Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,how...Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.展开更多
We study the trimer state in a three-body system,where two of the atoms are subject to Rashba-type spin-orbit coupling and spin-dependent loss while interacting spin-selectively with the third atom.The short-time cond...We study the trimer state in a three-body system,where two of the atoms are subject to Rashba-type spin-orbit coupling and spin-dependent loss while interacting spin-selectively with the third atom.The short-time conditional dynamics of the three-body system is effectively governed by a non-Hermitian Hamiltonian with an imaginary Zeeman field.Remarkably,the interplay of non-Hermitian single particle dispersion and the spin-selective interaction results in a Borromean state and an enlarged trimer phase.The stability of trimer state can be reflected by the imaginary part of trimer energy and the momentum distribution of trimer wave function.We also show the phase diagram of the three-body system under both real and imaginary Zeeman fields.Our results illustrate the interesting consequence of non-Hermitian spectral symmetry on the few-body level,which may be readily observable in current cold-atom experiments.展开更多
This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker...This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))analog.It demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation.The resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.展开更多
Strong coupling between resonantly matched surface plasmons of metals and excitons of quantum emitters results in the formation of new plasmon-exciton hybridized energy states.In plasmon-exciton strong coupling,plasmo...Strong coupling between resonantly matched surface plasmons of metals and excitons of quantum emitters results in the formation of new plasmon-exciton hybridized energy states.In plasmon-exciton strong coupling,plasmonic nanocavities play a significant role due to their ability to confine light in an ultrasmall volume.Additionally,two-dimensional transition metal dichalcogenides(TMDCs) have a significant exciton binding energy and remain stable at ambient conditions,making them an excellent alternative for investigating light-matter interactions.As a result,strong plasmon-exciton coupling has been reported by introducing a single metallic cavity.However,single nanoparticles have lower spatial confinement of electromagnetic fields and limited tunability to match the excitonic resonance.Here,we introduce the concept of catenary-shaped optical fields induced by plasmonic metamaterial cavities to scale the strength of plasmon-exciton coupling.The demonstrated plasmon modes of metallic metamaterial cavities offer high confinement and tunability and can match with the excitons of TMDCs to exhibit a strong coupling regime by tuning either the size of the cavity gap or thickness.The calculated Rabi splitting of Au-MoSe_2 and Au-WSe_2 heterostructures strongly depends on the catenary-like field enhancement induced by the Au cavity,resulting in room-temperature Rabi splitting ranging between 77.86 and 320 me V.These plasmonic metamaterial cavities can pave the way for manipulating excitons in TMDCs and operating active nanophotonic devices at ambient temperature.展开更多
Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic h...Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic hydrogels are prepared by regulating the complexation effect,solution polarity and curing speed.Meanwhile,collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination.Subsequently,two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect.FeCo/nitrogen-doped carbon(NC)aerogel demonstrates an ultra-strong microwave absorption of−85 dB at an ultra-low loading of 5%.After reducing the time taken by atom shifting,a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained,which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles.Furthermore,both aerogels show excellent thermal insulation property,and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology.The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels,which will enable the development and application of novel and lightweight stealth coatings.展开更多
Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pos...Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.展开更多
We investigate the nature of the strong coupling constant and related physics.Through the analysis of accumulated experimental data around the world,we employ the ability of machine learning to unravel its physical la...We investigate the nature of the strong coupling constant and related physics.Through the analysis of accumulated experimental data around the world,we employ the ability of machine learning to unravel its physical laws.The result of our efforts is a formula that captures the expansive panorama of the distribution of the strong coupling constant across the entire energy range.展开更多
In this study,Kagome superconductors,i.e.,CsV_(3)Sb_(5)single crystals and its Ta-doped variant,Cs(V_(0.86)Ta_(0.14))_(3)Sb_(5),were studied in detail via specific heat measurements.Results revealed that the charge de...In this study,Kagome superconductors,i.e.,CsV_(3)Sb_(5)single crystals and its Ta-doped variant,Cs(V_(0.86)Ta_(0.14))_(3)Sb_(5),were studied in detail via specific heat measurements.Results revealed that the charge density wave(CDW)was suppressed and the superconducting transition temperature(Tc)considerably increased from 2.8 to 4.6K upon Ta doping.The electronic specific heat of CsV_(3)Sb_(5)was fitted with a model comprising an s-wave gap and a highly anisotropic extended s-wave gap,where 2Δ/kBTc was smaller than the weak coupling limit of 3.5.Cs(V_(0.86)Ta_(0.14))_(3)Sb_(5) exhibited two isotropic s-wave gaps and yielded a larger gap of 2Δ/kBTc=5.04,indicating a significant enhancement in superconducting coupling.This evolution was attributed to the increased density of states near the Fermi level released by CDW gap suppression.These findings demonstrated that Ta doping enhanced superconducting coupling and variation of gap structure in CsV_(3)Sb_(5).展开更多
