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Enhancing the deep-red/near-infrared fluorescence of higher rylene diimides via the chalcogen-annulation strategy

Science China Chemistry 2024年第4期67卷 1324-1333页

作者： Kai Chen Xiao Chen Ke Hu Yilun Zhao Yujian Liu Guogang Liu Jinquan Chen Wei Jiang Zhigang Shuai da-Hui Qu Zhaohui Wang Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research CenterFrontiers Science Center for Materiobiology and Dynamic ChemistryInstitute of Fine ChemicalsSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China Key Laboratory of Organic Optoelectronics and Molecular Engineering Department of ChemistryTsinghua UniversityBeijing 100084China State Key Laboratory of Precision Spectroscopy East China Normal University500 Dongchuan RoadShanghai 200241China

Deep-red/near-infrared fluorescence is highly suitable for bioimaging owing to its ability to deeply penetrate tissues,organs,and live ***,developing organic fluorophores with high deep-red/near-infrared fluorescence quantum yield(Φ_(FL))and fluorescent brightness remain a significant challenge owing to the energy gap ***,we developed a straightforward and effective chalcogen-annulation strategy by introducing O,S and Se into the bay region of TDI and QDI fluorophores,realizing the increase ofΦFLand fluorescent brightness up to 10 *** our best knowledge,this study potentially stands as the pioneering instance showcasing the anti-heavy-atom effect of chalcogens,and the absoluteΦFL(93%)and fluorescent brightness(128,200 cm^(-1)mol^(-1)L)of Se-TDI is among top deep-red/near-infrared organic fluorophores currently *** femtosecond transient absorption(fs-TA)measurements show the absence of obvious changes of the excited state lifetime after the introduction of chalcogens in TDI and QDI fluorophores,indicating that intersystem crossing(ISC)can be neglected in TDI and QDI *** calculations further reveal the chalcogen-annulation strategy increase the radiative rates and reduce the reorganization energy of several accepting modes at the ground state in TDI fluorophores,leading to the suppression of internal conversion(IC)*** chalcogen-annulation strategy,which effectively increases the Φ_(FL)and restricts the IC processes,while remaining unaffected by the heavy-atom effect,offers novel insights and theoretical support for the design and synthesis of deep-red/near-infrared organic fluorophores with high Φ_(FL)and fluorescent brightness.

关键词： π-extended rylene diimides chalcogen-annulation strategy deep-red/near-infrared fluorescence

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Spontaneous anchoring Cl intoα-Co(OH)_(2) as efficient and stable oxygen reduction electrocatalysts for seawater battery

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Rare Metals 2024年第7期43卷 3074-3083页

作者： Wang Zheng Xue-Rong Zheng Qi Lu Yan-Hui Cao Yang Wang Hai-Peng Fu Jin-Feng Zhang Yi-da Deng Wen-Bin Hu School of Materials Science and Engineering Key Laboratory of Advanced Ceramics and Machining Technology of Ministry of EducationTianjin UniversityTianjin 300072China State Key Laboratory of Marine Resource Utilization in South China Sea School of Materials Science and EngineeringHainan UniversityHaikou 570228China Key Laboratory of Electromagnetic Processing of Materials Ministry of EducationNortheastern UniversityShenyang 110819China

Seawater battery is an advanced energy storage system that enables conversion of chemical energy to electricity by consuming metals,dissolved oxygen and seawater in anode,cathode and electrolyte,***,the oxygen reduction reaction(ORR)activity and stability of electrocatalysts can be easily deactivated due to the severe Cl~-permeation and corrosion in seawater ***,we developed a structural buffer engineering strategy by spontaneously anchoring Cl~-intoα-Co(OH)_(2) as efficient and stable ORR electrocatalysts,in which the ultrathinα-Co(OH)_(2) nanosheets were synthesized using an ultrafast solution high-temperature shock(SHTS)*** large lattice space(~0.8 nm)of layeredα-Co(OH)_(2) ensured the spontaneously penetration of Cl~-into the lattice structure and replaced part of OH~-to formα-Co(OH)_(2-x)Cl_*** continuous leaching and compensating of saturated Cl inα-Co(OH)_(2-x)Cl_x could enhance the Cl~-corrosion resistance and modulate electronic structure of Co metallic sites,thus improving the ORR electrocatalytic activity and stability in seawater ***α-Co(OH)_(2-x)Cl_x seawater batteries display superior onset and half-wave potentials of 0.71 and 0.66 V,respectively,which are much better than the counterparts ofα-Co(OH)_(2) and ofβ-Co(OH)_(2) with no Cl~-penetrating and no buffer ***α-Co(OH)_(2-x)Cl_x-based seawater batteries display stable open-circuit potential of 1.69 V and outstanding specific capacity of 1345 mAh·g^(-1).

