The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid ...The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid syntheses of aromatic scaffolds that contains deuterium remain an important yet elusive task.State-of-the-art approaches mainly relied on the transition metal-catalyzed C-H deuteration via the assistance of directing groups(DGs),which often suffered from over-deuteration and lengthy step counts required for installation and/or removal of DG.Herein,we report a generalizable synthetic linchpin strategy for the facile preparation of the ortho-deuterated aromatic core.Through capture of aryne-derived 1,3-zwitterion with heavy water,we synthesized an array of ortho-deuterated aryl sulfonium salts.These novel linchpins not only participated the transition metal catalyzed cross-coupling reaction as nucleophiles,but also served as aryl radical reservoirs under photochemical or electrochemical conditions,enabling facile and precise access to structurally diverse deuterated aromatics.Moreover,we have disclosed a novel EDA complex enabled direct arylation of phosphines under visible-light irradiation,further expanding the utility of our platform approach.展开更多
Current improved Empirical Mode Decomposition(EMD)methods enhance the accurate identification of peak and valley points in mechanical signals through noise-assisted filtering techniques,thereby improving the mode deco...Current improved Empirical Mode Decomposition(EMD)methods enhance the accurate identification of peak and valley points in mechanical signals through noise-assisted filtering techniques,thereby improving the mode decomposition performance,which is of great significance in extracting fault features from mechanical signals.However,noise-assisted filtering leads to the loss of critical features in mechanical signals and introduces a large amount of residual noise into Intrinsic Mode Functions(IMFs)that obscure signal features.To address these issues,a Precise Identification-based Mode Decomposition(PIMD)method is proposed.This method directly enhances the ability of EMD to precisely identify peak and valley points by using a proposed precise identifi-cation approach,which improves mode decomposition performance and avoids the negative impacts of noise-assisted filtering,thus benefiting the extraction of more mechanical fault features.Simulation results show that the proposed PIMD method can precisely identify peak and valley points of signals with noise of different signal-tonoise ratios and perform a highly rigorous high-low frequency decomposition,significantly outperforming EMD.Finally,mechanical fault diagnostic experiments on four bearing cases and two gear cases demonstrate that,compared to four mainstream methods,the PIMD method exhibits the best mode decomposition perfor-mance and can extract more and clearer mechanical fault features.展开更多
The development of robust anode-electrolyte interfaces(AEI)with enhanced compatibility and mechanical strength is critical for regulating zinc-ion nucleation kinetics,suppressing dendrite formation,and advancing zinc-...The development of robust anode-electrolyte interfaces(AEI)with enhanced compatibility and mechanical strength is critical for regulating zinc-ion nucleation kinetics,suppressing dendrite formation,and advancing zinc-ion battery commercialization.To address persistent interface degradation during battery cycling,we propose a novel manufacturing strategy utilizing digital-light-processing(DLP)3D printing.This approach enables programmable regulation of gel-polymer electrolyte(GPE)structures through layer-by-layer photopolymerization,achieving precision regulation of macro-microstructures and interfacial stresses.The DLP-manufactured GPEs feature cross-scale structures combining dense porous networks with smooth surface topography,providing abundant electrochemical active sites and stable interfacial contact.Multiphase-field simulations integrated with in-situ/ex-situ characterizations reveal stress-enhanced zinc deposition mechanisms,where optimized interfacial stress eliminates AEI contact instability,ensuring rapid mass transfer between electrode and electrolyte.Under regulated interface stress,the symmetrical cell demonstrates stability exceeding 2000 hours,and the full cell retains 91.72%capacity after 8000 ultralong cycles,with reliable operation under extreme temperature conditions(-10℃/60℃).The precise regulation of interfacial stresses establishes stable AEI configurations,demonstrating a transformative approach to durable zinc-ion battery design.展开更多
Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymer...Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymers(MIPs).To implement this synergistic strategy,bioinspired surface engineering was used to incorporate dual covalent receptors via precise post-imprinting modifications(PIMs)onto mesoporous silica nanosheets.The prepared sorbents(denoted as‘‘D-PMIPs”)were utilized to improve the specific identification of adenosine 5-monophosphate(AMP).Significantly,the mesoporous silica nanosheets possess a high surface area of approximately 498.73 m^(2)·g^(-1),which facilitates the formation of abundant specific recognition sites in the D-PMIPs.The dual covalent receptors are valuable for estab-lishing the spatial orientation and arrangement of AMP through multiple cooperative interactions.PIMs enable precise site-specific functionalization within the imprinted cavities,leading to the tailor-made formation of complementary binding sites.The maximum number of high-affinity binding sites(Nmax)of the D-PMIPs is 39.99 lmol·g^(-1),which is significantly higher than that of imprinted sorbents with a sin-gle receptor(i.e.,S-BMIPs or S-PMIPs).The kinetic data of the D-PMIPs can be effectively described by a pseudo-second-order model,indicating that the main binding mechanism involves synergistic chemisorption from boronate affinity and the pyrimidine base.This study suggests that using dual cova-lent receptors and PIMs is a reliable approach for creating imprinted sorbents with high selectivity,allow-ing for the controlled engineering of imprinted sites.展开更多
Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features.Herein,we successfull...Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features.Herein,we successfully synthesized an 11-core copper(Ⅰ)-alkynyl nanocluster(Cu11),which is stabilized by alkynyl ligands derived from a photosensitive rhodamine dye molecule.Notably,this Cu11cluster exhibited excellent photocatalytic hydrogen evolution activity(8.13 mmol g-1h-1)even in the absence of a mediator and noble metal co-catalyst.Furthermore,when Cu11clusters were loaded onto the surface of TiO_(2)nanosheets,the resultant Cu11@TiO_(2)nanocomposites exhibited a significant enhancement in hydrogen evolution efficiency,which is 60 times higher than that of pure TiO_(2)nanosheets.The incorporation of Cu11clusters within the Cu11@TiO_(2)effectively inhibits the recombination of photogenerated electrons and holes,thereby accelerating the charge separation and migration in the composite material.This work introduces a novel perspective for designing highly active copper cluster-based photocatalysts.展开更多
Strategic fluorination of solvent,a prominent strategy to enhance the electrolyte oxidation resistance and engineer a robust cathode-electrolyte interface,is crucial for realizing high-voltage lithium-ion batteries.Ac...Strategic fluorination of solvent,a prominent strategy to enhance the electrolyte oxidation resistance and engineer a robust cathode-electrolyte interface,is crucial for realizing high-voltage lithium-ion batteries.Actually,the adaptability of fluorinated solvents to high voltages is critically determined by the degree of fluorination and the fluorination site,yet lacks systematic design principles.Herein,we introduce a solvent screening descriptor based on ionization energy and Fukui function to assess molecular and site-specific reactivity.Computational and experimental results demonstrate that an optimal solvent with low ground-state energies and reactive sites is required as an ideal candidate for high-voltage electrolytes.Among derivatives from anisole,(trifluoromethoxy)benzene is identified as a superior candidate,enabling the formulation of a low reactivity solution(LPT)as electrolyte.Remarkably,the prepared Li‖LCO cell using LPT electrolyte maintained a high-capacity retention of 78.8%after 600 cycles at 4.5 V.In addition,the formation of an inorganic-rich interphase from LPT electrolyte effectively suppresses structural degradation to ensure a fast dynamic behavior.The utilization of LPT electrolyte also greatly reduces the amount of heat released and the production of O_(2)gas,which is favorable for addressing thermal runaway hazards.This screening strategy offers a practical approach for the design of flame-retardant high-voltage electrolytes.展开更多
Plants continuously generate new organs throughout their lives-a feat orchestrated by stem cells tucked within growing tips.But how do these cells know precisely when and where to divide?The answer lies in the walls s...Plants continuously generate new organs throughout their lives-a feat orchestrated by stem cells tucked within growing tips.But how do these cells know precisely when and where to divide?The answer lies in the walls surrounding them.Researchers led by Dr.YANG Weibing from the Center for Excellence in Molecular Plant Sciences of the Chinese Academy of Sciences have discovered that cell wall stiffness acts as a molecular guide,directing stem cell division with remarkable precision.展开更多
Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalit...Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.展开更多
With the development of education and technology,the construction of research public platforms has emerged as a critical initiative for many universities and top-tier public hospitals.The core and most fundamental fun...With the development of education and technology,the construction of research public platforms has emerged as a critical initiative for many universities and top-tier public hospitals.The core and most fundamental function of a basic public platform is to aggregate large instruments and specific resources,providing open services for instrumental analysis and sample testing.Optimized management and high-quality,efficient services are essential for such platforms.This article elucidates the construction of a research public platform in West China Hospital,focusing on the adoption of hierarchical management and precise services.The core of the hierarchical management lies in building a multi-level service platform composed of routine support platforms,advanced technology platforms,and specially qualification platforms,while establishing a talent hierarchy that differentiates between core and routine positions.This structure is designed to accurately meet the diverse needs of users and enhance resource efficiency.By implementing user access control with differentiated permissions for internal and external users and a dynamic credit-based review system,the laboratory can ensure safe and efficient operations.The four service modes—instrument usage,in-lab experiments,sample testing,and collaborative projects—are precisely aligned with various research scenarios.Proactive engagement with grant-funded projects,customized services for research groups,and a multidimensional training system further strengthen the platform's support for major scientific research tasks.Through systematic management and service innovation,this model achieves efficient integration and sustainable development of platform resources,providing a valuable reference for the construction of public platforms in similar medical institutions.展开更多
This study explores the use of the Global Navigation Satellite System(GNSS)precise point positioning(PPP)technology to determine the natural vibration periods of towering structures through simulations and field testi...This study explores the use of the Global Navigation Satellite System(GNSS)precise point positioning(PPP)technology to determine the natural vibration periods of towering structures through simulations and field testing.During the simulation phase,a GNSS receiver captured vi-bration waveforms generated by a single-axis motion simulator based on preset signal parameters,analyzing how different satellite system configurations affect the efficiency of extracting vibration parameters.Subsequently,field tests were conducted on a high-rise steel singletube tower.The results indicate that in the simulation environment,no matter the PPP positioning data under single GPS or multisystem combination,the vibration frequency of singleaxis motion simulator can be accurately extracted after frequency do-main analysis,with multisystem setups providing more precise amplitude parameters.In the field test,the natural vibration periods of the main vibration modes of high-rise steel single-tube tower measured by PPP technology closely match the results of the first two modes derived from finite element analysis.The first mode period calculated by the em-pirical formula is approximately 6%higher than those determined through finite element analysis and PPP.This study demonstrates the potential of PPP for structural vibration analysis,offering significant benefits for assessing dynamic responses and monitoring the health of towering structures.展开更多
