Recent advancements have led to the synthesis of various new metal-containing explosives,particularly energetic metal-organic frameworks(EMOFs),which feature high-energy ligands within well-ordered crystalline structu...Recent advancements have led to the synthesis of various new metal-containing explosives,particularly energetic metal-organic frameworks(EMOFs),which feature high-energy ligands within well-ordered crystalline structures.These explosives exhibit significant advantages over traditional compounds,including higher density,greater heats of detonation,improved mechanical hardness,and excellent thermal stability.To effectively evaluate their detonation performance,it is crucial to have a reliable method for predicting detonation heat,velocity,and pressure.This study leverages experimental data and outputs from the leading commercial computer code to identify suitable decomposition pathways for different metal oxides,facilitating straightforward calculations for the detonation performance of alkali metal salts,and metal coordination compounds,along with EMOFs.The new model enhances predictive reliability for detonation velocities,aligning more closely with experimental results,as evi-denced by a root mean square error(RMSE)of 0.68 km/s compared to 1.12 km/s for existing methods.Furthermore,it accommodates a broader range of compounds,including those containing Sr,Cd,and Ag,and provides predictions for EMOFs that are more consistent with computer code outputs than previous predictive models.展开更多
As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants....As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.展开更多
The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts hav...The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.展开更多
Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TM...Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TMOs)are regarded as potential substitutes for PGMs because of their stability in oxidizing environments and excellent catalytic performance.In this study,comprehensive investigation into the influence of elastic strains on the adsorption energies of carbon(C),hydrogen(H)and oxygen(O)on TMOs was conducted.Based on density functional theory(DFT)calculations,these effects in both tetragonal structures(PtO_(2),PdO_(2))and hexagonal structures(ZnO,CdO),along with their respective transition metals were systematically explored.It was identified that the optimal adsorption sites on metal oxides pinpointed the top of oxygen or the top of metal atom,while face-centered cubic(FCC)and hexagonal close-packed(HCP)holes were preferred for the transition metals.Furthermore,under the influence of elastic strains,the results demonstrated significant disparities in the adsorption energies of H and O between oxides and transition metals.Despite these differences,the effect of elastic strains on the adsorption energies of C,H and O on TMOs mirrored those on transition metals:adsorption energies increased under compressive strains,indicating weaker adsorption,and decreased under tension strains,indicating stronger adsorption.This behavior was rationalized based on the d-band model for adsorption atop a metallic atom or the p-band model for adsorption atop an oxygen atom.Consequently,elastic strains present a promising avenue for tailoring the catalytic properties of TMOs.展开更多
The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and ...The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.展开更多
In this study,the electronic transition properties and structural analysis of the metal complexes(Ni(Ⅱ),Co(Ⅱ),Cu(Ⅱ)and Mn(Ⅱ))of three different polymer ligands were performed by using XRF and X-ray diffraction(XRD...In this study,the electronic transition properties and structural analysis of the metal complexes(Ni(Ⅱ),Co(Ⅱ),Cu(Ⅱ)and Mn(Ⅱ))of three different polymer ligands were performed by using XRF and X-ray diffraction(XRD)techniques,respectively.The structural analysis of the polymers and their complexes were performed by XRD technique and some of the polymers were found to be in the face-centred cubic(fcc)structure.In addition,the values of the present K X-ray intensity ratios are significantly greater than the values reported in literature.展开更多
The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nit...The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.展开更多
