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Axial enantiomers with donor-regulated TADF feature for multicolor circularly polarized electroluminescence

Science China Chemistry 2024年第6期67卷 2039-2045页

作者： chen-Hao Guo wen-Long Zhao ke-ke Tan w.i-chen Guo Liheng Feng Chuan-Feng chen Meng Li School of Chemistry and Chemical Engineering Shanxi UniversityTaiyuan030006China Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Molecular Recognition and FunctionInstitute of ChemistryChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China

This study optimized the TADF feature of axial chiral enantiomers through precise donor engineering,and multicolor CP-TADFwas achieved in the axial chiral *** pairs of axial enantiomers with donor-regulated TADF feature,namely(R/S)-TPCBD,(R/S)-DPCBD,and(R/S)-DPACBD,were synthesized by introducing carbazole donors with different substituents onto biphenyl cyanide *** the electron-donating ability of donors increases,the emission of these axial enantiomers ranges from 455,476 to 552 nm,their singlet-triplet energy gaps(ΔE_(ST))gradually decrease from 0.30,0.22 to 0.02 e V,accompanied by an increasement in the transition rate(k_(RiSC))of RiSC process,and the k_(RiSC)of DPACBD could reach up to 7.16×10^(5)s^(-1).These axial enantiomers also exhibit mirror-image CD and circularly polarized luminescence(CPL)***,OLEDs based on TPCBD,DPCBD,and DPACBD as emitter were then fabricated,w.ich displayed blue,green,and orange electroluminescence with EQE_(max)of 13.0%,16.4%,and 25.0%,*** results also exhibited a phenomenon of device efficiency increasing with the enhancement of donor ***,the CP-OLEDs using(R/S)-TPCBD,(R/S)-DPCBD and(R/S)-DPACBD as emitters displayed intense CPEL signals with g_(EL)values of 3.4×10^(-3)/-4.1×10^(-3),3.2×10^(-3)/-3.1×10^(-3)and2.3×10^(-3)/-2.1×10^(-3),*** convenient molecular engineering of donor regulation in the same molecular skeleton,CP-TADF materials with multicolor CPEL and improved device performance could be conveniently achieved.

关键词： axial chirality thermally activated delayed fluorescence circularly polarized luminescence electroluminescence organic light-emitting diodes

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Atomically Dispersed Ruthenium Catalysts with Open Hollow Structure for Lithium-Oxygen Batteries

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Nano-Micro Letters 2024年第2期16卷 154-164页

作者： Xin chen Yu Zhang Chang chen Huinan Li Yuran Lin ke Yu Caiyun Nan chen chen Beijing Advanced innovation Center for Materials Genome Engineering Institute of Solid State ChemistryUniversity of Science and Technology BeijingBeijing 100083People’s Republic of China Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084People’s Republic of China Beijing key Laboratory of Energy Conversion and Storage Materials institution College of ChemistryBeijing Normal UniversityBeijing 100875People’s Republic of China

Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at ***,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen *** one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox *** the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic ***,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.

关键词： Atomically dispersed Open hollow structure Discharge product Lithium Oxygen battery

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Efficient nitrite-to-ammonia electroreduction over Zr-Ni frustrated Lewis acid-base pairs

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Science China Chemistry 2024年第5期67卷 1707-1714页

作者： Ying Zhang Zhuohang Li wenyu Du Kai chen ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrochemical NO_(2)~--to-NH_(3) conversion(NO_(2)RR) offers a green route to NH_(3) electrosynthesis, w.ile developing efficient NO_(2)RR catalysis systems at high current densities remains a grand challenge. Herein, we report an efficient Zr-NiO catalyst with atomically dispersed Zr-dopants incorporated in NiO lattice, delivering the exceptional NO_(2)RR performance with industriallevel current density(>0.2 A cm^(-2)). in situ spectroscopic measurements and theoretical simulations reveal the construction of ZrNi frustrated Lewis acid-base pairs(FLPs) on Zr-Ni O, w.ich can substantially increase the number of absorbed nitrite(NO_(2)~-),promote the activation and protonation of NO_(2)~- and concurrently hamper the H coverage, boosting the activity and selectivity of Zr-NiO towards the NO_(2)RR. Remarkably, Zr-NiO exhibits the exceptional performance in a flow cell with high Faradaic efficiency for NH_(3) of 94.0% and NH_(3)yield rate of 1,394.1 μmol h^(-1)cm^(-2) at an industrial-level current density of 228.2 m A cm^(-2),placing it among the best NO_(2)RR electrocatalysts for NH_(3) production.

