Targeted Construction of Amorphous MoSx with an Inherent Chain Molecular Structure for Improved Pseudocapacitive Lithium-Ion Response

Owing to low ion/electron conductivity and large volume change, transitional metal dichalcogenides (TMDs) suffer from inferior cycle stability and rate capability when used as the anode of lithium-ion batteries (LIBs). To overcome these disadvantages, amorphous molybdenum sulfide (MoS_x) nanospheres were prepared and coated with an ultrathin carbon layer through a simple one-pot reaction. Combining X-ray photoelectron spectroscopy (XPS) with theoretical calculations, MoS_x was confirmed as having a special chain molecular structure with two forms of S bonding (S²⁻ and S₂²⁻), the optimal adsorption sites of Li⁺ were located at S₂²⁻. As a result, the MoS_x electrode exhibits superior cycle and rate capacities compared with crystalline 2H-MoS₂ (e.g., delivering a high capacity of 612.4 mAh g⁻¹ after 500 cycles at 1 A g⁻¹). This is mainly attributed to more exposed active S₂²⁻ sites for Li storage, more Li⁺ transfer pathways for improved ion conductivity, and suppressed electrode structure pulverization of MoS_x derived from the inherent chain-like molecular structure. Quantitative charge storage analysis further demonstrates the improved pseudocapacitive contribution of amorphous MoS_x induced by fast reaction kinetics. Moreover, the morphology contrast after cycling demonstrates the dispersion of active materials is more uniform for MoS_x than 2H-MoS₂, suggesting the MoS_x can well accommodate the volume stress of the electrode during discharging. Through regulating the molecular structure, this work provides an effective targeted strategy to overcome the intrinsic issues of TMDs for high-performance LIBs.     

微型气相色谱仪热导检测器放大电路设计

Agilent公司生产的Agilent 3000+系列色谱仪是微型气相色谱仪(micro GC)的典型代表,其热导检测器的信号放大电路和模数转换器(analog-to-digital convertor, ADC)存在功耗大、工作温度过高等不足.文中分析了micro GC电路的功能需求,从选用低噪声的24 bit Δ-Σ ADC ADS1255入手,设计了高共模电压容限、低噪声的全差分放大电路及其他外围电路,并且对全差分放大电路建立了噪声模型,计算了其噪声理论值,优化了系统设计参数.另外,还设计了一个测试平台,对所设计的全差分放大电路和ADC的性能进行了全面的测试评估,结果表明新设计的热导检测器放大电路与ADC的总噪声(以美国材料与试验协会(ASTM)标准值计)仅为1.25 μV,总功耗降低了3.7 W,满足micro GC的功能需求,而且可靠性高、体积小、结构简单,可用于新一代micro GC的研发和生产.     

Search of truncation of (N−1) electron basis containing full connected triple excitations in computing main and satellite ionization potentials via Fock‐space coupled cluster approach

A valence‐universal multireference coupled cluster (VUMRCC) theory, realized via the eigenvalue independent partitioning (EIP) route, has been implemented with full inclusion of triples excitations for computing and analyzing the entire main and several satellite peaks in the ionization potential spectra of several molecules. The EIP‐VUMRCC method, unlike the traditional VUMRCC theory, allows divergence‐free homing‐in to satellite roots which would otherwise have been plagued by intruders, and is thus numerically more robust to obtain more efficient and dependable computational schemes allowing more extensive use of the approach. The computed ionization potentials (IPs) as a result of truncation of the (N−1) electron basis manifold involving virtual functions such as 2h‐p and 3h‐2p by different energy thresholds varying from 5 to 15 a.u. with 1 a.u. intervals as well as thresholds such as 20, 25, and 30 a.u. have been carefully looked into. Cutoff at around 25 a.u. turns out to be an optimal threshold. Molecules such as C₂H₄ and C₂H₂ (X = D,T), and N₂ and CO (X = D,T,Q) with Dunning's cc‐pVXZ bases have been investigated to determine all main and 2h‐p shake‐up and 3h‐2p double shake‐up satellite IPs. We believe that the present work will pave the way to a wider application of the method by providing main and satellite IPs for some problematic N‐electron closed shell systems. © 2013 Wiley Periodicals, Inc.     

