Magnets exhibiting the Kitaev interaction,a bond-dependent magnetic interaction in honeycomb lattices,are generally regarded as promising candidates for hosting novel phenomena like quantum spin liquid states.However,...Magnets exhibiting the Kitaev interaction,a bond-dependent magnetic interaction in honeycomb lattices,are generally regarded as promising candidates for hosting novel phenomena like quantum spin liquid states.However,realizing such magnets remains a significant challenge.Recently,some studies have suggested honeycomb magnets A_(3)Ni_(2)XO_(6)(A=Li,Na;X=Bi,Sb)with a high spin S=1 could serve as potential candidates for realizing strong Kitaev interactions.In this work,we systematically investigate their magnetic properties,with a particular emphasis on their Kitaev interactions,using first-principles calculations and Monte Carlo simulations.Our results indicate that all A_(3)Ni_(2)XO_(6)compounds are zigzag antiferromagnets,and their magnetic moments almost tend to be out of plane.We find that their dominant magnetic interactions are the nearest-neighbor ferromagnetic and third-nearest-neighbor antiferromagnetic Heisenberg interactions,while their Kitaev interactions are extremely weak.By analyzing their electronic structures and the mechanism of generating their magnetic interactions,we reveal that either artificially tuning spin-orbit coupling or applying strain cannot produce sufficient spin-orbit entangled states to realize the intriguing Kitaev interactions.Our work advances the understanding of the magnetism in A_(3)Ni_(2)XO_(6)compounds and provides insights for further exploration of Kitaev physics in honeycomb magnets.展开更多
We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atom...We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.Key words:C-lignin;adsorption;We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.展开更多
By adopting stochastic density functional theory(SDFT)and mixed stochastic-deterministic density functional theory(MDFT)methods,we perform first-principles calculations to predict the shock Hugoniot curves of boron(pr...By adopting stochastic density functional theory(SDFT)and mixed stochastic-deterministic density functional theory(MDFT)methods,we perform first-principles calculations to predict the shock Hugoniot curves of boron(pressure P=7.9×10^(3)-1.6×10^(6) GPa and temperature T=25-2800 eV),silicon(P=2.6×10^(3)-7.9×10^(5) GPa and T=21.5-1393 eV),and aluminum(P=5.2×10^(3)-9.0×10^(5) GPa and T=25-1393 eV)over wide ranges of pressure and temperature.In particular,we systematically investigate the impact of different cutoff radii in norm-conserving pseudopotentials on the calculated properties at elevated temperatures,such as pressure,ionization energy,and equation of state.By comparing the SDFT and MDFT results with those of other first-principles methods,such as extended first-principles molecular dynamics and path integral Monte Carlo methods,we find that the SDFT and MDFT methods show satisfactory precision,which advances our understanding of first-principles methods when applied to studies of matter at extremely high pressures and temperatures.展开更多
The structural, electronic and elastic properties of common intermetallic compounds in FeTiCoNiVCrMnCuAI system high entropy alloy were investigated by the first principles calculation. The calculation results of form...The structural, electronic and elastic properties of common intermetallic compounds in FeTiCoNiVCrMnCuAI system high entropy alloy were investigated by the first principles calculation. The calculation results of formation enthalpy and cohesive energy show that FeTi, Fe2Ti, AlCrFe2, Co2Ti, AlMn2V and Mn2Ti phases may form in the formation process of the alloy. Further studies show that FeTi, FezTi, AlCrFe2, Co2Ti and AlMn2V phases with higher shear modulus and elastic modulus would be excellent strengthening phases in high entropy alloy and would improve the hardness of the alloy. In addition, the partial density of states was investigated for revealing the bonding mode, and the analyses on the strength of p-d hybridization also reveal the underlying mechanism for the elastic properties of these compounds.展开更多
Low dimensional materials are suitable candidates applying in next-generation high-performance electronic,optoelectronic,and energy storage devices because of their uniquely physical and chemical properties.In particu...Low dimensional materials are suitable candidates applying in next-generation high-performance electronic,optoelectronic,and energy storage devices because of their uniquely physical and chemical properties.In particular,one-dimensional(1D)atomic wires(AWs)exfoliating from 1D van der Waals(vdW)bulks are more promising in next generation nanometer(nm)even sub-nm device applications owing to their width of few-atoms scale and free dandling bonds states.Although several 1D AWs have been experimentally prepared,few 1D AW candidates could be practically applied in devices owing to lack of enough suitable 1D AWs.Herein,367 kinds of 1D AWs have been screened and the corresponding computational database including structures,electronic structures,magnetic states,and stabilities of these 1D AWs has been organized and established.Among these systems,unary and binary 1D AWs with relatively small exfoliation energy are thermodynamically stable and theoretically feasible to be exfoliated.More significantly,rich quantum states emerge,such as 1D semiconductors,1D metals,1D semimetals,and 1D magnetism.This database will offer an ideal platform to further explore exotic quantum states and exploit practical device applications using 1D materials.The database are openly available at http://www.dx.doi.org/10.11922/sciencedb.j00113.00004.展开更多
