Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenati...Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenation and C–C coupling limit the C_(2)H_(4)generation.Herein,CuxP/g-C_(3)N_(4) heterojunction prepared by an in-situ phosphating technique,achieved collaborative photocatalytic CO_(2) and H2O,producing CO and C_(2)H_(4)as the main products.Notably,the selectivity of C_(2)H_(4)produced by CuxP/g-C_(3)N_(4) attained to 64.25%,which was 9.85 times that of CuxP(6.52%).Detailed time-resolution photoluminescence spectra,femtosecond transient absorption spectroscopy tests and density functional theory(DFT)calculation validate the ultra-fast interfacial electron transfer mechanism in CuxP/g-C_(3)N_(4) heterojunction.Successive*H on P sites caused by adsorbed H2O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO_(2)RR process over CuxP/g-C_(3)N_(4).With the aid of mediated asymmetric Cu and P dual sites by g-C_(3)N_(4) nanosheet,the produced*CHO shows an energetically favorable for C–C coupling.The coupling formed*CHOCHO further accepts photoexcited efficient e–and*H to deeply produce C_(2)H_(4)according to the C^(2+)intermediates,which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation.The novel insight mechanism offers an essential understanding for the development of CuxP-based heterojunctions for photocatalytic CO_(2) to C^(2+)value-added fuels.展开更多
Copper(Cu)-based catalysts show significant potential for producing high value-added C_(2+)products in electrocatalytic CO_(2)/CO reduction reactions(CO(2)RR).However,the structural reconfiguration during operation po...Copper(Cu)-based catalysts show significant potential for producing high value-added C_(2+)products in electrocatalytic CO_(2)/CO reduction reactions(CO(2)RR).However,the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site,especially under similar mass transport conditions.Herein,three typical and commercial Cu-based catalysts(Cu,CuO,and Cu_(2)O)are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer.Notably,only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction,thus achieving the highest FE of 86.7% for C_(2+)products at a current density of 500 mA cm^(-2) and maintaining a stable electrolysis over 110 h at a current of 200 mA cm^(-2).The influence of chemical valence state of Cu,electrochemical surface area,and local pH were firstly investigated and ruled out for the significant FE differences.Finally,based on the structure analysis from high resolution transmission electron microscope,OH-adsorption,in situ infrared spectroscopy and density functional theory calculations,it is suggested that the asymmetric C-C coupling(via ^(*)CHO and ^(*)CO)is the most probable reaction pathway for forming C_(2+)products,with Cu(100)-dominant grain boundaries(GBs)being the most favorable active sites.These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.展开更多
A thoroughly mechanistic understanding of the electrochemical CO reduction reaction(eCORR)at the interface is significant for guiding the design of high-performance electrocatalysts.However,unintentionally ignored fac...A thoroughly mechanistic understanding of the electrochemical CO reduction reaction(eCORR)at the interface is significant for guiding the design of high-performance electrocatalysts.However,unintentionally ignored factors or unreasonable settings during mechanism simulations will result in false positive results between theory and experiment.Herein,we computationally identified the dynamic site preference change of CO adsorption with potentials on Cu(100),which was a previously unnoticed factor but significant to potential-dependent mechanistic studies.Combined with the different lateral interactions among adsorbates,we proposed a new C–C coupling mechanism on Cu(100),better explaining the product distribution at different potentials in experimental eCORR.At low potentials(from–0.4 to–0.6 V_(RHE)),the CO forms dominant adsorption on the bridge site,which couples with another attractively aggregated CO to form a C–C bond.At medium potentials(from–0.6 to–0.8 VRHE),the hollow-bound CO becomes dominant but tends to isolate with another adsorbate due to the repulsion,thereby blocking the coupling process.At high potentials(above–0.8 VRHE),the CHO intermediate is produced from the electroreduction of hollow-CO and favors the attraction with another bridge-CO to trigger C–C coupling,making CHO the major common intermediate for C–C bond formation and methane production.We anticipate that our computationally identified dynamic change in site preference of adsorbates with potentials will bring new opportunities for a better understanding of the potential-dependent electrochemical processes.展开更多
Research interest in the electrochemical reduction reaction of carbon dioxide(CO_(2)RR)into multicarbon(C_(2+))compounds has been growing significantly with numerous theoretical and experimental studies employing a va...Research interest in the electrochemical reduction reaction of carbon dioxide(CO_(2)RR)into multicarbon(C_(2+))compounds has been growing significantly with numerous theoretical and experimental studies employing a variety of surface modification techniques,such as strong support interactions,heteroatom doping,surface functionalization,and morphology and defect engineering.The collective goal of these strategies is to fine-tune the electrochemical properties of catalysts,thereby breaking the C-C coupling barrier to achieve efficient and selective formation of C_(2+)products.In this review,we critically examine these research efforts,with a particular focus on achieving a comprehensive understanding of the innovative catalyst surface that dictates pathways for electrochemical CO_(2)RR to C_(2+)compounds.We begin by discussing the essential characteristics of catalyst surfaces that demonstrate superior catalytic activity and selectivity.Next,we explore the range of strategies used to create conducive catalyst surfaces.Finally,we provide an overview of catalytic performance and selectivity of materials in synthesizing C_(2+)products based on some high-throughput density functional theory and machine learning screening techniques.展开更多
The copper-based electrocatalysts feature attractive potentials of converting CO_(2)into multi-carbon(C_(2+))products,while the instability of Cu-O often induces the reduction of Cu^(+)/Cu^(0) catalytic sites at the c...The copper-based electrocatalysts feature attractive potentials of converting CO_(2)into multi-carbon(C_(2+))products,while the instability of Cu-O often induces the reduction of Cu^(+)/Cu^(0) catalytic sites at the cathode and refrains the capability of stable electrolysis especially at high powers.In this work,we developed an Erbium(Er)oxide-modified Cu(Er-O-Cu)catalyst with enhanced covalency of Cu-O and more stable active sites.The f-p-d coupling strengthens the covalency of Cu-O,and the stability of Cu^(+)sites under electroreduction condition is critical for promoting the C-C coupling and improving the C_(2+)product selectivity.As a result,the Er-O-Cu sites exhibited a high Faradaic efficiency of C_(2+)products(FEC_(2+))of 86%at 2200 mA cm^(-2),and a peak partial current density of|j_(C2+)|of 1900 mA cm^(-2),comparable to the best reported values for the CO_(2)-to-C_(2+)electroreduction.The CO_(2)electrolysis by the Er-O-Cu sites was further scaled up to 100 cm^(2)to achieve high-power(~200 W)electrolysis with ethylene production rate of 16 mL min^(-1).展开更多
