Classical computation of electronic properties in large-scale materials remains challenging.Quantum computation has the potential to offer advantages in memory footprint and computational scaling.However,general and v...Classical computation of electronic properties in large-scale materials remains challenging.Quantum computation has the potential to offer advantages in memory footprint and computational scaling.However,general and viable quantum algorithms for simulating large-scale materials are still limited.We propose and implement random-state quantum algorithms to calculate electronic-structure properties of real materials.Using a random state circuit on a small number of qubits,we employ real-time evolution with first-order Trotter decomposition and Hadamard test to obtain electronic density of states,and we develop a modified quantum phase estimation algorithm to calculate real-space local density of states via direct quantum measurements.Furthermore,we validate these algorithms by numerically computing the density of states and spatial distributions of electronic states in graphene,twisted bilayer graphene quasicrystals,and fractal lattices,covering system sizes from hundreds to thousands of atoms.Our results manifest that the random-state quantum algorithms provide a general and qubit-efficient route to scalable simulations of electronic properties in large-scale periodic and aperiodic materials.展开更多
Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantia...Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.展开更多
Self-trapped excitons(STEs),known for their unique radiative properties,have been harnessed in diverse photonic devices;however,their comprehensive understanding and manipulation remain elusive.In this study,we presen...Self-trapped excitons(STEs),known for their unique radiative properties,have been harnessed in diverse photonic devices;however,their comprehensive understanding and manipulation remain elusive.In this study,we present novel experimental and theoretical evidence revealing the hybrid nature and optical tunability of STE state in Cs_(2)Ag_(0.4)Na_(0.6)InCl_(6).The detection of the Fano resonance in laser energy-dependent Raman and photoluminescence spectra indicates the emergence of an exciton-phonon hybrid state,arising from robust quantum interference between the discrete phonon and continuum exciton states.Moreover,we demonstrate continuous tuning of this hybrid state with the energy and intensity of the laser field.These findings lay the foundation for a comprehensive understanding of the nature of STE and their potential for state control.展开更多
The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate me...The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate mechanical properties of electrolyte and unstable interfaces in high-voltage SSLMB s.Herein,we design an asymmetric composite solid-state electrolyte(ACSE)composed of a cellulose framework in situ self-assembled with zeolitic imidazolate framework nanosheets(CP@MOF)embedded in a polymer matrix.The CP@MOF network provides the electrolyte with an elastic modulus of 1.19 GPa,effectively resisting Li dendrite penetration.Furthermore,theoretical calculations guided the compositional design of ACSE to address asynchronous interfacial requirements at cathode/electrolyte and anode/electrolyte interfaces,facilitating stable interphase formation and thus ensuring prolonged cycling of SSLMBs.Consequently,Li symmetric cells achieve extended cycling stability(>5000 h)with minimal polarization.The NCM811|Li full cell maintains 84.9%capacity retention after 350 cycles.Notably,assembled NCM811 pouch cells deliver practical energy densities of 337.9 Wh kg^(-1)and 711.7 Wh L^(-1),demonstrating exceptional application potential.This work provides novel insights into the application of ACSEs for high-energy-density SSLMBs.展开更多
The dense heterogeneous network provides standardized connectivity and access guarantees for 5G communication services.However,the complex network environment and high level of dynamism pose challenges to network sele...The dense heterogeneous network provides standardized connectivity and access guarantees for 5G communication services.However,the complex network environment and high level of dynamism pose challenges to network selection decisions.Existing vertical handover algorithms often overlook the dynamic nature of user mobility and network condition,resulting in problems such as handover failure and frequent handover,ultimately impacting the quality of the user communication service.To address these problems,we propose an intelligent switching method,iMALSTM-DQN,which integrates an improved Multi-level Associative Long Short-Term Memory model(iMALSTM)with Deep Reinforcement Learning(DRL).The algorithm leverages iMALSTM to predict the global network state in the next moment based on the global user movement trajectory and historical network status information within a region,thereby enhancing the prediction accuracy of network states.Subsequently,based on the predicted network state,we employ the Deep Q Network(DON)model to make handover decisions,adaptively determining the optimal switching and network selection strategy through interaction with the environment.Experimental results demonstrate that the proposed algorithm enhances decision timeliness,significantly reduces the number of switch failures,and alleviates the problem of frequent handovers resulting from network dynamics.展开更多
