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
MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Here...MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Herein,a unique MoS_(2)/FeS_(2)/C heterojunction with abundant defects and hollow structure(MFCHHS)was constructed.The synergy of defect engineering in MoS_(2),FeS_(2),and the carbon layer of MFCHHS with a larger specific surface area provides multiple storage sites of Na^(+)corresponding to the surface-controlled process.The MoS_(2)/FeS_(2)/C heterostructure and rich defects in MoS_(2) and carbon layer lower the Na^(+) diffusion energy barrier.Additionally,the construction of MoS_(2)/FeS_(2) heterojunction promotes electron transfer at the interface,accompanying with excellent conductivity of the carbon layer to facilitate reversible electrochemical reactions.The abundant defects and mismatches at the interface of MoS_(2)/FeS_(2) and MoS_(2)/C heterojunctions could relieve lattice stress and volume change sequentially.As a result,the MFCHHS anode exhibits the high capacity of 613.1 mA h g^(-1)at 0.5 A g^(-1) and 306.1 mA h g^(-1) at 20 A g^(-1).The capacity retention of 85.0%after 1400 cycles at 5.0 A g^(-1) is achieved.The density functional theory(DFT)calculation and in situ transmission electron microscope(TEM),Raman,ex-situ X-ray photon spectroscopy(XPS)studies confirm the low volume change during intercalation/deintercalation process and the efficient Na^(+)storage in the layered structure of MoS_(2) and carbon layer,as well as the defects and heterostructures in MFCHHS.We believe this work could provide an inspiration for constructing heterojunction with abundant defects to foster fast electron and Na^(+) diffusion kinetics,resulting in excellent rate capability and cycling stability.展开更多
Type-Ⅱband alignment can realize the efficient charge transfer and separation at the semiconductor heterointerface,which results in photoluminescence(PL)quenching.Recently,several researches demonstrated great enhanc...Type-Ⅱband alignment can realize the efficient charge transfer and separation at the semiconductor heterointerface,which results in photoluminescence(PL)quenching.Recently,several researches demonstrated great enhancement of localized PL at the interface of type-Ⅱtwo-dimensional(2D)heterostructure.However,the dominant physical mechanism of this enhanced PL emission has not been well understood.In this work,we symmetrically study the exciton dynamics of type-Ⅱlateral heterostructures of monolayer MoS_(2) and WS_(2) at room temperatures.The strong PL enhancement along the one-dimensional(1D)heterointerface is associated with the trion emission of the WS_(2) shell,while a dramatic PL quenching of neutral exciton is observed on the MoS_(2) core.The enhanced quantum yield of WS2trion emission can be explained by charge-transfer-enhanced photoexcited carrier dynamics,which is facilitated by resonance hole transfer from MoS_(2) side to WS_(2) side.This work sheds light on the 1D exciton photophysics in lateral heterostructures,which has the potential to lead to new concepts and applications of optoelectronic device.展开更多
Van der Waals heterostructures based on the two-dimensional(2D)semiconductor materials have attracted increasing attention due to their attractive properties.In this work,we demonstrate a high-sensitive back-gated pho...Van der Waals heterostructures based on the two-dimensional(2D)semiconductor materials have attracted increasing attention due to their attractive properties.In this work,we demonstrate a high-sensitive back-gated phototransistor based on the vertical HfSe_(2)/MoS_(2)heterostructure with a broad-spectral response from near-ultraviolet to near-infrared and an efficient gate tunability for photoresponse.Under bias,the phototransistor exhibits high responsivity of up to 1.42×103A/W,and ultrahigh specific detectivity of up to 1.39×1015cm·Hz^(1/2)·W^(-1).Moreover,it can also operate under zero bias with remarkable responsivity of 10.2 A/W,relatively high specific detectivity of 1.43×1014cm·Hz^(1/2)·W^(-1),ultralow dark current of 1.22 f A,and high on/off ratio of above 105.These results should be attributed to the fact that the vertical HfSe_(2)/MoS_(2)heterostructure not only improves the broadband photoresponse of the phototransistor but also greatly enhances its sensitivity.Therefore,the heterostructure provides a promising candidate for next generation high performance phototransistors.展开更多
