Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen e...Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.展开更多
The complex aerodynamic interaction between tandem tilt-wing and multi-rotor directly affects the wing surface flow and rotor thrust,making it a critical factor during the tilt transition process of this configuration...The complex aerodynamic interaction between tandem tilt-wing and multi-rotor directly affects the wing surface flow and rotor thrust,making it a critical factor during the tilt transition process of this configuration of rotorcraft.The aerodynamic interaction of tandem tilt-wing and multi-rotor is investigated based on the CFD method.The aerodynamic effect of multi tilt-rotor is simulated as virtual disk modeling by adding source terms to the Navier-Stokes equations,effectively reducing the calculation time while maintaining the accuracy of aerodynamic interaction calculations.Aerodynamic forces and flow field characteristics of the tandem tilt-wing and multi-rotor under different tilt angles are compared between cases with and without aerodynamic interaction.Furthermore,the differences in aerodynamic forces between dynamic tilt transition and fixed-angle conditions were compared.The results show that the aerodynamic interaction of multi-rotor obviously increases the lift of front tilt-wing at different tilt angles,the wing lift under interaction is increased by more than 40%compared with isolated wing at tilt angle of 15°for the computation in this paper,which is related to the increase of wing flow velocity and the suppression of flow separation caused by multi-rotor;the wing blocking effect will increase rotor thrust,especially near the tilt angles of 30°and 45°;the increases of rear wing lift and rear rotor thrust under aerodynamic interaction are not significant because of suppression by the front wing’s downwash;the unsteady effects during dynamic tilting have a relatively minor impact on aerodynamic interaction,with the aerodynamic forces on the rotors and wings during the dynamic tilting process showing little difference from those under corresponding fixed tilt angles.展开更多
Peptides play important roles in chemistry,medicinal chemistry and life science,due to their high efficiency and specificity,unusual biological and therapeutic properties.As naturally occurring peptides often face wit...Peptides play important roles in chemistry,medicinal chemistry and life science,due to their high efficiency and specificity,unusual biological and therapeutic properties.As naturally occurring peptides often face with their intrinsic limitations including metabolic instability and low membrane permeability,the strategies for synthesizing unnatural amino acids and peptides are explored.Among the methods for modifying amino acids and peptides,chemo-and site-selective approaches are preferred because of the ability to fine-tuning structural features.Recently,transition metal-catalyzed Csingle bondH activation has been employed for the functionalization of amino acids and peptides.Through domino Csingle bondH activation/annulation,a series of structurally complex and diverse amino acids and peptides is constructed.This review highlights recent advances in the synthesis of unnatural amino acids and peptides via transition metal-catalyzed Csingle bondH activation/annulation.展开更多
Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy infl...Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy influence the competitiveness of economies,while the level of energy consumption impacts the standard of living for individuals.This paper aims to examine environmental challenges and steps for a sustainable transition towards a hydrogen economy,focusing on its potential as an alternative to fossil fuels and the importance of developing the hydrogen paradigm.The research methodology is based on a combination of qualitative and quantitative methods,including an analysis of global and regional trends in the energy transition,the impact of various forms of hydrogen production(green,blue,gray hydrogen)on greenhouse gas emissions,and a comparison of existing policies and strategies in different countries transitioning to a sustainable hydrogen economy.Research results show that green hydrogen,produced via electrolysis using renewable energy sources,holds the greatest potential for reducing greenhouse gas emissions,while gray and blue hydrogen can serve as transitional options.The development of the hydrogen paradigm,rooted in innovative technologies,renewable energy sources,and international cooperation,is crucial for decarbonization and the creation of a sustainable global economy,despite challenges such as high costs and the need for global coordination.The hydrogen paradigm is becoming a cornerstone of these efforts,laying the foundation for a long-term,sustainable global economy.Currently,over 180 hydrogen transport projects,60 distribution projects,80 storage projects,30 terminal and port projects,and more than 220 hydrogen production projects are under development worldwide.The global momentum of the hydrogen transition helps mitigate climate change and build a sustainable future.展开更多
Fe_(3)Sn_(2),a ferromagnetic metal with a kagome lattice,serves as an ideal platform for exploring topological electronic states and Berry curvature due to its unique band structure.However,systematic reports on the t...Fe_(3)Sn_(2),a ferromagnetic metal with a kagome lattice,serves as an ideal platform for exploring topological electronic states and Berry curvature due to its unique band structure.However,systematic reports on the transport properties of Fe_(3)Sn_(2)nanosheets remain scarce.We present temperature-dependent transport property measurements of Fe_(3)Sn_(2)nanosheets synthesized via chemical vapor deposition on Si/SiO_(2)substrates.The samples exhibit a robust anomalous Hall effect from 40 K to 300 K,along with a magnetoresistance sign reversal at 40 K at high magnetic fields,indicating a spin reorientation from in-plane to out-of-plane.Notably,a sharp crossover in the dominant transport contribution from electrons to holes near 200 K is observed,accompanied by distinct anomalous Hall behaviors in the two regimes,indicating a temperature-induced Lifshitz transition within the multi-band system.This divergence is potentially linked to a topological reconstruction of the Fermi surface across the transition.Our findings highlight the tunability of topological transport in two-dimensional kagome magnets and provide new insights into the interplay between band topology,dimensionality and magnetic order.展开更多
The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulat...The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.展开更多