The chimera states underlying many realistic dynamical processes have attracted ample attention in the area of dynamical systems.Here, we generalize the Kuramoto model with nonlocal coupling incorporating higher-order...The chimera states underlying many realistic dynamical processes have attracted ample attention in the area of dynamical systems.Here, we generalize the Kuramoto model with nonlocal coupling incorporating higher-order interactions encoded with simplicial complexes.Previous works have shown that higher-order interactions promote coherent states.However, we uncover the fact that the introduced higher-order couplings can significantly enhance the emergence of the incoherent state.Remarkably, we identify that the chimera states arise as a result of multi-attractors in dynamic states.Importantly, we review that the increasing higher-order interactions can significantly shape the emergent probability of chimera states.All the observed results can be well described in terms of the dimension reduction method.This study is a step forward in highlighting the importance of nonlocal higher-order couplings, which might provide control strategies for the occurrence of spatial-temporal patterns in networked systems.展开更多
We investigate the ground states of spin-orbit coupled spin-1 Bose-Einstein condensates in the presence of Zeeman splitting.By introducing the generalized momentum operator,the linear version of the system is solved e...We investigate the ground states of spin-orbit coupled spin-1 Bose-Einstein condensates in the presence of Zeeman splitting.By introducing the generalized momentum operator,the linear version of the system is solved exactly,yielding a set of Bessel vortices.Additionally,based on linear solution and using variational approximation,the solutions for the full nonlinear system and their ground state phase diagrams are derived,including the vortex states with quantum numbers m=0,1,as well as mixed states.In this work,mixed states in spin-1 spin-orbit coupling(SOC)BEC are interpreted for the first time as weighted superpositions of three vortex states.Furthermore,the results also indicate that under strong Zeeman splitting,the system cannot form localized states.The variational solutions align well with numerical simulations,showing stable evolution and meeting the criteria for long-term observation in experiments.展开更多
Density limit has long been a widely studied issue influencing the operating range of tokamaks.The rapid growth of the m/n=2/1(where m and n are poloidal and toroidal mode numbers,respectively)tearing mode is generall...Density limit has long been a widely studied issue influencing the operating range of tokamaks.The rapid growth of the m/n=2/1(where m and n are poloidal and toroidal mode numbers,respectively)tearing mode is generally regarded as a primary precursor to the density limit disruption.In this experiment,the coupling of the m/n=1/1 mode and the m/n=2/1 mode in highdensity plasma was observed.During a sawtooth cycle,the frequencies of the two modes gradually converge until they become equal.After that,toroidal coupling occurs between the 1/1 and 2/1 modes,resulting in a mutually fixed phase relationship.With the occurrence of toroidal coupling,the 2/1 mode is stabilized.Prior to the disruption,the cessation of the 1/1 and 2/1 mode coupling,along with the rapid growth in the amplitude of the 2/1 mode,can be observed.Additionally,under the same parameters,comparing discharges with or without the 1/1 mode,it is found that the presence of the 1/1 mode leads to higher plasma density and temperature parameters.展开更多
This study investigates the dynamical behaviors of nearest neighbor asymmetric coupled systems in a confined space.First, the study derivative analytical stability and synchronization conditions for the asymmetrically...This study investigates the dynamical behaviors of nearest neighbor asymmetric coupled systems in a confined space.First, the study derivative analytical stability and synchronization conditions for the asymmetrically coupled system in an unconfined space, which are then validated through numerical simulations. Simulation results show that asymmetric coupling has a significant impact on synchronization conditions. Moreover, it is observed that irrespective of whether the system is confined, an increase in coupling asymmetry leads to a hastened synchronization pace. Additionally, the study examines the effects of boundaries on the system's collective behaviors via numerical experiments. The presence of boundaries ensures the system's stability and synchronization, and reducing these boundaries can expedite the synchronization process and amplify its effects. Finally, the study reveals that the system's output amplitude exhibits stochastic resonance as the confined boundary size increases.展开更多
Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Exploring stable and robust catalysts to replace the current toxic CuCr based catalysts for dehydrogenative coupling of ethanol to ethyl acetate is a challenging but promising task.Herein,novel NiIn based catalysts we...Exploring stable and robust catalysts to replace the current toxic CuCr based catalysts for dehydrogenative coupling of ethanol to ethyl acetate is a challenging but promising task.Herein,novel NiIn based catalysts were developed by tailoring Ni catalysts with Indium(In)for this reaction.Over the optimal Ni0.1Zn0.7Al0.3InOx catalyst,the ethyl acetate selectivity reached 90.1%at 46.2%ethanol conversion under the conditions of 548 K and a weight hourly space velocity of 1.9 h^(-1)in the 370 h time on stream.Moreover,the ethyl acetate productivity surpassed 1.1 g_(ethyl acetate)g_(catalyst)^(-1)h^(-1),,one of the best performance in current works.According to catalyst characterizations and conditional experiments,the active sites for dehydrogenative coupling of ethanol to ethyl acetate were proved to be Ni4In alloys.The presence of In tailored the chemical properties of Ni,and subsequently inhibited the C-C cracking and/or condensation reactions during ethanol conversions.Over Ni4In alloy sites,ethanol was dehydrogenated into acetaldehyde,and then transformed into acetyl species with the removal of H atoms.Finally,the coupling between acetyl species and surface-abundant ethoxyde species into ethyl acetate was achieved,affording a high ethyl acetate selectivity and catalyst stability.展开更多
