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1.
SO2在Ni(111)表面分解吸附的理论研究 总被引：1，自引：0，他引：1
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. 相似文献
2.
A recently designed single-crystal surface calorimeter has been deployed to measure the energy difference between two solid surface structures. The clean Pt{100} surface is reconstructed to a stable phase in which the surface layer of platinum atoms has a quasi-hexagonal structure. By comparison of the heats of adsorption of CO and of C(2)H(4) on this stable Pt{100}-hex phase with those on a metastable Pt{100}-(1x1) surface, the energy difference between the two clean phases was measured as 20 +/- 3 and 25 +/- 3 kilojoules per mole of surface platinum atoms. 相似文献
3.
The atomic force microscope (AFM) was used to image an electrode surface at atomic resolution while the electrode was under potential control in a fluid electrolyte. A new level of subtlety was observed for each step of a complete electrochemical cycle that started with an Au(111) surface onto which bulk Cu was electrodeposited. The Cu was stripped down to an underpotential-deposited monolayer and finally returned to a bare Au(111) surface. The images revealed that the underpotential-deposited monolayer has different structures in different electrolytes. Specifically, for a perchloric acid electrolyte the Cu atoms are in a close-packed lattice with a spacing of 0.29 +/- 0.02 nanometer (nm). For a sulfate electrolyte they are in a more open lattice with a spacing of 0.49 +/- 0.02 nm. As the deposited Cu layer grew thicker, the Cu atoms converged to a (111)-oriented layer with a lattice spacing of 0.26 +/- 0.02 nm for both electrolytes. A terrace pattern was observed during dissolution of bulk Cu. Images were obtained of an atomically resolved Cu monolayer in one region and an atomically resolved Au substrate in another in which a 30 degrees rotation of the Cu monolayer lattice from the Au lattice is clearly visible. 相似文献
4.
Inelastic electron tunneling spectroscopy at low temperatures was used to investigate vibrations of Au(111) and Cu(111). The low-energy peaks at 9 millielectron volts (meV) on Au(111) and 21 meV on Cu(111) are attributed to phonons at surfaces. On Au(111), the phonon energy is not influenced by the different stacking of the surface atoms, but it is considerably influenced by different atomic distances within the surface layer. The spatial variation of the phonon excitation is measured in inelastic electron tunneling maps on Au(111), which display atomic resolution. This atomic resolution is explained in terms of site-specific phonon excitation probabilities. 相似文献
5.
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。 相似文献
6.
Quantification of the influence of surface structure on C--h bond activation by iridium and platinum
The trapping-mediated dissociative chemisorption of ethane on the closest packed Ir(111) surface has been investigated, and the activation energy and preexponential factor of the surface reaction rate coefficient have been measured. These results are compared to those of ethane activation on Pt(111) and on the missing row reconstructed Ir(110)-(1x2) and Pt(110)-(1x2) surfaces, allowing a quantitative determination of the effect surface structure has on the catalytic activation of C-H bonds. In the order Pt(111), Pt(110)-(1x2), Ir(111), and Ir(110)-(1x2), the activation energies for the dissociative chemisorption of ethane are 16.6, 10.5, 10.3, and 5.5 kilocalories per mole, demonstrating that the electronic and geometric effects are of approximately equal importance for ethane activation on these catalysts. 相似文献
7.
竹材化学成分分析和表面性能表征 总被引：5，自引：0，他引：5
系统地研究了不同竹龄、部位毛竹(Phgllochysheterocyclavar.pubscense)化学成分的差异;应用化学光电子能谱仪(ESCA)和红外光谱(FTIR)对竹材的表面性能进行了分析表征。结果表明:不同竹龄竹材抽提物差异较大;竹材从根部到梢部,pH值逐渐增加;从竹青到竹黄,pH值逐渐降低;竹青表面的氧原子大于竹黄表面氧原子的比例;竹材的表面主要以木质素和各种抽提物为主,而纤维素和半纤维素含量明显低于木质素和抽提物;靠近竹青处的竹材表面的半纤维素含量低于竹黄,竹青的表面的羟基震动强于竹黄,且竹青表面的活性自由羟基的数量高于竹黄表面。 相似文献
8.
