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Synergistic asymmetric diarylation of tethered alkenes via C–H functionalization of simple(hetero)arenes

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Science China Chemistry 2024年第8期67卷 2710-2718页

作者： jian Yao Can zhao Lili Shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry and Shanghai Hongkong Joint Laboratory in Chemical Synthesis Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 200032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

By virtue of the atom-and step-economy, utilization of simple arenes as a supplant of pre-prepared aryl metal species or aryl halides for the synthesis of arylated chiral molecules has attracted great attention from the synthetic community. While transition-metal-catalyzed enantioselective diarylation of tethered alkenes has been employed to prepare important chiral cyclic compounds, the direct use of simple arenes as aryl precursors is still underdeveloped, probably due to the difficulties in the effective control of the reactivity, site-selectivity and/or enantioselectivity. Herein we report an asymmetric Pd/Ag dual metal catalytic system for the non-directed, site-and enantioselective domino Heck/intermolecular C–H functionalization of *** studies showed that Pd and Ag act in cooperation in the catalysis and the chiral bisphosphine ligand plays a bifunctional role, i.e., assisting the silver species in the cleavage of the aryl C–H bond, while inducing the enantioselectivity on direct complexation with palladium. This method provides an efficient approach to the corresponding chiral oxindoles with good enantiomeric excesses from a broad scope of arenes, including fluoroarenes, heteroarenes and several complex products derived from medicines or natural products.

关键词： asymmetric Pd/Ag dual metal catalytic system simple arenes C–H functionalization bifunctional role chiral oxindoles

In Situ Growth of 2D Metal–Organic Framework Ion Sieve Interphase for Reversible Zinc Anodes

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Energy & Environmental Materials 2024年第6期7卷 158-166页

作者： Jing Sun Qinping jian Bin Liu Pengzhu Lin Tianshou zhao Department of Mechanical and Aerospace Engineering The Hong Kong University of Science and TechnologyClear Water BayKowloonHong Kong SARChina Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055China

Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high ***,the service life of zinc metal anodes is severely constrained by critical challenges,including dendrites,water-induced hydrogen evolution,and *** this study,a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition *** ultrathin interphase layer(~1μm)is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1Å,which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions,contributing to a uniform and highly reversible zinc *** the shielding of the interphase layer,an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and~700 h at 1 mA cm^(−2),far exceeding that of the bare zinc anodes(250 and 70 h).Furthermore,as a proof-of-concept demonstration,the full cell paired with MnO_(2) cathode demonstrates improved rate performances and stable cycling(1200 cycles at 1 A g−1).This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.

关键词： 2D MOF desolvation interphase ion sieve zinc anode

Leader-follower Optimal Selection Method for Distributed Control System in Active Distribution Networks

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CSEE Journal of Power and Energy Systems 2024年第1期10卷 314-323页

作者： jian Le Liangang zhao Cao Wang Qian Zhou Yang Wang School of Electrical Engineering and Automation Wuhan UniversityWuhan 430072China

Aiming at the shortcomings of a traditional centralized control in an active distribution network(AND),this paper proposes a leader-follower distributed group cooperative control strategy to realize multiple operation and control tasks for an *** distributed information exchange protocols of the distributed generation(DG)group devoted to node voltage regulation or exchange power control are developed using a DG power utilization ratio as the consensus *** these bases,this study further investigates the leader optimal selection method for a DG group to improve the response speed of the distributed control ***,a single or multiple leader selection model is established to minimize the constraints of the one-step convergence factor and the number of leaders to improve the response speed of the distributed control *** simulation results of the IEEE 33 bus standard test system show the effectiveness of the proposed distributed control *** addition,the response speed of a DG control group can be improved effectively when the single or multiple leaders are selected optimally.

关键词： Active distribution1network consensus algorithm leader-follower system mixed-integer semidefinite programming optimal distributed control

An aptamer-driven DNA nanodevice for improved delivery of synthetic immunostimulants

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Nano Research 2024年第10期17卷 9078-9083页

作者： Dejie Lu Zhenghan Di Lele Li jian zhao Li Zheng Guangxi Engineering Center in Biomedical Materials for Tissue and Organ Regeneration Collaborative Innovation Centre of Regenerative Medicine and Medical BioResource Development and ApplicationGuangxi Key Laboratory of Regenerative MedicineThe First Affiliated Hospital of Guangxi Medical UniversityGuangxi Medical UniversityNanning 530021China CAS Key Laboratory for Biomedical Effects of Nanomaterials and Nanosafety National Center for Nanoscience and TechnologyBeijing 100190China

Efficient delivery of therapeutics to immune cells remains a formidable challenge for cancer *** this work,we demonstrate that an aptamer-driven DNA nanodevice,constructed through linkage of a synthetic immunostimulant(Toll-like receptor 9 agonist:CpG motif)to an aptamer,could significantly enhance the immunostimulatory activity by facilitating the uptake and retention of therapeutics in *** administration of the DNA nanodevice results in efficient tumor growth inhibition in both breast cancer and melanoma mouse *** studies suggest that the DNA nanodevice leads to reeducation of tumor-associated macrophages and ultimately to reversing the tumor immune *** strategy for aptamer-mediated and vehicle-free delivery of immunostimulatory oligonucleotides provides a potential platform for cancer immunotherapy.

