Transition-metal dichalcogenides hosting multiple competing structural and electronic phases are thus ideal platforms for constructing polytype heterostructures with emergent quantum properties.However,controlling pha...Transition-metal dichalcogenides hosting multiple competing structural and electronic phases are thus ideal platforms for constructing polytype heterostructures with emergent quantum properties.However,controlling phase transitions to form diverse heterostructures inside a single crystal remains challenging.In this study,we realize vertical/lateral polytype heterostructures in a hole-doped Mott insulator via thermal annealing-induced structural transitions.Raman spectroscopy,atomic force microscopy and scanning Kelvin probe force microscopy confirm the coexistence of T-H polytype heterostructures.Atomic-scale scanning tunneling microscopy/spectroscopy measurements reveal the transparent effect in 1H/1T vertical heterostructures,where positive bias voltage induces in a pronounced superposition of the√13×√13 CDW of the 1T-layer on the 1H-layer.By systematically comparing the 1T/1H and 1T/1T interfaces,we demonstrate that the metallic 1H-layer induces a Coulomb screening effect on the 1T-layer,suppressing the formation of CDW domain walls and forming more ordered electronic states.These results clarify the interfacial coupling between distinct quantum many-body phases and establish a controllable pathway for constructing two-dimensional polytype heterostructures with tunable electronic properties.展开更多
Microwave absorption(MA)materials often face poor synergy between impedance matching and attenuation in the low-frequency range.Balancing permittivity and permeability through magnetic-dielectric synergy is a promisin...Microwave absorption(MA)materials often face poor synergy between impedance matching and attenuation in the low-frequency range.Balancing permittivity and permeability through magnetic-dielectric synergy is a promising strategy to address this issue.To realize the synergy,herein,Sn whiskers with an in situ oxide layer served as substrates for magnetic-loss-active CoNi nanosheet growth,forming a hierarchical CoNi@SnO2@Sn(CNS)heterostructure.The CNS absorber achieves a minimum reflection loss(RLmin)value of-62.29 dB with an effective absorption bandwidth(EAB)of 2.2 GHz,covering the entire C-band with 70%absorption at only 2.61 mm thickness.The nanosheet design of CoNi enhances magnetic anisotropy to promote natural resonance,while the conductive Sn core and abundant Sn/SnO2 and CoNi/SnO2 heterointerfaces facilitate conduction loss and dielectric polarization.When composited into a thermoplastic polyurethane(TPU)matrix,the resulting CNS/TPU-2 film(20 wt%CNS)exhibits an RLmin value of-61.04 dB and a 2.5 GHz EAB.Its in-plane and through-plane thermal conductivities reach 2.41 and 0.51 W m-1 K-1,representing 4.1 and 2.6 times those of pure TPU films,respectively,facilitating heat dissipation from protected devices.This work provides valuable insights into magnetic-dielectric synergy for low-frequency MA of 1D metal-based materials,offering promising potential for 5G communications and flexible electronics.展开更多
Interfacial superconductivity(IS)has been a topic of intense interest in condensed matter physics,due to its unique properties and exotic photoelectrical performance.However,there are few reports about IS systems cons...Interfacial superconductivity(IS)has been a topic of intense interest in condensed matter physics,due to its unique properties and exotic photoelectrical performance.However,there are few reports about IS systems consisting of two insulators.Here,motivated by the emergence of an insulator-metal transition in type-Ⅲ heterostructures and the superconductivity in some“special”two-dimensional(2D)semiconductors via electron doping,we predict that the 2D heterostructure SnSe2/PtTe2 is a model system for realizing IS by using firstprinciples calculations.Our results show that due to slight but crucial interlayer charge transfer,SnSe2/PtTe2 turns to be a type-Ⅲ heterostructure with metallic properties and shows a superconducting transition with the critical temperature(Tc)of 3.73 K.Similar to the enhanced electron–phonon coupling(EPC)in the electrondoped SnSe2 monolayer,the IS in the SnSe2/PtTe2 heterostructure mainly originates from the metallized SnSe2 layer.Furthermore,we find that its superconductivity is sensitive to tensile lattice strain,forming a domeshaped superconducting phase diagram.Remarkably,at 7%biaxial tensile strain,the superconducting Tc can increase more than twofold(8.80 K),resulting from softened acoustic phonons at thepoint and enhanced EPC strength.Our study provides a concrete example for realizing IS in type-Ⅲ heterostructures,which waits for future experimental verification.展开更多
Constructing heterogeneous microstructures has been demonstrated as an effective strategy to overcome the strength-ductility trade-off in magnesium(Mg)alloys.Here,a dual-heterogeneous microstructure was fabricated in ...Constructing heterogeneous microstructures has been demonstrated as an effective strategy to overcome the strength-ductility trade-off in magnesium(Mg)alloys.Here,a dual-heterogeneous microstructure was fabricated in a Mg-6.49Gd-2.74Y-0.45Zr(wt.%)alloy via additive friction stir deposition(AFSD),featuring alternating fine grain(FG)bands embedded with dense nanoscale multiphase clusters and coarse grain(CG)bands containing sparse clusters.This unique architecture leads to simultaneous enhancement of strength and ductility.The AFSD alloy exhibits an elongation of 19.5% and a yield strength of 262.2 MPa,which can be enhanced to 411.0 MPa following peak aging treatment.The formation mechanisms of heterogeneous microstructures and their influence on mechanical properties were systematically investigated.Fragmented rare earth(RE)-containing eutectic phases at grain boundaries induced recrystallization via particle-stimulated nucleation(PSN).Their subsequent complete and rapid dissolution led to the formation of supersaturated RE solid solutions,which promoted the precipitation of nanoscale multiphase clusters with pronounced pinning effects,ultimately leading to the growth of differential grains and the formation of dual-heterostructures.Furthermore,CG/FG interfaces were found to activate non-basal slip systems within adjacent grains,while the nanoscale multiphase clusters can effectively hindered dislocation motion.The synergic effect of these mechanisms contributed to the simultaneous enhancement of strength and ductility.This study provides fundamental insights for developing high-performance Mg-RE alloys.展开更多
Catalytic regeneration stands as a pivotal technology to address the high-energy-consumption bottleneck inherent in the regeneration step of amine-based CO2capture systems.However,existing solid acid catalysts suff...Catalytic regeneration stands as a pivotal technology to address the high-energy-consumption bottleneck inherent in the regeneration step of amine-based CO2capture systems.However,existing solid acid catalysts suffer from insufficient density of acidic sites and poor proton-electron transfer synergy,which severely limits their practical applications.To address this challenge,this study designed and fabricated a two-dimensional zirconium phosphate@graphene oxide(ZrP@GO)heterostructured catalyst with a built-in interfacial electric field,and proposed for the first time a"dual-acid synergy mediated by electron transfer"catalytic mechanism:a built-in electric field is constructed through the interfacial electron coupling between ZrP and GO,which precisely regulates the activity of Brønsted acid/Lewis acid sites and achieves dynamic matching between the function of acid sites and the proton-coupled electron transfer(PCET)process.Compared with the non-catalytic system,the optimal ZrP@GO-10 composite increases the instantaneous CO2desorption rate by 1090%,reduces the regeneration heat duty by 60%,and maintains excellent catalytic stability after 10 desorption cycles.Density functional theory(DFT)calculations reveal that the interfacial electron coupling effect of ZrP@GO constructs a"bond activation-proton transfer"dual-path synergy mechanism by directionally regulating the charge density distribution and enhancing the PCET reaction kinetics.This mechanism can simultaneously reduce the cleavage energy barrier of the carbamate C-N bond and the deprotonation energy barrier of protonated amines(MEAH+),clarifying the essence of the catalyst for achieving low-temperature and low-energy consumption regeneration from a theoretical perspective.This study provides a novel and efficient catalytic paradigm for amine solution regeneration,and promotes the practical application of amine-based CO2capture technology.展开更多