Electrochemical carbon dioxide reduction reaction(CO_(2)RR)produces valuable chemicals by consuming gaseous CO_(2)as well as protons from the electrolyte.Protons,produced by water dissociation in alkaline electrolyte,...Electrochemical carbon dioxide reduction reaction(CO_(2)RR)produces valuable chemicals by consuming gaseous CO_(2)as well as protons from the electrolyte.Protons,produced by water dissociation in alkaline electrolyte,are critical for the reaction kinetics which involves multiple proton coupled electron transfer steps.Herein,we demonstrate that the two key steps(CO_(2)-^(*)COOH and^(*)CO-^(*)COH)efficiency can be precisely tuned by introducing proper amount of water dissociation center,i.e.,Fe single atoms,locally surrounding the Cu catalysts.In alkaline electrolyte,the Faradaic efficiency(FE)of multi-carbon(C^(2+))products exhibited a volcano type plot depending on the density of water dissociation center.A maximum FE for C^(2+)products of 73.2%could be reached on Cu nanoparticles supported on N-doped Carbon nanofibers with moderate Fe single atom sites,at a current density of 300 mA cm^(–2).Experimental and theoretical calculation results reveal that the Fe sites facilitate water dissociation kinetics,and the locally generated protons contribute significantly to the CO_(2)activation and^(*)CO protonation process.On the one hand,in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(in-situ ATR-SEIRAS)clearly shows that the^(*)COOH intermediate can be observed at a lower potential.This phenomenon fully demonstrates that the optimized local water dissociation kinetics has a unique advantage in guiding the hydrogenation reaction pathway of CO₂molecules and can effectively reduce the reaction energy barrier.On the other hand,abundant^(*)CO and^(*)COH intermediates create favorable conditions for the asymmetric^(*)CO-^(*)COH coupling,significantly increasing the selectivity of the reaction for C^(2+)products and providing strong support for the efficient conversion of related reactions to the target products.This work provides a promising strategy for the design of a dual sites catalyst to achieve high FE of C^(2+)products through the optimized local water dissociation kinetics.展开更多
Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing het...Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.展开更多
A fundamental study on C-C coupling,that is the crucial step in the Fischer-Tropsch synthesis(FTS)process to obtain multi-carbon products,is of great importance to tailor catalysts and then guide a more promising path...A fundamental study on C-C coupling,that is the crucial step in the Fischer-Tropsch synthesis(FTS)process to obtain multi-carbon products,is of great importance to tailor catalysts and then guide a more promising pathway.It has been demonstrated that the coupling of CO with the metal carbide can represent the early stage in the FTS process,while the related mechanism is elusive.Herein,the reactions of the CuC3H-and CuC3-cluster anions with CO have been studied by using mass spectrometry and theoretical calculations.The experimental results showed that the coupling of CO with the C3H-moiety of CuC3H can generate the exclusive ion product COC3H-.The reactivity and selectivity of this reaction of CuC3H-with CO are greatly higher than that of the reaction of CuC3-with CO,and this H-assisted C-C coupling process was rationalized by theoretical calculations.展开更多
Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a...Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.展开更多
Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O cr...Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.展开更多
Photo-reforming methanol into valuable chemicals represents an energetically sustainable alternative to conventional thermal catalysis,yet controlling-specific C-C coupling way still remains elusive.In this work,we re...Photo-reforming methanol into valuable chemicals represents an energetically sustainable alternative to conventional thermal catalysis,yet controlling-specific C-C coupling way still remains elusive.In this work,we report a sulfide-based photocatalytic paradigm,where atomic-level control of nickel species directly dictates reaction selectivity.The electrostatic constructing ZnIn_(2)S_(4)/Zn_(0.5)Cd_(0.5)S(ZIS/ZCS)heterostructures enable single atom Ni to facilitate ethylene glycol(EG)production with a rate of 11.2 mmol·gcat^(−1)·h^(−1),surpassing reported non-precious metal systems,whereas the Ni aggregates drive exclusive formaldehyde formation.The operando spectroscopy and density functional theory reveal dual roles of Ni as electron reservoir and chemical bond breakage inducers,lowering C-H activation barriers while stabilizing·CH2OH intermediates for cross-coupling.This interfacial configuration engineering creates an electron highway that couples carrier dissociation with radical recombination kinetics,achieving atom-economic steering of methanol oxidative valorization.The metal dispersion assisting catalysis correlation here provides a design blueprint for selective bond scission and reconstruction in sustainable organic synthesis.展开更多
The coupling reactions of methanol and long-chain alkanes(n-dodecane,n-tetradecane and n-hexadecane)over CHA-type molecular sieves were studied in a fixed bed reactor.Over SAPO-34 and SSZ-13,it was found that the indu...The coupling reactions of methanol and long-chain alkanes(n-dodecane,n-tetradecane and n-hexadecane)over CHA-type molecular sieves were studied in a fixed bed reactor.Over SAPO-34 and SSZ-13,it was found that the induction period of methanol conversion was shortened by the introduction of long-chain alkanes.However,the addition of long-chain alkanes had little influence on the product distribution.Polymethylbenzenes and the derivatives were the main retained species on spent SSZ-13 catalyst,while adamantanes were the main retained species on SAPO-34.This indicates that coking species formation was mainly related to the further transformation of long-chain alkane/methanol coupling products at acid sites of the molecular sieve.These findings provide valuable information of long chain alkanes conversion and methanol reaction behavior of induction period over small pore CHA molecular sieves.展开更多
Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)...Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)bond construction often rely on expensive and scarce transition metal catalysts,raising concerns about sustainability and environmental impact.To address these challenges,we develop a bifunctional photocatalyst,phloroglucinol carbon quantum dot(PG-CQD).It facilitates catalytic transfer hydrogenation(CTH)with IPA as the hydrogen donor.PG-CQDs exhibit both dehydrogenation and reduction activities,enabling the formation of vicinal diols under mild conditions with visible light irradiation.We propose a CTH mechanism that has been successfully validated through experiments.The catalytic system demonstrates remarkable versatility,enabling the synthesis of various vicinal diols from diverseα-keto ester substrates with good or excellent yields.These findings offer a sustainable synthetic strategy that aligns with green chemistry principles and establish a promising pathway for the development of environmentally benign and energy-efficient organic transformations.展开更多
Wire arc additive manufacturing(WAAM)has emerged as a promising approach for fabricating large-scale components.However,conventional WAAM still faces challenges in optimizing microstructural evolution,minimizing addit...Wire arc additive manufacturing(WAAM)has emerged as a promising approach for fabricating large-scale components.However,conventional WAAM still faces challenges in optimizing microstructural evolution,minimizing additive-induced defects,and alleviating residual stress and deformation,all of which are critical for enhancing the mechanical performance of the manufactured parts.Integrating interlayer friction stir processing(FSP)into WAAM significantly enhances the quality of deposited materials.However,numerical simulation research focusing on elucidating the associated thermomechanical coupling mechanisms remains insufficient.A comprehensive numerical model was developed to simulate the thermomechanical coupling behavior in friction stir-assisted WAAM.The influence of post-deposition FSP on the coupled thermomechanical response of the WAAM process was analyzed quantitatively.Moreover,the residual stress distribution and deformation behavior under both single-layer and multilayer deposition conditions were investigated.Thermal analysis of different deposition layers in WAAM and friction stir-assisted WAAM was conducted.Results show that subsequent layer deposition induces partial remelting of the previously solidified layer,whereas FSP does not cause such remelting.Furthermore,thermal stress and deformation analysis confirm that interlayer FSP effectively mitigates residual stresses and distortion in WAAM components,thereby improving their structural integrity and mechanical properties.展开更多
This study aims to promote the optimization and upgrading of the economic structure in rural areas of China by focusing on the coupling coordination mechanism between digital economy–agriculture integration and rural...This study aims to promote the optimization and upgrading of the economic structure in rural areas of China by focusing on the coupling coordination mechanism between digital economy–agriculture integration and rural revitalization.By examining panel data from 30 Chinese provinces,autonomous regions,and municipalities between 2011 and 2022,the research constructs a weight-based evaluation system that integrates subjective and objective methods and a coupling coordination model to reveal its dynamic evolution patterns.Key findings indicate that digital economy–agriculture integration and rural revitalization achieve cross-coupling through critical activities.The impact of digital-agriculture integration on advancing rural revitalization lags by 2–3 years.Although the coupling development degree between the two systems continues to improve,it remains at the stage of primary coordination.Regional disparities are significant,showing a gradient pattern of“high degree of coupling development in the east and low degree of coupling development in the west.”展开更多
Multilayer complex dynamical networks,characterized by the intricate topological connections and diverse hierarchical structures,present significant challenges in determining complete structural configurations due to ...Multilayer complex dynamical networks,characterized by the intricate topological connections and diverse hierarchical structures,present significant challenges in determining complete structural configurations due to the unique functional attributes and interaction patterns inherent to different layers.This paper addresses the critical question of whether structural information from a known layer can be used to reconstruct the unknown intralayer structure of a target layer within general weighted output-coupling multilayer networks.Building upon the generalized synchronization principle,we propose an innovative reconstruction method that incorporates two essential components in the design of structure observers,the cross-layer coupling modulator and the structural divergence term.A key advantage of the proposed reconstruction method lies in its flexibility to freely designate both the unknown target layer and the known reference layer from the general weighted output-coupling multilayer network.The reduced dependency on full-state observability enables more deployment in engineering applications with partial measurements.Numerical simulations are conducted to validate the effectiveness of the proposed structure reconstruction method.展开更多
The F_(1)-ATPase and V_(1)-ATPase are rotary biomotors.Alignment of their amino acid sequences,which originate from bovine heart mitochondria(1BMF)and Enterococcus hirae(3VR6),respectively,demonstrates that the segmen...The F_(1)-ATPase and V_(1)-ATPase are rotary biomotors.Alignment of their amino acid sequences,which originate from bovine heart mitochondria(1BMF)and Enterococcus hirae(3VR6),respectively,demonstrates that the segment forming the ATP catalytic pocket is highly conserved.Single-molecule experiments,however,have revealed subtle differences in efficiency between the F_(1) and V_(1) motors.Here,we perform both atomistic and coarse-grained molecular dynamics simulations to investigate the mechanochemical coupling and coordination in F_(1) and V_(1) ATPase.Our results show that the correlation between conformational changes in F_(1) is stronger than that in V_(1),indicating that the mechanochemical coupling in F_(1) is tighter than in V_(1).Moreover,the unidirectional rotation of F_(1) is more processive than that of V_(1),which accounts for the higher efficiency observed in F_(1) and explains the occasional backward steps detected in single-molecule experiments on V_(1).展开更多
