Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the...Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the shuttle effect of soluble lithium sulfide species,the insulating nature of sulfur,and the fast capacity decay of the electrodes.Various efforts are devoted to address these problems through questing more conductive hosts with abundant polysulfide chemisorption sites,as well as modifying the separators to physically/chemically retard the polysulfides migration.Two dimensional transition metal carbides,carbonitrides and nitrides,so-called MXenes,are ideal for confining the polysulfides shuttling effects due to their high conductivity,layered structure as well as rich surface terminations.As such,MXenes have thus been widely studied in Li-S batteries,focusing on the conductive sulfur hosts,polysulfides interfaces,and separators.Therefore,in this review,we summarize the significant progresses regarding the design of multifunctional MXene-based Li-S batteries and discuss the solutions for improving electrochemical performances in detail.In addition,challenges and perspectives of MXenes for Li-S batteries are also outlined.展开更多
In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaA...In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaAs heterojunction device exhibited obvious photovoltaic behavior to 808 nm illumination,indicating that the near-infrared photodetector can be used as a self-driven device without external power supply.Further device analysis showed that the hybrid heterojunction exhibited a high on/off ratio of 1.16×10^5 measured at 808 nm under zero bias voltage.The responsivity and specific detectivity of photodetector were estimated to be 171.34 mA/W and 2.36×10^11 Jones,respectively.Moreover,the device showed excellent stability and reliable repeatability.After 2 months,the photoelectric characteristics of the near-infrared photodetector hardly degrade in air,attributable to the good stability of the PdSe2.Finally,the PdSe2/GaAs-based heterojunction device can also function as a near-infrared light sensor.展开更多
The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demo...The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar nanobubbles.The interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth transformation.On the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a round-shape.Especially,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D materials.This can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface catalysis.Furthermore,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding conditions.These findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.展开更多
Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained...Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained by a liquid-phase exfoliation of h-BN powders and incorporated into EVA coatings for improving the safety performance of 1,3,5,7-tetranitro-1,3,5,7-tetrazocane(HMX).HBNNSs and ethylene-vinyl acetate copolymer(EVA)were introduced to HMX by a solvent-slurry process.For comparison,the HMX/EVA and HMX/EVA/graphene(HMX/EVA/G)composites were also prepared by a similar process.The morphology,crystal form,surface element distribution,thermal decomposition property and impact sensitivity of HMX/EVA/hBNNSs composites were contrastively investigated.Results showed that as prepared HMX/EVA/hBNNSs composites were well coated with hBNNSs and EVA,and exhibited better thermal stability and lower impact sensitivity than that of HMX/EVA and HMX/EVA/G composites,suggesting superior performance of desensitization of hBNNSs in explosives.展开更多
Exploring new strategies to broaden the upper/lower limit of thermal conductivity is of great interest to develop thermal management materials that can adapt to extreme environments.In this work,we employ an interfaci...Exploring new strategies to broaden the upper/lower limit of thermal conductivity is of great interest to develop thermal management materials that can adapt to extreme environments.In this work,we employ an interfacial ion regulation to enhance the thermal insulation performance of 2D layered double hydroxide nanosheets.The introduction of interfacial ion enlarges the interplanar spacing of Co(OH)_(2) nanosheets from 4.64 to 8.05 ?,which reduces phonon scattering length perpendicular to the two-dimensional plane and leads to enhanced interlayer thermal insulation.The interfacial ion-regulated Co(OH)_(2)(named as Co(OH)_(2)-M^(x-)) exhibits 3-fold enhancement of thermal insulation through decreasing the thermal conductivity to as low as 0.15 W m^(-1) K^(-1),which is among the top values in 2D solid materials.We anticipate that interfacial ion regulation for 2D nanosheets paves a new avenue to break through the thermal insulation limit.展开更多
Black phosphorus(BP),especially for BP nanosheets,with unique layered structure among two dimensional(2D)materials has attracted much attention due to its outstanding physical properties,such as ultra-high mobility,in...Black phosphorus(BP),especially for BP nanosheets,with unique layered structure among two dimensional(2D)materials has attracted much attention due to its outstanding physical properties,such as ultra-high mobility,in-plane anisotropic properties.However,the small horizontal-size of reported BP limits its applications in the integrated circuit or some functional devices.In this work,a solvothermalassisted liquid-phase exfoliation technique is firstly employed for preparing large size and high-quality BP nanosheets.In the high-polar acetonitrile solvent,solvothermal treatment weakens the Van der Waals forces of block BP.Together with the subsequently ultrasonic processing,effective exfoliation of large size and high-quality BP nanosheets are realized.The TEM,AFM and Raman results indicate that the prepared BP nanosheets are high quality with an average thickness of about 2 nm,and the horizontalsize is up to 10μm.This facile and effective method for exfoliated BP nanosheets provides a promising strategy for the exfoliation of other 2D materials.展开更多
