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High-Performance Recyclable Furan-based Epoxy Resin and Its Carbon Fiber Composites with Dense Hydrogen Bonding

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Chinese Journal of Polymer Science 2024年第1期42卷 73-86,I0008页

作者： Chang-Bo Zhao Lu-Kun Feng Hui Xie Ming-Liang Wang Bing Guo Zhi-Yong Xue Cai-Zhen Zhu Jian Xu Advanced Materials Research institute North China Electric Power UniversityBejing 102206China institute of Low-Dimensional Materials Genome Initiative College of Chemistry and Environmental EngineeringShenzhen UniversityShenzhen 518060China Chengdu institute of organic chemistry Chinese Academy of SciencesChengdu 610041China School of Science and Shenzhen Key Laboratory of Flexible Printed Electronics Technology and Shenzhen Key Laboratory of Advanced Functional Carbon Materials Research and Comprehensive ApplicationHarbin Institute of TechnologyShenzhen 518055China

The emerging biomass-based epoxy vitrimers hold great potential to fulfill the requirements for sustainable development of *** the existence of dynamic chemical bonds in vitrimers often reduces both the thermal and mechanical properties of epoxy resins, it is challenging to produce recyclable epoxy vitrimers with both excellent mechanical properties and good thermal stability. Herein, a monomer 4-(((5-(hydroxymethyl)furan-2-yl)methylene)amino)phenol(FCN) containing furan ring with potential to form high density of hydrogen bonding among repeating units is designed and copolymerized with glycerol triglycidyl ether to yield epoxy resin(FCN-GTE), which intrinsically has dual hydrogen bond networks, dynamic imine structure and resultant high performance. Importantly, as compared to the BPA-GTE, the FCN-GTE exhibits significantly improved mechanical properties owing to the increased density of hydrogen bond network and physical crosslinking interaction. Furthermore, density functional theory(DFT) calculation and in situ FTIR analysis is conducted to decipher the formation mechanism of hydrogen bond network. In addition, the FCN-GTE possesses superior UV shielding, chemical degradation, and recyclability because of the existence of abundant imine bonds. Notably, the FCN-GTE-based carbon fiber composites could be completely recycled in an amine *** study provides a facile strategy for synthesizing recyclable biomass-based high-performance epoxy vitrimers and carbon fiber composites.

关键词： Furan Hydrogen bond network Dynamic Schiff base Carbon fiber composites Recycling

A Dynamic Covalent Bonding-based Nanoplatform for Intracellular Co-Delivery of Protein Drugs and Chemotherapeutics with Enhanced Anti-Cancer Effect

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Chinese Journal of Polymer Science 2024年第5期42卷 559-569,I0005页

作者： Sai-Nan Liu Jia-Hui Meng Li-Yun Cui Hua Chen Lin-Qi Shi Ru-Jiang Ma Key Laboratory of Functional Polymer Materials of Ministry of Education Institute of Polymer ChemistryTianjin Key Laboratory of Functional Polymer MaterialsState Key Laboratory of Medicinal Chemical BiologyFrontiers Science Center for New Organic MatterCollege of ChemistryNankai UniversityTianjin300071China Haihe Laboratory of Sustainable Chemical Transformations Tianjin300192China