There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of t...There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of traditional rechargeable batteries with the superior power density and long life of supercapacitors(SCs).Nevertheless,the development of LICs is still hampered by limited kinetic processes and capacity mismatch between the cathode and anode.Metal-organic frameworks(MOFs)and their derivatives have received significant attention because of their extensive specific surface area,different pore structures and topologies,and customizable functional sites,making them compelling candidate materials for achieving high-performance LICs.MOF-derived carbons,known for their exceptional electronic conductivity and large surface area,provide improved charge storage and rapid ion transport.MOF-derived transition metal oxides contribute to high specific capacities and improved electrochemical stability.Additionally,MOF-derived metal compounds/carbons provide combined effects that increase both the capacitive and Faradaic reactions,leading to a superior overall performance.The review begins with an overview of the fundamental principles of LICs,followed by an exploration of synthesis strategies and ligand selection for MOF-based composite materials.It then analyzes the advantages of original MOFs and their derived materials,such as carbon materials and metal compounds,in enhancing LIC performance.Finally,the review discusses the major challenges faced by MOFs and their derivatives in LIC applications and offers future research directions and recommendations.展开更多
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
Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite end...Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite endows it with abundant catalytically active sites,thereby accelerating the reduction of I_(3)^(-).More importantly,the dye-sensitized solar cells(DSSCs)prepared by scraping it on flexible titanium mesh with low resistance had low series resistance(Rs).Electrochemical characterizations revealed that the DSSCs employing the FMS/CC counter electrode achieved a power conversion efficiency(PCE)of ca.9.51%(surpassing the ca.8.15%efficiency of the Pt counter electrode),open-circuit voltage(Voc)of ca.0.79 V,short-circuit current density(Jsc)of ca.18.31 mA·cm^(-2),and fill factor(FF)of ca.0.65.Moreover,after 100 times of cyclic voltammetry(CV)test,the CV curve remained unchanged,indicating the excellent stability of FMS/CC in the electrolyte containing I_(3)^(-)/I^(-).展开更多
Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an excep...Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an exceptionalspecific capacitance of 190.8 mAh·g^(-1)at 1 A·g^(-1),greatly higher than the corresponding monometallic sulfides MnS(31.7 mAh·g^(-1))and Co_(3)S_(4)(86.7 mAh·g^(-1)).Impressively,the as-assembled MnCo_(2)S_(4)||porous carbon(PC)hybridsupercapacitor(HSC),showed an outstanding energy density of 76.88 Wh·kg^(-1)at a power density of 374.5 W·kg^(-1),remarkable cyclic performance with a capacity retention of 86.8% after 10000 charge-discharge cycles at 5 A·g^(-1),and excellent Coulombic efficiency of 99.7%.展开更多
Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since ...Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since the mechanical exfoliation of graphene in 2004. Starting from graphene, 2D materials now have become a big family with numerous members and diverse categories. The unique structural features and physicochemical properties of 2D materials make them one class of the most appealing candidates for a wide range of potential applications. In particular, we have seen some major breakthroughs made in the field of 2D materials in last five years not only in developing novel synthetic methods and exploring new structures/properties but also in identifying innovative applications and pushing forward commercialisation. In this review, we provide a critical summary on the recent progress made in the field of 2D materials with a particular focus on last five years. After a brief backgroundintroduction, we first discuss the major synthetic methods for 2D materials, including the mechanical exfoliation, liquid exfoliation, vapor phase deposition, and wet-chemical synthesis as well as phase engineering of 2D materials belonging to the field of phase engineering of nanomaterials(PEN). We then introduce the superconducting/optical/magnetic properties and chirality of 2D materials along with newly emerging magic angle 2D superlattices. Following that, the promising applications of 2D materials in electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, we present the theoretic calculations and simulations of 2D materials. Finally, after concluding the current progress, we provide some personal discussions on the existing challenges and future outlooks in this rapidly developing field.展开更多
Transition metal sulfides(TMSs)-based materials have been extensively investigated as effective non-noble catalysts for various applications.However,the exploration of TMSs-based catalysts for hydrogenation of nitro c...Transition metal sulfides(TMSs)-based materials have been extensively investigated as effective non-noble catalysts for various applications.However,the exploration of TMSs-based catalysts for hydrogenation of nitro compounds is limited.Herein,CoSx/NC catalysts were prepared by solvothermal sulfurization of ZIF-67,followed by high-temperature annealing(300–600℃)under NH3 atmosphere.It was found that the structures and compositions of the as-prepared CoSx/NC can be readily tuned by varying the annealing temperature.Particularly,CoSx/NC-500,which possesses higher degree of S defects and larger specific surface areas,can achieve high conversion,selectivity and stability for catalytic reduction of nitro compounds into amines under mild reaction conditions.展开更多
