The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we desi...The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.展开更多
A new coordination polymer [Cd(bimc)2]n was obtained by the reaction of Hbimc with Cd(NO3) 2·4H2O in NaOH solution, and characterized by elemental analysis, IR and singlecrystal X-ray diffraction. The crystal...A new coordination polymer [Cd(bimc)2]n was obtained by the reaction of Hbimc with Cd(NO3) 2·4H2O in NaOH solution, and characterized by elemental analysis, IR and singlecrystal X-ray diffraction. The crystal belongs to orthorhombic, space group Pbcn with a = 12.533(4), b = 15.705(5), c = 15.200(5) A, V= 2991.8(15) A^3, Mr = 434.68, Z = 8, Dc = 1.930 g/cm^3, F(000) = 1712,μ(MoKa) = 1.492 mm^-1, the final R = 0.0410 and wR = 0.0804 for 1661 observed reflections (I 〉 2σ(I)). The Cd atom exhibits a distorted six-coordinate CdNzOa octahedral coordination geometry. The complex molecules are linked by both μ2-(η2-O, O^-), NI and μ2-(η2-O, O^-), N3 coordination modes of ligands to form cross-like wave (4, 4) layer structures which are further stacked through interlayer hydrogen bonds and π-π stacking interactions in an offset fashion to form a 3D supramolecular structure.展开更多
A new thiostannate,[tmdpH2]Sn3S7 1(tmdp = 4,4'-trimethylenedipiperidine),has been synthesized under solvothermal conditions and characterized by elemental analysis,IR spectroscopy,and single-crystal X-ray diffracti...A new thiostannate,[tmdpH2]Sn3S7 1(tmdp = 4,4'-trimethylenedipiperidine),has been synthesized under solvothermal conditions and characterized by elemental analysis,IR spectroscopy,and single-crystal X-ray diffraction analysis.In 1,the Sn3S4 secondary incomplete cubane-like building units are bridged by μ2-S atoms to form Sn12S12 rings which are then joined parallelly to the [001] plane,giving the final 2D(Sn3S7^2-)n layer of(6,3) network.The layers are stacked along the c axis so that 24-membered ring channels are generated,in which the organic cations are accommodated.The compound crystallizes in monoclinic,space group C2/c,with a=23.052(3),b=13.4039(12),c=18.412(2)A,β=120.112(4)°,V=4921.3(9)A^3,C13H28N2S7Sn3,Mr=792.86,Z=8,Dc=2.140 g/cm^3,F(000)=3056,μ=3.619 mm^-1,the final R=0.0488 and wR=0.1125 for 4607 observed reflections with I〉2σ(I).展开更多
A new ion-pair complex, [BzMeQ1]2[Ni(nmt)2]1([BzMeQ1]^+ = 1-benzyl-4-ntethylquino- linium, mnta- -- maleonitriledithiolate) has been synthesized and structurally characterized by IR, ESI-MS and X-ray diffraction ...A new ion-pair complex, [BzMeQ1]2[Ni(nmt)2]1([BzMeQ1]^+ = 1-benzyl-4-ntethylquino- linium, mnta- -- maleonitriledithiolate) has been synthesized and structurally characterized by IR, ESI-MS and X-ray diffraction methods. Complex 1 is of triclinic, space group PI, with a = 9.079(2), b = 10.154(2), c = 11.243(2)A, α= 81.58(1), β= 69.63(1), γ = 68.02(1)°, V= 940.1(3)A3, Dc = 1.427 g/cm^3, Z = 1, F(000) = 418 and R = 0.0442. A 2D layer structure is formed via the cation-cation π…π and C-H…π interactions observed in the solid state of the complex.展开更多
Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine...Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine functionalized 3DCOF(3D-An-COF-F)formed by entangled 2D sql nets.The structure of 3D-An-COF-F was determined by the combination of continuous rotation electron diffraction technique and modelling based on the chemical information from real space.Interestingly,compared to the isostructural 3D-An-COF without F atom s,3DAn-COF-F showed an improved CO_(2)sorption ability and higher CO_(2)/N_(2)selectivity.Our study not only demonstrated the generality of constructing 3D COFs with entangled 2D nets by introducing bulky groups vertically in planar building blocks,but also will expand the diversity of 3D COFs for various applications.展开更多