When two layers of graphene are stacked with a twist angle of approximately 1.1°,strong interlayer coupling gives rise to a pair of flat bands in twisted bilayer graphene(TBG),resulting in pronounced electron–el...When two layers of graphene are stacked with a twist angle of approximately 1.1°,strong interlayer coupling gives rise to a pair of flat bands in twisted bilayer graphene(TBG),resulting in pronounced electron–electron interactions.At half filling of the flat bands,TBG exhibits correlated insulating states.Here,we investigate the electrical transport properties of heterostructures composed of TBG and the antiferromagnetic insulator chromium oxychloride(CrOCl),and propose a strategy to modulate the correlated insulating states in TBG.During the transition from a conventional phase to a strong interfacial coupling phase,kink-like features are observed in the charge neutrality point(CNP),correlated insulating state,and band insulating state.Under a perpendicular magnetic field,the system exhibits broadened quantum Hall plateaus in the strong interfacial coupling regime.Electrons localized in the CrOCl layer screen the bottom gate,rendering the carrier density in TBG less sensitive to variations in the bottom gate voltage.These phenomena are well captured by a charge-transfer model between TBG and CrOCl.Our results provide insights into the control of electronic correlations and topological states in graphene moirésystems via interfacial charge coupling.展开更多
State constraints in nonlinear systems are commonly pursued by resorting to barrier functions,which enforce constraints over the entire duration of system operation.We propose a universal intermittent state-constraine...State constraints in nonlinear systems are commonly pursued by resorting to barrier functions,which enforce constraints over the entire duration of system operation.We propose a universal intermittent state-constrained solution,which not only offers flexibility by activating constraints just during specific time periods of interest to the user,but also successfully accommodates different types of constraint boundaries.The innovative shifting functions are proposed to facilitate seamless transitions between constrained and unconstrained operational phases,resulting in more user-friendly design and implementation.By blending an improved shifting transformation into intermittent constraint design,we construct a universal barrier function upon the constrained states,with which our control strategy removes the limitations on constraint functions and completely obviates the feasibility conditions.Furthermore,a modified fuzzy approximator driven by the prediction error rather than the tracking error achieves decoupling of the control and estimation loops,which not only ensures the estimation performance,but also facilitates proof of stability.Finally,the effectiveness of the proposed scheme is assessed by numerical simulation.展开更多
1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained ...1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained attention.The performance of routine LIBs is approaching the ceiling,particularly in terms of energy density,making it difficult to meet the ever-increasing demand for energy density[1].展开更多
High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instab...High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.展开更多
Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identifi...Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identified numerous crystal structures with the Li_(3)MX_(6)composition,although many remain unexplored across various chemical systems.In this research,we developed a comprehensive method to examine all conceivable space groups and structures within theLi-M-X system,where M includes In,Ga,and La,and X includes F,Cl,Br,and 1.Our findings revealed two metastable structures:Li_(3)InF_(6)with P3c1 symmetry and Li_(3)InI_(6)with C2/c symmetry,exhibiting ionic conductivities of 0.55 and 2.18mS/cm at 300K,respectively.Notably,the trigonal symmetry of Li3InF6 demonstrates that high ionic conductivities are not limited to monoclinic structures but can also be achieved with trigonal symmetries.The electrochemical stability windows,mechanical properties,and reaction energies of these materials with known cathodes suggest their potential for use in all-solid-state batteries.Additionally,we predicted the stability of novel materials,including Li_(5)InCl_(8),Li_(5)InBr_(8),Li_(5)InI_(8),LiIn_(2)Cl_(9),LiIn_(2)Br_(9),and LiIn_(2)I_(9).展开更多
Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies ...Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.展开更多
This paper investigates the adaptive optimal tracking control(AOTC)for underactuated surface vessels(USVs).Compared to the majority of existing studies,the control strategy in this paper innovatively combines an exten...This paper investigates the adaptive optimal tracking control(AOTC)for underactuated surface vessels(USVs).Compared to the majority of existing studies,the control strategy in this paper innovatively combines an extended state observer(ESO)with reinforcement learning(RL).The designed ESO has high estimation accuracy and robust disturbance rejection capabilities for the unmeasurable information for USVs.To obtain the AOTC,the actor–critic(AC)networks based on RL are constructed to solve the Hamilton–Jacobi–Bellman(HJB)equations.Due to the uncertainties,it is challenging to obtain the optimal controller by directly solving the HJB equations.To address this issue,this paper employs neural networks(NNs)to approximate the uncertainties and solves the optimal controller via AC-RL and ESO.In addition,the adaptive parameters of the optimal controller is trained in parallel with AC networks,which can ensure that the trained networks can further improve tracking performance.The boundedness of AOTC for USVs is shown by Lyapunov stability theorem.Finally,simulation results demonstrate the effectiveness of the proposed algorithm.展开更多
CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stab...CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.展开更多
Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and ...Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and unstable,making high-quality single-crystal growth,characterization,and measurements difficult,and most do not exhibit superconductivity at ambient pressure.In contrast,La_(3) In stands out for its ambient-pressure superconductivity(T_(C)∼9.4 K)and the availability of high-quality single crystals.Here,we investigate its low-energy electronic structure using angle-resolved photoemission spectroscopy and first-principles calculations.The bands near the Fermi energy(E_(F))are mainly derived from La 5d and In 5p orbitals.A saddle point is directly observed at the Brillouin zone(BZ)boundary,while a three-dimensional Van Hove singularity crosses E_(F) at the BZ corner.First-principles calculations further reveal topological Dirac surface states within the bulk energy gap above E_(F).The coexistence of a high density of states and in-gap topological surface states near𝐸F suggests that La3In offers a promising platform for tuning superconductivity and exploring possible topological superconducting phases through doping or external pressure.展开更多
The hybridization gap in strained-layer InAs/In_(x)Ga_(1−x) Sb quantum spin Hall insulators(QSHIs)is significantly enhanced compared to binary InAs/GaSb QSHI structures,where the typical indium composition,x,ranges be...The hybridization gap in strained-layer InAs/In_(x)Ga_(1−x) Sb quantum spin Hall insulators(QSHIs)is significantly enhanced compared to binary InAs/GaSb QSHI structures,where the typical indium composition,x,ranges between 0.2 and 0.4.This enhancement prompts a critical question:to what extent can quantum wells(QWs)be strained while still preserving the fundamental QSHI phase?In this study,we demonstrate the controlled molecular beam epitaxial growth of highly strained-layer QWs with an indium composition of x=0.5.These structures possess a substantial compressive strain within the In_(0.5)Ga_(0.5)Sb QW.Detailed crystal structure analyses confirm the exceptional quality of the resulting epitaxial films,indicating coherent lattice structures and the absence of visible dislocations.Transport measurements further reveal that the QSHI phase in InAs/In_(0.5)Ga_(0.5)Sb QWs is robust and protected by time-reversal symmetry.Notably,the edge states in these systems exhibit giant magnetoresistance when subjected to a modest perpendicular magnetic field.This behavior is in agreement with the𝑍2 topological property predicted by the Bernevig–Hughes–Zhang model,confirming the preservation of topologically protected edge transport in the presence of enhanced bulk strain.展开更多
Electrocatalytic glucose oxidation to high-value chemicals provides a sustainable route for biomass valorization.NiCo-based catalysts have emerged as promising candidates for glucose oxidation reaction owing to the in...Electrocatalytic glucose oxidation to high-value chemicals provides a sustainable route for biomass valorization.NiCo-based catalysts have emerged as promising candidates for glucose oxidation reaction owing to the intrinsic activity of Ni and Co catalytic centers.However,the dynamic evolution and atomic-scale synergy between these centers remain elusive.Herein,we fabricated NiCo_(2)O_(4)nanosheets supported on nickel foam,where Ni preferentially occupies tetrahedral sites to regulate the electronic configuration of octahedral Co.Experimental and theoretical results demonstrate that the incorporation of tetrahedral Ni induces low-to-intermediate spin transition in octahedral Co,thereby optimizing eg orbital occupancy and stabilizing active sites.This spin-state engineering establishes Ni-Co synergistic catalytic centers for the selective oxidation of glucose to formate(FA).At higher potential(≥1.4 V vs.RHE),octahedral Co undergoes reconstruction into excessive active CoOOH and CoO_(2)species,resulting in glucose overoxidation to CO_(2)and intensified competitive oxygen evolution.In contrast,at lower potentials(<1.4 V vs.RHE),tetrahedral Ni facilitates electron delocalization across the Ni–O–Co lattice,thereby stabilizing octahedral Co for glucose adsorption and oxidation.Subsequently,a coupled electrocatalytic system was constructed,achieving 80.7%FA yield with 91.3%Faradaic efficiency(FE)at NiCo_(2)O_(4)anode and H2 evolution rate of 696μmol h^(−1)with 99.9%FE at Pt cathode for 2 h under 1.35 V vs.RHE.This work provides a deep insight into spin-state regulation of the catalytic center,offering valuable guidance for rational catalyst design.展开更多
Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promo...Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt.Thus,TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries.However,the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains,which greatly reduces the dissociation of lithium salts.Herein,a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate)(PEGDA)in fully dispersed TPU.Hence a stretchable solid-state electrolyte(denoted as TELL and the contrast sample was denoted as TLL)with high ionic conductivity of 7.18×10^(-4) S/cm was obtained at room temperature.The Li^(+)transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm^(2),while the contrast sample is short-circuited after 634 h of cycling.The LiFePO_(4)|TELL|Li cell achieves a capacity retention of 78.93%after 200 cycles at 2 C.The LiFePO_(4)|TLL| Li cellonly gains the capacity retention of 51.9%after 50 cyclesat the same current density.So,the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.展开更多
Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth ...Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.展开更多
The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts rem...The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.展开更多
Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the i...Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the in situ grown 2D perovskite passivation layers typically comprise a mixture of multiple dimensionalities at the interface,where band alignment has only been portrayed qualitatively and empirically.Herein,the interface states for precisely phase-tailored 2D perovskite passivated PSCs are quantitatively investigated.In comparison to traditional passivation molecules,2D perovskite layers based on 4-trifluoromethyl-phenylethylammonium iodide(CF3PEAI)exhibit an increased work function,introducing desirable downward band bending to eliminate the Schottky Barrier.Furthermore,precisely phase-tailored 2D layers could modulate the interface trap density and energetics.The n=1 film delivers optimal performance with a hole extraction efficiency of 95.1%.The optimized n-i-p PSCs in the two-step method significantly improve PCE to 25.40%,along with enhanced photostability and negligible hysteresis.It highlights that tailoring in the composition and phase distribution of the 2D perovskite layer could modulate the interface states at the 2D/3D interface.展开更多
基金supported by the Major Project for the Integration of ScienceEducation and Industry (Grant No.2025ZDZX02)。
文摘Classical computation of electronic properties in large-scale materials remains challenging.Quantum computation has the potential to offer advantages in memory footprint and computational scaling.However,general and viable quantum algorithms for simulating large-scale materials are still limited.We propose and implement random-state quantum algorithms to calculate electronic-structure properties of real materials.Using a random state circuit on a small number of qubits,we employ real-time evolution with first-order Trotter decomposition and Hadamard test to obtain electronic density of states,and we develop a modified quantum phase estimation algorithm to calculate real-space local density of states via direct quantum measurements.Furthermore,we validate these algorithms by numerically computing the density of states and spatial distributions of electronic states in graphene,twisted bilayer graphene quasicrystals,and fractal lattices,covering system sizes from hundreds to thousands of atoms.Our results manifest that the random-state quantum algorithms provide a general and qubit-efficient route to scalable simulations of electronic properties in large-scale periodic and aperiodic materials.
基金National Natural Science Foundation of China,Grant/Award Number:52272225。
文摘Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.
基金funding support from the National Natural Science Foundation of China(Grant No.12525405)funding support from the National Natural Science Foundation of China(Grant No.12393831)the CAS Project for Young Scientists in Basic Research(Grant No.YSBR-120)。
文摘Self-trapped excitons(STEs),known for their unique radiative properties,have been harnessed in diverse photonic devices;however,their comprehensive understanding and manipulation remain elusive.In this study,we present novel experimental and theoretical evidence revealing the hybrid nature and optical tunability of STE state in Cs_(2)Ag_(0.4)Na_(0.6)InCl_(6).The detection of the Fano resonance in laser energy-dependent Raman and photoluminescence spectra indicates the emergence of an exciton-phonon hybrid state,arising from robust quantum interference between the discrete phonon and continuum exciton states.Moreover,we demonstrate continuous tuning of this hybrid state with the energy and intensity of the laser field.These findings lay the foundation for a comprehensive understanding of the nature of STE and their potential for state control.
基金the financial support from the National Natural Science Foundation of China(52072307,22408198)the Fundamental Research Funds for the Central Universities(XJJSKYQD202533)。
文摘The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate mechanical properties of electrolyte and unstable interfaces in high-voltage SSLMB s.Herein,we design an asymmetric composite solid-state electrolyte(ACSE)composed of a cellulose framework in situ self-assembled with zeolitic imidazolate framework nanosheets(CP@MOF)embedded in a polymer matrix.The CP@MOF network provides the electrolyte with an elastic modulus of 1.19 GPa,effectively resisting Li dendrite penetration.Furthermore,theoretical calculations guided the compositional design of ACSE to address asynchronous interfacial requirements at cathode/electrolyte and anode/electrolyte interfaces,facilitating stable interphase formation and thus ensuring prolonged cycling of SSLMBs.Consequently,Li symmetric cells achieve extended cycling stability(>5000 h)with minimal polarization.The NCM811|Li full cell maintains 84.9%capacity retention after 350 cycles.Notably,assembled NCM811 pouch cells deliver practical energy densities of 337.9 Wh kg^(-1)and 711.7 Wh L^(-1),demonstrating exceptional application potential.This work provides novel insights into the application of ACSEs for high-energy-density SSLMBs.