关键词： Seawater battery Oxygen reduction electrocatalyst Solution high-temperature shock Structural buffer engineering

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Visible-light photoredox-catalyzed carboxylation of aryl epoxides with CO_(2)

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Chinese Chemical Letters 2024年第7期35卷 281-284页

作者： Tian-Yu Gao Xiao-Yan Mo Shu-Rong Zhang Yuan-Xu Jiang Shu-Ping Luo Jian-Heng Ye da-Gang Yu Key Laboratory of Green Chemistry&Technology of Ministry of Education College of ChemistrySichuan UniversityChengdu 610064China State Key Laboratory Breeding Base of Green Chemistry-Synthesis Technology Zhejiang University of TechnologyHangzhou 310014China State Key Laboratory of Elemento-Organic Chemistry Nankai UniversityTianjin 300071China

Herein, we report the first visible-light photoredox-catalyzed carboxylation of aryl epoxides with CO_(2)to synthesize hydroxy acid derivatives. A variety of valuable β-, γ-, δ-, ε–hydroxy acid derivatives are obtained in moderate to high yields under mild conditions. This protocol shows noteworthy functionalgroup compatibility, high chemo-and regioselectivities under transition-metal-free conditions with an inexpensive organo-dye as photosensitizer. Mechanistic studies indicate that the benzylic carbanion is generated as an intermediate via the sequential single electron transfer(SSET) process.

关键词： Carbon dioxide Epoxides Visible-light photoredox catalysis Hydroxy acid Sequential single electron transfer

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Surface diffraction beamline at the SSRF

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Nuclear Science and Techniques 2024年第7期35卷 47-57页

作者： Yue-Liang Gu Xu Zheng Xing-Min Zhang Bin Zhao Guang-Zhi Yin da-Ming Zhu Yuan-He Sun Xing-Yu Gao Xiao-Long Li Shanghai Advanced Research Institute Chinese Academy of Sciences239 Zhangheng RoadPudong DistrictShanghai201204China

BL02U2 of the Shanghai Synchrotron Radiation Facility is a surface diffraction beamline with a photon flux of 5.5×10^(12) photons/s at 10 keV and a beam size of 160µm×80µm at the sample *** is dedicated to studying surfaces(solid-vacuum,solid-gas)and interfaces(solid-solid,solid-liquid,and liquid-liquid)in nanoscience,condensed matter,and soft matter systems using various surface scattering techniques over an energy range of 4.8-28 keV with transmission and reflection ***,BL02U2 has a high energy resolution,high angular resolution,and low beam divergence,which can provide excellent properties for X-ray diffraction experiments,such as grazing incident X-ray diffraction,X-ray reflectivity,crystal truncation rods,and liquid X-ray *** of in situ environments can also be provided for the samples *** paper describes the setup of the new beamline and its applications in various fields.

关键词： Surface and interface Beamline Surface diffraction Microstructure

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ZnGa_(2)S_(4):an infrared nonlinear optical material with large second-harmonic generation response and wide band gap

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Rare Metals 2024年第1期43卷 395-401页

作者： Chen-Yang Zhang Xiao-Nan Niu Yan-Feng Wei Shu-Xing Zhou da-Qing Yang Ying Wang Jian Wang Bing-Bing Zhang College of Chemistry and Materials Science Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of EducationState Key Laboratory of New Pharmaceutical Preparations and ExcipientsHebei UniversityBaoding 071002China Hubei Key Laboratory of Low Dimensional Optoelectronic Materials and Devices Hubei University of Arts and ScienceXiangyang 441053China Hubei Longzhong Laboratory Xiangyang 441000China Department of Chemistry and Biochemistry Wichita State UniversityKansas 67260USA

High-performance nonlinear optical(NLO)crystals are crucial devices to convert wavelength of solid-state *** play an indispensable role in the research of infrared NLO *** this work,ternary chalcogenide ZnGa_(2)S_(4) ... 详细信息

关键词： optical nonlinear harmonic

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Leaf habit differentiation explains trait tradeoffs across savanna woody plants

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Forest Ecosystems 2024年第3期11卷 287-295页

作者： Yangsiding Wang da Yang German Vargas G. Guangyou Hao Jennifer S.Powers Yan Ke Qin Wang Yunbing Zhang Jiaolin Zhang CAS Key Laboratory of Tropical Forest Ecology Xishuangbanna Tropical Botanical GardenChinese Academy of SciencesMenglaYunnan 666303China University of Chinese Academy of Sciences Beijing 100049China School of Biological Sciences University of UtahSalt Lake CityUT 84112USA CAS Key Laboratory of Forest Ecology and Management Institute of Applied EcologyChinese Academy of SciencesShenyang 110016China Department of Ecology Evolution and BehaviorUniversity of MinnesotaSt PaulMN 55108USA

