As a representative transition metal dichalcogenides(TMD),NiTe_(2)has an ultra-fast optical response,high carrier mobility,and excellent environmental stability.It has a broad application prospect in the fields of ene...As a representative transition metal dichalcogenides(TMD),NiTe_(2)has an ultra-fast optical response,high carrier mobility,and excellent environmental stability.It has a broad application prospect in the fields of ener-gy,biomedicine,optoelectronic devices,and so on.At present,there have been scant reports on the application of NiTe_(2)in the field of ultrafast photonics.In this work,NiTe_(2)was synthesized by chemical vapor deposition(CVD)and integrated with a tapered optical fiber to achieve mode-locking in an erbium-doped fiber laser(EDFL)and a thu-lium-doped fiber laser(TDFL).The mode-locked EDFL exhibited a pulse width of 678 fs and an output power of 3.92 mW.The pulse width of mode-locked TDFL was estimated to have a pulse width of 694 fs with an output power of 21.64 mW.These results demonstrate that NiTe_(2)is an effective saturable absorber material with potential applica-tions in the field of ultrafast optics.展开更多
Copper is a versatile material,commonly utilized in power transmission and electronic devices,but its relative high reactivity necessitates a long-lasting protective technique.Here,we report a method that combines pla...Copper is a versatile material,commonly utilized in power transmission and electronic devices,but its relative high reactivity necessitates a long-lasting protective technique.Here,we report a method that combines plasma-enhanced non-equilibrium magnetron sputtering physical vapor deposition(PEUMS-PVD)and anodization to construct a self-healing three-dimensional Ti/Al-doped TiO_(2)nanotubes/Ti_(3)AlC_(2)coating on the surface of Cu substrates.This novel strategy enhances the corrosion resistance of copper substrates in marine environments,with corrosion current densities of up to 4.5643×10^(−8)A/cm^(2).Among them,the doping of nano-aluminum particles makes the coating self-healing.The mechanistic analysis of the corrosion behaviors during early immersion experiments was conducted using electrochemical noise,and revealed that during the initial stages of coating immersion,uniform corrosion predominates,with a minor occurrence of localized corrosion.展开更多
We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generate...We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generated from 65330 CCSD(T)-F12a/aug-cc-pVTZ ab initio data points,with counterpoise correction,applied to eliminate basis set superposition error(BSSE).We performed quasi-classical trajectory simulations using this PES to investigate the rotational energy transfer dynamics.Our results reveal complex energy transfer mechanisms,with significant rotational excitation and relaxation dependent on collision energy and initial rotational states.The 9D PES provides a more accurate representation of the CO_(2)-CO system,offering new insights into molecular dynamics and interaction mechanisms.展开更多
Two-dimensional energetic materials(2DEMs),characterized by their exceptional interlayer sliding properties,are recognized as exemplar of low-sensitivity energetic materials.However,the diversity of available 2DEMs is...Two-dimensional energetic materials(2DEMs),characterized by their exceptional interlayer sliding properties,are recognized as exemplar of low-sensitivity energetic materials.However,the diversity of available 2DEMs is severely constrained by the absence of efficient methods for rapidly predicting crystal packing modes from molecular structures,impeding the high-throughput rational design of such materials.In this study,we employed quantified indicators,such as hydrogen bond dimension and maximum planar separation,to quickly screen 172DEM and 16 non-2DEM crystal structures from a crystal database.They were subsequently compared and analyzed,focusing on hydrogen bond donor-acceptor combinations,skeleton features,and intermolecular interactions.Our findings suggest that theπ-πpacking interaction energy is a key determinant in the formation of layered packing modes by planar energetic molecules,with its magnitude primarily influenced by the strongest dimericπ-πinteraction(π-π2max).Consequently,we have delineated a critical threshold forπ-π2max to discern layered packing modes and formulated a theoretical model for predictingπ-π2max,grounded in molecular electrostatic potential and dipole moment analysis.The predictive efficacy of this model was substantiated through external validation on a test set comprising 31 planar energetic molecular crystals,achieving an accuracy of 84%and a recall of 75%.Furthermore,the proposed model shows superior classification predictive performance compared to typical machine learning methods,such as random forest,on the external validation samples.This contribution introduces a novel methodology for the identification of crystal packing modes in 2DEMs,potentially accelerating the design and synthesis of high-energy,low-sensitivity 2DEMs.展开更多
Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key appr...Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key approach to unlocking this potential.In this work,we construct a two-dimensional/twodimensional(2D/2D)FeSe_(2)/protonated carbon nitride(FeSe_(2)/PCN)heterostructure to promote the interfacial charge transfer dynamics,leading to a four-fold improved conversion efficiency of photocatalytic CO_(2)reduction with near 100%CO selectivity.Combining in situ X-ray photoelectron spectroscopy,in situ soft X-ray absorption spectroscopy,and femtosecond transient absorption spectroscopy,it is revealed that FeSe_(2)acts as an electron acceptor upon photoexcitation,introducing an additional electron transfer pathway from PCN to FeSe_(2)that suppresses radiative recombination and promotes charge transfer.In situ X-ray absorption fine structure spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy,and density functional theory calculation further unravel that the electron-enriched FeSe_(2)functions as the active sites for CO_(2)activation and significantly reduces the energy barrier of key intermediate COOH*formation,which is the rate-determined step for CO generation.This work underscores the importance of regulating photocarrier relaxation pathways to achieve effective spatial charge separation for promoted photocatalytic CO_(2)reduction and demonstrates the powerful functions of in situ spectroscopies in in-depth understanding of the photocatalytic mechanism.展开更多