Two-dimensional(2D)moirématerials have attracted a lot of attention and opened a new research frontier of twistronics due to their novel physical properties.Although great progress has been achieved,the inability...Two-dimensional(2D)moirématerials have attracted a lot of attention and opened a new research frontier of twistronics due to their novel physical properties.Although great progress has been achieved,the inability to precisely and reproducibly manipulate the twist angle hinders the further development of twistronics.Here,we demonstrated an atomic force microscope(AFM)tip manipulation method to control the interlayer twist angle of epitaxial MoS_(2)/graphene heterostructure with an ultra-high accuracy better than 0.1°.Furthermore,conductive AFM and spectroscopic characterizations were conducted to show the effects of the twist angle on moirépattern wavelength,phonons and excitons.Our work provides a technique to precisely control the twist angle of 2D moirématerials,enabling the possibility to establish the phase diagrams of moiréphysics with twist angle.展开更多
电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解...电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解污染物或生成有附加值的产物,能够带来多重效益.尿素氧化反应(UOR)具有较低的理论电压(0.37V),是替代OER的潜在反应之一.然而,UOR中复杂的六电子转移严重阻碍了尿素电解的整体效率.因此,设计经济且高效的电催化剂来促进UOR固有的缓慢动力学过程非常必要.硒化镍具有电子构型多样和结构调控灵活等优点,被认为是有效的UOR催化剂.然而,UOR过程涉及催化剂表面多种反应中间体的吸附/解吸,单相催化剂要同时满足多种反应中间的吸附/解吸是一项艰巨的挑战.众所周知,非均相电催化涉及电子转移以及电催化剂表面反应物和产物的吸附和解吸.因此,催化剂的电催化性能在很大程度上取决于材料表面的电子特性.通过构建异质结构是一种有效策略,可以调节电催化剂的电子结构,优化反应中间体的化学吸附行为,实现不同组份高效协同电催化.研究表明,通过界面工程优化结构和电子特性可进一步促进UOR的动力学.MoSe_(2)具有良好的稳定性和导电性,与镍基催化剂组合构建异质结构能够改善电催化反应中的催化动力学.本文通过简单的水热和低温硒化方法构建了异质NiSe_(2)/MoSe_(2)微球作为UOR的电催化剂.差分电荷密度和Mulliken电荷分析结果表明,MoSe_(2)与NiSe_(2)的耦合引起界面处的电荷重新分布,促使电子从NiSe_(2)向MoSe_(2)转移,更容易形成高价态Ni(NiOOH)活性物种.另外,异质界面的构建优化了催化剂表面的电子结构并调节d带中心,改变反应途径,降低反应能垒,从而提高UOR的反应活性.异质结NiSe_(2)/MoSe_(2)微球由于其独特的结构特征、强的协同耦合作用、增加的活性中心和高含量的高价Ni3+物种的综合优势而具有高效的催化性能.当负载在玻碳电极上时,仅需1.33 V的电压就能驱动10 m Acm^(-2)的电流密度,该活性优于大多数已报道的非贵金属UOR催化剂.将NiSe_(2)/MoSe_(2)催化剂组装到UOR//HER电解槽中时,NiSe_(2)/MoSe_(2)|Pt/C具有较低的操作电压和长期稳定性,在1.47 V的电池电压下电流密度达到10 m Acm^(-2),比单纯的水电解降低了约220 m V.与OER相比,热力学上有利的UOR可以作为阳极OER替代反应.综上,本文为能源/环境相关的催化反应提供了一个有效的催化剂体系,对构建高效异质结催化系统具有借鉴意义.展开更多
A series of MoS_(2)-modified CuO(CuO/MoS_(2))heterostructures were successfully fabricated.The photodegradation properties of organic dyes were explored in detail under visible light.The photocatalytic results demonst...A series of MoS_(2)-modified CuO(CuO/MoS_(2))heterostructures were successfully fabricated.The photodegradation properties of organic dyes were explored in detail under visible light.The photocatalytic results demonstrate that the CuO/MoS_(2)-3 heterostructure delivers superior degradation rates towards methyl violet dye(MV)and rhodamine B(RhB),reaching 99.8%and 95.3%within 30 min,respectively.The decent photodegradation activity is due to improved visible light adsorption and faster transfer of electron-hole pairs.The radical trapping experiments show that superoxide radicals(O_(2)^(-))and holes(h+)are the main active species in the removal of MV.Furthermore,the CuO/MoS_(2)-3 composite possesses the prominent stability and recyclability.This work offers a highly sustainable technique for designing a high-efficiency photocatalyst to remove environmental pollutants.展开更多
