Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor.Herein,a novel core-shell heterostructured electrode,combining CoS hollow na...Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor.Herein,a novel core-shell heterostructured electrode,combining CoS hollow nanorods with NiCoMn-layered double hydroxides(LDH)ternary metal nanosheets,were prepared on carbon cloth by reasonably controlled vulcanization and electrodeposition.By optimizing electrodeposition conditions,the material's structure and properties can be fine-tuned.The enhanced capacitance of the optimized carbon cloth(CC)@CoS/NiCoMn-LDH-300 electrode(4256.0 F g^(-1))lies in the open space provided by CoS and the establishment of a new charge transfer channel across the interfaces of CC@CoS/NiCoMn-LDH-300 nanosheets.This is further demonstrated by Density functional theory(DFT)simulations based on OHadsorption energy,which produces faster redox charge kinetics and significantly enhances the electrode's energy storage capacity.The hybrid supercapacitor,integrating the optimized CC@CoS/NiCoMn-LDH-300 electrode with active carbon,demonstrates the highest energy density of 86 Wh kg^(-1)(under the power density of 850 W kg^(-1))and the long cycle stability of 89.7%.This study aims to go beyond simple binary LDH by constructing a ternary LDH with a hierarchical core-shell heterostructure to provide an effective and feasible new concept for high-performance supercapacitor electrode materials via rational structure design.展开更多
Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective int...Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.展开更多
Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an u...Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent requirement.In this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and SIBs.The optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active sites.Co_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in SIB.Density functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical properties.This heterostructure building technique may pave the way for the development of high-performance LIBs and SIBs.Furthermore,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.展开更多
Graphene, with its zero-bandgap electronic structure, is a highly promising ultra-broadband light absorbing material.However, the performance of graphene-based photodetectors is limited by weak absorption efficiency a...Graphene, with its zero-bandgap electronic structure, is a highly promising ultra-broadband light absorbing material.However, the performance of graphene-based photodetectors is limited by weak absorption efficiency and rapid recombination of photoexcited carriers, leading to poor photodetection performance. Here, inspired by the photogating effect, we demonstrated a highly sensitive photodetector based on graphene/WSe_(2) vertical heterostructure where the WSe_(2) layer acts as both the light absorption layer and the localized grating layer. The graphene conductive channel is induced to produce more carriers by capacitive coupling. Due to the strong light absorption and high external quantum efficiency of multilayer WSe_(2), as well as the high carrier mobility of graphene, a high photocurrent is generated in the vertical heterostructure. As a result, the photodetector exhibits ultra-high responsivity of 3.85×10~4A/W and external quantum efficiency of 1.3 × 10~7%.This finding demonstrates that photogating structures can effectively enhance the sensitivity of graphene-based photodetectors and may have great potential applications in future optoelectronic devices.展开更多
Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveragi...Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.展开更多
Lithium-oxygen batteries(LOBs)with high energy density are a promising advanced energy storage technology.However,the slow cathodic redox kinetics during cycling causes the discharge products to fail to decompose in t...Lithium-oxygen batteries(LOBs)with high energy density are a promising advanced energy storage technology.However,the slow cathodic redox kinetics during cycling causes the discharge products to fail to decompose in time,resulting in large polarization and battery failure in a short time.Therefore,a self-supporting interconnected nanosheet array network NiCo_(2)O_(4)/MnO_(2)with a Mott-Schottky heterostructure on titanium paper(TP-NCO/MO)is ingeniously designed as an efficient cathode catalyst material for LOBs.This heterostructure can accelerate electron transfer and influence the charge transfer process during adsorption of intermediate by triggering the interface disturbance at the heterogeneous interface,thus accelerating oxygen reduction and oxygen evolution kinetics and regulating product decomposition,which is expected to solve the above problems.The meticulously designed unique structural advantages enable the TP-NCO/MO cathode catalyst to exhibit an astounding ultra-long cycle life of 800 cycles and an extraordinarily low overpotential of 0.73 V.This study utilizes a simple method to cleverly regulate the morphology of the discharge products by constructing a Mott-Schottky heterostructure,providing important reference for the design of efficient catalysts aimed at optimizing the adsorption of reaction intermediates.展开更多
Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR)...Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.展开更多
The drive for efficient thermal management has intensified with the miniaturization of electronic devices.This study explores the modulation of phonon transport within graphene by introducing silicon nanoparticles inf...The drive for efficient thermal management has intensified with the miniaturization of electronic devices.This study explores the modulation of phonon transport within graphene by introducing silicon nanoparticles influenced by van der Waals forces.Our approach involves the application of non-equilibrium molecular dynamics to assess thermal conductivity while varying the interaction strength,leading to a noteworthy reduction in thermal conductivity.Furthermore,we observe a distinct attenuation in length-dependent behavior within the graphene-nanoparticles system.Our exploration combines wave packet simulations with phonon transmission calculations,aligning with a comprehensive analysis of the phonon transport regime to unveil the underlying physical mechanisms at play.Lastly,we conduct transient molecular dynamics simulations to investigate interfacial thermal conductance between the nanoparticles and the graphene,revealing an enhanced thermal boundary conductance.This research not only contributes to our understanding of phonon transport but also opens a new degree of freedom for utilizing van der Waals nanoparticle-induced resonance,offering promising avenues for the modulation of thermal properties in advanced materials and enhancing their performance in various technological applications.展开更多