With high surface-to-volume ratio,the abundant surface states and high carrier concentration are challenging the nearinfrared photodetection behaviors of narrow band gap semiconductors nanowires.In this study,the narr...With high surface-to-volume ratio,the abundant surface states and high carrier concentration are challenging the nearinfrared photodetection behaviors of narrow band gap semiconductors nanowires.In this study,the narrow band gap semiconductor of Bi_(2)O_(2)Se nanosheets(NSs)is adopted to construct mixed-dimensional heterojunctions with GaSb nanowires(NWs)for demonstrating the impressive self-powered NIR photodetection.Benefiting from the built-in electric field of~140 meV,the as-constructed NW/NS mixeddimensional heterojunction self-powered photodetector shows the low dark current of 0.07 pA,high I_(light)/I_(dark)ratio of 82 and fast response times of<2/2 ms at room temperature.The self-powered photodetector performance can be further enhanced by fabricating the NW array/NS mixed-dimensional heterojunction by using a contact printing technique.The excellent photodetection performance promises the asconstructed NW/NS mixed-dimensional heterojunction self-powered photodetector in imaging and photocommunication.展开更多
The single-layer Ti_(3)C_(2)T_(x)/MXene has become a special electromagnetic wave absorber near the terahertz band because of its abundant surface groups and excellent conductivity.However,the macro-preparation of sin...The single-layer Ti_(3)C_(2)T_(x)/MXene has become a special electromagnetic wave absorber near the terahertz band because of its abundant surface groups and excellent conductivity.However,the macro-preparation of single-layer Ti_(3)C_(2)T_(x)/MXene shows significantly difficult to influence its application.The two-dimensional Ti_(3)C_(2)T_(x)is easily prepared to have high production,but its weak absorption ability due to high surface conductivity also restricts its application.To realize the strong electromagnetic wave absorption of two-dimensional Ti_(3)C_(2)T_(x)/MXene,a new strategy with magnetic FeNi nanoparticles decorating Ti_(3)C_(2)T_(x)/MXene composites(FeNi-Ti_(3)C_(2)T_(x))were proposed and the effective electromagnetic wave absorption features covering 170-220 GHz that means the absorption band width reach 50 GHz.With an absorber composite film thickness being only 0.6 mm,the absorptivity of the composite is enhanced with the increase of decorating FeNi nanoparticles and promote up to 75%when the FeNi nanoparticles loading content reaches 30 wt%.The improvement of absorption is attributed to the introduction of soft magnetic FeNi to adjust the high surface conductivity of MXene and improve the electromagnetic balance of the absorber.展开更多
Microplastics(MPs)are ubiquitous in the environment,continuously undergo aging processes and release toxic chemical substances.Understanding the environmental behaviors of MPs is critical to accurately evaluate their ...Microplastics(MPs)are ubiquitous in the environment,continuously undergo aging processes and release toxic chemical substances.Understanding the environmental behaviors of MPs is critical to accurately evaluate their long-term ecological risk.Generalized twodimensional correlation spectroscopy(2D-COS)is a powerful tool for MPs studies,which can dig more comprehensive information hiding in the conventional one-dimensional spectra,such as infrared(IR)and Raman spectra.The recent applications of 2D-COS in analyzing the behaviors and fates of MPs in the environment,including their aging processes,and interactions with natural organicmatter(NOM)or other chemical substances,were summarized systematically.The main requirements and limitations of current approaches for exploring these processes are discussed,and the corresponding strategies to address these limitations and drawbacks are proposed as well.Finally,new trends of 2D-COS are prospected for analyzing the properties and behaviors of MPs in both natural and artificial environmental processes.展开更多
We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-o...We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.展开更多
The size effects were experimentally investigated and the underlying mechanism was analyzed.The results reveal that,as the specimen size increases,the interconnectivity of macropores slightly decreases.This in turn co...The size effects were experimentally investigated and the underlying mechanism was analyzed.The results reveal that,as the specimen size increases,the interconnectivity of macropores slightly decreases.This in turn constrains the diffusion of CO_(2) and moisture in the specimens,resulting in an increase in the discrepancy between the internal and external carbonation degrees.An increase in cement paste thickness simultaneously decreases the quantity,average size,and interconnectivity of macropores,lowering the diffusion efficacy of CO_(2) and moisture and exacerbating the overall heterogeneity in carbonation.Moreover,the gradual blockage of macropores leads to the emergence of localized ‘occluded zones’ with much lower carbonation degree.The reduction in aggregate size significantly alters the average diameter and connectivity of macropores,leading to notable change to overall non-uniformity.This study provides insight into improving the CO_(2) curing effect of pervious concrete products and developing uniform curing methods.展开更多
Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),Cr...Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),CrS_(2)with one S vacancy(v-CrS_(2)), and Ti doped CrS_(2)(Ti@CrS_(2)). The results have shown that the pristine CrS_(2)exhibits inert character for NO activation. However, v-CrS_(2)and Ti@CrS_(2)can exhibit enhanced interaction with NO, due to increased charge transfer between NO and substrates(0.52–0.75 e) and enhanced adsorption energies of NO on the catalysts(-0.96~-1.64 e V), compared to the situation of CrS_(2)(0.065 e/-0.30 e V). From the free energy profiles of NO electro-reduction to NH3, we can see that the v-CrS_(2)and Ti@CrS_(2)all exhibit ultralow limiting potentials of-0.03~-0.47 V, following both*NOH and*NHO mechanisms. Therefore, introducing vacancy and doping are all promising modification strategies for NORR catalysts. The results have provided a new idea for the search of catalysts for efficient electrocatalytic reduction of NO.展开更多
Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can prov...Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can provide additional momentum and influence the scat-tering process involving one or two phonons,only the idealized defects without any structural details are considered in tra-ditional DRR theory.Here,the second-order DRR spectra of WSe_(2) monolayer with different types of defects are calculated involving the combinations of acoustic and optical phonons in the vicinity of K(K')and M points of the Brillouin zone.The electronic band structures are modified due to the presence of defects,and the band unfolding method is adopted to show the bending of valence and conduction bands for the defective WSe_(2) monolayers.The associ-ated phononic band structures also exhibit different changes in phonon dispersion curves,re-sulting in different DRR spectra corresponding to the different types of defects in the WSe_(2) monolayers.For example,the existence of W vacancy in the WSe_(2) monolayer would result in downshifts in vibrational frequencies and asymmetrical broadenings in linewidths for most combination modes due to the dramatic changes in contour shape of electronic valleys at K and K'.Moreover,the scattering from K to Q is found to be forbidden for the two Se vacan-cies because of the elevation of conduction band at the Q point.Our work highlights the role of defect structures in the intervalley scattering and may provide better understanding in the underlying physics of DRR process in 2D materials.展开更多
