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Recent developments in electrosynthesis of nitriles and electrocatalytic cyanations

Journal of Energy Chemistry 2022年第7期31卷 542-575,I0014页

作者： Haiyan Hu Shanxuan Wu Fachao Yan Mohamed Makha Yuxia Sun Chen-Xia Du yuehui li State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICPCenter for Excellence in Molecular SynthesisLanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000GansuChina University of Chinese Academy of Sciences Zhengzhou 450001HenanChina College of Chemistry Zhengzhou UniversityBeijing 100049China

Nitrile compounds are a class of high-value chemicals and versatile intermediates which can easily be transformed into a variety of useful products bearing functional groups such as carboxyl, carbamoyl, aminomethyl, ketyl and heterocyclic derivatives. Various thermal catalytic cyanation procedures have been devised and scaled up industrially while developing alternative methods are actively pursued. The access to these classes of molecules electrochemically offers greener alternatives to their preparation. The development of electrochemical synthesis of cyano-containing compounds under mild conditions with low energy consumption will imminently become indispensable approaches for industrial production of nitriles. The electrochemical cyanation presents many challenges from the toxicity of cyanide to the development of catalysts and the design of electrochemical cells. Electrochemical cyanation reaction offers promise to conveniently accessing nitriles but still requires efficient electro-catalysts, safe protocols and scale up considerations. This review discusses recent progress in the field of electrochemical synthesis of nitrile compounds placing emphasis on electro-synthetic and electro-catalytic mechanism aspects while making reference to original works to highlight the progress in this area.

关键词： Cyano compounds Nitriles Cyanation Electrosynthesis Electrocatalysis

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经由N-硼基酰胺中间体的酰胺高效转化合成腈类化合物

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有机化学 2024年第2期44卷 638-643页

作者：李洋董亚楠李跃辉中国科学院兰州化学物理研究所苏州实验室羰基合成与选择氧化国家重点实验室兰州730000 中国科学院大学北京100049

以HBpin为硼基化试剂和脱氧剂,以CsF为催化剂实现了伯酰胺的脱水转化,以良好到优秀的产率制备了多种腈类化合物.该方法操作简便,克级放大实验目标产物的产率为96%,且催化体系对多种官能团,如卤素、三氟甲基、杂环和氨基等表现出良好的... 详细信息

以HBpin为硼基化试剂和脱氧剂,以CsF为催化剂实现了伯酰胺的脱水转化,以良好到优秀的产率制备了多种腈类化合物.该方法操作简便,克级放大实验目标产物的产率为96%,且催化体系对多种官能团,如卤素、三氟甲基、杂环和氨基等表现出良好的兼容性,结果表明该方法具有较好的应用潜力.机理研究表明原位生成N-硼基酰胺中间体和氢气释放是反应顺利发生的关键,生成热力学稳定的硼酸酐和腈类产物是这个形式上的酰胺脱水反应的驱动力.

关键词：氟化铯催化伯酰胺腈硼烷

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Iron-catalyzed hydroaminocarbonylation of alkynes:Selective and efficient synthesis of primaryα,β-unsaturated amides

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Chinese Chemical Letters 2022年第11期33卷 4842-4845页

作者： Zijun Huang Jia Tang Xiongwei Jiang Tianle Xie Minmin Zhang Donghui Lan Shaofeng Pi Zhengde Tan Bing Yi yuehui li Hunan Province Key Laboratory of Environmental Catalysis and Waste Rechemistry College of Materials and Chemical EngineeringHunan Institute of EngineeringXiangtan 411104China State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICPLanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000China

α,β-Unsaturated primary amides are important intermediates and building blocks in organic synthesis.Herein,we report a ligand-free iron-catalyzed hydroaminocarbonylation of alkynes using NH_(4)HCO_(3)as the ammonia source,enabling the highly efficient and regioselective synthesis of linearα,β-unsaturated primary amides.Various aromatic and aliphatic alkynes are transformed into the desired linearα,β-unsaturated primary amides in good to excellent yields.Further studies show that using NH_(4)HCO_(3)as the ammonia source is key to obtain good yields and selectivity.The utility of this route is demonstrated with the synthesis of linearα,β-unsaturated amides including vanilloid receptor-1 antagonist TRPV-1.

关键词： Iron-catalyzed Alkynes Ammonium bicarbonate Aminocarbonylation linearα,β-unsaturated amides

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Tunable synthesis of furfurylamines orβ-amino alcohols via Ru-catalyzed N–H functionalization using biomass-derived polyols

Green Synthesis and Catalysis

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Green Synthesis and Catalysis 2022年第3期3卷 259-264页

作者： Le Jia Xue Wang Xiaolong Gao Mohamed Makha Xi-Cun Wang yuehui li State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICPLanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000China College of Chemistry and Chemical Engineering Northwest Normal UniversityLanzhou 730070China

We report the highly efficient conversion of readily available biomass-derived polyols with amines to valuable furfurylamines orβ-amino alcohols compounds using ruthenium catalysis.The reaction outcome is readily tuned by the simple addition of 4Åmolecular sieves(furfurylamines vs.β-amino alcohols)with high chemo-selectivity.The proposed reaction mechanism involves ruthenium-catalyzed hydrogen borrowing for the reduction of the imine intermediate and C–C bond cleavage of polyols via a retro-aldol process.A series of arylamines was suc-cessfully transformed into the desired products with moderate to good yields.

