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Chinese Journal of Chemistry 2024年第8期42卷 873-878页

作者： Jian Long Zhiwu Lu Xiao-Lin Li Peng Xue Wen-Bo Liu engineering research center of organosilicon compounds&materials(Ministry of Education)and College of Chemistry and Molecular Sciences Wuhan UniversityWuhanHubei430072 China

Comprehensive Summary,The azepine ring is a prominent structural scaffold in biologically significant molecules. In this study, we present a Ni(II)-catalyzed asymmetric difunctionalization of alkynes, involving intermolecular regioselective arylation and intramolecular nitrile addition, enabling the synthesis of enantioenriched azepine derivatives. This reaction simultaneously installs an all-carbon quaternary stereocenter and introduces an unprotected imine functionality, showing great promise for subsequent transformations. The reaction exhibits good tolerance toward various functional groups, resulting in high yields and enantioselectivities. The synthetic utility of this methodology is further demonstrated through gram-scale synthesis and product derivatization. This research offers an efficient approach to the synthesis of seven-membered nitrogen heterocycles.

关键词： Nickel Asymmetric catalysis N-Heterocycles Alkyne functionalization Quaternary centers

Synthesis of Organofluorine compounds with Acylsilanes

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Chinese Journal of Chemistry 2024年第8期42卷 887-902页

作者： Youyuan Guo Gang Zhou Xiao Shen The Institute for Advanced Studies Engineering Research Center of Organosilicon Compounds&MaterialsMinistry of EducationWuhan University299 Bayi RoadWuhanHubei430072 China

Comprehensive Summary,Organofluorine compounds are central in synthetic chemistry,medicinal chemistry and material chemistry.In this review,we summarize the investigations on the synthesis of organofluorine compounds with acylsilanes.For the non-fluorinated acylsilanes,the in situ generation of difluoroenoxysilanes from the reactions of the acylsilanes with trifluoromethylation reagents is the major pathway,leading to the facile preparation of variousα,α-difluoroketones.For the fluoroalkylacylsilanes,apart from the in situ generation of difluoroenoxysilanes through anion Brook rearrangement,radical Brook rearrangement of the photoexcited acylsilanes and the selective control of reactivities of the biradicals pave the way for the synthesis of a variety of organofluorine compounds.In general,most of these reactions gave racemic products,and the asymmetric synthesis of organofluorine compounds with acylsilanes is still rare,which would be a future.

关键词： Acylsilanes Organofluorine compounds Brook rearrangement Radical rearrangement β-Fluoride elimination Asymmetric catalysis Photocatalysis Defluoroalkylation

Solid Bi_(2)O_(3)-derived nanostructured metallic bismuth with high formate selectivity for the electrocatalytic reduction of CO_(2)

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International Journal of Minerals,Metallurgy and materials 2024年第4期31卷 803-811页

作者： Xiaoyan Wang Safeer Jan Zhiyong Wang Xianbo Jin College of Chemistry and Molecular Sciences Hubei Key Laboratory of Electrochemical Power SourcesWuhan UniversityWuhan 430072China engineering research center of organosilicon compounds&materials Ministry of EducationWuhan 430072China

CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon neutralization.However,available catalysts for CO_(2) reduction are still characterized by limited stability and activity.Recently,metallic bismuth(Bi)has emerged as a promising catalyst for CO_(2) ER.Herein,we report the solid cathode electroreduction of commercial micronized Bi2O3as a straightforward approach for the preparation of nanostructured Bi.At-1.1 V versus reversible hydrogen electrode in a KHCO3aqueous electrolyte,the resulting nanostructure Bi delivers a formate current density of~40 mA·cm^(-2) with a current efficiency of~86%,and the formate selectivity reaches97.6% at-0.78 V.Using nanosized Bi2O3as the precursor can further reduce the primary particle sizes of the resulting Bi,leading to a significantly increased formate selectivity at relatively low overpotentials.The high catalytic activity of nanostructured Bi is attributable to the ultrafine and interconnected Bi nanoparticles in the nanoporous structure,which exposes abundant active sites for CO_(2) electrocatalytic reduction.

