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Enantioselective copper-catalyzed dearomative borylative cyclization of indoles and mechanistic insights

Science China Chemistry 2025年第2期68卷 670-678页

作者： Yanfei Li Xuetao Li Zheng Zhang Yiliang Zhang Xiuping Yuan Jianjun Yin Simin Wang Wei Guan Qian Zhang Tao Xiong jilin province key laboratory of organic functional molecular design&synthesis Department of ChemistryNortheast Normal UniversityChangchun 130024China Institute of functional Material Chemistry Department of ChemistryNortheast Normal UniversityChangchun 130024China State key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Chemical Engineering Harbin Normal UniversityHarbin 150025China

Alicyclic nitrogen heterocycles,such as enantioenriched polycyclic fused[1,2-a]indoline derivatives,are widespread in natural products,agrochemicals and pharmaceutical *** methods predominantly rely on the recent emerging Heck-type catalytic asymmetric dearomatization(CADA)protocol,wherein noble palladium catalysts commonly necessitate the form arylPd species-triggered these *** contrast,a more sustainable base metal catalysis paradigm through alkyl metal species disrupting the aromaticity,that is,the utilization of challenging asymmetric Csp3–Csp3 bond formation entry to such important chiral densely functionalized polycyclic molecular scaffolds,remains an elusive ***,we report the first copper-catalyzed dearomative borylative cyclization of indoles under mild reaction conditions,affording an array of valuable Bpin-containing pyrrolo-fused[1,2-a]indolines bearing four consecutive stereogenic centers with excellent enantioand *** synthetic potential was documented via an array of useful *** functional theory(DFT)calculation studies elucidated the origin of the chemo-,regio-,enantio-and diastereoselectivities of this conversion.

关键词： copper catalysis dearomatization borylative cyclization indoles DFT calculations

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Cyano migration-mediated radical-polar crossover cyclopropanation

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Science China Chemistry 2025年第1期68卷 241-248页

作者： Ziqiang Wang Yasu Chen Jie Li Chen Zhu key laboratory of organic synthesis of Jiangsu province College of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Study and Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

We report a novel cyano migration-mediated radical-polar crossover process,whereby both the sulfonylcyanation of aliphatic alkenes and the formation of cyclopropanes are concurrently *** transformation yields a diverse array of multisubstituted cyclopropanes under mild photocatalytic *** studies elucidate that the reaction proceeds via intramolecular nucleophilic substitution,leading to the formation of the cyclopropane derivatives.

关键词： cyclopropanation cyano migration radical-polar crossover radical reactions

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Dip2a regulates stress susceptibility in the basolateral amygdala

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Neural Regeneration Research 2025年第6期20卷 1735-1748页

作者： Jing Li Zixuan He Weitai Chai Meng Tian Huali Yu Xiaoxiao He Xiaojuan Zhu key laboratory of molecular Epigenetics Ministry of Education Institute of Genetics and CytologyNortheast Normal UniversityChangchunJilin ProvinceChina

Dysregulation of neurotransmitter metabolism in the central nervous system contributes to mood disorders such as depression, anxiety, and post–traumatic stress disorder. Monoamines and amino acids are important types of neurotransmitters. Our previous results have shown that disco-interacting protein 2 homolog A(Dip2a) knockout mice exhibit brain development disorders and abnormal amino acid metabolism in serum. This suggests that DIP2A is involved in the metabolism of amino acid–associated neurotransmitters. Therefore, we performed targeted neurotransmitter metabolomics analysis and found that Dip2a deficiency caused abnormal metabolism of tryptophan and thyroxine in the basolateral amygdala and medial prefrontal cortex. In addition, acute restraint stress induced a decrease in 5-hydroxytryptamine in the basolateral amygdala. Additionally, Dip2a was abundantly expressed in excitatory neurons of the basolateral amygdala, and deletion of Dip2a in these neurons resulted in hopelessness-like behavior in the tail suspension test. Altogether, these findings demonstrate that DIP2A in the basolateral amygdala may be involved in the regulation of stress susceptibility. This provides critical evidence implicating a role of DIP2A in affective disorders.

关键词： 5-hydroxytryptamine acute restraint stress basolateral amygdala CaMKII neurons DIP2A metabolomics neurotransmitters principal component analysis stress susceptibility tryptophan

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Synergistic BrΦnsted/Lewis acid catalyzed atroposelective synthesis of aryl-β-naphthol

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Chinese Chemical Letters 2025年第1期36卷 293-298页

作者： Jiajun Lu Zhehui Liao Tongxiang Cao Shifa Zhu key laboratory of functional molecular Engineering of Guang-dong province School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou 510640China School of Chemistry and Chemical Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China State key laboratory of Elemento-organic Chemistry Nankai UniversityTianjin 300071China

Axially chiral binaphthol have achieved great success in asymmetric *** toα-binaphthol,axially chiral aryl-β-naphthol are far less ***,we report a method of asymmetric catalysis to constructβ-naphthol with up to 99%yield,95.5:4.5 enantiomeric ratio,using alkynyl esters as precursors and chiral phosphonic acid(CPA)/Lewis acid as *** steps involve oxygen transfer and de novo arene formation to set up the chiral ***,this methodology provides a versatile platform for structurally divergent synthesis of atroposelectiveβ-naphthol analogs,which are widely found in bioactive molecules and asymmetric catalysts.

