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Cobalt-Catalyzed Switchable[4+1]and[4+1+1]Spirocyclization of Aromatic Amides with 2-Diazo-1H-indene-1,3(2H)-dione:Access to Spiro Indene-2,1'-isoindolinones and Spiro Isochroman-3,1'-isoindolinones

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Chinese Journal of Chemistry 2024年第4期42卷 363-369页

作者： Bin li Mengmeng Xie Jingyu li Nana Shen Xinying zhang Xuesen fan State Key Laboratory of Antiviral Drugs Pingyuan LaboratoryKey Laboratory of Green Chemical Media and ReactionsKey Laboratory for Yellow River and Huai River Water Environmental Pollution ControlMinistry of EducationSchool of EnvironmentSchool of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiangHenan453007 China

Herein,we report a condition-controlled divergent synthesis of spiro indene-2,1'-isoindolinones and spiro isochroman-3,1'-isoindolinones through cobalt-catalyzed formal[4+1]and[4+1+1]spirocyclization of aromatic amides with 2-diazo-1H-indene-1,3(2H)-dione.When the reaction is carried out under air in ethyl acetate,spiro indene-2,1'-isoindolinones are formed through Co(II)-catalyzed C—H/N—H[4+1]spirocyclization.When the reaction is run under O2 in CH3CN,on the other hand,spiro isochroman-3,1'-isoindolinones are generated through Baeyer-Villiger oxidation of the in situ formed spiro indene-2,1'-isoindolinones with O2 as a cheaper and environmental-friendly oxygen source.In general,these protocols have advantages such as using non-precious and earth-abundant metal catalyst,no extra additive,high efficiency and regioselectivity.A gram-scale synthesis and the removal of the directing group further highlight its utility.

关键词： Spiro indene-2,1'-isoindolinones Spiro isochroman-3,1'-isoindolinones 3d Transition metals Cobalt-catalyzed C-H Activation Switchable[4+1]and[4+1+1]spirocyclization Aromatic amides 2-Diazo-1H-indene-1,3(2H)-dione

Engineering tantalum nitride for efficient photoelectrochemical water splitting

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Science China Chemistry 2024年第7期67卷 2171-2180页

作者： Beibei zhang Zeyu fan Yanbo li Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaChengdu 610054China

Photoelectrochemical(PEC)water splitting is a promising energy conversion strategy for directly converting solar energy into green hydrogen fuel.Constructing an efficient PEC device,finding an efficient photoanode material with a suitable band gap and favorable band-edge positions is essential.Tantalum nitride(Ta_(3)N_(5))meets these fundamental requirements,and its theoretical maximum solar-to-hydrogen(STH)conversion efficiency can reach 15.9%.Consequently,it has been widely applied as a photoanode material for the PEC oxygen evolution reaction(OER).However,severe bulk and interface charge recombination,along with sluggish water oxygen kinetics,seriously limits its STH conversion efficiency for PEC water splitting.Herein,this feature article briefly reviews recent advances by our research group in improving the STH conversion efficiency of the Ta_(3)N_(5)photoanode using various strategies,including defect engineering,construction of a gradient band structure,interface engineering,and surface modification of self-healing OER cocatalyst.Up to now,the obtained half-cell STH efficiency has exceeded 4%,providing a solid foundation for the development of tandem PEC devices for unbiased solar-driven overall water splitting toward practical application.

关键词： Photoelectrochemical water splitting tantalum nitride defect engineering interface engineering oxygen evolution cocatalyst

Monogamy and polygamy for the generalized W-class states using unified-(q,s)entropy

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Science China(Physics,Mechanics & Astronomy) 2024年第1期67卷 10-22页

作者： Bo li Bing Xie Zhanjun zhang Heng fan School of Computer and Computing Science Hangzhou City UniversityHangzhou 310015China Department of Mathematics East China University of TechnologyNanchang 330013China School of Information&Electronic Engineering(Sussex Artificial Intelligence Institute) Zhejiang Gongshang UniversityHangzhou 310018China Institute of Physics Chinese Academy of SciencesBeijing 100190China

