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Chinese Journal of Polymer Science 2025年第2期43卷 278-288页

作者： Ming-Hang Wang Fan Yang Yong-Jian Zhang shanghai key laboratory for molecular engineering of chiral drugs Frontiers Science Center for Transformative Moleculesand School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai200240China Sichuan Research Institute Shanghai Jiao Tong UniversityChengdu610042China

Control crosslink network and chain connectivity are essential to develop shape memory polymers(SMPs)with high shape memory capabilities,adjustable response temperature,and satisfying mechanistical *** this study,novel poly(ε-caprolactone)(PCL)-poly(2-vinyl)ethylene glycol(PVEG)copolymers bearing multi-pendant vinyl groups is synthesized by branched-selective allylic etherification polymerization of vinylethylene carbonate(VEC)with linear and tetra-arm PCLs under a synergistic catalysis of palladium complex and boron *** thiol-ene photo-click reaction of PCL-PVEG copolymers with multifunctional thiols can rapidly access a serious crosslinked SMPs with high shape memory *** thermal properties,mechanical properties and response temperature of the obtained SMPs are tunable by the variation of PCL prepolymers,vinyl contents and functionality of ***,high elastic modulus in the rubbery plateau region can be maintained effectively owing to high-density topological networks of the PCL *** addition,the utility of the present SMPs is further demonstrated by the post-functionalization via thiol-ene photo-click chemistry.

关键词： Shape memory polymers Polycaprolactone Thiol-ene photo-crosslink Controlled crosslinking density Tunable response temperature

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

Synthesis of ordered mesoporous crystalline boron phosphate scaffold with double diamond surface structure

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Science China Chemistry 2025年第2期68卷 590-600页

作者： Chao Wang Wen-Duo Lu Jiao Wang Shunai Che An-Hui Lu Lu Han School of Chemical Science and engineering Tongji UniversityShanghai 200092China State key laboratory of Fine Chemicals Liaoning Key Laboratory for Catalytic Conversion of Carbon ResourcesSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China School of Chemistry and Chemical engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

Ordered mesoporous materials have received great attention due to their well-defined pore structures and potential applications in catalysis,adsorption,separation,drug delivery,*** various compositions of mesoporous solids have been successfully prepared,the preparation of crystalline non-metallic oxyacid salts with ordered mesoporosity remains a major ***,we report the synthesis of a mesoporous solid acid crystalline boron phosphate(BPO_(4))catalyst with a bicontinuous shifted double diamond(SDD)hyperbolic surface *** BPO_(4) scaffold was obtained by synergistic selfassembly in a mixed solvent of water and tetrahydrofuran using the diblock copolymer poly(ethylene oxide)-block-polystyrene as template and phosphoric acid and orthoboric acid as inorganic *** structure consists of two sets of diamond networks adjacent to each other with a mesostructural scale tetragonal symmetry(space group I4_(1)/amd)with unit cell parameters of a=80 nm and c=113 nm,which affords the scaffold a specific surface area of 44 m^(2)/*** a solid acid catalytic material,the SDD BPO_(4) scaffold exhibited excellent catalytic activity at room temperature with a conversion of furfural to 2-(dimethoxymethyl)furan over 70%and can be reused after recovery without serious loss of *** the propane oxidative dehydrogenation reaction,SDD BPO_(4) demonstrated high olefin productivity and selectivity while maintaining high reaction *** study provides ideas for the preparation of ordered mesoporous crystalline catalytic materials and demonstrates their potential for practical applications.

关键词： boron phosphate mesoporous material self-assembly block copolymer catalyst

Co nanoparticles confined in mesopores of MFI zeolite for selective syngas conversion to heavy liquid hydrocarbon fuels

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Chinese Journal of Catalysis 2025年第1期68卷 246-258页

作者： Neng Gong Quanzheng Deng Yujiao Wang Zitao Wang Lu Han Peng Wu Shun'ai Che School of Chemical Science and engineering Tongji UniversityShanghai 200092China Multi-scale Porous Materials Center Institute of Advanced Interdisciplinary Studies&School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 400044China State key laboratory of Inorganic Synthesis&Preparative Chemistry Jilin UniversityChangchun 130015JilinChina shanghai key laboratory of Green Chemistry and Chemical Processes State Key Laboratory of Petroleum Molecular&Process EngineeringSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China School of Chemistry and Chemical engineering Frontiers Science Center for Transformative MoleculesState Key Laboratory of Metal Matrix CompositesShanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai 200240China