The volume change behavior of natural gas hydrate-bearing sediment is essential as it influences settlement,strength,and stiffness,which directly affect the stability of hydrate reservoirs during hydrate extraction or...The volume change behavior of natural gas hydrate-bearing sediment is essential as it influences settlement,strength,and stiffness,which directly affect the stability of hydrate reservoirs during hydrate extraction or in response to environmental changes.The volume change is influenced not only by stress but also by the formation and dissociation of hydrates.This study adopted a customized apparatus for one-dimensional compression tests,allowing independent control of gas pressure and effective stress.Tests were conducted on samples with different hydrate saturations along various temperature-gas pressure-effective stress paths,yielding some conclusions related to compressibility and creep.An unusual phenomenon was observed under low-stress conditions:hydrate formation led to shrinkage rather than expansion.Three potential mechanisms behind this occurrence were discussed.As hydrate saturation increases,the yield stress rises while the compression and swelling indexes remain minimally affected.After hydrate dissociation,the compression curve of hydrate-bearing sediment drops to that of hydrate-free sediment.Once hydrate is formed,the compression curve of hydrate-free sediment gradually approaches that of hydrate-bearing sediment during the subsequent loading.Under low-stress conditions,the creep of both hydrate-free and hydrate-bearing sediments is very weak.However,when stress increases,significantly beyond the yield stress,the creep of both sediments increases significantly,with hydrate-bearing sediment exhibiting much greater creep than hydrate-free sediment.展开更多
Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible s...Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible structural degradation.To overcome these limitations,we propose a rationally engineered nanoreactor architecture that stabilizes defect-rich MoS_(2)via interlayer incorporation of a carbon monolayer,followed by encapsulation within a nitrogen-doped carbon shell,forming a MoSSe@NC heterostructure.This tailored structure synergistically accelerates both K^(+)diffusion kinetics and electron transfer,enabling unprecedented rate performance(107 mAh g^(-1)at 10 Ag^(-1))and ultralong cyclability(86.5%capacity retention after 1200 cycles at 3 A g^(-1)).Mechanistic insights reveal a distinctive“adsorption-conversion”pathway,where sulfur vacancies on exposed S-Mo-S basal planes act as preferential K^(+)adsorption sites,effectively suppressing parasitic phase transitions during intercalation.In situ X-ray diffraction and transmission electron microscopy corroborate the structural reversibility of the conversion reaction,with the carbon matrix dynamically accommodating strain while preserving electrode integrity.This work not only advances the understanding of defect-driven interfacial chemistry in conversion-type materials but also provides a versatile strategy for designing high-performance anodes in next-generation PIBs through heterostructure engineering.展开更多
Crossflow instability will be present when the vehicle has an angle of attack in hypersonic flow,and it might play a dominant role in hypersonic boundary layer transition.By far the mechanism of crossflow instability-...Crossflow instability will be present when the vehicle has an angle of attack in hypersonic flow,and it might play a dominant role in hypersonic boundary layer transition.By far the mechanism of crossflow instability-induced hypersonic boundary layer transition is still out of understanding,although the large effort has been devoted.Upon this work,the overall roughness effect on instabilities in hypersonic flow was researched experimentally.Surface flush-mounted pressure sensors and infrared camera were employed to investigate the instability waves when different rough surfaces were deployed.The results reveal that the moderate surface roughness level on cone model can suppress the growth of crossflow instabilities at certain azimuthal angles in hypersonic flow.展开更多
The interactions between clouds and aerosols represent one of the largest uncertainties in assessing the Earth's radiation budget, highlighting the importance of research on the transition zone(TZ) within the clou...The interactions between clouds and aerosols represent one of the largest uncertainties in assessing the Earth's radiation budget, highlighting the importance of research on the transition zone(TZ) within the cloud-aerosol continuum.This study assesses the global distribution of TZ conditions, analyzes its optical characteristics, and determines the cloud or aerosol types most commonly associated with them, using the cloud-aerosol discrimination(CAD) score of the CloudAerosol Lidar with Orthogonal Polarization(CALIOP) instrument on the CALIPSO satellite. The CAD score classifies clouds and aerosols by the probability density functions of attenuated backscatter, total color ratio, volume depolarization ratio, altitude, and latitude. After applying several filters to avoid artifacts, the TZ was identified as those atmospheric layers that cannot be clearly classified as clouds or aerosols, layers within the no-confidence range(NCR) of the CAD score, and cirrus fringes. The optical characteristics of NCR layers exhibit two main clusters: Cluster 1, with properties between high-altitude ice clouds and aerosols(e.g., wispy cloud fragments), and Cluster 2, with properties between water clouds and aerosols at lower altitudes(e.g., large hydrated aerosols). Our results highlight the significant ubiquity of TZ conditions, which appear in 9.5% of all profiles and comprise 6.4% of the detected layers. Cluster 1 and cirrus-fringe layers predominate near the ITCZ and in mid-latitudes, whereas Cluster 2 layers are more frequent over the oceans along the central West African and East Asian coasts, where elevated smoke and dusty marine aerosols are common.展开更多
The moment a media delegation from the Republic of the Congo arrived at the Othello Kitchenware Museum on 18 November 2025,they were greeted with a vivid show of Guangdong’s industrial strength.Standing before them w...The moment a media delegation from the Republic of the Congo arrived at the Othello Kitchenware Museum on 18 November 2025,they were greeted with a vivid show of Guangdong’s industrial strength.Standing before them was not a typical exhibition hall,but a building shaped like a gleaming stainless-steel cooking pot.展开更多
The buoyancy-induced flow constitutes a core scientific issue for thermal management of electronic devices and thermal design of energy systems,where accurate characterization of flow and heat transfer is essential to...The buoyancy-induced flow constitutes a core scientific issue for thermal management of electronic devices and thermal design of energy systems,where accurate characterization of flow and heat transfer is essential to improve thermal efficiency.In this work,buoyancy-induced flow above two heating elements flush-mounted at the bottom of a square enclosure containing air is numerically investigated over a range of Rayleigh numbers(0<Ra≤1.5×10^(8)),with a focus on equal and unequal heat flux conditions under a constraint of constant total thermal energy input.Distinct flow transitions are observed in both cases,leading to the identification of three flow regimes:Steady,periodic unsteady,and chaotic unsteady.Two types of periodic flows are distinguished,in which the first is a periodic flow dominated by a fundamental frequency(FF)and its integer-multiple frequencies(INTMF),while the second is a more complex periodic flow featuring FF,INTMF,and their sub-harmonics.The transitions between these regimes are affected by the relative heat flux of the two heaters.When the heat flux of the two heaters is unequal,the range of Rayleigh numbers corresponding to periodic flow is suppressed.It is also found that the time-averaged maximum temperature of the strong heater increases more rapidly with Ra,while that of the weak heater increases more slowly,reflecting the interaction between buoyancy-driven flow dynamics and asymmetric heat input.Analysis of the time-averaged Nusselt number demonstrates that heat dissipation from the isothermal walls remains roughly equivalent,even when the heat flux of the two heaters differs by a factor of two.These findings highlight the critical roles of Rayleigh number,the number of heaters,and the heat flux ratio of the heaters in determining heat transfer and flow characteristics for buoyancy-driven convection systems,providing important theoretical support and design references for engineering scenarios such as electronic devices and design of new energy systems.展开更多
