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Universal design of three-dimensional porous graphene-iron based promotors for kinetically rationalized lithium-sulfur chemistry

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Journal of Energy Chemistry 2025年第1期100卷 192-200页

作者： Hua Gao Yunfeng Zhang Menglei Wang Ruoxuan Yang Shuai Feng Xuan Cao Yaping Zhang Zhongyuan Lu Yingze Song state key laboratory of Environment-Friendly Energy Materials School of Materials and Chemistry Southwest University of Science and Technology School of Material Science and Engineering Henan University of Technology College of Chemistry and Chemical Engineering Taishan University

Lithium-sulfur （Li-S） batteries are widely deemed to be one of the most potential candidates for future secondary batteries because of their remarkable energy ***,notorious polysulfide shuttling and retarded sulfur reaction kinetics pose significant obstacles to the further application of Li-S *** rationally designed highly active electrocatalysts can facilitate polysulfide conversion,the universal and scalable synthesis strategies need to be ***,a universal synthetic strategy to construct a series of three-dimensional （3D） porous graphene-iron （3DGr-Fe） based electrocatalysts involving 3DGr-FeP,3DGr-Fe3C,and 3DGr-Fe3Se4is exploited for manipulating the Li-S redox *** has been observed that the implementation of a 3D porous Gr architecture leads to the well-designed conductive networks,while the uniformly dispersed iron nanoparticles introduce an abundance of active sites,fostering the lithium polysulfide conversion,thereby bolstering the overall electrochemical *** Li-S battery with the 3DGr-Fe based electrocatalyst exhibits remarkable capacity retention of 94.8%upon 100 times at 0.2 ***,the soft-packaged Li-S pouch cell based on such a 3DGr-Fe electrocatalyst delivers superior capacity of 1060.71 mA h g-1and guarantees for the continuous 30 min work of fan *** investigation gives comprehensive insights into the design,synthesis,and mechanism of 3DGr-Fe based electrocatalysts with high activity toward efficient and durable Li-S batteries.

关键词： Redox reactions

Synthesis of chiral phosphine derivatives through a copper（I）-catalyzed desymmetric SNAr reaction

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Science China Chemistry 2025年

作者： Shuai Zhang Pei-Zhi Liu Yan-Bo Li Qi Zhang Jun-Zhao Xiao Yi-Fan Wang Tian-Yu Wei Jia-Wei Jiang Ye Wang Qian Peng Liang Yin key laboratory of Fluorine and Nitrogen Chemistry and Advanced Materials Shanghai Institute of Organic Chemistry University of Chinese Academy of Sciences Chinese Academy of Sciences state key laboratory of Elemento-Organic Chemistry and Tianjin key laboratory of Biosensing and Molecular Recognition College of Chemistry Frontiers Science Center for New Organic Matter Nankai University Haihe laboratory of Sustainable Chemical Transformations

Axially chiral phosphines are a class of extremely important ligands in asymmetric catalysis. Herein, an unprecedented copper（I）-catalyzed asymmetric SNAr reaction with HP（S）R2is uncovered, which delivers a series of axially chiral phosphine derivatives in high yields with excellent enantioselectivity. Furthermore, the diastereoselective reaction with the kinetic resolution of racemic HP（S）ArR proceeds smoothly, providing the products with moderate diastereoselectivity and excellent enantioselectivity. Control experiments indicate that HP（S）Ph2is much more active than HPPh2and HP（O）Ph2as the pronucleophile in the present reaction. It is found that the SNAr reaction （the first SNAr） proceeds in a desymmetric manner, providing the desired chiral products while a continued SNAr reaction （the second SNAr） slightly occurs in a kinetic resolution manner in the present catalytic system, which enhances the ee of the desired chiral products. DFTcalculations support a concerted reaction pathway rather than a step-wise mechanism. Finally, axially chiral olefin-phosphines produced by the present method work as suitable ligands in Pdcatalyzed asymmetric allylic substitution with C-, N-, and O-nucleophiles and Rh-catalyzed asymmetric addition of arylboronic acid to benzil.