基金National Key Research and Development Program of China(No.2022YFB3903404,2024YFC3015403)National Natural Science Foundation of China(NSFC No.42271431,42271425)Hubei Province Major Science and Technology Innovation Program(2024BAA011)。
文摘The dense heterogeneous network provides standardized connectivity and access guarantees for 5G communication services.However,the complex network environment and high level of dynamism pose challenges to network selection decisions.Existing vertical handover algorithms often overlook the dynamic nature of user mobility and network condition,resulting in problems such as handover failure and frequent handover,ultimately impacting the quality of the user communication service.To address these problems,we propose an intelligent switching method,iMALSTM-DQN,which integrates an improved Multi-level Associative Long Short-Term Memory model(iMALSTM)with Deep Reinforcement Learning(DRL).The algorithm leverages iMALSTM to predict the global network state in the next moment based on the global user movement trajectory and historical network status information within a region,thereby enhancing the prediction accuracy of network states.Subsequently,based on the predicted network state,we employ the Deep Q Network(DON)model to make handover decisions,adaptively determining the optimal switching and network selection strategy through interaction with the environment.Experimental results demonstrate that the proposed algorithm enhances decision timeliness,significantly reduces the number of switch failures,and alleviates the problem of frequent handovers resulting from network dynamics.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.52225207 and 52350001)the Shanghai Pilot Program for Basic Research–Fudan University 21TQ1400100(Grant No.21TQ006)the Shanghai Municipal Science and Technology Major Project(Grant No.2019SHZDZX01)。
文摘When two layers of graphene are stacked with a twist angle of approximately 1.1°,strong interlayer coupling gives rise to a pair of flat bands in twisted bilayer graphene(TBG),resulting in pronounced electron–electron interactions.At half filling of the flat bands,TBG exhibits correlated insulating states.Here,we investigate the electrical transport properties of heterostructures composed of TBG and the antiferromagnetic insulator chromium oxychloride(CrOCl),and propose a strategy to modulate the correlated insulating states in TBG.During the transition from a conventional phase to a strong interfacial coupling phase,kink-like features are observed in the charge neutrality point(CNP),correlated insulating state,and band insulating state.Under a perpendicular magnetic field,the system exhibits broadened quantum Hall plateaus in the strong interfacial coupling regime.Electrons localized in the CrOCl layer screen the bottom gate,rendering the carrier density in TBG less sensitive to variations in the bottom gate voltage.These phenomena are well captured by a charge-transfer model between TBG and CrOCl.Our results provide insights into the control of electronic correlations and topological states in graphene moirésystems via interfacial charge coupling.
基金supported by the Fundamental Research Funds for the Central Universities(N2404005)the National Key Research and Development Program of China(2018YFA0702200)+2 种基金Liaoning Revitalization Talents Program(XLYC1801005)the National Natural Science Foundation of China(U23B20118)the Nature Science Foundation of Liaoning Province of China(2022JH25/10100008)。
文摘State constraints in nonlinear systems are commonly pursued by resorting to barrier functions,which enforce constraints over the entire duration of system operation.We propose a universal intermittent state-constrained solution,which not only offers flexibility by activating constraints just during specific time periods of interest to the user,but also successfully accommodates different types of constraint boundaries.The innovative shifting functions are proposed to facilitate seamless transitions between constrained and unconstrained operational phases,resulting in more user-friendly design and implementation.By blending an improved shifting transformation into intermittent constraint design,we construct a universal barrier function upon the constrained states,with which our control strategy removes the limitations on constraint functions and completely obviates the feasibility conditions.Furthermore,a modified fuzzy approximator driven by the prediction error rather than the tracking error achieves decoupling of the control and estimation loops,which not only ensures the estimation performance,but also facilitates proof of stability.Finally,the effectiveness of the proposed scheme is assessed by numerical simulation.
基金supported by the Beijing Natural Science Foundation(L243019)the National Natural Science Foundation of China(22393900,22393904)+3 种基金the National Key Research and Development Program(2021YFB2500300)the JBGS project from Ordos(JBGS2024001)the Tsinghua University Initiative Scientific Research Programthe“Shuimu Tsinghua Scholar Program of Tsinghua University”。
文摘1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained attention.The performance of routine LIBs is approaching the ceiling,particularly in terms of energy density,making it difficult to meet the ever-increasing demand for energy density[1].
基金supported by the National Key R&D Program of China(2021YFB3800300).
文摘High-nickel cathode,LiNi0.8Co0.1Mn0.1O_(2)(NCM811),and sulfide-solid electrolyte are a promising combination for all-solid-state lithium batteries(ASSLBs).However,this combination faces the issue of interfacial instability between the cathode and electrolyte.Given the surface alkalinity of NCM811,we propose a strategy to construct a solid-polymer-electrolyte(SPE)interphase on NCM811 surface by leveraging the surface alkaline residues to nucleophilically initiate the in-situ ring-opening polymerization of cyclic organic molecules.As a proof-of-concept,this study demonstrates that the ring-opening copolymerization of 1,3-dioxolane and maleic anhydride produces a homogeneous,compact,and conformal SPE layer on NCM811 surface to prevent the cathode from contact and reaction with Li6PS5Cl solid-state electrolyte.Consequently,the SPE-modified-NCM811 in ASSLBs exhibits high capacities of 193.5 mA h g^(-1) at 0.2 C,160.9 mA h g^(-1) at 2.0 C and 112.3 mA h g^(-1) at 10 C,and particularly,excellent long-term cycling stabilities over 11000 cycles with a 71.95%capacity retention at 10 C at 25℃,as well as a remained capacity of 117.9 mA h g^(-1) after 8000 cycles at 30 C at 60℃,showing a great application prospect.This study provides a new route for creating electrochemically and structurally stable solid-solid interfaces for ASSLBs.
