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Synergistic silver-mediated and palladium-catalyzed nondirected olefination of aryl C–H bond: quick access to multi-substituted aryl olefins

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Science China Chemistry 2024年第3期67卷 882-889页

作者： jian Yao Lili Shao Xiaohong Huo Xiaoming Wang Shanghai Key Laboratory for Molecular Engineering of Chiral Drugs Frontiers Science Center for Transformative MoleculesSchool of Chemistry and Chemical EngineeringShanghai Jiao Tong UniversityShanghai 200240China State Key Laboratory of Organometallic Chemistry Center for Excellence in Molecular SynthesisShanghai Institute of Organic ChemistryChinese Academy of SciencesShanghai 20032China School of Chemistry and Materials Science Hangzhou Institute for Advanced StudyUniversity of Chinese Academy of SciencesHangzhou 310024China

Transition metal-catalyzed olefination of aryl C-H bond is a powerful tool for the synthesis of alkenes. While the Pd-catalyzed oxidative C-H olefination of arenes, also known as Fujiwara-Moritani reaction, has been established as one of the most efficient methods, the substrates are largely limited to terminal olefins with electron-withdrawing group(s). Herein, we report a synergistic silver-mediated and palladium-catalyzed non-directed C-H olefination of arenes with vinyl(pseudo)halides, which offers a complementary strategy to the typical Fujiwara-Moritani reaction. The reactions proceeded well for a variety of halogenated arenes, heteroarenes, and olefin substrates, providing an efficient access to various multi-substituted aryl olefins, including trisubstituted/tetrasubstituted olefins and several complex olefins derived from medicines or natural products. Mechanistic studies indicated a bimetallic Pd/Ag cooperation is operative in the catalysis, i.e., the reaction is initiated by aryl C-H bond cleavage via ligation with phosphine/Ag species, followed by transferring of the aryl moiety to a vinyl palladium intermediate,which is in turn formed by oxidative addition of vinyl(pseudo)halide to a Pd complex. This method enables the synthesis of a wide range of challenging multi-substituted vinyl products from simple arenes(directing-group free) in a streamlined and controllable fashion.

关键词： direct C–H olefination multi-substituted aryl alkenes bimetallic Pd/Ag cooperation C–H functionalization

ON THE SOBOLEV DOLBEAULT COHOMOLOGY OF A DOMAIN WITH PSEUDOCONCAVE BOUNDARIES

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Acta Mathematica Scientia 2024年第2期44卷 431-444页

作者：陈健 School of Mathematics and Statistics Wuhan UniversityWuhan430072China

In this note,we mainly make use of a method devised by Shaw[15]for studying Sobolev Dolbeault cohomologies of a pseudoconcave domain of the type Ω=Ω\∪_(j=1^(m))Ω_(j),where Ω and {Ω_(j)}_(j=1^(m)■Ω are bounded pseudoconvex domains in ℂ^(n) with smooth boundaries,and Ω_(1),…,Ω_(m) are mutually *** main results can also be quickly obtained by virtue of[5].

关键词： Cauchy-Riemann equations pseudoconcave domains δ-Neumann operator Bergman spaces

Force-position collaborative optimization of rope-driven snake manipulator for capturing non-cooperative space targets

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Chinese Journal of Aeronautics 2024年第9期37卷 369-384页

作者： Xiaofeng LI jian TIAN Cheng WEI Xibin CAO School of Astronautics Harbin Institute of TechnologyHarbin 150001China Beijing Instiuteof Spacecraft System Engineering China Academy of Space TechnolgyBeijing 100094Chia

With the rapid development of space activities,non-cooperative space targets increase swiftly,such as failed satellites and upper stages,threating normal spacecrafts *** there are some problems in the capture process,such as excessive collision and fast tumbling of targets,manipulator with redundant Degrees of Freedom(DOFs)can be used to improve the compliance and therefore solve these *** Rope-Driven Snake Manipulator(RDSM)is a combina-tion of hyper-redundant DOFs and better compliance,and therefore it is suitable for capturing *** this paper,a snake manipulator mechanism is designed,and the complete kinematic model and system dynamic model considering RDSM,target and contact is ***,to obtain the configuration of joint with hyper-redundant DOFs,an improved motion dexterity index is pro-posed as the joint motion optimization ***,the force-position collaborative optimization index is designed to adjust active stiffness,and the impedance control method based on the modified index is used to capture the space ***,the proposed force-position collaborative opti-mization method is verified by virtual prototype *** results demonstrate that based on the proposed method,the collision force is reduced by about 25%compared to normal impe-dance control,showing higher safety.