Efficient intracellular delivery of protein drugs is critical for protein *** combination of protein drugs with chemotherapeutics represents a promising strategy in enhancing anti-cancer ***,co-delivery systems for efficient delivery of these two kinds of drugs are still lacking because of their different ***,we show a well-designed delivery system based on dynamic covalent bond for efficient intracellular co-delivery of ribonuclease A(RNase A)and doxorubicin(DOX).Two polymers,PEG-b-P(Asp-co-AspDA)and PAE-b-P(Asp-co-AspPBA),and two 2-acetylphenylboronic acid(2-APBA)-functionalized drugs,2-APBA-RNase A and 2-APBA-DOX,self-assemble into mixed-shell nanoparticles(RNase A/DOX@MNPs)via dynamic phenylboronic acid(PBA)-catechol bond between PBA and dopamine(DA)*** PBA-catechol bond endows the nanoparticles with high stability and excellent stimulus-responsive drug release *** the slight acidic environment at tumor tissue,RNase A/DOX@MNPs are positively charged,promoting their *** cellular uptake into endosome,further protonation of PAE chains leads to the rupture of endosomes because of the proton sponge effect and the cleavage of PBA-catechol bond promotes the release of two *** cytoplasm,the high level of GSH removed the modification of 2-APBA on *** restored RNase A and DOX show a synergistic and enhanced antic-cancer *** system may be a promising platform for intracellular co-delivery of protein drugs and chemotherapeutics.

关键词： Drug co-delivery Combination therapy Dynamic covalent bond

Uncovering the dominant contribution of intermediate volatility compounds in secondary organic aerosol formation from biomass-burning emissions

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National Science Review 2024年第3期11卷 150-158页

作者： Kun Li Jun Zhang David M.Bell Tiantian Wang Houssni Lamkaddam Tianqu Cui Lu Qi Mihnea Surdu Dongyu Wang Lin Du Imad El Haddad Jay G.Slowik Andre S.H.Prevot Environment Research institute Shandong University Laboratory of Atmospheric chemistry Paul Scherrer Institute

organic vapors from biomass burning are a major source of secondary organic aerosols(SOAs). Previous smog chamber studies found that the SOA contributors in biomass-burning emissions are mainly volatile organic compounds(VOCs). While intermediate volatility organic compounds(IVOCs) are efficient SOA precursors and contribute a considerable fraction of biomass-burning emissions, their contribution to SOA formation has not been directly observed. Here, by deploying a newly-developed oxidation flow reactor to study SOA formation from wood burning, we find that IVOCs can contribute ～70% of the formed SOA, i.e.>2 times more than VOCs. This previously missing SOA fraction is interpreted to be due to the high wall losses of semi-volatile oxidation products of IVOCs in smog chambers. The finding in this study reveals that SOA production from biomass burning is much higher than previously thought, and highlights the urgent need for more research on the IVOCs from biomass burning and potentially other emission sources.

关键词： atmospheric chemistry biomass burning secondary organic aerosol intermediate volatility organic compounds

Identification and characterization of camptothecin tailoring enzymes in Nothapodytes tomentosa

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Journal of Integrative Plant Biology 2024年第6期66卷 1158-1169页

作者： Yin Chen Jian-Ping Huang Yong-Jiang Wang Meng-Ling Tu Junheng Li Bingyan Xu Guoqing Peng Jing Yang Sheng-Xiong Huang State Key Laboratory of phytochemistry and Plant Resources in West China and Yunnan Key Laboratory of Natural Medicinal chemistry Kunming Institute of BotanyChinese Academy of SciencesKunming 650201China University of Chinese Academy of Sciences Beijing 100049China Key Laboratory for Economic Plants and Biotechnology Kunming Institute of BotanyChinese Academy of SciencesKunming 650201China

Camptothecin is a complex monoterpenoid indole alkaloid with remarkable antitumor *** that two C-10 modified camptothecin derivatives,topotecan and irinotecan,have been approved as potent anticancer agents,there is a critical need for methods to access other aromatic ringfunctionalized congeners(e.g.,C-9,C-10,etc.).However,contemporary methods for chemical oxidation are generally harsh and low-yielding when applied to the camptothecin scaffold,thereby limiting the development of modified *** herein,we have identified four tailoring enzymes responsible for C-9 modifications of camptothecin from Nothapodytes tomentosa,via metabolomic and transcriptomic *** consist of a cytochrome P450(Nt CPT9H)which catalyzes the regioselective oxidation of camptothecin to 9-hydroxycamptothecin,as well as two methyltransferases(Nt OMT1/2,converting 9-hydroxycamptothecin to 9-methoxycamptothecin),and a uridine diphosphate-glycosyltransferase(Nt UGT5,decorating 9-hydroxycamptothecin to9-β-D-glucosyloxycamptothecin).Importantly,the critical residues that contribute to the specific catalytic activity of Nt CPT9H have been elucidated through molecular docking and mutagenesis *** work provides a genetic basis for producing camptothecin derivatives through metabolic *** will hasten the discovery of novel C-9 modified camptothecin derivatives,with profound implications for pharmaceutical manufacture.

