SO2在Ni(111)表面分解吸附的理论研究

采用密度泛函理论(DFT)的广义梯度近似(GGA)方法对SO2及其分解片段的吸附结构和性质进行了理论研究.计算结果表明:在Ni(111)表面上SO2以S,O原子顶位平铺吸附最稳定;SO3以C3v轴倾斜表面吸附;SO自由基存在两种可能的吸附结构,一种是平铺吸附于Ni(111)面,另一种是以S端垂直吸附穴位,S原子在穴位为最优吸附位.对各吸附体系的态密度及电子转移分析表明,SOx吸附中均为衬底镍原子向硫的氧化物转移电子,改变了S—O键之间的电子分布,导致其键长变长,这有利于硫氧化物在镍表面的解离反应.S原子在Ni(111)表面的吸附中,Ni原子的s轨道向S原子转移电子,这与O的吸附机理有所不同.     

Surface charge--induced ordering of the au(111) surface

Synchrotron surface x-ray scattering (SXS) studies have been carried out at the Au(lll)/electrolyte interface to determine the influence of surface charge on the microscopic arrangement of gold surface atoms. At the electrochemical interface, the surface charge density can be continuously varied by controlling the applied potential. The top layer of gold atoms undergoes a reversible phase transition between the (1 x 1) bulk termination and a (23 x radical3) reconstructed phase on changing the electrode potential. In order to differentiate the respective roles of surface charge and adsorbates, studies were carried out in 0.1 M NaF, NaCl, and NaBr solutions. The phase transition occurs at an induced surface charge density of 0.07 +/- 0.02 electron per atom in all three solutions.     

A homomolecular porous network at a Cu(111) surface

Anthraquinone molecules self-assemble on a Cu(111) surface into a large two-dimensional honeycomb network (square root of 304 x square root of 304)R23 degrees with pore diameters of approximately 50 A. The spontaneous formation of a pattern containing pores roughly five times larger than the size of the constituent molecules is unprecedented. The network originates from a delicate balance between substrate-mediated repulsion and intermolecular attraction involving an unusual chemical motif: hydrogen bonding between a carbonyl oxygen and an aromatic hydrogen atom. Substrate-mediated long-range adsorbate-adsorbate repulsion has been observed on anisotropic surfaces and in the context of the absence of pattern formation. Its applicability for the design of tailored molecular films is explored here.     

甲醇、CO和水在Pt（111）表面吸附的理论研究

基于第一性原理的密度泛函理论,利用密度泛函理论和周期平板模型相结合的方法,并使用MaterimalsStudio4.0软件中的Dmol 34.0程序包来模拟甲醇、CO、水在Pt(111)表面的吸附反应,计算出各位点的吸附能、态密度以及能带分析图.     

CH_3OD在Si(111)表面上的TDS研究

本文运用热脱吸附谱方法(TDS)研究了室温下CH_3OD在Si(Ⅲ)表面上的吸附,对所取得的H_2, HD及D_2的热脱吸附谱进行了分析和比较,并计算出它们的脱吸附能和预指数因子.     

Oxygen-mediated diffusion of oxygen vacancies on the TiO2(110) surface

Defects such as oxygen vacancies play a crucial role in the surface properties of transition metal oxides. By means of time-resolved, high-resolution scanning tunneling microscopy, we unraveled an adsorbate-mediated diffusion mechanism of oxygen vacancies on rutile TiO2(110). Adsorbed oxygen molecules mediate vacancy diffusion through the loss of an oxygen atom to a vacancy and the sequential capture of an oxygen atom from a neighboring bridging oxygen row, leading to an anisotropic oxygen vacancy diffusion pathway perpendicular to the bridging oxygen rows.     

Electron transfer-induced dynamics of oxygen molecules on the TiO2(110) surface

Diffusion of oxygen molecules on transition metal oxide surfaces plays a vital role for the understanding of catalysis and photocatalysis on these materials. By means of time-resolved scanning tunneling microscopy, we provide evidence for a charge transfer-induced diffusion mechanism for O2 molecules adsorbed on a rutile TiO2(110) surface. The O2 hopping rate depended on the number of surface donors (oxygen vacancies), which determines the density of conduction band electrons. These results may have implications for the understanding of oxidation processes on metal oxides in general.     

Elementary structural motifs in a random network of cytosine adsorbed on a gold(111) surface

Nonsymmetrical organic molecules adsorbed on solid surfaces may assemble into random networks, thereby providing model systems for organic glasses that can be directly observed by scanning tunneling microscopy (STM). We investigated the structure of a disordered cytosine network on a gold(111) surface created by thermal quenching, to temperatures below 150 K, of the two-dimensional fluid present on the surface at room temperature. Comparison of STM images to density functional theory calculations allowed us to identify three elementary structural motifs (zigzag filaments and five- and six-membered rings) that underlie the whole supramolecular random network. The identification of elementary structural motifs may provide a new framework for understanding medium-range order in amorphous and glassy systems.     

