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Asymmetric reversible structural switching of a diene coordination polymer promoted by UV-visible light

Science China chemistry 2024年第2期67卷 536-541页

作者： Yong Wang Qiaoqiao Zhang Yong-Yong Cao Qi Liu Brendan F.Abrahams Jian-Ping Lang College of chemistry Chemical Engineering and MaterialsSoochow UniversitySuzhou215123China state Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai200032China College of biological Chemical Science and EngineeringJiaxing UniversityJiaxing314001China School of chemistry University of MelbourneVictoria3010Australia

In natural and artificial systems,reversible reactions are commonly asymmetric with respect to the time scale and nature of the stimuli which drive the forward and backward *** applications for which switching behavior is required,it is desirable that the reversible reaction goes as close to symmetric as possible;however,such systems are ***,we report an example of ultraviolet(UV)-visible light-regulated asymmetric reversible structural switching involving a diene-based coordination polymer,CP1 and its monocyclobutane product,*** is possible to cycle at least ten times through a forward [2+2] photocycloaddition reaction and the reverse,photocleavage reaction.A single cycle can be completed within a few *** transformation is accompanied by fast and distinct fluorescence changes,arising from optimisation of the reaction *** functional theory calculations allow rationalisation of the asymmetric reversible transformation between CP1 and CP1a rather than between CP1 and its dicyclobutane product *** work provides a clear illustration of reversible structural switching which approaches symmetric behaviour with respect to reaction rate and *** insights gained from this work also assist in the design of fast,reversible switching materials.

关键词： asymmetrical reversible structural switching coordination polymer photocycloaddition UV-visible light-controlled fluorescence switching

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Manipulating Film Formation Kinetics Enables Organic Photovoltaic Cells with 19.5%Efficiency

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CCS chemistry 2024年第1期6卷 218-229页

作者： Jianqiu Wang Pengqing Bi Yafei Wang Zhong Zheng Zhihao Chen Jiawei Qiao Wenxuan Wang Jiayao Li Cunbin An Shaoqing Zhang Xiaotao Hao Jianhui Hou state Key Laboratory of Polymer Physics and chemistry Beijing National Laboratory for Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190 university of Chinese Academy of sciences Beijing 100049 School of chemistry and biological Engineering University of Science and Technology BeijingBeijing 100083 School of Physics State Key Laboratory of Crystal MaterialsShandong UniversityJinan 250100

Organic photovoltaic(OPV)cells have demonstrated remarkable performance in small,spin-coated *** significant challenges persist in the form of large efficiency losses due to the fact that the ideal morphology cannot be preserved in the transition of small-area cells to large-scale ***,the ternary strategy of incorporating the third component FTCC-Br into the active layer of PB2:BTP-eC9 is employed to improve absorption response,optimize morphology,and reduce charge recombination,leading to a power conversion efficiency(PCE)of 19.5%(certified as 19.1%by the National Institute of Metrology,China).Moreover,the addition of FTCC-Br can control the aggregation kinetics of the active layer during the film formation process,transferring the optimal morphology to the blade-coated large-area *** on the highly efficient ternary bulk heterojunction,the 50 cm^(2) OPVmodules exhibited a PCE of 15.2%with respect to the active ***,the ternary OPV cells retain 80%of its initial PCE after 4000 h under continuous *** work demonstrates that the addition of a third component has the potential to improve the efficiency and stability of large-area organic solar cells.

关键词： organic photovoltaic cells morphology control large area cells ternary strategy power conventional efficiency

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Synergistically enhanced dielectric, insulating and thermally conductive performances of sandwich PMMA based dielectric films

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Progress in Natural Science:Materials International 2024年第3期34卷 591-597页

作者： Dongmei Zhang Yufan Li Yuchao Li Zhonggui Sun Hanxue Zhu Lujia Yang Yanhu Zhan Yankai Li Shi Wang Jun-Wei Zha School of Mathematical sciences Liaocheng University School of Materials Science and Engineering Liaocheng University state Key Laboratory of Organic Electronics and Information Displays & Institute of Advanced Materials (IAM) Nanjing University of Posts & Telecommunications School of chemistry and biological Engineering University of Science and Technology Beijing

