Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
Interplay between topology and magnetism can give rise to exotic properties in topological materials.Two-dimensional bismuth has been extensively studied owing to its topological states with a strong spin-orbit coupli...Interplay between topology and magnetism can give rise to exotic properties in topological materials.Two-dimensional bismuth has been extensively studied owing to its topological states with a strong spin-orbit coupling,and 1T-VTe_(2)monolayer theoretically predicted to host an intrinsic magnetism as experimentally suggested.In this work,we successfully constructed a vertical heterostructure composed of the two-dimensional Bi(110)monolayer and 1T-VTe_(2)monolayer by using molecular beam epitaxy(MBE).Scanning tunneling microscopy(STM)measurements revealed that the growth of Bi preferably occurs along the step edges of the VTe_(2)monolayer,forming a Bi(110)monolayer on top of the VTe_(2)monolayer next to a peripheral Bi bilayer.The Bi(100)/VTe_(2)heterostructure exhibits a specific lattice registry with a well-defined moiréperiodicity.Scanning tunneling spectroscopy(STS)measurements further unveiled an universal suppression in the local density-of-states at the boundary of the Bi(110)/VTe_(2)bilayer.By examining the atomic structures of Bi(110)boundaries,we found this effect does not originate from the previously proposed atomic reconstruction at the step edge of Bi(110),but is likely related to the magnetic properties of the VTe_(2)monolayer.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 SnSe_(2)/PtTe_(2) is a model system for realizing IS by using firstprinciples calculations.Our results show that due to slight but crucial interlayer charge transfer,SnSe_(2)/PtTe_(2) turns to be a type-Ⅲ heterostructure with metallic properties and shows a superconducting transition with the critical temperature(T_(c))of 3.73 K.Similar to the enhanced electron–phonon coupling(EPC)in the electrondoped SnSe_(2) monolayer,the IS in the SnSe_(2)/PtTe_(2) heterostructure mainly originates from the metallized SnSe_(2) 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 T_(c) can increase more than twofold(8.80 K),resulting from softened acoustic phonons at the𝑀point 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
Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthes...Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.展开更多
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
Metal halide perovskites have emerged as highly promising candidates for the emissive layer in next-generation light-emitting diodes(LEDs)due to their narrow emission linewidths,high photoluminescence quantum yields,a...Metal halide perovskites have emerged as highly promising candidates for the emissive layer in next-generation light-emitting diodes(LEDs)due to their narrow emission linewidths,high photoluminescence quantum yields,and tunable emission wavelengths.Achieving high-performance perovskite LEDs(Pe LEDs)requires the emissive layer to possess efficient radiative recombination,low defect density,minimal ion mobility,and effective carrier confinement.Perovskite/perovskite heterostructure(PPHS)offers a compelling approach for engineering emissive layers with these desired attributes,owing to their ability to passivate surface defects,tailor bandgaps,and suppress ion migration.Pe LEDs based on PPHS have demonstrated superior performance compared to single-phase devices,particularly in terms of external quantum efficiency and operational stability.This review provides a comprehensive overview of the typical PPHS architectures applied in Pe LEDs,including vertical,lateral,and bulk configurations.We discuss representative fabrication strategies and the associated optoelectronic properties of these heterostructures,highlighting the mechanisms by which they enhance device efficiency and stability.Finally,we explore the remaining challenges and prospects for the application of PPHS in Pe LEDs and other luminescent technologies.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 La_(0.7)Sr_(0.3)MnO_(3-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
MnO_(2) emerges as a promising cathode material for aqueous zinc-ion batteries(AZIBs)due to its high theoretical capacity and ideal working voltage.However,inherent limitations in low electrical conductivity and struc...MnO_(2) emerges as a promising cathode material for aqueous zinc-ion batteries(AZIBs)due to its high theoretical capacity and ideal working voltage.However,inherent limitations in low electrical conductivity and structural instability restrict its widespread application.Herein,we fabricated layered δ-MnO_(2) and introduced Cu and Ce metal ions for structural regulation,thus constructing a δ/a-MnO_(2) heterostructure within the δ-MnO_(2) matrix,forming a heterointerface that simultaneously enhances the electrical conductivity and structural stability of the material.In this system,Cu^(2+)acts as a catalyst,promoting the reduction of high-valent Mn to Mn^(2+)and enabling local two-electron transfer,which significantly increases the discharge specific capacity of MnO_(2).For Ce^(3+),it functions as a structural regulator,inducing the partial transformation of δ-MnO_(2) to a-MnO_(2) and