Photodetectors operating in the shortwave infrared region are of great significance due to their extensive applications in both commercial and military fields.Narrowbandgap two-dimensional layered materials(2DLMs)are ...Photodetectors operating in the shortwave infrared region are of great significance due to their extensive applications in both commercial and military fields.Narrowbandgap two-dimensional layered materials(2DLMs)are considered as the promising candidates for constructing nextgeneration high-performance infrared photodetectors.Nevertheless,the performance of 2DLMs-based photodetectors can hardly satisfy the requirements of practical applications due to their weak optical absorption.In the present study,a strategy was proposed to design high-performance shortwave infrared photodetectors by integrating metalorganic frameworks(MOFs)nanoparticles with excellent optical absorption characteristics and 2DLM with high mobility.Further,this study demonstrated the practicability of this strategy in a MOF/2DLM(Ni-CAT-1/Bi_(2)Se_(3))hybrid heterojunction photodetector.Due to the transfer of photo-generated carriers from the MOF to Bi_(2)Se_(3),the MOF nanoparticles integrated on the Bi_(2)Se_(3) layer can increase the photocurrent by 2-3 orders of magnitude.The resulting photodetector presented a high responsivity of 4725 A W^(−1) and a superior detectivity of 3.5×10^(13) Jones at 1500 nm.The outstanding performance of the hybrid heterojunction arises from the synergistic function of the enhanced optical absorption and photogating effect.In addition,the proposed device construction strategy combining MOF photosensitive materials with 2DLMs shows a high potential for the future high-performance shortwave infrared photodetectors.展开更多
Two-dimensional layered material/semiconductor heterostructures have emerged as a category of fascinating architectures for developing highly efficient and low-cost photodetection devices.Herein,we present the constru...Two-dimensional layered material/semiconductor heterostructures have emerged as a category of fascinating architectures for developing highly efficient and low-cost photodetection devices.Herein,we present the construction of a highly efficient flexible light detector operating in the visible-near infrared wavelength regime by integrating a PdTe2 multilayer on a thin Si film.A representative device achieves a good photoresponse performance at zero bias including a sizeable current on/off ratio exceeding 105,a decent responsivity of~343 mA/W,a respectable specific detectivity of~2.56×10^(12)Jones,and a rapid response time of 4.5/379μs,under 730 nm light irradiation.The detector also displays an outstanding long-term air stability and operational durability.In addition,thanks to the excellent flexibility,the device can retain its prominent photodetection performance at various bending radii of curvature and upon hundreds of bending tests.Furthermore,the large responsivity and rapid response speed endow the photodetector with the ability to accurately probe heart rate,suggesting a possible application in the area of flexible and wearable health monitoring.展开更多
Two-dimensional(2D)layered silicon telluride(SizTes)nanocrystals were compressed to 12 GPa using diamond anvil cell techniques.Optical measurements show a color change from transparent red to opaque black indicating a...Two-dimensional(2D)layered silicon telluride(SizTes)nanocrystals were compressed to 12 GPa using diamond anvil cell techniques.Optical measurements show a color change from transparent red to opaque black indicating a semiconductor-to-metal phase transition.Raman scattering was used to observe the stiffening of the crystal lattice and subsequent phase behavior.A possible phase transition was observed.at 9.5±0.5 GPa evidenced by the disappearance of the Atg stretching mode.SizTes was intercalated with elemental manganese to^1 at.%.Intercalation lowers the pressure of the proposed phase transition to 7.5±1 GPa.Raman modes show both phonon stiffening and phonon softening,suggesting negative linear compressibility.These results provide fundamental insight into the high-pressure optical phonon behavior of silicon telluride and illuminate how a specific electron-donating intercalant can chemically alter pressure-dependent optical phonon behavior.展开更多
Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a...Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.展开更多
Thermoelectric technologies have caught our intense attention due to their ability of heat conversion into electricity.The considerable efforts have been taken to develop and enhance thermoelectric properties of mater...Thermoelectric technologies have caught our intense attention due to their ability of heat conversion into electricity.The considerable efforts have been taken to develop and enhance thermoelectric properties of materials over the past several decades.Recently,twodimensional layered materials are making the promise for potential applications of thermoelectric devices because of the excellent physical and structural properties.Here,a comprehensive coverage about recent progresses in thermoelectric properties of typical two dimensional(2D)layered materials,including the theoretical and experimental results,is provided.Moreover,the potential applications of 2D thermoelectric materials are also involved.These results indicate that the development of 2D thermoelectric materials take a key role in the flexible electronic devices with thermoelectric technologies.展开更多
A new zinc(Ⅱ) compound, [Zn(BTA)(UCA)]n (1, HBTA = 1,2,3-benzotriazole, HUCA = 4-imidazoleacrylic acid), has been synthesized via the hydrothermal reactions of Zn(OAC)2.2H20, HBTA and HUCA. The crystal stru...A new zinc(Ⅱ) compound, [Zn(BTA)(UCA)]n (1, HBTA = 1,2,3-benzotriazole, HUCA = 4-imidazoleacrylic acid), has been synthesized via the hydrothermal reactions of Zn(OAC)2.2H20, HBTA and HUCA. The crystal structure is of monoclinic, space group P21/c with a = 7.450(3), b = 18.911 (8), c = 9.198(4) A, fl = 94.317(8)°, V = 1292.2(9) A3, C12HgNsO2Zn, Mr = 320.63, Z = 4, Dc = 1.648 g/cm3, F(000) = 648,/z = 1.909 mm-1, R= 0.0255 and wR= 0.0655 for 2104 observed reflections (I 〉 2a(/)). Single-crystal X-ray diffraction analysis revealed that compound 1 features a two-dimensional (2D) layered framework based on benzotriazole controlled dinuclear [Zn2(BTA)2] subunits. Furthermore, these 2D layers are threaded into a 3D supramolecular framework via the direction of intermolecular hydrogen bonds and π-π interactions. In addition, the thermal stability and fluorescence property of compound 1 were also investigated.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
Lithium-ion capacitors(LICs) of achieving high power and energy density have garnered significant attention. However, the kinetics unbalance between anode and cathode can impede the application of LICs. Vanadium nitri...Lithium-ion capacitors(LICs) of achieving high power and energy density have garnered significant attention. However, the kinetics unbalance between anode and cathode can impede the application of LICs. Vanadium nitride(VN) with a high theoretical specific capacity(~ 1200 m Ah·g^(-1)) is a better pseudocapacitive anode to match the response of cathode in LICs. However, the insertion/extraction of Li-ions in VN's operation results in significant volume expansion. Herein, the VN/N-r GO-5composite that three-dimentional(3D) dicyandiamidederived-carbon(DDC) tightly wrapped VN quantum dots(VN QDTs) on two-dimentional(2D) reduced graphene oxid(r GO) was prepared by a facile strategy. The VN QDTs can reduce ion diffusion length and improve charge transfer kinetics. The 2D r GO as a template provides support for nanoparticle dispersion and improves electrical conductivity. The 3D DDC tightly encapsulated with VN QDTs mitigates agglomeration of VN particles as well as volume expansion. Correspondingly, the LICs with VN/Nr GO-5 composite as anode and activated carbon(AC) as cathode were fabricated, which exhibits a high energy density and power density. Such strategy provides a perspective for improving the electrochemical properties of LIC anode materials by suppressing volume expansion and enhancing conductivity.展开更多