A tri-layered(B-G-B) dielectric films were simply prepared by alternatively spin-coating boron nitride/polymethylmethacrylate(BN/PMMA, B) and graphene nanosheets(GNS/PMMA, G) compound solutions. The structure, morphology, thermal conductivity, and particularly the dielectric and relaxation behaviors were systematically studied. Results showed that a good exfoliation and dispersion of BN and GNS can be simply achieved through intensive mechanical compounding with PMMA in the internal mixer. The dielectric constant and breakdown strength of the obtained 1-3-1(B-G-B) sandwich composite film reached 4.3(@1 kHz) and 458.6kV/mm, being 119 % and 113 % higher than that of pure PMMA, respectively. Furthermore, the overall thermal conductivity of sandwich 1-3-1 composite increased by 112 % due to the addition of thermally conductive BN and GNS. The sandwich design strategy provided an effective way of achieving good permittivity, high insulation, and improved thermal conductivity simultaneously, showing potential applications in the miniaturization and integration of electronic devices.

关键词： Sandwich structure Breakdown strength Thermal conductivity Dielectric constant Composites

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Higher levels of the lipophilic antioxidants coenzyme Q_(10) and vitamin E in long-lived termite queens than in short-lived workers

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Insect Science 2024年第1期31卷 201-210页

作者： Eisuke Tasaki Yorihiro Yamamoto Yoshihito Iuchi Department of biological chemistry Graduate School of Sciences and Technology for InnovationYamaguchi UniversityYamaguchiJapan School of Bioscience and Biotechnology Tokyo University of TechnologyHachiojiTokyoJapan

Termite queens and kings live longer than nonreproductive *** molecular mechanisms contributing to their long lifespan have been investigated;however,the underlying biochemical explanation remains *** Q(CoQ),a component of the mitochondrial electron transport chain,plays an essential role in the lipophilic antioxidant defense *** beneficial effects on health and longevity have been well studied in several ***,we demonstrated that long-lived termite queens have significantly higher levels of the lipophilic antioxidant CoQ_(10) than *** chromatography analysis revealed that the levels of the reduced form of CoQ_(10) were 4 fold higher in the queen's body than in the worker's *** addition,queens showed 7 fold higher levels of vitamin E,which plays a role in antilipid peroxidation along with CoQ,than ***,the oral administration of CoQ_(10) to termites increased the CoQ_(10) redox state in the body and their survival rate under oxidative *** findings suggest that CoQ_(10) acts as an efficient lipophilic antioxidant along with vitamin E in long-lived termite *** study provides essential biochemical and evolutionary insights into the relationship between CoQ_(10) concentrations and termite lifespan extension.

关键词： antioxidant defense system coenzyme Q termite queens vitamin E

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Macrophage modulation with dipeptidyl peptidase-4 inhibitors:A new frontier for treating diabetic cardiomyopathy?

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World Journal of Diabetes 2024年第9期15卷 1847-1852页

作者： Saeed Mohammadi Ahmed Al-Harrasi Natural and Medical sciences Research Center University of NizwaNizwa 616Oman Department of biological sciences and chemistry University of NizwaNizwa 616Oman

This editorial introduces the potential of targeting macrophage function for diabetic cardiomyopathy(DCM)treatment by dipeptidyl peptidase-4(DPP-4)*** et al studied teneligliptin,a DPP-4 inhibitor used for diabetes management,and its potential cardioprotective effects in a diabetic mouse *** suggested teneligliptin administration may reverse established markers of DCM,including cardiac hypertrophy and compromised *** also inhibited the NLRP3 inflammasome and reduced inflammatory cytokine production in diabetic *** play crucial roles in DCM *** hyperglycemia disturbs the balance between pro-inflammatory(M1)and antiinflammatory(M2)macrophages,favoring a pro-inflammatory state contributing to heart ***,we highlight the potential of DPP-4 inhibitors to modulate macrophage function and promote an anti-inflammatory *** compounds may achieve this by elevating glucagon-like peptide-1 levels and potentially inhibiting the NLRP3 *** studies on teneligliptin in combination with other therapies targeting different aspects of DCM could be suggested for developing more effective treatment strategies to improve cardiovascular health in diabetic patients.