The dynamic range of the nuclear magnetic resonance gyroscope can be effectively improved through the closedloop control scheme,which is crucial to its application in inertial measurement.This paper presents the analy...The dynamic range of the nuclear magnetic resonance gyroscope can be effectively improved through the closedloop control scheme,which is crucial to its application in inertial measurement.This paper presents the analytical transfer function of Xe closed-loop system in the nuclear magnetic resonance gyroscope considering Rb–Xe coupling effect.It not only considers the dynamic characteristics of the system more comprehensively,but also adds the influence of the practical filters in the gyro signal processing system,which can obtain the accurate response characteristics of signal frequency and amplitude at the same time.The numerical results are compared with an experimentally verified simulation program,which indicate great agreement.The research results of this paper are of great significance to the practical application and development of the nuclear magnetic resonance gyroscope.展开更多
Underground engineering often passes through water-rich fractured rock masses, which are prone to fracture and instability under the long-term coupling of in-situ stress field and pore water(P-W) pressure, ultimately ...Underground engineering often passes through water-rich fractured rock masses, which are prone to fracture and instability under the long-term coupling of in-situ stress field and pore water(P-W) pressure, ultimately threatening the stability of underground structures. In order to explore the mechanical properties of rocks under H-M coupling, the corresponding damage constitutive(D-C) model has become the focus of attention. Considering the inadequacy of the current research on rock strength parameters,energy evolution characteristics and D-C model under H-M coupling, the mechanical properties of typical sandstone samples are discussed based on laboratory tests. The results show that the variation of characteristic stresses of sandstone under H-M coupling conforms to the normalized attenuation equation and Mohr-Coulomb(M-C) criterion. The P-W pressure mechanism of sandstone exhibits a dynamic change from softening effect to H-M fracturing effect. The closure stress is mainly provided by cohesive strength, while the initiation stress, damage stress, and peak stress are jointly dominated by cohesive strength and friction strength. In addition, residual stress is attributed to the friction strength formed by the bite of the fracture surface. Subsequently, the energy evolution characteristics of sandstone under H-M coupling were studied, and it was found that P-W pressure weakened the energy storage capacity and energy dissipation capacity of sandstone, and H-M fracturing was an important factor in reducing its energy storage efficiency. Finally, combined with energy dissipation theory and statistical damage theory, two types of D-C models considering P-W pressure are proposed accordingly, and the model parameters can be determined by four methods. The application results indicate that the proposed and modified D-C models have high reliability, and can characterize the mechanical behavior of sandstone under H-M coupling, overcome the inconvenience of existing D-C models due to excessive mechanical parameters,and can be applied to the full-range stress–strain process. The results are conducive to revealing the deformation and damage mechanisms of rocks under H-M coupling, and can provide theoretical guidance for related engineering problems.展开更多
The safety and durability of lithium-ion batteries under mechanical constraints depend significantly on electrochemical,thermal,and mechanical fields in applications.Characterizing and quantifying the multi-field coup...The safety and durability of lithium-ion batteries under mechanical constraints depend significantly on electrochemical,thermal,and mechanical fields in applications.Characterizing and quantifying the multi-field coupling behaviors requires interdisciplinary efforts.Here,we design experiments under mechanical constraints and introduce an in-situ analytical framework to clarify the complex interaction mechanisms and coupling degrees among multi-physics fields.The proposed analytical framework integrates the parameterization of equivalent models,in-situ mechanical analysis,and quantitative assessment of coupling behavior.The results indicate that the significant impact of pressure on impedance at low temperatures results from the diffusion-controlled step,enhancing kinetics when external pressure,like 180 to 240 k Pa at 10℃,is applied.The diversity in control steps for the electrochemical reaction accounts for the varying impact of pressure on battery performance across different temperatures.The thermal expansion rate suggests that the swelling force varies by less than 1.60%per unit of elevated temperature during the lithiation process.By introducing a composite metric,we quantify the coupling correlation and intensity between characteristic parameters and physical fields,uncovering the highest coupling degree in electrochemical-thermal fields.These results underscore the potential of analytical approaches in revealing the mechanisms of interaction among multi-fields,with the goal of enhancing battery performance and advancing battery management.展开更多
In underground engineering with complex conditions,the bolt(cable)anchorage support system is in an environment where static and dynamic stresses coexist,under the action of geological conditions such as high stresses...In underground engineering with complex conditions,the bolt(cable)anchorage support system is in an environment where static and dynamic stresses coexist,under the action of geological conditions such as high stresses and strong disturbances and construction conditions such as the application of high prestress.It is essential to study the support components performance under dynamic-static coupling conditions.Based on this,a multi-functional anchorage support dynamic-static coupling performance test system(MAC system)is developed,which can achieve 7 types of testing functions,including single component performance,anchored net performance,anchored rock performance and so on.The bolt and cable mechanical tests are conducted by MAC system under different prestress levels.The results showed that compared to the non-prestress condition,the impact resistance performance of prestressed bolts(cables)is significantly reduced.In the prestress range of 50–160 k N,the maximum reduction rate of impact energy resisted by different types of bolts is 53.9%–61.5%compared to non-prestress condition.In the prestress range of 150–300 k N,the impact energy resisted by high-strength cable is reduced by76.8%–84.6%compared to non-prestress condition.The MAC system achieves dynamic-static coupling performance test,which provide an effective means for the design of anchorage support system.展开更多