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Dielectric-ion-conductive ZnNb2O6 layer enabling rapid desolvation and diffusion for dendrite-free Zn metal batteries

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Journal of Energy Chemistry 2025年第1期100卷 693-701页

作者： Haifeng Yang Jian Wang Panpan Zhang Xiaomin Cheng Qinghua Guan Jing Dong Bixian Chen Lujie Jia Jing Zhang Yongzheng Zhang Yunjian Liu Hongzhen Lin School of Materials Science and Engineering Jiangsu University i-Lab & CAS key laboratory of Nanophotonic Materials and Devices Suzhou Institute of Nano-Tech and Nano-Bionics Chinese Academy of Sciences Helmholtz Institute Ulm (HIU) Karlsruhe Institute of Technology (KIT) School of Materials Science and Engineering Xi'an University of Technology state key laboratory of Chemical Engineering East China University of Science and Technology

Rechargeable aqueous zinc-metal batteries （AZMBs） are promising candidates for large-scale energy storage systems due to their low cost and high ***,their performance and sustainability are significantly hindered by the sluggish desolvation kinetics at the electrode/electrolyte interface and the corresponding hydrogen evolution reaction where active water molecules tightly participate in the Zn（H2O）62+solvation ***,learnt from self-generated solid electrolyte interphase （SEI） in anodes,the dielectric but ion-conductive zinc niobate nanoparticles artificial layer is constructed on metallic Zn surface （ZNB@Zn）,acting as a rapid desolvation *** zincophilic and dielectric-conductive properties of ZNB layer accelerate interfacial desolvation/diffusion and suppress surface corrosion or dendrite formation,achieving uniform Zn plating/stripping behavior,as confirmed by electronic/optical microscopies and interface spectroscopical measurements together with theoretical ***,the as-prepared ZNB@Zn electrode exhibits excellent cycling stability of over 2000 h and robust reversibility （99.54%） even under high current density and depth of discharge ***,the assembled ZNB@Zn-based full cell displays high capacity-retention rate of 80.21%after 3000 cycles at 5 A g-1and outstanding rate performance up to 10 A *** large-areal pouch cell is stabilized for hundreds of cycles,highlighting the bright prospects of the dielectric but ion-conductive layer in further application of AZMBs.

关键词： Zn metal battery Dielectric artificial layer Rapid ion diffusion Zincophilic diffusion Active water inhibition

SEFormer:A Lightweight CNN-Transformer Based on Separable Multiscale Depthwise Convolution and Efficient Self-Attention for Rotating Machinery Fault Diagnosis

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Computers, Materials & Continua 2025年第1期82卷 1417-1437页

作者： Hongxing Wang Xilai Ju Hua Zhu Huafeng Li state key laboratory of Mechanics and Control for Aerospace Structures Nanjing University of Aeronautics and AstronauticsNanjing210016China School of Computer Science and Engineering Nanyang Technological UniversitySingapore639798Singapore

Traditional data-driven fault diagnosis methods depend on expert experience to manually extract effective fault features of signals,which has certain ***,deep learning techniques have gained prominence as a central focus of research in the field of fault diagnosis by strong fault feature extraction ability and end-to-end fault diagnosis ***,utilizing the respective advantages of convolution neural network(CNN)and Transformer in local and global feature extraction,research on cooperating the two have demonstrated promise in the field of fault ***,the cross-channel convolution mechanism in CNN and the self-attention calculations in Transformer contribute to excessive complexity in the cooperative *** complexity results in high computational costs and limited industrial *** tackle the above challenges,this paper proposes a lightweight CNN-Transformer named as SEFormer for rotating machinery fault ***,a separable multiscale depthwise convolution block is designed to extract and integrate multiscale feature information from different channel dimensions of vibration ***,an efficient self-attention block is developed to capture critical fine-grained features of the signal from a global ***,experimental results on the planetary gearbox dataset and themotor roller bearing dataset prove that the proposed framework can balance the advantages of robustness,generalization and lightweight compared to recent state-of-the-art fault diagnosis models based on CNN and *** study presents a feasible strategy for developing a lightweight rotating machinery fault diagnosis framework aimed at economical deployment.

关键词： CNN-Transformer separable multiscale depthwise convolution efficient self-attention fault diagnosis

Leader-follower: Human-centered intention-guided controller for novel SuperLimb with application to load-carrying scenarios

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Science China Technological Sciences 2025年第1期 325-338页

作者： Qinghua ZHANG Xianglong LI Hongwei JING Kerui SUN Yuancheng LI Sikai ZHAO Lele LI Haotian JU Ziqi WANG Rui WU Tianjiao ZHENG Jie ZHAO Yanhe ZHU The state key laboratory of Robotics and System Harbin Institute of Technology The Learning Algorithms and Systems laboratory School of Engineeringécole Polytechnique Fédérale de Lausanne

