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Stereoselective synthesis of substituted 1,3-dienes from propargylic esters: electrophilic-metal or redox catalysis?

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Science China Chemistry 2024年第5期67卷 1384-1396页

作者： Mengfu Dai liangliang song liang-An Chen Jiangsu Collaborative Innovation Center of Biomedical Functional Materials Jiangsu Key Laboratory of New Power BatteriesSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources International Innovation Center for Forest Chemicals and MaterialsCollege of Chemical EngineeringNanjing Forestry UniversityNanjing 210037China

1,3-Diene architectures are not only widely present in natural products, pharmaceuticals, and functional organic materials but also serve as versatile building blocks to furnish important functionalized molecules in synthetic chemistry due to conjugated repeating C=C units. Accordingly, various strategies to access substituted 1,3-dienes in a stereoselective manner have been developed. However, chemo-, regio-and stereoselective synthesis of highly substituted 1,3-dienes still remains elusive and challenging. Readily available propargylic esters have emerged as an appealing class of synthetic intermediates for accessing functionalized 1,3-dienes, especially challenging tri-or tetrasubstituted variants, via transition-metal catalysis, including electrophilic metal and redox neutral catalysis. This review, for the first time, systematically highlights recent advances in transitionmetal catalyzed synthesis of substituted 1,3-dienes from propargylic esters, discusses the mechanisms and synthetic utilities, and gives the remaining challenges and potential opportunities in this field.

关键词： 1 3-diene propargylic ester Lewis acid redox catalysis transition metal

Fine-grained grid computing model for Wi-Fi indoor localization in complex environments

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Journal of Electronic Science and Technology 2024年第1期22卷 42-52页

作者： Yan liang song Chen Xin Dong Tu Liu School of Computer Engineering Chengdu Technological UniversityChengdu611730China HAN Networks Corporation Limited Beijing100094China

The fingerprinting-based approach using the wireless local area network(WLAN)is widely used for indoor ***,the construction of the fingerprint database is quite *** when the position of the access point(AP)or wall changes,updating the fingerprint database in real-time is *** appropriate indoor localization approach,which has a low implementation cost,excellent real-time performance,and high localization accuracy and fully considers complex indoor environment factors,is preferred in location-based services(LBSs)*** this paper,we proposed a fine-grained grid computing(FGGC)model to achieve decimeter-level localization *** points(RPs)are generated in the grid by the FGGC ***,the received signal strength(RSS)values at each RP are calculated with the attenuation factors,such as the frequency band,three-dimensional propagation distance,and walls in complex *** a result,the fingerprint database can be established automatically without manual measurement,and the efficiency and cost that the FGGC model takes for the fingerprint database are superior to previous *** proposed indoor localization approach,which estimates the position step by step from the approximate grid location to the fine-grained location,can achieve higher real-time performance and localization accuracy *** mean error of the proposed model is 0.36 m,far lower than that of previous ***,the proposed model is feasible to improve the efficiency and accuracy of Wi-Fi indoor *** also shows high-accuracy performance with a fast running speed even under a large-size *** results indicate that the proposed method can also be suitable for precise marketing,indoor navigation,and emergency rescue.

关键词： Fine-grained grid computing (FGGC) Indoor localization Path loss Random forest Reference points(RPs)

Surfactant-assisted crystallization of lysozyme and its mechanism

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Particuology 2024年第7期90卷 199-208页

作者： Yujie song Rongfei Ren Min Su Zhihan liang Qi Hao School of Chemical Engineering Hebei University of TechnologyTianjin 300130China

Surfactants were used to assist in the crystallization of *** types of surfactants with different structures(sodium dodecyl sulfate,cetyltrimethylammonium bromide,or betaine hydrochloride[BH])were *** study indicated that three surfactants were all capable of shortening the crystallization induction time of lysozyme,with BH inducing the shortest crystallization induction time(t=1 min)and the largest crystal size(37μm).The molecular interactions among each of the three surfactants aforementioned and lysozyme were also investigated by *** was found that hydrogen bonding dominantly acted between the carboxyl structure of the surfactant BH and the lysozyme,which produced the most favorable conformation for the self-assembly of lysozyme(promote lysozyme orderly aggregation and shorten the crystallization induction time).On this basis,the mechanism of surfactant-promoted lysozyme crystallization was proposed.

关键词： Protein Crystallization Surfactant Lysozyme Molecular interaction Mechanism

Heterobimetallic[NiCo]integration in a hydrogenase mimic for boosting light-driven hydrogen evolution in CaTiO_(3)

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Nano Research 2024年第8期17卷 6888-6894页

作者： Kang Li Juanji Hong Ningning song Zhanjun Guo Minmin liang Experimental Center of Advanced Materials School of Materials Science&EngineeringBeijing Institute of TechnologyBeijing 10081China

