtained from the traditional method using different conserved variables.The probability density functions ofλfor all data,different times,and different heights can be well-fitted by a log-normal distribution,which supports the assumed stochastic entrainment process in previous studies.Further analysis demonstrate that the relationship betweenλand the vertical velocity is better than other thermodynamic/dynamical properties;thus,the vertical velocity is recommended as the primary influencing factor for the parameterization ofλin the future.The results of this study enhance the theoretical understanding ofλand its influencing factors and shed new light on the development ofλparameterization.展开更多
CaO–SiO_(2)compounds compromise one of the most common series of oxide particles in liquid steels, which could significantly affect the service performance of the steels as crack initiation sites. However, the struct...CaO–SiO_(2)compounds compromise one of the most common series of oxide particles in liquid steels, which could significantly affect the service performance of the steels as crack initiation sites. However, the structural, electronic, and mechanical properties of the compounds in CaO–SiO_(2)system are still not fully clarified due to the difficulties in the experiments. In this study, a thorough investigation of these properties of CaO–SiO_(2)compound particles in steels was conducted based on first-principles density functional theory. Corresponding phases were determined by thermodynamic calculation, including gamma dicalcium silicate(γ-C2S), alpha-prime(L) dicalcium silicate(αL′-C2S), alpha-prime(H) dicalcium silicate(αH′-C2S), alpha dicalcium silicate(α-C2S), rankinite(C3S2), hatrurite(C3S), wollastonite(CS), and pseudowollastonite(Ps-CS). The results showed that the calculated crystal structures of the eight phases agree well with the experimental results. All the eight phases are stable according to the calculated formation energies, and γ-C2S is the most stable. O atom contributes the most to the reactivity of these phases. The Young’s modulus of the eight phases is in the range of 100.63–132.04 GPa. Poisson’s ratio is in the range of0.249–0.281. This study provided further understanding concerning the CaO–SiO_(2)compound particles in steels and fulfilled the corresponding property database, paving the way for inclusion engineering and design in terms of fracture-resistant steels.展开更多
Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum ...Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.展开更多
In this study,a microscopic method for calculating the nuclear level density(NLD)based on the covariant density functional theory(CDFT)is developed.The particle-hole state density is calculated by a combinatorial meth...In this study,a microscopic method for calculating the nuclear level density(NLD)based on the covariant density functional theory(CDFT)is developed.The particle-hole state density is calculated by a combinatorial method using single-particle level schemes obtained from the CDFT,and the level densities are then obtained by considering collective effects such as vibration and rotation.Our results are compared with those of other NLD models,including phenomenological,microstatisti-cal and nonrelativistic Hartree–Fock–Bogoliubov combinatorial models.This comparison suggests that the general trends among these models are essentially the same,except for some deviations among the different NLD models.In addition,the NLDs obtained using the CDFT combinatorial method with normalization are compared with experimental data,including the observed cumulative number of levels at low excitation energies and the measured NLDs.The CDFT combinatorial method yields results that are in reasonable agreement with the existing experimental data.展开更多
As one of the important aspects of upgrading coal tar,the ultra-deep removal of metal ions via the complexation method was investigated by screening four complexing agents and performing density functional theory(DFT)...As one of the important aspects of upgrading coal tar,the ultra-deep removal of metal ions via the complexation method was investigated by screening four complexing agents and performing density functional theory(DFT)simulations.Analysis of the compositions and contents of the metallic compounds in the coal tar revealed that the main components were iron and calcium naphthenates.Direct filtration reduced the mechanical impurity content from 0.24%to 0.0752%,indicating that most of the large particles could be easily removed.Among the four complexing agents,namely,acetic acid,oxalic acid,citric acid,and ethylenediaminetetraacetic acid,oxalic acid exhibited the best demetallization performance.The DFT simulations suggested that the high performance of oxalic acid originated from its 1:1 coordination mode,rigid dicarboxyl structure,and greater binding energy.展开更多
Density functional theory(DFT)is used to calculate the most stable structures of Zr_(n)(n=2-5)clusters as well as the adsorption energy values of Zr_(n)(n=2-5)clusters after adsorbing single water molecule.The results...Density functional theory(DFT)is used to calculate the most stable structures of Zr_(n)(n=2-5)clusters as well as the adsorption energy values of Zr_(n)(n=2-5)clusters after adsorbing single water molecule.The results reveal that there is a significant linear relationship between the adsorption energy values and the energy gaps of the Zr_(n)(n=2-5)clusters.Furthermore,the calculations of the reaction paths between Zr_(n)(n=2-5)and single water molecule show that water molecule can react with Zr_(n)(n=2-5)clusters to dissociate,producing hydrogen,and O atoms mix with the clusters to generate Zr_(n)O(n=2-5),all of which are exothermic reactions.According to the released energy,the Zr4 cluster is the most efficient in Zr_(n)(n=2-5)clusters reacting with single water molecule.The natural population analysis(NPA)and density of states(DOS)demonstrate the production of hydrogen and orbital properties in different energy ranges,respectively,jointly forecasting that Zr_(n)O(n=2-5)will probably continue to react with more water molecules.Our findings contribute to better understanding of Zr's chemical reactivity,which can conduce to the development of effective Zr-based catalysts and hydrogen-production methods.展开更多
Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR cataly...Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.展开更多
Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway...Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.展开更多
This paper presents a linearized approach for the controller design of the shape of output probability density functions for general stochastic systems. A square root approximation to an output probability density fun...This paper presents a linearized approach for the controller design of the shape of output probability density functions for general stochastic systems. A square root approximation to an output probability density function is realized by a set of B-spline functions. This generally produces a nonlinear state space model for the weights of the B-spline approximation. A linearized model is therefore obtained and embedded into a performance function that measures the tracking error of the output probability density function with respect to a given distribution. By using this performance function as a Lyapunov function for the closed loop system, a feedback control input has been obtained which guarantees closed loop stability and realizes perfect tracking. The algorithm described in this paper has been tested on a simulated example and desired results have been achieved.展开更多
In polyester fiber industrial processes,the prediction of key performance indicators is vital for product quality.The esterification process is an indispensable step in the polyester polymerization process.It has the ...In polyester fiber industrial processes,the prediction of key performance indicators is vital for product quality.The esterification process is an indispensable step in the polyester polymerization process.It has the characteristics of strong coupling,nonlinearity and complex mechanism.To solve these problems,we put forward a multi-output Gaussian process regression(MGPR)model based on the combined kernel function for the polyester esterification process.Since the seasonal and trend decomposition using loess(STL)can extract the periodic and trend characteristics of time series,a combined kernel function based on the STL and the kernel function analysis is constructed for the MGPR.The effectiveness of the proposed model is verified by the actual polyester esterification process data collected from fiber production.展开更多
The main problem of quantum mechanics is to elucidate why the probability density is the modulus square of wave function. For the purpose of solving this problem, we explored the possibility of deducing the fundamenta...The main problem of quantum mechanics is to elucidate why the probability density is the modulus square of wave function. For the purpose of solving this problem, we explored the possibility of deducing the fundamental equation of quantum mechanics by starting with the probability density. To do so, it is necessary to formulate a new theory of quantum mechanics distinguished from the previous ones. Our investigation shows that it is possible to construct quantum mechanics in phase space as an alternative autonomous formulation and such a possibility enables us to study quantum mechanics by starting with the probability density rather than the wave function. This direction of research is contrary to configuration-space formulation of quantum mechanics starting with the wave function. Our work leads to a full understanding of the wave function as the both mathematically and physically sufficient representation of quantum-mechanical state which supplements information on quantum state given solely by the probability density with phase information on quantum state. The final result of our work is that quantum mechanics in phase space satisfactorily elucidates the relation between the wave function and the probability density by using the consistent procedure starting with the probability density, thus corroborating the ontological interpretation of the wave function and withdrawing a main assumption of quantum mechanics.展开更多
Cement density monitoring plays a vital role in evaluating the quality of cementing projects,which is of great significance to the development of oil and gas.However,the presence of inhomogeneous cement distribution a...Cement density monitoring plays a vital role in evaluating the quality of cementing projects,which is of great significance to the development of oil and gas.However,the presence of inhomogeneous cement distribution and casing eccentricity in horizontal wells often complicates the accurate evaluation of cement azimuthal density.In this regard,this paper proposes an algorithm to calculate the cement azimuthal density in horizontal wells using a multi-detector gamma-ray detection system.The spatial dynamic response functions are simulated to obtain the influence of cement density on gamma-ray counts by the perturbation theory,and the contribution of cement density in six sectors to the gamma-ray recorded by different detectors is obtained by integrating the spatial dynamic response functions.Combined with the relationship between gamma-ray counts and cement density,a multi-parameter calculation equation system is established,and the regularized Newton iteration method is employed to invert casing eccentricity and cement azimuthal density.This approach ensures the stability of the inversion process while simultaneously achieving an accuracy of 0.05 g/cm^(3) for the cement azimuthal density.This accuracy level is ten times higher compared to density accuracy calculated using calibration equations.Overall,this algorithm enhances the accuracy of cement azimuthal density evaluation,provides valuable technical support for the monitoring of cement azimuthal density in the oil and gas industry.展开更多