Three-dimensional(3D)covalent organic frameworks(COFs)have attracted extensive attention as photocatalysts for CO_(2)reduction reactions.Introducing metal atoms is essential for enhancing activity,but previous metal s...Three-dimensional(3D)covalent organic frameworks(COFs)have attracted extensive attention as photocatalysts for CO_(2)reduction reactions.Introducing metal atoms is essential for enhancing activity,but previous metal sites in 3D COFs predominantly exhibit symmetrical coordination,making them unsuitable for CO_(2)activation.Here,we design a 3D COF with 2,2'-pyridine linked around tetra-(4-anilyl)methane(TCM-Bpy-COF),where Co^(2+)is asymmetrically coordinated by bipyridine and acetates(TCMBpy-COF-CoAc).The TCM-Bpy-COF-CoAc exhibits outstanding photocatalytic CO_(2)reduction performance under weak visible light,achieving a CO evolution rate of 26,650μmol g^(-1)h^(-1)under 5 W of lightemitting-diode(LED)lamp and high apparent quantum efficiency.The performance far exceeds that of symmetrically coordinated bipyridine-Co-bipyridine TCM-Bpy-COF and surpasses most reported COF-based photocatalysts.In-situ spectral characterizations and theoretical calculations show that asymmetric N,O-coordination around the Co^(2+)center polarizes electron density and lowers reaction energy barriers of^(*)COOH intermediates,enhancing the conversion of CO_(2)to CO.This work inspires the design of 3D COF-based photocatalysts with highly catalytic efficiency.展开更多
Ordered NiCo_(2)O_(4)/rGO nanowire arrays(NWAs)grown on a Ni foam substrate were synthesized using a template-free hydrothermal method and employed as an electrode with outstanding electrochemical properties for super...Ordered NiCo_(2)O_(4)/rGO nanowire arrays(NWAs)grown on a Ni foam substrate were synthesized using a template-free hydrothermal method and employed as an electrode with outstanding electrochemical properties for supercapacitors.After conducting a series of time-variable controlled experiments,the structure,morphology,and electrochemical properties of NiCo_(2)O_(4)/rGO NWAs were analyzed to find the most suitable growth time.Benefited from such unique array architectures,the designed NiCo_(2)O_(4)/rGO NWAs electrode demonstrates significant electrochemical properties,showing a specific capacitance of 2418 F·g^(-1)at a charge-discharge current density of 1 A·g^(-1).Moreover,it demonstrates exceptional stability,maintaining a capacity retention of 81.5%after undergoing 2,000 cycles,even when subjected to a current density of 10 A·g^(-1).The reason of high stability is that the spacing between the nanowire arrays is large and the diffusion resistance of the electrolyte is significantly reduced,which facilitates the diffusion of the electrolyte into the interior of the electrodes and establishes an effective contact with the surface of the nanowires.Furthermore,the NiCo_(2)O_(4)/rGO nanowire array grows directly on the Ni foam without binder,which establishes rapid electron transport pathways on the Ni foam substrate,resulting in excellent electrochemical properties.展开更多
In this paper,we investigate the(2+1)-dimensional three-component long-wave-short-wave resonance interaction system,which describes complex systems and nonlinear wave phenomena in physics.By employing the Hirota bilin...In this paper,we investigate the(2+1)-dimensional three-component long-wave-short-wave resonance interaction system,which describes complex systems and nonlinear wave phenomena in physics.By employing the Hirota bilinear method,we derive the general nondegenerate N-soliton solution of the system,where each short-wave component contains N arbitrary functions of the independent variable y.The presence of these arbitrary functions in the analytical solution enables the construction of a wide range of nondegenerate soliton types.Finally,we illustrate the structural features of several novel nondegenerate solitons,including M-shaped,multiple double-hump,and sawtooth double-striped solitons,as well as interactions between nondegenerate solitons,such as dromion-like solitons and solitoffs,with the aid of figures.展开更多
Based on the unique catalytic properties of precious metals,the introduction of precious metals into metal oxide semiconductors will greatly improve the gas-sensitive properties of materials.As a new type of porous ma...Based on the unique catalytic properties of precious metals,the introduction of precious metals into metal oxide semiconductors will greatly improve the gas-sensitive properties of materials.As a new type of porous material,metal–organic frameworks(MOF)can be used for gas separation and adsorption due to their adjustable pore size and acceptable thermal stability.In this work,the ZIF-71 MOF was synthesized on CuO nanofibers doped with different concentrations of Ru to form a Ru–CuO@ZIF-71 nanocomposite sensor,which was then used for H_(2)S detection.The sensor shows sensitivity to trace amounts of H_(2)S gas(100 ppb),and the response is greatly enhanced at the optimal Ru doping ratio and operating temperature.The introduction of the ZIF-71 membrane can significantly increase the selectivity of the sensor while further improving the sensitivity.Finally,the possible sensing mechanism of the Ru–CuO@ZIF-71 sensor was explored.The enhancement of the H_(2)S gas sensing properties may be attributed to the catalysis of Ru and the formation of the Schottky junction at the Ru–CuO interface.Besides,the calculation based on density functional theory reveals enhanced adsorption capacities of CuO for H_(2)S after Ru doping.Therefore,the Ru–CuO@ZIF-71 sensor has strong application potential in exhaled gas detection and portable detection of H_(2)S gas in industrial environments.展开更多