The coupling effects among the flow field,temperature distribution and structural deformation in a turbine cannot be ignored,particularly during flight cycles when the turbine experiences varied operational states.Rel...The coupling effects among the flow field,temperature distribution and structural deformation in a turbine cannot be ignored,particularly during flight cycles when the turbine experiences varied operational states.Relying solely on steady-state solutions cannot predict the detrimental effects caused by hysteresis.Consequently,this paper employs a quasi-steady-state fluid-thermalstructure multidisciplinary coupling solution method,integrating transient solid heat conduction with steady-state flow field and static structural deformation solutions.After conducting a numerical simulation of a three-dimensional,five-stage,low-pressure turbine air system,the following conclusions are drawn:when boundary conditions attain high-power states through processes that are numerically identical but in opposite directions,slight variations in solid deformation significantly impact the flow field;when boundary conditions attain high-power states through processes that are directionally consistent but have different numerical values,the influence of the boundary condition change rate on the flow field surpasses that of solid deformation.In terms of turbine design parameters,a large difference in stage-reaction between adjacent stages at the lower radius of the turbine can lead to significant changes in the disc cavity flow field during flight cycles.The difference in the stage-reaction of 0.23 at 10%blade height in adjacent stages may induce severe gas ingress in the stator disc cavity.Thus,it is crucial to minimize this difference and to appropriately extend the duration of the deceleration phase to ensure the turbine's safe operation.展开更多
Based on the Smit-Suhl formula,we propose a universal approach for solving the magnon-magnon coupling problem in bilayer coupled systems(e.g.,antiferromagnets).This method requires only the energy expression,enabling ...Based on the Smit-Suhl formula,we propose a universal approach for solving the magnon-magnon coupling problem in bilayer coupled systems(e.g.,antiferromagnets).This method requires only the energy expression,enabling the automatic derivation of analytical expressions for the eigenmatrix elements via symbolic computation,eliminating the need for tedious manual calculations.Using this approach,we investigate the impact of magnetic hysteresis on magnon-magnon coupling in a system with interlayer Dzyaloshinskii-Moriya interaction(DMI).The magnetic hysteresis leads to an asymmetric magnetic field dependence of the resonance frequency and alters the number of degeneracy points between the pure optical and acoustic modes.Moreover,it can result in the coupling strength at the gap of the f–H phase diagram being nearly vanishing,contrary to the conventionally expected maximum.These results deepen the understanding of the effect of interlayer DMI on magnon–magnon coupling and the proposed universal method significantly streamlines the solving process of magnon–magnon coupling problems.展开更多
This study presents an implicit multiphysics coupling method integrating Computational Fluid Dynamics(CFD),the Multiphase Particle-in-Cell(MPPIC)model,and the Finite Element Method(FEM),implemented with OpenFOAM,Calcu...This study presents an implicit multiphysics coupling method integrating Computational Fluid Dynamics(CFD),the Multiphase Particle-in-Cell(MPPIC)model,and the Finite Element Method(FEM),implemented with OpenFOAM,CalculiX,and preCICE to simulate fluid-particle-structure interactions with large deformations.Mesh motion in the fluid field is handled using the radial basis function(RBF)method.The particle phase is modeled by MPPIC,where fluid-particle interaction is described through momentum exchange,and inter-particle collisions are characterized by collision stress.The structural field is solved by nonlinear FEM to capture large deformations induced by geometric nonlinearity.Coupling among fields is realized through a partitioned,parallel,and non-intrusive iterative strategy,ensuring stable transfer and convergence of interface forces and displacements.Notably,the influence of particles on the structure is not direct but mediated by the fluid,while structural motion directly affects particle dynamics.The results demonstrate that the proposed approach effectively captures multiphysics interaction processes and provides a valuable reference for numerical modeling of coupled fluid-particle-structure systems.展开更多
文摘Light-driven CO_(2) reduction reaction(CO_(2)RR)to value-added ethylene(C2H4)holds significant promise for addressing energy and environmental challenges.While the high energy barriers for*CO intermediates hydrogenation and C–C coupling limit the C_(2)H_(4)generation.Herein,CuxP/g-C_(3)N_(4) heterojunction prepared by an in-situ phosphating technique,achieved collaborative photocatalytic CO_(2) and H2O,producing CO and C_(2)H_(4)as the main products.Notably,the selectivity of C_(2)H_(4)produced by CuxP/g-C_(3)N_(4) attained to 64.25%,which was 9.85 times that of CuxP(6.52%).Detailed time-resolution photoluminescence spectra,femtosecond transient absorption spectroscopy tests and density functional theory(DFT)calculation validate the ultra-fast interfacial electron transfer mechanism in CuxP/g-C_(3)N_(4) heterojunction.Successive*H on P sites caused by adsorbed H2O splitting with moderate hydrogenation ability enables the multi-step hydrogenation during CO_(2)RR process over CuxP/g-C_(3)N_(4).With the aid of mediated asymmetric Cu and P dual sites by g-C_(3)N_(4) nanosheet,the produced*CHO shows an energetically favorable for C–C coupling.The coupling formed*CHOCHO further accepts photoexcited efficient e–and*H to deeply produce C_(2)H_(4)according to the C^(2+)intermediates,which has been detected by in-situ diffuse reflectance infrared Fourier transform spectroscopy and interpreted by DFT calculation.The novel insight mechanism offers an essential understanding for the development of CuxP-based heterojunctions for photocatalytic CO_(2) to C^(2+)value-added fuels.
文摘Copper(Cu)-based catalysts show significant potential for producing high value-added C_(2+)products in electrocatalytic CO_(2)/CO reduction reactions(CO(2)RR).However,the structural reconfiguration during operation poses substantial challenges in identifying the intrinsic catalytic active site,especially under similar mass transport conditions.Herein,three typical and commercial Cu-based catalysts(Cu,CuO,and Cu_(2)O)are chosen as representatives to elucidate the structure-activity relationship of CORR in the membrane electrode assembly electrolyzer.Notably,only the Cu catalyst demonstrates the most suppression of hydrogen evolution reaction,thus achieving the highest FE of 86.7% for C_(2+)products at a current density of 500 mA cm^(-2) and maintaining a stable electrolysis over 110 h at a current of 200 mA cm^(-2).The influence of chemical valence state of Cu,electrochemical surface area,and local pH were firstly investigated and ruled out for the significant FE differences.Finally,based on the structure analysis from high resolution transmission electron microscope,OH-adsorption,in situ infrared spectroscopy and density functional theory calculations,it is suggested that the asymmetric C-C coupling(via ^(*)CHO and ^(*)CO)is the most probable reaction pathway for forming C_(2+)products,with Cu(100)-dominant grain boundaries(GBs)being the most favorable active sites.These findings provide deeper insights into the synergistic relationship between crystal facets and GBs in electrocatalytic systems.