MoTe_(2) has emerged as a promising candidate in the field of integrated circuits,memristive devices,and catalysts,owing to its polymorphic nature across different phases.Experimentally,strain engineering has been dem...MoTe_(2) has emerged as a promising candidate in the field of integrated circuits,memristive devices,and catalysts,owing to its polymorphic nature across different phases.Experimentally,strain engineering has been demonstrated as an effective approach for manipulating the phase transition of MoTe_(2),but the mechanism remains unclear.The strain-dependent phase transition and its micro-mechanisms have been investigated based on first principle calculations.As demonstrated,critical strain and phase transition path from H→T'phases are strongly governed by the applied strain's orientation,magnitude,and triaxiality.At the atomic level,nonzero movements of Te atoms within the phase transition domain with mechanical unloading have been clarified,together with an advanced understanding on the impact of strain on Te-vacancies migration.These insights advanced the knowledge of MoTe_(2) phase transition behavior and demonstrated the large space to explore potential applications through strain,defect,and phase engineering.展开更多
A flow transition prediction method for calculating effects of Reynolds numbers on aerodynamic characteristics of airfoil is developed,and the accuracy of the method is verified by wind tunnel experiment data and othe...A flow transition prediction method for calculating effects of Reynolds numbers on aerodynamic characteristics of airfoil is developed,and the accuracy of the method is verified by wind tunnel experiment data and other calculation results.On these basics,the infrared thermal imager experiment results of the flow transition in lowspeed wind tunnel and the aerodynamic characteristics experiment results with variable Reynolds number in highspeed wind tunnel are carried out respectively,and compared with the numerical results of helicopter rotor airfoil.Specially,effects of Reynolds numbers on airfoil aerodynamic characteristics by means of flow transition under different working conditions are researched and some meaningful conclusions are obtained.The calculation method,experiment method and results as well as the flow transition analysis conclusions for aerodynamic characteristics can be used for the design of helicopter rotor airfoil,especially for the helicopters under the high altitude and low Reynolds number working conditions.展开更多
The glass transition temperature(T_(g))of styrene-butadiene rubber(SBR)is a key parameter determining its low-temperature flexibility and processing performance.Accurate prediction of T_(g)is crucial formaterial desig...The glass transition temperature(T_(g))of styrene-butadiene rubber(SBR)is a key parameter determining its low-temperature flexibility and processing performance.Accurate prediction of T_(g)is crucial formaterial design and application optimisation.Addressing the limitations of traditional experimental measurements and theoretical models in terms of efficiency,cost,and accuracy,this study proposes a machine learning prediction framework that integrates multi-model ensemble and Bayesian optimization by constructing a multi-component feature dataset and algorithm optimization strategy.Based on the constructed high-quality dataset containing 96 SBR samples,ninemachine learning models were employed to predict the T_(g)of SBR and compare their prediction performance.Ultimately,aGPR-XGBoost mixed model was constructed through model ensemble,achieving high-precision prediction with R^(2)values greater than 0.9 on both the training and test sets.Further feature attribution and local effect analysis were conducted using feature analysis methods such as SHAP and ALE,revealing the nonlinear influence patterns of various components on T_(g),providing a theoretical basis for SBR formulation design and T_(g)regulation.The machine learning prediction framework established in this study combines high-precision prediction with interpretability,significantly enhancing the prediction performance of the T_(g)of SBR.It offers an efficient tool for SBR molecular design and holds great potential for promotion and application.展开更多
Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules wi...Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules with spatially heterogeneous patterns and slower dynamics compared to bulk water.Both the confinement and the surface atomic structures can induce the water phase transitions at low dimensional spaces.Here,we review how the phase transitions of interfacial water affect the surface physical behaviors,such as wetting,ice nucleation and the terahertz-wave-water interactions,from solid materials to the biological surfaces.These works help extend our knowledge of the physics properties of the interfacial water,particularly the multi-phase behaviors in materials and biology sciences.展开更多
AIM:To determine whether paeonol(Pae),a naturally occurring phenolic compound,can serve as an effective pharmacological inhibitor of posterior capsular opacification(PCO).METHODS:A rat model of cataract surgery—induc...AIM:To determine whether paeonol(Pae),a naturally occurring phenolic compound,can serve as an effective pharmacological inhibitor of posterior capsular opacification(PCO).METHODS:A rat model of cataract surgery—induced PCO was established,and Pae was administered via anterior chamber injection to evaluate its preventive effect on capsular opacification and fibrotic remodeling.Histological and immunohistochemical analyses were performed to assess epithelial-mesenchymal transition(EMT)—related changes in lens epithelial cells(LECs).Ex vivo lens capsule cultures were employed to examine the expression of Vimentin and Zonula Occludens-1(ZO-1)by immunofluorescence and immunohistochemistry.In the human LEC line SRA01/04,EMT marker expression at both mRNA and protein levels was analyzed following transforming growth factor beta 2(TGF-β2)stimulation,with Pae treatment.Western blotting and immunofluorescence were used to investigate the effect of Pae on TGF-β/Smad signaling and AMP-activated protein kinase(AMPK)activation.Molecular docking was performed to predict Pae–AMPK binding,and rescue experiments with AMPK inhibition were conducted to validate the mechanistic pathway.RESULTS:Pae significantly reduced capsular opacification and fibrotic remodeling in the rat PCO model compared with controls.In LECs,Pae markedly suppressed TGF-β2–induced EMT,evidenced by decreased expression of mesenchymal markers,such as Vimentin,Fibronectin,Collagen 1A1,α-SMA and preserved epithelial junctional protein ZO-1.Mechanistically,Pae was predicted to directly interact with the catalytic pocket of AMPK,which was experimentally confirmed by enhanced AMPK phosphorylation and nuclear translocation(P<0.05).This activation disrupted canonical TGF-β/Smad signaling,leading to suppression of EMT.Rescue experiments using AMPK inhibition abrogated the anti-EMT effect of Pae,further validating the AMPK-dependent mechanism.CONCLUSION:Pae exerts a potent inhibitory effect on PCO formation by blocking EMT of LECs through direct activation of AMPK and subsequent disruption of TGF-β/Smad signaling.展开更多