Due to the pristine interface of the 2D/3D face-tunneling heterostructure with an ultra-sharp doping profile, the 2D/3D tunneling field-effect transistor(TFET) is considered as one of the most promising low-power devi...Due to the pristine interface of the 2D/3D face-tunneling heterostructure with an ultra-sharp doping profile, the 2D/3D tunneling field-effect transistor(TFET) is considered as one of the most promising low-power devices that can simultaneously obtain low off-state current(IOFF), high on-state current(ION) and steep subthreshold swing(SS). As a key element for the 2D/3D TFET, the intensive exploration of the tunnel diode based on the 2D/3D heterostructure is in urgent need.The transfer technique composed of the exfoliation and the release process is currently the most common approach to fabricating the 2D/3D heterostructures. However, the well-established transfer technique of the 2D materials is still unavailable.Only a small part of the irregular films can usually be obtained by mechanical exfoliation, while the choice of the chemical exfoliation may lead to the contamination of the 2D material films by the ions in the chemical etchants. Moreover, the deformation of the 2D material in the transfer process due to its soft nature also leads to the nonuniformity of the transferred film,which is one of the main reasons for the presence of the wrinkles and the stacks in the transferred film. Thus, the large-scale fabrication of the high-quality 2D/3D tunnel diodes is limited. In this article, a comprehensive transfer technique that can mend up the shortages mentioned above with the aid of the water and the thermal release tape(TRT) is proposed. Based on the method we proposed, the MoS_(2)/Si tunnel diode is experimentally demonstrated and the transferred monolayer MoS_(2) film with the relatively high crystal quality is confirmed by atomic force microscopy(AFM), scanning electron microscopy(SEM), and Raman characterizations. Besides, the prominent negative differential resistance(NDR) effect is observed at room temperature, which verifies the relatively high quality of the MoS_(2)/Si heterojunction. The bilayer MoS_(2)/Si tunnel diode is also experimentally fabricated by repeating the transfer process we proposed, followed by the specific analysis of the electrical characteristics. This study shows the advantages of the transfer technique we proposed and indicates the great application foreground of the fabricated 2D/3D heterostructure for ultralow-power tunneling devices.展开更多
Hybrid organic–inorganic perovskite thin films have attracted much attention in optoelectronic and information fields because of their intriguing properties. Due to quantum confinement effects, ultrathin films in nm ...Hybrid organic–inorganic perovskite thin films have attracted much attention in optoelectronic and information fields because of their intriguing properties. Due to quantum confinement effects, ultrathin films in nm scale usually show special properties. Here, we report on the growth of methylammonium lead iodide(MAPbI_(3)) ultrathin films via co-deposition of PbI_2 and CH_3NH_3I(MAI) on chemical-vapor-deposition-grown monolayer MoS_(2) as well as the corresponding photoluminescence(PL) properties at different growing stages. Atomic force microscopy and scanning electron microscopy measurements reveal the MoS_(2) tuned growth of MAPbI_(3) in a Stranski–Krastanov mode. PL and Kelvin probe force microscopy results confirm that MAPbI_(3) /MoS_(2) heterostructures have a type-Ⅱ energy level alignment at the interface. Temperaturedependent PL measurements on layered MAPbI_(3) (at the initial stage) and on MAPbI_(3) crystals in averaged size of 500 nm(at the later stage) show rather different temperature dependence as well as the phase transitions from tetragonal to orthorhombic at 120 and 150 K, respectively. Our findings are useful in fabricating MAPbI_(3) /transition-metal dichalcogenide based innovative devices for wider optoelectronic applications.展开更多
