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Science China Chemistry 2024年第7期67卷 2306-2313页

作者： Dong-Yue Cai Weiming Shi Zhao-Hui Jin Zhi-Xiang Yu Jin-Xin Zhao Jian-Min Yue State key laboratory of Drug Research Shanghai Institute of Materia MedicaChinese Academy of SciencesShanghai 201203China University of Chinese Academy of Sciences Beijing 100049China Beijing National laboratory for molecular Sciences(BNLMS) Key Laboratory of Bioorganic Chemistry and Molecular Engineering of Ministry of EducationCollege of ChemistryPeking UniversityBeijing 100871China

Mimicking biosynthetic pathways of hongkonoids led to the development of a new Cu(Ⅰ)-catalyzed[3+2]cycloaddition ofα-hydroxyketone andβ-keto enol ethers,affording tetrahydrofuran acetals in a highly diastereoselective manner and 100%atom *** studies on the mechanism disclosed a concerted but asynchronous Michael addition/aldol *** the same importance,this methodology provides a practical biomimetic approach for one-step construction of the dibenzylbutyrolactol lignan backbone starting from two phenyl propane derivatives,opening up a powerful new approach for lignan synthesis,which is showcased by succinct total syntheses of two biologically important aryltetralin-type lignans,β-apopicropodophyllin and *** the mild and operationally simple conditions,the developed chemistry might have a promising prospect in potential industrial applications.

关键词： [3+2]cycloaddition transition-metal catalysis tetrahydrofuran lignans natural products

New sustainable polymers with on-demand depolymerization property

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Science China Chemistry 2024年第9期67卷 2803-2841页

作者： Yangyang Sun Zesheng An Yanshan Gao Rongrong Hu Ye Liu Hua Lu Xiao-Bing Lu Xuan Pang Anjun Qin Yong Shen Youhua Tao Yu-Zhong Wang Junpeng Wang Gang Wu Guang-Peng Wu Tie-Qi Xu Xing-Hong Zhang Yuetao Zhang Zhenbiao Zhang Jian-Bo Zhu Miao Hong Zhibo Li State key laboratory of Organometallic Chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China State key laboratory Base of Eco-Chemical engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao266042China State key laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China State key laboratory of Luminescent Materials and Devices Guangdong Provincial Key Laboratory of Luminescence from Molecular AggregatesSouth China University of TechnologyGuangzhou 510640China State key laboratory of Fine Chemicals Frontiers Science Center for Smart MaterialsDalian University of TechnologyDalian 116024China Beijing National laboratory for molecular Sciences Center for Soft Matter Science and EngineeringKey Laboratory of Polymer Chemistry and Physics of Ministry of EducationCollege of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871China key laboratory of Polymer Ecomaterials Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China The Collaborative Innovation Center for Eco-Friendly and Fire-Safety Polymeric Materials(MoE) National Engineering Laboratory of Eco-Friendly Polymeric Materials(Sichuan)College of ChemistryState Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu 610064China School of Polymer Science and Polymer engineering the University of AkronAkronOH 44325USA MOE key laboratory of Macromolecular Synthesis and Functionalization Department of Polymer Science and EngineeringZhejiang UniversityHangzhou 310027China State and Local Joint engineering laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and ApplicationSuzhou Key Laboratory of Macromolecular Design and Precision SynthesisCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

To combat the crisis of today's synthetic polymers arising from unsustainable production and disposal,it is essential for the synthetic polymer community to reshape the current polymer industry with sustainable *** an emerging class of sustainable polymers,the development of chemically depolymerizable polymers(CDPs),which can undergo closed-loop depolymerization/repolymerization cycles to reproduce virgin polymers without the loss of properties from recovered monomers,offers an ideal solution to preserve finite natural resources,provides a feasible solution to the end-of-life issue of polymer waste,and thereby establishes a circular materials ***,two grand key challenges have been encountered in the establishment of practically useful CDPs:how to balance polymerization and depolymerization ability and how to unify conflicted depolymerizability and physical ***,this critical review article presents our vision for summarizing feasible strategies to overcome the above two significant challenges and the design principles for constructing an ideal CDP by highlighting selected major progress made in this rapidly expanding field.