基金supported by the Higher Education and Science Committee of Armenia in the frames of the research projects 20TTSG-2F010, 23AA-2F033 and ANSEF (EN-matsc-2660) grant.
文摘Halide solid-state electrolytes have gained significant attention in recent years due to their high ionic conductivity,making them promising candidates for future all-solid-state batteries.Recent studies have identified numerous crystal structures with the Li_(3)MX_(6)composition,although many remain unexplored across various chemical systems.In this research,we developed a comprehensive method to examine all conceivable space groups and structures within theLi-M-X system,where M includes In,Ga,and La,and X includes F,Cl,Br,and 1.Our findings revealed two metastable structures:Li_(3)InF_(6)with P3c1 symmetry and Li_(3)InI_(6)with C2/c symmetry,exhibiting ionic conductivities of 0.55 and 2.18mS/cm at 300K,respectively.Notably,the trigonal symmetry of Li3InF6 demonstrates that high ionic conductivities are not limited to monoclinic structures but can also be achieved with trigonal symmetries.The electrochemical stability windows,mechanical properties,and reaction energies of these materials with known cathodes suggest their potential for use in all-solid-state batteries.Additionally,we predicted the stability of novel materials,including Li_(5)InCl_(8),Li_(5)InBr_(8),Li_(5)InI_(8),LiIn_(2)Cl_(9),LiIn_(2)Br_(9),and LiIn_(2)I_(9).
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.52302303,52472247,52172229,52272201,52072136,51972257)the Natural Science Foundation of Hubei Province(JCZRYB202500537).
文摘Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.
基金supported by the National Natural Science Foundation of China under Grants 62203338,62173259 and U1913602Zhejiang Provincial Natural Science Foundation of China under Grant LZ24F0390006the Postdoctoral Science Foundation of China under Grant 2022M722485.
文摘This paper investigates the adaptive optimal tracking control(AOTC)for underactuated surface vessels(USVs).Compared to the majority of existing studies,the control strategy in this paper innovatively combines an extended state observer(ESO)with reinforcement learning(RL).The designed ESO has high estimation accuracy and robust disturbance rejection capabilities for the unmeasurable information for USVs.To obtain the AOTC,the actor–critic(AC)networks based on RL are constructed to solve the Hamilton–Jacobi–Bellman(HJB)equations.Due to the uncertainties,it is challenging to obtain the optimal controller by directly solving the HJB equations.To address this issue,this paper employs neural networks(NNs)to approximate the uncertainties and solves the optimal controller via AC-RL and ESO.In addition,the adaptive parameters of the optimal controller is trained in parallel with AC networks,which can ensure that the trained networks can further improve tracking performance.The boundedness of AOTC for USVs is shown by Lyapunov stability theorem.Finally,simulation results demonstrate the effectiveness of the proposed algorithm.
基金financially supported by the National Key R&D Program of China(2024YFF0506302)the National Natural Science Foundation of China(52372246)+1 种基金the Frontier Technologies R&D Program of Jiangsu(BF2024041)the Shanghai Engineering Research Center of Inorganic Energy Materials and Electric Power Sources(18DZ2280800)。
文摘CO_(2) hydrogenation using protonic ceramic electrolysis cells(PCECs)to produce fuel gases such as CH_(4)and CO has been considered as a promising technology for effective CO_(2) utilization.However,the long-term stability of conventional PCECs based on Y and Yb doped BaZrO_(3)-BaCeO_(3)(BCZYYb)proton conductors is severely limited by their susceptibility to carbonate formation under high concentration CO_(2) .In this work,a new type PCEC based on CO_(2) -tolerant La_(5.6)WO_(11.4-δ)(LWO)material is firstly constructed.A three-layer porous-dense-porous LWO ceramic scaffold is fabricated via a pressing,dip-coating and cosintering process,followed by Ni and La_(0.6)Sr_(0.4)CoO_(3-δ)(LSC)catalyst impregnation to ensure the chemical compatibility among materials and form an efficient PCEC-based CO_(2) hydrogenation reactor.Benefits from the synergistic catalysis of nano nickel and LWO,the reactor gets a CH_(4)selectivity of over 50%at 600℃under 20%CO_(2) concentration,and it operates stably for over 320 h at 600–650℃under high CO_(2) concentrations of 50–80%,showing no degradation in CO_(2) conversion rate or CH_(4)selectivity.Postmortem analysis demonstrates that the CO_(2) absorption characteristics of LWO and the morphological uniformity of nano nickel lead to stable CO_(2) methanation.This study provides a viable strategy for designing highly stable PCEC-based CO_(2) hydrogenation reactors.