The accessibility of urban public transit directly influences residents’quality of life,travel behavior,and social equity.Its correlation with housing prices has garnered significant attention across disciplines such...The accessibility of urban public transit directly influences residents’quality of life,travel behavior,and social equity.Its correlation with housing prices has garnered significant attention across disciplines such as geography,economics,and urban planning.Although much existing research focuses on the impact of individual transportation facilities on housing prices,there is a notable gap in comprehensive analyses that assess the influence of overall urban transit accessibility on housing market dynamics.This study selected the main urban area of Hefei,China,as a case to investigate the spatial distribution of housing prices and evaluate public transit accessibility in 2022.Employing techniques such as the optimized parameter geographical detector and local spatial regression models,the study aimed to elucidate the effects and underlying mechanisms of urban transit accessibility on housing prices.The findings revealed that:1)housing prices in Hefei exhibited a clustered spatial pattern,with high prices concentrated in the city center and lower prices in peripheral areas,forming three distinct high-price hotspots with a‘belt-like’distribution;2)public transit accessibility showed a‘coreperiphery’structure,with accessibility declining in a‘circumferential’pattern around the city center.Based on the‘housing price-accessibility’dimension,four categories were identified:high price-high accessibility(37.25%),high price-low accessibility(19.07%),low price-high accessibility(21.95%),and low price-low accessibility(21.73%);3)the impact of transit accessibility on housing prices was spatially heterogeneous,with bus travel showing the strongest explanatory power(0.692),followed by automobile,subway,and bicycle travel.The interaction of these transportation modes generated a synergistic effect on housing price differentiation,with most influencing factors contributing more than 25%.These findings offer valuable insights for optimizing the spatial distribution of public transit infrastructure and improving both urban housing quality and residents’living standards.展开更多
In Chin.Phys.B 34114704(2025),Eq.(7)and the associated unit notation were incorrect.The correct ones are present here.Since Eq.(7)is an in-built expression in the simulation package,the correction is purely typographi...In Chin.Phys.B 34114704(2025),Eq.(7)and the associated unit notation were incorrect.The correct ones are present here.Since Eq.(7)is an in-built expression in the simulation package,the correction is purely typographical and does not affect the simulation procedure,numerical results,or the conclusions.展开更多
During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective r...During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective reconstruction regulation strategies.In this study,we first explored the reconstruction mechanism of CoS_(2)during OER from the perspective of electronic structure and identified two possible pathways:the OH-assisted mechanism and the O-assisted mechanism.Further verification showed that these mechanisms are universally applicable to other TMSs(e.g.,FeS_(2)).Based on the reconstruction mechanism,we investigated the basic reasons for the influence of various regulation strategies,such as vacancy modification and facet engineering,on the reconstruction ability.This verified that the method of analyzing the change in the reconstruction ability of catalysts based on the reconstruction mechanism has a high degree of applicability.Importantly,we proposed a core regulation strategy:the coordination symmetry regulation strategy.Specifically,by breaking the symmetry of the surface coordination environment of TMSs(such as introducing heteroatom doping or strain),the reconstruction process will be facilitated.Our findings provide a comprehensive mechanistic explanation for the reconstruction of TMS catalysts and offer a new idea for the rational design of OER catalysts with controllable reconstruction capacity.展开更多
基金Supported by the National Natural Science Foundation of China(No.52273056)the Science and Technology Development Program of Jilin Province,China(No.YDZJ202501ZYTS305)。
文摘Electrochemical water splitting represents a sustainable technology for hydrogen(H_(2))production.However,its large-scale implementation is hindered by the high overpotentials required for both the cathodic hydrogen evolution reaction(HER)and the anodic oxygen evolution reaction(OER).Transition metal-based catalysts have garnered significant research interest as promising alternatives to noble-metal catalysts,owing to their low cost,tunable composition,and noble-metal-like catalytic activity.Nevertheless,systematic reviews on their application as bifunctional catalysts for overall water splitting(OWS)are still limited.This review comprehensively outlines the principal categories of bifunctional transition metal electrocatalysts derived from electrospun nanofibers(NFs),including metals,oxides,phosphides,sulfides,and carbides.Key strategies for enhancing their catalytic performance are systematically summarized,such as heterointerface engineering,heteroatom doping,metal-nonmetal-metal bridging architectures,and single-atom site design.Finally,current challenges and future research directions are discussed,aiming to provide insightful perspectives for the rational design of high-performance electrocatalysts for OWS.
基金supported by the National Key Laboratory of Helicopter Aeromechanics Fund(No.2024-CXPT-GF-JJ-093-05).
文摘The complex aerodynamic interaction between tandem tilt-wing and multi-rotor directly affects the wing surface flow and rotor thrust,making it a critical factor during the tilt transition process of this configuration of rotorcraft.The aerodynamic interaction of tandem tilt-wing and multi-rotor is investigated based on the CFD method.The aerodynamic effect of multi tilt-rotor is simulated as virtual disk modeling by adding source terms to the Navier-Stokes equations,effectively reducing the calculation time while maintaining the accuracy of aerodynamic interaction calculations.Aerodynamic forces and flow field characteristics of the tandem tilt-wing and multi-rotor under different tilt angles are compared between cases with and without aerodynamic interaction.Furthermore,the differences in aerodynamic forces between dynamic tilt transition and fixed-angle conditions were compared.The results show that the aerodynamic interaction of multi-rotor obviously increases the lift of front tilt-wing at different tilt angles,the wing lift under interaction is increased by more than 40%compared with isolated wing at tilt angle of 15°for the computation in this paper,which is related to the increase of wing flow velocity and the suppression of flow separation caused by multi-rotor;the wing blocking effect will increase rotor thrust,especially near the tilt angles of 30°and 45°;the increases of rear wing lift and rear rotor thrust under aerodynamic interaction are not significant because of suppression by the front wing’s downwash;the unsteady effects during dynamic tilting have a relatively minor impact on aerodynamic interaction,with the aerodynamic forces on the rotors and wings during the dynamic tilting process showing little difference from those under corresponding fixed tilt angles.