In this work,we have reported the synthesis and spectroscopic characterization of captopril(Cap)coordination compounds:Cu(Cap)·2H 2O,Cr(Cap)·H 2O,Zn(Cap)·3H 2O and Mg(Cap)4.Herein,it is worthily mention...In this work,we have reported the synthesis and spectroscopic characterization of captopril(Cap)coordination compounds:Cu(Cap)·2H 2O,Cr(Cap)·H 2O,Zn(Cap)·3H 2O and Mg(Cap)4.Herein,it is worthily mentioned that the FTIR spectroscopic technique was employed to recognized the nature of coordination between captopril ligand and copper,chromium,zinc and magnesium(Ⅱ)metal ions.In view of the infrared spectroscopic tool,the copper(Ⅱ)metal ion coordinated toward captopril drug ligand through sulfur atom of SH group dependent on the absent of stretching vibration band of—SH.Based on this result,the stretching motion ofνa(COO)shifts clearly indicates that Cu 2+,Cr 2+,Zn 2+and Mg 2+the carboxylic group is employed as coordinative site for all compounds as a metal-ligand coordinative bond.As a general behavior,it is verified that the coordination compound thermal stability(considering the release of captopril molecules,not the release of water molecules)is affected by the metal cation radius:minor radius is associated with higher thermal stability,probably due to a higher metal-captopril bond dissociation enthalpy.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-lumines...Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-luminescence(PL)quantum yield of monolayer(1L)TMDs is still quite low at room temperature,which severely lim-its their practical applications.Here we report a PL enhancement effect of 1L WS_(2) at room temperature when con-structing it into 1L-WS_(2)/hBN/1L-MoS_(2) vertical HSs.The PL enhancement factors(EFs)can be up to 4.2.By using transient absorption(TA)spectroscopy,we demonstrate that the PL enhancement effect is due to energy transfer from 1L MoS_(2) to 1L WS_(2).The energy transfer process occurs on a picosecond timescale and lasts more than one hundred picoseconds which indicates a prominent contribution from exciton-exciton annihilation.Furthermore,the PL en-hancement effect of 1L WS_(2) can be observed in 2L-MoS_(2)/hBN/1L-WS_(2) and 3L-MoS_(2)/hBN/1L-WS_(2) HSs.Our study provides a comprehensive understanding of the energy transfer process in the PL enhancement of 2D TMDs and a fea-sible way to optimize the performance of TMD-based optoelectronic devices.展开更多
The study of oxide heteroepitaxy has been hindered by the issues of misfit strain and substrate clamping,which impede both the optimization of performance and the acquisition of a fundamental understanding of oxide sy...The study of oxide heteroepitaxy has been hindered by the issues of misfit strain and substrate clamping,which impede both the optimization of performance and the acquisition of a fundamental understanding of oxide systems.Recently,however,the development of freestanding oxide membranes has provided a plausible solution to these substrate limitations.Single-crystalline functional oxide films can be released from their substrates without incurring significant damage and can subsequently be transferred to any substrate of choice.This paper discusses recent advancements in the fabrication,adjustable physical properties,and various applications of freestanding oxide perovskite films.First,we present the primary strategies employed for the synthesis and transfer of these freestanding perovskite thin films.Second,we explore the main functionalities observed in freestanding perovskite oxide thin films,with special attention to the tunable functionalities and physical properties of these freestanding perovskite membranes under varying strain states.Next,we encapsulate three representative devices based on freestanding oxide films.Overall,this review highlights the potential of freestanding oxide films for the study of novel functionalities and flexible electronics.展开更多
Novel transition metal complexes of bis(diarylsubstitutedthiophosphoryl)imines ligand derived from O,O-di(p-methoxylphenyl)thiophosphoryl chloride and O,O-di-(p-methoxylphenyl)thiophosphoryl amine with Cu(Ⅱ ),Co( Ⅱ)...Novel transition metal complexes of bis(diarylsubstitutedthiophosphoryl)imines ligand derived from O,O-di(p-methoxylphenyl)thiophosphoryl chloride and O,O-di-(p-methoxylphenyl)thiophosphoryl amine with Cu(Ⅱ ),Co( Ⅱ) ,Ni( Ⅱ) ,Fe(Ⅱ ) and Mn( Ⅱ ) were synthesized. The formation mechanism of complexes and their stereochemistry structures were investigated according to elemental analysis,infrared spectra and 31P-nuclear magnetic resonance spectra. The extractions of the ligand for different divalent metal ions,such as Zn(Ⅱ ),Cd( Ⅱ) ,Cu( Ⅱ) ,Ni( Ⅱ ),Fe( Ⅱ) ,Sn( Ⅱ) ,Mn( Ⅱ) ,Pd( Ⅱ) ,Hg( Ⅱ) and Fe(Ⅲ),were investigated in sulphate solution,respectively. The results show the metal atom is coordinated by 4 sulfur atoms in a square-planar fashion,and the titled compound has not only powerful ability to coordinate with cadmium from aqueous solution with a high extractive rate about 61.20% and a relatively weak complexation for other divalent metals with the extractive rate from 2.46% to 36.66%,but also a good selectivity to Fe(Ⅲ ).展开更多
Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inf...Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inferior to that of platinum(Pt)metal.Preparation of multi-elemental alloy and construction of heterostructure are considered as highly effective methods to enhance hydrogen production activity.Herein,a novel quaternary CoMoSSe alloy with heterostructure was synthesized on the surface of carbon black(CB)particles(CoMoSSe@CB)by a simple Sol-Gel process and thereafter served as HER catalyst.Compared to CoSe@CB and MoS2@CB electrocatalysts,CoMoSSe@CB exhibits superior HER activity with a low overpotential of 190 mV at-10 mA·cm^(-2) and a Tafel slope of 62 mV·dec^(-1).This improvement is attributed to the alloying effects among Co,Mo,S and Se,as well as the heterogeneous structure in the composite material,which regulate the electronic structure and intermediate free energy,thereby increasing the number of active sites and enhancing charge-transfer ability.This work can provide new ideas and concepts for designing novel and efficient TMD electrocatalysts.展开更多
基金the research committee at Malek Ashtar University of Technology (MUT) for their invaluable support of this project
文摘Recent advancements have led to the synthesis of various new metal-containing explosives,particularly energetic metal-organic frameworks(EMOFs),which feature high-energy ligands within well-ordered crystalline structures.These explosives exhibit significant advantages over traditional compounds,including higher density,greater heats of detonation,improved mechanical hardness,and excellent thermal stability.To effectively evaluate their detonation performance,it is crucial to have a reliable method for predicting detonation heat,velocity,and pressure.This study leverages experimental data and outputs from the leading commercial computer code to identify suitable decomposition pathways for different metal oxides,facilitating straightforward calculations for the detonation performance of alkali metal salts,and metal coordination compounds,along with EMOFs.The new model enhances predictive reliability for detonation velocities,aligning more closely with experimental results,as evi-denced by a root mean square error(RMSE)of 0.68 km/s compared to 1.12 km/s for existing methods.Furthermore,it accommodates a broader range of compounds,including those containing Sr,Cd,and Ag,and provides predictions for EMOFs that are more consistent with computer code outputs than previous predictive models.
基金This work was financially supported by the Science and Technology project of Jiangsu province(BN2015021,XZ-SZ201819).
文摘As a main oxidizer in solid composite propellants,ammonium perchlorate(AP)plays an important role because its thermal decomposition behavior has a direct influence on the characteristic of solid composite propellants.To improve the performance of solid composite propellant,it is necessary to take measures to modify the thermal decomposition behavior of AP.In recent years,transition metal oxides and carbon-supported transition metal oxides have drawn considerable attention due to their extraordinary catalytic activity.In this review,we highlight strategies to enhance the thermal decomposition of AP by tuning morphology,varying the types of metal ion,and coupling with carbon analogue.The enhanced catalytic performance can be ascribed to synergistic effect,increased surface area,more exposed active sites,and accelerated electron transportation and so on.The mechanism of AP decomposition mixed with catalyst has also been briefly summarized.Finally,a conclusive outlook and possible research directions are suggested to address challenges such as lacking practical application in actual formulation of solid composite propellant and batch manufacturing.
文摘The hydrogen evolution reaction(HER)is a promising way to produce hydrogen,and the use of non-precious metals with an excellent electrochemical performance is vital for this.Carbon-based transition metal catalysts have high activity and stability,which are important in reducing the cost of hydrogen production and promoting the development of the hydrogen production industry.However,there is a lack of discussion regarding the effect of carbon components on the performance of these electrocatalysts.This review of the literature discusses the choice of the carbon components in these catalysts and their impact on catalytic performance,including electronic structure control by heteroatom doping,morphology adjustment,and the influence of self-supporting materials.It not only analyzes the progress in HER,but also provides guidance for synthesizing high-performance carbon-based transition metal catalysts.