Transition metal dichalcogenides are attractive anode materials for sodium ion batteries(SIBs)due to their high theoretical capacity and large interlayer spacing.However,its practical application is hampered by the sl...Transition metal dichalcogenides are attractive anode materials for sodium ion batteries(SIBs)due to their high theoretical capacity and large interlayer spacing.However,its practical application is hampered by the sluggish kinetics of Na^(+)insertion and structure collapse caused by Na^(+)insertion/deinsertion.Herein,the heterostructures of MoSe_(2) nanosheets vertically growing on bowl-like carbon(MoSe_(2)@C)are designed and prepared by a template method coupled with selenization treatment to boost storage sodium performance.The hollow and collapse could provide enough storage space for Na^(+)and alleviate the volume expansion during the charge/discharge processes.MoSe_(2) nanosheets vertically grown on carbon could expose more active sites for adsorbing Na^(+)to enhance the utilization rate of electrode materials.Moreover,building heterostructures by combining different phase components could facilitate Na^(+)diffusion and advance reaction kinetics.Benefiting from these merits,the bowl-like MoSe_(2)@C shows outstanding reversible capacity(356.8 mAh·g^(-1) after 1500 cycles at 1 A·g^(-1))and remarkable rate performance(249.9 mAh·g^(-1)10 A·g^(-1)).展开更多
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the National Natural Science Foundation of China(NSFC)(22105059,22279112)the Talent Introduction Program of Hebei Agricultural University(YJ201810)+5 种基金the Youth Topnotch Talent Foundation of Hebei Provincial Universities(BJK2022023)the Natural Science Foundation of Hebei Province(B2022203018)the Fok Ying-Tong Education Foundation of China(171064)the Natural Science Foundation of Shandong Province,China(ZR2021QE192)the China Postdoctoral Science Foundation(2018M630747)the 333 Talent Program of Hebei Province(C20221018)for their support。
文摘MoS_(2) is a promising anode material in sodium-ion battery technologies for possessing high theoretical capacity.However,the sluggish Na^(+) diffusion kinetics and low electronic conductivity hinder the promises.Herein,a unique MoS_(2)/FeS_(2)/C heterojunction with abundant defects and hollow structure(MFCHHS)was constructed.The synergy of defect engineering in MoS_(2),FeS_(2),and the carbon layer of MFCHHS with a larger specific surface area provides multiple storage sites of Na^(+)corresponding to the surface-controlled process.The MoS_(2)/FeS_(2)/C heterostructure and rich defects in MoS_(2) and carbon layer lower the Na^(+) diffusion energy barrier.Additionally,the construction of MoS_(2)/FeS_(2) heterojunction promotes electron transfer at the interface,accompanying with excellent conductivity of the carbon layer to facilitate reversible electrochemical reactions.The abundant defects and mismatches at the interface of MoS_(2)/FeS_(2) and MoS_(2)/C heterojunctions could relieve lattice stress and volume change sequentially.As a result,the MFCHHS anode exhibits the high capacity of 613.1 mA h g^(-1)at 0.5 A g^(-1) and 306.1 mA h g^(-1) at 20 A g^(-1).The capacity retention of 85.0%after 1400 cycles at 5.0 A g^(-1) is achieved.The density functional theory(DFT)calculation and in situ transmission electron microscope(TEM),Raman,ex-situ X-ray photon spectroscopy(XPS)studies confirm the low volume change during intercalation/deintercalation process and the efficient Na^(+)storage in the layered structure of MoS_(2) and carbon layer,as well as the defects and heterostructures in MFCHHS.We believe this work could provide an inspiration for constructing heterojunction with abundant defects to foster fast electron and Na^(+) diffusion kinetics,resulting in excellent rate capability and cycling stability.