Two‐dimensional transition metal dichalcogenides(TMDs)play host to a wide range of novel topological states,such as quantum spin Hall insulators,superconductors,and Weyl semimetals.The rich polymorphism in TMDs sugge...Two‐dimensional transition metal dichalcogenides(TMDs)play host to a wide range of novel topological states,such as quantum spin Hall insulators,superconductors,and Weyl semimetals.The rich polymorphism in TMDs suggests that phase engineering can be used to switch between different charge order states.Intercalation of atoms or molecules into the van der Waals gap of TMDs has emerged as a powerful approach to modify the properties of the material,leading to phase transition or the formation of substoichiometric phases via compositional tuning,thus broadening the electronic and optical landscape of these materials for a wide range of applications.Here,we review the current efforts in the preparation of intercalated TMD.The challenges and opportunities for intercalated TMDs to create a new device paradigm for material science are discussed.展开更多
Two-dimensional(2 D) materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosh...Two-dimensional(2 D) materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosheets(CONs) with large lateral sizes(up to 200 mm) and high aspect ratios(〉20 000) at the air-water interface through the Langmuir-Blodgett method. These CONs exhibit good crystallinity proved by high resolution transmission electron microscopy(HRTEM) and selected area electron diffraction(SAED). In addition, the hydrophobicity of these CONs can be systematically adjusted by the introduction of various functional groups, making them suitable as functional coating and membrane materials.展开更多
Two-dimensional transition metal dichalcogenide semiconductors have emerged as promising candidates for optoelectronic devices with unprecedented properties and ultra-compact footprints. However, the high sensitivity ...Two-dimensional transition metal dichalcogenide semiconductors have emerged as promising candidates for optoelectronic devices with unprecedented properties and ultra-compact footprints. However, the high sensitivity of atomically thin materials to the surrounding dielectric media imposes severe limitations on their practical applicability. Hence, to enable the effective integration of these materials in devices, the development of reliable encapsulation procedures that preserve their physical properties is required. Here, the excitonic photoluminescence (at room temperature and 10 K) is assessed on mechanically exfoliated WSe2 monolayer flakes encapsulated with SiOx and AlxOy layers by means of chemical and physical deposition techniques. Conformal coating on untreated and non- functionalized flakes is successfully achieved by all the techniques examined, with the exception of atomic layer deposition, for which a cluster-like oxide coating is formed. No significant compositional or strain state changes in the flakes are detected upon encapsulation, independently of the technique adopted. Remarkably, our results show that the optical emission of the flakes is strongly influenced by the stoichiometry quality of the encapsulating oxide. When the encapsulation is carried out with slightly sub-stoichiometric oxides, two remarkable phenomena are observed. First, dominant trion (charged exciton) photoluminescence is detected at room temperature, revealing a clear electrical doping of the monolayers. Second, a strong decrease in the optical emission of the monolayers is observed, and attributed to non-radiative recombination processes and/or carrier transfer from the flake to the oxide. Power- and temperature-dependent photoluminescence measurements further confirm that stoichiometric oxides obtained by physical deposition lead to a successful encapsulation, opening a promising route for the development of integrated two-dimensional devices.展开更多
基金the support from an Empa interal research grant.
文摘Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the shuttle effect of soluble lithium sulfide species,the insulating nature of sulfur,and the fast capacity decay of the electrodes.Various efforts are devoted to address these problems through questing more conductive hosts with abundant polysulfide chemisorption sites,as well as modifying the separators to physically/chemically retard the polysulfides migration.Two dimensional transition metal carbides,carbonitrides and nitrides,so-called MXenes,are ideal for confining the polysulfides shuttling effects due to their high conductivity,layered structure as well as rich surface terminations.As such,MXenes have thus been widely studied in Li-S batteries,focusing on the conductive sulfur hosts,polysulfides interfaces,and separators.Therefore,in this review,we summarize the significant progresses regarding the design of multifunctional MXene-based Li-S batteries and discuss the solutions for improving electrochemical performances in detail.In addition,challenges and perspectives of MXenes for Li-S batteries are also outlined.