Navigation satellites generally use satellite-ground and inter-satellite observation data for precise orbit determination.In orbit determination,the satellite position is often referenced to the satellite’s centroid,...Navigation satellites generally use satellite-ground and inter-satellite observation data for precise orbit determination.In orbit determination,the satellite position is often referenced to the satellite’s centroid,while the observational measurements are referenced to the satellite’s antenna phase center.The deviation between the satellite’s centroid and the antenna phase center forms the satellite antenna phase center error,which affects the precision of orbit determination.This paper takes a global navigation satellite system(GNSS)MEO satellite as an example and analyzes the actual situation of the satellite antenna phase center deviation and phase center variation based on the ground calibration data of the in-orbit satellite antenna phase center and the satellite’s in-orbit working status.The analysis shows that the antenna phase center variation caused by the satellite’s in-orbit operation is only at the centimeter level,which has a limited impact on orbit determination accuracy.The main source of precise orbit determination error is the satellite antenna phase center deviation,which can be corrected using ground calibration data.展开更多
This article provides a comprehensive review of the advancements in the application of artificial intelligence(AI)technology in the modernization of traditional Chinese medicine(TCM)compound prescriptions,and emphasiz...This article provides a comprehensive review of the advancements in the application of artificial intelligence(AI)technology in the modernization of traditional Chinese medicine(TCM)compound prescriptions,and emphasizes recent research developments,including intelligent design,prediction of mechanisms of action,and precise application of TCM compound prescriptions.The integration of multi-omics data,deep learning algorithms,and knowledge graph technologies has established novel technical avenues for the modernization research of TCM.This study systematically analyzes the advantages and challenges associated with AI technologies in the research of TCM compound prescriptions,highlighting issues such as data heterogeneity,limited interpretability of AI models,and the absence of standardized procedures.Furthermore,this article examines the prospective developmental trajectories within this field,highlighting the importance of synergistic collaboration between AI and traditional pharmacology to improve the clinical applicability and effectiveness of TCM.The objective is to offer valuable insights into the modernization of TCM driven by AI and to stimulate further research in this area.展开更多
Atomically precise palladium(Pd)clusters are emerging as versatile nanomaterials with applications in catalysis and biomedicine.This study explores the synthesis,structure evolution,and catalytic properties of Pd clus...Atomically precise palladium(Pd)clusters are emerging as versatile nanomaterials with applications in catalysis and biomedicine.This study explores the synthesis,structure evolution,and catalytic properties of Pd clusters stabilized by cyclohexanethiol(HSC_(6)H_(11))ligands.Using electrospray ionization mass spectrometry(ESI-MS)and single-crystal X-ray diffraction(SXRD),structures of the Pd clusters ranging from Pd4(SC_(6)H_(11))8 to Pd18(SC_(6)H_(11))36 were determined.This analysis revealed a structure evolution from polygonal to elliptical geometries of the PdnS2n frameworks as the cluster size increased.UV-Vis-NIR spectroscopy,combined with quantum chemical calculations,elucidated changes in the electronic structure of the clusters.Catalytic studies on the Sonogashira cross-coupling reactions demonstrated a size-dependent decline in activity attributed to variations in structural arrangements and electronic properties.Mechanistic insights proposed a distinctive Pd(Ⅱ)-Pd(Ⅳ)catalytic cycle.This research underscores how ligands and cluster size influence the structures and properties of Pd clusters,offering valuable insights for the future design and application of Pd clusters in advanced catalysis and beyond.展开更多
The vehicle-road coupling dynamics problem is a prominent issue in transportation,drawing significant attention in recent years.These dynamic equations are characterized by high-dimensionality,coupling,and time-varyin...The vehicle-road coupling dynamics problem is a prominent issue in transportation,drawing significant attention in recent years.These dynamic equations are characterized by high-dimensionality,coupling,and time-varying dynamics,making the exact solutions challenging to obtain.As a result,numerical integration methods are typically employed.However,conventional methods often suffer from low computational efficiency.To address this,this paper explores the application of the parameter freezing precise exponential integrator to vehicle-road coupling models.The model accounts for road roughness irregularities,incorporating all terms unrelated to the linear part into the algorithm's inhomogeneous vector.The general construction process of the algorithm is detailed.The validity of numerical results is verified through approximate analytical solutions(AASs),and the advantages of this method over traditional numerical integration methods are demonstrated.Multiple parameter freezing precise exponential integrator schemes are constructed based on the Runge-Kutta framework,with the fourth-order four-stage scheme identified as the optimal one.The study indicates that this method can quickly and accurately capture the dynamic system's vibration response,offering a new,efficient approach for numerical studies of high-dimensional vehicle-road coupling systems.展开更多
