Probing the Local Reaction Environment During High Turnover Carbon Dioxide Reduction with Ag-Based Gas Diffusion Electrodes

Discerning the influence of electrochemical reactions on the electrode microenvironment is an unavoidable topic for electrochemical reactions that involve the production of OH⁻ and the consumption of water. That is particularly true for the carbon dioxide reduction reaction (CO₂RR), which together with the competing hydrogen evolution reaction (HER) exert changes in the local OH⁻ and H₂O activity that in turn can possibly affect activity, stability, and selectivity of the CO₂RR. We determine the local OH⁻ and H₂O activity in close proximity to a CO₂-converting Ag-based gas diffusion electrode (GDE) with product analysis using gas chromatography. A Pt nanosensor is positioned in the vicinity of the working GDE using shear-force-based scanning electrochemical microscopy (SECM) approach curves, which allows monitoring changes invoked by reactions proceeding within an otherwise inaccessible porous GDE by potentiodynamic measurements at the Pt-tip nanosensor. We show that high turnover HER/CO₂RR at a GDE lead to modulations of the alkalinity of the local electrolyte, that resemble a 16 m KOH solution, variations that are in turn linked to the reaction selectivity.     

Charge redistribution and a shortening of the Fe—As bond at the quantum critical point of SmO1–xFxFeAs

Many researchers have pointed out that there is a quantum critical point (QCP) in the F‐doped SmOFeAs system. In this paper, the electronic structure and local structure of the superconductive FeAs layer in SmO_1–xF_xFeAs as a function of the F‐doping concentration have been investigated using Fe and As K‐edge X‐ray absorption spectroscopy. Experiments performed on the X‐ray absorption near‐edge structure showed that in the vicinity of the QCP the intensity of the pre‐edge feature at the Fe‐edge decreases continuously, while there is a striking rise of the shoulder‐peak at the As edge, suggesting the occurrence of charge redistribution near the QCP. Further analysis on the As K‐edge extended X‐ray absorption fine structure demonstrated that the charge redistribution originates mostly from a shortening of the Fe—As bond at the QCP. An evident relationship between the mysterious QCP and the fundamental Fe—As bond was established, providing new insights on the interplay between QCP, charge dynamics and the local structural Fe—As bond in Fe‐based superconductors.     

面向数据挖掘的静态电源综合故障诊断研究

静态电源是机场桥载设备最重要的组成部件之一,应用非常广泛。然而,其产生的频发故障会造成设备利用率低、修复率时长和经济损失等问题,在基于桥载设备的安监系统上,提出了静态电源综合故障诊断方法,通过数据挖掘软件,建立了静态电源故障诊断预测模型。通过在线数据库测试结果表明得到了综合故障诊断方法在预测静态电源故障上显现的特点,得到了静态电源的未来状态,实现了对静态电源的实时故障进行预测,进而为解决故障提供方向和目标,最终达到降低经济损失最大化的目的。     

A local parallel superconvergence method for the incompressible flow by coarsening projection

In this article, we investigate a local parallel superconvergence method by coarsening projection for the incompressible Stokes flow. The method is a combination of the local superconvergence technique and the given framework of local parallel method. For the smooth subdomains, the local superconvergence method is applied in a higher order finite dimensional space corresponding to an appropriate coarse mesh on interior domain. Moreover, a useful and flexible local parallel method is designed to obtain the local parallel superconvergence results of presented method, which offset theoretical limitation of the model without the smoothness of the exact solution and a priori regularity of the underlying problem over the whole domain. © 2014 Wiley Periodicals, Inc. Numer Methods Partial Differential Eq 31: 1209–1223, 2015     

纳米银对铕配合物荧光性质的影响(英文)