Population density functions have long been used to describe the spatial structure of regional population distributions.Several studies have been conducted to examine the population distribution in Shandong Province,C...Population density functions have long been used to describe the spatial structure of regional population distributions.Several studies have been conducted to examine the population distribution in Shandong Province,China,but few have applied regional density functions to the analysis.Therefore,based on the 2000,2010,and 2020 population censuses,this study used monocentric and polycentric regional density functions to study the characteristics of population agglomeration and diffusion in Shandong.This is followed by an in-depth discussion based on population growth rate data and hot-and cold-spot analyses.The results showed that the Shandong Province population was spatially unevenly distributed.Population growth rates were higher in urban centers and counties,with more significant changes in population size in the eastern coastal areas than in the inland areas.As verified in this study,the logarithmic form of the single-center regional density function R2 was greater than 0.8,which was in line with the population spatial structure of Shandong Province.During the study period,the estimated population density of the regional center and the absolute value of the regional population density gradient both increased,indicating a clear and increasing trend of centripetal agglomeration of regional centers over the study period.Overall,the R2 value of the multicenter region density function was higher than that of the single-center region density function.The polycentric regional density function showed that the population density gradient of some centers had a downward trend,which reflected the spatial development trend of outward diffusion in these centers.Meanwhile,the variation in the estimated population density and the population density gradient exhibited differences in the central population distribution patterns at different levels.展开更多
The wave/particle duality of particles in Physics is well known. Particles have properties that uniquely characterize them from one another, such as mass, charge and spin. Charged particles have associated Electric an...The wave/particle duality of particles in Physics is well known. Particles have properties that uniquely characterize them from one another, such as mass, charge and spin. Charged particles have associated Electric and Magnetic fields. Also, every moving particle has a De Broglie wavelength determined by its mass and velocity. This paper shows that all of these properties of a particle can be derived from a single wave function equation for that particle. Wave functions for the Electron and the Positron are presented and principles are provided that can be used to calculate the wave functions of all the fundamental particles in Physics. Fundamental particles such as electrons and positrons are considered to be point particles in the Standard Model of Physics and are not considered to have a structure. This paper demonstrates that they do indeed have structure and that this structure extends into the space around the particle’s center (in fact, they have infinite extent), but with rapidly diminishing energy density with the distance from that center. The particles are formed from Electromagnetic standing waves, which are stable solutions to the Schrödinger and Classical wave equations. This stable structure therefore accounts for both the wave and particle nature of these particles. In fact, all of their properties such as mass, spin and electric charge, can be accounted for from this structure. These particle properties appear to originate from a single point at the center of the wave function structure, in the same sort of way that the Shell theorem of gravity causes the gravity of a body to appear to all originate from a central point. This paper represents the first two fully characterized fundamental particles, with a complete description of their structure and properties, built up from the underlying Electromagnetic waves that comprise these and all fundamental particles.展开更多
Using density functional methods,some properties were studied such as the energies and compositions of frontier molecular orbitals and the atomic charges,which are related to the reactive behavior of thioureas contain...Using density functional methods,some properties were studied such as the energies and compositions of frontier molecular orbitals and the atomic charges,which are related to the reactive behavior of thioureas containing different N-substituent groupings.The calculation results indicate that the N-substituent groupings have significant effect on the flotation performance of thiourea collectors.The order of electron-donating ability is N-propyl-N'-benzyl-thiourea(PBZYTU)>N-propyl-N'-ethyl-thiourea (PETU)>N-propyl-N'-allyl-thiourea(PALTU)>>N-propyl-N'-acetyl-thiourea(PACTU)>N-propyl-N'-ethoxycarbonyl-thiourea (PECTU)>N-propyl-N'-benzoyl-thiourea(PBZOYTU),and the order of feedback-electron-accepting ability is PBZOYTU> PACTU>PECTU>>PALTU>PETU>PBZYTU.This implies that PBZOYTU,PACTU or PECTU can react with copper atoms having(t2g) 6 (eg) 3Cu(II)or t 6e 4Cu(I)configuration on the surfaces of copper sulfide minerals through normal covalent bond and back donation covalent bond,and exhibit excellently collecting performance for copper sulfide minerals.These are consistent with the experimental data reported in the literatures.展开更多
基金supported by the National Key Research and Development Program of China(2020YFA0712900)the National Natural Science Foundation of China(12371093,12071197,12122102 and 12071431)+2 种基金the Key Project of Gansu Provincial National Science Foundation(23JRRA1022)the Fundamental Research Funds for the Central Universities(2233300008 and lzujbky-2021-ey18)the Innovative Groups of Basic Research in Gansu Province(22JR5RA391).