This study aimed to develop efficient and stable non-precious metal electrocatalysts for the hydrogen evolution reaction(HER),addressing the limitations of current catalysts such as insufficient activity and high cost...This study aimed to develop efficient and stable non-precious metal electrocatalysts for the hydrogen evolution reaction(HER),addressing the limitations of current catalysts such as insufficient activity and high cost.A self-supported CeS/NiS/Ni3N/SSM electrocatalyst with abundant heterointerfaces was successfully constructed on a stainless steel mesh(SSM)via an electrodeposition combined with hightemperature solid-gas phase sulfidationitridation strategy.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)analyses confirm the successful introduction of CeS and the strong electronic interaction among the three phases of CeS,NiS,and Ni3N.The doping of Ce induces a redistribution of interface charges,forming electron-deficient Ni centers and optimizing the hydrogen adsorption energy.Scanning electron microscopy(SEM)and transmission electron microscopy(TEM)characterizations reveal that the introduction of CeS transforms the smooth agglomerated particles of NiS/Ni3N into a hierarchical porous structure composed of nanoclusters,significantly increasing the electrochemically active area and constructing clear heterointerfaces,which facilitates the exposure of active sites and mass transfer processes.Density functional theory calculations further indicate that the CeS/NiS/Ni3N heterostructure exhibits a hydrogen adsorption Gibbs free energy(ΔGH*)close to zero(-0.16 eV),significantly superior to that of single components,thereby optimizing the reaction kinetics.The results demonstrate that CeS/NiS/Ni3N/SSM delivers outstanding HER performance in 1 mol/L KOH,requiring an overpotential of only 73.6 mV to achieve the 10 mA/cm2 current density,with a Tafel slope of 87.6 mV/dec,and maintains excellent stability for at least 48 h.This work illustrates that constructing heterointerfaces with simultaneous electronic modulation and structural optimization provides an effective pathway for designing high-performance non-precious metal electrocatalysts.展开更多
CoP has become a research hotspot for supercapacitor electrode materials because of its considerable theoretical capacitance and metalloid nature,but its commercial application remains hampered by structural instabili...CoP has become a research hotspot for supercapacitor electrode materials because of its considerable theoretical capacitance and metalloid nature,but its commercial application remains hampered by structural instability and sluggish ion kinetics.Herein,a high-performance double-hollow porous heterostructured CoP/Cu3P microsphere is assembled using a hydrothermal reaction and phosphating process.The collaborative interaction between the heterostructure and double-hollow microsphere leads to a suppression of volume change,expansion of the active surface,and ion diffusion.The developed CoP/Cu3P sample demonstrates a specific capacitance of 1172.4 F g-1 at 1.0 A g-1 along with outstanding rate capability (capacitance retains 58.5% of its value as current density increases by 20 times),and cycling stability (i.e.,10,000 cycles,90.0% of its original capacitance).Post-cycling analysis shows minimal morphological change,validating the structural robustness of the CoP/Cu3P microspheres.Furthermore,operating at a high voltage of 1.6 V,the asymmetric CoP/Cu3P supercapacitor demonstrates remarkable energy density (44.1 Wh kg-1) and power density (846.8 W kg-1) while maintaining 84.7% of the maximum capacity even after 20,000 cycles,highlighting its exceptional performance.The influence of the electrochemical performance is further verified through first-principles calculations and indicates the promising application prospects in electrical energy storage.展开更多
Fe-Cr-Ni-Cu alloy has been extensively utilized over the past few decades due to its low cost yet high strength.Nevertheless,the poor ductility of this alloy limits its real application in industrial fields.In this st...Fe-Cr-Ni-Cu alloy has been extensively utilized over the past few decades due to its low cost yet high strength.Nevertheless,the poor ductility of this alloy limits its real application in industrial fields.In this study,a soft Fe-Cr-Ni alloy was combined with a Fe-Cr-Ni-Cu alloy by laser-directed energy deposition(LDED)to fabricate the laminated Fe-Cr-Ni/Fe-Cr-Ni-Cu heterostructure,which achieved a high strain hardening capacity and superior strength-ductility balance.Results illustrate that the homogeneous Fe-Cr-Ni-Cu alloy exhibits the largest ultimate tensile strength(UTS)of 990.5±20.41 MPa and contrarily,the lowest fracture elongation(FE)of 11.65%±1.97%.In comparison,the heterostructure which underwent LDED with UTS of 913.01±6.99 MPa and FE of 36.4%±1.59%demonstrates a more than threefold increase in ductility with a slight sacrifice in strength compared to the homogeneous Fe-Cr-Ni-Cu alloy.The exceptional mechanical property of the heterostructure can be attributed to the hetero-deformation-induced(HDI)strengthening and strain hardening,precipitation strengthening,and transformation-induced plasticity(TRIP)effect.HDI strengthening,strain hardening,and TRIP effect collectively contribute to the enhancement of both strength and ductility,while precipitation strengthening also improves the strength.This work proposes a new strategy for the preparation of high-strength alloys with excellent ductility throughout the design of the laminated heterostructure with alternating soft and hard phases via an LDED technology,providing insights for the development of advanced materials with superior mechanical properties.展开更多
Titanium matrix composites(TMCs)offer significant enhancements in strength and heat resistance while pre-serving the low-density characteristic of advanced lightweight titanium alloys.However,ultra-strong,high-tempera...Titanium matrix composites(TMCs)offer significant enhancements in strength and heat resistance while pre-serving the low-density characteristic of advanced lightweight titanium alloys.However,ultra-strong,high-temperature TMCs are typically brittle at room temperature.Here,we overcome this limitation reporting a novel hierarchical,heterostructured design that achieving a 9.5% ductility-exceeding that of the TA15 matrix alloy-along with a remarkable tensile strength of nearly 1.4 GPa at room temperature and 700 MPa at 600℃.This design forms hard,fine-grained regions homogeneously embedded within a soft,coarse-grained matrix.The hierarchical architecture facilitates the emergence of hetero-deformation-induced(HDI)stresses and strain partitioning,thereby enhancing strain hardening and dislocation activity.Our design strategy provides a pathway to achieving not only an optimal combination of strength-ductility at room-temperature but also exceptional high-temperature resistance.展开更多
The preparation process of metal clad plates with large thickness ratios(>20)requires ensuring the substrate thickness while also achieving good mechanical properties,a challenge that traditional rolling processes ...The preparation process of metal clad plates with large thickness ratios(>20)requires ensuring the substrate thickness while also achieving good mechanical properties,a challenge that traditional rolling processes struggle to meet.In this study,TA1/1060/AZ31 clad plates with large thickness ratios(>40)and engineered heterostructures were fabricated via heterothermal rolling,achieving synergistic enhancements in bonding strength and tensile properties.This is attributed to localized interfacial strain concentration induced by the temperature gradient,and sustained strain hardening within the multiscale heterostructured magnesium matrix.The study reveals that the temperature gradient variation in the normal direction of the matrix causes considerable gradation in its deformation mechanisms and microstructure,resulting in diverse heterostructures.In the hot roller zone,high temperatures and large strains promoted the formation of low-angle grain boundaries(LAGBs)with distinct distribution patterns.In contrast,deformation in the cold roller zone was stress-dominated,where the competition between tensile twins andslip changed at low temperatures.Furthermore,LAGB evolution andslip activity differences caused zone-specific variations in discontinuous dynamic recrystallization(CDRX),affecting dislocation density and grain refinement.The higher CDRX degree in the cold roller zone(soft domain)delayed failure in the hot roller zone(hard domain),while heterogeneities in grain size and texture enhanced strain hardening.The dense presence ofdislocations within grains further confirmed the continuous strain hardening behavior.This study provides new insights for the fabrication of metal clad plates with large thickness ratios and the development of novel heterostructures.展开更多