基金supported by the National Natural Science Foundation of China(No.61575059,No.61675062,No.21501038)the Fundamental Research Funds for the Central Universities(No.JZ2018HGPB0275,No.JZ2018HGTA0220,and No.JZ2018HGXC0001).
文摘In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaAs heterojunction device exhibited obvious photovoltaic behavior to 808 nm illumination,indicating that the near-infrared photodetector can be used as a self-driven device without external power supply.Further device analysis showed that the hybrid heterojunction exhibited a high on/off ratio of 1.16×10^5 measured at 808 nm under zero bias voltage.The responsivity and specific detectivity of photodetector were estimated to be 171.34 mA/W and 2.36×10^11 Jones,respectively.Moreover,the device showed excellent stability and reliable repeatability.After 2 months,the photoelectric characteristics of the near-infrared photodetector hardly degrade in air,attributable to the good stability of the PdSe2.Finally,the PdSe2/GaAs-based heterojunction device can also function as a near-infrared light sensor.
基金the National Natural Science Foundation of China(Nos.21872169,91845109,21688102,and 21825203)the National Key R&D Program of China(No.2016YFA0200200)+2 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17020000)China Postdoctoral Science Foundation(No.2019M651997)Natural Science Foundation of Jiangsu Province(No.BK20200257).
文摘The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar nanobubbles.The interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth transformation.On the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a round-shape.Especially,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D materials.This can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface catalysis.Furthermore,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding conditions.These findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.
基金The project was supported by Equipment Pre-research Key Laboratory Fund(No.6142020305)The authors would like to thank Shiyanjia Lab(www.shiyanjia.com)for the support of XPS test.
文摘Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained by a liquid-phase exfoliation of h-BN powders and incorporated into EVA coatings for improving the safety performance of 1,3,5,7-tetranitro-1,3,5,7-tetrazocane(HMX).HBNNSs and ethylene-vinyl acetate copolymer(EVA)were introduced to HMX by a solvent-slurry process.For comparison,the HMX/EVA and HMX/EVA/graphene(HMX/EVA/G)composites were also prepared by a similar process.The morphology,crystal form,surface element distribution,thermal decomposition property and impact sensitivity of HMX/EVA/hBNNSs composites were contrastively investigated.Results showed that as prepared HMX/EVA/hBNNSs composites were well coated with hBNNSs and EVA,and exhibited better thermal stability and lower impact sensitivity than that of HMX/EVA and HMX/EVA/G composites,suggesting superior performance of desensitization of hBNNSs in explosives.
基金supported by the National Basic Research Program of China (2017YFA0206702)the National Natural Science Foundation of China (21925110, 21890751, 91745113)+6 种基金the China Postdoctoral Science Foundation (2019TQ0299)the Fundamental Research Funds for the Central Universities (WK 2060190084)the Natural Science Foundation of China (U1832168)the Anhui Provincial Natural Science Foundation (1808085MB26)the Fundamental Research Funds for the Central Universities (WK5290000001)the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB36000000)China National Postdoctoral Program for Innovative Talents (BX2021283)。
文摘Exploring new strategies to broaden the upper/lower limit of thermal conductivity is of great interest to develop thermal management materials that can adapt to extreme environments.In this work,we employ an interfacial ion regulation to enhance the thermal insulation performance of 2D layered double hydroxide nanosheets.The introduction of interfacial ion enlarges the interplanar spacing of Co(OH)_(2) nanosheets from 4.64 to 8.05 ?,which reduces phonon scattering length perpendicular to the two-dimensional plane and leads to enhanced interlayer thermal insulation.The interfacial ion-regulated Co(OH)_(2)(named as Co(OH)_(2)-M^(x-)) exhibits 3-fold enhancement of thermal insulation through decreasing the thermal conductivity to as low as 0.15 W m^(-1) K^(-1),which is among the top values in 2D solid materials.We anticipate that interfacial ion regulation for 2D nanosheets paves a new avenue to break through the thermal insulation limit.
基金This work was supported by the National Natural Science Foundation of China(51702203,51772182,21471093)the Program for Key Science&Technology Innovation Team of Shaanxi Province(2012KCT-21),the 111 Project(B14041)the Fundamental Research Funds for the Central Universities(GK201501007).