Designing Fischer-Tropsch synthesis(FTS)catalysts to selectively produce liquid hydrocarbon fuels is a crucial ***,we selectively introduced Co nanoparticles(NPs)into the micropores and mesopores of an ordered mesoporous MFI zeolite(OMMZ)through impregnation,which controlled the carbon number distribution in the FTS products by tuning the position of catalytic active sites in differently sized *** Co precursors coordinated by acetate with a size of 9.4×4.2×2.5Åand by 2,2‘-bipyridine with a size of 9.5×8.7×7.9Å,smaller and larger than the micropores(ca.5.5Å)of MFI,made the Co species incorporated in OMMZ's micropores and mesopores,*** carbon number products synthesized with the Co NPs confined in mesopores were larger than that in *** high jet and diesel selectivities of 66.5%and 65.3%were achieved with Co NPs confined in micropores and mesopores of less acidic Na-type OMMZ,*** and jet selectivities of 76.7%and 70.8%were achieved with Co NPs confined in micropores and mesopores of H-type OMMZ with Brönsted acid sites,respectively.A series of characterizations revealed that the selective production of diesel and jet fuels was due to the C-C cleavage suppressing of heavier hydrocarbons by the Co NPs located in mesopores.

关键词： Fischer-Tropsch synthesis Heavy liquid hydrocarbon fuel Co nanoparticle Ordered mesoporous MFI zeolite C-C cleavage

A rechargeable and portable hydrogen storage system grounded on soda water

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Chinese Chemical Letters 2025年第3期36卷 333-338页

作者： Lingyun Shen Shenxiang Yin Qingshu Zheng Zheming Sun Wei Wang Tao Tu shanghai key laboratory of molecular Catalysts and Innovative Materials Department of Chemistry Fudan University Frontiers Science Center for Transformative Molecules Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs School of Chemistry and Chemical Engineering and Zhangjiang Institute for Advanced Study Shanghai Jiao Tong University State key laboratory of Organometallic Chemistry Shanghai Institute of Organic Chemistry Chinese Academy of Sciences Departments of Pharmacology and Toxicology and Chemistry and Biochemistry University of Arizona State key laboratory of High-efficiency Utilization of Coal and Green Chemical engineering School of Chemistry and Chemical EngineeringNingxia University

The bicarbonate-formate（HCO-3– HCO-2） interconversion provides a promising cycle for a conveniently accessible hydrogen storage system via reversible dehydrogenation and hydrogenation processes. Existing catalytic systems often use organic solvents, tedious optimization as well as manipulation of pH values,solvent, pressure and various additives. Herein, we present an operational, robust, safe and cost-effective catalytic system for hydrogen storage and liberation. We have established a unique catalytic system with two different solid organometallic assemblies（NHC-Ru and NHC-Ir） that facilitate the reversible transformation between sodium formate and bicarbonate in aqueous solutions collaboratively and efficiently. Notably, the NHC-Ru catalyst is privileged for the hydrogenation of sodium bicarbonate, whereas the NHC-Ir component enables the dehydrogenation of sodium formate, all in a single reaction vessel. What sets this system apart is its simplicity. The H2discharging and recharging is simply regulated by heating the mixture with or without H2. Remarkably, this process requires no extra additives or supplementary treatments. Moreover, the reversible hydrogen storage system is durable and can be reused for over 30 cycles without a discernible decline in activity and selectivity. The strategic paradigm in this study shows significant practical potential in hydrogen fuel cell applications.

关键词： Dehydrogenation Hydrogen storage Hydrogenation N-Heterocyclic carbene Soda water

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

Oscillatory flow reactor facilitates fast photochemical Wolff rearrangement toward synthesis ofα-substituted amides in flow

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Chinese Chemical Letters 2025年第2期36卷 361-365页

作者： Huashan Huang Jingze Chen Luyun Zhang Hong Yan Siqi Li Fen-Er Chen Institute of Pharmaceutical Science and Technology College of ChemistryFuzhou UniversityFuzhou 350108China key laboratory of Natural Medicines of the Changbai Mountain Ministry of EducationMolecular Medicine Research CenterCollege of PharmacyYanbian UniversityYanji 133002China engineering Center of Catalysis and Synthesis for chiral Molecules Department of ChemistryFudan UniversityShanghai 200433China shanghai engineering Center of Industrial Catalysis for chiral drugs Shanghai 200433China

A visible light-promoted fast photochemical Wolff rearrangement was developed toward synthesis ofα-substituted amides in continuous flow with the use of a photochemical oscillatory flow reactor(POFR).The control experiment indicates that a fast process of the Wolff rearrangement(<40 s)is ***,this protocol does not require excess use of any reactants,and the resultingα-substituted amides could be isolated by recrystallization in good to excellent yields.

