It is an important and challenging task to develop new infrared(IR)birefringent materials to promote the development of laser technology.In this work,a novel thioantimonate with the highest Cu-to-Sb ratio in the quate...It is an important and challenging task to develop new infrared(IR)birefringent materials to promote the development of laser technology.In this work,a novel thioantimonate with the highest Cu-to-Sb ratio in the quaternary X/Cu/Sb/Q(X=cations;Q=chalcogen)system,namely CsCu_(3)SbS_(4),was structurally designed and prepared by the strategy of alkali metal introduction into known Cu_(3)SbS_(4).Interestingly,CsCu_(3)SbS_(4)has novel two-dimensional anionic[Cu_(3)SbS_(4)]^(−)layers formed by the unprecedented onedimensional[Cu_(3)S_(3)S_(3/2)]^(6−)chains and discrete[SbS_(3)]_(3)−clusters.Meanwhile,compared with the prototype Cu_(3)SbS_(4),CsCu_(3)SbS_(4)realizes an enormous birefringence boost from 0 to 0.232,which was confirmed by both experimental results and theoretical calculations.This study enriches the sources of thioantimonates and sheds more light on the structure–property relationships of IR birefringent materials.展开更多
Two-dimensional layered materials(2DLMs)have attracted growing attention in optoelectronic devices due to their intriguing anisotropic physical properties.Different members of 2DLMs exhibit unique anisotropic electric...Two-dimensional layered materials(2DLMs)have attracted growing attention in optoelectronic devices due to their intriguing anisotropic physical properties.Different members of 2DLMs exhibit unique anisotropic electrical,optical,and thermal properties,fundamentally related to their crystal structure.Among them,directional heat transfer plays a vital role in the thermal management of electronic devices.Here,we use density functional theory calculations to investigate the thermal transport properties of representative layered materials:β-InSe,γ-InSe,MoS2,and h-BN.We found that the lattice thermal conductivities ofβ-InSe,γ-InSe,MoS_(2),and h-BN display diverse anisotropic behaviors with anisotropy ratios of 10.4,9.4,64.9,and 107.7,respectively.The analysis of the phonon modes further indicates that the phonon group velocity is responsible for the anisotropy of thermal transport.Furthermore,the low lattice thermal conductivity of the layered InSe mainly comes from low phonon group velocity and atomic masses.Our findings provide a fundamental physical understanding of the anisotropic thermal transport in layered materials.We hope this study could inspire the advancement of 2DLMs thermal management applications in next-generation integrated electronic and optoelectronic devices.展开更多
The past decade has witnessed a dramatic increase in interest in emerging photodetectors built from two-dimensional(2D)layered materials.A major driver of this trend is the growing demands for lightweight,uncooled,and...The past decade has witnessed a dramatic increase in interest in emerging photodetectors built from two-dimensional(2D)layered materials.A major driver of this trend is the growing demands for lightweight,uncooled,and even flexible photodetection technology.However,2D layered materials always suffer from low light absorption coefficients due to their atomically thin nature.Impact ionization,which can achieve carrier multiplication,is a promising strategy to design 2D photodetectors with high detection efficiency.In this review,typical types of photodetection mechanisms in 2D photodetectors are first summarized.We then discuss the avalanche mechanism induced by impact ionization and avalanche photodetectors based on conventional silicon and III–V compound semiconductors.Finally,a host of emerging avalanche photodetectors based on 2D materials and their van der Waals heterostructures,and their potential applications in the field of photon-counting technologies are detailed.By reviewing the recent progress and discussing challenges faced by 2D avalanche photodetectors,this review aims to provide perspectives on future research directions of 2D material-based ultrasensitive photodetectors such as single-photon detectors.展开更多
Two-dimensional(2D)multilayer kagome materials hold significant research value for regulating kagome-related physical properties and exploring quantum effects.However,their development is hindered by the scarcity of a...Two-dimensional(2D)multilayer kagome materials hold significant research value for regulating kagome-related physical properties and exploring quantum effects.However,their development is hindered by the scarcity of available material systems,making the identification of novel 2D multilayer kagome candidates particularly important.In this work,three types of 2D materials with trilayer kagome lattices,namely Sc_(6)S_(5)X_(6)(X=Cl,Br,I),are predicted based on first-principles calculations.These 2D materials feature two kagome lattices composed of Sc atoms and one kagome lattice composed of S atoms.Stability analysis indicates that these materials can exist as free-standing 2D materials.Electronic structure calculations reveal that Sc_(6)S_(5)X_(6)are narrow-bandgap semiconductors(0.76–0.95 e V),with their band structures exhibiting flat bands contributed by Sc-based kagome lattices and Dirac band gaps resulting from symmetry breaking.The sulfur-based kagome lattice in the central layer contributes an independent flat band below the Fermi level.Additionally,Sc_(6)S_(5)X_(6)exhibit high carrier mobility,with hole and electron mobilities reaching up to 10^(3)cm^(2)·V^(-1)·s^(-1),indicating potential applications in low-dimensional electronic devices.This work provides an excellent example for the development of novel multilayer 2D kagome materials.展开更多
In the present study,the effect of material microstructure on the mechanical response of a two-dimensional elastic layer perfectly bonded to a substrate is examined under surface loadings.In the current model,the subs...In the present study,the effect of material microstructure on the mechanical response of a two-dimensional elastic layer perfectly bonded to a substrate is examined under surface loadings.In the current model,the substrate is treated as an elastic half plane as opposed to a rigid base,and this enables its applications in practical cases when the modulus of the layer(e.g.,the coating material)and substrate(e.g.,the coated surface)are comparable.The material microstructure is modeled using the generalized continuum theory of couple stress elasticity.The boundary value problems are formulated in terms of the displacement field and solved in an analytical manner via the Fourier transform and stiffness matrix method.The results demonstrate the capability of the present continuum theory to efficiently model the size-dependency of the response of the material when the external and internal length scales are comparable.Furthermore,the results indicated that the material mismatch and substrate stiffness play a crucial role in the predicted elastic field.Specifically,the study also addresses significant discrepancy of the response for the case of a layer resting on a rigid substrate.展开更多