Sulfide nanocrystals and their composites have shown great potential in the thermoelectric(TE)field due to their extremely low thermal conductivity.Recently a solid and hollow metastable Au2S nanocrystalline has been ...Sulfide nanocrystals and their composites have shown great potential in the thermoelectric(TE)field due to their extremely low thermal conductivity.Recently a solid and hollow metastable Au2S nanocrystalline has been successfully synthesized.Herein,we study the TE properties of this bulk Au2S by first-principles calculations and semiclassical Boltzmann transport theory,which provides the basis for its further experimental studies.Our results indicate that the highly twofold degeneracy of the bands appears at theΓpoint in the Brillouin zone,resulting in a high Seebeck coefficient.Besides,Au2S exhibits an ultra-low lattice thermal conductivity(~0.88 W·m^-1·K^-1 at 700 K).At 700 K,the thermoelectric figure of merit of the optimal p-type doping is close to 1.76,which is higher than 0.8 of ZrSb at 700 K and 1.4 of PtTe at 750 K.Our work clearly demonstrates the advantages of Au2S as a TE material and would greatly inspire further experimental studies and verifications.展开更多
Hydrogen incorporation is critical for explaining defect energies, structure parameters and other physical characteristics of minerals and understanding mantle dynamics. This work analyzed the hydrogen complex defects...Hydrogen incorporation is critical for explaining defect energies, structure parameters and other physical characteristics of minerals and understanding mantle dynamics. This work analyzed the hydrogen complex defects in jadeite by the plane-wave pseudo-potential method based on density functional theory, and optimized the atomic positions and lattice constants in all configurations （different defective systems）. Incorporation mechanisms considered for hydrogen （H） in jadeite include： （1） hydrogen incorporating with the 02 site oxygen and coexisting with M2 vacancy; （2） one H atom combined with an AI atom replacing Si in tetrahedron; （3） 4H atoms directly replacing Si in tetrahedron and （4） 3H atoms replacing Al on the M1 site. The four incorporation mechanisms mentioned above form the corresponding VNa-Hi, Alsi-Hi, Vsi-4Hi and VAr3Hi point defects. The molecular dynamics simulation to the ideal, VNa-Hi, Alsi-Hi, Vsi-4Hi and VAr3Hi point defects under the P-T conditions of 900 K, 2 GPa, the Vsa-Hi and Alsi-Hi point defects under different pressures at T = 900 K, and Alsj-Hj point defects under different temperatures at P = 3 GPa was performed to examine the preferential mode of hydrogen incorporation in jadeite by means of first-principles calculations. The calculations show that the averaged O-H bond-length in the hydrogen point defects system decreased in the order of Alsi-Hi, VNa-HI, Vsl-4Hf and VAI-3Hi. VNa-HI complex defects result in a contraction of the jadeite volume and the presence of Alsi-Hi, Vsi-4H~ and VAI-3Hi defects could increase the superceli volume, which is the most obvious in the VAt-3Hi defects. The energy of formation of Also-HI and VA[-3HI complex defects was much lower than that of other defect systems. The VAI-3Hi defects system has the lowest energy and the shortest O-H bond-length, suggesting that this system is the most favorable. The analytical results of vacancy formation energy, O-H bond- length, and the stability of the hydrogen defects in jadeite have suggested that the preferred hydration incorporation mode in jadeite is VAI-3Hi complex defect.展开更多
Graphene is an ideal reinforcing phase for a high-performance composite filler,which is of great theoretical and practical significance for improving the wettability and reliability of the filler.However,the poor adso...Graphene is an ideal reinforcing phase for a high-performance composite filler,which is of great theoretical and practical significance for improving the wettability and reliability of the filler.However,the poor adsorption characteristics between graphene and the silver base filler significantly affect the application of graphene filler in the brazing field.It is a great challenge to improve the adsorption characteristics between a graphene and silver base filler.To solve this issue,the adsorption characteristic between graphene and silver was studied with first principle calculation.The effects of Ga,Mo,and W on the adsorption properties of graphene were explored.There are three possible adsorbed sites,the hollow site(H),the bridge site(B),and the top site(T).Based on this research,the top site is the most preferentially adsorbed site for Ag atoms,and there is a strong interaction between graphene and Ag atoms.Metal element doping enhances local hybridization between C or metal atoms and Ag.Furthermore,compared with other doped structures(Ga and Mo),W atom doping is the most stable adsorption structure and can also improve effective adsorption characteristic performance between graphene and Ag.展开更多
One way of improving the magnetic properties of RECo5(RE = rare earth) compounds, especially the magnetic anisotropy energy (MAE), is to dope them with some additives such as Fe, Ni, Cu. Those dopants bring changes in...One way of improving the magnetic properties of RECo5(RE = rare earth) compounds, especially the magnetic anisotropy energy (MAE), is to dope them with some additives such as Fe, Ni, Cu. Those dopants bring changes in both lattice geometry and magnetic properties of the compounds. In this paper, the effects of doping on YCo5-x,Fex and YCo5-x Agx were studied in two simple but effective ways: first, the geometric effect induced by doping and then, the pure doping role namely without any geometric changes. The calculated results indicate that the magnetic moments of Co show a transition from a high spin state to a low one with the change of the volume of the cell in all YCo5, YCo3Fe2 and YCo3Ag2 alloys. The change of c/a ratio with constant lattice parameter a also influences drastically the magnetic moments and the MAE. As the geometric structure is not changed, it is found that the doping effects of magnetic element Fe and non-magnetic element Ag are quite different.展开更多