We describe the entanglement distribution and restricted shareability of the multipartite generalized W-class states and their reduced density matrix under arbitrary partitions by using monogamy and polygamy relation based on the unified-(q,s)entropy.Firstly,we provide an analytical formula of unified-(q,s)entanglement(UE)and an analytical lower bound of unified-(q,s)entanglement of assistance(UEo A)for a reduced density matrix of a generalized W-class state.Then,we use these two analytical formulas to derive the monogamy and polygamy inequalities for a reduced density matrix of a qudit generalized W-class(GW)state.We establish two partition-dependent residual entanglements based on the new monogamy relation,which is helpful to obtain a comprehensive analysis of entanglement dynamics of generalized W-class states.Further,we investigate tighter monogamy and polygamy relations based on the power ofαth(α≥0)for UE andβth(β≥0)for UEo A,respectively.The results show that the entanglement distribution characteristics of generalized W-class states satisfying stronger constraints can be described more accurately.

关键词： monogamy polygamy multiqudit unified entropy

Stochastic resonance of spinor condensates in optical cavity

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Science China(Physics,Mechanics & Astronomy) 2024年第3期67卷 80-87页

作者： Zheng-Chun li Bixuan fan Lu Zhou Weiping zhang School of Physics and Astronomy and Tsung-Dao Lee InstituteShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Precision Spectroscopy School of Physics and Electronic ScienceEast China Normal UniversityShanghai 200241China College of Physics and Communication Electronics Jiangxi Normal UniversityNanchang 330022China Shanghai Branch Hefei National LaboratoryShanghai 201315China Shanghai Research Center for Quantum Sciences Shanghai 201315China Collaborative Innovation Center of Extreme Optics Shanxi UniversityTaiyuan 030006China

Stochastic resonance is a phenomenon in which adding random noise to a system enhances the detection or transmission of a weak signal. It occurs when the noise interacts with the system's nonlinearity, thus improving signal-to-noise ratio and increasing sensitivity. Although parametric resonances in an atomic spinor Bose-Einstein condensate have been investigated, the question of whether one can observe stochastic resonance in such a system persists. In this study we propose a scheme for generating stochastic resonance in a cavity-spinor Bose-Einstein condensate coupling system. We demonstrate stochastic resonance through numerical calculations using the mean-field theory and truncated Wigner approximation methods. Furthermore, the characteristics of the system's response to noise and periodic signals are studied in detail. This study unravels a new scheme for observing stochastic resonance via linking atomic many-body physics with cavity quantum electrodynamics.

关键词： spinor condensate stochastic resonance optical cavity

Solvent-free carbon sphere nanofluids towards intelligent lubrication regulation

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Friction 2024年第1期12卷 95-109页

作者： Sheng zhang Wen li Xiaoliang MA Xiaoqiang fan Minhao ZHU Tribology Research Institute School of Mechanical EngineeringSouthwest Jiaotong UniversityChengdu 610031China Key Laboratory of Advanced Technologies of Materials Ministry of EducationSchool of Materials Science and EngineeringSouthwest Jiaotong UniversityChengdu 610031China

By simply switching the electrical circuit installed on steel/steel contact,the tribological behaviors of nanofluids(NFs)can be regulated in real time,thereby achieving the desired performance of friction reduction and wear resistance.Herein,solvent-free carbon spherical nanofluids(C-NFs)were successfully prepared for intelligent lubrication regulation.C-NFs with excellent lubrication performance can immediately reduce the coefficient of friction(COF)despite applying a weak electric potential(1.5 V).Moreover,polyethylene glycol 400(PEG400)containing 5.0 wt%C-NFs remained responsive to electrical stimulation under the intermittent voltage application with an average coefficient of friction(ACOF)reduction of 20.8%over PEG400.Such intelligent lubrication regulation of C-NFs under an external electric field(EEF)mainly depends on the orderly arranged double-electric adsorption film of ion canopy-adsorbed carbon spheres(CSs).The intermittent electrical application can continuously reinforce the adsorption film and its durability for real-time controlling the sliding interfaces.Electrical-stimulation-responsive intelligent lubricants provide a new technical support for realizing intelligent stepless control of devices.