The prohibitive cost of platinum for catalyzing the cathodic oxygen reduction reaction (ORR) has hampered the widespread use of polymer electrolyte fuel cells. We describe a family of non-precious metal catalysts that approach the performance of platinum-based systems at a cost sustainable for high-power fuel cell applications, possibly including automotive power. The approach uses polyaniline as a precursor to a carbon-nitrogen template for high-temperature synthesis of catalysts incorporating iron and cobalt. The most active materials in the group catalyze the ORR at potentials within ~60 millivolts of that delivered by state-of-the-art carbon-supported platinum, combining their high activity with remarkable performance stability for non-precious metal catalysts (700 hours at a fuel cell voltage of 0.4 volts) as well as excellent four-electron selectivity (hydrogen peroxide yield <1.0%). 相似文献
9.
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. 相似文献
10.
Cossaro A Mazzarello R Rousseau R Casalis L Verdini A Kohlmeyer A Floreano L Scandolo S Morgante A Klein ML Scoles G 《Science (New York, N.Y.)》2008,321(5891):943-946
The structure of self-assembled monolayers (SAMs) of long-chain alkyl sulfides on gold(111) has been resolved by density functional theory-based molecular dynamics simulations and grazing incidence x-ray diffraction for hexanethiol and methylthiol. The analysis of molecular dynamics trajectories and the relative energies of possible SAM structures suggest a competition between SAM ordering, driven by the lateral van der Waals interaction between alkyl chains, and disordering of interfacial Au atoms, driven by the sulfur-gold interaction. We found that the sulfur atoms of the molecules bind at two distinct surface sites, and that the first gold surface layer contains gold atom vacancies (which are partially redistributed over different sites) as well as gold adatoms that are laterally bound to two sulfur atoms. 相似文献
11.
应用分子动力学方法模拟研究了Re在Ni和Ni3Al中的分布及其对材料微结构的影响.研究发现,Re的添加量影响Ni和Ni3Al晶体中空位的产生,但Re在Ni中对体系结构的破坏程度小于其在Ni3Al中占据Ni位时的程度.在Ni中,Re添加量较少且增大空位比时,其结构依然能保持稳定;随着Re数目的增多,空位比的增大,其影响逐渐变得明显.Re在Ni3Al中占据Ni,Re含量或空位比较小时,结构皆会出现局部不稳定.随着Re添加量的增多,结构的破坏程度加剧.然而Re占据Ni3Al中的Al位时其结构并未发生明显的变化,直至Re的添加量大至1%和空位比增至1%~1.5 % 时体系中才出现局部不稳定.相比而言,Re置换Al比置换Ni时对体系结构的影响较弱,在Ni3Al中Re占据Al位比占据Ni位更稳定. 相似文献
12.
森林地表死可燃物对森林火灾具有重要影响,研究地表死可燃物含水率对林火管理具有重要意义。以内蒙古大兴安岭不同地区不同林型地表死可燃物含水率为研究对象,利用2004年秋季防火期至2017年春季防火期大兴安岭林区(根河市、鄂伦春旗、牙克石市、阿尔山市)林分下地表死可燃物含水率数据,运用SPSS软件分析主要火环境因子对地表死可燃物含水率的影响。结果表明:(1)林中气温、林中相对湿度、枯枝落叶层质量、枯枝落叶层温度以及林内灌木盖度是影响地表死可燃物含水率变化的重要因子。(2)各地区春季与秋季、春季与全年地表死可燃物含水率预测的平均绝对误差和平均相对误差差异均不显著(P>0.05),而秋季与全年的平均绝对误差和平均相对误差均极显著(P<0.01),说明秋季防火期预测模型精度优于春季防火期预测模型精度。地表死可燃物含水率预测,需要根据不同防火期的特点建立不同的预测模型,并相对应地引入更具有显著性影响的火环境因子,为林火预测预报提供更精准的参考。 相似文献
13.
[目的]分析珲春市苹果梨主产区土壤微量元素的地球化学特征。[方法]在吉林省珲春市苹果梨果品基地采集32个表层土样和3个剖面土样,研究了微量元素在表层土壤中的含量及在土壤剖面中土壤地球化学特征。[结果]土壤微量元素Cr(K=0.894)和Co(0.904)平均含量与全国土壤平均值基本相当;As(0.341)、Hg(0.550)、Cu(0.659)、Ni(0.677)、Se(0.702)、Cd(0.774)和Zn(0.812)低于全国土壤平均值;Pb(1.029)的高于全国土壤平均值。在3个剖面中,As、Cr、Co、Cu、Zn和Ni呈现出底土层>心土层>表土层的趋势;Cd呈现出表土层>底土层>心土层;Hg和Pb呈现出底土层>表土层>心土层;而Se基本呈现出下部含量高于上部。[结论]该区表层土壤大部分微量元素含量较低;在3层剖面中未表现出明显的特征。 相似文献
14.