With the development of Moore's law, the future trend of devices will inevitably be shrinking and integration to further achieve size reduction. The emergence of new two-dimensional non-layered materials(2DNLMs) n...With the development of Moore's law, the future trend of devices will inevitably be shrinking and integration to further achieve size reduction. The emergence of new two-dimensional non-layered materials(2DNLMs) not only enriches the 2D material family to meet future development, but also stimulates the global enthusiasm for basic research and application technologies in the 2D field. Van der Waals(vd W) heterostructures, in which two-dimensional layered materials(2DLMs)are physically stacked layer by layer, can also occur between 2DLMs and 2DNLMs hybrid heterostructures, providing an alternative platform for nanoelectronics and optoelectronic applications. Here, we outline the recent developments of2DLMs/2DNLMs hybrid heterostructures, with particular emphasis on major advances in synthetic methods and applications. And the categories and crystal structures of 2DLMs and 2DNLMs are also shown. We highlight some promising applications of the heterostructures in electronics, optoelectronics, and catalysis. Finally, we provide conclusions and future prospects in the 2D materials field.展开更多
The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an over...The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an overwhelming tendency,providing powerful tools for remote health monitoring and personal health management.Among many candidates,two-dimensional(2D)materials stand out due to several exotic mechanical,electrical,optical,and chemical properties that can be efficiently integrated into atomic-thin films.While previous reviews on 2D materials for biodevices primarily focus on conventional configurations and materials like graphene,the rapid development of new 2D materials with exotic properties has opened up novel applications,particularly in smart interaction and integrated functionalities.This review aims to consolidate recent progress,highlight the unique advantages of 2D materials,and guide future research by discussing existing challenges and opportunities in applying 2D materials for smart wearable biodevices.We begin with an in-depth analysis of the advantages,sensing mechanisms,and potential applications of 2D materials in wearable biodevice fabrication.Following this,we systematically discuss state-of-the-art biodevices based on 2D materials for monitoring various physiological signals within the human body.Special attention is given to showcasing the integration of multi-functionality in 2D smart devices,mainly including self-power supply,integrated diagnosis/treatment,and human–machine interaction.Finally,the review concludes with a concise summary of existing challenges and prospective solutions concerning the utilization of2D materials for advanced biodevices.展开更多
Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemist...Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.展开更多
Environmental catalysis has been considered one of the important research topics.Some technologies(e.g.,photocatalysis and electrocatalysis)have been intensively developed with the advance of synthetic technologies of...Environmental catalysis has been considered one of the important research topics.Some technologies(e.g.,photocatalysis and electrocatalysis)have been intensively developed with the advance of synthetic technologies of catalytical materials.In 2019,we discussed the development trend of this field,and wrote a roadmap on this topic in Chinese Chemical Letters(30(2019)2065-2088).Nowadays,we discuss it again from a new viewpoint along this road.In this paper,several subtopics are discussed,e.g.,photocatalysis based on titanium dioxide,violet phosphorus,graphitic carbon and covalent organic frameworks,electrocatalysts based on carbon,metal-and covalent-organic framework.Finally,we hope that this roadmap can enrich the development of two-dimensional materials in environmental catalysis with novel understanding,and give useful inspiration to explore new catalysts for practical applications.展开更多
Layered materials,such as graphite and molybdenum disulfide,are promising for electrode materials and microelectronic devices due to their excellent ion-intercalating properties.However,the intercalation and de-interc...Layered materials,such as graphite and molybdenum disulfide,are promising for electrode materials and microelectronic devices due to their excellent ion-intercalating properties.However,the intercalation and de-intercalation of ions,causing structural deformation and material property variations,would affect battery performance and alter external field responses.The complex problem coupling multiphysics is significant for study and poses a crucial research challenge.This paper reviews the coupling between mechanics,electrochemistry,and electrics during the reaction process,including in situ experimental characterization,theoretical modeling,and design considerations at various scales.Current research has focused on experimental observations beyond the nanoscale and continuum phenomenological models.Further advancements in characterizing layered structural evolution,electron cloud interactions at the atomic level,and developing physics-based multi-field models are essential.展开更多
We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-o...We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.展开更多