关键词： chemically depolymerizable polymers sustainable polymers depolymerization monomer recovery degradation plastics

Increase of chiral sensing ability in host-guest chemistry by magnetic anisotropy

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Science China Chemistry 2024年第8期67卷 2775-2782页

作者： Jia-Liang Chen Bin Li Feng Yang Tiesheng Shi Xun-Cheng Su State key laboratory of Elemento-organic Chemistry Tianjin Key Laboratory of Biosensing and Molecular RecognitionCollege of ChemistryNankai UniversityTianjin 300071China College of Chemistry Chemical Engineering and Materials ScienceZaozhuang UniversityZaozhuang 277160China

Enantiomeric molecules generally play distinct functions in chemistry,biology,and *** physical and chemical properties of chiral analytes lay difficulty in discrimination and quantification of the *** report herein an efficient approach of increasing the chiral sensing ability ofβ-cyclodextrin(β-CD),a widely used host molecule,in the hostguest chemistry by magnetic anisotropy.A rigid and chiral lanthanide binding tag was attached to theβ-CD to amplify the changes of nuclear magnetic resonance(NMR)signals in the host-guest recognition *** installation of the paramagnetic lanthanide ion inβ-CD greatly enhances the enantiomeric discrimination up to 30-fold in comparison with the diamagneticβ-CD *** addition,the magnitude of the paramagnetic effects is tunable according to the diverse range of paramagnetic strength of the lanthanide *** reported method significantly increases the chiral sensing ability ofβ-CD,which can be applied to other host *** transferred paramagnetic effects,pseudocontact shifts(PCSs)and paramagnetic relaxation enhancements(PREs),from the host to the guest molecules,are valuable structural restraints to determine the absolute stereochemistry of the chiral *** strategy does not need modification of the analytes and is complementary to the reported analytical methods that rely on the functionalization of the chiral analytes.

关键词： chiral recognition nuclear magnetic resonance host-guest chemistry magnetic anisotropy lanthanide ions

Self-powered stimuli responsive material for dual stimulation of heat and guest molecules

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Chinese Chemical Letters 2024年第2期35卷 590-593页

作者： Jintao Men Ke Xu Taiting Sha Lei He Yan Xu Jie Mu Tijian Yin Qiong Ye Jiangsu key laboratory for Science and Applications of molecular Ferroelectrics and School of Chemistry and Chemical engineering Southeast UniversityNanjing 211189China

Stimuli-responsive smart materials exhibit reverse chemical/physical changes in response to external stimuli and research on stimuli-responsive smart materials with self-powered properties is still uncultivated ***,we report perovskite crystalline self-powered multiple stimuli-responsive materials triggered by chemical and thermal stimuli.[HMEP]PbI_(3)·(H_(2)O)(1;HMEP is a hydroxytris(1-methylethyl)phosphorus cation)crystallizes in a chiral space group P 21 at 293 K and has the piezoelectric reaction(d_(33)=10 pC/N and output voltage=1 V)of self-powered modes,this value is larger than the value of 3 pC/N for the classical piezoelectric material *** materials can generate energy due to mechanical deformation,and using thermal heating to lose water,[HMEP]PbI_(3)(2)can be obtained.2 crystallizes in the non-centrosymmetric space group,undergoes two reversible phase transitions at 243/255 K and 315/348 K,and shows second harmonic generation ***,2 can return to the hydrated form 1 after absorbing *** work will lay the foundation for self-powered stimuli-responsive compounds and contribute to the construction of novel organic-inorganic hybrid materials with second harmonic generation switching.

关键词： Self-powered Dual stimulation reactive Phase transition SHG switch Organic-inorganic hybrid perovskite

Effect of samarium doping on the activity and sulfur resistance of Ce/MnFeO_(x) catalyst for low-temperature selective catalytic reduction of NO_(x) by ammonia

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Chinese Journal of Chemical engineering 2024年第7期71卷 272-282页

作者： Qiyao Zhang Shuangshuang Zhang Xu Hu Yongmin Huang key laboratory of Specially Functional Polymeric Materials and Related Technology School of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