关键词： Synergistic catalysis Atropisomerism Aryl-β-naphthol Enantioselectivity Tandem reaction

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Fluorinated poly(p-triphenylene isatin)anion exchange membranes based on hydrophilic hydroxyl side chain modulation for fuel cells

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Journal of Energy Chemistry 2025年第1期100卷 702-709页

作者： Yiman Gu Yanchao Zhang Zhanyu Li Yijia Lei Baozeng Sun Xiaoyu Yu Zhe Wang College of Chemistry and Life Science Changchun University of TechnologyChangchun 130012JilinChina College of Chemical Engineering Changchun University of TechnologyChangchun 130012JilinChina School of Materials Science and Engineering Changchun University of TechnologyChangchun 130012JilinChina key laboratory of Advanced functional Polymer Membrane Materials of jilin province Changchun 130012JilinChina

The development of alkaline fuel cells is moving forward at an accelerated pace,and the application of ether-free bonded polymers to anion exchange membranes(AEMs)has been widely ***,the question of the“trade-off”between AEM ionic conductivity and dimensional stability remains *** strategy of inducing microphase separation to improve the performance of AEM has attracted much attention recently,but the design of optimal molecular structures is still being ***,this work introduced different ratios of 3-bromo-1,1,1-trifluoroacetone(x=40,50,and 60)into the main chain of poly(p-terphenylene isatin).Because fluorinated groups have excellent hydrophobicity,hydrophilic hydroxyl-containing side chains are introduced to jointly adjust the formation of phase separation *** results show that PTI-PTF_(50)-NOH AEM with the appropriate fluorinated group ratio has the best ionic conductivity and alkali stability under the combined effect of *** has an ionic conductivity of 133.83 mS cm^(-1)at 80°*** addition,the OH-conductivity remains at 89%of the initial value at 80°C and 3 M KOH for 1056 h of *** cell polarization curve based on PTI-PTF_(50)-NOH shows a power density of 734.76 mW cm^(-2)at a current density of 1807.7 mA cm^(-2).

关键词： Anion exchange membranes Poly(p-terphenylene isatin) Hydrophilic-hydrophobic phase separation Fluorinated group

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Solid-state synthesis of mesoporous metals via mechanochemical coordination self-assembly

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Science China Chemistry 2025年第2期68卷 492-498页

作者： Hailong Xiong Chunyu Qi Lantian Xue Ling Zhang Hanyu Liu Zhen-An Qiao State key laboratory of Inorganic synthesis and Preparative Chemistry Jilin UniversityChangchun 130012China State key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China State key laboratory of Superhard Materials College of PhysicsJilin UniversityChangchun 130012China Hefei National Research Center for Physical Sciences at the Microscale University of Science and Technology of ChinaHefei 230026China

Mesoporous metals with large surface area,high pore volume,and uniform pore structure hold excellent advantages for various ***,the state-of-the-art synthesis methods are still limited to wet chemistry,which requires excessive solvents and a time-consuming drying ***,we report a facile and general mechanochemical coordination self-assembly strategy to prepare mesoporous metals(e.g.,Rh,Ru,Ir,Pt,Pd,Ag,Co,and Ni)with remarkable porous properties by using metal chlorides and cationic polymer *** with the wet chemistry process,this method proceeds without solvents and does not need complicated experimental conditions and long synthetic periods,which not only greatly reduces the consumption of cost and energy and environmental pollution,but also improves the synthesis efficiency and yield of target *** believe the developed approach will provide a general pathway for the scalable preparation of advanced porous materials.

关键词： mechanochemistry self-assembly mesoporous materials mesoporous metals electrocatalysis

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Radical functionalization of 1,6-Diene via Transannular Cyano Migration:synthesis of Polysubstituted Cyclopentanes

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Chinese Journal of Chemistry 2025年第4期43卷 437-442页

作者： Ziqiang Wang Yasu Chen Chen Zhu Frontiers Science Center for Transformative Molecules Zhangjiang Institute for Advanced Studyand Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong University800 Dongchuan RoadShanghai 200240China key laboratory of organic synthesis of Jiangsu province College of ChemistryChemical Engineering and Materials ScienceSoochow University199 Ren-Ai RoadSuzhouJiangsu 215123China

An efficient transannular cyano migration is reported for gem-dicyano-1,6-diene,which is triggered by the addition of external arylsulfonyl *** overall transformation proceeds through a sequence of intramolecular 5-exo-trig cyclization,suprafacial 1,4-cyano migration,and the capture by H or D atom,leading to the production of valuable polysubstituted cyclopentanes under mild photoredox catalytic *** reaction is adapted to a wide range of sodium(hetero)arylsulfinates,demonstrating good functional group *** method provides a new protocol for radical-mediated functional group migration.

