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Spin effect on redox acceleration and regioselectivity in Fe-catalyzed alkyne hydrosilylation

National Science Review 2024年第2期11卷 155-167页

作者： Peng He Meng-Yang Hu Jin-Hong Li Tian-Zhang Qiao yi-Lin Lu Shou-fei zhu Frontiers Science Center for New Organic Matter State Key Laboratory and Institute of Elemento-Organic Chemistry Nankai University

Iron catalysts are ideal transition metal catalysts because of the Earths abundant, cheap, biocompatible features of iron salts. Iron catalysts often have unique open-shell structures that easily undergo spin crossover in chemical transformations, a feature rarely found in noble metal catalysts. Unfortunately, little is known currently about how the open-shell structure and spin crossover affect the reactivity and selectivity of iron catalysts, which makes the development of iron catalysts a low efficient trial-and-error program. In this paper, a combination of experiments and theoretical calculations revealed that the iron-catalyzed hydrosilylation of alkynes is typical spin-crossover catalysis. Deep insight into the electronic structures of a set of well-defined open-shell active formal Fe(0) catalysts revealed that the spin-delocalization between the iron center and the 1,10-phenanthroline ligand effectively regulates the iron center's spin and oxidation state to meet the opposite electrostatic requirements of oxidative addition and reductive elimination, respectively,and the spin crossover is essential for this electron transfer process. The triplet transition state was essential for achieving high regioselectivity through tuning the nonbonding interactions. These findings provide an important reference for understanding the effect of catalyst spin state on reaction. It is inspiring for the development of iron catalysts and other Earth-abundant metal catalysts, especially from the point of view of ligand development.

关键词： spin effect spin-delocalization spin crossover iron-catalysis alkyne hydrosilylation

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Effect of rare earth on primary carbides in H13 die steel and their addition method:a review

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Journal of Iron and Steel Research(International) 2024年第3期31卷 531-551页

作者： Jing-feng Wang Lin-zhu Wang Chao-yi Chen Xiang Wang fei Zhao School of Materials and Metallurgy Guizhou UniversityGuiyang 550025GuizhouChina Zhengzhou Railway Vocational and Technical College Zhengzhou 450000HenanChina Guizhou Provincial University Key Laboratory of High Performance Battery Materials Guizhou UniversityGuiyang 550025GuizhouChina Shougang Guiyang Special Steel Co. Guiyang 550005GuizhouChina

Larger-sized primary carbides lead to stress concentration during the application of H13 hot-work die steel,resulting in microcracks and fatigue failure.Rare earth was usually added to modify the carbides and inclusions.The existing literature is reviewed on the effect of rare earth on primary carbides in H13 steel.A comprehensive review on the effect of rare earth on the characteristics of primary carbides,i.e.,number,size,morphology,and thermal stability in H13 steel,was done.The precipitation mechanism and nucleation of primary carbides with rare earth were summarized.The position and form of rare earth in steel and their effects on alloying elements segregation were reviewed.The addition techniques of rare earth in H13 steel were compared,and the prospects for other uncommon rare earth and emerging technology were present.Based on the current references,it can be known that adding rare earth facilitated refined and dispersed primary carbides.The size of primary carbides would be reduced,and their morphology would be improved because the rare earth inclusions formed in H13 steel can act as nucleation cores forγ-Fe orδ-Fe,refining the dendritic structure.Besides,the number of primary carbides at grain boundaries would be significantly reduced.However,rare earth had little impact on thermal stability.The nucleation of primary carbides tended to be inhibited due to the modification of inclusions by rare earth which were likely to be nucleation cores for primary carbides.Rare earth had been reported to affect the mechanism and process of primary carbide precipitation.Additionally,the addition of rare earth can inhibit the segregation of alloying elements and carbon diffusion by calculation.Thus,laboratory experiments and theoretical calcu-lations need to be conducted to study the states and evolution of rare earth steels.