The electronic structures,chemical bonding,elastic and optical properties of the novel hP24 phase WB3 were investigated by using density-functional theory(DFT) within generalized gradient approximation(GGA).The calcul...The electronic structures,chemical bonding,elastic and optical properties of the novel hP24 phase WB3 were investigated by using density-functional theory(DFT) within generalized gradient approximation(GGA).The calculated energy band structures show that the hP24 phase WB3 is metallic material.The density of state(DOS) and the partial density of state(PDOS) calculations show that the DOS near the Fermi level is mainly from the W 5d and B 2p states.Population analysis suggests that the chemical bonding in hP24-WB3 has predominantly covalent characteristics with mixed covalent-ionic characteristics.Basic physical properties,such as lattice constant,bulk modulus,shear modulus and elastic constants Cij were calculated.The elastic modulus E and Poisson ratio υ were also predicted.The results show that hP24-WB3 phase is mechanically stable and behaves in a brittle manner.Detailed analysis of all optical functions reveals that WB3 is a better dielectric material,and reflectivity spectra show that WB3 can be promised as good coating material in the energy regions of 8.5-11.4 eV and 14.5-15.5 eV.展开更多
The structural, anisotropic elastic properties and the ideal compressive and tensile strengths of titanium diboride (TiB_(2)) were investigated using first-principles calculations based on density functional theory. T...The structural, anisotropic elastic properties and the ideal compressive and tensile strengths of titanium diboride (TiB_(2)) were investigated using first-principles calculations based on density functional theory. The stress-strain relationships of TiB2 under 〈10i0〉, 〈12i0〉, and 〈0001〉 compressive loads were calculated. Our results showed that the ideal uniaxial compressive strengths are |σ〈02i0〉)| = 142.96 GPa, |σ〈0001〉 ] = 188.75 GPa, and |σ〈10i0〉| = 245.33 GPa, at strains -0.16, -0.32, and -0.24, respectively. The variational trend is just the opposite to that of the ideal tensile strength with σ〈10i0〉 = 44.13 GPa, σ〈0001〉 = 47.03 GPa, and σ〈i2i0〉 = 56.09 GPa, at strains 0.14, 0.28, and 0.22, respectively. Furthermore, it was found that TiB2 is much stronger under compression than in tension. The ratios of the ideal compressive to tensile strengths are 5.56, 2.55, and 4.01 for crystallographic directions (10i0), 〈12i0〉, and 〈0001〉, respectively. The present results are in excellent agreement with the most recent experimental data and should be helpful to the understanding of the compressive property of TiB2.展开更多
The global greenhouse effect makes it urgent to deal with the increasing greenhouse gases. In this paper the performance of MgO-decorated carbon nanotubes for CO2 adsorption is investigated through first principles ca...The global greenhouse effect makes it urgent to deal with the increasing greenhouse gases. In this paper the performance of MgO-decorated carbon nanotubes for CO2 adsorption is investigated through first principles calculations. The results show that the MgO-decorated carbon nanotubes can adsorb CO2 well and are relatively insensitive to O2 and N2 at the same time. The binding energy arrives at 1.18 eV for the single-MgO-decorated carbon nanotube adsorbing one CO2 molecule, while the corresponding values for O2 and N2 are 0.55 eV and 0.06 eV, respectively. In addition, multi-molecule adsorption is also proved to be very satisfactory. These results indicate that MgO-decorated carbon nanotubes have great potential applications in industrial and environmental processes.展开更多
In this study the pseudo-potential method is used to investigate the structural, electronic, and thermodynamic proper- ties of ZnOl_xSx semiconductor materials. The results show that the electronic properties are foun...In this study the pseudo-potential method is used to investigate the structural, electronic, and thermodynamic proper- ties of ZnOl_xSx semiconductor materials. The results show that the electronic properties are found to be improved when calculated by using LDA ~ U functional as compared with local density approximation （LDA）. At various concentrations the ground-state properties are determined for bulk materials ZnO, ZnS, and their tertiary alloys in cubic zinc-blende phase. From the results, a minor difference is observed between the lattice parameters from Vegard＇s law and other calculated results, which may be due to the large mismatch between lattice parameters of binary compounds ZnO and ZnS. A small deviation in the bulk modulus from linear concentration dependence is also observed for each of these alloys. The ther- modynamic properties, including the phonon contribution to Helmholtz free energy △F, phonon contribution to internal energy △E, and specific iheat at constant-volume Cv, are calculated within quasi-harmonic approximation based on the calculated phonon dispersion relations.展开更多
We report a study of the electronic structure and optical properties of uranium dioxide （U02） based on the ab-initio density-functional theory and using the generalized gradient approximation. To correctly describe ...We report a study of the electronic structure and optical properties of uranium dioxide （U02） based on the ab-initio density-functional theory and using the generalized gradient approximation. To correctly describe the strong correlation between 5 f electrons of a uranium atom, we employ the on-site Hubbard U correction term and optimize the correlation parameter of the bulk uranium dioxide. Then we give the structural and electronic properties of the ground state of uranium dioxide. Based on the accurate electronic structure, we calculate the complex dielectric function of UO2 and the related optieM properties, such as reflectivity, refractive index, extinction index, energy loss spectra, and absorption coefficient.展开更多