Identifying how leaf habit subdivisions link to the fast–slow and avoidance–tolerance trait tradeoffs can provide new insight into divergence in ecophysiological strategies among plant functional groups. Here, we tested a hypothesis that the differentiation across deciduous, semi-deciduous and evergreen woody species contributes to physiological trait tradeoffs in a dry-hot valley savanna. We investigated 11 photosynthetic, morphological and hydraulic traits of 24 species including 8 deciduous, 10 semi-deciduous and 6 evergreen species. Deciduous species were grouped in the fast and avoidance side associated with high values of maximum photosynthetic rates,stomatal conductance and leaf size, while evergreen species were grouped in the slow and tolerance side associated with high photosynthetic water use efficiency, leaf mass per area, sapwood density, Huber value, leaf water potential at turgor loss point and water potential causing 50% loss of stem hydraulic conductance. Semideciduous species generally had intermediate trait values and represented different physiological characteristics when compared to deciduous and evergreen species. The physiological trait tradeoffs showed a close linkage to the differentiation of these three leaf habits. Our findings clearly reveal trait tradeoffs related to fast–slow and avoidance–tolerance strategies among diverse savanna plants, suggesting a syndrome in multiple ecophysiology strategies across different leaf habits.

关键词： Dry-hot habitat Gas exchange Hydraulics Phenology Tolerance Valley savanna

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Construction of metal-organic frameworks with unsaturated Cu sites for efficient and fast reduction of nitroaromatics:A combined experimental and theoretical study

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Chinese Chemical Letters 2024年第8期35卷 514-519页

作者： Longlong Geng Huiling Liu Wenfeng Zhou Yong-Zheng Zhang Hongliang Huang da-Shuai Zhang Hui Hu Chao Lv Xiuling Zhang Suijun Liu Shandong Provincial Key Laboratory of Monocrystalline Silicon Semiconductor Materials and Technology College of Chemistry and Chemical EngineeringDezhou UniversityDezhou 253023China School of Chemistry and Chemical Engineering Shandong University of TechnologyZibo 255000China State Key Laboratory of Separation Membranes and Membrane Processes School of Chemical Engineering and TechnologyTiangong UniversityTianjin 300387China School of Chemistry and Chemical Engineering Jiangxi Provincial Key Laboratory of Functional Molecular Materials ChemistryJiangxi University of Science and TechnologyGanzhou 341000China

Metal-organic frameworks(MOFs)functionalized with open metal sites(OMSs)have received widespread attention in various applications due to their fascinating electronic properties and unique interactions with guest ***,rational tailoring of the coordination environment of metal nodes dur-ing the synthesis of MOFs remains a great challenge due to their tendency of saturated coordination with ***,we reported the construction of three new MOFs featuring unsaturated Cu(Ⅱ)sites,namely[Cu(HCOO)(pzta)]_(n)(HL-1),{[Cu(PTA)0.5(pzta)(H_(2)O)]·2H_(2)O}_(n)(HL-2)and[Cu(NA)0.5(pzta)]_(n)(HL-3)(Hpzta=3-pyrazinyl-1,2,4-triazole;PTA=terephthalic acid;NA=1,4-naphthalene dicarboxylic acid),based on the mixed-linker strategy via specific selection of versatile Hpzta ligand and carboxylate ***-markably,the obtained MOFs exhibited excellent activity and good recyclability for the catalytic reduction of nitroaromatics under mild conditions(25℃and 1 atm).In particular,the complete conversion of 4-nitrophenol(4-NP)took only 30 s on HL-2,reaching a record-high TOF value compared with previously reported metal *** combined experimental and theoretical studies on HL-2 revealed that the open Cu site with positive-charged nature could improve the adsorption and subsequent electron trans-port between the substrates,and was responsible for the outstanding *** work shined lights on the further enhancement of performance for MOFs through rational OMSs construction.

关键词： Metal-organic frameworks Open metal sites Catalysis Copper node 4-Nitrophenol

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Determinant variables on the isotopic values of particulate organic matter in a neotropical floodplain

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Journal of Oceanology and Limnology 2024年第4期42卷 1173-1185页

作者： Vinícius de ANDRADE URBANO Matheus MAXIMILIAN RATZ SCOARIZE Gustavo HENRIQUE ZAIA ALVES Driele DELANIRA-SANTOS Marcela da SILVA CAETANO Evanilde BENEDITO Departamento de Biologia(DBI) Laboratório de Ecologia EnergéticaUniversidade Estadual de Maringá(UEM)Maringá87020-900Brasil Programa de Pós-graduação em Ecologia de Ambientes Aquáticos Continentais(PEA) Universidade Estadual de Maringá(UEM)Maringá87020-900Brasil Departamento de Biologia Geral Universidade Estadual de Ponta Grossa(UEPG)Campus UvaranasPonta Grossa 84030-900Brasil Australian Rivers Institute(ARI) Griffith UniversityNathan QLD 4111Australia