关键词： bismuth carbon dioxide electrocatalysis formate solid electroreduction

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Molecular origin for pH-responsive wormlike micelles of zwitterionic surfactants triggered by aromatic acid derivatives

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ChemPhysMater

ChemPhysMater 2024年第2期3卷 230-238页

作者： Shuo Lu Yonghang Cheng Jinfeng Dong Xuefeng Li engineering research center of organosilicon compounds&materials Ministry of EducationCollege of Chemistry and Molecular SciencesWuhan UniversityWuhan 430072China

Introduction of aromatic acid derivatives(AADs)into zwitterionic surfactants is an efficient method to prepare wormlike micelles with pH-controllable viscosity;however,the coincident molecular origin of AAD/zwitterionic surfactant binary mixtures remains unclear.Herein,the self-assembly of hydroxyl derivatives of benzoic acid(BA)and cetyldimethyl betaine(BS-16)mixtures in water was systematically assessed,and various factors,such as the molecular structure,molar ratio of AAD and BS-16,and solution pH,were investigated.The structure-property relationship of AAD/BS-16 binary mixtures was established,which provided the molecular origin for the effect of AAD on micellar microstructures and the pH-induced morphological transitions.The ortho-substituted hydroxyl moiety in the BA molecule facilitated the formation of larger wormlike micelles,whereas the effect of the meta-substituted moiety was less significant.The para-substituted hydroxyl moiety in BA did not favor micellar growth.This moiety exhibited similar characteristics to the increasing hydroxyl moiety number in the AAD molecules or solution pH where the negative effects of steric hindrance and electrostatic interactions of molecules in micelles aredominant.

关键词： Zwitterionic surfactants Aromatic acid derivatives pH response Wormlike micelles Spherical micelles Viscosity

Stereodivergent synthesis ofα-fluoroα-azaarylγ-butyrolactones via cooperative copper and iridium catalysis

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Fundamental research 2024年第1期4卷 77-85页

作者： Kui Tian Xin Chang Lu Xiao Xiu-Qin Dong Chun-Jiang Wang College of Chemistry and Molecular Sciences Engineering Research Center of Organosilicon Compounds&MaterialsMinistry of EducationWuhan UniversityWuhan 430072China State Key Laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryShanghai 230021China Suzhou Institute of Wuhan University Suzhou 215123China

The development of stereodivergent synthetic methods to access all four stereoisomers of biologically importantα-fluoroγ-butyrolactones containing vicinal stereocenters is of great importance and poses a formidable challenge owing to ring strain and steric hindrance.Herein,a novel asymmetric[3+2]annulation ofα-fluoroα-azaaryl acetates with vinylethylene carbonate was successfully developed through Cu/Ir-catalyzed cascade allylic alkylation/lactonization,affording a variety of enantioenrichedα-fluoroγ-butyrolactones bearing vicinal stereogenic centers with high reaction efficiency and excellent levels of both stereoselectivity and regioselectivity(up to 98%yield,generally>20:1 dr and>99%ee).Notably,all four stereoisomers of these pharmaceutically valuable molecules could be accessed individually via simple permutations of two enantiomeric catalysts.In addition,other azaaryl acetates bearingα-methyl,α-chlorine orα-phenyl group were tolerated well in this transformation.Reaction mechanistic investigations were conducted to explore the process of this bimetallic catalysis based on the results of reaction intermediates,isotopic labelling experiments,and kinetic studies.

