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Copper-catalyzed oxidative phosphonoheteroarylation of alkenes with phosphonates and N-heteroarenes via P-H/C-H functionalization

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Organic Chemistry Frontiers 2022年第2期9卷 476-480页

作者： Chong-Hui Xu Zhi-Qiang Xiong Yang Li Yan-Ping Zhu Jin-Heng Li key laboratory of Jiangxi province for Persistent Pollutants Control and Resources Recycle Nanchang Hangkong UniversityNanchang 330063China School of Pharmacy Key Laboratory of Molecular Pharmacology and Drug EvaluationMinistry of EducationCollaborative Innovation Center of Advanced Drug Delivery System and Biotech Drugs in Universities of ShandongYantai UniversityYantaiShandong264005China State key laboratory of Applied Organic Chemistry Lanzhou UniversityLanzhou 730000China School of Chemistry and chemical engineering Henan Normal UniversityXinxiangHenan 475004China

A copper-catalyzed oxidative intermolecular phosphonoheteroarylation of alkenes with phosphonates and nucleophilic N-heteroarenes(such as indoles and pyrroles)involving P-H/C-H functionalization for the synthesis of highly valuable β-(N-heteroaryl)-alkylphosphonates is disclosed.This method allows the incorporation of two functional groups,a phosphonate and a N-heteroarene,into the alkene in a single reaction step through oxidative formation of the P-centered radicals,addition across the CvC bond,single electron oxidation and C-H functionalization cascades.

关键词： oxidative phosphonate catalyzed

Shapeable carbon fiber networks with hierarchical porous structure for high-performance Zn–I;batteries

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Science China Chemistry 2022年第2期65卷 391-398页

作者： Yulong He Miaomiao Liu Song Chen Jintao Zhang key laboratory for Colloid and Interface Chemistry Ministry of EducationSchool of Chemistry and Chemical EngineeringShandong UniversityJinan 250100China

Aqueous rechargeable zinc-iodine batteries(ZIBs)emerging as a promising energy storage alternative have attracted considerable attention.However,ZIBs still suffer from the severe shuttle effect of polyiodide and poor reversibility,leading to the poor cycling lifetime and potential safety issues.Herein,the assembly of Al-based metal-organic frameworks(Al-MOFs)in the presence of polyacrylonitrile(PAN)via electrospinning technique enables the formation of Al-MOF/PAN fibers.With the subsequent pyrolysis,the hierarchical porous carbon fibers with nitrogen doping(NPCNFs)are prepared for loading iodine.Benefiting from the confinement effect of the highly porous carbon network and the nitrogen doping,the self-supported carbon nanofiber electrode is capable of inhibiting the shuttle effect of polyiodide species.Especially,the in-situ Raman spectroscopy reveals the reversible two-step conversion reaction between iodine and polyiodide,which enables the best cycling stability for over 6,000 cycles with negligible capacity.This work demonstrates an efficient approach to regulating the porous structure and surface properties in the design of advanced iodine electrodes for high-performance ZIBs.

关键词： free-standing flexibility hierarchical pore structure nitrogen-doping zinc-iodine batteries

Directional preparation of naphthalene oil-rich tar from Beisu low-rank coal by low-temperature catalytic pyrolysis

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Carbon Resources Conversion 2020年第1期3卷 67-75页

作者： Tao Liu Xiuli Zhang Yongzhuo Liu Lingyun Wang Qingjie Guo key laboratory of clean chemical engineering of colleges and universities of shandong province Qingdao University of Science and TechnologyQingdao 266042People’s Republic of China State key laboratory of High-efficiency Utilization of Coal and Green chemical engineering Ningxia UniversityYinchuan 750021People’s Republic of China

Low-rank coal(LRC)can be converted to high value-added naphthalene and its alkylated derivatives through low-temperature catalytic pyrolysis.In this paper,the catalytic pyrolysis of Beisu LRC in a fixed-bed at low temperature was investigated.And the catalytic effects of HZSM-5,low-temperature carbocoal(LtC),and LtC-HZSM-5 on the content and yield of naphthalene oil were examined.The results showed that the generation of naphthalene oil in low-temperature LRC pyrolysis(LT-LP)process could be improved when LtC(prepared at 550℃)or HZSM-5 was individually used as a catalyst.Compared with sole pyrolysis of raw LRC,the addition of the LtC-HZSM-5 catalyst increased the content of naphthalene oil from 11.19 wt.%to 31.49 wt%.And the yield of naphthalene oil was increased from 1.07 wt%to 5.31 wt%.The reactions of micromolecular hydrogen-containing radicals(⋅MHCR)were optimized by LtC.⋅MHCR could be captured in relatively low-temperature region(200-400℃)and released at high temperature by LtC.The generation of phenolics was inhibited by HZSM-5.As a result,the naphthalene oil-rich tar was obtained through low-temperature LtC-HZSM-5 catalytic pyrolysis of Beisu LRC.