基金Science and Technology Commission of Shanghai Municipality(21ZR1472900,22ZR1471600)。
文摘Platinum(Pt)-based noble metal catalysts(PGMs)are the most widely used commercial catalysts,but they have the problems of high cost,low reserves,and susceptibility to small-molecule toxicity.Transition metal oxides(TMOs)are regarded as potential substitutes for PGMs because of their stability in oxidizing environments and excellent catalytic performance.In this study,comprehensive investigation into the influence of elastic strains on the adsorption energies of carbon(C),hydrogen(H)and oxygen(O)on TMOs was conducted.Based on density functional theory(DFT)calculations,these effects in both tetragonal structures(PtO_(2),PdO_(2))and hexagonal structures(ZnO,CdO),along with their respective transition metals were systematically explored.It was identified that the optimal adsorption sites on metal oxides pinpointed the top of oxygen or the top of metal atom,while face-centered cubic(FCC)and hexagonal close-packed(HCP)holes were preferred for the transition metals.Furthermore,under the influence of elastic strains,the results demonstrated significant disparities in the adsorption energies of H and O between oxides and transition metals.Despite these differences,the effect of elastic strains on the adsorption energies of C,H and O on TMOs mirrored those on transition metals:adsorption energies increased under compressive strains,indicating weaker adsorption,and decreased under tension strains,indicating stronger adsorption.This behavior was rationalized based on the d-band model for adsorption atop a metallic atom or the p-band model for adsorption atop an oxygen atom.Consequently,elastic strains present a promising avenue for tailoring the catalytic properties of TMOs.
文摘The transition metal complexes of triaminoguanidine(TAG-M,where M=Cobalt(Co)or Iron(Fe))have been prepared.The catalytic effect of these complexes on the thermolysis of energetic composite based on nitrocellulose and diethylene glycol dinitrate,has been investigated.Extensive characterization of the resulting energetic composites was carried out using scanning electron microscopy(SEM),X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR),and differential scanning calorimetry(DSC).Isoconversional kinetic analysis was performed to determine the Arrhenius parameters associated with the thermolysis of the elaborated energetic formulations.It is found that TAG-M complexes have strong catalytic effect on the thermo-kinetic decomposition of NC/DEGDN by decreasing the apparent activation energy and significantly increased the total heat release.The models that govern the decomposition processes are also studied,and it is revealed that different reaction processes are accomplished by introduction metal complexes of triaminoguanidine.Overall,this study serves as a valuable reference for future research focused on the investigation of catalytic combustion features of solid propellants.
基金Scientific Research Fund of Kahramanmaras Sutcu Imam University,Turkey(2012/3-7YLS)
文摘In this study,the electronic transition properties and structural analysis of the metal complexes(Ni(Ⅱ),Co(Ⅱ),Cu(Ⅱ)and Mn(Ⅱ))of three different polymer ligands were performed by using XRF and X-ray diffraction(XRD)techniques,respectively.The structural analysis of the polymers and their complexes were performed by XRD technique and some of the polymers were found to be in the face-centred cubic(fcc)structure.In addition,the values of the present K X-ray intensity ratios are significantly greater than the values reported in literature.
基金partially supported by National Natural Science Foundation of China(52172250)Institute of Process Engineering(IPE)Project for Frontier Basic Research(QYJC-2023-06)。
文摘The use of lithium-sulfur(Li-S)batteries is limited by sulfur redox reactions involving multi-phase transformations,especially at low-temperatures.To address this issue,we report a material(FCNS@NCFs)consisting of nitrogen-doped carbon fibers loaded with a ternary metal sulf-ide((Fe,Co,Ni)_(9)S_(8))for use as the sulfur host in Li-S batteries.This materi-al was prepared using transfer blot filter paper as the carbon precursor,thiourea as the source of nitrogen and sulfur,and FeCl_(3)·6H_(2)O,CoCl_(2)·6H_(2)O and NiCl_(2)·6H_(2)O as the metal ion sources.It was synthesized by an impreg-nation method followed by calcination.The nitrogen doping significantly in-creased the conductivity of the host,and the metal sulfides have excellent catalytic activities.Theoretical calculations,and adsorption and deposition experiments show that active sites on the surface of FCNS@NCFs selectively adsorb polysulfides,facilitate rapid adsorption and conversion,prevent cathode passivation and inhib-it the polysulfide shuttling.The FCNS@NCFs used as the sulfur host has excellent electrochemical properties.Its initial dis-charge capacity is 1639.0 mAh g^(−1) at 0.2 C and room temperature,and it remains a capacity of 1255.1 mAh g^(−1) after 100 cycles.At−20~C,it has an initial discharge capacity of 1578.5 mAh g^(−1) at 0.2 C,with a capacity of 867.5 mAh g^(−1) after 100 cycles.Its excellent performance at both ambient and low temperatures suggests a new way to produce high-performance low-temper-ature Li-S batteries.
