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Photoredox-catalyzed C-glycosylation of peptides with glycosyl bromides

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Chinese Chemical Letters 2024年第6期35卷 263-267页

作者： Chen Li Ziyuan Zhao Shouyun Yu State key laboratory of Analytical chemistry for Life Science Jiangsu Key Laboratory of Advanced Organic MaterialsChemistry and Biomedicine Innovation Center(ChemBIC)School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Glycosyl radicals,produced under mild photoredox conditions,show unique utility in the preparation of C-linked *** herein report the construction of C-glycosidic bonds on α,β-dehydroalanine(DHA)of peptides with easily available glycosyl bromides as glycosyl radical precursors under highly anomeric control,leading to C-glycosylation modifications of *** method not only has outstanding functional group compatibility,but also is feasible in near-physiological conditions(pH~7 and temperature T≤37℃ in aqueous media).

关键词： Glycosylation C-Glycosides Glycopeptides Dehydroalanine Photoredox catalysis

Tunable artificial plasmonic nanolaser with wide spectrum emission operating at room temperature

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Chinese Physics B 2024年第5期33卷 466-471页

作者：周鹏郭佳琦梁琨金磊梁熊玉李俊强邓绪彦秦建宇张家森于丽 State key laboratory of Information Photonics and Optical Communications School of ScienceBeijing University of Posts and TelecommunicationsBeijing 100876China State key laboratory for Artificial Microstructures and mesoscopic Physics School of PhysicsPeking UniversityBeijing 100876China Peking University Yangtze Delta Institute of Optoelectronics Peking UniversityNantong 226010China

With the rapid development of information and communication technology,a key objective in the field of optoelectronic integrated devices is to reduce the nano-laser size and energy *** nanolasers are unable to exceed the diffraction limit and typically exhibit low modulation rates of several *** contrast,plasmonic nanolaser utilizes highly confined surface plasmon polariton(SPP)mode that can exceed diffraction limit and their strong Purcell effect can accelerate the modulation rates to several ***,we propose a parametrically tunable artificial plasmonic nanolasers based on metal–insulator–semiconductor–insulator–metal(MISIM)structure,which demonstrates its ability to compress the mode field volume toλ/*** the pump power increases,the proposed artificial plasmonic nanolaser exhibits 20-nm-wide output ***,we investigate the effects of various cavity parameters on the nanolaser’s output threshold,offering potentials for realizing low-threshold artificial plasmonic ***,we observe a blue shift in the center wavelength of the nanolaser output with thinner gain layer thickness,predominantly attributed to the increased exciton–photon coupling *** work brings inspiration to several areas,including spaser-based interconnects,nano-LEDs,spontaneous emission control,miniaturization of photon condensates,eigenmode engineering of plasmonic nanolasers,and optimal design driven by artificial intelligence(AI).

关键词： surface plasmon polaritons nanolaser ultrafast MISIM

Molecule aging induced by electron attacking

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Journal of Energy chemistry 2024年第6期93卷 519-525,I0013页

作者： Ping Song Yining Dong Xue Gong Mingbo Ruan Baoxin Ni Xuanhao Mei Kun Jiang Weilin Xu State key laboratory of Electroanalytical chemistry and Jilin Province key laboratory of Low Carbon Chemical Power Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of Chin1Hefei 230026AnhuiChina Shanghai key laboratory of Molecular Catalysis and Innovative Materials Collaborative Innovation Center of Chemistry for Energy MaterialsDepartment of ChemistryFudan UniversityShanghai 200438China

Here we propose a new concept of"molecule aging":with some special treatment,a molecule could be"aged"by losing some unknown tiny particles or pieces from atoms in the molecule,Such"aging"or loss of unknown tiny particles does not change apparently its molecular structure or chemical composition,but some physicochemical properties could be changed *** further confirm such"molecule aging"via a long-term electron attacking to age water(H_(2)O)*** IR spectra show no structural difference between the fresh water and the aged one,while the NMR spectra show that the electron attacking can decrease the size of water *** facts indicate that the electron attacking indeed can"affect"the structure of water molecule slightly but without damaging to its basic molecule *** exploration reveals that the hydrogen evolution reaction(HER)activity of the aged water molecule is lower than the fresh water on the same Pt/C *** density functional theory calculations indicate that the shortened O-H bond in H_(2)O indeed can present lower HER activity,so the observed size decrease of water clusters from NMR probably could be attributed to the shortening of O-H bond in water *** results indicate significantly that the molecule aging can produce materials with new functions for new possible applications.