关键词： Asymmetric catalysis α-Fluoroγ-butyrolactones Synergistic catalysis Cascade reaction Stereodivergent synthesis

Asymmetric Two-Component Alkenyl Catellani Reaction for the Construction of C—N Axial Chirality

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Chinese Journal of Chemistry 2024年第7期42卷 699-704页

作者： Chenggui Wu Ze-Shui Liu Yong Shang Chang Liu Shuang Deng Hong-Gang Cheng Hengjiang Cong Yinchun Jiao Qianghui Zhou Sauvage center for Molecular Sciences Engineering Research Center of Organosilicon Compounds&Materials(Ministry of Education)Hubei Key Lab on Organic and Polymeric OptoElectronic MaterialsCollege of Chemistry and Molecular SciencesThe Institute for Advanced Studiesand TaiKang Center for Life and Medical SciencesWuhan UniversityWuhanHubei 430072China Key Laboratory of Xin'an Medicine Ministry of EducationAnhui University of Chinese MedicineHefeiAnhui 230038China School of Chemistry and Chemical engineering Hunan University of Science and TechnologyXiangtanHunan 411201China

Herein,we report an asymmetric two-component alkenyl Catellani reaction for the construction of C—N axial chirality through a palladium/chiral norbornene cooperative catalysis and an axial-to-axial chirality transfer process.Various partially aromatic iodinated 2-pyridones,quinolones,coumarin and uracil substrates react with 2,6-disubstituted aryl bromides with a tethered amide group,to afford a wide variety of polycyclic C—N atropisomers(38 examples,up to 97%e.e.).The obtained C—N axial chirality originates from the preformed transient C—C axial chirality with high fidelity.The synthetic utility of this chemistry is demonstrated by facile prepa-ration of complex quinoline and pyridine based C—N atropisomers through a N-deprotection and aromatization sequence.In addi-tion,a remote axial-to-central diastereoinduction process dictated by C—N axial chirality is observed with excellent diastereocontrol.

关键词： Alkenyl Catellani reaction Asymmetric catalysis Atropisomerism Axial-to-axial chirality transfer Heterocycles

On-surface synthesis and characterization of polyynic carbon chains

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National Science Review 2024年第3期11卷 192-199页

作者： Wenze Gao Wei Zheng Luye Sun Faming Kang Zheng Zhou Wei Xu Interdisciplinary materials research center School of Materials Science and Engineering Tongji University

Carbyne, an elusive sp-hybridized linear carbon allotrope, has fascinated chemists and physicists for decades. Due to its high chemical reactivity and extreme instability, carbyne was much less explored in contrast to the sp2-hybridized carbon allotropes such as graphene. Herein, we report the on-surface synthesis of polyynic carbon chains by demetallization of organometallic polyynes on the Au（111） surface;the longest one observed consists of ～60 alkyne units（120 carbon atoms）. The polyynic structure of carbon chains with alternating triple and single bonds was unambiguously revealed by bond-resolved atomic force microscopy. Moreover, an atomically precise polyyne, C14, was successfully produced via tip-induced dehalogenation and ring-opening of the decachloroanthracene molecule(C14Cl10) on a bilayer NaCl/Au（111） surface at 4.7 K, and a band gap of 5.8 eV was measured by scanning tunnelling spectroscopy,in a good agreement with the theoretical HOMO–LUMO gap（5.48 eV）.

关键词： polyyne scanning probe microscopy carbon allotrope on-surface synthesis organometallic polyyne

Ternary-phase layered cathodes toward ultra-stable and highrate sodium ion storage

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Rare Metals 2024年第4期43卷 1589-1598页

作者： Wen-Ji Yin Pei-Dan Su Qi Lu Xiao-Qiong Li Ji-Ming Peng Teng-Fei Zhou Ge-Meng Liang Yu-Liang Cao Hong-Qiang Wang Qing-Yu Li Si-Jiang Hu Guangxi Key Laboratory of Low Carbon Energy materials School of Chemistry and Pharmaceutical SciencesGuangxi Normal University Institutes of Physical Science and Information Technology Anhui University Department of Chemistry and Pharmaceutical Sciences Guilin Normal College College of Chemistry and Chemical engineering Huanggang Normal University School of Chemical engineering and Advanced materials The University of Adelaide engineering research center of organosilicon compounds and materials of Ministry of Education College of Chemistry and Molecular SciencesWuhan University