Noble metal nanoclusters have attracted great scientific interests due to their tempting properties and applications.Significant strides have been made in recent years to synthesis atomically precise nanoclusters by u...Noble metal nanoclusters have attracted great scientific interests due to their tempting properties and applications.Significant strides have been made in recent years to synthesis atomically precise nanoclusters by utilizing polyoxometalates as protecting ligands.Remarkably,the group of Professor Suzuki from the University of Tokyo has made a great contribution in this field.Here we spotlight on four related papers in this area and present a brief highlight of these publications.展开更多
With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our resu...With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our results show that the recollision time window can be precisely controlled within an isolated time interval of several hundred attoseconds, which is useful for understanding the subcycle correlated electron dynamics. More interestingly, the correlated electron momentum distribution (CEMD) exhibits a strong dependence on laser intensity. That is, at lower laser intensity, CEMD is located in the first quadrant. As the laser intensity increases,CEMD shifts almost completely to the second and fourth quadrants, and then gradually to the third quadrant.The underlying physics governing the CEMD's dependence on laser intensity is explained.展开更多
Crustal deformation can provide constraints for studying earthquake rupture and shock wave transmission for the Mw9.0 eastern Japan great earthquake. Using the single- epoch precise point positioning （PPP） method an...Crustal deformation can provide constraints for studying earthquake rupture and shock wave transmission for the Mw9.0 eastern Japan great earthquake. Using the single- epoch precise point positioning （PPP） method and the appropriate positioning flow, we process GPS data from six IGS （International GNSS Service） sites （e.g., MIZU, TSK2, USUD, MTKA, AIRA and KSMV） located in Japan and obtain the positioning results with centimeter scale precision. The displacement time series of the six sites are analyzed using the least squares spectral analysis method to estimate deformations caused by the Mw9.0 mainshock and the Mw7.9 aftershock, and the cumulative displacements after 1 day. Mainshock displacements at station MIZU, the nearest site to the mainshock in the North （N）, East （E）, and Up （U） directions, are -1.202 m, 2.180 m and -0.104 m, respectively, and the cumulative deformations after 1 day are -1.117 m, 2.071 m and -0.072 m, respectively. The displacements at station KSMV, the nearest site to the Mw7.9 aftershock in the N, E and U directions, are -0.032 m, 0.742 m and -0.345 m, respectively. The other sites obviously experienced eastern movements and subsidence. The deformation vectors indicate that the horizontal displacements caused by the earthquake point to the epicenter and rupture. Elastic bounds evidently took place at all sites. The results indicate that the crustal movements and earthquake were part of a megathrust caused by the Pacific Plate sinking under the North American Plate to the northeast of Japan island arc.展开更多
The HY-2 satellite carrying a satellite-borne GPS receiver is the first Chinese radar altimeter satellite, whose radial orbit determination precision must reach the centimeter level. Now HY-2 is in the test phase so t...The HY-2 satellite carrying a satellite-borne GPS receiver is the first Chinese radar altimeter satellite, whose radial orbit determination precision must reach the centimeter level. Now HY-2 is in the test phase so that the observations are not openly released. In order to study the precise orbit determination precision and procedure for HY-2 based on the satellite- borne GPS technique, the satellite-borne GPS data are simulated in this paper. The HY-2 satellite-borne GPS antenna can receive at least seven GPS satellites each epoch, which can validate the GPS receiver and antenna design. What＇s more, the precise orbit determination processing flow is given and precise orbit determination experiments are conducted using the HY-2-borne GPS data with both the reduced-dynamic method and the kinematic geometry method. With the 1 and 3 mm phase data random errors, the radial orbit determination precision can achieve the centimeter level using these two methods and the kinematic orbit accuracy is slightly lower than that of the reduced-dynamic orbit. The earth gravity field model is an important factor which seriously affects the precise orbit determination of altimeter satellites. The reduced-dynamic orbit determination experiments are made with different earth gravity field models, such as EIGEN2, EGM96, TEG4, and GEMT3. Using a large number of high precision satellite-bome GPS data, the HY-2 precise orbit determination can reach the centimeter level with commonly used earth gravity field models up to above 50 degrees and orders.展开更多
基金supported by the National Natural Science Foundation of China (Nos.22271010 and 21702013)。
文摘The deuterium labeling has garnered significant interest in drug discovery due to its critical role on improving pharmacokinetic and metabolic properties.However,despite its pharmaceutical value,the general and rapid syntheses of aromatic scaffolds that contains deuterium remain an important yet elusive task.State-of-the-art approaches mainly relied on the transition metal-catalyzed C-H deuteration via the assistance of directing groups(DGs),which often suffered from over-deuteration and lengthy step counts required for installation and/or removal of DG.Herein,we report a generalizable synthetic linchpin strategy for the facile preparation of the ortho-deuterated aromatic core.Through capture of aryne-derived 1,3-zwitterion with heavy water,we synthesized an array of ortho-deuterated aryl sulfonium salts.These novel linchpins not only participated the transition metal catalyzed cross-coupling reaction as nucleophiles,but also served as aryl radical reservoirs under photochemical or electrochemical conditions,enabling facile and precise access to structurally diverse deuterated aromatics.Moreover,we have disclosed a novel EDA complex enabled direct arylation of phosphines under visible-light irradiation,further expanding the utility of our platform approach.