关键词： solvent-free carbon spherical nanofluids(C-NFs) intelligent lubrication regulation lubrication performance adsorption film

Bioinspired metal-organic framework nanozyme reinforced with thermosensitive hydrogel for regulating inflammatory responses in Parkinson’s disease

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Nano Research 2024年第2期17卷 858-865页

作者： Xiaowan fan Tao zhang Xin Ding Yushuo Gu Qing li Wei Jiang Kelong fan Nanozyme Medical Center Academy of Medical ScienceZhengzhou UniversityZhengzhou 450001China Department Central-China Branch of National Center for Cardiovascular DiseasesHean Cardiovascular Disease CenterFuwai Central-China HospitalCentral China Fuwai Hospital of Zhengzhou UniversityZhengzhou 450046China Application Center for Precision Medicine the Second Affiliated Hospital of Zhengzhou UniversityZhengzhou 450052China CAS Engineering Laboratory for Nanozyme Key Laboratory of Protein and Peptide PharmaceuticalsInstitute of BiophysicsChinese Academy of SciencesBeijing 100101China University of Chinese Academy of Sciences Beijing 101408China Department of General Surgery Strategic Support Force Medical CenterBeijing 100101China Department of Anesthesiology Pain and Perioperative MedicineThe First Affiliated Hospital of Zhengzhou UniversityZhengzhou 450052China

Parkinson’s disease(PD)is a prevalent neurodegenerative disorder accompanied by movement disorders and neuroinflammatory injury.Anti-inflammatory intervention to regulate oxidative stress in the brain is beneficial for managing PD.However,traditional natural antioxidants have failed to meet the clinical treatment demands due to insufficient activity and sustainability.Herein,Cu-doping zeolite imidazolate framework-8(ZIF-8)nanozyme is designed to simulate Cu/Zn superoxide dismutase(SOD)by biomimetic mineralization.The nanozyme composite is then integrated into thermosensitive hydrogel(poly(lactic-co-glycolic acid)-poly(ethylene glycol)-poly(lactic-co-glycolic acid)(PLGA-PEG-PLGA))to form an effective antioxidant system(Cu-ZIF@Hydrogel).The thermosensitive hydrogel incorporating nanozymes demonstrate distinct viscoelastic properties aimed at enhancing local nanozyme adhesion,prolonging nanozyme retention time,and modulating antioxidant activity,thus significantly improving the bioavailability of nanozymes.At the cellular and animal levels of PD,we find that Cu-ZIF@Hydrogel bypass the blood-brain barrier and efficiently accumulate in the nerve cells.Moreover,the Cu-ZIF@Hydrogel significantly alleviate the PD’s behavioral and pathological symptoms by reducing the neuroinflammatory levels in the lesion site.Therefore,the hydrogel-incorporating nanozyme system holds great potential as a simple and reliable avenue for managing PD.

关键词： bioinspired nanozyme thermosensitive hydrogel Parkinson’s disease oxidative stress neuroinflammatory

Research on Performance Optimization of Spark Distributed Computing Platform

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Computers, Materials & Continua 2024年第5期79卷 2833-2850页

作者： Qinlu He fan zhang Genqing Bian Weiqi zhang Zhen li School of Information and Control Engineering Xi’an University of Architecture and TechnologyXi’an710054China Shaanxi Institute of Metrology Science Xi’an710043China

Spark,a distributed computing platform,has rapidly developed in the field of big data.Its in-memory computing feature reduces disk read overhead and shortens data processing time,making it have broad application prospects in large-scale computing applications such as machine learning and image processing.However,the performance of the Spark platform still needs to be improved.When a large number of tasks are processed simultaneously,Spark’s cache replacementmechanismcannot identify high-value data partitions,resulting inmemory resources not being fully utilized and affecting the performance of the Spark platform.To address the problem that Spark’s default cache replacement algorithm cannot accurately evaluate high-value data partitions,firstly the weight influence factors of data partitions are modeled and evaluated.Then,based on this weighted model,a cache replacement algorithm based on dynamic weighted data value is proposed,which takes into account hit rate and data difference.Better integration and usage strategies are implemented based on LRU(LeastRecentlyUsed).Theweight update algorithm updates the weight value when the data partition information changes,accurately measuring the importance of the partition in the current job;the cache removal algorithm clears partitions without useful values in the cache to releasememory resources;the weight replacement algorithm combines partition weights and partition information to replace RDD partitions when memory remaining space is insufficient.Finally,by setting up a Spark cluster environment,the algorithm proposed in this paper is experimentally verified.Experiments have shown that this algorithmcan effectively improve cache hit rate,enhance the performance of the platform,and reduce job execution time by 7.61%compared to existing improved algorithms.