The development of highly efficient and stable nonprecious metal electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial to advance proton exchange membrane(PEM)water electrolysis.In this work,a dual ...The development of highly efficient and stable nonprecious metal electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial to advance proton exchange membrane(PEM)water electrolysis.In this work,a dual synergistic strategy was proposed by constructing a Ce-modified MnO2/MnO heterostructure.The catalyst exhibited outstanding OER performance,achieving a low overpotential of 335 mV at 10 mA cm-2in 0.5 M H2SO4,along with exceptional long-term stability,sustaining operation for 115 h at a high current density of 1 A cm-2.Mechanistic studies revealed that the outstanding performance originates from the dual synergistic effects:The built-in electric field at the heterointerface optimizes the adsorption of oxygen intermediates and alters the rate-determining step;the introduced Ce species,through orbital hybridization and charge transfer enhancement,promotes reaction kinetics.Furthermore,the electron-deficient state of MnO2induced by the internal electric field effectively suppresses excessive Mn dissolution,ensuring exceptional stability in acidic media.展开更多
The chemical bonds at heterogeneous interfaces can optimize the hydrogen adsorption free energy(ΔGH*)by reconfiguring the electronic structure,while an in-depth understanding of the hydrogen adsorption configurati...The chemical bonds at heterogeneous interfaces can optimize the hydrogen adsorption free energy(ΔGH*)by reconfiguring the electronic structure,while an in-depth understanding of the hydrogen adsorption configuration is key to identifying the optimal active sites for enhancing hydrogen evolution performance.Here,we synthesize a wide-pH hydrogen evolution reaction(HER)-active Ni3ZnC0.7/WC heterostructure electrocatalyst uniformly anchored on a carbon framework through a one-step calcination method.Experimental and theoretical results demonstrate that Ni-W bridge bonds within the Ni3ZnC0.7/WC heterointerfaces can induce strong electronic interactions,which help to facilitate electron transfer and optimize theΔGH*,thereby enabling extremely excellent catalytic activity.Consequently,owing to its enhanced inherent activity and favorable electrical conductivity,Ni3ZnC0.7/WC exhibits exceptional catalytic performance for HER(94 and 173 mV at 10 mA/cm2)in alkaline and acidic conditions.Additionally,it can maintain durability for at least 565 h under acidic conditions and 582 h under alkaline conditions,respectively,validating its excellent catalytic stability across a broad pH range.This research provides a new perspective and theoretical basis for designing efficient and stable HER electrocatalysts through interface chemical bond engineering.展开更多
Light-activated gas sensors hold significant potential in environmental monitoring and smart Internet of Things(IoT)owing to their advantage in room temperature operation.Nevertheless,due to a narrow light absorption ...Light-activated gas sensors hold significant potential in environmental monitoring and smart Internet of Things(IoT)owing to their advantage in room temperature operation.Nevertheless,due to a narrow light absorption range,high photocarrier recombination rate,and weak redox activity of the sensing material,the performance enhancement of the current light-activated gas sensors is still impeded.Herein,a full-spectrum solar light-activated gas sensor is designed based on W18O49/Ag2S nanocomposites with an S-scheme heterostructure for the highly sensitive detection of NO2 at room temperature.Under solar light illumination,the gas sensor exhibits a high response of 430.84%to 1 ppm NO2,which is over 11 times higher than that based on pristine W18O49 or Ag2S components.Moreover,the sensor demonstrates excellent repeatability fast responseecovery times(5/3 s),low limit of detection(50 ppb),high selectivity,and satisfactory long-term stability.The enhanced sensing performance might arise from the broadened light-harvesting capability and the unique charge carrier transfer mechanism in the S-scheme heterostructure.A Bluetooth-enabled portable monitoring system is further developed to achieve real-time NO2 monitoring and wireless visualization.This work provides theoretical insights and experimental validation for the effectiveness of S-scheme heterostructure in enhancing room-temperature gas-sensing performance,demonstrating the prospective application potential for IoT-related environmental monitoring.展开更多
Supercapacitors are indispensable for next-generation energy storage,achieving high energy density and long-term durability remains a formidable challenge.Conventional CoS suffers from poor conductivity,while Ti3C_...Supercapacitors are indispensable for next-generation energy storage,achieving high energy density and long-term durability remains a formidable challenge.Conventional CoS suffers from poor conductivity,while Ti3C2faces severe restacking.Herein,we report a novel synthesis strategy that integrates metal-organic framework(MOF)growth with electrostatic self-assembly to construct heterojunction of CoS nanotubes coated with ultrathin Ti3C2nanofilms.Material characterization via SEM,TEM,XRD,and XPS systematically confirms the heterostructure formation,and chemical composition.This rational design synergistically leverages CoS high pseudocapacitance and Ti3C2metallic conductivity while the heterostructure mitigates restacking,enhances charge transfer,and stabilizes interfacial interactions.Density functional theory(DFT)calculations reveal strengthened OH-adsorption at the Co-Ti interface(Ead=1.106 eV).Consequently,the CoS/Ti3C2@CC delivers a remarkable specific capacitance of 1034.21 F g-1 at 1 A g-1.Assembled into a supercapacitor,CoS/Ti3C2@CC//AC achieves a high energy density of 74.22 Wh kg-1 at 800 W kg-1,maintaining 89.13%initial capacitance after 10,000 cycles.Significantly,it exhibits a remarkably low leakage current(0.23μA)and ultra-prolonged voltage retention(47.14%after 120 h),underscoring exceptional durability.This work pioneers a rational heterostructure engineering strategy by integrating MOF-derived architectures with conductive MXene nanofilms,offering critical insights for the development of ultra-durable supercapacitors.展开更多
Metal halide perovskites(MHPs)have been accelerating next generation high performance solar cells due to their high charge carrier transport and optoelectronic properties.However,their thermoelectric properties fall b...Metal halide perovskites(MHPs)have been accelerating next generation high performance solar cells due to their high charge carrier transport and optoelectronic properties.However,their thermoelectric properties fall behind their optoelectronic counterparts,although they have ultralow thermal conductivities and are highly suitable for low grade heat harvesting.A major challenge is how to efficiently dope MHPs in order to achieve high electrical conductivities.As the state-of-the-art MHP for thermoelectric energy conversion,CsSnI3 shows unusual metallic behavior due to the intrinsic Sn vacancies,but it undergoes complex polymorphic phase transitions which hinders its carrier mobility.In this work,we report,for the first time,synthesis of a novel MHP-based thermoelectric device using bulk CsSnI3.This is achieved by leveraging stable polymorphic phase mixing(of orthorhombic and tetragonal phases)and electronic heterostructure.CsSnI3 synthesized by spark-plasma sintering with carbon fiber inclusion shows highly enhanced Seebeck coefficient of~250μV/K,resulting from successful control of the degree of polymorphic phase mixing.The CsSnI3 demonstrates high electrical conductivity of~8400 S/m,attributed to its high carrier mobility.Our approach to control the phase mixing suppresses lattice thermal conductivity to~0.4 W/(m K)through the phonon-boundary scattering.First-principle calculations of the two phases and the phase-interface confirm the strong effect of hybridization and reconstruction of structure at the interface of two phases,which decouples the Seebeck coefficient from electrical conductivity here.The optimized CsSnI3 achieves a power factor of 311μW/(m K2)and ZT of 0.27±0.04,the highest among all reported bulk MHPs.The MHP-based thermoelectric device operates stably across temperature differences of 40 to 260 K,delivering a power density of 3.5 W/m2.This work unlocks the potential of emerging MHPs for thermoelectric devices for low-grade heat harvesting.This could also enable synergistic cooperation between photovoltaic and thermoelectric effects in MHPs for more efficient renewable solar and thermal energy co-harvesting.展开更多