文摘There is an urgent need for lithium-ion capacitors(LICs)that have both high energy and high power densities to meet the continuously growing energy storage demands.LICs effectively balance the high energy density of traditional rechargeable batteries with the superior power density and long life of supercapacitors(SCs).Nevertheless,the development of LICs is still hampered by limited kinetic processes and capacity mismatch between the cathode and anode.Metal-organic frameworks(MOFs)and their derivatives have received significant attention because of their extensive specific surface area,different pore structures and topologies,and customizable functional sites,making them compelling candidate materials for achieving high-performance LICs.MOF-derived carbons,known for their exceptional electronic conductivity and large surface area,provide improved charge storage and rapid ion transport.MOF-derived transition metal oxides contribute to high specific capacities and improved electrochemical stability.Additionally,MOF-derived metal compounds/carbons provide combined effects that increase both the capacitive and Faradaic reactions,leading to a superior overall performance.The review begins with an overview of the fundamental principles of LICs,followed by an exploration of synthesis strategies and ligand selection for MOF-based composite materials.It then analyzes the advantages of original MOFs and their derived materials,such as carbon materials and metal compounds,in enhancing LIC performance.Finally,the review discusses the major challenges faced by MOFs and their derivatives in LIC applications and offers future research directions and recommendations.
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.
文摘Herein,an FMS/CC composite was successfully fabricated by depositing FeMoS_(4)onto a pristine carbon fiber cloth(CC)substrate via a facile two-step hydrothermal method.The amorphous nature of the FMS/CC compos-ite endows it with abundant catalytically active sites,thereby accelerating the reduction of I_(3)^(-).More importantly,the dye-sensitized solar cells(DSSCs)prepared by scraping it on flexible titanium mesh with low resistance had low series resistance(Rs).Electrochemical characterizations revealed that the DSSCs employing the FMS/CC counter electrode achieved a power conversion efficiency(PCE)of ca.9.51%(surpassing the ca.8.15%efficiency of the Pt counter electrode),open-circuit voltage(Voc)of ca.0.79 V,short-circuit current density(Jsc)of ca.18.31 mA·cm^(-2),and fill factor(FF)of ca.0.65.Moreover,after 100 times of cyclic voltammetry(CV)test,the CV curve remained unchanged,indicating the excellent stability of FMS/CC in the electrolyte containing I_(3)^(-)/I^(-).
文摘Porous spherical MnCo_(2)S_(4) was synthesized by a simple solvothermal method.Thanks to the well-designedbimetallic composition and the unique porous spherical structure,the MnCo_(2)S_(4) electrode exhibited an exceptionalspecific capacitance of 190.8 mAh·g^(-1)at 1 A·g^(-1),greatly higher than the corresponding monometallic sulfides MnS(31.7 mAh·g^(-1))and Co_(3)S_(4)(86.7 mAh·g^(-1)).Impressively,the as-assembled MnCo_(2)S_(4)||porous carbon(PC)hybridsupercapacitor(HSC),showed an outstanding energy density of 76.88 Wh·kg^(-1)at a power density of 374.5 W·kg^(-1),remarkable cyclic performance with a capacity retention of 86.8% after 10000 charge-discharge cycles at 5 A·g^(-1),and excellent Coulombic efficiency of 99.7%.