The self-made MnFeO_(x) catalysts doped with cerium and samarium were prepared by impregnation method for low-temperature selective catalytic reduction(SCR)by *** this work,the surface properties of the series of MnFe-based catalysts were *** results indicate Sm-modified catalyst have superior low-temperature SCR activity;NO_(x) conversion maintained at nearby to 100%at 90℃ to 240℃.In addition,The N_(2) selectivity of Sm doping remains above 80%in the range of 60℃ to 150℃.In SO_(2) poisoning test,the NO_(x) conversion can be remained>90%after 10 h of *** XPS,NH_(3)-TPD and H_(2)-TPR results show the catalyst with Sm doping enhances the acid sites and oxidation catalytic sites of mixed oxides serves for improving oxygen vacancies and transfer *** situ diffuse reflaxions infrared Fourier transformations spectroscopy(DRIFTS)results show that NO_(x) is more easily adsorbed on the surface after Sm doping,which provided favorable conditions for the NH_(3)-SCR reaction to *** reaction at the catalyst surface will follow the L-H reaction mechanism by transient reaction test.

关键词： SCR Sm doping Catalyst Sulfur resistance In situ DRIFTS Selectivity

MnO_(2)-coated nanodiamond-driven photodynamic therapy for enhanced antitumor effect by addressing hypoxia and glutathione depletion

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Particuology 2024年第9期92卷 305-315页

作者： Jicheng Cui Dongmei Zhang Hui Qiao Zeyu Yan Wenxia Zhang Yingqi Li key laboratory of Chemical Biology and molecular engineering of Ministry of Education Institute of Molecular ScienceShanxi UniversityTaiyuan030006China Taiyuan Central Hospital Taiyuan030009China School of Chemistry and Chemical engineering Shanxi UniversityTaiyuan030006China

The generation of reactive oxygen species(ROS)at the tumor site to induce destruction is emerging as a novel strategy for cancer treatment,which involves photodynamic therapy(PDT).Nevertheless,tumors typically create a hypoxic environment and are equipped with an endogenous antioxidant defense system that could potentially impede the efficiency of the therapeutic *** overcome these drawbacks,herein,a tumor microenvironment-responsive the ND-PAA-CD-Ce6@MnO_(2)(NPCC@M)delivery system was fabricated by disulfide bond coupling chlorin e6(Ce6)to nanodiamond(ND)and further wrapped by MnO_(2)nanosheets to facilitate *** use of disulfide bond not only stabilizes Ce6 in the blood circulation to prevent premature leakage,but also destroys the antioxidant barrier of overexpressed glutathione(GSH)in tumor ***,the outer MnO_(2)was rapidly degraded by the endogenous hydrogen peroxide(H_(2)O_(2))in the acidic pH and GSH within the tumor cells,which leads to an abundance of O_(2)and while increases the level of 1O_(2)under laser *** results eventually broke the redox homeostasis and attenuate hypoxia,thereby inducing apoptosis and necrosis of tumor *** in vitro and in vivo biological effect has revealed a good biosafety profile and a high tumor suppression *** a novel ND-based system with tumor microenvironment-modulating capability to elevate oxygen content and promote GSH consumption in tumor cells opens new opportunities for enhanced ROS treatment paradigms.

关键词： Nanodiamond Photodynamic Chlorin e6 MnO_(2) Tumor suppression

Construction of remote cyano-substituted quaternary carbon centers via nickel-catalyzed migratory hydrocyanation of unconjugated dienes

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Science China Chemistry 2024年第10期67卷 3397-3405页

作者： Yidan Xing Rongrong Yu Mingdong Jiao Ting Wang Xianjie Fang key laboratory of Organosilicon Chemistry and Material Technology of Ministry of Education Key Laboratory of Organosilicon Material Technology of Zhejiang ProvinceCollege of MaterialChemistry and Chemical EngineeringHangzhou Normal UniversityHangzhou 311121China Shanghai key laboratory for molecular engineering of Chiral Drugs School of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China

The transition-metal-catalyzed migratory functionalization has emerged as a robust protocol for the building of C–C bonds remote from the“initiation”***,a similar strategy for the construction of quaternary carbon centers is still underdeveloped and only a limited number of reports ***,we report a nickel-catalyzed migratory hydrocyanation of unconjugated dienes to construct remote cyano-substituted quaternary carbon *** transformation features exceptional regioselectivity,mild reaction conditions,broad substrate scope and high *** synthetic utility of this method has been highlighted by a series of product derivatizations,and the potential of this transformation has been extended to synthesize TRPV1 antagonist and the key intermediate in the total synthesis of *** functional theory(DFT)studies unveiled that the specific catalytic pocket assumed a significant role in the selective formation of cyano-substituted quaternary carbon centers.