基金Supported by National Natural Science Foundation of China(Grant No.52075236)Opening Foundation of Intelligent Manufacturing Technology(Shantou University),Ministry of Education(Grant No.STME2024002)+1 种基金Hundred Doctor and Hundred Enterprise,Science and Technology Project,Ji'an City(Grant No.42064001)Guangdong Provincial University Innovation Team Project(Grant No.2020KCXTD012).
文摘Current improved Empirical Mode Decomposition(EMD)methods enhance the accurate identification of peak and valley points in mechanical signals through noise-assisted filtering techniques,thereby improving the mode decomposition performance,which is of great significance in extracting fault features from mechanical signals.However,noise-assisted filtering leads to the loss of critical features in mechanical signals and introduces a large amount of residual noise into Intrinsic Mode Functions(IMFs)that obscure signal features.To address these issues,a Precise Identification-based Mode Decomposition(PIMD)method is proposed.This method directly enhances the ability of EMD to precisely identify peak and valley points by using a proposed precise identifi-cation approach,which improves mode decomposition performance and avoids the negative impacts of noise-assisted filtering,thus benefiting the extraction of more mechanical fault features.Simulation results show that the proposed PIMD method can precisely identify peak and valley points of signals with noise of different signal-tonoise ratios and perform a highly rigorous high-low frequency decomposition,significantly outperforming EMD.Finally,mechanical fault diagnostic experiments on four bearing cases and two gear cases demonstrate that,compared to four mainstream methods,the PIMD method exhibits the best mode decomposition perfor-mance and can extract more and clearer mechanical fault features.
基金supported by National Natural Science Foundation of China(U22A20193)National Key Research and Development Program of China(2024YFB3409000)+1 种基金TCL science and technology innovation fund(20231751)Fundamental Research Funds for the Central Universities(No.2024ZYGXZR066)。
文摘The development of robust anode-electrolyte interfaces(AEI)with enhanced compatibility and mechanical strength is critical for regulating zinc-ion nucleation kinetics,suppressing dendrite formation,and advancing zinc-ion battery commercialization.To address persistent interface degradation during battery cycling,we propose a novel manufacturing strategy utilizing digital-light-processing(DLP)3D printing.This approach enables programmable regulation of gel-polymer electrolyte(GPE)structures through layer-by-layer photopolymerization,achieving precision regulation of macro-microstructures and interfacial stresses.The DLP-manufactured GPEs feature cross-scale structures combining dense porous networks with smooth surface topography,providing abundant electrochemical active sites and stable interfacial contact.Multiphase-field simulations integrated with in-situ/ex-situ characterizations reveal stress-enhanced zinc deposition mechanisms,where optimized interfacial stress eliminates AEI contact instability,ensuring rapid mass transfer between electrode and electrolyte.Under regulated interface stress,the symmetrical cell demonstrates stability exceeding 2000 hours,and the full cell retains 91.72%capacity after 8000 ultralong cycles,with reliable operation under extreme temperature conditions(-10℃/60℃).The precise regulation of interfacial stresses establishes stable AEI configurations,demonstrating a transformative approach to durable zinc-ion battery design.
基金supported by the National Natural Science Foundation of China(22078132,22108103,and U22A20413)the Open Funding Project of the National Key Labora-tory of Biochemical Engineering(2021KF-02)+3 种基金China Postdoctoral Science Foundation(2021M691301)Jiangsu Key Research and Development Program(BE2022356)the Postdoctoral Fellowship Program of China Postdoctoral Science Foundation(CPSF)(GZ20230989)Jiangsu Agricultural Independent Innovation Fund Project(CX(21)3079).
文摘Expanding the specific surface area of substrates and carrying out precise surface engineering of imprinted nanocavities are crucial methods for enhancing the identification efficiency of molecularly imprinted polymers(MIPs).To implement this synergistic strategy,bioinspired surface engineering was used to incorporate dual covalent receptors via precise post-imprinting modifications(PIMs)onto mesoporous silica nanosheets.The prepared sorbents(denoted as‘‘D-PMIPs”)were utilized to improve the specific identification of adenosine 5-monophosphate(AMP).Significantly,the mesoporous silica nanosheets possess a high surface area of approximately 498.73 m^(2)·g^(-1),which facilitates the formation of abundant specific recognition sites in the D-PMIPs.The dual covalent receptors are valuable for estab-lishing the spatial orientation and arrangement of AMP through multiple cooperative interactions.PIMs enable precise site-specific functionalization within the imprinted cavities,leading to the tailor-made formation of complementary binding sites.The maximum number of high-affinity binding sites(Nmax)of the D-PMIPs is 39.99 lmol·g^(-1),which is significantly higher than that of imprinted sorbents with a sin-gle receptor(i.e.,S-BMIPs or S-PMIPs).The kinetic data of the D-PMIPs can be effectively described by a pseudo-second-order model,indicating that the main binding mechanism involves synergistic chemisorption from boronate affinity and the pyrimidine base.This study suggests that using dual cova-lent receptors and PIMs is a reliable approach for creating imprinted sorbents with high selectivity,allow-ing for the controlled engineering of imprinted sites.