关键词： electrochemical nitrite-to-ammonia conversion frustrated Lewis acid-base pairs(FLPs) in situ spectroscopy theoretical computations

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Lewis Base Catalyzed Selenofunctionalization of Alkynes with Acid-Controlled Divergent Chemoselectivity

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Chinese Journal of Chemistry 2024年第14期42卷 1623-1629页

作者： Ling-Ling chen Ren-Fei Cao Hua ke Zhi-Min chen School of Chemistry and Chemical Engineering Shanghai Key Laboratory for Molecular Engineering of Chiral DrugsShanghai Jiao Tong UniversityShanghai200240 China Engineering Technology Research Center for Environmental Protection Materials Pingxiang UniversityPingxiangJiangxi337055 China

Lewis base catalyzed and Brønsted acid controlled chemodivergent electrophilic selenofunctionalizations of alkynes were developed for the first *** selenium-containing tetrasubstituted alkenes were readily obtained in moderate to excellent yields with complete E/Z *** the substrates were 1-ethynyl naphthol derivatives,linear selenium-containing tetrasubstituted alkenes were produced via intermolecular oxygen nucleophilic attack in the absence of acid additive;in contrast,cyclic selenium-containing tetrasubstituted alkenes were generated through intramolecular carbon nucleophilic capture with the addition of Brønsted acid.

关键词： Alkynes Electrophilic addition Chemoselectivity Lewis base catalysis Selenofunctionalization

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Smart Contract Vulnerability Detection Method Based on Feature Graph and Multiple Attention Mechanisms

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Computers, Materials & Continua 2024年第5期79卷 3023-3045页

作者： Zhenxiang He Zhenyu Zhao ke chen Yanlin Liu School of Cyber Security Gansu University of Political Science and LawLanzhou730070China

The fast-paced development of blockchain technology is ***,the security concerns of smart contracts represent a significant challenge to the stability and dependability of the entire blockchain *** smart contract vulnerability detection primarily relies on static analysis tools,w.ich are less efficient and *** deep learning methods have improved detection efficiency,they are unable to fully utilize the static relationships within ***,we have adopted the advantages of the above two methods,combining feature extraction mode of tools with deep learning ***,we have constructed corresponding feature extraction mode for different vulnerabilities,w.ich are used to extract feature graphs from the source code of smart ***,the node features in feature graphs are fed into a graph convolutional neural network for training,and the edge features are processed using a method that combines attentionmechanismwith gated ***,the revised node features and edge features are concatenated through amulti-head *** result of the splicing is a global representation of the entire feature *** method was tested on three types of data:Timestamp vulnerabilities,reentrancy vulnerabilities,and access control vulnerabilities,where the F1 score of our method reaches 84.63%,92.55%,and 61.36%.The results indicate that our method surpasses most others in detecting smart contract vulnerabilities.