关键词： Spark memory optimization memory replacement strategy

Kinetic and mechanism of the reaction between Cl and several mono-methyl branched alkanes

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Journal of Environmental Sciences 2024年第1期135卷 474-482页

作者： Yan Chen Weigang Wang Junling li li Zhou Bo Shi Cici fan Ke Wang Hao zhang Hong li Maofa Ge State Key Laboratory for Structural Chemistry of Unstable and Stable Species Beijing National Laboratory for Molecular Sciences(BNLMS)CAS Research/Education Center for Excellence in Molecular SciencesInstitute of ChemistryChinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China State Key Laboratory of Environmental Criteria and Risk Assessment Chinese Research Academy of Environmental SciencesBeijing 100012China National Engineering Research Center for Flue Gas Desulfurization Department of Environmental Science and EngineeringSichuan UniversityChengdu 610065China College of Chemistry and Materials Science Hebei Normal UniversityShijiazhuang 050024China

Branched alkanes are ubiquitous in the troposphere and play an important role in the chemical processes.In this work,the rate constants and products for the reaction of Cl atoms with 3-methylhexane and 2-methylheptane were measured at room temperature(298±0.2K)and atmospheric pressure using a conventional relative rate method.The rate constants of 3-methylhexane and 2-methylheptane in units of cm~3/(mol·sec)are(3.09±0.31)×10^(-10)and(3.67±0.40)×10^(-10),respectively.Furthermore,the corresponding atmospheric lifetime of the studied branched alkanes with Cl was 6.92-89.90 hours and 5.82-75.69 hours,respectively.The estimated atmospheric lifetimes indicated that the reaction with Cl atoms could be the most important atmospheric degradation pathway for 3-methylhexane and2-methylheptane.Primary gas-phase products of the reactions were identified and quantified,and particle-phase products were also obtained.The atmosphere oxidation mechanism of Cl atoms with 3-methylhexane and 2-methylheptane is proposed.The SOA yields of 3-methylhexane and 2-methylheptane from the reaction of Cl atoms were determined to be7.96%±0.89%and 13.35%±1.50%respectively.Overall,the results reveal that the primary loss process of branched alkanes is the reaction with Cl atoms,which impacts its degradation on a regional scale.

关键词： 3-Methylhexane 2-Methylheptane Chlorine atoms Kinetics Mechanism

PURP: A Scalable System for Predicting Short-Term Urban TrafficFlow Based on license Plate Recognition Data

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Big Data Mining and Analytics 2024年第1期7卷 171-187页

作者： Shan zhang Qinkai Jiang Hao li Bin Cao Jing fan School of Computer Science and Technology Zhejiang University of TechnologyHangzhou 310000China

Accurate and efficient urban traffic flow prediction can help drivers identify road traffic conditions in real-time,consequently helping them avoid congestion and accidents to a certain extent.However,the existing methods for real-time urban traffic flow prediction focus on improving the model prediction accuracy or efficiency while ignoring the training efficiency,which results in a prediction system that lacks the scalability to integrate real-time traffic flow into the training procedure.To conduct accurate and real-time urban traffic flow prediction while considering the latest historical data and avoiding time-consuming online retraining,herein,we propose a scalable system for Predicting short-term URban traffic flow in real-time based on license Plate recognition data(PURP).First,to ensure prediction accuracy,PURP constructs the spatio-temporal contexts of traffic flow prediction from license Plate Recognition(LPR)data as effective characteristics.Subsequently,to utilize the recent data without retraining the model online,PURP uses the nonparametric method k-Nearest Neighbor(namely KNN)as the prediction framework because the KNN can efficiently identify the top-k most similar spatio-temporal contexts and make predictions based on these contexts without time-consuming model retraining online.The experimental results show that PURP retains strong prediction efficiency as the prediction period increases.

关键词： traffic flow prediction k-Nearest Neighbor(KNN) license Plate Recognition(LPR)data spatio-temporalcontext