Based on first-principles calculations,we investigate the electronic band structures and topological properties of heterostructure BiTeCl/HfTe_(2) under c-direction strain.In the primitive structure,this material unde...Based on first-principles calculations,we investigate the electronic band structures and topological properties of heterostructure BiTeCl/HfTe_(2) under c-direction strain.In the primitive structure,this material undergoes a phase transition from an insulator with a narrow indirect gap to a metal by strong spin-orbital coupling.When strain effect is considered,band inversion at time-reversal invariant point Z is responsible for the topological phase transition.These nontrivial topologies are caused by two different types of band crossings.The observable topological surface states in(110)surface also support that this material experiences topological phase transition twice.The layered heterostructure with van der Waals force provides us with a new desirable platform upon which to control topological phase transition and construct topological superconductors.展开更多
Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air batteries.However,the active sites in def...Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air batteries.However,the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage,leading to rapid degradation of activity.Herein,we design a van der Waals heterostructure comprised of vitamin C(VC)and defective carbon(DC)to not only boost the activity but also enhance the durability and storage stability of the DC-VC electrocatalyst.The formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation,thus significantly enhancing the electrochemical durability and storage anti-aging performance.Moreover,the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the ORR.These findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory calculations.It is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up,and the ORR performance of the largely produced electrocatalyst is demonstrated to be very consistent.Furthermore,the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.展开更多
The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy b...The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER.In this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor.The RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water dissociation.This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.展开更多
The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuni...The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.展开更多
Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and u...Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.展开更多
The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox kinetics.Herein,a tungsten and molybdenum nitride heterostructur...The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox kinetics.Herein,a tungsten and molybdenum nitride heterostructure functionalized with hollow metal-organic framework-derived carbon(W_(2)N/Mo_(2)N)was proposed as the sulfur host.The hollow spherical structure provides storage space for sulfur,enhances electrical conductivity,and inhibits volume expansion.The metal atoms in the nitrides bonded with lithium polysulfides(Li PSs)through Lewis covalent bonds,enhancing the high catalytic activity of the nitrides and effectively reducing the energy barrier of Li PSs redox conversion.Moreover,the high intrinsic conductivity of nitrides and the ability of the heterostructure interface to accelerate electron/ion transport improved the Li+transmission.By leveraging the combined properties of strong adsorption and high catalytic activity,the sulfur host effectively inhibited the shuttle effect and accelerated the redox kinetics of Li PSs.High-efficiency Li+transmission,strong adsorption,and the efficient catalytic conversion activities of Li PSs in the heterostructure were experimentally and theoretically verified.The results indicate that the W_(2)N/Mo_(2)N cathode provides stable,and long-term cycling(over 2000 cycles)at 3 C with a low attenuation rate of 0.0196%per cycle.The design strategy of a twinborn nitride heterostructure thus provides a functionalized solution for advanced Li-S batteries.展开更多
Manipulating strain mode and degree that can be applied to epitaxial complex oxide thin films have been a cornerstone of strain engineering.In recent years,lift-off and transfer technology of the epitaxial oxide thin ...Manipulating strain mode and degree that can be applied to epitaxial complex oxide thin films have been a cornerstone of strain engineering.In recent years,lift-off and transfer technology of the epitaxial oxide thin films have been developed that enabled the integration of heterostructures without the limitation of material types and crystal orientations.Moreover,twisted integration would provide a more interesting strategy in artificial magnetoelectric heterostructures.A specific twist angle between the ferroelectric and ferromagnetic oxide layers corresponds to the distinct strain regulation modes in the magnetoelectric coupling process,which could provide some insight in to the physical phenomena.In this work,the La_(0.67)Sr_(0.33)MnO_(3)(001)/0.7Pb(Mg_(1/3)Nb_(2/3))O_(3)-0.3PbTiO_(3)(011)(LSMO/PMN-PT)heterostructures with 45.and 0.twist angles were assembled via water-etching and transfer process.The transferred LSMO films exhibit a fourfold magnetic anisotropy with easy axis along LSMO<110>.A coexistence of uniaxial and fourfold magnetic anisotropy with LSMO[110]easy axis is observed for the 45°Sample by applying a 7.2 kV cm^(−1)electrical field,significantly different from a uniaxial anisotropy with LSMO[100]easy axis for the 0°Sample.The fitting of the ferromagnetic resonance field reveals that the strain coupling generated by the 45°twist angle causes different lattice distortion of LSMO,thereby enhancing both the fourfold and uniaxial anisotropy.This work confirms the twisting degrees of freedom for magnetoelectric coupling and opens opportunities for fabricating artificial magnetoelectric heterostructures.展开更多
Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4...Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.展开更多
