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An unprecedented synthesis of axially chiral biaryls by rearrangement and aromatization of carbocations with central-to-axial conversion of chirality

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Science China Chemistry 2024年第9期67卷 2998-3003页

作者： qi Liu xue-Dong Li Liang Cheng Li Liu Beijing National Laboratory for Molecular Sciences(BNLMS) CAS Key Laboratory of Molecular Recognition and FunctionCAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The central-to-axial chirality conversion represents a fascinating class of chemical processes consisting of the destruction of stereogenic centers and the simultaneous installation of axial chiral elements,which provides efficient methods for the preparation of axially chiral ***,developing catalytic asymmetric approaches for constructing these central chirality precursors and the efficient central-to-axial chirality conversion remains a challenge due to the requirement of aromatization or elimination *** this work,we have developed an unprecedented enantioselective intramolecular FriedelCrafts alkylation with unactivated-ketone carbonyls from which a chiral tertiary alcohol was generated with high efficiency and excellent *** addition,the central-to-axial chirality conversion strategy has been successfully applied to the synthesis of enantioenriched biaryls via a less-explored carbocation-initiated rearrangement and aromatization under the promotion of Lewis *** methodology provided a straightforward and sustainable access to a broad range of biaryl-2-carboxylic acid and in excellent yields(up to 92%)and excellent central-to-axial chirality conversion(up to 99%conversion percentage).This work could be a great model for developing new methods for synthesizing axially chiral biaryls and a general protocol for the rearrangement and aromatization of carbocations for further functionalization.

关键词： br?nsted acid catalysis desymmetrization phosphoric acid axially chiral biaryls central-to-axial conversion

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L-Type Calcium Channel Modulates Low-Intensity Pulsed Ultrasound-Induced Excitation in Cultured Hippocampal Neurons

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Neuroscience Bulletin 2024年第7期40卷 921-936页

作者： Wen-Yong Fan Yi-Ming Chen Yi-Fan Wang Yu-qi Wang Jia-qi Hu Wen-Xu Tang Yi feng qian Cheng Lei xue State Key Laboratory of Medical Neurobiology and MOE Frontiers Center for Brain Science Fudan UniversityShanghai 200433China Department of Physiology and Neurobiology School of Life SciencesFudan UniversityShanghai 200438China Institute of Acoustics School of Physics Science and EngineeringTongji UniversityShanghai 200092China Key Laboratory of Spine and Spinal Cord Injury Repair and Regeneration of Ministry of Education Tongji UniversityShanghai 200070China Center for Rehabilitation Medicine Department of Pain ManagementZhejiang Provincial People's HospitalAffliated People's HospitalHangzhou Medical CollegeHangzhou 310014China Department of Critical Care Medicine Shanghai General HospitalShanghai Jiaotong University School of MedicineShanghai 200080China Shanghai Research Institute for Intelligent Autonomous Systems Tongji UniversityShanghai 201210China Research Institute of Intelligent Complex Systems Fudan UniversityShanghai 200433China

As a noninvasive technique,ultrasound stimulation is known to modulate neuronal activity both in vitro and in *** latest explanation of this phenomenon is that the acoustic wave can activate the ion channels and further impact the electrophysiological properties of targeted ***,the underlying mechanism of low-intensity pulsed ultrasound(LIPUS)-induced neuro-modulation effects is still ***,we characterize the excitatory effects of LIPUS on spontaneous activity and the intracellular Ca^(2+)homeostasis in cultured hippocampal *** whole-cell patch clamp recording,we found that 15 min of 1-MHz LIPUS boosts the frequency of both spontaneous action potentials and spontaneous excitatory synaptic currents(sEPSCs)and also increases the amplitude of sEPSCs in hippocampal *** phenomenon lasts for>10 min after LIPUS *** with Ca^(2+)imaging,we clarified that LIPUS increases the[Ca^(2+)]cyto level by facilitating L-type Ca^(2+)channels(LTCCs).In addition,due to the[Ca^(2+)]cyto elevation by LIPUS exposure,the Ca^(2+)-dependent CaMKII-CREB pathway can be activated within 30 min to further regulate the gene transcription and protein *** work suggests that LIPUS regulates neuronal activity in a Ca^(2+)-dependent manner via *** may also explain the multi-activation effects of LIPUS beyond *** stimulation potentiates spontaneous neuronal activity by increasing Ca^(2+)influx.