The structural, magnetic and electronic properties of the double perovskite Ba2SmNbO6 （for the simple cubic structure where no octahedral tilting exists anymore） are studied using the density functional theory withi...The structural, magnetic and electronic properties of the double perovskite Ba2SmNbO6 （for the simple cubic structure where no octahedral tilting exists anymore） are studied using the density functional theory within the generalized gradient approximation as well as taking into account the on-site Coulomb repulsive interaction. The total energy, the spin magnetic moment, the band structure and the density of states are calculated. The optimization of the lattice constants is 8.5173 A, which is in good agreement with the experimental value 8.5180 A. The calculations reveal that Ba2SmNbO6 has a stable ferromagnetic ground state and the spin magnetic moment per molecule is 5.00μB/f.u. which comes mostly from the Sin3＋ ion only. By analysis of the band structure, the compound exhibits the direct band gap material and half-metallic ferromagnetic nature with 100% spin-up polarization, which implies potential applications of this new lanthanide compound in magneto-electronic and spintronic devices.展开更多
Calorimetric measurements are performed to determine the specific heat of Si-xat.% Ge(where x = 0, 10, 30,50, 70, 90 and 100) alloys within a broad temperature range from 123 to 823 K. The measured specific heat incre...Calorimetric measurements are performed to determine the specific heat of Si-xat.% Ge(where x = 0, 10, 30,50, 70, 90 and 100) alloys within a broad temperature range from 123 to 823 K. The measured specific heat increases dramatically at low temperatures, and the composition dependence of specific heat is evaluated from the experimental results. Meanwhile, the specific heat at constant volume, the thermal expansion, and the bulk modulus of Si and Ge are investigated by the first principle calculations combined with the quasiharmonic approximation. The negative thermal expansion is observed for both Si and Ge. Furthermore, the isobaric specific heat of Si and Ge is calculated correspondingly from OK to their melting points, which is verified by the measured results and accounts for the temperature dependence in a still boarder range.展开更多
In order to have a better understanding of the electronic structures and physical properties of Cu<sub>2-<span style="white-space:nowrap;"><em>δ</em></span></sub>X (X = S...In order to have a better understanding of the electronic structures and physical properties of Cu<sub>2-<span style="white-space:nowrap;"><em>δ</em></span></sub>X (X = Se, S, Te) copper chalcogenides. First principles were performed to calculate the chemical shift, band structure, and electron density of states of Cu<span style="white-space:nowrap;"><sub>2-<em>δ</em></sub></span>X (X = Se, S, Te). By comparing our calculation results with previous experimental works, we found that the predicted electronic structures of Cu<sub>2</sub>Se, Cu<sub>2</sub>Te and Cu<sub>2</sub>S transform from semimetal to semiconductor after adding on-site Coulomb U, which reflects the real properties of the materials. By using (Density Functional Theory) DFT + U method, the calculation result is close to the real electronic structure. The calculation result of chemical shift of adding U does not reach the ideal expectation, and the reason is not clear at present. In this paper, the theoretical electronic structures of Cu<sub>2</sub>Se, Cu<sub>2</sub>Te and Cu<sub>2</sub>S are better calculated by DFT + U method and compared with the actual properties. The effect of Cu-s electron on the chemical shift is understood, and a theoretical result of the chemical shift is calculated, which provides a powerful reference for the subsequent research and understanding of the electronic structure and physical properties of the compounds with S groups of Cu.展开更多
The plane wave pseudo-potential method was used to investigate the structural, electronic, and elastic properties of Cd Se_（1-x）Te_x in the zinc blende phase. It is observed that the electronic properties are improv...The plane wave pseudo-potential method was used to investigate the structural, electronic, and elastic properties of Cd Se_（1-x）Te_x in the zinc blende phase. It is observed that the electronic properties are improved considerably by using LDA ＋ U as compared to the LDA approach. The calculated lattice constants and bulk moduli are also comparable to the experimental results. The cohesive energies for pure Cd Se and Cd Te binary and their mixed alloys are calculated. The second-order elastic constants are also calculated by the Lagrangian theory of elasticity. The elastic properties show that the studied material has a ductile nature.展开更多
Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-depo...Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.展开更多
Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),Cr...Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),CrS_(2)with one S vacancy(v-CrS_(2)), and Ti doped CrS_(2)(Ti@CrS_(2)). The results have shown that the pristine CrS_(2)exhibits inert character for NO activation. However, v-CrS_(2)and Ti@CrS_(2)can exhibit enhanced interaction with NO, due to increased charge transfer between NO and substrates(0.52–0.75 e) and enhanced adsorption energies of NO on the catalysts(-0.96~-1.64 e V), compared to the situation of CrS_(2)(0.065 e/-0.30 e V). From the free energy profiles of NO electro-reduction to NH3, we can see that the v-CrS_(2)and Ti@CrS_(2)all exhibit ultralow limiting potentials of-0.03~-0.47 V, following both*NOH and*NHO mechanisms. Therefore, introducing vacancy and doping are all promising modification strategies for NORR catalysts. The results have provided a new idea for the search of catalysts for efficient electrocatalytic reduction of NO.展开更多
基金supported by the National Key R&D Program of China(Grant Nos.2024-YFA1408303 and 2022YFA1403301)the National Natural Sciences Foundation of China(Grant Nos.12474247 and 92165204)+1 种基金support from Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices(Grant No.2022B1212010008)Research Center for Magnetoelectric Physicsof Guangdong Province(Grant No.2024B0303390001).