文摘Assume that L is a non-negative self-adjoint operator on L^(2)(ℝ^(n))with its heat kernels satisfying the so-called Gaussian upper bound estimate and that X is a ball quasi-Banach function space onℝ^(n) satisfying some mild assumptions.Let HX,L(ℝ^(n))be the Hardy space associated with both X and L,which is defined by the Lusin area function related to the semigroup generated by L.In this article,the authors establish various maximal function characterizations of the Hardy space HX,L(ℝ^(n))and then apply these characterizations to obtain the solvability of the related Cauchy problem.These results have a wide range of generality and,in particular,the specific spaces X to which these results can be applied include the weighted space,the variable space,the mixed-norm space,the Orlicz space,the Orlicz-slice space,and the Morrey space.Moreover,the obtained maximal function characterizations of the mixed-norm Hardy space,the Orlicz-slice Hardy space,and the Morrey-Hardy space associated with L are completely new.
基金the support of the National Natural Science Foundation of China(Grant No.51472074).
文摘Understanding the adsorption interactions between carbon materials and sulfur compounds has far-reaching impacts,in addition to their well-known important role in energy storage and conversion,such as lithium-ion batteries.In this paper,properties of intrinsic B or Si single-atom doped,and B-Si codoped graphene(GR)and graphdiyne(GDY)were investigated by using density functional theory-based calculations,in which the optimal doping configurations were explored for potential applications in adsorbing sulfur compounds.Results showed that both B or Si single-atom doping and B-Si codoping could substantially enhance the electron transport properties of GR and GDY,improving their surface activity.Notably,B and Si atoms displayed synergistic effects for the codoped configurations,where B-Si codoped GR/GDY exhibited much better performance in the adsorption of sulfurcontaining chemicals than single-atom doped systems.In addition,results demonstrated that,after B-Si codoping,the adsorption energy and charge transfer amounts of GDY with sulfur compounds were much larger than those of GR,indicating that B-Si codoped GDY might be a favorable material for more effectively interacting with sulfur reagents.
基金Project supported by the Fundamental Research Fund for the Central Universities of Chinathe Research Project for Independently Cultivate Talents of Hebei Agricultural University (Grant No.ZY2023007)。
文摘Combining the mean field Pozhar-Gubbins(PG)theory and the weighted density approximation,a novel method for local thermal conductivity of inhomogeneous fluids is proposed.The correlation effect that is beyond the mean field treatment is taken into account by the simulation-based empirical correlations.The application of this method to confined argon in slit pore shows that its prediction agrees well with the simulation results,and that it performs better than the original PG theory as well as the local averaged density model(LADM).In its further application to the nano-fluidic films,the influences of fluid parameters and pore parameters on the thermal conductivity are calculated and investigated.It is found that both the local thermal conductivity and the overall thermal conductivity can be significantly modulated by these parameters.Specifically,in the supercritical states,the thermal conductivity of the confined fluid shows positive correlation to the bulk density as well as the temperature.However,when the bulk density is small,the thermal conductivity exhibits a decrease-increase transition as the temperature is increased.This is also the case in which the temperature is low.In fact,the decrease-increase transition in both the small-bulk-density and low-temperature cases arises from the capillary condensation in the pore.Furthermore,smaller pore width and/or stronger adsorption potential can raise the critical temperature for condensation,and then are beneficial to the enhancement of the thermal conductivity.These modulation behaviors of the local thermal conductivity lead immediately to the significant difference of the overall thermal conductivity in different phase regions.
基金supported by the National Natural Science Foundation of China(22168002,22108070,21878078)the Natural Science Foundation of Guangxi Province(2020GXNSFAA159119)+2 种基金the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2021Z012)the Open Fund of the State Key Laboratory of Molecular Reaction Dynamics in DICP(SKLMRD-K202106)the Young Elite Scientists Sponsorship Program by CAST(2022QNRC001)。
文摘Extensive experimental studies have been performed on the Diels-Alder(DA)reactions in ionic liquids(ILs),which demonstrate that the IL environment can significantly influence the reaction rates and selectivity.However,the underlying microscopic mechanism remains ambiguous.In this work,the multiscale reaction density functional theory is applied to explore the effect of 1-butyl-3-methylimidazolium hexafluorophosphate([BMIM][PF_(6)])solvent on the reaction of cyclopentadiene(CP)with acrolein,methyl acrylate,or acrylonitrile.By analyzing the free energy landscape during the reaction,it is found that the polarization effect has a relatively small influence,while the solvation effect makes both the activation free energy and reaction free energy decrease.In addition,the rearrangement of local solvent structure shows that the cation spatial distribution responds more evidently to the reaction than the anion,and this indicates that the cation plays a dominant role in the solvation effect and so as to affect the reaction rates and selectivity of the DA reactions.
