单层MXene纳米片Ti2N电磁特性的过渡金属(Sc、V、Zr)掺杂效应

二维材料MXene纳米片由于具有较大的比表面积和较高的电子迁移率而受到广泛的关注。本文采用基于密度泛函理论的第一性原理计算,对单层MXene纳米片Ti₂N电磁特性的过渡金属(Sc、V、Zr)掺杂效应进行了系统研究。结果表明,所有过渡金属掺杂体系结合能均为负值,结构均稳定;其中Ti₂N-Sc体系的形成能为-2.242 eV,结构更易形成,且保持稳定;掺杂后Ti₂N-Sc、Ti₂N-Zr体系磁矩增大;此外,Ti₂N-Sc体系中保留了较高的自旋极化率,达到84.9%,可预测该体系在自旋电子学中具有潜在的应用价值。     

紫色球杆菌视紫红质光谱特性的机器学习研究

近年来，机器学习等人工智能技术被应用于蛋白质工程，其在蛋白质结构、功能预测、催化活性等研究中具有独特优势。在未知蛋白质结构的情况下，将蛋白质序列和功能特性与机器学习相结合，基于序列-活性关系（innovative sequence-activity relationship，ISAR）算法，将蛋白质氨基酸序列数字化，用快速傅里叶变换（fast four transform，FFT）进行预处理，再进行偏最小二乘回归建模，可在数据集较少情况下拟合得到最佳模型。通过机器学习对紫色球杆菌视紫红质（gloeobacter violaceus rhodopsin，GR）的突变体蛋白质氨基酸序列与光谱最大吸收波长进行建模，获得了最佳模型。用最佳索引LEVM760106建模得到的确定系数R² 为0.944，均方误差E为11.64。用小波变换进行的预处理，其R² 虽也约为0.944，但E大于11.64，不及FFT进行的预处理。方法较好地解决了蛋白质序列与功能特性之间的数学建模问题，在蛋白质工程中可为预测更优的突变体提供支持。     

Portfolio Selection and Risk Control for an Insurer With Uncertain Time Horizon and Partial Information in an Anticipating Environment

Methodology and Computing in Applied Probability - This paper is devoted to the study of an optimal investment and risk control problem for an insurer. The risky asset process and the insurance...     

Semiconducting Polymer Dots with Dual-Enhanced NIR-IIa Fluorescence for Through-Skull Mouse-Brain Imaging

Fluorescence probes in the NIR-IIa region show drastically improved imaging owing to the reduced photon scattering and autofluorescence in biological tissues. Now, NIR-IIa polymer dots (Pdots) are developed with a dual fluorescence enhancement mechanism. First, the aggregation induced emission of phenothiazine was used to reduce the nonradiative decay pathways of the polymers in condensed states. Second, fluorescence quenching was minimized by different levels of steric hindrance to further boost the fluorescence. The resulting Pdots displayed a fluorescence QY of ca. 1.7 % in aqueous solution, suggesting an enhancement of ca. 21 times in comparison with the original polymer in tetrahydrofuran (THF) solution. Small-animal imaging by using the NIR-IIa Pdots exhibited a remarkable improvement in penetration depth and signal to background ratio, as confirmed by through-skull and through-scalp fluorescent imaging of the cerebral vasculature of live mice.     

Precise Synthesis of Poly(thioester)s with Diverse Structures by Copolymerization of Cyclic Thioanhydrides and Episulfides Mediated by Organic Ammonium Salts

The precise synthesis of poly(thioester)s with diverse structures is still a significant challenge in the polymeric materials field. Herein, we report a novel approach to the synthesis of well‐defined poly(thioester)s by the controlled alternating copolymerization of cyclic thioanhydrides and episulfides induced by simple organic ammonium salts. Both the cation and anion have strong effects on the copolymerization. [PPN]OAc ([PPN]=bis(triphenylphosphine)iminium) with a bulky cation was proven to be efficient in initiating this polymerization, yielding poly(thioester)s with a completely alternating structure, controlled molecular weight, and narrow polydispersity. The poly(thioester) obtained from succinic thioanhydride and propylene sulfide is a typical semicrystalline material, possessing a high refractive index of up to 1.78. Because it uses readily available monomers, this method is expected to open up a new route to poly(thioester)s with diverse structures and properties.     

