Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is ...Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is still challenging.Herein,we present a facile ion exchange and phosphating processes to transform intestine-like CoNiP_(x)@P,N-C into lotus pod-like CoNiFeP_(x)@P,N-C heterostructure in which numerous P,N-codoped carboncoated CoNiFeP_(x)nanoparticles tightly anchors on the 2D carbon matrix.Meanwhile,the as-prepared CoNiFeP_(x)@P,N-C enables a core-shell structure,high specific surface area,and hierarchical pore structure,which present abundant heterointerfaces and fully exposed active sites.Notably,the incorporation of Fe can also induce electron transfer in CoNiP_(x)@P,IM-C,thereby promoting the oxygen evolution reaction.Consequently,CoNiFeP_(x)@P,IM-C delivers a low overpotential of 278 mV(vs RHE)at a current density of10 mA cm^(-1)and inherits excellent long-term stability with no observable current density decay after 30 h of chronoamperometry test.This work not only highlights heteroatom induction to tune the electronic structure but also provides a facile approach for developing advanced and stable oxygen evolution reaction electrocatalysts with abundant heterointerfaces.展开更多
Calculation of total energies of the electronic ground states of atoms forms the basis for the frozen-core pseudopotentials used in atomistic calculations of much larger scale. Reference values for these energies prov...Calculation of total energies of the electronic ground states of atoms forms the basis for the frozen-core pseudopotentials used in atomistic calculations of much larger scale. Reference values for these energies provide a benchmark for the validation of new software to calculate such potentials. In addition, basic atomic-scale electronic properties such as the (first) ionization energy provide a simple check on the approximation used in the calculation method. We present a comparison of the total energies and ionization energies of atoms Z = 1 - 92 calculated in density functional theory with several levels of exchange-correlation functional and the Hartree-Fock method, comparing ionization energies to experiment. We also investigate the role of relativistic treatment on these energies.展开更多
As more business is conduced over the Internet, the fair exchange problem assumes increasing importance. However, the problem of multi-party fair exchange has not been studied as widely as the more fundamental problem...As more business is conduced over the Internet, the fair exchange problem assumes increasing importance. However, the problem of multi-party fair exchange has not been studied as widely as the more fundamental problem of 2-party fair exchange. Recently, Franklin arid Tsudik proposed two protocols for n-party multi-item exchange on FC'98, SUCEX-1 and SUCES-2. This paper first gives an attack on the proposed protocol SUCEX-1, then presents two protocols for multi-item exchange, one is an improved protocol of SUCEX-1, another is the extension of protocol SUCEX-2.展开更多
The electronic structures and magnetic properties of SmCo7-xMx (M=Ti, Si, Zr, Hf, Cu, B, Ag, Ga, Mn) compounds are investigated by using a spin-polarized MS-Xα method. The results show that the long-range ferromagn...The electronic structures and magnetic properties of SmCo7-xMx (M=Ti, Si, Zr, Hf, Cu, B, Ag, Ga, Mn) compounds are investigated by using a spin-polarized MS-Xα method. The results show that the long-range ferromagnetic order is determined by a stronger 3d-5d interaction, rather than the traditional RKKY interaction, and the effects of doping element M on 3d-5d coupling are negligible in Sm-Co-based compounds. The nonmagnetic dopant Si atoms have a larger effect on the moments of 2e site although they preferably occupy the Co 3g sites, which results in the stronger uniaxial anisotropy of this compound. Analysis of the formation energies indicates that 5d-element doped compounds are more stable than other dopants, and furthermore, they have a higher Curie temperature above room temperature, which will be in favor of their potential application as high-temperature permanent magnets.展开更多
E-commerce protocols for the electronic purchase of goods are difficult to design and implement due to their complexity and high security demands. Fairness of such protocols in literature highly depends on an addition...E-commerce protocols for the electronic purchase of goods are difficult to design and implement due to their complexity and high security demands. Fairness of such protocols in literature highly depends on an additional TTP(trusted third party). However, it is difficult to find such a TTP in some situations. In addition, fairness for customers has been neither fully considered nor well satisfied in existing electronic purchasing protocols. In this paper, a new protocol FEP (fair electronic purchase) without a special TTP but an online bank is presented based on a concurrent digital signature scheme. The FEP protocol guarantees fair electronic purchase of goods via electronic payment between consumers, merchants and their online banks. The protocol is practical and the analysis based on the game logics shows that it achieves the properties of viability, fairness, and timeliness.展开更多