基金Project supported by the National Natural Science Foundation of China(Grant No.61804047)the Training Program for the Natural Science Foundation of Henan Normal University,China(Grant No.2017PL02)+2 种基金the Scientific Research Start-up Foundation for Ph D of Chaohu University,China(Grant No.KYQD-2023012)the Natural Science Foundation Henan Province of China(Grant No.232300421236)the High Performance Computing Center(HPCC)of Henan Normal University,China。
文摘Type-Ⅱband alignment can realize the efficient charge transfer and separation at the semiconductor heterointerface,which results in photoluminescence(PL)quenching.Recently,several researches demonstrated great enhancement of localized PL at the interface of type-Ⅱtwo-dimensional(2D)heterostructure.However,the dominant physical mechanism of this enhanced PL emission has not been well understood.In this work,we symmetrically study the exciton dynamics of type-Ⅱlateral heterostructures of monolayer MoS_(2) and WS_(2) at room temperatures.The strong PL enhancement along the one-dimensional(1D)heterointerface is associated with the trion emission of the WS_(2) shell,while a dramatic PL quenching of neutral exciton is observed on the MoS_(2) core.The enhanced quantum yield of WS2trion emission can be explained by charge-transfer-enhanced photoexcited carrier dynamics,which is facilitated by resonance hole transfer from MoS_(2) side to WS_(2) side.This work sheds light on the 1D exciton photophysics in lateral heterostructures,which has the potential to lead to new concepts and applications of optoelectronic device.
基金Project supported by the National Natural Science Foundation of China(Grant No.51702245)the Fundamental Research Funds for the Central Universities(Grant No.WUT2021III065JC)
文摘Van der Waals heterostructures based on the two-dimensional(2D)semiconductor materials have attracted increasing attention due to their attractive properties.In this work,we demonstrate a high-sensitive back-gated phototransistor based on the vertical HfSe_(2)/MoS_(2)heterostructure with a broad-spectral response from near-ultraviolet to near-infrared and an efficient gate tunability for photoresponse.Under bias,the phototransistor exhibits high responsivity of up to 1.42×103A/W,and ultrahigh specific detectivity of up to 1.39×1015cm·Hz^(1/2)·W^(-1).Moreover,it can also operate under zero bias with remarkable responsivity of 10.2 A/W,relatively high specific detectivity of 1.43×1014cm·Hz^(1/2)·W^(-1),ultralow dark current of 1.22 f A,and high on/off ratio of above 105.These results should be attributed to the fact that the vertical HfSe_(2)/MoS_(2)heterostructure not only improves the broadband photoresponse of the phototransistor but also greatly enhances its sensitivity.Therefore,the heterostructure provides a promising candidate for next generation high performance phototransistors.
基金Project supported by the Natioanl Natural Science Foundation of China(Grant Nos.62122084,12074412,61888102,and 11834017)。
文摘Two-dimensional(2D)moirématerials have attracted a lot of attention and opened a new research frontier of twistronics due to their novel physical properties.Although great progress has been achieved,the inability to precisely and reproducibly manipulate the twist angle hinders the further development of twistronics.Here,we demonstrated an atomic force microscope(AFM)tip manipulation method to control the interlayer twist angle of epitaxial MoS_(2)/graphene heterostructure with an ultra-high accuracy better than 0.1°.Furthermore,conductive AFM and spectroscopic characterizations were conducted to show the effects of the twist angle on moirépattern wavelength,phonons and excitons.Our work provides a technique to precisely control the twist angle of 2D moirématerials,enabling the possibility to establish the phase diagrams of moiréphysics with twist angle.