文摘A thoroughly mechanistic understanding of the electrochemical CO reduction reaction(eCORR)at the interface is significant for guiding the design of high-performance electrocatalysts.However,unintentionally ignored factors or unreasonable settings during mechanism simulations will result in false positive results between theory and experiment.Herein,we computationally identified the dynamic site preference change of CO adsorption with potentials on Cu(100),which was a previously unnoticed factor but significant to potential-dependent mechanistic studies.Combined with the different lateral interactions among adsorbates,we proposed a new C–C coupling mechanism on Cu(100),better explaining the product distribution at different potentials in experimental eCORR.At low potentials(from–0.4 to–0.6 V_(RHE)),the CO forms dominant adsorption on the bridge site,which couples with another attractively aggregated CO to form a C–C bond.At medium potentials(from–0.6 to–0.8 VRHE),the hollow-bound CO becomes dominant but tends to isolate with another adsorbate due to the repulsion,thereby blocking the coupling process.At high potentials(above–0.8 VRHE),the CHO intermediate is produced from the electroreduction of hollow-CO and favors the attraction with another bridge-CO to trigger C–C coupling,making CHO the major common intermediate for C–C bond formation and methane production.We anticipate that our computationally identified dynamic change in site preference of adsorbates with potentials will bring new opportunities for a better understanding of the potential-dependent electrochemical processes.
基金financial support from the National Natural Science Foundation of China(grant no.22373027)。
文摘Research interest in the electrochemical reduction reaction of carbon dioxide(CO_(2)RR)into multicarbon(C_(2+))compounds has been growing significantly with numerous theoretical and experimental studies employing a variety of surface modification techniques,such as strong support interactions,heteroatom doping,surface functionalization,and morphology and defect engineering.The collective goal of these strategies is to fine-tune the electrochemical properties of catalysts,thereby breaking the C-C coupling barrier to achieve efficient and selective formation of C_(2+)products.In this review,we critically examine these research efforts,with a particular focus on achieving a comprehensive understanding of the innovative catalyst surface that dictates pathways for electrochemical CO_(2)RR to C_(2+)compounds.We begin by discussing the essential characteristics of catalyst surfaces that demonstrate superior catalytic activity and selectivity.Next,we explore the range of strategies used to create conducive catalyst surfaces.Finally,we provide an overview of catalytic performance and selectivity of materials in synthesizing C_(2+)products based on some high-throughput density functional theory and machine learning screening techniques.
基金the National Key Research and Development Program of China(2024YFB4106400,2024YFB4106401)the National Natural Science Foundation of China(22025502,U23A20552)。
文摘The copper-based electrocatalysts feature attractive potentials of converting CO_(2)into multi-carbon(C_(2+))products,while the instability of Cu-O often induces the reduction of Cu^(+)/Cu^(0) catalytic sites at the cathode and refrains the capability of stable electrolysis especially at high powers.In this work,we developed an Erbium(Er)oxide-modified Cu(Er-O-Cu)catalyst with enhanced covalency of Cu-O and more stable active sites.The f-p-d coupling strengthens the covalency of Cu-O,and the stability of Cu^(+)sites under electroreduction condition is critical for promoting the C-C coupling and improving the C_(2+)product selectivity.As a result,the Er-O-Cu sites exhibited a high Faradaic efficiency of C_(2+)products(FEC_(2+))of 86%at 2200 mA cm^(-2),and a peak partial current density of|j_(C2+)|of 1900 mA cm^(-2),comparable to the best reported values for the CO_(2)-to-C_(2+)electroreduction.The CO_(2)electrolysis by the Er-O-Cu sites was further scaled up to 100 cm^(2)to achieve high-power(~200 W)electrolysis with ethylene production rate of 16 mL min^(-1).
文摘Electrochemical carbon dioxide reduction reaction(CO_(2)RR)produces valuable chemicals by consuming gaseous CO_(2)as well as protons from the electrolyte.Protons,produced by water dissociation in alkaline electrolyte,are critical for the reaction kinetics which involves multiple proton coupled electron transfer steps.Herein,we demonstrate that the two key steps(CO_(2)-^(*)COOH and^(*)CO-^(*)COH)efficiency can be precisely tuned by introducing proper amount of water dissociation center,i.e.,Fe single atoms,locally surrounding the Cu catalysts.In alkaline electrolyte,the Faradaic efficiency(FE)of multi-carbon(C^(2+))products exhibited a volcano type plot depending on the density of water dissociation center.A maximum FE for C^(2+)products of 73.2%could be reached on Cu nanoparticles supported on N-doped Carbon nanofibers with moderate Fe single atom sites,at a current density of 300 mA cm^(–2).Experimental and theoretical calculation results reveal that the Fe sites facilitate water dissociation kinetics,and the locally generated protons contribute significantly to the CO_(2)activation and^(*)CO protonation process.On the one hand,in-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(in-situ ATR-SEIRAS)clearly shows that the^(*)COOH intermediate can be observed at a lower potential.This phenomenon fully demonstrates that the optimized local water dissociation kinetics has a unique advantage in guiding the hydrogenation reaction pathway of CO₂molecules and can effectively reduce the reaction energy barrier.On the other hand,abundant^(*)CO and^(*)COH intermediates create favorable conditions for the asymmetric^(*)CO-^(*)COH coupling,significantly increasing the selectivity of the reaction for C^(2+)products and providing strong support for the efficient conversion of related reactions to the target products.This work provides a promising strategy for the design of a dual sites catalyst to achieve high FE of C^(2+)products through the optimized local water dissociation kinetics.