Clearance-fit(side-fit)spline joints are a key component in a permanent magnet synchronous motor(PMSM)in electric submersible pumping wells.The nonuniform spline clearance affects the output performance of a PMSM.A co...Clearance-fit(side-fit)spline joints are a key component in a permanent magnet synchronous motor(PMSM)in electric submersible pumping wells.The nonuniform spline clearance affects the output performance of a PMSM.A concept for energy conservation is optimized in this study to improve the modeling accuracy of electromagnetic torque.However,most existing computation models are one-way model with a magneto-mechanical simulation.In this study,a more accurate two-way coupling method is presented for simulating the electromagnetic and mechanical characteristics of PMSM.Additionally,importance should be attached to this two-way magneto-mechanical coupling methodology in an actual simulation.The coupled power,electrical and magnetic energy,and electromagnetic torque equations are solved iteratively until convergence for PMSMs with a segmented rotor and a non-segmented rotor.The optimal electromagnetic torque is obtained for different rotor configurations with the change of temperatures and rotational speeds.The results show that the output performance and electromagnetic torque of the PMSM are seriously affected by the effects of two-way magneto-mechanical coupling and nonuniform spline clearance.The proposed two-way coupling model gives more reasonable predictions than other one-way models do,because the power transfer between the electrical and magnetic energy can be modeled more accurately.The self-centralizing performance of clearance-fit splines and the sensitivity to the radial clearance magnitude lead to the reduction of the electromagnetic torque for the PMSM.Additionally,the electromagnetic torques decrease with the enhanced rotor temperatures and rotational speeds.The best rotor temperature and rotational speed are chosen through a comparison of the experimental results,and then the optimal electromagnetic torque is provided to ensure the output performance of the PMSM in electric submersible pumping wells.展开更多
The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in ele...The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.展开更多
基金financially supported by the National Natural Science Foundation of China(Grants nos.62201411,62371378,22205168,52302150 and 62304171)the China Postdoctoral Science Foundation(2022M722500)+1 种基金the Fundamental Research Funds for the Central Universities(Grants nos.ZYTS2308 and 20103237929)Startup Foundation of Xidian University(10251220001).
文摘Defects-rich heterointerfaces integrated with adjustable crystalline phases and atom vacancies,as well as veiled dielectric-responsive character,are instrumental in electromagnetic dissipation.Conventional methods,however,constrain their delicate constructions.Herein,an innovative alternative is proposed:carrageenan-assistant cations-regulated(CACR)strategy,which induces a series of sulfides nanoparticles rooted in situ on the surface of carbon matrix.This unique configuration originates from strategic vacancy formation energy of sulfides and strong sulfides-carbon support interaction,benefiting the delicate construction of defects-rich heterostructures in M_(x)S_(y)/carbon composites(M-CAs).Impressively,these generated sulfur vacancies are firstly found to strengthen electron accumulation/consumption ability at heterointerfaces and,simultaneously,induct local asymmetry of electronic structure to evoke large dipole moment,ultimately leading to polarization coupling,i.e.,defect-type interfacial polarization.Such“Janus effect”(Janus effect means versatility,as in the Greek two-headed Janus)of interfacial sulfur vacancies is intuitively confirmed by both theoretical and experimental investigations for the first time.Consequently,the sulfur vacancies-rich heterostructured Co/Ni-CAs displays broad absorption bandwidth of 6.76 GHz at only 1.8 mm,compared to sulfur vacancies-free CAs without any dielectric response.Harnessing defects-rich heterostructures,this one-pot CACR strategy may steer the design and development of advanced nanomaterials,boosting functionality across diverse application domains beyond electromagnetic response.
基金supported by the National Natural Science Foundation of China(Grant No.11974331)。
文摘We study the trimer state in a three-body system,where two of the atoms are subject to Rashba-type spin-orbit coupling and spin-dependent loss while interacting spin-selectively with the third atom.The short-time conditional dynamics of the three-body system is effectively governed by a non-Hermitian Hamiltonian with an imaginary Zeeman field.Remarkably,the interplay of non-Hermitian single particle dispersion and the spin-selective interaction results in a Borromean state and an enlarged trimer phase.The stability of trimer state can be reflected by the imaginary part of trimer energy and the momentum distribution of trimer wave function.We also show the phase diagram of the three-body system under both real and imaginary Zeeman fields.Our results illustrate the interesting consequence of non-Hermitian spectral symmetry on the few-body level,which may be readily observable in current cold-atom experiments.
基金supported by the National Natural Science Foundation of China(U21A20331,81903743,22005322,22279151,and 22275004)National Science Fund for Distinguished Young Scholars(21925506).
文摘This study presents experimental evidence of the dependence of non-radiative recombination processes on the electron-phonon coupling of perovskite in perovskite solar cells(PSCs).Via A-site cation engineering,a weaker electron-phonon coupling in perovskite has been achieved by introducing the structurally soft cyclohexane methylamine(CMA^(+))cation,which could serve as a damper to alleviate the mechanical stress caused by lattice oscillations,compared to the rigid phenethyl methylamine(PEA^(+))analog.It demonstrates a significantly lower non-radiative recombination rate,even though the two types of bulky cations have similar chemical passivation effects on perovskite,which might be explained by the suppressed carrier capture process and improved lattice geometry relaxation.The resulting PSCs achieve an exceptional power conversion efficiency(PCE)of 25.5%with a record-high opencircuit voltage(V_(OC))of 1.20 V for narrow bandgap perovskite(FAPbI_(3)).The established correlations between electron-phonon coupling and non-radiative decay provide design and screening criteria for more effective passivators for highly efficient PSCs approaching the Shockley-Queisser limit.