In recent years,as the dimensions of the conventional semiconductor technology is approaching the physical limits,while the multifunction circuits are restricted by the relatively fixed characteristics of the traditio...In recent years,as the dimensions of the conventional semiconductor technology is approaching the physical limits,while the multifunction circuits are restricted by the relatively fixed characteristics of the traditional metal−oxide−semiconductor field-effect transistors,reconfigurable devices that can realize reconfigurable characteristics and multiple functions at device level have been seen as a promising method to improve integration density and reduce power consumption.Owing to the ultrathin structure,effective control of the electronic characteristics and ability to modulate structural defects,two-dimensional(2D)materials have been widely used to fabricate reconfigurable devices.In this review,we summarize the working principles and related logic applications of reconfigurable devices based on 2D materials,including generating tunable anti-ambipolar responses and demonstrating nonvolatile operations.Furthermore,we discuss the analog signal processing applications of anti-ambipolar transistors and the artificial intelligence hardware implementations based on reconfigurable transistors and memristors,respectively,therefore highlighting the outstanding advantages of reconfigurable devices in footprint,energy consumption and performance.Finally,we discuss the challenges of the 2D materials-based reconfigurable devices.展开更多
Moiré superlattices have revolutionized the study of two-dimensional materials, enabling unprecedented control over their electronic, magnetic, optical, and mechanical properties. This review provides a comprehen...Moiré superlattices have revolutionized the study of two-dimensional materials, enabling unprecedented control over their electronic, magnetic, optical, and mechanical properties. This review provides a comprehensive analysis of the latest advancements in moiré physics, focusing on the formation of moiré superlattices due to rotational misalignment or lattice mismatch in two-dimensional materials. These superlattices induce flat band structures and strong correlation effects,leading to the emergence of exotic quantum phases, such as unconventional superconductivity, correlated insulating states,and fractional quantum anomalous Hall effects. The review also explores the underlying mechanisms of these phenomena and discusses the potential technological applications of moiré physics, offering insights into future research directions in this rapidly evolving field.展开更多
In the field of lithium-ion battery cathode materials, lithium-rich layered oxide materials have garnered significant attention due to their exceptional discharge specific capacity and high operating voltage. However,...In the field of lithium-ion battery cathode materials, lithium-rich layered oxide materials have garnered significant attention due to their exceptional discharge specific capacity and high operating voltage. However, their limitations in terms of cycling stability and rate capability remain major impediments to their wider application. In this study, an innovative approach was employed by simultaneously utilizing the acidic and oxidative properties of phosphomolybdic acid to generate a spinel structure and in-situ coating of a conductive polymer(polypyrrole) on the surface of lithium-rich layered oxide materials. This strategy aimed to mitigate structural degradation during charge-discharge cycles, enhance the ionic/electronic conductivity, and suppress side reactions. Experimental results demonstrated that after 200 cycles at a current density of 1 C, the modified sample exhibited a discharge specific capacity of 193.4 m Ah/g, with an improved capacity retention rate of 83.3% and a minimal voltage decay of only 0.27 V. These findings provide compelling support for the development and application of next-generation high-performance lithium-ion batteries.展开更多
Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient cat...Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.展开更多
Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a...Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a layered anti-perovskite structure,has attracted significant interest for its high capacity and facile synthesis.In this study,density functional theory calculations were performed to systematically investigate the phase stability,ionic conductivity,and voltage characteristics of Na_(2)Fe_(2)OS_(2)as a model system for anti-perovskite layered cathode materials.The compound exhibits excellent phase stability,and its equilibrium potential was calculated for the series Na_(x)Fe_(2)OCh_(2)(0<±<2)(where Ch represents chalcogenides).Naion transport analysis using the climbing image nudged elastic band method reveals a relatively low migration barrier(~0.47eV)along a dingonal pathway,indicating efficient Na^(+)mobility.To expand the materials design space,we systematically explored the effects of substituting Fe with various transition metals and replacing S with Se in NaaTM_(2)OCh_(2)structures.Among the variants studied,Na_(2)Mn_(2)OS_(2) demonstrates the most favorable combination of high voltage(~2.51V),robust phase stability,and superior energy density(~427 W-h/kg).This comprehensive comparison of transition metal substitutions provides vnluable insights for the rational design and experimental development of next-generation anti-perovskite layered cathode materials for sodium-ion batteries.展开更多
Recent studies in van der Waals coupled two-dimensional(2D) bilayer materials have demonstrated a new freedom for material engineering by the formation of moiré pattern. By tuning the twist angle between two laye...Recent studies in van der Waals coupled two-dimensional(2D) bilayer materials have demonstrated a new freedom for material engineering by the formation of moiré pattern. By tuning the twist angle between two layers, one can modulate their electronic band structures and therefore the associated electrical transport and optical properties, which are distinct from the original ones of each individual layer. These new properties excite great passion in the exploration of new quantum states and possible applications of 2D bilayers. In this article, we will mainly review the prevailing fabrication methods and emerging physical properties of twisted bilayer materials and lastly give out a perspective of this topic.展开更多
The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-princip...The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-principles calculations,we investigate both electronic structures and magnetic orderings of bulk and monolayer of chromium diiodides(CrI2).We demonstrate a counter-intuitive fact that the ground state of the free-standing monolayer of CrI2 is antiferromagnetic though the bulk possesses macroscopic ferromagnetic ordering.The interlayer interaction remains antiferromagnetic up to few-layer scenarios.The unique feature of CrI2 makes it an ideal workbench to investigate the relation between magnetic couplings and interlayer van der Waals interactions,and may offer an opportunity to 2D antiferromagnetic spintronic devices.展开更多