forming the δ/a-MnO_(2) heterostructure.Further supported by density functional theory(DFT)calculations and in-situ characterization results,the heterointerface between a-MnO_(2) andδ-MnO_(2) generates an internal electric field due to the difference in Fermi levels.This not only effectively enhances the electron transfer capability but also significantly improves structural stability.Benefiting from these advantages,the Cu,Ce co-incorporated MnO_(2)(CCMO)cathode delivers a high discharge capacity of 455.4 mAh g^(-1)at 0.2 A g^(-1)and maintains 191.2 mAh g^(-1)specific capacity after 1500 cycles with 95%capacity retention at 2 A g^(-1),which is significantly better than non-doped MnO_(2).This strategy of structural regulation and heterostructure construction using vip ions offers a new approach for developing high-performance Mn-based cathode materials for AZIBs.展开更多
Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics...Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics,and free electron radiation devices.Particularly,they are promising platforms for studying thermionic emission.It is illustrated that using vdW heterostructure-based thermionic emission can enhance heat transfer in vacuum devices.As a proof of concept,the approach is demonstrated to offer a promising solution for the long-standing overheating issue in X-ray tubes.Specifically,it is shown that the saturated target temperature of a 2000 W X-ray tube can be reduced from around 1200℃ to 490℃.Additionally,it is also demonstrated that by reducing the height of the Schottky barrier formed in the vdW heterostructures,the thermionic cooling performance can be enhanced.The findings pave the way for the development of high-power X-ray tubes.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-Bi_(2)S_(3))nanorods with bonding heterostructures to improve thermoelectric performance.The approach employed iodine doping to introduce additional electrons,thereby regulating the band structure of Bi_(2)S_(3)and 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-Bi_(2)S_(3)nanorods were incorporated into poly-L-lactic acid(PLLA)scaffolds to confer antitumor functionality.According to the results,the bonding heterostructures enhanced the conductivity of Bi_(2)S_(3)and reduced its thermal conductivity,significantly enhancing thermoelectric efficacy.The heterostructures reduced the bandgap of Bi_(2)S_(3)from 1.23 to 0.88 eV,enabling optical absorption in the NIR-Ⅱregion.The ROS tests showed that the PLLA/I-Bi_(2)S_(3)scaffold exhibited good photothermal effects and ROS generation under 1064-nm laser irradiation.The antitumor efficacy of the PLLA/I-Bi_(2)S_(3)scaffold reached 84.6%against MG-63 cells,demonstrating its exceptional potential in cancer treatment.展开更多
The electrocatalytic reduction of nitrate to ammonia(NO_(3)^(−)RR)offers a sustainable alternative to energy-intensive industrial NH3 synthesis.Tandem catalysis has shown promise in overcoming the multi-step complexit...The electrocatalytic reduction of nitrate to ammonia(NO_(3)^(−)RR)offers a sustainable alternative to energy-intensive industrial NH3 synthesis.Tandem catalysis has shown promise in overcoming the multi-step complexity of NO_(3)^(−)RR,yet challenges remain in optimizing performance and elucidating tandem mechanisms.Herein,we report a Cu@Co/CoFe-P tandem electrocatalyst featuring a phosphorus-doped heterostructure with dual active sites(Cu-P and Co/CoFe-P).This catalyst achieves an exceptional NH_(3)yield of 175.40 mg h^(−1)cm^(−2)and a record-high current density exceeding 2 A cm^(−2),with the electro-synthesized NH3 directly converted into NH4Cl.In situ spectroscopic analysis and density functional theory(DFT)calculations reveal a novel desorption-reactivation tandem mechanism:(1)the Cu-P domain preferentially reduces NO_(3)^(−)to*NO_(2),which desorbs as stable NO_(2)^(−);(2)the Co/CoFe-P domain subsequently reactivates NO_(2)^(−),and converts it efficiently into NH3.Moreover,phosphorus doping enhances*H supply,while Fe alloying with Co promotes NO_(2)^(−)hydrogenation,ensuring an efficient and synchronized tandem pathway for NO_(3)^(−)RR.The proposed*NO_(2)desorption-reactivation mechanism deepens the understanding of NO_(3)^(−)RR tandem process,thereby paving the way for designing more efficient tandem electrocatalysts.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@SnO_(2)@Sn(CNS)heterostructure.The CNS absorber achieves a minimum reflection loss(RL_(min))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/SnO_(2) and CoNi/SnO_(2) 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 RL_(min) 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
The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising c...The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.展开更多
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
基金financially supported by the National Key Research and Development Program of China(Grant No.2021YFA1400403)the National Natural Science Foundation of China(Grant Nos.12374183,92165205)+2 种基金the Natural Science Foundation of Jiangsu Province(Grant No.BK20233001)the Innovation Program for Quantum Science and Technology(Grant No.2021ZD0302800)the Fundamental Research Funds for the Central Universities(Grant No.020414380207).