Recently,significant experimental advancements in achieving topological phases have been reported in van der Waals(vdW)heterostructures involving graphene.Here,using first-principles calculations,we investigate graphe...Recently,significant experimental advancements in achieving topological phases have been reported in van der Waals(vdW)heterostructures involving graphene.Here,using first-principles calculations,we investigate graphene/CoBr_(2)(Gr/CoBr_(2))heterostructures and find that an enhancement of in-plane magnetic anisotropy(IMA)energy in monolayer CoBr_(2) can be accomplished by reducing the interlayer distance of the vdW heterostructures.In addition,we clarify that the enhancement of IMA energy primarily results from two factors:one is the weakness of the Co-d_(xy) and Co-d_(x^(2)-y^(2)) orbital hybridization and the other is the augmentation of the Co-d_(yz) and Co-d_(z)2 orbital hybridization.Meanwhile,calculation results suggest that the Kosterlitz–Thouless phase transition temperature(TKT)of a 2D XY magnet Gr/CoBr_(2)(23.8 K)is higher than that of a 2D XY monolayer CoBr_(2)(1.35 K).By decreasing the interlayer distances,the proximity effect is more pronounced and band splitting appears.Moreover,by taking into account spin–orbit coupling,a band gap of approximately 14.3 meV and the quantum anomalous Hall effect(QAHE)are attained by decreasing the interlayer distance by 1.0 A.Inspired by the above conclusions,we design a topological field transistor device model.Our results support that the vdW interlayer distance can be used to modulate the IMA energy and QAHE of materials,providing a pathway for the development of new low-power spintronic devices.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-lumines...Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-luminescence(PL)quantum yield of monolayer(1L)TMDs is still quite low at room temperature,which severely lim-its their practical applications.Here we report a PL enhancement effect of 1L WS_(2) at room temperature when con-structing it into 1L-WS_(2)/hBN/1L-MoS_(2) vertical HSs.The PL enhancement factors(EFs)can be up to 4.2.By using transient absorption(TA)spectroscopy,we demonstrate that the PL enhancement effect is due to energy transfer from 1L MoS_(2) to 1L WS_(2).The energy transfer process occurs on a picosecond timescale and lasts more than one hundred picoseconds which indicates a prominent contribution from exciton-exciton annihilation.Furthermore,the PL en-hancement effect of 1L WS_(2) can be observed in 2L-MoS_(2)/hBN/1L-WS_(2) and 3L-MoS_(2)/hBN/1L-WS_(2) HSs.Our study provides a comprehensive understanding of the energy transfer process in the PL enhancement of 2D TMDs and a fea-sible way to optimize the performance of TMD-based optoelectronic devices.展开更多
For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development...For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development of modern semiconductor spintronics are the generation,detection,and manipulation of spin currents.Here,the transport characteristics of a spin current generated by spin pumping through a GeBi semiconductor barrier in Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures were investigated systematically.The effective spin-mixing conductance and inverse spin Hall voltage to quantitatively describe the spin transport characteristics were extracted.The spin-injection efficiency in the Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures is comparable to that of the Y_(3)Fe_(5)O_(12)/Pt bilayer,and the inverse spin Hall voltage exponential decays with the increase in the barrier thickness.Furthermore,the band gap of the GeBi layer was tuned by changing the Bi content.The spin-injection efficiency at the YIG/semiconductor interface and the spin transportation within the semiconductor barrier are related to the band gap of the GeBi layer.Our results may be used as guidelines for the fabrication of efficient spin transmission structures and may lead to further studies on the impacts of different kinds of barrier materials.展开更多
Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S...Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S_(4) heterostructures with strong hetero-interface interaction and abundant contact were constructed via an impregnation-annealing strategy.Efficient charge transfer from ZnIn_(2)S_(4) to WSe_(2)was evidenced by transient absorption spectroscopy in crafted heterostructures owing to the tight and2D face-to-face contact.As a result,the prepared WSe_(2)/ZnIn_(2)S_(4) heterostructures exhibited boosted photocatalytic performance and a highest hydrogen evolution rate of 3.377 mmol/(g h)was achieved with an apparent quantum yield of 45.7%at 420 nm.The work not only provides new strategies to achieve efficient 2D/2D heterostructures but also paves the way for the development of green hydrogen in the future.展开更多
基金supported by the National Natural Science Foundation of China(52203147)the Zhejiang Provincial Natural Science Foundation of China(LQ22B010006)+2 种基金the significant science and technology projects of LongMen Laboratory in Henan Province(231100221100)the significant science and technology projects of LongMen Laboratory in Henan Province(231100220100)the Key research and development program of Henan province(231111222200).
文摘Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor.Herein,a novel core-shell heterostructured electrode,combining CoS hollow nanorods with NiCoMn-layered double hydroxides(LDH)ternary metal nanosheets,were prepared on carbon cloth by reasonably controlled vulcanization and electrodeposition.By optimizing electrodeposition conditions,the material's structure and properties can be fine-tuned.The enhanced capacitance of the optimized carbon cloth(CC)@CoS/NiCoMn-LDH-300 electrode(4256.0 F g^(-1))lies in the open space provided by CoS and the establishment of a new charge transfer channel across the interfaces of CC@CoS/NiCoMn-LDH-300 nanosheets.This is further demonstrated by Density functional theory(DFT)simulations based on OHadsorption energy,which produces faster redox charge kinetics and significantly enhances the electrode's energy storage capacity.The hybrid supercapacitor,integrating the optimized CC@CoS/NiCoMn-LDH-300 electrode with active carbon,demonstrates the highest energy density of 86 Wh kg^(-1)(under the power density of 850 W kg^(-1))and the long cycle stability of 89.7%.This study aims to go beyond simple binary LDH by constructing a ternary LDH with a hierarchical core-shell heterostructure to provide an effective and feasible new concept for high-performance supercapacitor electrode materials via rational structure design.