关键词： Polyols Furfurylamines β-Amino alcohols Ru-catalyzed

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Well-dispersed Mn/g-C_(3)N_(4)as bifunctional catalysts for selective epoxidation of olefins and carbon dioxide cycloaddition

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Chinese Chemical Letters 2023年第12期34卷 150-154页

作者： Minxing Du Yuxia Sun Jiaojiao Zhao Haiyan Hu liwei Sun yuehui li State Key Laboratory for Oxo Synthesis and Selective Oxidation Suzhou Research Institute of LICPCenter for Excellence in Molecular SynthesisLanzhou Institute of Chemical Physics(LICP)Chinese Academy of SciencesLanzhou 730000China University of Chinese Academy of Sciences Beijing 100049China

Epoxidation is an important chemical process for the production of epoxides,key building blocks in chemical industry.Despite great efforts being made to facilitate this process,it remains a significant challenge to develop cost-effective,environmental-friendly,and selective catalysts.Herein,we reported a highly dispersed Mn supported by g-C_(3)N_(4)(Mn/g-C_(3)N_(4))with Mn loading up to 2.56 wt%.The Mn/g-CN_(4)exhibited satisfied catalytic performance for olefin epoxidation with excellent conversion(91%),high selectivity(93%)as well as outstanding recycling stability.Further analysis revealed the importance of Mn-N structure for the generation of active oxo-containing species and subsequent oxygen atom transfer.Besides,an efficient synthesis of cyclic carbonates from styrene epoxide and CO_(2)has been achieved(88%conversion,89%selectivity)based on the polar Mn-N coordinated characteristics of Mn/g-C_(3)N_(4)catalyst.

关键词： Well-dispersed Mn catalyst Bifunctional catalyst Epoxidation CO_(2) Cycloaddition

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电子文件归档和电子档案管理新模式实践

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兰台世界 2024年第3期 98-100,105页

作者：李月惠沈阳市纪委监委综合保障中心

数字转型时代,信息技术的成熟为档案事业的发展提供了机遇和挑战。随着办公自动化的发展,越来越多的电子文件和网络信息逐渐被人们接受并广泛利用,电子文件归档方法以及如何安全、有效地管理和利用电子档案,成为众多档案工作者思考的问... 详细信息

数字转型时代,信息技术的成熟为档案事业的发展提供了机遇和挑战。随着办公自动化的发展,越来越多的电子文件和网络信息逐渐被人们接受并广泛利用,电子文件归档方法以及如何安全、有效地管理和利用电子档案,成为众多档案工作者思考的问题。经过不断探索和反复实践,随着电子档案管理制度紧紧追逐信息技术的不断更新,自动融合归档技术和集成模块式档案管理方式,已成为推动数字档案建设发展的关键。

关键词：电子文件归档档案管理新模式

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High-efficient generation algorithm for large random active shield

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Science China(Information Sciences) 2019年第3期62卷 211-213页

作者： Ruishan XIN Yidong YUAN Jiaji HE yuehui li Yiqiang ZHAO School of Microelectronics Tianjin University Tianjin Key Laboratory of Imaging and Sensing Microelectronic Technology Tianjin University

Dear editor,Security integrated circuits play important roles in trusted platform modules [1], embedded devices, etc. However, invasive attacks [2] are serious threats on such circuits. Active shield is regarded as an... 详细信息

关键词： DC High-efficient generation algorithm for large random active shield CMA Pb

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桑叶提取物对蛋鸡生产性能、蛋品质及血清生化指标的影响

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中国饲料 2024年第12期 133-136页

作者：段卫平李跃辉南阳农业职业学院河南南阳473000

文章旨在研究桑叶提取物对蛋鸡生产性能、蛋品质及血清生化指标的影响。试验将400只五黑蛋鸡随机分成4组,各组蛋鸡分别饲喂基础日粮+0 mg/kg(Ⅰ组)、100 mg/kg(Ⅱ组)、200 mg/kg(Ⅲ组)、400 mg/kg(Ⅳ组)桑叶提取物,每组5个重复,每个重... 详细信息