文摘Interplay between topology and magnetism can give rise to exotic properties in topological materials.Two-dimensional bismuth has been extensively studied owing to its topological states with a strong spin-orbit coupling,and 1T-VTe_(2)monolayer theoretically predicted to host an intrinsic magnetism as experimentally suggested.In this work,we successfully constructed a vertical heterostructure composed of the two-dimensional Bi(110)monolayer and 1T-VTe_(2)monolayer by using molecular beam epitaxy(MBE).Scanning tunneling microscopy(STM)measurements revealed that the growth of Bi preferably occurs along the step edges of the VTe_(2)monolayer,forming a Bi(110)monolayer on top of the VTe_(2)monolayer next to a peripheral Bi bilayer.The Bi(100)/VTe_(2)heterostructure exhibits a specific lattice registry with a well-defined moiréperiodicity.Scanning tunneling spectroscopy(STS)measurements further unveiled an universal suppression in the local density-of-states at the boundary of the Bi(110)/VTe_(2)bilayer.By examining the atomic structures of Bi(110)boundaries,we found this effect does not originate from the previously proposed atomic reconstruction at the step edge of Bi(110),but is likely related to the magnetic properties of the VTe_(2)monolayer.
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)。
文摘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 SnSe_(2)/PtTe_(2) is a model system for realizing IS by using firstprinciples calculations.Our results show that due to slight but crucial interlayer charge transfer,SnSe_(2)/PtTe_(2) turns to be a type-Ⅲ heterostructure with metallic properties and shows a superconducting transition with the critical temperature(T_(c))of 3.73 K.Similar to the enhanced electron–phonon coupling(EPC)in the electrondoped SnSe_(2) monolayer,the IS in the SnSe_(2)/PtTe_(2) heterostructure mainly originates from the metallized SnSe_(2) 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 T_(c) can increase more than twofold(8.80 K),resulting from softened acoustic phonons at the𝑀point 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 the National Natural Science Foundation of China (No.52274304)。
文摘Developing catalysts with excellent stability while significantly reducing the overpotential of the oxygen evolution reaction(OER) is crucial for advancing overall water splitting(OWS) systems.In this study,we synthesized the electrode material Ce-NiCo-LDHs@SnO_(2)/NF through a two-step hydrothermal reaction,where Ce-doped NiCo-LDHs are grown on nickel foam modified by a SnO_(2) layer.Ce doping adjusts the internal electronic distribution of Ni Co-LDHs,while the introduction of the SnO_(2) layer enhances electron transfer capability.Together,these factors contribute to the reduction of the OER energy barrier and experimental evidence confirms that the reaction proceeds via the lattice oxygen evolution mechanism(LOM).Consequently,Ce-NiCo-LDHs@SnO_(2)/NF exhibits high level electrochemical performance in OER,requiring only 234 m V overpotential to achieve a current density of 10 m A/cm^(2),with a Tafel slope of just 27.39 m V/dec.When paired with Pt/C/NF,an external potential of only 1.54 V is needed to drive OWS to attain a current density amounting to 10 m A/cm^(2).Furthermore,the catalyst demonstrates stability for 100 h during the OWS stability test.This study underscores the feasibility of enhancing the OER performance through Ce doping and the introduction of a conductive SnO_(2) layer.