基金financially supported by the National Natural Science Foundation of China(No.22305101)the Natural Science Foundation of Jiangsu Province(No.BK20231032)+2 种基金the Special Fund Project of Jiangsu Province for Scientific and Technological Innovation in Carbon Peaking and Carbon Neutrality(No.BK20220023)the Fundamental Research Funds for the Central Universities(No.JUSRP123020)the Startup Funding at Jiangnan University(No.1045219032220100)。
文摘Engineering the desired dual metal sites to realize C-C coupling of CO_(2)is of great importance for the practical applications of CO_(2)electroreduction reaction(CER).Herein,an efficient strategy for constructing heterogeneous Pt^(δ+)-Cu^(δ+)dual sites to strengthen the generation and coupling of*CO and*CHO(or*COH)during CER process is presented in this work.The radiilarger Pt not only stabilizes the Cu^(δ+)ut also induces a tensile strain in Pt^(δ+)-Cu^(δ+)dual sites.The obtained Pt^(δ+)-Cu^(δ+)dual sites achieve a total Faradaic efficiency and current density of C2products with 70.9%and586.9 mA·cm-2at-1.20 V(vs.RHE),which is higher than that of Cu^(δ+)single site(55.4%,286.9 mA·cm^(-2)).The in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy(ATR-SEIRAS)reveals that the Pt^(δ+)-Cu^(δ+)dual sites can promote the generation of C1intermediates(such as*CO,*COOH,*COH,and*CHO)and C-C coupling.Additional in situ surface-enhanced Raman spectra demonstrate that Pt^(δ+)Cu^(δ+)dual sites can induce the generation of the high-frequency peak for*CO_(atop),thus accelerating the C-C coupling.This work provides a promising avenue for stabilizing and enhancing the performance of Cu^(δ+)sites toward CER.
基金supported by the National Natural Science Foundation of China(No.21773254)the Youth Innovation Promotion Association Chinese Academy of Sciences(No.2016030)。
文摘A fundamental study on C-C coupling,that is the crucial step in the Fischer-Tropsch synthesis(FTS)process to obtain multi-carbon products,is of great importance to tailor catalysts and then guide a more promising pathway.It has been demonstrated that the coupling of CO with the metal carbide can represent the early stage in the FTS process,while the related mechanism is elusive.Herein,the reactions of the CuC3H-and CuC3-cluster anions with CO have been studied by using mass spectrometry and theoretical calculations.The experimental results showed that the coupling of CO with the C3H-moiety of CuC3H can generate the exclusive ion product COC3H-.The reactivity and selectivity of this reaction of CuC3H-with CO are greatly higher than that of the reaction of CuC3-with CO,and this H-assisted C-C coupling process was rationalized by theoretical calculations.
基金the National Natural Science Foundation of China(51303083)the National Natural Science Foundation of China for Excellent Young Scholars(51922050)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20191293)the Fundamental Research Funds for the Central Universities(30920021123)。
文摘Photothermal catalytic CO_(2) conversion provides an effective solution targeting carbon neutrality by synergistic utilization of photon and heat.However,the C-C coupling initiated by photothermal catalysis is still a big challenge.Herein,a three-dimensional(3D)hierarchical W_(18)O_(49)/WTe_(2) hollow nanosphere is constructed through in-situ embodying of oxygen vacancy and tellurium on the scaffold of WO_(3).The light absorption towards near-infrared spectral region and CO_(2) adsorption are enhanced by the formation of half-metal WTe_(2) and the unique hierarchical hollow architecture.Combining with the generation of oxygen vacancy with strengthened CO_(2) capture,the photothermal effect on the samples can be sufficiently exploited for activating the CO_(2) molecules.In particular,the close contact between W_(18)O_(49)and WTe_(2) largely promotes the photoinduced charge separation and mass transfer,and thus the~*CHO intermediate formation and fixedness are facilitated.As a result,the C-C coupling can be evoked between tungsten and tellurium atoms on WTe_(2).The ethylene production by optimized W_(18)O_(49)/WTe_(2) reaches 147.6μmol g^(-1)with the selectivity of 80%.The in-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)calculations are performed to unveil the presence and significance of aldehyde intermediate groups in C-C coupling.The half-metallic WTe_(2) cocatalyst proposes a new approach for efficient CO_(2) conversion with solar energy,and may especially create a new platform for the generation of multi-carbon products.
基金the financial support from the National Natural Science Foundation of China (Nos.U23A20677,22022610 and 52400137)"Pioneer" and "Leading Goose" R&D Program of Zhejiang (Nos.2022C03146 and 2023C03017)+2 种基金China Postdoctoral Science Foundation (No.2024T170805)Zhejiang Provincial Natural Science Foundation of China (No.LDT23E06015B06)the support of the Research Computing Center in College of Chemical and Biological Engineering at Zhejiang University for assistance with the calculations。
文摘Cuprous oxide(Cu_(2)O) is one of the most promising catalysts for electrochemical conversion of CO_(2) into value-added C_(2) products.The efficiency of CO_(2)-to-C_(2) conversion is highly dependent on the Cu_(2)O crystal plane orientation and the corresponding adsorbed ^(*)CO species.Herein,we constructed high-index crystal planes(311) in Cu_(2)O(CO-Cu_(2)O) via a facile self-selective CO-induced strategy under a CO atmosphere,which was verified by high-resolution transmission electron microscopy(HR-TEM) and atomic force microscopy(AFM) results.By exploiting the high surface energy of the high index crystal planes,^(*)CO species are stabilized in CO-Cu_(2)O during CO_(2)RR,resulting in exceptional catalytic performance for CO_(2)-to-C_(2)products.In situ infrared spectroscopy revealed that both atop-type(^(*)CO_(atop)) and hollow-type(^(*)CO_(hollow)) adsorption of ^(*)CO species occurred on the CO-Cu_(2)O.The asymmetric C-C coupling energy barrier between ^(*)CO_(atop) and ^(*)CO_(hollow) in(311) crystal plane decreases by 47.8 % compared to the symmetric coupling of ^(*)CO_(atop) in conventional(100) crystal planes.Consequently,the Faradaic efficiency of C_(2) products generated with CO-Cu_(2)O was increased by as high as 100 % compared to that with pristine Cu_(2)O.
基金supported by the National Natural Science Foundation of China(No.22275139)the Key Project of Natural Science Foundation of Tianjin City(No.22JCZDJC00510)The authors thank the Shanghai Synchrotron Radiation Facility of Experiment Assist System(https://cstr.cn/31124.02.SSRF.LAB)for the assistance on BL11B.