基金supported by the National Natural Science Foundation of China(Grant Nos.12222413,12174443,12274459,and 12404266)the National Key R&D Program of China(Grant Nos.2023YFA1406500,2022YFA1403800,and 2022YFA1403103)+3 种基金the Natural Science Foundation of Shanghai (Grant No.23ZR1482200)the Natural Science Foundation of Ningbo (Grant No.2024J019)the Science Research Project of Hebei Education Department (Grant No.BJ2025060)the funding of Ningbo Yongjiang Talent Program。
文摘Superconducting elect rides have attracted growing attention for their potential to achieve high superconducting transition temperatures(T_(C))under pressure.However,many known elect rides are chemically reactive and unstable,making high-quality single-crystal growth,characterization,and measurements difficult,and most do not exhibit superconductivity at ambient pressure.In contrast,La_(3) In stands out for its ambient-pressure superconductivity(T_(C)∼9.4 K)and the availability of high-quality single crystals.Here,we investigate its low-energy electronic structure using angle-resolved photoemission spectroscopy and first-principles calculations.The bands near the Fermi energy(E_(F))are mainly derived from La 5d and In 5p orbitals.A saddle point is directly observed at the Brillouin zone(BZ)boundary,while a three-dimensional Van Hove singularity crosses E_(F) at the BZ corner.First-principles calculations further reveal topological Dirac surface states within the bulk energy gap above E_(F).The coexistence of a high density of states and in-gap topological surface states near𝐸F suggests that La3In offers a promising platform for tuning superconductivity and exploring possible topological superconducting phases through doping or external pressure.
基金supported by the Strategic Priority Research Program of Chinese Academy of Sciences (Grant Nos.XDB28000000 and XDB0460000)the Quantum Science and Technology-National Science and Technology Major Project (Grant No.2021ZD0302600)the National Key Research and Development Program of China(Grant No.2024YFA1409002)。
文摘The hybridization gap in strained-layer InAs/In_(x)Ga_(1−x) Sb quantum spin Hall insulators(QSHIs)is significantly enhanced compared to binary InAs/GaSb QSHI structures,where the typical indium composition,x,ranges between 0.2 and 0.4.This enhancement prompts a critical question:to what extent can quantum wells(QWs)be strained while still preserving the fundamental QSHI phase?In this study,we demonstrate the controlled molecular beam epitaxial growth of highly strained-layer QWs with an indium composition of x=0.5.These structures possess a substantial compressive strain within the In_(0.5)Ga_(0.5)Sb QW.Detailed crystal structure analyses confirm the exceptional quality of the resulting epitaxial films,indicating coherent lattice structures and the absence of visible dislocations.Transport measurements further reveal that the QSHI phase in InAs/In_(0.5)Ga_(0.5)Sb QWs is robust and protected by time-reversal symmetry.Notably,the edge states in these systems exhibit giant magnetoresistance when subjected to a modest perpendicular magnetic field.This behavior is in agreement with the𝑍2 topological property predicted by the Bernevig–Hughes–Zhang model,confirming the preservation of topologically protected edge transport in the presence of enhanced bulk strain.
基金financially supported by the National Natural Science Foundation of China (22472199)Chinese Universities Scientific Fund (15055009)Central University Guided Funds for Building World-Class Universities (Disciplines) and Advancing Characteristic Development
文摘Electrocatalytic glucose oxidation to high-value chemicals provides a sustainable route for biomass valorization.NiCo-based catalysts have emerged as promising candidates for glucose oxidation reaction owing to the intrinsic activity of Ni and Co catalytic centers.However,the dynamic evolution and atomic-scale synergy between these centers remain elusive.Herein,we fabricated NiCo_(2)O_(4)nanosheets supported on nickel foam,where Ni preferentially occupies tetrahedral sites to regulate the electronic configuration of octahedral Co.Experimental and theoretical results demonstrate that the incorporation of tetrahedral Ni induces low-to-intermediate spin transition in octahedral Co,thereby optimizing eg orbital occupancy and stabilizing active sites.This spin-state engineering establishes Ni-Co synergistic catalytic centers for the selective oxidation of glucose to formate(FA).At higher potential(≥1.4 V vs.RHE),octahedral Co undergoes reconstruction into excessive active CoOOH and CoO_(2)species,resulting in glucose overoxidation to CO_(2)and intensified competitive oxygen evolution.In contrast,at lower potentials(<1.4 V vs.RHE),tetrahedral Ni facilitates electron delocalization across the Ni–O–Co lattice,thereby stabilizing octahedral Co for glucose adsorption and oxidation.Subsequently,a coupled electrocatalytic system was constructed,achieving 80.7%FA yield with 91.3%Faradaic efficiency(FE)at NiCo_(2)O_(4)anode and H2 evolution rate of 696μmol h^(−1)with 99.9%FE at Pt cathode for 2 h under 1.35 V vs.RHE.This work provides a deep insight into spin-state regulation of the catalytic center,offering valuable guidance for rational catalyst design.