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)+3 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。
文摘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 Advanced Talents Incubation Program of Hebei University(No.521100224235)the National Natural Science Foundation of China(No.52503363)the Natural Science Foundation of Hebei Province(No.E2025201009)。
文摘Metal halide perovskites have emerged as highly promising candidates for the emissive layer in next-generation light-emitting diodes(LEDs)due to their narrow emission linewidths,high photoluminescence quantum yields,and tunable emission wavelengths.Achieving high-performance perovskite LEDs(Pe LEDs)requires the emissive layer to possess efficient radiative recombination,low defect density,minimal ion mobility,and effective carrier confinement.Perovskite/perovskite heterostructure(PPHS)offers a compelling approach for engineering emissive layers with these desired attributes,owing to their ability to passivate surface defects,tailor bandgaps,and suppress ion migration.Pe LEDs based on PPHS have demonstrated superior performance compared to single-phase devices,particularly in terms of external quantum efficiency and operational stability.This review provides a comprehensive overview of the typical PPHS architectures applied in Pe LEDs,including vertical,lateral,and bulk configurations.We discuss representative fabrication strategies and the associated optoelectronic properties of these heterostructures,highlighting the mechanisms by which they enhance device efficiency and stability.Finally,we explore the remaining challenges and prospects for the application of PPHS in Pe LEDs and other luminescent technologies.
基金the financial support from the National Key Research and Development Program of China(2023YFB2504000)。
文摘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 La_(0.7)Sr_(0.3)MnO_(3-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 National Natural Science Foundation of China(no.52574348)the Natural Science Foundation of Hebei Province(nos.E2024501010 and B2024501004)+3 种基金the Shijiazhuang Basic Research Project(no.241790667A)the Fundamental Research Funds for the Central Universities(no.N2423013)the National College Students Innovation and Entrepreneurship Training Program(no.202419145017)the Performance Subsidy Fund for Key Laboratory of Dielectric,Electrolyte Functional Material Hebei Province(no.22567627H)。
文摘MnO_(2) emerges as a promising cathode material for aqueous zinc-ion batteries(AZIBs)due to its high theoretical capacity and ideal working voltage.However,inherent limitations in low electrical conductivity and structural instability restrict its widespread application.Herein,we fabricated layered δ-MnO_(2) and introduced Cu and Ce metal ions for structural regulation,thus constructing a δ/a-MnO_(2) heterostructure within the δ-MnO_(2) matrix,forming a heterointerface that simultaneously enhances the electrical conductivity and structural stability of the material.In this system,Cu^(2+)acts as a catalyst,promoting the reduction of high-valent Mn to Mn^(2+)and enabling local two-electron transfer,which significantly increases the discharge specific capacity of MnO_(2).For Ce^(3+),it functions as a structural regulator,inducing the partial transformation of δ-MnO_(2) to a-MnO_(2) and forming the δ/a-MnO_(2) heterostructure.Further supported by density functional theory(DFT)calculations and in-situ characterization results,the heterointerface between a-MnO_(2) andδ-MnO_(2) generates an internal electric field due to the difference in Fermi levels.This not only effectively enhances the electron transfer capability but also significantly improves structural stability.Benefiting from these advantages,the Cu,Ce co-incorporated MnO_(2)(CCMO)cathode delivers a high discharge capacity of 455.4 mAh g^(-1)at 0.2 A g^(-1)and maintains 191.2 mAh g^(-1)specific capacity after 1500 cycles with 95%capacity retention at 2 A g^(-1),which is significantly better than non-doped MnO_(2).This strategy of structural regulation and heterostructure construction using vip ions offers a new approach for developing high-performance Mn-based cathode materials for AZIBs.
基金supported by National Natural Science Foundation of China(61921002 and 92163204)。
文摘Van der Waals(vdW)heterostructures have attracted much attention due to their distinctive optical,electrical,and thermal properties,demonstrating promising potential in areas such as photocatalysis,ultrafast photonics,and free electron radiation devices.Particularly,they are promising platforms for studying thermionic emission.It is illustrated that using vdW heterostructure-based thermionic emission can enhance heat transfer in vacuum devices.As a proof of concept,the approach is demonstrated to offer a promising solution for the long-standing overheating issue in X-ray tubes.Specifically,it is shown that the saturated target temperature of a 2000 W X-ray tube can be reduced from around 1200℃ to 490℃.Additionally,it is also demonstrated that by reducing the height of the Schottky barrier formed in the vdW heterostructures,the thermionic cooling performance can be enhanced.The findings pave the way for the development of high-power X-ray tubes.