关键词： Rare earth H13 die steel Primary carbide Nucleation Dendritic structure

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Self-assembly of perovskite nanocrystals:From driving forces to applications

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Journal of Energy Chemistry 2024年第1期88卷 561-578,I0013页

作者： yi Li fei Zhang School of Chemical Engineering and Technology Tianjin UniversityTianjin 300072China Collaborative Innovation Center of Chemical Science and Engineering(Tianjin) Tianjin 300072China

Self-assembly of metal halide perovskite nanocrystals(NCs)into superlattices can exhibit unique collective properties,which have significant application values in the display,detector,and solar cell field.This review discusses the driving forces behind the self-assembly process of perovskite NCs,and the commonly used self-assembly methods and different self-assembly structures are detailed.Subsequently,we summarize the collective optoelectronic properties and application areas of perovskite superlattice structures.Finally,we conclude with an outlook on the potential issues and future challenges in developing perovskite NCs.

关键词： Self-assembly Metal halide perovskite Nanocrystals Driving forces

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Collembolans maintain a core microbiome responding to diverse soil ecosystems

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Soil Ecology Letters 2024年第1期6卷 33-46页

作者： Zhe-Lun Liu Dong zhu yi-fei Wang Yong-Guan zhu Min Qiao State Key Laboratory of Urban and Regional Ecology Research Center for Eco-Environmental SciencesChinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China Key Lab of Urban Environment and Health Institute of Urban EnvironmentChinese Academy of SciencesXiamen 361021China

The unique gut habitat led to a core intestinal micro-biome in diverse soil ecosystems.The collembolan guts may help eliminate soil pathogens.Host-selection carried more weight on community assembly of gut microbiome.Soil invertebrates are widely distributed in the ecosystem and are essential for soil ecological processes.Inverte-brate gut microbiome plays an important role in host health and has been considered as a hidden microbial repository.However,little is known about how gut microbiome in soil invertebrates respond to diverse soil ecosystems.Based on a laboratory microcosm experiment,we characterized the assembling of microbiome of soil collembolans(Folsomia candida)from six representative regions of the soil ecosystem which they inhabit.Results showed that collembolan gut microbial communities differed significantly from their surrounding soil microbial communities.A dominant core gut microbiome was identified in gut habitat.Community analyses indicated that deterministic process dominated in the community assembly of collembolan gut microbiome.The results further demonstrate a dominant contribution of host selection in shaping gut microbiome.It is also worthy to mention that pathogens,such as common agricultural phytopathogenic fungi Fusarium,were involved in core microbiome,indicating that collembolans could act as vectors of pathogens.Our results unravelled the existence of gut core microbiome of collembolans in soil ecosystems and provided new insights for under-standing the crucial role of gut microbiome of soil fauna in maintaining microbial biodiversity and stability of soil ecosystems.

关键词： gut microbiome collembolan core microbiome community assembly

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6DOF pose estimation of a 3D rigid object based on edge-enhanced point pair features

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Computational Visual Media 2024年第1期10卷 61-77页

作者： Chenyi Liu fei Chen Lu Deng Renjiao yi Lintao Zheng Chenyang zhu Jia Wang Kai Xu College of Computing National University of Defense TechnologyChangsha410073China Department of Spine Surgery the Second Xiangya HospitalCentral South UniversityChangsha410011China Clinical Nursing Teaching and Research Section the Second Xiangya HospitalChangsha410011China College of Meteorology and Oceanography National University of Defense TechnologyChangsha410073China Beijing Institute of Tracking and Communication Technology Beijing100094China

The point pair feature(PPF)is widely used for 6D pose estimation.In this paper,we propose an efficient 6D pose estimation method based on the PPF framework.We introduce a well-targeted down-sampling strategy that focuses on edge areas for efficient feature extraction for complex geometry.A pose hypothesis validation approach is proposed to resolve ambiguity due to symmetry by calculating the edge matching degree.We perform evaluations on two challenging datasets and one real-world collected dataset,demonstrating the superiority of our method for pose estimation for geometrically complex,occluded,symmetrical objects.We further validate our method by applying it to simulated punctures.