基金financially supported by the National Natural Science Foundation of China(Nos.52263010 and 52372188)2023 Introduction of studying abroad talent program,Henan Provincial Key Scientific Research Project of Collegesand Universities(No.23A150038)+1 种基金Key Scientific Research Project of Education Department of Henan Province(No.22A150042)the National students'platform for innovation and entrepreneurship training program(No.201910476010).
文摘Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt.Thus,TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries.However,the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains,which greatly reduces the dissociation of lithium salts.Herein,a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate)(PEGDA)in fully dispersed TPU.Hence a stretchable solid-state electrolyte(denoted as TELL and the contrast sample was denoted as TLL)with high ionic conductivity of 7.18×10^(-4) S/cm was obtained at room temperature.The Li^(+)transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm^(2),while the contrast sample is short-circuited after 634 h of cycling.The LiFePO_(4)|TELL|Li cell achieves a capacity retention of 78.93%after 200 cycles at 2 C.The LiFePO_(4)|TLL| Li cellonly gains the capacity retention of 51.9%after 50 cyclesat the same current density.So,the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.
基金supported by the National Natural Science Foundation of China(Grant Nos.52002094)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2025A1515011995)+3 种基金the Shenzhen Science and Technology Innovation Program(GXWD20221030205923001)the Shandong Provincial Natural Science Foundation of China(Grant Nos.ZR2024QE525)the Shenzhen Key Laboratory of New Materials Technology(Grant Nos.SYSPG20241211173609003)the State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.2024-Z-17,2024-T-08)。
文摘Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.
基金financially supported by the Sichuan Science and Technology Program (Grant No. 2025NSFSC0139)the China Postdoctoral Science Foundation (Grant No.2023MD734228)+10 种基金funding from Generalitat de Catalunya 2021SGR00457supported by MCIN with funding from European Union NextGenerationEU(PRTR-C17.I1)by Generalitat de Catalunya (In-CAEM Project)the support from the project AMaDE(PID2023-149158OB-C43)funded by MCIN/AEI/10.13039/501100011033/by “ERDF A way of making Europe”by the “European Union”supported by the Severo Ochoa program from Spanish MCIN/AEI (Grant No.:CEX2021-001214-S)funded by the CERCA Programme/Generalitat de Catalunyaperformed in the framework of Universitat Autònoma de Barcelona Materials Science PhD programfunding from the CSC-UAB PhD scholarship program. ICN2 is founding member of e-DREAM[87]
文摘The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.
基金supported by the National Natural Science Foundation of China(Nos.62304111,62304110,22579136)the National Key Research and Development Program of China(2024YFE0201800)+6 种基金the China Postdoctoral Science Foundation(No.2024M761492)the Project of State Key Laboratory of Organic Electronics and Information Displays(Nos.GDX2022010009,GZR2023010046)the Natural Science Research Start-up Foundation of Recruiting Talents of Nanjing University of Posts and Telecommunications(No.NY223053)the Science and Technology Project of Jiangsu(Science and Technology Cooperation Project of HongKong,Macao and Taiwan,No.BZ2023059)Shaanxi Fundamental Science Research Project for Mathematics and Physics(No.22jSY015)Young Talent Fund of Xi'an Association for Science and Technology(No.959202313020)Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems(No.2023B1212010003).
文摘Surface passivation via two-dimensional(2D)perovskite has emerged as a promising strategy to enhance the performance of perovskite solar cells(PSCs)due to the effective compensation of interfacial states.However,the in situ grown 2D perovskite passivation layers typically comprise a mixture of multiple dimensionalities at the interface,where band alignment has only been portrayed qualitatively and empirically.Herein,the interface states for precisely phase-tailored 2D perovskite passivated PSCs are quantitatively investigated.In comparison to traditional passivation molecules,2D perovskite layers based on 4-trifluoromethyl-phenylethylammonium iodide(CF3PEAI)exhibit an increased work function,introducing desirable downward band bending to eliminate the Schottky Barrier.Furthermore,precisely phase-tailored 2D layers could modulate the interface trap density and energetics.The n=1 film delivers optimal performance with a hole extraction efficiency of 95.1%.The optimized n-i-p PSCs in the two-step method significantly improve PCE to 25.40%,along with enhanced photostability and negligible hysteresis.It highlights that tailoring in the composition and phase distribution of the 2D perovskite layer could modulate the interface states at the 2D/3D interface.