基金supported by the Natural Science Foundation of Jiangsu Province(No.BK20220409)the National Natural Science Foundation of China(No.22401153)+2 种基金the FWO[Fund for Scientific Research-Flanders(Belgium)]for financial support(recipient Erik V.Van der Eycken)the Research Council of the KU Leuven(recipient Erik V.Van der Eycken)the support of the"RUDN University Strategic Academic Leadership Program"(recipient Erik V.Van der Eycken).
文摘Peptides play important roles in chemistry,medicinal chemistry and life science,due to their high efficiency and specificity,unusual biological and therapeutic properties.As naturally occurring peptides often face with their intrinsic limitations including metabolic instability and low membrane permeability,the strategies for synthesizing unnatural amino acids and peptides are explored.Among the methods for modifying amino acids and peptides,chemo-and site-selective approaches are preferred because of the ability to fine-tuning structural features.Recently,transition metal-catalyzed Csingle bondH activation has been employed for the functionalization of amino acids and peptides.Through domino Csingle bondH activation/annulation,a series of structurally complex and diverse amino acids and peptides is constructed.This review highlights recent advances in the synthesis of unnatural amino acids and peptides via transition metal-catalyzed Csingle bondH activation/annulation.
文摘Discussions about the future of energy sources and environmental sustainability are becoming critical on a global scale.The energy sector plays a central role in the economy,as the availability and cost of energy influence the competitiveness of economies,while the level of energy consumption impacts the standard of living for individuals.This paper aims to examine environmental challenges and steps for a sustainable transition towards a hydrogen economy,focusing on its potential as an alternative to fossil fuels and the importance of developing the hydrogen paradigm.The research methodology is based on a combination of qualitative and quantitative methods,including an analysis of global and regional trends in the energy transition,the impact of various forms of hydrogen production(green,blue,gray hydrogen)on greenhouse gas emissions,and a comparison of existing policies and strategies in different countries transitioning to a sustainable hydrogen economy.Research results show that green hydrogen,produced via electrolysis using renewable energy sources,holds the greatest potential for reducing greenhouse gas emissions,while gray and blue hydrogen can serve as transitional options.The development of the hydrogen paradigm,rooted in innovative technologies,renewable energy sources,and international cooperation,is crucial for decarbonization and the creation of a sustainable global economy,despite challenges such as high costs and the need for global coordination.The hydrogen paradigm is becoming a cornerstone of these efforts,laying the foundation for a long-term,sustainable global economy.Currently,over 180 hydrogen transport projects,60 distribution projects,80 storage projects,30 terminal and port projects,and more than 220 hydrogen production projects are under development worldwide.The global momentum of the hydrogen transition helps mitigate climate change and build a sustainable future.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1403503,2022YFA1602802,2023YFA1607400,and 2024YFA1613200)Beijing Natural Science Foundation(Grant No.JQ23022)supported by the Synergetic Extreme Condition User Facility and the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302600)。
文摘Fe_(3)Sn_(2),a ferromagnetic metal with a kagome lattice,serves as an ideal platform for exploring topological electronic states and Berry curvature due to its unique band structure.However,systematic reports on the transport properties of Fe_(3)Sn_(2)nanosheets remain scarce.We present temperature-dependent transport property measurements of Fe_(3)Sn_(2)nanosheets synthesized via chemical vapor deposition on Si/SiO_(2)substrates.The samples exhibit a robust anomalous Hall effect from 40 K to 300 K,along with a magnetoresistance sign reversal at 40 K at high magnetic fields,indicating a spin reorientation from in-plane to out-of-plane.Notably,a sharp crossover in the dominant transport contribution from electrons to holes near 200 K is observed,accompanied by distinct anomalous Hall behaviors in the two regimes,indicating a temperature-induced Lifshitz transition within the multi-band system.This divergence is potentially linked to a topological reconstruction of the Fermi surface across the transition.Our findings highlight the tunability of topological transport in two-dimensional kagome magnets and provide new insights into the interplay between band topology,dimensionality and magnetic order.
基金supported by the National Natural Science Foundation of China(52402166)the Science and Technology Development Fund+2 种基金Macao SAR(0065/2023/AFJ,0116/2022/A3)the Australian Research Council(DE220100154)the Natural Science Foundation of Guangdong Province(2025A1515011120)。
文摘The dissolvable polysulfides and sluggish Li_2S conversion kinetics are acknowledged as two significant challenges in the application lithium-sulfur(Li-S)batteries.Herein,we introduce a dual-doping strategy to modulate the electronic structure of MoS_(2),thereby obtaining a multifunctional catalyst that serves as an efficient sulfur host.The W/V dual single-atomdoped MoS_(2)grown on carbon nanofibers(CMWVS)demonstrates a strong adsorption ability for lithium polysulfides,suppressing the shuttle effects.Additionally,the doping process also results in the phase transition from 2H-MoS_(2)to 1T-MoS_(2)and generates sufficient edge sulfur atoms,promoting the charge/electron transfer and enriching the reaction sites.All these merits contribute to the superior conversion reaction kinetics,leading to the outstanding Li-S battery performance.When fabricated as cathodes by compositing with sulfur,the CMWVS/S cathode delivers a high capacity of 1481.7 mAh g^(-1)at 0.1 C(1 C=1672 mAh g^(-1))and maintains 816.3 m Ah g^(-1)after 1000 cycles at 1.0 C,indicating outstanding cycling stability.Even under a high sulfur loading of 7.9 mg cm^(-2)and lean electrolyte conditions(E/S ratio of 9.0μL mg^(-1)),the cathode achieves a high areal capacity of 8.2 m Ah cm^(-2),showing great promise for practical Li-S battery applications.This work broadens the scope of doping strategies in transition-metal dichalcogenides by tailoring their electronic structures,providing insightful direction for the rational development of high-efficiency electrocatalysts for advanced Li-S battery applications.