文摘Photo-reforming methanol into valuable chemicals represents an energetically sustainable alternative to conventional thermal catalysis,yet controlling-specific C-C coupling way still remains elusive.In this work,we report a sulfide-based photocatalytic paradigm,where atomic-level control of nickel species directly dictates reaction selectivity.The electrostatic constructing ZnIn_(2)S_(4)/Zn_(0.5)Cd_(0.5)S(ZIS/ZCS)heterostructures enable single atom Ni to facilitate ethylene glycol(EG)production with a rate of 11.2 mmol·gcat^(−1)·h^(−1),surpassing reported non-precious metal systems,whereas the Ni aggregates drive exclusive formaldehyde formation.The operando spectroscopy and density functional theory reveal dual roles of Ni as electron reservoir and chemical bond breakage inducers,lowering C-H activation barriers while stabilizing·CH2OH intermediates for cross-coupling.This interfacial configuration engineering creates an electron highway that couples carrier dissociation with radical recombination kinetics,achieving atom-economic steering of methanol oxidative valorization.The metal dispersion assisting catalysis correlation here provides a design blueprint for selective bond scission and reconstruction in sustainable organic synthesis.
基金Supported by National Natural Science Foundation of China(21991093)。
文摘The coupling reactions of methanol and long-chain alkanes(n-dodecane,n-tetradecane and n-hexadecane)over CHA-type molecular sieves were studied in a fixed bed reactor.Over SAPO-34 and SSZ-13,it was found that the induction period of methanol conversion was shortened by the introduction of long-chain alkanes.However,the addition of long-chain alkanes had little influence on the product distribution.Polymethylbenzenes and the derivatives were the main retained species on spent SSZ-13 catalyst,while adamantanes were the main retained species on SAPO-34.This indicates that coking species formation was mainly related to the further transformation of long-chain alkane/methanol coupling products at acid sites of the molecular sieve.These findings provide valuable information of long chain alkanes conversion and methanol reaction behavior of induction period over small pore CHA molecular sieves.
基金National Natural Science Foundation of China(Nos.21902023 and 21901252)Shanghai Pujiang Program,China(No.19PJ1400300)+1 种基金Professor of Special Appointment(Eastern Scholar),ChinaShanghai Institutions of Higher Education Fundamental Research Funds for the Central Universities,China(No.0900000155)。
文摘Catalytic reduction reactions using isopropanol(IPA)as a transfer hydrogenating agent are gaining significant attention due to the low cost and large-scale production of IPA.Traditional methods for carbon-carbon(C—C)bond construction often rely on expensive and scarce transition metal catalysts,raising concerns about sustainability and environmental impact.To address these challenges,we develop a bifunctional photocatalyst,phloroglucinol carbon quantum dot(PG-CQD).It facilitates catalytic transfer hydrogenation(CTH)with IPA as the hydrogen donor.PG-CQDs exhibit both dehydrogenation and reduction activities,enabling the formation of vicinal diols under mild conditions with visible light irradiation.We propose a CTH mechanism that has been successfully validated through experiments.The catalytic system demonstrates remarkable versatility,enabling the synthesis of various vicinal diols from diverseα-keto ester substrates with good or excellent yields.These findings offer a sustainable synthetic strategy that aligns with green chemistry principles and establish a promising pathway for the development of environmentally benign and energy-efficient organic transformations.
基金National Key Research and Development Program of China(2022YFB4600902)Shandong Provincial Science Foundation for Outstanding Young Scholars(ZR2024YQ020)。
文摘Wire arc additive manufacturing(WAAM)has emerged as a promising approach for fabricating large-scale components.However,conventional WAAM still faces challenges in optimizing microstructural evolution,minimizing additive-induced defects,and alleviating residual stress and deformation,all of which are critical for enhancing the mechanical performance of the manufactured parts.Integrating interlayer friction stir processing(FSP)into WAAM significantly enhances the quality of deposited materials.However,numerical simulation research focusing on elucidating the associated thermomechanical coupling mechanisms remains insufficient.A comprehensive numerical model was developed to simulate the thermomechanical coupling behavior in friction stir-assisted WAAM.The influence of post-deposition FSP on the coupled thermomechanical response of the WAAM process was analyzed quantitatively.Moreover,the residual stress distribution and deformation behavior under both single-layer and multilayer deposition conditions were investigated.Thermal analysis of different deposition layers in WAAM and friction stir-assisted WAAM was conducted.Results show that subsequent layer deposition induces partial remelting of the previously solidified layer,whereas FSP does not cause such remelting.Furthermore,thermal stress and deformation analysis confirm that interlayer FSP effectively mitigates residual stresses and distortion in WAAM components,thereby improving their structural integrity and mechanical properties.
基金Youth project under the National Social Science Foundation of China(15CJY054)key project in Philosophy and Social Sciences funded by the Chongqing Municipal Education Commission(22SKGH091)。
文摘This study aims to promote the optimization and upgrading of the economic structure in rural areas of China by focusing on the coupling coordination mechanism between digital economy–agriculture integration and rural revitalization.By examining panel data from 30 Chinese provinces,autonomous regions,and municipalities between 2011 and 2022,the research constructs a weight-based evaluation system that integrates subjective and objective methods and a coupling coordination model to reveal its dynamic evolution patterns.Key findings indicate that digital economy–agriculture integration and rural revitalization achieve cross-coupling through critical activities.The impact of digital-agriculture integration on advancing rural revitalization lags by 2–3 years.Although the coupling development degree between the two systems continues to improve,it remains at the stage of primary coordination.Regional disparities are significant,showing a gradient pattern of“high degree of coupling development in the east and low degree of coupling development in the west.”
基金Project supported by the National Natural Science Foun-dation of China(Grant No.62373197)the Natural Science Foundation of the Higher Education Institutions of Jiangsu Province,China(Grant No.23KJB120010)+1 种基金the Industry-University-Research Cooperation Project of Jiangsu Province,China(Grant No.BY20251038)the Cultivation and In-cubation Project of the College of Automation,Nanjing Uni-versity of Posts and Telecommunications.