In this work,we study wave state transitions of the(2+1)-dimensional Kortewegde Vries-Sawada-Kotera-Ramani(2KdVSKR)equation by analyzing the characteristic line and phase shift.By converting the wave parameters of the...In this work,we study wave state transitions of the(2+1)-dimensional Kortewegde Vries-Sawada-Kotera-Ramani(2KdVSKR)equation by analyzing the characteristic line and phase shift.By converting the wave parameters of the N-soliton solution into complex numbers,the breath wave solution is constructed.The lump wave solution is derived through the long wave limit method.Then,by choosing appropriate parameter values,we acquire a number of transformed nonlinear waves whose gradient relation is discussed according to the ratio of the wave parameters.Furthermore,we reveal transition mechanisms of the waves by exploring the nonlinear superposition of the solitary and periodic wave components.Subsequently,locality,oscillation properties and evolutionary phenomenon of the transformed waves are presented.And we also prove the change in the geometrical properties of the characteristic lines leads to the phenomena of wave evolution.Finally,for higher-order waves,a range of interaction models are depicted along with their evolutionary phenomena.And we demonstrate that their diversity is due to the fact that the solitary and periodic wave components produce different phase shifts caused by time evolution and collisions.展开更多
Subsurface rocks,as complex porous media,exhibit multiscale pore structures and intricate physical properties.Digital rock physics technology has become increasingly influential in the study of subsurface rock propert...Subsurface rocks,as complex porous media,exhibit multiscale pore structures and intricate physical properties.Digital rock physics technology has become increasingly influential in the study of subsurface rock properties.Given the multiscale characteristics of rock pore structures,direct three-dimensional imaging at sub-micrometer and nanometer scales is typically infeasible.This study introduces a method for reconstructing porous media using multidimensional data,which combines one-dimensional pore structure parameters with two-dimensional images to reconstruct three-dimensional models.The pore network model(PNM)is stochastically reconstructed using one-dimensional parameters,and a generative adversarial network(GAN)is utilized to equip the PNM with pore morphologies derived from two-dimensional images.The digital rocks generated by this method possess excellent controllability.Using Berea sandstone and Grosmont carbonate samples,we performed digital rock reconstructions based on PNM extracted by the maximum ball algorithm and compared them with stochastically reconstructed PNM.Pore structure parameters,permeability,and formation factors were calculated.The results show that the generated samples exhibit good consistency with real samples in terms of pore morphology,pore structure,and physical properties.Furthermore,our method effectively supplements the micropores not captured in CT images,demonstrating its potential in multiscale carbonate samples.Thus,the proposed reconstruction method is promising for advancing porous media property research.展开更多
Recently, during the investigations on planetary oceans, Hirota-Satsuma-Ito-type models have been developed. In this paper, for a(2+1)-dimensional generalized variable-coefficient Hirota-Satsuma-Ito system describing ...Recently, during the investigations on planetary oceans, Hirota-Satsuma-Ito-type models have been developed. In this paper, for a(2+1)-dimensional generalized variable-coefficient Hirota-Satsuma-Ito system describing the fluid dynamics of shallow-water waves in an open ocean, non-characteristic movable singular manifold and symbolic computation enable an oceanic auto-B?cklund transformation with three sets of the oceanic solitonic solutions. The results rely on the oceanic variable coefficients in that system. Future oceanic observations might detect some nonlinear features predicted in this paper, and relevant oceanographic insights might be expected.展开更多
A series of Al-Ti-B master alloys were prepared by different preparation routes,and the TiB2 particles in the master alloys were extracted and analyzed.It is found that the forming process has significant influence on...A series of Al-Ti-B master alloys were prepared by different preparation routes,and the TiB2 particles in the master alloys were extracted and analyzed.It is found that the forming process has significant influence on the three-dimensional morphology of TiB2 particles.Different preparation routes result in different reaction forms,which accounts for the morphology variation of TiB2 particles.When the Al-Ti-B master alloy is prepared using ＂halide salt＂ route,TiB2 particles exhibit hexagonal platelet morphology and are independent with each other.In addition,the reaction temperature almost does not have influence on the morphology of TiB2 particles.However,TiB2 particles exhibit different morphologies at different reaction temperatures when the master alloys are prepared with Al-3B and Ti sponge.When the master alloy is prepared at 850 ℃,a kind of TiB2 particle agglomeration forms with a size larger than 5 μm.The TiB2 particles change to layered stacking morphology even dendritic morphology with the reaction temperature reaching up to 1200 ℃.展开更多
基金Supported by Guangdong Basic and Applied Basic Research Fund,China(2024A1515012429)。
文摘As a representative transition metal dichalcogenides(TMD),NiTe_(2)has an ultra-fast optical response,high carrier mobility,and excellent environmental stability.It has a broad application prospect in the fields of ener-gy,biomedicine,optoelectronic devices,and so on.At present,there have been scant reports on the application of NiTe_(2)in the field of ultrafast photonics.In this work,NiTe_(2)was synthesized by chemical vapor deposition(CVD)and integrated with a tapered optical fiber to achieve mode-locking in an erbium-doped fiber laser(EDFL)and a thu-lium-doped fiber laser(TDFL).The mode-locked EDFL exhibited a pulse width of 678 fs and an output power of 3.92 mW.The pulse width of mode-locked TDFL was estimated to have a pulse width of 694 fs with an output power of 21.64 mW.These results demonstrate that NiTe_(2)is an effective saturable absorber material with potential applica-tions in the field of ultrafast optics.
基金Projects(42106051,42006046,U2106206) supported by the National Natural Science Foundation of ChinaProject(22373501D) supported by Hebei Provincial Key R&D Program,China。
文摘Copper is a versatile material,commonly utilized in power transmission and electronic devices,but its relative high reactivity necessitates a long-lasting protective technique.Here,we report a method that combines plasma-enhanced non-equilibrium magnetron sputtering physical vapor deposition(PEUMS-PVD)and anodization to construct a self-healing three-dimensional Ti/Al-doped TiO_(2)nanotubes/Ti_(3)AlC_(2)coating on the surface of Cu substrates.This novel strategy enhances the corrosion resistance of copper substrates in marine environments,with corrosion current densities of up to 4.5643×10^(−8)A/cm^(2).Among them,the doping of nano-aluminum particles makes the coating self-healing.The mechanistic analysis of the corrosion behaviors during early immersion experiments was conducted using electrochemical noise,and revealed that during the initial stages of coating immersion,uniform corrosion predominates,with a minor occurrence of localized corrosion.