关键词： aptamer immunostimulatory oligonucleotides DNA nanodevice tumor-associated macrophages cancer therapy

Isotopic characteristics and source analysis of atmospheric ammonia during agricultural periods in the Xichuan area of the Danjiangkou Reservoir

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Journal of Environmental Sciences 2024年第2期136卷 460-469页

作者： Xiaoshu Chen Tongqian zhao Chunyan Xiao Xiaoming guo Feihong Chen Institute of Resources and Environment Henan Polytechnic UniversityJiaozuo 454000China

Nitrogen deposition is an important means of exogenous nitrogen input in reservoir *** activities around the reservoir lead to a sharp increase in the concentration of ammonia in the atmosphere,which poses a threat to the reservoir water *** the contribution of agricultural ammonia release to atmospheric NH_(x)(gaseous NH_(3)and particulate NH_(4)^(+)),in the reservoir area can provide a theoretical foundation for local reactive nitrogen *** collected atmospheric NH_(3)and NH_(4)^(+)samples during the agricultural periods and analyzed the isotopic characteristics of atmospheric NH_(x)and the contribution rates of different ammonia sources in the Xichuan area of the Danjiangkou *** results showed that the initialδ~(15)N values of NH_(3)(-30.0‰to–7.2‰)and particulate NH_(4)^(+)(–33‰to+4.9‰for finer and coarser particles,respectively)are different,and their contribution ratios from dissimilar ammonia sources are also different,among which NH_(4)^(+)is more susceptible to meteorological ***,since the atmospheric NH_(x)in the Xichuan area is mainly gaseous NH_(3),the final sources of atmospheric ammonia nitrogen source depend on gaseous NH_(3).Agricultural sources(59%-74%)were the main NH_(3)sources in this *** them,the fertilizer use emission was dominant;it had the highest contribution rate in summer during the agricultural period and a more prominent impact in areas with less human *** regulation of the application of high-ammonia releasing fertilizer,especially during the agricultural period in summer,is an effective way to reduce the threat of atmospheric ammonia to water health.

关键词： Danjiangkou reservoir Atmospheric ammonia nitrogen Isotope Ammonia source analysis Agricultural sources

Heat transfer and temperature evolution in underground mininginduced overburden fracture and ground fissures: Optimal time window of UAV infrared monitoring

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International Journal of Mining Science and Technology 2024年第1期34卷 31-50页

作者： Yixin zhao Kangning Zhang Bo Sun Chunwei Ling Jihong guo Beijing Key Laboratory for Precise Mining of Intergrown Energy and Resources China University of Mining and Technology-BeijingBeijing 100083China School of Energy&Mining Engineering China University of Mining and Technology-BeijingBeijing 100083China State Key Laboratory of Coal Resources and Safe Mining China University of Mining and Technology-BeijingBeijing 100083China

Heat transfer and temperature evolution in overburden fracture and ground fissures are one of the essential topics for the identification of ground fissures via unmanned aerial vehicle(UAV) infrared imager. In this study, discrete element software UDEC was employed to investigate the overburden fracture field under different mining conditions. Multiphysics software COMSOL were employed to investigate heat transfer and temperature evolution of overburden fracture and ground fissures under the influence of mining condition, fissure depth, fissure width, and month alternation. The UAV infrared field measurements also provided a calibration for numerical simulation. The results showed that for ground fissures connected to underground goaf(Fissure Ⅰ), the temperature difference increased with larger mining height and shallow buried depth. In addition, Fissure Ⅰ located in the boundary of the goaf have a greater temperature difference and is easier to be identified than fissures located above the mining goaf. For ground fissures having no connection to underground goaf(Fissure Ⅱ), the heat transfer is affected by the internal resistance of the overlying strata fracture when the depth of Fissure Ⅱ is greater than10 m, the temperature of Fissure Ⅱ gradually equals to the ground temperature as the fissures’ depth increases, and the fissures are difficult to be identified. The identification effect is most obvious for fissures larger than 16 cm under the same depth. In spring and summer, UAV infrared identification of mining fissures should be carried out during nighttime. This study provides the basis for the optimal time and season for the UAV infrared identification of different types of mining ground fissures.