文摘电催化水分解是实现绿色制氢的理想方法之一.然而,阳极析氧反应(OER)固有的缓慢动力学和高理论电压(1.23V),使得电解水制氢的能效受到严重限制.采用理论电位更低和热力学更有利的小分子氧化反应替代OER过程,可以在降低电能耗的同时降解污染物或生成有附加值的产物,能够带来多重效益.尿素氧化反应(UOR)具有较低的理论电压(0.37V),是替代OER的潜在反应之一.然而,UOR中复杂的六电子转移严重阻碍了尿素电解的整体效率.因此,设计经济且高效的电催化剂来促进UOR固有的缓慢动力学过程非常必要.硒化镍具有电子构型多样和结构调控灵活等优点,被认为是有效的UOR催化剂.然而,UOR过程涉及催化剂表面多种反应中间体的吸附/解吸,单相催化剂要同时满足多种反应中间的吸附/解吸是一项艰巨的挑战.众所周知,非均相电催化涉及电子转移以及电催化剂表面反应物和产物的吸附和解吸.因此,催化剂的电催化性能在很大程度上取决于材料表面的电子特性.通过构建异质结构是一种有效策略,可以调节电催化剂的电子结构,优化反应中间体的化学吸附行为,实现不同组份高效协同电催化.研究表明,通过界面工程优化结构和电子特性可进一步促进UOR的动力学.MoSe_(2)具有良好的稳定性和导电性,与镍基催化剂组合构建异质结构能够改善电催化反应中的催化动力学.本文通过简单的水热和低温硒化方法构建了异质NiSe_(2)/MoSe_(2)微球作为UOR的电催化剂.差分电荷密度和Mulliken电荷分析结果表明,MoSe_(2)与NiSe_(2)的耦合引起界面处的电荷重新分布,促使电子从NiSe_(2)向MoSe_(2)转移,更容易形成高价态Ni(NiOOH)活性物种.另外,异质界面的构建优化了催化剂表面的电子结构并调节d带中心,改变反应途径,降低反应能垒,从而提高UOR的反应活性.异质结NiSe_(2)/MoSe_(2)微球由于其独特的结构特征、强的协同耦合作用、增加的活性中心和高含量的高价Ni3+物种的综合优势而具有高效的催化性能.当负载在玻碳电极上时,仅需1.33 V的电压就能驱动10 m Acm^(-2)的电流密度,该活性优于大多数已报道的非贵金属UOR催化剂.将NiSe_(2)/MoSe_(2)催化剂组装到UOR//HER电解槽中时,NiSe_(2)/MoSe_(2)|Pt/C具有较低的操作电压和长期稳定性,在1.47 V的电池电压下电流密度达到10 m Acm^(-2),比单纯的水电解降低了约220 m V.与OER相比,热力学上有利的UOR可以作为阳极OER替代反应.综上,本文为能源/环境相关的催化反应提供了一个有效的催化剂体系,对构建高效异质结催化系统具有借鉴意义.
基金the National Natural Science Foundation of China(51572185)Natural Science Foundation of Shanxi Province(202203021211158 and 20210302123173)the Key Research and Developmen program of Shanxi Province(International Cooperation,201903D421079)for the financial support.
文摘A series of MoS_(2)-modified CuO(CuO/MoS_(2))heterostructures were successfully fabricated.The photodegradation properties of organic dyes were explored in detail under visible light.The photocatalytic results demonstrate that the CuO/MoS_(2)-3 heterostructure delivers superior degradation rates towards methyl violet dye(MV)and rhodamine B(RhB),reaching 99.8%and 95.3%within 30 min,respectively.The decent photodegradation activity is due to improved visible light adsorption and faster transfer of electron-hole pairs.The radical trapping experiments show that superoxide radicals(O_(2)^(-))and holes(h+)are the main active species in the removal of MV.Furthermore,the CuO/MoS_(2)-3 composite possesses the prominent stability and recyclability.This work offers a highly sustainable technique for designing a high-efficiency photocatalyst to remove environmental pollutants.