基金supported by the National Natural Science Foundation of China(Nos.22371263 and U2004193)Natural Science Foundation of Henan Province(No.232300421225)。
文摘Metal nanoclusters with well-defined atomic structures offer significant promise in the field of catalysis due to their sub-nanometer size and tunable organic-inorganic hybrid structural features.Herein,we successfully synthesized an 11-core copper(Ⅰ)-alkynyl nanocluster(Cu11),which is stabilized by alkynyl ligands derived from a photosensitive rhodamine dye molecule.Notably,this Cu11cluster exhibited excellent photocatalytic hydrogen evolution activity(8.13 mmol g-1h-1)even in the absence of a mediator and noble metal co-catalyst.Furthermore,when Cu11clusters were loaded onto the surface of TiO_(2)nanosheets,the resultant Cu11@TiO_(2)nanocomposites exhibited a significant enhancement in hydrogen evolution efficiency,which is 60 times higher than that of pure TiO_(2)nanosheets.The incorporation of Cu11clusters within the Cu11@TiO_(2)effectively inhibits the recombination of photogenerated electrons and holes,thereby accelerating the charge separation and migration in the composite material.This work introduces a novel perspective for designing highly active copper cluster-based photocatalysts.
基金financial support from the National Natural Science Foundation of China(22522814,22278378,and 52402318)Zhejiang Provincial Natural Science Foundation of China(LDQ24E030001 and LQN25E020003)Science Foundation of Zhejiang Sci-Tech University(22212011-Y and 24212149-Y).
文摘Strategic fluorination of solvent,a prominent strategy to enhance the electrolyte oxidation resistance and engineer a robust cathode-electrolyte interface,is crucial for realizing high-voltage lithium-ion batteries.Actually,the adaptability of fluorinated solvents to high voltages is critically determined by the degree of fluorination and the fluorination site,yet lacks systematic design principles.Herein,we introduce a solvent screening descriptor based on ionization energy and Fukui function to assess molecular and site-specific reactivity.Computational and experimental results demonstrate that an optimal solvent with low ground-state energies and reactive sites is required as an ideal candidate for high-voltage electrolytes.Among derivatives from anisole,(trifluoromethoxy)benzene is identified as a superior candidate,enabling the formulation of a low reactivity solution(LPT)as electrolyte.Remarkably,the prepared Li‖LCO cell using LPT electrolyte maintained a high-capacity retention of 78.8%after 600 cycles at 4.5 V.In addition,the formation of an inorganic-rich interphase from LPT electrolyte effectively suppresses structural degradation to ensure a fast dynamic behavior.The utilization of LPT electrolyte also greatly reduces the amount of heat released and the production of O_(2)gas,which is favorable for addressing thermal runaway hazards.This screening strategy offers a practical approach for the design of flame-retardant high-voltage electrolytes.
文摘Plants continuously generate new organs throughout their lives-a feat orchestrated by stem cells tucked within growing tips.But how do these cells know precisely when and where to divide?The answer lies in the walls surrounding them.Researchers led by Dr.YANG Weibing from the Center for Excellence in Molecular Plant Sciences of the Chinese Academy of Sciences have discovered that cell wall stiffness acts as a molecular guide,directing stem cell division with remarkable precision.
基金supported by the open funds of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, Chinathe funding from Guangdong Natural Science Funds (No. 2023A0505050107)。
文摘Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.
基金supported by Sichuan University AI-Driven In-novative Experimental Technology Research Project(SCU2025047).
文摘With the development of education and technology,the construction of research public platforms has emerged as a critical initiative for many universities and top-tier public hospitals.The core and most fundamental function of a basic public platform is to aggregate large instruments and specific resources,providing open services for instrumental analysis and sample testing.Optimized management and high-quality,efficient services are essential for such platforms.This article elucidates the construction of a research public platform in West China Hospital,focusing on the adoption of hierarchical management and precise services.The core of the hierarchical management lies in building a multi-level service platform composed of routine support platforms,advanced technology platforms,and specially qualification platforms,while establishing a talent hierarchy that differentiates between core and routine positions.This structure is designed to accurately meet the diverse needs of users and enhance resource efficiency.By implementing user access control with differentiated permissions for internal and external users and a dynamic credit-based review system,the laboratory can ensure safe and efficient operations.The four service modes—instrument usage,in-lab experiments,sample testing,and collaborative projects—are precisely aligned with various research scenarios.Proactive engagement with grant-funded projects,customized services for research groups,and a multidimensional training system further strengthen the platform's support for major scientific research tasks.Through systematic management and service innovation,this model achieves efficient integration and sustainable development of platform resources,providing a valuable reference for the construction of public platforms in similar medical institutions.
基金The National Natural Science Foundation of China(No.41974214).