文摘Magnets exhibiting the Kitaev interaction,a bond-dependent magnetic interaction in honeycomb lattices,are generally regarded as promising candidates for hosting novel phenomena like quantum spin liquid states.However,realizing such magnets remains a significant challenge.Recently,some studies have suggested honeycomb magnets A_(3)Ni_(2)XO_(6)(A=Li,Na;X=Bi,Sb)with a high spin S=1 could serve as potential candidates for realizing strong Kitaev interactions.In this work,we systematically investigate their magnetic properties,with a particular emphasis on their Kitaev interactions,using first-principles calculations and Monte Carlo simulations.Our results indicate that all A_(3)Ni_(2)XO_(6)compounds are zigzag antiferromagnets,and their magnetic moments almost tend to be out of plane.We find that their dominant magnetic interactions are the nearest-neighbor ferromagnetic and third-nearest-neighbor antiferromagnetic Heisenberg interactions,while their Kitaev interactions are extremely weak.By analyzing their electronic structures and the mechanism of generating their magnetic interactions,we reveal that either artificially tuning spin-orbit coupling or applying strain cannot produce sufficient spin-orbit entangled states to realize the intriguing Kitaev interactions.Our work advances the understanding of the magnetism in A_(3)Ni_(2)XO_(6)compounds and provides insights for further exploration of Kitaev physics in honeycomb magnets.
基金Funded by the Hubei Province Key Research Foundation for Water Resources,China(No.HBSLKY2023035)the National College Students’Innovation and Entrepreneurship Training Program,China(No.202310500012)the Wuhan Talents Outstanding Young Talents Program。
文摘We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.Key words:C-lignin;adsorption;We investigated the adsorption mechanisms including physical and chemical adsorption for heavy metals(Cd,Pb,Zn,Co,Cu)on C-lignin using density functional theory(DFT)simulations.Physical adsorption,involving metal atoms near carbon atoms,is found to be endothermic;meanwhile,chemical adsorption,where hydroxyl groups replace metal ions,is exothermic and spontaneous.Pb exhibits the highest physical adsorption potential,while Cu and Co demonstrate the strongest chemical adsorption due to their highly negative adsorption energies.These findings provide valuable insights into the design of eco-friendly nano lignocellulosic composite films for effective heavy metal removal from contaminated water sources.
基金supported by the National Key R&D Program of China under Grant No.2025YFB3003603the National Natural Science Foundation of China under Grant Nos.12135002 and 12105209.
文摘By adopting stochastic density functional theory(SDFT)and mixed stochastic-deterministic density functional theory(MDFT)methods,we perform first-principles calculations to predict the shock Hugoniot curves of boron(pressure P=7.9×10^(3)-1.6×10^(6) GPa and temperature T=25-2800 eV),silicon(P=2.6×10^(3)-7.9×10^(5) GPa and T=21.5-1393 eV),and aluminum(P=5.2×10^(3)-9.0×10^(5) GPa and T=25-1393 eV)over wide ranges of pressure and temperature.In particular,we systematically investigate the impact of different cutoff radii in norm-conserving pseudopotentials on the calculated properties at elevated temperatures,such as pressure,ionization energy,and equation of state.By comparing the SDFT and MDFT results with those of other first-principles methods,such as extended first-principles molecular dynamics and path integral Monte Carlo methods,we find that the SDFT and MDFT methods show satisfactory precision,which advances our understanding of first-principles methods when applied to studies of matter at extremely high pressures and temperatures.
基金Project supported by the National Key Laboratory Opening Funding of Advanced Composites in Special Environments in Harbin Institute of Technology,China
文摘The structural, electronic and elastic properties of common intermetallic compounds in FeTiCoNiVCrMnCuAI system high entropy alloy were investigated by the first principles calculation. The calculation results of formation enthalpy and cohesive energy show that FeTi, Fe2Ti, AlCrFe2, Co2Ti, AlMn2V and Mn2Ti phases may form in the formation process of the alloy. Further studies show that FeTi, FezTi, AlCrFe2, Co2Ti and AlMn2V phases with higher shear modulus and elastic modulus would be excellent strengthening phases in high entropy alloy and would improve the hardness of the alloy. In addition, the partial density of states was investigated for revealing the bonding mode, and the analyses on the strength of p-d hybridization also reveal the underlying mechanism for the elastic properties of these compounds.
基金the National Key Research and Development Program of China(Grant No.2017YFE0129000)the National Natural Science Foundation of China(Grant Nos.51871121,11874223,and 11404172).
文摘Low dimensional materials are suitable candidates applying in next-generation high-performance electronic,optoelectronic,and energy storage devices because of their uniquely physical and chemical properties.In particular,one-dimensional(1D)atomic wires(AWs)exfoliating from 1D van der Waals(vdW)bulks are more promising in next generation nanometer(nm)even sub-nm device applications owing to their width of few-atoms scale and free dandling bonds states.Although several 1D AWs have been experimentally prepared,few 1D AW candidates could be practically applied in devices owing to lack of enough suitable 1D AWs.Herein,367 kinds of 1D AWs have been screened and the corresponding computational database including structures,electronic structures,magnetic states,and stabilities of these 1D AWs has been organized and established.Among these systems,unary and binary 1D AWs with relatively small exfoliation energy are thermodynamically stable and theoretically feasible to be exfoliated.More significantly,rich quantum states emerge,such as 1D semiconductors,1D metals,1D semimetals,and 1D magnetism.This database will offer an ideal platform to further explore exotic quantum states and exploit practical device applications using 1D materials.The database are openly available at http://www.dx.doi.org/10.11922/sciencedb.j00113.00004.