关键词： Low-intensity pulsed ultrasound Neuromodulation L-type calcium channel Hippocampal neuron

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Tendencies of alloyed engineering in BiOX-based photocatalysts:a state-of-the-art review

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Rare Metals 2024年第4期43卷 1488-1512页

作者： Yan-Dong Sun Chao Zeng xue Zhang Zi-qi Zhang Bo Yang Sheng-qi Guo Tianjin Key Laboratory of Clean Energy and Pollutant Control School of Energy and Environmental EngineeringHebei University of TechnologyTianjin300401China State-Province Joint Engineering Laboratory of Zeolite Membrane Materials Institute of Advanced MaterialsCollege of Chemistry and Chemical EngineeringJiangxi Normal UniversityNanchang330022China Anhui Province Key Laboratory of Pollutant Sensitive Materials and Environmental Remediation School of Physics and Electronic InformationAnhui Province Industrial Generic Technology Research Center for Alumics MaterialsHuaibei Normal UniversityHuaibei235000China

Energy-saving and environmentally friendly photocatalysis has emerged as a popular research area in response to issues with energy scarcity and environmental *** to the unique layer-like structure,BiOX(Cl,Br,I)is frequently used in ***,inherent flaws in BiOX,such as an inappropriate band gap and low carrier separation efficiency,restrict its capacity for *** to the tunable grouping layer,alloying engineering is employed to optimize the intrinsic properties of BiOX and alloyed BiOX becomes a promising photocatalytic *** review describes the structure of BiOX,where tunable halogen layers provide favorable conditions for the implementation of alloying engineering to improve intrinsic *** article compares the effects and mechanisms of alloying engineering on the optimization of the energy band structure and carrier behavior of BiOX,and lists various modification methods used to improve the optimization of the intrinsic properties by alloying engineering,including defect engineering,morphology control as well as the synergy between alloying and other modification methods(bismuth-rich strategies,cation doping,construction of heterojunctions and plasma resonance effects).Subsequently,applications of alloyed BiOX in energy and environmental fields are summarized,including contaminant degradation,antibacterial,CO_(2)reduction,nitrogen fixation and organic ***,we summarize the current challenges and future directions of alloyed *** is expected that this work will provide guidance and assistance for an in-depth study and understanding of the mechanisms of alloying engineering to optimize intrinsic properties and design alloyed BiOX with higher photocatalytic activity.

关键词： Bismuth oxyhalide Photocatalytic Alloyed engineering Microstructural regulation Application

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A review on WO_(3)-based composite photocatalysts:synthesis,catalytic mechanism and diversified applications

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Rare Metals 2024年第8期43卷 3441-3459页

作者： xue Zhang Zi-qi Zhang Yan-Dong Sun Xiao-Jia Ma feng-Xian Jin Fang-Yuan Zhang Wei-Guang Han Bo-Xiong Shen Sheng-qi Guo College of Energy and Environmental Engineering Hebei University of TechnologyTianjin 300401China Department of Food and Chemical Engineering Liuzhou Institute of TechnologyLiuzhou 545616China

Photocatalysis as an emerging "green" energy conversion technology has attracted domestic and international *** technology uses semiconductor photocatalysts to convert solar energy into directly usable chemical energy,showing great potential for application in environmental pollutant purification and clean energy production,with broad development *** many semiconductor materials,tungsten trioxide(WO_(3)) is favored by researchers in the field of photocatalysis because of its good visible light response and excellent valence band hole oxidation ***,a large number of photocatalysts based on WO_(3),in particular W03-based composite photocatalysts,have been reported,and their applications cover a wide range of *** order to promote the development of WO_(3)-based photocatalysts and provide a reference for colleagues,we present a systematic summary of the applications and research progress of W03-based composites in the field of photocatalysis in recent *** from the structural properties of WO_(3)itself,this article summarizes the preparation methods and structure-activity relationships of WO_(3)-based composite ***,it introduces the current application status of existing WO_(3)-based composite photocatalysts in CO_(2) reduction,hydrogen production,nitrogen fixation,and pollutant ***,the development prospects were analyzed.

关键词： WO_(3)-based composite photocatalysts Intrinsic characteristic Preparation method Reaction mechanism Applications

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Drosophila X virus-like particles as delivery carriers for improved oral insecticidal efficacy of scorpion Androctonus australis peptide against the invasive fruit fly,Drosophila suzukii

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Insect Science 2024年第3期31卷 847-858页

作者： qi xue Luc Swevers Clauvis Nji Tizi Taning Faculty of Bioscience Engineering Department of Plants and CropsGhent UniversityGhentBelgium Insect Molecular Genetics and Biotechnology Institute of Biosciences and ApplicationsNational Centre for Scientific Research"Demokritos"AthensGreece