CH_3自由基和O（~3P）反应机理的量子化学研究

用分子轨道从头计算MP2（full）方法和密度泛函理论（DFT）中的B3LYP方法 研究了CH_3自由基和三线态O原子反应的微观机理，优化得到了反应途径上的反应 物、过渡态、中间体和产物的几何构型，通过振动分析对过渡态和中间体构型进行 了确认，在G3不平上计算了能量，同时用经典过渡态理论对该反应的绝对速率常数 进行了理论计算。研究结果表明：CH_3自由基与O（~3P）反应有四条不同的放热反 应通道，主反应通道为IM1→TS1→CH_2O + H，同时反应可彻底裂解生成CO, H_2 及H。     

DSC measurements on full thickness mice skin

Highly lipophilic basic drugs, the antiestrogens AE1 and AE2 shall be delivered transdermally. DSC as an additional tool in combination with classic investigation techniques should be used to clarify permeation enhancement. Skin treatment with pure solvents, polyethyleneglycol (PG) and dimethylisosorbide (DMI), slightly changed the phase transition temperatures. Formulations containing lauric acid markedly shifted these transitions to lower temperatures, indicating a lipid-fluidising action of lauric acid. In those cases an additional endothermic peak was observed around 40°C, which is attributed to the melting of crystalline lauric acid. Since the DSC program started at -20°C, it is very likely that lauric acid in the skin samples crystallized. A formulation of polyethyleneglycol and lauric acid leads to significantly higher deposition of lauric acid into the skin, in opposition to dimethylisosorbide/lauric acid formulation. These findings correspond to the results from our in-vitro permeation studies, where a significantly higher transdermal steady-state flux of lauric acid from polyethyleneglycol-formulation in comparison to dimethylisosorbide-formulation was observed. By this unique combination of polyethyleneglycol and lauric acid, the barrier is obviously modified in a way, which allows the highly lipophilic antiestrogens to permeate easily through the skin. So, from this formulation steady-state fluxes of AE-1 were observed, representing approximately the same value compared to the unhindered permeation through skin without stratum corneum. The grade of temperature shift on the skin lipids to lower temperatures can be correlated with softening effects and the enhancement potential of the formulation. This revised version was published online in July 2006 with corrections to the Cover Date.     

First isolation of a flavonoid from Juniperus procera using ethyl acetate extract

Phytochemical investigation of the ethyl acetate extract of the leaves of Juniperus procera growing in south Saudi Arabia Enemas region led to the isolation of a new flavonoid using different chromatographic methods (i.e. paper, thin layer and column chromatography). The isolated flavonoid was identified and established by m.p., ¹H-NMR, ¹³C-NMR, UV and MS spectral analysis. The isolated compound was identified as 3′,4′,3,7-tetrahydroxyflavone.     

基于影像处理的干涉测量相位重构研究

随着计算机技术和光电成像元件的发展,影像信息处理技术已经在无损检测、医学检测以及干涉测量等领域得到广泛应用。本文主要研究了影像信息在干涉测量领域的波前相位提取方法。干涉条纹图是干涉测量领域中影像信息的载体,在干涉条纹处理方面,针对空域卡雷算法的特点,提出一种基于影像处理的单幅闭合干涉条纹图相位重构新算法。在空域卡雷算法处理方法的基础上,利用迭代修正算法对干涉图相位进行二次逼近,实现了对单幅干涉条纹图的高精度相位重构。Matlab仿真结果表明,迭代修正后的相位残差降低了25.8%,表明该算法在空域卡雷算法的基础上能够有效提高相位重构精度,实现干涉测量领域中影像信息的高精度处理。     

物理化学课程“热化学”主题学习历程研究——化学师范生知识建构的文本分析

为深入了解地方性师范院校化学师范生知识建构习惯和水平，探讨他们在大学专业基础课程中的学习历程，以物理化学课程中以“融合科学读写特色”的“热化学”学案作为研究载体，研究对象在学案引导下开展自学活动，并在阅读教材和文献基础上进行科学写作。采用量表工具针对大学生自学效果和反思活动进行评价，并采用SOLO分类评价科学写作作品，采用KWL工具评价学生的科学阅读收获。结果发现研究对象学习动机不强，不擅长在新的学科知识学习中联系已有专业课程知识，基于文本学习的建构活动水平极低，可能是因为他们在应试背景下的基础知识并未形成体系，先修课程中并未培养元认知学习策略。     

一种基于本体的个性化搜索引擎模型

利用信息检索、本体和个性化搜索等相关知识,构建一种基于本体的个性化搜索引擎模型PSMBO.该模型由用户界面、查询请求处理模块、检索模块、查询结果处理模块、兴趣学习模块以及用户兴趣知识库和本体知识库七个部分组成.该模型在一定程度上提高了搜索引擎在查准率和查全率方面的性能.