基金supported by the National Natural Science Foundation of China(Grant Nos.42175099,42027804,42075073)the Innovative Project of Postgraduates in Jiangsu Province in 2023(Grant No.KYCX23_1319)+3 种基金supported by the National Natural Science Foundation of China(Grant No.42205080)the Natural Science Foundation of Sichuan(Grant No.2023YFS0442)the Research Fund of Civil Aviation Flight University of China(Grant No.J2022-037)supported by the National Key Scientific and Technological Infrastructure project“Earth System Science Numerical Simulator Facility”(Earth Lab)。
文摘The process of entrainment-mixing between cumulus clouds and the ambient air is important for the development of cumulus clouds.Accurately obtaining the entrainment rate(λ)is particularly important for its parameterization within the overall cumulus parameterization scheme.In this study,an improved bulk-plume method is proposed by solving the equations of two conserved variables simultaneously to calculateλof cumulus clouds in a large-eddy simulation.The results demonstrate that the improved bulk-plume method is more reliable than the traditional bulk-plume method,becauseλ,as calculated from the improved method,falls within the range ofλvalues obtained from the traditional method using different conserved variables.The probability density functions ofλfor all data,different times,and different heights can be well-fitted by a log-normal distribution,which supports the assumed stochastic entrainment process in previous studies.Further analysis demonstrate that the relationship betweenλand the vertical velocity is better than other thermodynamic/dynamical properties;thus,the vertical velocity is recommended as the primary influencing factor for the parameterization ofλin the future.The results of this study enhance the theoretical understanding ofλand its influencing factors and shed new light on the development ofλparameterization.
基金supported by the National Natural Science Foundation of China (No. 52174297)Fundamental Research Funds for the Central Universities (No. FRF-TP-20026A1)+1 种基金the special grade of China Postdoctoral Science Foundation (No. 2021T140050)supported by USTB MatCom of Beijing Advanced Innovation Center for Materials Genome Engineering。
文摘CaO–SiO_(2)compounds compromise one of the most common series of oxide particles in liquid steels, which could significantly affect the service performance of the steels as crack initiation sites. However, the structural, electronic, and mechanical properties of the compounds in CaO–SiO_(2)system are still not fully clarified due to the difficulties in the experiments. In this study, a thorough investigation of these properties of CaO–SiO_(2)compound particles in steels was conducted based on first-principles density functional theory. Corresponding phases were determined by thermodynamic calculation, including gamma dicalcium silicate(γ-C2S), alpha-prime(L) dicalcium silicate(αL′-C2S), alpha-prime(H) dicalcium silicate(αH′-C2S), alpha dicalcium silicate(α-C2S), rankinite(C3S2), hatrurite(C3S), wollastonite(CS), and pseudowollastonite(Ps-CS). The results showed that the calculated crystal structures of the eight phases agree well with the experimental results. All the eight phases are stable according to the calculated formation energies, and γ-C2S is the most stable. O atom contributes the most to the reactivity of these phases. The Young’s modulus of the eight phases is in the range of 100.63–132.04 GPa. Poisson’s ratio is in the range of0.249–0.281. This study provided further understanding concerning the CaO–SiO_(2)compound particles in steels and fulfilled the corresponding property database, paving the way for inclusion engineering and design in terms of fracture-resistant steels.
基金the funding support from Shanghai Sailing Program (19YF1411000)National Natural Science Foundation of China (21878080, 21808058)Ningxia Science Foundation (2019AAC03282)。
文摘Production of light olefins from CO_(2), the primary greenhouse gases, is of great importance to mitigate the adverse effects of CO_(2) emission on environment and to supply the value-added products from nonpetroleum resource. However, development of robust catalyst with controllable selectivity and stability remains a challenge. Herein, we report that Zn-promoted Fe catalyst can boost the stable and selective production of light olefins from CO_(2). Specifically, the Zn-promoted Fe exhibits a highly stable activity and olefin selectivity over 200 h time-on-stream compared to the unpromoted Fe catalyst, primarily owing to the preservation of active χ-Fe_(5)C_(2) phase. Structural characterizations of the spent catalysts suggest that Zn substantially regulates the content of iron carbide on the surface and suppresses the reoxidation of bulk iron carbide during the reaction. DFT calculations confirm that adsorption of surface carbon atoms and graphene-like carbonaceous species are not thermochemically favored on Zn-promoted Fe catalyst. Carbon deposition by CAC coupling reactions of two surface carbon atoms and dehydrogenation of CH intermediate are also inhibited. Furthermore, the effects of Zn on antioxidation of iron carbide were also investigated. Zn favored the hydrogenation of surface adsorbed oxygen atoms to H_(2)O and the desorption of H_(2)O, which reduces the possibility of surface carbide being oxidized by the chemisorbed oxygen.