Atomic resolution of the silicon (111)-(7x7) surface by atomic force microscopy

Achieving high resolution under ultrahigh-vacuum conditions with the force microscope can be difficult for reactive surfaces, where the interaction forces between the tip and the samples can be relatively large. A force detection scheme that makes use of a modified cantilever beam and senses the force gradient through frequency modulation is described. The reconstructed silicon (111)-(7x7) surface was imaged in a noncontact mode by force microscopy with atomic resolution (6 angstroms lateral, 0.1 angstrom vertical).     

Energy dependence of abstractive versus dissociative chemisorption of fluorine molecules on the silicon (111)-(7x7) surface

Scanning tunneling microscopy and monoenergetic molecular beams have been used to obtain real-space atomic images of the competition between abstractive and dissociative chemisorption. The size distribution of Si-F adsorbates on the Si(111)-(7x7) surface was examined as a function of the incident translational energy of the F(2) molecules. For F(2) molecules with 0.03 electron volt of incident energy, the dominant adsorbate sites were isolated Si-F species. As an F(2) molecule with low translational energy collides with the surface, abstraction occurs and only one of the F atoms chemisorbs; the other is ejected into the gas phase. For F(2) molecules with 0.27 electron volt of incident energy, many adjacent Si-F adsorbates (dimer sites) were observed because F(2) molecules with high translational energy collide with the surface and chemisorb dissociatively so that both F atoms react to form adjacent Si-F adsorbates. For halogens with very high incident energy (0.5-electron volt Br(2)), dissociative chemisorption is the dominant adsorption mechanism and dimer sites account for nearly all adsorbates.     

Water diffusion and clustering on Pd(111)

The adsorption, diffusion, and clustering of water molecules on a Pd(111) surface were studied by scanning tunneling microscopy. At 40 kelvin, low-coverage water adsorbs in the form of isolated molecules, which diffuse by hopping to nearest neighbor sites. Upon collision, they form first dimers, then trimers, tetramers, and so on. The mobility of these species increased by several orders of magnitude when dimers, trimers, and tetramers formed, and decreased again when the cluster contained five or more molecules. Cyclic hexamers were found to be particularly stable. They grow with further exposure to form a commensurate hexagonal honeycomb structure relative to the Pd(111) substrate. These observations illustrate the change in relative strength between intermolecular hydrogen bonds and molecule-substrate bonds as a function of water cluster size, the key property that determines the wetting properties of materials.     

The Self-Assembly Mechanism of Alkanethiols on Au(111)

The self-assembly mechanism of alkanethiol monolayers on the (111) surface of gold was discovered with the use of an ultrahigh-vacuum scanning tunneling microscope. Monolayer formation follows a two-step process that begins with condensation of low-density crystalline islands, characterized by surface-aligned molecular axes, from a lower density lattice-gas phase. At saturation coverage of this phase, the monolayer undergoes a phase transition to a denser phase by realignment of the molecular axes with the surface normal. These studies reveal the important role of molecule-substrate and molecule-molecule interactions in the self-assembly of these technologically important material systems.     

Structure of the hydrated alpha-Al(2)O(3) (0001) surface

The physical and chemical properties of the hydrated alpha-Al(2)O(3) (0001) surface are important for understanding the reactivity of natural and synthetic aluminum-containing oxides. The structure of this surface was determined in the presence of water vapor at 300 kelvin by crystal truncation rod diffraction at a third-generation synchrotron x-ray source. The fully hydrated surface is oxygen terminated, with a 53% contracted double Al layer directly below. The structure is an intermediate between alpha-Al(2)O(3) and gamma-Al(OH)(3), a fully hydroxylated form of alumina. A semiordered oxygen layer about 2.3 angstroms above the terminal oxygen layer is interpreted as adsorbed water. The clean alpha-Al(2)O(3) (0001) surface, in contrast, is Al terminated and significantly relaxed relative to the bulk structure. These differences explain the different reactivities of the clean and hydroxylated surfaces.     

Identification of the products from the reaction of chlorine with the silicon(111)-(7x7) surface

The various products from the reaction of chlorine (Cl) with the adatom layer of the Si(111)-(7x7) surface have been identified with scanning tunneling microscopy (STM). Initially, a single Cl atom reacts with the adatom dangling bond. At higher surface coverage, additional Cl atoms insert themselves into the Si-Si backbonds between the adatom and rest-atom layers, producing adatoms that have reacted with two or three Cl atoms. These products are characterized by different registries with respect to the underlying rest layer and appear in STM images as adatoms of different sizes, consistent with the breaking of Si-Si backbonds and the formation ofnew Si-Cl bonds.     

C原子在金刚石(100)和(111)面的低能沉积

利用分子动力学模拟研究了低于室温下低能C原子碰撞金刚石(100)和(111)面的微观过程.模拟中采用Brenner导出的多体参数化势,并采用Langevin分子动力学方法模拟系统的退火过程.结果表明,在100 K温度下,当入射C原子能量降至0.1 eV时,易于在(111)面生长近完美的金刚石单层.对(100)面,需更高的能量形成类金刚石SP3杂化结构.