基金the National Natural Science Foundation of China(Grant Nos.11504312,11775102,and 11805088)the National Basic Research Program of China(Grant No.2015CB921103)+2 种基金China Postdoctoral Science Foundation(Grant No.2018M641477)Guangdong Provincial Department of Science and Technology,China(Grant No.2018A0303100013)the Fundamental Research Funds for the Central Universities,China(Lanzhou University,Grant No.lzujbky-2018-19).
文摘Sulfide nanocrystals and their composites have shown great potential in the thermoelectric(TE)field due to their extremely low thermal conductivity.Recently a solid and hollow metastable Au2S nanocrystalline has been successfully synthesized.Herein,we study the TE properties of this bulk Au2S by first-principles calculations and semiclassical Boltzmann transport theory,which provides the basis for its further experimental studies.Our results indicate that the highly twofold degeneracy of the bands appears at theΓpoint in the Brillouin zone,resulting in a high Seebeck coefficient.Besides,Au2S exhibits an ultra-low lattice thermal conductivity(~0.88 W·m^-1·K^-1 at 700 K).At 700 K,the thermoelectric figure of merit of the optimal p-type doping is close to 1.76,which is higher than 0.8 of ZrSb at 700 K and 1.4 of PtTe at 750 K.Our work clearly demonstrates the advantages of Au2S as a TE material and would greatly inspire further experimental studies and verifications.
基金supported by the National Natural Science Foundation of China (grants No.41172051 and 41472042)the Specialized Research Fund for the Doctoral Program of Higher Education of China (grant No.20060491504)
文摘Hydrogen incorporation is critical for explaining defect energies, structure parameters and other physical characteristics of minerals and understanding mantle dynamics. This work analyzed the hydrogen complex defects in jadeite by the plane-wave pseudo-potential method based on density functional theory, and optimized the atomic positions and lattice constants in all configurations （different defective systems）. Incorporation mechanisms considered for hydrogen （H） in jadeite include： （1） hydrogen incorporating with the 02 site oxygen and coexisting with M2 vacancy; （2） one H atom combined with an AI atom replacing Si in tetrahedron; （3） 4H atoms directly replacing Si in tetrahedron and （4） 3H atoms replacing Al on the M1 site. The four incorporation mechanisms mentioned above form the corresponding VNa-Hi, Alsi-Hi, Vsi-4Hi and VAr3Hi point defects. The molecular dynamics simulation to the ideal, VNa-Hi, Alsi-Hi, Vsi-4Hi and VAr3Hi point defects under the P-T conditions of 900 K, 2 GPa, the Vsa-Hi and Alsi-Hi point defects under different pressures at T = 900 K, and Alsj-Hj point defects under different temperatures at P = 3 GPa was performed to examine the preferential mode of hydrogen incorporation in jadeite by means of first-principles calculations. The calculations show that the averaged O-H bond-length in the hydrogen point defects system decreased in the order of Alsi-Hi, VNa-HI, Vsl-4Hf and VAI-3Hi. VNa-HI complex defects result in a contraction of the jadeite volume and the presence of Alsi-Hi, Vsi-4H~ and VAI-3Hi defects could increase the superceli volume, which is the most obvious in the VAt-3Hi defects. The energy of formation of Also-HI and VA[-3HI complex defects was much lower than that of other defect systems. The VAI-3Hi defects system has the lowest energy and the shortest O-H bond-length, suggesting that this system is the most favorable. The analytical results of vacancy formation energy, O-H bond- length, and the stability of the hydrogen defects in jadeite have suggested that the preferred hydration incorporation mode in jadeite is VAI-3Hi complex defect.
基金the Extracurricular Open Experiment of Southwest Petroleum University(No.KSZ18513)the State Key Program of National Natural Science Foundation of China(No.51474181).
文摘Graphene is an ideal reinforcing phase for a high-performance composite filler,which is of great theoretical and practical significance for improving the wettability and reliability of the filler.However,the poor adsorption characteristics between graphene and the silver base filler significantly affect the application of graphene filler in the brazing field.It is a great challenge to improve the adsorption characteristics between a graphene and silver base filler.To solve this issue,the adsorption characteristic between graphene and silver was studied with first principle calculation.The effects of Ga,Mo,and W on the adsorption properties of graphene were explored.There are three possible adsorbed sites,the hollow site(H),the bridge site(B),and the top site(T).Based on this research,the top site is the most preferentially adsorbed site for Ag atoms,and there is a strong interaction between graphene and Ag atoms.Metal element doping enhances local hybridization between C or metal atoms and Ag.Furthermore,compared with other doped structures(Ga and Mo),W atom doping is the most stable adsorption structure and can also improve effective adsorption characteristic performance between graphene and Ag.