基金supported by the National Natural Science Foundation of China(Grant No.42171135)the Science and Technology Program of CNOOC Research Institute(Grant No.2023OTKK03)the“CUG Scholar”Scientific Research Funds at China University of Geosciences(Project No.2022098).
文摘The volume change behavior of natural gas hydrate-bearing sediment is essential as it influences settlement,strength,and stiffness,which directly affect the stability of hydrate reservoirs during hydrate extraction or in response to environmental changes.The volume change is influenced not only by stress but also by the formation and dissociation of hydrates.This study adopted a customized apparatus for one-dimensional compression tests,allowing independent control of gas pressure and effective stress.Tests were conducted on samples with different hydrate saturations along various temperature-gas pressure-effective stress paths,yielding some conclusions related to compressibility and creep.An unusual phenomenon was observed under low-stress conditions:hydrate formation led to shrinkage rather than expansion.Three potential mechanisms behind this occurrence were discussed.As hydrate saturation increases,the yield stress rises while the compression and swelling indexes remain minimally affected.After hydrate dissociation,the compression curve of hydrate-bearing sediment drops to that of hydrate-free sediment.Once hydrate is formed,the compression curve of hydrate-free sediment gradually approaches that of hydrate-bearing sediment during the subsequent loading.Under low-stress conditions,the creep of both hydrate-free and hydrate-bearing sediments is very weak.However,when stress increases,significantly beyond the yield stress,the creep of both sediments increases significantly,with hydrate-bearing sediment exhibiting much greater creep than hydrate-free sediment.
基金financially supported by the supported by Shandong Provincial Natural Science Foundation(ZR2024MB108)Taishan Young Scholar Program(tsqn202312312)Excellent Young Scholars of the Shandong Provincial Natural Science Foundation(Overseas)(2023HWYQ-112)。
文摘Conversion-type electrode materials hold significant promise for potassium-ion batteries(PIBs)due to their high theoretical capacities,yet their practical deployment is hindered by sluggish kinetics and irreversible structural degradation.To overcome these limitations,we propose a rationally engineered nanoreactor architecture that stabilizes defect-rich MoS_(2)via interlayer incorporation of a carbon monolayer,followed by encapsulation within a nitrogen-doped carbon shell,forming a MoSSe@NC heterostructure.This tailored structure synergistically accelerates both K^(+)diffusion kinetics and electron transfer,enabling unprecedented rate performance(107 mAh g^(-1)at 10 Ag^(-1))and ultralong cyclability(86.5%capacity retention after 1200 cycles at 3 A g^(-1)).Mechanistic insights reveal a distinctive“adsorption-conversion”pathway,where sulfur vacancies on exposed S-Mo-S basal planes act as preferential K^(+)adsorption sites,effectively suppressing parasitic phase transitions during intercalation.In situ X-ray diffraction and transmission electron microscopy corroborate the structural reversibility of the conversion reaction,with the carbon matrix dynamically accommodating strain while preserving electrode integrity.This work not only advances the understanding of defect-driven interfacial chemistry in conversion-type materials but also provides a versatile strategy for designing high-performance anodes in next-generation PIBs through heterostructure engineering.
基金supported by the National Natural Science Foundation of China(No.11972357)。
文摘Crossflow instability will be present when the vehicle has an angle of attack in hypersonic flow,and it might play a dominant role in hypersonic boundary layer transition.By far the mechanism of crossflow instability-induced hypersonic boundary layer transition is still out of understanding,although the large effort has been devoted.Upon this work,the overall roughness effect on instabilities in hypersonic flow was researched experimentally.Surface flush-mounted pressure sensors and infrared camera were employed to investigate the instability waves when different rough surfaces were deployed.The results reveal that the moderate surface roughness level on cone model can suppress the growth of crossflow instabilities at certain azimuthal angles in hypersonic flow.
基金funded through project NUBOLOSYTI (PID2023149972NB-100) of the Spanish Ministry of Science and Innovation (MICINN)supported by an IFUdG 2022 fellowship。
文摘The interactions between clouds and aerosols represent one of the largest uncertainties in assessing the Earth's radiation budget, highlighting the importance of research on the transition zone(TZ) within the cloud-aerosol continuum.This study assesses the global distribution of TZ conditions, analyzes its optical characteristics, and determines the cloud or aerosol types most commonly associated with them, using the cloud-aerosol discrimination(CAD) score of the CloudAerosol Lidar with Orthogonal Polarization(CALIOP) instrument on the CALIPSO satellite. The CAD score classifies clouds and aerosols by the probability density functions of attenuated backscatter, total color ratio, volume depolarization ratio, altitude, and latitude. After applying several filters to avoid artifacts, the TZ was identified as those atmospheric layers that cannot be clearly classified as clouds or aerosols, layers within the no-confidence range(NCR) of the CAD score, and cirrus fringes. The optical characteristics of NCR layers exhibit two main clusters: Cluster 1, with properties between high-altitude ice clouds and aerosols(e.g., wispy cloud fragments), and Cluster 2, with properties between water clouds and aerosols at lower altitudes(e.g., large hydrated aerosols). Our results highlight the significant ubiquity of TZ conditions, which appear in 9.5% of all profiles and comprise 6.4% of the detected layers. Cluster 1 and cirrus-fringe layers predominate near the ITCZ and in mid-latitudes, whereas Cluster 2 layers are more frequent over the oceans along the central West African and East Asian coasts, where elevated smoke and dusty marine aerosols are common.