基金financially supported by the National Natural Science Foundation of China(No.22173104)。
文摘We present a comprehensive study of the CO_(2)-CO interaction potential using a 9-dimensional(9D)potential energy surface(PES)constructed with the fundamental invariant-neural networks(FINN)method.The PES was generated from 65330 CCSD(T)-F12a/aug-cc-pVTZ ab initio data points,with counterpoise correction,applied to eliminate basis set superposition error(BSSE).We performed quasi-classical trajectory simulations using this PES to investigate the rotational energy transfer dynamics.Our results reveal complex energy transfer mechanisms,with significant rotational excitation and relaxation dependent on collision energy and initial rotational states.The 9D PES provides a more accurate representation of the CO_(2)-CO system,offering new insights into molecular dynamics and interaction mechanisms.
基金support from National Natural Science Foundation of China(Grant Nos.22275145,22305189and 21875184)Natural Science Foundation of Shaanxi Province(Grant Nos.2022JC-10 and 2024JC-YBQN-0112).
文摘Two-dimensional energetic materials(2DEMs),characterized by their exceptional interlayer sliding properties,are recognized as exemplar of low-sensitivity energetic materials.However,the diversity of available 2DEMs is severely constrained by the absence of efficient methods for rapidly predicting crystal packing modes from molecular structures,impeding the high-throughput rational design of such materials.In this study,we employed quantified indicators,such as hydrogen bond dimension and maximum planar separation,to quickly screen 172DEM and 16 non-2DEM crystal structures from a crystal database.They were subsequently compared and analyzed,focusing on hydrogen bond donor-acceptor combinations,skeleton features,and intermolecular interactions.Our findings suggest that theπ-πpacking interaction energy is a key determinant in the formation of layered packing modes by planar energetic molecules,with its magnitude primarily influenced by the strongest dimericπ-πinteraction(π-π2max).Consequently,we have delineated a critical threshold forπ-π2max to discern layered packing modes and formulated a theoretical model for predictingπ-π2max,grounded in molecular electrostatic potential and dipole moment analysis.The predictive efficacy of this model was substantiated through external validation on a test set comprising 31 planar energetic molecular crystals,achieving an accuracy of 84%and a recall of 75%.Furthermore,the proposed model shows superior classification predictive performance compared to typical machine learning methods,such as random forest,on the external validation samples.This contribution introduces a novel methodology for the identification of crystal packing modes in 2DEMs,potentially accelerating the design and synthesis of high-energy,low-sensitivity 2DEMs.
基金supported by the National Natural Science Foundation of China(12241502,92045301)Fundamental Research Funds for the Central Universities(20720220010)+7 种基金USTC Research Funds of the Double First-Class Initiative(YD2310002012)the Launching Special Funds of Scientific Research for Introduced Talents from University of Science and Technology of China(KY2310000060)National Key Research and Development Program of China(2019YFA0405602)Anhui Provincial Natural Science Foundation(2408085QB049)the Instruments Center for Physical Science and USTC Center for Micro and Nanoscale Research and Fabrication,University of Science and Technology of Chinathe solid supports from the BL03U,BL10B,and BL12B beamlines of the National Synchrotron Radiation Laboratory(NSRL,Hefei)the Shanghai Synchrotron Radiation Facility(SSRF,Shanghai)of BL11B(https://cstr.cn/31124.02.SSRF.BL11B)and BL14W1(https://cstr.cn/31124.02.SSRF.BL14W1)beamlines for the assistance on XAFS measurementsAnhui Chuangpu Instruments Co.,Ltd.for the assistance in the test of Table XAFS。
文摘Photocatalytic CO_(2)reduction into value-added chemicals holds significant promise for carbon-neutral recycling and solar-to-fuel conversion.Enhancing reaction efficiency by manipulating charge transfer is a key approach to unlocking this potential.In this work,we construct a two-dimensional/twodimensional(2D/2D)FeSe_(2)/protonated carbon nitride(FeSe_(2)/PCN)heterostructure to promote the interfacial charge transfer dynamics,leading to a four-fold improved conversion efficiency of photocatalytic CO_(2)reduction with near 100%CO selectivity.Combining in situ X-ray photoelectron spectroscopy,in situ soft X-ray absorption spectroscopy,and femtosecond transient absorption spectroscopy,it is revealed that FeSe_(2)acts as an electron acceptor upon photoexcitation,introducing an additional electron transfer pathway from PCN to FeSe_(2)that suppresses radiative recombination and promotes charge transfer.In situ X-ray absorption fine structure spectroscopy,in situ diffuse reflectance infrared Fourier transform spectroscopy,and density functional theory calculation further unravel that the electron-enriched FeSe_(2)functions as the active sites for CO_(2)activation and significantly reduces the energy barrier of key intermediate COOH*formation,which is the rate-determined step for CO generation.This work underscores the importance of regulating photocarrier relaxation pathways to achieve effective spatial charge separation for promoted photocatalytic CO_(2)reduction and demonstrates the powerful functions of in situ spectroscopies in in-depth understanding of the photocatalytic mechanism.
基金the Natural Science Foundation of Shandong Province(Nos.ZR2022JQ05 and ZR2024MF010).
文摘With high surface-to-volume ratio,the abundant surface states and high carrier concentration are challenging the nearinfrared photodetection behaviors of narrow band gap semiconductors nanowires.In this study,the narrow band gap semiconductor of Bi_(2)O_(2)Se nanosheets(NSs)is adopted to construct mixed-dimensional heterojunctions with GaSb nanowires(NWs)for demonstrating the impressive self-powered NIR photodetection.Benefiting from the built-in electric field of~140 meV,the as-constructed NW/NS mixeddimensional heterojunction self-powered photodetector shows the low dark current of 0.07 pA,high I_(light)/I_(dark)ratio of 82 and fast response times of<2/2 ms at room temperature.The self-powered photodetector performance can be further enhanced by fabricating the NW array/NS mixed-dimensional heterojunction by using a contact printing technique.The excellent photodetection performance promises the asconstructed NW/NS mixed-dimensional heterojunction self-powered photodetector in imaging and photocommunication.