The 2D-layer compound ([Na-2(C8H12N2O3)(4)(C2H6SO)(4)(W6O19)](n) 1, M-r = 2133.98) synthesized by the reaction of sodium tungstate and barbitone sodium in the solution of DMSO and water has been characterized by IR an...The 2D-layer compound ([Na-2(C8H12N2O3)(4)(C2H6SO)(4)(W6O19)](n) 1, M-r = 2133.98) synthesized by the reaction of sodium tungstate and barbitone sodium in the solution of DMSO and water has been characterized by IR and Raman spectra, elemental analysis and TGA. X-ray diffraction analysis indicates that Compound 1 crystallizes in the monoclinic system, space group C2/c with a 14.8026(4), b = 17.3012(3), c = 19.6379(5) A, beta = 98.6300 degrees, V = 4972.4(2) angstrom(3), Z = 4, F(000) 3928, D-c = 2.851 and mu = 14.101 mm(-1). 1 has a two-dimensional layer structure with hexapolyoxotungstate building blocks and coordinated sodium chains.展开更多
In this paper,we proposal stream surface and stream layer.By using classical tensor calculus,we derive 3-D Navier-Stokes Equations(NSE)in the stream layer under semigeodesic coordinate system,Navier-Stokes equation on...In this paper,we proposal stream surface and stream layer.By using classical tensor calculus,we derive 3-D Navier-Stokes Equations(NSE)in the stream layer under semigeodesic coordinate system,Navier-Stokes equation on the stream surface and 2-D Navier-Stokes equations on a two dimensional manifold. After introducing stream function on the stream surface,a nonlinear initial-boundary value problem satisfies by stream function is obtained,existence and uniqueness of its solution are proven.Based this theory we proposal a new method called"dimension split method"to solve 3D NSE.展开更多
The title compound, [Cu2(DMPz)2PMo12O40]·HDMPz (1, DMPz = 2,5-dimethyl pyrazine), has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in triclinic, space group...The title compound, [Cu2(DMPz)2PMo12O40]·HDMPz (1, DMPz = 2,5-dimethyl pyrazine), has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in triclinic, space group P1 with a = 11.075(2), b = 11.551(2), c = 11.886(2) A.α = 106.352(2), β = 109.862(3), γ = 109.504(1)°, V = 1206.8(3) A3, C18H26CU2Mo12N6O40P, Mr = 2275.78, Z = 1, Dc = 3.131 g/cm3, μ = 4.011 mm^-1, F(000) = 1073, S = 1.066, the final R = 0.0389 and wR = 0.1056 for 3739 observed reflections with I 〉 2σ(I). The structural analysis indicates that the title compound is composed of Keggin clusters [PMo12O40]3- connected by one-dimensional [CB(DMPz)]2n^2n+ chains to form a two-dimensional grid layer with holes occupied by monoprotonated DMPz molecules. In the solid of the title compound, the 2D grid layers are stacked together in an ABAB packing mode.展开更多
文摘The rapid recombination of photo-generated electron-hole pairs,insufficient active sites,and strong photocorrosion have considerably restricted the practical application of Cd S in photocatalytic fields.Herein,we designed and constructed a 2D/2D/2D layered heterojunction photocatalyst with cascaded 2D coupling interfaces.Experiments using electron spin resonance spectroscopy,ultraviolet photoelectron spectroscopy,and in-situ irradiation X-ray photoelectron spectroscopy were conducted to confirm the 2D layered CdS/WO_(3) step-scheme(S-scheme)heterojunctions and CdS/MX ohmic junctions.Impressively,it was found that the strong interfacial electric fields in the S-scheme heterojunction photocatalysts could effectively promote spatially directional charge separation and transport between CdS and WO_(3) nanosheets.In addition,2D Ti_(3)C_(2) MXene nanosheets with a smaller work function and excellent metal conductivity when used as a co-catalyst could build ohmic junctions with Cd S nanosheets,thus providing a greater number of electron transfer pathways and hydrogen evolution sites.Results showed that the highest visible-light hydrogen evolution rate of the optimized MX-Cd S/WO_(3) layered multi-heterostructures could reach as high as 27.5 mmol/g/h,which was 11.0 times higher than that of pure CdS nanosheets.Notably,the apparent quantum efficiency reached 12.0% at 450 nm.It is hoped that this study offers a reliable approach for developing multifunctional photocatalysts by integrating S-scheme and ohmic-junction built-in electric fields and rationally designing a 2D/2D interface for efficient light-to-hydrogen fuel production.