关键词： point pair feature(PPF) pose estimation object recognition 3D point cloud

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Elliptical encirclement control capable of reinforcing performances for UAVs around a dynamic target

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Defence Technology（防务技术） 2024年第2期32卷 104-119页

作者： fei Zhang Xingling Shao yi Xia Wendong Zhang National Key Laboratory for Electronic Measurement Technology School of Instrument and ElectronicsNorth University of ChinaTaiyuan030051China

Most researches associated with target encircling control are focused on moving along a circular orbit under an ideal environment free from external disturbances.However,elliptical encirclement with a time-varying observation radius,may permit a more flexible and high-efficacy enclosing solution,whilst the non-orthogonal property between axial and tangential speed components,non-ignorable environmental perturbations,and strict assignment requirements empower elliptical encircling control to be more challenging,and the relevant investigations are still open.Following this line,an appointed-time elliptical encircling control rule capable of reinforcing circumnavigation performances is developed to enable Unmanned Aerial Vehicles(UAVs)to move along a specified elliptical path within a predetermined reaching time.The remarkable merits of the designed strategy are that the relative distance controlling error can be guaranteed to evolve within specified regions with a designer-specified convergence behavior.Meanwhile,wind perturbations can be online counteracted based on an unknown system dynamics estimator(USDE)with only one regulating parameter and high computational efficiency.Lyapunov tool demonstrates that all involved error variables are ultimately limited,and simulations are implemented to confirm the usability of the suggested control algorithm.

关键词： Elliptical encirclement Reinforced performances Wind perturbations UAVs

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Deep-reinforcement-learning-based UAV autonomous navigation and collision avoidance in unknown environments

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Chinese Journal of Aeronautics 2024年第3期37卷 237-257页

作者： fei WANG Xiaoping zhu Zhou ZHOU Yang TANG School of Astronautics Northwestern Polytechnical UniversityXi’an 710072China School of Aeronautics Northwestern Polytechnical UniversityXi’an 710072China

In some military application scenarios,Unmanned Aerial Vehicles(UAVs)need to perform missions with the assistance of on-board cameras when radar is not available and communication is interrupted,which brings challenges for UAV autonomous navigation and collision avoidance.In this paper,an improved deep-reinforcement-learning algorithm,Deep Q-Network with a Faster R-CNN model and a Data Deposit Mechanism(FRDDM-DQN),is proposed.A Faster R-CNN model(FR)is introduced and optimized to obtain the ability to extract obstacle information from images,and a new replay memory Data Deposit Mechanism(DDM)is designed to train an agent with a better performance.During training,a two-part training approach is used to reduce the time spent on training as well as retraining when the scenario changes.In order to verify the performance of the proposed method,a series of experiments,including training experiments,test experiments,and typical episodes experiments,is conducted in a 3D simulation environment.Experimental results show that the agent trained by the proposed FRDDM-DQN has the ability to navigate autonomously and avoid collisions,and performs better compared to the FRDQN,FR-DDQN,FR-Dueling DQN,YOLO-based YDDM-DQN,and original FR outputbased FR-ODQN.

关键词： Faster R-CNN model Replay memory Data Deposit Mechanism(DDM) Two-part training approach Image-based Autonomous Navigation and Collision Avoidance(ANCA) Unmanned Aerial Vehicle(UAV)

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An electron-transfer[Fe_(2)Co_(2)]square complex exhibiting unprecedented wide room-temperature hysteresis

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Science China Chemistry 2024年第4期67卷 1198-1207页

作者： Xin-Hua Zhao yi-fei Deng Jia-Tao Chen Jiong Yang Yuan-zhu Zhang Department of Chemistry Southern University of Science and Technology(SUSTech)Shenzhen 518055China