High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance de...High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance degradation caused by unstable cathode-electrolyte interphase(CEI)evolution during longterm cycling.To address this issue,we propose a novel surface modification strategy using La0.7Sr0.3MnO3-σ(LSMO)nanodots,which exhibit high electronic co nductivity and excellent corrosion resistance.These nanodots act as stable anchoring sites,facilitating the formation of a robust CEI on LRMO,The LSMOmodified cathode demonstrates significantly improved anionic redox reversibility,effectively mitigating transition metal migration and lattice oxygen loss.Furthermore,the optimized interfacial electrochemical kinetics ensure sustained rapid Li+diffusion throughout cycling,while the formation of a stable trilayer CEI structure suppresses electrolyte decomposition.Benefiting from these synergistic effects,the LSMO nanodot-engineered LRMO cathode delivers outstanding cycling stability,retaining 97.4%capacity after 300 cycles at 1 C.This work not only highlights the critical role of nanodot heterostructures in stabilizing CEI but also provides a new approach to designing high-voltage cathodes with superior interfacial compatibility and long-term durability.展开更多
The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly import...The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly important for improving its electrochemical performance.Herein,phosphorus-modified graphene encapsulated Sn6O4(OH)4nanoparticles composite(P-Sn6O4(OH)4@RGO)with crystalline-amorphous heterostructure has been successfully designed and prepared.The design of crystalline-amorphous structure has largely enhanced the active sites,and the construction of a graphene encapsulation structure has greatly alleviated volume expansion.Notably,P-Sn6O4(OH)4@RGO obtained an excellent high-rate longterm cycling performance for lithium-ion batteries anode,reaching a high specific capacity of 970 m Ah/g at 1.0 A/g after 1450 cycles.This work demonstrates that restructuring the electrode material's structure and phase through phosphorus modification can effectively improve the electrochemical performance of tin-based electrode materials.展开更多
Titanium(Ti)-steel composite joints are prone to the formation of compounds such as TiC,TiFe,and TiFe2 during solid‐phase bonding.This phenomenon leads to premature failure and significantly reduces the bonding quali...Titanium(Ti)-steel composite joints are prone to the formation of compounds such as TiC,TiFe,and TiFe2 during solid‐phase bonding.This phenomenon leads to premature failure and significantly reduces the bonding quality of the joints.However,the fracture behavior of the joint influenced by these compounds,particularly on the initiation of cracks,is yet to be elucidated.Therefore,a comprehensive investigation of the fracture behavior of Ti-steel joints is essential for understanding interfacial failure mechanisms.This paper presents the fabrication of a joint between pure titanium TA2 and 45 steel,prepared through solid‐phase diffusion bonding.The original morphology of the bonding interface was characterized using scanning electron microscopy and transmission electron microscopy.Subsequently,the tensile fracture behavior of the interface was observed in real‐time using an in situ tensile stage within the TEM.The results indicate that a continuous TiC reaction layer formed at the interface during bonding,with the phase composition on either side of the interface beingα‐Fe and TiC at the microscopic scale.In situ tensile results revealed that cracks were found to initiate not at theα‐Fe/TiC interface,but approximately 200 nm from the interface on the steel side.This is attributed to the strain localization in the steel region caused by inconsistent deformation between the two phases.This finding provides theoretical guidance for microstructural design and quality optimization of Ti-steel heterostructures.展开更多
Recurrence of solid tumors after surgical resection is a major barrier to tissue regeneration.As an emerging treatment strategy,photo-thermo-electric therapy ablates tumor cells via photothermal effects and generates ...Recurrence of solid tumors after surgical resection is a major barrier to tissue regeneration.As an emerging treatment strategy,photo-thermo-electric therapy ablates tumor cells via photothermal effects and generates reactive oxygen species(ROS)via thermoelectric effects to disrupt heat shock proteins,thereby suppressing their protective function in tumor cells.However,conventional materials suffer from low thermoelectric efficiency and weak tissue penetration ability.In this study,we fabricated iodine-doped bismuth sulfide(I-Bi2S3)nanorods with bonding heterostructures to improve thermoelectric performance.The approach employed iodine doping to introduce additional electrons,thereby regulating the band structure of Bi2S3and exploiting the dual low-energy vibration effect of the heterostructures to reduce thermal conductivity.More importantly,controlling the type of heterostructure modulated the bandgap width,thereby expanding the light absorption range to the higher-penetration near-infrared(NIR)-Ⅱregion for deep tissue treatment.The I-Bi2S3nanorods were incorporated into poly-L-lactic acid(PLLA)scaffolds to confer antitumor functionality.According to the results,the bonding heterostructures enhanced the conductivity of Bi2S3and reduced its thermal conductivity,significantly enhancing thermoelectric efficacy.The heterostructures reduced the bandgap of Bi2S3from 1.23 to 0.88 eV,enabling optical absorption in the NIR-Ⅱregion.The ROS tests showed that the PLLA/I-Bi2S3scaffold exhibited good photothermal effects and ROS generation under 1064-nm laser irradiation.The antitumor efficacy of the PLLA/I-Bi2S3scaffold reached 84.6%against MG-63 cells,demonstrating its exceptional potential in cancer treatment.展开更多
Electrocatalytic oxidation of cyclohexanone(KOR)to adipic acid provides a sustainable and value-added pathway for coupled hydrogen evolution(HER).However,the weak adsorption of the reactants and intermediates leads to...Electrocatalytic oxidation of cyclohexanone(KOR)to adipic acid provides a sustainable and value-added pathway for coupled hydrogen evolution(HER).However,the weak adsorption of the reactants and intermediates leads to poor reaction kinetics and product yield.Herein,we synthesized MoNi4/MoO2 heterostructures via phase conversion to engineer a large work function difference that optimizes the Ni electronic structure.This design enhances cyclohexanone adsorption and regulates intermediates,achieving 85%Faradaic efficiency for production of adipic acid and a 2 mmol h-1 cm-2 production rate,along with an ampere-level current.In a membrane electrode assembly electrolyzer for KOR-assisted HER,this catalyst displays 1 A current with 12.1 mol adipic acid production and 3.34 L H2 generation over 8 h,maintaining stability for 56 h at 3 A.Optimized Ni electronic structure achieved through heterojunction-induced charge redistribution strengthens cyclohexanone adsorption and lowers the energy barriers for key intermediates(C6H10O2*and C6H10O3*),boosting oxidation activity.This study presents a novel heterojunction engineering strategy that synergistically enhances reactant adsorption and optimizes intermediate reaction kinetics,offering a tailored approach for efficient catalytic systems.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.92477128,92580137,92477205,12374200,11604063,11974422,and 12104504)the National Key R&D Program of China(MOST)(Grant No.2023YFA1406500)+4 种基金the Strategic Priority Research Program(Chinese Academy of Sciences,CAS)(Grant No.XDB30000000)the Fundamental Research Funds for the Central Universities and Research Funds of Renmin University of China(Grant No.21XNLG27)supported by the Outstanding Innovative Talents Cultivation Funded Programs 2023 of the Renmin University of Chinaan outcome of“Two-dimensional anisotropic series of materials FePd2+xTe2:a structural modulation study from the atomic scale to the mesoscopic scale”(RUC25QSDL128)funded by the“Qiushi Academic-Dongliang”Talent Cultivation Project at Renmin University of China in 2025。
摘要Transition-metal dichalcogenides hosting multiple competing structural and electronic phases are thus ideal platforms for constructing polytype heterostructures with emergent quantum properties.However,controlling phase transitions to form diverse heterostructures inside a single crystal remains challenging.In this study,we realize vertical/lateral polytype heterostructures in a hole-doped Mott insulator via thermal annealing-induced structural transitions.Raman spectroscopy,atomic force microscopy and scanning Kelvin probe force microscopy confirm the coexistence of T-H polytype heterostructures.Atomic-scale scanning tunneling microscopy/spectroscopy measurements reveal the transparent effect in 1H/1T vertical heterostructures,where positive bias voltage induces in a pronounced superposition of the√13×√13 CDW of the 1T-layer on the 1H-layer.By systematically comparing the 1T/1H and 1T/1T interfaces,we demonstrate that the metallic 1H-layer induces a Coulomb screening effect on the 1T-layer,suppressing the formation of CDW domain walls and forming more ordered electronic states.These results clarify the interfacial coupling between distinct quantum many-body phases and establish a controllable pathway for constructing two-dimensional polytype heterostructures with tunable electronic properties.