基金This work was supported by the NNSFC (No. 30460153 20561001), NSF of Guangxi Province (No. 0447019), and the Teaching and Research Award Program for Outstanding Young Teachers in Higher Education Institutions of Chinese Ministry of Education
文摘A new coordination polymer [Cd(bimc)2]n was obtained by the reaction of Hbimc with Cd(NO3) 2·4H2O in NaOH solution, and characterized by elemental analysis, IR and singlecrystal X-ray diffraction. The crystal belongs to orthorhombic, space group Pbcn with a = 12.533(4), b = 15.705(5), c = 15.200(5) A, V= 2991.8(15) A^3, Mr = 434.68, Z = 8, Dc = 1.930 g/cm^3, F(000) = 1712,μ(MoKa) = 1.492 mm^-1, the final R = 0.0410 and wR = 0.0804 for 1661 observed reflections (I 〉 2σ(I)). The Cd atom exhibits a distorted six-coordinate CdNzOa octahedral coordination geometry. The complex molecules are linked by both μ2-(η2-O, O^-), NI and μ2-(η2-O, O^-), N3 coordination modes of ligands to form cross-like wave (4, 4) layer structures which are further stacked through interlayer hydrogen bonds and π-π stacking interactions in an offset fashion to form a 3D supramolecular structure.
基金supported by the 973 Program (2007CB815301 and 2006CB932904)the National Natural Science Foundation of China (20333070, 20673118, 20871114)+1 种基金the Science Foundation of CAS (KJCX2-YW-M05)Fujian Province (2006L2005, 2006J0014, 2006F3132)
文摘A new thiostannate,[tmdpH2]Sn3S7 1(tmdp = 4,4'-trimethylenedipiperidine),has been synthesized under solvothermal conditions and characterized by elemental analysis,IR spectroscopy,and single-crystal X-ray diffraction analysis.In 1,the Sn3S4 secondary incomplete cubane-like building units are bridged by μ2-S atoms to form Sn12S12 rings which are then joined parallelly to the [001] plane,giving the final 2D(Sn3S7^2-)n layer of(6,3) network.The layers are stacked along the c axis so that 24-membered ring channels are generated,in which the organic cations are accommodated.The compound crystallizes in monoclinic,space group C2/c,with a=23.052(3),b=13.4039(12),c=18.412(2)A,β=120.112(4)°,V=4921.3(9)A^3,C13H28N2S7Sn3,Mr=792.86,Z=8,Dc=2.140 g/cm^3,F(000)=3056,μ=3.619 mm^-1,the final R=0.0488 and wR=0.1125 for 4607 observed reflections with I〉2σ(I).
基金the President's Science Foundation of South China Agricultural University (No. 2005K092)
文摘A new ion-pair complex, [BzMeQ1]2[Ni(nmt)2]1([BzMeQ1]^+ = 1-benzyl-4-ntethylquino- linium, mnta- -- maleonitriledithiolate) has been synthesized and structurally characterized by IR, ESI-MS and X-ray diffraction methods. Complex 1 is of triclinic, space group PI, with a = 9.079(2), b = 10.154(2), c = 11.243(2)A, α= 81.58(1), β= 69.63(1), γ = 68.02(1)°, V= 940.1(3)A3, Dc = 1.427 g/cm^3, Z = 1, F(000) = 418 and R = 0.0442. A 2D layer structure is formed via the cation-cation π…π and C-H…π interactions observed in the solid state of the complex.
基金financially supported by the National Natural Science Foundation of China(Nos.22225503,U21A20285 and 22375153)the Hubei Provincial Natural Science Foundation of China(No.2023AFA011)the Fundamental Research Funds for Central Universities(No.2042023kf0127)。
文摘Constructing three dimensional(3D)covalent organic frameworks(COFs)through the entanglement of two dimensional(2D)nets is a promising but underdeveloped strategy.Herein,we report the design and synthesis of a fluorine functionalized 3DCOF(3D-An-COF-F)formed by entangled 2D sql nets.The structure of 3D-An-COF-F was determined by the combination of continuous rotation electron diffraction technique and modelling based on the chemical information from real space.Interestingly,compared to the isostructural 3D-An-COF without F atom s,3DAn-COF-F showed an improved CO_(2)sorption ability and higher CO_(2)/N_(2)selectivity.Our study not only demonstrated the generality of constructing 3D COFs with entangled 2D nets by introducing bulky groups vertically in planar building blocks,but also will expand the diversity of 3D COFs for various applications.
