The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous pollutants...The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous pollutants.It is proposed that the formation and diffusion of Ov originate from its outstanding reduction property.However,the formation and diffusion process of Ov over the surface of ceria at the atomic level is still unknown.Herein,the structural and valence evolution of CeO_(2)(111)surfaces in reductive,oxidative and vacuum environments from room temperature up to 700℃was studied with in situ aberration-corrected environmental transmission electron microscopy(ETEM)experiments.Ov is found to form under a high vacuum at elevated temperatures;however,the surface can recover to the initial state through the adsorption of oxygen atoms in an oxygen-contained environment.Furthermore,in hydrogen environment,the step-CeO_(2)(111)surface is not stable at elevated temperatures;thus,the steps tend to be eliminated with increasing temperature.Combined with first-principles density function calculations(DFT),it is proposed that O-terminated surfaces would develop in a hypoxic environment due to the dynamic diffusion of Ov from the outer surface to the subsurface.Furthermore,in a reductive environment,H2 facilitates the formation and diffusion of Ov while Ce-terminated surfaces develope.These results reveal dynamic atomic-scale interplay between the nanoceria surface and gas,thereby providing fundamental insights into the Ov-dependent reaction of nano-CeO_(2) during catalytic processes.展开更多
The temperature dependence of lattice constants is studied by using first-principles calculations to determine the effects of in-plane stiffness and charge transfer on the thermal expansions of monolayer semiconductin...The temperature dependence of lattice constants is studied by using first-principles calculations to determine the effects of in-plane stiffness and charge transfer on the thermal expansions of monolayer semiconducting transition metal dichalcogenides.Unlike the corresponding bulk material,our simulations show that monolayer MX2(M = Mo and W;X = S,Se,and Te) exhibits a negative thermal expansion at low temperatures,induced by the bending modes.The transition from contraction to expansion at higher temperatures is observed.Interestingly,the thermal expansion can be tailored regularly by alteration of the M or X atom.Detailed analysis shows that the positive thermal expansion coefficient is determined mainly by the in-plane stiffness,which can be expressed by a simple relationship.Essentially the regularity of this change can be attributed to the difference in charge transfer between the different elements.These findings should be applicable to other two-dimensional systems.展开更多
On the basis of first-principles density functional calculations, the present study sheds theoretical insight on ultrathin carbon nanotube (UCNT) and hydrogenated ultrathin carbon nanotube (HUCNT) for use as poten...On the basis of first-principles density functional calculations, the present study sheds theoretical insight on ultrathin carbon nanotube (UCNT) and hydrogenated ultrathin carbon nanotube (HUCNT) for use as potential materials not only for Li-ion battery anode but also for high-capacity hydrogen storage. The highest Li storage capacities in UCNT and HUCNT can be of LiC4 and LiC4H2, respectively, which are higher than that in graphite and LiC6. Binding between Li (Ca) atoms and these materials are found to be enhanced considerably. Each Li (Ca) atom may bind multi-hydrogen molecules, and the adsorption energies are ideally suited for storing hydrogen under ambient conditions, and the predicted weight percentage of molecular hydrogen are in the range of 6.4-12 wt% exceeding the target set by the United States Department of Energy.展开更多
We theoretically and computationally show the simplest realization of SOC using two-level cold atoms interacting with only one laser beam.The underlying mechanism is based on the non-adiabatic nature of laser-atom int...We theoretically and computationally show the simplest realization of SOC using two-level cold atoms interacting with only one laser beam.The underlying mechanism is based on the non-adiabatic nature of laser-atom interaction,with the Rabi frequency being not much larger than the kinetic energy of the atom.We use Zitterbewegung oscillation to further illustrate the effects of the synthesized SOC on the quantum dynamics of the two-level cold atoms.We expect our proposal to be of experimental interest in the quantum simulation of SOC-related physics.展开更多
The adsorption effects of 3d transitional metal (TM) adatoms on electronic and magnetic properties of monolayer and bilayer MoS2 sheets have been investigated by using first-principle calculations based on the densi...The adsorption effects of 3d transitional metal (TM) adatoms on electronic and magnetic properties of monolayer and bilayer MoS2 sheets have been investigated by using first-principle calculations based on the density functional theory. The calculated results suggest that both monolayer and bilayer MoS2 sheets have power abilities of absorbing 3d TM atoms. The interlayer adsorption of bilayer MoSa is relatively more stable than the surface adsorption of monolayer MoS2. The 3d TM adatoms and the neighboring S atoms behave a clear covalent-binding character. It was found that TM adatoms induce certain impurity states within the band gap of the pristine MoS2 sheet which result in the systems magnetically semiconducting or half metallic. The adsorbed systems for Cr and Co on the surface of monolayer MoS2 sheet, as well as Sc, Cr and Fe in the interlayer of bilayer MoSa sheet exhibit half-metallic behavior. And the other 3d TM- adsorbed systems are magnetic semiconductor except for Ni species.展开更多
