Design of a surface alloy catalyst for steam reforming

Detailed studies of elementary chemical processes on well-characterized single crystal surfaces have contributed substantially to the understanding of heterogeneous catalysis. Insight into the structure of surface alloys combined with an understanding of the relation between the surface composition and reactivity is shown to lead directly to new ideas for catalyst design. The feasibility of such an approach is illustrated by the synthesis, characterization, and tests of a high-surface area gold-nickel catalyst for steam reforming.     

木材表面化学特征的ESR与ESCA分析

用电子自旋共振波谱仪(ESR)和X—射线光电子能谱仪(ESCA)分析了经砂磨、紫外线幅射和浸提处理后木材表面化学特征的变化。结果表明:经过砂磨后,木材表面自由基含量增多,含氧官能团增多;在紫外光幅射下,木材表面自由基增加,但含氧官能基变化甚微;未经浸提的木材表面被脂肪酸所复盖。根据测试结果,对木材表面的机械化学反应和光氧化反应以及表面钝化的机制作了分析和讨论。     

Water at hydrophobic surfaces: weak hydrogen bonding and strong orientation effects

Vibrational studies that selectively probe molecular structure at CCl4/H2O and hydrocarbon/H2O interfaces show that the hydrogen bonding between adjacent water molecules at these interfaces is weak, in contrast to generally accepted models of water next to fluid hydrophobic surfaces that suggest strong hydrogen bonding. However, interactions between these water molecules and the organic phase result in substantial orientation of these weakly hydrogen-bonded water molecules in the interfacial region. The results have important implications for understanding water adjacent to hydrophobic surfaces and the penetration of water into hydrophobic phases.     

Atomic arrangements at metal surfaces

The termination of a solid induces changes in the locations of the outermost atoms of the solid. The changes can be minor or as dramatic as the rearrangement of the atoms into a different crystallographic group. Surface crystallography studies have determined that all surfaces are altered by forces induced at the solid-vacuum interface. At the least, the outermost atomic layers are displaced away from positions that they would have had in the bulk environment. Results from experimental and theoretical investigations for the Al(110) surface are discussed to illustrate present understanding of the surface atomic displacements. Some effects that the truncation- induced forces have on the surfaces of binary metal alloys are also discussed.     

Direct observation of chemical bond dynamics on surfaces

The dynamics of chemisorbed species as they swing to-and-fro on their adsorption sites may be directly observed with electron-stimulated desorption. The observation of the thermal disorder in adsorbate chemical bond directions, through studies of the thermal excitation of librational modes, allows one to visualize the potential energy surfaces controlling the structure and dynamics of adsorbates on single crystal metal and semiconductor surfaces. This information may be useful in understanding surface diffusion as well as the spatial aspects of surface chemical reactions.     

Quantum States and atomic structure of silicon surfaces

The electronic and geometric structures of surfaces are closely related to each other. Conventional surface science techniques can study one or the other, but not both at the same time. Recent developments in scanning tunneling microscopy have made it possible to study simultaneously the electronic and geometric structure of Si(111) and Si(001) surfaces. Surface states can be atomically resolved in space and energy; thus the electronic structure of single atoms on surfaces can be studied in detail. The various surface states observed on silicon surfaces are found to derive from different atomic-scale features in the surface geometric structure. Scanning tunneling microscopy has now bridged the gap between electronic and geometric structure, providing a unique opportunity to obtain a better understanding of many surface processes at the atomic level.     

Gas-phase ion chemistry

Progress has been made in the understanding of potential energy surfaces for unimolecular ion dissociations and ion-molecule reactions. With recent advances in instrumentation, many new techniques have been developed to generate and study ions, ion-molecule complexes, and large ionic clusters. Developments in ion spectroscopy have enabled considerable advances to be made in the determination of ion structures.     

Molecular interactions and hydrogen bond tunneling dynamics: some new perspectives

The recent development of tunable far-infrared lasers and other high-resolution spectroscopic probes of weakly bound clusters is having a significant impact on our understanding of intermolecular forces and on the complex quantum tunneling dynamics that occur in hydrogen-bonded systems. Far-infrared studies of a variety of interactions are discussed, including several prototypical water-hydrophobe complexes, the water trimer, and the ammonia dimer. Particular attention is paid to the inversion of spectroscopic data to yield detailed intermolecular potential energy surfaces. Investigations of nonpairwise additivity are also described.     

Near--Atomic Resolution Imaging of Ferroelectric Liquid Crystal Molecules on Graphite by STM

Near-atomic resolution images of a two-dimensional heteroepitaxial crystal composed of the relatively "functionally rich" chiral liquid crystal mesogen MDW 74 on graphite have been obtained by scanning tunneling microscopy (STM). This work is aimed at developing an improved understanding of the commercially crucial phenomenon of liquid crystal alignment by studying well-characterized surfaces. Herein is reported molecular-level characterization of the surface underlying a ferroelectric liquid crystal in situ, a requisite starting point for understanding the liquid crystal-solid interface at the molecular level. The results are also important in the context of developing a model for the molecular. origins of the contrast observed in STM images of organic monolayers on conductor surfaces. The data and analysis provide strong evidence that neither frontier orbital alone (highest occupied or lowest unoccupied molecular orbital) is sufficient to describe the observed tunneling efficiency.     