基金supported by the Australian Research Council (DP200101353)。
文摘Strong coupling between resonantly matched surface plasmons of metals and excitons of quantum emitters results in the formation of new plasmon-exciton hybridized energy states.In plasmon-exciton strong coupling,plasmonic nanocavities play a significant role due to their ability to confine light in an ultrasmall volume.Additionally,two-dimensional transition metal dichalcogenides(TMDCs) have a significant exciton binding energy and remain stable at ambient conditions,making them an excellent alternative for investigating light-matter interactions.As a result,strong plasmon-exciton coupling has been reported by introducing a single metallic cavity.However,single nanoparticles have lower spatial confinement of electromagnetic fields and limited tunability to match the excitonic resonance.Here,we introduce the concept of catenary-shaped optical fields induced by plasmonic metamaterial cavities to scale the strength of plasmon-exciton coupling.The demonstrated plasmon modes of metallic metamaterial cavities offer high confinement and tunability and can match with the excitons of TMDCs to exhibit a strong coupling regime by tuning either the size of the cavity gap or thickness.The calculated Rabi splitting of Au-MoSe_2 and Au-WSe_2 heterostructures strongly depends on the catenary-like field enhancement induced by the Au cavity,resulting in room-temperature Rabi splitting ranging between 77.86 and 320 me V.These plasmonic metamaterial cavities can pave the way for manipulating excitons in TMDCs and operating active nanophotonic devices at ambient temperature.
基金the National Natural Science Foundation of China(22265021)the Aeronautical Science Foundation of China(2020Z056056003).
文摘Metal–organic gel(MOG)derived composites are promising multi-functional materials due to their alterable composition,identifiable chemical homogeneity,tunable shape,and porous structure.Herein,stable metal–organic hydrogels are prepared by regulating the complexation effect,solution polarity and curing speed.Meanwhile,collagen peptide is used to facilitate the fabrication of a porous aerogel with excellent physical properties as well as the homogeneous dispersion of magnetic particles during calcination.Subsequently,two kinds of heterometallic magnetic coupling systems are obtained through the application of Kirkendall effect.FeCo/nitrogen-doped carbon(NC)aerogel demonstrates an ultra-strong microwave absorption of−85 dB at an ultra-low loading of 5%.After reducing the time taken by atom shifting,a FeCo/Fe3O4/NC aerogel containing virus-shaped particles is obtained,which achieves an ultra-broad absorption of 7.44 GHz at an ultra-thin thickness of 1.59 mm due to the coupling effect offered by dual-soft-magnetic particles.Furthermore,both aerogels show excellent thermal insulation property,and their outstanding radar stealth performances in J-20 aircraft are confirmed by computer simulation technology.The formation mechanism of MOG is also discussed along with the thermal insulation and electromagnetic wave absorption mechanism of the aerogels,which will enable the development and application of novel and lightweight stealth coatings.
基金supported by the National Natural Science Foundation of China(22075133,62288102,22375091,21971114,and 21701086)the Jiangsu Provincial Funds(BX2022013)。
文摘Au is considered as one of the most promising catalysts for nitrogen reduction reaction(NRR),however maximizing the activity utilization rate of Au and understanding the synergistic effects between Au and carriers pose ongoing challenges.Herein,we systematically explore the synergistic catalytic effect of incorporating Au with boron clusters for accelerating NRR kinetics.An in-situ abinitio strategy is employed to construct B-doped Au nanoparticles(2-6 nm in diameter)loaded on BO_(x) substrates(AuBO_(x)),in which B not only modulates the surface electronic structure of Au but also forms strong coupling interactions to stabilize the nanoparticles.The electrochemical results show that Au-BO_(x) possesses excellent NRR activity(NH_(3) yield of 48.52μg h^(-1)mg_(cat)^(-1),Faraday efficiency of 56.18%),and exhibits high stability and reproducibility throughout the electrocatalytic NRR process.Theoretical calculations reveal that the introduction of B induces the formation of both Au dangling bond and Au-B coupling bond.which considerably facilitates the hydrogenation of~*N_(2)^(-)~*NH_(3).The present work provides a new avenue for the preparation of metal-boron materials achieved by one-step reduction and doping process,utilizing boron clusters as reducing and stabilizing agents.
基金supported by the National Natural Science Foundation of China(Grant Nos.12065014,12047501,12247101,and 12335001)the Natural Science Foundation of Gansu Province(Grant No.22JR5RA266)+5 种基金the West Light Foundation of Chinese Academy of Sciences(Grant No.21JR7RA201)supported by the China National Funds for Distinguished Young Scientists(Grant No.11825503)the National Key Research and Development Program of China(Grant No.2020YFA0406400)the 111 Project(Grant No.B20063)the fundamental Research Funds for the Central Universitiesthe Project for Top-Notch Innovative Talents of Gansu province。
文摘We investigate the nature of the strong coupling constant and related physics.Through the analysis of accumulated experimental data around the world,we employ the ability of machine learning to unravel its physical laws.The result of our efforts is a formula that captures the expansive panorama of the distribution of the strong coupling constant across the entire energy range.
基金National Key R&D Program of China(Grant Nos.2022YFA1403201,2022YFA1403400,and 2020YFA0308800)National Natural Science Foundation of China(Grant Nos.11927809,12061131001,11974171,92065109,and 12204231)Fundamental Research Funds for the Central Universities(Grant No.020414380208).