关键词： Aging of molecules Electron attacking Full width at half maxima Hydrogen evolution reaction

Chiral thermally activated delayed fluorescence materials for circularly polarized organic light-emitting diodes

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Science China chemistry 2024年第4期67卷 1097-1116页

作者： Li Yuan Yi-Pin Zhang You-Xuan Zheng State key laboratory of Coordination chemistry Collaborative Innovation Center of Advanced MicrostructuresJiangsu Key Laboratory of Advanced Organic MaterialsSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Chirality is an important natural characteristic of organic molecules,and chiral organic molecules have shown extensive application in areas such as pharmaceutical development and material *** from the ability to achieve circularly polarized luminescence(CPL),chiral luminescent materials have shown potential applications in anti-glare display,optical communication and,3D display,*** to the ability to harvest both singlet and triplet excitons by a fast reverse intersystem crossing process without involving noble metals,chiral thermally activated delayed fluorescence(TADF)materials with point chirality,axial chirality,planar chirality and helical chirality are regarded as the state-of-the-art materials for circularly polarized organic light-emitting diodes(CP-OLEDs).In recent years,the chiral TADF materials and CP-OLEDs have rapidly developed,but unfortunately,the dissymmetry factors(g)are far from the requirement of practical *** ideal emitters and devices should have both high efficiency and a g factor,or at least a balance between these two *** review gives an overview of recent progress in chiral TADF materials,with a particular focus on the chiral skeleton,CPL property and device ***,the molecular design concept,device structure and methods to improve the g factors of chiral materials and CP-OLEDs are also discussed.

关键词： chiral thermally activated delayed fluorescence material chiral skeleton circularly polarized luminescence circularly polarized organic light-emitting diodes dissymmetry factor

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Design and construction of size-controlled CoO/CS catalysts for Fischer–Tropsch synthesis

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Nano Research 2024年第4期17卷 2520-2527页

作者： Wei Sun Ting Kuang Guiyou Wei Yue Li Yaqin Liu Shuai Lyu Yuhua Zhang Jinlin Li Li Wang key laboratory of Catalysis and Energy Materials chemistry of Ministry of Education&Hubei key laboratory of Catalysis and Materials Science South-Central Minzu UniversityWuhan 430074China Hubei key laboratory of Biomass Fibers and Eco-dyeing&Finishing College of Chemistry and Chemical EngineeringWuhan Textile UniversityWuhan 430200China

The use of supported Co-based catalysts is widespread in various catalytic reactions due to their unique *** structural sensitivity of these catalysts is closely linked to their particle size and crystal ***,comprehending the structure–activity relationship requires the development of well-defined Co-based ***,we employed a colloidal wet chemical process and a heterogeneous nucleation method to prepare well-defined Co-based catalysts supported by inert carbon *** nanospheres’surface possesses abundant functional groups that efficiently capture metal complexes and facilitate the nucleation and growth of CoO *** adjusting the Co source concentration,solvent molar ratio,and nucleation growth kinetics,we successfully prepared CoO/carbon sphere(CS)catalysts with different particle sizes and crystal *** influence of metallic face-centered cubic(fcc)-Co^(0) particle size in the range of 6.6–17.6 nm on the performance of Fischer–Tropsch synthesis(FTS)using well-defined CoO/CS catalysts has been *** result demonstrated that the turnover frequency(TOF)remained constant for CoO/CS catalysts with metallic fcc-Co^(0) particle size larger than 7.7 ***,both the selectivity and the activity changed for CoO/CS catalysts with smaller particles(<7.7 nm).Significantly,when metallic fcc-Co^(0) particle size was reduced from 17.6 to 7.7 nm,the cobalt time yield increased to 6.7μmolCO·gCo^(-1)·s^(-1),indicating improved catalytic *** the same time,the CH_(4) selectivity decreased to 4.9%,suggesting a higher preference for hydrocarbon *** findings demonstrate the importance of particle size in Co catalyzed Fischer–Tropsch *** use of well-defined CoO/CS catalysts offers valuable insights into the structure–activity relationship,leading to a better understanding of Co catalyzed Fischer–Tropsch synthesis.

关键词： Fischer–Tropsch synthesis(FTS) cobalt size effects phase effects carbon nanospheres

Nature-inspired design of droplet-synthesized polymeric nanoelectrode for photoelectrochemical microRNA sensing within single cells

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Science Bulletin 2024年第2期69卷 159-162页

作者： Si-Yuan Yu Yi-Li Liu Zheng Li Dechen Jiang Jing-Juan Xu Hong-Yuan Chen Wei-Wei Zhao State key laboratory of Analytical chemistry for Life Science School of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210023China

Nanoelectrodes have been shown to be powerful tools for nanoscopic research on single entities,deepening the understanding of heterogeneity and stochastics for single molecules,nanoparticles and cells[1–3].However,despite their importance,current nanoelectrode preparations are highly restrained to flame/electrochemical etching,metal sputtering,electrochemical deposition,etc.[3],resulting in a limited range of materials(mainly gold,platinum and carbon)for potential-resolved detection of redox-active species(Table S1 online).The enrichment of preparation methods to introduce novel materials and mechanisms should prove significant for the development of nanoelectrodes.