基金supported by the National Key R&D Program of China(Nos.2023YFF0718303 and 2022YFB3504804)the National Natural Science Foundation of China(Nos.51871219,52031014 and 52401255)the Science and Technology Project of Shenyang City(No.22-101-0-27).
文摘The single-layer Ti_(3)C_(2)T_(x)/MXene has become a special electromagnetic wave absorber near the terahertz band because of its abundant surface groups and excellent conductivity.However,the macro-preparation of single-layer Ti_(3)C_(2)T_(x)/MXene shows significantly difficult to influence its application.The two-dimensional Ti_(3)C_(2)T_(x)is easily prepared to have high production,but its weak absorption ability due to high surface conductivity also restricts its application.To realize the strong electromagnetic wave absorption of two-dimensional Ti_(3)C_(2)T_(x)/MXene,a new strategy with magnetic FeNi nanoparticles decorating Ti_(3)C_(2)T_(x)/MXene composites(FeNi-Ti_(3)C_(2)T_(x))were proposed and the effective electromagnetic wave absorption features covering 170-220 GHz that means the absorption band width reach 50 GHz.With an absorber composite film thickness being only 0.6 mm,the absorptivity of the composite is enhanced with the increase of decorating FeNi nanoparticles and promote up to 75%when the FeNi nanoparticles loading content reaches 30 wt%.The improvement of absorption is attributed to the introduction of soft magnetic FeNi to adjust the high surface conductivity of MXene and improve the electromagnetic balance of the absorber.
基金supported by the National Natural Science Foundation of China(Nos.52293444 and 22076209)the Key R&D Project of Ningxia(No.2021BEG02006).
文摘Microplastics(MPs)are ubiquitous in the environment,continuously undergo aging processes and release toxic chemical substances.Understanding the environmental behaviors of MPs is critical to accurately evaluate their long-term ecological risk.Generalized twodimensional correlation spectroscopy(2D-COS)is a powerful tool for MPs studies,which can dig more comprehensive information hiding in the conventional one-dimensional spectra,such as infrared(IR)and Raman spectra.The recent applications of 2D-COS in analyzing the behaviors and fates of MPs in the environment,including their aging processes,and interactions with natural organicmatter(NOM)or other chemical substances,were summarized systematically.The main requirements and limitations of current approaches for exploring these processes are discussed,and the corresponding strategies to address these limitations and drawbacks are proposed as well.Finally,new trends of 2D-COS are prospected for analyzing the properties and behaviors of MPs in both natural and artificial environmental processes.
基金financially supported by National Natural Science Foundation of China(No.22275149)Fundamental Research Funds for the Central Universities(No.SWU118105)the Next-Generation Advanced Energy Materials Program of BatteroTech Co.,Ltd.
文摘We propose and investigate a novel stable two-dimensional(2D)AlO_(2)with anomalous stoichiometric ratios based on first-principles calculation.2D AlO_(2)has metallic properties.It possesses the rare in-plane and out-of-plane negative Poisson's ratio(NPR)phenomenon,originating from its special sawtooth-like structure.The absolute value of the NPR decreases as the number of layers increases.The adsorption of volatile organic compounds(VOCs)including CH_(2)O,C_(2)H_(3)Cl and C_(6)H_(6)by AlO_(2)exhibit small adsorption distance,large adsorption energy,large charge transfer and significant density of states(DOS)changes,indicating the presence of strong interactions.The desorption time of each gas molecule on the AlO_(2)surface is also evaluated,and the results further suggest that the desorption of VOCs can be controlled by changing the temperature to achieve the recycling of AlO_(2).These interesting properties make 2D AlO_(2)a promising material for electronic,mechanical and sensing applications for VOCs.
基金Funded by the National Natural Science Foundation of China (No.22203066)the 6th Young Elite Scientist Sponsorship Program by China Association for Science and Technology (No.2020QNRC001)。
文摘The size effects were experimentally investigated and the underlying mechanism was analyzed.The results reveal that,as the specimen size increases,the interconnectivity of macropores slightly decreases.This in turn constrains the diffusion of CO_(2) and moisture in the specimens,resulting in an increase in the discrepancy between the internal and external carbonation degrees.An increase in cement paste thickness simultaneously decreases the quantity,average size,and interconnectivity of macropores,lowering the diffusion efficacy of CO_(2) and moisture and exacerbating the overall heterogeneity in carbonation.Moreover,the gradual blockage of macropores leads to the emergence of localized ‘occluded zones’ with much lower carbonation degree.The reduction in aggregate size significantly alters the average diameter and connectivity of macropores,leading to notable change to overall non-uniformity.This study provides insight into improving the CO_(2) curing effect of pervious concrete products and developing uniform curing methods.
基金funded by the Natural Science Foundation of China (No. 21603109)the Henan Joint Fund of the National Natural Science Foundation of China (No. U1404216)+1 种基金the Scientific Research Program Funded by Shaanxi Provincial Education Department (No. 20JK0676)supported by Natural Science Basic Research Program of Shanxi (Nos. 2022JQ-108, 2022JQ096)。
文摘Electrocatalytic reduction of NO(NORR) is an effective method for NH_(3) synthesis, due to low bonding energy of N–O bond. In this work, we have investigated many CrS_(2)based catalysts, including pristine CrS_(2),CrS_(2)with one S vacancy(v-CrS_(2)), and Ti doped CrS_(2)(Ti@CrS_(2)). The results have shown that the pristine CrS_(2)exhibits inert character for NO activation. However, v-CrS_(2)and Ti@CrS_(2)can exhibit enhanced interaction with NO, due to increased charge transfer between NO and substrates(0.52–0.75 e) and enhanced adsorption energies of NO on the catalysts(-0.96~-1.64 e V), compared to the situation of CrS_(2)(0.065 e/-0.30 e V). From the free energy profiles of NO electro-reduction to NH3, we can see that the v-CrS_(2)and Ti@CrS_(2)all exhibit ultralow limiting potentials of-0.03~-0.47 V, following both*NOH and*NHO mechanisms. Therefore, introducing vacancy and doping are all promising modification strategies for NORR catalysts. The results have provided a new idea for the search of catalysts for efficient electrocatalytic reduction of NO.