Light-drive hydrogen production using titanium-based perovskite is one sustainable way to reduce current reliance on fossil fuels,but its wide applications are still limited by high electron−hole recombination and sluggish surface ***,the developments for low-cost and highly efficient co-catalysts remain *** by natural[NiFe]-hydrogenase active center structure,a hydrogenase-mimic,NiCo_(2)S_(4) nanozyme was synthesized,and subsequently decorated onto the CaTiO_(3) to catalyze the hydrogen evolution reaction(HER).Among the following test,CaTiO_(3)with a 15%loading of NiCo_(2)S_(4) nanozyme exhibited the highest HER rate of 307.76μmol·g^(–1)·h^(–1),which is 60 times higher than that of the CaTiO_(3) *** results reveal that NiCo_(2)S_(4) not only significantly increased the charge separation efficiency of the photogenerated carriers,but also substantively lowered the HER activation *** studies show that NiCo_(2)S_(4) readily splits H_(2)O by forming the Ni(OH)-Co intermediate and only Ni in the bimetallic center alters the oxidation state during the HER process in a manner analogous to the[NiFe]-*** contrast to the often-expensive synthetic catalysts that rely on rare elements such as ruthenium and platinum,this study shows a promising way to develop the nature-inspired cocatalysts to enhance the photocatalysts’HER performance.

关键词： hydrogen evolution reaction hydrogenase-mimic nanozyme photocatalyst water-splitting

Identification of FIR systems under difference-driven scheduled quantized observations

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Control Theory and Technology 2024年第2期22卷 163-172页

作者： Dong liang Ruizhe Jia Fengwei Jing Yong song Jin Guo School of Automation and Electrical Engineering University of Science and Technology BeijingBeijing100083China Key Laboratory of Knowledge Automation for Industrial Processes Ministry of EducationBeijing100083China National Engineering Research Center for Advanced Rolling and Intelligent Manufacturing University of Science and Technology BeijingBeijing100083China

In networked system identification,how to effectively use communication resources and improve convergence speed is the focus of ***,there is an inherent contradiction between the two *** this paper,the event-driven communication is used to save communication resources for the identification of finite impulse response systems,and the input design is carried out to meet the requirements of convergence ***,a difference-driven communication is ***,the performance of the communication mechanism is analyzed,and the calculation method of its communication rate is *** that,according to the communication rate and the convergence rate of the identification algorithm,the input design problem is transformed into a constrained optimization problem,and the algorithm for finding the optimal solution is *** addition,considering the case that the output is quantized by multiple thresholds,the way to calculate its communication rate is given and the influence of threshold number on communication rate is ***,the effectiveness of the algorithm is verified by simulation.

关键词： System identification FIR system Difference-driven Quantized observation

Missing Value Imputation for Radar-Derived Time-Series Tracks of Aerial Targets Based on Improved Self-Attention-Based Network

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Computers, Materials & Continua 2024年第3期78卷 3349-3376页

作者： Zihao song Yan Zhou Wei Cheng Futai liang Chenhao Zhang Department of Early Warning Intelligence Early Warning AcademyWuhan430019China

The frequent missing values in radar-derived time-series tracks of aerial targets(RTT-AT)lead to significant challenges in subsequent data-driven ***,the majority of imputation research focuses on random missing(RM)that differs significantly from common missing patterns of *** method for solving the RM may experience performance degradation or failure when applied to RTT-AT *** autoregressive deep learning methods are prone to error accumulation and long-term dependency *** this paper,a non-autoregressive imputation model that addresses the issue of missing value imputation for two common missing patterns in RTT-AT is *** model consists of two probabilistic sparse diagonal masking self-attention(PSDMSA)units and a weight fusion *** learns missing values by combining the representations outputted by the two units,aiming to minimize the difference between the missing values and their actual *** PSDMSA units effectively capture temporal dependencies and attribute correlations between time steps,improving imputation *** weight fusion unit automatically updates the weights of the output representations from the two units to obtain a more accurate final *** experimental results indicate that,despite varying missing rates in the two missing patterns,our model consistently outperforms other methods in imputation performance and exhibits a low frequency of deviations in estimates for specific missing *** to the state-of-the-art autoregressive deep learning imputation model Bidirectional Recurrent Imputation for Time Series(BRITS),our proposed model reduces mean absolute error(MAE)by 31%~50%.Additionally,the model attains a training speed that is 4 to 8 times faster when compared to both BRITS and a standard Transformer model when trained on the same ***,the findings from the ablation experiments demonstrate that the PSDMSA,the weight fusion unit,cascade network design

关键词： Missing value imputation time-series tracks probabilistic sparsity diagonal masking self-attention weight fusion

Enhanced Flexoelectricity in Barium Titanate-Cellulose Composite Thin Films

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Acta Mechanica Solida Sinica 2024年第4期37卷 521-527页

作者： Wensi Xing Hongyu Cao Xin Zhang Xu liang Jianwei song Shengping Shen Chemomechanics and Intelligent Media Laboratory State Key Laboratory for Strength and Vibration of Mechanical StructuresSchool of Aerospace EngineeringXi’an Jiaotong UniversityXi’an710049China

Biopolymers,the potential flexoelectric materials,are environment-friendly,degradable,lightweight,cost-effective,and possess remarkable processing properties catering to the requirements of advanced ***,the flexoelectric coefficient of biopolymers is normally much weaker than that of ceramic materials,limiting their potential applications for designing high-performance green electromechanical coupling *** improve the flexoelectric response in biopolymers,we composited barium titanate(BTO)with 2,2,6,6-tetramethylpiperidine-1-oxyl-oxidized cellulose nanofibrils(TOCNF)to enhance the flexoelectric response of *** to the high permittivity and flexoelectric effect of BTO,the relative dielectric constant and flexoelectric coefficient of 33.3 wt%BTO-TOCNF films reached 30.94@1 kHz and 50.05±1.88 nC/m@1 Hz,which were almost 172 times and 27 times higher than those of TOCNF,*** composite thin film contains high dielectric constant and flexoelectric coefficient,as well as excellent *** study provided a straightforward and efficient method for improving the flexoelectric effect of biopolymers,and demonstrated its great potential applications in flexoelectric-based devices.