文摘The moment a media delegation from the Republic of the Congo arrived at the Othello Kitchenware Museum on 18 November 2025,they were greeted with a vivid show of Guangdong’s industrial strength.Standing before them was not a typical exhibition hall,but a building shaped like a gleaming stainless-steel cooking pot.
基金supported by the Tianjin Education Commission Research Program Project(No.2024KJ105)。
文摘The buoyancy-induced flow constitutes a core scientific issue for thermal management of electronic devices and thermal design of energy systems,where accurate characterization of flow and heat transfer is essential to improve thermal efficiency.In this work,buoyancy-induced flow above two heating elements flush-mounted at the bottom of a square enclosure containing air is numerically investigated over a range of Rayleigh numbers(0<Ra≤1.5×10^(8)),with a focus on equal and unequal heat flux conditions under a constraint of constant total thermal energy input.Distinct flow transitions are observed in both cases,leading to the identification of three flow regimes:Steady,periodic unsteady,and chaotic unsteady.Two types of periodic flows are distinguished,in which the first is a periodic flow dominated by a fundamental frequency(FF)and its integer-multiple frequencies(INTMF),while the second is a more complex periodic flow featuring FF,INTMF,and their sub-harmonics.The transitions between these regimes are affected by the relative heat flux of the two heaters.When the heat flux of the two heaters is unequal,the range of Rayleigh numbers corresponding to periodic flow is suppressed.It is also found that the time-averaged maximum temperature of the strong heater increases more rapidly with Ra,while that of the weak heater increases more slowly,reflecting the interaction between buoyancy-driven flow dynamics and asymmetric heat input.Analysis of the time-averaged Nusselt number demonstrates that heat dissipation from the isothermal walls remains roughly equivalent,even when the heat flux of the two heaters differs by a factor of two.These findings highlight the critical roles of Rayleigh number,the number of heaters,and the heat flux ratio of the heaters in determining heat transfer and flow characteristics for buoyancy-driven convection systems,providing important theoretical support and design references for engineering scenarios such as electronic devices and design of new energy systems.
基金supported by NSFC Grants(Nos.12032004,11872114,and 11502150)Natural Science Foundation of Hebei Province of China(No.A2016210060)+1 种基金The Higher Education Youth Talents Program of Hebei Province of China(No.BJ2017052)Science and Technology Project of Hebei Education Department(No.QN2020204)。
文摘MoTe_(2) has emerged as a promising candidate in the field of integrated circuits,memristive devices,and catalysts,owing to its polymorphic nature across different phases.Experimentally,strain engineering has been demonstrated as an effective approach for manipulating the phase transition of MoTe_(2),but the mechanism remains unclear.The strain-dependent phase transition and its micro-mechanisms have been investigated based on first principle calculations.As demonstrated,critical strain and phase transition path from H→T'phases are strongly governed by the applied strain's orientation,magnitude,and triaxiality.At the atomic level,nonzero movements of Te atoms within the phase transition domain with mechanical unloading have been clarified,together with an advanced understanding on the impact of strain on Te-vacancies migration.These insights advanced the knowledge of MoTe_(2) phase transition behavior and demonstrated the large space to explore potential applications through strain,defect,and phase engineering.
文摘A flow transition prediction method for calculating effects of Reynolds numbers on aerodynamic characteristics of airfoil is developed,and the accuracy of the method is verified by wind tunnel experiment data and other calculation results.On these basics,the infrared thermal imager experiment results of the flow transition in lowspeed wind tunnel and the aerodynamic characteristics experiment results with variable Reynolds number in highspeed wind tunnel are carried out respectively,and compared with the numerical results of helicopter rotor airfoil.Specially,effects of Reynolds numbers on airfoil aerodynamic characteristics by means of flow transition under different working conditions are researched and some meaningful conclusions are obtained.The calculation method,experiment method and results as well as the flow transition analysis conclusions for aerodynamic characteristics can be used for the design of helicopter rotor airfoil,especially for the helicopters under the high altitude and low Reynolds number working conditions.
基金supported by the National Natural Science Foundation of China(grant numbers 52250357 and 52203003).
文摘The glass transition temperature(T_(g))of styrene-butadiene rubber(SBR)is a key parameter determining its low-temperature flexibility and processing performance.Accurate prediction of T_(g)is crucial formaterial design and application optimisation.Addressing the limitations of traditional experimental measurements and theoretical models in terms of efficiency,cost,and accuracy,this study proposes a machine learning prediction framework that integrates multi-model ensemble and Bayesian optimization by constructing a multi-component feature dataset and algorithm optimization strategy.Based on the constructed high-quality dataset containing 96 SBR samples,ninemachine learning models were employed to predict the T_(g)of SBR and compare their prediction performance.Ultimately,aGPR-XGBoost mixed model was constructed through model ensemble,achieving high-precision prediction with R^(2)values greater than 0.9 on both the training and test sets.Further feature attribution and local effect analysis were conducted using feature analysis methods such as SHAP and ALE,revealing the nonlinear influence patterns of various components on T_(g),providing a theoretical basis for SBR formulation design and T_(g)regulation.The machine learning prediction framework established in this study combines high-precision prediction with interpretability,significantly enhancing the prediction performance of the T_(g)of SBR.It offers an efficient tool for SBR molecular design and holds great potential for promotion and application.
基金supported by the National Natural Science Foundation of China(Grant Nos.22576126,12074394,12022508).
文摘Water molecules can form hydrogen bonds.At the solid surfaces,the preferential alignment of water molecules due to the heterogeneous atomic distributions can induce ordered hydrogen bond networks of water molecules with spatially heterogeneous patterns and slower dynamics compared to bulk water.Both the confinement and the surface atomic structures can induce the water phase transitions at low dimensional spaces.Here,we review how the phase transitions of interfacial water affect the surface physical behaviors,such as wetting,ice nucleation and the terahertz-wave-water interactions,from solid materials to the biological surfaces.These works help extend our knowledge of the physics properties of the interfacial water,particularly the multi-phase behaviors in materials and biology sciences.
基金Supported by the Projects of Medical and Health Technology Development Program in Shandong Province(No.202107021009)Shandong Provincial Traditional Chinese Medicine Science and Technology Project(No.M-2023118).