关键词： Flow photochemistry Oscillatory flow reactor Wolff rearrangement Ketene α-Substituted amides

Double[5]carbohelicene:facile synthesis,chiroptical properties,isomerization study,and lasing application

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Science China Chemistry 2025年第1期68卷 233-240页

作者： Peipei Liu Yantong Li Meng-Xiang Wu Hao Kang Xiao-Li Zhao Lin Xu Linlin Liu Xiaodong Li Junfeng Fang Zhiwei Fang Ya Cheng Hai-Bo Yang Huakang Yu Xueliang Shi State key laboratory of Petroleum molecular&Process engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200062China School of Physics and Optoelectronics South China University of TechnologyGuangzhou 510640China School of Physics and Electronic Science Engineering Research Center of Nanophotonics&Advanced InstrumentMinistry of EducationEast China Normal UniversityShanghai 200241China State key laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200241China Institute of Polymer Optoelectronic Materials&Devices State Key Laboratory of Luminescent Materials&DevicesSouth China University of TechnologyGuangzhou 510640China

Double carbohelicenes have attracted considerable attention due to their aesthetic structures,distinctπ-conjugation extension,inherent chirality,and intriguing optical and electronic ***,the concise de novo synthesis of a new double[5]carbohelicene 1 together with its chiroptical properties,isomerization process and lasing application is presented.1 was synthesized by a simple protocol involving the formation of a 6,6′-bipentacene as the key *** is worth noting that1 existed as two diastereomers 1-PP/MM and 1-PM,which were successfully isolated and unambiguously confirmed by Xray *** optical resolution of the racemic 1-PP/MM was successfully achieved by chiral-phase highperformance liquid chromatography(HPLC),and 1-PP and 1-MM were characterized by circular ***,it was found that 1-PP/MM could be completely isomerized to 1-PM upon heating,and the detailed thermodynamics and kinetics of the isomerization process were systematically investigated.1-PM exhibited deep-red luminescence with emission maximum at 723 nm and fluorescence quantum yield as high as 32.95%.Consequently,we can showcase the lasing application of 1-PM by doping with epoxy resin to assemble a bottle microlaser spontaneously,which the lasing wavelength is 796.6 nm at a threshold of 0.8 m J cm^(-2).We believe that our studies,including the facile synthesis methodology,detailed isomerization studies,and lasing application,will shed some light on the design and synthesis of novel carbohelical systems with more functions.

关键词： double carbohelicene optical resolution organic laser isomerization X-ray diffraction

Tandem asymmetric propargylic amination/carboxylative cyclization reaction to chiral 5-methylidene-2-oxazolidinones using CO2 as C1 synthon

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Science China Chemistry 2025年第4期 1402-1411页

作者： Zheng Zhang Zhi-Hao Zhang Ying Sun Yun-Hao Tang Yi-Zhuo Yang Feng Zhou Jian Zhou State key laboratory of Petroleum molecular & Process engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesShanghai Engineering Research Center of Molecular Therapeutics and New Drug DevelopmentSchool of Chemistry and Molecular EngineeringEast China Normal University State key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of Sciences

We report a tandem asymmetric Cu-catalyzed propargylic amination（ACPA）/Ag-catalyzed carboxylative cyclization（SCC）with CO2to 5-methylidene-2-oxazolidinones, even with tetrasubstituted stereocenters. By varying pyridine bisoxazoline（PYBOX） ligands, a general and highly enantioselective ACPA of unprecedentedly broad scope of secondary propargylic acetates and primary amines is achieved. Both α-aryl and α-aliphatic propargylic acetates could react with either aromatic or aliphatic primary amines to give the corresponding N-aryl or N-aliphatic ethynylamines with α-aliphatic or α-aryl groups in over 90% ee for use in the next step. The key to developing this one-pot sequence is to use a chelator triethylenetetramine（TETA） to mask the copper ion, to avoid its negative effect on Ag-catalyzed cyclization, whilst releasing PYBOX to activate the silver catalyst. With the methylidene moiety, these oxazolidinones can be readily elaborated. The value of the sequence is further shown by the catalytic enantioselective total synthesis of（–）-cytoxazone and the potent ezetimibe analogue.

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

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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