关键词： Naphthalene oil Low-temperature carbocoal HZSM-5 Low-rank coal Catalytic pyrolysis

Diverse Structural Design Strategies of MXene‑Based Macrostructure for High‑Performance Electromagnetic Interference Shielding

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Nano-Micro Letters 2023年第12期15卷 419-448页

作者： Yue Liu Yadi Wang Na Wu Mingrui Han Wei Liu Jiurong Liu Zhihui Zeng key laboratory for Liquid‑Solid Structural Evolution and Processing of Materials School of Materials Science and EngineeringShandong UniversityJinan 250061People’s Republic of China Department of Mechanical engineering The Hong Kong Polytechnic UniversityKowloonHong Kong 999077People’s Republic of China State key laboratory of Crystal Materials Institute of Crystal MaterialsShandong 250100China Shenzhen Research Institute of shandong University ShenzhenChina School of Chemistry and chemical engineering Shandong UniversityShandong 250100China

There is an urgent demand for flexible,lightweight,mechanically robust,excellent electromagnetic interference(EMI)shielding materials.Two-dimensional(2D)transition metal carbides/nitrides(MXenes)have been potential candidates for the construction of excellent EMI shielding materials due to their great electrical electroconductibility,favorable mechanical nature such as flexibility,large aspect ratios,and simple processability in aqueous media.The applicability of MXenes for EMI shielding has been intensively explored;thus,reviewing the relevant research is beneficial for advancing the design of high-performance MXene-based EMI shields.Herein,recent progress in MXene-based macrostructure development is reviewed,including the associated EMI shielding mechanisms.In particular,various structural design strategies for MXene-based EMI shielding materials are highlighted and explored.In the end,the difficulties and views for the future growth of MXene-based EMI shields are proposed.This review aims to drive the growth of high-performance MXene-based EMI shielding macrostructures on basis of rational structural design and the future high-efficiency utilization of MXene.

关键词： MXene Composite Electromagnetic interference shielding Microstructure Electronics

Probing the intriguing frictional behavior of hydrogels during alternative sliding velocity cycles

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摩擦:英文版 2023年第12期11卷 2329-2341页

作者： Yiming ZHAO Gang YI Jiuyu CUI Ziqian ZHAO Yonggan YAN Luxing WEI Jinlong SHAO Hongbo ZENG Jun HUANG key laboratory of High Efficiency and clean Mechanical Manufacture of Ministry of Education National Demonstration Center for Experimental Mechanical Engineering EducationSchool of Mechanical EngineeringShandong UniversityJinan 250061China shandong key laboratory of Advanced Organosilicon Materials and Technologies Zibo 256401China Department of chemical and Materials engineering University of AlbertaEdmontonAlberta T6G 1H9Canada Department of Periodontology School and Hospital of StomatologyCheeloo College of MedicineShandong University&Shandong Key Laboratory of Oral Tissue RegenerationJinan 250061China shandong engineering laboratory for Dental Materials and Oral Tissue Regeneration Jinan 250012China

Understanding the friction behavior of hydrogels is critical for the long-term stability of hydrogelrelated bioengineering applications.Instead of maintaining a constant sliding velocity,the actual motion of bio-components(e.g.,articular cartilage and cornea)often changes abruptly.Therefore,it is important to study the frictional properties of hydrogels serving under various sliding velocities.In this work,an unexpected low friction regime(friction coefficientμengineering applications such as artificial cartilage.

关键词： hydrogel friction alternative sliding velocity ultra-low friction coefficient drag reduction

Silver-catalyzed three-component reaction: synthesis of N^2-substituted 1,2,3-triazoles via direct benzylic amination

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Science China Chemistry 2019年第8期62卷 1001-1006页

作者： Zhenhua Liu Wenjing Hao Wen Gao Guangyu Zhu Xiang Li Lili Tong Bo Tang College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Functionalized Probes for Chemical Imaging in Universities of ShandongKey Laboratory of Molecular and Nano ProbesMinistry of EducationShandong Provincial Key Laboratory of Clean Production of Fine ChemicalsShandong Normal University

A novel Ag(Ⅰ)-catalyzed benzylic amination reaction with in situ generation of NH-1,2,3-triazoles for N^2-substituted 1,2,3 triazole scaffolds is described. This protocol is achieved with easily accessible substrate, broad functional group, good re gioselectivity, thus providing the efficient and practical method to diverse N^2-substituted 1,2,3-triazole rings with moderate t good yields.