关键词： Cyano migration Cyclopentane 1,6-Diene Photoredox catalysis Radical reactions Radicals Cyclization Rearrangement

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Generation of Isolated Attosecond Pulses by the Harmonic Spectrum of MgO under a Three-Color Laser Pulse

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Chinese Physics Letters 2025年第1期42卷 48-52页

作者： Jiaqi Chen Wenli Jiang Yue Qiao Yujun Yang Jigen Chen School of Materials Science and Engineering Taizhou UniversityTaizhou 318000China Institute of Atomic and molecular Physics Jilin UniversityChangchun 130012China jilin Provincial key laboratory of Applied Atomic and molecular Spectroscopy(jilin University) Changchun 130012China

This study examines the high-order harmonic radiation behavior of MgO crystals driven by combined pulses based on the numerical solution of the semiconductor Bloch *** found that compared with the monochromatic pulse,the MgO crystal can radiate a continuous harmonic spectrum with two platforms driven by the three-color combined *** reason is that under the three-color combined pulse,the electron ionization and recombination can be effectively controlled within a half-optical cycle of the laser *** this continuous spectrum,we synthesized an isolated attosecond pulse with a duration of approximately 370 *** study provides a new perspective on all-solid-state compact optical devices.

关键词： pulse optical harmonic

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Modulation of the octahedral structure and potential superconductivity of La_(3)Ni_(2)O_(7)through strain engineering

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Science China(Physics,Mechanics & Astronomy) 2025年第3期68卷 145-152页

作者： Zihao Huo Zhihui Luo Peng Zhang Aiqin Yang Zhengtao Liu Xiangru Tao Zihan Zhang Shumin Guo Qiwen Jiang Wenxuan Chen Dao-Xin Yao Defang Duan Tian Cui key laboratory of Material Simulation Methods&Software of Ministry of Education State Key Laboratory of Superhard MaterialsCollege of PhysicsJilin UniversityChangchun130012China Center for Neutron Science and Technology Guangdong Provincial Key Laboratory of Magnetoelectric Physics and DevicesState Key Laboratory of Optoelectronic Materials and TechnologiesSchool of PhysicsSun Yat-sen UniversityGuangzhou510275China MOE key laboratory for Non-equilibrium synthesis and Modulation of Condensed Matter Shaanxi Province Key Laboratory of Advanced Functional Materials and Mesoscopic PhysicsSchool of PhysicsXi’an Jiaotong UniversityXi’an710049China Institute of High Pressure Physics School of Physical Science and TechnologyNingbo UniversityNingbo315211China

The recent transport measurements of La_(3)Ni_(2)O_(7)uncovered a“right-triangle”shape of the superconducting dome in the pressure-temperature(P-T)phase *** by this,we perform theoretical first-principles studies of La_(3)Ni_(2)O_(7)with the pressure ranging from 0 to 100 ***,we reveal a pressure dependence of the Ni-d_(z^(2))electron density at the Fermi energy(n_(z)^(E_(F)))that highly coincides with such *** this basis,we further explore the electronic structure under uniaxial *** tracking the stress response of n_(z)^(E_(F)),we propose that superconductivity can be achieved by applying only ~2GPa of compression along the c *** idea is further exemplified from the perspectives of lattice distortion,band structure,Fermi surface and superconducting phase *** also discuss the possible charge modulation under the stress and provide an insight into the relation between nz E Fand the superconducting T_(c)in La_(3)Ni_(2)O_(7)*** study provides new routes to the search of high-T_(c)superconductors in future experiments.

关键词： nickelate superconductors density functional theory strong correlated systems strain engineering

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synthesis and Photochromism of Diazocine Derivatives:Relationship Between Photoswitching Properties and molecular Structures

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Chemical Research in Chinese Universities 2025年第1期41卷 33-39页

作者： WANG Yaxin CHEN Yulan key laboratory of organic Integrated Circuit Ministry of Education&Tianjin Key Laboratory of Molecular Optoelectronic SciencesDepartment of ChemistrySchool of ScienceTianjin UniversityTianjin300072P.R.China State key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun130012P.R.China

We design and synthesize five novel diazocine derivatives,using diazocine as the core,amide or imine bonds as the connecting units attached with different peripheral *** photoisomerization yield and thermal stability of these derivatives are tested by^(1)H NMR and UV-Vis absorption *** them,the imine-linked derivative exhibits the lowest photoisomerization efficiency,while the amide-linked ones show an elevated switching efficiency in transitioning from the cis to the trans configuration,compared to the unmodified 3,3′-***,based on experiments together with density functional theory(DFT)calculations,we find that the thermal stability of these derivatives is associated with the electron cloud density and steric hindrance of their *** to these unique photophysical properties,diazocine derivatives provide a foundation for the development and application of molecular optical switches.

关键词： Diazocine Photoisomerization Thermal stability

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