ASP服务基础平台的研究与开发

随着科学技术的进步与发展,ASP服务基础平台的研究与开发也受到了广泛的关注。本文主要对ASP服务基础平台体系结构、ASP服务基础平台的研究与开发进行探析。     

Pentapnictogen heterocyclic monoanions: Structure,stability, and aromaticity

Inorganic planar ring-shape molecules with 4n + 2 π electrons are always the focus of experimental synthesis and theoretical research due to their potential aromaticity and stability. In this work, the whole series of five-membered heterocycle monoanions X _nY_5-n⁻ (X, Y = group 15 elements; n = 1-4) were thoroughly investigated by means of density functional theory calculations. They all have large formation energies and HOMO-LUMO gap energies, suggesting the potential thermodynamic and kinetic stability. Their aromaticities are comparable to that of typical aromatic hydrocarbons. Their thermal stabilities were firmly established by the ab initio molecular dynamics simulations. As most of them are predicted for the first time, their various spectra were simulated for experimental characterization. Furthermore, we demonstrate that these five-membered cyclic anions can be employed as η⁵-ligand to construct novel all-inorganic metallocenes, which may serve as the building blocks of low-dimensional nanomaterials.     

基于感知域测量值的自适应压缩采样方法

现有的自适应采样方法需要在采集端获得原始信号,这在实际的蒸发波导相关气象要素压缩感知过程中不易实现。针对这一问题,提出了一种以测量值数据特征为依据的采样率自适应设定方法。该方法以能量表征各信号块的重要性,以观测值能量近似估计原信号块能量,根据感知域中测量值的能量变化自适应地为各块设定采样数目。理论分析和实验表明,该方法的重构性能优于传统自适应方法,相同采样率下可获得更高的重构信噪比。     

SVGLR:全新的长读测序基因分型算法

文中基于三代测序数据提出了一种动态规划的基因分型算法。首先,根据改进的Needleman-Wunsch序列比对算法将基因组中所有变异的序列分别进行比对,根据比对矩阵生成用于分类的匹配向量序列。然后,提出序列分类算法,根据分类结果计算基因型,确定变异的合子性。在公开数据集上,使用该算法进行基因分型实验,实验结果表明该算法的精确率和F1指标均有所提高,有着较好的基因分型结果。     

Single Atoms of Iron on MoS2 Nanosheets for N2 Electroreduction into Ammonia

Efforts have been devoted to achieving a highly efficient artificial synthesis of ammonia (NH₃). Reported herein is a novel Fe-MoS₂ catalyst with Fe atomically dispersed onto MoS₂ nanosheets, imitating natural nitrogenase, to boost N₂ electroreduction into NH₃ at room temperature. The Fe-MoS₂ nanosheets exhibited a faradic efficiency of 18.8 % with a yield rate of 8.63 μg mg_cat.⁻¹ h⁻¹ for NH₃ at −0.3 V versus the reversible hydrogen electrode. The mechanism study revealed that the electroreduction of N₂ was promoted and the competing hydrogen evolution reaction was suppressed by decorating the edge sites of S in MoS₂ with the atomically dispersed Fe, resulting in high catalytic performance for the electroreduction of N₂ into NH₃. This work provides new ideas for the design of catalysts for N₂ electroreduction and strengthens the understanding about N₂ activation over Mo-based catalysts.     

含吗啉基片段的水杨醛席夫碱类化合物的合成及其淬灭1,1-二苯基-2-三硝基苯肼自由基性能

通过3-氟-4-吗啉基苯胺和取代水杨醛缩合反应,合成了14个含吗啉基片段水杨醛席夫碱类化合物(Ⅰa-Ⅰn)。通过核磁共振波谱仪(NMR)、傅里叶变换红外光谱仪(FTIR)、液相色谱-质谱联用仪(LC-MS)和元素分析等技术手段研究了产物的结构和淬灭1,1-二苯基-2-三硝基苯肼(DPPH)自由基的活性。 结果表明,在0.02~0.10 g/L,所有化合物均表现出一定的淬灭DPPH自由基活性。 其中,化合物Ⅰd和Ⅰf表现出较为优异的性能,化合物Ⅰd的活性在30%~55%,化合物Ⅰf的活性则大于50%。 随着化合物Ⅰd、Ⅰh、Ⅰj和Ⅰn质量浓度的增大,其淬灭DPPH自由基的活性均呈现增强趋势。     