基金supported by the National Natural Science Foundation of China(21825103 and 51727809)the Natural Science Foundation of Hubei Province(2019CFA002)+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyXMBZ018)China Postdoctoral Science Foundation(2021M691108)。
文摘Photodetectors operating in the shortwave infrared region are of great significance due to their extensive applications in both commercial and military fields.Narrowbandgap two-dimensional layered materials(2DLMs)are considered as the promising candidates for constructing nextgeneration high-performance infrared photodetectors.Nevertheless,the performance of 2DLMs-based photodetectors can hardly satisfy the requirements of practical applications due to their weak optical absorption.In the present study,a strategy was proposed to design high-performance shortwave infrared photodetectors by integrating metalorganic frameworks(MOFs)nanoparticles with excellent optical absorption characteristics and 2DLM with high mobility.Further,this study demonstrated the practicability of this strategy in a MOF/2DLM(Ni-CAT-1/Bi_(2)Se_(3))hybrid heterojunction photodetector.Due to the transfer of photo-generated carriers from the MOF to Bi_(2)Se_(3),the MOF nanoparticles integrated on the Bi_(2)Se_(3) layer can increase the photocurrent by 2-3 orders of magnitude.The resulting photodetector presented a high responsivity of 4725 A W^(−1) and a superior detectivity of 3.5×10^(13) Jones at 1500 nm.The outstanding performance of the hybrid heterojunction arises from the synergistic function of the enhanced optical absorption and photogating effect.In addition,the proposed device construction strategy combining MOF photosensitive materials with 2DLMs shows a high potential for the future high-performance shortwave infrared photodetectors.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.62275002,51902078,62074048,62075053)the Anhui Provincial Natural Science Foundation(2008085MF205)the Fundamental Research Funds for the Central Universities(JZ2020HGTB0051,PA2020GDKC0024).
文摘Two-dimensional layered material/semiconductor heterostructures have emerged as a category of fascinating architectures for developing highly efficient and low-cost photodetection devices.Herein,we present the construction of a highly efficient flexible light detector operating in the visible-near infrared wavelength regime by integrating a PdTe2 multilayer on a thin Si film.A representative device achieves a good photoresponse performance at zero bias including a sizeable current on/off ratio exceeding 105,a decent responsivity of~343 mA/W,a respectable specific detectivity of~2.56×10^(12)Jones,and a rapid response time of 4.5/379μs,under 730 nm light irradiation.The detector also displays an outstanding long-term air stability and operational durability.In addition,thanks to the excellent flexibility,the device can retain its prominent photodetection performance at various bending radii of curvature and upon hundreds of bending tests.Furthermore,the large responsivity and rapid response speed endow the photodetector with the ability to accurately probe heart rate,suggesting a possible application in the area of flexible and wearable health monitoring.
文摘Two-dimensional(2D)layered silicon telluride(SizTes)nanocrystals were compressed to 12 GPa using diamond anvil cell techniques.Optical measurements show a color change from transparent red to opaque black indicating a semiconductor-to-metal phase transition.Raman scattering was used to observe the stiffening of the crystal lattice and subsequent phase behavior.A possible phase transition was observed.at 9.5±0.5 GPa evidenced by the disappearance of the Atg stretching mode.SizTes was intercalated with elemental manganese to^1 at.%.Intercalation lowers the pressure of the proposed phase transition to 7.5±1 GPa.Raman modes show both phonon stiffening and phonon softening,suggesting negative linear compressibility.These results provide fundamental insight into the high-pressure optical phonon behavior of silicon telluride and illuminate how a specific electron-donating intercalant can chemically alter pressure-dependent optical phonon behavior.
基金the support from the National Natural Science Foundation of China(21878271,51702284,21878270,and 21961160742)the Zhejiang Provincial Natural Science Foundation of China(LR19B060002)+8 种基金the Fundamental Research Funds for the Central Universitiesthe Startup Foundation for Hundred-Talent Program of Zhejiang Universitythe Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(2019R01006)Key Laboratory of Marine Materials and Related Technologies,CASZhejiang Key Laboratory of Marine Materials and Protective Technologies(2020K10)the support of the NSFC 21501138the Natural Science Foundation of Hubei Province(2019CFB556)Science Research Foundation of Wuhan Institute of Technology(K2019039)the Australian Research Council(ARC)and QUT Centre for Materials Science for partial support.