Supernumerary robotic arms(SuperLimb) are a new type of wearable robot that works closely with humans as a third hand to augment human operation capability. Accurate conveyance of wearers' intentions, allocation of roles, and humancentered interaction considerations are the key points in the process of human–SuperLimb collaboration. This paper proposes a human-centered intention-guided leader–follower controller that relies on the dynamic modeling of SuperLimb with application to load-carrying scenarios. The proposed leader–follower controller takes the human as the leader and the SuperLimb as the follower, achieving effective information communication, autonomous coordination, and good force compliance between SuperLimb, humans, and the environment under human safety assurance. First, the human–SuperLimb dynamic system is modeled to achieve force interaction with the environment and wearer. Second, to achieve the precise intention extraction of humans, pose data from five visual odometry sensors are fused to capture the human state, the generalized position, the velocity of hands, and the surface electromyography signals from two myoelectric bracelets sensors are processed to recognize the natural hand gestures during load-carrying scenarios by a designed Swin transformer network. Then, based on the real-time distance detection between human and mechanical limbs, the security assurance and force-compliant interaction of the human–SuperLimb system are realized. Finally, the human hand muscle intention recognition, human–robot safety strategy verification,and comparative load-carrying experiments with and without the proposed method are conducted on the SuperLimb *** showed that the task parameters are well estimated to produce more reasonable planning trajectories, and SuperLimb could well understand the wearer's intentions to switch different SuperLimb actions. The proposed sensor-based human–robot communication framework motivates future studies of o

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Nitrogen addition promotes soil carbon accumulation globally

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Science China Life Sciences 2025年第1期 284-293页

作者： Xuemei Yang Suhui Ma Erhan Huang Danhua Zhang Guoping Chen Jiangling Zhu Chengjun Ji Biao Zhu Lingli Liu Jingyun Fang Institute of Ecology College of Urban and Environmental Sciencesand Key Laboratory for Earth Surface Processes of the Ministry of EducationPeking University Ministry of Education key laboratory for Transboundary Ecosecurity of Southwest China School of Ecology and Environmental ScienceYunnan University state key laboratory of Vegetation and Environmental Change Institute of BotanyChinese Academy of Sciences

Soil is the largest carbon(C) reservoir in terrestrial ecosystems and plays a crucial role in regulating the global C cycle and climate *** nitrogen(N) deposition has been widely considered as a critical factor affecting soil organic carbon(SOC) storage, but its effect on SOC components with different stability remains unclear. Here, we analyzed extensive empirical data from 304 sites worldwide to investigate how SOC and its components respond to N addition. Our analysis showed that N addition led to a significant increase in bulk SOC(6.7%), with greater increases in croplands(10.6%) and forests(6.0%) compared to grasslands(2.1%). Regarding SOC components, N addition promoted the accumulation of plant-derived C(9.7%–28.5%) over microbial-derived C(0.2%), as well as labile(5.7%) over recalcitrant components(–1.2%), resulting in a shift towards increased accumulation of plant-derived labile C. Consistently, N addition led to a greater increase in particulate organic C(11.9%) than mineral-associated organic C(3.6%), suggesting that N addition promotes C accumulation across all pools, with more increase in unstable than stable pools. The responses of SOC and its components were best predicted by the N addition rate and net primary productivity. Overall, our findings suggest that N enrichment could promote the accumulation of plant-derived and non-mineral associated C and a subsequent decrease in the overall stability of soil C pool, which underscores the importance of considering the effects of N enrichment on SOC components for a better understanding of C dynamics in soils.

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Development of a general circumferentially nonuniform heat transfer fuel rod model for subchannel analysis and application to helical fuel rods

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Science China Technological Sciences 2025年

作者： Junsen FU Junlong LI Xiaowen WANG Qi ZHANG Yao XIAO Hanyang GU School of Mechanical Engineering Shanghai Jiao Tong University key laboratory of Nuclear Power Systems and Equipment of the Ministry of Education Shanghai Jiao Tong University National key laboratory of Nuclear Reactor Technology Nuclear Power Institute of China state key laboratory of Nuclear Power Safety Technology and Equipment Shanghai Jiao Tong University