文摘Research on two-dimensional(2D) materials has been explosively increasing in last seventeen years in varying subjects including condensed matter physics, electronic engineering, materials science, and chemistry since the mechanical exfoliation of graphene in 2004. Starting from graphene, 2D materials now have become a big family with numerous members and diverse categories. The unique structural features and physicochemical properties of 2D materials make them one class of the most appealing candidates for a wide range of potential applications. In particular, we have seen some major breakthroughs made in the field of 2D materials in last five years not only in developing novel synthetic methods and exploring new structures/properties but also in identifying innovative applications and pushing forward commercialisation. In this review, we provide a critical summary on the recent progress made in the field of 2D materials with a particular focus on last five years. After a brief backgroundintroduction, we first discuss the major synthetic methods for 2D materials, including the mechanical exfoliation, liquid exfoliation, vapor phase deposition, and wet-chemical synthesis as well as phase engineering of 2D materials belonging to the field of phase engineering of nanomaterials(PEN). We then introduce the superconducting/optical/magnetic properties and chirality of 2D materials along with newly emerging magic angle 2D superlattices. Following that, the promising applications of 2D materials in electronics, optoelectronics, catalysis, energy storage, solar cells, biomedicine, sensors, environments, etc. are described sequentially. Thereafter, we present the theoretic calculations and simulations of 2D materials. Finally, after concluding the current progress, we provide some personal discussions on the existing challenges and future outlooks in this rapidly developing field.
基金Projects(21636010,21878342)supported by the National Natural Science Foundation of ChinaProject(2019JJ50758)supported by the Hunan Provincial Natural Science Foundation of China+1 种基金Project(2019TP1001)supported by the Hunan Provincial Science and Technology Plan Project of ChinaProject(CX20190097)supported by the Fundamental Research Funds for the Central Universities,China。
文摘Transition metal sulfides(TMSs)-based materials have been extensively investigated as effective non-noble catalysts for various applications.However,the exploration of TMSs-based catalysts for hydrogenation of nitro compounds is limited.Herein,CoSx/NC catalysts were prepared by solvothermal sulfurization of ZIF-67,followed by high-temperature annealing(300–600℃)under NH3 atmosphere.It was found that the structures and compositions of the as-prepared CoSx/NC can be readily tuned by varying the annealing temperature.Particularly,CoSx/NC-500,which possesses higher degree of S defects and larger specific surface areas,can achieve high conversion,selectivity and stability for catalytic reduction of nitro compounds into amines under mild reaction conditions.
基金The Deanship of Scientific Research at Princess Nourah bint Abdulrahman University,through the Research Groups Program Grant no.(RGP-1440-0003)
文摘In this work,we have reported the synthesis and spectroscopic characterization of captopril(Cap)coordination compounds:Cu(Cap)·2H 2O,Cr(Cap)·H 2O,Zn(Cap)·3H 2O and Mg(Cap)4.Herein,it is worthily mentioned that the FTIR spectroscopic technique was employed to recognized the nature of coordination between captopril ligand and copper,chromium,zinc and magnesium(Ⅱ)metal ions.In view of the infrared spectroscopic tool,the copper(Ⅱ)metal ion coordinated toward captopril drug ligand through sulfur atom of SH group dependent on the absent of stretching vibration band of—SH.Based on this result,the stretching motion ofνa(COO)shifts clearly indicates that Cu 2+,Cr 2+,Zn 2+and Mg 2+the carboxylic group is employed as coordinative site for all compounds as a metal-ligand coordinative bond.As a general behavior,it is verified that the coordination compound thermal stability(considering the release of captopril molecules,not the release of water molecules)is affected by the metal cation radius:minor radius is associated with higher thermal stability,probably due to a higher metal-captopril bond dissociation enthalpy.