基金Project supported by National Key Project for Basic Research of China (20005CB623605)NSF of Fujian Province (E0320002, A0510013)
文摘One way of improving the magnetic properties of RECo5(RE = rare earth) compounds, especially the magnetic anisotropy energy (MAE), is to dope them with some additives such as Fe, Ni, Cu. Those dopants bring changes in both lattice geometry and magnetic properties of the compounds. In this paper, the effects of doping on YCo5-x,Fex and YCo5-x Agx were studied in two simple but effective ways: first, the geometric effect induced by doping and then, the pure doping role namely without any geometric changes. The calculated results indicate that the magnetic moments of Co show a transition from a high spin state to a low one with the change of the volume of the cell in all YCo5, YCo3Fe2 and YCo3Ag2 alloys. The change of c/a ratio with constant lattice parameter a also influences drastically the magnetic moments and the MAE. As the geometric structure is not changed, it is found that the doping effects of magnetic element Fe and non-magnetic element Ag are quite different.
基金Project(11271121)supported by the National Natural Science Foundation of ChinaProject(11JJ2002)supported by the Natural Science Foundation of Hunan Province,China+1 种基金Project(11K038)supported by Key Laboratory of Computational and Stochastic Mathematics of Ministry of Education of ChinaProject(2013GK3130)supported by the Scientific and Technological Plan of Hunan Province,China
文摘The electronic structures,chemical bonding,elastic and optical properties of the novel hP24 phase WB3 were investigated by using density-functional theory(DFT) within generalized gradient approximation(GGA).The calculated energy band structures show that the hP24 phase WB3 is metallic material.The density of state(DOS) and the partial density of state(PDOS) calculations show that the DOS near the Fermi level is mainly from the W 5d and B 2p states.Population analysis suggests that the chemical bonding in hP24-WB3 has predominantly covalent characteristics with mixed covalent-ionic characteristics.Basic physical properties,such as lattice constant,bulk modulus,shear modulus and elastic constants Cij were calculated.The elastic modulus E and Poisson ratio υ were also predicted.The results show that hP24-WB3 phase is mechanically stable and behaves in a brittle manner.Detailed analysis of all optical functions reveals that WB3 is a better dielectric material,and reflectivity spectra show that WB3 can be promised as good coating material in the energy regions of 8.5-11.4 eV and 14.5-15.5 eV.
文摘The structural, anisotropic elastic properties and the ideal compressive and tensile strengths of titanium diboride (TiB_(2)) were investigated using first-principles calculations based on density functional theory. The stress-strain relationships of TiB2 under 〈10i0〉, 〈12i0〉, and 〈0001〉 compressive loads were calculated. Our results showed that the ideal uniaxial compressive strengths are |σ〈02i0〉)| = 142.96 GPa, |σ〈0001〉 ] = 188.75 GPa, and |σ〈10i0〉| = 245.33 GPa, at strains -0.16, -0.32, and -0.24, respectively. The variational trend is just the opposite to that of the ideal tensile strength with σ〈10i0〉 = 44.13 GPa, σ〈0001〉 = 47.03 GPa, and σ〈i2i0〉 = 56.09 GPa, at strains 0.14, 0.28, and 0.22, respectively. Furthermore, it was found that TiB2 is much stronger under compression than in tension. The ratios of the ideal compressive to tensile strengths are 5.56, 2.55, and 4.01 for crystallographic directions (10i0), 〈12i0〉, and 〈0001〉, respectively. The present results are in excellent agreement with the most recent experimental data and should be helpful to the understanding of the compressive property of TiB2.
基金Project supported by the National Natural Science foundation of China (Grant No.60925016)
文摘The global greenhouse effect makes it urgent to deal with the increasing greenhouse gases. In this paper the performance of MgO-decorated carbon nanotubes for CO2 adsorption is investigated through first principles calculations. The results show that the MgO-decorated carbon nanotubes can adsorb CO2 well and are relatively insensitive to O2 and N2 at the same time. The binding energy arrives at 1.18 eV for the single-MgO-decorated carbon nanotube adsorbing one CO2 molecule, while the corresponding values for O2 and N2 are 0.55 eV and 0.06 eV, respectively. In addition, multi-molecule adsorption is also proved to be very satisfactory. These results indicate that MgO-decorated carbon nanotubes have great potential applications in industrial and environmental processes.
基金the Higher Education Commission of Pakistan for partial funding.
文摘In this study the pseudo-potential method is used to investigate the structural, electronic, and thermodynamic proper- ties of ZnOl_xSx semiconductor materials. The results show that the electronic properties are found to be improved when calculated by using LDA ~ U functional as compared with local density approximation （LDA）. At various concentrations the ground-state properties are determined for bulk materials ZnO, ZnS, and their tertiary alloys in cubic zinc-blende phase. From the results, a minor difference is observed between the lattice parameters from Vegard＇s law and other calculated results, which may be due to the large mismatch between lattice parameters of binary compounds ZnO and ZnS. A small deviation in the bulk modulus from linear concentration dependence is also observed for each of these alloys. The ther- modynamic properties, including the phonon contribution to Helmholtz free energy △F, phonon contribution to internal energy △E, and specific iheat at constant-volume Cv, are calculated within quasi-harmonic approximation based on the calculated phonon dispersion relations.