基金Project supported by the National Natural Science Foundation of China (Grant No.61851405)。
文摘Due to the pristine interface of the 2D/3D face-tunneling heterostructure with an ultra-sharp doping profile, the 2D/3D tunneling field-effect transistor(TFET) is considered as one of the most promising low-power devices that can simultaneously obtain low off-state current(IOFF), high on-state current(ION) and steep subthreshold swing(SS). As a key element for the 2D/3D TFET, the intensive exploration of the tunnel diode based on the 2D/3D heterostructure is in urgent need.The transfer technique composed of the exfoliation and the release process is currently the most common approach to fabricating the 2D/3D heterostructures. However, the well-established transfer technique of the 2D materials is still unavailable.Only a small part of the irregular films can usually be obtained by mechanical exfoliation, while the choice of the chemical exfoliation may lead to the contamination of the 2D material films by the ions in the chemical etchants. Moreover, the deformation of the 2D material in the transfer process due to its soft nature also leads to the nonuniformity of the transferred film,which is one of the main reasons for the presence of the wrinkles and the stacks in the transferred film. Thus, the large-scale fabrication of the high-quality 2D/3D tunnel diodes is limited. In this article, a comprehensive transfer technique that can mend up the shortages mentioned above with the aid of the water and the thermal release tape(TRT) is proposed. Based on the method we proposed, the MoS_(2)/Si tunnel diode is experimentally demonstrated and the transferred monolayer MoS_(2) film with the relatively high crystal quality is confirmed by atomic force microscopy(AFM), scanning electron microscopy(SEM), and Raman characterizations. Besides, the prominent negative differential resistance(NDR) effect is observed at room temperature, which verifies the relatively high quality of the MoS_(2)/Si heterojunction. The bilayer MoS_(2)/Si tunnel diode is also experimentally fabricated by repeating the transfer process we proposed, followed by the specific analysis of the electrical characteristics. This study shows the advantages of the transfer technique we proposed and indicates the great application foreground of the fabricated 2D/3D heterostructure for ultralow-power tunneling devices.
基金Project supported by the National Natural Science Foundation of China (Grant Nos.11874427 and 11804395)the Fundamental Research Funds for the Central Universities of Central South University (Grant No.2020zzts377)。
文摘Hybrid organic–inorganic perovskite thin films have attracted much attention in optoelectronic and information fields because of their intriguing properties. Due to quantum confinement effects, ultrathin films in nm scale usually show special properties. Here, we report on the growth of methylammonium lead iodide(MAPbI_(3)) ultrathin films via co-deposition of PbI_2 and CH_3NH_3I(MAI) on chemical-vapor-deposition-grown monolayer MoS_(2) as well as the corresponding photoluminescence(PL) properties at different growing stages. Atomic force microscopy and scanning electron microscopy measurements reveal the MoS_(2) tuned growth of MAPbI_(3) in a Stranski–Krastanov mode. PL and Kelvin probe force microscopy results confirm that MAPbI_(3) /MoS_(2) heterostructures have a type-Ⅱ energy level alignment at the interface. Temperaturedependent PL measurements on layered MAPbI_(3) (at the initial stage) and on MAPbI_(3) crystals in averaged size of 500 nm(at the later stage) show rather different temperature dependence as well as the phase transitions from tetragonal to orthorhombic at 120 and 150 K, respectively. Our findings are useful in fabricating MAPbI_(3) /transition-metal dichalcogenide based innovative devices for wider optoelectronic applications.
基金supported by the National Natural Science Foundation of China(No.U21A2077)the Taishan Scholar Project Foundation of Shandong Province(No.ts20190908)the Natural Science Foundation of Shandong Province(Nos.ZR2021ZD05,ZR2022QB200).
文摘Transition metal dichalcogenides are attractive anode materials for sodium ion batteries(SIBs)due to their high theoretical capacity and large interlayer spacing.However,its practical application is hampered by the sluggish kinetics of Na^(+)insertion and structure collapse caused by Na^(+)insertion/deinsertion.Herein,the heterostructures of MoSe_(2) nanosheets vertically growing on bowl-like carbon(MoSe_(2)@C)are designed and prepared by a template method coupled with selenization treatment to boost storage sodium performance.The hollow and collapse could provide enough storage space for Na^(+)and alleviate the volume expansion during the charge/discharge processes.MoSe_(2) nanosheets vertically grown on carbon could expose more active sites for adsorbing Na^(+)to enhance the utilization rate of electrode materials.Moreover,building heterostructures by combining different phase components could facilitate Na^(+)diffusion and advance reaction kinetics.Benefiting from these merits,the bowl-like MoSe_(2)@C shows outstanding reversible capacity(356.8 mAh·g^(-1) after 1500 cycles at 1 A·g^(-1))and remarkable rate performance(249.9 mAh·g^(-1)10 A·g^(-1)).