基金provided by Guizhou Provincial Science and Technology Projects for Platform and Talent Team Plan(GCC[2023]007)Fok Ying Tung Education Foundation(171095)National Natural Science Foundation of China(11964006).
文摘Considering the serious electromagnetic wave(EMW)pollution problems and complex application condition,there is a pressing need to amalgamate multiple functionalities within a single substance.However,the effective integration of diverse functions into designed EMW absorption materials still faces the huge challenges.Herein,reduced graphene oxide/carbon foams(RGO/CFs)with two-dimensional/three-dimensional(2D/3D)van der Waals(vdWs)heterostructures were meticulously engineered and synthesized utilizing an efficient methodology involving freeze-drying,immersing absorption,secondary freeze-drying,followed by carbonization treatment.Thanks to their excellent linkage effect of amplified dielectric loss and optimized impedance matching,the designed 2D/3D RGO/CFs vdWs heterostructures demonstrated commendable EMW absorption performances,achieving a broad absorption bandwidth of 6.2 GHz and a reflection loss of-50.58 dB with the low matching thicknesses.Furthermore,the obtained 2D/3D RGO/CFs vdWs heterostructures also displayed the significant radar stealth properties,good corrosion resistance performances as well as outstanding thermal insulation capabilities,displaying the great potential in complex and variable environments.Accordingly,this work not only demonstrated a straightforward method for fabricating 2D/3D vdWs heterostructures,but also outlined a powerful mixeddimensional assembly strategy for engineering multifunctional foams for electromagnetic protection,aerospace and other complex conditions.
基金financially supported by the Open Fund of Energy and Materials Chemistry Joint Laboratory of SCNU and TINCI,China (SCNU-TINCI-202207)。
文摘Solving the problems of low electrical conductivity and poor cycling durability in transition metal oxidesbased anode materials for lithium-ion batteries(LIBs)and sodium-ion batteries(SIBs)has already turned into an urgent requirement.In this paper,we successfully synthesized Co_(2)VO_(4)/Co compounds with Co-VMOF(metal-organic framework)as a sacrificial template and investigated their electrochemical mechanism in order to improve the electrochemical properties of LIBs and SIBs.The optimized heaping configuration and the existence of metallic Co catalyzed the formation of radical ions,thereby facilitating higher conductivity,shortening Li+and Na+transport paths,and providing more active sites.Co_(2)VO_(4)/Co constructed with 2-methylimidazole as a ligand showed a discharge capacity of 1605.1 mA h g^(-1)after 300 cycles at 0.1 A g^(-1)in LIB and 677.2 mA h g^(-1)in SIB.Density functional theory(DFT)calculation emphasizes the crucial role of Co_(2)VO_(4)/Co in enhancing electrode conductivity,decreasing the migratory energy barrier,and thereby strengthening electrochemical properties.This heterostructure building technique may pave the way for the development of high-performance LIBs and SIBs.Furthermore,the problem of the low first-loop coulombic efficiency faced by transition metal oxides is improved.
基金Project supported by the National Natural Science Foundation of China (Grant No.11974379)the National Key Basic Research and Development Program of China (Grant No.2021YFC2203400)Jiangsu Vocational Education Integrated Circuit Technology “Double-Qualified” Famous Teacher Studio (Grant No.2022-13)。
文摘Graphene, with its zero-bandgap electronic structure, is a highly promising ultra-broadband light absorbing material.However, the performance of graphene-based photodetectors is limited by weak absorption efficiency and rapid recombination of photoexcited carriers, leading to poor photodetection performance. Here, inspired by the photogating effect, we demonstrated a highly sensitive photodetector based on graphene/WSe_(2) vertical heterostructure where the WSe_(2) layer acts as both the light absorption layer and the localized grating layer. The graphene conductive channel is induced to produce more carriers by capacitive coupling. Due to the strong light absorption and high external quantum efficiency of multilayer WSe_(2), as well as the high carrier mobility of graphene, a high photocurrent is generated in the vertical heterostructure. As a result, the photodetector exhibits ultra-high responsivity of 3.85×10~4A/W and external quantum efficiency of 1.3 × 10~7%.This finding demonstrates that photogating structures can effectively enhance the sensitivity of graphene-based photodetectors and may have great potential applications in future optoelectronic devices.
基金financial support from the Swiss National Science Foundation via the Southeast Asia–Europe Joint Funding Scheme 2020(Grant No.IZJFZ2_202476)funding from the National Natural Science Foundation of China(Grant Nos.22209118 and 00301054A1073)the Fundamental Research Funds for the Central Universities(Grant Nos.1082204112A26,20826044D3083,and 20822041G4080)。
文摘Poor cycling stability in lithium–sulfur(Li–S)batteries necessitates advanced electrode/electrolyte design and innovative interlayer architectures.Heterogeneous catalysis has emerged as a promising approach,leveraging the adsorption and catalytic performance on lithium polysulfides(LiPSs)to inhibit LiPSs shuttling and improve redox kinetics.In this study,we report an ultrathin and laminar SnO_(2)@MXene heterostructure interlayer(SnO_(2)@MX),where SnO_(2) quantum dots(QDs)are uniformly distributed across the MXene layer.The combined structure of SnO_(2) QDs and MXene,along with the creation of numerous active boundary sites with coordination electron environments,plays a critical role in manipulating the catalytic kinetics of sulfur species.The Li–S cell with the SnO_(2)@MX-modified separator not only demonstrates superior electrochemical performance compared to cells with a bare separator but also induces homogeneous Li deposition during cycling.As a result,an areal capacity of 7.6 mAh cm^(-2) under a sulfur loading of 7.5 mg cm^(-2) and a high stability over 500 cycles are achieved.Our work demonstrates a feasible strategy of utilizing a laminar separator interlayer for advanced Li–S batteries awaiting commercialization and may shed light on the understanding of heterostructure catalysis with enhanced reaction kinetics.
