A CO Adsorption Site Change Induced by Copper Substitution in a Ruthenium Catalyst for Enhanced CO Oxidation Activity

Ru is an important catalyst in many types of reactions. Specifically, Ru is well known as the best monometallic catalyst for oxidation of carbon monoxide (CO) and has been practically used in residential fuel cell systems. However, Ru is a minor metal, and the supply risk often causes violent fluctuations in the price of Ru. Performance‐improved and cost‐reduced solid‐solution alloy nanoparticles of the Cu‐Ru system for CO oxidation are now presented. Over the whole composition range, all of the Cu_xRu_1?x nanoparticles exhibit significantly enhanced CO oxidation activities, even at 70 at % of inexpensive Cu, compared to Ru nanoparticles. Only 5 at % replacement of Ru with Cu provided much better CO oxidation activity, and the maximum activity was achieved by 20 at % replacement of Ru by Cu. The origin of the high catalytic performance was found as CO site change by Cu substitution, which was investigated using in situ Fourier transform infrared spectra and theoretical calculations.     

Cobalt(II)-Catalyzed [4+2] Annulation of Picolinamides with Alkynes via C−H Bond Activation

A cobalt(II)-catalyzed [4+2] annulation of picolinamides with alkynes via C−H bond activation has been developed. The operationally simple annulation reaction allows for the synthesis of acyl-substituted 1H-benzoquinoline bearing multiple aromatic rings (up to 96 % yield) without co-oxidant or other oxidation factors under mild conditions. Several control experiments were carried out. This practical [4+2] annulation provides an efficient route to access highly functionalized compounds.     

黑龙江省矿区生态破坏与地质灾害及其防治

黑龙江省矿产分布情况和开发概况以及矿业开发在经济发展中占有重要地位 ;在矿业开发过程中引起的诸多生态破坏和地质灾害及其引起的危害 ,已引起高度重视 ;本文在综合论述黑龙江省矿区发展所带来各项利弊后提出了具体的防治对策。     

Direct and inverse problems for electromagnetic scattering by a doubly periodic structure with a partially coated dielectric

Consider the problem of scattering of electromagnetic waves by a doubly periodic Lipschitz structure. The medium above the structure is assumed to be homogenous and lossless with a positive dielectric coefficient. Below the structure there is a perfect conductor with a partially coated dielectric boundary. We first establish the well‐posedness of the direct problem in a proper function space and then obtain a uniqueness result for the inverse problem by extending Isakov's method. Copyright © 2009 John Wiley & Sons, Ltd.     

提高超声测距分辨力的分析与设计

本文分析了分辨力误差的定量关系，并以此为指导选择和设计超声发射，接收，测时等电路以及数字滤波方法，提亢超声测距的精度和分辩力。     

Theoretic calculation for understanding the oxidation process of 1,4-dimethoxybenzene-based compounds as redox shuttles for overcharge protection of lithium ion batteries

The effect of substituents on the oxidation potential for the one-electron reaction of 1,4-dimethoxybenzene was understood with a theoretical calculation based on density functional theory (DFT) at the level of B3LYP/6-311+G(d). It is found that the oxidation potential for the one-electron reaction of 1,4-dimethoxybenzene is 4.13 V (vs Li/Li(+)) and can be changed from 3.8 to 5.9 V (vs Li/Li(+)) by substituting electron-donating or electron-withdrawing groups for the hydrogen atoms on the aromatic ring. These potentials are in the range of the limited potentials for the lithium ion batteries using different cathode materials, and thus the substituted compounds can be selected as the redox shuttles for the overcharge prevention of these batteries. The oxidation potential of 1,4-dimethoxybenzene decreases when the hydrogen atoms are replaced with electron-donating groups but increases when replaced with electron-withdrawing groups. The further oxidation of these substituted compounds was also analyzed on the basis of the theoretic calculation.     

Binary clusters AuPt and Au6Pt: structure and reactivity within density functional theory

Within density functional theory with the general gradient approximation for the exchange and correlation, the bimetallic clusters AuPt and Au(6)Pt have been studied for their structure and reactivity. The bond strength of AuPt lies between those of Au(2) and Pt(2), and it is closer to that of Au(2). The Pt atom is the reactive center in both AuPt and AuPt(+) according to electronic structure analysis. AuPt(+) is more stable than AuPt. Au(6)Pt prefers electronic states with low multiplicity. The most stable conformation of Au(6)Pt is a singlet and has quasi-planar hexagonal frame with Pt lying at the hexagonal center. The doping of Pt in Au cluster enhances the chemical regioselectivity of the Au cluster. The Pt atom essentially serves as electron donor and the Au atoms bonded to the Pt atom acts as electron acceptor in Au(6)Pt. The lowest triplet of edge-capped rhombus Au(6)Pt clusters is readily accessible with very small singlet-triplet energy gap (0.32 eV). O(2) prefers to adsorb on Au and CO prefers to adsorb on Pt. O(2) and CO have stronger adsorption on AuPt than they do on Au(6)Pt. CO has a much stronger adsorption on AuPt bimetallic cluster than O(2) does. The adsorption of CO on Pt modifies the geometry of AuPt bimetallic clusters.     

Novel molecularly imprinted microsphere using a single chiral monomer and chirality-matching (S)-ketoprofen template

We designed and synthesized a cinchonine derivative to be used as a novel chiral monomer. It was employed in a dual role of functional monomer and cross-linking monomer, displaying multi-binding sites for the template (S)-ketoprofen. Monodisperse molecularly imprinted core-shell microspheres were prepared using surface imprinting method on silica gel. The results show a substantial synergistic effect in the enantioselective recognition, confirming our initial hypothesis. Computational simulation of the monomer and template pre-arrangement strongly supports our proposed chiral recognition mechanism for the imprinted microspheres.     

功能材料在蛋白质组研究中的应用进展

随着对蛋白质组鉴定深度、定量准确性及分析速度越来越高的要求,对蛋白质组学方法的研发提出了新的挑战。为了应对这些挑战,传统的蛋白质组学方法因其灵敏度低、准确性差以及耗时长等不足已经难以满足蛋白质组学研究领域不断提出的新需求。而将通过光、电、磁、热、化学、生化等作用合成具有特定功能的材料用于蛋白质组的研究,可以克服传统蛋白质组学分析技术的局限性,为蛋白质组学研究起到促进作用。该文对功能材料在蛋白质组研究中应用的新进展进行综述。