Switchable molecules with magnetic bistability that can function at standard conditions are highly desirable from the perspective of practical applications.Over the last decade,significant progress has been made in modulating thermally induced electrontransfer-coupled spin transition(ETCST)events between diamagnetic{Fe_(LS)^(Ⅱ)(μ-CN)Co_(LS)^(Ⅲ)}and paramagnetic{Fe_(LS)^(Ⅲ)(μ-CN)-Co_(HS)^(Ⅱ)}electron configurations(named LS and HS,respectively,for short)within the Fe/Co mixed-valence cyanometallate complexes.Herein,we prepared a novel[Fe_(2)Co_(2)]square complex[(pzTp)Fe(CN)_(3)Co(bnbpen)]_(2)[NO_(3)]_(2)·4CH_(3)OH·2.5H_(2)O(1·Solv)and its desolvated phase[(pzTp)Fe(CN)_(3)Co(bnbpen)]_(2)[NO_(3)]_(2)(1),obtained via single-crystal-to-single-crystal(SCSC)transformation.Complex 1·Solv remaining in the diamagnetic state below room temperature exhibits an irreversible ETCST behavior accompanied by desolvation upon heating.Notably,complex 1 displays an unprecedented rate-dependent ETCST behaviour involving with two diamagnetic LS states(a dynamically favoured LS1 state and a thermodynamically favoured LS2state),between which a net one-way transition from LS1 to LS2 is accessible likely via a structural phase transition(SPT)above255 K.Consequently,two well separated transition channels(HS?LS1 at around 255 K and HS←→LS2 in the temperature range of 317-350 K)are achieved according to either fast(>20 K/min)or slow rate(<1 K/min),respectively.At a moderate rate of 3 K/min,complex 1 shows a wide hysteresis of 66 K centered at 328 K,the largest yet reported for discrete Fe/Co cyanometallate complexes.Complex 1 represents the first ETCST example coupled with dynamic SPT,providing a new strategy for manipulating bistability within this fascinating cyanometallate family.

关键词： switchable molecules cyanometallate complexes electron transfer hysteresis structural phase transition

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Clinical efficacy of femtosecond laser-assisted phacoemulsification in diabetic cataract patients

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World Journal of Clinical Cases 2024年第10期12卷 1733-1741页

作者： yi-fei Tang Zhi-Hui Duan Department of Glaucoma and Cataracts Han Yang Eyegood Ophthalmic HospitalWuhan 430056Hubei ProvinceChina

BACKGROUND Diabetic patients with cataracts encounter specific difficulties during cataract surgery due to alterations in microcirculation,blood supply,metabolism,and the microenvironment.Traditional phacoemulsification may not fully tackle these issues,especially in instances with substantial preoperative astigmatism.The utilization of femtosecond laser-assisted phacoemulsification,in conjunction with Toric intraocular lens(IOL)implantation,offers a potentially more efficient strategy.This research seeks to evaluate the efficacy and possible complications of this approach in diabetic cataract patients.AIM To investigate the clinical efficacy and complications of femtosecond laser-assisted phacoemulsification combined with Toric IOL implantation in diabetic cataract patients,comparing it with traditional phacoemulsification methods.METHODS This retrospective study enrolled 120 patients with diabetes cataract from May 2019 to May 2021.The patients were divided into two groups:the control group underwent traditional phacoemulsification and Toric IOL implantation,while the treatment group received Len Sx femtosecond laser-assisted treatment.Outcome measures included naked eye vision,astigmatism,high-level ocular phase difference detection,clinical efficacy,and complication.RESULTS There were no significant preoperative differences in astigmatism or naked eyesight between the two groups.However,postoperative improvements were observed in both groups,with the treatment group showing greater enhancements in naked eye vision and astigmatism six months after the procedure.High-level corneal phase difference tests also indicated significant differences in favor of the treatment group.CONCLUSION This study suggests that femtosecond laser-assisted phacoemulsification combined with Toric IOL implantation appears to be more effective in enhancing postoperative vision in diabetic cataract patients compared to traditional methods offering valuable insights for clinical practice.

关键词： Diabetic cataract Femtosecond laser-assisted phacoemulsification Toric intraocular lens implantation Naked vision

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Phosphine-Catalyzed [4+3] Annulation Reaction of Indole Derivatives with MBH Carbonates:A Facile Access to Indole-1,2-fused 1,4-Diazepinones and Azepines

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Chinese Journal of Chemistry 2024年第3期42卷 271-275页

作者： Yannan zhu Haoran Jiang yi-Ning Wang Faculty of Chemistry and Chemical Engineering Yancheng Institute of TechnologyYanchengJiangsu224051 China

A phosphine-catalyzed [4+3] annulation between dinucleophilic indole derivatives and Morita−Baylis−Hillman (MBH) carbonates was discovered by using the N1 and N4′/C4′ nucleophilicities of the indole precursors,in which indoles act as four atom synthons. This protocol provides an efficient and facile access to indole-1,2-fused 1,4-diazepinones and azepines in good to high yields in one step,which illustrates potential synthetic utilities in drug discovery.

关键词： Phosphine catalysis [4+3]Annulation Indole derivatives Nitrogen heterocycles Organocatalysis

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