基金the financial support from the National Natural Science Foundation of China (grant nos. 51971184 and 51931006)the Natural Science Foundation of Fujian Province of China (no. 2023J01033)+1 种基金the Fundamental Research Funds for the Central Universities of China (Xiamen University: no. 20 720 200 068)the “Double First Class” Foundation of Materials Intelligent Manufacturing Discipline of Xiamen University
文摘Lithium-oxygen batteries(LOBs)with high energy density are a promising advanced energy storage technology.However,the slow cathodic redox kinetics during cycling causes the discharge products to fail to decompose in time,resulting in large polarization and battery failure in a short time.Therefore,a self-supporting interconnected nanosheet array network NiCo_(2)O_(4)/MnO_(2)with a Mott-Schottky heterostructure on titanium paper(TP-NCO/MO)is ingeniously designed as an efficient cathode catalyst material for LOBs.This heterostructure can accelerate electron transfer and influence the charge transfer process during adsorption of intermediate by triggering the interface disturbance at the heterogeneous interface,thus accelerating oxygen reduction and oxygen evolution kinetics and regulating product decomposition,which is expected to solve the above problems.The meticulously designed unique structural advantages enable the TP-NCO/MO cathode catalyst to exhibit an astounding ultra-long cycle life of 800 cycles and an extraordinarily low overpotential of 0.73 V.This study utilizes a simple method to cleverly regulate the morphology of the discharge products by constructing a Mott-Schottky heterostructure,providing important reference for the design of efficient catalysts aimed at optimizing the adsorption of reaction intermediates.
基金financially supported by the National Natural Science Foundation of China (52363028)the Natural Science Foundation of Guangxi Province (2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject (GUIKE AD23023004,GUIKE AD20297039)
文摘Precisely tailoring the surface electronic structures of electrocatalysts for optimal hydrogen binding energy and hydroxide binding energy is vital to improve the sluggish kinetics of hydrogen oxidation reac-tion(HOR).Herein,we employ a partial desulfurization strategy to construct a homologous Ru-RuS_(2) heterostructure anchored on hollow mesoporous carbon nanospheres(Ru-RuS_(2)@C).The disparate work functions of the heterostructure contribute to the spontaneous formation of a unique built-in electric field,accelerating charge transfer and boosting conductivity of electrocatalyst.Consequently,Ru-RuS_(2)@C exhibits robust HOR electrocatalytic activity,achieving an exchange current density and mass activity as high as 3.56 mA cm^(-2) and 2.13 mAμg_(Ru)^(-1),respectively.exceeding those of state-of-the-art Pt/C and most contemporary Ru-based HOR electrocatalysts.Surprisingly,Ru-RuS_(2)@C can tolerate 1000 ppm of cO that lacks in Pt/C.Comprehensive analysis reveals that the directional electron transfer across Ru-RuS_(2) heterointerface induces local charge redistribution in interfacial region,which optimizes and balances the adsorption energies of H and OH species,as well as lowers the energy barrier for water formation,thereby promoting theHoR performance.
基金funded in parts by the National Natural Science Foundation of China (Grant No.12105242)Yunnan Fundamental Research Project (Grant Nos.202201AT070161 and 202301AW070006)support from the Graduate Scientific Research and Innovation Fund of Yunnan University (Grant No.KC-22221060)。
文摘The drive for efficient thermal management has intensified with the miniaturization of electronic devices.This study explores the modulation of phonon transport within graphene by introducing silicon nanoparticles influenced by van der Waals forces.Our approach involves the application of non-equilibrium molecular dynamics to assess thermal conductivity while varying the interaction strength,leading to a noteworthy reduction in thermal conductivity.Furthermore,we observe a distinct attenuation in length-dependent behavior within the graphene-nanoparticles system.Our exploration combines wave packet simulations with phonon transmission calculations,aligning with a comprehensive analysis of the phonon transport regime to unveil the underlying physical mechanisms at play.Lastly,we conduct transient molecular dynamics simulations to investigate interfacial thermal conductance between the nanoparticles and the graphene,revealing an enhanced thermal boundary conductance.This research not only contributes to our understanding of phonon transport but also opens a new degree of freedom for utilizing van der Waals nanoparticle-induced resonance,offering promising avenues for the modulation of thermal properties in advanced materials and enhancing their performance in various technological applications.
文摘Based on first-principles calculations,we investigate the electronic band structures and topological properties of heterostructure BiTeCl/HfTe_(2) under c-direction strain.In the primitive structure,this material undergoes a phase transition from an insulator with a narrow indirect gap to a metal by strong spin-orbital coupling.When strain effect is considered,band inversion at time-reversal invariant point Z is responsible for the topological phase transition.These nontrivial topologies are caused by two different types of band crossings.The observable topological surface states in(110)surface also support that this material experiences topological phase transition twice.The layered heterostructure with van der Waals force provides us with a new desirable platform upon which to control topological phase transition and construct topological superconductors.