基金supported by the National Natural Sci-ence Foundation of China(No.22174135,No.21790352)the National Key R&D Program of China(No.2021YFA1500500,No.2016YFA0200600)+4 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB36000000)Anhui Initiative in Quantum Information Technologies(No.AHY090100)CAS Project for Young Scientists in Basic Research(No.YSBR-054)Innovation Program for Quantum Science and Technology(No.2021ZD0303301)the Fundamental Research Funds for the Central Universities.
文摘Double-resonance Raman(DRR)scattering in two-di-mensional(2D)materials describes the intravalley or intervalley scattering of an electron or a hole excited by incident photons.Although the presence of defects can provide additional momentum and influence the scat-tering process involving one or two phonons,only the idealized defects without any structural details are considered in tra-ditional DRR theory.Here,the second-order DRR spectra of WSe_(2) monolayer with different types of defects are calculated involving the combinations of acoustic and optical phonons in the vicinity of K(K')and M points of the Brillouin zone.The electronic band structures are modified due to the presence of defects,and the band unfolding method is adopted to show the bending of valence and conduction bands for the defective WSe_(2) monolayers.The associ-ated phononic band structures also exhibit different changes in phonon dispersion curves,re-sulting in different DRR spectra corresponding to the different types of defects in the WSe_(2) monolayers.For example,the existence of W vacancy in the WSe_(2) monolayer would result in downshifts in vibrational frequencies and asymmetrical broadenings in linewidths for most combination modes due to the dramatic changes in contour shape of electronic valleys at K and K'.Moreover,the scattering from K to Q is found to be forbidden for the two Se vacan-cies because of the elevation of conduction band at the Q point.Our work highlights the role of defect structures in the intervalley scattering and may provide better understanding in the underlying physics of DRR process in 2D materials.
基金financial support from the National Natural Science Foundation of China(No.22072183)the Natural Science Foundation of Hunan Province,China(No.2022JJ30690)supported in part by the High Performance Computing Center of Central South University。
文摘Three-dimensional(3D)covalent organic frameworks(COFs)have attracted extensive attention as photocatalysts for CO_(2)reduction reactions.Introducing metal atoms is essential for enhancing activity,but previous metal sites in 3D COFs predominantly exhibit symmetrical coordination,making them unsuitable for CO_(2)activation.Here,we design a 3D COF with 2,2'-pyridine linked around tetra-(4-anilyl)methane(TCM-Bpy-COF),where Co^(2+)is asymmetrically coordinated by bipyridine and acetates(TCMBpy-COF-CoAc).The TCM-Bpy-COF-CoAc exhibits outstanding photocatalytic CO_(2)reduction performance under weak visible light,achieving a CO evolution rate of 26,650μmol g^(-1)h^(-1)under 5 W of lightemitting-diode(LED)lamp and high apparent quantum efficiency.The performance far exceeds that of symmetrically coordinated bipyridine-Co-bipyridine TCM-Bpy-COF and surpasses most reported COF-based photocatalysts.In-situ spectral characterizations and theoretical calculations show that asymmetric N,O-coordination around the Co^(2+)center polarizes electron density and lowers reaction energy barriers of^(*)COOH intermediates,enhancing the conversion of CO_(2)to CO.This work inspires the design of 3D COF-based photocatalysts with highly catalytic efficiency.
文摘Ordered NiCo_(2)O_(4)/rGO nanowire arrays(NWAs)grown on a Ni foam substrate were synthesized using a template-free hydrothermal method and employed as an electrode with outstanding electrochemical properties for supercapacitors.After conducting a series of time-variable controlled experiments,the structure,morphology,and electrochemical properties of NiCo_(2)O_(4)/rGO NWAs were analyzed to find the most suitable growth time.Benefited from such unique array architectures,the designed NiCo_(2)O_(4)/rGO NWAs electrode demonstrates significant electrochemical properties,showing a specific capacitance of 2418 F·g^(-1)at a charge-discharge current density of 1 A·g^(-1).Moreover,it demonstrates exceptional stability,maintaining a capacity retention of 81.5%after undergoing 2,000 cycles,even when subjected to a current density of 10 A·g^(-1).The reason of high stability is that the spacing between the nanowire arrays is large and the diffusion resistance of the electrolyte is significantly reduced,which facilitates the diffusion of the electrolyte into the interior of the electrodes and establishes an effective contact with the surface of the nanowires.Furthermore,the NiCo_(2)O_(4)/rGO nanowire array grows directly on the Ni foam without binder,which establishes rapid electron transport pathways on the Ni foam substrate,resulting in excellent electrochemical properties.
基金supported by the National Natural Science Foundation of China,Grant No.12375006。
文摘In this paper,we investigate the(2+1)-dimensional three-component long-wave-short-wave resonance interaction system,which describes complex systems and nonlinear wave phenomena in physics.By employing the Hirota bilinear method,we derive the general nondegenerate N-soliton solution of the system,where each short-wave component contains N arbitrary functions of the independent variable y.The presence of these arbitrary functions in the analytical solution enables the construction of a wide range of nondegenerate soliton types.Finally,we illustrate the structural features of several novel nondegenerate solitons,including M-shaped,multiple double-hump,and sawtooth double-striped solitons,as well as interactions between nondegenerate solitons,such as dromion-like solitons and solitoffs,with the aid of figures.
基金supported by the National Natural Science Foundation of China(Nos.52003297 and 22302233)the Open Project of State Key Laboratory of Chemical Safety(No.SKLCS-2024020)+2 种基金the National Key R&D Program of China(Nos.2022YFB3205501 and 2022YFB3205504)and the Fundamental Research Funds for the Central Universities(No.24CX02014A)the Fund of State Key Laboratory of Deep Oil and Gas,China University of Petroleum(East China).