关键词： silver-catalyzed alkynes 1,2,3-triazoles amination

Construction of nanocarriers based on nucleic acids and their applications in nanobiology delivery systems

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National Science Review 2022年第5期9卷 181-195页

作者： Yingshu Guo Xiuping Cao Xiaofei Zheng Sk Jahir Abbas Juan Li Weihong Tan shandong Provincial key laboratory of Molecular engineering School of Chemistry and Chemical EngineeringQilu University of Technology (Shandong Academy of Sciences) School of Chemistry and chemical engineering Linyi University Institute of Molecular Medicine State Key Laboratory of Oncogenes and Related Genes Renji Hospital Shanghai Jiao Tong University School of MedicineCollege of Chemistry and Chemical Engineering Shanghai Jiao Tong University Institute of Cancer and Basic Medicine Chinese Academy of Sciences The Cancer Hospital of the University of Chinese Academy of Sciences

In recent years,nanocarriers based on nucleic acids have emerged as powerful and novel nanocarriers that are able to meet the demand for cancer-cell-specific targeting.Functional dynamics analysis revealed good bio compatibility,low toxicity and programmable structures,and their advantages include controllable size and modifiability.The development of novel hybrids has focused on the distinct roles of biosensing,drug and gene delivery,vaccine transport,photosensitization,counteracting drug resistance and functioning as carriers and logic gates.This review is divided into three parts:(ⅰ) DNA nanocarriers,(ⅱ) RNA nanocarriers and(ⅲ) DNA/RNA hybrid nanocarriers and their applications in nanobiology delivery systems.We also provide perspectives on possible future directions for growth in this field.

关键词： nanocarriers based on nucleic acids biosensing targeted delivery cell

Strong interface interaction and internal electric field promote electron transfer of Bi_(2)O_(2)S/NiFe_(2)O_(4) heterojunction for photocatalytic antibiotic degradation

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Journal of Materials Science & Technology 2023年第27期158卷 145-155页

作者： Shaoxuan Pang Yilin Dong Dongyu Xu Qiuwen Wang Weihong Gao Lijun Zhang Kang Wang Guangming Zhang Longyi Lv Yuguo Xia Zhijun Ren Pengfei Wang School of Energy and Environmental engineering Hebei University of TechnologyTianjin 300401China Tianjin key laboratory of clean Energy and Pollutant Control Tianjin 300401China School of Chemistry and chemical engineering National Engineering Research Center for Colloidal MaterialsShandong UniversityJinan 250100China

Heterojunction photocatalysts have shown considerable activities for organic pollutants degradation.However,the faint connection interface and inferior charge shift efficiency critically block the property of heterojunction photocatalysis.Herein,Bi_(2)O_(2)S/NiFe_(2)O_(4) nanosheets heterojunction with ultrastrong inter-face interaction and high internal electric field are designed by an in-situ growth method.Tentative and theoretical consequences prove that the interfacial interaction and internal electric field not only act as the electron flow bridge but also decrease the electrons shift energy obstacle,thus speeding up electrons transfer and achieving effective spatial electron-hole separation.Therefore,a large amount of·O_(2)^(-)and holes as active species were generated.Remarkably,Bi_(2)O_(2) S/NiFe_(2)O_(4) establishes a considerably boosted photocatalytic performance for tetracycline degradation(0.032 min^(-1)),which is about 14.2-fold and 7.8-fold of the pristine BOS and NFO,respectively.This work provides a promising motivation for modulating charge transfer by interface control and internal electric field to boost photocatalytic performance.

关键词： Bi_(2)O_(2)S/NiFe_(2)O_(4) S-scheme heterojunction Ultrastrong interface interaction Internal electric field Active species Photocatalytic degradation

Constructing a multifunctional mesoporous composite of metallic cobalt nanoparticles and nitrogen-doped reduced graphene oxides for high-performance lithium-sulfur batteries

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Carbon Energy 2022年第2期4卷 142-154页

作者： Luhai Gai Chenhao Zhao Ya Zhang Zhibiao Hu Qiang Shen key laboratory for Colloid and Interface Chemistry of Education Ministry School of Chemistry and Chemical EngineeringShandong UniversityJinanChina Fujian Provincial key laboratory of clean Energy Materials College of Chemistry&MaterialsLongyan UniversityLongyanChina

Electrochemical properties of lithium-sulfur(Li-S)batteries are mainly hindered by both the insulating nature of elemental sulfur(i.e.,molecular S8)and the shuttling effect or sluggish redox kinetics of lithium polysulfide intermediates(Li_(2)S_(n),3≤n≤8).In this paper,a three-dimensional mesoporous reduced graphene oxide-based nanocomposite,with the embedding of metallic Co nanoparticles and the doping of elemental N(Co/NrGO),and its simply ground mixture with powdered S at a mass ratio of 1:6(Co/NrGO/S)are prepared and used as cathode-/separator-coated interlayers and working electrodes in assembled Li-S cells,respectively.One of the effective cell configurations is to paste composite Co/NrGO onto both the S-loading cathode and separator,showing good cycling stability(1070mAh g^(−1) in the 100th cycle at 0.2 C),highrate capability(835mAh g^(−1),2.0 C),and excellent durability(905mAh g^(−1) in the 250th cycle at 0.5 or 0.2 C).Compared with the experimental results of Co-absent NrGO,electrochemical properties of various Co/NrGO-based cell configurations clearly show multiple functions of Co/NrGO,indicating that the absence of Co/NrGO coatings and/or Co nanoparticles may be inadequate to achieve superior S availability of assembled Li-S batteries.

关键词： high-performance mechanism lithium-sulfur batteries multifunctional three-dimensional mesoporous reduced graphene oxide-based nanocomposite