关键词： camptothecin biosynthesis enzymatic assay Nothapodytes tomentosa tailoring enzyme transcriptomic analysis

Self-Assembled Protein Hybrid Nanofibrils for Photosynthetic Hydrogen Evolution

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CCS chemistry 2024年第3期6卷 812-823页

作者： Weijian Chen Xiantao Hu Andi Hu Luyang Ji Yiming Huang Hao Heng Fude Feng Shu Wang Department of Polymer Science and Engineering School of Chemistry and Chemical EngineeringNanjing UniversityJiangsuNanjing 210023 Beijing National Laboratory for Molecular Sciences Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190

In artificial photosynthesis systems,synthetic diiron complexes are popular[FeFe]-hydrogenase mimics,which are attractive for the fabrication of photocatalyst-protein hybrid structures to amplify hydrogen(H2)generation ***,constructing a highly bionic and efficient catalytic hybrid system is a major ***,we designed an ideal hybrid nanofibrils system that incorporates the crucial components:(1)a[FeFe]-H2ase mimic,which has a three-arm architecture(named triFeFe)for more interaction sites and higher catalytic activity and(2)uniform hybrid nanofibrils as the biological environment in which cysteine-catalyst coordination and the hydrogen-bonding network play a vital role in both catalyst binding and hydrogen evolution reaction *** assembled hybrid nanofibrils achieve efficient H2 generation with a turnover number of 2.3×103,outperforming previously reported diiron catalyst-protein hybrid ***,the hybrid nanofibrils work with photosynthetic thylakoids to produce H2,without extra photosensitizers or electron shuttle proteins,which advances the bioengineering of living systems for solar-driven biofuel production.

关键词： hybrid photocatalyst in situ assembly amyloid fibrils photosynthetic hydrogen evolution thylakoid

Recovery and in-situ reduction of precious metals by graphdiyne and graphdiyne oxide for antibacterial use

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Rare Metals 2024年第4期43卷 1747-1757页

作者： Ming-Ji Jiang Ya-Na Zhang Ling-Shen Meng Jing Kang Yong-Jun Li Alideertu Dong College of chemistry and Chemical Engineering Inner Mongolia UniversityHohhot010021China Engineering Research Center of Dairy Quality and Safety Control Technology Ministry of EducationInner Mongolia UniversityHohhot010021China Department of chemistry University of ZurichCH-8057ZurichSwitzerland Laboratory of organic Solids and Beijing National Laboratory for Molecular Sciences Institute of ChemistryChinese Academy of SciencesBeijing100190China

Based on the in-situ self-reduction and chemical stability,graphdiyne(GDY)and graphdiyne oxide(GDYO)are used as trapping agents to investigate the ability for recovering Au^(3+),Ag^+,and Pd^(2+)under different pH values and interfering *** strong acidity at pH=1,these two agents demonstrate high select recovery towards the three precious metal ions,which could be insitu reduced to nanoparticles(NPs).In addition,superparamagnetic Fe_(3)O_(4)NPs are deposited on the surfaces of GDY and *** magnetic responses enable GDYFe_(3)O_(4)to recover precious metals conveniently and efficiently by the aid of an external magnetic *** study also confirms the antibacterial activity of the as-recovered NPs deposited on GDY and GDYO against Escherichia coli and Staphylococcus aureus(1×10^(5)colony-forming unit(CFU)·mL^(-1)),and the antibacterial rates are 100%.This strategy of recovering precious metals and subsequently reusing to combat pathogens will be of great significance for environmental remediation and biomedical applications.