基金financially supported by the National Natural Science Foundation of China (51874197)the Natural Science Foundation of Shanghai (21ZR1429400,22ZR1429700)。
文摘Metal-free defective carbon materials with abundant active sites have been widely studied as low-cost and efficient oxygen reduction reaction(ORR)electrocatalysts in metal-air batteries.However,the active sites in defective carbon are easily subjected to serious oxidation or hydroxylation during ORR or storage,leading to rapid degradation of activity.Herein,we design a van der Waals heterostructure comprised of vitamin C(VC)and defective carbon(DC)to not only boost the activity but also enhance the durability and storage stability of the DC-VC electrocatalyst.The formation of VC van der Waals between DC and VC is demonstrated to be an effective strategy to protect the defect active sites from oxidation and hydroxylation degradation,thus significantly enhancing the electrochemical durability and storage anti-aging performance.Moreover,the DC-VC van der Waals can reduce the reaction energy barrier to facilitate the ORR.These findings are also confirmed by operando Fourier transform infrared spectroscopy and density functional theory calculations.It is necessary to mention that the preparation of this DC-VC electrocatalyst can be scaled up,and the ORR performance of the largely produced electrocatalyst is demonstrated to be very consistent.Furthermore,the DC-VC-based aluminum-air batteries display very competitive power density with good performance maintenance.
基金supported by the National Natural Science Foundation of China (21721003,22202080 and 22034006)。
文摘The slow water dissociation is the rate-determining step that slows down the reaction rate in alkaline hydrogen evolution reaction(HER).Optimizing the surface electronic structure of the catalyst to lower the energy barrier of water dissociation and regulating the binding strength of adsorption intermediates are crucial strategy for boosting the catalytic performance of HER.In this study,RuO_(2)/BaRuO_(3)(RBRO)heterostructures with abundant oxygen vacancies and lattice distortion were in-situ constructed under a low temperature via the thermal decomposition of gel-precursor.The RBRO heterostructures obtained at 550℃ exhibited the highest HER activity in 1 M KOH,showing an ultra-low overpotential of 16 mV at 10 mA cm^(-2)and a Tafel slope of 33.37 m V dec^(-1).Additionally,the material demonstrated remarkable durability,with only 25 mV of degradation in overpotential after 200 h of stability testing at 10 mA cm^(-2).Density functional theory calculations revealed that the redistribution of charges at the heterojunction interface can optimize the binding energies of H*and OH*and effectively lower the energy barrier of water dissociation.This research offers novel perspectives on surpassing the water dissociation threshold of alkaline HER catalysts by means of a systematic design of heterogeneous interfaces.
基金supported by the National Natural Science Foundation of China (52173286, 52207249)Major basic research project of Natural Science Foundation of Shandong Province (ZR2023ZD12)+1 种基金the State Key Laboratory of Marine Resource Utilization in South China Sea (Hainan University) (MRUKF2023013)Open Program of Guangxi Key Laboratory of Information Materials (221024-K)。
文摘The inherent catalytic anisotropy of two-dimensional(2D) materials has limited the enhancement of LiO_(2) batteries(LOBs) performance due to the significantly different adsorption energies on 2D and edge surfaces.Tuning the adsorption strength in 2D materials to the reaction intermediates is essential for achieving high-performance LOBs.Herein,a MnS/MoS_(2) heterostructure is designed as a cathode catalyst by adjusting the adsorption behavior at the surface.Different from the toroidal-like discharge products on the MoS_(2) cathode,the MnS/MoS_(2) surface displays an improved adsorption energy to reaction species,thereby promoting the growth of the film-like discharge products.MnS can disturb the layer growth of MoS_(2),in which the stack edge plane features a strong interaction with the intermediates and limits the growth of the discharge products.Experimental and theoretical results confirm that the MnS/MoS_(2) heterostructure possesses improved electron transfer kinetics at the interface and plays an important role in the adsorption process for reaction species,which finally affects the morphology of Li_2O_(2),In consequence,the MnS/MoS_(2) heterostructure exhibits a high specific capacity of 11696.0 mA h g^(-1) and good cycle stability over 1800 h with a fixed specific capacity of 600 mA h g^(-1) at current density of100 mA g^(-1) This work provides a novel interfacial engineering strategy to enhance the performance of LOBs by tuning the adsorption properties of 2D materials.