Insect-specific neurotoxic peptides derived from the venoms of scorpions and spiders can cause acute paralysis and death when injected into insects,offering a promising insecticidal component for insect pest ***,effective delivery systems are required to help neurotoxic peptides pass through the gut barrier into the hemolymph,where they can ***,we investigated the potential of a novel nanocarrier,Drosophila X virus-like particle(DXV-VLP),for delivering a neurotoxin from the scorpion Androctonus australis Hector(AaIT)against the invasive pest fruit fly,Drosophila *** results show that the fusion proteins of DXV polyproteins with AalT peptide at their Ctermini could be sufficiently produced in Lepidoptera Hi5 cells in a soluble form using the recombinant baculovirus expression system,and could self-assemble into VLPs with similar particle morphology and size to authentic DXV *** addition,the AalT peptides displayed on DXV-VLPs retained their toxicity,as demonstrated in injection bioassays that resulted in severe mortality(72%)in adults after 72 *** fed to adults,mild mortality was observed in the group treated with DXV-AalT(38%),while no mortality occurred in the group treated with AaIT peptide,thus indicating the significant role of DXV-VLPs in delivering AalT ***,this proof-of-concept study demonstrates for the first time that VLPs can be exploited to enhance oral delivery of insect-specific neurotoxic peptides in the context of pest ***,it provides insights for further improvements and potentially the development of neurotoxin-based bioinsecticides and/or transgenic crops for insect pest control.

关键词： AalT Drosophila suzuki nanocarrier neurotoxic peptides pest control virus-like particle(VLP)

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The regulatory mechanism of rapid lignification for timely anther dehiscence

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Journal of Integrative Plant Biology 2024年第8期66卷 1788-1800页

作者： Jing-Shi xue Yi-feng feng Ming-qi Zhang qin-Lin Xu Ya-Min Xu Jun-qin Shi Li-Fang Liu Xiao-feng Wu Shui Wang Zhong-Nan Yang Shanghai Key Laboratory of Plant Molecular Sciences College of Life SciencesShanghai Normal UniversityShanghai 200234China National Key Laboratory of Plant Molecular Genetics CAS Center for Excellence in Molecular Plant SciencesInstitute of Plant Physiology and EcologyChinese Academy of SciencesShanghai 200032China University of the Chinese Academy of Sciences Beijing 100049China Development Center of Plant Germplasm Resources College of Life SciencesShanghai Normal UniversityShanghai 200234China

Anther dehiscence is a crucial event in plant reproduction,tightly regulated and dependent on the lignification of the anther *** this study,we investigated the rapid lignification process that ensures timely anther dehiscence in *** findings reveal that endothecium lignification can be divided into two distinct *** Phase Ⅰ,lignin precursors are synthesized without polymerization,while Phase Ⅱ involves simultaneous synthesis of lignin precursors and *** transcription factors MYB26,NST1/2,and ARF17 specifically regulate the pathway responsible for the synthesis and polymerization of lignin monomers in Phase Ⅱ.MYB26-NST1/2 is the key regulatory pathway responsible for endothecium lignification,while ARF17 facilitates this process by interacting with ***,our results demonstrate that the lignification of the endothecium,which occurs within approximately 26 h,is much faster than that of the vascular *** findings provide valuable insights into the regulation mechanism of rapid lignification in the endothecium,which enables timely anther dehiscence and successful pollen release during plant reproduction.

关键词： anther dehiscence ARF17 endothecium lignin MYB26 NST

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Will the 2022 compound heatwaveedrought extreme over the Yangtze River Basin become Grey Rhino in the future?

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Advances in Climate Change Research 2024年第3期15卷 547-556页

作者： Ai-qing feng qing-Chen CHAO Lu-Lu LIU Ge GAO Guo-Fu WANG xue-Jun ZHANG qi-Guang WANG China Meteorological Administration Key Laboratory for Climate Prediction Studies National Climate CentreBeijing 100081China Key Laboratory of Land Surface Pattern and Simulation Institute of Geographic Sciences and Natural Resources ResearchChinese Academy of SciencesBeijing 100101China China Institute of Water Resources and Hydropower Research Beijing 100038China China Meteorological Administration Training Centre China Meteorological AdministrationBeijing 100081China