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)。
文摘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-Bi_(2)S_(3))nanorods with bonding heterostructures to improve thermoelectric performance.The approach employed iodine doping to introduce additional electrons,thereby regulating the band structure of Bi_(2)S_(3)and 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-Bi_(2)S_(3)nanorods were incorporated into poly-L-lactic acid(PLLA)scaffolds to confer antitumor functionality.According to the results,the bonding heterostructures enhanced the conductivity of Bi_(2)S_(3)and reduced its thermal conductivity,significantly enhancing thermoelectric efficacy.The heterostructures reduced the bandgap of Bi_(2)S_(3)from 1.23 to 0.88 eV,enabling optical absorption in the NIR-Ⅱregion.The ROS tests showed that the PLLA/I-Bi_(2)S_(3)scaffold exhibited good photothermal effects and ROS generation under 1064-nm laser irradiation.The antitumor efficacy of the PLLA/I-Bi_(2)S_(3)scaffold reached 84.6%against MG-63 cells,demonstrating its exceptional potential in cancer treatment.
基金supported financially by the Key Project of the National Ministry of Science and Technology (No.2022YFC3705005)the Open Foundation of Key Laboratory of Industrial Ecology and Environmental Engineering,MOE (KLIEEE-22-05)
文摘The electrocatalytic reduction of nitrate to ammonia(NO_(3)^(−)RR)offers a sustainable alternative to energy-intensive industrial NH3 synthesis.Tandem catalysis has shown promise in overcoming the multi-step complexity of NO_(3)^(−)RR,yet challenges remain in optimizing performance and elucidating tandem mechanisms.Herein,we report a Cu@Co/CoFe-P tandem electrocatalyst featuring a phosphorus-doped heterostructure with dual active sites(Cu-P and Co/CoFe-P).This catalyst achieves an exceptional NH_(3)yield of 175.40 mg h^(−1)cm^(−2)and a record-high current density exceeding 2 A cm^(−2),with the electro-synthesized NH3 directly converted into NH4Cl.In situ spectroscopic analysis and density functional theory(DFT)calculations reveal a novel desorption-reactivation tandem mechanism:(1)the Cu-P domain preferentially reduces NO_(3)^(−)to*NO_(2),which desorbs as stable NO_(2)^(−);(2)the Co/CoFe-P domain subsequently reactivates NO_(2)^(−),and converts it efficiently into NH3.Moreover,phosphorus doping enhances*H supply,while Fe alloying with Co promotes NO_(2)^(−)hydrogenation,ensuring an efficient and synchronized tandem pathway for NO_(3)^(−)RR.The proposed*NO_(2)desorption-reactivation mechanism deepens the understanding of NO_(3)^(−)RR tandem process,thereby paving the way for designing more efficient tandem electrocatalysts.
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).
文摘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@SnO_(2)@Sn(CNS)heterostructure.The CNS absorber achieves a minimum reflection loss(RL_(min))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/SnO_(2) and CoNi/SnO_(2) 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 RL_(min) 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financial support from 2024 Domestic Visiting Scholar Program for Teachers'Professional Development in Universities(Grant No.FX2024022)National Natural Science Foundation of China(Grant No.61904043)。
文摘The development of optoelectronic technologies demands photodetectors with miniaturization,broadband operation,high sensitivity,and low power consumption.Although 2D van der Waals(vd W)heterostructures are promising candidates due to their built-in electric fields,ultrafast photocarrier separation,and tunable bandgaps,defect states limit their performance.Therefore,the modulation of the optoelectronic properties in such heterostructures is imperative.Surface charge transfer doping(SCTD)has emerged as a promising strategy for non-destructive modulation of electronic and optoelectronic characteristics in two-dimensional materials.In this work,we demonstrate the construction of high-performance p-i-n vertical heterojunction photodetectors through SCTD of MoTe_(2)/ReS_(2)heterostructure using p-type F_(4)-TCNQ.Systematic characterization reveals that the interfacial doping process effectively amplifies the built-in electric field,enhancing photogenerated carrier separation efficiency.Compared to the pristine heterojunction device,the doped photodetector exhibits remarkable visible to nearinfrared(635-1064 nm)performance.Particularly under 1064 nm illumination at zero bias,the device achieves a responsivity of 2.86 A/W and specific detectivity of 1.41×10^(12)Jones.Notably,the external quantum efficiency reaches an exceptional value of 334%compared to the initial 11.5%,while maintaining ultrafast response characteristics with rise/fall times of 11.6/15.6μs.This work provides new insights into interface engineering through molecular doping for developing high-performance vd W optoelectronic devices.