基金financially supported by the Natural Science Foundation of Shandong Province(ZR2021QB055,ZR2023MB017,ZR2022JQ10)the National Natural Science Foundation of China(21901146,220781792,22274083)。
文摘Constructing heterostructure is considered as an effective strategy to address the sluggish electronic and ionic kinetics of anode materials for sodium ion batteries(SIBs).However,realizing the orientated growth and uniform distribution of the heterostructure is still a great challenge.Herein,the regulated novel CoSe_(2)/NiSe_(2)heterostructure confined in N-doped carbon nanofibers(CoSe_(2)/NiSe_(2)@N-C)are prepared by using Co/Ni-ZIF template,in which,the CoSe_(2)/NiSe_(2)heterostructures realize uniform distribution on a micro level.Benefiting from the unique heterostructure and N-doped carbon nanofibers,the CoSe_(2)/NiSe_(2)@N-C deliveries superior rate capability and durable cycle lifespan with a reversible capacity of 400.5 mA h g^(-1)after 5000 cycles at 2 A g^(-1).The Na-ion full battery with CoSe_(2)/NiSe_(2)@N-C anode and layered oxide cathode displays a remarkable energy density of 563 W h kg^(-1)with 241.1 W kg^(-1)at 0.1 A g^(-1).The theoretical calculations disclose that the periodic and directional built-in electric-field along with the heterointerfaces of CoSe_(2)/NiSe_(2)@N-C can accelerate electrochemical reaction kinetics.The in(ex)situ experimental measurements reveal the reversible conversion reaction and stable structure of CoSe_(2)/NiSe_(2)@N-C during Na+insertion/extraction.The study highlights the potential ability of precisely controlled heterostructure to stimulate the electrochemical performances of advanced anode for SIBs.
基金supported by the National Natural Science Foundation of China (52202104)the China Postdoctoral Science Foundation (2021T140433,2020M683408)+6 种基金the Joint Funds of the Zhejiang Provincial Natural Science Foundation of China (LZY23B030002)the Quzhou Science and Technology Bureau Project (2021D006)the International Cooperation Projects of Sichuan Provincial Department of Science and Technology (2021YFH0126)the Fundamental Research Funds for the Central Universities (ZYGX2020ZB016)the Key Research and Development Program of Yunnan Province China (202103AA080019)the Yunnan Major Scientific and Technological Projects (202202AG050003)the Foundation of Key Laboratory of Advanced Technique&Preparation for Renewable Energy Materials,Ministry of Education,Yunnan Normal University (OF2022-04)。
文摘The practical application of lithium-sulfur(Li-S)batteries,as promising next-generation batteries,is hindered by their shuttle effect and the slow redox kinetics.Herein,a tungsten and molybdenum nitride heterostructure functionalized with hollow metal-organic framework-derived carbon(W_(2)N/Mo_(2)N)was proposed as the sulfur host.The hollow spherical structure provides storage space for sulfur,enhances electrical conductivity,and inhibits volume expansion.The metal atoms in the nitrides bonded with lithium polysulfides(Li PSs)through Lewis covalent bonds,enhancing the high catalytic activity of the nitrides and effectively reducing the energy barrier of Li PSs redox conversion.Moreover,the high intrinsic conductivity of nitrides and the ability of the heterostructure interface to accelerate electron/ion transport improved the Li+transmission.By leveraging the combined properties of strong adsorption and high catalytic activity,the sulfur host effectively inhibited the shuttle effect and accelerated the redox kinetics of Li PSs.High-efficiency Li+transmission,strong adsorption,and the efficient catalytic conversion activities of Li PSs in the heterostructure were experimentally and theoretically verified.The results indicate that the W_(2)N/Mo_(2)N cathode provides stable,and long-term cycling(over 2000 cycles)at 3 C with a low attenuation rate of 0.0196%per cycle.The design strategy of a twinborn nitride heterostructure thus provides a functionalized solution for advanced Li-S batteries.
基金supported by the National Key Research and Development Program of China (Grant No. 2021YFB3201800)Natural Science Foundation of China (Grant Nos. U22A2019, 91964109, 52372123)+3 种基金State Key Laboratory for Mechanical Behavior of Materials (No. 20222405)Innovation Capability Support Program of Shaanxi (Grant No. 2021TD-12)National 111 Project of China (B14040)support from the Instrumental Analysis Center of Xi’an Jiaotong University
文摘Manipulating strain mode and degree that can be applied to epitaxial complex oxide thin films have been a cornerstone of strain engineering.In recent years,lift-off and transfer technology of the epitaxial oxide thin films have been developed that enabled the integration of heterostructures without the limitation of material types and crystal orientations.Moreover,twisted integration would provide a more interesting strategy in artificial magnetoelectric heterostructures.A specific twist angle between the ferroelectric and ferromagnetic oxide layers corresponds to the distinct strain regulation modes in the magnetoelectric coupling process,which could provide some insight in to the physical phenomena.In this work,the La_(0.67)Sr_(0.33)MnO_(3)(001)/0.7Pb(Mg_(1/3)Nb_(2/3))O_(3)-0.3PbTiO_(3)(011)(LSMO/PMN-PT)heterostructures with 45.and 0.twist angles were assembled via water-etching and transfer process.The transferred LSMO films exhibit a fourfold magnetic anisotropy with easy axis along LSMO<110>.A coexistence of uniaxial and fourfold magnetic anisotropy with LSMO[110]easy axis is observed for the 45°Sample by applying a 7.2 kV cm^(−1)electrical field,significantly different from a uniaxial anisotropy with LSMO[100]easy axis for the 0°Sample.The fitting of the ferromagnetic resonance field reveals that the strain coupling generated by the 45°twist angle causes different lattice distortion of LSMO,thereby enhancing both the fourfold and uniaxial anisotropy.This work confirms the twisting degrees of freedom for magnetoelectric coupling and opens opportunities for fabricating artificial magnetoelectric heterostructures.