基金Project supported by the National Key Research and Development Plan(2021YFA1200201)the Natural Science Foundation of China(51872008)+1 种基金the"111"Project under the DB18015 grantBeijing Outstanding Young Scientists Projects(BJJWZYJH01201910005018)。
文摘The extremely high structural tolerance of ceria to oxygen vacancies(Ov)has made it a desirable catalytic material for the hydrocarbon oxidation to chemicals and pharmaceuticals and the reduction of gaseous pollutants.It is proposed that the formation and diffusion of Ov originate from its outstanding reduction property.However,the formation and diffusion process of Ov over the surface of ceria at the atomic level is still unknown.Herein,the structural and valence evolution of CeO_(2)(111)surfaces in reductive,oxidative and vacuum environments from room temperature up to 700℃was studied with in situ aberration-corrected environmental transmission electron microscopy(ETEM)experiments.Ov is found to form under a high vacuum at elevated temperatures;however,the surface can recover to the initial state through the adsorption of oxygen atoms in an oxygen-contained environment.Furthermore,in hydrogen environment,the step-CeO_(2)(111)surface is not stable at elevated temperatures;thus,the steps tend to be eliminated with increasing temperature.Combined with first-principles density function calculations(DFT),it is proposed that O-terminated surfaces would develop in a hypoxic environment due to the dynamic diffusion of Ov from the outer surface to the subsurface.Furthermore,in a reductive environment,H2 facilitates the formation and diffusion of Ov while Ce-terminated surfaces develope.These results reveal dynamic atomic-scale interplay between the nanoceria surface and gas,thereby providing fundamental insights into the Ov-dependent reaction of nano-CeO_(2) during catalytic processes.
基金supported by the National Natural Science Foundation of China(Grant Nos.11274280 and 11104254)the National Basic Research Program of China(Grant No.2012CB921300)
文摘The temperature dependence of lattice constants is studied by using first-principles calculations to determine the effects of in-plane stiffness and charge transfer on the thermal expansions of monolayer semiconducting transition metal dichalcogenides.Unlike the corresponding bulk material,our simulations show that monolayer MX2(M = Mo and W;X = S,Se,and Te) exhibits a negative thermal expansion at low temperatures,induced by the bending modes.The transition from contraction to expansion at higher temperatures is observed.Interestingly,the thermal expansion can be tailored regularly by alteration of the M or X atom.Detailed analysis shows that the positive thermal expansion coefficient is determined mainly by the in-plane stiffness,which can be expressed by a simple relationship.Essentially the regularity of this change can be attributed to the difference in charge transfer between the different elements.These findings should be applicable to other two-dimensional systems.
基金Supported by the National Basic Research Program of China under Grant No 2012CB921300, and the National Natural Science Foundation of China under Grant Nos 11274280 and 11104254.
文摘On the basis of first-principles density functional calculations, the present study sheds theoretical insight on ultrathin carbon nanotube (UCNT) and hydrogenated ultrathin carbon nanotube (HUCNT) for use as potential materials not only for Li-ion battery anode but also for high-capacity hydrogen storage. The highest Li storage capacities in UCNT and HUCNT can be of LiC4 and LiC4H2, respectively, which are higher than that in graphite and LiC6. Binding between Li (Ca) atoms and these materials are found to be enhanced considerably. Each Li (Ca) atom may bind multi-hydrogen molecules, and the adsorption energies are ideally suited for storing hydrogen under ambient conditions, and the predicted weight percentage of molecular hydrogen are in the range of 6.4-12 wt% exceeding the target set by the United States Department of Energy.
基金Supported by the National Research Foundation and Ministry of Education,Singapore under Grant No WBS:R-710-000-008-271by the National Natural Science Foundation of China under Grant No 11105123.
文摘We theoretically and computationally show the simplest realization of SOC using two-level cold atoms interacting with only one laser beam.The underlying mechanism is based on the non-adiabatic nature of laser-atom interaction,with the Rabi frequency being not much larger than the kinetic energy of the atom.We use Zitterbewegung oscillation to further illustrate the effects of the synthesized SOC on the quantum dynamics of the two-level cold atoms.We expect our proposal to be of experimental interest in the quantum simulation of SOC-related physics.
基金financially supported by the National Basic Research Program of China (No. 2012CB921300)
文摘The adsorption effects of 3d transitional metal (TM) adatoms on electronic and magnetic properties of monolayer and bilayer MoS2 sheets have been investigated by using first-principle calculations based on the density functional theory. The calculated results suggest that both monolayer and bilayer MoS2 sheets have power abilities of absorbing 3d TM atoms. The interlayer adsorption of bilayer MoSa is relatively more stable than the surface adsorption of monolayer MoS2. The 3d TM adatoms and the neighboring S atoms behave a clear covalent-binding character. It was found that TM adatoms induce certain impurity states within the band gap of the pristine MoS2 sheet which result in the systems magnetically semiconducting or half metallic. The adsorbed systems for Cr and Co on the surface of monolayer MoS2 sheet, as well as Sc, Cr and Fe in the interlayer of bilayer MoSa sheet exhibit half-metallic behavior. And the other 3d TM- adsorbed systems are magnetic semiconductor except for Ni species.