研究了纳米银对稀土铕-吡啶-2,6-二羧酸配合物(Eu(Ⅲ)C7H5NO4,Eu(Ⅲ)DPA)的荧光性质的影响。随着纳米银浓度增加,荧光强度先增强而后逐渐下降。较大粒径的纳米银使Eu(Ⅲ)DPA荧光增强效率较大,且达到最大荧光增强效率所需的纳米银浓度较低。在高浓度Eu(Ⅲ)DPA溶液体系中,纳米银导致荧光猝灭。电偶极子跃迁发射荧光增强效率大于磁偶极子跃迁发射荧光增强效率。分析认为,纳米银对Eu(Ⅲ)DPA荧光性质的影响与表面等离子体共振与激发态荧光中心强烈耦合以及表面等离子体再吸收有关。同时,纳米银对铕配合物的不对称率有影响,其影响因素与局域电磁场增强,折射率以及配位场有关。     

Study of relaxation processes in polyethylene and polystyrene by positron annihilation

Relaxation processes in polyethylene (PE) and polystyrene (PS) were studied by positron annihilation technique. For PE, above the glass transition temperature, T_g, the size of free volumes and its concentration were increased by the micro-Brownian motion of molecules. For PS, local motions of molecules in backbone chains were found to start above 260 K. However, these local motions were suppressed by an interphenyl correlation. For both PE and PS, below 250–260 K, the formation probability of positronium atoms increased with decreasing temperature. This fact was assigned to the freezing in of the local motions of molecules. For PS, an onset of the local motions of molecules was observed above 100 K. These motions were expected to be associated with liberation of phenyl groups. © 1996 John Wiley & Sons, Inc.     

Short-range order in some polymer melts from X-ray diffraction

Wide-angle X-ray diffraction measurements were performed on polymer melts of isotactic and syndiotactic polypropylene (IPP and SPP), poly(ethylenepropylene) (PEP), polystyrene (PS), polyisobutylene (PIB), and polyethylene (PE), to study the dependence of the short-range structure of polymer liquids on chain architecture. Total structure functions, which comprise intra- and intermolecular contributions, were derived from the scattering data. The trivial Fourier components of the intramolecular structure (C(SINGLE BOND)>C ≃ 1.54 Å and C(SINGLE BOND)C(SINGLE BOND)C ≃ 2.55 Å) were subtracted from the total structure functions. The remaining functions contain only those intramolecular contributions dependent on the chain's conformational degrees of freedom, plus the intramolecular contributions. The structural differences between the polymers in momentum space are discerned only when the trivial components are subtracted. This subtraction also reduces the effects of truncation errors on Fourier transformation to real space. The short-range structure of PIB appears very different compared to all the others, which correlates with anomalies in a number of physical properties for this polymer. © 1996 John Wiley & Sons, Inc.     

NESTED GRID METHODS FOR AN OCEAN MODEL: A COMPARATIVE STUDY

In this paper a comparison is carried out between three correction methods for multigrid local mesh refinement in oceanic applications: FIC, LDC and the direct method (DM) proposed by Spall and Holland. This study is based on a nested primitive equation model developed by Laugier on the basis of the code OPA (LODYC). The external barotropic problem is solved using any of the three local grid correction algorithms yielding an interactive nested grid model. The non-linear elliptic equation for the barotropic streamfunction tendency is solved on two nested grids, called the global and the zoom grid, that interact between themselves. The zoom grid is entirely embedded within the global domain with a horizontal grid step ratio of 3:1. The computation on the global grid supplies the boundary conditions for the zoom grid region and the fine grid fields are used to correct the global coarse solution. The three local correction methods are tested on two problems relevant to oceanic circulation phenomena proposed by Spall and Holland: a barotropic modon and an anticyclonic vortex. The results show that the nesting technique is a very efficient way to solve these problems in terms of a gain in precision compared with the required CPU time. The two-domain model with local mesh refinement allows one both to manage effectively the open boundary conditions for the local grid and to correct the global solution thanks to the zoom solution. In the case of the modon propagation the three local correction methods provide approximately the same results. For the baroclinic vortex it appears that the two iterative methods are more efficient than the direct one.