天冬氨酸在Cu(001)表面吸附的扫描隧道显微镜研究

用扫描隧道显微镜(STM)研究了室温下天冬氨酸在Cu(001)表面的吸附行为.实验发现,在较 低的覆盖度下,天冬氨酸分子在Cu(001)表面存在两种吸附状态.从STM数据估算出两种吸附 状态下天冬氨酸分子在Cu(001)表面的扩散激活能分别为079±001eV,088±005eV. 随着覆盖度的提高,天冬氨酸分子最终在Cu(001)表面形成一均匀衬度的吸附层,但并不形 成有序吸附结构,也不能使台阶发生小面化.天冬氨酸分子的这些吸附特点是迄今研究过的 所有氨基酸在Cu(001)表面吸附时不具有的. 关键词： 表面吸附 扫描隧道显微镜 氨基酸     

Comparison of density-functional approaches and Monte Carlo simulations for free planar films of liquid

Density functionals proposed in the literature for describing the behaviour of liquid helium at T =0 K are examined. In so doing, several properties of the ground states of free films of superfluid ⁴ He are calculated by using zero- and finite-range density functional theories and these results are compared to that computed with Monte Carlo simulations. We mainly focus the attention on the energy per particle of the slabs, the surface tension and the width of the liquid-vacuum interfaces, all as a function of the inverse of coverage. The largest differences are found in the case of the surface widths. Received 26 July 1999     

N2H4在NiFe(111)合金表面吸附稳定性和电子结构的第一性原理研究

采用基于色散校正的密度泛函理论进行了第一性原理研究, 详细分析了肼(N₂H₄)在Ni₈Fe₈/Ni(111)合金表面稳定吸附构型的吸附稳定性和电子结构及成键性质. 通过比较发现, 肼分子以桥接方式吸附在表面的两个Fe原子上是最稳定的吸附构型, 其吸附能为-1.578 eV/N₂H₄. 同时发现, 肼分子在这一表面上吸附稳定性的趋势为: 桥位比顶位吸附更有利, 且在Fe原子上比在Ni原子上的吸附作用更强. 进一步分析了不同吸附位点上稳定吸附构型的电子结构、电荷密度转移以及电子局域化情况. 结果发现: 相同吸附位点的电子态密度图基本一致, 并且N原子的p轨道和与之相互作用的表面原子的d轨道之间存在态密度上的重叠; 吸附后电荷密度则主要从肼分子转移到表面原子之上; 在电子局域化函数切面图中也发现吸附后电子被局域到肼分子的N原子和相邻的表面原子之间. 这些电子结构的表征都充分说明肼分子与表面原子之间通过电荷转移形成了强烈的配位共价作用.     

Photoelectron diffraction study of a catalytically active overlayer: C2H2 on Pd{111}

A quantitative structure determination of a newly discovered (2×2) adsorption phase of acetylene chemisorbed on Pd{111} has been performed by scanned-energy mode photoelectron diffraction: this phase corresponds to the threshold coverage for the catalytic conversion of acetylene to benzene. The carbon atoms in the C₂H₂ molecule are located almost over bridge sites with a C–C bond length of 1.34+0.10 Å, the centre of the molecule being positioned almost over a hollow site. Of the two hollow sites the hcp site (directly above a second layer Pd atom) is favoured, particularly by a subset of the data most sensitive to this aspect of the structure, but the full analysis indicates that the fcc site (above a third layer Pd atom) cannot formally be excluded. The adsorption site adopted by acetylene in the higher coverage phase on Pd{111} is essentially identical. This is the dominant structure in the coverage regime which is catalytically active for the conversion of acetylene to benzene. The implications of these findings for acetylene coupling reactions over Pd{111} are discussed.     

Formation of ordered micro-porous membranes

Regular micro-porous polymeric membranes have recently been discovered by rapidly evaporating a solution of CS₂ containing poly(p-phenylene)-block-polystyrene [#!ref1!#]. 1,2-dichloroethane (a chlorated solvent in which polystyrene gel phase has never been observed) is also found to produce ordered structures, which definitively excludes eventual effect of the gelation process during the membrane formation. The observation of the solution surface during the solvent evaporation reveals the growing of micron-sized water droplets trapped at the surface and forming compact aggregates. The study of the solution/water interface shows that the water droplets profile is in agreement with the pore shape observed in the membranes. Moreover, the copolymer was found to precipitate at the interface, forming a layer encapsulating the droplets and preventing their coalescence. In that way, the final structure results from the droplets stacking under the action of large surface currents. Finally, we argue that the decisive element in the formation of ordered structures is the ability of the polymer to precipitate at the solution/water interface, which seems to be related the star-polymer microstructure. Received: 18 August 1998     