基金supported by the Natural Science Foundation of Jilin Province(No.20220101017JC)National Natural Science Foundation of China(No.11675063)Key Laboratory of Nuclear Data Foundation(JCKY2020201C157).
文摘In this study,a microscopic method for calculating the nuclear level density(NLD)based on the covariant density functional theory(CDFT)is developed.The particle-hole state density is calculated by a combinatorial method using single-particle level schemes obtained from the CDFT,and the level densities are then obtained by considering collective effects such as vibration and rotation.Our results are compared with those of other NLD models,including phenomenological,microstatisti-cal and nonrelativistic Hartree–Fock–Bogoliubov combinatorial models.This comparison suggests that the general trends among these models are essentially the same,except for some deviations among the different NLD models.In addition,the NLDs obtained using the CDFT combinatorial method with normalization are compared with experimental data,including the observed cumulative number of levels at low excitation energies and the measured NLDs.The CDFT combinatorial method yields results that are in reasonable agreement with the existing experimental data.
基金the National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)the National Natural Science Foundation of China(22078347)the Key Research and Development Program of Hebei Province,China(21373303D).
文摘As one of the important aspects of upgrading coal tar,the ultra-deep removal of metal ions via the complexation method was investigated by screening four complexing agents and performing density functional theory(DFT)simulations.Analysis of the compositions and contents of the metallic compounds in the coal tar revealed that the main components were iron and calcium naphthenates.Direct filtration reduced the mechanical impurity content from 0.24%to 0.0752%,indicating that most of the large particles could be easily removed.Among the four complexing agents,namely,acetic acid,oxalic acid,citric acid,and ethylenediaminetetraacetic acid,oxalic acid exhibited the best demetallization performance.The DFT simulations suggested that the high performance of oxalic acid originated from its 1:1 coordination mode,rigid dicarboxyl structure,and greater binding energy.
基金Project supported by the Open Research Fund of Computational Physics Key Laboratory of Sichuan Province,Yibin University,China(Grant No.YBXYJSWL-ZD-2020-005)the Student’s Platform for Innovation and Entrepreneurship Training Program,China(Grant No.S202110616084)。
文摘Density functional theory(DFT)is used to calculate the most stable structures of Zr_(n)(n=2-5)clusters as well as the adsorption energy values of Zr_(n)(n=2-5)clusters after adsorbing single water molecule.The results reveal that there is a significant linear relationship between the adsorption energy values and the energy gaps of the Zr_(n)(n=2-5)clusters.Furthermore,the calculations of the reaction paths between Zr_(n)(n=2-5)and single water molecule show that water molecule can react with Zr_(n)(n=2-5)clusters to dissociate,producing hydrogen,and O atoms mix with the clusters to generate Zr_(n)O(n=2-5),all of which are exothermic reactions.According to the released energy,the Zr4 cluster is the most efficient in Zr_(n)(n=2-5)clusters reacting with single water molecule.The natural population analysis(NPA)and density of states(DOS)demonstrate the production of hydrogen and orbital properties in different energy ranges,respectively,jointly forecasting that Zr_(n)O(n=2-5)will probably continue to react with more water molecules.Our findings contribute to better understanding of Zr's chemical reactivity,which can conduce to the development of effective Zr-based catalysts and hydrogen-production methods.
基金supported by the National Natural Science Foundation of China(92061125,21978294)Beijing Natural Science Foundation(Z200012)+3 种基金Jiangxi Natural Science Foundation(20212ACB213009)DNL Cooperation Fund,CAS(DNL201921)Self-deployed Projects of Ganjiang Innovation Academy,Chinese Academy of Sciences(E055B003)Hebei Natural Science Foundation(B2020103043)。
文摘Developing novel oxygen reduction reaction(ORR)catalysts with high activity is urgent for proton exchange membrane fuel cells.Herein,we investigated a group of size-dependent Pt-based catalysts as promising ORR catalysts by density functional theory calculations,ranging from single-atom,nanocluster to bulk Pt catalysts.The results showed that the ORR overpotential of these Pt-based catalysts increased when its size enlarged to the nanoparticle scale or reduced to the single-atom scale,and the Pt_(38)cluster had the lowest ORR overpotential(0.46 V)compared with that of Pt_(111)(0.57 V)and single atom Pt(0.7 V).Moreover,we established a volcano curve relationship between the ORR overpotential and binding energy of O*(ΔE_(O*),confirming the intermediate species anchored on Pt38cluster with suitable binding energy located at top of volcano curve.The interaction between intermediate species and Pt-based catalysts were also investigated by the charge distribution and projected density of state and which further confirmed the results of volcano curve.