文摘This study explores the use of the Global Navigation Satellite System(GNSS)precise point positioning(PPP)technology to determine the natural vibration periods of towering structures through simulations and field testing.During the simulation phase,a GNSS receiver captured vi-bration waveforms generated by a single-axis motion simulator based on preset signal parameters,analyzing how different satellite system configurations affect the efficiency of extracting vibration parameters.Subsequently,field tests were conducted on a high-rise steel singletube tower.The results indicate that in the simulation environment,no matter the PPP positioning data under single GPS or multisystem combination,the vibration frequency of singleaxis motion simulator can be accurately extracted after frequency do-main analysis,with multisystem setups providing more precise amplitude parameters.In the field test,the natural vibration periods of the main vibration modes of high-rise steel single-tube tower measured by PPP technology closely match the results of the first two modes derived from finite element analysis.The first mode period calculated by the em-pirical formula is approximately 6%higher than those determined through finite element analysis and PPP.This study demonstrates the potential of PPP for structural vibration analysis,offering significant benefits for assessing dynamic responses and monitoring the health of towering structures.
文摘Navigation satellites generally use satellite-ground and inter-satellite observation data for precise orbit determination.In orbit determination,the satellite position is often referenced to the satellite’s centroid,while the observational measurements are referenced to the satellite’s antenna phase center.The deviation between the satellite’s centroid and the antenna phase center forms the satellite antenna phase center error,which affects the precision of orbit determination.This paper takes a global navigation satellite system(GNSS)MEO satellite as an example and analyzes the actual situation of the satellite antenna phase center deviation and phase center variation based on the ground calibration data of the in-orbit satellite antenna phase center and the satellite’s in-orbit working status.The analysis shows that the antenna phase center variation caused by the satellite’s in-orbit operation is only at the centimeter level,which has a limited impact on orbit determination accuracy.The main source of precise orbit determination error is the satellite antenna phase center deviation,which can be corrected using ground calibration data.
文摘This article provides a comprehensive review of the advancements in the application of artificial intelligence(AI)technology in the modernization of traditional Chinese medicine(TCM)compound prescriptions,and emphasizes recent research developments,including intelligent design,prediction of mechanisms of action,and precise application of TCM compound prescriptions.The integration of multi-omics data,deep learning algorithms,and knowledge graph technologies has established novel technical avenues for the modernization research of TCM.This study systematically analyzes the advantages and challenges associated with AI technologies in the research of TCM compound prescriptions,highlighting issues such as data heterogeneity,limited interpretability of AI models,and the absence of standardized procedures.Furthermore,this article examines the prospective developmental trajectories within this field,highlighting the importance of synergistic collaboration between AI and traditional pharmacology to improve the clinical applicability and effectiveness of TCM.The objective is to offer valuable insights into the modernization of TCM driven by AI and to stimulate further research in this area.
基金supported by the Start-Up Research Funding of Fujian Normal University(No.Y0720326K13)the National Natural Science Foundation of China(Nos.22103035 and 22033005)+2 种基金the National Key R&D Program of China(No.2022YFA1503900)Shenzhen Science and Technology Program(No.RCYX20231211090357078)Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002).
文摘Atomically precise palladium(Pd)clusters are emerging as versatile nanomaterials with applications in catalysis and biomedicine.This study explores the synthesis,structure evolution,and catalytic properties of Pd clusters stabilized by cyclohexanethiol(HSC_(6)H_(11))ligands.Using electrospray ionization mass spectrometry(ESI-MS)and single-crystal X-ray diffraction(SXRD),structures of the Pd clusters ranging from Pd4(SC_(6)H_(11))8 to Pd18(SC_(6)H_(11))36 were determined.This analysis revealed a structure evolution from polygonal to elliptical geometries of the PdnS2n frameworks as the cluster size increased.UV-Vis-NIR spectroscopy,combined with quantum chemical calculations,elucidated changes in the electronic structure of the clusters.Catalytic studies on the Sonogashira cross-coupling reactions demonstrated a size-dependent decline in activity attributed to variations in structural arrangements and electronic properties.Mechanistic insights proposed a distinctive Pd(Ⅱ)-Pd(Ⅳ)catalytic cycle.This research underscores how ligands and cluster size influence the structures and properties of Pd clusters,offering valuable insights for the future design and application of Pd clusters in advanced catalysis and beyond.
基金Supported by the National Natural Science Foundation of China(No.U22A20246)the Key Project of Natural Science Foundation of Hebei Province of China(Basic Research Base Project)(No.A2023210064)the Science and Technology Program of Hebei Province of China(Nos.246Z1904G and 225676162GH)。
文摘The vehicle-road coupling dynamics problem is a prominent issue in transportation,drawing significant attention in recent years.These dynamic equations are characterized by high-dimensionality,coupling,and time-varying dynamics,making the exact solutions challenging to obtain.As a result,numerical integration methods are typically employed.However,conventional methods often suffer from low computational efficiency.To address this,this paper explores the application of the parameter freezing precise exponential integrator to vehicle-road coupling models.The model accounts for road roughness irregularities,incorporating all terms unrelated to the linear part into the algorithm's inhomogeneous vector.The general construction process of the algorithm is detailed.The validity of numerical results is verified through approximate analytical solutions(AASs),and the advantages of this method over traditional numerical integration methods are demonstrated.Multiple parameter freezing precise exponential integrator schemes are constructed based on the Runge-Kutta framework,with the fourth-order four-stage scheme identified as the optimal one.The study indicates that this method can quickly and accurately capture the dynamic system's vibration response,offering a new,efficient approach for numerical studies of high-dimensional vehicle-road coupling systems.