Scleractinian coral exoskeletons: surface microarchitecture and attachment scar patterns

Scanning electron microscopic studies have revealed the configurations of the growth surfaces of scleractinian coral exoskeletons. Skeletal surfaces exhibit profuse growths of minute elongate aragonite crystals which, on basal and mural surfaces, are punctuated by scars. It is suggested that these scars are sites of attachment for the specialized processes that connect the living tissues of polyps to the nonliving skeleton. Patterns formed by the attachment scars are taxonomically significant.     

Low-pressure, metastable growth of diamond and "diamondlike" phases

Diamond may be grown at low pressures where it is the metastable form of carbon. Recent advances in a wide variety of plasma and electrical discharge methods have led to dramatic increases in growth rates. All of these methods have certain aspects in common, namely, the presence of atomic hydrogen and the production of energetic carbon-containing fragments under conditions that support high mobilities on the diamond surface. Some understanding of the processes taking place during nucleation and growth of diamond has been achieved, but detailed molecular mechanisms are not yet known. Related research has led to the discovery of a new class of materials, the "diamondlike" phases. Vapor-grown diamond and diamondlike materials may have eventual applications in abrasives, tool coatings, bearing surfaces, electronics, optics, tribological surfaces, and corrosion protection.     

Biomaterial-centered infection: microbial adhesion versus tissue integration

Biomaterials are being used with increasing frequency for tissue substitution. Complex devices such as total joint replacements and the total artificial heart represent combinations of polymers and metal alloys for system and organ replacement. The major barriers to the extended use of these devices are the possibility of bacterial adhesion to biomaterials, which causes biomaterial-centered infection, and the lack of successful tissue integration or compatibility with biomaterial surfaces. Interactions of biomaterials with bacteria and tissue cells are directed not only by specific receptors and outer membrane molecules on the cell surface, but also by the atomic geometry and electronic state of the biomaterial surface. An understanding of these mechanisms is important to all fields of medicine and is derived from and relevant to studies in microbiology, biochemistry, and physics. Modifications to biomaterial surfaces at an atomic level will allow the programming of cell-to-substratum events, thereby diminishing infection by enhancing tissue compatibility or integration, or by directly inhibiting bacterial adhesion.     

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.     

Inducing and viewing the rotational motion of a single molecule

Tunneling electrons from the tip of a scanning tunneling microscope were used to induce and monitor the reversible rotation of single molecules of molecular oxygen among three equivalent orientations on the platinum(111) surface. Detailed studies of the rotation rates indicate a crossover from a single-electron process to a multielectron process below a threshold tunneling voltage. Values for the energy barrier to rotation and the vibrational relaxation rate of the molecule were obtained by comparing the experimental data with a theoretical model. The ability to induce the controlled motion of single molecules enhances our understanding of basic chemical processes on surfaces and may lead to useful single-molecule devices.     

Fast ion bombardment of ices and its astrophysical implications

Ices such as water, carbon dioxide, and methane are now known to be pervasive constituents of the solar system and probably of the interstellar medium as well. Many of these ices and ice-covered surfaces are exposed to bombardment by the energetic ions of space. Laboratory experiments have been carried out to study the effects of such bombardment. Surprisingly efficient erosion of ice layers is associated with electronic excitation of the ices by the ions. These results are a challenge to an understanding of the physical processes involved and have implications for a number of astrophysical problems of current interest.     

Low-Energy Electron Diffraction: Improved experimental methods provide new information on the structure of surfaces of solids

This discussion of a few preliminary experiments with nickel points out some of the potential uses of low energy electron diffraction in improving our understanding of many types of surface phenomena. The first, and probably the most basic use, is in the study of clean surfaces. As illustrated in this article, the physical properties of the surface layer of atoms may be totally unlike those in the bulk of the crystal. It is necessary to understand such phenomena before a thorough understanding of chemical effects on surfaces can be achieved. The adsorption of gases, oxidation and corrosion, and the formation of epitaxial layers can all be studied in great detail by low energy electron diffraction.     

Dyscalculia: from brain to education

Recent research in cognitive and developmental neuroscience is providing a new approach to the understanding of dyscalculia that emphasizes a core deficit in understanding sets and their numerosities, which is fundamental to all aspects of elementary school mathematics. The neural bases of numerosity processing have been investigated in structural and functional neuroimaging studies of adults and children, and neural markers of its impairment in dyscalculia have been identified. New interventions to strengthen numerosity processing, including adaptive software, promise effective evidence-based education for dyscalculic learners.     

Hidden fermi surface nesting and charge density wave instability in low-dimensional metals

The concept of hidden Fermi surface nesting was introduced to explain the general observation that certain low-dimensional metals with several partially filled bands exhibit charge density wave (CDW) instabilities, although their individual Fermi surfaces do not reveal the observed nesting vectors. This concept was explored by considering the Fermi surfaces of the purple bronze AMo(6)O(17) (A = sodium or potassium) and then observing the CDW spatial fluctuations expected from its hidden nesting on the basis of diffuse x-ray scattering experiments. The concept of hidden Fermi surface nesting is essential for understanding the electronic instabilities of low-dimensional metals.     

Interactions between the microbiota and the immune system

The large numbers of microorganisms that inhabit mammalian body surfaces have a highly coevolved relationship with the immune system. Although many of these microbes carry out functions that are critical for host physiology, they nevertheless pose the threat of breach with ensuing pathologies. The mammalian immune system plays an essential role in maintaining homeostasis with resident microbial communities, thus ensuring that the mutualistic nature of the host-microbial relationship is maintained. At the same time, resident bacteria profoundly shape mammalian immunity. Here, we review advances in our understanding of the interactions between resident microbes and the immune system and the implications of these findings for human health.