关键词： Capturing non-cooperative spacetargets Rope-driven snakemanipu-lator Force-position collaborative optimization Redundant degrees of free-dom Active stiffness adjustment

NAD(P)H inspired CO_(2) reduction and beyond

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Science China Chemistry 2024年第4期67卷 1044-1046页

作者： Wenjin Dong jian Liu Qingdao Institute of Bioenergy and Bioprocess Technology Chinese Academy of SciencesShandong Energy InstituteQingdao 266101China

The catalytic reduction of carbon dioxide to fuels and valueadded chemicals under mild conditions is recognized as a promising strategy to alleviate the energy *** the Calvin cycle of natural photosynthesis,CO_(2)reduction is achieved using cofactor nicotinamide adenine dinucleotide phosphate(NADPH)as a practical catalyst,shedding light on the biomimetic metal-free reduction of CO_(2).

关键词： dioxide dinucleotide catalyst

Physical neural networks with self-learning capabilities

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Science China(Physics,Mechanics & Astronomy) 2024年第8期67卷 23-42页

作者： Weichao Yu Hangwen Guo jiang Xiao jian Shen State Key Laboratory of Surface Physics and Institute for Nanoelectronic Devices and Quantum Computing Fudan UniversityShanghai 200433China Zhangjiang Fudan International Innovation Center Fudan UniversityShanghai 201210China Department of Physics Fudan UniversityShanghai 200433China Shanghai Research Center for Quantum Sciences Shanghai 201315China Collaborative Innovation Center of Advanced Microstructures Nanjing 210093China

Physical neural networks are artificial neural networks that mimic synapses and neurons using physical systems or *** networks harness the distinctive characteristics of physical systems to carry out computations effectively,potentially surpassing the constraints of conventional digital neural networks.A recent advancement known as“physical self-learning”aims to achieve learning through intrinsic physical processes rather than relying on external *** article offers a comprehensive review of the progress made in implementing physical self-learning across various physical *** learning strategies that contribute to the realization of physical self-learning are *** challenges in understanding the fundamental mechanism of learning,this work highlights the progress towards constructing intelligent hardware from the ground up,incorporating embedded self-organizing and self-adaptive dynamics in physical systems.

关键词： self-learning physical neural networks neuromorphic computing physical learning

Data-Driven Active Disturbance Rejection Control of Plant-Protection Unmanned Ground Vehicle Prototype: A Fuzzy Indirect Iterative Learning Approach

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IEEE/CAA Journal of Automatica Sinica 2024年第8期11卷 1892-1894页

作者： Tao Chen Ruiyuan Zhao jian Chen Zichao Zhang College of Engineering China Agricultural UniversityBeijing 100083China Key Laboratory of Smart Agricultural Technology in Tropical South China Ministry of Agriculture and Rural AffairsGuangzhou 510642China

Dear Editor,This letter proposes a fuzzy indirect iterative learning(FIIL)active disturbance rejection control(ADRC)scheme to address the impact of uncertain factors of plant-protection unmanned ground vehicle(UGV),in which ADRC is a data-driven model-free control algorithm that only relies on the input and output data of the *** on the established nonlinear time-varying dynamic model including dynamic load(medicine box),the FIIL technology is adopted to turn the bandwidth and control channel gain online,in which the fuzzy logic system is used to update the gain parameters of iterative learning in real *** and experiment show the FIIL-ADRC scheme has better control performance.