文摘Multilayer complex dynamical networks,characterized by the intricate topological connections and diverse hierarchical structures,present significant challenges in determining complete structural configurations due to the unique functional attributes and interaction patterns inherent to different layers.This paper addresses the critical question of whether structural information from a known layer can be used to reconstruct the unknown intralayer structure of a target layer within general weighted output-coupling multilayer networks.Building upon the generalized synchronization principle,we propose an innovative reconstruction method that incorporates two essential components in the design of structure observers,the cross-layer coupling modulator and the structural divergence term.A key advantage of the proposed reconstruction method lies in its flexibility to freely designate both the unknown target layer and the known reference layer from the general weighted output-coupling multilayer network.The reduced dependency on full-state observability enables more deployment in engineering applications with partial measurements.Numerical simulations are conducted to validate the effectiveness of the proposed structure reconstruction method.
基金supported by the National Natural Science Foundation of China(Grant Nos.22193032 and 32401033)the Research Fund of Wenzhou Institute,Chinese Academy of Sciences(Grant Nos.WIUCASQD2020009,WIUCASQD2023005,XSZD2024004,2021HZSY0061,and WIUCASICTP2022)。
文摘The F_(1)-ATPase and V_(1)-ATPase are rotary biomotors.Alignment of their amino acid sequences,which originate from bovine heart mitochondria(1BMF)and Enterococcus hirae(3VR6),respectively,demonstrates that the segment forming the ATP catalytic pocket is highly conserved.Single-molecule experiments,however,have revealed subtle differences in efficiency between the F_(1) and V_(1) motors.Here,we perform both atomistic and coarse-grained molecular dynamics simulations to investigate the mechanochemical coupling and coordination in F_(1) and V_(1) ATPase.Our results show that the correlation between conformational changes in F_(1) is stronger than that in V_(1),indicating that the mechanochemical coupling in F_(1) is tighter than in V_(1).Moreover,the unidirectional rotation of F_(1) is more processive than that of V_(1),which accounts for the higher efficiency observed in F_(1) and explains the occasional backward steps detected in single-molecule experiments on V_(1).
基金supported by the National Science and Tech-nology Major Project,China(No.J2019-II-0012-0032)。
文摘The coupling effects among the flow field,temperature distribution and structural deformation in a turbine cannot be ignored,particularly during flight cycles when the turbine experiences varied operational states.Relying solely on steady-state solutions cannot predict the detrimental effects caused by hysteresis.Consequently,this paper employs a quasi-steady-state fluid-thermalstructure multidisciplinary coupling solution method,integrating transient solid heat conduction with steady-state flow field and static structural deformation solutions.After conducting a numerical simulation of a three-dimensional,five-stage,low-pressure turbine air system,the following conclusions are drawn:when boundary conditions attain high-power states through processes that are numerically identical but in opposite directions,slight variations in solid deformation significantly impact the flow field;when boundary conditions attain high-power states through processes that are directionally consistent but have different numerical values,the influence of the boundary condition change rate on the flow field surpasses that of solid deformation.In terms of turbine design parameters,a large difference in stage-reaction between adjacent stages at the lower radius of the turbine can lead to significant changes in the disc cavity flow field during flight cycles.The difference in the stage-reaction of 0.23 at 10%blade height in adjacent stages may induce severe gas ingress in the stator disc cavity.Thus,it is crucial to minimize this difference and to appropriately extend the duration of the deceleration phase to ensure the turbine's safe operation.
基金supported by the National Key Research and Development Program of China (MOST)(Grant No.2022YFA1402800)the Chinese Academy of Sciences (CAS) Presidents International Fellowship Initiative (PIFI)(Grant No.2025PG0006)+3 种基金the National Natural Science Foundation of China (NSFC)(Grant Nos.51831012,12274437,and 52161160334)the CAS Project for Young Scientists in Basic Research (Grant No.YSBR-084)the CAS Youth Interdisciplinary Teamthe China Postdoctoral Science Foundation (Grant No.2025M773402)。
文摘Based on the Smit-Suhl formula,we propose a universal approach for solving the magnon-magnon coupling problem in bilayer coupled systems(e.g.,antiferromagnets).This method requires only the energy expression,enabling the automatic derivation of analytical expressions for the eigenmatrix elements via symbolic computation,eliminating the need for tedious manual calculations.Using this approach,we investigate the impact of magnetic hysteresis on magnon-magnon coupling in a system with interlayer Dzyaloshinskii-Moriya interaction(DMI).The magnetic hysteresis leads to an asymmetric magnetic field dependence of the resonance frequency and alters the number of degeneracy points between the pure optical and acoustic modes.Moreover,it can result in the coupling strength at the gap of the f–H phase diagram being nearly vanishing,contrary to the conventionally expected maximum.These results deepen the understanding of the effect of interlayer DMI on magnon–magnon coupling and the proposed universal method significantly streamlines the solving process of magnon–magnon coupling problems.
基金supported in part by the Mining Hydraulic Technology and Equipment Engineering Research Center,Liaoning Technical University,Fuxin,China(Grant No.MHTE23-R04)the Fundamental Research Funds for the Central Universities(ID N25BSS068).
文摘This study presents an implicit multiphysics coupling method integrating Computational Fluid Dynamics(CFD),the Multiphase Particle-in-Cell(MPPIC)model,and the Finite Element Method(FEM),implemented with OpenFOAM,CalculiX,and preCICE to simulate fluid-particle-structure interactions with large deformations.Mesh motion in the fluid field is handled using the radial basis function(RBF)method.The particle phase is modeled by MPPIC,where fluid-particle interaction is described through momentum exchange,and inter-particle collisions are characterized by collision stress.The structural field is solved by nonlinear FEM to capture large deformations induced by geometric nonlinearity.Coupling among fields is realized through a partitioned,parallel,and non-intrusive iterative strategy,ensuring stable transfer and convergence of interface forces and displacements.Notably,the influence of particles on the structure is not direct but mediated by the fluid,while structural motion directly affects particle dynamics.The results demonstrate that the proposed approach effectively captures multiphysics interaction processes and provides a valuable reference for numerical modeling of coupled fluid-particle-structure systems.