关键词： Heat transfer Overburden fracture Ground fissures Infrared thermal imaging Unmanned aerial vehicle(UAV) COMSOL simulation

Highly crystallization-induced emissive luminophores with mechanoluminescent features for two-photon harvesting fluorescence imaging and latent fingerprint identification

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Nano Research 2024年第7期17卷 6475-6482页

作者： jian Lu Juan Gao Rui-Xuan Qian Shuai-Hua Wang Fa-Kun Zheng guo-Cong guo Fujian Science and Technology Innovation Laboratory for Optoelectronic Information of China Fuzhou 350108China State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of MatterChinese Academy of SciencesFuzhou 350002China

Fluorescence imaging can be employed in fields of medical treatment,astronomical exploration,and national defense *** fluorescence imaging often takes the single-photon techniques,which is vulnerable to background interference and ***,two-photon fluorescence imaging can achieve much higher-resolution fluorescence imaging for reducing scattering and deeper ***,by assembling the tetraphenylethylene backbones with nontoxic and non-noble K^(+)ions,compound 1([(Hdma)K(H_(2)ettc)]_(n),H_(4)ettc=4',4''',4''''',4'''''''-(ethene-1,1,2,2-tetrayl)tetrakis(([1,1'-biphenyl]-4-carboxylic acid)))with the crystallization-induced emissions exhibited charming fluorescence imaging under two-photon excitation microscopy(TPEM).Besides,luminescent powders based on compound 1 can achieve high-resolution fingerprint recognition,providing secure access control and identification for a novel authentication *** with the commercial fluorescent dyes coumarin-6,the as-synthesized compound 1 showed great solvent stability,indicating its durability against harsh ***,compound 1 shows mechanoluminescent properties for the perturbation of weak supramolecular interactions within ordered arrangements of the H_(2)ettc^(2−)*** novel compound has provided an important insight to the development of twophoton fluorescence imaging and advanced external-stimuli responsive materials.

关键词： crystallization-induced emission fluorescence imaging two-photon absorption fingerprint recognition mechanoluminescence

Analysis on the turning point of dynamic in-plane compressive strength for a plain weave composite

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Defence Technology（防务技术） 2024年第2期32卷 485-495页

作者： Xiaoyu Wang Zhixing Li Licheng guo Zhenxin Wang Jiuzhou zhao Department of Astronautic Science and Mechanics Harbin Institute of TechnologyHarbin150001China AECC Commercial Aircraft Engine Co LTDShanghai201108China

Experimental investigations on dynamic in-plane compressive behavior of a plain weave composite were performed using the split Hopkinson pressure bar. A quantitative criterion for calculating the constant strain rate of composites was established. Then the upper limit of strain rate, restricted by stress equilibrium and constant loading rate, was rationally estimated and confirmed by tests. Within the achievable range of 0.001/s-895/s, it was found that the strength increased first and subsequently decreased as the strain rate increased. This feature was also reflected by the turning point(579/s) of the bilinear model for strength prediction. The transition in failure mechanism, from local opening damage to completely splitting destruction, was mainly responsible for such strain rate effects. And three major failure modes were summarized under microscopic observations: fiber fracture, inter-fiber fracture, and interface delamination. Finally, by introducing a nonlinear damage variable, a simplified ZWT model was developed to characterize the dynamic mechanical response. Excellent agreement was shown between the experimental and simulated results.

关键词： Plain weave composite Dynamic strength Quantitative criterion Turning point Failure mechanism

Development of a novel Eu^(3+)-doped tantalate red-emitting phosphor for w-LEDs application

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Journal of Rare Earths 2024年第8期42卷 1479-1488,I0003页

作者： Fan Zeng Jingjing Ru Bing zhao Feiyun guo jianzhong Chen College of Chemistry and Materials Fujian Province University Key Laboratory of Green Energy and Environment CatalysisNingde Normal University.Ningde352100China School of Environment and Resources School of Carbon Neutral and Modern IndustryFujian Normal UniversityFuzhou350007China College of Information and Mechanical&Electrical Engineering Ningde Normal UniversityNingde352100China College of Chemistry Fuzhou UniversityFuzhou350108China

Two novel phosphors LiBa_(4(1-x))Eu_(4x)Ta_(3)O_(12)(H-LBTO:xEu^(3+)) and Li_(0.25)Ba_(1-x)Eu_(x)Ta_(0.75)O_(3)(C-LBTO:xEu^(3+))were prepared successfully by a molten salt *** transformation between these two structures was realized by changing the sintering temperature or changing the Eu^(3+) ions concentration,which was also demonstrated by the X-ray diffraction(XRD),scanning electron microscopy(SEM),diffuse reflectance spectra(DRS),and photoluminescence excitation(PLE) analyses,Both the sintering temperature and the Eu^(3+)ions doping concentration have significant impact on the formation of the crystal *** these phosphors sintered at 1023 K exhibit two major luminescence lines at 594 and 614 nm under nearUV light of 395 nm excitation,corresponding to Eu^(3+)ions typical transitions of ^(5)D_(0)→^(7)F_(1) and ^(5)D_(0)→^(7)F_(2).The optimum concentration of Eu^(3+) ions is 9 mol% for C-LBTO:xEu^(3+) samples and the quenching interaction type is the nearest-neighbor ion *** thermal stability of the C-LBTO:0.09Eu^(3+)sample was investigated in detail and the device application further suggests that C-LBTO:0.09Eu^(3+) can be used as a red phosphor for near-UV excited w-LEDs in lighting.

关键词： Phosphor Tantalate LED device Rare earths