Nowadays,lithium-ion batteries(LIBs)play a crucial role in modern society in the aspect of portable electronic devices and large-scale smart grids.However,the current performance of lithium-ion batteries has been unab...Nowadays,lithium-ion batteries(LIBs)play a crucial role in modern society in the aspect of portable electronic devices and large-scale smart grids.However,the current performance of lithium-ion batteries has been unable to meet the growing expectations of society and scientific community.Herein,we have synthetically investigated availability of 2D Ni-TABQ monolayer as anode based on DFT for LIBs applications.Our findings have demonstrated that 2D Ni-TABQ monolayer is a semiconductor with a small band gap of 0.2 eV,which suggest that the electronic property of 2D Ni-TABQ monolayer would take place an evident shift from semiconductor property to metallic property after Li adsorption.Furthermore,we checked the stability of 2D Ni-TABQ monolayer and investigated the viability of exfoliation from bulk multilayer Ni-TABQ to form 2D Ni-TABQ monolayer in the light of exfoliation energy and binding energy.We continuously studied electrochemical properties of 2D Ni-TABQ monolayer with respect of theoretical specific capacity,Li-ion diffusion barriers and open-circuit voltage.During the charging process,2D Ni-TABQ monolayer can achieve a high specific capacity of 722 m Ah/g with an open-circuit voltage range from 1.12 V to 0.22 V.These aforementioned results make the 2D Ni-TABQ monolayer a promising anode for LIBs.展开更多
The fascinating Dirac cone in honeycomb graphene,which underlies many unique electronic properties,has inspired the vast endeavors on pursuing new two-dimensional(2D)Dirac materials.Based on the density functional the...The fascinating Dirac cone in honeycomb graphene,which underlies many unique electronic properties,has inspired the vast endeavors on pursuing new two-dimensional(2D)Dirac materials.Based on the density functional theory method,a 2D material Zn3Si2 of honeycomb transition-metal silicide with intrinsic Dirac cones has been predicted.The Zn3Si2 monolayer is dynamically and thermodynamically stable under ambient conditions.Importantly,the Zn3Si2 monolayer is a room-temperature 2D Dirac material with a spin-orbit coupling energy gap of 1.2 meV,which has an intrinsic Dirac cone arising from the special hexagonal lattice structure.Hole doping leads to the spin polarization of the electron,which results in a Dirac half-metal feature with single-spin Dirac fermion.This novel stable 2D transition-metal-silicon-framework material holds promises for electronic device applications in spintronics.展开更多
基金supported by the National Natural Science Foundation of China(No.52171277,51778570,51879230,21771179,and 22175175)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZR118)+2 种基金the Natural Science Foundation of Fujian Province(2019J01133)the Natural Science Basic Research Program of Shaanxi(2020JQ-710)the Doctoral Scientific Research Startup Foundation of Shaanxi University of Science and Technology(2018BJ-07).
文摘It is an important and challenging task to develop new infrared(IR)birefringent materials to promote the development of laser technology.In this work,a novel thioantimonate with the highest Cu-to-Sb ratio in the quaternary X/Cu/Sb/Q(X=cations;Q=chalcogen)system,namely CsCu_(3)SbS_(4),was structurally designed and prepared by the strategy of alkali metal introduction into known Cu_(3)SbS_(4).Interestingly,CsCu_(3)SbS_(4)has novel two-dimensional anionic[Cu_(3)SbS_(4)]^(−)layers formed by the unprecedented onedimensional[Cu_(3)S_(3)S_(3/2)]^(6−)chains and discrete[SbS_(3)]_(3)−clusters.Meanwhile,compared with the prototype Cu_(3)SbS_(4),CsCu_(3)SbS_(4)realizes an enormous birefringence boost from 0 to 0.232,which was confirmed by both experimental results and theoretical calculations.This study enriches the sources of thioantimonates and sheds more light on the structure–property relationships of IR birefringent materials.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFA1402502)the National Natural Science Foundation of China(Grant Nos.12004131,22090044,and 62125402)Calculations were performed in part at the high-performance computing center of Jilin University.
文摘Two-dimensional layered materials(2DLMs)have attracted growing attention in optoelectronic devices due to their intriguing anisotropic physical properties.Different members of 2DLMs exhibit unique anisotropic electrical,optical,and thermal properties,fundamentally related to their crystal structure.Among them,directional heat transfer plays a vital role in the thermal management of electronic devices.Here,we use density functional theory calculations to investigate the thermal transport properties of representative layered materials:β-InSe,γ-InSe,MoS2,and h-BN.We found that the lattice thermal conductivities ofβ-InSe,γ-InSe,MoS_(2),and h-BN display diverse anisotropic behaviors with anisotropy ratios of 10.4,9.4,64.9,and 107.7,respectively.The analysis of the phonon modes further indicates that the phonon group velocity is responsible for the anisotropy of thermal transport.Furthermore,the low lattice thermal conductivity of the layered InSe mainly comes from low phonon group velocity and atomic masses.Our findings provide a fundamental physical understanding of the anisotropic thermal transport in layered materials.We hope this study could inspire the advancement of 2DLMs thermal management applications in next-generation integrated electronic and optoelectronic devices.
文摘The past decade has witnessed a dramatic increase in interest in emerging photodetectors built from two-dimensional(2D)layered materials.A major driver of this trend is the growing demands for lightweight,uncooled,and even flexible photodetection technology.However,2D layered materials always suffer from low light absorption coefficients due to their atomically thin nature.Impact ionization,which can achieve carrier multiplication,is a promising strategy to design 2D photodetectors with high detection efficiency.In this review,typical types of photodetection mechanisms in 2D photodetectors are first summarized.We then discuss the avalanche mechanism induced by impact ionization and avalanche photodetectors based on conventional silicon and III–V compound semiconductors.Finally,a host of emerging avalanche photodetectors based on 2D materials and their van der Waals heterostructures,and their potential applications in the field of photon-counting technologies are detailed.By reviewing the recent progress and discussing challenges faced by 2D avalanche photodetectors,this review aims to provide perspectives on future research directions of 2D material-based ultrasensitive photodetectors such as single-photon detectors.