The increasingly frequent and severe regional-scale compound heatwave-drought extreme events(CHDEs),driven by global warming,present formidable challenges to ecosystems,residential livelihoods,and economic ***,uncertainty persists regarding the future trend of CHDEs and their insights into regional spatiotemporal *** integrating daily meteorological data from observations in 1961-2022 and global climate models(GCMs)based on the Shared Socioeconomic Pathways,the evolution patterns of CHDEs were compared and examined among three sub-catchments of the Yangtze River Basin,and the return periods of CHDE in 2050s and 210Os were *** findings indicate that the climate during the 2022 CHDE period was the warmest and driest recorded in 1961-2022,with precipitation less than 154.5 mm and a mean daily maximum temperature 3.4°C higher than the average of 1981-2010,whereas the char-acteristics in the sub-catchments exhibited temporal and spatial *** July-August 2022,the most notable feature of CHDE was its extremeness since 1961,with return periods of~200-year in upstream,80-year in midstream,and 40-year in downstream,*** 2050,the return periods witnessed 2022 CHDE would likely be reduced by *** towards 2100,under the highest emission scenario of SSP585,it was projected to substantially increase the frequency of CHDEs,with return periods reduced to one-third in the upstream and downstream,as well as halved in the *** findings provide valuable insights into the changing risks associated with forthcoming climate extremes,emphasizing the urgency of addressing these challenges in regional management and sustainable development.

关键词： Compound extreme event Joint return period Drought Heatwave Climate change Yangtze River Basin

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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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Sound event localization and detection based on deep learning

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Journal of Systems Engineering and Electronics 2024年第2期35卷 294-301页

作者： ZHAO Dada DING Kai qi Xiaogang CHEN Yu feng Hailin School of Mathematics and Statistics Xidian UniversityXi’an 710071China Science and Technology on Near-Surface Detection Laboratory Wuxi 214035China

Acoustic source localization(ASL)and sound event detection(SED)are two widely pursued independent research *** recent years,in order to achieve a more complete spatial and temporal representation of sound field,sound event localization and detection(SELD)has become a very active research *** paper presents a deep learning-based multioverlapping sound event localization and detection algorithm in three-dimensional ***-Mel spectrum and generalized cross-correlation spectrum are joined together in channel dimension as input *** features are classified and regressed in parallel after training by a neural network to obtain sound recognition and localization results *** channel attention mechanism is also introduced in the network to selectively enhance the features containing essential information and suppress the useless ***,a thourough comparison confirms the efficiency and effectiveness of the proposed SELD *** experiments show that the proposed algorithm is robust to reverberation and environment and can achieve higher recognition and localization accuracy compared with the baseline method.

关键词： sound event localization and detection(SELD) deep learning convolutional recursive neural network(CRNN) channel attention mechanism

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A robust viscoelastic surfactant tolerating 20% HCl up to 150℃ for oil well stimulation

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Petroleum Science 2024年第3期21卷 1865-1874页

作者： Ji Wang Ning qi Hong-Yao Yin Yu-Jun feng Polymer Research Institute State Key Laboratory of Polymer Materials EngineeringSichuan UniversityChengdu610065SichuanPR.China Tianfu Yongxing Laboratory New Theory and Technology of CO_(2) Capture Research CenterChengdu610065SichuanPR China School of Petroleum Engineering China University of Petroleum(East China)Qingdao266580ShandongPR China

Viscoelastic surfactants(VES)are often used as viscous diverters in acidizing stimulation to prolong the acid consumption time and maximize zonal coverage of the acid for improving well ***,the ceiling temperature of commercial VES cannot exceed 120℃in practical use because of the poor thermal stability and fragile molecular structure,hindering their implementation in hightemperature oil reservoirs,i.e.,≥150℃.Here we synthesized a novel C22-tailed diamine,N-erucaminopropyl-N,N-dimethylamine(EDPA),and examined comparatively its rheological behavior,assemblies morphology and molecular stability in 20 wt%HCl with a commercial VES,erucyl dimethyl amidopropyl betaine(EDAB).The feasibility of EDPA for acidizing stimulation was assessed by acid etching of carbonate rock with its HCl solution at 150℃.Rheological results showed that the 2.5 wt%EDPA—20 wt%HCl solution maintains stable viscosity of 90 m Pa s at 150℃for 60 min,while that of 2.0 wt%EDAB HCl solution is just 1 m Pa s under identical conditions.1H NMR spectra and cryo-TEM observations revealed that the chemical structure and self-assembled architectures of EDPA remained intact in such context,but the EDAB suffered from degradation due to the hydrolysis of the amide group,accounting for the poor heat-resistance and *** reaction rate of 2.5 wt%EDPA HCl solution with carbonate rock was one order of magnitude lower than that of 20 wt%HCl solution at 150℃,underpinning the potential of EDPA to be used in the high-temperature reservoirs *** work improved the thermal tolerance of VES in highly concentrated HCl solution,paving a feasible way for the acidization of high-temperature reservoir environments(~150℃).

关键词： Viscoelastic surfactants Thermal stability Self-diverting acid Wormlike micelles Acidizing stimulation

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