关键词： Active scheme iterative

Impact of initial fluctuations and nuclear deformations in isobar collisions

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Nuclear Science and Techniques 2024年第6期35卷 155-162页

作者： jian-Fei Wang Hao-Jie Xu Fu-Qiang Wang Department of Modern Physics University of Science and Technology of ChinaHefei 230026China School of Science Huzhou UniversityHuzhou 313000China Strong-Coupling Physics International Research Laboratory(SPiRL) Huzhou UniversityHuzhou 313000China Department of Physics and Astronomy Purdue UniversityWest LafayetteIN 47907USA

Relativistic isobar^(96)_(44)Ru+^(96)_(44)Ru and^(96)_(40)Zr+^(96)_(40)Zrcollisions have revealed intricate differences in their nuclear size and shape,inspiring unconventional studies of nuclear structure using relativistic heavy ion *** this study,we investigate the relative differences in the mean multiplicityR_()and the secondR_(ε2)and third-order eccentricityR_(ε3)between isobar collisions using initial state Glauber *** is found that initial fluctuations and nuclear deformations have negligible effects on R_()in most central collisions,while both are important for the R_(ε2)and R_(ε3),the degree of which is sensitive to the underlying nucleonic or sub-nucleonic degree of *** features,compared to real data,may probe the particle production mechanism and the physics underlying nuclear structure.

关键词： Relativistic isobar collisions Initial fluctuations Nuclear deformation

Automatic modulation recognition of radio fuzes using a DR2D-based adaptive denoising method and textural feature extraction

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Defence Technology（防务技术） 2024年第4期34卷 328-338页

作者： Yangtian Liu Xiaopeng Yan Qiang Liu Tai An jian Dai Science and Technology on Electromechanical Dynamic Control Laboratory School of Mechatronical EngineeringBeijing Institute of TechnologyBeijing 100081China China Research and Development Academy of Machinery Equipment Beijing 100089China

The identification of intercepted radio fuze modulation types is a prerequisite for decision-making in interference ***,the electromagnetic environment of modern battlefields is complex,and the signal-to-noise ratio(SNR)of such environments is usually low,which makes it difficult to implement accurate recognition of radio *** solve the above problem,a radio fuze automatic modulation recognition(AMR)method for low-SNR environments is ***,an adaptive denoising algorithm based on data rearrangement and the two-dimensional(2D)fast Fourier transform(FFT)(DR2D)is used to reduce the noise of the intercepted radio fuze intermediate frequency(IF)***,the textural features of the denoised IF signal rearranged data matrix are extracted from the statistical indicator vectors of gray-level cooccurrence matrices(GLCMs),and support vector machines(SVMs)are used for *** DR2D-based adaptive denoising algorithm achieves an average correlation coefficient of more than 0.76 for ten fuze types under SNRs of-10 d B and above,which is higher than that of other typical *** trained SVM classification model achieves an average recognition accuracy of more than 96%on seven modulation types and recognition accuracies of more than 94%on each modulation type under SNRs of-12 d B and above,which represents a good AMR performance of radio fuzes under low SNRs.

关键词： Automatic modulation recognition Adaptive denoising Data rearrangement and the 2D FFT(DR2D) Radio fuze

The reaction mechanism and interfacial crystallization of Al nanoparticle-embedded Ni under shock loading

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Defence Technology（防务技术） 2024年第3期33卷 114-124页

作者： Yifan Xie jian-Li Shao Rui Liu Pengwan Chen State Key Laboratory of Explosion Science and Technology Beijing Institute of TechnologyBeijing100081China Explosion Protection and Emergency Disposal Technology Engineering Research Center of the Ministry of Education Beijing100039China

The shock-induced reaction mechanism and characteristics of Ni/Al system,considering an Al nanoparticle-embedded Ni single crystal,are investigated through molecular dynamics *** the shock melting of Al nanoparticle,interfacial crystallization and dissolution are the main *** reaction degree of Al particle first increases linearly and then logarithmically with time driven by rapid mechanical mixing and following *** reaction rate increases with the decrease of particle diameter,however,the reaction is seriously hindered by interfacial crystallization when the diameter is lower than 9 nm in our ***,we found a negative exponential growth in the fraction of crystallized Al atoms,and the crystallinity of B2-NiAl(up to 20%)is positively correlated with the specific surface area of Al *** can be attributed to the formation mechanism of B2-NiAl by structural evolution of finite mixing layer near the collapsed *** shock melting of both Al particle and Ni matrix,the liquid-liquid phase inter-diffusion is the main reaction mechanism that can be enhanced by the formation of internal *** addition,the enhanced diffusion is manifested in the logarithmic growth law of mean square displacement,which results in an almost constant reaction rate similar to the mechanical mixing process.

关键词： Shock-induced reaction Molecular dynamics simulations Interfacial crystallization Reaction mechanism