关键词： Blockchain smart contracts deep learning graph neural networks

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Effects of electrothermal ageing on dielectric performance of metallised biaxial orientation polypropylene film capacitors in strong magnetic fields

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High Voltage 2024年第4期9卷 911-919页

作者： Haoliang Liu Boxue Du Meng Xiao ke chen Yanw.i Ma School of Electrical and information Engineering Tianjin UniversityTianjinChina institute of Electrical Engineering Chinese Academy of SciencesBeijingChina

The dielectric performance of the pristine and the electrothermal-aged metallised polypropylene capacitors are investigated under different magnetic *** energy storage capacity decreases under the magnetic *** 12 T,the capacitance value of the pristine capacitors decreases by 8.4%-17%and that of the aged capacitors declines by 15%-20%.The dielectric loss is reduced by 2.6%-6.3%,but the equivalent series resistance shows an 8.3%-23.1%*** leakage conductivity increases to 202%-354%,w.ich leads to a weakened voltage holding *** addition to the effects of the magnetic fields,the impacts of ageing have also been *** effects of the magnetic field and ageing on the electrical parameters of the capacitors are discussed *** molecular chains of the dielectric are oxidised and decomposed during the ageing process,w.ich reduces the insulating properties of the *** magnetic field inhibits polarisation by changing the polarisation behaviour through Lorentz force and excites the electrons to enhance charge transmission.

关键词： magnetic performance fields

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High-resolution recognition of FOAM modes via an improved EfficientNet V2 based convolutional neural network

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Frontiers of physics 2024年第3期19卷 175-183页

作者： Youzhi Shi Zuhai Ma Hongyu chen Yougang ke Yu chen Xinxing Zhou international Collaborative Laboratory of 2D Materials for Optoelectronics Science and Technology Institute of Microscale OptoelectronicsShenzhen UniversityShenzhen 518060China key Laboratory of Low-Dimensional Quantum Structures and Quantum Control of Ministry of Education Synergetic Innovation Center for Quantum Effects and ApplicationsSchool of Physics and ElectronicsHunan Normal UniversityChangsha 410081China key Laboratory of Hunan Province on information Photonics and Freespace Optical Communications School of Information Science and EngineeringHunan Institute of Science and TechnologyYueyang 414006China

Vortex beam with fractional orbital angular momentum (FOAM) is the excellent candidate for improving the capacity of free-space optical (FSO) communication system due to its infinite modes. Therefore, the recognition of FOAM modes with higher resolution is always of great concern. in this work, through an improved EfficientNetV2 based convolutional neural network (CNN), we experimentally achieve the implementation of the recognition of FOAM modes with a resolution as high as 0.001. To the best of our knowledge, it is the first time this high resolution has been achieved. Under the strong atmospheric turbulence (AT) (C_(n)^(2)=10^(-15)m^(-2/3)), the recognition accuracy of FOAM modes at 0.1 and 0.01 resolution with our model is up to 99.12% and 92.24% for a long transmission distance of 2000 m. Even for the resolution at 0.001, the recognition accuracy can still remain at 78.77%. This work provides an effective method for the recognition of FOAM modes, w.ich may largely improve the channel capacity of the free-space optical communication.

关键词： OAM free-space optical communication deep learning convolutional neural network

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Single-atom Co alloyed Ru for electrocatalytic nitrite reduction to ammonia

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Nano Research 2024年第5期17卷 3660-3666页

作者： Fuzhou wang Jiaqi Xiang Guike Zhang Kai chen ke Chu School of Materials Science and Engineering Lanzhou Jiaotong UniversityLanzhou 730070China

Electrochemical converting NO_(2)^(-)into NH_(3)(NO_(2)RR)holds an enormous prospect to attain efficient NH_(3) electrosynthesis and polluted NO_(2)^(-)***,we report single-atom Co alloyed Ru(Co_(1)Ru)as an efficient and durable NO_(2)RR *** experimental and theoretical investigations reveal that single-atom Co alloying of Ru enables the construction of Co_(1)-Ru heteronuclear active sites to synergistically promote NO_(2)^(-)activation/hydrogenation w.ile suppressing the competitive H_(2) evolution,rendering the greatly enhanced activity and selectivity of Co_(1)Ru towards the NO_(2)***,Co_(1)Ru assembled within a flow cell exhibits an impressive NH_(3) yield rate of 2379.2μmol·h^(-1)·cm^(-2) with an NH_(3)-Faradaic efficiency of 92%at a high current density of 415.9 mA·cm^(-2),w.ich is among the highest NO_(2)RR performances reported to date.