基金supported by the National Natural Science Foundation of China(52171033,52431003,U23A20574)the Fundamental Research Funds for the Central Universities(2242025K20004)the SEU Innovation Capability Enhancement Plan for Doctoral Students(CXJH_SEU 24148,CXJH_SEU 25036).
摘要Microwave absorption(MA)materials often face poor synergy between impedance matching and attenuation in the low-frequency range.Balancing permittivity and permeability through magnetic-dielectric synergy is a promising strategy to address this issue.To realize the synergy,herein,Sn whiskers with an in situ oxide layer served as substrates for magnetic-loss-active CoNi nanosheet growth,forming a hierarchical CoNi@SnO2@Sn(CNS)heterostructure.The CNS absorber achieves a minimum reflection loss(RLmin)value of-62.29 dB with an effective absorption bandwidth(EAB)of 2.2 GHz,covering the entire C-band with 70%absorption at only 2.61 mm thickness.The nanosheet design of CoNi enhances magnetic anisotropy to promote natural resonance,while the conductive Sn core and abundant Sn/SnO2 and CoNi/SnO2 heterointerfaces facilitate conduction loss and dielectric polarization.When composited into a thermoplastic polyurethane(TPU)matrix,the resulting CNS/TPU-2 film(20 wt%CNS)exhibits an RLmin value of-61.04 dB and a 2.5 GHz EAB.Its in-plane and through-plane thermal conductivities reach 2.41 and 0.51 W m-1 K-1,representing 4.1 and 2.6 times those of pure TPU films,respectively,facilitating heat dissipation from protected devices.This work provides valuable insights into magnetic-dielectric synergy for low-frequency MA of 1D metal-based materials,offering promising potential for 5G communications and flexible electronics.
基金supported by the National Key R&D Program of China (Grant Nos.2022YFA1403103 and 2019YFA0308603)the National Natural Science Foundation of China (Grant No.12304167)the Shandong Provincial Natural Science Foundation of China (Grant No.ZR2023QA020)。
摘要Interfacial superconductivity(IS)has been a topic of intense interest in condensed matter physics,due to its unique properties and exotic photoelectrical performance.However,there are few reports about IS systems consisting of two insulators.Here,motivated by the emergence of an insulator-metal transition in type-Ⅲ heterostructures and the superconductivity in some“special”two-dimensional(2D)semiconductors via electron doping,we predict that the 2D heterostructure SnSe2/PtTe2 is a model system for realizing IS by using firstprinciples calculations.Our results show that due to slight but crucial interlayer charge transfer,SnSe2/PtTe2 turns to be a type-Ⅲ heterostructure with metallic properties and shows a superconducting transition with the critical temperature(Tc)of 3.73 K.Similar to the enhanced electron–phonon coupling(EPC)in the electrondoped SnSe2 monolayer,the IS in the SnSe2/PtTe2 heterostructure mainly originates from the metallized SnSe2 layer.Furthermore,we find that its superconductivity is sensitive to tensile lattice strain,forming a domeshaped superconducting phase diagram.Remarkably,at 7%biaxial tensile strain,the superconducting Tc can increase more than twofold(8.80 K),resulting from softened acoustic phonons at thepoint and enhanced EPC strength.Our study provides a concrete example for realizing IS in type-Ⅲ heterostructures,which waits for future experimental verification.
基金supported by National Key Research and Development Program of China[grant number 2024YFB3715301]National Natural Science Foundation of China[grant numbers 52374392,52101018].
摘要Constructing heterogeneous microstructures has been demonstrated as an effective strategy to overcome the strength-ductility trade-off in magnesium(Mg)alloys.Here,a dual-heterogeneous microstructure was fabricated in a Mg-6.49Gd-2.74Y-0.45Zr(wt.%)alloy via additive friction stir deposition(AFSD),featuring alternating fine grain(FG)bands embedded with dense nanoscale multiphase clusters and coarse grain(CG)bands containing sparse clusters.This unique architecture leads to simultaneous enhancement of strength and ductility.The AFSD alloy exhibits an elongation of 19.5% and a yield strength of 262.2 MPa,which can be enhanced to 411.0 MPa following peak aging treatment.The formation mechanisms of heterogeneous microstructures and their influence on mechanical properties were systematically investigated.Fragmented rare earth(RE)-containing eutectic phases at grain boundaries induced recrystallization via particle-stimulated nucleation(PSN).Their subsequent complete and rapid dissolution led to the formation of supersaturated RE solid solutions,which promoted the precipitation of nanoscale multiphase clusters with pronounced pinning effects,ultimately leading to the growth of differential grains and the formation of dual-heterostructures.Furthermore,CG/FG interfaces were found to activate non-basal slip systems within adjacent grains,while the nanoscale multiphase clusters can effectively hindered dislocation motion.The synergic effect of these mechanisms contributed to the simultaneous enhancement of strength and ductility.This study provides fundamental insights for developing high-performance Mg-RE alloys.
基金National Natural Science Foundation of China(NSFC-Nos.W2511010,22222802,22138002,and U23A20118)National Key R&D Program of China(2023YFB4103900)+3 种基金Hunan Provincial Natural Science Foundation(2025JJ50064)Postgraduate Scientific Research Innovation Project of Hunan Province(CX20240038)China Postdoctoral Science Foundation(2025M771162)China Outstanding Engineer Training Plan for Students of Chemical Engineering&Technology in Hunan University(MOE-No.2011-40)。
摘要Catalytic regeneration stands as a pivotal technology to address the high-energy-consumption bottleneck inherent in the regeneration step of amine-based CO2capture systems.However,existing solid acid catalysts suffer from insufficient density of acidic sites and poor proton-electron transfer synergy,which severely limits their practical applications.To address this challenge,this study designed and fabricated a two-dimensional zirconium phosphate@graphene oxide(ZrP@GO)heterostructured catalyst with a built-in interfacial electric field,and proposed for the first time a"dual-acid synergy mediated by electron transfer"catalytic mechanism:a built-in electric field is constructed through the interfacial electron coupling between ZrP and GO,which precisely regulates the activity of Brønsted acid/Lewis acid sites and achieves dynamic matching between the function of acid sites and the proton-coupled electron transfer(PCET)process.Compared with the non-catalytic system,the optimal ZrP@GO-10 composite increases the instantaneous CO2desorption rate by 1090%,reduces the regeneration heat duty by 60%,and maintains excellent catalytic stability after 10 desorption cycles.Density functional theory(DFT)calculations reveal that the interfacial electron coupling effect of ZrP@GO constructs a"bond activation-proton transfer"dual-path synergy mechanism by directionally regulating the charge density distribution and enhancing the PCET reaction kinetics.This mechanism can simultaneously reduce the cleavage energy barrier of the carbamate C-N bond and the deprotonation energy barrier of protonated amines(MEAH+),clarifying the essence of the catalyst for achieving low-temperature and low-energy consumption regeneration from a theoretical perspective.This study provides a novel and efficient catalytic paradigm for amine solution regeneration,and promotes the practical application of amine-based CO2capture technology.