基金supported by the Fundamental Research Funds for the Central Universities(WUT:2024IVA052 and Grant No.104972025KFYjc0089)。
文摘Two-dimensional(2D)multilayer kagome materials hold significant research value for regulating kagome-related physical properties and exploring quantum effects.However,their development is hindered by the scarcity of available material systems,making the identification of novel 2D multilayer kagome candidates particularly important.In this work,three types of 2D materials with trilayer kagome lattices,namely Sc_(6)S_(5)X_(6)(X=Cl,Br,I),are predicted based on first-principles calculations.These 2D materials feature two kagome lattices composed of Sc atoms and one kagome lattice composed of S atoms.Stability analysis indicates that these materials can exist as free-standing 2D materials.Electronic structure calculations reveal that Sc_(6)S_(5)X_(6)are narrow-bandgap semiconductors(0.76–0.95 e V),with their band structures exhibiting flat bands contributed by Sc-based kagome lattices and Dirac band gaps resulting from symmetry breaking.The sulfur-based kagome lattice in the central layer contributes an independent flat band below the Fermi level.Additionally,Sc_(6)S_(5)X_(6)exhibit high carrier mobility,with hole and electron mobilities reaching up to 10^(3)cm^(2)·V^(-1)·s^(-1),indicating potential applications in low-dimensional electronic devices.This work provides an excellent example for the development of novel multilayer 2D kagome materials.
基金The authors gratefully acknowledge support provided by the Thailand Research Fund(Grant No.RTA6280012)Furthermore,the first author gratefully acknowledges the financial support from the Graduate School and Faculty of Engineering,Chulalongkorn University,during her visit at Durham University.
文摘In the present study,the effect of material microstructure on the mechanical response of a two-dimensional elastic layer perfectly bonded to a substrate is examined under surface loadings.In the current model,the substrate is treated as an elastic half plane as opposed to a rigid base,and this enables its applications in practical cases when the modulus of the layer(e.g.,the coating material)and substrate(e.g.,the coated surface)are comparable.The material microstructure is modeled using the generalized continuum theory of couple stress elasticity.The boundary value problems are formulated in terms of the displacement field and solved in an analytical manner via the Fourier transform and stiffness matrix method.The results demonstrate the capability of the present continuum theory to efficiently model the size-dependency of the response of the material when the external and internal length scales are comparable.Furthermore,the results indicated that the material mismatch and substrate stiffness play a crucial role in the predicted elastic field.Specifically,the study also addresses significant discrepancy of the response for the case of a layer resting on a rigid substrate.
基金Project supported by the National Natural Science Fundation of China (Grant Nos. 61731019, 60908012, 61575008, and 61775007)the Beijing Natural Science Foundation (Grant Nos. 4182015 and 4202010)。
文摘With the development of Moore's law, the future trend of devices will inevitably be shrinking and integration to further achieve size reduction. The emergence of new two-dimensional non-layered materials(2DNLMs) not only enriches the 2D material family to meet future development, but also stimulates the global enthusiasm for basic research and application technologies in the 2D field. Van der Waals(vd W) heterostructures, in which two-dimensional layered materials(2DLMs)are physically stacked layer by layer, can also occur between 2DLMs and 2DNLMs hybrid heterostructures, providing an alternative platform for nanoelectronics and optoelectronic applications. Here, we outline the recent developments of2DLMs/2DNLMs hybrid heterostructures, with particular emphasis on major advances in synthetic methods and applications. And the categories and crystal structures of 2DLMs and 2DNLMs are also shown. We highlight some promising applications of the heterostructures in electronics, optoelectronics, and catalysis. Finally, we provide conclusions and future prospects in the 2D materials field.
基金the support from the National Natural Science Foundation of China(22272004,62272041)the Fundamental Research Funds for the Central Universities(YWF-22-L-1256)+1 种基金the National Key R&D Program of China(2023YFC3402600)the Beijing Institute of Technology Research Fund Program for Young Scholars(No.1870011182126)。
文摘The proliferation of wearable biodevices has boosted the development of soft,innovative,and multifunctional materials for human health monitoring.The integration of wearable sensors with intelligent systems is an overwhelming tendency,providing powerful tools for remote health monitoring and personal health management.Among many candidates,two-dimensional(2D)materials stand out due to several exotic mechanical,electrical,optical,and chemical properties that can be efficiently integrated into atomic-thin films.While previous reviews on 2D materials for biodevices primarily focus on conventional configurations and materials like graphene,the rapid development of new 2D materials with exotic properties has opened up novel applications,particularly in smart interaction and integrated functionalities.This review aims to consolidate recent progress,highlight the unique advantages of 2D materials,and guide future research by discussing existing challenges and opportunities in applying 2D materials for smart wearable biodevices.We begin with an in-depth analysis of the advantages,sensing mechanisms,and potential applications of 2D materials in wearable biodevice fabrication.Following this,we systematically discuss state-of-the-art biodevices based on 2D materials for monitoring various physiological signals within the human body.Special attention is given to showcasing the integration of multi-functionality in 2D smart devices,mainly including self-power supply,integrated diagnosis/treatment,and human–machine interaction.Finally,the review concludes with a concise summary of existing challenges and prospective solutions concerning the utilization of2D materials for advanced biodevices.