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs)and their heterostructures(HSs)exhibit unique optical properties and show great promise for developing next-generation optoelectronics.However,the photo-luminescence(PL)quantum yield of monolayer(1L)TMDs is still quite low at room temperature,which severely lim-its their practical applications.Here we report a PL enhancement effect of 1L WS_(2) at room temperature when con-structing it into 1L-WS_(2)/hBN/1L-MoS_(2) vertical HSs.The PL enhancement factors(EFs)can be up to 4.2.By using transient absorption(TA)spectroscopy,we demonstrate that the PL enhancement effect is due to energy transfer from 1L MoS_(2) to 1L WS_(2).The energy transfer process occurs on a picosecond timescale and lasts more than one hundred picoseconds which indicates a prominent contribution from exciton-exciton annihilation.Furthermore,the PL en-hancement effect of 1L WS_(2) can be observed in 2L-MoS_(2)/hBN/1L-WS_(2) and 3L-MoS_(2)/hBN/1L-WS_(2) HSs.Our study provides a comprehensive understanding of the energy transfer process in the PL enhancement of 2D TMDs and a fea-sible way to optimize the performance of TMD-based optoelectronic devices.
基金supported by the Fundamental Research Funds for the Central Universities(WK9990000102,WK2030000035).
文摘The study of oxide heteroepitaxy has been hindered by the issues of misfit strain and substrate clamping,which impede both the optimization of performance and the acquisition of a fundamental understanding of oxide systems.Recently,however,the development of freestanding oxide membranes has provided a plausible solution to these substrate limitations.Single-crystalline functional oxide films can be released from their substrates without incurring significant damage and can subsequently be transferred to any substrate of choice.This paper discusses recent advancements in the fabrication,adjustable physical properties,and various applications of freestanding oxide perovskite films.First,we present the primary strategies employed for the synthesis and transfer of these freestanding perovskite thin films.Second,we explore the main functionalities observed in freestanding perovskite oxide thin films,with special attention to the tunable functionalities and physical properties of these freestanding perovskite membranes under varying strain states.Next,we encapsulate three representative devices based on freestanding oxide films.Overall,this review highlights the potential of freestanding oxide films for the study of novel functionalities and flexible electronics.
基金Project([2004]52) supported by the Scientific Research Foundation for the Returned Overseas Chinese Scholars
文摘Novel transition metal complexes of bis(diarylsubstitutedthiophosphoryl)imines ligand derived from O,O-di(p-methoxylphenyl)thiophosphoryl chloride and O,O-di-(p-methoxylphenyl)thiophosphoryl amine with Cu(Ⅱ ),Co( Ⅱ) ,Ni( Ⅱ) ,Fe(Ⅱ ) and Mn( Ⅱ ) were synthesized. The formation mechanism of complexes and their stereochemistry structures were investigated according to elemental analysis,infrared spectra and 31P-nuclear magnetic resonance spectra. The extractions of the ligand for different divalent metal ions,such as Zn(Ⅱ ),Cd( Ⅱ) ,Cu( Ⅱ) ,Ni( Ⅱ ),Fe( Ⅱ) ,Sn( Ⅱ) ,Mn( Ⅱ) ,Pd( Ⅱ) ,Hg( Ⅱ) and Fe(Ⅲ),were investigated in sulphate solution,respectively. The results show the metal atom is coordinated by 4 sulfur atoms in a square-planar fashion,and the titled compound has not only powerful ability to coordinate with cadmium from aqueous solution with a high extractive rate about 61.20% and a relatively weak complexation for other divalent metals with the extractive rate from 2.46% to 36.66%,but also a good selectivity to Fe(Ⅲ ).
基金Scientific Research and Innovation Team Program of Sichuan University of Science and Engineering(SUSE652B004,2024RC13)Special Basic Cooperative Research Programs of Yunnan Provincial Undergraduate Universities Association(202101BA070001-085)。
文摘Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inferior to that of platinum(Pt)metal.Preparation of multi-elemental alloy and construction of heterostructure are considered as highly effective methods to enhance hydrogen production activity.Herein,a novel quaternary CoMoSSe alloy with heterostructure was synthesized on the surface of carbon black(CB)particles(CoMoSSe@CB)by a simple Sol-Gel process and thereafter served as HER catalyst.Compared to CoSe@CB and MoS2@CB electrocatalysts,CoMoSSe@CB exhibits superior HER activity with a low overpotential of 190 mV at-10 mA·cm^(-2) and a Tafel slope of 62 mV·dec^(-1).This improvement is attributed to the alloying effects among Co,Mo,S and Se,as well as the heterogeneous structure in the composite material,which regulate the electronic structure and intermediate free energy,thereby increasing the number of active sites and enhancing charge-transfer ability.This work can provide new ideas and concepts for designing novel and efficient TMD electrocatalysts.