关键词： Diabetic cardiomyopathy Macrophage Dipeptidyl peptidase-4 inhibitor Teneligliptin NLRP3 inflammasome Glucagon-like peptide-1

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Stable hydrogen-bonded organic frameworks and their photo-and electro-responses

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Nano Research 2024年第8期17卷 7675-7699页

作者： Ying Hou Xin-Song Huang Sheng-Hao Gong Chen Liu Yangyang Liu Tian-Fu Liu state Key Laboratory of Structural chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China university of Chinese Academy of sciences Beijing 100049China Department of chemistry and Biochemistry California State UniversityLos AngelesCalifornia 90032USA College of chemistry and Materials Science Fujian Normal UniversityFuzhou 350007China

Hydrogen-bonded organic frameworks(HOFs)are a recent class of porous materials that have garnered considerable research interest owing to their distinctive *** can be constructed through judicious selection of H-bonding motifs,which are further enforced by other weak intermolecular interactions such asπ–πstacking,van der Waals forces,and framework *** advantage of these interactions,we can expand the functional field of HOFs by introducing active ***,researchers have made substantial advancements in using HOFs for chemical sensing,catalysis,proton conduction,biological applications,and *** low bonding energy of H-bonds allows for precise control over the concentration of ligands in solvents,forming diverse HOF *** varied structures offer significant advantages for producing HOFs with photo-responsive and electro-responsive ***,the presence of H-bonds in HOFs results in their inherent lower stability compared to metal-organic frameworks(MOFs)and covalent-organic frameworks(COFs)formed via coordination and covalent bonds,*** a result,the pursuit of stable and innovative HOF materials with novel functional sites remains an ongoing *** review provides an overview of recent research progress in the development of new strategies for stable HOF synthesis and applications of HOFs with stimuli-responsive *** first classified all synthetic methods reported to date and discussed the stable HOFs synthesized,as well as their unique properties and *** addition,we summarized the applications of HOFs utilizing their synergistic responses to external stimuli,including photo,electrical,pressure,and chemical *** systematically reviewed stable HOF synthesis and applications,which may lead to a deeper understanding of the structure–activity relationship for these materials and guide future HOF design.

关键词： stable hydrogen-bonded organic frameworks(HOFs) photo-response electro-response photoelectric synergistic response

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Copper-catalyzed enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides via α-imino copper carbenes

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Science China chemistry 2024年第9期67卷 2982-2988页

作者： En-He Huang Li-Gao Liu You-Wei Yin Hao-Xuan Dong Ji-Jia Zhou Xin Lu Bo Zhou Long-Wu Ye Key Laboratory for Chemical Biology of Fujian Province and state Key Laboratory of Physical chemistry of Solid Surfaces College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005China state Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

α-Imino metal carbenes are versatile intermediates in organic synthesis,and have broad applications in the assembly of divergent ***,the catalytic enantioselective desymmetrization based onα-imino metal carbenes has not been developed to ***,we disclose an enantioselective desymmetrizing C(sp^(2))-H functionalization of azide-ynamides viaα-imino copper carbenes,leading to the efficient assembly of divergent chiral indoloazepines in generally moderate to excellent yields with high ***,this reaction represents the first enantioselective desymmetrization based onα-imino metal *** synthetic transformations and biological tests show the potential utility of this ***,computational studies are employed to elucidate the reaction mechanism and the origin of enantioselectivity.

关键词： enantioselective desymmetrization metal carbenes copper catalysis nitrene transfer alkynes

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An octopamine-specific GRAB sensor reveals a monoamine relay circuitry that boosts aversive learning

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National Science Review 2024年第5期11卷 186-201页

作者： Mingyue Lv Ruyi Cai Renzimo Zhang Xiju Xia Xuelin Li Yipan Wang Huan Wang Jianzhi Zeng Yifei Xue Lanqun Mao Yulong Li state Key Laboratory of Membrane Biology School of Life SciencesPeking University state Key Laboratory of Brain and Cognitive Science Institute of Biophysics Chinese Academy of Sciences PKU-IDG/Mc Govern Institute for Brain Research Yuanpei College Peking University Peking-Tsinghua Center for Life sciences Academy for Advanced Interdisciplinary Studies Peking University Peking university–Tsinghua university–National Institute of biological sciences Joint Graduate Program Academy for Advanced Interdisciplinary Studies Peking University Institute of Molecular Physiology Shenzhen Bay Laboratory College of chemistry Beijing Normal University Chinese Institute for Brain Research