文摘Based on the unique catalytic properties of precious metals,the introduction of precious metals into metal oxide semiconductors will greatly improve the gas-sensitive properties of materials.As a new type of porous material,metal–organic frameworks(MOF)can be used for gas separation and adsorption due to their adjustable pore size and acceptable thermal stability.In this work,the ZIF-71 MOF was synthesized on CuO nanofibers doped with different concentrations of Ru to form a Ru–CuO@ZIF-71 nanocomposite sensor,which was then used for H_(2)S detection.The sensor shows sensitivity to trace amounts of H_(2)S gas(100 ppb),and the response is greatly enhanced at the optimal Ru doping ratio and operating temperature.The introduction of the ZIF-71 membrane can significantly increase the selectivity of the sensor while further improving the sensitivity.Finally,the possible sensing mechanism of the Ru–CuO@ZIF-71 sensor was explored.The enhancement of the H_(2)S gas sensing properties may be attributed to the catalysis of Ru and the formation of the Schottky junction at the Ru–CuO interface.Besides,the calculation based on density functional theory reveals enhanced adsorption capacities of CuO for H_(2)S after Ru doping.Therefore,the Ru–CuO@ZIF-71 sensor has strong application potential in exhaled gas detection and portable detection of H_(2)S gas in industrial environments.
基金supported by the National Natural Science Foundation of China(12371255,11975306)the Xuzhou Basic Research Program Project(KC23048)+1 种基金the Six Talent Peaks Project in Jiangsu Province(JY-059)the 333 Project in Jiangsu Province and the Fundamental Research Funds for the Central Universities of CUMT(2024ZDPYJQ1003).
文摘In this work,we study wave state transitions of the(2+1)-dimensional Kortewegde Vries-Sawada-Kotera-Ramani(2KdVSKR)equation by analyzing the characteristic line and phase shift.By converting the wave parameters of the N-soliton solution into complex numbers,the breath wave solution is constructed.The lump wave solution is derived through the long wave limit method.Then,by choosing appropriate parameter values,we acquire a number of transformed nonlinear waves whose gradient relation is discussed according to the ratio of the wave parameters.Furthermore,we reveal transition mechanisms of the waves by exploring the nonlinear superposition of the solitary and periodic wave components.Subsequently,locality,oscillation properties and evolutionary phenomenon of the transformed waves are presented.And we also prove the change in the geometrical properties of the characteristic lines leads to the phenomena of wave evolution.Finally,for higher-order waves,a range of interaction models are depicted along with their evolutionary phenomena.And we demonstrate that their diversity is due to the fact that the solitary and periodic wave components produce different phase shifts caused by time evolution and collisions.
基金supported by the Shandong Provincial Natural Science Foundation(ZR2024MD116)National Natural Science Foundation of China(Grant Nos.42174143,42004098)Technology Innovation Leading Program of Shaanxi(No.2024 ZC-YYDP-27).
文摘Subsurface rocks,as complex porous media,exhibit multiscale pore structures and intricate physical properties.Digital rock physics technology has become increasingly influential in the study of subsurface rock properties.Given the multiscale characteristics of rock pore structures,direct three-dimensional imaging at sub-micrometer and nanometer scales is typically infeasible.This study introduces a method for reconstructing porous media using multidimensional data,which combines one-dimensional pore structure parameters with two-dimensional images to reconstruct three-dimensional models.The pore network model(PNM)is stochastically reconstructed using one-dimensional parameters,and a generative adversarial network(GAN)is utilized to equip the PNM with pore morphologies derived from two-dimensional images.The digital rocks generated by this method possess excellent controllability.Using Berea sandstone and Grosmont carbonate samples,we performed digital rock reconstructions based on PNM extracted by the maximum ball algorithm and compared them with stochastically reconstructed PNM.Pore structure parameters,permeability,and formation factors were calculated.The results show that the generated samples exhibit good consistency with real samples in terms of pore morphology,pore structure,and physical properties.Furthermore,our method effectively supplements the micropores not captured in CT images,demonstrating its potential in multiscale carbonate samples.Thus,the proposed reconstruction method is promising for advancing porous media property research.
基金financially supported by the Scientific Research Foundation of North China University of Technology (Grant Nos.11005136024XN147-87 and 110051360024XN151-86)。
文摘Recently, during the investigations on planetary oceans, Hirota-Satsuma-Ito-type models have been developed. In this paper, for a(2+1)-dimensional generalized variable-coefficient Hirota-Satsuma-Ito system describing the fluid dynamics of shallow-water waves in an open ocean, non-characteristic movable singular manifold and symbolic computation enable an oceanic auto-B?cklund transformation with three sets of the oceanic solitonic solutions. The results rely on the oceanic variable coefficients in that system. Future oceanic observations might detect some nonlinear features predicted in this paper, and relevant oceanographic insights might be expected.
基金Project(50625101) supported by the National Science Fund for Distinguished Young Scholars of ChinaProject supported by Graduate Independent Innovation Foundation of Shandong University(GIIFSDU),ChinaProject(51071097) supported by the National Natural Science Foundation of China
文摘A series of Al-Ti-B master alloys were prepared by different preparation routes,and the TiB2 particles in the master alloys were extracted and analyzed.It is found that the forming process has significant influence on the three-dimensional morphology of TiB2 particles.Different preparation routes result in different reaction forms,which accounts for the morphology variation of TiB2 particles.When the Al-Ti-B master alloy is prepared using ＂halide salt＂ route,TiB2 particles exhibit hexagonal platelet morphology and are independent with each other.In addition,the reaction temperature almost does not have influence on the morphology of TiB2 particles.However,TiB2 particles exhibit different morphologies at different reaction temperatures when the master alloys are prepared with Al-3B and Ti sponge.When the master alloy is prepared at 850 ℃,a kind of TiB2 particle agglomeration forms with a size larger than 5 μm.The TiB2 particles change to layered stacking morphology even dendritic morphology with the reaction temperature reaching up to 1200 ℃.