基金the National Natural Science Foundation of China(Nos.41406090,42176045)the Science Foundation of Qingdao Agricultural University(No.631302)+1 种基金the Fujian Key Laboratory of Functional Marine Sensing Materials,Minjiang University(No.MJUKF-FMSM202102)the Natural Science Foundation of Shandong Province(Nos.ZR2019 MB020,ZR2020MB119)。
文摘Polybrominated diphenyl ethers(PBDEs)are a kind of serious pollutants in the ocean.Biodegradation is considered as an economical and safe way for PBDEs removal and reductive debromination dominates the initial pathway of anaerobic degradation.On the basis of experimental study,Octa-BDE 197,Hepta-BDE 183,Hexa-BDE 153,Penta-BDE 99 and Tetra-BDE 47 were selected as the initial degradation objects,and their debromination degradation were studied using density functional theory.The structures were optimized by Gaussian 09 program.Furthermore,the molecular orbitals and charge distribution were analyzed.All C-Br bond dissociation energies at different positions including ortho,meta and para bromine atoms were calculated and the sequence of debromination was obtained.There is a close relationship between molecular structure,charge,molecular orbital and C-Br bond.All PBDEs exhibited similar debromination pathways with preferential removal of meta and para bromines.
文摘This paper presents a linearized approach for the controller design of the shape of output probability density functions for general stochastic systems. A square root approximation to an output probability density function is realized by a set of B-spline functions. This generally produces a nonlinear state space model for the weights of the B-spline approximation. A linearized model is therefore obtained and embedded into a performance function that measures the tracking error of the output probability density function with respect to a given distribution. By using this performance function as a Lyapunov function for the closed loop system, a feedback control input has been obtained which guarantees closed loop stability and realizes perfect tracking. The algorithm described in this paper has been tested on a simulated example and desired results have been achieved.
基金Natural Science Foundation of Shanghai,China(No.19ZR1402300)。
文摘In polyester fiber industrial processes,the prediction of key performance indicators is vital for product quality.The esterification process is an indispensable step in the polyester polymerization process.It has the characteristics of strong coupling,nonlinearity and complex mechanism.To solve these problems,we put forward a multi-output Gaussian process regression(MGPR)model based on the combined kernel function for the polyester esterification process.Since the seasonal and trend decomposition using loess(STL)can extract the periodic and trend characteristics of time series,a combined kernel function based on the STL and the kernel function analysis is constructed for the MGPR.The effectiveness of the proposed model is verified by the actual polyester esterification process data collected from fiber production.
文摘The main problem of quantum mechanics is to elucidate why the probability density is the modulus square of wave function. For the purpose of solving this problem, we explored the possibility of deducing the fundamental equation of quantum mechanics by starting with the probability density. To do so, it is necessary to formulate a new theory of quantum mechanics distinguished from the previous ones. Our investigation shows that it is possible to construct quantum mechanics in phase space as an alternative autonomous formulation and such a possibility enables us to study quantum mechanics by starting with the probability density rather than the wave function. This direction of research is contrary to configuration-space formulation of quantum mechanics starting with the wave function. Our work leads to a full understanding of the wave function as the both mathematically and physically sufficient representation of quantum-mechanical state which supplements information on quantum state given solely by the probability density with phase information on quantum state. The final result of our work is that quantum mechanics in phase space satisfactorily elucidates the relation between the wave function and the probability density by using the consistent procedure starting with the probability density, thus corroborating the ontological interpretation of the wave function and withdrawing a main assumption of quantum mechanics.
基金The authors would like to acknowledge the support of the National Natural Science Foundation of China(41974127,42174147).References。
文摘Cement density monitoring plays a vital role in evaluating the quality of cementing projects,which is of great significance to the development of oil and gas.However,the presence of inhomogeneous cement distribution and casing eccentricity in horizontal wells often complicates the accurate evaluation of cement azimuthal density.In this regard,this paper proposes an algorithm to calculate the cement azimuthal density in horizontal wells using a multi-detector gamma-ray detection system.The spatial dynamic response functions are simulated to obtain the influence of cement density on gamma-ray counts by the perturbation theory,and the contribution of cement density in six sectors to the gamma-ray recorded by different detectors is obtained by integrating the spatial dynamic response functions.Combined with the relationship between gamma-ray counts and cement density,a multi-parameter calculation equation system is established,and the regularized Newton iteration method is employed to invert casing eccentricity and cement azimuthal density.This approach ensures the stability of the inversion process while simultaneously achieving an accuracy of 0.05 g/cm^(3) for the cement azimuthal density.This accuracy level is ten times higher compared to density accuracy calculated using calibration equations.Overall,this algorithm enhances the accuracy of cement azimuthal density evaluation,provides valuable technical support for the monitoring of cement azimuthal density in the oil and gas industry.