基金the financial support from the Key Research and Development Program sponsored by the Ministry of Science and Technology(MOST)(2022YFB4002000,2022YFA1203400)the National Natural Science Foundation of China(22102172,22072145,22372155,22005294,21925205,21721003)。
文摘Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.
基金Project supported by the National Natural Science Foundation of China(Grant No.52173283)Taishan Scholar Program of Shandong Province(Grant No.ts20190939)Independent Cultivation Program of Innovation Team of Jinan City(Grant No.2021GXRC043).
文摘Recently,significant experimental advancements in achieving topological phases have been reported in van der Waals(vdW)heterostructures involving graphene.Here,using first-principles calculations,we investigate graphene/CoBr_(2)(Gr/CoBr_(2))heterostructures and find that an enhancement of in-plane magnetic anisotropy(IMA)energy in monolayer CoBr_(2) can be accomplished by reducing the interlayer distance of the vdW heterostructures.In addition,we clarify that the enhancement of IMA energy primarily results from two factors:one is the weakness of the Co-d_(xy) and Co-d_(x^(2)-y^(2)) orbital hybridization and the other is the augmentation of the Co-d_(yz) and Co-d_(z)2 orbital hybridization.Meanwhile,calculation results suggest that the Kosterlitz–Thouless phase transition temperature(TKT)of a 2D XY magnet Gr/CoBr_(2)(23.8 K)is higher than that of a 2D XY monolayer CoBr_(2)(1.35 K).By decreasing the interlayer distances,the proximity effect is more pronounced and band splitting appears.Moreover,by taking into account spin–orbit coupling,a band gap of approximately 14.3 meV and the quantum anomalous Hall effect(QAHE)are attained by decreasing the interlayer distance by 1.0 A.Inspired by the above conclusions,we design a topological field transistor device model.Our results support that the vdW interlayer distance can be used to modulate the IMA energy and QAHE of materials,providing a pathway for the development of new low-power spintronic devices.
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-luminescence(PL)quantum yield of monolayer(1L)TMDs is still quite low at room temperature,which severely lim-its their practical applications.Here we report a PL enhancement effect of 1L WS_(2) at room temperature when con-structing it into 1L-WS_(2)/hBN/1L-MoS_(2) vertical HSs.The PL enhancement factors(EFs)can be up to 4.2.By using transient absorption(TA)spectroscopy,we demonstrate that the PL enhancement effect is due to energy transfer from 1L MoS_(2) to 1L WS_(2).The energy transfer process occurs on a picosecond timescale and lasts more than one hundred picoseconds which indicates a prominent contribution from exciton-exciton annihilation.Furthermore,the PL en-hancement effect of 1L WS_(2) can be observed in 2L-MoS_(2)/hBN/1L-WS_(2) and 3L-MoS_(2)/hBN/1L-WS_(2) HSs.Our study provides a comprehensive understanding of the energy transfer process in the PL enhancement of 2D TMDs and a fea-sible way to optimize the performance of TMD-based optoelectronic devices.
基金Project supported by the National Key Research and Development Program of China(Grant No.2021YFA0718701)the China Postdoctoral Science Foundation(Grant No.2022M722888)the National Natural Science Foundation of China(Grant Nos.12174347 and 12004340).
文摘For the past few years,germanium-based semiconductor spintronics has attracted considerable interest due to its potential for integration into mainstream semiconductor technology.The main challenges in the development of modern semiconductor spintronics are the generation,detection,and manipulation of spin currents.Here,the transport characteristics of a spin current generated by spin pumping through a GeBi semiconductor barrier in Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures were investigated systematically.The effective spin-mixing conductance and inverse spin Hall voltage to quantitatively describe the spin transport characteristics were extracted.The spin-injection efficiency in the Y_(3)Fe_(5)O_(12)/GeBi/Pt heterostructures is comparable to that of the Y_(3)Fe_(5)O_(12)/Pt bilayer,and the inverse spin Hall voltage exponential decays with the increase in the barrier thickness.Furthermore,the band gap of the GeBi layer was tuned by changing the Bi content.The spin-injection efficiency at the YIG/semiconductor interface and the spin transportation within the semiconductor barrier are related to the band gap of the GeBi layer.Our results may be used as guidelines for the fabrication of efficient spin transmission structures and may lead to further studies on the impacts of different kinds of barrier materials.
基金financially supported by the National Natural Science Foundation of China (No.52106259)the Fundamental Research Funds for the Central Universities (2024MS013)Key Research and Development Program of Shaanxi (Program No.2022LL-JB-08)。
文摘Green hydrogen is urgently required for sustainable development of human beings and rational construction of heterostructures holds great promising for photocatalytic hydrogen generation.Herein,2D/2D WSe_(2)/ZnIn_(2)S_(4) heterostructures with strong hetero-interface interaction and abundant contact were constructed via an impregnation-annealing strategy.Efficient charge transfer from ZnIn_(2)S_(4) to WSe_(2)was evidenced by transient absorption spectroscopy in crafted heterostructures owing to the tight and2D face-to-face contact.As a result,the prepared WSe_(2)/ZnIn_(2)S_(4) heterostructures exhibited boosted photocatalytic performance and a highest hydrogen evolution rate of 3.377 mmol/(g h)was achieved with an apparent quantum yield of 45.7%at 420 nm.The work not only provides new strategies to achieve efficient 2D/2D heterostructures but also paves the way for the development of green hydrogen in the future.