基金financial support from the Natural Science Foundation of Shandong Province of China(ZR2023ME051,ZR2019MEM020)。
文摘Facilitating anion redox chemistry is an effective strategy to increase the capacity of layered oxides for sodium-ion batteries.Nevertheless,there remains a paucity of literature pertaining to the oxygen redox chemistry of O3-type layered oxide cathode materials.This work systematically investigates the effect of Fe doping on the anionic oxygen redox chemistry and electrochemical reactions in O3-NaNi_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1)O_(2).The results of the density functional theory(DFT)calculations indicate that the electrons of the O 2p occupy a higher energy level.In the ex-situ X-ray photoelectron spectrometer(XPS)of O 1s,the addition of Fe facilitates the lattice oxygen(O^(n-))to exhibit enhanced activity at 4.45 V.The in-situ X-ray diffraction(XRD)demonstrates that the doping of Fe effectively suppresses the Y phase transition at high voltages.Furthermore,the Galvanostatic Intermittent Titration Technique(GITT)data indicate that Fe doping significantly increases the Na~+migration rate at high voltages.Consequently,the substitution of Fe can elevate the cut-off voltage to 4.45 V,thereby facilitating electron migration from O^(2-).The redox of O^(2-)/O^(n-)(n<2)contributes to the overall capacity.O3-Na(Ni_(0.4)Cu_(0.1)Mn_(0.4)Ti_(0.1))_(0.92)Fe_(0.08)O_(2)provides an initial discharge specific capacity of 180.55 mA h g^(-1)and71.6%capacity retention at 0.5 C(1 C=240 mA g^(-1)).This work not only demonstrates the beneficial impact of Fe substitution for promoting the redox activity and reversibility of O^(2-)in 03-type layered oxides,but also guarantees the structural integrity of the cathode materials at high voltages(>4.2 V).It offers a novel avenue for investigating the anionic redox reaction in O3-type layered oxides to design advanced cathode materials.
基金supported by the National Natural Science Foundation of China(Nos.52272290,21972030,52073119,and 52373210)the Natural Science Foundation of Jilin Province(No.20230101029JC)+1 种基金the Fundamental Research Program of Shanxi Province(No.202303021212159)the Monash University Malaysia–ASEAN grant(No.ASE-000010)。
文摘Environmental catalysis has been considered one of the important research topics.Some technologies(e.g.,photocatalysis and electrocatalysis)have been intensively developed with the advance of synthetic technologies of catalytical materials.In 2019,we discussed the development trend of this field,and wrote a roadmap on this topic in Chinese Chemical Letters(30(2019)2065-2088).Nowadays,we discuss it again from a new viewpoint along this road.In this paper,several subtopics are discussed,e.g.,photocatalysis based on titanium dioxide,violet phosphorus,graphitic carbon and covalent organic frameworks,electrocatalysts based on carbon,metal-and covalent-organic framework.Finally,we hope that this roadmap can enrich the development of two-dimensional materials in environmental catalysis with novel understanding,and give useful inspiration to explore new catalysts for practical applications.
基金supported by the National Key R&D Program of China(Grant No.2023YFB2408000).
文摘Layered materials,such as graphite and molybdenum disulfide,are promising for electrode materials and microelectronic devices due to their excellent ion-intercalating properties.However,the intercalation and de-intercalation of ions,causing structural deformation and material property variations,would affect battery performance and alter external field responses.The complex problem coupling multiphysics is significant for study and poses a crucial research challenge.This paper reviews the coupling between mechanics,electrochemistry,and electrics during the reaction process,including in situ experimental characterization,theoretical modeling,and design considerations at various scales.Current research has focused on experimental observations beyond the nanoscale and continuum phenomenological models.Further advancements in characterizing layered structural evolution,electron cloud interactions at the atomic level,and developing physics-based multi-field models are essential.
基金financially supported by National Natural Science Foundation of China(No.22275149)Fundamental Research Funds for the Central Universities(No.SWU118105)the Next-Generation Advanced Energy Materials Program of BatteroTech Co.,Ltd.
文摘We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.
基金support from the National Key Research and Development Program of China(Grant nos.2024YFA1409700 and 2023YFA1407000)the National Natural Science Foundation of China(Grant no.62374158).
文摘In recent years,as the dimensions of the conventional semiconductor technology is approaching the physical limits,while the multifunction circuits are restricted by the relatively fixed characteristics of the traditional metal−oxide−semiconductor field-effect transistors,reconfigurable devices that can realize reconfigurable characteristics and multiple functions at device level have been seen as a promising method to improve integration density and reduce power consumption.Owing to the ultrathin structure,effective control of the electronic characteristics and ability to modulate structural defects,two-dimensional(2D)materials have been widely used to fabricate reconfigurable devices.In this review,we summarize the working principles and related logic applications of reconfigurable devices based on 2D materials,including generating tunable anti-ambipolar responses and demonstrating nonvolatile operations.Furthermore,we discuss the analog signal processing applications of anti-ambipolar transistors and the artificial intelligence hardware implementations based on reconfigurable transistors and memristors,respectively,therefore highlighting the outstanding advantages of reconfigurable devices in footprint,energy consumption and performance.Finally,we discuss the challenges of the 2D materials-based reconfigurable devices.