文摘Solar-driven photoelectrochemical(PEC)water splitting systems are highly promising for converting solar energy into clean and sustainable chemical energy.In such PEC systems,an integrated photoelectrode incorporates a light harvester for absorbing solar energy,an interlayer for transporting photogenerated charge carriers,and a co-catalyst for triggering redox reactions.Thus,understanding the correlations between the intrinsic structural properties and functions of the photoelectrodes is crucial.Here we critically examine various 2D layered photoanodes/photocathodes,including graphitic carbon nitrides,transition metal dichalcogenides,layered double hydroxides,layered bismuth oxyhalide nanosheets,and MXenes,combined with advanced nanocarbons(carbon dots,carbon nanotubes,graphene,and graphdiyne)as co-catalysts to assemble integrated photoelectrodes for oxygen evolution/hydrogen evolution reactions.The fundamental principles of PEC water splitting and physicochemical properties of photoelectrodes and the associated catalytic reactions are analyzed.Elaborate strategies for the assembly of 2D photoelectrodes with nanocarbons to enhance the PEC performances are introduced.The mechanisms of interplay of 2D photoelectrodes and nanocarbon co-catalysts are further discussed.The challenges and opportunities in the field are identified to guide future research for maximizing the conversion efficiency of PEC water splitting.
基金Thanks for the support of the National Key R&D Program of China under Grant No.2016YFA0200400 and the National Natural Science Foundation of China under Grant No.51627805。
文摘Thermoelectric technologies have caught our intense attention due to their ability of heat conversion into electricity.The considerable efforts have been taken to develop and enhance thermoelectric properties of materials over the past several decades.Recently,twodimensional layered materials are making the promise for potential applications of thermoelectric devices because of the excellent physical and structural properties.Here,a comprehensive coverage about recent progresses in thermoelectric properties of typical two dimensional(2D)layered materials,including the theoretical and experimental results,is provided.Moreover,the potential applications of 2D thermoelectric materials are also involved.These results indicate that the development of 2D thermoelectric materials take a key role in the flexible electronic devices with thermoelectric technologies.
基金Supported by the 973 Program of China(2011CBA00505)the"Strategic Priority Research Program"of the Chinese Academy of Sciences(XDA07070200,XDA09030102)the Science Foundation of Fujian Province(2006L2005)
文摘A new zinc(Ⅱ) compound, [Zn(BTA)(UCA)]n (1, HBTA = 1,2,3-benzotriazole, HUCA = 4-imidazoleacrylic acid), has been synthesized via the hydrothermal reactions of Zn(OAC)2.2H20, HBTA and HUCA. The crystal structure is of monoclinic, space group P21/c with a = 7.450(3), b = 18.911 (8), c = 9.198(4) A, fl = 94.317(8)°, V = 1292.2(9) A3, C12HgNsO2Zn, Mr = 320.63, Z = 4, Dc = 1.648 g/cm3, F(000) = 648,/z = 1.909 mm-1, R= 0.0255 and wR= 0.0655 for 2104 observed reflections (I 〉 2a(/)). Single-crystal X-ray diffraction analysis revealed that compound 1 features a two-dimensional (2D) layered framework based on benzotriazole controlled dinuclear [Zn2(BTA)2] subunits. Furthermore, these 2D layers are threaded into a 3D supramolecular framework via the direction of intermolecular hydrogen bonds and π-π interactions. In addition, the thermal stability and fluorescence property of compound 1 were also investigated.