关键词： electrode deepening restrained

Synergism of solar-driven interfacial evaporation and photo-Fenton Cr(Ⅵ) reduction by sustainable Bi-MOF-based evaporator from waste polyester

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Journal of Energy chemistry 2024年第7期94卷 527-540页

作者： Zifen Fan Jie Liu Huajian Liu Lijie Liu Yan She Xueying Wen Huiyue Wang Guixin Hu Ran Niu Jiang Gong key laboratory of Material chemistry for Energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureHubei Engineering Research Center for Biomaterials and Medical Protective MaterialsSemiconductor Chemistry CenterSchool of Chemistry and Chemical EngineeringHuazhong University of Science andTechnologyWuhan430074HubeiChina

The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade ***,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is ***,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater ***,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic *** to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of *** integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced *** the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.

关键词： Interfacial solar steam generation Cr(VI)reduction Photo-Fenton reaction Metal-organic framework Waste plastic upcycling

Rational design of ZnCdS/TpPa-1-COF heterostructure photocatalyst by strengthening the interface connection in solar hydrogen production reactions

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Nano Research 2024年第3期17卷 1027-1034页

作者： Di Yang Zhi-Gang Li Xinghao Zhang Zenghuan Ren Weihan Lu Haining Liu Xiaomeng Guo Jijie Zhang Xian-He Bu Tianjin key laboratory of Metal and Molecule-Based Material chemistry School of Materials Science and EngineeringNankai UniversityTianjin 300350China College of chemistry and Pharmaceutical Engineering Hebei University of Science and TechnologyShijiazhuang 050018China State key laboratory of Elemento-Organic chemistry College of ChemistryNankai UniversityTianjin 300071China

ZnCdS quantum dots(QDs)are highly coveted in photocatalysis research for their exceptional visible-light responses and high light-absorption ***,their practical application is hindered by their tendency to aggregate,due to having high surface *** address this issue,herein,a heterostructure is synthesized by growing ZnCdS QDs with a size of approximately 5 nm onto the surface of a two-dimensional(2D)covalent organic framework(COF),*** approach suppresses the aggregation of the QDs and improves their *** ZnCdS/TpPa-1-COF composite exhibited a peak hydrogen evolution rate of 6244.16μmol·g^(-1)·h^(-1),which was 2.89 and 4.18 times greater than that of ZnCdS and TpPa-1-COF,*** zero-dimensional/two-dimensional(0D/2D)heterojunction formed by ZnCdS and TpPa-1-COF generates a strong interfacial force,which is attributed to the intimate contact between the *** connections accelerate charge separation,improve the utilisation of reduced electrons,and reduce the extent of agglomeration of the ZnCdS QDs,thereby resulting in high hydrogen production activity of the ***,the photocatalytic mechanism is studied using Kelvin probe force microscopy and theoretical *** study offers a novel approach for creating sulfide photocatalysts and is crucial for investigating the potential practical applications of the related photocatalysts.

关键词： covalent organic frameworks quantum dots photocatalysis hydrogen generation heterojunction

Genome mining of sulfonated lanthipeptides reveals unique cyclic peptide sulfotransferases

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Acta Pharmaceutica Sinica B 2024年第6期14卷 2773-2785页

作者： Meng Wang Wen-Wei Li Zhe Cao Jianong Sun Jiang Xiong Si-Qin Tao Tinghong Lv Kun Gao Shangwen Luo Shi-Hui Dong State key laboratory of Applied Organic chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou 730000China

Although sulfonation plays crucial roles in various biological processes and is frequently utilized in medicinal chemistry to improve water solubility and chemical diversity of drug leads,it is rare and underexplored in ribosomally synthesized and post-translationally modified peptides(RiPPs).Biosynthesis of RiPPs typically entails modification of hydrophilic residues,which substantially increases their chemical stability and bioactivity,albeit at the expense of reducing water *** explore sulfonated RiPPs that may have improved solubility,we conducted co-occurrence analysis of RiPP class-defining enzymes and sulfotransferase(ST),and discovered two distinctive biosynthetic gene clusters(BGCs)encoding both lanthipeptide synthetase(LanM)and *** expressing these BGCs,we characterized the structures of novel sulfonated lanthipeptides and determined the catalytic details of LanM and *** demonstrate that SslST-catalyzed sulfonation is leader-independent but relies on the presence of A ring formed by *** LanM and ST are promiscuous towards residues in the A ring,but ST displays strict regioselectivity toward *** recognition of cyclic peptide by ST was further *** evaluation underscores the significance of the ST-catalyzed *** study sets up the starting point to engineering the novel lanthipeptide STs as biocatalysts for hydrophobic lanthipeptides improvement.

关键词： Lanthipeptides Sulfotransferases Sulfonation Biosynthesis Genome mining