文摘In this study,Kagome superconductors,i.e.,CsV_(3)Sb_(5)single crystals and its Ta-doped variant,Cs(V_(0.86)Ta_(0.14))_(3)Sb_(5),were studied in detail via specific heat measurements.Results revealed that the charge density wave(CDW)was suppressed and the superconducting transition temperature(Tc)considerably increased from 2.8 to 4.6K upon Ta doping.The electronic specific heat of CsV_(3)Sb_(5)was fitted with a model comprising an s-wave gap and a highly anisotropic extended s-wave gap,where 2Δ/kBTc was smaller than the weak coupling limit of 3.5.Cs(V_(0.86)Ta_(0.14))_(3)Sb_(5) exhibited two isotropic s-wave gaps and yielded a larger gap of 2Δ/kBTc=5.04,indicating a significant enhancement in superconducting coupling.This evolution was attributed to the increased density of states near the Fermi level released by CDW gap suppression.These findings demonstrated that Ta doping enhanced superconducting coupling and variation of gap structure in CsV_(3)Sb_(5).
基金Project supported by the National Natural Science Foundation of China (Grants Nos.12375031 and 11905068)the Natural Science Foundation of Fujian Province, China (Grant No.2023J01113)the Scientific Research Funds of Huaqiao University (Grant No.ZQN-810)。
文摘The chimera states underlying many realistic dynamical processes have attracted ample attention in the area of dynamical systems.Here, we generalize the Kuramoto model with nonlocal coupling incorporating higher-order interactions encoded with simplicial complexes.Previous works have shown that higher-order interactions promote coherent states.However, we uncover the fact that the introduced higher-order couplings can significantly enhance the emergence of the incoherent state.Remarkably, we identify that the chimera states arise as a result of multi-attractors in dynamic states.Importantly, we review that the increasing higher-order interactions can significantly shape the emergent probability of chimera states.All the observed results can be well described in terms of the dimension reduction method.This study is a step forward in highlighting the importance of nonlocal higher-order couplings, which might provide control strategies for the occurrence of spatial-temporal patterns in networked systems.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(Grant No.2023A1515110198)the Natural Science Foundation of Guangdong Province,China(Grant Nos.2024A1515030131 and 2021A1515010214)+2 种基金the National Natural Science Foundation of China(Grant Nos.12274077,11905032,and 12475014)the Research Fund of the Guangdong-Hong Kong-Macao Joint Laboratory for Intelligent Micro-Nano Optoelectronic Technology(Grant No.2020B1212030010)the Israel Science Foundation(Grant No.1695/22).
文摘We investigate the ground states of spin-orbit coupled spin-1 Bose-Einstein condensates in the presence of Zeeman splitting.By introducing the generalized momentum operator,the linear version of the system is solved exactly,yielding a set of Bessel vortices.Additionally,based on linear solution and using variational approximation,the solutions for the full nonlinear system and their ground state phase diagrams are derived,including the vortex states with quantum numbers m=0,1,as well as mixed states.In this work,mixed states in spin-1 spin-orbit coupling(SOC)BEC are interpreted for the first time as weighted superpositions of three vortex states.Furthermore,the results also indicate that under strong Zeeman splitting,the system cannot form localized states.The variational solutions align well with numerical simulations,showing stable evolution and meeting the criteria for long-term observation in experiments.
基金supported by National Natural Science Foundation of China(Nos.12175227 and 51821005)the Fundamental Research Funds for the Central Universities(No.USTC 20210079)the Collaborative Innovation Program of Hefei Science Center,CAS(No.2022HSC-CIP022)。
文摘Density limit has long been a widely studied issue influencing the operating range of tokamaks.The rapid growth of the m/n=2/1(where m and n are poloidal and toroidal mode numbers,respectively)tearing mode is generally regarded as a primary precursor to the density limit disruption.In this experiment,the coupling of the m/n=1/1 mode and the m/n=2/1 mode in highdensity plasma was observed.During a sawtooth cycle,the frequencies of the two modes gradually converge until they become equal.After that,toroidal coupling occurs between the 1/1 and 2/1 modes,resulting in a mutually fixed phase relationship.With the occurrence of toroidal coupling,the 2/1 mode is stabilized.Prior to the disruption,the cessation of the 1/1 and 2/1 mode coupling,along with the rapid growth in the amplitude of the 2/1 mode,can be observed.Additionally,under the same parameters,comparing discharges with or without the 1/1 mode,it is found that the presence of the 1/1 mode leads to higher plasma density and temperature parameters.
基金Project supported by the Natural Science Foundation of Shandong Province of China for the Youth (Grant No. ZR2023QA102)。
文摘This study investigates the dynamical behaviors of nearest neighbor asymmetric coupled systems in a confined space.First, the study derivative analytical stability and synchronization conditions for the asymmetrically coupled system in an unconfined space, which are then validated through numerical simulations. Simulation results show that asymmetric coupling has a significant impact on synchronization conditions. Moreover, it is observed that irrespective of whether the system is confined, an increase in coupling asymmetry leads to a hastened synchronization pace. Additionally, the study examines the effects of boundaries on the system's collective behaviors via numerical experiments. The presence of boundaries ensures the system's stability and synchronization, and reducing these boundaries can expedite the synchronization process and amplify its effects. Finally, the study reveals that the system's output amplitude exhibits stochastic resonance as the confined boundary size increases.