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financially supported by the National Natural Science Foundation of China (Nos.22005167 and 21905152)Shandong Provincial Natural Science Foundation of China (Nos.ZR2020QB125, ZR2020MB045 and ZR2022QE003)+2 种基金China Postdoctoral Science Foundation (Nos.2021M693256, 2021T140687 and 2022M713249)Qingdao Postdoctoral Applied Research Project, Taishan Scholar Project of Shandong Province of China (No.tsqn202211160)the Youth Innovation Team Project for Talent Introduction and Cultivation in Universities of Shandong Province。
文摘Lithium-ion capacitors(LICs) of achieving high power and energy density have garnered significant attention. However, the kinetics unbalance between anode and cathode can impede the application of LICs. Vanadium nitride(VN) with a high theoretical specific capacity(~ 1200 m Ah·g^(-1)) is a better pseudocapacitive anode to match the response of cathode in LICs. However, the insertion/extraction of Li-ions in VN's operation results in significant volume expansion. Herein, the VN/N-r GO-5composite that three-dimentional(3D) dicyandiamidederived-carbon(DDC) tightly wrapped VN quantum dots(VN QDTs) on two-dimentional(2D) reduced graphene oxid(r GO) was prepared by a facile strategy. The VN QDTs can reduce ion diffusion length and improve charge transfer kinetics. The 2D r GO as a template provides support for nanoparticle dispersion and improves electrical conductivity. The 3D DDC tightly encapsulated with VN QDTs mitigates agglomeration of VN particles as well as volume expansion. Correspondingly, the LICs with VN/Nr GO-5 composite as anode and activated carbon(AC) as cathode were fabricated, which exhibits a high energy density and power density. Such strategy provides a perspective for improving the electrochemical properties of LIC anode materials by suppressing volume expansion and enhancing conductivity.
基金The project was supported by the 973 program of the MOST (001CB108906), the National Natural Science Foundation of China (20425313, 20333070 and 20303021), the Natural Science Foundation of Fujian Province, the Chinese Academy of Sciences and Fujian University of Technology (GY-Z0321)
文摘The 2D-layer compound ([Na-2(C8H12N2O3)(4)(C2H6SO)(4)(W6O19)](n) 1, M-r = 2133.98) synthesized by the reaction of sodium tungstate and barbitone sodium in the solution of DMSO and water has been characterized by IR and Raman spectra, elemental analysis and TGA. X-ray diffraction analysis indicates that Compound 1 crystallizes in the monoclinic system, space group C2/c with a 14.8026(4), b = 17.3012(3), c = 19.6379(5) A, beta = 98.6300 degrees, V = 4972.4(2) angstrom(3), Z = 4, F(000) 3928, D-c = 2.851 and mu = 14.101 mm(-1). 1 has a two-dimensional layer structure with hexapolyoxotungstate building blocks and coordinated sodium chains.
文摘In this paper,we proposal stream surface and stream layer.By using classical tensor calculus,we derive 3-D Navier-Stokes Equations(NSE)in the stream layer under semigeodesic coordinate system,Navier-Stokes equation on the stream surface and 2-D Navier-Stokes equations on a two dimensional manifold. After introducing stream function on the stream surface,a nonlinear initial-boundary value problem satisfies by stream function is obtained,existence and uniqueness of its solution are proven.Based this theory we proposal a new method called"dimension split method"to solve 3D NSE.
基金supported by the Natural Science Foundation of Fujian Province (2006F3135,2006F3141,2007HZ0001-1)the Fund of Fujian Key Laboratory of Nanomaterials (2006L2005)
文摘The title compound, [Cu2(DMPz)2PMo12O40]·HDMPz (1, DMPz = 2,5-dimethyl pyrazine), has been synthesized and characterized by single-crystal X-ray diffraction analysis. It crystallizes in triclinic, space group P1 with a = 11.075(2), b = 11.551(2), c = 11.886(2) A.α = 106.352(2), β = 109.862(3), γ = 109.504(1)°, V = 1206.8(3) A3, C18H26CU2Mo12N6O40P, Mr = 2275.78, Z = 1, Dc = 3.131 g/cm3, μ = 4.011 mm^-1, F(000) = 1073, S = 1.066, the final R = 0.0389 and wR = 0.1056 for 3739 observed reflections with I 〉 2σ(I). The structural analysis indicates that the title compound is composed of Keggin clusters [PMo12O40]3- connected by one-dimensional [CB(DMPz)]2n^2n+ chains to form a two-dimensional grid layer with holes occupied by monoprotonated DMPz molecules. In the solid of the title compound, the 2D grid layers are stacked together in an ABAB packing mode.