Controlled Synthesis of Ni-Doped MoS2 Hybrid Electrode for Synergistically Enhanced Water-Splitting Process

The development of high-efficiency, low-cost, and earth-abundant electrocatalysts for overall water splitting remains a challenge. In this work, Ni-modified MoS₂ hybrid catalysts are grown on carbon cloth (Ni-Mo-S@CC) through a one-step hydrothermal treatment. The optimized Ni-Mo-S@CC catalyst shows excellent hydrogen evolution reaction (HER) activity with a low overpotential of 168 mV at a current density of 10 mA cm⁻² in 1.0 m KOH, which is lower than those of Ni-Mo-S@CC (1:1), Ni-Mo-S@CC (3:1), and pure MoS₂. Significantly, the Ni-Mo-S@CC hybrid catalyst also displays outstanding oxygen evolution reaction (OER) activity with a low overpotential of 320 mV at a current density of 10 mA cm⁻², and remarkable long-term stability for 30 h at a constant current density of 10 mA cm⁻². Experimental results and theoretical analysis based on density functional theory demonstrate that the excellent electrocatalytic performance can be attributed mainly to the remarkable conductivity, abundant active sites, and synergistic effect of the Ni-doped MoS₂. This work sheds light on a unique strategy for the design of high-performance and stable electrocatalysts for water-splitting electrolyzers.     

氨基三唑分子印迹聚合物的制备及性能表征

采用分子印迹技术,以氨基三唑(AMI)为模板分子,异丁醇为溶剂,甲基丙烯酸(MAA)为功能单体,乙二醇二甲基丙烯酯(EDMA)为交联剂,合成了氨基三唑分子印迹聚合物(AMI-MIP)。采用静态平衡结合实验和选择性实验评价了AMI-MIP对底物分子的结合特性及分子识别性能,并进行了吸附动力学研究。结果表明,AMI-MIP对AMI存在不同亲和力的两类结合位点,且对AMI具有很高的选择吸附特性和良好的分子识别性能,AMI-MIP对AMI的吸附行为可用准二级吸附动力学方程加以描述。     

匀浆提取-超高效液相色谱-串联质谱法测定烟草中亚硝胺含量

提出了超高效液相色谱-串联质谱法测定烟草中N-亚硝基降烟碱(NNN)、N-亚硝基新烟草碱(NAT)、N-亚硝基假木贼碱(NAB)和4-甲基亚硝基吡啶基丁酮(NNK)等4种亚硝胺含量的方法。烟草样品经0.1mol.L-1乙酸铵溶液匀浆提取,离心分离取上清液过Waters AcquityUPLC BEH C18色谱柱(2.1mm×100mm,1.7μm)分离,以乙腈和0.01mol.L-1乙酸铵溶液按不同体积混合作流动相梯度洗脱。串联质谱测定中采用电喷雾离子源正离子模式和多反应监测模式检测,同位素内标法定量。NNK、NNN、NAB和NAT的检出限(3s)分别为0.06,0.17,0.15,0.053μg.L-1。方法的加标回收率在92.1%～104%之间;日内和日间相对标准偏差(n=7)分别为2.7%～3.3%和3.5%～4.2%。     

Effect of Axial Ligands on the Molecular Configurations,Stability, Reactivity,and Photodynamic Activities of Silicon Phthalocyanines

To demonstrate the effect of axial ligands on the structure–activity relationship, a series of axially substituted silicon phthalocyanines (SiPcs) have been synthesized with changes to the axial ligands. The reactivity of the axial ligand upon shielding by the phthalocyanine ring current, along with their stability, photophysical, and photodynamic therapy (PDT) activities were compared and evaluated for the first time. As revealed by single‐crystal XRD analysis, rotation of the axial ? OMe ligands was observed in SiPc 3 , which resulted in two molecular configurations coexisting synchronously in both the solid and solution states and causing a split of the phthalocyanine α protons in the ¹H NMR spectra that is significantly different from all SiPcs reported so far. The remarkable photostability, good singlet oxygen quantum yield, and efficient in vitro photodynamic activity synergistically show that compound 3 is one of the most promising photosensitizers for PDT.