基金Project supported by the Natural Science Foundation of Inner Mongolia Autonomous Region(2025MS02002,2024MS02004)the Key Research and Development and Achievement Transformation Program of Inner Mongolia Autonomous Region(2025YFHH0096)Graduate Scientific Research Innovation Project of Inner Mongolia(KC2025055B)。
摘要This study aimed to develop efficient and stable non-precious metal electrocatalysts for the hydrogen evolution reaction(HER),addressing the limitations of current catalysts such as insufficient activity and high cost.A self-supported CeS/NiS/Ni3N/SSM electrocatalyst with abundant heterointerfaces was successfully constructed on a stainless steel mesh(SSM)via an electrodeposition combined with hightemperature solid-gas phase sulfidationitridation strategy.X-ray diffraction(XRD)and X-ray photoelectron spectroscopy(XPS)analyses confirm the successful introduction of CeS and the strong electronic interaction among the three phases of CeS,NiS,and Ni3N.The doping of Ce induces a redistribution of interface charges,forming electron-deficient Ni centers and optimizing the hydrogen adsorption energy.Scanning electron microscopy(SEM)and transmission electron microscopy(TEM)characterizations reveal that the introduction of CeS transforms the smooth agglomerated particles of NiS/Ni3N into a hierarchical porous structure composed of nanoclusters,significantly increasing the electrochemically active area and constructing clear heterointerfaces,which facilitates the exposure of active sites and mass transfer processes.Density functional theory calculations further indicate that the CeS/NiS/Ni3N heterostructure exhibits a hydrogen adsorption Gibbs free energy(ΔGH*)close to zero(-0.16 eV),significantly superior to that of single components,thereby optimizing the reaction kinetics.The results demonstrate that CeS/NiS/Ni3N/SSM delivers outstanding HER performance in 1 mol/L KOH,requiring an overpotential of only 73.6 mV to achieve the 10 mA/cm2 current density,with a Tafel slope of 87.6 mV/dec,and maintains excellent stability for at least 48 h.This work illustrates that constructing heterointerfaces with simultaneous electronic modulation and structural optimization provides an effective pathway for designing high-performance non-precious metal electrocatalysts.
基金financially supported by the National Natural Science Foundation of China(Grant No.52172227)the Natural Science Foundation of Hubei Province(Grant No.2023AFA114)+4 种基金Zhuhai Science and Technology Innovation Bureau(Grant No.2220004002402)the National Natural Science Foundation of China(Grant No.12104523)the Key Technologies R&D Program of Henan Province(Grant No.232102240082)the Key Scientific Research Project Plan of Henan Colleges and Universities(Grant No.24A140030)Hubei Three Gorges Laboratory Innovation Fund(Grant No.SC232014)。
摘要CoP has become a research hotspot for supercapacitor electrode materials because of its considerable theoretical capacitance and metalloid nature,but its commercial application remains hampered by structural instability and sluggish ion kinetics.Herein,a high-performance double-hollow porous heterostructured CoP/Cu3P microsphere is assembled using a hydrothermal reaction and phosphating process.The collaborative interaction between the heterostructure and double-hollow microsphere leads to a suppression of volume change,expansion of the active surface,and ion diffusion.The developed CoP/Cu3P sample demonstrates a specific capacitance of 1172.4 F g-1 at 1.0 A g-1 along with outstanding rate capability (capacitance retains 58.5% of its value as current density increases by 20 times),and cycling stability (i.e.,10,000 cycles,90.0% of its original capacitance).Post-cycling analysis shows minimal morphological change,validating the structural robustness of the CoP/Cu3P microspheres.Furthermore,operating at a high voltage of 1.6 V,the asymmetric CoP/Cu3P supercapacitor demonstrates remarkable energy density (44.1 Wh kg-1) and power density (846.8 W kg-1) while maintaining 84.7% of the maximum capacity even after 20,000 cycles,highlighting its exceptional performance.The influence of the electrochemical performance is further verified through first-principles calculations and indicates the promising application prospects in electrical energy storage.
基金financially supported by the State Key Laboratory in Hong Kong from the Innovation and Technology Commission(ITC)of the Government of the Hong Kong Special Administrative Region(HKSAR),Chinathe General Research Fund(GRF)of the Research Grants Council(RGC)of the Hong Kong Special Administrative Region(HKSAR),China(Grant No.PolyU 15220724)+1 种基金the Research Committee of the Hong Kong Polytechnic University(Grant No.RN4T)the Technology and Innovation Commission of Shenzhen Municipality(Grant No.GJHZ20240218111401003).
摘要Fe-Cr-Ni-Cu alloy has been extensively utilized over the past few decades due to its low cost yet high strength.Nevertheless,the poor ductility of this alloy limits its real application in industrial fields.In this study,a soft Fe-Cr-Ni alloy was combined with a Fe-Cr-Ni-Cu alloy by laser-directed energy deposition(LDED)to fabricate the laminated Fe-Cr-Ni/Fe-Cr-Ni-Cu heterostructure,which achieved a high strain hardening capacity and superior strength-ductility balance.Results illustrate that the homogeneous Fe-Cr-Ni-Cu alloy exhibits the largest ultimate tensile strength(UTS)of 990.5±20.41 MPa and contrarily,the lowest fracture elongation(FE)of 11.65%±1.97%.In comparison,the heterostructure which underwent LDED with UTS of 913.01±6.99 MPa and FE of 36.4%±1.59%demonstrates a more than threefold increase in ductility with a slight sacrifice in strength compared to the homogeneous Fe-Cr-Ni-Cu alloy.The exceptional mechanical property of the heterostructure can be attributed to the hetero-deformation-induced(HDI)strengthening and strain hardening,precipitation strengthening,and transformation-induced plasticity(TRIP)effect.HDI strengthening,strain hardening,and TRIP effect collectively contribute to the enhancement of both strength and ductility,while precipitation strengthening also improves the strength.This work proposes a new strategy for the preparation of high-strength alloys with excellent ductility throughout the design of the laminated heterostructure with alternating soft and hard phases via an LDED technology,providing insights for the development of advanced materials with superior mechanical properties.
摘要Titanium matrix composites(TMCs)offer significant enhancements in strength and heat resistance while pre-serving the low-density characteristic of advanced lightweight titanium alloys.However,ultra-strong,high-temperature TMCs are typically brittle at room temperature.Here,we overcome this limitation reporting a novel hierarchical,heterostructured design that achieving a 9.5% ductility-exceeding that of the TA15 matrix alloy-along with a remarkable tensile strength of nearly 1.4 GPa at room temperature and 700 MPa at 600℃.This design forms hard,fine-grained regions homogeneously embedded within a soft,coarse-grained matrix.The hierarchical architecture facilitates the emergence of hetero-deformation-induced(HDI)stresses and strain partitioning,thereby enhancing strain hardening and dislocation activity.Our design strategy provides a pathway to achieving not only an optimal combination of strength-ductility at room-temperature but also exceptional high-temperature resistance.
基金supported by the National Natural Science Foundation of China(52275362,51904205)National Key R&D Program of China(2018YFA0707301)+3 种基金Shanxi Provincial Basic Research Program(202203021224003)Xinjiang Intelligent Equipment Research Institute Directed Commissioned Scientific Research Project(XJYJY2024014)Henan Provincial Department of Science and Technology Research Project(Grant No.252102220067)Open Research Fund from the Hai’an&Taiyuan University of Technology Advanced Manufacturing and Intelligent Equipment Industrial Research Institute(2024HA-TYUTKFYF008).
摘要The preparation process of metal clad plates with large thickness ratios(>20)requires ensuring the substrate thickness while also achieving good mechanical properties,a challenge that traditional rolling processes struggle to meet.In this study,TA1/1060/AZ31 clad plates with large thickness ratios(>40)and engineered heterostructures were fabricated via heterothermal rolling,achieving synergistic enhancements in bonding strength and tensile properties.This is attributed to localized interfacial strain concentration induced by the temperature gradient,and sustained strain hardening within the multiscale heterostructured magnesium matrix.The study reveals that the temperature gradient variation in the normal direction of the matrix causes considerable gradation in its deformation mechanisms and microstructure,resulting in diverse heterostructures.In the hot roller zone,high temperatures and large strains promoted the formation of low-angle grain boundaries(LAGBs)with distinct distribution patterns.In contrast,deformation in the cold roller zone was stress-dominated,where the competition between tensile twins andslip changed at low temperatures.Furthermore,LAGB evolution andslip activity differences caused zone-specific variations in discontinuous dynamic recrystallization(CDRX),affecting dislocation density and grain refinement.The higher CDRX degree in the cold roller zone(soft domain)delayed failure in the hot roller zone(hard domain),while heterogeneities in grain size and texture enhanced strain hardening.The dense presence ofdislocations within grains further confirmed the continuous strain hardening behavior.This study provides new insights for the fabrication of metal clad plates with large thickness ratios and the development of novel heterostructures.