关键词： electrochemical converting NO_(2)-into NH3 single-atom alloys theoretical computations industrial-level current density

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Effect of Operation Parameters on the Thermal Characteristics in a Planar Solid Oxide Fuel Cell

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Journal of Thermal Science 2024年第5期33卷 1974-1989页

作者： wANG Mingyuan wANG ke wANG Yongqing chen Jiangshuai AN Bo TU Shantung School of Mechanics and Safety Engineering Zhengzhou UniversityZhengzhou 450001China key Laboratory of Process Heat Transfer and Energy Saving of Henan Province Zhengzhou UniversityZhengzhou 450002China School of Mechanical and Power Engineering Zhengzhou UniversityZhengzhou 450001China key Laboratory of Pressure Systems and Safety(MOE) East China University of Science&TechnologyShanghai 200237China

Effective operation strategies in the solid oxide fuel cell(SOFC)can adjust the spatial distribution of temperature gradient favoring the long-term *** investigate the effects of different operating conditions on the thermal behavior inside SOFC,a three-dimensional model is developed in this *** model is verified by comparing it with the experimental *** heat generation rate and its variation under different operating conditions are *** combined effects of operating voltage and gas temperature are considered to be the key factor influencing the temperature *** to the original case,the temperature of SOFC decreases by 21.4 K when the fuel velocity reaches 5 m/*** the maximum temperature gradient increases by21.2%.Meanw.ile,higher fuel velocities can eliminate about 32%of the area with higher temperature *** when the oxidant velocity reaches 7.5 m/s,the peak temperature gradient effectively decreases by 16.59%.Simultaneous adjustment of the oxidant and fuel velocities can effectively reduce the peak temperature gradient and increase the safety *** effects of operation conditions on the temperature gradient of the cell are clarified in this study,w.ich can be a reference for further research on the reliability of SOFCs.

关键词： SOFC heat generation temperature gradient distribution heat source thermal behavior

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Effects of grain's shape-and size-polydispersities,orientation,and area fraction on tortuosity and permeability of 2D granular media

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Particuology 2024年第7期90卷 535-557页

作者： ke Cao Huisu chen Mohammad iqbal Khan Mingqi Li Lin Liu Jiangsu key Laboratory of Construction Materials School of Materials Science and EngineeringSoutheast UniversityNanjing 211189China Department of Civil Engineering College of EngineeringKing Saud UniversityP.O.Box 800Riyadh 11421Saudi Arabia School of Civil and Transportation Engineering Hebei University of TechnologyTianjin 300401China College of Civil and Transportation Engineering Hohai UniversityNanjing210098China

The microstructure of granular media, including grain's shape- and size-polydispersities, orientation, and area fraction can potentially affect its permeability. However, few studies consider the coupling effects of these features. This work employs geometrical probability and stereology to establish quantitative relationships between the above microstructural features and the geometric tortuosity of the two-dimensional granular media containing superellipse, superoval, and polygon grains. Then the lattice Boltzmann method (LBM) is used to determine the permeabilities of these granular media. By combining the tortuosity model and the LBM-derived permeabilities, modified K–C equations are formulated to predict the permeability and the shape factor, considering the grain's shape- and size-polydispersities, orientation, and area fraction. The reliability of these methods can be verified by comparing them with both our simulations and available experimental, theoretical, and numerical data reported in the literature. The findings implicate that the tortuosity and permeability of the granular media are strongly correlated with the grain's shape, orientation, and area fraction but unaffected by the size polydispersity and spatial arrangement of grains. Only circularity is not enough to derive a unified formula for considering the impact of grain shape on tortuosity and permeability, other shape parameters need to be explored in the future.

关键词： Geometric tortuosity Konzey-Carman equation Shape and size ploydispersities Grain orientation Lattice Boltzmann method Granular media

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