基金Project supported by the National Key R&D Program of China (Grant No. 2019YFA0307800)the National Natural Science Foundation of China (Grant No. 12074377)+2 种基金Fundamental Research Funds for the Central Universities,the International Partnership Program of Chinese Academy of Sciences (Grant No. 211211KYSB20210007)the China Postdoctoral Science Foundation (Grant No. 2024M753465)the Postdoctoral Fellowship Program (Grade C) of China Postdoctoral Science Foundation (Grant No. GZC20241893)。
文摘Moiré superlattices have revolutionized the study of two-dimensional materials, enabling unprecedented control over their electronic, magnetic, optical, and mechanical properties. This review provides a comprehensive analysis of the latest advancements in moiré physics, focusing on the formation of moiré superlattices due to rotational misalignment or lattice mismatch in two-dimensional materials. These superlattices induce flat band structures and strong correlation effects,leading to the emergence of exotic quantum phases, such as unconventional superconductivity, correlated insulating states,and fractional quantum anomalous Hall effects. The review also explores the underlying mechanisms of these phenomena and discusses the potential technological applications of moiré physics, offering insights into future research directions in this rapidly evolving field.
基金supported partially by projects of National Natural Science Foundation of China (Nos. 52272200, 51972110, 52102245, 52102203 and 52072121)State Key Laboratory of Alternate Electrical Power System with Renewable Energy Sources (Nos. LAPS21004, LAPS202114)+5 种基金Beijing Natural Science Foundation (Nos. 2222076, 2222077)Hebei Natural Science Foundation (No. E2022502022)Huaneng Group Headquarters Science and Technology Project (No. HNKJ20-H88)2022 Strategic Research Key Project of Science and Technology Commission of the Ministry of Education, China Postdoctoral Science Foundation (No. 2022M721129)the Fundamental Research Funds for the Central Universities (Nos. 2022MS030, 2021MS028, 2020MS023, 2020MS028)the NCEPU "Double First-Class" Program。
文摘In the field of lithium-ion battery cathode materials, lithium-rich layered oxide materials have garnered significant attention due to their exceptional discharge specific capacity and high operating voltage. However, their limitations in terms of cycling stability and rate capability remain major impediments to their wider application. In this study, an innovative approach was employed by simultaneously utilizing the acidic and oxidative properties of phosphomolybdic acid to generate a spinel structure and in-situ coating of a conductive polymer(polypyrrole) on the surface of lithium-rich layered oxide materials. This strategy aimed to mitigate structural degradation during charge-discharge cycles, enhance the ionic/electronic conductivity, and suppress side reactions. Experimental results demonstrated that after 200 cycles at a current density of 1 C, the modified sample exhibited a discharge specific capacity of 193.4 m Ah/g, with an improved capacity retention rate of 83.3% and a minimal voltage decay of only 0.27 V. These findings provide compelling support for the development and application of next-generation high-performance lithium-ion batteries.
基金National Natural Science Foundation of China,Grant/Award Number:22179029Fundamental Research Funds for the Central Universities,Grant/Award Number:buctrc202324+2 种基金Young Elite Scientists Sponsorship Program by BAST,Grant/Award Number:BYESS2023093Ministero dell'Istruzione,dell'Universitàe della Ricerca,Grant/Award Number:2022FNL89YKempestiftelserna。
文摘Selective oxidation of amines to imines through electrocatalysis is an attractive and efficient way for the chemical industry to produce nitrile compounds,but it is limited by the difficulty of designing efficient catalysts and lack of understanding the mechanism of catalysis.Herein,we demonstrate a novel strategy by generation of oxyhydroxide layers on two-dimensional iron-doped layered nickel phosphorus trisulfides(Ni1-xFexPS_(3))during the oxidation of benzylamine(BA).In-depth structural and surface chemical characterizations during the electrocatalytic process combined with theoretical calculations reveal that Ni(1-x)FexPS_(3) undergoes surface reconstruction under alkaline conditions to form the metal oxyhydroxide/phosphorus trichalcogenide(NiFeOOH/Ni1-xFexPS_(3))heterostructure.Interestingly,the generated heterointerface facilitates BA oxidation with a low onset potential of 1.39 V and Faradaic efficiency of 53%for benzonitrile(BN)synthesis.Theoretical calculations further indicate that the as-formed NiFeOOH/Ni1-xFexPS_(3) heterostructure could offer optimum free energy for BA adsorption and BN desorption,resulting in promising BN synthesis.
基金supported by the National Natural Science Foundation of China(Grant Nos.12404264 and 22209067)Shenzhen Basic Research Program(Natural Science Foundation)Key Project of Basic Research(Grant No.JCYJ20241202123916023)Shenzhen Science and Technology Program(Grant No.KQTD20200820113047086)。
文摘Sodium-ion batteries have emerged as promising alternatives to lithium-ion batteries due to their abundant raw material reserves,low cost,enhanced safety,and environmental sustainability.Na_(2)Fe_(2)OS_(2),featuring a layered anti-perovskite structure,has attracted significant interest for its high capacity and facile synthesis.In this study,density functional theory calculations were performed to systematically investigate the phase stability,ionic conductivity,and voltage characteristics of Na_(2)Fe_(2)OS_(2)as a model system for anti-perovskite layered cathode materials.The compound exhibits excellent phase stability,and its equilibrium potential was calculated for the series Na_(x)Fe_(2)OCh_(2)(0<±<2)(where Ch represents chalcogenides).Naion transport analysis using the climbing image nudged elastic band method reveals a relatively low migration barrier(~0.47eV)along a dingonal pathway,indicating efficient Na^(+)mobility.To expand the materials design space,we systematically explored the effects of substituting Fe with various transition metals and replacing S with Se in NaaTM_(2)OCh_(2)structures.Among the variants studied,Na_(2)Mn_(2)OS_(2) demonstrates the most favorable combination of high voltage(~2.51V),robust phase stability,and superior energy density(~427 W-h/kg).This comprehensive comparison of transition metal substitutions provides vnluable insights for the rational design and experimental development of next-generation anti-perovskite layered cathode materials for sodium-ion batteries.