基金financially supported by the Foundation of Jilin Educational Committee(JJKH20231298KJ)Natural Scientific Foundation of Jilin Province Science and Technology Department(20230101032JC)
文摘Noble metal nanoclusters have attracted great scientific interests due to their tempting properties and applications.Significant strides have been made in recent years to synthesis atomically precise nanoclusters by utilizing polyoxometalates as protecting ligands.Remarkably,the group of Professor Suzuki from the University of Tokyo has made a great contribution in this field.Here we spotlight on four related papers in this area and present a brief highlight of these publications.
基金supported by the National Natural Science Foundation of China (Grant No. 12074329)Nanhu Scholars Program for Young Scholars of Xinyang Normal University。
文摘With a three-dimensional semiclassical ensemble method, we theoretically investigated the nonsequential double ionization of Ar driven by the spatially inhomogeneous few-cycle negatively chirped laser pulses. Our results show that the recollision time window can be precisely controlled within an isolated time interval of several hundred attoseconds, which is useful for understanding the subcycle correlated electron dynamics. More interestingly, the correlated electron momentum distribution (CEMD) exhibits a strong dependence on laser intensity. That is, at lower laser intensity, CEMD is located in the first quadrant. As the laser intensity increases,CEMD shifts almost completely to the second and fourth quadrants, and then gradually to the third quadrant.The underlying physics governing the CEMD's dependence on laser intensity is explained.
基金supported partially by the National Natural Science Foundation of China(No.40974004 and 40974016)the Key Laboratory of Surveying and Mapping Technology on Island and Reef of NASMG,China(No.2011A01)the Key Laboratory of Advanced Surveying Engineering of NASMG,China(No.TJES1101)
文摘Crustal deformation can provide constraints for studying earthquake rupture and shock wave transmission for the Mw9.0 eastern Japan great earthquake. Using the single- epoch precise point positioning （PPP） method and the appropriate positioning flow, we process GPS data from six IGS （International GNSS Service） sites （e.g., MIZU, TSK2, USUD, MTKA, AIRA and KSMV） located in Japan and obtain the positioning results with centimeter scale precision. The displacement time series of the six sites are analyzed using the least squares spectral analysis method to estimate deformations caused by the Mw9.0 mainshock and the Mw7.9 aftershock, and the cumulative displacements after 1 day. Mainshock displacements at station MIZU, the nearest site to the mainshock in the North （N）, East （E）, and Up （U） directions, are -1.202 m, 2.180 m and -0.104 m, respectively, and the cumulative deformations after 1 day are -1.117 m, 2.071 m and -0.072 m, respectively. The displacements at station KSMV, the nearest site to the Mw7.9 aftershock in the N, E and U directions, are -0.032 m, 0.742 m and -0.345 m, respectively. The other sites obviously experienced eastern movements and subsidence. The deformation vectors indicate that the horizontal displacements caused by the earthquake point to the epicenter and rupture. Elastic bounds evidently took place at all sites. The results indicate that the crustal movements and earthquake were part of a megathrust caused by the Pacific Plate sinking under the North American Plate to the northeast of Japan island arc.
基金supported partially by the National Natural Science Foundation of China (Nos. 40974004 and 40974016)Key Laboratory of Dynamic Geodesy of CAS, China (No. L09-01) R&I Team Support Program and the Graduate Science and Technology Foundation of SDUST, China (No. YCA110403)
文摘The HY-2 satellite carrying a satellite-borne GPS receiver is the first Chinese radar altimeter satellite, whose radial orbit determination precision must reach the centimeter level. Now HY-2 is in the test phase so that the observations are not openly released. In order to study the precise orbit determination precision and procedure for HY-2 based on the satellite- borne GPS technique, the satellite-borne GPS data are simulated in this paper. The HY-2 satellite-borne GPS antenna can receive at least seven GPS satellites each epoch, which can validate the GPS receiver and antenna design. What＇s more, the precise orbit determination processing flow is given and precise orbit determination experiments are conducted using the HY-2-borne GPS data with both the reduced-dynamic method and the kinematic geometry method. With the 1 and 3 mm phase data random errors, the radial orbit determination precision can achieve the centimeter level using these two methods and the kinematic orbit accuracy is slightly lower than that of the reduced-dynamic orbit. The earth gravity field model is an important factor which seriously affects the precise orbit determination of altimeter satellites. The reduced-dynamic orbit determination experiments are made with different earth gravity field models, such as EIGEN2, EGM96, TEG4, and GEMT3. Using a large number of high precision satellite-bome GPS data, the HY-2 precise orbit determination can reach the centimeter level with commonly used earth gravity field models up to above 50 degrees and orders.