文章旨在研究桑叶提取物对蛋鸡生产性能、蛋品质及血清生化指标的影响。试验将400只五黑蛋鸡随机分成4组,各组蛋鸡分别饲喂基础日粮+0 mg/kg(Ⅰ组)、100 mg/kg(Ⅱ组)、200 mg/kg(Ⅲ组)、400 mg/kg(Ⅳ组)桑叶提取物,每组5个重复,每个重复20只,试验为期7周。结果表明,(1)与Ⅰ组相比,Ⅲ组料蛋比显著降低(P<0.05);Ⅳ组产蛋率显著提高(P<0.05),料蛋比显著降低(P<0.05)。(2)与Ⅰ组相比,Ⅲ组、Ⅳ组蛋黄颜色、哈氏单位显著提高(P<0.05)。(3)与Ⅰ组相比,Ⅲ组蛋鸡血清中葡萄糖含量显著降低(P<0.05);Ⅳ组蛋鸡血清中低密度脂蛋白、葡萄糖含量显著降低(P<0.05)。综上所述,在五黑蛋鸡基础日粮中添加200、400 mg/kg的桑叶提取物可提高蛋鸡的生产性能、蛋品质及血清生化指标,其中添加水平为400 mg/kg时效果最佳。

关键词：桑叶提取物五黑鸡生产性能蛋品质血清生化指标

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Correlating the electronic structures of metallic/semiconducting MoTe2 interface to its atomic structures

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National Science Review 2021年第2期8卷 108-114页

作者： Bo Han Chen Yang Xiaolong Xu yuehui li Ruochen Shi Kaihui liu Haicheng Wang Yu Ye Jing Lu Dapeng Yu Peng Gao Electron Microscopy Laboratory and International Center for Quantum Materials School of PhysicsPeking University Department of Material Physics and Chemistry University of Science and Technology Beijing State Key Laboratory for Artificial Microstructure &Mesoscopic Physics School of PhysicsPeking University Academy for Advanced Interdisciplinary Studies Peking University Collaborative Innovation Center of Quantum Matter State Key Laboratory of Advanced Materials for Smart Sensing GRINM Group Co.Ltd.Beijingand GRIMAT Engineering Institute Co.Ltd. Shenzhen Key Laboratory of Quantum Science and Engineering

Contact interface properties are important in determining the performances of devices that are based on atomically thin two-dimensional(2D) materials, especially for those with short channels. Understanding the contact interface is therefore important to design better devices. Herein, we use scanning transmission electron microscopy, electron energy loss spectroscopy, and first-principles calculations to reveal the electronic structures within the metallic(1T)-semiconducting(2H) MoTe2coplanar phase boundary across a wide spectral range and correlate its properties to atomic structures. We find that the 2 H-MoTe2excitonic peaks cross the phase boundary into the 1 T phase within a range of approximately 150 nm. The1 T-MoTe2crystal field can penetrate the boundary and extend into the 2H phase by approximately two unit-cells. The plasmonic oscillations exhibit strong angle dependence, that is a red-shift of π +σ(approximately 0.3–1.2 e V) occurs within 4 nm at 1 T/2 H-MoTe2boundaries with large tilt angles, but there is no shift at zero-tilted boundaries. These atomic-scale measurements reveal the structure–property relationships of the 1 T/2 H-MoTe2boundary, providing useful information for phase boundary engineering and device development based on 2 D materials.

关键词： MoTe_2 phase engineering coplanar phase boundary EELS

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Atomic origin of spin-valve magnetoresistance at the SrRuO3 grain boundary

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National Science Review 2020年第4期7卷 755-762页

作者： Xujing li li Yin Zhengxun Lai Mei Wu Yu Sheng Lei Zhang Yuanwei Sun Shulin Chen Xiaomei li Jingmin Zhang yuehui li Kaihui liu Kaiyou Wang Dapeng Yu Xuedong Bai Wenbo Mi Peng Gao Electron Microscopy Laboratory School of Physics Peking University Beijing National Laboratory for Condensed Matter Physics and Institute of Physics Chinese Academy of Sciences Tianjin Key Laboratory of Low Dimensional Materials Physics and Preparation Technology School of Science Tianjin University International Center for Quantum Materials Peking University State Key Laboratory of Superlattices and Microstructures Institute of Semiconductors Chinese Academy of Sciences State Key Laboratory for Artificial Microstructure & Mesoscopic Physics School of Physics Peking University Collaborative Innovation Centre of Quantum Matter College of Materials Science and Opto-Electronic Technology University of Chinese Academy of Sciences Shenzhen Institute for Quantum Science and Engineering and Department of Physics Southern University of Science and Technology

Defects exist ubiquitously in crystal materials, and usually exhibit a very different nature from the bulk matrix.Hence, their presence can have significant impacts on the properties of devices.Although it is well accepted that the properties of defects are determined by their unique atomic environments, the precise knowledge of such relationships is far from clear for most oxides because of the complexity of defects and difficulties in characterization.Here, we fabricate a 36.8°Sr RuO3grain boundary of which the transport measurements show a spin-valve magnetoresistance.We identify its atomic arrangement, including oxygen,using scanning transmission electron microscopy and spectroscopy.Based on the as-obtained atomic structure, the density functional theory calculations suggest that the spin-valve magnetoresistance occurs because of dramatically reduced magnetic moments at the boundary.The ability to manipulate magnetic properties at the nanometer scale via defect control allows new strategies to design magnetic/electronic devices with low-dimensional magnetic order.

关键词： spin-valve magnetic defects electron microscopy grain boundary

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