关键词： Graphdiyne In-situ reduction Recovery Precious metals Antibacterial

Large-area flexible organic photovoltaic modules

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Science China chemistry 2024年第10期67卷 3189-3190页

作者： Yongfang Li Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic SolidsInstitute of ChemistryChinese Academy of SciencesBeijing 100190China Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and DevicesCollege of ChemistryChemical Engineering and Materials ScienceSoochow UniversitySuzhou 215123China

organic solar cells(OSCs)have the advantages of light weight and excellent mechanical stability[1].The OSCs can be an ideal candidate as portable and wearable energy sources to power portable electronics,internet of things,***,power conversion efficiency(PCE)of the small-area OSCs have reached around 20%[2].This makes the community more confident about this technology moving into practical applications.

关键词： portable internet stability

Porous Indium Nanocrystals on Conductive Carbon Nanotube Networks for High-Performance CO2-to-Formate Electrocatalytic Conversion

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Energy & Environmental Materials 2024年第4期7卷 413-421页

作者： Liangping Xiao Rusen Zhou Tianqi Zhang Xiaoxiang Wang Renwu Zhou Patrick J.Cullen Kostya (Ken) Ostrikov Department of Physics Research Institute for Biomimetics and Soft Matter Fujian Provincial Key Laboratory for Soft Functional Materials Jiujiang Research Institute Xiamen University School of chemistry and Physics QUT Centre for Materials Science and QUT Centre for a Waste-Free World Queensland University of Technology(QUT) School of Chemical and Biomolecular Engineering University of Sydney

Ever-increasing emissions of anthropogenic carbon dioxide （CO2） cause global environmental and climate *** by biological photosynthesis,developing effective strategies NeuNlto up-cycle CO2into high-value organics is *** CO2reduction reaction （CO2RR） is highly promising to convert CO2into economically viable carbon-based chemicals or fuels under mild process conditions.

关键词： CO2RR conductive network electrocatalysts formate

Palladium-catalyzed multi components oxy-aminofluorination and aminofluorination of gem-difluoroalkenes

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Chinese Chemical Letters 2024年第2期35卷 420-425页

作者： Fen Wu Xin Li Junbiao Chang Dachang Bai State Key Laboratory of Antiviral Drugs NMPA Key Laboratory for Research and Evaluation of Innovative DrugKey Laboratory of Green Chemical Media and ReactionsMinistry of EducationSchool of Chemistry and Chemical EngineeringPingyuan LaboratoryHenan Normal UniversityXinxiang 453007China State Key Laboratory of Organometallic chemistry Shanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China

Organofluorine compounds are widely used in the realm of drug discovery and material ***,we developed palladium catalyzed intermolecular aminofluorination and oxy-aminofluorination of gem‑difluoroalkenes with N-fluorobenzenesulfonimide(NFSI),in which NFSI was used as the nitrogen source and *** reaction provides an efficient and straightforward synthesis route of a series ofα-trifluoromethyl benzylic ***,three/four components oxy-aminofluorination processes were realized to giveα-trifluoromethyl benzylic ether with a terminal amino group,which proceed through C(sp^(3))-O bond cleavage of easily available ether and simultaneous introduced a fluorine,an amino and an oxy substituent in one pot with excellent *** divergent reactivity not only included the incorporation of one ether molecular,but also much more challenged two ether insertion with excellent selectivity through succession C(sp^(3))-O bonds *** protocol allows for concise synthesis of high value amines with fluoroalkyl-substituents and selectively transformation of easily available ethers by high-valent palladium catalysis.

关键词： Palladium Multi components Aminofluorination Oxy-aminofluorination C(sp^(3))-O bond cleavage