基金financially supported by the National Key Research and Development Program of China(Grant No.2022YFC3900804)。
摘要The development of highly efficient and stable nonprecious metal electrocatalysts for the acidic oxygen evolution reaction(OER)is crucial to advance proton exchange membrane(PEM)water electrolysis.In this work,a dual synergistic strategy was proposed by constructing a Ce-modified MnO2/MnO heterostructure.The catalyst exhibited outstanding OER performance,achieving a low overpotential of 335 mV at 10 mA cm-2in 0.5 M H2SO4,along with exceptional long-term stability,sustaining operation for 115 h at a high current density of 1 A cm-2.Mechanistic studies revealed that the outstanding performance originates from the dual synergistic effects:The built-in electric field at the heterointerface optimizes the adsorption of oxygen intermediates and alters the rate-determining step;the introduced Ce species,through orbital hybridization and charge transfer enhancement,promotes reaction kinetics.Furthermore,the electron-deficient state of MnO2induced by the internal electric field effectively suppresses excessive Mn dissolution,ensuring exceptional stability in acidic media.
基金supported by the National Natural Science Foundation of China(No.22179074,52572110,U22A20144)Scientific Research Program Funded by Shaanxi Provincial Education Department(Program No.25JC014)+2 种基金the Key Research and Development Program of Shaanxi Province(2024GX-YBXM-434)the International S&T Cooperation Foundation of Shaanxi Province(2025GHGHJD-002)the Key Program for International S&T Cooperation Projects of Shaanxi Province(2023GHZD-08)。
摘要The chemical bonds at heterogeneous interfaces can optimize the hydrogen adsorption free energy(ΔGH*)by reconfiguring the electronic structure,while an in-depth understanding of the hydrogen adsorption configuration is key to identifying the optimal active sites for enhancing hydrogen evolution performance.Here,we synthesize a wide-pH hydrogen evolution reaction(HER)-active Ni3ZnC0.7/WC heterostructure electrocatalyst uniformly anchored on a carbon framework through a one-step calcination method.Experimental and theoretical results demonstrate that Ni-W bridge bonds within the Ni3ZnC0.7/WC heterointerfaces can induce strong electronic interactions,which help to facilitate electron transfer and optimize theΔGH*,thereby enabling extremely excellent catalytic activity.Consequently,owing to its enhanced inherent activity and favorable electrical conductivity,Ni3ZnC0.7/WC exhibits exceptional catalytic performance for HER(94 and 173 mV at 10 mA/cm2)in alkaline and acidic conditions.Additionally,it can maintain durability for at least 565 h under acidic conditions and 582 h under alkaline conditions,respectively,validating its excellent catalytic stability across a broad pH range.This research provides a new perspective and theoretical basis for designing efficient and stable HER electrocatalysts through interface chemical bond engineering.
基金financially supported by the National Natural Science Foundation of China(Grant Nos.62571471,62101477,and 62471425)the Science and Technology Innovation Program of Hunan Province(Grant No.2023RC3133)+1 种基金Hunan Provincial Natural Science Foundation of China(Grant No.2026JJ50226)the Scientific Research Foundation of Hunan Provincial Education Department(Grant No.25B0167).
摘要Light-activated gas sensors hold significant potential in environmental monitoring and smart Internet of Things(IoT)owing to their advantage in room temperature operation.Nevertheless,due to a narrow light absorption range,high photocarrier recombination rate,and weak redox activity of the sensing material,the performance enhancement of the current light-activated gas sensors is still impeded.Herein,a full-spectrum solar light-activated gas sensor is designed based on W18O49/Ag2S nanocomposites with an S-scheme heterostructure for the highly sensitive detection of NO2 at room temperature.Under solar light illumination,the gas sensor exhibits a high response of 430.84%to 1 ppm NO2,which is over 11 times higher than that based on pristine W18O49 or Ag2S components.Moreover,the sensor demonstrates excellent repeatability fast responseecovery times(5/3 s),low limit of detection(50 ppb),high selectivity,and satisfactory long-term stability.The enhanced sensing performance might arise from the broadened light-harvesting capability and the unique charge carrier transfer mechanism in the S-scheme heterostructure.A Bluetooth-enabled portable monitoring system is further developed to achieve real-time NO2 monitoring and wireless visualization.This work provides theoretical insights and experimental validation for the effectiveness of S-scheme heterostructure in enhancing room-temperature gas-sensing performance,demonstrating the prospective application potential for IoT-related environmental monitoring.
基金supported by the National Natural Science Foundation of China(22201107,52203147)Zhejiang Provincial Natural Science Foundation of China(MS25B040011)significant science and technology projects of LongMen Laboratory in Henan Province(231100220100).
摘要Supercapacitors are indispensable for next-generation energy storage,achieving high energy density and long-term durability remains a formidable challenge.Conventional CoS suffers from poor conductivity,while Ti3C2faces severe restacking.Herein,we report a novel synthesis strategy that integrates metal-organic framework(MOF)growth with electrostatic self-assembly to construct heterojunction of CoS nanotubes coated with ultrathin Ti3C2nanofilms.Material characterization via SEM,TEM,XRD,and XPS systematically confirms the heterostructure formation,and chemical composition.This rational design synergistically leverages CoS high pseudocapacitance and Ti3C2metallic conductivity while the heterostructure mitigates restacking,enhances charge transfer,and stabilizes interfacial interactions.Density functional theory(DFT)calculations reveal strengthened OH-adsorption at the Co-Ti interface(Ead=1.106 eV).Consequently,the CoS/Ti3C2@CC delivers a remarkable specific capacitance of 1034.21 F g-1 at 1 A g-1.Assembled into a supercapacitor,CoS/Ti3C2@CC//AC achieves a high energy density of 74.22 Wh kg-1 at 800 W kg-1,maintaining 89.13%initial capacitance after 10,000 cycles.Significantly,it exhibits a remarkably low leakage current(0.23μA)and ultra-prolonged voltage retention(47.14%after 120 h),underscoring exceptional durability.This work pioneers a rational heterostructure engineering strategy by integrating MOF-derived architectures with conductive MXene nanofilms,offering critical insights for the development of ultra-durable supercapacitors.
基金funding support by the National Natural Science Foundation of China(52276076 and 52120105009)the Thousand Young Talents Program of China(BE0200006)+2 种基金funding support by the Department for Energy Security and Net Zero,ACT Program(Accelerating CCS Technologies,Horizon2020,691712)for Project NEXTCCUS(327327)the European Union’s Horizon Europe research and innovation program for the SUNPEROM project,Grant Agreement No.101223212University College London’s Research,Innovation and Global Engagement,UCL–Korea University Strategic Partner Fund for their financial support。
摘要Metal halide perovskites(MHPs)have been accelerating next generation high performance solar cells due to their high charge carrier transport and optoelectronic properties.However,their thermoelectric properties fall behind their optoelectronic counterparts,although they have ultralow thermal conductivities and are highly suitable for low grade heat harvesting.A major challenge is how to efficiently dope MHPs in order to achieve high electrical conductivities.As the state-of-the-art MHP for thermoelectric energy conversion,CsSnI3 shows unusual metallic behavior due to the intrinsic Sn vacancies,but it undergoes complex polymorphic phase transitions which hinders its carrier mobility.In this work,we report,for the first time,synthesis of a novel MHP-based thermoelectric device using bulk CsSnI3.This is achieved by leveraging stable polymorphic phase mixing(of orthorhombic and tetragonal phases)and electronic heterostructure.CsSnI3 synthesized by spark-plasma sintering with carbon fiber inclusion shows highly enhanced Seebeck coefficient of~250μV/K,resulting from successful control of the degree of polymorphic phase mixing.The CsSnI3 demonstrates high electrical conductivity of~8400 S/m,attributed to its high carrier mobility.Our approach to control the phase mixing suppresses lattice thermal conductivity to~0.4 W/(m K)through the phonon-boundary scattering.First-principle calculations of the two phases and the phase-interface confirm the strong effect of hybridization and reconstruction of structure at the interface of two phases,which decouples the Seebeck coefficient from electrical conductivity here.The optimized CsSnI3 achieves a power factor of 311μW/(m K2)and ZT of 0.27±0.04,the highest among all reported bulk MHPs.The MHP-based thermoelectric device operates stably across temperature differences of 40 to 260 K,delivering a power density of 3.5 W/m2.This work unlocks the potential of emerging MHPs for thermoelectric devices for low-grade heat harvesting.This could also enable synergistic cooperation between photovoltaic and thermoelectric effects in MHPs for more efficient renewable solar and thermal energy co-harvesting.