基金This research was funded by the Shandong Provincial Natural Science Foundation(grant number ZR202102240088).
文摘Population density functions have long been used to describe the spatial structure of regional population distributions.Several studies have been conducted to examine the population distribution in Shandong Province,China,but few have applied regional density functions to the analysis.Therefore,based on the 2000,2010,and 2020 population censuses,this study used monocentric and polycentric regional density functions to study the characteristics of population agglomeration and diffusion in Shandong.This is followed by an in-depth discussion based on population growth rate data and hot-and cold-spot analyses.The results showed that the Shandong Province population was spatially unevenly distributed.Population growth rates were higher in urban centers and counties,with more significant changes in population size in the eastern coastal areas than in the inland areas.As verified in this study,the logarithmic form of the single-center regional density function R2 was greater than 0.8,which was in line with the population spatial structure of Shandong Province.During the study period,the estimated population density of the regional center and the absolute value of the regional population density gradient both increased,indicating a clear and increasing trend of centripetal agglomeration of regional centers over the study period.Overall,the R2 value of the multicenter region density function was higher than that of the single-center region density function.The polycentric regional density function showed that the population density gradient of some centers had a downward trend,which reflected the spatial development trend of outward diffusion in these centers.Meanwhile,the variation in the estimated population density and the population density gradient exhibited differences in the central population distribution patterns at different levels.
文摘The wave/particle duality of particles in Physics is well known. Particles have properties that uniquely characterize them from one another, such as mass, charge and spin. Charged particles have associated Electric and Magnetic fields. Also, every moving particle has a De Broglie wavelength determined by its mass and velocity. This paper shows that all of these properties of a particle can be derived from a single wave function equation for that particle. Wave functions for the Electron and the Positron are presented and principles are provided that can be used to calculate the wave functions of all the fundamental particles in Physics. Fundamental particles such as electrons and positrons are considered to be point particles in the Standard Model of Physics and are not considered to have a structure. This paper demonstrates that they do indeed have structure and that this structure extends into the space around the particle’s center (in fact, they have infinite extent), but with rapidly diminishing energy density with the distance from that center. The particles are formed from Electromagnetic standing waves, which are stable solutions to the Schrödinger and Classical wave equations. This stable structure therefore accounts for both the wave and particle nature of these particles. In fact, all of their properties such as mass, spin and electric charge, can be accounted for from this structure. These particle properties appear to originate from a single point at the center of the wave function structure, in the same sort of way that the Shell theorem of gravity causes the gravity of a body to appear to all originate from a central point. This paper represents the first two fully characterized fundamental particles, with a complete description of their structure and properties, built up from the underlying Electromagnetic waves that comprise these and all fundamental particles.
基金Project(50604016)supported by the National Natural Science Foundation of ChinaProject(2007B52)supported by the Foundation for the Author of National Excellent Doctoral Dissertation of China+3 种基金Project(NCET-08-0568)supported by the Program for New Century Excellent Talents in Chinese UniversityProject(2007CB613602)supported by the National Basic Research Program of ChinaProject(2007AA06Z122)supported by the National High-tech Research and Development Program of ChinaProject(2007BAB22B01)supported by the National Science and Technology Support Project of China
文摘Using density functional methods,some properties were studied such as the energies and compositions of frontier molecular orbitals and the atomic charges,which are related to the reactive behavior of thioureas containing different N-substituent groupings.The calculation results indicate that the N-substituent groupings have significant effect on the flotation performance of thiourea collectors.The order of electron-donating ability is N-propyl-N'-benzyl-thiourea(PBZYTU)>N-propyl-N'-ethyl-thiourea (PETU)>N-propyl-N'-allyl-thiourea(PALTU)>>N-propyl-N'-acetyl-thiourea(PACTU)>N-propyl-N'-ethoxycarbonyl-thiourea (PECTU)>N-propyl-N'-benzoyl-thiourea(PBZOYTU),and the order of feedback-electron-accepting ability is PBZOYTU> PACTU>PECTU>>PALTU>PETU>PBZYTU.This implies that PBZOYTU,PACTU or PECTU can react with copper atoms having(t2g) 6 (eg) 3Cu(II)or t 6e 4Cu(I)configuration on the surfaces of copper sulfide minerals through normal covalent bond and back donation covalent bond,and exhibit excellently collecting performance for copper sulfide minerals.These are consistent with the experimental data reported in the literatures.