The addition of a small number of lead atoms to a germanium(111) surface reduces the energy barrier for activated processes, and with a tunneling microscope it is possible to observe concerted atomic motions and metastable structures on this surface near room temperature. The formation and annihilation of these metastable structural surface excitations is associated with the shift in position of large numbers of germanium surface atoms along a specific row direction like beads on an abacus. The effect provides a mechanism for understanding the transport of atoms on a semiconductor surface. 相似文献
15.
The [As@Ni12@As20]3- ion was prepared from As7(3-) and Ni(COD)2 in ethylenediamine solutions and isolated as the Bu4P+ salt (As, arsenic; Ni, nickel; COD, cyclooctadiene; Bu, butyl; P, phosphorus). The anion contains an icosahedral [Ni12(mu12-As)]3- fragment that resides at the center of an As20 dodecahedral (fullerene) cage to give an onion-skin-like [As@Ni12@As20]3- cluster with Ih point symmetry. The icosahedron and pentagonal dodecahedron are reciprocal platonic solids, and the 32 surface atoms form a dimpled geodesic sphere composed of 60 triangular faces. In the gas phase, the [As@Ni12@As20]3- ion sequentially loses all 21 As atoms to form a series of Ni12As(21-x) clusters where 0 相似文献
16.
妙峰山油松林分结构与地表潜在火行为相关性分析 总被引：1，自引：1，他引：0
17.
Studies in heterogeneous catalysis have long speculated on or have provided indirect evidence for the role of hydrogen embedded in the catalyst bulk as a primary reactant. This report describes experiments carried out under single-collision conditions that document the distinctive reactivity of hydrogen embedded in the bulk of the metal catalyst. Specifically, the bulk H atom is shown to be the reactive species in the hydrogenation of CH(3) adsorbed on Ni(111) to form CH(4), while the H atoms bound to the surface were unreactive. These results unambiguously demonstrate the importance of bulk species to heterogeneous catalytic chemistry. 相似文献
18.
The miniaturization of magnetic devices toward the limit of single atoms calls for appropriate tools to study their magnetic properties. We demonstrate the ability to measure magnetization curves of individual magnetic atoms adsorbed on a nonmagnetic metallic substrate with use of a scanning tunneling microscope with a spin-polarized tip. We can map out low-energy magnetic interactions on the atomic scale as evidenced by the oscillating indirect exchange between a Co adatom and a nanowire on Pt(111). These results are important for the understanding of variations that are found in the magnetic properties of apparently identical adatoms because of different local environments. 相似文献
19.
为了研究林下可燃物含水率的空间异质性状况,在东北林业大学老爷岭生态站附近对落叶松林下地表可燃物按试验地的坡位分3个方向进行取样。其中:沿坡上至坡下定为垂直方向,与之垂直的方向定为水平方向,垂直方向和水平方向的夹角平分线方向定为斜向。对每个方向凋落物层和腐殖质层分层取样,并计算含水率,利用常规统计和地统计学中的半方差分析处理数据。研究结果表明,可燃物含水率相对变异较大的是斜向样带,变异系数为0.46。除水平方向的凋落物层可燃物外,其他样带可燃物含水率都有明显的空间相关性,斜向凋落物层基台值最大(1.632),总体上看,凋落物层可燃物含水率的异质性程度比腐殖质层高。可燃物含水率在3个方向半方差与距离相关性高,具有明显的各向异性。其中,凋落物层各向异性十分明显,腐殖质层各向异性变异复杂近不明显。通过模拟取样估测样地总体含水率,结果表明:控制取样间隔距离可以提高取样精度,在取样间隔距离为2～8 m、取样强度在7个以上时,标准误差已经减少至10%以下;随机取样需要更大的取样强度且误差较大,不具优越性。 相似文献
20.
Bimetallic electrodes are used in a number of electrochemical processes, but the role of particular arrangements of surface metal atoms (ensembles) has not been studied directly. We have evaluated the electrochemical/catalytic properties of defined atomic ensembles in atomically flat PdAu(111) electrodes with variable surface stoichiometry that were prepared by controlled electrodeposition on Au(111). These properties are derived from infrared spectroscopic and voltammetric data obtained for electrode surfaces for which the concentration and distribution of the respective metal atoms are determined in situ by atomic resolution scanning tunneling microscopy with chemical contrast. Palladium monomers are identified as the smallest ensemble ("critical ensemble") for carbon monoxide adsorption and oxidation, whereas hydrogen adsorption requires at least palladium dimers. 相似文献