基金the financial support from the National Key Research and Development Program of China(2023YFB2504000)。
摘要High-voltage Li-rich Mn-based oxide(LRMO)cathodes are promising for breaking through the energy density limits of lithium-ion batteries,yet their practical application remains limited by electrochemical performance degradation caused by unstable cathode-electrolyte interphase(CEI)evolution during longterm cycling.To address this issue,we propose a novel surface modification strategy using La0.7Sr0.3MnO3-σ(LSMO)nanodots,which exhibit high electronic co nductivity and excellent corrosion resistance.These nanodots act as stable anchoring sites,facilitating the formation of a robust CEI on LRMO,The LSMOmodified cathode demonstrates significantly improved anionic redox reversibility,effectively mitigating transition metal migration and lattice oxygen loss.Furthermore,the optimized interfacial electrochemical kinetics ensure sustained rapid Li+diffusion throughout cycling,while the formation of a stable trilayer CEI structure suppresses electrolyte decomposition.Benefiting from these synergistic effects,the LSMO nanodot-engineered LRMO cathode delivers outstanding cycling stability,retaining 97.4%capacity after 300 cycles at 1 C.This work not only highlights the critical role of nanodot heterostructures in stabilizing CEI but also provides a new approach to designing high-voltage cathodes with superior interfacial compatibility and long-term durability.
基金supported by the Natural Science Foundation of Shandong Province(Nos.ZR2024QE450,ZR2024QB302 and ZR2024QB004)the Taishan Scholars and Young Experts Program of Shandong Province(No.tsqn202211249)Research Program of Qilu Institute of Technology(Nos.QIT 23TP019,QIT23TP010 and QIT24NN007)。
摘要The large volume expansion and rapid capacity attenuation of tin-based electrodes are the main factors limiting their commercial application.The reasonable design of electrode material structure is particularly important for improving its electrochemical performance.Herein,phosphorus-modified graphene encapsulated Sn6O4(OH)4nanoparticles composite(P-Sn6O4(OH)4@RGO)with crystalline-amorphous heterostructure has been successfully designed and prepared.The design of crystalline-amorphous structure has largely enhanced the active sites,and the construction of a graphene encapsulation structure has greatly alleviated volume expansion.Notably,P-Sn6O4(OH)4@RGO obtained an excellent high-rate longterm cycling performance for lithium-ion batteries anode,reaching a high specific capacity of 970 m Ah/g at 1.0 A/g after 1450 cycles.This work demonstrates that restructuring the electrode material's structure and phase through phosphorus modification can effectively improve the electrochemical performance of tin-based electrode materials.
基金financially supported by the Fundamental Research Funds for the Central Universities(Grant No.2024CDJGF‐038)the National Natural Science Foundation of China(Grant Nos.52001037 and U21A2048).
摘要Titanium(Ti)-steel composite joints are prone to the formation of compounds such as TiC,TiFe,and TiFe2 during solid‐phase bonding.This phenomenon leads to premature failure and significantly reduces the bonding quality of the joints.However,the fracture behavior of the joint influenced by these compounds,particularly on the initiation of cracks,is yet to be elucidated.Therefore,a comprehensive investigation of the fracture behavior of Ti-steel joints is essential for understanding interfacial failure mechanisms.This paper presents the fabrication of a joint between pure titanium TA2 and 45 steel,prepared through solid‐phase diffusion bonding.The original morphology of the bonding interface was characterized using scanning electron microscopy and transmission electron microscopy.Subsequently,the tensile fracture behavior of the interface was observed in real‐time using an in situ tensile stage within the TEM.The results indicate that a continuous TiC reaction layer formed at the interface during bonding,with the phase composition on either side of the interface beingα‐Fe and TiC at the microscopic scale.In situ tensile results revealed that cracks were found to initiate not at theα‐Fe/TiC interface,but approximately 200 nm from the interface on the steel side.This is attributed to the strain localization in the steel region caused by inconsistent deformation between the two phases.This finding provides theoretical guidance for microstructural design and quality optimization of Ti-steel heterostructures.
基金National Key Research and Development Program of China(No.2023YFB4605800)The National Natural Science Foundation of China(Nos.52475362,52365046,and 52465041)+3 种基金Jiangxi Provincial Natural Science Foundation of China(No.20224ACB204013)Jiangxi Provincial Key Laboratory of Additive Manufacturing of Implantable Medical Device(No.2024SSY11161)Jiangxi Provincial Department of Education Science and Technology Project(No.GJJ2400708)Jiangxi Province Science and Technology Program(Nos.20252BAC200317 and 20252BEJ730195)。
摘要Recurrence of solid tumors after surgical resection is a major barrier to tissue regeneration.As an emerging treatment strategy,photo-thermo-electric therapy ablates tumor cells via photothermal effects and generates reactive oxygen species(ROS)via thermoelectric effects to disrupt heat shock proteins,thereby suppressing their protective function in tumor cells.However,conventional materials suffer from low thermoelectric efficiency and weak tissue penetration ability.In this study,we fabricated iodine-doped bismuth sulfide(I-Bi2S3)nanorods with bonding heterostructures to improve thermoelectric performance.The approach employed iodine doping to introduce additional electrons,thereby regulating the band structure of Bi2S3and exploiting the dual low-energy vibration effect of the heterostructures to reduce thermal conductivity.More importantly,controlling the type of heterostructure modulated the bandgap width,thereby expanding the light absorption range to the higher-penetration near-infrared(NIR)-Ⅱregion for deep tissue treatment.The I-Bi2S3nanorods were incorporated into poly-L-lactic acid(PLLA)scaffolds to confer antitumor functionality.According to the results,the bonding heterostructures enhanced the conductivity of Bi2S3and reduced its thermal conductivity,significantly enhancing thermoelectric efficacy.The heterostructures reduced the bandgap of Bi2S3from 1.23 to 0.88 eV,enabling optical absorption in the NIR-Ⅱregion.The ROS tests showed that the PLLA/I-Bi2S3scaffold exhibited good photothermal effects and ROS generation under 1064-nm laser irradiation.The antitumor efficacy of the PLLA/I-Bi2S3scaffold reached 84.6%against MG-63 cells,demonstrating its exceptional potential in cancer treatment.
摘要Electrocatalytic oxidation of cyclohexanone(KOR)to adipic acid provides a sustainable and value-added pathway for coupled hydrogen evolution(HER).However,the weak adsorption of the reactants and intermediates leads to poor reaction kinetics and product yield.Herein,we synthesized MoNi4/MoO2 heterostructures via phase conversion to engineer a large work function difference that optimizes the Ni electronic structure.This design enhances cyclohexanone adsorption and regulates intermediates,achieving 85%Faradaic efficiency for production of adipic acid and a 2 mmol h-1 cm-2 production rate,along with an ampere-level current.In a membrane electrode assembly electrolyzer for KOR-assisted HER,this catalyst displays 1 A current with 12.1 mol adipic acid production and 3.34 L H2 generation over 8 h,maintaining stability for 56 h at 3 A.Optimized Ni electronic structure achieved through heterojunction-induced charge redistribution strengthens cyclohexanone adsorption and lowers the energy barriers for key intermediates(C6H10O2*and C6H10O3*),boosting oxidation activity.This study presents a novel heterojunction engineering strategy that synergistically enhances reactant adsorption and optimizes intermediate reaction kinetics,offering a tailored approach for efficient catalytic systems.