关键词： chain-walking regioselectivity remote cyanation quaternary carbon centers unconjugated dienes

Recent progress on rapid diagnosis of COVID-19 by point-of-care testing platforms

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Chinese Chemical Letters 2024年第3期35卷 66-75页

作者： Ya-Nan Tang Dingding Jiang Xuejun Wang Yunqi Liu Dacheng Wei State key laboratory of molecular engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200433China Institute of molecular Materials and Devices Fudan UniversityShanghai 200433China

The outbreak of COVID-19 has drawn great attention around the ***-CoV-2 is a highly infectious virus with occult transmission by many mutations and a long incubation *** particular,the emergence of asymptomatic infections has made the epidemic even more ***,early diagnosis and timely management of suspected cases are essential measures to control the spread of the *** simple,portable,and accurate diagnostic techniques for SARS-CoV-2 is the key to epidemic *** advantages of point-of-care testing technology make it play an increasingly important role in viral detection and *** review summarizes the point-of-care testing platforms developed by nucleic acid detection,immunological detection,and nanomaterial-based biosensors ***,this paper provides a prospect for designing future highly accurate,cheap,and convenient SARS-CoV-2 diagnostic technology.

关键词： COVID-19 Point-of-care testing platforms Nucleic acid detection Asymptomatic infection Biosensors

Selective oxidation using in-situ generated hydrogen peroxide over titanosilicates

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Chinese Journal of Structural Chemistry 2024年第6期43卷 12-14页

作者： Zhipeng Wan Hao Xu Peng Wu State key laboratory of Petroleum molecular&Process engineering Shanghai Key Laboratory of Green Chemistry and Chemical ProcessesSchool of Chemistry and Molecular Engineering East China Normal UniversityShanghai200062China Institute of Eco-Chongming Shanghai202162China

Titanosilicates are a class of heteroatom-containing zeolitic materials with tetrahedrally coordinated Ti^(4+)ions incorporated into crystalline zeolite frameworks,with TS-1,Ti-MWW and Ti-MOR as representative and attractive selective oxidation *** liquid-phase oxidations of a variety of substrates such as olefins and ketones with the green oxidant of H_(2)O_(2)over titanosilicates under mild conditions have attracted considerable research interests in the clean production of fine and bulk chemicals,among which propylene epoxidation and cyclohexanone ammoximation have been industrialized[1].

关键词： silicate zeolite propylene

Evolution of hollow nanosphere to microtube in the self-assembly of chiral dansyl derivatives and inversed circularly polarized luminescence

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Chinese Chemical Letters 2024年第7期35卷 285-290页

作者： Sifan Du Yuan Wang Fulin Wang Tianyu Wang Li Zhang Minghua Liu Beijing key laboratory for Science and Application of Functional molecular and Crystalline Materials Department of Chemistry and Chemical EngineeringSchool of Chemistry and Biological EngineeringUniversity of Science and Technology BeijingBeijing 100083China National laboratory for molecular Science(BNLMS) CAS Key Laboratory of ColloidInterface and Chemical ThermodynamicsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China

Here,we designed asymmetric(m DS)and symmetrical(d DS)chiral V-shaped molecules by linking one or two dansyl groups to trans-1,2-cyclohexane diamine and investigated the solvent-regulated structural transformation and inversed circularly polarized luminescence(CPL)in the *** increasing water volume fraction(fw)in the mixed solvent of water/acetonitrile,asymmetric mDS selfassembled into hollow nanospheres and microtubes,while solid nanospheres and solid microplates were corresponding to symmetric d *** this transformation process,the emission of m DS and d DS was changed from yellow-green to blue and cyan color,which was ascribed to twisted intramolecular charge transfer(TICT)and locally excited(LE)fluorescence of V-shaped DS *** conformation of N,Ndimethyl groups with respect to naphthalene ring also led to the transformation of *** tubular and platelike structures had stronger and reversed CPL signals in comparison with spheroidal *** chiral information of DS assembly could be effective transferred to achiral Nile red via co-assembly strategy,which endowed Nile red exhibiting inversed induced CPL signal regulated by water *** work provides a method for achieving a variety of self-assembled structures with adjustable chiroptical properties.

关键词： CPL inversion Hollow structure Self-assembly Dansyl Chirality transfer