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金supported by the National Science Foundation of China(21776268,21721004,22108274 and 22378383)“Transformational Technologies for Clean Energy and Demonstration”,Strategic Priority Research Program of the Chinese Academy of Sciences,(XDA 21060200)support provided by Shanxi Yanchang Petroleum(Group)Co.,Ltd.(yc-hw-2022ky-02).
文摘Exploring stable and robust catalysts to replace the current toxic CuCr based catalysts for dehydrogenative coupling of ethanol to ethyl acetate is a challenging but promising task.Herein,novel NiIn based catalysts were developed by tailoring Ni catalysts with Indium(In)for this reaction.Over the optimal Ni0.1Zn0.7Al0.3InOx catalyst,the ethyl acetate selectivity reached 90.1%at 46.2%ethanol conversion under the conditions of 548 K and a weight hourly space velocity of 1.9 h^(-1)in the 370 h time on stream.Moreover,the ethyl acetate productivity surpassed 1.1 g_(ethyl acetate)g_(catalyst)^(-1)h^(-1),,one of the best performance in current works.According to catalyst characterizations and conditional experiments,the active sites for dehydrogenative coupling of ethanol to ethyl acetate were proved to be Ni4In alloys.The presence of In tailored the chemical properties of Ni,and subsequently inhibited the C-C cracking and/or condensation reactions during ethanol conversions.Over Ni4In alloy sites,ethanol was dehydrogenated into acetaldehyde,and then transformed into acetyl species with the removal of H atoms.Finally,the coupling between acetyl species and surface-abundant ethoxyde species into ethyl acetate was achieved,affording a high ethyl acetate selectivity and catalyst stability.
基金the Natural Science Foundation of China(Grant Nos.61701515 and U23B2066)the Nat-ural Science Foundation of Hunan Province,China(Grant No.2021JJ40700)the Research Project of National Uni-versity of Defense Technology(Grant No.ZK22-18).
文摘The dynamic range of the nuclear magnetic resonance gyroscope can be effectively improved through the closedloop control scheme,which is crucial to its application in inertial measurement.This paper presents the analytical transfer function of Xe closed-loop system in the nuclear magnetic resonance gyroscope considering Rb–Xe coupling effect.It not only considers the dynamic characteristics of the system more comprehensively,but also adds the influence of the practical filters in the gyro signal processing system,which can obtain the accurate response characteristics of signal frequency and amplitude at the same time.The numerical results are compared with an experimentally verified simulation program,which indicate great agreement.The research results of this paper are of great significance to the practical application and development of the nuclear magnetic resonance gyroscope.
基金funding support from the National Natural Science Foundation of China(Nos.52174088 and 42277154)the Independent Innovation Research Fund Graduate Free Exploration Project(No.104972024JYS0007)supported by Wuhan University of Technology.
文摘Underground engineering often passes through water-rich fractured rock masses, which are prone to fracture and instability under the long-term coupling of in-situ stress field and pore water(P-W) pressure, ultimately threatening the stability of underground structures. In order to explore the mechanical properties of rocks under H-M coupling, the corresponding damage constitutive(D-C) model has become the focus of attention. Considering the inadequacy of the current research on rock strength parameters,energy evolution characteristics and D-C model under H-M coupling, the mechanical properties of typical sandstone samples are discussed based on laboratory tests. The results show that the variation of characteristic stresses of sandstone under H-M coupling conforms to the normalized attenuation equation and Mohr-Coulomb(M-C) criterion. The P-W pressure mechanism of sandstone exhibits a dynamic change from softening effect to H-M fracturing effect. The closure stress is mainly provided by cohesive strength, while the initiation stress, damage stress, and peak stress are jointly dominated by cohesive strength and friction strength. In addition, residual stress is attributed to the friction strength formed by the bite of the fracture surface. Subsequently, the energy evolution characteristics of sandstone under H-M coupling were studied, and it was found that P-W pressure weakened the energy storage capacity and energy dissipation capacity of sandstone, and H-M fracturing was an important factor in reducing its energy storage efficiency. Finally, combined with energy dissipation theory and statistical damage theory, two types of D-C models considering P-W pressure are proposed accordingly, and the model parameters can be determined by four methods. The application results indicate that the proposed and modified D-C models have high reliability, and can characterize the mechanical behavior of sandstone under H-M coupling, overcome the inconvenience of existing D-C models due to excessive mechanical parameters,and can be applied to the full-range stress–strain process. The results are conducive to revealing the deformation and damage mechanisms of rocks under H-M coupling, and can provide theoretical guidance for related engineering problems.
基金supported by the National Science Fund for Excellent Youth Scholars of China(52222708)the National Natural Science Foundation of China(51977007)。
文摘The safety and durability of lithium-ion batteries under mechanical constraints depend significantly on electrochemical,thermal,and mechanical fields in applications.Characterizing and quantifying the multi-field coupling behaviors requires interdisciplinary efforts.Here,we design experiments under mechanical constraints and introduce an in-situ analytical framework to clarify the complex interaction mechanisms and coupling degrees among multi-physics fields.The proposed analytical framework integrates the parameterization of equivalent models,in-situ mechanical analysis,and quantitative assessment of coupling behavior.The results indicate that the significant impact of pressure on impedance at low temperatures results from the diffusion-controlled step,enhancing kinetics when external pressure,like 180 to 240 k Pa at 10℃,is applied.The diversity in control steps for the electrochemical reaction accounts for the varying impact of pressure on battery performance across different temperatures.The thermal expansion rate suggests that the swelling force varies by less than 1.60%per unit of elevated temperature during the lithiation process.By introducing a composite metric,we quantify the coupling correlation and intensity between characteristic parameters and physical fields,uncovering the highest coupling degree in electrochemical-thermal fields.These results underscore the potential of analytical approaches in revealing the mechanisms of interaction among multi-fields,with the goal of enhancing battery performance and advancing battery management.