Self-consistent ab initio calculations, based on the density functional theory (DFT) and using the full potential linear augmented plane wave (FLAPW) method, are performed to investigate both electronic and magnet...Self-consistent ab initio calculations, based on the density functional theory (DFT) and using the full potential linear augmented plane wave (FLAPW) method, are performed to investigate both electronic and magnetic properties of the MnS layers. Polarized spin and spin-orbit coupling are included in the calculations within the framework of the antiferromagnetic state between two adjacent Mn layers. Magnetic moments considered to lie along axes are computed. Obtained data from ab initio calculations are used as input data for the high temperature series expansion (HTSE) calculations to compute other magnetic parameters. The zero-field high temperature static susceptibility series of the spin-4.39 nearest-neighbour Heisenberg model on centred face cubic (FCC) and lattices is thoroughly analysed by a power series coherent anomaly method (CAM). The exchange interactions between the magnetic atoms, the N@el temperature, and the critical exponent associated with the magnetic susceptibility are obtained for the MnS layer.展开更多
The spin-polarized MS-Xα method is employed to study the electronic structure and the magnetic property of the SmCo5 compound.According to the calculated results, the magnetic moment per Sm is 1.29μB in the SmCo5 co...The spin-polarized MS-Xα method is employed to study the electronic structure and the magnetic property of the SmCo5 compound.According to the calculated results, the magnetic moment per Sm is 1.29μB in the SmCo5 compound, which agrees with that of experiments.The analyzed result reveals that some negative exchange couplings occurring at six energy levels induce the distinct decrease of Curie temperature and the magnetic moment per Co.The valence electron numbers of 2.48, which are derived from the orbital hybridization from s, p, d and f functions between Sm and Co atoms, are transferred to Sm(5d0) orbital.Therefore, the exchange interactions between 3d ~ 5d electrons lead to the magnetic coupling between Sm and Co, which results in the long-range ferromagnetic-order inside the SmCo5 compound.展开更多
The variation of the three-dimensional(3D)structure of the membrane electrode of a fuel cell during proton exchange cycling involves the corrosion/compaction of the carbon support.The increasing degradation of the car...The variation of the three-dimensional(3D)structure of the membrane electrode of a fuel cell during proton exchange cycling involves the corrosion/compaction of the carbon support.The increasing degradation of the carbon structure continuously reduces the electrocatalytic performance of proton exchange membrane fuel cells(PEM-FCs).This phenomenon can be explained by performing 3D tomographic analysis at the nanoscale.However,conventional tomographic approaches which present limited experimental feasibility,cannot perform such evaluation and have not provided sufficient structural information with statistical significance thus far.Therefore,a reliable methodology is required for the 3D geometrical evaluation of the carbon structure.Here,we propose a segmented tomographic approach which employs pore network analysis that enables the visualization of the geometrical parameters corresponding to the porous carbon structure at a high resolution.This approach can be utilized to evaluate the 3D structural degradation of the porous carbon structure after cycling in terms of local surface area,pore size distribution,and their 3D networking.These geometrical parameters of the carbon body were demonstrated to be substantially reduced owing to the cycling-induced degradation.This information enables a deeper understanding of the degradation phenomenon of carbon supports and can contribute to the development of stable PEM-FC electrodes.展开更多
The rates of electron exchange between oxidized and reduced forms of sev- eral derivatives of ferrocene(1-3)have been measured in acetonitrile by the NMR line h(?)oadening method at 25℃。It was found that the r(?)tes...The rates of electron exchange between oxidized and reduced forms of sev- eral derivatives of ferrocene(1-3)have been measured in acetonitrile by the NMR line h(?)oadening method at 25℃。It was found that the r(?)tes vary with the lengtn of the substitutent chain and the potential of E_(Fe(Ⅲ)/Fe(Ⅱ))in the ferrocene derivatives.展开更多
Parametric instabilities induced by the nonlinear interaction between high frequency quantum Langmuir waves and low frequency quantum ion-acoustic waves in quantum plasmas with the electron exchange-correlation effect...Parametric instabilities induced by the nonlinear interaction between high frequency quantum Langmuir waves and low frequency quantum ion-acoustic waves in quantum plasmas with the electron exchange-correlation effects are presented.By using the quantum hydrodynamic equations with the electron exchange-correlation correction,we obtain an effective quantum Zaharov model,which is then used to derive the modified dispersion relations and the growth rates of the decay and four-wave instabilities.The influences of the electron exchange-correlation effects and the quantum effects on the existence of quantum Langmuir waves and the parametric instabilities are discussed in detail.It is shown that the electron exchange-correlation effects and quantum effects are strongly coupled.The quantum Langmuir wave can propagate in quantum plasmas only when the electron exchange-correlation effects and the quantum effects satisfy a certain condition.The electron exchange-correlation effects tend to enhance the parametric instabilities,while quantum effects suppress the instabilities.展开更多
Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of ...Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of the electronic structure of NiS_(x),which accelerates the dissociation of H2O and the adsorption of OH−in the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)processes,respectively.In addition,the magnetically active Mo-NiS_(x)/NF can further enhance the HER and OER activity under an applied magnetic field due to the magnetoresistance effect and the ferromagnetic(FM)exchange-field penetration effect.As a result,Mo-NiS_(x)/NF requires low overpotentials of 307 mV at 50mA cm^(−2)(for OER)and 136 mV at 10mA cm^(−2)(for HER)under a magnetic field of 10000 G.Furthermore,the electrolytic cell constructed by the bifunctional Mo-NiS_(x)/NFs as both the cathode and the anode shows a low cell voltage of 1.594 V at 10 mA cm^(−2)with optimal stability over 60 h under the magnetic field.Simultaneous enhancement of the HER and OER processes by an external magnetic field through rational design of electrocatalysts might be promising for overall water splitting applications.展开更多
The total absolute cross sections of single-and double-electron capture (SEC and DEC) in the collisions of He^(2+)with He and Ne^(8+)with O_(2),N_(2),and CH_(4) were studied in the energy ranges 3.5–50 keV/u and 2.8...The total absolute cross sections of single-and double-electron capture (SEC and DEC) in the collisions of He^(2+)with He and Ne^(8+)with O_(2),N_(2),and CH_(4) were studied in the energy ranges 3.5–50 keV/u and 2.8–40 keV/u,respectively.Through a deep analysis of the experimental systematic uncertainties in the measurement procedure and data evaluation,the error in the experimental results of the SEC cross sections is less than 9%.Within the uncertainties,the present results of the He^(2+)–He collision show good consistency with previous measurements,validating the experimental system and paving the way for precise measurements of EC cross sections for a variety of ions and neutral gases.The present measurements allow for a test of EC theory and provide crucial EC cross section data for the establishment of plasma models in fusion research and astrophysical X-ray studies.展开更多
基金supported by the National Natural Science Foundation of China(No.22269010)the Jiangxi Provincial Natural Science Foundation(No.20224BAB214021)+3 种基金the Training Program for Academic and Technical Leaders of Major Disciplines in Jiangxi Province(No.20212BCJ23020)the Science and Technology Project of Jiangxi Provincial Department of Education(No.GJJ211305)the Jingdezhen Science and Technology Planning Project(No.20212GYZD009-04)the Graduate Innovation Fund of Jiangxi Province(YC2022-s880)
文摘Transition metal phosphides with metallic properties are a promising candidate for electrocatalytic water oxidation,and developing highly active and stable metal phosphide-based oxygen evolution reaction catalysts is still challenging.Herein,we present a facile ion exchange and phosphating processes to transform intestine-like CoNiP_(x)@P,N-C into lotus pod-like CoNiFeP_(x)@P,N-C heterostructure in which numerous P,N-codoped carboncoated CoNiFeP_(x)nanoparticles tightly anchors on the 2D carbon matrix.Meanwhile,the as-prepared CoNiFeP_(x)@P,N-C enables a core-shell structure,high specific surface area,and hierarchical pore structure,which present abundant heterointerfaces and fully exposed active sites.Notably,the incorporation of Fe can also induce electron transfer in CoNiP_(x)@P,IM-C,thereby promoting the oxygen evolution reaction.Consequently,CoNiFeP_(x)@P,IM-C delivers a low overpotential of 278 mV(vs RHE)at a current density of10 mA cm^(-1)and inherits excellent long-term stability with no observable current density decay after 30 h of chronoamperometry test.This work not only highlights heteroatom induction to tune the electronic structure but also provides a facile approach for developing advanced and stable oxygen evolution reaction electrocatalysts with abundant heterointerfaces.
文摘Calculation of total energies of the electronic ground states of atoms forms the basis for the frozen-core pseudopotentials used in atomistic calculations of much larger scale. Reference values for these energies provide a benchmark for the validation of new software to calculate such potentials. In addition, basic atomic-scale electronic properties such as the (first) ionization energy provide a simple check on the approximation used in the calculation method. We present a comparison of the total energies and ionization energies of atoms Z = 1 - 92 calculated in density functional theory with several levels of exchange-correlation functional and the Hartree-Fock method, comparing ionization energies to experiment. We also investigate the role of relativistic treatment on these energies.