基金Project supported by the National Key R&D Program of China(Grant Nos.2016YFA0300903 and 2016YFA0300804)National Equipment Program of China(Grant No.ZDYZ2015-1)+3 种基金Beijing Graphene Innovation Program,China(Grant No.Z181100004818003)Beijing Municipal Science&Technology Commission,China(Grant No.Z181100004218006)Bureau of Industry and Information Technology of Shenzhen,China(Graphene platform contract No.201901161512)the Key R&D Program of Guangdong Province,China(Grant No.2019B010931001)
文摘Recent studies in van der Waals coupled two-dimensional(2D) bilayer materials have demonstrated a new freedom for material engineering by the formation of moiré pattern. By tuning the twist angle between two layers, one can modulate their electronic band structures and therefore the associated electrical transport and optical properties, which are distinct from the original ones of each individual layer. These new properties excite great passion in the exploration of new quantum states and possible applications of 2D bilayers. In this article, we will mainly review the prevailing fabrication methods and emerging physical properties of twisted bilayer materials and lastly give out a perspective of this topic.
基金This work was supported by the National Natural Science Foundation of China(No.11404043)Graduate Research Innovation Project of Chongqing(No.CYS18253).
文摘The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-principles calculations,we investigate both electronic structures and magnetic orderings of bulk and monolayer of chromium diiodides(CrI2).We demonstrate a counter-intuitive fact that the ground state of the free-standing monolayer of CrI2 is antiferromagnetic though the bulk possesses macroscopic ferromagnetic ordering.The interlayer interaction remains antiferromagnetic up to few-layer scenarios.The unique feature of CrI2 makes it an ideal workbench to investigate the relation between magnetic couplings and interlayer van der Waals interactions,and may offer an opportunity to 2D antiferromagnetic spintronic devices.
基金financially supported by the National Natural Science Foundation of China(No.52173246)Natural Science Foundation of Jilin Province(No.20220508141RC)+3 种基金DoubleThousand Talents Plan of Jiangxi Province(No.jxsq2023102005)111 Project(No.B13013)Education Department of Jilin Province(No.JJKH20221154KJ)Shccig-Qinling Program。
文摘Nowadays,lithium-ion batteries(LIBs)play a crucial role in modern society in the aspect of portable electronic devices and large-scale smart grids.However,the current performance of lithium-ion batteries has been unable to meet the growing expectations of society and scientific community.Herein,we have synthetically investigated availability of 2D Ni-TABQ monolayer as anode based on DFT for LIBs applications.Our findings have demonstrated that 2D Ni-TABQ monolayer is a semiconductor with a small band gap of 0.2 eV,which suggest that the electronic property of 2D Ni-TABQ monolayer would take place an evident shift from semiconductor property to metallic property after Li adsorption.Furthermore,we checked the stability of 2D Ni-TABQ monolayer and investigated the viability of exfoliation from bulk multilayer Ni-TABQ to form 2D Ni-TABQ monolayer in the light of exfoliation energy and binding energy.We continuously studied electrochemical properties of 2D Ni-TABQ monolayer with respect of theoretical specific capacity,Li-ion diffusion barriers and open-circuit voltage.During the charging process,2D Ni-TABQ monolayer can achieve a high specific capacity of 722 m Ah/g with an open-circuit voltage range from 1.12 V to 0.22 V.These aforementioned results make the 2D Ni-TABQ monolayer a promising anode for LIBs.
基金the National Natural Science Foundation of China(Grant Nos.11674136 and 11564022)Yunnan Province for Recruiting High-Caliber Technological Talents,China(Grant No.1097816002)+3 种基金Reserve Talents for Yunnan Young and Middle-aged Academic and Technical Leaders,China(Grant No.2017HB010)the Academic Qinglan Project of KUST(Grant No.1407840010)the Analysis and Testing Fund of KUST(Grant No.2017M20162230010)the High-level Talents of KUST(Grant No.1411909425)。
文摘The fascinating Dirac cone in honeycomb graphene,which underlies many unique electronic properties,has inspired the vast endeavors on pursuing new two-dimensional(2D)Dirac materials.Based on the density functional theory method,a 2D material Zn3Si2 of honeycomb transition-metal silicide with intrinsic Dirac cones has been predicted.The Zn3Si2 monolayer is dynamically and thermodynamically stable under ambient conditions.Importantly,the Zn3Si2 monolayer is a room-temperature 2D Dirac material with a spin-orbit coupling energy gap of 1.2 meV,which has an intrinsic Dirac cone arising from the special hexagonal lattice structure.Hole doping leads to the spin polarization of the electron,which results in a Dirac half-metal feature with single-spin Dirac fermion.This novel stable 2D transition-metal-silicon-framework material holds promises for electronic device applications in spintronics.
