不同变质程度煤的高分辨率透射电镜分析

利用高分辨率透射电子显微镜(HRTEM)分析了三种不同变质程度煤样的结构特征。基于傅里叶-反傅里叶变换方法,并结合Matlab、Arcgis和Auto CAD软件,通过图像分析技术,获得了HRTEM照片的晶格条纹参数。结果表明,三种煤样的晶格条纹呈现不同特征,按条纹长度分别归属于1×1-8×8共计八个类型。以3×3为临界点,在1×1和2×2中,ML-8中芳香层片的比例高于DP-4和XM-3;在3×3-8×8中,ML-8中芳香层片的比例低于DP-4和XM-3。对比HRTEM和XRD参数d002发现,随着镜质组反射率的增加d002都呈现递减趋势。     

Enhanced Catalytic Activity in Liquid‐Exfoliated FeOCl Nanosheets as a Fenton‐Like Catalyst

A facile liquid‐phase exfoliation method to prepare few‐layer FeOCl nanosheets in acetonitrile by ultrasonication is reported. The detailed exfoliation mechanism and generated products were investigated by combining first‐principle calculations and experimental approaches. The similar cleavage energies of FeOCl (340 mJ m^?2) and graphite (320 mJ m^?2) confirm the experimental exfoliation feasibility. As a Fenton reagent, FeOCl nanosheets showed outstanding properties in the catalytic degradation of phenol in water at room temperature, under neutral pH conditions, and with sunlight irradiation. Apart from the increased surface area of the nanosheets, the surface state change of the nanosheets also plays a key role in improving the catalytic performance. The changes of charge density, density of states (DOS), and valence state of Fe atoms in the exfoliated FeOCl nanosheets versus plates illustrated that surface atomistic relationships made the few‐layer nanosheets higher activity, indicating the exfoliation process of the FeOCl nanosheets also brought about surface state changes.     

Asymmetric Hydrosilylation of Aromatic Ketones Catalyzed by an Economical and Effective Copper-Diphosphine Catalytic System in Air

In the presence of the inexpensive and non‐toxic polymethylhydrosiloxane, the combination of copper(II) acetate and a chiral diphosphine displayed high catalytic efficiency in the asymmetric hydrosilylation of a series of aromatic ketones in air atmosphere and at room temperature. (R)‐1‐Arylethanols were obtained with up to 99% yield and 93% enantiomeric excess. Meanwhile, the electron effect and steric hindrance of substituents on the aromatic ring had an interesting influence on both the yields and enantioselectivities. Furthermore, a possible mechanism was presented to explain the influence of some key factors on the reaction.     

A Hexagonal Covalent Porphyrin Framework as an Efficient Support for Gold Nanoparticles toward Catalytic Reduction of 4‐Nitrophenol

A hexagonal porphyrin‐based porous organic polymer, namely, CPF‐1, was constructed by 3+2 ketoenamine condensation of the C₂‐symmetric porphyrin diamine 5,15‐bis(4‐aminophenyl)‐10,20‐diphenylporphyrin and 1,3,5‐triformylphloroglucinol. This material exhibits permanent porosity and excellent thermal and chemical stability. CPF‐1 can be employed as a superior supporting substrate to immobilize Au nanoparticles (NPs) as a result of the strong interactions between Au NPs and the CPF support. An Au@CPF‐1 hybrid was synthesized by an interfacial solution infiltration method with NaBH₄ as reducing agent. Au NPs (5 nm) grew on CPF‐1 and were distributed without aggregation. Moreover, Au@CPF‐1 exhibits superior catalytic activity compared to many other reported Au‐based catalysts for the reduction of 4‐nitrophenol in the presence of NaBH₄. In addition, Au@CPF‐1 has excellent stability and recyclability, and it can be reused for three successive reaction cycles without loss of activity. The dense distribution of phenyl rings on the channel walls of the CPF support can reasonably be regarded as the active sites that adsorb the 4‐nitrophenol molecule through hydrogen‐bonding and C?H ??? π interactions, as was confirmed by the X‐ray structure of model compound DAPP‐Benz.     

Asymmetric Michael Addition of Aldimino Esters with Chalcones Catalyzed by Silver/Xing‐Phos: Mechanism‐Oriented Divergent Synthesis of Chiral Pyrrolines

The mechanism‐oriented reaction design for the divergent synthesis of chiral molecules from simple starting materials is highly desirable. In this work, aromatic amide‐derived nonbiarylatropisomer/silver (silver/Xing‐Phos) complex was used to catalyze the Michael addition of glycine aldimino esters to chalcones and successfully applied to the subsequent cyclocondensation to afford substituted cis‐Δ(1)‐pyrroline derivatives with up to 98 % ee. Besides the inherent performance of the chiral Ag/Xing‐Phos catalyst system, it was found that the workup of such reactions played an important role for the stereoselective construction of stereodivergent Δ(1)‐pyrrolines, in which an epimerization of the cis‐Δ(1)‐pyrrolines to the trans‐isomers during was revealed.     

一元h-F凸函数的导数判别法

利用h-F凸函数的定义,在h满足一定条件的情况下,导出满足条件P1,P2的h-F凸函数的等价条件.     

Prediction of allergic reaction risk of Shenmai injection based on real-world evidence coupled with UPLC–Q-TOF-MS

The allergic reaction (AR) of Chinese herbal injection (CHI) has become one of the most noticeable focuses of public health in China. However, it still remains a considerable controversy as to whether low-molecular-weight components in CHI have potential sensitization. In this study, the relationship between AR and low-molecular-weight component profile of Shenmai injection was explored by an interdisciplinary technology integrating real-world evidence and ultra-performance liquid chromatography–quadrupole time-of-flight mass spectroscopy (UPLC–Q-TOF-MS). The AR information of hospitalized patients was obtained by comprehensively analyzing real-world evidence from January 2015 to June 2019 at two Chinese hospitals. The UPLC–Q-TOF-MS was exploited to systematically investigate the low-molecular-weight component profile with 50–1500 m/z mass range, and 3725 MS1 peaks were detected. The optimized partial least squares discriminant analysis model was established to map the influence of low-molecular-weight components on AR. The results of this study showed that high levels of organic acids administered intravenously might be a potential risk factor for inducing AR. By using this method, Shenmai injection with high AR risk could be recognized precisely with 100% accuracy before clinical use.