Abstract：

Microscopic processes for low-energy carbon atoms impacting on diamond (111) and (100) surfaces at temperature lower than room temperature are studied using molecular dynamics simulations. A realistic multibody parameterized potential developed by Brenner was used in the simulations. Langevin molecular dynamics was used to simulate the annealing process of the system under study. The results indicate that it is easy to grow a nearly perfect monolayer of diamond on the (111) surfaces when the incident energy of the carbon atoms is lowered to 0. 1 eV at 100 K. For (100) surface, on the other hand, higher incident energy is more favorable for forming diamondlike sp3 hybrids.     

El Nino/La Nina事件对许昌气候的影响

根据1971～2009年期间发生的El Nino/La Nina事件和许昌市气象资料,利用统计分析的方法分析了1971年以来许昌气温、降水、旱涝灾害与El Nino/La Nina事件之间的关系,初步揭示了El Nino/La Nina事件对许昌气候的影响。结果表明,许昌市39年来温度和降水均有升高的趋势;厄尔尼诺年平均气温比正常年份高0.1℃,平均降水量比正常年份少34mm,厄尔尼诺次年降水增加,降水量多于正常年份35.3mm;拉尼娜年气温上升且波动较大,拉尼娜发生年平均气温比正常年份高0.3℃,拉尼娜年降水量多于正常年份2.3mm,拉尼娜次年降水量少于正常年份15.5mm;从气温来讲,拉尼娜年许昌气温的上升幅度要大于厄尔尼诺年气温的上升幅度。从降水量上来讲,厄尔尼诺年对许昌降水量的影响度要大于拉尼娜年对降水的影响度。El/La事件对许昌市旱涝灾害影响显著,拉尼娜年发生大涝灾害的几率较大。     

Self-Assembly of n-Alkyl Thiols as Disulfides on Au(111)

A grazing incidence x-ray diffraction study of CH(3)(CH(2))(9)SH self-assembled on the (111) surface of gold revealed a disulfide head group structure, which provides a context in which to understand the structure and self-assembly process of this widely studied system. The structure consists of a nearly hexagonal two-dimensional arrangement of the hydrocarbon chains with a dimerization of the sulfur head groups (accommodated through a gauche bond), resulting in a S-S spacing of 2.2 angstroms. These results demonstrate the importance of internal molecular degrees of freedom in the templating of "soft" organic materials on inorganic substrates.     

表没食子儿茶素没食子酸酯（EGCG）生物活性研究进展

综述近年来国内外有关EGCG生物活性的研究进展,着重阐述EGCG在抗氧化、保护神经系统、抗肿瘤及保护心脑血管方面的活性,综述其在免疫、内分泌和代谢酶抑制方面的研究成果,展望这一研究领域的发展前景和发展方向,期望为茶多酚类物质深入研究及产品开发提供思路。     

用响应面法优化小球藻絮凝沉降工艺的研究

以氢氧化钙为絮凝剂,对海水小球藻Chlorella vulgaris絮凝工艺效果进行了试验研究。单因素试验结果表明,当絮凝时间为60⁸0 min、氢氧化钙添加量为0.680 min、氢氧化钙添加量为0.6⁰.8 g/L和藻液pH为80.8 g/L和藻液pH为8¹0时,最有利于小球藻的采收。在单因素试验的基础上,利用响应面法对小球藻的絮凝条件进行了优化,建立了二次回归模型。通过分析得出:各因素对小球藻采收率均有极显著性影响(P<0.01),影响次序为氢氧化钙添加量>絮凝时间>藻液pH;絮凝时间与藻液pH以及氢氧化钙添加量与藻液pH的交互作用对小球藻采收率均有极显著性影响(P<0.01)。利用回归方程预测小球藻的最佳絮凝条件,当絮凝时间为77 min、氢氧化钙添加量为0.7 g/L、小球藻液pH为9.3时,小球藻的采收率可达93.9%。     

(111)晶面暴露的NiO纳米催化剂的制备及其CO催化氧化性能

采用溶剂热法,以Ni(NO_3)_3·6H_2O、均苯三甲酸以及N,N-二甲基甲酰胺(DMF)为原料快速合成金属有机骨架材料Ni_3(BTC)_2·12H_2O晶体。以Ni_3(BTC)_2·12H_2O为前体,通过焙烧得到具有(111)面的NiO颗粒用于CO催化氧化反应,并与由硝酸镍热解得到的NiO(R)催化剂进行对比。通过X射线衍射(XRD)、N_2物理吸附-脱附、透射电子显微镜(TEM)以及X射线光电子能谱(XPS)等方法对具有(111)面的NiO颗粒的组成、结构和形貌进行表征。CO催化氧化结果表明,具有(111)面的NiO颗粒的催化活性优于普通NiO催化剂的催化活性。