With the shortage of lithium resources,sodiumion batteries（SIBs） are considered one of the most promising candidates for lithium-ion batteries.P2-type and O3-type layered oxides are one of the few cathodes that can access high energy density.However,they usually exhibit structural change,capacity decay,and slow Na ion kinetic.Herein,we present layered ternary-phase cathodes with P2,P3 and O3 phases by a lattice doping strategy,which is demonstrated by X-ray diffraction（XRD） refinement.Combining the characteristics of P2,P3 and O3 phases,the layered composites show performance improvement during long-term battery cycling.In particular,Na0.7Li0.1Co0.3-Fe0.3Mn0.3O2（NLCFM） delivers a reversible capacity of120.1 mAh·g-1at 0.1C(1.0C=175 mA·g-1) with a superior capacity retention of 72.5% after 1000 cycles at10.0C.This work offers insights into the development of advanced cathode materials for SIBs.

关键词： Sodium-ion battery Cathode material Layered oxides Lattice doping Mixed phase

Recent Advances in Asymmetric Structural Composites for Excellent Electromagnetic Interference Shielding: A Review

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Chinese Journal of Polymer Science 2024年第6期42卷 693-710页

作者： Ying Zhou Bai Xue Lan Xie Chang-Mei Wu Qiang Zheng Department of Polymer materials and engineering College of Materials and Metallurgy Guizhou University National engineering research center for Compounding and Modification of Polymer materials National and Local Joint Engineering Research Center for Functional Polymer Membrane Materials and Membrane Processes State Key Laboratory of Public Big Data Guizhou University Department of Polymer Science and engineering Zhejiang University

Since electromagnetic pollution is detrimental to human health and the environment, numerous efforts have been successively made to achieve excellent electromagnetic interference shielding effectiveness(EMI SE) via designing the hierarchical structures for electromagnetic interference(EMI) shielding polymer composites. Among the plentiful structures, the asymmetric structures are currently a hot spot, principally categorizing into multi-layered, porous, fibrous, and segregated asymmetric structures, which endows the high EMI shielding performance for polymer composites incorporated with magnetic, conductive, and/or dielectric micro/nano-fillers, due to the “absorption-reflection-reabsorption” shielding mechanism. Therefore, this review provides the retrospection and summary of the efforts with respect to abundant asymmetric structures and multifunctional micro/nano-fillers for enhancing EMI shielding properties, which is conducive to the booming development of polymeric EMI shielding materials for the promising prospect in modern electronics and 5-generation(5G) technology.

关键词： Asymmetric structure Microano functional filler Polymer composite Electromagnetic interference shielding

Structurally Flexible 2D Spacer for Suppressing the Electron-Phonon Coupling Induced Non-Radiative Decay in Perovskite Solar Cells

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Nano-Micro Letters 2024年第9期16卷 325-340页

作者： Ruikun Cao Kexuan Sun Chang Liu Yuhong Mao Wei Guo Ping Ouyang Yuanyuan Meng Ruijia Tian Lisha Xie Xujie Lü Ziyi Ge Zhejiang Provincial engineering research center of Energy Optoelectronic materials and Devices Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201People’s Republic of China School of materials Science and Chemical engineering Ningbo UniversityNingbo 315211People’s Republic of China center of materials Science and Optoelectronics engineering University of Chinese Academy of SciencesBeijing 100049People’s Republic of China center for High Pressure Science and Technology Advanced research(HPSTAR) Shanghai 201203People’s Republic of China

This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))analog.It demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation.The resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.

关键词： Electron-phonon coupling A-site cation engineering Non-radiative recombination

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