基金Supported by the National Natural Science Foundation of China(No.60173032,No.69973031)
文摘As more business is conduced over the Internet, the fair exchange problem assumes increasing importance. However, the problem of multi-party fair exchange has not been studied as widely as the more fundamental problem of 2-party fair exchange. Recently, Franklin arid Tsudik proposed two protocols for n-party multi-item exchange on FC'98, SUCEX-1 and SUCES-2. This paper first gives an attack on the proposed protocol SUCEX-1, then presents two protocols for multi-item exchange, one is an improved protocol of SUCEX-1, another is the extension of protocol SUCEX-2.
基金Project supported by the National Natural Science Foundation of China (Grant Nos 10847134 and 60471042)the Natural Science Foundation of Shandong Province, China (Grant No Y2005A05)
文摘The electronic structures and magnetic properties of SmCo7-xMx (M=Ti, Si, Zr, Hf, Cu, B, Ag, Ga, Mn) compounds are investigated by using a spin-polarized MS-Xα method. The results show that the long-range ferromagnetic order is determined by a stronger 3d-5d interaction, rather than the traditional RKKY interaction, and the effects of doping element M on 3d-5d coupling are negligible in Sm-Co-based compounds. The nonmagnetic dopant Si atoms have a larger effect on the moments of 2e site although they preferably occupy the Co 3g sites, which results in the stronger uniaxial anisotropy of this compound. Analysis of the formation energies indicates that 5d-element doped compounds are more stable than other dopants, and furthermore, they have a higher Curie temperature above room temperature, which will be in favor of their potential application as high-temperature permanent magnets.
基金the National High Technology Research and Development Program of China (2007AA01Z471)
文摘E-commerce protocols for the electronic purchase of goods are difficult to design and implement due to their complexity and high security demands. Fairness of such protocols in literature highly depends on an additional TTP(trusted third party). However, it is difficult to find such a TTP in some situations. In addition, fairness for customers has been neither fully considered nor well satisfied in existing electronic purchasing protocols. In this paper, a new protocol FEP (fair electronic purchase) without a special TTP but an online bank is presented based on a concurrent digital signature scheme. The FEP protocol guarantees fair electronic purchase of goods via electronic payment between consumers, merchants and their online banks. The protocol is practical and the analysis based on the game logics shows that it achieves the properties of viability, fairness, and timeliness.
文摘Self-consistent ab initio calculations, based on the density functional theory (DFT) and using the full potential linear augmented plane wave (FLAPW) method, are performed to investigate both electronic and magnetic properties of the MnS layers. Polarized spin and spin-orbit coupling are included in the calculations within the framework of the antiferromagnetic state between two adjacent Mn layers. Magnetic moments considered to lie along axes are computed. Obtained data from ab initio calculations are used as input data for the high temperature series expansion (HTSE) calculations to compute other magnetic parameters. The zero-field high temperature static susceptibility series of the spin-4.39 nearest-neighbour Heisenberg model on centred face cubic (FCC) and lattices is thoroughly analysed by a power series coherent anomaly method (CAM). The exchange interactions between the magnetic atoms, the N@el temperature, and the critical exponent associated with the magnetic susceptibility are obtained for the MnS layer.
基金Project supported by the National High Technology Research and Development Program of China( 2002AA324050 ), and Natural Science Foundation of Shandong (Y2002D9)
文摘The spin-polarized MS-Xα method is employed to study the electronic structure and the magnetic property of the SmCo5 compound.According to the calculated results, the magnetic moment per Sm is 1.29μB in the SmCo5 compound, which agrees with that of experiments.The analyzed result reveals that some negative exchange couplings occurring at six energy levels induce the distinct decrease of Curie temperature and the magnetic moment per Co.The valence electron numbers of 2.48, which are derived from the orbital hybridization from s, p, d and f functions between Sm and Co atoms, are transferred to Sm(5d0) orbital.Therefore, the exchange interactions between 3d ~ 5d electrons lead to the magnetic coupling between Sm and Co, which results in the long-range ferromagnetic-order inside the SmCo5 compound.