Studies on radon adsorption characteristics of different charcoals used as amplifiers for the track detectors

Ten sorts of charcoals were studied regarding their use as amplifier in the design of a personal dosimeter. It consists of a combination of a Makrofol detector and activated charcoal. The calibration factor for the Makrofol using the charcoals as an amplifier is about ten times higher comparing with an exposure without charcoal. The best results were obtained with Carboxen 563. The background radioactivity of charcoals must also be considered in the dosimeter's design.     

铁原子吸附联苯烯单层电子结构的第一性原理

联苯烯单层由碳原子的四元、六元和八元环组成,具有与石墨烯相似的单原子层结构.2021年5月,Science首次报道了该材料的实验合成,引起了科研工作者的极大关注.基于第一性原理的密度泛函方法,研究了铁原子在联苯烯单层的吸附构型并分析了其电子结构.结构优化、吸附能和分子动力学的计算表明,联苯烯单层的四元环空位是铁原子最稳定的吸附位点,吸附能可达1.56 eV.电子态密度计算表明铁3d电子与碳的2p电子有较强的轨道杂化,同时电荷转移计算显示铁原子向近邻碳原子转移的电荷约为0.73个电子,说明联苯烯单层与吸附的铁原子之间形成了稳定的化学键.另外,铁原子吸附于联苯烯单层后体系显磁性,铁原子上局域磁矩大小约为1.81μB,方向指向面外.因此,本文确认了联苯烯单层是比石墨烯更好的铁原子吸附载体且体系有磁性,这为研究吸附材料的电磁、输运、催化等特性提供了新的平台.     

碳纳米锥吸附Na的第一性原理计算

本文采用第一性原理计算结合从头算分子动力学的方法,研究了碳纳米锥(CNC)、B和N掺杂碳纳米锥(B-CNC和N-CNC)的稳定性,结果表明CNC、B-CNC和N-CNC均可以稳定存在.在此基础上分别研究了Na原子在CNC、B-CNC和N-CNC上的吸附行为.结果表明：1) Na原子在CNC五元碳环中心顶部位置的吸附最强,吸附能为-2.52 eV. CNC的能隙(Eg)为1.96 eV. 2) B和N掺杂CNC后,B-CNC和N-CNC的导电性均显著增强. 3)与CNC相比,Na原子在B-CNC上的吸附增强,而在N-CNC上的吸附则显著减弱.这表明B-CNC有望作为Na离子电池的负极材料.本文的研究结果对以CNC为负极材料的Na离子电池的研究提供了理论指导.     

Magnetically‐Confined Fe‐Mn Bimetallic Oxide Encapsulation as an Efficient and Recoverable Adsorbent for Arsenic(III) Removal

Synthesis of bimetallic‐oxide‐encapsulated magnetic nanoparticles is still significantly challenging and has rarely been attempted previously, due to the effects of lattice mismatch, weak chemical interactions and variances in growth rates between different components, as well as the difficulty in process control for uniform co‐deposition. In the present work, Fe‐Mn bimetallic oxide (FMBO) nanoplatelet encapsulated magnetic nanoparticles (Mag‐FeMn) are prepared by controlled engineering of the interparticle coupling of Fe₃O₄ and FMBO, with its multifunctional capabilities highlighted in terms of the potentially superior As(III) sequestration and convenient recoverability. Multiple characterization techniques are employed to examine the derived morphologies and to accurately resolve both compositionally and magnetically the hierarchical structure in detail. The synthesized magnetic composites retain highly porous structure with the main components of Fe₂O₃, FeOOH, Fe₃O₄, and Mn₃O₄. Mag‐FeMn exhibits a quite competitive high capacity for As(III) capture (56.1 mg g^–1), whereby As(III) oxidation coupled with synchronous sorption contributes to the improved performance. The unique heterostructure of FMBO encapsulation with an embedded magnetic core would be applicable to help with rational synthesis of other bimetallic oxide encapsulated magnetic nanoparticles, and definitely shows promise for the development of new nanotechnology enabled approaches for adsorption‐based water purification.