Study of nano‐Cu/SiO2 catalysts for highly selective hydrogenation of acetophenone

Hydrogenation of acetophenone over nano‐Cu/SiO₂ catalysts was investigated. The catalysts, prepared by a liquid precipitation method using various precipitating agents, were characterized using low‐temperature nitrogen adsorption, X‐ray diffraction, temperature‐programmed desorption of ammonia, hydrogen temperature‐programmed reduction, transmission electron microscopy and X‐ray photoelectron spectroscopy. It was found that the catalysts prepared by a homogeneous precipitation method had better activity and stability than those prepared by a co‐precipitation method. The catalyst prepared using urea as precipitating agent had well‐dispersed copper species, high surface area and abundant pore structure. The catalytic performance and mechanism of the Cu/SiO₂ catalysts were further studied. It was found that the activity and stability of the catalysts could be improved by adjusting the proportion of Cu⁺/(Cu⁺ + Cu⁰). The sample prepared using urea as precipitating agent presented higher activity and selectivity. Also, the catalyst prepared using urea maintained a high catalytic performance while being continuously used for 150 h under the optimal reaction conditions.     

Spatially modulated polarimetry based on a vortex retarder and Fourier analysis

We report a spatially modulated polarimetry scheme by using a zero-order vortex half-wave retarder(ZVHR)and a spatial Fourier analysis method.A ZVHR is employed to analyze the input polarized light and convert it into a vectorial optical field,and an analyzer is set after the ZVHR to form an hourglass intensity pattern due to the spatial polarization modulation.Then,the input light’s Stokes parameters can be calculated by spatial Fourier analysis of the hourglass pattern with a single shot.The working principle of the polarimeter has been analyzed by the Stokes-Mueller formalism,and some quantitative measuring experiments of different polarization states have been demonstrated.The experimental results indicate that the proposed polarimeter is accurate,robust,and simple to use.     

水化硅酸钙纳米压痕分子动力学模拟方法优化

针对水化硅酸钙纳米压痕模型忽视了压头与基底之间相互作用的问题，由尺寸差异引起的金刚石压头难以计算的问题，以及Wittmann模型无法得到实际接触面积的问题，提出了新的模型与计算方法．结合分子动力学方法，采用金刚石压头-Wittmann模型基底的组合方式构建无定形态水化硅酸钙纳米压痕试验模型．在建模阶段，考虑到压头模型与基底模型粒子间尺寸差异，提出了等比例替换模型，通过公式推导并就不同尺寸模拟结果验证了等比例替换模型的可行性．在计算阶段，提出了局部前处理的弛豫方法进行模拟．确定最大荷载位置处的接触面积为546 nm2，进而求出水化硅酸钙模型硬度H为0.84 GPa、折合模量Er为30.52 GPa．并通过纳米压痕试验，验证了模拟结果的准确性，证明了模型的科学性，对今后水化硅酸钙(C-S-H)纳米层面的模拟具有重要借鉴意义．     

Construction of Cyclobutanes by Multicomponent Cascade Reactions in Homogeneous Solution through Visible-Light Catalysis

[2+2] Photocycloaddition of two olefins is a general method to assemble the core scaffold, cyclobutane, found in numerous bioactive molecules. A new approach to synthesize cyclobutanes through multicomponent cascade reactions by merging aldol reaction and Witting reaction with visible-light-induced [2+2] cycloaddition is reported. An array of cyclobutanes with high selectivity has been achieved from commercially available aldehydes, ketones (or phosphorus ylide), and olefins with visible-light irradiation of a catalytic amount of (fac-tris(2-phenylpyridinato-C₂,N)iridium) ([Ir(ppy)₃]) at room temperature. Control experiments and spectroscopic studies revealed that the triplet–triplet energy transfer from the excited [Ir(ppy)₃]* to enones, generated in situ from aldehyde and ketone or aldehyde and phosphorus ylide, is responsible for these simple and efficient muticomponent transformations.     

热熔还原法制备超硬复合相氮化碳及其工艺探索

本文采用热熔还原法,以聚氯乙烯、氯化铵、氧化铁为原料制备复合超硬相氮化碳(α/β-C3 N4).采用X射线衍射仪(XRD)、扫描电子显微镜(SEM)以及透射电子显微镜(TEM)对样品进行表征.在此基础上分析了不同温度和原料配比下合成复合相C3 N4的物相组成及形貌变化.结果表明样品形貌随着原料配比的不同在颗粒、棒状、纳米线之间转变.当C、N和Fe之间摩尔比为3:4:0.4时,所制备出的样品呈纳米线状,纳米线的直径约为15 nm,结晶性良好.而在其它配比下,只能获得棒状或颗粒状α/β复合相C3 N4.