基金supported by the Technology Innovation Program(No.20011712)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by Advanced Facility Center for Quantum Technology in SKKUthe National R&D Program through the National Research Foundation of Koera(NRF)funded by Ministry of Science and ICT(No.2020M3F3A2A01082618)。
文摘The variation of the three-dimensional(3D)structure of the membrane electrode of a fuel cell during proton exchange cycling involves the corrosion/compaction of the carbon support.The increasing degradation of the carbon structure continuously reduces the electrocatalytic performance of proton exchange membrane fuel cells(PEM-FCs).This phenomenon can be explained by performing 3D tomographic analysis at the nanoscale.However,conventional tomographic approaches which present limited experimental feasibility,cannot perform such evaluation and have not provided sufficient structural information with statistical significance thus far.Therefore,a reliable methodology is required for the 3D geometrical evaluation of the carbon structure.Here,we propose a segmented tomographic approach which employs pore network analysis that enables the visualization of the geometrical parameters corresponding to the porous carbon structure at a high resolution.This approach can be utilized to evaluate the 3D structural degradation of the porous carbon structure after cycling in terms of local surface area,pore size distribution,and their 3D networking.These geometrical parameters of the carbon body were demonstrated to be substantially reduced owing to the cycling-induced degradation.This information enables a deeper understanding of the degradation phenomenon of carbon supports and can contribute to the development of stable PEM-FC electrodes.
文摘The rates of electron exchange between oxidized and reduced forms of sev- eral derivatives of ferrocene(1-3)have been measured in acetonitrile by the NMR line h(?)oadening method at 25℃。It was found that the r(?)tes vary with the lengtn of the substitutent chain and the potential of E_(Fe(Ⅲ)/Fe(Ⅱ))in the ferrocene derivatives.
基金Project supported by the National Natural Science Foundation of China (Grant No. 10975114)the Foundation for the Creation of Science and Technology of the Northwest Normal University of China (Grant No. NWNU-KJCXGC-03-48)
文摘Parametric instabilities induced by the nonlinear interaction between high frequency quantum Langmuir waves and low frequency quantum ion-acoustic waves in quantum plasmas with the electron exchange-correlation effects are presented.By using the quantum hydrodynamic equations with the electron exchange-correlation correction,we obtain an effective quantum Zaharov model,which is then used to derive the modified dispersion relations and the growth rates of the decay and four-wave instabilities.The influences of the electron exchange-correlation effects and the quantum effects on the existence of quantum Langmuir waves and the parametric instabilities are discussed in detail.It is shown that the electron exchange-correlation effects and quantum effects are strongly coupled.The quantum Langmuir wave can propagate in quantum plasmas only when the electron exchange-correlation effects and the quantum effects satisfy a certain condition.The electron exchange-correlation effects tend to enhance the parametric instabilities,while quantum effects suppress the instabilities.
基金National Natural Science Foundation of China,Grant/Award Numbers:21871065,22071038Heilongjiang Touyan Team,Grant/Award Number:HITTY‐20190033Interdisciplinary Research Foundation of HIT,Grant/Award Number:IR2021205。
文摘Herein,we report bifunctional molybdenum-doped nickel sulfide on nickel foam(Mo-NiS_(x)/NF)for magnetic field-enhanced overall water splitting under alkaline conditions.Proper doping of Mo can lead to optimization of the electronic structure of NiS_(x),which accelerates the dissociation of H2O and the adsorption of OH−in the hydrogen evolution reaction(HER)and the oxygen evolution reaction(OER)processes,respectively.In addition,the magnetically active Mo-NiS_(x)/NF can further enhance the HER and OER activity under an applied magnetic field due to the magnetoresistance effect and the ferromagnetic(FM)exchange-field penetration effect.As a result,Mo-NiS_(x)/NF requires low overpotentials of 307 mV at 50mA cm^(−2)(for OER)and 136 mV at 10mA cm^(−2)(for HER)under a magnetic field of 10000 G.Furthermore,the electrolytic cell constructed by the bifunctional Mo-NiS_(x)/NFs as both the cathode and the anode shows a low cell voltage of 1.594 V at 10 mA cm^(−2)with optimal stability over 60 h under the magnetic field.Simultaneous enhancement of the HER and OER processes by an external magnetic field through rational design of electrocatalysts might be promising for overall water splitting applications.
基金supported by the National Key R&D Program of China (No. 2022YFA1602504)the National Natural Science Foundation of China (Nos. 12204110 and U1832201)Shanghai Leading Academic Discipline Project (Project No. B107)。
文摘The total absolute cross sections of single-and double-electron capture (SEC and DEC) in the collisions of He^(2+)with He and Ne^(8+)with O_(2),N_(2),and CH_(4) were studied in the energy ranges 3.5–50 keV/u and 2.8–40 keV/u,respectively.Through a deep analysis of the experimental systematic uncertainties in the measurement procedure and data evaluation,the error in the experimental results of the SEC cross sections is less than 9%.Within the uncertainties,the present results of the He^(2+)–He collision show good consistency with previous measurements,validating the experimental system and paving the way for precise measurements of EC cross sections for a variety of ions and neutral gases.The present measurements allow for a test of EC theory and provide crucial EC cross section data for the establishment of plasma models in fusion research and astrophysical X-ray studies.