Synthesis of hydrothermally stable and long-range ordered Ce-MCM-48 and Fe-MCM-48 materials

The hydrothermally stable and long-range ordered Ce-MCM-48 and Fe-MCM-48 were conveniently synthesized at 393 K for 24 h by directly adding fluoride ions to the initial gel without posttreatment and pH adjustment. The Ce-MCM-48 with a Si/Ce of 200 and 100, which were prepared by directly adding fluoride ions, could still maintain their mesoporous structures after refluxing in boiling water for 3 days. The incorporation of Ce into MCM-48 could enhance the hydrothermal stability of MCM-48 in the absence of fluoride ions; however, the incorporation of Fe into MCM-48 materials barely improved the hydrothermal stability of MCM-48 materials. The effect of adding NaF was much more efficient in enhancement of hydrothermal stability than that of the incorporation of Ce. The addition of fluoride ions mainly improves the degree of polymerization of silicates. The Ce(4+) ions in Ce-MCM-48 appear to be present partly in tetrahedral coordination in the framework and partly as CeO(2) particles on the surface of framework. The Ce positioned on the surface of pore walls and in the framework both provide the protection against water attack.     

Single C59N molecule as a molecular rectifier

We report a new kind of experimental realization of a molecular rectifier, which is based on a single azafullerene C59N molecule in a double-barrier tunnel junction via the single electron tunneling effect. An obvious rectifying effect is observed. The positive onset voltage is about 0.5-0.7 V, while the negative onset voltage is about 1.6-1.8 V. Theoretical analyses show that the half-occupied molecular orbital of the C59N molecule and the asymmetric shift of the molecular Fermi level when the molecule is charged are responsible for the molecular rectification.     

A theoretical study of the Y$\mathsf{_{3}}$O clusters

Hybrid density functional calculations are performed to study the structural and electronic properties of neutral, anionic and cationic Y₃O clusters. The most stable structures of these clusters are found to be triply bridging oxygen atom structures with C_S symmetry. The ground states of Y₃O, Y₃O^- and Y₃O ⁺ are doublet (²A), triplet (³A) and singlet (¹A), respectively. The calculated electron affinities and ionization potentials are in good agreement with the available experimental data. Time-dependent density functional theory is used to calculate the low-lying excited states. A theoretical assignment for the features in the experimental photoelectron spectra is given.Received: 5 November 2003, Published online: 20 January 2004PACS: 36.40.Mr Spectroscopy and geometrical structure of clusters - 31.15.Ew Density-functional theory - 34.50.Gb Electronic excitation and ionization of molecules; intermediate molecular states (including lifetimes, state mixing, etc.)     

A rationally designed two-dimensional MoSe2/Ti2CO2 heterojunction for photocatalytic overall water splitting: simultaneously suppressing electron–hole recombination and photocorrosion

Electron–hole recombination and photocorrosion are two challenges that seriously limit the application of two-dimensional (2D) transition metal dichalcogenides (TMDs) for photocatalytic water splitting. In this work, we propose a 2D van der Waals MoSe₂/Ti₂CO₂ heterojunction that features promising resistance to both electron–hole recombination and photocorrosion existing in TMDs. By means of first-principles calculations, the MoSe₂/Ti₂CO₂ heterojunction is demonstrated to be a direct Z-scheme photocatalyst for overall water splitting with MoSe₂ and Ti₂CO₂ serving as photocatalysts for hydrogen and oxygen evolution reactions, respectively, which is beneficial to electron–hole separation. The ultrafast migration of photo-generated holes from MoSe₂ to Ti₂CO₂ as well as the anti-photocorrosion ability of Ti₂CO₂ are responsible for photocatalytic stability. This heterojunction is experimentally reachable and exhibits a high solar-to-hydrogen efficiency of 12%. The strategy proposed here paves the way for developing 2D photocatalysts for water splitting with high performance and stability in experiments.

The two challenges of electron–hole recombination and photocorrosion for two-dimensional transition metal dichalcogenides in the application of photocatalytic water splitting are simultaneously suppressed by rational design of heterojunctions.     

基于本征系数的大口径望远镜失调量解算

针对大口径望远镜光学系统内部空间限制的特点,为了实现失调量校正,提出了一种基于本征系数的失调量解算方法.该方法首先利用波前曲率传感器的原理,通过交替测量前后离焦面的方式采集光斑图.然后,利用无需分区探测的本征函数法进行波前重构,利用本征系数来表征系统波像差,并依据失调量建立灵敏度矩阵模型.最后,根据失调状态与理想状态的本征系数即可求解出失调量.与其他技术途径相比,该方法具有无需添加光学元件、无需分区探测、运算简单的特点.主镜直径为1.8m的望远镜实验结果表明,当次镜偏心距离范围为--0.9～0.9 mm、倾斜角范围为--0.2°～0.2°时,利用本征系数灵敏度矩阵法得到的计算值的误差均小于10％,对大口径望远镜中的应用具有一定的意义.     

水下弹性微穿孔吸声结构吸声系数研究

利用模态叠加法建立了水介质微穿孔板的数学模型,基于声电类比法得到其等效电路模型。研究了弹性微穿孔板和弹性背腔对垂直入射吸声系数的影响。与空气介质中的微穿孔板不同,水下微穿孔板因结构阻抗不足,难以取得满意的吸声效果,为此提出了增强型微穿孔吸声结构,并在水介质阻抗管内对理论结果予以验证。结果表明,随着增强型弹性微穿孔板弯曲刚度的增大,其在[20,2000]Hz范围内的平均吸声系数得到提高,逐步趋近于刚性微穿孔板的结果,弹性背板使微穿孔吸声结构的吸声峰向低频移动,低频吸声效果得到提高。