Key Role of a-Top CO on Terrace Sites of Metallic Pd Clusters for CO Oxidation

Pd-based catalysts are the most widely used for CO oxidation because of their outstanding catalytic activity and thermal stability. However, fundamental understanding of the detailed catalytic processes occurring on Pd-based catalysts under realistic conditions is still lacking. In this study, we investigated CO oxidation on metallic Pd clusters supported on Al₂O₃ and SiO₂. High-angle annular dark-field scanning transmission electron microscopy revealed the formation of similar-sized Pd clusters on Al₂O₃ and SiO₂. In contrast, CO chemisorption analysis indicated a gradual change in the dispersion of Pd (from 0.79 to 0.2) on Pd/Al₂O₃ and a marginal change in the dispersion (from 0.4 to 0.24) on Pd/SiO₂ as the Pd loading increased from 0.27 to 5.5 wt %; these changes were attributed to differences in the metal-support interactions. Diffuse reflectance infrared Fourier-transform spectroscopy revealed that fewer a-top CO species were present in Pd supported on Al₂O₃ than those in Pd supported on SiO₂, which is related to the morphological differences in the metallic Pd clusters on these two supports. Despite the different dispersion profiles and surface characteristics of Pd, O₂ titration demonstrated that linearly bound CO (with an infrared signal at 2090 cm⁻¹) reacted first with oxygen in the case of CO-saturated Pd on Al₂O₃ and SiO₂, which suggests that a-top CO on the terrace site plays an important role in CO oxidation. The experimental observations were corroborated by periodic density functional calculations, which confirmed that CO oxidation on the (111) terrace sites is most plausible, both kinetically and thermodynamically, compared to that on the edge or corner sites. This study will deepen the fundamental understanding of the effect of Pd clusters on CO oxidation under reaction conditions.     

Macroscopic Polarization Change of Mononuclear Valence Tautomeric Cobalt Complexes Through the Use of Enantiopure Ligand

The crystallization of a complex having electron transfer properties in a polar space group can induce the polarization switching of a crystal in a specific direction, which is attractive for the development of sensors, memory devices, and capacitors. Unfortunately, the probability of crystallization in a polar space group is usually low. Noticing that enantiopure compounds crystallize in Sohncke space groups, this paper reports a strategy for the molecular design of non-ferroelectric polarization switching crystals based on the use of intramolecular electron transfer and chirality. In addition, this paper describes the synthesis of a mononuclear valence tautomeric (VT) cobalt complex bearing an enantiopure ligand. The introduction of enantiomer enables the crystallization of the complex in the polar space group (P2₁). The polarization of the crystals along the b-axis direction is not canceled out and the VT transition is accompanied by a change in the macroscopic polarization of the polar crystal. Polarization switching via electron transfer is realized at around room temperature.     

A Category of Restricted Modules for the Ovisenko-Roger Algebra

In this paper, we study a category of restricted modules for the Ovsienko-Roger algebra, which is an extension of the Virasoro algebra of its tensor density module of degree one. We construct and characterize simple modules in this category and give natural free field realizations of certain restricted modules using the Weyl vertex algebra.

     

Transition Metal Doping Induces Ti3+ to Promote the Performance of SrTiO3@TiO2 Visible Light Photocatalytic Reduction of CO2 to Prepare C1 Product.

Transition metal Fe, Co, Ni and Cu doped strontium titanate-rich SrTiO₃@TiO₂ (STO@T) materials were prepared by hydrothermal method. The prepared doped materials exhibit better photocatalytic CO₂ reduction to CH₄ ability under visible light conditions. Among them, Fe-doped and undoped SrTiO₃@TiO₂ under visible light conditions CO₂ reduction products only CO, while M-STO@T (M=Co, Ni, Cu) samples converted CO₂ to CH₄. The average methane yield of Ni-doped STO@T samples are as high as 73.85 μmol g⁻¹ h⁻¹. The production of methane is mainly due to the increase in the response of the doped samples to visible light. And the increase in the separation rate of photogenerated electrons and holes and the efficiency of electron transport caused by the generation of impurity levels. The impurity level caused by Ti³⁺ plays an important role in the production of methane by CO₂ visible light reduction. Ni doping effectively improves the photocatalytic performance of STO@T and CO₂ reduction mechanism were explained.     

A luminescent Zn(II)-Containing Complex: Selective Sensing of Cr(VI) Anion and Application Values on Tuberculosis Care Through Increasing the Antibacterial Response of Macrophages

Journal of Fluorescence - A new Zn(II)-bearing metal-organic framework (MOF), namely, {[Zn2(L)2(H2O)]·8H2O·DMF}n (1) has been generated via applying...     

零误差计算

研究采用有误差的数值计算来获得无误差的准确值具有重要的理论价值和应用价值.这种通过近似的数值方法获得准确结果的计算被称为零误差计算.本文首先指出,只有一致离散集合中的数才能够开展零误差计算,即有非零隔离界的数集,这也是"数"可以进行零误差计算的一个充要条件.以此为基本出发点,本文分析代数数零误差计算的最低理论精度,该精度对应于恢复近似代数数的准确值时必要的误差控制条件,但由于所采用恢复算法的局限性,这一理论精度往往不能保证成功恢复出代数数的准确值.为此,本文给出采用PSLQ (partial-sum-LQ-decomposition)算法进行代数数零误差计算所需的精度控制条件,与基于LLL (Lenstra-Lenstra-Lovász)算法相比,该精度控制条件关于代数数次数的依赖程度由二次降为拟线性,从而可降低相应算法的复杂度.最后探讨零误差计算未来的发展趋势.     

Preparation and Properties of Sr3B2O6:Dy3+, Eu3+ White Phosphors Using the High-Temperature Solid-State Method

Journal of Applied Spectroscopy - Sr3B2O6:Dy3+, Eu3+ single-matrix white-light-emitting materials are prepared using the high-temperature solid-state method. The microstructure, emission spectrum,...     

Electro-assisted Molecular Assembly Giving Atomic-Scale Catalytic Active-Site Detection

The artificially accurate design of nonmetal electrocatalysts’ active site has been a huge challenge because no pure active species with the specific structure could be strictly controlled by traditional synthetic methods. Species with a multiconfiguration in the catalyst hinder identification of the active site and the subsequent comprehension of the reaction mechanism. We have developed a novel electro-assisted molecular assembly strategy to obtain a pure pentagon ring on perfect graphene avoiding other reconstructed structures. More importantly, the active atom was confirmed by the subtle passivation process as the topmost carbon atom. Recognition of the carbon-defect electrocatalysis reaction mechanism was first downsized to the single-atom scale from the experimental perspective. It is expected that this innovative electro-assisted molecular assembly strategy could be extensively applied in the active structure-controlled synthesis of nonmetal electrocatalysts and verification of the exact active atom.     

Hybrid control strategy of delayed neural networks and its application to sampled-data systems: an impulsive-based bilateral looped-functional approach

Nonlinear Dynamics - In this work, the problem of hybrid control strategy for delayed neural networks is investigated via an impulsive-based bilateral looped-functional (IBBLF) approach. Firstly, a...