Particulate organic matter(POM)is an important energy source for aquatic consumers,understanding its origin and composition is essential for understanding the energetic dynamics of aquatic *** aim of this study was to analyze the relationship between POM and phytoplankton(isotopic values and chlorophyll concentration)and abiotic variables during dry and rainy *** was conducted in rivers and lagoons in the floodplain of the Upper Paraná*** found a greater difference in ^(δ13)C values of POM between sampling points than between seasons,indicating that the composition of regional sources influences the composition of POM more than dry and rainy *** addition,the concentration of chlorophyll during the dry season was positively correlated with ^(δ13)C values during that rainy ***,we found a relationship between factors limiting the growth of phytoplankton and ^(δ13)C values of POM,such as phosphate ions,indicating that variables that regulate phytoplankton growth tend to influence the composition of POM in river ***,maintaining the variables that regulate the phytoplankton community is of fundamental importance for the composition of POM,an important energy source in aquatic environments.

关键词： freshwater wetland stable isotopes food web subtropical environment

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Causal relationship between circulating vitamin C and 25-hydroxyvitamin D concentrations and common mental disorders-a Mendelian randomization study

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Food Science and Human Wellness 2024年第4期13卷 1877-1885页

作者： Yuanyuan Wang Lirong Dong Meng Zhao Shiyu Yin Pan da Dengfeng Xu Yifei Lu Jiayue Xia Niannian Wang Shaokang Wang Guiju Sun Key Laboratory of Environmental Medicine and Engineering of Ministry of Education and Department of Nutrition and Food HygieneSchool of Public HealthSoutheast UniversityNanjing 210009China Department of Integrated Service and Management Jiangsu Provincial Center for Disease Control and PreventionNanjing 210009China

Mental disorders seriously affect people’s health and social *** Mendelian randomization(MR)study was designed to investigate the causal relationship between circulating vitamin C(VC)or 25-hydroxyvitamin D(25(OH)D)levels and mental *** data used for the MR analysis were derived from the summary genome-wide association studies(GWAS)database for VC and 25(OH)D and from the Finn Gen consortium for fourteen mental *** on the inverse variance weighted(IVW)method,we found a potential causal association between circulating VC and anxiety disorders(IVW:OR=1.139,95%CI:1.023-1.269,P=0.018).However,no causal association was found between VC or 25(OH)D and other mental disorders(P>0.05).In the reverse MR analysis,individuals with Alzheimer’s disease was causally associated with higher concentrations of circulating VC(P=0.012),while individuals with anxiety disorders had a negative association between the concentrations of 25(OH)D(P=0.012).However,the current evidence does not support a causal relationship between VC or 25(OH)D and other mental *** addition,there was no causal association between circulating VC and 25(OH)D(P>0.05).Future studies are needed to confirm these findings and to elucidate the mechanisms of potential causality.

关键词： Circulating vitamin C 25-Hydroxyvitamin D Mental disorder Mendelian randomization

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Machine Learning-Based Intelligent Auscultation Techniques in Congenital Heart Disease:Application and Development

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Congenital Heart Disease 2024年第2期19卷 219-231页

作者： Yang Wang Xun Yang Mingtang Ye Yuhang Zhao Runsen Chen Min da Zhiqi Wang Xuming Mo Jirong Qi Department of Cardiothoracic Surgery Children’s Hospital of Nanjing Medical UniversityNanjingChina

Congenital heart disease(CHD),the most prevalent congenital ailment,has seen advancements in the“dual indi-cator”screening *** facilitates the early-stage diagnosis and treatment of children with CHD,subse-quently enhancing their survival *** cardiac auscultation offers an objective reflection of cardiac abnormalities and function,its evaluation is significantly influenced by personal experience and external factors,rendering it susceptible to misdiagnosis and *** recent years,continuous progress in artificial intelli-gence(AI)has enabled the digital acquisition,storage,and analysis of heart sound signals,paving the way for intelligent CHD auscultation-assisted diagnostic *** there has been a surge in studies based on machine learning(ML)within CHD auscultation and diagnostic technology,most remain in the algorithmic research phase,relying on the implementation of specific datasets that still await verification in the clinical *** paper provides an overview of the current stage of AI-assisted cardiac sounds(CS)auscultation technology,outlining the applications and limitations of AI auscultation technology in the CHD *** aim is to foster further development and refinement of AI auscultation technology for enhanced applications in CHD.

关键词： Congenital heart disease heart sound auscultation artificial intelligence machine learning

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