关键词： Flexoelectricity Cellulose BaTiO_(3) Composite Thin films

Boron nitride nanofibers enhanced composite PEO-based solid-state polymer electrolytes for lithium metal batteries

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Chinese Chemical Letters 2024年第6期35卷 216-221页

作者： Qianqian song Yunting Zhang Jianli liang Si Liu Jian Zhu Xingbin Yan School of Materials Science and Engineering Sun Yat-Sen UniversityGuangzhou 510275China College of Physics and Materials Science Tianjin Normal UniversityTianjin 300387China Department of Chemistry&Center of Super-Diamond and Advanced Films(COSDAF) City University of Hong KongHong Kong 999077China Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology School of Physics and Optoelectronic EngineeringFoshan UniversityFoshan 528225China

Polyethylene oxide(PEO)-based solid-state polymer electrolytes(SPEs)are limited by their poor cyclic stability and inferior ionic conductivity for applicating in high-safety,long-cycling and high-energy-density lithium metal ***,porous boron nitride nanofibers(BNNFs)are filled into PEO-based SPE,which significantly suppresses Li dendrites growth and enhances the electrochemical performance of Li metal *** with high porosity have more active sites to connect with PEO,which can effectively reduce the crystallinity of the PEO matrix and enhance its ionic ***,owing to the hardness and good stability of BNNFs,BNNFs/PEO/Li TFSI electrolyte exhibits a wider electrochemical window,better mechanical property and higher thermal stability compared with PEO/Li TFSI ***,the Li symmetric cell composed of 1%BNNFs/PEO/Li TFSI performs good cyclic stability(>1800 h),and the Li||1%BNNFs/PEO/Li TFSI||LFP full battery shows obviously improved performances in charge-discharge polarization voltage,discharge specific capacity,rate performance and cyclic stability than the Li||PEO/Li TFSI||LFP battery.

关键词： Solid-state polymer electrolyte Boron nitride nanofibers Lithium metal battery Ionic conductivity Li dendrite

Catalytic behavior of Mo-Bi-Fe-Co-K-M-O(M=Ce,Gd,CeGd)catalysts for selective oxidation of isobutene

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Journal of Rare Earths 2024年第1期42卷 84-93,I0003页

作者： Qinghui Li Huahua Zhao Jian Yang Jun Zhao liang Yan Huanling song Lingjun Chou State Key Laboratory for Oxo Synthesis and Selective Oxidation Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou730000China University of Chinese Academy of Sciences Beijing100049China

The further improvement of methacrolein(MAL)selectivity from isobutene(IB)oxidation is crucial and *** this study,based on the typical Mo-Bi-Fe-Co-K-O mixed metal oxide,the rare earth element Gd-doped,Ce-doped and CeGd co-doped catalysts were prepared by co-precipitation strategy to increase the selectivity of MAL from 47.9%to 49.8%,64.2% and 68.6%,*** order to elucidate in-depth the promoting effect of Ce and/or Gd,various characterizations were utilized including X-ray diffraction patterns(XRD),Raman,X-ray fluorescence spectrometry(XRF),X-ray photoelectron spectroscopy(XPS),O_(2)-temperature programmed desorption(O_(2)-TPD),H2-temperature programmed reduction(H2-TPR),CO_(2)-temperature programmed desorption(CO_(2)-TPD),IB-temperature programmed desorption(i-C4-TPD)and in-situ IB-Fourier transform infrared spectroscopy(IB-FTIR).Both Ce and Gd finely regulate the bulk and surface structure of the catalyst,thus altering the redox ability,oxygen mobility and storage ability and *** with Ce,Gd addition slightly regulates the variation of Co^(2+)/Co^(3+)redox couples,greatly enhances the interaction among the components on the catalyst,thus only increases the content of surface oxygen species and has little effect on their *** Cecontaining catalyst performs stronger oxygen storage and migration ability,thus leading to the overproduction of surface Odefectspecies,which are proposed to be the active sites for the production of MAL and *** CeGd co-doped catalyst possesses the proper content of surface Odefectspecies,thus exhibits much higher MAL ***,the promoting mechanism of Ce and/or Gd over IB oxidation is ***,this work is helpful for understanding the influence of rare earth elements on the structure of mixed metal oxides and the olefin selective oxidation reaction.

关键词： Mixed metal oxide catalyst Rare earth element Isobutene Selective oxidation Methacrolein