基金supported by the National Natural Science Foundation of China(Nos.51927807,52074164,42277174,42077267 and 42177130)the Natural Science Foundation of Shandong Province,China(No.ZR2020JQ23)China University of Mining and Technology(Beijing)Top Innovative Talent Cultivation Fund for Doctoral Students(No.BBJ2023048)。
文摘In underground engineering with complex conditions,the bolt(cable)anchorage support system is in an environment where static and dynamic stresses coexist,under the action of geological conditions such as high stresses and strong disturbances and construction conditions such as the application of high prestress.It is essential to study the support components performance under dynamic-static coupling conditions.Based on this,a multi-functional anchorage support dynamic-static coupling performance test system(MAC system)is developed,which can achieve 7 types of testing functions,including single component performance,anchored net performance,anchored rock performance and so on.The bolt and cable mechanical tests are conducted by MAC system under different prestress levels.The results showed that compared to the non-prestress condition,the impact resistance performance of prestressed bolts(cables)is significantly reduced.In the prestress range of 50–160 k N,the maximum reduction rate of impact energy resisted by different types of bolts is 53.9%–61.5%compared to non-prestress condition.In the prestress range of 150–300 k N,the impact energy resisted by high-strength cable is reduced by76.8%–84.6%compared to non-prestress condition.The MAC system achieves dynamic-static coupling performance test,which provide an effective means for the design of anchorage support system.
基金financially supported by National Natural Science Foundation of China(Grant Nos.52074161 and 52005281)Taishan Scholar Project of Shandong Province(Grant No.tsqn202211177)+2 种基金Shandong Provincial Plan for Introduction and Cultivation of Young Pioneers in Colleges and Universities(Grant No.2021-Qing Chuang-30613019)Natural Science Foundation of Shandong Province(Grant Nos.ZR2022ME173 and ZR2023QE011)Projects of CNOOC Research Institute Ltd.(Grant Nos.CCL2023RCPS0237RSN and CCL2023RCPS0319RSN)。
文摘Clearance-fit(side-fit)spline joints are a key component in a permanent magnet synchronous motor(PMSM)in electric submersible pumping wells.The nonuniform spline clearance affects the output performance of a PMSM.A concept for energy conservation is optimized in this study to improve the modeling accuracy of electromagnetic torque.However,most existing computation models are one-way model with a magneto-mechanical simulation.In this study,a more accurate two-way coupling method is presented for simulating the electromagnetic and mechanical characteristics of PMSM.Additionally,importance should be attached to this two-way magneto-mechanical coupling methodology in an actual simulation.The coupled power,electrical and magnetic energy,and electromagnetic torque equations are solved iteratively until convergence for PMSMs with a segmented rotor and a non-segmented rotor.The optimal electromagnetic torque is obtained for different rotor configurations with the change of temperatures and rotational speeds.The results show that the output performance and electromagnetic torque of the PMSM are seriously affected by the effects of two-way magneto-mechanical coupling and nonuniform spline clearance.The proposed two-way coupling model gives more reasonable predictions than other one-way models do,because the power transfer between the electrical and magnetic energy can be modeled more accurately.The self-centralizing performance of clearance-fit splines and the sensitivity to the radial clearance magnitude lead to the reduction of the electromagnetic torque for the PMSM.Additionally,the electromagnetic torques decrease with the enhanced rotor temperatures and rotational speeds.The best rotor temperature and rotational speed are chosen through a comparison of the experimental results,and then the optimal electromagnetic torque is provided to ensure the output performance of the PMSM in electric submersible pumping wells.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.52161135302,22105087)the Postdoctoral Research Foundation of China(Grant No.2022M721360)the Natural Science Foundation of Jiangsu Province(Grant No.BK20210446)。
文摘The d-d orbital coupling induced by crystal-phase engineering can effectively adjust the electronic structure of electrocatalysts,thus showing significant catalytic performance,while it has been rarely explored in electrochemical acetonitrile reduction reaction(ARR)to date.Herein,we successfully realize the structural transformation of Pd Cu metallic aerogels(MAs)from face-centered cubic(FCC)to body-centered cubic(BCC)through annealing treatment.Specifically,the BCC Pd Cu MAs exhibit excellent ARR performance with high ethylamine selectivity of 90.91%,Faradaic efficiency of 88.60%,yield rate of 316.0 mmol h^(-1)g^(-1)_(Pd+Cu)and long-term stability for consecutive electrolysis within 20 h at-0.55 V vs.reversible hydrogen electrode,outperforming than those of FCC Pd Cu MAs.Under the membrane electrode assembly system,BCC Pd Cu MAs also demonstrate excellent ethylamine yield rate of 389.5 mmol h^(-1)g^(-1)_(Pd+Cu).Density functional theory calculation reveals that the d-d orbital coupling in BCC Pd Cu MAs results in an evident correlation effect for the interaction of Pd and Cu sites,which boosts up the Cu sites electronic activities to enhance ARR performance.Our work opens a new route to develop efficient ARR electrocatalysts from the perspective of crystalline structure transformation.
