First-principles calculations based on density functional theory were performed to study the effect of alloying on the thermodynamic stability of MgH2 hydride （rutile and fluorite structures） with transitional meta...First-principles calculations based on density functional theory were performed to study the effect of alloying on the thermodynamic stability of MgH2 hydride （rutile and fluorite structures） with transitional metals （TM=Sc, Ti, Y） and group IIA elements （M=Ca, Sr, Ba）. The results indicate that fluorite structure of these hydrides are more stable than its relative rutile structure at low alloying content （less 20%）, structural destabilization of MgH2 appears in the alloying cases of Ti, Sr and Ba respectively. The structure-transition point from rutile structure to fluorite structure is at around 20% for MgH2-TM, and about 40% for MgH2-M. The formation enthalpy of fluorite Mg0.5Ba0.52 is about 0.3 eV and higher than that of fluorite MgH2, indicating that its hydrogen-desorption temperature at atmospheric pressure will be much lower than that of pure MgH2. Good consistency between experimental and calculated data suggests that above-adopted method is useful to predict structural transition and properties of MgH2 based hydrides for hydrogen storage.展开更多
Collective behaviours of active particle systems have gained great research attentions in re- cent years. Here we present a mode-coupling theory （MCT） framework to study the glass transition of a mixture system of a...Collective behaviours of active particle systems have gained great research attentions in re- cent years. Here we present a mode-coupling theory （MCT） framework to study the glass transition of a mixture system of active and passive Brownian particles. The starting point is an eff）ctive Smoluchowski equation, which governs the dynamics of the probability dis- tribution function in the position phase space. With the assumption of the existence of a nonequilibrium steady state, we are able to obtain dynamic equations for the intermediate scattering functions （ISFs）, wherein an irreducible memory function is introduced which in turn can be written as functions of the ISFs based on standard mode-coupling approximations. The effect of particle activity is included through an effective difIusion coefficient which can be obtained via short time simulations. By calculating the long-time limit of the ISF, the Debye-Waller （DW） factor, one can determine the critical packing fraction ηc of glass transition. We find that for active-passive （AP） mixtures with the same particle sizes, ηc increases as the partial fraction of active particle xA increases, which is in agreement with previous simulation works. For system with different active/passive particle sizes, we find an interesting reentrance behaviour of glass transition, i.e., ηc shows a non-monotonic dependence on xa. In addition, such a reentrance behaviour would disappear if the particle activity is large enough. Our results thus provide a useful theoretical scheme to study glass transition behaviour of active-passive mixture systems in a promising way.展开更多
文摘First-principles calculations based on density functional theory were performed to study the effect of alloying on the thermodynamic stability of MgH2 hydride （rutile and fluorite structures） with transitional metals （TM=Sc, Ti, Y） and group IIA elements （M=Ca, Sr, Ba）. The results indicate that fluorite structure of these hydrides are more stable than its relative rutile structure at low alloying content （less 20%）, structural destabilization of MgH2 appears in the alloying cases of Ti, Sr and Ba respectively. The structure-transition point from rutile structure to fluorite structure is at around 20% for MgH2-TM, and about 40% for MgH2-M. The formation enthalpy of fluorite Mg0.5Ba0.52 is about 0.3 eV and higher than that of fluorite MgH2, indicating that its hydrogen-desorption temperature at atmospheric pressure will be much lower than that of pure MgH2. Good consistency between experimental and calculated data suggests that above-adopted method is useful to predict structural transition and properties of MgH2 based hydrides for hydrogen storage.
基金supported by the Ministry of Science and Technology of China(No.2016YFA0400904and No.2013CB834606)the National Natural Science Foundation of China(No.21673212,No.21521001,No.21473165,No.21403204)the Fundamental Research Funds for the Central Universities(No.WK2030020028 and No.2340000074)
文摘Collective behaviours of active particle systems have gained great research attentions in re- cent years. Here we present a mode-coupling theory （MCT） framework to study the glass transition of a mixture system of active and passive Brownian particles. The starting point is an eff）ctive Smoluchowski equation, which governs the dynamics of the probability dis- tribution function in the position phase space. With the assumption of the existence of a nonequilibrium steady state, we are able to obtain dynamic equations for the intermediate scattering functions （ISFs）, wherein an irreducible memory function is introduced which in turn can be written as functions of the ISFs based on standard mode-coupling approximations. The effect of particle activity is included through an effective difIusion coefficient which can be obtained via short time simulations. By calculating the long-time limit of the ISF, the Debye-Waller （DW） factor, one can determine the critical packing fraction ηc of glass transition. We find that for active-passive （AP） mixtures with the same particle sizes, ηc increases as the partial fraction of active particle xA increases, which is in agreement with previous simulation works. For system with different active/passive particle sizes, we find an interesting reentrance behaviour of glass transition, i.e., ηc shows a non-monotonic dependence on xa. In addition, such a reentrance behaviour would disappear if the particle activity is large enough. Our results thus provide a useful theoretical scheme to study glass transition behaviour of active-passive mixture systems in a promising way.