Octopamine（OA）,analogous to norepinephrine in vertebrates,is an essential monoamine neurotransmitter in invertebrates that plays a significant role in various biological functions,including olfactory associative ***,the spatial and temporal dynamics of OA in vivo remain poorly understood due to limitations associated with the currently available methods used to detect *** overcome these limitations,we developed a genetically encoded GPCR activation-based（GRAB） OA sensor called *** sensor is highly selective for OA and exhibits a robust and rapid increase in fluorescence in response to extracellular *** GRABOA1.0,we monitored OA release in the Drosophila mushroom body（MB）,the fly's learning center,and found that OA is released in response to both odor and shock stimuli in an aversive learning *** OA release requires acetylcholine（ACh） released from Kenyon cells,signaling via nicotinic ACh ***,we discovered that OA amplifies aversive learning behavior by augmenting dopamine-mediated punishment signals via Octβ1R in dopaminergic neurons,leading to alterations in synaptic plasticity within the ***,our new GRABOA1.0sensor can be used to monitor OA release in real time under physiological conditions,providing valuable insights into the cellular and circuit mechanisms that underlie OA signaling.

关键词： octopamine dopamine GRAB sensor learning and memory

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Living Chinese Herbal Scaffolds from Microfluidic Bioprinting for Wound Healing

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Research 2024年第1期2023卷 107-118页

作者： Xiaocheng Wang Jinxuan Jia Mengying Niu Wenzhao Li Yuanjin Zhao Department of Rheumatology and Immunology Nanjing Drum Tower HospitalSchool of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China Oujiang Laboratory(Zhejiang Lab for Regenerative Medicine Vision and Brain Health)Wenzhou InstituteUniversity of Chinese Academy of SciencesWenzhouZhejiang 325001China state Key Laboratory of Bioelectronics School of Biological Science and Medical EngineeringSoutheast UniversityNanjing 210096China chemistry and Biomedicine Innovation Center Nanjing UniversityNanjing 210023China

biological scaffolds have been widely employed in wound healing applications,while their practical efficiency is compromised by insufficient oxygen delivery to the 3-dimensional constructs and inadequate nutrient supply for the long-term healing ***,we present an innovative living Chinese herbal scaffold to provide a sustainable oxygen and nutrient supply for promoting wound *** a facile microfluidic bioprinting strategy,a traditional Chinese herbal medicine(Panax notoginseng saponins[PNS])and a living autotrophic microorganism(microalgae Chlorella pyrenoidosa[MA])were successfully encapsulated into the *** encapsulated PNS could be gradually released from the scaffolds,which promoted cell adhesion,proliferation,migration,and tube formation in *** addition,benefiting from the photosynthetic oxygenation of the alive MA,the obtained scaffolds would produce sustainable oxygen under light illumination,exerting a protective effect against hypoxia-induced cell *** on these features,we have demonstrated through in vivo experiments that these living Chinese herbal scaffolds could efficiently alleviate local hypoxia,enhance angiogenesis,and thereby accelerate wound closure in diabetic mice,indicating their great potential in wound healing and other tissue repair applications.

关键词： healing wound protective

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Electronic engineering of Co-Ru diatomic sites and Ru nanoparticles for synergistic promotion of hydrogen evolution

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Nano Research 2024年第5期17卷 3714-3723页

作者： Wei Zhang Cong Li Yongyong Cao Jun-Yang Ji Zhao-Chen Li Zheng Niu Hongwei Gu Pierre Braunstein Jian-Ping Lang College of chemistry Chemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China state Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China College of biological Chemical Science and EngineeringJiaxing UniversityJiaxing 314001China Universitéde Strasbourg-CNRS Institut de Chimie(UMR 7177 CNRS)4 rue Blaise Pascal-CS 9003267081 StrasbourgFrance

The coexistence of multi-component active sites like single-atom sites,diatomic sites(DAS)and nanoclusters is shown to result in superior performances in the hydrogen evolution reaction(HER).Metal diatomic sites are more complex than single-atom sites but their unique electronic structures can lead to significant enhancement of the HER *** the synthesis and identification of DAS is usually challenging,we report a simple access to a diatomic catalyst by anchoring Co-Ru DAS on nitrogen-doped carbon supports along with Ru nanoparticles(NPs).Experimental and theoretical results revealed the atomic-level characteristics of Co-Ru sites,their strong electronic coupling and their synergy with Ru NPs within the *** unique electronic structure of the catalyst resulted in an excellent HER activity and stability in alkaline *** work provides a valuable insight into a widely applicable design of diatomic catalysts with multi-component active sites for highly efficient HER electrocatalysis.

关键词： Co-Ru diatomic sites Ru nanoparticles multiple active sites synergistic effect hydrogen evolution reaction

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