文摘AIM:To determine whether paeonol(Pae),a naturally occurring phenolic compound,can serve as an effective pharmacological inhibitor of posterior capsular opacification(PCO).METHODS:A rat model of cataract surgery—induced PCO was established,and Pae was administered via anterior chamber injection to evaluate its preventive effect on capsular opacification and fibrotic remodeling.Histological and immunohistochemical analyses were performed to assess epithelial-mesenchymal transition(EMT)—related changes in lens epithelial cells(LECs).Ex vivo lens capsule cultures were employed to examine the expression of Vimentin and Zonula Occludens-1(ZO-1)by immunofluorescence and immunohistochemistry.In the human LEC line SRA01/04,EMT marker expression at both mRNA and protein levels was analyzed following transforming growth factor beta 2(TGF-β2)stimulation,with Pae treatment.Western blotting and immunofluorescence were used to investigate the effect of Pae on TGF-β/Smad signaling and AMP-activated protein kinase(AMPK)activation.Molecular docking was performed to predict Pae–AMPK binding,and rescue experiments with AMPK inhibition were conducted to validate the mechanistic pathway.RESULTS:Pae significantly reduced capsular opacification and fibrotic remodeling in the rat PCO model compared with controls.In LECs,Pae markedly suppressed TGF-β2–induced EMT,evidenced by decreased expression of mesenchymal markers,such as Vimentin,Fibronectin,Collagen 1A1,α-SMA and preserved epithelial junctional protein ZO-1.Mechanistically,Pae was predicted to directly interact with the catalytic pocket of AMPK,which was experimentally confirmed by enhanced AMPK phosphorylation and nuclear translocation(P<0.05).This activation disrupted canonical TGF-β/Smad signaling,leading to suppression of EMT.Rescue experiments using AMPK inhibition abrogated the anti-EMT effect of Pae,further validating the AMPK-dependent mechanism.CONCLUSION:Pae exerts a potent inhibitory effect on PCO formation by blocking EMT of LECs through direct activation of AMPK and subsequent disruption of TGF-β/Smad signaling.
基金Under the auspices of the National Natural Science Foundation of China(No.42271224,41901193)Ministry of Edu cation Humanities and Social Sciences Research Planning Fund Project of China(No.24YJAZH190)+1 种基金Anhui Province Excellent Youth Research Project in Universities(No.2022AH030019)Anhui Social Sciences Innovation Development Research Project(No.2024CXQ503)。
文摘The accessibility of urban public transit directly influences residents’quality of life,travel behavior,and social equity.Its correlation with housing prices has garnered significant attention across disciplines such as geography,economics,and urban planning.Although much existing research focuses on the impact of individual transportation facilities on housing prices,there is a notable gap in comprehensive analyses that assess the influence of overall urban transit accessibility on housing market dynamics.This study selected the main urban area of Hefei,China,as a case to investigate the spatial distribution of housing prices and evaluate public transit accessibility in 2022.Employing techniques such as the optimized parameter geographical detector and local spatial regression models,the study aimed to elucidate the effects and underlying mechanisms of urban transit accessibility on housing prices.The findings revealed that:1)housing prices in Hefei exhibited a clustered spatial pattern,with high prices concentrated in the city center and lower prices in peripheral areas,forming three distinct high-price hotspots with a‘belt-like’distribution;2)public transit accessibility showed a‘coreperiphery’structure,with accessibility declining in a‘circumferential’pattern around the city center.Based on the‘housing price-accessibility’dimension,four categories were identified:high price-high accessibility(37.25%),high price-low accessibility(19.07%),low price-high accessibility(21.95%),and low price-low accessibility(21.73%);3)the impact of transit accessibility on housing prices was spatially heterogeneous,with bus travel showing the strongest explanatory power(0.692),followed by automobile,subway,and bicycle travel.The interaction of these transportation modes generated a synergistic effect on housing price differentiation,with most influencing factors contributing more than 25%.These findings offer valuable insights for optimizing the spatial distribution of public transit infrastructure and improving both urban housing quality and residents’living standards.
文摘In Chin.Phys.B 34114704(2025),Eq.(7)and the associated unit notation were incorrect.The correct ones are present here.Since Eq.(7)is an in-built expression in the simulation package,the correction is purely typographical and does not affect the simulation procedure,numerical results,or the conclusions.
基金supported by the National Key Research and Development program(2022YFA1504000)the National Natural Science Foundation of China(22302101)+4 种基金the Fundamental Research Funds for the Central Universities(63185015)the Shenzhen Science and Technology Program(JCYJ20210324121002007,JCYJ20230807151503007)the Yunnan Provincial Science and Technology Project at Southwest United Graduate School(202402AO370001)the China Postdoctoral Science Foundation(2022M721699)the Guangdong Basic and Applied Basic Research Foundation(2024A1515010347).
文摘During the oxygen evolution reaction(OER),reconstruction of transition metal sulfides(TMSs)is inevitable.However,the lack of a clear theoretical understanding of this process has impeded the development of effective reconstruction regulation strategies.In this study,we first explored the reconstruction mechanism of CoS_(2)during OER from the perspective of electronic structure and identified two possible pathways:the OH-assisted mechanism and the O-assisted mechanism.Further verification showed that these mechanisms are universally applicable to other TMSs(e.g.,FeS_(2)).Based on the reconstruction mechanism,we investigated the basic reasons for the influence of various regulation strategies,such as vacancy modification and facet engineering,on the reconstruction ability.This verified that the method of analyzing the change in the reconstruction ability of catalysts based on the reconstruction mechanism has a high degree of applicability.Importantly,we proposed a core regulation strategy:the coordination symmetry regulation strategy.Specifically,by breaking the symmetry of the surface coordination environment of TMSs(such as introducing heteroatom doping or strain),the reconstruction process will be facilitated.Our findings provide a comprehensive mechanistic explanation for the reconstruction of TMS catalysts and offer a new idea for the rational design of OER catalysts with controllable reconstruction capacity.