The subchannel analysis method is one of the most crucial transient safety analysis methods in the thermal design of nuclear reactors. The nonuniformity of circumferential heat transfer is slight in conventional pressurized water reactor (PWR)cores, but it is significant in advanced reactors with wire-wrapped or helical fuel rods. Predicting circumferentially nonuniform heat transfer behavior can be challenging owing to the complex geometry of helical fuel rods. In this study, a general circumferentially nonuniform heat transfer fuel rod (GCNF) model is developed to predict the fuel central temperature and circumferential heat flux and wall temperature. This model incorporates a refined two-dimensional fuel conduction model and circumferential nonuniform shape factor, addressing the dual factors contributing to the circumferential nonuniformity of helical fuel rods. An empirical correlation for the nonuniform shape factor is developed based on the computational fluid dynamics (CFD) results, and it is implemented to the subchannel code. The newly developed model is applied to a helical fuel annulus and validated by comparing the prediction results with CFD data. The maximum wall temperature predicted by the code is 1.15°C lower than the value calculated through CFD. In terms of the heat flux, the maximum value at the inner corner is22 kW lower than that obtained from the CFD prediction. The accurate prediction of circumferentially nonuniform heat transfer in helical fuel, concerning the surface heat flux and cladding temperature, addresses existing shortcomings in helical fuel subchannel analysis methods. Additionally, the capability to predict the fuel central temperature is essential for the safety analysis to determine whether fuel rods are melting. The generality of the model framework allows it to be used for the prediction of circumferential nonuniform heat transfer behavior in other types of fuel assemblies.

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Ultrastrong room-temperature phosphorescence in cucurbit[8]uril-mediated crystalline supramolecules for ratiometric detection of phenethylamine

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Science China Chemistry 2025年

作者： Qingyu Niu Yingxiang Ye Lingna Su Xu He Zhiqiang Li Yu Liu School of Chemical Engineering and Technology Hebei University of Technology Fujian Provincial key laboratory of Polymer Materials College of Chemistry and Materials Science Fujian Normal University key laboratory of Advanced Energy Materials Chemistry (Ministry of Education) Nankai University College of Chemistry State Key Laboratory of Elemento-Organic Chemistry Nankai University

It is a great challenge to modulate purely organic fluorescence-phosphorescence dual emission in aqueous solution because the excited singlet and triplet states are in competition with each other. Herein, we report a crystalline 1:2 host-guest formed by selfassembly of 4-(4-bromophenyl)-pyridinium derivatives and cucurbit[8]uril, in which a rigid environment rich in weak interactions is directly demonstrated. Due to the inhibition of non-radiative transition and stabilization of triplet exciton in the crystalline environment, the crystalline inclusion complex exhibits ultralong room-temperature phosphorescence lifetime of 3.21 ms with an room-temperature phosphorescence(RTP) quantum yield up to 16.29%. Interestingly, the crystalline 1:2 hostguest complex demonstrates the ability of rapid identification and sensitive fluorescence-phosphorescence ratiometric detection behavior toward phenethylamine, a drug analogue, with a limit of detection as low as 27.5 nM. We believe that this study will undoubtedly broaden the utilizing scopes of RTP and offer a novel avenue for psychoactive substances monitoring.

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Rational modulation of fluorophosphate cathode by anionic groups to reduce the polarization behavior for fast-charging sodium-ion batteries

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Journal of Energy Chemistry 2025年第1期100卷 509-521页

作者： Xinyuan Wang Fan Zhang Xingyu Zhou Qian Wang Changyu Liu Yangyang Liu Hui Wang Xiaojie Liu key laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education College of Chemistry & Materials Science Northwest University

Na3V2（PO4）2O2F （VP） is recognized as a promising cathode material for sodium-ion batteries due to its stable structural framework and high specific *** functional theory （DFT） and finite element simulations show that incorporating SO42-into VP decreases its band gap,lowers the migration energy barrier,and ensures a uniform Na+concentration gradient and stress distribution during charge and discharge ***,the average Na+diffusion coefficient of Na3V2（PO4）1.95（SO4）0.05O2F（VPS-1） is roughly double that of VP,leading to enhanced rate capability (80 C,75.5 mAh g-1) and cycling stability (111.0 mAh g-1capacity after 1000 cycles at 10 C current density) for ***-1 exhibits outstanding fast-charging capabilities,achieving an 80%state of charge in just 8.1 *** assembled VPS-1//SbSn/NPC full cell demonstrated stable cycling over 200 cycles at a high 5 C current,maintaining an average coulombic efficiency of 95.35%.

关键词： Anionic group modulation Polarization behavior Fast-charging Sodium-ion battery Fluorophosphate Cathode