文摘Black phosphorus(BP),especially for BP nanosheets,with unique layered structure among two dimensional(2D)materials has attracted much attention due to its outstanding physical properties,such as ultra-high mobility,in-plane anisotropic properties.However,the small horizontal-size of reported BP limits its applications in the integrated circuit or some functional devices.In this work,a solvothermalassisted liquid-phase exfoliation technique is firstly employed for preparing large size and high-quality BP nanosheets.In the high-polar acetonitrile solvent,solvothermal treatment weakens the Van der Waals forces of block BP.Together with the subsequently ultrasonic processing,effective exfoliation of large size and high-quality BP nanosheets are realized.The TEM,AFM and Raman results indicate that the prepared BP nanosheets are high quality with an average thickness of about 2 nm,and the horizontalsize is up to 10μm.This facile and effective method for exfoliated BP nanosheets provides a promising strategy for the exfoliation of other 2D materials.
基金Ministry of Education—Singapore,Grant/Award Number:MOE2018‐T3‐1‐005。
文摘Two‐dimensional transition metal dichalcogenides(TMDs)play host to a wide range of novel topological states,such as quantum spin Hall insulators,superconductors,and Weyl semimetals.The rich polymorphism in TMDs suggests that phase engineering can be used to switch between different charge order states.Intercalation of atoms or molecules into the van der Waals gap of TMDs has emerged as a powerful approach to modify the properties of the material,leading to phase transition or the formation of substoichiometric phases via compositional tuning,thus broadening the electronic and optical landscape of these materials for a wide range of applications.Here,we review the current efforts in the preparation of intercalated TMD.The challenges and opportunities for intercalated TMDs to create a new device paradigm for material science are discussed.
基金supported by National University of Singapore No. CENGas R-261-508-001-646)Ministry of Education – Singapore ( 13No. MOE Ac RF Tier 1 R-279-000-472-112)
文摘Two-dimensional(2 D) materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosheets(CONs) with large lateral sizes(up to 200 mm) and high aspect ratios(〉20 000) at the air-water interface through the Langmuir-Blodgett method. These CONs exhibit good crystallinity proved by high resolution transmission electron microscopy(HRTEM) and selected area electron diffraction(SAED). In addition, the hydrophobicity of these CONs can be systematically adjusted by the introduction of various functional groups, making them suitable as functional coating and membrane materials.
基金The authors would like to thank Georgios Katsaros and Tim Wehling for valuable discussions. Stephan Br~iuer, Albin Schwarz, and Ursula Kainz are ackno- wledged for technical support. A. M. acknowledges the financial support through BES-2013-062593. G. G. acknowledges support from the Austrian Science Fund through project P 28018-B27. I. Z. acknowledges financial support from the Swiss National Science Foundation research grant (No. 200021_165784). This work was partially funded by the Austrian Science Fund through the projects P24471 and P26830, and by the Spanish Ministry for Economy and Competitiveness trough the project MINECO/FEDER TEC2015-69916- C2-1-R.
文摘Two-dimensional transition metal dichalcogenide semiconductors have emerged as promising candidates for optoelectronic devices with unprecedented properties and ultra-compact footprints. However, the high sensitivity of atomically thin materials to the surrounding dielectric media imposes severe limitations on their practical applicability. Hence, to enable the effective integration of these materials in devices, the development of reliable encapsulation procedures that preserve their physical properties is required. Here, the excitonic photoluminescence (at room temperature and 10 K) is assessed on mechanically exfoliated WSe2 monolayer flakes encapsulated with SiOx and AlxOy layers by means of chemical and physical deposition techniques. Conformal coating on untreated and non- functionalized flakes is successfully achieved by all the techniques examined, with the exception of atomic layer deposition, for which a cluster-like oxide coating is formed. No significant compositional or strain state changes in the flakes are detected upon encapsulation, independently of the technique adopted. Remarkably, our results show that the optical emission of the flakes is strongly influenced by the stoichiometry quality of the encapsulating oxide. When the encapsulation is carried out with slightly sub-stoichiometric oxides, two remarkable phenomena are observed. First, dominant trion (charged exciton) photoluminescence is detected at room temperature, revealing a clear electrical doping of the monolayers. Second, a strong decrease in the optical emission of the monolayers is observed, and attributed to non-radiative recombination processes and/or carrier transfer from the flake to the oxide. Power- and temperature-dependent photoluminescence measurements further confirm that stoichiometric oxides obtained by physical deposition lead to a successful encapsulation, opening a promising route for the development of integrated two-dimensional devices.