基金Supported by the New Century Excellent Talents in University in Ministry of Education of China under Grant No NCET-09-0867
文摘We report a study of the electronic structure and optical properties of uranium dioxide （U02） based on the ab-initio density-functional theory and using the generalized gradient approximation. To correctly describe the strong correlation between 5 f electrons of a uranium atom, we employ the on-site Hubbard U correction term and optimize the correlation parameter of the bulk uranium dioxide. Then we give the structural and electronic properties of the ground state of uranium dioxide. Based on the accurate electronic structure, we calculate the complex dielectric function of UO2 and the related optieM properties, such as reflectivity, refractive index, extinction index, energy loss spectra, and absorption coefficient.
文摘The structural, magnetic and electronic properties of the double perovskite Ba2SmNbO6 （for the simple cubic structure where no octahedral tilting exists anymore） are studied using the density functional theory within the generalized gradient approximation as well as taking into account the on-site Coulomb repulsive interaction. The total energy, the spin magnetic moment, the band structure and the density of states are calculated. The optimization of the lattice constants is 8.5173 A, which is in good agreement with the experimental value 8.5180 A. The calculations reveal that Ba2SmNbO6 has a stable ferromagnetic ground state and the spin magnetic moment per molecule is 5.00μB/f.u. which comes mostly from the Sin3＋ ion only. By analysis of the band structure, the compound exhibits the direct band gap material and half-metallic ferromagnetic nature with 100% spin-up polarization, which implies potential applications of this new lanthanide compound in magneto-electronic and spintronic devices.
基金Supported by the National Natural Science Foundation of China under Grant Nos 51522102,51734008,51327901 and 51474175
文摘Calorimetric measurements are performed to determine the specific heat of Si-xat.% Ge(where x = 0, 10, 30,50, 70, 90 and 100) alloys within a broad temperature range from 123 to 823 K. The measured specific heat increases dramatically at low temperatures, and the composition dependence of specific heat is evaluated from the experimental results. Meanwhile, the specific heat at constant volume, the thermal expansion, and the bulk modulus of Si and Ge are investigated by the first principle calculations combined with the quasiharmonic approximation. The negative thermal expansion is observed for both Si and Ge. Furthermore, the isobaric specific heat of Si and Ge is calculated correspondingly from OK to their melting points, which is verified by the measured results and accounts for the temperature dependence in a still boarder range.
文摘In order to have a better understanding of the electronic structures and physical properties of Cu<sub>2-<span style="white-space:nowrap;"><em>δ</em></span></sub>X (X = Se, S, Te) copper chalcogenides. First principles were performed to calculate the chemical shift, band structure, and electron density of states of Cu<span style="white-space:nowrap;"><sub>2-<em>δ</em></sub></span>X (X = Se, S, Te). By comparing our calculation results with previous experimental works, we found that the predicted electronic structures of Cu<sub>2</sub>Se, Cu<sub>2</sub>Te and Cu<sub>2</sub>S transform from semimetal to semiconductor after adding on-site Coulomb U, which reflects the real properties of the materials. By using (Density Functional Theory) DFT + U method, the calculation result is close to the real electronic structure. The calculation result of chemical shift of adding U does not reach the ideal expectation, and the reason is not clear at present. In this paper, the theoretical electronic structures of Cu<sub>2</sub>Se, Cu<sub>2</sub>Te and Cu<sub>2</sub>S are better calculated by DFT + U method and compared with the actual properties. The effect of Cu-s electron on the chemical shift is understood, and a theoretical result of the chemical shift is calculated, which provides a powerful reference for the subsequent research and understanding of the electronic structure and physical properties of the compounds with S groups of Cu.
文摘The plane wave pseudo-potential method was used to investigate the structural, electronic, and elastic properties of Cd Se_（1-x）Te_x in the zinc blende phase. It is observed that the electronic properties are improved considerably by using LDA ＋ U as compared to the LDA approach. The calculated lattice constants and bulk moduli are also comparable to the experimental results. The cohesive energies for pure Cd Se and Cd Te binary and their mixed alloys are calculated. The second-order elastic constants are also calculated by the Lagrangian theory of elasticity. The elastic properties show that the studied material has a ductile nature.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFF0609000)National Natural Science Foundation of China(Grant Nos.52171034 and 52101037)Postdoctoral Fellowship Program of CPSFara(No.GZB20230944).
文摘Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.
基金funded by the Natural Science Foundation of China (No. 21603109)the Henan Joint Fund of the National Natural Science Foundation of China (No. U1404216)+1 种基金the Scientific Research Program Funded by Shaanxi Provincial Education Department (No. 20JK0676)supported by Natural Science Basic Research Program of Shanxi (Nos. 2022JQ-108, 2022JQ096)。
文摘Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),CrS_(2)with one S vacancy(v-CrS_(2)), and Ti doped CrS_(2)(Ti@CrS_(2)). The results have shown that the pristine CrS_(2)exhibits inert character for NO activation. However, v-CrS_(2)and Ti@CrS_(2)can exhibit enhanced interaction with NO, due to increased charge transfer between NO and substrates(0.52–0.75 e) and enhanced adsorption energies of NO on the catalysts(-0.96~-1.64 e V), compared to the situation of CrS_(2)(0.065 e/-0.30 e V). From the free energy profiles of NO electro-reduction to NH3, we can see that the v-CrS_(2)and Ti@CrS_(2)all exhibit ultralow limiting potentials of-0.03~-0.47 V, following both*NOH and*NHO mechanisms. Therefore, introducing vacancy and doping are all promising modification strategies for NORR catalysts. The results have provided a new idea for the search of catalysts for efficient electrocatalytic reduction of NO.
